非贵金属催化剂用于丙烷脱氢的研究进展

doi:10.19964/j.issn.1006-4990.2023-0274

摘要/Abstract

摘要：

丙烯是一种重要的工业原料，主要用于生产聚丙烯、丙烯腈、异丙醇、丙酮和环氧丙烷等。随着对丙烯需求的日益增长，丙烷脱氢技术已被广泛应用于丙烯工业生产中。铂基、铬基催化剂虽然在丙烷脱氢反应中的活性很高，却容易中毒失活。金属氧化物作为可替代型非贵金属催化剂被人们广泛关注。首先，介绍金属氧化物催化丙烷脱氢的反应路径及失活机理，指出增强C—H活化能力、缓解活性组分重构及还原是提高金属氧化物丙烷脱氢性能的关键。然后，对几种代表性的金属氧化物催化剂进行了详细的综述，总结归纳各类催化剂的作用机制及活性物种，并分析讨论相应催化剂存在的问题。最后提出未来丙烷脱氢催化剂的重点研究方向，有望为低碳烷烃活化直接制取化学品提供新的思路。

关键词: 丙烷脱氢, 金属氧化物, 活性位点, 反应路径, 稳定性, 非贵金属催化剂

Abstract:

Propylene is an important industrial raw material mainly used in the production of polypropylene，acrylonitrile，isopropyl alcohol，acetone and propylene oxide.With the increasing demand for propylene，the technology of propane dehydrogenation has been widely used in the industrial production of propylene.Although platinum-based and chromium-based catalysts have high activity in propane dehydrogenation，they are also prone to poisoning and deactivation.Metal oxides have attracted widespread attention as alternative non-precious metal catalysts.Firstly，the reaction pathway and deactivation mechanism of propane dehydrogenation catalyzed by metal oxides were introduced.It was pointed out that enhancing the C—H activation ability，alleviating the reconstruction and reduction of active components were the key to improving the propane dehydrogenation performance of metal oxide catalysts.Then，several representative metal oxide catalysts were reviewed in detail，the mechanism of action and active species of various catalysts were summarized，and the existing problems of corresponding catalysts were analyzed and discussed.Finally，key research directions for future propane dehydrogenation catalysts were proposed，which was expected to provide new ideas for the direct production of chemicals through the activation of low-carbon alkanes.

Key words: propane dehydrogenation, metal oxides, active site, reaction pathway, stability, non-precious metal catalysts

中图分类号:

TQ138

王延苏, 刘国柱, 于海斌. 非贵金属催化剂用于丙烷脱氢的研究进展[J]. 无机盐工业, 2023, 55(12): 1-11.

WANG Yansu, LIU Guozhu, YU Haibin. Research progress of non-precious metal catalysts for propane dehydrogenation[J]. Inorganic Chemicals Industry, 2023, 55(12): 1-11.

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催化剂	反应温度/℃	反应原料比	丙烷初始转化率/%	丙烯选择性/%	失活速率K_d/h^-1
VO _x /ZrO₂^［13］	550	φ（C₃H₈）∶φ（H₂）∶φ（N₂）=7∶36∶7	25	85	0.549
VO _x /Al₂O₃^［14］	600	φ（C₃H₈）∶φ（H₂）∶φ（N₂）=7∶7∶11	32	约94	0.245
Mo－V－O^［15］	550	φ（C₃H₈）∶φ（N₂）=19∶81	36	89
Ga₈Al₂O₁₅^［16］	500	φ（C₃H₈）∶φ（N₂）=1∶39	49.7	91.7	0.086
［Fe］ZSM-5（MFI）^［17］	530		约7.2	约78
Sn-HMS^［18］	600	φ（C₃H₈）∶φ（N₂）=5∶95	约40	约90
SnO₂/SiO₂^［19］	600	φ（C₃H₈）∶φ（N₂）=5∶95	约30	约85
Fe_Ⅱ/SiO₂^［9］	650	φ（C₃H₈）∶φ（Ar）=3∶97	4.9	>99
Co-Al₂O₃-HT^［20］	590	φ（C₃H₈）∶φ（H₂）∶φ（N₂）=1∶0.8∶3.2	23	约97	0.06
VO _x /meso-Al₂O₃^［21］	510	φ（C₃H₈）∶φ（N₂）=4∶1	70	约85	0.169
GaO _x /SiO₂^［22］	580	φ（C₃H₈）∶φ（N₂）=1∶10	65	约90	0.136
Co–Al₂O₃–IMP^［20］	590	φ（C₃H₈）∶φ（H₂）∶φ（N₂）=1：0.8：3.2	21.2	94.6	0.16
Co（II）/SiO₂^［23］	550	φ（C₃H₈）∶φ（Ar）=20∶80	710	72	0.07
Co/SiO₂^［24］	550	φ（C₃H₈）∶φ（He）=3∶97	3.5	92	0.008 5
0.5CoSiBeta^［25］	600	φ（C₃H₈）∶φ（N₂）=5∶95	19	98.2	0.04
Co-Zr/SiO₂^［24］	550	φ（C₃H₈）∶φ（He）=3∶97	8.7	96	0.011 5
ZnO/Beta^［26］	600	φ（C₃H₈）∶φ（N₂）=5∶95	52	约93	0.095

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