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Resources, Conservation & Recycling 133 (2018) 375–384

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Resources, Conservation & Recycling


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Full length article

Element-based optimization of waste ceramic materials and glasses T


recycling

Ichiro Daigoa, , Shin Kiyoharab, Tomoki Okadac,d, Daisaku Okamotoe, Yoshikazu Gotoa
a
Graduate School of Engineering, The University of Tokyo, Japan, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan
b
Institute of Industrial Science, The University of Tokyo, Japan, 4-6-1 Komaba, Meguro, Tokyo 153-8505, Japan
c
School of Engineering, The University of Tokyo, Japan, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan
d
Kobe Steel, Ltd., Japan, 1 Kanazawa-cho, Kakogawa-shi, Hyogo, 675-0137, Japan
e
Kishiyama Co., Ltd., Japan, 1-54, Gamo-higashi-cho, Koshigaya-shi, Saitama, 343-0841, Japan

A R T I C L E I N F O A B S T R A C T

Keywords: Many waste ceramic materials and glasses (CerG) such as glass, concrete, pottery, porcelain, brick, and tiles are
Glass recycling landfilled because they have been recognized to be less conducive to recycling. In this study, to enhance the
Recycling of ceramics recyclability of ceramic materials and glasses, a linear model to minimize natural resource consumption of CerG
Refractories materials production is proposed. The model focuses on elementally based contents of substances in the CerG
Ironmaking slag
materials. The model demonstrates a case for major industrial ceramic materials consisting of eleven oxides:
Sewage sludge
CerG
Al2O3, B2O3, CaO, Fe2O3, K2O, MgO, MnO, Na2O, P2O5, SiO2, and TiO2 in Japan. In addition to the ceramic
materials and glasses within the eleven oxide systems, application of the same natural resources to by-products
or waste materials such as ironmaking slag and sewage sludge molten ash, are included in this analysis. In the
proposed model, for minimizing natural resource consumption to produce the target CerG, linear programming
was employed to assess waste generation and new production of CerG, subject to supply and demand balance
and elemental tolerance ranges of chemical compositions in CerG materials. Two discrepancies were found
between the proposed model and the characteristics of materials or usages of materials. Therefore, in the case
study, several kinds of CerG materials were not applicable in the analysis. Even though costs for recovered
materials restrict economic feasibility for recycling waste CerG, economic aspects were not taken into con-
sideration in the analysis. In addition, impurity contamination during recovery processes restricts recycling of
CerG. If those two factors (which may restrict the current recycling systems) were ignored, around two-thirds of
the current natural resource consumption for CerG could be reduced by promoting recycling in the case of Japan.
Further, new recyclable paths could be found by those analyses such as ironmaking slag for flat glass, glass
bottles, and glass wool; and sewage sludge molten slag for tiles.

1. Introduction et al., 2017). Meanwhile, their raw materials are abundant and prac-
tically inexhaustible; large amounts of waste are generated and dumped
Ceramic materials and glasses (CerG) have been used in natural into landfill sites every year (Du and Tan 2013; Jani and Hogland
forms from ancient times (Ashby 2005) as stone, flint, and pottery. 2014). In addition, greenhouse gas emissions associated with the
Recently, industrial CerG such as porcelain, fused silica, cement, re- mining and transportation of the large amounts of raw materials and
fractories, and soda-lime glass, have been widely used. The CerG and the production of the materials should not be ignored (Jani and
raw materials for these are produced in large amounts (USGS 2017): Hogland 2014). Madivate et al. (1996) revealed mechanisms of the
4.20 billion tonnes of cement, 700 million tonnes of wollastonite, 350 energy requirement in reactions and proposed measures for energy
million tonnes of lime, 56 million tonnes of clays, 53 million tonnes of saving such as using cullets, replacing carbonates in the glass batch
soda ash, and 23 million tonnes of feldspar were produced in the world with corresponding hydroxides, and reducing the melting temperature.
in 2016. On the other hand, their end-of-life materials are hardly re- Therefore, recycling of CerG can effectively contribute to reducing the
covered and recycled, except for concrete recycling for construction amounts of dumping and GHG emissions associated with CerG pro-
aggregates and cullet glass recycling (Jani and Hogland 2014; Santos duction.


Corresponding author.
E-mail address: daigo@material.t.u-tokyo.ac.jp (I. Daigo).

https://doi.org/10.1016/j.resconrec.2017.11.012
Received 11 May 2017; Received in revised form 17 November 2017; Accepted 17 November 2017
Available online 28 November 2017
0921-3449/ © 2017 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/BY/4.0/).
I. Daigo et al. Resources, Conservation & Recycling 133 (2018) 375–384

