Ni基重整催化剂失活机理研究进展

doi:10.16085/j.issn.1000-6613.2021-0310

摘要/Abstract

摘要：

H₂是一种清洁、绿色的燃料和能源载体。目前工业上应用较为成熟的生产工艺是重整反应制氢。其中，Ni基重整催化剂由于其高储量、高活性和低成本的优点而受到研究人员的广泛关注，但在反应过程中存在易因烧结、积炭和中毒等原因而失活的问题。因此，如何提高Ni基重整催化剂的反应稳定性是一个急需解决的问题。本文介绍了上述三种引起Ni基重整催化剂失活的主要原因，并从调控金属Ni粒子粒径、增强金属-载体相互作用、形成晶格氧或表面氧物种以及Ni粒子纳米结构调控四个方面阐述了近年来在抑制失活并提高Ni基重整催化剂反应性能和稳定性领域所取得的研究进展，并且提出优化反应条件、调变化学组成和调控Ni粒子纳米结构将是提高Ni基催化剂在重整反应过程中的稳定性的有效方法。

关键词: Ni基催化剂, 重整反应, 烧结, 积炭, 中毒, 失活

Abstract:

Hydrogen is a clean and green fuel and energy source. Its production through reforming reaction is currently one of the mature processing technologies in chemical industries. Ni-based catalysts have attracted extensive attentions of researchers because of their high availability, high activity and low cost. However, the deactivation of catalysts often occurs due to sintering, carbon deposition and poisoning during the reaction. How to improve the stability of the Ni-based reforming catalysts is still a problem to be solved. In this paper, three main reasons for the deactivation of Ni-based reforming catalysts are summarized. In addition, the research progress in improving the reaction performance and the stability of Ni-based reforming catalysts in recent years is reviewed from the aspects of the regulation of size and nanostructure of Ni particle, enhancement of the metal-support interaction as well as the formation of lattice oxygen or surface oxygen species. Finally, it also shows that the optimization of reaction conditions, adjusting the chemical composition and tailoring the nanostructure of Ni particle can be used to improve the stabilities of Ni-based catalysts in the reforming reaction.

Key words: Ni-based catalysts, reforming reaction, sintering, carbon deposition, poisoning, deactivation

中图分类号:

O643.3

林俊明, 岑洁, 李正甲, 杨林颜, 姚楠. Ni基重整催化剂失活机理研究进展[J]. 化工进展, 2022, 41(1): 201-209.

LIN Junming, CEN Jie, LI Zhengjia, YANG Linyan, YAO Nan. Development on deactivation mechanism of Ni-based reforming catalysts[J]. Chemical Industry and Engineering Progress, 2022, 41(1): 201-209.

图/表 6

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烧结原因	催化剂	反应	文献
Ni-载体相互作用较弱	Ni/SiO₂，Ni/TiO₂，Ni/ZrO₂	甲烷干重整	［17］
过高助剂含量	10Ni/xCe（x=10，15）	甲烷干重整	［18］
较高蒸汽含量	Ni/Al₂O₃	蒸汽重整	［19］
	NiAl₂O₄尖晶石	氧化蒸汽重整	［20］
	Ni-CZO	甲烷蒸汽重整	［21］
反应物甲苯浓度增加	FCR-4，RUA	甲苯蒸汽重整	［22］

烧结原因	催化剂	反应	文献
Ni-载体相互作用较弱	Ni/SiO₂，Ni/TiO₂，Ni/ZrO₂	甲烷干重整	［17］
过高助剂含量	10Ni/xCe（x=10，15）	甲烷干重整	［18］
较高蒸汽含量	Ni/Al₂O₃	蒸汽重整	［19］
	NiAl₂O₄尖晶石	氧化蒸汽重整	［20］
	Ni-CZO	甲烷蒸汽重整	［21］
反应物甲苯浓度增加	FCR-4，RUA	甲苯蒸汽重整	［22］

积炭类型	反应类型	催化剂	对反应的影响	文献
包覆炭	甲烷干重整	Ni-CaO-ZrO₂	包覆炭会覆盖活性中心引起催化剂失活	［34，39-40］
	甲烷干重整	Ni/SBA-15
	生物油氧化蒸汽重整	Ni/CeO₂，NiAl₂O₄尖晶石等
丝状炭	乙醇蒸汽重整	Ni/La₂O₃-α-Al₂O₃	丝状炭不会阻塞活性位，对失活影响较小，但随着反应时间延长会堵塞反应管	［27，37］
丝状炭	甲烷干重整	Ni/Al₂O₃，Ni/CeO₂	丝状炭不会阻塞活性位，对失活影响较小，但随着反应时间延长会堵塞反应管	［27，37］
无定形炭	CO₂重整生物油	Ni/Al₂O₃	无定形炭高度分散在催化剂表面或催化剂微孔中导致催化剂快速失活	［28］
无定形炭	甲烷干重整	Ni-CaO-ZrO₂	无定形炭既可以参与反应，也可以作为其他类型炭物种的前体	［29］
聚合物炭	甲烷蒸汽重整	Ni/ZrO₂	聚合物炭会包裹催化剂降低其反应活性	［32］
碳纳米管	甲烷干重整	Ni/ZrO₂	碳纳米管对催化剂失活影响较小	［39］
碳纳米管	甲苯蒸汽重整	Ni/Al₂O₃	顶端生长碳纳米管对失活影响较小；底部生长碳纳米管会覆盖活性位，降低催化活性	［41］

积炭类型	反应类型	催化剂	对反应的影响	文献
包覆炭	甲烷干重整	Ni-CaO-ZrO₂	包覆炭会覆盖活性中心引起催化剂失活	［34，39-40］
	甲烷干重整	Ni/SBA-15
	生物油氧化蒸汽重整	Ni/CeO₂，NiAl₂O₄尖晶石等
丝状炭	乙醇蒸汽重整	Ni/La₂O₃-α-Al₂O₃	丝状炭不会阻塞活性位，对失活影响较小，但随着反应时间延长会堵塞反应管	［27，37］
丝状炭	甲烷干重整	Ni/Al₂O₃，Ni/CeO₂	丝状炭不会阻塞活性位，对失活影响较小，但随着反应时间延长会堵塞反应管	［27，37］
无定形炭	CO₂重整生物油	Ni/Al₂O₃	无定形炭高度分散在催化剂表面或催化剂微孔中导致催化剂快速失活	［28］
无定形炭	甲烷干重整	Ni-CaO-ZrO₂	无定形炭既可以参与反应，也可以作为其他类型炭物种的前体	［29］
聚合物炭	甲烷蒸汽重整	Ni/ZrO₂	聚合物炭会包裹催化剂降低其反应活性	［32］
碳纳米管	甲烷干重整	Ni/ZrO₂	碳纳米管对催化剂失活影响较小	［39］
碳纳米管	甲苯蒸汽重整	Ni/Al₂O₃	顶端生长碳纳米管对失活影响较小；底部生长碳纳米管会覆盖活性位，降低催化活性	［41］

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