废塑料催化裂解制低碳烯烃、轻质燃料油和芳烃的研究进展

摘要/Abstract

摘要： 随着全球废塑料量的不断增加以及化石能源的不断减少，碳资源循环利用已引起人们的广泛关注。催化裂解是当前废塑料回收利用的一种很有前景的处理方案，可解决环境污染及能源短缺问题。本文主要针对废塑料催化裂解制备轻质燃料油及高附加值产品进行综述，探讨废塑料组成、反应温度、反应器类型及催化剂类型对低碳烯烃、轻质燃料油和芳烃收率的影响，并简述废塑料催化裂解制低碳烯烃、轻质燃料油和芳烃的应用前景；此外，基于现阶段研究进展及存在的问题提出发展方向和思路，该研究可为废塑料的高效转化及高值化利用提供借鉴。

关键词: 废塑料, 催化裂解, 低碳烯烃, 轻质燃料油, 芳烃

Abstract: With the increasing production of waste plastics and the reduction of fossil energy, the issue of carbon resources recycling has attracted widespread attention. Catalytic pyrolysis technology is a promising treatment solution for the recycling of waste plastics at present, which can solve the problems of environmental pollution and energy shortage. In this paper, the production of light fuel oil and high value-added products by catalytic cracking of waste plastics were reviewed, the effects of waste plastics composition, reaction temperature, reactor type, and catalyst type on the yield of light olefins, light fuel oil and aromatics were investigated, and the application prospect of catalytic cracking of waste plastics to produce light olefins, light fuel oils and aromatics was briefly described. This research was of great significance to the efficient conversion and high-value utilization of waste plastics.

Key words: waste plastics, catalytic pyrolysis, light olefins, light fuel oil, aromatics

许强朱建华朱永红. 废塑料催化裂解制低碳烯烃、轻质燃料油和芳烃的研究进展[J]. 石油炼制与化工, 2023, 54(5): 125-132.

参考文献

[1] Kusenberg M, Eschenbacher A, Djokic M R, et al.Opportunities and challenges for the application of post-consumer plastic waste pyrolysis oils as steam cracker feedstocks: To decontaminate or not to decontaminate?[J].Waste Management, 2022, 138:83-115 [2]Geyer R, Jambeck J R, Law K L.Production,use,and fate of all plastics ever made[J].Science Advances, 2017, 3(7):e1700782- [3]Sardon H, Dove A P.Plastics recycling with a difference[J].Science, 2018, 360(6387):380-381 [4]Meys R, Katelhon A, Bachmann M, et al.Achieving net-zero greenhouse gas emission plastics by a circular carbon economy[J].Science, 2021, 374(6563):71-76 [5]Ignatyev I A, Thielemans W, Vander Beke B.Recycling of Polymers: A Review[J].ChemSusChem, 2014, 7(6):1579-1593 [6]Al-Salem S M, Lettieri P, Baeyens J.The valorization of plastic solid waste (PSW) by primary to quaternary routes: From re-use to energy and chemicals[J].Progress in Energy and Combustion Science, 2010, 36(1):103-129 [7]Brems A, Baeyens J, Dewil R.Recycling and Recovery of Post-Consumer Plastic Solid Waste in a European Context[J].Thermal Science, 2012, 16(3):669-685 [8]Kosloski-Oh S C, Wood Z A, Manjarrez Y, et al.Catalytic methods for chemical recycling or upcycling of commercial polymers[J].Materials Horizons, 2021, 8(4):1084-1129 [9]Morris J.Recycling versus incineration: an energy conservation analysis[J].Journal of Hazardous Materials, 1996, 47(1-3):277-293 [10] Kunwar B, Cheng H N, Chandrashekaran S R, et al.Plastics to fuel: a review[J].Renewable & Sustainable Energy Reviews, 2016, 54:421-428 [11] Zhao X, Korey M, Li K, et al.Plastic waste upcycling toward a circular economy[J].Chemical Engineering Journal, 2022, 428:31928- [12] Passamonti F J, Sedran U.Recycling of waste plastics into fuels. LDPE conversion in FCC[J].Applied Catalysis B: Environmental, 2012, 125:499-506 [13] Eschenbacher