pubs.acs.

org/est Article

Material Flows of Polyurethane in the United States

Chao Liang, Ulises R. Gracida-Alvarez, Ethan T. Gallant, Paul A. Gillis, Yuri A. Marques,
Graham P. Abramo, Troy R. Hawkins,* and Jennifer B. Dunn*
Cite This: Environ. Sci. Technol. 2021, 55, 14215−14224 Read Online

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ABSTRACT: Today, polyurethanes are effectively not recycled and are made principally from nonrenewable, fossil-fuel-derived
resources. This study provides the first high-resolution material flow analysis of polyurethane flows through the U.S. economy,
tracking back to fossil fuels and covering polyurethane-relevant raw materials, trade, production, manufacturing, uses, historical
stocks, and waste management. According to our analysis, in 2016, 2900 thousand tonnes (kt) of polyurethane were produced in the
United States and 920 kt were imported for consumption, 2000 kt entered the postconsumer waste streams, and 390 kt were
recycled and returned to the market in the form of carpet underlayment. The domestic production of polyurethane consumed 1100
kt of crude oil and 1100 kt of natural gas. With the developed polyurethane flow map, we point out the limitation of the existing
mechanical recycling methods and identify that glycolysis, a chemical recycling method, can be used to recycle the main components
of postconsumer polyurethane waste. We also explore how targeting biobased pathways could influence the supply chain and
downstream markets of polyurethane and reduce the consumption of fossil fuels and the exposure to toxic precursors in
polyurethane production.
KEYWORDS: polyurethane, material flow analysis, recycling, circular economy, biobased feedstock, sustainability

■ INTRODUCTION
Polyurethane is one of the most versatile materials in the
world. It can be produced in various forms and used in a
variety of markets. It ranked sixth in worldwide polymer
production in 20181 with a global market of 65.5 billion
dollars.2 This market is expected to reach 105.2 billion dollars
by 2025.3
However, polyurethane poses environmental and human
health concerns at various points across its life cycle.4 Like
other plastics, this versatile polymer is made from fossil fuels
and its production emits greenhouse gases (GHG). Nicholson
et al. reported that the United States (U.S.) annual GHG
emissions from polyurethane production is estimated to be 7.8
million metric tons.5 Additionally, methylene diphenyl
diisocyanate (MDI) and toluene diisocyanate (TDI), two of
the main precursors for polyurethane, are classified as
carcinogenic, mutagenic, and reprotoxic (CMR), which could
cause health issues after prolonged exposure.4 At the end of
their life, polyurethane products are mostly incinerated or
© 2021 The Authors. Published by
American Chemical Society
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landfilled, creating undesirable environmental effects, such as
land resource consumption and toxin and GHG emissions.
These health and environmental concerns associated with
polyurethane and its supply chain have led to several policies
that aim to reduce polyurethane’s environmental effects. For
example, several countries (mostly in Europe) have banned the
landfill disposal of municipal solid waste, which limits disposal
options for many types of polyurethane. Both the European
Union (EU) and the U.S. Environmental Protection Agency
(EPA) have issued regulations to progressively or potentially
ban isocyanates.4,6 To increase the safety and sustainability of
Received: June 4, 2021
Revised: August 30, 2021
Accepted: September 14, 2021
Published: October 7, 2021
https://doi.org/10.1021/acs.est.1c03654
Environ. Sci. Technol. 2021, 55, 14215−14224
 Table 1. Summary of Data Sourcesa,b
category reference description
primary energy primary energy to isocyanates and polyols (except polyester polyols) 32 material and total energy consumption of crude oil and natural gas to
isocyanates and polyols (except polyester polyols)
primary energy to polyester polyols 33 material and total energy consumption of crude oil and natural gas to
polyester polyols
primary energy to additives 36 material and total energy consumption of crude oil and natural gas to
blowing agents and flame retardants
precursor chemicals TDI, pure MDI, and polymeric MDI 29 demand of TDI and MDI, distribution of precursors to intermediate
products
specialty isocyanates, polyether polyols, polyester polyols, PTMEG, acrylic polyols, and additives 30, 31 demand of specialty isocyanates and polyols, distribution of precursors to
intermediate products
production of polyurethane products 31, 37 total polyurethane production amount, share of polyurethane production by
polyurethane materials type
rigid foams to appliances, rigid foams to building and construction 39 share of rigid foams used in building and construction, and appliances
Environmental Science & Technology

rigid foams to packaging, transportation, others 40 quantity of rigid foams to packaging, transportation, and other end-use
markets
flexible foams 39 share of flexible foams by end-use markets
adhesives and sealants, binders, coatings, and elastomers 30, 31 demand of adhesives and sealants, binders, coatings, elastomers, and
distribution of these products to end-use markets
end-use markets building and construction, transportation, EEE, machinery and foundry, packaging, textile, apparel and 38 distribution of polyurethane by end-use markets
