聚乙烯常规及微波催化热解产物分布特征的研究进展

doi:10.16085/j.issn.1000-6613.2024-2128

化工进展 ›› 2025, Vol. 44 ›› Issue (6): 3224-3237.DOI: 10.16085/j.issn.1000-6613.2024-2128

• 专栏：化工过程强化 • 上一篇

聚乙烯常规及微波催化热解产物分布特征的研究进展

张莹¹^,²(), 郑雪梅²^,³, 马爱元²^,³(), 田时泓⁴()

^1.大连大学环境与化学工程学院，辽宁大连 116622
^2.六盘水师范学院化学与材料工程学院，贵州六盘水 553004
^3.贵州省煤碳洁净利用重点实验室，贵州六盘水 553004
^4.中国科学院重庆绿色智能技术研究院大气环境研究中心，重庆 400714

收稿日期:2024-12-31 修回日期:2025-03-25 出版日期:2025-06-25 发布日期:2025-07-08
通讯作者: 马爱元,田时泓
作者简介:张莹（2000—），女，硕士研究生，研究方向为塑料催化热解。E-mail：zy2000202109@163.com。
基金资助:
贵州省煤炭洁净利用重点实验室(黔科合平台人才[2020]2001);六盘水市科技局科技发展项目(52020-2023-0-2-6);六盘水市科技局科技发展项目(52020-2024-0-2-8);重庆市北碚区科技人才与自主创新专项(2024-19)

Research progress based on conventional and microwave pyrolysis behavior of polyethylene

ZHANG Ying¹^,²(), ZHENG Xuemei²^,³, MA Aiyuan²^,³(), TIAN Shihong⁴()

^1.College of Environmental and Chemical Engineering, Dalian University, Dalian 116622, Liaoning, China
^2.School of Chemistry and Materials Engineering, Liupanshui Normol University, Liupanshui 553004, Guizhou, China
^3.Guizhou Provincial Key Laboratory of Coal Clean Utilization, Liupanshui 553004, Guizhou, China
^4.Research Center for Atmospheric Environment, Chongqing Institute of Green and Intelligent Technology, Chinese Academy of Sciences, Chongqing 400714, China

Received:2024-12-31 Revised:2025-03-25 Online:2025-06-25 Published:2025-07-08
Contact: MA Aiyuan, TIAN Shihong

摘要/Abstract

摘要：

聚烯烃类塑料制品因碳氢链结构化学稳定性好、难自然降解，其处理方式备受关注。催化热解技术被认为是废塑料回收利用的绿色方法。区别于常规热解技术的低效能和低产率，微波催化热解因加热速率快、受热均匀、能量转换率高，能显著提升微波转化效率，提高高价值化学品的产率与品质。本文从常规和微波催化热解的工艺应用出发，系统阐述过渡金属（Fe、Co、Ni等）负载型催化剂对常规催化热解聚乙烯产生的气液固三相产物的影响，以及铁基复合金属催化剂和分子筛类催化剂对微波催化热解聚乙烯产生的氢气、碳纳米管和芳烃油的选择性差异，梳理了常规和微波催化热解废塑料的产物分布规律，对比了铁基复合催化剂对常规和微波催化热解产物的选择性，探讨了常规及微波催化热解废塑料的反应机理和发展趋势。针对微波催化热解废塑料催化剂的性能问题，提出开发具有良好吸波性能和催化能力的催化剂来提高微波利用率和催化活性，进一步改善微波催化废塑料高附加值产品的质量，最后对微波热解废塑料产物的可控性和纯度进行了展望。

关键词: 聚乙烯, 常规热解, 微波热解, 催化剂, 催化机理

Abstract:

