金属氧化物在OX-ZEO催化剂中催化CO x 加氢制低碳烯烃研究进展

doi:10.16085/j.issn.1000-6613.2022-0422

摘要/Abstract

摘要：

金属氧化物-分子筛（OX-ZEO）双功能催化剂可实现CO _x 加氢制低碳烯烃的高选择性转化。本文概述了OX-ZEO催化CO _x 加氢制低碳烯烃反应中金属氧化物的研究进展，通过对CO _x 加氢制甲醇/乙烯反应热力学分析指出了“接力催化”的优势，重点讨论了金属氧化物的种类和组成、制备方法及金属氧化物和分子筛的“亲密度”对催化性能的影响，探讨了催化反应机理、氧空位的作用及抑制副反应的策略。分析了OX-ZEO催化反应面临的问题和挑战，展望了OX-ZEO催化体系的发展趋势，认为通过元素掺杂、助剂修饰、优化制备条件等可提高金属氧化物的氧空位含量，进而可提高催化活性，也可通过对金属氧化物进行表面疏水改性抑制副产物CO₂，提高C原子利用率。

关键词: 合成气, 二氧化碳, 低碳烯烃, 金属氧化物, 双功能催化剂, 氧空位

Abstract:

Metal oxide-zeolite (OX-ZEO) bifunctional catalyst can convert CO _x hydrogenation into light olefins with high selectivity. In this work, the progresses of metal oxide in OX-ZEO catalyst for CO _x hydrogenation to light olefins are summarized, the advantages of “relay catalysis” are expounded through the thermodynamic analysis of CO _x hydrogenation to methanol/ethylene reaction, and the type and composition of metal oxide, OX-ZEO preparation method and the influence of “proximity” between oxide and SAPO-34 are mainly discussed. The catalytic reaction mechanism, the role of oxygen vacancy and the strategy to suppress side reactions are discussed. The problems and challenges of the OX-ZEO catalytic route are analyzed, and the development trend of the OX-ZEO catalytic system is prospected. It is believed that the catalytic activity can be improved by increasing the oxygen vacancies of metal oxides through elemental doping, promoter modification or optimizing preparation conditions, etc. Moreover, the by-product CO₂ generation can be suppressed by hydrophobic surface modification of the metal oxides to improve the utilization of C atoms.

Key words: syngas, carbon dioxide, light olefins, metal oxide, bifunctional catalyst, oxygen vacancy

中图分类号:

O643

张鹏, 孟凡会, 杨贵楠, 李忠. 金属氧化物在OX-ZEO催化剂中催化CO _x 加氢制低碳烯烃研究进展[J]. 化工进展, 2022, 41(8): 4159-4172.

ZHANG Peng, MENG Fanhui, YANG Guinan, LI Zhong. Progress of metal oxide in OX-ZEO catalyst for CO _x hydrogenation to light olefins[J]. Chemical Industry and Engineering Progress, 2022, 41(8): 4159-4172.

图/表 11

图1 CO x 加氢经OX-ZEO双功能催化剂合成低碳烯烃示意图以及影响性能关键因素

图2 合成气制甲醇/乙烯以及CO2加氢制甲醇/乙烯平衡转化率和组成

图3 ZnCrO x /SAPO-34催化剂在不同H2/CO比条件下的催化性能及稳定性评价[13]

图4 ZnZrO x /SAPO-34双功能催化剂催化CO2加氢制低碳烯烃示意图[30]

图5 In2O3颗粒尺寸对合成气转化制低碳烯烃反应性能的影响[52]

图6 不同温度处理下MTV-UiO-66(ZnZr)到HO-ZnZrO@C结构的演变[56]

图7 金属氧化物与SAPO-34结合方式对反应性能影响[7, 17, 60]

图8 物理混合的Zn-Cr/SAPO-34与核壳结构Zn-Cr@SAPO-34催化剂不同的传质过程的对比[61]

图9 合成气经烯酮中间体合成低碳烯烃反应机理[5, 13, 63]

图10 CO x 加氢经甲醇/二甲醚中间体合成低碳烯烃反应机理[10, 20]

图11 金属氧化物表面氧空位含量和CO转化率关系[26]

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