Recently, new recycling technologies have been studied (Du and metallic aluminium in a glass cullet is strictly prohibited in glass pro-
Tan 2013). Several studies (Matteucci et al., 2002; Tucci and Rambaldi, duction (Wischnat et al., 1993). In reality, the recycling of CerG is re-
2006; Faira and Holanda 2016) introduced the possibility of recycling stricted by chemical composition and by economic feasibility (Federico
waste soda-lime glass for porcelain stoneware tiles. Although the new and Chidiac, 2009). The total cost for liberation, treatment, and
recycling scheme still requires technological modifications to the pro- transportation to provide recyclable waste CerG should not exceed the
cesses and has a tolerable share in feedstocks, waste glass could be used price of raw materials that can be substituted by recycling the waste
as a substitutable raw material for naturally occurring sodic feldspar. CerG. In many cases, the raw materials for CerG are inexpensive, and
Karamanova et al., 2011 introduced new ceramic materials containing CerG producers have rarely exhibited concern about the effects of their
ironmaking slag. As long as ironmaking slag is mixed with Kaoline and depletion in the industry (Ruth and Dell’Anno 1997). We, however,
silica sand at an appropriate portion, the new ceramics have higher focus only on the theoretical possibility of CerG recycling. In other
property than conventional tiles in terms of bending strength and words, the economic feasibility of recycling is not taken into con-
hardness. Badiee et al. (2008) and Teo et al. (2014) introduced re- sideration because future legislation and/or economic conditions may
cycling of steelmaking slag generated at electric arc furnace for ceramic overcome current economic barriers.
tiles with the combination of steelmaking slag, ball clay, feldspar and To numerate the ceramic materials that are widely used at present,
silica. Even though the two studies tried in different batch composi- we investigated materials and applications of raw materials for CerG.
tions, the recycled tiles showed good characteristics. Kikuchi (1998) Major raw materials for CerG were identified from USGS Mineral
demonstrated recycling sewage sludge with incineration ash by vi- Commodity Summaries (US Geological Survey, 2017) as clay, dolomite,
trification resulted in molten slag, into tiles and slag wool. Chen and Lin feldspar, limestone, silica sand and silica rock, soda ash, talc, pyr-
(2009) proposed a new technology of the nano-SiO2 additive for por- ophyllite, and wollastonite. Here, kyanite and related minerals were not
celain clay tile containing incinerated sewage sludge ash, which in- taken into account due to their low consumption, which is less than a
crease replacement ratio of the sewage sludge. Lin et al. (2008) in- million tonnes annually at the global level. Materials and applications
troduced recycling incinerated sewage sludge into the body of glazed of the minerals are listed in the appendix (Table A1), which distin-
tiles. In addition, Zhou et al. (2013) proposed a new recycling process guishes between CerG materials and non-ceramic materials and appli-
for sewage sludge without drying. Many recycling technologies for cations. Some applications of non-ceramic materials can be regarded as
cement and concrete reclaimed from waste glass (container or packa- CerG. The applications of rainmaking and steelmaking generate ir-
ging glass, flat glass, domestic or tableware glass and continuous fila- onmaking slag (also referred to as blast furnace slag) and steelmaking
ment glass fibers) (Rashad 2014), ironmaking slag (Tae et al., 2017), slag, respectively. Those slags also consist of similar compositions to
steelmaking slag (Anastasiou et al., 2014), sewage sludge (Smol et al., CerG materials. The application of water treatment partially generates
2015) and recycled concrete aggregate (Poon and Chan 2007) have sewage sludge, which is treated with drying furnaces and melting fur-
been introduced. As reviewed, those technologies have tried to recycle naces, resulting in molten slag. Ironmaking slag, steelmaking slag and
different waste CerG mainly into tiles, cement and concrete which may sewage sludge molten slag were included in the target materials of this
be tolerant for raw materials. study.
The newly proposed recycling technologies can be implemented due The materials selected above were tabulated, of which the major
to the similarity of chemical compositions between glass and ceramic chemical components are indicated qualitatively in Table 1. Here,
materials (Sikora et al., 2016). To promote the recycling of waste glass materials that have different chemical compositions in each material
and ceramic materials, further new recycling paths are required. From group were distinguished. It was found that many industrial CerG
the viewpoint of chemical composition, new applications of waste materials are made of combinations of similar oxide components.
ceramic materials are expected to be found. In this study, to enhance Theoretical possibilities for CerG recycling are considered by the si-
recycling of waste industrial ceramic and glass materials, a new method milarity of chemical compositions, which can identify new recycling
to find recycling possibilities was proposed on the basis of element-wise schemes. In ceramic materials, there is a material which consists of
contents of oxides in the ceramic materials. other than oxides, such as silicon carbide. For preserving the similarity
of compositions, other CerG materials than oxide-based ones are ex-
2. Model development cluded in this analysis. Even in the list shown in Table 1, friction pro-
ducts, converter slag, and electric arc furnace (EAF) oxidizing slag do
2.1. Oxide-based ceramic materials and glasses (CerG) not consist only of oxides, but also of metals, carbonate, sulfate and/or
sulfide, which should be excluded from this analysis.
Theoretically, ceramic materials and glasses are distinguished be-
cause ceramic materials are crystalline solids and glasses are amor-
2.2. Optimization of recycling
phous solids. Hereafter the recycling of those materials by melting or
sintering was taken into consideration. In the recycling of those mate-
Recycling waste CerG can contribute to reducing the dumping of
rials, crystalline or non-crystalline composition in raw materials is not
waste CerG and the consumption of naturally occurring minerals. We
relevant whereas the chemical compositions are always determinative
optimized a system of waste CerG recycling in terms of minimizing
(Souza et al., 2010; Bernardo et al., 2008; Bernardo et al., 2010). Due to
natural mineral consumption. Linear programming was employed to
the similarity of compositions between ceramic materials and glasses,
optimize the supply-demand between the generation of waste CerG and
they are regarded as the same group of materials (CerG) in this study.
the production of CerG products. The minimization of natural mineral
Industrial CerG are produced from naturally occurring clay and sand
consumption and the maximization of recycled waste CerG could find
and in general consist of metallic and non-metallic oxides. Production
the same optimal supply-demand. In reality, recycling waste CerG is
processes of CerG cannot extract impurities or separate substances.
subject to constraints of chemical composition and mass balance, which
Chemical compositions of CerG products are decided by the fraction of
are imposed on the optimization. The optimization calculation for
raw materials which are converted into a homogeneous liquid (Jani and
natural mineral consumption can be expressed by the following equa-
Hogland 2014; Ruth and Dell’Anno 1997). In practice, when waste
tions.
CerG is recycled to produce new CerG materials, the chemical compo-
sitions of recovered waste CerG have to meet requirements of the target
Minimizing: ∑ ∑ Xij
CerG material. When a substance that should be strictly avoided in a j i∈N
CerG material is contained in a waste CerG, the waste CerG cannot be
recycled as a CerG material (Jani and Hogland 2014). For instance, subject to:

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I. Daigo et al. Resources, Conservation & Recycling 133 (2018) 375–384

Table 1
Chemical compositions of ceramic materials.

