Fuschi Et Al 2022 Microplastics in The Great Lakes Environmental Health and Socioeconomic Implications and Future

pubs.acs.
org/journal/ascecg Perspective
Microplastics in the Great Lakes: Environmental, Health, and

Socioeconomic Implications and Future Directions
Claire Fuschi, Haihui Pu, Margaret MacDonell, Kurt Picel, Maria Negri, and Junhong Chen*
Cite This: ACS Sustainable Chem. Eng. 2022, 10, 14074−14091 Read Online
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ABSTRACT: Microplastics (MPs) are tiny pieces of plastic (<5 mm) that have been manufactured, shed from textiles, or formed as
the degradation products of macroplastics. They can be taken up by aquatic organisms, leading to their incorporation into the food
chain. Humans can consume MPs from fish as well as other impacted sources including bottled and tap water. MPs may pose risks to
exposed organisms, and they can also act as vectors carrying additional adsorbed chemical pollutants and pathogens. MPs are an
especially important focus regarding the Great Lakes because plastics comprise most of the litter, and the Great Lakes serve as a
source of drinking water for 40 million people. This perspective summarizes the current state of MP pollution in the Great Lakes and
potential risks posed to the environment, wildlife, and humans. A survey of detection, separation, and quantification methods is
included. Potential remedies are explored, focusing on policy, human behavior, and the goal of a circular economy. Further research
directions include standardizing detection and removal methods, assessing the health risk of MPs in the Great Lakes, and evaluating
mitigation options.
KEYWORDS: Microplastics, Pollution, Great Lakes, Hazards, Regulation
■ INTRODUCTION
Microplastics (MPs) are pieces of plastic less than 5 mm in
Primary MPs can also be generated by washing clothes made
of polymer fabrics such as polyester, nylon, and acrylic,3 just as
length,1 and they exist in a variety of shapes, sizes, colors, microfibers can be generated by washing natural fabrics such as
polymer types, and densities. MPs can originate from multiple cotton and wool. Various estimates of MPs in surface waters
sources, and they are reported to have been found in 90% of across the globe suggest that microfibers from multiple sources
surface waters worldwide.2 Primary MPs are manufactured for might account for roughly 70% to 90% of the total.2 Ross et al.
analyzed MPs in the Arctic Ocean and found that 73% of
commercial and industrial uses, such as glitter3 and nurdles
synthetic fibers present in the collected samples were polyester
(which are pellets used to make plastic products).4 These
microfibers and resembled characteristics of polyethylene
materials are not readily biodegradable, so when MPs enter the
terephthalate (PET) from textiles, suggesting that much of the
environment, they tend to persist. Until a few years ago, a
ocean’s MPs could originate from home laundry.6 Vassilenko et
number of exfoliant cleansers contained microbeads smaller
al. reported that a single clothing item could release more than a
than 2 mm in diameter at levels up to 10% by weight.5 Most
microbeads in personal care products are 1 mm or smaller.
Although the United States banned these beads from rinse-off Received: May 15, 2022
cosmetics and over-the-counter drugs such as toothpaste in Revised: September 14, 2022
2015 (the ban went into effect in 2018), many years of Published: October 18, 2022
discharges prior to the ban and releases from other products
have resulted in their presence in U.S. surface waters, including
the Great Lakes.
© 2022 The Authors. Published by
American Chemical Society https://doi.org/10.1021/acssuschemeng.2c02896
14074 ACS Sustainable Chem. Eng. 2022, 10, 14074−14091
ACS Sustainable Chemistry & Engineering pubs.acs.org/journal/ascecg Perspective
hundred to seven hundred thousand fibers during a laundry from a WWTP over a year.22 Because most influent MPs are
cycle, with a wide range of values affected by conditions ranging removed to the WWTP sludge, the land application of these
from the ratio of water to textile to temperature, use of detergent, biosolids (most often to amend soil on agricultural lands) can be
first laundering, and more.7,8 The same study estimates that the a source of MPs in aquatic systems via surface runoff.
annual release of microfibers to the aquatic environment from all Meanwhile, WWTP sludges that are disposed of in landfills
households in Canada and the United States combined could also represent a source of MPs in the terrestrial environment.
total 878 t, with U.S. households accounting for more than 90% Sewage overflow events21 and stormwater runoff23 are other
(per more than 127 million households compared with 14 sources of MPs in aquatic environments. As an example of the
million for Canada, based on 2018 and 2017 census data, latter, Werbowski et al. found that stormwater runoff in the San
respectively).6 Interestingly, the reported average number of Francisco Bay contained many more MP particles than
natural microfibers released from laundering cotton and wool wastewater effluent, with fibers and black rubber fragments,
textiles was essentially the same as the highest average among all likely originating from road-worn tires, comprising about 85% of
synthetic textiles reported (which was for mechanically treated all particles in the runoff.23
polyester fleeces and jerseys, about 6-fold higher than that for MPs are also found in drinking water, from both bottled and
woven nylon textiles with filament-type yarn). tap water samples. In a study of 159 samples from 14 countries,
Secondary MPs originate from fragmentation of larger plastics Kosuth et al. found that 81% contained anthropogenic particles,
like water bottles and plastic bags due to environmental a general term indicating MPs.24 From the more than 30 samples
degradation processes that include biodegradation, photo- across 19 U.S. cities, the mean concentration was about 9
degradation, oxidative degradation, thermal degradation, and particles/L. In a study of three drinking water treatment plants in
hydrolysis.9,10 Because of the vast amount of macroplastics that the Czech Republic, Pivokonsky et al. found that MP removal
enter the environment, many have assumed that most MPs are efficiencies ranged from 70%−83%. For MP fibers, the treatment
secondary MPs.11,12 Globally, the most commonly produced plant that used only basic coagulation, flocculation, and sand
polymers are polyethylene (PE), including high- and low- filtration achieved a removal efficiency of 25%, while the two
density (HDPE and LDPE), polypropylene (PP), polyvinyl plants that included a conventional activated carbon finishing
chloride (PVC), polystyrene (PS), including expanded poly- step achieved 80% to 90% removal.25 Like for wastewater
styrene (EPS), and PET.13,14 These polymers are also treatment, the authors found that, in general, traditional
commonly found in freshwater systems. Among their many drinking water treatment processes are promising for removing
uses, PVC, PS, and PET are used to make food and beverage MPs and suggested optimizing conditions (such as coagulant
containers and packaging; HDPE and LDPE are used to make dose, pH, and residence time) as well as evaluating more
plastic bags, bottles, and other containers; and PP is used to advanced treatment technologies to increase removal efficien-
make bottles and other containers as well as toys.15−17 Thus, cies.26
many of the MPs contaminating the Great Lakes are likely the Because MPs are so common and persistent in the
result of macroplastic degradation. environment, questions arise regarding potential ecological
Wastewater treatment plants (WWTPs) are a source of MPs and human health effects as well as potential remedies and
in aquatic environments.18 From a recent review of 21 studies, mitigations. The Great Lakes are a source of drinking water for
Iyare et al. reported that, on average, preliminary and primary 40 million people, 10% of the United States population and 30%
treatment WWTPs remove 72% of MPs from influent of the Canadian population. The Great Lakes account for 84% of
wastewaters, while plants with secondary treatment remove North America’s surface fresh water and 21% of all surface fresh
88% and those with tertiary treatment remove 94%.19 In 2014, water in the world, and their maritime economy supports more
Arvai et al. reported that nearly 1,450 municipal WWTPs than 300,000 jobs, translating to $8.8 billion in wages.27
collectively discharged 4.8 billion gallons of treated effluent daily Considering just one aspect of this economy, the Great Lakes
to the Great Lakes basin, and treatment plants with secondary commercial, recreational, and tribal fisheries are valued at over
and higher treatment accounted for 98% of the total wastewater $7 billion annually and support over 75,000 jobs.28 Thus, MP
flow discharged to the basin. The authors also noted that contamination in the Great Lakes has the potential for
secondary treatment is a minimum standard for U.S. WWTPs, substantial impacts, and the need to better understand, control,
and analyses of treatment performance with respect to total and reduce this contamination is increasingly urgent.
