金属催化剂烧结机制及抗烧结策略

doi:10.16085/j.issn.1000-6613.2022-0688

摘要/Abstract

摘要：

高温反应环境下金属催化剂易发生烧结，从而导致其活性降低甚至失活。因此，提高其热稳定性是多相催化的重大挑战。本文综述了金属催化剂以颗粒迁移和Ostwald熟化为主的两种烧结机制，整理了通过颗粒粒径分布、颗粒生长动力学、原位透射电镜观测、实验与计算预测四种判断烧结机制的方法；指出温度、化学势、催化剂自身物性是影响烧结的主要因素。其中，温度影响金属颗粒的动能，是引起烧结的主要物理因素；化学势大小受金属与载体间相互作用影响，是影响烧结的化学因素之一。同时围绕金属-载体相互作用、空间限域及其他新颖的抗烧结策略，总结了近年来在提高催化剂抗烧结性能方面的研究进展。最后从催化剂制备、结构分析和性能测试方面，提出了基于抗烧结金属催化剂研究及构建的发展方向。

关键词: 催化剂, 烧结, 失活, 抗烧结策略

Abstract:

Metal-based catalysts suffer from sintering of metal particles at high temperature, which causes the decline of catalytic performance and even deactivation. Therefore, improving the thermal stability of metal-based catalysts becomes a critical challenge for heterogeneous catalysis. In this review, the two main sintering mechanisms for metal-based catalyst has elaborated, including particle migration and Ostwald ripening. Four approaches to determine the sintering mechanism by particle size distribution, particle growth kinetics, in situ transmission electron microscopy analysis, and experimental and computational prediction were established. Among them, temperature affects the kinetic energy of metal particle, which is the main physical factor for particle sintering, while chemical potential, as one of the chemical factors for particle sintering, is greatly affected by the metal-support interaction. In addition, we summarized the research progress in developing the sintering-resistant catalysts on the basis of metal-support interaction, spatial confinement and other novel structure strategies. Furthermore, the development and goal for the research and construction of sintering-resistant catalysts are proposed from the aspects of catalyst preparation, structure analysis and catalytic performance.

Key words: catalyst, sintering, deactivation, sintering-resistant strategies

中图分类号:

O643.3

曹敏, 毛玉娇, 王倩倩, 李莎, 闫晓亮. 金属催化剂烧结机制及抗烧结策略[J]. 化工进展, 2023, 42(2): 744-755.

CAO Min, MAO Yujiao, WANG Qianqian, LI Sha, YAN Xiaoliang. Sintering mechanism and sintering-resistant strategies for metal-based catalyst[J]. Chemical Industry and Engineering Progress, 2023, 42(2): 744-755.

图/表 6

图1 本综述的主要观点概述

图2 金属催化剂主要的两种烧结机制(a) 颗粒迁移机理，颗粒间迁移聚集；(b) Ostwald熟化机理，颗粒表面物种迁移至其他颗粒

图3 Ni颗粒负载在MgAl2O4上的Ostwald熟化过程[15]（1mbar=102Pa）

图4 Ni/γ-Mo2N催化剂的原位二次电子STEM表征[53](a)~(d) 在不同预处理温度下，H2: N2=3∶1气氛下Ni颗粒在γ-Mo2N载体上随时间变化的ESE/STEM图；(e)~(g)为图(b)~(d)中黄色圆圈作为选定区域的高分辨电镜图；(h) Ni-4nm/γ-Mo2N催化剂在520℃下处理22min的高分辨电镜图

图5 空间限域稳定催化剂示意图[12, 70, 81](a) coat-Ni和imp-Ni的TEM图[70]；(b) MOFs封装的活性位点和不同表面位点在CO2加氢反应中的作用示意图[81]；(c) 调控颗粒间距减缓Pt/C催化剂烧结示意图[12]

图6 特殊结构催化剂抗烧结策略示意图[91-92](a) NOSCE的抗烧结策略示意图[91]：在Tammann温度以上，掺杂Mo的Ni颗粒在单晶MgO载体边缘移动，并稳定在高能台阶边缘的动态迁移过程、每个阶段的代表性TEM图和反应条件下不同时间NiMoCat的同步加速器分析；(b) 构筑粗糙凹凸表面结构的抗烧结策略示意图[92]

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