生物质与塑料催化共热解技术研究进展

doi:10.16085/j.issn.1000-6613.2022-1316

化工进展 ›› 2023, Vol. 42 ›› Issue (5): 2655-2665.DOI: 10.16085/j.issn.1000-6613.2022-1316

生物质与塑料催化共热解技术研究进展

王志伟¹^,²(), 郭帅华¹^,², 吴梦鸽¹^,², 陈颜¹^,², 赵俊廷¹^,², 李辉³, 雷廷宙⁴

^1.河南工业大学环境工程学院，河南郑州 450001
^2.河南工业大学碳中和研究院，河南郑州 450001
^3.湖南省林业科学院省部共建木本油料资源利用国家重点实验室，湖南长沙 410004
^4.常州大学城乡矿山研究院，江苏常州 213164

收稿日期:2022-07-13 修回日期:2022-08-18 出版日期:2023-05-10 发布日期:2023-06-02
通讯作者: 王志伟
作者简介:王志伟（1980—），男，博士，研究员，研究方向为生物质热化学转化技术、有机固体废弃物高效处理技术。E-mail：bioenergy@163.com。
基金资助:
国家重点研发项目(2019YFD1100604);中国欧盟地平线项目(MJ-2020-D-09);中原科技创新领军人才项目(194200510028)

Recent advances on catalytic co-pyrolysis of biomass and plastic

WANG Zhiwei¹^,²(), GUO Shuaihua¹^,², WU Mengge¹^,², CHEN Yan¹^,², ZHAO Junting¹^,², LI Hui³, LEI Tingzhou⁴

^1.School of Environmental Engineering, Henan University of Technology, Zhengzhou 450001, Henan, China
^2.Institute for Carbon Neutrality, Henan University of Technology, Zhengzhou 450001, Henan, China
^3.State Key Laboratory of Utilization of Woody Oil Resource, Hunan Academy of Forestry, Changsha 410004, Hunan, China
^4.Institute of Urban and Rural Mining, Changzhou University, Changzhou 213164, Jiangsu, China

Received:2022-07-13 Revised:2022-08-18 Online:2023-05-10 Published:2023-06-02
Contact: WANG Zhiwei

摘要/Abstract

摘要：

生物质是唯一一种可再生碳源，其高效利用是解决能源与环境问题的纽带。近年来，基于化石能源的塑料制品使用和废弃量快速增加，其难于自然降解，对环境造成严重威胁。生物质与塑料的催化共热解技术能够得到选择性更高的产品，进而提升高附加值产物的产率和品质，是生物质与塑料规模化利用的重要方向。本文从生物质与塑料高效转化的角度出发，梳理了生物质与塑料催化共热解技术研究进展，对生物质与塑料共热解机理、ZSM-5基催化剂共热解、过渡金属基催化剂共热解、碱/碱土金属催化剂共热解、多催化剂共热解等不同种类的催化共热解研究前沿进行了综述，并对比了原位催化和非原位催化的共热解方式，展望了生物质与塑料催化共热解的主要技术和发展方向，以期为生物质与塑料的高效协同转化提供方法参考和研究思路。

关键词: 生物质, 塑料, 共热解, 催化剂, 催化方式

Abstract:

Biomass is the only renewable carbon source, and its efficient utilization is the link to solve energy and environmental problems. In recent years, waste of plastic products based on fossil energy has increased rapidly because of their huge consumption. However, plastic is difficult to degrade naturally, thus posing a serious threat to the environment. The catalytic co-pyrolysis technology of biomass and plastic can obtain more selective products, and improve the yield and quality of products, which is an important direction for large-scale utilization of biomass and plastic. From the perspective of efficient conversion of biomass and plastic, recent advances on catalytic co-pyrolysis of biomass and plastic were summarized in the paper. Mechanism of co-pyrolysis of biomass and plastic, and advances of the co-pyrolysis with different types of catalyst, such as ZSM-5-based catalyst, transition metal-based catalyst, alkali/alkaline earth metal catalyst, and multi-catalysts, were reviewed. Catalytic co-pyrolysis with in-situ and non-in-situ mode were compared. Prospects for the primary technology and future development direction of catalytic co-pyrolysis of biomass and plastic were pursued, which may provide technical references and research ideas for the efficient synergistic conversion of biomass and plastic.

Key words: biomass, plastic, co-pyrolysis, catalyst, catalytic mode

中图分类号:

TK06

王志伟, 郭帅华, 吴梦鸽, 陈颜, 赵俊廷, 李辉, 雷廷宙. 生物质与塑料催化共热解技术研究进展[J]. 化工进展, 2023, 42(5): 2655-2665.