wastewater flow showed that more than 95% of the wastewater
discharged into the Great Lakes basin met the performance
requirement for advanced treatment.20 Thus, most WWTPs
■ CURRENT STATE OF MICROPLASTIC POLLUTION
IN THE GREAT LAKES
discharging to this basin are capturing most of the MPs they The Great Lakes span more than 94,000 square miles and
receive, consistent with the general finding that 90% or more of account for 95% of surface freshwater in the United States and
MPs in influent wastewaters are removed to the sludge of a 18% of the world’s surface freshwater supply. Given this scale,
WWTP. our understanding of MP pollution across the Great Lakes is
Despite the small fraction released with effluent, individual very limited. As public awareness of MPs in the environment has
particle and fiber counts can be substantial and accumulation is increased, so too have research studies, and more information
ongoing. A study by Conley et al. of three WWTPs in South continues to be developed that helps frame the issues. According
Carolina reported MP removal efficiencies ranging from about to calculations by the Rochester Institute of Technology, nearly
85% to more than 97%. Using source modeling, they estimated 22 million pounds of plastic debris enter the Great Lakes every
that for smaller plants with lower removal efficiencies, up to 600 year, with most (11.6 million pounds) entering Lake Michigan.
million MP particles might be released daily.21 For an annual Following that are Lake Erie (5.6 million pounds), Lake Ontario
perspective, Freeman et al. estimated that even a removal (3.2 million pounds), Lake Huron (1.4 million pounds), and
efficiency of 99% for particles with any dimension less than 100 Lake Superior (more than 70,000 pounds).29 Further, most
μm could lead to upward of 100 billion MP particles released shoreline litter is plastic. For example, of more than 25,000
14075 https://doi.org/10.1021/acssuschemeng.2c02896
ACS Sustainable Chem. Eng. 2022, 10, 14074−14091
Figure 1. (A) Reported concentrations of MPs within the surface waters of five lakes in the Great Lakes system. (B) Three studies report MPs
concentrations within Lake Superior. Note change of scale on Y-axis between (A) and (B). Reprinted with permission from ref 34. Copyright 2021
Elsevier.
pounds of trash volunteers removed from Great Lakes beaches Earn et al. published an in-depth review in which they
in 2021, more than 85% was at least partly plastic.30 Debris that collected data from 11 papers to summarize the current state of
collects on shorelines likely fragments into smaller pieces over knowledge regarding MP concentrations in the Great Lakes.34
time, adding to existing MPs in the lake system. They reported high variation among studies, likely based on
The distribution of polymers in the lake system varies, as sample locations and sampling and analysis methods. Overall,
illustrated by a study from Lenaker et al. of 20 sediment samples reported surface water concentrations ranged from 0 to about
from Lake Michigan and 12 from Lake Erie.31 They reported 318,000 particles/km2 in Lake Superior,34−37 886,000 particles/
that PET, HDPE, and semisynthetic cellulose (S.S. Cellulose) km2 in Lake Huron,34−36 100,000 particles/km2 in Lake
were most common among the 37 particles analyzed from Lake Michigan,38 and 1,264,000 particles/km2 in Lake Erie,34−36
Michigan sediment; and synthetic cellulose, PP, and PVC were with a similar upper value (nearly 1,244,000 particles/km2)
most common among the 44 particles analyzed from Lake Erie reported for Lake St. Clair (note that this relatively small lake has
sediment. The authors also synthesized results of other Great roughly 1% the volume of Lake Ontario and is not typically
Lakes studies that reported low-density MPs such as EPS foams included in the set of Great Lakes)34 (Figure 1A). Earn et al.
and PP fragments were more abundant in surface water samples ranked the lakes from highest to lowest by average MP
while higher-density particles such as PET were more abundant concentrations in round numbers, as follows: Lake St. Clair
lower in the water column and into the sediment. Also, fibers (355,000 particles/km2), Lake Erie (162,000 particles/km2),
were much more prevalent in surface samples from the Lake Huron (111,000 particles/km2), Lake Superior (35,000
tributaries than in the Great Lakes. Those results suggested particles/km2), and Lake Michigan (17,000 particles/km2). Cox
et al. published a study quantifying the concentration of MPs in
denser particles are likely settling out in the Great Lakes, which
Lake Superior surface water after Earn et al. published their
could help explain the difference in relative abundance of fibers
review, reporting about 30,000 particles/km2 on average,39
in tributary versus lake surface water samples. These findings are
which is very similar to the average reported by Earn et al. As
consistent with the those of Koelmans et al. from their review of
noted, these estimates are from a relative handful of measure-
multiple studies that focused on MPS in freshwater−notably ments considering the vast expanse of the Great Lakes, and
that the relative abundance of polymer types likely reflects reported concentrations range over multiple orders of
plastic production and polymer density differences.10 magnitude. Earn et al. illustrated the high variability across the
McNeish et al. sampled fish from three Lake Michigan limited set of samples for a single lake, as shown in Figure 1B.34
tributaries and analyzed them for the presence of MPs. They The average MP concentrations presented in studies of the
found that 85% of the fish (across 11 different taxa) contained Great Lakes are comparable to those from marine surveys in the
MPs in their digestive tracts, with an average of 13 particles per South Pacific Gyre, the North Atlantic Gyre, and the North
fish.32 MPs have also been found in the guts of fish from Lake Pacific Gyre−which have been reported as 26,900 particles/km2,
Ontario and Lake Superior, making up 35% to 59% of the total 20,300 particles/km2 and 334,300 particles/km2,10,40,41 respec-
anthropogenic particles found in the fish, and surpassing levels of tively, suggesting that the Great Lakes are similarly polluted with
MPs found in marine organisms.33 Kosuth et al. investigated the plastics as those impacted marine settings. Interestingly, the
level of MPs in 12 brands of beer made with water sourced from Great Lakes may be more at risk to MP creation than oceanic
the Great Lakes, as well as tap water from seven of the nine gyres according to Driedger et al.42 This is because the surface
municipalities represented within the brands. The average currents in the Great Lakes are not steady like in oceanic gyres
concentration found in beer was about 4 particles/L, and the and instead are impacted by short bursts of surface wind stress.