Material products and applications Ceramic materials and glasses Major chemical components

Cement Cementa Al2O3, CaO, Fe2O3, MgO, SO3, SiO2


Tiles Tilesb Al2O3, CaO, Fe2O3, K2O, MgO, Na2O, SiO2, TiO2
Sanitaryware Potteryc Al2O3, CaO, Fe2O3, K2O, MgO, Na2O, SiO2, TiO2
Refractory Refractorya Al2O3, CaO, Fe2O3, K2O, MgO, Na2O, SiO2, TiO2
Clay bricks Clay d Al2O3, CaO, Fe2O3, MgO, MnO, K2O, P2O5, SO3, SiO2, TiO2
Pottery Pottery (plateware) e Al2O3, CaO, Fe2O3, K2O, MgO, Na2O, SiO2, TiO2
Friction products Brake pad f Al2O3, BaSO4, CaCO3, Cu, Fe, MgO, K2O6・TiO2, SnS, ZrO2
Glassg Flat glass Al2O3, CaO, MgO, Na2O, SiO2
Bottle glass Al2O3, CaO, Fe2O3, K2O, MgO, Na2O, SiO2
Glass fiber Al2O3, B2O3, CaO, Fe2O3, K2O, MgO, MnO, Na2O, SiO2
Glass woolh Al2O3, B2O3, CaO, Fe2O3, K2O, MgO, P2O5, Na2O, SiO2
Substrates glass Al2O3, B2O3, CaO, Fe2O3, MgO, MnO, SiO2
Fluorescent glass Al2O3, B2O3, CaO, Fe2O3, K2O, MgO, Na2O, SiO2
Ironmakingi Ironmaking slag Al2O3, CaO, MgO, MnO, SiO2
Steelmakingi Converter slag Al2O3, CaO, Fe, Fe2O3, MgO, MnO, P2O5, SiO2
EAF Oxidizing slag Al2O3, CaO, Fe, Fe2O3, MgO, MnO, SiO2
EAF Reducing slag Al2O3, CaO, Fe2O, Fe2O3, MgO, MnO, SiO2
Water treatment Sewage sludge molten slagj Al2O3, CaO, Fe2O3, P2O5, SiO2

EAF: electric arc furnace.


a
The Ceramic Society of Japan (2002).
b
Matteucci et al. (2002).
c
Tarhan et al. (2017).
d
Eliche-Quesada et al. (2017).
e
Wu et al. (2013).
f
Menapace et al. (2017).
g
Yamane et al. (2010).
h
National Research Council (2000).
i
Nippon Slag Association (2017).
j
Kanchanapiya et al. (2006).

m
c jk ≤ ∑ bik Xij / ∑ Xij analyzed using the model. When it is developed for a large number of
i i (1) oxides, various kinds of CerG can be taken into account. Data used for
the model, however, are more complicated and less available.
c jkM ≥ ∑ bik Xij / ∑ Xij
(2) Therefore, the target oxides should cover adequate kinds of oxides
i i
concerning the CerG.
∑ Xij = Pj The conditions of tolerance for chemical compositions are discussed
i (3) from the viewpoint of materials science. When more than one pure
component is present, compositions of components, temperatures, and
∑ Xij ≤ Gi pressures decide the phase of the mixture at equilibrium. For instance,
j (4)
in the Na2O-SiO2 system, even at ordinary temperatures and pressures,
where, Xij stands for the amount of raw material i consumed in the there are three kinds of compound: sodium orthosilicate (Na4SiO4),
production of material j, N is a set of natural resources within the set of sodium metasilicate (Na2SiO3), and sodium disilicate (Na2Si2O5); there
raw materials, bik stands for the chemical composition of oxide k in raw are four possible phases as combinations of those compounds and two
material i, cM m
jk and cjk stand for lower and upper tolerance levels of the pure oxides (Kahlenberg 2010). Ternary systems become more complex
chemical composition of oxide k in the produced material j, respec- because they are based on three binary systems. In the CaO–Al2O3–SiO2
tively, Pj stands for demand of the produced material j, and Gi stand for system, there are many more kinds of compounds: anorthite,
the generation potential of the raw material i (i ∉ N). CaO–Al2O3, CaO–2Al2O3, CaO–6Al2O3, 3CaO–Al2O3, corundum, cris-
Under the inequality constraint (1), for every chemical composition tobalite, gehlenite, hatrurite, mullite, pseudo-wollastanite, rankinite,
of oxide k, the average of raw materials for the production of material j and tridymite (Mao et al., 2006). Because the properties of materials
(the right side) should be larger than the lower bound of tolerance for differ with their phases, the phase boundaries represent tolerance
the chemical composition of oxide k in the production of material j (the ranges. In ternary and higher-arity systems, the boundaries do not show
right side). Under the inequality constraint (2), for every chemical linearity. Consequently, in a mixture of several kinds of oxides, it is
composition of oxide k, the average chemical composition should be hard to apply linear inequality constraints theoretically. Therefore,
smaller than the upper bound, as well. tolerance ranges should be empirically decided in the forms of the
The equality constraint (3) ensures the mass balances for every linear conditions. The empirical conditions are demonstrated by case
product j between the total of raw materials and the corresponding studies in the following sections.
products. The inequality constraint (4) ensures for every raw material i
that the total consumption of raw materials (the left side) should be 3. A case study demonstration
smaller than the generation potential. Under the equality constraint (3),
the total consumption of natural resources and secondary resources is 3.1. Eleven oxide systems in Japan
always same. Therefore, in this optimization model, saving amounts of
natural resource consumption equal to saving amounts of waste mate- The model developed above can be performed for any recycling
rials disposed. system. In this chapter, as a case, we applies the model to Japanese
The proposed optimal model is applicable for any number of oxides CerG recycling system in the year 2012. Through this case study, ef-
indexed as k above. When an optimal model is demonstrated for a small fectiveness and limitations of the proposed model are discussed in the
number of oxides, CerG that contain other target oxides cannot be next chapter.

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I. Daigo et al. Resources, Conservation & Recycling 133 (2018) 375–384

