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A Reviewofinnovationsindisbondingtechniquesforrepair 2014
A Reviewofinnovationsindisbondingtechniquesforrepair 2014
art ic l e i nf o a b s t r a c t
Article history: The recycling, recovery and reuse of End-of-Life Vehicles (ELVs) have raised worldwide concerns. This
Accepted 13 December 2013 paper identied drivers for new joining solutions in the automotive industry and specically reviewed
Available online 14 January 2014 current use of adhesive technology. From an ELV recycling point of view, rapid assembly and disassembly
Keywords: joining solutions were identied as key technology drivers. Innovations in adhesive disbonding
Disbonding technologies were reviewed and suggestions for the most promising future disbonding technologies
Adhesive have been proposed.
End-of-Life Vehicles & 2014 Elsevier Ltd. All rights reserved.
Automotive
Recycling
Reuse
Data issued by the International Organisation of Motor Vehicle There are two main drivers for change. These are international
Manufacturers showed that the global automotive industry has legislation on ELV and the demand (including future security of
gradually recovered from the economic crisis in 2008; global supply) of materials.
vehicle production reached 84.1 million units in 2012 compared
to 61.8 million units in 2009 [1]. This can mainly be attributed to 2.1. End-of-life Vehicles (ELVs)
the signicant increases in vehicle ownership seen in developing
countries such as China and India. In 2009 for example, car 2.1.1. Processing of End-of-Life Vehicles
production in China was the highest of all car producing countries, End-of-Life Vehicles are normally either scrapped for recycling
reaching 13.79 million [2]. From a sustainable development or simply abandoned on the road. In terms of the latter choice, the
perspective, growing concerns have been raised about the envir- abandoned vehicles not only cause obstruction and safety pro-
onmental impacts of automotive vehicles and their increasing blems in the public place but also waste resources. The research
numbers, including energy consumption, greenhouse gas emis- conducted by Melissa et al. showed that the devaluation of scrap
sions, waste generation and End-of-Life Vehicle (ELV) recycling. metal, a poor vehicle registration system, weak legislation and the
The objective of this paper is to investigate the latter of these growth of cheap second-hand vehicles all contributed to an
concerns, particularly focusing on ELV recycling problems from a increase in the amount of abandoned vehicles [3]
joining solution perspective. In Section 2, current ELV processing The recycling, recovery and reuse of ELVs have already raised
procedures and legislative initiatives have been reviewed and worldwide concerns. Various nations have implemented different
analysed. Challenges which are likely to be incurred by the strategies to deal with the issues which vary considerably in
production of future vehicles have also been taken into considera- severity [2,47].
tion. A new joining solution with the essential characteristic of As product-take-back and legislation requirements on producer
rapid disassembly is identied as a key technology driver. Section responsibility are implemented, the use of recycled materials is
3 discusses the current use of adhesive bonding in the automotive increasingly important [8].
industry and a thorough review of recent innovations in adhesive In the EU, to ensure End-of-Life Vehicles are disposed of
disassembly technology is provided in Section 4. properly, ELV legislations and Environmental Permitting Regula-
tions require all vehicles to be taken to Authorised Treatment
n
Facilities (ATFs) for depollution, dismantlement and deregistration.
Correspondence to: Department of Mechanical Engineering and Mathematical
Sciences (MEMS), Oxford Brookes University, Wheatley Campus, Wheatley, Oxford
A Certicate of Destruction (CoD) will be issued for the last owner
OX33 1HX, United Kingdom. Tel.: 44 1865 483 568. of the vehicle after deregistration. Updated information of all the
E-mail address: [email protected] (Y. Lu). registered ATFs in the UK can be found on Environment Agency0 s
0143-7496/$ - see front matter & 2014 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.ijadhadh.2014.01.021
120 Y. Lu et al. / International Journal of Adhesion & Adhesives 50 (2014) 119127
Fig. 2. The recycling and recovery rate of ELVs at European Union in 2008 [97].
