Int J Life Cycle Assess

DOI 10.1007/s11367-013-0624-y

LCA OF WASTE MANAGEMENT SYSTEMS

Design of recycling system for poly(methyl methacrylate)

(PMMA). Part 1: recycling scenario analysis
Yasunori Kikuchi & Masahiko Hirao & Takashi Ookubo &
Akinobu Sasaki

Received: 17 October 2012 / Accepted: 5 July 2013

# Springer-Verlag Berlin Heidelberg 2013

Abstract Methods Based on the differences between PMMA grades

Introduction In this series of papers, we present a poly(methyl and their life cycles, we developed a life cycle model and
methacrylate) (PMMA) recycling system design based on designed a range of scenarios for PMMA recycling. We
environmental impacts, chemical hazards, and resource avail- obtained monomer recycling process inventory data based
ability. We evaluated the recycling system by life cycle assess- on the operational results of a pilot plant. Using this process
ment, environment, health, and safety method, and material inventory data, we quantified life cycle greenhouse gas (LC-
flow analysis. GHG) emissions and fossil resource consumption, and we
Purpose Previous recycling systems have not focused on calculated the LIME single index.
highly functional plastics such as PMMA, partly because of Results and discussion PMMA produces more than twice the
lower available volumes of waste PMMA compared with amount of GHG emissions than other commodity resins.
other commodity plastics such as polyethylene or polypropyl- Through scenario and sensitivity analyses, we demonstrated
ene. However, with the popularization of PMMA-containing that monomer recycling is more effective than mechanical
products such as liquid crystal displays, the use of PMMA is recycling. Operational modifications in the monomer recycling
increasing and this will result in an increase in waste PMMA process can potentially decrease LC-GHG emissions.
in the future. The design and testing of recycling systems and Conclusions Highly functional plastics should be recycled
technologies for treating waste PMMA is therefore a high while maintaining their key functions, such as the high
research priority. In this study, we analyze recycling of transparency of PMMA. Monomer recycling has the poten-
PMMA monomers under a range of scenarios. tial to achieve a closed-loop recycling of PMMA.

Responsible editor: Yasunari Matsuno Keywords Highly functional plastics . Operational

modification . Plastic grade . PMMA pyrolysis . Simulation
Y. Kikuchi (*)
Presidential Endowed Chair for “Platinum Society”, Organization
for Interdisciplinary Research Project, The University of Tokyo, Ito Abbreviations
International Research Center, 7-3-1 Hongo, Bunkyo-ku, BHET Bis(hydroxylethyl) terephthalate
113-0033 Tokyo, Japan CR Chemical recycling
e-mail: [email protected]
DMT Dimethyl terephthalate
Y. Kikuchi : M. Hirao HEA Home electrical appliances
Department of Chemical System Engineering, The University of H-sheet High molecular weight PMMA sheet
Tokyo, 7-3-1 Hongo, Bunkyo-ku, 113-8656 Tokyo, Japan LIME Japanese life-cycle impact assessment method
M. Hirao based on endpoint modeling
e-mail: [email protected] LGP Light guide panel
T. Ookubo : A. Sasaki
L-pellet Low molecular weight PMMA pellet
Mitsubishi Rayon, Co., Ltd, 1-1, Marunouchi 1-Chome, L-sheet Low molecular weight PMMA sheet
Chiyoda-ku, 100-8253 Tokyo, Japan MMA Methyl methacrylate
T. Ookubo MR Material recycling (mechanical recycling)
e-mail: [email protected] OAE Office automation equipment
A. Sasaki PE Polyethylene
e-mail: [email protected] PET Polyethylene terephthalate
 Int J Life Cycle Assess