Before preparing data for the analysis, oxides which are taken into reactivity (Seetharaman et al., 2013). As marked in Table 3, several
consideration have to be selected. We focused on eleven oxides (Al2O3, CerG were not taken into consideration due to the reasons above.
B2O3, CaO, Fe2O3, K2O, MgO, MnO, Na2O, P2O5, SiO2, and TiO2) which Checkmarks in the supply side shown in Table 3 are described in 3.3.
CerG materials such as tiles, pottery, refractories, glasses, iron and steel Even with the best available technology, some CerG production
making slags, and sewage sludge molten slag, made with as shown in processes need to strictly avoid impurities that are not included in the
Table 1. Then, the CerG materials that have more than 1% oxide con- eleven oxides. For instance, flat glass production will not tolerate
tent than the eleven oxides were excluded from the analysis. Cement membranes, films, papers, etc. larger than 10 mm, steel larger than
and clay bricks were not involved in the target CerG materials since 1 mm, and any metallic aluminium, copper, or nickel (AGC, 2006).
their chemical compositions include sulfur trioxide. The impurity con- Tolerance for impurities mixed with waste CerG such as metals, varies
tent of 1% was determined as a cutoff to simply demonstrate the ana- among the CerG materials, which is an important factor restricting re-
lysis. In this model, the number of oxides and the cutoff can be arbi- cycling (Wischnat et al., 1993). Therefore, those impurities are re-
trarily selected not to exclude materials which a practitioner intends to garded as a component of CerG beyond the eleven oxides (as a proxy).
analyze. The tolerance and contaminated contents of impurities could not be
And then, the following parameters are required for the optimiza- quantitatively identified. Therefore, the proxy was defined as binary
tion: demand, Pj, tolerance of chemical compositions in the products, data that stands for acceptability of impurities. Even if the binary data
cM m
jk and cjk, supply potentials, Gi, and chemical compositions in waste were used in linear programming, they perform well because they can
CerG, bik. The preparation of these data is described in the following distinguish the tolerance to impurities. The lower bound of every ma-
sections. terial is 0, the upper bounds for some materials that accept mixing
impurities with raw materials are 1, and the upper bounds for other
3.2. Data preparation for CerG production materials are 0. Although the colors of glass bottles are realized by
chemical composition, additives for the colors are not larger than 1%.
On the demand side, the annual production and tolerance of che- Because this study tolerates 1% of other compositions beyond the
mical contents of CerG were investigated. The demands of the target eleven oxides in total, the difference of chemical composition because
CerG materials, Pj, are assumed to be the same as the amounts of of colors was not characterized. Nevertheless, colored glass cullet
production that could be obtained from statistics for 2012, as shown in cannot be consumed for clear glass. Another binary parameter as a
Table 2. proxy for color was added as the thirteenth parameter.
Tolerance ranges of chemical contents in the produced materials, cM From a technological viewpoint, it should be assumed that glass
jk
and cm cullet would not be used for the production of tiles. Especially in the
jk, are rarely obtained. One of reasons was accessibility to the data
because the ranges are not intended to be published. Some settings production of fully vitrified tiles (porcelain stoneware tiles), consuming
relied on empirical knowledge of production experts as indicated in vitrified soda-lime glass cullet results in worse mechanical and tribo-
Table 2. The tolerance ranges of chemical contents may not vary over logical performance than not consuming it due to factors such as in-
time at least the production process or properties of materials are creasing shrinkage, decreasing bulk density, etc. Matteucci et al. (2002)
changed. Although the year for a composition data was not identified, experimentally proved that the tolerable portion of soda-lime cullet in
the data is assumed to be applicable to the year for production, that is, raw materials is less than 5%. In this analysis, the fourteenth compo-
2012. The second reason was difficulty to uniquely identify the range nent added was for the restriction on the usage of glass cullet. Ranges of
due to various different compositions in the products; such as sani- chemical composition for each material are shown in Table 2.
taryware and, plateware (Mommsen et al., 1998 and Wu et al., 2013).
The third reason was definability of the linear rages from the viewpoint 3.3. Data preparation for waste CerG generation
of materials science; such as several kinds of refractories, glass fiber,
substrate glass, ironmaking, steelmaking and water treatment. As On the supply side, the annual generation of waste CerG and their
mentioned before, tolerance ranges for some CerG materials cannot be chemical compositions were investigated. It is generally difficult to
described by linear chemical compositions because they are restricted observe annual generation potentials of waste CerG, Gi, directly, and to
by their properties such as melting temperature, viscosity, and obtain statistical data. Therefore, the generation potential of each

Table 2
Ranges of chemical composition for each produced CerG material. Up: upper boundary, Lo: Lower boundary. Units for substances are percent. Binary data are given for the impurity, Imp.;
the color, Col.; and glass cullet, Cull.

CerG materials SiO2 TiO2 Al2O3 Fe2O3 CaO MgO K2O Na2O MnO P2O5 B2O3 Imp. Col. Cull. Annual production [thousand tonne/year]

Tilesa Up 75.0 N.D. 25.0 N.D. N.D. N.D. 3.8 10.7 N.D. N.D. 0.0 1 1 0 448
Lo 65.0 0.0 4.4 0.0 0.0 0.0 1.9 0.61 0.0 0.0 0.0 0 0 0
b
Flat glass Up 73.0 1.0 2.1 0.12 9.5 5.5 2.0 16.0 0.05 N.D. 0.0 0 0 1 1 101
Lo 67.0 0.0 1.2 0.01 6.5 2.5 0.01 12.0 0.0 0.0 0.0 0 0 0
c
Bottle glass (clear) Up 75.5 1.0 2.2 0.08 12.7 1.6 0.9 14.0 0.05 N.D. 0.0 0 0 1 578
Lo 69.5 0.0 1.4 0.0 9.7 0.0 0.7 12.0 0.0 0.0 0.0 0 0 0
c
Bottle glass (brown) Up 75.6 1.0 2.4 0.31 12 1.7 1.3 14.0 0.06 N.D. 0.0 0 1 1 557
Lo 69.6 0.0 1.6 0.21 9 0.0 1.1 12.0 0.0 0.0 0.0 0 0 0
c
Bottle glass (others) Up 74.9 1.0 2.4 0.2 12.1 1.8 1.4 14.0 0.05 N.D. 0.0 0 1 1 130
Lo 68.9 0.0 1.6 0.1 9.1 0.0 1.2 12.0 0.0 0.0 0.0 0 0 0
b
Glass wool Up 75.6 1.0 2.4 0.31 12.7 5.5 2.0 14.0 0.05 N.D. 25.5 1 0 1 214
Lo 67.0 0.0 1.2 0.0 6.5 0.0 0.0 12.0 0.0 0.0 0.0 0 0 0
b
Fluorescent glass Up 75.7 N.D. 5.6 N.D. 3.0 N.D. 12.0 8.0 N.D. N.D. 25.5 1 0 1 28
Lo 69.7 0.0 1.2 0.0 0.3 0.0 0.5 0.3 0.0 0.0 8.0 0 0 0

N.D.: For these oxides, the upper limit was not decided because these contents do not cause serious effects on material properties at least at low concentrations and because the
compositions do not increase substantially.
a
Private communications with Marumi Toryo Co., Ltd. and CRYSTAL CLAY Corp.
b
Our assumptions confirmed by experts.
c
Private communications with Glass bottle 3R promotion association, Japan.