website [9]. Autogreen and Car take back are the two major free for ferrous and non-ferrous metals. The resulting residue is termed
take-back service providers with ATFs throughout the UK. Within as Automotive Shredder Residue (ASR), also referred to as auto
the ATF process, a network of companies cooperates in the uff or auto shredder uff [12]. Fig. 2 illustrates the size and scale
recycling process. For example, in the UK, EMR focuses on the of ASR production in Europe in 2008.
scrap metal recycling while sending the plastic rich fraction to
their joint venture partners, MBA Polymers Inc, which specialises
in separating and recycling different types of polymers. 2.1.2. Automotive shredder residue (ASR)
Fig. 1 reviews the general processing procedures of ELVs. The Vigano et al. [5] estimated that EU countries produced approxi-
recycling process of a range of separated materials at this stage mately 1.92.3 million tons of ASR annually. This accounted for
was detailed in the studies conducted by Baeyens et al. [10,11]. The approximately 10% of the total number of hazardous wastes
remaining parts pass through a shredder and separation process produced and up to 60% of the total shredding wastes [13]. ASR,
Y. Lu et al. / International Journal of Adhesion & Adhesives 50 (2014) 119127 121
constituting up to 25 wt% of the vehicle, is composed of a variety (d) Environmental Permitting (England and Wales) Regulations SI
of materials including metal, rubber, wood, dirt, textile, glass and 2010/675 on environmental permits and exemptions.
up to 27 different types of plastics, although PP, PUR, PVC, ABS,
PMMA and PET are generally identied as the major types [6,13].
The composition of ASR can differ signicantly depending on the
2.2.2. Asia
shredding and post-shredding methods applied.
In Japan, the End-of-Life Vehicles recycling law, prompted by
Since the 1970s, landll treatment and incineration have been
limited natural resource and land resource for landll sites, was
the two major ASR processing methods. Landll treatment still
introduced in 2005 [18,19]. It is similar to the EU counterpart but
remains the most widely used method. In some parts of the world,
extended to cover virtually all vehicles; the EU directive is
certain measures are required, such as immobilising heavy metals
restricted to passenger vehicles and light commercial vans
before disposing in landlls. In addition to the environmental
only [2]. The law stipulated that it is the automakers responsibility
problems and ever increasingly stringent legislations, landll
to provide dismantling manuals whilst vehicle owners will be
treatment has now become cost-prohibitive and less appealing
charged for the treatment of ELVs.
as an ASR processing method [14].
In South Korea, the Act for Resource Recycling of Electrical
To meet the European targets for the reuse, recycling and
and Electronic Equipment and Vehicles offers the scheme for both
recovery of ELVs set by the EU Directive, research has focused on
the manufacturers and importers in terms of the restrictions on
either more complete dismantling methods or ASR processing
hazardous substances (from 1st July, 2008), recycling rates, design
techniques. Vermeulen et al. [12] believed that dismantling more
and methods recycling, etc. [20] Unlike the EU directive, this Act
materials before shredding is not economically viable in Western
does not address the recycling issues of tyres, batteries or air bags.
countries. This was attributed to the relatively high labour cost
In China, Statute 307 regulates the disposal of ELVs in China. In
(compared to Asian countries) required in the dismantling process.
2001, the State Council of the Peoples Republic of China enacted
From this point of view, a more efcient disassembly characteristic
the End-of-Life Vehicle Recycling Regulation, i.e. the Statute 307,
for future joining technology seems an obvious development.
which stipulates the responsibilities of local government and ELV
Coates et al. [15] conducted research focusing on both developing
recycling industry regarding registration capital and capacity of
design methods to facilitate ELV recovery and current ELV proces-
dismantling activities [21].