A, Varghese R J, Abbas-Abadi M S, et al.Maximizing light olefins and aromatics as high value base chemicals via single step catalytic conversion of plastic waste[J].Chemical Engineering Journal, 2022, 428:132087- [14] Zhang F, Wang F, Wei X, et al.From trash to treasure: Chemical recycling and upcycling of commodity plastic waste to fuels, high-valued chemicals and advanced materials[J].Journal of Energy Chemistry, 2022, 69:369-388 [15]Butler E, Devlin G, Mcdonnell K.Waste Polyolefins to Liquid Fuels via Pyrolysis: Review of Commercial State-of-the-Art and Recent Laboratory Research[J].Waste and Biomass Valorization, 2011, 2(3):227-255 [16] Rajendran K M, Chintala V, Sharma A, et al.Review of catalyst materials in achieving the liquid hydrocarbon fuels from municipal mixed plastic waste (MMPW)[J].Materials Today Communications, 2020, 24:100982- [17]Achilias D S, Roupakias C, Megalokonomos P, et al.Chemical recycling of plastic wastes made from polyethylene (LDPE and HDPE) and polypropylene (PP)[J].Journal of Hazardous Materials, 2007, 149(3):536-542 [18]Lin Y H, Yang M H.Tertiary recycling of polyethylene waste by fluidised-bed reactions in the presence of various cracking catalysts[J].Journal of Analytical and Applied Pyrolysis, 2008, 83(1):101-109 [19]Murata K, Brebu M, Sakata Y.The effect of silica-alumina catalysts on degradation of polyolefins by a continuous flow reactor[J].Journal of Analytical and Applied Pyrolysis, 2010, 89(1):30-38 [20]Liu W, Hu C, Yang Y, et al.Influence of ZSM-5 zeolite on the pyrolytic intermediates from the co-pyrolysis of pubescens and LDPE[J].Energy Conversion and Management, 2010, 51(5):1025-1032 [21]Mastral J F, Berrueco C, Gea M, et al.Catalytic degradation of high density polyethylene over nanocrystalline HZSM-5 zeolite[J].Polymer Degradation and Stability, 2006, 91(12):3330-3338 [22] Santos B P S, Almeida D, Marques M D V, et al.Petrochemical feedstock from pyrolysis of waste polyethylene and polypropylene using different catalysts[J]. Fuel, 2018, 215:515-521 [23]Jia X Q, Qin C, Friedberger T, et al.Efficient and selective degradation of polyethylenes into liquid fuels and waxes under mild conditions[J].Science Advances, 2016, 2(6):e1501591- [24] Abnisa F, Daud W M a W.A review on co-pyrolysis of biomass: An optional technique to obtain a high-grade pyrolysis oil[J].Energy Conversion and Management, 2014, 87:71-85 [25] Sharma B K, Moser B R, Vermillion K E, et al.Production, characterization and fuel properties of alternative diesel fuel from pyrolysis of waste plastic grocery bags[J].Fuel Processing Technology, 2014, 122:79-90 [26] Sharuddin S D A, Abnisa F, Daud W M a W, et al.Energy recovery from pyrolysis of plastic waste: Study on non-recycled plastics (NRP) data as the real measure of plastic waste[J].Energy Conversion and Management, 2017, 148:925-934 [27] Park K B, Jeong Y S, Guzelciftci B, et al.Two-stage pyrolysis of polystyrene: Pyrolysis oil as a source of fuels or benzene, toluene, ethylbenzene, and xylenes[J].Applied Energy, 2020, 259:114240- [28] Zhou H, Wu C F, Onwudili J A, et al.Polycyclic aromatic hydrocarbons (PAH) formation from the pyrolysis of different municipal solid waste fractions[J].Waste Management, 2015, 36:136-146 [29] Singh R K, Ruj B.Time and temperature depended