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I. Daigo et al. Resources, Conservation & Recycling 133 (2018) 375–384

Table 3
List of CerG materials which are excluded from this analysis. Checkmarks indicate reasons for the exclusion from demand side and/or supply side.

Material products and applications Ceramic materials and glasses and Demand side (CerG production) Supply side (waste CerG generation)
applications
Limitations in chemical Composite materials and Dissipative applications
compositions additives

Tiles Tiles ✓
Sanitaryware Pottery ✓ ✓
Refractories Fireclay refractories ✓ ✓
Alumina refractories ✓
Basic refractories ✓ ✓
Zircon refractories ✓ ✓
Castable refractories ✓ ✓
Gunning refractories ✓ ✓
Pottery Pottery (plateware) ✓ ✓
Glass Soda-lime glass (flat glass)
Bottle glass
Glass fiber ✓ ✓
Glass wool ✓
Substrates glass ✓
Fluorescent glass
Ironmaking Ironmaking process ✓
Steelmaking EAF reducing process ✓
Water treatment Water treatment process ✓

Table 4
Chemical compositions for waste CerG. Units for substances are percent. Binary data are given for the impurity, Imp.; the color, Col.; and glass cullet, Cull.

SiO2 TiO2 Al2O3 Fe2O3 CaO MgO K2 O Na2O MnO P2O5 B2O3 Imp. Col. Cull Annual waste generation [thousand tonnes/year]

Waste flat glass a


71.0 0.0 1.7 0.1 8.0 4.0 0.5 14.0 0.0 0.0 0.0 1 0 1 814
Waste glass bottles (clear) b 72.5 0.0 1.8 0.03 11.2 0.1 0.8 13.1 0.0 0.0 0.0 0 0 1 578
Waste glass bottles (brown) b 72.6 0.0 2.0 0.26 10.5 0.2 1.2 13.1 0.01 0.0 0.0 0 1 1 557
Waste glass bottles (others) b 71.9 0.0 2.0 0.15 10.6 0.3 1.3 13.1 0.0 0.0 0.0 0 1 1 130
Waste fluorescent glassc 72.7 0.0 3.1 0.0 1.2 0.0 4.5 4.3 0.0 0.0 14.1 1 0 1 37
Waste substrate glassd 68.6 0.0 16.4 0.0 9.5 5.2 0.0 0.0 0.0 0.0 0.0 1 0 1 44
Waste alumina refractoriese 0.9 0.2 92.7 0.1 0.8 5.0 0.1 0.1 0.0 0.0 0.0 0 0 0 186
Ironmaking slag f 33.8 1.3 13.4 0.4 41.7 7.4 0.31 0.31 0.30 0.10 0.0 0 0 0 24 639
EAF reducing slag g 18.8 0.0 16.5 0.3 55.1 7.3 0.0 0.0 1.0 0.10 0.0 0 0 0 997
Sewage sludge molten slagh 32.0 0.91 15.4 9.50 28.2 2.13 0.90 0.70 0.49 10.8 0.0 0 0 0 5 097
Silica rocki 97.8 0.03 2.0 0.01 0.05 0.05 0.0 0.0 0.0 0.0 0.0 0 0 0
Silica sandi 99.8 0.03 0.04 0.01 0.05 0.05 0.0 0.0 0.0 0.0 0.0 0 0 0
Feldspari 75.2 0.03 14.5 0.23 0.62 0.04 6.08 3.3 0.0 0.0 0.0 0 0 0
Clayi 65.4 0.54 30.2 1.78 0.27 0.4 1.2 0.26 0.0 0.0 0.0 0 0 0
Pyrophyllitei 77.7 0.38 20.3 0.25 0.08 0.13 0.65 0.49 0.0 0.0 0.0 0 0 0
Limestonei 1.02 0.0 0.34 0.17 97.6 0.82 0.0 0.0 0.0 0.02 0.0 0 0 0
Dolomitei 0.67 0.0 0.09 0.08 63.8 35.3 0.0 0.0 0.0 0.04 0.0 0 0 0
Talci 65.9 0.0 0.08 0.07 0.44 33.5 0.0 0.01 0.0 0.0 0.0 0 0 0
Soda ashi 0.0 0.0 0.0 0.0 0.0 0.0 0.0 100 0.0 0.0 0.0 0 0 0
Boraxi 0.0 0.0 0.0 0.0 0.0 0.0 0.0 30.8 0.0 0.0 69.2 0 0 0

a
Private communication.
b
The Ceramic Society of Japan (2002).
c
Yamane et al. (2010).
d
Kawaguchi and Miwa (2012) and Tokunaga et al. (2013).ePrivate communication.
f
Division of Basic research on Slag Utilization (1979), Katayama et al. (2017), Eguchi et al. (2014) and Igarashi et al. (2012).
g
Nippon Slag Association (2017).
h
Ozaki (2011) and Komatsuzaki et al. (2006).
i
Kogyo Gijutsu Rengo Kaigi Yogyo Rengo Bukai (1992).

material in the CerG was estimated by dynamic material flow analysis, statistics. In Table 4, the annual generation of waste CerG for the year
which was employed in previous material flow analysis studies (Müller 2012, Gi, is shown.
et al., 2014 and Daigo et al., 2015) (see S-1 in Supporting Information Chemical compositions of the generated materials, bik, were also
for details). For applications that are not used as parts of finished estimated. The limitations considered in the supply side are different
products, the annual generation of waste CerG from those applications from those on the demand side. Four different applications of CerG
was estimated by statistics and/or technical information of those pro- were distinguished basically by the forms when they are recovered and
cesses. Waste aluminium refractories generated from steelmakers were it was individually considered whether those applications can be taken
taken into account. The annual generation was estimated by generation into consideration. First, some kinds of CerG materials are used as
amounts per unit of crude steel production and the total production of mono-materials and assembled in final products. In those applications
crude steel in Japan. The annual generation of ironmking slag, EAF of CerG, the composition of CerG materials when they are disused does
steelmaking slag, and sewage sludge molten slag were obtained from not change from the initial composition. In the actual waste