Polyolefin plastic products have attracted much attention due to their good chemical stability in the structure of the hydrocarbon chain and are difficult to degrade naturally. Catalytic pyrolysis technology is considered a green method for recycling waste plastics. Different from the low efficiency and low yield of conventional pyrolysis technologies, microwave catalytic pyrolysis can significantly improve microwave conversion efficiency and improve the yield and quality of high-value chemicals due to its fast heating rate, uniform heating and high energy conversion rate. Based on the application of conventional and microwave catalytic pyrolysis, this paper systematically explained the effect of transition metal (Fe, Co, Ni, etc.) supported catalysts on gas-liquid solid three-phase products produced by conventional catalytic pyrolysis polyethylene, as well as the selectivity differences between iron-based composite metal catalysts and molecular sieve catalysts on hydrogen, carbon nanotubes and aromatic oils produced by microwave catalytic pyrolysis polyethylene, sorted out the product distribution rules of conventional and microwave catalytic pyrolysis waste plastics, compared the selectivity of iron-based composite catalysts on conventional and microwave catalytic pyrolysis products, and explored the reaction mechanism and development trend of conventional and microwave catalytic pyrolysis waste plastics. In response to the performance of microwave catalytic pyrolysis waste plastic catalyst, it was proposed to develop catalysts with good wave absorption performance and catalytic capabilities to improve microwave utilization and catalytic activity, and further to improve the quality of high-value-added products of microwave catalytic waste plastics. Finally, the controllability and purity of microwave pyrolysis waste plastic products were expected.

Key words: polyethylene, conventional cracking, microwave cracking, catalyst, catalytic mechanism

中图分类号:

TQ203.2

张莹, 郑雪梅, 马爱元, 田时泓. 聚乙烯常规及微波催化热解产物分布特征的研究进展[J]. 化工进展, 2025, 44(6): 3224-3237.

ZHANG Ying, ZHENG Xuemei, MA Aiyuan, TIAN Shihong. Research progress based on conventional and microwave pyrolysis behavior of polyethylene[J]. Chemical Industry and Engineering Progress, 2025, 44(6): 3224-3237.

图/表 9

表1 常规催化热解聚乙烯的产物产率

催化剂	反应温度	塑料种类	氢气产率	液体产率	固体产率	文献
Fe/Al₂O₃	800℃	LDPE	50.60%	—	—	[9]
Ni/Al₂O₃	800℃	LDPE	36.60%	—	—	[9]
Co/Al₂O₃	800℃	LDPE	31.30%	—	—	[9]
Cu/Al₂O₃	800℃	LDPE	26.00%	—	—	[9]
Fe/SiO₂(L)	800℃	PP	25.60mmol/g $p l a s t i c$	—	—	[10]
Ni/SiO₂(L)	800℃	PP	22.60mmol/g $p l a s t i c$	—	—	[10]
Ni-Fe/Al₂O₃	800℃	mix-plastics	31.80mmol/g $p l a s t i c$	—	—	[11]
Fe-Ni/MCM-41	800℃	mix-plastics	38.10mmol/g $p l a s t i c$	—	—	[12]
Ni-Co/ZSM-5	900℃	PP	28.70mmol/g $p l a s t i c$	—	—	[13]
Ni/ZSM-5	800℃	HDPE	64.50%	—	—	[14]
Ga-Mo/HZSM-5	600℃	HDPE	—	82% aromatics	—	[15]
Ni-WO₃/Al₂O₃-Hβ	—	PE	—	86.20% liquid	—	[16]
Ni/HZSM-5	400℃	HDPE	—	28.90% aromatics	—	[17]
Ni/Al₂O₃	800℃	HDPE	51.51mmol/g $p l a s t i c$	64.20% liquid	1.98% carbon	[18]
1% Ni/Y	600℃	HDPE	—	85% aromatics	—	[19]
1% Ga/Y	600℃	HDPE	—	93% aromatics	—	[19]
1% Fe/Y	600℃	HDPE	—	94% aromatics	—	[19]
1% Co/Y	600℃	HDPE	—	80% aromatics	—	[19]
Ga/HZSM-5	—	LLDPE	—	66.54% MAHs		[20]
CaO-Ga/HZSM-5	—	LLDPE	—	72.85% MAHs	—	[20]
P-Ga/HZSM-5	550℃	LDPE	—	90.70% MAHs	—	[21]
Ga-Na/HZSM-5	650℃	PP	—	67.20% aromatics	—	[22]
Ni/AC	700℃	mix-plastics	4.24%	—	34.50% carbon	[23]
Fe/AC	700℃	mix-plastics	1.97%	—	12.40% carbon	[23]
Fe-Ni/Al₂O₃(Sg)	800℃	PP	25.14mmol/g $p l a s t i c$	20.00% liquid	36.00% carbon	[24]
Fe/MgO	900℃	PP	—	—	33.30% carbon	[25]
Fe/Al₂O₃	800℃	HDPE	56.00%	20.00% liquid	36.90% carbon	[26]
Ni/Al₂O₃	800℃	PE	17.31mmol/g $p l a s t i c$	28.95% liquid	25.64% carbon	[27]
Ni/ZrO₂	800℃	PE	22.01mmol/g $p l a s t i c$	40.22% liquid	16.03% carbon	[28]
Ni/TiO₂	800℃	PE	20.74mmol/g $p l a s t i c$	30.72% liquid	26.53% carbon	[28]
Ni/Nb₂O₃	800℃	PE	12.04mmol/g $p l a s t i c$	34.84% liquid	8.51% carbon	[28]
Ni/Al₂O₃	800℃	PE	36.77mmol/g $p l a s t i c$	23.81% liquid	36.54% carbon	[28]
Fe-Ni-Mg	800℃	LDPE	35.27mmol/g $p l a s t i c$	26.71% liquid	32.30% carbon	[29]
Ni-Co/Al₂O₃	950℃	PE	—	—	25.50% carbon	[30]
Fe-Ni	800℃	mix-plastics	73.93%	8.80% liquid	50.90% carbon	[31]
Fe-Ni	700℃	PE	—	—	20.00% carbon	[32]
Fe/Al₂O₃	800℃	PP	58.70%	18.10% liquid	30.20% carbon	[33]