footwear, furniture and bedding, and other end-use markets
waste collection building and construction 50−52 construction waste amount, share of plastics in construction waste, and share
of polyurethane in plastics in construction wastes
vehicles 36, 53, 54 number of vehicles that became waste, share of plastics in vehicle, and share

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of polyurethane in plastics in vehicle
other transportation proportional to that of vehicles
electronics 25, 55, 56 electronics waste amount, share of polyurethane in the wastes
appliances 25, 55, 56 appliances waste amount, share of polyurethane in the wastes
machinery and foundry log-normal algorithm
packaging log-normal algorithm
textile, apparel, and footwear 57, 58 textile waste amount (including apparel and footwear), share of
polyurethane in the wastes
pubs.acs.org/est

furniture and bedding 55 furniture and furnishings waste amount (including bedding), share of
polyurethane in the wastes
carpet underlayment 41, 55, carpets and rugs waste amount, share of polyurethane in the wastes
59, 60
other end-use products log-normal algorithm
municipal polyurethane wastes 49, 61 plastics waste amount in municipal solid wastes, share of polyurethane in
plastics in municipal solid wastes
waste management landfill, incineration, and recycling 42−44 share of recycling, U.S.-specific ratio of landfill to incineration for plastics in
municipal solid wastes
recycling (industrial and postconsumer wastes to carpet underlayment) 41 amount of domestic industrial flexible foam scrap, amount of domestic
postconsumer flexible foam scrap
a
Data for trade and in-use stock are not included. bTDI, toluene diisocyanate; MDI, methylene diphenyl diisocyanate; PTMEG, polytetramethylene ether glycol; and EEE, electrical and electronic
equipment.
Article

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https://doi.org/10.1021/acs.est.1c03654
Environmental Science & Technology
polyurethane, biobased production pathways and recycling
technologies are under development7−11 to increase the
amount of renewable feedstocks and secondary materials in
the polyurethane supply chain. With the implementation of
regulations and the development of technologies, polyurethane
status quo could be dramatically altered, causing shifts in the
polyurethane supply chain, markets for precursors, and use
patterns of downstream products. To understand the
sustainability implications of these shifts, a comprehensive
and thorough understanding of today’s polyurethane material
flows is necessary.
Material flow analysis (MFA) is an approach to tracking the
flows and stocks of target materials within a system defined in
space and time.12 MFAs can be static (a snapshot of a system
in time). This approach was widely used in early MFAs. It is
often appropriate for understanding a material system when
data resources are limited.12,13 Alternatively, MFAs can be
dynamic (over a time interval) and use historical trends to
create future scenarios. This is a key advance but usually
requires considerable resources.12,14 The MFA has been used
to study many different types of materials to provide a basis for
decision making,15 improve the circularity of economy,16 and
determine the challenges and opportunities for designing
environmentally beneficial materials and processes.17 Aside
from several studies that analyzed the flows of poly(vinyl
chloride) (PVC) 18,19 and poly(ethylene terephthalate)
(PET),20 most early MFAs of plastics considered them as a
single class of materials without distinguishing individual
polymers.21−24 Since 2018, several studies have addressed
more polymers including linear low-density polyethylene, low-
density polyethylene, high-density polyethylene, polypropy-
lene, polystyrene, expanded polystyrene, and acrylonitrile
butadiene styrene.25−27 However, for polyurethane, only
Heller and colleagues28 provide a material flow analysis in
the United States, which merely includes the quantity of total
U.S. production and its share in the end-use markets. To the
best of our knowledge, our study is the first high-resolution
and complete analysis of polyurethane material flows in the
United States.
This study tracked the annual polyurethane flow in the
United States in 2016. Flows are tracked back to the primary
energy level to identify opportunities for incorporating
recovered polymer materials and those derived from biomass.
Overall, the MFA covers raw materials, polyurethane
production, end-use products manufacturing, use, trade, and
waste collection and management. The historical in-use stock
and the components of the collected waste were analyzed to
determine the challenges and opportunities of polyurethane
recycling and the possible shift of polyurethane components in
postconsumer wastes in the future.
■
MATERIALS AND METHODS
Compared to some extensively investigated polymers, such as
PVC and PET, the data for polyurethane across almost all
investigated stages are very sparse. This study considered data
from various sources but prioritized public data from
governmental resources, industry associations, and peer-
reviewed literature to minimize discrepancies. The following
sections describe the origin of data records used to quantify
polyurethane flows (summarized in Table 1), which also point
out the data gaps we encountered and describe how we dealt
with them.