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I. Daigo et al. Resources, Conservation & Recycling 133 (2018) 375–384

management processes, however, some of those CerG are recovered the combination of raw materials using the average compositions of
with other materials as impurities because they are used with other each raw material given in Table 4 meet the corresponding tolerance
materials in the final products (Wischnat et al., 1993; Matteucci et al., ranges given in Table 2. The set of raw materials in Table 5 is likely to
2002). Singularly used CerG materials are taken into consideration and represent the current situation in Japan. The chemical compositions
the twelfth element was used as a proxy for impurity, as introduced in prepared in this section were also validated. On the basis of those data,
the previous sub-section. Second, some kinds of CerG materials are used optimal analyses are conducted in the next section.
as composite materials and assembled in final products. It is practically
difficult to liberate those CerG materials in end-of-life products from the 3.5. Optimization
embedded materials in the composite materials. Those CerG materials
used as part of composite materials were not considered as supply of As described above, production of the CerG materials (demand side)
waste CerG. For instance, glass wool (short glass fiber), which is used and the waste CerG (supply side) were selected and used for optimi-
for insulation materials with resins is unlikely to be liberated. Third, zation. The result of optimization analysis was obtained as Table 6,
dissipative applications of CerG cannot discharge any waste CerG. For which indicated natural resource consumption reduction of 469 thou-
instance, castable refractories used on inner walls of furnaces are dis- sand tonnes. Glass cullet was found to have excellent recycling poten-
sipative during use. Fourth, some kinds of CerG inherently have addi- tial. Although impurities and colors restrict CerG recycling, recycling
tional processes that may change chemical compositions. For instance, could be enhanced. Therefore, one of the factors restricting current
pottery (excluding porcelain) is a porous form of clay in which a thin CerG recycling could be economic feasibility. From the viewpoint of
vitrified layer is required on the surface (glaze) to hold liquid. Even for chemical composition, ironmaking slag, EAF reduction slag, and sewage
porcelain, glaze can serve as a design on the surface. Although the sludge molten slag are suitable for flat glass, glass wool, and tiles, re-
composition of the glaze is similar to CerG, various kinds of composi- spectively. Clay and limestone originally used for tiles could be com-
tions make it difficult to decide the average chemical compositions of pletely replaced with a combination of sewage sludge molten slag and
pottery. These CerG are not the same as composite materials, but in the feldspar. It was considered that sewage sludge molten slag could sub-
context of this analysis, this fourth category is the same as the second stitute limestone in terms of supplying calcia, and feldspar could
category, which was not taken into account. The selection of CerG compensate silica and alumina originally supplied by clay. On average,
materials for supply side is summarized in Table 3. the natural resource consumed for the production of tiles could be re-
Chemical compositions of the selected CerG materials were obtained duced by at least 10 thousand tonnes. With regard to sewage sludge,
as shown in Table 4. The compositions of those industrial materials may various options have been investigated that allow recycling and bene-
not vary over time. Therefore, all collected data is assumed to be ap- ficial resource recovery, in which reclaimed tile is one of major options
plicable to the year for generation, that is, 2012. In addition, chemical (Donatello and Cheeseman, 2013). Whereas, neither flat glass con-
compositions of natural resources were also surveyed. The average taining ironmaking slag nor glass wool containing steelmaking slag
chemical compositions for natural resources are shown in Table 4, have been studied so much, that is, those recycling paths which sub-
which is used for the analysis, though in reality natural resources de- stantially contribute recycling of CerG could be found by this analysis.
rived from a specific site are consumed according to their chemical
compositions, which vary between different mineral localities. Wol- 3.6. Scenario analysis
lastonite was eliminated from the natural resources listed in Table A1
because it is commonly obtained in North America, the Nordic coun- Recycling could be enhanced, if factors which severely restrict their
tries, and south Europe, but is not common in Japan (US Geological recycling would be relaxed. Here, two restrictions are selected to ad-
Survey, 2017). Borax was added to fulfill the boron trioxide require- dress the enhancement of recycling: the contamination of impurities in
ment for fluorescent glass. waste CerG materials and the consumption of glass cullet in the pro-
duction of tiles. Optimization analyses were conducted with and
3.4. Validation of data without those restrictions as scenarios in this section.
From the technological point of view, innovative glass-ceramic tiles
Data for the supply side and the demand side were defined as the whose mechanical and tribological performance become worse by
chemical compositions of waste CerG and the tolerance range of CerG consuming glass cullet are appropriately addressed in the processes, can
materials, respectively. Before conducting the optimization, the con- consume 60% of glass cullet and have similar properties to conven-
sistency of data was validated. Ideally, when the chemical compositions tional porcelain stoneware tiles (Bernardo et al., 2008). In the first
of raw materials for a CerG material are averaged, it should equal the scenario, the production of tiles consumes up to 60% of glass cullet
investigated value of the CerG material. The investigated chemical even if the cullet is recovered with impurities. The result of this sce-
compositions for natural resources would be different from those of nario showed that 155 thousand tonnes of natural resource con-
natural resources that are actually consumed for those CerG materials sumption—which is approximately 10% of the current con-
because of the different localities of minerals. Therefore, it is hard to sumption—could be reduced from the result shown in 3.5. Glass cullet
demonstrate the average compositions using those chemical composi- recovered from flat glass and glass bottles could be consumed for tiles,
tions averaged from different localities of minerals. In addition, there is resulting in eliminating silica sand consumption. Even in optimal re-
no statistical data of raw materials for each CerG after year 2002 in cycling under the current restriction, the production of tiles could
Japan. However, at least a chemical composition of a combination of consume sewage sludge molten slag in half of the raw materials.
raw materials has to fulfill the tolerance range of materials introduced Therefore, additional recycling potentials are limited for tiles. The op-
in the optimization as an inequality constraint. timized recycling flows not only for this scenario but also for following
Several actual conditions were obtained as follows: the portion of scenarios are shown in Fig. 2. In addition, the figures in the form of
natural resources and secondary resources for some CerG materials matrix indicating the complete combinations of waste materials and
during years 1997–2001 (the latest five years); the total consumption of materials production are shown in the Supporting Information as well.
glass cullet for flat glass, glass bottles, and glass wool; the share of raw Second, the mixing of impurities was ignored. It means that the
materials for glass bottles which were provided by industry; kinds of chemical contents of waste CerG are the same as those of produced
natural resources used as raw materials for glass wool; and the fact that CerG. In this analysis, the usability of glass cullet would be improved
glass fiber never use waste CerG. Under these conditions, the combi- because impurities are not contaminated. However, the glass cullet is
nation of raw materials for the CerG materials shown in Table 5 is not allowed to be consumed in the production of tiles. The result of this
approved because the weighted averages of chemical compositions in scenario showed that 1.04 million tonnes of natural resource

380
I. Daigo et al. Resources, Conservation & Recycling 133 (2018) 375–384

Table 5
The current combination of raw materials for CerG materials. Rows indicate generation of waste CerG and column indicate production of CerG materials. The total consumption of each
waste CerG is shown in the last column. Units are thousand tonnes.