WANG Zhiwei, GUO Shuaihua, WU Mengge, CHEN Yan, ZHAO Junting, LI Hui, LEI Tingzhou. Recent advances on catalytic co-pyrolysis of biomass and plastic[J]. Chemical Industry and Engineering Progress, 2023, 42(5): 2655-2665.

图/表 8

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原料	生物质与塑料比例	催化剂	原料与催化剂比例	热解温度 /℃	主要产物	催化效果	参考文献
烘焙木材/PS	1∶4	HZSM-5	9∶1	500~650	酚类化合物、芳香烃和其他化合物	芳烃产率提高接近70%	[45]
纤维素/LDPE	1∶1	HZSM-5	1∶1	600	芳香烃	反应活性有效提高，反应活化能显著降低	[36]
烘焙黄杨/HDPE	1∶1	HZSM-5	1∶10	600	芳香化合物	芳香烃产率高于总值	[46]
小麦秸秆/PS	1∶1	HZSM-5	2∶1	500	有机液体产品	与非催化结果相比，HZSM-5在CCP中的应用显著降低了总液体产率，增加了气态产物	[47]
纤维素/PE	1∶1	HZSM-5	1∶2	650	热解油	HZSM-5促进了共热解的Diels-Alder反应，导致醇和糖化合物的还原	[48]
玉米芯/PE	1∶1	HZSM-5	1∶20	600	芳香烃和固体残渣	增加芳香烃和烯烃，而降低固体残渣和碳氧化物的产量	[49]
柳枝/HDPE	1∶1	HZSM-5	1∶15	650	芳族烃	在催化剂的作用下，共热解的芳香烃产率都高于柳枝或单独的HDPE热解	[50]

原料	生物质与塑料比例	催化剂	原料与催化剂比例	热解温度 /℃	主要产物	催化效果	参考文献
烘焙木材/PS	1∶4	HZSM-5	9∶1	500~650	酚类化合物、芳香烃和其他化合物	芳烃产率提高接近70%	[45]
纤维素/LDPE	1∶1	HZSM-5	1∶1	600	芳香烃	反应活性有效提高，反应活化能显著降低	[36]
烘焙黄杨/HDPE	1∶1	HZSM-5	1∶10	600	芳香化合物	芳香烃产率高于总值	[46]
小麦秸秆/PS	1∶1	HZSM-5	2∶1	500	有机液体产品	与非催化结果相比，HZSM-5在CCP中的应用显著降低了总液体产率，增加了气态产物	[47]
纤维素/PE	1∶1	HZSM-5	1∶2	650	热解油	HZSM-5促进了共热解的Diels-Alder反应，导致醇和糖化合物的还原	[48]
玉米芯/PE	1∶1	HZSM-5	1∶20	600	芳香烃和固体残渣	增加芳香烃和烯烃，而降低固体残渣和碳氧化物的产量	[49]
柳枝/HDPE	1∶1	HZSM-5	1∶15	650	芳族烃	在催化剂的作用下，共热解的芳香烃产率都高于柳枝或单独的HDPE热解	[50]

原料	温度/℃	转换范围/%	活化能/kJ·mol^-1	指前因子/min^-1	参考文献
纤维素/PE-Ni-1	223~319	5.08~30.31	41.63	3.04×10²	[54]
纤维素/PE-Co-1	409~509	40.14~94.16	71.52	2.40×10⁴
纤维素/PE-Co-1	211~253	5.05~20.16	67.20	3.81×10⁵
纤维素/PE-Fe-1	416~484	38.92~79.64	72.52	2.45×10⁴
纤维素/PE-Fe-1	178~271	5.78~25.55	29.88	2.99×10¹
纤维素/PE-Mn-1	406~499	39.89~90.15	67.39	1.09×10⁴
纤维素/PE-Mn-1	216~267	7.86~26.93	52.14	8.88×10³
纤维素/PE-Ni-0.5	393~501	75.22	101.43	3.75×10⁶	[55]
纤维素/PE-Ni-0.5	185~402	28.89	14.08	1.93×10^-1
纤维素/PE-Co-0.5	402~500	61.95	91.65	9.20×10⁵
纤维素/PE-Co-0.5	207~392	24.11	8.99	4.96×10²
纤维素/PE-Fe-0.5	392~537	55.02	51.32	5.62×10²
纤维素/PE-Fe-0.5	212~390	15.65	7.79	2.38×10²
纤维素/PE-Mn-0.5	390~498	72.42	93.76	1.03×10⁶
纤维素/PE-Mn-0.5	231~396	21.08	23.50	1.23×10⁰