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Precursors for the U.S. Polyurethane Industry. The
quantities of TDI, pure MDI, and polymeric MDI used to
produce various polyurethane products are estimated based
upon interviews with associated industrial manufacturers,
processors, producers, users, and associations that are
conducted by the American Chemistry Council (ACC).29
The quantities of specialty isocyanates, polyether polyols,
polyester polyols, polytetramethylene ether glycols (PTMEG),
acrylic polyols, and additives used to produce various
polyurethane products are from survey-based industrial data
for the United States, Canada, and Mexico published by
ACC.30 We scale these values by 0.81, the share of U.S.
polyurethane production among these countries, as reported
by ICIS.31
Primary Energy for the U.S. Polyurethane Industry.
The material and total energy consumption of crude oil and
natural gas to isocyanates and polyols are estimated by
multiplying the consumption data per unit of precursors
reported by Franklin Associates32 and polyurethane Europe33
by the quantities of the precursors reconciled by STAN34 (see
the “Data Reconciliation” section).
According to the literature,35 additives for polyurethane
production mainly include flame retardants, blowing agents,
cross-linking agents, and catalysts. After analyzing industrial
polyurethane formulations, blowing agents and flame retard-
ants are found to be the two main components in additives and
are considered in this study. The primary energy used to
produce the blowing agent is estimated based on its life cycle
inventory reported by GREET.36
Additional details regarding the primary energies for the U.S.
polyurethane industry are given in “Details on fossil fuel
consumption” in the Supporting Information.
U.S. Polyurethane Industry. Total U.S. polyurethane
production is based upon a market report for 2016 and 2017.37
Again, the data are for the United States, Canada, and Mexico
and are therefore scaled to reflect U.S. flows with a factor of
0.81.31 Quantities of intermediate products are calculated
based on the reported shares.37
U.S. Manufacturing. The quantities of polyurethane used
in end-use products (except carpet underlayment) are obtained
from ACC.38 For this study, we separate virgin polyurethane
used for carpet underlayment from the “furniture and bedding”
category and merge them with the recycled flexible foam scrap
to create the “carpet underlayment” category.
To complete the tracking of polyurethane flows, it is
necessary to estimate the distribution of intermediate products
to different end-use markets. For rigid foams used in the
building and construction and appliances markets, we use the
share reported by Thomas et al.39 The quantities of rigid foams
to transportation, packaging, and other end-use markets are
based on those reported by Forman.40 The distribution of
flexible foams to different end-use markets is based on Thomas
et al.39 and the shares of adhesives and sealants, binders,
coatings, and elastomers in various end-use markets are those
reported by ACC.30
U.S. Waste Collection. Polyurethane waste is categorized
as industrial (waste generated during manufacturing) and
postconsumer (waste generated after use). In this study, the
industrial waste only includes the flexible foam scrap (trim
foams) generated during the manufacturing of end-use
products, whose quantity is reported by the Carpet Cushion
Council (CCC).41 Based on our experience, trim foams are
mainly generated during the manufacturing of furniture and
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Figure 1. Reconciled U.S. flow of polyurethane in 2016 (thousand tonnes). Drawn using E!Sankey software. TDI, toluene diisocyanate; MDI,
methylene diphenyl diisocyanate; PTMEG, polytetramethylene ether glycol; EEE, electrical and electronic equipment; and CASE, coatings,
adhesives, sealants, binders, and elastomers. Note: the data for primary energy was not reconciled. All of the numbers displayed were rounded to
one or two significant digits.
mattresses. Additionally, a higher percentage of waste flexible
foams is generated from furniture manufacturing than from
mattress manufacturing because the foams embedded in the
furniture are more irregular. To reconcile the data from
CCC,41 this study assumes 45% of the flexible foams used in
furniture manufacturing and 25% of the flexible foams used in
mattress manufacturing become trim foams. Polyurethane
scraps generated from other processes are not included in the
recycling stream in our analysis.
Postconsumer waste from various end-use products are
estimated based on the U.S. EPA data, calculated through the
log-normal algorithm,28 or estimated based on the proportion
to other categories, which are described in detail in the
Supporting Information.