PMMA Poly(methyl methacrylate) parts of electronic devices were not included in the previous
PP Polypropylene analyses such as the recycling in Japan of household appli-
PS Polystyrene ances and other consumer electronics by Nakano et al. (2007)
PTA Purified terephthalic acid and Andrae and Andersen (2010).
RPF Refused plastic/paper fuel No reports are currently available on the end of life of
TR Thermal recycling (thermal recovery) PMMA contained in LCD products. It seems that PMMA
waste in Japan may be mixed with other plastic wastes such
as shredder residue and then treated in the same ways as
1 Introduction other commodity resins. Mixed plastics may not be recycled
effectively and the quality of recycled materials needs care-
Recycling of plastics is an important issue. Examples of ful assessment to increase recycling efficiency in plastic
previous work in this area include life cycle assessment recycling systems as studied by Nakatani and Hirao (2011).
(LCA) of an Italian plastic recycling system as solid waste In this regard, however, recycled materials by mechanical
(Arena et al. 2003a, b), waste management of soft drink recycling of PMMA mixed with other plastics may not make
packaging systems in Mexico (Romero-Hernández et al. full use of the features of PMMA such as its high transpar-
2009), and the transboundary recycling of polyethylene tere- ency. Because of the enforcement of recycling laws and
phthalate (PET) bottles between Japan and China (Nakatani regulations for home electronic devices (METI 2001) and
et al. 2010). Clift (1997) categorized plastic recycling tech- recycling laws for personal computers (PC3R Promotion
nologies into reuse, mechanical recycling, depolymerization Association, Japan 2003), LCD display panels contained in
or monomer recycling, chemical recycling and pyrolysis, and such electronic devices are now being collected and are
energy recovery. Many alternative processes have been re- available for recycling.
ported and assessed such as recycling options for the manage- Monomer recycling of plastics is a technology with the
ment of plastic packaging wastes (Perugini et al. 2005) and potential to enable closed-loop recycling. Some monomer
feedstock recycling in blast and electric furnaces as materials recycling technologies have been reported and assessed, e.g.,
for reducing oxidized iron to replace cokes (Shimada et al. monomer recycling of PET bottles in Japan (Sugiyama et al.
2005). The quality of products derived from waste plastics 2006). For PET bottles, monomer recycling plants were
recycled materials was analyzed for evaluating substitutability constructed for bottle-to-bottle closed-loop or bottle-to-fiber
of fresh plastics made from fossil resources (Nakatani et al. open-loop recycling (Nakatani and Hirao 2011; Nakatani et al.
2011; Nakatani and Hirao 2011) and developing a robust 2010; Sinha et al. 2010). For PMMA, Achilias (2007) and
recycling system (Fujii et al. 2012). In this regard, however, Lopez et al. (2010) studied pyrolysis using different reactor
the plastics treated in these studies are mainly commodity types in the laboratory. A pilot plant revealed that collected
resins such as polyethylene (PE), polypropylene (PP), poly- PMMA waste can be recycled to methyl methacrylate (MMA)
styrene (PS), polyvinyl chloride (PVC), and PET, which are monomer and then used for producing new PMMA products
the most commonly used plastics (JPIF 2012; Plastics 2011). (MRC 2011; Nakagawa 2007; Sasaki et al. 2008). Several
In addition to high-volume plastics such as PE and PP, experiments have been done for characterizing its applicabil-
other plastics in use have special purposes. Poly(methyl meth- ity as actual recycling process (Nakagawa 2007).
acrylate) (PMMA) is one such specially used plastic because In this study, we aim to design a PMMA recycling system
of its significantly high transparency, resistance to weather with a PMMA monomer recycling plant. In practice, several
and impact, and technical properties. The shipment of PMMA assessments are required for appropriate implementation of
makes up about 1–2 % of the total shipments of all plastics in new technology into practice, including three types of evalu-
Japan (JPIF 2012) and Europe (Plastics 2011), and PMMA is ation of global environmental impacts, local chemical risks,
used in products requiring high-level transparency and resis- and feasibility studies (Kikuchi and Hirao 2009). In this series
tance, e.g., automobile lamp covers, lighting equipment, opti- of papers, we assess the acceptability of a PMMA recycling
cal fibers, and light guide panels (LGP) of liquid crystal process as a social technology by an evaluation of different
displays (LCDs). With the increased popularity of LCD prod- aspects of the PMMA monomer recycling process. Firstly, we
ucts, it is likely that the use and stored amount of PMMA has conduct an LCA to quantify global environmental impacts
also increased. Although the amount of waste PMMA includ- originating from the PMMA life cycle with or without the
ed in such appliances will also increase in the future, there are inclusion of a monomer recycling plant (MRC 2011).
currently no effective recycling systems for PMMA. Dodbiba Recycling scenarios are set as the different recycling routes
et al. (2008) studied the recycling of plastic waste from in Japan. We consider the substitutability of recycled products
discarded television sets and Hischier and Baudin (2010) for all recycling scenarios. Secondly, we consider operational
conducted LCA of plasma televisions; however, no previous modifications to improve the performance of the monomer
analysis of the plastics used in LGP is available. The PMMA recycling process and the impact on the total life cycle.
Int J Life Cycle Assess