sing economics. Their research highlighted the importance of a
The Automotive Products Recycling Technology Policy [22] was
shift from manual vehicle dismantling to large volume automated
enacted by the National Development and Reform Commission
post-fragmentation separation in achieving the 2015 target of 95%
(NDRC) in 2006 aiming at establishing the ELV recycling system,
recycling set by the EU Directive.
including developing and promoting scrapped automotive pro-
ducts [2]. However, the enforcement was comparatively weak
compared with Korea and Japan. This policy established a mini-
2.2. Legislation mum of 85% reuse and recovery target by 2010. The use of
hazardous chemicals such as lead, cadmium, hexavalent chro-
With the ever growing concerns for the recycling of End-of-Life mium and mercury is prohibited.
Vehicles, legislation has developed in many parts of the world. The
content below cited examples from Europe, Asia and America to
2.2.3. America
compare and contrast legislations in different regions.
In the United States, no legislation has been developed on a
federal level to address ELV recycling issues even though attempts
2.2.1. European Union have been made by some senators since 1991. The main argument
So far, the most inuential legislation is the ELV Directive 2000/ appears to be that enacting legislations are not considered an
53/EC, which is enacted under the European Commission0 s priority effective method to improve recycling [19].
waste streams programme [16]. According to this EU Directive [17], Instead, large manufacturers in the USA have shared this
member states must ensure that ELVs are transferred to ATFs and responsibility. In 1992, Ford, Chrysler and General Motors initiated
properly recycled. Manufacturers are also encouraged to limit the use a Vehicle Recycling Partnership to facilitate sustainable vehicle
of hazardous substances and increase the use of recycled materials in recycling both in North America and around the world [16].
new vehicles. Targets have also been set in different stages: Another term often referred to in the USA is Product Stewardship
which means every party involved in the lifespan of product share
From 1st of July, 2003: vehicles put on the market cannot the responsibility for reducing its environmental impact.
contain lead, mercury, cadmium or hexavalent chromium
(materials and components exempted are referred in the annex 2.3. Recycling issues for future vehicles
of the Directive).
From 1st of January, 2006: reuse and recovery of a minimum of Due to the depletion of natural resources and exacerbating
85% per vehicle on average (recycling 80%) for vehicles pro- environmental issues, fuel efciency and CO2 emission are two
duced after 1980; reuse and recovery of 75% per vehicle on major concerns. One effective approach to these problems is to
average (recycling 70%) for vehicles produced before 1980. reduce vehicle weight due to the fact that approximately 75%
From 1st of January, 2015: increase the reuse and recovery rate of fuel consumption is caused by vehicle weight [23]. For example,
to 95% while the reuse and recycling rate to 85%. a 100 kg reduction in weight could save 0.4 l/100 km fuel
consumption.
Other major legislations that can affect the disposal of shredder Engines, running gears, and chassis frames, among other
residues in EU include: components, have been increasingly made of lightweight
metals [24]. Low-weight, cost-effectiveness, production times,
(a) Directive 2000/76/EC on the incineration of waste. ease of installation are expected to be some of the key features
(b) Directive 1999/31/EC on the disposal of waste in landlls. for future automotive vehicle components. OEMs today have
(c) Registration, Evaluation, Authorisation, and Restriction of intensied their efforts in using lightweight materials such as
Chemical Substances Directive (REACH). polymers and composites, as substitutes of ferrous materials. Fig. 3
122 Y. Lu et al. / International Journal of Adhesion & Adhesives 50 (2014) 119127
3. Adhesive bonding in automotive industry An emerging application for adhesives in body assembly is the
construction of the space frame. Over the past decades, adhesively
The automotive industry is facing challenges of joining dissim- bonded space frames including box-beam structure have been
ilar materials while maintaining mechanical properties and dur- employed by a number of car manufacturers in concept cars and
ability, especially in structural applications. Adhesive bonding is low volume models (e.g. Jaguar XJ220, Ford AIV, Lotus Elise and
now extensively considered to be the replacement of conventional Aston Martin Vanquish) [3638]. The relatively demanding
joining methods such as riveting, bolting and welding. Here is a mechanical property requirements for this major structural com-
list of major advantages: ponent necessitate the application of high quality adhesive bonds.