average in tap water sourced from the Great Lakes was about 1.6 The Great Lakes also have a greater shoreline-to-surface area
particles/L.24 These studies and others indicate the extent to ratio, and these two factors combined would intensify debris
which MPs permeate the Great Lakes ecosystems. interactions with the shoreline where plastic debris is subject to
more intense mechanical and photooxidative degradation.43 In mg/L for 7 days induced microbiome dysbiosis and changes in
fact, macroplastic debris from the Great Lakes has already been metabolomic profiles.54 In another 48 h aquatic toxicity test with
confirmed to be undergoing mechanical and oxidative weath- a different MP, exposure of the freshwater crustacean Daphnia
ering, suggesting they are degrading into MPs. Of samples from magna to ground (milled) PET textile microfibers led to
Lakes Huron, St. Clair, and Erie combined, 78% and 37% increased mortality at concentrations of 12.5 to 100 mg/L
showed signs of mechanical and oxidative degradation, (variability was high).55 Meanwhile, in a terrestrial invertebrate
respectively.44 The hydraulic residence time of water in the toxicity study, earthworms exposed to PS MPs at concentrations
Great Lakes may also play a role in the amount of MPs that of 1−2% g/g soil for 30 days exhibited decreased growth and
persist in each lake. For example, Hoffman and Hittinger29,45 increased mortality.56
modeled MP movement throughout the Great Lakes and found Earn et al. completed a review of 75 studies that investigated
that Lake Michigan and Lake Superior had the lowest number of the impacts of plastic debris on freshwater biota. 99% were
particles leaving to other lakes. They hypothesized this was due laboratory studies (where concentrations are 10 orders of
to the longer hydraulic residence times of Lake Superior (173 magnitude higher than in the environment), and nearly all tested
years) and Lake Michigan (62 years) compared to Lake Huron MPs, measuring effects such as mechanical stress or changes in
(21 years), Lake Ontario (7.5 years), and Lake Erie (2.7 reproduction, behavior, growth, and development.34 They
years).29,45 More research is warranted to explore the sources found that of nearly 400 effects tested across the studies, 60%
and fate of MPs across the Great Lakes, to understand potential were detected−and about two-thirds of these were at
exposures. ecologically relevant levels that spanned organism, population,
■ POTENTIAL HAZARDS
MPs and nanoplastics (NPs) have been shown to contaminate
community, and ecosystem. From their analysis of 20 studies,
Earn et al. determined that the likelihood of an effect being
detected is influenced by the type, size, and shape of MP tested.
every level of the food web in the Great Lakes−spanning algae,46 Regarding shape, they noted that although microfibers caused an
invertebrates, mussels47 and fish,32,33 and they have been shown effect in 58% of cases, all those data points were from the same
to bioaccumulate in both freshwater and marine species.48,49 In study. Based on data from 5 studies, they found that spheres
addition to the hazards posed by these MPs, chemicals added were reported to cause an effect in 45% of cases, while data from
during plastics production such as plasticizers and flame 19 studies indicated that fragments caused an effect in 24% of
retardants can leach out as they degrade in the environment. cases. The authors acknowledged that others had reported fibers
Moreover, MPs can carry sorbed pollutants and bacteria in and fragments tended to be more harmful than spheres.
biofilm that establishes on their surfaces. Given the scale of the Regarding size, like others, Earn et al. concluded that the
Great Lakes, relatively few data are available to quantitatively smaller the MP, the more likely it is an effect will be detected.
assess hazards and risks associated with its MPs. More This pattern was especially seen in spheres, with the smallest
information is needed about the suite of compositions, particles (0.01 to 0.09 μm) causing an effect in 88% of instances
characteristics, environmental fate and transport aspects, and while only 43% and 27% of effects were detected in the next
concentrations of MPs at numerous exposure points over the larger size classes (1−9 and 10−90 μm, respectively). An
wide range of environmental conditions in space and time that increasing number and severity of effects for smaller particles is a
represent the Great Lakes system. With regard to ecological
trend that has been shown in literature,57−59 likely due to the
hazards, in a quality criteria assessment of MP effect studies,
ability of smaller micro- and nanosized particles to cross the
deRuijter et al. found that the weight of evidence was strongest
intestinal barrier and translocate to other systems and
for mechanisms related to inhibition of food assimilation and/or
tissues.60,61
decreased nutritional value and those related to internal and
Furthermore, the surfaces of MP particles can serve as a
external physical damage.50 Food dilution can occur when
organisms ingest low-calorie MPs, supplementing some of their substrate for biofilm growth, which can lead to the sorption of
normal food intake. Koelmans et al. examined nine studies that other pollutants, including the (hydrophobic) per- and
quantified the hazardous concentrations for (the most sensitive) polyfluoroalkyl substances (PFAS).62 Researchers from the
5% of the species in an aquatic community (HC5) and found Illinois Sustainable Technology Center submerged samples of
that reported values ranged from less than 1 to about 100,000 three common types of MPs in Muskegon Lake water and in the
particles/L, with a median of nearly 76 particles/L.12 channel connecting it to Lake Michigan for one and three
Laboratory experiments can shed light on what potential months, and in the laboratory water for one month. They found
effects may occur from MP exposure, recognizing that relevance that PFAS consistently adhered to all types of MP particles, and
to environmental exposure conditions is crucial if results are to that the MPs adsorbed more PFAS from lake or channel water
be useful for risk assessments. The rodent model has been used than from laboratory water, 24 to 259 times compared to 1/7 to
for decades to assess potential human toxicity. In a 90-day rat 1/4 times the background levels. PFAS amount adsorbed ranged
study (representing subchronic exposure), ingestion of water from 0.052 nanogram to 0.87 nanogram PFAS per gram of
containing 5 mg/Land 50 mg/L of PS MPs induced plastic in the Muskegon Lake water. This is likely due to the
cardiomyocyte apoptosis and oxidative stress, with implications organic matter in the lake water that formed biofilms on the MPs
for subsequent heart fibrosis and cardiac dysfunction.51 In a and aided adsorption.62 Two heavily studied PFAS, perfluor-
mouse study, ingestion of water containing PS MPs at 0.1 and 1 ooctanoic acid (PFOA) and perfluorooctanesulfonic acid
mg/L induced gut damage and metabolic disorders at the higher (PFOS), can cause cancer, reproductive and developmental
dose.52 For ecotoxicity, medaka are a common test organism. issues, liver and kidney damage, and immunological effects in
Exposure of this fish to a nominal concentration of 100,000 PS laboratory animals.63 Vosshage et al. found that snails (R.
MP particles/L for 48 h led to inhibition of growth and egg balthica) that grazed on biofilms grown on plastic substrates
production.53 In a related species, exposures of larval zebrafish to exhibited reduced growth rates compared to the control which
PS MPs 5 and 50 μm in diameter at concentrations of 0.1 and 1 fed on biofilms grown on glass.64
Moreover, biofilms are not only composed of the same mesh size can create wide variability depending on the pore size,
microbes found in the surrounding water environment but with smaller pores leading to much higher collection
include bacteria that are distinct, and sometimes more concentrations.80 For instance, plankton nets can recover MP
pathogenic than the surrounding environment. Wu et al. concentrations 30 times higher than manta nets.81 Nets and
found that compared to biofilms on rocks and leaves, biofilms pumps allow for the collection of large water samples which
on MPs “selectively enriched” certain antibiotic-resistant genes leads to a more accurate and representative concentration.80
(ARGs) and other pathogenic bacteria.65 McCormick et al. Reducing the sample size can be done by filtering the larger
found that MPs collected from nine Illinois rivers had initial water sample with decreasing steel meshes.82 However,
microbiomes that were less diverse than the corresponding the issue of contamination arises as Nylon nets and pumps may
natural substrates, and contained greater populations of lead to the addition of MPs to samples.80 Sampling from lake
common human intestinal pathogens.66 Biofilm formation sediment is also an option to test for MPs. Both water and
ends with the formation of top-level communities or the sediment samples are affected by variability due to MP
diffusion of biofilms into the water matrix,67 which suggests that properties such as density, and environmental conditions such
biofilms on MPs could serve as vectors of pathogenic bacteria. as winds and currents. However, sediment sampling can at least
The observed interaction between MPs and microbiome has limit the variability due to humidity, which can impact water
implications regarding the effect of ingested MPs on an samples.80
organism’s gut flora. It could serve as another means of harming Regarding separation, filtering or sieving is the most common
an animal or human, as the gut microbiome is linked to the method to initially separate MPs from water and sediment. Next,
immune system.68 one can utilize density separation (flotation) by adding the
MP consumption affects aquatic wildlife and humans alike. sample to a salt-saturated solution. Sodium iodide (NaI) is
Senathirajah and Palanisami found that the average person perhaps one of the best options for this step, as it can be recycled
consumes up to a credit card’s worth of plastic (5 g) per week.69 for multiple cycles and does not harm the environment.