fuel gas generation from pyrolysis of real world municipal plastic waste[J].Fuel, 2016, 174:164-171 [30]Lee K H, Noh N S, Shin D H, et al.Comparison of plastic types for catalytic degradation of waste plastics into liquid product with spent FCC catalyst[J].Polymer Degradation and Stability, 2002, 78(3):539-544 [31] Mangesh V L, Padmanabhan S, Tamizhdurai P, et al.Experimental investigation to identify the type of waste plastic pyrolysis oil suitable for conversion to diesel engine fuel[J].Journal of Cleaner Production, 2020, 246:119066- [32] Kassargy C, Awad S, Burnens G, et al.Experimental study of catalytic pyrolysis of polyethylene and polypropylene over USY zeolite and separation to gasoline and diesel-like fuels[J].Journal of Analytical and Applied Pyrolysis, 2017, 127:31-37 [33] Verma A, Sharma S, Pramanik H.Pyrolysis of waste expanded polystyrene and reduction of styrene via in-situ multiphase pyrolysis of product oil for the production of fuel range hydrocarbons[J].Waste Management, 2021, 120:330-339 [34] Inayat A, Fasolini A, Basile F, et al.Chemical recycling of waste polystyrene by thermo-catalytic pyrolysis: A description for different feedstocks, catalysts and operation modes[J].Polymer Degradation and Stability, 2022, 201:109981- [35]Achilias D S, Kanellopoulou I, Megalokonomos P, et al.Chemical recycling of polystyrene by pyrolysis: Potential use of the liquid product for the reproduction of polymer[J].Macromolecular Materials and Engineering, 2007, 292(8):923-934 [36]?epelio?ullar ?, Pütün A E.Utilization of Two Different Types of Plastic Wastes from Daily and Industrial Life[J].Journal of Selcuk University Natural and Applied Science, 2013, 2(2):694-706 [37]Yoshioka T, Kitagawa E, Mizoguchi T, et al.High selective conversion of poly(ethylene terephthalate) into oil using Ca(OH)2[J].Chemistry Letters, 2004, 33(3):282-283 [38]Yoshioka T, Handa T, Grause G, et al.Effects of metal oxides on the pyrolysis of poly(ethylene terephthalate)[J].Journal of Analytical and Applied Pyrolysis, 2005, 73(1):139-144 [39] Sharuddin S D A, Abnisa F, Daud W M a W, et al.A review on pyrolysis of plastic wastes[J].Energy Conversion and Management, 2016, 115:308-326 [40] Wang J, Jiang J, Wang X, et al.Converting polycarbonate and polystyrene plastic wastes into aromatic hydrocarbons via catalytic fast co-pyrolysis[J].Journal of Hazardous Materials, 2020, 386:121970- [41]Wu J, Chen T, Luo X, et al.TGFTIR analysis on co-pyrolysis behavior of PE,PVC and PS[J].Waste Management, 2014, 34(3):676-82 [42] Peng Y, Wang Y, Ke L, et al.A review on catalytic pyrolysis of plastic wastes to high-value products[J].Energy Conversion and Management, 2022, 254:115243- [43]Miskolczi N, Bartha L, Deák G.Thermal degradation of polyethylene and polystyrene from the packaging industry over different catalysts into fuel-like feed stocks[J].Polymer Degradation and Stability, 2006, 91(3):517-526 [44] Singh R K, Ruj B, Sadhukhan A K, et al.Thermal degradation of waste plastics under non-sweeping atmosphere: Part 1: Effect of temperature, product optimization, and degradation mechanism[J].Journal of Environmental Management, 2019, 239:395-406 [45] Abbas-Abadi M S, Haghighi M N, Yeganeh H, et al.Evaluation of pyrolysis process parameters on polypropylene degradation