U.S. Waste Management. In this study, industrial and
postconsumer waste are managed in three ways: landfilling,
incineration, and recycling with shares of 58, 12, and 30%,
respectively. The recycling share is based on values reported in
two studies. First, Gómez-Rojo et al.42 report that in Europe in
2016, 31.1% of polyurethane waste was recycled. Second,
Gadhave et al.43 report that in the world in 2015, 29.7% of
polyurethane waste was recycled. Considering that the
percentage of incineration in Europe is usually higher than in
the United States and the global value is not necessarily
reflective of common practice in the United States, this study
adopts a U.S.-specific ratio of landfill (83%) to incineration
(17%) for discarded plastics in municipal solid waste in 2016
as the U.S. EPA reports.44 Flows of polyurethane waste to
aquatic and other environments are negligible.45,46
The flexible polyurethane foam scrap is either used to
manufacture carpet underlayment through “rebonding,” where
the quantities of U.S. domestic industrial and postconsumer
wastes are reported by CCC41 or exported to other countries.
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The details of these two options are provided in “Trade of
waste” in the Supporting Information. It should be noted that
the quantity of polyurethane wastes exported in 2016 might
not reflect today’s situation. According to the United States
International Trade Commission (USITC), the export of
plastic wastes (PET excluded) decreased from 704 thousand
tonnes (kt) in 2016 to 228 kt in 2019.47 This is mainly because
China, previously the main recipient and processor of U.S.
exported plastic wastes, banned the import of most plastic
wastes in January 2018. Although other countries accepted
some plastic waste in China’s place (e.g., Bangladesh, Laos,
Turkey), eventually, these nations were overwhelmed and
tightened the rules of waste imports.47,48
International Trade. The mass flows associated with the
international trade of polyurethane precursors and intermedi-
ate products are based on trade flows reported by the
USITC.47 The mass flows associated with the international
trade of polyurethane-containing end-use goods (indirect
imports and exports) are calculated by multiplying polyur-
ethane concentration (kg polyurethane/kg goods) by traded
goods mass. The polyurethane concentration is estimated
based on literature, market reports, or our own estimates.
Where available, the mass of traded goods is extracted directly
from USITC, or in cases where other units are reported, mass
is calculated with estimated conversions. We assumed that the
only type of waste polyurethane that is imported into the
United States is the flexible foam scrap.41 The amount of
exported waste is estimated based on USITC47 reports and
polyurethane concentration in plastic waste reported by Kumar
and Thakur.49 More details of the trade data are given in the
Supporting Information.
U.S. Use Phase. In addition to the polyurethane
introduced to the use phase in 2016, we also incorporate
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Figure 2. Reconciled U.S. flow of polyurethane in 2016 (thousand tonnes) highlighting polyurethane material types. Drawn using E!Sankey
software. TDI, toluene diisocyanate; MDI, methylene diphenyl diisocyanate; PTMEG, polytetramethylene ether glycol; and EEE, electrical and
electronic equipment. Note: the data for primary energy was not reconciled. All of the numbers displayed were rounded to one or two significant
digits.
estimates of polyurethane produced or traded in previous years
(1973−2015) that remained in use in 2016. Furthermore, the
distribution of the collected waste by polyurethane production
time is calculated. The in-use stocks and wastes are calculated
with the following three steps: (1) estimate the quantity of
polyurethane production and polyurethane used in end-use
markets between 1973 and 2016; (2) estimate the average
lifetime and standard deviation of polyurethane embedded in
end-use products; (3) use log-normal distribution to calculate
in-use stocks and wastes. More details of the data presented in
the use phase in Figure 1 are given in “In-use stock details” and
“Material flow analysis of polyurethane” in the Supporting
Information.
Data Reconciliation. To reconcile mass flows across
various data sources, the STAN34 software package was used.
STAN is widely used in MFA and employs a reconciliation
process based on weighted least-squares minimization. The
standard error of each data source used in STAN was
estimated through an uncertainty analysis following the
methods of Kawechi et al.25 and Laner et al.,21 which are
based on five different data quality indicators: geographical,
temporal, and material representativeness, completeness, and
source reliability. A detailed method description and a
comparison of the input data and the reconciled data are
given in the Supporting Information. Figure S3 illustrates the
influence of data reconciliation on MFA results.
■
RESULTS
In total, 3700 kt of polyurethane were consumed in the United
States in 2016. Two thousand nine hundred thousand tonnes
were produced domestically, 920 kt were imported for
consumption, and 280 kt were exported. Two thousand
thousand tonnes were discarded, and 390 kt were recycled and
returned to the manufacturing of carpet underlayment. Among
the recycled polyurethane, 110 kt were from the postconsumer
waste, resulting in a 5.5% of end-of-life recycling rate (recycled
postconsumer polyurethane divided by the end-of-life polyur-
ethane generated). This rate is lower than the average end-of-
life recycling rate of U.S. plastics in 2015 estimated by Di et
al.27 (6.2%) and EPA61 (9%).