Another study by Cox et al. found that the humans may ingest up However, it cannot be used with a cellulose filter as they can
to 39,000−52,000 particles annually (depending on age and sex) react to turn the filter black and make visual inspection
from seafood, sugars, salts, honey, and alcohol alone. When difficult.80 Oil can be added to salt-saturated solutions to
considering inhalation of MPs, the annual counts rise to improve recovery rates.83 If instead elutriation is used, a liquid
74,000−121,000 particles. Drinking only bottled water adds such as water is injected at the bottom of the sample inside a
90,000 particles annually, averaged across age and sex, while column, which takes advantage of the buoyancy of MPs to
drinking tap water adds an average of 4,000 particles annually.70 separate them from the sinking sediment.84 Elutriation may
Additional evidence for the human consumption of MPs comes allow for better representativeness because it is easier to use for
from Schwabl et al., who analyzed human excrement for MPs larger volume samples.
and confirmed their presence in the stool of all eight study The next step is the removal of organic matter, which helps to
participants.71 Nanoplastics have even been detected and simplify the identification of MPs, as dark pieces of organic
quantified in human blood.72 The potential negative effects of matter can be confused with MPs. Digestion of organic material
MPs are not only relevant to wildlife either. Han et al. found that can be achieved through oxidative, acidic, alkaline, or enzymatic
exposure to MPs made of polyvinyl chloride (PVC) and methods. However, the acidic and alkaline methods may both
acrylonitrile butadiene styrene (ABS) at concentrations of 0.01 damage or discolor the plastics, which can lead to inaccurate
mg/mL to 1 mg/mL over 4 days caused human-derived cells to counts, especially when the quantification relies on visual
release interleukin 6 (IL-6) and tumor necrosis factor-α (TNF- inspection.85 Enzymatic digestion effectiveness can vary but it is
α) proteins in an immune response.73 Schirinzi et al. have safer than acidic or alkaline digestion.86 Hydrogen peroxide
demonstrated that human cerebral and epithelial cells exposed (H2O2) is an oxidizing agent which digests organic matter more
to low doses of polyethylene (PE) and polypropylene (PP) MPs efficiently than acids and bases, and does not damage the MPs.87
(10 ng/mL to 10 μg/mL) undergo oxidative stress in the form of There are two main categories of detection methods: visual
reactive oxygen species (ROS) generation.74 There is growing inspection and chemical characterization. Visual inspection
evidence that nanoplastics can undergo cellular uptake in the entails the utilization of a stereoscope or microscope to find and
lungs and gut.75−78 The extent and implications of MP and NP quantify MP particles visually. However, this method is time-
bioaccumulation in humans should be more thoroughly consuming and creates large sources of error because it is
investigated. subjective. Thus, it is not recommended for particles smaller
MP ingestion can be hazardous due to food dilution and than <500 μm.88 Visual inspection can lead to variances in total
physical damage to organisms.50 The biofilms that grow on MP count as great as 40%, due to factors such as experience and
surfaces allow pollutants to become concentrated and can serve fatigue.89 Further, up to 70% of visually detected MPs may be
as vectors for harmful bacteria populations. There is even other materials that are misclassified.90 This is because it is
evidence that plastics (and other man-made debris) can difficult to discern actual MPs from organic materials. However,
transport invasive species across bodies of water.79 The potential the advantages to this method include that it is widely accessible
for MPs to cause harm to the environment, aquatic ecosystems, and allows the classification of MP particles by size, color, and
human health, and transmit illness must be further researched. shape which can help determine their origins. Also, staining the
■ DETECTION, SEPARATION, AND QUANTIFICATION

METHODS
particles with dye, such as in Nile Red staining, can improve
accuracy and result in recovery rates as high as 96.6%.91
Regarding chemical characterization, there are several
The MP detection process consists of collection, separation, commonly used methods. Fourier transform infrared spectros-
inspection, and finally quantification. According to an in-depth copy (FTIR), Raman spectrometry, and thermal analysis as
literature survey by Prata et al., the most common collection pyrolysis gas chromatography−mass spectrometry (py-GC-MS)
method used is nets, followed by pumps, and last sieves. Net are highly accurate, and FTIR and Raman can preserve the MP
Figure 2. Food, Energy, Water, and Plastic nexus. Adapted with permission from ref 99. Copyright 2018 American Chemical Society.
particles. However, these methods are time-consuming, and

require complex equipment and trained personnel. Also, FTIR
■ FOOD, ENERGY, WATER, PLASTIC NEXUS
MPs play an important role in the food, energy, water nexus, and
can lose accuracy with particles under 20 μm, and the accuracy even the food, energy, water, waste nexus, as illustrated in Figure
of Raman spectroscopy can be worsened by fluorescent 2. Each aspect is integrally tied to one another.99 First, fossil fuels
pigments and additives. These drawbacks limit the widespread are used to make plastics.100 If the world aims to keep the global
application of these methods and prevent on-site detection.80 temperature from rising below 1.5 °C (as stated in the Paris
Scanning electron microscopy (SEM) analysis is helpful for Climate Agreement (2015)), then greenhouse gas emissions
discerning small plastic particles but is not appropriate for large from the plastic lifecycle must be drastically reduced. If plastic
samples. A novel detection device consisting of a portable optical production and incineration grow as planned, related green-
sensor which can detect transparent and translucent MPs in house emissions could reach 1.34 gigatons per year in 2030. This
water was developed in 2019.92 However, there is still a need for equates to more than 295 new 500-megawatt coal-fired power
widespread, portable, inexpensive, and accessible detection plants. Plastic-related greenhouse emissions could reach over 56
methods. gigatons in 2050, which is 10 to 13% of the entire remaining
Standardization of collection and detection procedures would carbon budget for the planet.100 The Center for Environmental
help to compare across different studies, as well as provide International Law (CIEL) suggests several methods of lessening
credibility to results. Prata et al. suggest defining a standard mesh the contribution of plastics to climate change in a 2019 report.
size, minimum volume of water, a standard sediment sampling These suggestions include stopping production of single-use
depth, and number of replicates that would provide sufficient plastic, preventing development of new fossil fuel infrastructure,
representativeness.80 Regarding sediment sampling, 11 samples moving toward zero-waste communities, enacting extended
per 100 m of beach can estimate MP concentration at a 90% producer responsibility, and creating ambitious goals for
confidence level.93 The National Oceanic and Atmospheric reducing greenhouse gas emissions from all sectors.100
Association (NOAA) recommends using 400 g per sediment The food industry also leads to greenhouse gas emissions,101
sample, followed by drying and weighing,94 while the Marine and plastic is often used in food packaging. When food is wasted,
Strategy Framework Directive (MSFD) technical subgroup both the food and plastic lead to greenhouse gas emissions and
suggests using at least five replicates of the top 5 cm of pollute the environment, either by sitting in landfills or through
sediment.95 Standardization of separation and digestion waste incineration.100,102 Furthermore, plastic packaging is
procedures could include defining NaI as the standard for salt thought to be a net good as it can extend the shelf life of
many food items. However, a 2018 report by the Friends of the
saturation or H2O2 as the standard for oxidative digestion.