原料	温度/℃	转换范围/%	活化能/kJ·mol^-1	指前因子/min^-1	参考文献
纤维素/PE-Ni-1	223~319	5.08~30.31	41.63	3.04×10²	[54]
纤维素/PE-Co-1	409~509	40.14~94.16	71.52	2.40×10⁴
纤维素/PE-Co-1	211~253	5.05~20.16	67.20	3.81×10⁵
纤维素/PE-Fe-1	416~484	38.92~79.64	72.52	2.45×10⁴
纤维素/PE-Fe-1	178~271	5.78~25.55	29.88	2.99×10¹
纤维素/PE-Mn-1	406~499	39.89~90.15	67.39	1.09×10⁴
纤维素/PE-Mn-1	216~267	7.86~26.93	52.14	8.88×10³
纤维素/PE-Ni-0.5	393~501	75.22	101.43	3.75×10⁶	[55]
纤维素/PE-Ni-0.5	185~402	28.89	14.08	1.93×10^-1
纤维素/PE-Co-0.5	402~500	61.95	91.65	9.20×10⁵
纤维素/PE-Co-0.5	207~392	24.11	8.99	4.96×10²
纤维素/PE-Fe-0.5	392~537	55.02	51.32	5.62×10²
纤维素/PE-Fe-0.5	212~390	15.65	7.79	2.38×10²
纤维素/PE-Mn-0.5	390~498	72.42	93.76	1.03×10⁶
纤维素/PE-Mn-0.5	231~396	21.08	23.50	1.23×10⁰

原料	生物质与塑料比例	催化剂	原料与催化剂比例	热解温度/℃	主要产物	催化效果	参考文献
稻秆/LDPE	4∶1	ZSM-5/Co	4∶1	550	—	Co/ZSM-5催化剂可降低纤维素和LDPE共热解过程中的活化能	[67]
小麦秸杆/PS	1∶1	HZSM-5/MZSM-5s	2∶1	500	有机液体产品	HZSM-5和MZSM-5在CCP中显著降低了总液体产率，增加了气态产物	[47]
木质素/LDPE	1∶0、2∶1、1∶1，1∶2、1∶3、0∶1	HZSM-5/MgO	1∶0、1∶2、1∶1、2∶1	450、500、550、600	气体、焦油、热解油	HZSM-5提高了芳烃的产量，而MgO促进了生产酚类的烷基化	[69]
玉米秸秆/LDPE	1∶5、1∶2、1∶1、2∶1、5∶1	HZSM-5/CeO₂	1∶1、2∶1、3∶1、4∶1、6∶1、8∶1	550	MAHs	在串联催化床中烃类的产率最高，单环芳烃的选择性最高	[70]
甘蔗渣/PS	1∶1	HZSM-5和CaO/MgO	1∶1	550	热解油	促进芳香烃的形成，抑制聚芳香烃和液体产率中的含氧物	[72]
竹屑/LDPE	1∶4、1∶3、1∶1、3∶2、3∶1	HZSM-5和 CeO₂/γ-Al₂O₃	—	600	芳族烃	与单独的HZSM-5相比，芳香烃的产率增加了34%	[74]
甘蔗渣/PET	1∶1	HZSM-5和 Na₂CO₃/γ-Al₂O₃	1∶5	700	总芳烃	该组合催化剂提高了芳香烃和烯烃化合物的产率，减少了焦炭的形成	[64]

生物质与塑料催化共热解技术研究进展

Recent advances on catalytic co-pyrolysis of biomass and plastic

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名称	缩写
索康美孚沸石-5，zeolite socony mobil-5	ZSM-5
高密度聚乙烯，high-density polyethylene	HDPE
低密度聚乙烯，low-density polyethylene	LDPE
非催化共热解，non catalytic co-pyrolysis	NCCP
催化共热解，catalytic co-pyrolysis	CCP
热重分析，thermogravimetric analysis	TGA
分析热裂解-气相色谱/质谱，pyrolyzer coupled with gas chromatography and mass spectrometry	Py-GC/MS
Flynn-Wall-Ozawa	FWO
单芳烃，monoaromatic hydrocarbons	MAHs
多芳烃，polycyclic hydrocarbons	PAHs
聚乙烯，polyethylene	PE
聚丙烯，polypropylene	PP
聚苯乙烯，polystyrene	PS
氢交换索康美孚沸石-5，hydrogen exchanged zeolite socony mobil-5	HZSM-5
碱/碱土金属，alkali/alkaline earth metals	AAEMs
有机相，organic products	OP
水相，aqueous products	AP
萘及其衍生物，naphthalene and its derivatives	NIDs
聚对苯二甲酸乙二醇酯，polyethylene terephthalate	PET
苯系物，benzene, toluene, ethylbenzene and xylene	BTEXs

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