Hence, both a part pre-treatment process and high performance
(a) All solids can be joined including combinations of dissimilar adhesives are typically used [36,37]. For example, the production
materials, although pre-treatment may be necessary. of the Lotus Elise space frame utilises both an anodising process
(b) More uniform distribution of stress and increased fatigue life. for the extruded aluminium components and a high performance
Y. Lu et al. / International Journal of Adhesion & Adhesives 50 (2014) 119127 123
Table 1
Volatile compounds of isothermal degradation of epoxy resin [95].
CH4 0 0 Trace nn nn
CO 0 0 0 n n
CO2 Too small for positive identication (220 1C300 1C) trace n
Propylene Too small for positive identication (220 1C340 1C)
Formaldehyde Suspected but too small for positive identication (220 1C340 1C)
Acrolein Trace nn nnn nnnn nnnn
Acetone Trace n nn nnn nnn
Allyl Alcohol Trace n nn nnn nnn
Water nn nnn nnnn nnnnn nnnnnn
single part heat cured epoxy (with tensile strength of around Adhesively bonded PMHs technologies were rst introduced
35 MPa and Young0 s modulus of about 2700 MPa) to achieve its and patented by Dow Automotive in 2003. Dow developed a low
desired properties [38]. energy surface adhesive to bond glass-bre reinforced polypropy-
The use of adhesives in space frame construction brings a lene to a metal stamping [47]. Compared to traditional hybrid front
number of benets. One of the most signicant ones is to fully end manufacturing such as rivet bonding and over-moulding,
extract the strength-to-weight benets offered by the light weight adhesive bonding improves the stiffness and minimises stress
aluminium alloys which cannot be easily welded without losing concentration by forming a continuous joint along the plastic to
properties [37,38]. The 68 kg adhesively bonded space frame of metal interface [48]. However, from an ELV recycling point of view,
the Lotus Elise achieved an astonishing 50% weight reduction to separate polymers from metals in this adhesively bonded hybrid
compared with an equivalent steel construction bonded with spot can be laborious and costly. Consequently, a method of rapid
welding [38]. Compared with welding techniques, adhesive bond- disassembly would be highly desirable.
ing also provides higher precision of the space frame structure due
to the elimination of distortion that comes with the localised high
temperature zone [31,38]. This is highly valued in high perfor- 4. Adhesive disassembly technology and recent advances
mance car structures because even tiny distortions (0.5 mm) to the
space frame can affect the handling of the vehicle [39]. Together 4.1. General methods for adhesive bonding disassembly
with other typical advantages brought by adhesive bonding, the
adhesively bonded automotive space frame has fully demon- Previous research [49] conducted within the Joining Technology
strated its merits over the past decades. Research Centre (JTRC) at Oxford Brookes University has summarised
However disadvantages also exist in an adhesively bonded methods for disassembly of adhesive joints from various areas. The
automotive space frame. The limited production rate caused by approaches for general adhesive bonding and novel methods have
the time consuming curing and joining processes is one of the been covered to a large extent.
major concerns. Recent developments in robotic and curing facil- The mechanical separation method of disbonding was identi-
ities has achieved a production rate of about 3000 units per ed as the most primitive approach. A range of patented works
annum for a hybrid adhesively bonded space frame, however [5053] have attempted to the assist disassembly process, yet
further developments are still needed for higher production there is a lack of clean separation of the substrates and the method
volume [37,38,40]. Also, the difculties for maintenance and is generally inefcient and laborious.
repairing should not be ignored. If an adhesively bonded space Thermally induced disassembly approaches can be achieved
frame is damaged in an accident, it cannot be repaired using through both thermal softening (exceeding the adhesives Tg)
conventional techniques as with a steel chassis. Replacement of and thermal decomposition (exceeding the temperature of
the whole space frame may occur under serious collision ammability-in-air or auto-ignition point). For the latter, the
[36,38,41]. major concerns are the toxic and irritant emission gases that are
produced as a result of chemical decomposition [5]. Table 1 shows
the reaction products determined after isothermal degradation.