Earth Europe found that although the amount of plastic
Regarding detection, standards for visual and chemical
packaging has increased since the 1950s in the EU, so has the
characterization could be defined as well.
amount of food waste. In certain situations, plastic packaging
Padervand et al. published a review of MP removal methods.
may actually serve to increase the amount of food waste that is
They found that the most effective methods out of those generated, such as with convenience foods like precut produce
reviewed are membrane bioreactors (>99%), conventional and salads.103 The report also gives recommendations on how to
activated sludge (98%), wastewater treatment plants (>95%), reduce plastic and food waste, which include investigating the
and algae adsorption (94.5%).18 Another highly effective causes of food waste and its intersection with plastic packaging,
method not included in the review is agglomeration-fixation and investing in waste prevention systems.103
by organosilanes (monomeric silicone-based chemicals)96 MPs are also presently tied to the food we consume because
which has an efficacy of up to 99.4%.97 Although effective they are present throughout the food chain and are often
removal methods exist, some experts fear that MP removal from consumed as a result of certain foods and drinks, bottled water
the environment is too gargantuan a task. The particles are versus tap water for example.70 Furthermore, the greenhouse gas
extremely pervasive; they are present throughout bodies of emissions from the food industry and plastic production
water, soil, and even raining from the sky.98 The best course of contribute to climate change, which then causes more extreme
action may be preventative measures to stop their entrance into weather patterns.104,105 This sometimes leads to overflow events
the environment in the first place. from flooding, which then contaminates surface waters with
Figure 3. Percentages of litter items in the Great Lakes grouped according to activity on an item-by-item basis. Reprinted with permission from ref 42.
Copyright 2015 Elsevier.
more MPs.106 MPs consumed by plankton can also reduce their can degrade into MPs over time. Another measure that prevents
ability to remove CO2 from the atmosphere.107 The issue of plastic pollution in the Great Lakes is the Annex V of the Great
macro- and microplastic pollution should be thought of as Lakes Water Quality Agreement (GLWQA) which prohibits
inherently tied to climate change and food security. vessels from dumping any garbage into the lakes. However, this
MP pollution and water quality are social inequality issues. A agreement does not cover the pollution originating from land.
report published by the organizations Dig Deep and the U.S. Some municipalities near the Great Lakes have prohibited
Water Alliance analyzed quantitative national data from the smoking on beaches, potentially decreasing the amount of
American Community Survey (ACS) and the U.S. Census macroplastic entering the lakes which then degrade into MPs
Bureau to characterize the water access gap in America.108 The over time. Cigarette butts are made of cellulose acetate, a
report found that race is the strongest predictor of water and photodegradable but not biodegradable plastic. Littering of
sanitation access. Black and Latinx households are twice as likely cigarette butts poses risks to the environment as they have
to lack indoor plumbing and Native American households are collected the chemicals from smoking, and thus toxic-infused
19-times as likely. Household income, education level, and plastic fragments may persist.111 A smoking ban on beaches may
unemployment rates are also predictors. Two million Americans reduce plastic pollution, given that cigarette butts account for
live without running water and basic indoor plumbing, and many much of the litter on all Great Lakes shorelines, according to
more without sanitation. Rural communities are also at risk, with data from Adopt-a-Beach and Great Canadian Shoreline
17% report having issues with safe drinking water. In some Cleanup in 2012 as shown in Figure 3.
states, the number of people without access to indoor plumbing Besides prohibitory measures to limit plastic pollution in the
is increasing.108 The Biden administration is focusing attention Great Lakes, there are also several ongoing projects to aid this
on the intersection of environmental protection and social effort. On the industry side, Operation Clean Sweep (OCS),
justice with an executive order called Tackling the Climate Crisis which is run by the American Chemistry Council and the
at Home and Abroad (2021), which includes the creation of the Plastics Industry Association, promotes best practices to help
government-wide Justice40 Initiative. This initiative aims to manufacturers prevent preproduction plastic such as pellets,
address environmental injustices, as well as deliver 40% of the flakes, and powder from entering waterways.112 However,
overall benefits of environmental justice-related federal invest- enrollment in this program is voluntary, and asking plastic
ments to communities that have been impacted disproportion- manufacturers to hold themselves accountable is not an infallible
ately by health, environmental, economic, and climate issues.109 system. NOAA created the Great Lakes Land-Based Marine
Plastic is inherently linked to energy, water, and food sectors. Debris Action Plan (2014−2019) to address pollution in the
Thus, solving the issue of macro- and microplastic pollution will
Great Lakes. The plan was in collaboration between govern-
be crucial in remedying problems regarding food, water, and
ments, researchers, NGOs, and businesses around the Great
energy, such as water pollution, food contamination, and
Lakes. After the completion of the plan, they have published an
greenhouse gas emissions from plastic manufacturing and waste.
Accomplishment Report with their results.113 Over five years,
■ SOLUTIONS
Finally, potential remedies to the situation should be explored.
NOAA has conducted research and published scientific articles,
guided management and policy makers, educated ∼180,000
people on plastic pollution in the Great Lakes, and removed
There are several measures currently in place that protect the 306,665 pounds of debris through volunteer efforts. Their plan
Great Lakes against MPs, but this protection could be more included identifying research needs surrounding MP pollution
extensive. The Microbead-Free Waters Act signed by President in a workshop held by the International Joint Commission
Obama in 2015 prevents the sale of microbeads in “rinse-off” between the Canadian and US governments, the results of which
cosmetic products. However, this rule allows microbeads to are discussed in the following section. They have also created an
continue to be used in other products such as lotion and online portal that summarizes different plastic-monitoring
makeup.110 It also does not address larger plastic debris, which projects in the Great Lakes, several of which focus on MPs.114
As part of the plan, the City of Cleveland Mayor’s Office of legislation banning microbeads in certain cosmetic products.124
Sustainability and NOAA have coordinated a plastic reduction Utilizing the findings others have published about microbead
campaign called “Don’t Break the Lake” regarding Lake Erie. concentrations, nonprofit organizations 5 Gyres Institute and
The campaign included social media outreach, posting signage Story of Stuff Project led a #BeadFree campaign that included
at water refill stations and grocery stores, mailed inserts in water educating the public and persuading manufacturers to remove
bills, and giveaways of reusable items. The number of reusable microbeads from products.125 Future efforts to effectively limit
bags used by customers have increased, according to preliminary plastic pollution are expected to increase in many directions.