2 Materials and methods the function of optical device by 0.2 % of impurity in recycled
MMA. Regarding contamination or impurities in the waste
2.1 Monomer recycling process PMMA stream, it was experimentally demonstrated that the
MMA monomer can be obtained with the same yield based on
Figure 1 shows the process block flow diagram of PMMA the inputted amount of PMMA, even if other types of resins
pyrolysis (MRC 2011). The process contains four segments, are mixed with waste PMMA (Nakagawa 2007; METI and
i.e., depolymerization, liquid recovery (which is the treatment MRC 2008; Sasaki 2008). Metals and other organic materials,
process for effluent gas from the reactor), purification of the e.g., paper, cause no problems in the reaction (Nakagawa
MMA monomer, and heat recovery from residue. The raw 2007; Ministry of Economy et al. 2008; Sasaki 2008). Impu-
material for this process is waste PMMA flakes and the rities are collected as residue or decomposed in the pyrolysis
product is recycled MMA monomer (99.8 % purity). The reactor, converted into low molecular weight substances, and
utility is heavy oil and electricity, and the inputted amount of incinerated in the heat recovery incinerator. This means that
which depends on the recovered heat from in-process residue. contamination with these types of impurities increases the
In the PMMA pyrolysis reactor, PMMA is decomposed by recovered heat. In this regard, however, PVC may be an
heat into MMA monomer and other substances such as methyl inhibitor and an undesirable contaminant of PMMA recycling
isobutyrate, methyl acrylate, and 1,4-cyclohexane dicarboxyl- by pyrolysis (Scheirs and Kaminsky 2006).
ic acid dimethyl ester, i.e., MMA dimer (Kaminsky and
Franck 1991; Scheirs and Kaminsky 2006). In the block flow 2.2 PMMA life cycle model based on plastic grade
diagram shown in Fig. 1, the liquid recovery segment com-
prises spray and liquid separation processes. The temperature Figure 2 shows the life cycle model of PMMA contained in
of effluent gas, named as cracking gases in Fig. 1, is increased products. PMMA has two main grades as a polymer: high
from 350 to 500 °C at atmospheric pressure and, after cooling and low molecular weight polymer grades. These two grades
to about room temperature, the crude MMA monomer of PMMA have slightly different physical properties. Al-
obtained is condensed before purification of MMA monomer. though high and low molecular weight PMMAs are both
The purification segment is composed of two distillation incorporated in the same type of products (LGP in LCD
columns, where the first column removes low-boiling-point panel), the size or other features of them are different. In
chemicals and the second column purifies the MMA mono- Fig. 2, we have specified three types of PMMA materials
mer. All residues from the liquid recovery and purification based on their categorization in Japanese statistical data
segments are used as fuel in the heat recovery segment for (Japan Petrochemical Industry Association JPIA 2012), i.e.,
heating sand used as a fluidized bed in the pyrolysis reactor. high molecular weight sheet (H-sheet), low molecular
Although the physical properties of recycled MMA at 99.8 % weight sheet (L-sheet), and low molecular weight pellet (L-
purity are almost the same as those of fresh MMA, recycled pellet). The products made from them are labeled as products
and fresh monomers have been mixed and used for optical A, B, and C, respectively. The sheet-type PMMA provides
devices in actual production. This is because such devices the raw materials for LGP of LCD products such as televi-
require high transparency enough for graphical function such sion sets, PC monitors, laptops, and mobile phones. Addi-
as color reproducibility, and the use of recycled MMA has a tionally, board products produced from PMMA sheet include
possibility to result in the unpredictable loss or reduction of components of furniture and information panels. On the