Figure 1 represents the estimated 2016 U.S. flow of
polyurethane. As shown in the figure, this study tracks the
polyurethane production back to primary energy (natural gas
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and crude oil). The mass inputs of natural gas and crude oil for
polyurethane production are almost the same, but the total
energy consumption of natural gas is much higher than that of
crude oil in the polyurethane supply chain. Polyurethane is
produced from three main types of precursors: isocyanates,
polyols, and additives. Among them, isocyanates and polyols
account for 89% of fossil fuel energy consumption. Compared
to the production of isocyanates, polyol production consumes
50% more primary energy. For the isocyanates, MDI, especially
polymeric MDI, is the dominant polyurethane precursor,
followed by TDI. For polyols, polyether polyols are the most
important for polyurethane precursors, followed by polyester
polyols. Among polyurethane types (intermediate products)
produced with these precursors, rigid foams and flexible foams
account for more than 60% of the total. This diagram shows
the distributions of precursors to intermediate products. For
example, polymeric MDI is the main material for rigid foams
and binders, and polyether polyols are the main material for
flexible foams.
Figure 1 also tracks the distributions of intermediate
products to end-use markets. The building and construction
category is the largest market (37%) for domestic polyur-
ethane, where rigid foams are the dominant component. This
category mainly consists of thermal insulation. Binders,
typically used in composite wood products, are also an
important component in this category. Transportation is the
second-largest market for polyurethane, where flexible foams
account for the largest portion. Automotive seating is a large
market for flexible foams. Furniture and bedding, electrical and
electronic equipment (EEE), machinery and foundry, pack-
aging, and carpet underlayment are also important markets for
polyurethane produced in the United States.
Figure 1 also incorporates the trade of precursors,
intermediate products, and end-use products. Compared to
imported precursors and intermediate products, the quantity of
polyurethane imported in end-use products is much larger.
The EEE, machinery and foundry category; textile, apparel,
and footwear category; and transportation category are the
three end-use market categories that consume the most
imported polyurethane. Compared to domestically produced
polyurethane, these sectors consume 1.2, 5.5, and 0.5 times
greater amounts of imported polyurethane, respectively. Of all
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polyurethane use categories, the transportation category
exports the most (23%) polyurethane.
The use phase of the diagram shows the amount of
polyurethane produced or traded in the different markets
between 1973 and 2016 and that remained in use in 2016. As
shown in Figure 1, the building and construction, trans-
portation, EEE, machinery and foundry, and carpet underlay-
ment categories account for the most in-use stocks in 2016,
which is a combined effect of large annual production and long
product lifetime.
Among all of the end-use markets, transportation, carpet
underlayment, EEE, and machinery and foundry generated the
most polyurethane waste in 2016. Figures 1 and 2 show the
distribution of polyurethane waste collected in 2016 by
production year. The waste collected in 2016 from all markets
is less than the polyurethane added to the corresponding
markets. This trend reflects variations in annual domestic
polyurethane production, which is generally increasing in the
United States over the last several decades. For the building
and construction category, there is a significant difference
between the flows entering and exiting the use phase, which is
a combined effect of increasing production and long product
lifetime. This suggests that more polyurethane from building
and construction will be available for potential recycling in the
future.
The collected polyurethane wastes are either landfilled,
incinerated, or recycled. Among these options, landfilling is the
dominant polyurethane waste management method. As shown
in the diagram, recycled polyurethanes are all flexible foams
and are all used for the manufacturing of carpet underlayment.
The majority of recycled flexible foams are industrial foam
scrap, consisting of approximately 46% of imports and 54% of
domestic wastes that come from the manufacturing of furniture
and bedding.
Figure 2 breaks down the flows of end-use products and
wastes into polyurethane types. As shown in the figure, trade,
especially the trade of end-use products, has a significant
influence on the share of polyurethane types in the U.S.
market. The majority of imports flow to three market
categories: (1) transportation, (2) EEE, machinery and
foundry, and (3) textile, apparel and footwear. Therefore,
more rigid foams, flexible foams, and elastomers, the main
polyurethane types in these three market categories, are
introduced into the United States.
Because of the differences in trade quantities and lifetimes of
the end-use products, the share of polyurethane types in
postconsumer waste is quite different from that in domestic
production. Flexible foams are the dominant type and account
for 46% of postconsumer wastes, while rigid foams only
account for 22%. In contrast, rigid foams account for the
largest portion of domestic production. The main reason for
the significant reduction of rigid foams in postconsumer wastes
is the product lifetime of building and construction, which is
the main market for rigid foams. Polyurethane products in that
sector are more long-lived than in others. If the trends of
production and trade hold constant, the main component of
the postconsumer waste will eventually shift to rigid foams.
