生物质与塑料共催化热解制备芳烃化合物研究进展

韩冬; 孙来芝; 陈雷; 杨双霞; 李天津; 谢新苹; 许美荣; 唐文东; 赵保峰; 司洪宇; 华栋梁

doi:10.1016/S1872-5813(23)60401-3

生物质与塑料共催化热解制备芳烃化合物研究进展

doi: 10.1016/S1872-5813(23)60401-3

韩冬^1,,
孙来芝^1, ,,
陈雷^1,,
杨双霞^1,,
李天津^1,,
谢新苹^1,,
许美荣^1,,
唐文东^2,,
赵保峰^1,,
司洪宇^1,,
华栋梁^1,

1.
齐鲁工业大学 (山东省科学院) 能源研究所山东省生物质气化技术重点实验室, 山东济南 250014
2.
山东艾蒙特新材料有限公司, 山东东营 257500

基金项目: 山东省自然科学基金（ZR2023MB040，ZR2022MB059, ZR2021QB156），山东省重点研发计划（重大科技创新工程）（2022CXGC010701），山东省科技型中小企业提升项目（2023TSGC0460），济南市“新高校20条”项目（202228018，2021GXRC053）和科教产融合试点工程项目（2022JBZ02-03，2023PX086，2022PX009）资助

详细信息

通讯作者:
Tel: 13220597603, E-mail：sunlz@sderi.cn

中图分类号: TK6
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出版历程
- 收稿日期: 2023-08-03
- 修回日期: 2023-10-20
- 录用日期: 2023-10-20
- 网络出版日期: 2023-12-05
- 刊出日期: 2024-04-03

Review on the progress in the production of aromatic hydrocarbons by co-catalytic pyrolysis of biomass and plastics

HAN Dong^1
,,
SUN Laizhi^{1
, ,},
CHEN Lei^1
,,
YANG Shuangxia^1
,,
LI Tianjin^1
,,
XIE Xinping^1
,,
XU Meirong^1
,,
TANG Wendong^2
,,
ZHAO Baofeng^1
,,
SI Hongyu^1
,,
HUA Dongliang^1
,

1.
Energy Research Institute of Qilu University of Technology (Shandong Academy of Sciences), Shandong Key Laboratory of Biomass Gasification Technology, Jinan 250014, China
2.
Shandong EMT New Material Co, Ltd, Dongying 257500, China

Funds: The project was supported by the Natural Science Foundation of Shandong Province (ZR2023MB040, ZR2022MB059, ZR2021QB156), the Key Research and Development Program of Shandong Province (2022CXGC010701), Shandong Province Science and Technology Small and Medium Enterprises Improvement Project(2023TSGC0460), Jinan City’s “20 New Colleges and Universities” project (202228018, 2021GXRC053), the Education and Industry Integration Innovation Pilot Project (2022JBZ02-03，2023PX086，2022PX009).

摘要

摘要: 芳烃，尤其苯、甲苯、二甲苯（BTX）等单环芳烃，是化工行业重要的基础原料，主要来源于化石燃料的催化重整与热裂解。生物质与塑料共催化热解制芳烃具有高效、环保、低成本、高选择性等优点，可以解决因生物质富氧、贫氢的特点造成热解产物氧含量高、芳烃收率和选择性低等问题。本工作主要综述了生物质与塑料共催化热解制备芳烃化合物的研究进展，介绍了共催化热解反应原料类别，重点论述了共催化热解反应催化剂，总结归纳了共催化热解双烯合成、烃池协同等反应机理。展望了生物质与塑料共催化热解未来的研究重心与发展方向，即通过研制高活性、高稳定性的改性分子筛催化剂来提高芳烃产率。
- 生物质 /
- 塑料 /
- 共催化热解 /
- 芳烃 /
- 催化剂
Abstract: Aromatic hydrocarbons, especially monocyclic aromatic hydrocarbons such as benzene, toluene, and xylene (BTX), are important basic raw materials in the chemical industry, which are mainly derived from the catalytic reforming and thermal cracking of fossil fuels. The co-catalytic pyrolysis of biomass and plastic to produce aromatics has the advantages of high efficiency, environmental protection, low cost, and high selectivity. It can solve the problems of pyrolysis products such as high oxygen content, low aromatics yield, and low selectivity, which are caused by the characteristics of biomass rich in oxygen and poor in hydrogen. This article reviewed the research progress of co-catalytic pyrolysis of biomass and plastics to prepare aromatic compounds. Firstly, the types of raw materials for co-catalytic pyrolysis were introduced, and then the co-catalytic pyrolysis catalysts were emphasized. The reaction mechanisms of co-catalytic pyrolysis of biomass and plastics, such as the synthesis of dienes and hydrocarbon pool synergy were summarized. Finally, the future research focus and development direction of co-catalytic pyrolysis of biomass and plastics were proposed, which is developing the highly active and stable modified molecular sieve catalysts in order to improve the aromatics yield.
- biomass /
- plastic /
- co catalytic pyrolysis /
- aromatic hydrocarbon /
- catalyst

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FIG. 3073. FIG. 3073.