Fig. 1 Outline of a PMMA

pyrolysis process pilot plant
 Int J Life Cycle Assess

Fig. 2 Life cycle model of two

grades of PMMA developed in
Japan

other hand, various categories of plastic products incorporate collected not as PMMA but as mixed plastics. According to an
pellet-type PMMA, including machine tools and parts, daily investigation of a treatment plant for scrapped cars, specific
necessities, and miscellaneous goods (Ministry of Economy parts made of a single resin such as bumpers are segregated for
et al. 2012). This is because the L-pellets can be molded and recycling to increase the ratio of car recycling. L-pellets, for
formed into designed shapes. L-sheet is one of the products example, are used in containers and packaging, and it is quite
from L-pellets. In this regard, however, H-sheet is produced difficult to segregate PMMA products from other materials.
by direct polymerization of the MMA monomer and cannot PMMA wastes mixed with other types of plastics can be
be produced by molding, because high molecular weight transported to CR, MR, TR, or landfilling processes as shown
PMMA cannot be melted to form a shape for products. in Fig. 2. A certain amount of waste PMMA can be recycled to
After PMMA products are used, they must be collected on MMA monomer with the same ratio as products A and B in
the individual pathways based on the condition of waste the CR process. R and landfilling are the same processes for
products containing PMMA. Existing recycling laws in Japan product C as for products A and B.
enable the collection of products A and B in Fig. 2. Most of
the PMMA product contained in LCD panels may be collect- 2.3 Evaluation settings
ed and treated in recycling plants (Hirasawa 1999). An inves-
tigation of an appliances recycling plant in Japan revealed that 2.3.1 Functional unit and impact category
LGPs in LCDs were gathered and accumulated as by-products
from the manual separation of valuable parts and metals in We defined the functional unit of LCA in this paper as the
LCD products (Fig. 3). LGP is almost 100 % pure PMMA use of one unit amount of PMMA, i.e., 1 kg in Japan. The
after removing dots of titanium oxide attached on the surface composition of products A, B, and C was set at the same ratio
of the LGP. PMMA boards included in construction waste can as the actual shipment of them based on PMMA statistics
also be collectable by segregating them from other boards. In
this regard, however, we define the collection stages of H- and
L-sheets as the same process as shown in Fig. 2. Collected
waste products A and B are transported to chemical recycling
(CR) meaning monomer recycling, thermal recovery (TR), or
landfill, but not to mechanical recycling (MR) because the
high molecular weight PMMA cannot be recycled mechani-
cally and it is not easy to distinguish between grades of
PMMA in collection sites and recycling plants. The TR or
landfilling process is the same in Japan as for other plastic
recycling, which includes the production and use of refuse
paper/plastic fuel (RPF), energy recovery in a cement kiln,
waste power generation, incineration without energy recovery,
and landfilling (Mayumi et al. 2010; PWMI 2010). On the Fig. 3 Waste LGPs made of PMMA piled inside a home appliance
other hand, molding materials, i.e., product C in Fig. 2, may be recycling plant
Int J Life Cycle Assess

