铜催化剂在涉氢反应中的失活机制和稳定策略

doi:10.16085/j.issn.1000-6613.2022-1007

摘要/Abstract

摘要：

铜基催化剂对C $̿$ O、C—H、O—H和H—H等化学键具有独特活性能力，因而被广泛应用于CO _x 、醛、酸、酯加氢和醇脱氢等涉氢反应中。然而铜纳米颗粒塔曼温度较低，容易发生颗粒聚集长大而导致催化剂不可逆失活，限制了铜基催化剂的广泛应用。本文首先从表面能、金属物种表面迁移等角度入手系统地介绍了铜基催化剂的失活机理。然后，根据失活原因回顾了铜基催化剂在增强金属与载体相互作用、空间物理固定和合金化等方面的多种稳定策略。最后，通过现有结果分析了未来铜基催化剂的发展方向，指出可以通过失活机理的深入研究，借鉴新材料合成工艺和方法，制备廉价的新型铜基催化剂，为涉氢反应催化剂长寿命运行奠定基础。

关键词: 纳米材料, 催化剂, 失活, 还原, 稳定性

Abstract:

Copper (Cu) based catalysts have unique activity in reactions with C $̿$ O, C—H, O—H and H—H bond activation, and have been widely used in hydrogenation reactions of CO _x, aldehydes, acids, esters and alcohol dehydrogenation reactions. However, due to the low Tamman temperature of Cu particles, they are easy to deactivate because of the irreversible particle aggregation, which limits their applications. Herein, the deactivation mechanism of Cu based catalysts was first introduced from the viewpoint of surface energy and particle migration on catalysts. Then, strategies for stabilizing Cu particles including enhancement of metal-support interaction, spatial fixation and alloying were reviewed. Finally, an outlook was present to highlight the direction for Cu based catalysts. Specifically, the deactivation mechanism for Cu based catalysts should be in-depth investigated, and novel catalyst synthesis technologies and methods should be developed to prepare stable and cheap catalysts for reactions with hydrogen.

Key words: nanomaterials, catalyst, deactivation, reduction, stability

中图分类号:

TQ426.81

殷铭, 郭晋, 庞纪峰, 吴鹏飞, 郑明远. 铜催化剂在涉氢反应中的失活机制和稳定策略[J]. 化工进展, 2023, 42(4): 1860-1868.

YIN Ming, GUO Jin, PANG Jifeng, WU Pengfei, ZHENG Mingyuan. Deactivation mechanisms and stabilizing strategies for Cu based catalysts in reactions with hydrogen[J]. Chemical Industry and Engineering Progress, 2023, 42(4): 1860-1868.

图/表 7

图1 催化剂烧结模式

图2 负载金属催化剂的表面能[10]R—金属颗粒球形半径；α—金属颗粒与载体的接触角；γme—金属颗粒表面能；γox—载体表面能；γint—金属和载体的表面能；d—测算金属在载体上的直径

图3 草酸二甲酯加氢反应中铜颗粒失活机制[13]1—分解；2—脱离本体；3—奥斯瓦尔德熟化；4—草酸二甲酯加氢

图4 Cu—O—SiO x 界面的构筑及其对草酸二甲酯加氢的促进作用[31, 36]

图5 铜催化剂的电镜表征[57]绿色—Al；蓝色—Si；红色—Cu

图6 Cu2O@ZIF-8催化剂的合成方法[63]

图7 0.1Pt10Cu/Al2O3单原子催化剂的HAADF-STEM图[(a)，Pt以单原子形式分散在Cu晶面]；(a)图的放大区域照片和颜色差异图(b，c)；Pt单原子在Cu (~2.1 nm)颗粒上的稳定性[(d)，暗红色为Pt原子的稳定位]；10Cu/Al2O3催化剂的HAADF-STEM图[(e)，标尺为1nm][79]

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