data.113 This result suggests that such campaigns can inspire
behavioral changes, whether reusable bags are the solution or
not. The campaign may have been aided by the issuance of a
■ FUTURE DIRECTIONS FOR REGULATIONS
Plastics can be helpful in achieving certain sustainability goals
toolkit to volunteer advocates listing best practices for such as lessening food waste by lengthening shelf life and
encouraging policy and management changes to limit plastic lessening fuel usage when transporting products due to its light
pollution, called “Plastic-Free Great Lakes: An Advocacy weight in comparison to other materials. MPs can currently be
Toolkit to Make a Difference in Your Community” published viewed as a pollution prevention and waste management issue
in 2018 by the Alliance for the Great Lakes.115 This toolkit rather than something to be done away with entirely, especially
discusses the effectiveness of different policy changes that have because there are currently no detailed standards about different
already occurred in response to plastic pollution in the Great types of MPs.126
Lakes, including the plastic bag fee in Chicago, community The NOAA Marine Debris Program hosted a Microplastics in
initiatives in Evanston, IL, and the refundable deposits on the Great Lakes workshop, gathering experts from governmen-
recyclable plastic items in Michigan and New York. The plastic tal, academic, and industry backgrounds which culminated in a
bag fee in Chicago has led to a 40% decrease in the number of report available online. They agreed on ten recommendations
plastic bags used per shopping trip and a 20% increase in for the International Joint Commission between Canada and the
customers who use reusable shopping bags, according to United States (IJC) to inform their response to the issue of MP
preliminary results.116 NOAA has now published a new five- pollution in the Great Lakes. Some of these recommendations
year plan for 2020−2025, available for viewing on their are to communicate research results to the public and decision
website.117 makers, utilize education, policy, and market-based instruments
Another effort focused on removing plastic pollution from the to encourage pollution prevention, conduct risk assessments
Great Lakes is spearheaded by the nonprofit organization regarding ecological and human health, invest in solution-based
Council of the Great Lakes Region (CGLR) called Great Lakes research, determine the sources and fate of MPs in the Great
Plastic Cleanup, in which 26 debris removal devices were Lakes through modeling, and adopt standardized sampling and
installed in marinas across the Great Lakes.118 The EPA also has analytical methods for measuring MPs.127
a Trash Free Waters (TFW) Program which is complementary Several tools are available to address pollution prevention and
to NOAA’s Marine Debris program. It aims to reduce the reduction. Market-based instruments including bans and fees are
amount of trash entering water bodies in the U.S., targeting zero effective, as it has been found that a fee for “bad” behavior may
trash in 10 years. To do this they will focus on U.S. and have a greater positive impact than a reward for “good” behavior,
international litter prevention strategies, researching impacts of modeling loss aversion. In Montgomery County, Maryland, it
macro- and microplastics on water quality, environment, and was found that a 5-cent tax on disposable plastic bags resulted in
human health, and building partnerships to encourage a 42% decrease in customers who used plastic bags, while a 5-
innovation in material reuse and packaging.119 cent tax reward on reusable bag usage resulted in virtually no
There is currently limited regulation of the large-scale and change in behavior. If each household in Montgomery County
systemic pollution originating from the plastic industry shopped once a week, this could lead to an annual decrease of 18
discharging waste. It is estimated that around 230,000 t of million plastic bags.128 This information can be utilized when
nurdles leak into the oceans every year.120 However, the Plastic drafting policies meant to mitigate plastic pollution. Existing
Pellet Free Waters Act introduced by Senator Dick Durbin in mitigation measures can also be further expanded, such as
2021, and other similar proposed legislation, would make the extending the Microbead-Free Waters Act to include more
EPA responsible for preventing plastic pellets (nurdles) and products than just rinse-off cosmetic products. However,
other preproduction plastic from being discharged into environmental costs of these decisions should be explored so
waterways by facilities that make, use, transport, or package that they are most effective at protecting the environment.
them.121 The Clean Water Act could also be utilized more often The NOAA workshop also suggested classifying MPs as a
to apply to plastic pollution.122 Currently, California is the only chemical of mutual concern (CMC) in the Great Lakes
state that has classified preproduction plastics as pollutants that Ecosystem under the Great Lakes Water Quality Agreement,
must be regulated under the Clean Water Act.123 Given the lack which would mean the United States and Canadian govern-
of extensive plastic pollution regulation on the industry side, the ments would be required to look into reduction strategies.127,129
burden of responsibility is borne largely by the public. Plastic bag Further, Gago et al. suggested that an International Legally
taxes and bans, plastic litter collection efforts on Great Lakes Binding Instrument (ILBI) be drafted to regulate MPs around
shorelines, and campaigns such as “Don’t Break the Lake” the globe.1 This could standardize regulations and make
attempt to encourage sustainable behavior.113 The Alliance for enforcing regulations easier.130 In June of 2021, the House
the Great Lakes’ advocacy toolkit further aims to raise Committee on Science, Space, and Technology: Subcommittee
community awareness of the issue of plastics pollution and on Environment had a hearing on Defining a National
encourages reaching out to legislators.115 Novel research can be “Oceanshot”: Accelerating Ocean and Great Lakes Science
a catalyst for widespread behavioral and policy changes. For and Technology. Although this effort mostly focuses on
example, Dr. Imogen Napper’s research group is credited for exploring and characterizing the entire ocean, plastic pollution
some of the fundamental research which led to an international likely plays a role in the Oceanshot. Dr. Robert Ballard, famed
Figure 4. (A) Estimated annual rates of plastic pollution entering the environment in million metric tons/year ±95% confidence interval from each
scenario from 2016 to 2040. The scenarios are Business as Usual (BAU), Collect and Dispose scenario (CDS), Recycling scenario (RES), Reduce and
Substitute scenario (RSS), and System Change scenario (SCS). (B) Present waste management costs (collection, sorting, recycling, and disposal) in
billion USD ± 95% confidence interval of plastic municipal solid waste by scenario from 2016 to 2040. Reprinted with permission from ref 150.
Copyright 2020 AAAS.
ocean explorer and a witness to the hearing, expressed the emissions, and resulted in a cumulative savings of $2.6 million
potential of marine farming and protecting ocean life as well as per year for Connecticut municipalities.133 Further, the EPR
expanding its productivity. Addressing the issue of plastic programs will likely not result in a rise in consumer prices. The
contamination in ocean crops will definitely play a role in Oregon Department of Environmental Quality of Canadian
realizing the concept of ocean agriculture.131 EPR programs concluded that prices had only risen by $0.0056
Moreover, the NOAA workshop recommended several per item.134 EPR measures could also demand that manufac-
pollution-prevention measures to the IJC. These include turers bear the responsibility of adding filters to washing
governments pursuing Polluter-Pays Principle and Extended
machines to collect microfibers from clothes before they pollute
Producer Responsibility (EPR) policies which would place the
responsibility of dealing with plastic at its end-of-life stage on the the environment.127 Other methods of limiting MP entrance
manufacturers.127 An example of this is a new law in Maine into water environments include the decentralized treatment of
which requires manufacturers to pay the cost of recycling filtration at point sources.135 Drain filters installed in plastic
programs.132 Another EPR program in Connecticut regarding pellet factories would prevent preproduction pellets from
mattresses, paint, electronics, and thermostat has mitigated entering waterways.136 Talvitie et al. advise that filters capable
more than 26 million pounds of waste since 2008, created more of catching MPs or other advanced treatment methods can also
than 100 jobs, mitigated 13 million kg of carbon equivalent be installed in more WWTPs.137 Filters installed by gas stations
or parking lots can also be used to collect MPs from road traffic materials and delivery systems, (iii) implementing design for
in stormwater according to Fälström and Anderberg.135 recycling, (iv) increasing collection capacity, (v) scaling up
Moreover, biodegradable plastics are a promising, but so-far sorting and mechanical recycling capacity, (vi) scaling up
incomplete solution to the plastic pollution problem. Biode- chemical conversion capacity, (vii) reducing post-collection
gradable plastics are plastic that can be degraded into CO2 and environmental leakage, and (viii) reducing trade in plastic
H2O by biological forces such as enzymatic breakdown or waste”. Their results demonstrated that the system change
metabolism by microorganism. Polylactic acid (PLA) and scenario was the cheapest option over time and resulted in the
polyhydroxyalkanoate (PHA) are two common biodegradable least plastic pollution, reducing the rate of pollution by 78%
polymers made from biobased feedstocks.138 Biodegradable compared to “business as usual” in 2040. However, it still
plastic and starch blends can be 70% starch by weight and still resulted in 644 million metric tons of plastic pollution.150 Figure
possess similar qualities as polymers, and are more cost-effective 4 presents a future trajectory of plastic pollution as well as the
than other biodegradable plastics.139 Although biodegradable management costs under various action scenarios. This analysis
and compostable plastic can be eventually broken down by suggests that rapidly implementing promising alternatives with
microorganisms under specific conditions, such as specialized the aid of appropriate standards, regulations, and education
industrial composters,140 many biodegradable plastics may could avoid the most serious impacts on the environment, the
never reach their desired end state, can contaminate batches global economy, and human health.
of recycled plastic, and end up in landfills or litter the Public perception of plastic pollution can have a major impact.