(Japan Petrochemical Industry Association JPIA 2012). The are sent to CR. Because the amount of PMMA in the form of
ratios have fluctuated slightly over the last 10 years. In this product C is larger than those of products A and B, the scenario
study, we adopted the 2009 ratios as representative values, settings on the waste from product C were generated as sce-
being 0.173, 0.131, and 0.696 kg for products A, B, and C, narios 3 and 4. Under scenario 3, we assume the recycling of
respectively. In previous studies, environmental impacts of collected product C in the MR process. At that time, collected
the plastic life cycle were analyzed based on greenhouse gas PMMA waste and other plastics are mixed. According to the
(GHG) emissions (Nakatani et al. 2010) with fossil resource existing literature and reports (JCPRA 2007), such mixed
consumption (Mayumi et al. 2010) or other impact catego- plastic pellets are used to produce plastic pallets, which can
ries (Shena et al. 2010). In this study, these indicators were reduce the amount of fresh PP, but not PMMA. Therefore, the
taken into account to the assessment of PMMA recycling recycling effects of mechanically recycling mixed plastic to
process. As for the impact categories, we evaluated Japanese mixed-plastic pellets can be considered as the substitution of
life-cycle impact assessment method based on endpoint fresh PP. As the process inventory for PMMA mechanical
modeling (LIME) single index with the consideration of recycling, we adopted the data from mechanical processing of
ozone depletion, global warming, acidification, air pollution PS (JLCA 2012) because PS sheet is applicable to similar types
in urban areas, photochemical oxidant creation, emission of of molding products, which means that their heat and mechan-
hazardous chemicals, ecotoxicity, eutrophication, and solid ical properties might be similar. In mechanical recycling of PS,
waste (Andrae 2009; JLCA 2012). waste PS is crushed, melted, and pelletized to produce recycled
PS pellet. In contrast, all PMMA waste is recycled in CR, and
2.3.2 Case study 1: recycling pathways MMA monomer is output in scenario 4. Recycled MMA can
be substituted for fresh MMA. We obtained the process inven-
In this case study, we quantified the recycling effects of PMMA tory data of PMMA monomer recycling from the operation
pyrolysis in the life cycle of PMMA. Table 1 displays the results of an actual pilot plant in June of 2009. Other recycling
recycling scenarios in case study 1. Scenario 1 is set as the process inventory data were obtained from the Japanese LCA
reference case, where all waste PMMA is incinerated without database (JEMAI 2007; JLCA 2012) and the literature on
energy recovery. In scenario 2, production loss is adequately plastic recycling (JCPRA 2007).
recycled, i.e., high and low molecular weight polymer grades We defined other settings for LCA as shown in Table 1. The
are recycled in CR and MR, respectively. PMMA waste after transportation distance in all scenarios was set as the same
use is transported for TR or landfilling, including the recycling value, 200 km, to compare recycling methods without the effect
effects of RPF, cement raw material/fuel, and waste power of location. This distance includes all required transportation
generation and the impacts of incineration and landfilling. after PMMA product assembly. We defined the treatment pro-
The distribution ratio for each process is assumed to be the cesses for waste PMMA products by using available inventory
same as the average ratio for industrial plastic waste, and these data. From the existing database (JLCA 2012), we determined
values were extracted from the statistical data in 2009 (PWMI two types of treatment processes for office automation equip-
2010). In scenario 3, the waste PMMAs from products A and B ment (OAE) and home electrical appliances (HEA): mixing

Table 1 Scenario settings in two case studies. Scenarios 1 to 4 are the settings in case study 1 and scenario 5 shows the settings of case study 2

Scenario 1 2 3 4 5

Plastic recycling Production H-MW Incineration CR (yield, 70 %) CR (yield, CR (yield, CR (yield,

settings loss 70 %) 70 %) 77 %)
L-MW Incineration MR MR MR MR
After use of products A Incineration RPF/ cement raw material and CR (yield, CR (yield, CR (yield,
and B fuel/ waste power generation/ 70 %) 70 %) 77 %)
After use of product C Incineration incineration/ landfilling MR (mixed-
plastic
pellet)
Other settings Transportation distance 200
(km)
Waste Products A Average of mixing treatment processes for OAE and Average of advanced treatment
treatment and B HEA processes for OAE and HEA
process Product C Average of mixing treatment processes for OAE and Average of advanced treatment
HEA and dismantling process for automobiles processes for OAE and HEA and
dismantling process for automobiles
 Int J Life Cycle Assess

