Research progress in aromatics production by biomass pyrolysis

doi:10.16085/j.issn.1000-6613.2024-1707

Abstract

Abstract:

Aromatic hydrocarbons are important chemical raw materials, especially monocyclic aromatic hydrocarbons (MAHs), which have high utilization value. At present, the production of MAHs mainly relies on the catalytic conversion of fossil fuels. With the depletion of fossil energy, developing a pyrolytic method using biomass as raw materials to produce aromatic hydrocarbons has the advantages of environmental protection and low cost, and is of great significance for the efficient utilization of biomass in China and the realization of the carbon peaking and carbon neutrality goals. Hence, the research progress of biomass pyrolysis to produce MAHs, including co-pyrolysis feedstocks, biomass pretreatment methods, catalyst selection and modification, and reaction mechanism were summarized, and the influence of ZSM-5 zeolite molecular sieve on the generation of aromatic hydrocarbons were analyzed. Multistage porous ZSM-5, metal-modified ZSM-5, co-pyrolysis of ZSM-5 with metal oxides, and nano-ZSM-5 were reviewed. The effects and mechanisms of pore structure, acid site distribution, micro-morphology and co-pyrolysis metal oxide types of ZSM-5 on the generation of aromatic hydrocarbons were evaluated. Finally, the future research directions of catalytic pyrolysis of biomass to produce aromatic hydrocarbons were proposed.

Key words: biomass, aromatic hydrocarbons, pyrolysis, molecular sieve, catalytic reaction

摘要：

芳烃是一类重要的化工原料，尤其是其中单环芳烃，具有较高的利用价值。当前单环芳烃制备主要依靠化石燃料的催化转化，随着化石能源的日益枯竭，开发以生物质为原料热解制备芳烃的技术具有环保、低成本的优势，且对于我国高效利用生物质、全面推进双碳目标的实现具有重要意义。本文主要总结了生物质热解制备单环芳烃的研究进展，从共热解原料、生物质预处理方法、催化剂的选择和改性、反应机理等方面进行了归纳，并重点分析了ZSM-5沸石分子筛对于芳烃生成的影响，综述了多级孔ZSM-5、金属改性ZSM-5、ZSM-5与金属氧化物共热解、纳米ZSM-5的研究进展，分析了ZSM-5的孔结构、酸性位点分布、微观形貌、共热解金属氧化物类型等因素对芳烃生成的作用与机理，最后展望了生物质催化热解制备芳烃的未来研究方向。

关键词: 生物质, 芳烃, 热解, 分子筛, 催化反应

CLC Number:

TIAN Xu, SHAO Jing’ai, JIANG Hao, ZHANG Junjie, CHEN Jianfeng, YANG Haiping, CHEN Hanping. Research progress in aromatics production by biomass pyrolysis[J]. Chemical Industry and Engineering Progress, 2025, 44(11): 6187-6199.

田旭, 邵敬爱, 蒋好, 张俊杰, 陈剑峰, 杨海平, 陈汉平. 生物质热解制备芳烃的研究进展[J]. 化工进展, 2025, 44(11): 6187-6199.

Figures/Tables 11

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催化剂	含氧化合物	烃类总量	烯烃	芳烃	烷烃
无催化剂	58.7	31.3	—	—	—
Mo-Ni/γ-Al₂O₃	7.2	86.4	35.3	31.4	13.8
Mo-Co/γ-Al₂O₃	4.2	92.6	33.4	28.9	25.7

催化剂	含氧化合物	烃类总量	烯烃	芳烃	烷烃
无催化剂	58.7	31.3	—	—	—
Mo-Ni/γ-Al₂O₃	7.2	86.4	35.3	31.4	13.8
Mo-Co/γ-Al₂O₃	4.2	92.6	33.4	28.9	25.7

样品	S_BET/m²·g^-1	S_micro/m²·g^-1	S_ext/m²·g^-1	V_total/cm³·g^-1	V_micro/cm³·g^-1	V_meso/cm³·g^-1
HZSM-5	360.11	263.23	96.88	0.21	0.11	0.10
N-ZSM-5	472.39	222.27	250.22	0.70	0.09	0.61