■
DISCUSSION
Challenges and Opportunities for Polyurethane
Recycling. Figures 1 and 2 provide “panoramic views” of
the polyurethane flow in the United States, which can help
identify opportunities and challenges for recycled/upcycled
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polyurethane and biobased polyurethane. Here, we discuss
three main opportunities, together with their challenges.
There Are Ample Feedstocks from Waste that Could
Support Increased Polyurethane Circularity. Currently,
among various polyurethane types, flexible foams are the
only type that is recycled on a large scale in the United States.
This is mainly because rebonding is the only polyurethane
recycling method operating at a commercial scale in the United
States. In this mechanical recycling, the flexible polyurethane
foam scrap is mixed with binders to produce padding-type
products. The adoption of this method in the United States
results in the “carpet underlayment loop” in Figure 1, the only
loop in the figure.
North America has the greatest demand globally for the
flexible polyurethane foam scrap, and the demand increased
from 285 kt in 2009 to 455 kt in 2013, according to European
Diisocyanate & Polyol Producers Association (ISOPA).62 This
demand is related to the use of carpet in domestic residences in
North America. The CCC also reported that the quantities of
recycled flexible polyurethane foams (recycled industrial waste
+ recycled postconsumer waste) in the United States increased
by 29.6% from 2011 to 2015.41 The recycled industrial scrap
was reported to increase by 84.7% from 2011 to 2015,41 which
might be associated with the increased demand for flexible
foam scrap and the increased market for mattresses and
furniture. Compared to the postconsumer flexible foam scrap,
the industrial scrap has never been contaminated by the
customers and is therefore preferred for mechanical recycling.
Partially for this reason, in addition to low recycling rates for
postconsumer waste, the postconsumer foam scrap makes up
less of the recycling loop in Figure 1. In 2016, only 11% of
flexible foams in postconsumer wastes were recycled and
reused domestically.
Although the current recycling rate in postconsumer waste is
low, secondary (from waste) feedstocks are ample and could
support polyurethane recycling. As shown in Figures 1 and 2,
the quantity of flexible foams in collected waste is higher than
the flexible foam domestic production. Ideally, all postcon-
sumer flexible foam would be recycled and reused, resulting in
secondary feedstocks satisfying the market demand. In
addition, like flexible foam, more elastomer waste is collected
than is produced. The amounts of collected coatings, adhesives
& sealants, and rigid foams wastes exceed 70, 50, and 40% of
their domestic demand, respectively.
It should be noted that considering industrial practice, the
recycling potential differs by polyurethane type. Generally, the
uniform polyurethane parts that can be easily dissembled from
end-use products have higher recycling potential, such as the
flexible polyurethane foam seat cushions and polyurethane
elastomer soles on shoes. For the cases in which the
polyurethane is spread on or dispensed in other materials
such as polyurethane binders in composite wood materials,
separating, collecting, and recycling these polyurethanes is
difficult. Among the polyurethane types, rigid foams, flexible
foams, and elastomers can be collected in a uniform material
relatively easily; in contrast, coatings, binders, adhesives, and
sealants, which are usually mixed with other materials in end-
use products, are difficult to separate. The end-use products
that contain a higher share of rigid foams, flexible foams, and
elastomers can be considered more promising for polyurethane
recycling.
Chemical Recycling Offers an Opportunity to Reduce U.S.
Demand for Polyols for Polyurethane Production. Mechan-
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ical recycling has significant limitations for polyurethane.
Although flexible foam scrap and used rebonded carpet
underlayment can be reused 8−10 times, it will inevitably
lose its foam resilience and reach the end of its life.63 In fact,
except metal, almost all materials can only undergo mechanical
recycling a limited number of times. Eventually, mechanically
recycled materials will unavoidably lose their function and
need to be discarded.62
Moreover, the durability of polyurethane products is an
obstacle to mechanical recycling. As shown in Table S5, the
lifetime of polyurethane in some end-use markets exceeds 10
years (e.g., transportation). For the building and construction
category, the average lifetime of polyurethane exceeds 30 years.
Over the decades of these materials’ useful life, some additives
used to produce polyurethane have been banned, restricted,
and phased out as Europur enumerates for some compounds in
polyurethane production 10 years ago.62 In mechanical
recycling, the material is reused in its polymer form, which
means the banned substance cannot be removed during
recycling. As a result, some of the collected polyurethane waste
might not be usable despite retaining its properties and
performance.