and advanced treatment processes. OAE and HEA treatment optimum purification settings and minimize the environmen-
processes include disassembling, scraping, shredding, and tal impacts. We compared the effect of the increased recovery
sorting processes, where valuable parts, metals, and plastics of recycled MMA with the increase in fuel consumption.
are separated. In the mixing treatment, plastics contained in Chemical process simulators can be employed to estimate
OAE and HEA are outputted as shredder dust, whereas they are the inventory of chemical process units (Iosif et al. 2010).
outputted as separated plastic wastes from advanced treatment Aspen Plus V7.3 (Aspen Technology, Inc., Burlington, MA,
process. A part of PMMA contained in product C is an auto- USA), a widely utilized process simulator used in previous
mobile component and the inventory data of treatment process- LCA studies (Iosif et al. 2010; Mendivil et al. 2006), was
es for scrapped cars are available (JLCA 2012). In this study, selected in this study for estimating inventories of modified
the inventory data for treating unit amounts of waste products processes. The two columns for purifying the MMA monomer
A, B, and C were assumed as the averages of OAE, HEA, and were simulated to estimate process inventory data. Other
cars as shown in Table 1. All required background inventory processes such as the pyrolysis reactor, spray, and flasher were
data were extracted from the Japanese LCA database (JEMAI not changed and their inventory data are set as the actual pilot
2007; JLCA 2012) and the literature on plastic recycling plant data. Figure 4 shows the simulation model developed on
(JCPRA 2007). Aspen Plus. The boundary of simulation was set as the puri-
fication and heat recovery units in Fig. 1. Crude MMA in
2.3.3 Case study 2: operational modification of the PMMA Fig. 4 includes components with lower and higher boiling
monomer recycling process points than pure MMA; the boiling point of which is about
101 °C. To separate such components, two distillation col-
The waste residue from the monomer recycling process is umns are utilized, where lower and higher boiling components
utilized as fuel on site as shown in Fig. 1. This approach are separated from MMA in first and second columns, respec-
may reduce fuel consumption and GHG emission. The waste tively. The RadFrac rigorous distillation model was selected
residue from the purification segment in Fig. 1 includes high and applied as the model for simulation in the Aspen Plus. The
amounts of MMA, which is also incinerated for heat recovery. incineration process for treating separated lower and higher
PMMA contains oxygen in its molecular structure, which boiling components, i.e., flows 2 and 5 in Fig. 4 from col-
leads to less heat generation than from PE or PP, whereas umns, and heat recovery was also simulated by an incinerator
PMMA has higher cumulative environmental loads per unit model in Aspen Plus. A pre-heater is inserted before feeding
amount of production than the other resins (PWMI 2009). The mixed residue to incinerator for increasing temperature suffi-
advantage of monomer recycling to the thermal recycling is ciently. Additionally, heat integration through a whole pro-
relatively higher than other plastics in case of PMMA. If the cesses was conducted based on pinch analysis (Biegler et al.
yield of MMA to the unit amount of waste PMMA is in- 1997). The minimum temperature between hot and cold
creased by operational modification, energy available for the streams was over 100 °C, which means that the recovered fuel
recycling process is reduced because of the decrease in residue is sufficiently available to meet the heat duty in this purification
used for fuel. In this study, we modified the purification part. To compensate for the degreased residue, i.e., fuel oil
segment comprising two distillation columns to specify the additive for pyrolysis part, by increasing MMAyield, additional

Fig. 4 Simulation model of MMA purification process developed on Aspen Plus

Int J Life Cycle Assess

fuel oil was utilized. The limitation of specification of devices the coefficient of simulation result and actual plant at the
and instruments, such as limit temperature of the material used same operation and plant settings was calculated and applied
for heat exchanger, was defined based on process engineering to estimate the process inventory from simulation results at
heuristics (Trambouze 2000). The number of stages and feed- different settings. The LCA settings were organized in Table 1
ing stage were fixed to the same settings as the actual pilot as scenario 5, where the yield was set as the highest value to
plant. The MMA yield was controlled by changing the distil- check the process with the largest recovery of MMA.
late rate of the second column, and the reflux ratios of both
columns and bottom rate of the first column were set as the
optimization parameters to minimize total energy demand. 3 Results
The simulation was performed with the change in recovery
yield of MMA monomer to waste PMMA from 0.7, value at Scenarios 1 to 4 in Fig. 5a show the results of case study 1.
the actual pilot plant, to 0.77, the highest value achievable by Scenario 1 shows the total life cycle greenhouse gas (LC-
distillation (see also “Discussion” section). At that time, sim- GHG) per functional unit without recycling methods. It has
ulation results did not correspond with the actual plant results the highest values, which means that all recycling processes
because of the simplification of actual energy demand, which can reduce LC-GHG emission. The reduction in the impact
includes energy demands for air conditioners, illumination, shown in scenario 2 demonstrates the recycling effects of
and cascade recycling of steam on site. To bridge such gaps, thermal recovery from waste PMMA. LC-GHG emissions