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图 1 AAEMs对纤维素与HDPE共热解的催化作用示意图^[40]

Figure 1 Schematic diagram of the catalytic effect of AAEMs on the co-pyrolysis of cellulose and HDPE^[40](with permission from Elsevier Publication)

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图 2 CaO对PVC与纤维素混合物非原位催化共热解反应效果示意图^[42]

Figure 2 Schematic diagram of the effect of CaO on the non-in-situ catalytic co-pyrolysis reaction of PVC cellulose mixture ^[42](with permission from ACS Publication)

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图 3 HZSM-5分子筛催化纤维素与PE共热解的化学机理示意图^[51]

Figure 3 Schematic diagram of the chemical mechanism of HZSM-5 molecular sieve catalyzed co-pyrolysis of cellulose and PE ^[51] (with permission from Springer Nature Publication)

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图 4 Ni-MCM-41催化剂对纤维素与PP共热解反应影响示意图^[60]

Figure 4 Schematic diagram of the influence of Ni-MCM-41 catalyst on the co-pyrolysis reaction of cellulose and PP^[60] (with permission from ACS Publication)

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图 5 ZSM-5、GaMFI、DS-GaMFI三种沸石催化效果示意图^[65]

Figure 5 Schematic diagram of catalytic effect of ZSM-5, GaMFI and DS-GaMFI zeolites^[65] (with permission from ACS Publication)

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图 6 纤维素与HDPE共催化热解制芳烃机理示意图^[70]

Figure 6 Schematic diagram of co-catalytic pyrolysis of cellulose and HDPE to aromatics ^[70] (with permission from Chemical Industry Press Publication)

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图 7 棕榈仁饼与PS共催化热解提质生物油反应途径示意图^[72]

Figure 7 Schematic diagram of reaction pathway of co-catalytic pyrolysis of palm kernel cake and PS to enhance bio-oil ^[72] (with permission from Elsevier Publication)

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图 8 木聚糖与PP在CaO催化下共热解生成芳烃的反应途径示意图^[74]

Figure 8 Schematic diagram of aromatics formation by co-pyrolysis of xylan and PP catalyzed by CaO ^[74] (with permission from Elsevier Publication)

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表 1 生物质与塑料共催化热解制备芳烃化合物常用原料、催化剂、反应条件、催化性能

Table 1 Common raw materials, catalysts, reaction conditions, and catalytic performance for preparation of aromatic compounds by co-catalytic pyrolysis of biomass and plastics

Raw material		Catalyst	Reaction conditions				Bio-oil/ Aromatic hydrocarbon yield /%	Main products in bio-oil	Ref.
biomass	plastic	Catalyst	ratio of raw material to mass	ratio of raw material to catalyst	pyrolysis temp. /℃	catalytic temp. /℃	Bio-oil/ Aromatic hydrocarbon yield /%	Main products in bio-oil	Ref.
Cellulose	HDPE	Na	1∶1		550	550		olefin	[40]
Bamboo	LDPE	CaO	1∶1	1∶2	450	550	9.76^a	alkanes, olefins	[37]
Cellulose	PE	MgO	1∶1	4∶1	700	700		olefin, aromatics	[41]
Cellulose	PVC	CaO	19∶1	1∶1	350	350	24.9^a	PAHs	[42]
Bamboo	LDPE	CeO₂	1∶1	1∶2	450	550		hydrocarbons	[37]
Poplar wood-polypropylene composite		Fe₂O₃	1∶1	1∶4	600	600		hydrocarbons	[44]
Chili straw	PP	HZSM-5	1∶1	1∶1	750	750	17.34^b	alkanes, olefins	[50]
Cellulose	LDPE	ZSM-5	1∶1	1∶15	650	650	47.46^b	aromatic	[52]
Wheat straw	Municipal Plastic Waste	β-zeolites	1∶1	2∶1	550	550	32.5^b	aromatic	[54]
Mandarin peel	HDPE	HY	1∶1	1∶1	600	600	5.06^b		[55]
Poplar wood-polypropylene composite		HUSY	1∶1	1∶4	600	600	60.83^b	aromatic	[56]
Wheat straw	HDPE	1%Zn-HZSM-5	3∶1	10∶1	550	550	25.12^b	acids, aromatics	[58]
Corn stalk	PP	1%Zn-3%Al-MCM-41	1∶1	1∶10	600	600	24.31^b	aromatic	[59]
Microcrystalline cellulose powder	PP	Ni-MCM-41	1∶1	1∶10	650	650	84.6^c	olefin, aromatics	[60]
Poplar wood sawdust	HDPE	（0.5 mol/L）ZSM-5	1∶1	1∶1	500	500	12.72^b	alkanes, olefins	[63]
Torrefied poplar wood sawdust	HDPE	Hierarchical HZSM-5	1∶1	1∶1	550	550	71.75^d	aromatic	[64]
Cellulose	PP	DS-GaMFI	1∶2	1∶15	550	550	52.7^b	aromatic	[65]
^a: bio-oil yield; ^b: proportion of aromatics in bio-oil; ^c: proportion of aromatics and olefins in bio-oil; ^d: proportion of monocyclic aromatic hydrocarbons in hydrocarbons.

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