表1 常规催化热解聚乙烯的产物产率

催化剂	反应温度	塑料种类	氢气产率	液体产率	固体产率	文献
Fe/Al₂O₃	800℃	LDPE	50.60%	—	—	[9]
Ni/Al₂O₃	800℃	LDPE	36.60%	—	—	[9]
Co/Al₂O₃	800℃	LDPE	31.30%	—	—	[9]
Cu/Al₂O₃	800℃	LDPE	26.00%	—	—	[9]
Fe/SiO₂(L)	800℃	PP	25.60mmol/g $p l a s t i c$	—	—	[10]
Ni/SiO₂(L)	800℃	PP	22.60mmol/g $p l a s t i c$	—	—	[10]
Ni-Fe/Al₂O₃	800℃	mix-plastics	31.80mmol/g $p l a s t i c$	—	—	[11]
Fe-Ni/MCM-41	800℃	mix-plastics	38.10mmol/g $p l a s t i c$	—	—	[12]
Ni-Co/ZSM-5	900℃	PP	28.70mmol/g $p l a s t i c$	—	—	[13]
Ni/ZSM-5	800℃	HDPE	64.50%	—	—	[14]
Ga-Mo/HZSM-5	600℃	HDPE	—	82% aromatics	—	[15]
Ni-WO₃/Al₂O₃-Hβ	—	PE	—	86.20% liquid	—	[16]
Ni/HZSM-5	400℃	HDPE	—	28.90% aromatics	—	[17]
Ni/Al₂O₃	800℃	HDPE	51.51mmol/g $p l a s t i c$	64.20% liquid	1.98% carbon	[18]
1% Ni/Y	600℃	HDPE	—	85% aromatics	—	[19]
1% Ga/Y	600℃	HDPE	—	93% aromatics	—	[19]
1% Fe/Y	600℃	HDPE	—	94% aromatics	—	[19]
1% Co/Y	600℃	HDPE	—	80% aromatics	—	[19]
Ga/HZSM-5	—	LLDPE	—	66.54% MAHs		[20]
CaO-Ga/HZSM-5	—	LLDPE	—	72.85% MAHs	—	[20]
P-Ga/HZSM-5	550℃	LDPE	—	90.70% MAHs	—	[21]
Ga-Na/HZSM-5	650℃	PP	—	67.20% aromatics	—	[22]
Ni/AC	700℃	mix-plastics	4.24%	—	34.50% carbon	[23]
Fe/AC	700℃	mix-plastics	1.97%	—	12.40% carbon	[23]
Fe-Ni/Al₂O₃(Sg)	800℃	PP	25.14mmol/g $p l a s t i c$	20.00% liquid	36.00% carbon	[24]
Fe/MgO	900℃	PP	—	—	33.30% carbon	[25]
Fe/Al₂O₃	800℃	HDPE	56.00%	20.00% liquid	36.90% carbon	[26]
Ni/Al₂O₃	800℃	PE	17.31mmol/g $p l a s t i c$	28.95% liquid	25.64% carbon	[27]
Ni/ZrO₂	800℃	PE	22.01mmol/g $p l a s t i c$	40.22% liquid	16.03% carbon	[28]
Ni/TiO₂	800℃	PE	20.74mmol/g $p l a s t i c$	30.72% liquid	26.53% carbon	[28]
Ni/Nb₂O₃	800℃	PE	12.04mmol/g $p l a s t i c$	34.84% liquid	8.51% carbon	[28]
Ni/Al₂O₃	800℃	PE	36.77mmol/g $p l a s t i c$	23.81% liquid	36.54% carbon	[28]
Fe-Ni-Mg	800℃	LDPE	35.27mmol/g $p l a s t i c$	26.71% liquid	32.30% carbon	[29]
Ni-Co/Al₂O₃	950℃	PE	—	—	25.50% carbon	[30]
Fe-Ni	800℃	mix-plastics	73.93%	8.80% liquid	50.90% carbon	[31]
Fe-Ni	700℃	PE	—	—	20.00% carbon	[32]
Fe/Al₂O₃	800℃	PP	58.70%	18.10% liquid	30.20% carbon	[33]