Fig. 5 Assessment results of scenarios in case studies 1 and 2. a LC-GHG. b Fossil resource use. c LIME single index (life cycle stage). d LIME
single index (impact category)
 Int J Life Cycle Assess

were reduced by about 10 % in scenario 1 by using recovered consumption, and the LIME single index. When analyzing
heat as a substitute for fossil fuel. The impact of PMMA recycling effects, the yields of recycled materials in PMMA
recycling on production loss is observed in the results of recycling plants have a comparatively large effect on the final
scenario 2, where about 4 % of LC-GHG in scenario 1 is results, which are set as 0.853 for the yield of PS mechanical
mitigated. Because scenario 4 has lower LC-GHG emissions recycling (JLCA 2012) and 0.7 for mechanical and monomer
than scenario 3, PMMA monomer recycling has a higher recycling processes, respectively. The sensitivity of a 10 %
ability to reduce LC-GHG emissions than does mechanical change in the yield of mechanical recycling, i.e., 0.768 to
recycling. The substitution of PMMA or PP leads to the 0.938, to LC-GHG, fossil resource consumption, and the
difference in the recycling effects of monomer recycling and LIME single index was 2.65, 11.8, and 5.06 %, respectively.
mechanical recycling, even though monomer recycling re- In this regard, the fossil resource consumption in scenario 3
quires more resources than does mechanical recycling. Hence, becomes almost the same as that in scenario 4 when the yield
the PMMA monomer recycling process has the highest priority of mechanical recycling is set at 0.768. This means that if the
in all recycling processes in terms of LC-GHG emissions. yield from mechanical recycling is lower than 0.768, the
Scenarios 1 to 4 in Fig. 5b–d show the results of case study 1 priority of scenarios 3 and 4, based on consumption of fossil
as assessed by fossil resource consumption and the LIME resources, is reversed. Because some mechanical recycling
single index. The recycling effects of MR and CR are different processes have much lower yields, e.g., 0.521, in a process
in terms of GHG emissions and fossil resource consumption as for waste containers and packaging (JLCA 2012), monomer
shown in the results of scenarios 3 and 4. It leads to the recycling of PMMA may also be a priority in terms of fossil
different order of scenarios 3 and 4 in GHG emission and resource consumption.
fossil resource consumption. As for the LIME single index, Existing systems of the collection and segregation of waste
the ranking of scenarios shows the same tendency as found in plastics are applicable for some types of product containing
the LC-GHG result, whereas the gap between scenarios 3 and PMMA. As mentioned in the “Materials and methods” section,
4 is slightly decreased in the result indicated by the LIME LCDs made from PMMA are collected and piled in the HEA
single index. Global warming potential has the largest contri- recycling process. The recycling process (Hirasawa 1999) is
bution to the LIME single index, and air pollution in urban regulated by the Home Appliance Recycling Act in Japan
areas is the second largest impact category. (METI 2001) and it has a role in the collection of valuable
Figure 5 shows the results of scenario 5, case study 2, materials such as rare earth elements (Yamasue et al. 2009).
where operational modifications were tested. It demonstrates Such systems can be adapted for the collection of PMMA For
that the increased yield of MMA monomer from 0.7 to 0.77 other molding products made from l-PMMA pellets, existing
results in a decrease in environmental impacts, fossil re- recycling systems such as cars, construction materials, and
source consumption, and the LIME single index. This means containers and packaging can also be adapted to collect PMMA.
that the recycling effect of increased recovery of MMA in PMMA pyrolysis has an advantage in that the yield of MMA to
monomer recycling is higher than the negative effect caused inputted waste PMMA is not greatly changed by contamination
by the requirement for increased fuel. Because of the high with other materials (MRC 2011; Nakagawa 2007; Sasaki et al.
environmental load of production of PMMA from fossil 2008); therefore, PMMA pyrolysis is a robust recycling process
fuels, the increased yield of MMA monomer in the PMMA (Fujii et al. 2012) for the possibility of contaminating various
pyrolysis process leads to an increase in the effect of mono- types of plastics in waste. Note that molding products contain-
mer recycling on GHG emission, fossil resource use, and the ing PMMA have not been investigated in detail, and so, further
LIME single index, even if additional fuel energy is required investigation and accumulation of statistical data are required.
for recovering MMA monomer from crude MMA in distil- The results shown in Fig. 5 demonstrate the recycling effect
lation columns. of PMMA pyrolysis. PMMA pyrolysis recycling may be more
efficient than mechanical recycling as shown in Fig. 5a, c–d.
PMMA tends to be used for products requiring excellent
4 Discussion transparency and climate resistance properties, and mechani-
cally recycled PMMA pellets cannot achieve such high per-
The environmental loads and fossil resource consumption for formance. With increasing requirements for plastics to replace
the production of PMMA and PP are different. Although conventional heavy materials such as glass or metal (Humbert
GHG emissions from PMMA production are more than twice et al. 2009; Ribeiro et al. 2006), PMMA can be used as a
as high as emissions from PP production, other environmental substitute for glass. LCD panels will be required to meet the
loads, especially SOx, NOx, and fossil resource consumption, demand for television sets (Display Search 2012). An ade-
are not significantly different. These differences in environ- quate recycling method for waste PMMA is required, and
mental loads and GHG emissions are reflected in the different PMMA pyrolysis can be an effective method for fulfilling
trends in the results indicated by LC-GHG, fossil resource the closed-loop recycling of MMA all over the world.
Int J Life Cycle Assess

