Continuous flow pyrolysis of virgin and waste polyolefins: a comparative study, process optimization and product characterization
Received date: 20 Nov 2023
Accepted date: 08 Feb 2024
Copyright
Under optimal process conditions, pyrolysis of polyolefins can yield ca. 90 wt % of liquid product, i.e., combination of light oil fraction and heavier wax. In this work, the experimental findings reported in a selected group of publications concerning the non-catalytic pyrolysis of polyolefins were collected, reviewed, and compared with the ones obtained in a continuously operated bench-scale pyrolysis reactor. Optimized process parameters were used for the pyrolysis of waste and virgin counterparts of high-density polyethylene, low-density polyethylene, polypropylene and a defined mixture of those (i.e., 25:25:50 wt %, respectively). To mitigate temperature drops and enhance heat transfer, an increased feed intake is employed to create a hot melt plastic pool. With 1.5 g·min–1 feed intake, 1.1 L·min–1 nitrogen flow rate, and a moderate pyrolysis temperature of 450 °C, the formation of light hydrocarbons was favored, while wax formation was limited for polypropylene-rich mixtures. Pyrolysis of virgin plastics yielded more liquid (maximum 73.3 wt %) than that of waste plastics (maximum 66 wt %). Blending polyethylenes with polypropylene favored the production of liquids and increased the formation of gasoline-range hydrocarbons. Gas products were mainly composed of C3 hydrocarbons, and no hydrogen production was detected due to moderate pyrolysis temperature.
Key words: waste plastics; polyolefins; chemical recycling; pyrolysis; alternative fuels; waste-to-energy
Ecrin Ekici , Güray Yildiz , Magdalena Joka Yildiz , Monika Kalinowska , Erol Şeker , Jiawei Wang . Continuous flow pyrolysis of virgin and waste polyolefins: a comparative study, process optimization and product characterization[J]. Frontiers of Chemical Science and Engineering, 2024 , 18(6) : 70 . DOI: 10.1007/s11705-024-2429-x
1 |
Abdy C , Zhang Y , Wang J , Yang Y , Artamendi I , Allen B . Pyrolysis of polyolefin plastic waste and potential applications in asphalt road construction: a technical review. Resources, Conservation and Recycling, 2022, 180: 106213
|
2 |
Salaudeen S A , Al-Salem S M , Sharma S , Dutta A . Pyrolysis of high-density polyethylene in a fluidized bed reactor: pyro-wax and gas analysis. Industrial & Engineering Chemistry Research, 2021, 60(50): 18283–18292
|
3 |
Elordi G , Olazar M , Lopez G , Artetxe M , Bilbao J . Product yields and compositions in the continuous pyrolysis of high-density polyethylene in a conical spouted bed reactor. Industrial & Engineering Chemistry Research, 2011, 50(11): 6650–6659
|
4 |
Miandad R , Barakat M A , Aburiazaiza A S , Rehan M , Nizami A S . Catalytic pyrolysis of plastic waste: a review. Process Safety and Environmental Protection, 2016, 102: 822–838
|
5 |
Dai L , Zhou N , Lv Y , Cheng Y , Wang Y , Liu Y , Cobb K , Chen P , Lei H , Ruan R . Pyrolysis technology for plastic waste recycling: a state-of-the-art review. Progress in Energy and Combustion Science, 2022, 93: 101021
|
6 |
Gabbar H A , Aboughaly M . Conceptual process design, energy and economic analysis of solid waste to hydrocarbon fuels via thermochemical processes. Processes, 2021, 9(12): 2149