样品	S_BET/m²·g^-1	S_micro/m²·g^-1	S_ext/m²·g^-1	V_total/cm³·g^-1	V_micro/cm³·g^-1	V_meso/cm³·g^-1
HZSM-5	360.11	263.23	96.88	0.21	0.11	0.10
N-ZSM-5	472.39	222.27	250.22	0.70	0.09	0.61

热解原料	反应器	催化剂选择	催化剂与原料质量比	热解温度/℃	催化温度/℃	芳烃产率/%	苯在芳烃中的占比/%	参考文献
竹材	固定床	Zn-P/HZSM-5	2∶1	450	550	72.28^①	16.57	[47]
木粉	Py-GC/MS	10%Mo/ZSM-5	10∶1	600	600	42.68^①	—	[43]
纤维素	Py-GC/MS	改性多级孔ZSM-5	20∶1	600	600	42.2^①	—	[63]
纤维素	Py-GC/MS	酸处理ZSM-5	1∶1	500	500	40.9^①	24.67	[35]
花生壳	Py-GC/MS	Zn改性ZSM-5	1∶1	550	550	22^①	—	[53]
微藻	Py-GC/MS	Cu改性HZSM-5（硅铝比80）	5∶1	550	550	21.16^①	11.81	[32]
纤维素二糖	Py-GC/MS	Fe（1.4%）修饰HZSM-5	10∶1	500	500	18.20^②	12.12	[45]
杨木木屑	Py-GC/MS	Fe-Ni/ZSM-5	1∶1	550	550	16.82^① 62.84mg/g^③	16	[34]
云南松	固定床	Zn负载HZSM-5	2∶1	450	500	14.94^①	7.5	[64]
松木木屑	Py-GC/MS	Ti(SO₄)₂-Mo₂N/HZSM-5	4∶3	650	650	10.92^①	42	[65]
木质素	固定床	负载3% Fe ZSM-5	2∶1	600	600	8.94^②	6.3	[46]
半纤维/素	非原位固定床	负载3% Fe ZSM-5	2∶1	600	600	6.77^①	33	[55]
玉米秸秆	Py-GC/MS	Zn/ZSM-5（硅铝比40）	1∶1	500	500	183mg/g^③	15.4	[54]
樟木	Py-GC/MS	微介孔ZSM-5	4∶1	600	600	91.84mg/g^③	12.82	[39]
玉米秸秆	Py-GC/MS	Fe浸渍HZSM-5	1∶1	800	800	25.43mg/g^③	—	[66]
玉米秸秆/HDPE 1∶1	TG-MS-FTIR	Cu改性HZSM-5	1∶1	550	550	59.82^①	—	[52]
木质素/LDPE1∶3	管式炉	Cu₂O/HZSM-5（5%）	1∶2	700	700	50.39^①	13	[18]
木耳菌渣/废聚烯烃 1∶1	固定床	Al₂O₃/ZSM-51∶1	1∶1	600	600	63.11^④	—	[61]
木屑	热探针热解装置	ZSM-5/CaO4∶1	5∶1	600	600	40^①	8.78	[59]
污水浮渣/玉米秸秆 2∶1	微波热解固定床	CaO/HZSM-51∶4	1∶1	550	550	35.77^①	—	[62]
水稻秸秆/PVC	Py-GC/MS	CaO/HZSM-5	1∶1	500	500	34.34^④	—	[67]
竹渣/废轮胎 1∶4	固定床	HZSM-5/CaO1∶1	2∶1	600	600	33.324^①	10.35	[37]
竹材/LDPE 1∶1	固定床	MgO/HZSM-52∶1	2∶1	450	550	20.39^①	12.62	[60]
纤维素	双催化固定床	CaO 15% ZSM-5 85%	2∶1	600	600	13.42^②	15	[57]
油饼	Py-GC/MS	Org-CaO/NZSM-51∶1	6∶1	500	550	75^①	—	[24]
水葫芦/废轮胎	固定床	多层MFI纳米片沸石	4∶1	1000	1000	69.18^④	—	[68]
山茶籽壳	管式炉	N-ZSM-5	3∶1	500	500	50.6^①	—	[42]