图1 Ni/ZSM-5、Co/ZSM-5、Ni-Co/ZSM-5催化热解塑料制氢气的反应机理示意图[13]

图2 分子筛负载Ni催化废塑料制芳烃反应过程图[18]

图3 铁基催化剂热解塑料制CNTs和H2机理图[24]

图4 铁基、钴基、镍基催化剂微波热解塑料的反应机理[34]

表2 微波催化热解聚乙烯类塑料的产物产率

催化剂	反应温度	塑料种类	氢气产率	液体产率	固体产率	文献
Fe/Ni-CeO₂@CNTs	800℃	HDPE	91.50%	—	20.00% carbon	[39]
FeAlO _x	—	PE	48.10mmol/g $p l a s t i c$	—	—	[40]
FeAlO _x	550℃	HDPE	55.60mmol/g $p l a s t i c$	—	—	[41]
7%FeAlO _x	500℃	HDPE	86.30%	—	—	[42]
22%FeAlO _x	500℃	HDPE	93.70%	—	—	[42]
30%Fe/FeAlO _x	330℃	HDPE	47.03mmol/g $p l a s t i c$	—	—	[43]
Fe-Co-Al	800℃	LDPE	61.39mmol/g $p l a s t i c$	—	—	[44]
Ni-Fe-Al	700℃	LDPE	60.50mmol/g $p l a s t i c$	—	—	[45]
ZSM-5	450℃	LDPE	—	32.58% liquid	—	[46]
ZSM-5	560℃	LDPE	—	47.40% liquid	—	[47]
MCM-41/HY	450℃	LDPE	—	63.75% liquid	—	[48]
HZSM-5/MgO	500℃	LDPE	—	90% aromatics	—	[49]
NiO/HY	450℃	LDPE	—	56.53% liquid	—	[50]
Ni-Fe/Al₂O₃	800℃	PP	65.10%	27.70% liquid	33.50% carbon	[51]
Ni-La	800℃	LDPE	—	—	82.20% carbon	[52]
Ni-Fe-Al	—	PP、LDPE、HDPE	83.10%	—	—	[53]
Fe-Ni	—	PE	415.00mmol/g $p l a s t i c$	—	—	[54]
Ni₁Fe₃O _x	700℃	LDPE	60.20mmol/g $p l a s t i c$	1.20% liquid	36.50% carbon	[55]
Ni₁Co₃O _x	700℃	LDPE	63.20mmol/g $p l a s t i c$	0.80% liquid	41.40% carbon	[55]
Ni₃Co₂O _x	700℃	LDPE	63.50mmol/g $p l a s t i c$	0.80% liquid	41.50% carbon	[55]
Fe-Ni/SiC	800℃	LDPE	73.89%	—	—	[56]
Al₂O₃-NiFe₂O₄	400℃	HDPE	90.60%	7.50% liquid	78.00% carbon	[57]
Al₂O₃-ZnFe₂O₄	400℃	HDPE	80.00%	7.50% liquid	71.50% carbon	[57]
Al₂O₃-MgFe₂O₄	400℃	HDPE	75.50%	6.25% liquid	74.00% carbon	[57]

