氧化铝基加氢脱硫催化剂研究进展

doi:10.16085/j.issn.1000-6613.2023-0311

摘要/Abstract

摘要：

加氢脱硫催化剂是加氢脱硫技术中不可或缺的部分，其中氧化铝负载的硫化态催化剂作为典型的加氢脱硫催化剂在工业生产中应用十分广泛。本文系统介绍了氧化铝基硫化态催化剂的研究进展，包括硫化态加氢脱硫催化剂活性相模型以及各种类型的助剂对加氢脱硫催化剂构效关系的影响。着重探讨了包括5种经典模型在内的活性相模型研究进展情况以及差异性和关联性；同时对各种类型（过渡金属以及包括ⅠA、ⅡA、ⅢA等在内的主族元素等）的助剂对加氢脱硫催化剂构效关系的影响进行了探讨。最后对加氢脱硫催化剂的未来发展方向进行了展望，指出从原子尺度上洞察催化剂的活性相结构、形态及其复杂的催化机理，结合对催化机理以及活性相的深刻认识，可控创制性能可调的高活性及选择性的多功能催化剂是未来加氢脱硫催化剂的重要方向。

关键词: 加氢脱硫, 催化剂, 氧化铝, 活性相, 助剂

Abstract:

Hydrodesulfurization (HDS) catalyst is an indispensable part of hydrodesulfurization technology. Especially, as a typical hydrodesulfurization catalyst, the alumina supported metal sulfide catalyst is widely used in the industrial production. In this paper, the research progress of alumina supported metal sulfide catalyst, including the active phase model of the catalysts and the effects of various additives on the structure-activity relationship of hydrodesulfurization catalysts, is systematically reviewed. Thereinto, the research progress of active phase models, including 5 classical models, and their differences and correlations are emphatically discussed. Meanwhile, the effects of various additives (transition metals and main group elements including ⅠA, ⅡA, ⅢA, etc.) on the structure-activity relationship of hydrodesulfurization catalysts are discussed. Finally, the future development direction of hydrodesulfurization catalysts is prospected. Understanding the structure and morphology of the active phase and the complex catalytic mechanism of the catalyst on the atomic scale, creating controllably highly active and selective multi-functional catalysts with adjustable properties basing on the deep understanding of the catalytic mechanism and the active phase are important directions for hydrodesulfurization catalysts in the future.

Key words: hydrodesulfurization, catalyst, alumina, active phase, additives

中图分类号:

TE624.9⁺3

陈晓贞, 刘丽, 杨成敏, 郑步梅, 尹晓莹, 孙进, 姚运海, 段为宇. 氧化铝基加氢脱硫催化剂研究进展[J]. 化工进展, 2024, 43(2): 948-961.

CHEN Xiaozhen, LIU Li, YANG Chengmin, ZHENG Bumei, YIN Xiaoying, SUN Jin, YAO Yunhai, DUAN Weiyu. Research progress of alumina-supported hydrodesulfurization catalyst[J]. Chemical Industry and Engineering Progress, 2024, 43(2): 948-961.

图/表 10

图1 NiMoS活性相的CUS位点和SH基团示意图[14]

图2 加氢脱硫催化剂STM和球棍模型图[8]

图3 NiMoS/Al2O3活性位点上DBT吸附转化图[21]

图4 硫化钼催化剂的Rim-Edge模型[22]

图5 NiMoS催化剂的Rim-Edge活性位DBT吸附示意图[24]

图6 不同催化剂Edge-Corner位点与性能的关系[27]

图7 NiMoWS/Al2O3中Ce质量分数及其脱硫活性间关系[39]

图8 硼加入对MoS2活性相的影响[55]

图9 F掺杂后的氧化铝质子核磁共振图[37]

图10 不同F掺杂顺序的催化剂HDS活性[68]

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