Chemical recycling regenerates material’s chemical constit-
uents and can overcome mechanical recycling’s limitations.
Glycolysis is the most widely used chemical recycling
method.64 In it, polyurethane waste is reacted with diols at
an elevated temperature to cleave the covalent bonds, breaking
the polyurethane down to lower-molecular-weight products.
Polyols are subsequently recovered for new polyurethane
synthesis.64 There are already several successful commercial-
scale glycolysis examples in Europe (e.g., Getzner Company in
Austria recycles polyurethane elastomer wastes). This tech-
nology can be used to recycle almost all types of polyurethane,
where the three most widely treated polyurethane types are
rigid foams, flexible foams, and elastomers,65 which are also the
three largest components in postconsumer wastes in 2016 (see
Figure 2). This technology therefore has the potential to
significantly reduce the demand for new polyols for polyur-
ethane production in the United States. With flexible foams
expected to dominate polyurethane types in postconsumer
waste for the next several decades, it is essential to further
develop glycolysis for flexible foams.
Opportunities to Incorporate Biomass as a Feedstock.
Incorporating biomass in the production of polyurethane can
reduce the demand for fossil fuel resources. As shown in Figure
1, polymeric MDI and polyether polyols are the two major
precursors for polyurethane production, which account for
more than 60% of fossil fuel material consumption. These
compounds are therefore two primary targets to be made with
biomass. Furthermore, Figure 1, as a “baseline” polyurethane
flow map, can help quantitatively evaluate the impact of
incorporating biobased materials on end-use markets and the
environment. For example, if polymeric MDI is made with
biobased materials, its influence (46% of the polyurethane
mass) on the building and construction market will be
significant. Polymeric MDI is the main precursor for rigid
foams and binders, which are mainly used in the building and
construction market. Comparatively, its influence (10% of the
polyurethane mass) on the transportation market will be very
minor. In addition, reductions in fossil fuel consumption and
GHG emissions from the replacement of fossil fuels with
biomass as feedstocks can be determined using Figure 1 and
life cycle inventory data.
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Nearly all major types of polyurethane could incorporate
greater amounts of biomass-derived precursors in their supply
chain, which is especially important for the types that are
difficult to be recycled. Both of the two main precursors,
polyols and isocyanates, can be produced from renewable
resources, such as vegetable oil66 and algal oil.67 According to
Figure 1, the renewable content in various polyurethane types
could range between 7 and 65% if using biobased polyols and
19−77% if using biobased isocyanates. Although the use of
bioisocyanate could circumvent the phosgenation reaction,
isocyanate-based polyurethane can generate toxic substances
when the waste products are incinerated and/or landfilled at
the end of life.68 The nonisocyanate polyurethane (NIPU)
route seems to be a promising possible alternative for PU
synthesis. There are four main NIPU routes: polycondensa-
tion, rearrangement, ring-opening-polymerization, and poly-
addition.68 Among them, NIPU manufactured by polyaddition
reaction of cyclic carbonates and polyamines resulting in the
formation of polyhydroxyruethane (PHU) has received much
attention.68 It could be produced in various forms to replace
almost all polyurethane types. Precursors for PHU, cyclic
carbonates and polyamines, can also be obtained from
renewable resources. Although currently the majority of
NIPU developed is partially renewable, a large scale of
partially renewable-NIPU can also significantly reduce the
consumption of fossil fuel in polyurethane supply chains.
Data Challenges. The data challenges encountered in this
study and other MFAs of plastics are an appeal for more
thorough and transparent data collection and sharing. Data
collection techniques also need to improve.
For the analysis of international trade, data from official
agencies, such as USITC or UN Comtrade, are widely used.
Compared to the trade of intermediate products and
precursors, the estimation of end-use products usually
introduces higher discrepancies because estimating the target
material concentration in various products is required.
Typically, this estimation is based on the target material
amount in a specific quantity of custom value (e.g., tonne
plastics/million US dollars) or mass of end-use products (e.g.,
kg polyurethane/kg commodity) in a general HTS category
(e.g., HTS code 2 level). If the trade is not reported in units of
mass and the material concentration is difficult to be estimated
based on custom value, additional estimation of a coefficient
for unit conversion (e.g., kg/quantity commodity) is usually
required, which could introduce further discrepancies. This
study estimated polyurethane concentration in an HTS code
4−10 level for most of the trade cases. Some categories in
USITC data can exhibit a wide weight range. One example of
such a category is “tanks” (8907.90.0060). In these instances, if
the trade quantity is high, different estimates of the commodity
weight could significantly influence analysis results. A possible
solution is to conduct sensitivity analyses for commodity
categories with wide ranges, but this type of analysis is very
time intensive. A more detailed description and a finer
classification of the commodity from the data provider could
significantly increase the estimate accuracy.