|
7 |
Zabaniotou A , Vaskalis I . Economic assessment of polypropylene waste (PP) pyrolysis in circular economy and industrial symbiosis. Energies, 2023, 16(2): 593
|
8 |
Jin Z , Chen D , Yin L , Hu Y , Zhu H , Hong L . Molten waste plastic pyrolysis in a vertical falling film reactor and the influence of temperature on the pyrolysis products. Chinese Journal of Chemical Engineering, 2018, 26(2): 400–406
|
9 |
Park K B , Jeong Y S , Kim J S . Activator-assisted pyrolysis of polypropylene. Applied Energy, 2019, 253: 113558
|
10 |
YangR XJanKChenC TChenW TWuK C. Thermochemical conversion of plastic waste into fuels, chemicals, and value-added materials: a critical review and outlooks. ChemSusChem. 2022, 8;15(11): e202200171
|
11 |
Jubinville D , Esmizadeh E , Saikrishnan S , Tzoganakis C , Mekonnen T . A comprehensive review of global production and recycling methods of polyolefin (PO) based products and their post-recycling applications. Sustainable Materials and Technologies, 2020, 25: e00188
|
12 |
Kumagai S , Nakatani J , Saito Y , Fukushima Y , Yoshioka T . Latest trends and challenges in feedstock recycling of polyolefinic plastics. Journal of the Japan Petroleum Institute, 2020, 63(6): 345–364
|
13 |
Butler E , Devlin G , McDonnell K . Waste polyolefins to liquid fuels via pyrolysis: review of commercial state-of-the-art and recent laboratory research. Waste and Biomass Valorization, 2011, 2(3): 227–255
|
14 |
Mertinkat J , Kirsten A , Predel M , Kaminsky W . Cracking catalysts used as fluidized bed material in the Hamburg pyrolysis process. Journal of Analytical and Applied Pyrolysis, 1999, 49(1): 87–95
|
15 |
Miller S , Shah N , Huffman G P . Conversion of waste plastic to lubricating base oil. Energy Fuels, 2005, 19(4): 1580–1586
|
16 |
Kodera Y , Ishihara Y , Kuroki T . Novel process for recycling waste plastics to fuel gas using a moving-bed reactor. Energy and Fuels, 2006, 20(1): 155–158
|
17 |
Kaminsky W . Thermal recycling of polymers. Journal of Analytical and Applied Pyrolysis, 1985, 8(C): 439–448
|
18 |
Kaminsky W . Recycling of polymeric materials by pyrolysis. Makromolekulare Chemie. Macromolecular Symposia, 1991, 48–49(1): 381–393
|
19 |
Milne B J , Behie L A , Berruti F . Recycling of waste plastics by ultrapyrolysis using an internally circulating fluidized bed reactor. Journal of Analytical and Applied Pyrolysis, 1999, 51(1): 157–166
|
20 |
Hernández M del R , Gómez A , García Á N , Agulló J , Marcilla A . Effect of the temperature in the nature and extension of the primary and secondary reactions in the thermal and HZSM-5 catalytic pyrolysis of HDPE. Applied Catalysis A: General, 2007, 317(2): 183–194
|
21 |
Kusenberg M , Eschenbacher A , Djokic M R , Zayoud A , Ragaert K , De Meester S , Van Geem K M . Opportunities and challenges for the application of post-consumer plastic waste pyrolysis oils as steam cracker feedstocks: to decontaminate or not to decontaminate?. Waste Management, 2022, 138: 83–115
|
22 |
Belbessai S , Azara A , Abatzoglou N . Recent advances in the decontamination and upgrading of waste plastic pyrolysis products: an overview. Processes, 2022, 10(4): 733
|
23 |