3.3. Case study 3: automotive front end module (FEM) Certain solvent or acid immersion techniques can also assist the
adhesive disassembly process. Polar solvents such as isopropyl
The front end module supports the cooling package, bonnet alcohol (IPA), methyl ethyl ketone (MEK) and acetone, can be very
latch mechanism, headlights, bumper and many other compo- effective in cleaning and degreasing substrate surfaces and are
nents. The major requirements for the FEM include crashworthi- mainly used in surface treatment processes [55,56].
ness, thermal and chemical stability, and durability. Polymer metal
hybrids (PMHs) technology has gained popularity in making 4.2. Tailored adhesive formulations for the ease of adhesive
automotive FEMs in recent years. The Lanxess group has been disassembly
developing PMHs technologies for many automakers [42]. BMW,
in its 1, 3 and X3 series, the new Audi TT and Audi A8 employed To a large extent, the electronic chip industry started the research
the Lanxess technology to produce front end modules [43,44]. for disassembly on adhesive formulations to enable rapid removal of
PMHs have been introduced as an approach to meet both struc- chips at end of life [5759]. Different approaches have been devel-
tural and non-structural requirements while at the same time oped in different areas. Battelle Memorial Institute [60] developed a
achieving a lightweight structure. thermally reversible isocyanate-based polymer formulation, the
In addition to injection over-moulding and metal over-moulding reversibility mechanism of which was based on the dissociation of
technologies, adhesive bonding is another major approach to man- the isocyanate-labile hydrogen based linkage to the isocyanate and
ufacture PMHs in the automotive industry [45,46]. labile-hydrogen starting groups. Upon disassociation, this polymer
124 Y. Lu et al. / International Journal of Adhesion & Adhesives 50 (2014) 119127
Table 2
Comparison and rating of disbonding techniques.
n
Overall Rating: 1n to 5n from low to high rates.
More importantly, additive-matrix incompatibility issues were change occurs as an additional interface is required for the RNC to
pointed out in this research. be inserted into the bondline. However, no further information
In terms of thermally expandable additives, an early work was disclosed.
patented by 3M [78] used inorganic materials such as dilated Reviewing most of these current studies on functional addi-
graphite, vermiculite, pearlite or mica as expanding additives. The tives, it is noted that none of the approaches mentioned create a
expandable additive content was generally specied as 1050 wt%. system sufciently effective for the disassembly of an adhesive
Initiation temperature was reported to be 250500 1C with expan- application in the automotive industry. Disassembly efciency and
sion ratio normally 1.1. It is also claimed that these additives could additive-matrix compatibility were identied to be two major
enhance the heat resistance of an adhesive. However, neither concerns, which were either vaguely mentioned or completely
experimental data nor any convincing proof was disclosed. neglected in most patented works. Some studies have identied
Expandable additives have also been used for adhesive disas- these problems to be main obstacles but failed to provide a
sembly in orthodontic application. The removal of orthodontic feasible solution. JTRCs research had identied additive-matrix
attachments has great risk of causing enamel damage if mechan- incompatibility and noted that the incorporation of additives affect
ical separation is undertaken improperly. The use of electrother- mechanical properties and durability by acting as weak links in the
mal, laser or ultrasonic methods may incur other problems such as matrix, or in some cases, reacting with the matrix. Magnus et al.