The high effectiveness of PMMA monomer recycling is even further, in spite of the additional fuel consumption used
partly because PMMA is composed of a single monomer. in MMA purification. This is because the production of new
PET, for example, has two monomers: ethylene glycol and MMA has a high environmental impact and recycling MMA
terephthalic acid. Although the monomer recycling of PET is is effective in reducing the overall life cycle impact.
also effective, the process flow of PMMA pyrolysis shown in Although the total amount of PMMA use is not large in
Fig. 1 is simpler than that of PET depolymerization through plastics, a closed-loop recycling system, which monomer
purified terephthalic acid (PTA) and dimethyl terephthalate recycling may achieve, can be established together with
(DMT) processes (Sugiyama et al. 2006). The complexity of recycling of other materials contained in these products such
chemical processes leads to high-energy consumption due to as base or rare metals (Yamasue et al. 2009). This was con-
the increase of process units such as reactors and separators, firmed in this study through investigations of recycling plants
which was shown in PET monomer recycling processes (Su- for home electronic appliances and automobiles, where each
giyama et al. 2006). Although BHET process in PET monomer component of the product is segregated as much as possible
recycling has small number of reactor and separator comparing by manual procedures (Hirasawa 1999) or by specialized
with PTA and DMT processes, the monomer recycling of PET scrapping machines. The PMMA monomer recycling process
is regarded as it has higher environmental impacts than the can contribute to the establishment of a recyclable society.
mechanical recycling of PET (Nakatani et al. 2010). Monomer
recycling of PMMA has an advantage in environmental im-
Acknowledgments The authors thank Tran Nghiep Nam, Takahiro
pacts than mechanical recycling of PMMA.
Izumi, Emiri Kakazu, Akira Sasaki, and Genya Tanaka for their coop-
To improve monomer recycling performance, MMA in- eration in data collection for LCA. Part of this study was supported by a
cluded in the crude MMA flow should be recovered as much Grant-in-Aid for Scientific Research (B) (no. 23360404) from the Japan
as possible. In case study 2, yields were increased from 0.7 to Society for the Promotion of Science.
0.77 by adopting a change in the operation of the two distil-
lation columns. The largest value in the distillation columns
settings in this case study was 0.77 because of the difficulties
in purifying MMA monomer by distillation. Considering the References
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