Tiles Flat glass Glass bottles (clear) Glass bottles (brown) Glass bottles (others) Glass wool Fluorescent glass Total consumption

Waste flat glass 0 0 0 0 0 44 0 44


Waste glass bottles (clear) 0 0 421 0 0 144 0 565
Waste glass bottles (brown) 0 0 0 406 95 0 0 501
Waste glass bottles (others) 0 0 0 0 0 0 0 0
Silica rock 0 172 0 89 11 14 0 286
silica sand 88 404 106 1 8 2 19 628
Feldspar 110 37 12 28 6 3 3 199
Clay 200 0 0 0 0 0 0 200
Limestone 50 16 5 2 1 3 1 77
Dolomite 0 84 9 17 5 0 0 114
Soda ash 0 108 25 15 5 3 0 155
Borax 0 0 0 0 0 0 6 6

Table 6
Summary of minimal natural resource consumption under the four conditions. Units are thousand tonnes. The conditions are corresponding to the number of figures.

Fig. 1 Fig. 2 (a) Fig. 2 (b) Fig. 2 (c)

Impurities in glass cullet are contaminated. Yes Yes No No


Glass cullet for the production of tiles is accepted. No Up to 60% No Up to 60%
The total consumption of natural resources 1196 1041 624 588
Silica sand and rock 877 730 457 421
Feldspar 114 105 112 112
Clay 0 0 0 0
Pyrophyllite 0 0 0 0
Limestone 0 0 0 0
Dolomite 0 0 0 0
Talc 46 46 0 0
Soda ash 157 157 28 28
Borax 3 3 27 27

consumption—which is around two thirds of the current consumption improve the recycling of CerG, especially of glasses, to a large extent.
for those CerG productions—could be reduced from the current con- Impurities that are mixed in the generated waste flat glass are con-
dition. As compared with the result shown in 3.5, another 572 thousand sumed by glass wool. In this scenario, instead of waste flat glass, glass
tonnes of natural resource—which is around one third of the current wool consumed waste fluorescent glass and ironmaking slag. At the
consumption—could be reduced. Due to pure liberation of waste flat same time, the total consumption of silica sand for glass wool increased.
glass, a large portion of waste flat glass could be used for the same It should be noted that a part of the reduction in silica sand con-
material, flat glass. At the same time, the consumption of silica sand sumption for flat glass was offset by the increase of consumption for
was substantially reduced. The liberation of waste flat glass could glass wool.

Fig. 1. The results of optimization analysis. Generation of waste CerG and


production of CerG materials are indicated on the left and right sides,
respectively.

381
I. Daigo et al. Resources, Conservation & Recycling 133 (2018) 375–384

Fig. 2. The results of optimization analysis for sce-


narios (a) under the condition that the production of
tiles permitted consuming glass cullet up to 60%
even if the cullet is recovered with impurities, (b)
under the condition that the contamination of im-
purities was ignored and that the glass cullet is not
allowed to be consumed in the production of tiles,
and (c)under the condition that glass cullet can be
used for tiles up to 60% and does not contain im-
purities. Generation of waste CerG and production of
CerG materials are indicated on the left and right
sides, respectively.

In the last scenario, glass cullet can be used for the production of the number of target substances. However, due to characteristics of
tiles up to 60% and does not contain impurities. The result of the op- waste management during which these cases take place, contents of
timization analysis indicated that natural resource consumption could impurities or portions of colors in cullet vary according to conditions.
not be reduced from the scenario in which glass cullet cannot be con- Empirically, every batch of waste CerG cannot be investigated to
sumed in the production of tiles because all of the recovered waste flat identify the compositions of them. Therefore, proxies used in the case
glass, waste glass bottles, and fluorescent glass could be recycled even study are beneficial.
in the former scenario. Permission for the cullet could additionally use The proposed model is applicable to other recycling systems at a
only approximately 40 thousand tonnes of waste substrate glass that factory level. For instance, when different kinds of waste CerG are
could not be recycled in the former scenario. treated in a factory, the model can propose recycling ways to minimize
Results of the optimization under the conditions are summarized in final disposals. On the other hand, a conceivable difficulty to apply this
Table 6. The current natural resource consumption of CerG produced is model is data availability. The data preparation can become easier
1 665 thousand tonnes. Even if conditions would not change from the because selection of target materials, the number of oxides for analysis,
current condition, around one third of the natural resource consump- the threshold of a cutoff, and introduction of proxies are flexible.
tion of CerG could be reduced. This result can be regarded as the base Oxide-based ceramic materials and glasses are defined as CerG and
condition without economic feasibility. Other conditions explored the regarded as a group of materials in the same system of recycling.
significance of two physical restrictions. The mixing of impurity in glass Although materials in the group were selected on the basis of chemical
cullet would reduce one third of the natural resource consumption. The compositions in Chapter 2, several CerG materials have to be excluded
permission for using cullet in tiles would not significantly enhance re- from the analysis in the case study, which could be limitations of our
cycling rates. The difference between those impacts is caused by the proposed model. One of them is characteristics of CerG which are not
total production of glasses and tiles. At least in Japan, the production of clearly related to chemical compositions. To overcome the limitation,
glass is larger than tiles. Lastly, though saving amounts of natural re- developing non-linear model, clarifying the relations, or approximation
source consumption were discussed, note that the same to saving in linear conditions are required. Second factor is a variety of chemical
amounts of natural resource consumption can be saved to dispose waste compositions in the same material. For the discussion on recycling, a
CerG materials at the same time in this optimization model. classification by chemical compositions is preferable. The third factor is
a combination with other substances in the final form of materials. The
4. Discussions fourth factor is recoverability of waste CerG. Those limitations could be
avoided, if waste CerG would be recovered and separated from other
The developed model for optimization was applied to a case study. materials. In reality, the cost of recovery and separation may exceed
In the case, however, several constraint conditions in recycling which economically feasible level. One of the most significant limitations in
could not be quantified in chemical composition were discovered. To the proposed model is that economic aspects were not taken into con-
take these conditions into account, binary data were defined as proxies sideration. In the case study, the possibility of recovery and liberation
besides the eleven oxides. In theory, impurities contaminated in end-of- was considered, which may be restricted by economic reasons.
life treatment and mixtures of different colored glass cullet could be Economic factors in recycling should be taken into consideration in
expressed in the form of chemical compositions if we would increase further studies.