products[J].Journal of Analytical and Applied Pyrolysis, 2014, 109:272-277 [46] Rodríguez E, Gutiérrez A, Palos R, et al.Fuel production by cracking of polyolefins pyrolysis waxes under fluid catalytic cracking (FCC) operating conditions[J].Waste Management, 2019, 93:162-172 [47]Lin Y H, Yang M H, Yeh T F, et al.Catalytic degradation of high density polyethylene over mesoporous and microporous catalysts in a fluidised-bed reactor[J].Polymer Degradation and Stability, 2004, 86(1):121-128 [48]López A, De Marco I, Caballero B M, et al.Catalytic pyrolysis of plastic wastes with two different types of catalysts: ZSM-5 zeolite and Red Mud[J].Applied Catalysis B: Environmental, 2011, 104(3-4):211-219 [49]Seo Y H, Lee K H, Shin D H.Investigation of catalytic degradation of high-density polyethylene by hydrocarbon group type analysis[J].Journal of Analytical and Applied Pyrolysis, 2003, 70(2):383-398 [50]Lee K H.Composition of aromatic products in the catalytic degradation of the mixture of waste polystyrene and high-density polyethylene using spent FCC catalyst[J].Polymer Degradation and Stability, 2008, 93(7):1284-1289 [51] Das P, Tiwari P.The effect of slow pyrolysis on the conversion of packaging waste plastics (PE and PP) into fuel[J].Waste Management, 2018, 79:615-624 [52] Ate? F, Miskolczi N, Borsodi N.Comparision of real waste (MSW and MPW) pyrolysis in batch reactor over different catalysts. Part I: Product yields, gas and pyrolysis oil properties[J].Bioresource Technology, 2013, 133:443-454 [53] Lovás P, Hudec P, Jambor B, et al.Catalytic cracking of heavy fractions from the pyrolysis of waste HDPE and PP[J].Fuel, 2017, 203:244-252 [54] Marino A, Aloise A, Hernando H, et al.ZSM-5 zeolites performance assessment in catalytic pyrolysis of PVC-containing real WEEE plastic wastes[J].Catalysis Today, 2022, 390-391:210-220 [55]Onwudili J A, Muhammad C, Williams P T.Influence of catalyst bed temperature and properties of zeolite catalysts on pyrolysis-catalysis of a simulated mixed plastics sample for the production of upgraded fuels and chemicals[J].Journal of the Energy Institute, 2019, 92(5):1337-1347 [56] Ratnasari D K, Nahil M A, Williams P T.Catalytic pyrolysis of waste plastics using staged catalysis for production of gasoline range hydrocarbon oils[J].Journal of Analytical and Applied Pyrolysis, 2017, 124:631-637 [57]Kaminsky W, Kim J-S.Pyrolysis of mixed plastics into aromatics[J].Journal of Analytical and Applied Pyrolysis, 1999, 51(1-2):127-134 [58]Huang W-C, Huang M-S, Huang C-F, et al.Thermochemical conversion of polymer wastes into hydrocarbon fuels over various fluidizing cracking catalysts[J].Fuel, 2010, 89(9):2305-2316 [59]Lin H T, Huang A S, Luo J W, et al.Hydrocarbon fuels produced by catalytic pyrolysis of hospital plastic wastes in a fluidizing cracking process[J].Fuel Processing Technology, 2010, 91(11):1355-1363 [60]Elordi G, Olazar M, Casta?o P, et al.Polyethylene Cracking on a Spent FCC Catalyst in a Conical Spouted Bed[J].Industrial & Engineering Chemistry Research, 2012, 51(43):14008-14017 [61]Olazar M, Lopez G, Amutio M, et al.Influence of FCC catalyst steaming on HDPE pyrolysis product distribution[J].Journal of Analytical and Applied Pyrolysis, 2009, 85(1-2):359-365 [62]Elordi G, Olazar M, Lopez G, et