environment.141−143 Biodegradable (especially oxo-biodegrad- The negative perception of microbeads helped get legislation
able) plastics may simply degrade more quickly into MPs in the passed to ban them, and campaigns such as “Don’t Break the
environment than traditional plastics because their degradation Lake” are proof that educating the public creates changes in
does not equate to full decomposition. 143,144 Further, behavior.113 Thus, education on other aspects of plastic
biodegradable and conventional plastics may be similarly pollution can have a huge impact as well. For example, educating
harmful to organisms, with 67% of both inducing toxicity the public about other sources of MPs such as clothes washing
(bioluminescence inhibition) in in vitro assays of bio- can promote more sustainable behavior such as washing fleece
luminescent bacterium Aliivibrio f ischeri.145 However, there clothes less or hand washing.6,113 Education on plastic pollution
are some environmental advantages to bioplastics. Biodegrad- originating from discarded trash may also help reduce littering,
able and compostable plastics made from plant-based chemicals especially on beaches. Similar to how pictorial health warning
can sequester CO2 in the product over their lifetime.146 labels on cigarette packages are effective at lowering smoking
Hypothetically, transitioning from conventional plastic to the rates and increasing quit attempts,151 signage posted at beaches
corn-based PLA could reduce U.S. plastic industry greenhouse or in stores may help the public make choices that avoid MP
gas emissions by 25%, and if traditional plastics were instead pollution. Labels on products that release MPs into the
produced through renewable energy, emissions could be environment may be effective at reducing their pollution by
reduced further. Bioplastics being produced by renewable inspiring changes in consumption habits. Education campaigns
sources may lead to near-zero carbon emission.147 Nonetheless, could increase public investment in sustainable plastic products.
if biobased plastic manufacturing is expanded to a global scale, There are many possible avenues to limit future plastic pollution
this would require cropland expansion−competing with food in the Great Lakes. These would require a united effort by
production−and possibly deforestation. This potential defor- government leaders, businesses, and the public in moving
estation, combined with the increased use of farm machinery toward this goal.
which runs on petroleum, could increase carbon emis-
sions.140,141,146
Conventional plastics can be better regulated when policy is
■ CIRCULAR ECONOMY
Plastic pollution is an expensive problem. Plans to tackle litter in
informed by standards, which are currently lacking. While the the Great Lakes could cost around $468 million annually.42
Microbead-Free Waters Act banned all microbeads in rinse-off According to an analysis conducted by Beaumont et al. (2019),
products, DeVitt et al. propose a new standard called plastic in marine environments results in a 1−5% decrease in
“Ecocyclable” which would define environmentally safe MPs marine output which corresponds to a $500−2,500 billion loss
based on degradability, bioaccumulation, and toxicity. A of benefits originating from the marine ecosystem annually. This
standard like “Ecocyclable” could be adopted to properly means that the annual cost associated with each ton of plastic
classify safe and unsafe MPs, as this will only make it easier to pollution is between $3,300-$33,000. The 18 metrics used to
enact legislation regulating MP usage and pollution going quantify marine output included not only wild food output but
forward.148 also water conditions, entertainment, and mediation of
Another interesting prospect for future plastics is utilizing wastes.152 Similarly, some value must be lost due to plastic
artificial intelligence (AI) and machine learning (ML) to design pollution in the Great Lakes.
novel polymers and simulate their behavior and properties, The issue of plastic pollution can be mitigated by investing in
including their potential toxicity. Wu et al. were able to train an solutions that will lead us closer to a plastic circular economy
algorithm on existing polymeric properties data and design (Figure 5). The Ellen MacArthur Foundation hosts a network of
thousands of hypothetical polymers with promising thermal businesses, cities, governments, universities, and leaders to foster
properties.149 Perhaps AI could help design plastics that could a circular economy. They define a circular economy as one
be easily broken down into mixtures, monomers, or other useful “based on the principles of designing out waste and pollution,
products with little environmental impact. keeping products and materials in use, and regenerating natural
Lau et al. modeled different scenarios for dealing with plastic systems”.153 The foundation has an initiative focused on plastic
pollution from 2016 to 2040. The “system change” scenario recycling called New Plastics Economy which connects more
involved all eight proposed interventions: “(i) reducing plastic than 1,000 organizations. The initiative is founded on three
quantity in the system, (ii) substituting plastics with alternative actions: Eliminate, Innovate, and Circulate to limit the amount
economy by recycling materials and limiting pollution will still

be progress.
Realizing a circular economy for plastics will require policy
changes and plastic industry regulation. The Ellen MacArthur
Foundation created the Plastics Pact Network which connects
initiatives involving organizations, businesses, NGOs, govern-
ments, and citizens across the world with the purpose of moving
toward a plastic circular economy. Countries with national pacts
include the UK, France, Chile, The Netherlands, South Africa,
Portugal, the US, Poland, and Canada. Regional pacts include
the European Plastics Pact and the Australia, New Zealand, and
Pacific Islands (ANZPAC) Plastics Pact.164 The Ellen
MacArthur Foundation also created the Global Commitment
to moving toward a circular economy which more than 500
organizations have joined, the companies among them
Figure 5. Circular economy for plastic, in which renewably sourced producing 20% of all the world’s plastic packaging. These
virgin feedstock is utilized in the design and production of reusable brands and retailers have utilized more recycled plastic since
plastic products. The plastic products can be used, reused, and either
joining the Global Commitment,165 and have been able to
recycled to become similar-quality plastic or anaerobically digested
and/or composted. collectively reduce their virgin plastic use by 2% since 2018, with
projections to decrease by an additional 17% by 2025. But
voluntary measures will not be enough to reach a circular plastic
of plastic used, develop more sustainable plastics, and recycle as economy as quickly as necessary. A first step was taken at the
much plastic as possible.154 United Nations Environmental Assembly (UNEA 5.2) in March
Currently, most plastics are not recycled, and those that are 2022, where 175 countries adopted a resolution called End
recycled are downcycled to produce lower quality plastics Plastic Pollution: Toward a legally binding instrument. This
through mechanical recycling. If plastics were recycled to would compel the International Negotiating Committee (INC)
produce more of the same high-quality plastics, as much as $80- to develop a legally binding UN Treaty addressing the full life
$120 billion that is currently lost through single-use plastic cycle of plastics by 2024. In the future, there should be more
packaging material annually could be gained back.155 There policies that support a circular economy adapted to regulate the
already exist efforts to industrialize chemical recycling processes plastic industry.166
which can achieve this. For example, Loop Industries claims the
ability to break down PET into monomers and then
repolymerize to produce virgin-quality PET.156 Companies
■ CONCLUSIONS AND FUTURE OUTLOOK
MP pollution is a multifaceted issue tied to food, water, and
like L’Oreal and PepsiCo have signed contracts to use their energy, posing threats to aquatic environments and health of all
recycled PET.157,158 A team at Lawrence Berkeley National organisms. The presence of MPs in the environment taints water
Laboratory has developed a plastic called PDK (poly diketoen- quality, contaminates food sources and products,70 and
amine) which can be recycled without lowering its quality, as it correlates to fossil fuel emissions through its manufacturing
can be broken down into monomers and separated from all and pollution.100 Moving toward the goal of a circular economy
additives simply by submerging in strong acid. Although the will be helpful in limiting the introduction of MPs into the
initial production of PDK is more expensive and carbon- environment. Collaborative efforts from government, industry,
demanding than conventional plastics, the recycling process of and the public will be required to derive solutions that effectively
PDK is competitive with conventional plastics. Conventional limit the entrance of MPs into the Great Lakes and other water
plastics PET and HDPE cost less than $1 per kg to produce and bodies.
result in 2.73 and 1.9 kg of CO2 emissions, respectively. More studies need to be conducted to gather data on MP
Although recycled PDK could be made for $1.50/kg, it would concentrations in the Great Lakes to gain a better understanding
lead to only 1.6 kg CO2/kg.159 of the sources and fate of MPs. Further research can be done to
Upcycling of plastics is another area of research that could determine the rate at which micro- and macroplastics are
help limit plastic waste and move toward a circular economy. degrading in the Great Lakes and what types of degrading effects
Catalysis can be utilized to break down reclaimed PET into are most impactful. The distribution and transportation of MPs
value-added products.160 For example, a team of scientists throughout the Great Lakes should be more thoroughly
headed by Dr. Massimiliano Delferro of Argonne National investigated. Optimal sampling and quantification methods
Laboratory has been able to convert single-use polyethylene should be standardized to allow for comparison across studies.