Kusenberg M , Eschenbacher A , Delva L , De Meester S , Delikonstantis E , Stefanidis G D , Ragaert K , Van Geem K M . Towards high-quality petrochemical feedstocks from mixed plastic packaging waste via advanced recycling: the past, present and future. Fuel Processing Technology, 2022, 238: 107474
|
24 |
Aguado J , Serrano D P , Escola J M , Garagorri E . Catalytic conversion of low-density polyethylene using a continuous screw kiln reactor. Catalysis Today, 2002, 75(1–4): 257–262
|
25 |
Arabiourrutia M , Elordi G , Lopez G , Borsella E , Bilbao J , Olazar M . Characterization of the waxes obtained by the pyrolysis of polyolefin plastics in a conical spouted bed reactor. Journal of Analytical and Applied Pyrolysis, 2012, 94: 230–237
|
26 |
ArabiourrutiaMElordiGOlazarMBilbaoJ. Pyrolysis of polyolefins in a conical spouted bed reactor: a way to obtain valuable products. Pyrolysis. Rijeka: INTECH, 2017, 285–304
|
27 |
Berrueco C , Mastral E J , Esperanza E , Ceamanos J . Production of waxes and tars from the continuous pyrolysis of high density polyethylene. Influence of operation variables. Energy & Fuels, 2002, 16(5): 1148–1153
|
28 |
Mastral F J , Esperanza E , García P , Juste M . Pyrolysis of high-density polyethylene in a fluidised bed reactor. Influence of the temperature and residence time. Journal of Analytical and Applied Pyrolysis, 2002, 63(1): 1–15
|
29 |
Mastral F J , Esperanza E , Berrueco C , Juste M , Ceamanos J . Fluidized bed thermal degradation products of HDPE in an inert atmosphere and in air-nitrogen mixtures. Journal of Analytical and Applied Pyrolysis, 2003, 70(1): 1–17
|
30 |
Mastral J F , Berrueco C , Ceamanos J . Pyrolysis of high-density polyethylene in free-fall reactors in series. Energy & Fuels, 2006, 20(4): 1365–1371
|
31 |
Mastral J F , Berrueco C , Ceamanos J . Modelling of the pyrolysis of high density polyethylene. Journal of Analytical and Applied Pyrolysis, 2007, 79(1–2): 313–322
|
32 |
WilliamsP TWilliamsE A. Fluidised bed pyrolysis of low density polyethylene to produce petrochemical feedstock. Journal of Analytical and Applied Pyrolysis, 1999, 51(1): 107–126
|
33 |
Zhao D , Wang X , Miller J B , Huber G W . The chemistry and kinetics of polyethylene pyrolysis: a process to produce fuels and chemicals. ChemSusChem, 2020, 13(7): 1764–1774
|
34 |
ArtetxeMLopezGAmutioMElordiGBilbaoJOlazarM. Light olefins from HDPE cracking in a two-step thermal and catalytic process. Chemical Engineering Journal, 2012, 207–208: 27–34
|
35 |
Artetxe M , Lopez G , Amutio M , Elordi G , Bilbao J , Olazar M . Cracking of high density polyethylene pyrolysis waxes on HZSM-5 catalysts of different acidity. Industrial & Engineering Chemistry Research, 2013, 52(31): 10637–10645
|
36 |
Auxilio A R , Choo W L , Kohli I , Chakravartula Srivatsa S , Bhattacharya S . An experimental study on thermo-catalytic pyrolysis of plastic waste using a continuous pyrolyser. Waste Management, 2017, 67: 143–154
|
37 |
Borsella E , Aguado R , De Stefanis A , Olazar M . Comparison of catalytic performance of an iron-alumina pillared montmorillonite and HZSM-5 zeolite on a spouted bed reactor. Journal of Analytical and Applied Pyrolysis, 2018, 130: 320–331
|
38 |
Abbas-Abadi M S , Zayoud A , Kusenberg M , Roosen M , Vermeire F , Yazdani P , Van Waeyenberg J , Eschenbacher A , Hernandez F J A , Kuzmanović M .
