丙烷脱氢制丙烯用单原子催化剂研究进展

doi:10.16085/j.issn.1000-6613.2020-2560

摘要/Abstract

摘要：

丙烯是一种重要的有机化工原料和石油化工原料中间体，近年来在国内外市场的需求量持续增长。丙烷直接脱氢制丙烯技术具有收率高、技术成熟、经济环保等优点，备受研究者们的广泛关注。文中综述了丙烷直接脱氢制丙烯用单原子催化剂的研究进展，介绍了单原子催化剂的丙烷脱氢反应机理，探讨了单原子催化剂的失活行为，总结了活性组分、助剂及载体对单原子催化剂催化丙烷脱氢性能的影响，并分析讨论了单原子催化剂在当前研究中存在的问题。最后针对单原子催化剂虽具有优异的丙烯选择性和稳定性，但存在丙烷脱氢活性依旧不足的问题，提出了调控单原子催化剂电子结构促进丙烷脱氢活性的设计思路，为未来丙烷脱氢制丙烯高效单原子催化剂的设计提供了指导方向。

关键词: 丙烷脱氢, 单原子催化剂, 失活, 活性, 电子结构, 设计

Abstract:

Propylene is an important organic chemical feedstock and intermediate in organic chemical and petrochemical industry. In recent years, the demand in domestic and foreign markets has been increasing. The direct dehydrogenation of propane to propylene has the advantages of high yield, technological maturity, economic and environmental benefit, etc., and hence has attracted wide attention from researchers. Recent research progress of single-atom catalysts for direct dehydrogenation of propane to propylene is reviewed in this work. The dehydrogenation reaction mechanism of propane and catalyst deactivation with single-atom catalysts is discussed. The effects of active components, additives and carriers on the propane dehydrogenation performance of single-atom catalysts are summarized. And the existing problems of single-atom catalysts in current researches are also analyzed and discussed. Finally, in view of the fact that the single-atom catalysts have excellent propylene selectivity and stability but insufficient propane dehydrogenation activity, the principles for promoting the propane dehydrogenation activity of single-atom catalysts by adjusting the electronic structure are proposed, which provides guidance for the design of high-efficiency single-atom catalysts for dehydrogenation of propane to propylene in the future.

Key words: propane dehydrogenation, single-atom catalysts, deactivation, reactivity, electronic structure, design

中图分类号:

O643

吴建国, 吴登峰, 程道建. 丙烷脱氢制丙烯用单原子催化剂研究进展[J]. 化工进展, 2021, 40(12): 6688-6695.

WU Jianguo, WU Dengfeng, CHENG Daojian. Advances in single-atom catalysts for dehydrogenation of propane to propylene[J]. Chemical Industry and Engineering Progress, 2021, 40(12): 6688-6695.

图/表 9

图1 Cu(111) 表面负载的单原子Pd催化剂丙烷脱氢反应机理示意图[11]

图2 丙烷脱氢反应Pt-Sn纳米团簇的自组装和再生过程[17]

图3 Pd/Cu单原子合金催化剂丙烷脱氢作用示意图[20]

图4 二维Ru-Pc单原子催化剂丙烷脱氢作用示意图[21]

图5 g-C3N4负载单金属原子的丙烯吸附能（Ead）与第一个C—H键解离反应能（ΔE）总和示意图[22]

表1 负载型Pt和Pt-Sn催化剂丙烷脱氢性能[17]

催化剂	丙烷转化率/%	丙烯选择性/%	炭质量分数/ %
Pt/CeO₂	100	0	0.9（3.4）
Pt-Sn/CeO₂	39.5	84.5	0.5（2.8）
Pt-Sn/Al₂O₃	32.6	71.4	0.3（3.0）

图6 不同助剂对Pt/SiO2催化剂丙烷脱氢性能的影响[27]

图7 不同比例Cu助剂对单原子Pt催化剂催化丙烷脱氢性能的影响[19]

图8 氮化硼与金属Pt之间的协同作用对丙烷催化脱氢作用示意图[40]

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