expensive equipment cost, potential pulpal damage and mucosal [84] successfully modied TEMs by grafting glycidyl methacrylate
burns [79,80]. Tsuruoka et al. [81] incorporated thermally expand- (GMA) on the surface. Atom transfer radical polymerisation using
able microspheres (TEMs) into 4-methacryloxyethyl trimellitate activators regenerated by electron transfer (ARGET ATRP) was
anhydride in methyl methacrylate initiated by tri-n-butyl borane employed. Special treatment was also used to retain the expansion
(4-META/MMA-TBB) resin adhesive, which is widely used for ratio of the TEMs.
bonding orthodontic brackets. The microspheres used in this study De-Bonding Ltd and Evonik have focused on developing a
were Matsumoto F-36D which starts to expand at 80 1C. They system with efcient disassembly processes. The research of De-
identied that an incorporation of 40 wt% of these microspheres Bonding Ltd has looked at the dismantling of automotive glazing
showed satisfactory bond strength before heating and a reduced on ELV by incorporating TEMs in the adhesive bondline [8587].
bond strength by a third within 8 s of heating. The Tokyo Institute In cooperation with the Armes group at Shefeld University, their
of Technology [82,83] also conducted research on adhesive dis- research [88] has successfully synthesised polypyrrole-coated
assembly using expanding microspheres manufactured by Matsu- TEMs which are only microns in size. The research investigated
moto. These studies also looked at its application for construction the effect of the TEMs on the delamination of the adhesive joints.
materials. The weight fraction of microspheres used and the An infra-red lamp was adopted as the heating source. Polypyrrole
roughness of adherent surfaces were found to be two major has a broad absorption peak (9001500 nm) in the infra-red. This
factors in determining the dismantalability of the bonded joints. provides the polypyrrole-coated TEMs with a very efcient ther-
Thermally expandable microspheres are generally constructed mal energy absorbance. Experimental results showed great poten-
with a thermoplastic polymer shell and hydrocarbon core, which tial for the application of reversible adhesion of car glazing and
has a low boiling temperature. The density reduces from about panels for both maintenance and recycling purposes.
1100 kg/m3 to 30 kg/m3 at elevated temperature [84]. TEMs were Evonik [89] developed a type of adhesive tape called Magsilica.
rst developed by Dow Chemical Co. and currently are being Magsilica is used as a nano susceptor which is basically a powder
manufactured by many companies such as Polychem Alloy, of iron oxide particles embedded in silicon dioxide nanoparticles.
Sekisui Chemical, Matsumoto Yushi Seiyaku, Akzo Nobel and These particles behave as nano magnets when subjected to
Sigma Aldrich. JTRC0 s research also investigated four different external magnetic eld, which can heat up for the purpose of
grades of physical foaming agents (TEMs) containing isobutene, curing and disassembly. This has achieved two major advantages:
isooctane or isopentane. These selected grades of additives pro- shortened cure times and reversible bonding. Evonik has patented
vide a range of activation temperatures and decomposition/expan- their work and showed several examples for its use [90]. A major
sion efciencies. concern is that conductive or magnetic components can cause
The Army Research Laboratory [75] has investigated a reactive electromagnetic shielding, which deactivates the heating mechan-
nanocomposite (RNC) approach to solve a rapid disassembly ism. McCurdy in JTRC [49] attempted to replicate the dismantling
problem. The disassembly is thermally triggered and a physical characteristics on a toughened epoxy adhesive incorporated with
126 Y. Lu et al. / International Journal of Adhesion & Adhesives 50 (2014) 119127
MagSilica powder. Half size single lap joints (ISO 4587) were made has generally received more attention because they can be
from 2 mm thick steel substrate with a 0.2 mm adhesive bondline introduced into existing adhesive products.
thickness. An induction heating method was adopted and a Functional additive/adhesive compatibility and disbonding
temperature of 120 1C (above epoxy resin Tg) was used to lead to efciency have been identied as the two major problems
debonding within 30 s. However, no satisfactory material separa- concerning functional additives.
tion was recorded. Reasons were attributed to the ineffectiveness
of direct induction heating which led to large residue strength of
structural adhesive.
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