al.Catalytic pyrolysis of HDPE in continuous mode over zeolite catalysts in a conical spouted bed reactor[J].Journal of Analytical and Applied Pyrolysis, 2009, 85(1-2):345-351 [63]Jung S H, Cho M H, Kang B S, et al.Pyrolysis of a fraction of waste polypropylene and polyethylene for the recovery of BTX aromatics using a fluidized bed reactor[J].Fuel Processing Technology, 2010, 91(3):277-284 [64]Nishino J, Itoh M, Fujiyoshi H, et al.Catalytic degradation of plastic waste into petrochemicals using Ga-ZSM-5[J].Fuel, 2008, 87(17-18):3681-3686 [65] Artetxe M, Lopez G, Amutio M, et al.Light olefins from HDPE cracking in a two-step thermal and catalytic process[J].Chemical Engineering Journal, 2012, 207-208:27-34 [66]Chlup Z, ?erny M, Strachota A, et al.Influence of pyrolysis temperature on fracture response in SiOC based composites reinforced by basalt woven fabric[J].Journal of the European Ceramic Society, 2014, 34(14):3389-3398 [67] Ibá?ez M, Artetxe M, Lopez G, et al.Identification of the coke deposited on an HZSM-5 zeolite catalyst during the sequenced pyrolysis-cracking of HDPE[J].Applied Catalysis B: Environmental, 2014, 148:436-445 [68]Elordi G, Olazar M, Lopez G, et al.Role of pore structure in the deactivation of zeolites (HZSM-5,H beta and HY) by coke in the pyrolysis of polyethylene in a conical spouted bed reactor[J].Applied Catalysis B-Environmental, 2011, 102(1-2):224-231 [69]Al-Khattaf S, D' agostino C, Akhtar M N, et al.The effect of coke deposition on the activity and selectivity of the HZSM-5 zeolite during ethylbenzene alkylation reaction in the presence of ethanol[J].Catalysis Science & Technology, 2014, 4(4):1017-1027 [70]Jae J, Tompsett G A, Foster A J, et al.Investigation into the shape selectivity of zeolite catalysts for biomass conversion[J].Journal of Catalysis, 2011, 279(2):257-268 [71] Eschenbacher A, Varghese R J, Delikonstantis E, et al.Highly selective conversion of mixed polyolefins to valuable base chemicals using phosphorus-modified and steam-treated mesoporous HZSM-5 zeolite with minimal carbon footprint[J].Applied Catalysis B: Environmental, 2022, 309:121251- [72] Fan L L, Liu L, Xiao Z G, et al.Comparative study of continuous-stirred and batch microwave pyrolysis of linear low-density polyethylene in the presence/absence of HZSM-5[J].Energy, 2021, 228:120612.- [73]Artetxe M, Lopez G, Amutio M, et al.Cracking of High Density Polyethylene Pyrolysis Waxes on HZSM-5 Catalysts of Different Acidity[J].Industrial & Engineering Chemistry Research, 2013, 52(31):10637-10645 [74]Marcilla A, Beltrán M I, Navarro R.Thermal and catalytic pyrolysis of polyethylene over HZSM5 and HUSY zeolites in a batch reactor under dynamic conditions[J].Applied Catalysis B: Environmental, 2009, 86(1-2):78-86 [75]Akubo K, Nahil M A, Williams P T.Aromatic fuel oils produced from the pyrolysis-catalysis of polyethylene plastic with metal-impregnated zeolite catalysts[J].Journal of the Energy Institute, 2019, 92(1):195-202 [76]Lin Y H, Yang M H.Catalytic pyrolysis of polyolefin waste into valuable hydrocarbons over reused catalyst from refinery FCC units[J].Applied Catalysis A: General, 2007, 328(2):132-139 [77]Marcilla A, Gómez-Siurana A, Berenguer D.Study of the influence of the characteristics of different acid solids in the catalytic