|
39 |
Ainali N M , Bikiaris D N , Lambropoulou D A . Aging effects on low- and high-density polyethylene, polypropylene and polystyrene under UV irradiation: an insight into decomposition mechanism by Py-GC/MS for microplastic analysis. Journal of Analytical and Applied Pyrolysis, 2021, 158: 105207
|
40 |
Frączak D , Fabiś G , Orlińska B . Influence of the feedstock on the process parameters, product composition and pilot-scale cracking of plastics. Material, 2021, 14(11): 3094
|
41 |
Walendziewski J . Continuous flow cracking of waste plastics. Fuel Processing Technology, 2005, 86(12–13): 1265–1278
|
42 |
Predel M , Kaminsky W . Pyrolysis of mixed polyolefins in a fluidized-bed reactor and on a pyro-GC/MS to yield aliphatic waxes. Polymer Degradation & Stability, 2000, 70(3): 373–385
|
43 |
Donaj P J , Kaminsky W , Buzeto F , Yang W . Pyrolysis of polyolefins for increasing the yield of monomers’ recovery. Waste Management, 2012, 32(5): 840–846
|
44 |
Miskolczi N , Wu C , Williams P T . Fuels by waste plastics using activated carbon, MCM-41, HZSM-5 and their mixture. MATEC Web of Conferences, 2016, 49: 1–6
|
45 |
Westerhout R W J , Waanders J , Kuipers J A M , Van Swaaij W P M . Recycling of polyethene and polypropene in a novel bench-scale rotating cone reactor by high-temperature pyrolysis. Industrial & Engineering Chemistry Research, 1998, 37(6): 2293–2300
|
46 |
Dubdub I , Al-Yaari M . Pyrolysis of mixed plastic waste: I. Kinetic study. Materials, 2020, 13(21): 4912
|
47 |
Cheng Y , Ekici E , Yildiz G , Yang Y , Coward B , Wang J . Applied machine learning for prediction of waste plastic pyrolysis towards valuable fuel and chemicals production. Journal of Analytical and Applied Pyrolysis, 2023, 169: 105857
|
48 |
Lopez G , Artetxe M , Amutio M , Bilbao J , Olazar M . Thermochemical routes for the valorization of waste polyolefinic plastics to produce fuels and chemicals. A review. Renewable & Sustainable Energy Reviews, 2017, 73: 346–368
|
49 |
YildizGRonsseFPrinsW. Catalytic fast pyrolysis over zeolites. Fast pyrolysis of biomass: advances in science and technology. The Royal Society of Chemistry, Cambridge 2017, 200–230
|
50 |
Diaz Silvarrey L S , Phan A N . Kinetic study of municipal plastic waste. International Journal of Hydrogen Energy, 2016, 41(37): 16352–16364
|
51 |
Saad J M , Williams P T , Zhang Y S , Yao D , Yang H , Zhou H . Comparison of waste plastics pyrolysis under nitrogen and carbon dioxide atmospheres: a thermogravimetric and kinetic study. Journal of Analytical and Applied Pyrolysis, 2021, 156: 105135
|
52 |
Jung S H , Cho M H , Kang B S , Kim J S . Pyrolysis of a fraction of waste polypropylene and polyethylene for the recovery of BTX aromatics using a fluidized bed reactor. Fuel Processing Technology, 2010, 91(3): 277–284
|
53 |
Anene A F , Fredriksen S B , Sætre K A , Tokheim L A . Experimental study of thermal and catalytic pyrolysis of plastic waste components. Sustainability, 2018, 10(11): 3979
|
54 |
Ekici E.&YildizG.. Determination of optimal pyrolysis process parameters to maximize gasoline like renewable fuel production from polypropylene. Innovations-Sustainability-Modernity-Openness Modern Solutions in Engineering (ISMO 2022), 44: 67–175 (eBook)
|
55 |
Chandrasekaran S R , Kunwar B , Moser B R , Rajagopalan N , Sharma B K . Catalytic thermal cracking of postconsumer waste plastics to fuels. 1. Kinetics and optimization. Energy & Fuels, 2015, 29(9): 6068–6077
|
56 |
SerranoD PAguadoJEscolaJ MGaragorriE. Conversion of low density polyethylene into petrochemical feedstocks using a continuous screw kiln reactor. Journal of Analytical and Applied Pyrolysis, 2001, 58–59: 789–801
|
57 |