(PE) into value-added products such as lubricants and waxes. Standards regarding what constitutes environmentally safe MPs
This is done by a catalysis reaction called hydrogenolysis.161 should be agreed on as well so that policies can be drafted with
Certain enzymes isolated from bacteria are also capable of proper background information.148 The pervasiveness of MP
degrading plastics, and can be utilized in future plastic recycling contamination throughout Great Lakes food webs should be
and upcycling processes.162 further explored. Laboratory experiments should be conducted
Truly infinite recycling and upcycling of materials may be to investigate effects of MPs on the health of Great Lakes
impossible due to the laws of thermodynamics, which posit that wildlife, paying attention to polymer, shape, and size of particles.
if entropy is lost somewhere in the universe, energy must be The extent of human MP consumption through drinking water
invested to do this, and that entropy is gained to an equal or sourced from the Great Lakes should be quantified, and the
greater amount elsewhere.163 Although a closed loop with no human health implications should be further characterized.
losses may never be achieved, moving closer to a circular These studies will inform future risk assessments regarding MPs.
These research efforts and quantitative risk assessments may Biographies

help motivate policy changes that prevent the production of
MPs to begin with, as well as garner public interest in the cause
of limiting MP pollution. With regards to policy, more should be
done to limit the entrance of MPs into the Great Lakes, paying
most attention to areas with highest MP counts such as regions
closest to cities, where more particles are likely to enter the
lakes.167 The beach cleanup efforts that take place around the
Great Lakes unfortunately cannot efficiently remove MPs, and
only collect from the shoreline. Actions such as equipping more
WWTPs whose effluents feed into the Great Lakes with the
advanced filtration systems to effectively remove MPs from
influents could reduce inputs. Smoking bans on more public Claire Fuschi holds a B.S. in Molecular Engineering from the University
Great Lakes beaches, as has already been banned in multiple of Chicago. She joined Professor Junhong Chen’s research group in the
Michigan cities, to limit plastic litter that will degrade into MPs second year of her undergraduate degree. Her research in the Chen
Group investigates the intersection of water and public health.
over time could also be beneficial.168 Effective EPR regulations
could limit MP pollution from manufacturers. Campaigns
aiming to educate the public on plastic pollution in the Great
Lakes could lead to widespread behavioral changes.113 The
pervasiveness of MPs in the Great Lakes must be remedied
quickly and robustly to preserve the ecosystem and protect the
health of wildlife and human inhabitants.
■ AUTHOR INFORMATION
Corresponding Author
Junhong Chen − Pritzker School of Molecular Engineering, The
University of Chicago, Chicago, Illinois 60637, United States;
Chemical Sciences and Engineering Division, Physical Sciences
and Engineering Directorate, Argonne National Laboratory, Haihui Pu received his Ph.D. from the University of Wisconsin
Lemont, Illinois 60439, United States; orcid.org/0000- Milwaukee in 2015. Before joining the University of Chicago as a Staff
0002-2615-1347; Email: [email protected] Scientist, he completed a Postdoctoral Appointment at University of
Wisocnsin-Milwaukee (UWM) and worked as a Sensor Scientist for
Authors NanoAffix Science, LLC. Pu received his M.S. degree from Fudan
Claire Fuschi − Pritzker School of Molecular Engineering, The University and his B.S. degree from Nanjing University of Science and
University of Chicago, Chicago, Illinois 60637, United States Technology in China. His research focuses on the first-principles/
Haihui Pu − Pritzker School of Molecular Engineering, The
molecular dynamics simulations and statistical thermodynamics
University of Chicago, Chicago, Illinois 60637, United States;
Chemical Sciences and Engineering Division, Physical Sciences modeling on novel two-dimensional nanomaterials for environmental
and Engineering Directorate, Argonne National Laboratory, and energy applications, which include field-effect transistor nano-
Lemont, Illinois 60439, United States sensors for detecting various target analytes of interest and energy
Margaret MacDonell − Environmental Science Division, storage devices.
Computing, Environment, and Life Sciences Directorate,
Argonne National Laboratory, Lemont, Illinois 60439, United
States
Kurt Picel − Environmental Science Division, Computing,
Environment, and Life Sciences Directorate, Argonne National
Laboratory, Lemont, Illinois 60439, United States
Maria Negri − Environmental Science Division, Computing,
Environment, and Life Sciences Directorate, Argonne National
Laboratory, Lemont, Illinois 60439, United States
Complete contact information is available at:
https://pubs.acs.org/10.1021/acssuschemeng.2c02896
Notes
The authors declare no competing financial interest.
Margaret MacDonell heads the Radiological, Chemical, and Environ-

mental Risk Analysis Department in the Environmental Science
Division of Argonne National Laboratory. She received her B.S. in
biology and M.S. in civil/environmental health engineering (CE/EHE)
from the University of Notre Dame, and her Ph.D. in CE/EHE from
Northwestern University. Her research focuses on mixed environ-
mental exposures, joint toxicity, and cumulative risk analyses with
recent applications emphasizing sustainability, resilience, and respon-
sible innovation for the circular economy. She is a Fellow and past
President of the Society for Risk Analysis, a Fellow of the Waste
Management Symposium, and senior scientist in the University of
Chicago Consortium for Advanced Science and Engineering.
Junhong Chen is currently a Crown Family Professor of Molecular

Engineering at Pritzker School of Molecular Engineering at the
University of Chicago and lead water strategist at Argonne National
Laboratory. He received his Ph.D. in mechanical engineering from the
University of Minnesota in 2002. His research interest lies in molecular
engineering of nanomaterials and nanodevices, particularly hybrid
nanomaterials featuring rich interfaces and nanodevices for sustainable
energy and environment. His approach is to combine multidisciplinary
experiments with first-principles calculations to design and discover
novel nanomaterials for engineering various sensing and energy devices
with superior performance.
Kurt Picel received his B.S. in Chemistry from Western Michigan

■ ACKNOWLEDGMENTS
This work was financially supported by the University of
University in 1976 and his Ph.D. in Environmental Health Sciences Chicago faculty startup fund and Laboratory Directed Research
from the University of Michigan in 1985. His research focusses on and Development (LDRD) funding from Argonne National
environmental and human health risks of chemical and radiological Laboratory, provided by the Director, Office of Science, of the
releases as well as on broader environmental risks from energy and U.S. Department of Energy under Contract No. DE-AC02-
industrial projects and processes including the lifecycle risks from 06CH11357.
plastics.
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■ DETECTION, SEPARATION, AND QUANTIFICATION

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Margaret MacDonell heads the Radiological, Chemical, and Environ-

Junhong Chen is currently a Crown Family Professor of Molecular

Kurt Picel received his B.S. in Chemistry from Western Michigan

p l a s t i c - u s - w a t e r w a y s - n e e d s # :̃ : t e x t = environmental safety. Environ. Sci. Pollut. Res. 2018, 25 (8), 7287−

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