382
I. Daigo et al. Resources, Conservation & Recycling 133 (2018) 375–384

Legislative measures are often enforced for promotion of recycling like this analysis can convey messages for the technological develop-
to overcome the restrictions caused by economic feasibility, such as ment and further enhancement of recycling.
Directive 2012/19/EU on waste electrical and electronic equipment The data prepared for the proposed model were successfully vali-
(Favot et al., 2016). Due to the absence of the economic aspects, the dated by realizing the current situation under the constraint conditions.
results obtained in the case study can suggest new legislative measures Results obtained by the proposed optimization model indicate the
including regulatory, economic, informational and organizational in- possibilities of a new recycling scheme: waste fluorescent glass for glass
struments (Rennings et al., 1999). The results indicated that there are wool; ironmaking slag for flat glass, glass bottles, and glass wool; EAF
relatively large amounts of recycling potentials in sewage sludge reduction slag for glass wool; and sewage sludge molten slag for tiles.
molten slag for tiles and ironmaking slag for flat glass. Whilst a cutoff Several theoretically possible new ways of recycling could be identified,
was 1% of chemical compositions in the analysis, specific substances as far as the economic feasibility and contamination of impurities were
are prohibited even less than 1% in flat glass (AGC, 2006). Even though ignored. Basically, many natural resources for ceramic materials and
the results suggested the new possibile recycling paths, further in- glasses are not expensive, i.e., the cost of recovering and liberating
vestigation is required to realize the recycling. We believe that the waste ceramic materials and glasses should not exceed the cost of
providing the possibilities as new recycling paths is the first step to natural resources. However, transportation costs for recovered mate-
promote recycling. rials are generally not economically feasible. Besides ignoring the
The CerG are industrial materials which are produced in similar economic feasibility, if waste glasses are liberated without impurities,
compositions even outside Japan. That is to say, the possibilities for around two thirds of the natural resource consumption in Japan for
new recycling schemes are applicable not only for Japan but also for ceramic materials and glasses can be reduced by promoting recycling.
other counties. But, as mentioned before, barriers in reality should be Recycling of waste ceramic materials and glasses would then be twice
investigated after conducting the proposed optimization, which may the current rate of recycling. These results let us conclude that those
differ among countries because economic conditions and regulations two factors that may restrict the current recycling systems should be
are not the same. resolved.

5. Conclusions
Acknowledgements
A linear model for the optimization of ceramic material and glass
recycling was proposed. Through the case study, we found that the most This work was supported by JSPS KAKENHI Grant Numbers
significant discrepancy between the model and available data is toler- 15H02860, 15H01750 and 26281056 and Environmental Economics
ance ranges of chemical contents in the produced materials. Therefore, and Policy Studies (The Third term) of the Ministry of the Environment,
in the case studies, many kinds of ceramic materials were not applicable Japan. The authors are grateful to So Kato at the Glass Recycling
on the demand side as target materials in the analysis. However, at least Committee of Japan; Shigeaki Moritani and former staffs at Flat glass
for finding a possibility for promoting recycling, roughly approximated manufacturers association of Japan; Tomomichi Yuki and Ken
conditions for the analysis are adequate. In order to extract more cer- Mineshige at Glass bottle 3R promotion association, Japan; Makoto
tain messages from the analysis, experiments to clarify the tolerance Segami at Electric Glass Industry Association of Japan; Shigeki
ranges for each material could contribute to that. Experiments not only Yoshinaga at Japan Glass Bottel Association; Toru Kudo at AGC Asahi
for higher performance of materials or higher efficiency of production Glass; Katsuya Kitayama at CRYSTAL CLAY Corp.; Kengo Ogawa at
but also for acceptance of secondary resources to provide further Marumi Toryo Co., Ltd.; Hidehiro Kuwatori, Dr. Tadashi Ikemoto, and
technological information applicable to those analyses are required Yuichi Kato at Nippon Steel & Sumitomo Metal Corporation; and
towards a sustainable society. At the same time, systemic approaches Kaneyuki Inoko and Yozo Shimizu at Donico Inter Co., Ltd.

Appendix A

Table A1
Ceramic material products, non-ceramic material products and other applications of major raw materials for glass and ceramic materials.

Minerals Materials and applications

Ceramic materials and glasses Non-ceramic materials and applications

a
Clays Bricks; cement; tiles; sanitaryware; Absorbents; drilling mud; foundry sand bond; heavy clay products; iron ore pelletizing; lightweight
refractory; aggregate; paper
Dolomite Refractory Agricultural; chemical; construction; environmental; industrial applications
Feldspar Ceramic tile; glass; pottery
Limestone Ironmaking; steelmaking; water treatment; construction; flue gas desulfurization; mining; paper and
pulp; precipitated calcium carbonate
Silica sand and Silica rock Cement; glass Sand for casting; silicon; additive in the production of foods
Soda ash Glass Water treatment; chemicals; distributors; flue gas desulfurization; pulp and paper; soap and
detergents
Talc and pyrophyllite Ceramics; roofing Cosmetics; paint; paper; plastics; rubber
Wallastonite Concrete; friction products; glass; Elastomer compounds; flux and conditioner for metallurgical processes; paint; thermoplastic and
sanitaryware; tiles thermoset resins

a
Including ball clay, bentonite, common clay, fire clay, fuller’s earth and kaolin.

383
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Appendix B. Supporting information

Supplementary data associated with this article can be found, in the online version, at http://dx.doi.org/10.1016/j.resconrec.2017.11.012.

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