Kusenberg M , Zayoud A , Roosen M , Thi H D , Abbas-Abadi M S , Eschenbacher A , Kresovic U , De Meester S , Van Geem K M . A comprehensive experimental investigation of plastic waste pyrolysis oil quality and its dependence on the plastic waste composition. Fuel Processing Technology, 2022, 227: 107090
|
58 |
Aguado R , Olazar M , San José M J , Gaisán B , Bilbao J . Wax formation in the pyrolysis of polyolefins in a conical spouted bed reactor. Energy & Fuels, 2002, 16(6): 1429–1437
|
59 |
Qureshi K M , Kay Lup A N , Khan S , Abnisa F , Wan Daud W M A . A technical review on semi-continuous and continuous pyrolysis process of biomass to bio-oil. Journal of Analytical and Applied Pyrolysis, 2018, 131: 52–75
|
60 |
ConesaJ AFontRMarcillaACaballeroJ A. Kinetic model for the continuous pyrolysis of two types of polyethylene in a fluidized bed reactor. Journal of Analytical and Applied Pyrolysis, 1997, 40–41(19): 419–431
|
61 |
Hernández M del R , García Á N , Marcilla A . Study of the gases obtained in thermal and catalytic flash pyrolysis of HDPE in a fluidized bed reactor. Journal of Analytical and Applied Pyrolysis, 2005, 73(2): 314–322
|
62 |
Mastellone M L , Perugini F , Ponte M , Arena U . Fluidized bed pyrolysis of a recycled polyethylene. Polymer Degradation & Stability, 2002, 76(3): 479–487
|
63 |
ASTM D7611/D7611M–21 “Standard practice for coding plastic manufactured articles for resin identification”. ASTM International, 2022
|
64 |
Ekici E.&YildizG.. Analysis of Pyrolysis Process Parameters for the Maximized Production of Gasoline-range Renewable Fuels from High-density Polyethylene. In: Proceedings of the 2022 International Symposium on Energy Management and Sustainability, Springer: Cham, 2022, 311–318
|
65 |
ISO 1928:2020 “Solid mineral fuels—determination of gross calorific value by the bomb calorimetric method and calculation of net calorific value”. ISO, 2020
|
66 |
Obidziński S , Joka Yildiz M , Dąbrowski S , Jasiński J , Czekała W . Application of post-flotation dairy sludge in the production of wood pellets: pelletization and combustion analysis. Energies, 2022, 15(24): 9427
|
67 |
Phyllis2 ECN Phyllis classification-Plastics. 2023 phyllis.nl/Browse/Standard/ECN-Phyllis#plastic. Accessed 07 Apr 2023
|
68 |
Gala A , Guerrero M , Serra J M . Characterization of post-consumer plastic film waste from mixed MSW in Spain: a key point for the successful implementation of sustainable plastic waste management strategies. Waste Management, 2020, 111: 22–33
|
69 |
Chowlu A C K , Reddy P K , Ghoshal A K . Pyrolytic decomposition and model-free kinetics analysis of mixture of polypropylene (PP) and low-density polyethylene (LDPE). Thermochimica Acta, 2009, 485(1–2): 20–25
|
70 |
Abbas-Abadi M S , Kusenberg M , Zayoud A , Roosen M , Vermeire F , Madanikashani S , Kuzmanović M , Parvizi B , Kresovic U , De Meester S , Van Geem K M . Thermal pyrolysis of waste versus virgin polyolefin feedstocks: the role of pressure, temperature and waste composition. Waste Management, 2023, 165: 108–118
|
71 |
Uemichi Y , Kashiwaya Y , Ayame A , Kanoh K . Formation of aromatic hydrocarbons in degradation of polyethylene over activated carbon catalyst. Chemical Letters, 1984, 13(1): 41–44
|
72 |
Murata K , Hirano Y , Sakata Y , Uddin M A . Basic study on a continuous flow reactor for thermal degradation of polymers. Journal of Analytical and Applied Pyrolysis, 2002, 65(1): 71–90
|
73 |
Murata K , Brebu M , Sakata Y . The effect of PVC on thermal and catalytic degradation of polyethylene, polypropylene and polystyrene by a continuous flow reactor. Journal of Analytical and Applied Pyrolysis, 2009, 86(1): 33–38
|
74 |