表2 微波催化热解聚乙烯类塑料的产物产率

催化剂	反应温度	塑料种类	氢气产率	液体产率	固体产率	文献
Fe/Ni-CeO₂@CNTs	800℃	HDPE	91.50%	—	20.00% carbon	[39]
FeAlO _x	—	PE	48.10mmol/g $p l a s t i c$	—	—	[40]
FeAlO _x	550℃	HDPE	55.60mmol/g $p l a s t i c$	—	—	[41]
7%FeAlO _x	500℃	HDPE	86.30%	—	—	[42]
22%FeAlO _x	500℃	HDPE	93.70%	—	—	[42]
30%Fe/FeAlO _x	330℃	HDPE	47.03mmol/g $p l a s t i c$	—	—	[43]
Fe-Co-Al	800℃	LDPE	61.39mmol/g $p l a s t i c$	—	—	[44]
Ni-Fe-Al	700℃	LDPE	60.50mmol/g $p l a s t i c$	—	—	[45]
ZSM-5	450℃	LDPE	—	32.58% liquid	—	[46]
ZSM-5	560℃	LDPE	—	47.40% liquid	—	[47]
MCM-41/HY	450℃	LDPE	—	63.75% liquid	—	[48]
HZSM-5/MgO	500℃	LDPE	—	90% aromatics	—	[49]
NiO/HY	450℃	LDPE	—	56.53% liquid	—	[50]
Ni-Fe/Al₂O₃	800℃	PP	65.10%	27.70% liquid	33.50% carbon	[51]
Ni-La	800℃	LDPE	—	—	82.20% carbon	[52]
Ni-Fe-Al	—	PP、LDPE、HDPE	83.10%	—	—	[53]
Fe-Ni	—	PE	415.00mmol/g $p l a s t i c$	—	—	[54]
Ni₁Fe₃O _x	700℃	LDPE	60.20mmol/g $p l a s t i c$	1.20% liquid	36.50% carbon	[55]
Ni₁Co₃O _x	700℃	LDPE	63.20mmol/g $p l a s t i c$	0.80% liquid	41.40% carbon	[55]
Ni₃Co₂O _x	700℃	LDPE	63.50mmol/g $p l a s t i c$	0.80% liquid	41.50% carbon	[55]
Fe-Ni/SiC	800℃	LDPE	73.89%	—	—	[56]
Al₂O₃-NiFe₂O₄	400℃	HDPE	90.60%	7.50% liquid	78.00% carbon	[57]
Al₂O₃-ZnFe₂O₄	400℃	HDPE	80.00%	7.50% liquid	71.50% carbon	[57]
Al₂O₃-MgFe₂O₄	400℃	HDPE	75.50%	6.25% liquid	74.00% carbon	[57]

图5 Ga/HZSM-5催化热解聚乙烯的反应路线[63]

图6 FeAlO x 催化剂作用下微波催化热解废塑料的机理[68]

图7 碳纤维布负载FeAlO x 催化剂作用下微波催化热解废塑料的机理[69]

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聚乙烯常规及微波催化热解产物分布特征的研究进展

Research progress based on conventional and microwave pyrolysis behavior of polyethylene

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