Regarding domestic flows, survey- or interview-based data
(such as ACC, EPA) are major data sources. These sources can
be limited by the design and coverage of the survey or
interview. Although the U.S. Department of Commerce
releases domestic industrial data (e.g., domestic supply/use
of commodities) periodically, these are usually categorized by
industry, making it difficult to gain detailed insights into the
https://doi.org/10.1021/acs.est.1c03654
Environ. Sci. Technol. 2021, 55, 14215−14224
Environmental Science & Technology
relationship between materials. In addition, values are
presented in dollars, which again requires assuming a
relationship between value and mass. To improve MFAs,
governmental statistics of domestic mass flows categorized by
commodities in units of mass are essential. These could be
enabled over time by technologies such as blockchain or the
internet of things, possibly even leading to real-time MFAs.
With better data sources as a foundation, MFAs can be of
increasing utility to design circular and sustainable materials
systems for polyurethane, other plastics, and other materials in
general.
■
ASSOCIATED CONTENT
*
sı Supporting Information
The Supporting Information is available free of charge at
https://pubs.acs.org/doi/10.1021/acs.est.1c03654.
Uncertainty analysis (Tables S1−S3); trade flow details
(Table S4, including raw materials, production,
manufacturing, uses, and wastes); fossil fuel consump-
tion details (isocyanates, polyols, and additives); in-use
stock details (Tables S5 and S7, Figure S1); waste
collection details (polyurethane in municipal solid waste,
building and construction, transportation, furniture and
bedding, textile, apparel and footwear, electrical and
electronic equipment, machinery and foundry, carpet
underlayment, packaging, other end-use markets); data
limitation; material flow analysis of polyurethane (Figure
S2); and data reconciliation (Figure S3) (PDF)
Flow data in Sankey diagram (XSLX)
Trade data (XSLX)
■
AUTHOR INFORMATION
Corresponding Authors
Troy R. Hawkins − Systems Assessment Center, Energy
Systems Division, Argonne National Laboratory, Lemont,
Illinois 60439, United States; Email: thawkins@anl.gov
Jennifer B. Dunn − Department of Chemical and Biological
Engineering, Northwestern University, Evanston, Illinois
60208, United States; Northwestern-Argonne Institute of
Science and Engineering, Evanston, Illinois 60208, United
States; orcid.org/0000-0002-2065-5106;
Email: jennifer.dunn1@northwestern.edu
Authors
Chao Liang − Institute for Sustainability and Energy at
Northwestern, Northwestern University, Evanston, Illinois
60208, United States; orcid.org/0000-0002-3307-7712
Ulises R. Gracida-Alvarez − Systems Assessment Center,
Energy Systems Division, Argonne National Laboratory,
Lemont, Illinois 60439, United States; orcid.org/0000-
0002-5061-169X
Ethan T. Gallant − Systems Assessment Center, Energy
Systems Division, Argonne National Laboratory, Lemont,
Illinois 60439, United States; Present Address: Bioproducts
and Biosystems Engineering, University of Minnesota, St.
Paul, Minnesota 55108, United States
Paul A. Gillis − The Dow Chemical Company, Polyurethane
R&D, Lake Jackson, Texas 77566, United States
Yuri A. Marques − The Dow Chemical Company,
Polyurethane R&D, Lake Jackson, Texas 77566, United
States
14222
pubs.acs.org/est Article
Graham P. Abramo − The Dow Chemical Company, Core
Research and Development, Collegeville, Pennsylvania 19426,
United States
Complete contact information is available at:
https://pubs.acs.org/10.1021/acs.est.1c03654
Notes
The authors declare no competing financial interest.
■
ACKNOWLEDGMENTS
Northwestern University and Argonne National Laboratory
were supported by the Office of Energy Efficiency and
Renewable Energy of the U.S. Department of Energy (DOE)
under contracts DE-EE0008928 and DE-AC02-06CH11357,
respectively. The authors are grateful to Nichole Fitzgerald and
Andrea Bailey of the Bioenergy Technologies Office for their
support and guidance. The views and opinions of the authors
expressed herein do not necessarily state or reflect those of the
U.S. Government or any agency thereof or of any commercial
entity. Neither the U.S. Government nor any agency thereof,
nor any of their employees or employees of contributing
companies, makes any warranty, expressed or implied, or
assumes any legal liability or responsibility for the accuracy,
completeness, or usefulness of any information, apparatus,
product, or process disclosed, or represents that its use would
not infringe privately owned rights.
■
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