Murata K , Brebu M , Sakata Y . The effect of silica-alumina catalysts on degradation of polyolefins by a continuous flow reactor. Journal of Analytical and Applied Pyrolysis, 2010, 89(1): 30–38
|
75 |
Breyer S , Mekhitarian L , Rimez B , Haut B . Production of an alternative fuel by the co-pyrolysis of landfill recovered plastic wastes and used lubrication oils. Waste Management, 2017, 60: 363–374
|
76 |
Kunwar B , Cheng H N , Chandrashekaran S R , Sharma B K . Plastics to fuel: a review. Renewable & Sustainable Energy Reviews, 2016, 54: 421–428
|
77 |
Phetyim N , Pivsa-Art S . Prototype co-pyrolysis of used lubricant oil and mixed plastic waste to produce a diesel-like fuel. Energies, 2018, 11(11): 2973
|
78 |
Marcilla A , Beltrán M I , Navarro R . Evolution of products during the degradation of polyethylene in a batch reactor. Journal of Analytical and Applied Pyrolysis, 2009, 86(1): 14–21
|
79 |
Al-Salem S M , Lettieri P . Kinetic study of high density polyethylene (HDPE) pyrolysis. Chemical Engineering Research & Design, 2010, 88(12): 1599–1606
|
80 |
Supriyanto Y P , Ylitervo T . Gaseous products from primary reactions of fast plastic pyrolysis. Journal of Analytical and Applied Pyrolysis, 2021, 158: 105248
|
81 |
Aguado R , Elordi G , Arrizabalaga A , Artetxe M , Bilbao J , Olazar M . Principal component analysis for kinetic scheme proposal in the thermal pyrolysis of waste HDPE plastics. Chemical Engineering Journal, 2014, 254: 357–364
|
82 |
Klippel M S , Martins M F . Physicochemical assessment of waxy products directly recovered from plastic waste pyrolysis: review and synthesis of characterization techniques. Polymer Degradation & Stability, 2022, 204: 110090
|
83 |
Thahir R , Irwan M , Alwathan A , Ramli R . Effect of temperature on the pyrolysis of plastic waste using zeolite ZSM-5 using a refinery distillation bubble cap plate column. Results in Engineering, 2021, 11: 100231
|
84 |
MERCK IR Spectrum Table & Chart. 2023: www.sigmaaldrich.com/TR/en/technical-documents/technical-article/analytical-chemistry/photometry-and-reflectometry/ir-spectrum-table
|
85 |
Gómez-Estaca J , López-de-Dicastillo C , Hernández-Muñoz P , Catalá R , Gavara R . Advances in antioxidant active food packaging. Trends in Food Science & Technology, 2014, 35(1): 42–51
|
86 |
Lau O W , Wong S K . Contamination in food from packaging material. Journal of Chromatography. A, 2000, 882(1–2): 255–270
|
87 |
Kamali A , Heidari S , Golzary A , Tavakoli O , Wood D A . Optimized catalytic pyrolysis of refinery waste sludge to yield clean high quality oil products. Fuel, 2022, 328: 125292
|
88 |
Kunwar B , Moser B R , Chandrasekaran S R , Rajagopalan N , Sharma B K . Catalytic and thermal depolymerization of low value post-consumer high density polyethylene plastic. Energy, 2016, 111: 884–892
|
89 |
Miskolczi N , Angyal A , Bartha L , Valkai I . Fuels by pyrolysis of waste plastics from agricultural and packaging sectors in a pilot scale reactor. Fuel Processing Technology, 2009, 90(7–8): 1032–1040
|
90 |
Park K B , Oh S J , Begum G , Kim J S . Production of clean oil with low levels of chlorine and olefins in a continuous two-stage pyrolysis of a mixture of waste low-density polyethylene and polyvinyl chloride. Energy, 2018, 157: 402–411
|
91 |
Mastral J F , Berrueco C , Gea M , Ceamanos J . Catalytic degradation of high density polyethylene over nanocrystalline HZSM-5 zeolite. Polymer Degradation & Stability, 2006, 91(12): 3330–3338
|
92 |
Park K B , Jeong Y S , Guzelciftci B , Kim J S . Characteristics of a new type continuous two-stage pyrolysis of waste polyethylene. Energy, 2019, 166(1): 343–351
|
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