pyrolysis of different polymers[J].Applied Catalysis A: General, 2006, 301(2):222-231 [78] Aguado J, Sotelo J L, Serrano D P, et al.Catalytic Conversion of Polyolefins into Liquid Fuels over MCM-41 Comparison with ZSM-5 and Amorphous SiO2-Al2O3[J].Energy & Fuels, 1997, 11(6):1225-1231 [79]Cardona S C, Corma A.Tertiary recycling of polypropylene by catalytic cracking in a semibatch stirred reactor Use of spent equilibrium FCC commercial catalyst[J].Applied Catalysis B: Environmental, 2000, 25(2-3):151-162 [80]Salmiaton A, Garforth A A.Multiple use of waste catalysts with and without regeneration for waste polymer cracking[J].Waste Management, 2011, 31(6):1139-1145 [81] Rodríguez E, Gutiérrez A, Palos R, et al.Co-cracking of high-density polyethylene (HDPE) and vacuum gasoil (VGO) under refinery conditions[J].Chemical Engineering Journal, 2020, 382:122602- [82]Lin Y H, Yang M H.Chemical catalysed recycling of waste polymers: Catalytic conversion of polypropylene into fuels and chemicals over spent FCC catalyst in a fluidised-bed reactor[J].Polymer Degradation and Stability, 2007, 92(5):813-821 [83] Rodríguez E, Palos R, Gutiérrez A, et al.Towards waste refinery: Co-feeding HDPE pyrolysis waxes with VGO into the catalytic cracking unit[J].Energy Conversion and Management, 2020, 207:112554- [84]Amghizar I, Vandewalle L A, Van Geem K M, et al.New Trends in Olefin Production[J].Engineering, 2017, 3(2):171-178 [85] Bai Y, Zhang G, Liu D, et al.The advance in catalytic pyrolysis of naphtha technology using ZSM-5 as catalyst[J].Applied Catalysis A: General, 2021, 628:118399- [86]王建明.催化裂解生产低碳烯烃技术和工业应用的进展[J].化工进展, 2011, 30(5):911-917 [87]周春艳.国内外乙烯市场分析[J].化学工业, 2021, 39(4):87-91 [88]刘治华, 李宇静.中国丙烯市场回顾及“十四五”展望[J].现代化工, 2021, 41(8):16-18 [89]侯雨璇, 王红秋, 鲜楠莹.世界丙烯生产技术进展与经济性分析[J].现代化工, 2020, 40(10):60-65 [90] Zheng J, L?bbert L, Chheda S, et al.Metal-organic framework supported single-site nickel catalysts for butene dimerization[J].Journal of Catalysis, 2022, 413:176-183 [91] Zhang H H, Liu R X, Yang Z Q, et al.Alkylation of isobutane/butene promoted by fluoride-containing ionic liquids[J].Fuel, 2018, 211:233-240 [92]王定博, 刘红梅, 刘晓玲.异丁烯资源的利用[J].石油化工, 2020, 49(12):1235-1240 [93]Angyal A, Miskolczi N, Bartha L.Petrochemical feedstock by thermal cracking of plastic waste[J].Journal of Analytical and Applied Pyrolysis, 2007, 79(1-2):409-414 [94]Miskolczi N, Angyal A, Bartha L, et al.Fuels by pyrolysis of waste plastics from agricultural and packaging sectors in a pilot scale reactor[J].Fuel Processing Technology, 2009, 90(7-8):1032-1040 [95] Kassargy C, Awad S, Burnens G, et al.Gasoline and diesel-like fuel production by continuous catalytic pyrolysis of waste polyethylene and polypropylene mixtures over USY zeolite[J].Fuel, 2018, 224:764-773 [96] Janarthanan K, Sivanandi P.Extraction and characterization of waste plastic pyrolysis oil for diesel engines[J].Journal of Cleaner Production, 2022, 366:132924- [97] Kaimal V K, Vijayabalan P.An investigation on the effects of using DEE additive in a DI diesel engine fuelled with waste plastic oil[J].Fuel, 2016, 180:90-96 [98] Baena-González J, Santamaria-Echart A, Aguirre J L, et al.Chemical recycling of plastic waste: Bitumen, solvents, and polystyrene from pyrolysis oil[J].Waste Management, 2020, 118:139-149