化工进展 ›› 2021, Vol. 40 ›› Issue (2): 577-593.DOI: 10.16085/j.issn.1000-6613.32020-1403

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CO2 高值化利用新途径:铁基催化剂CO2加氢制烯烃研究进展

张超1(), 张玉龙1, 朱明辉1, 孟博2, 涂维峰2, 韩一帆1,2()   

  1. 1.化学工程联合国家重点实验室,华东理工大学,上海 200237
    2.先进功能材料制造教育部工程中心,郑州大学,河南 郑州 450001
  • 收稿日期:2020-07-20 修回日期:2020-10-28 出版日期:2021-02-05 发布日期:2021-02-09
  • 通讯作者: 韩一帆
  • 作者简介:张超(1994—),男,博士研究生,研究方向为CO2高值化利用。E-mail:18930618287@163.com
  • 基金资助:
    国家重点研发计划(2018YFB0605803);上海市青年科技英才扬帆计划(19YF1410600)

New pathway for CO2 high-valued utilization: Fe-based catalysts for CO2 hydrogenation to low olefins

Chao ZHANG1(), Yulong ZHANG1, Minghui ZHU1, Bo MENG2, Weifeng TU2, Yifan HAN1,2()   

  1. 1.State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
    2.Engineering Research Center of Advanced Functional Material Manufacturing of Ministry of Education, Zhengzhou University, Zhengzhou 450001, Henan, China
  • Received:2020-07-20 Revised:2020-10-28 Online:2021-02-05 Published:2021-02-09
  • Contact: Yifan HAN

摘要:

大气中CO2浓度逐年升高,而其高值化利用是实现减排的重要途径之一。低碳烯烃是重要的化工原料,CO2作为碳源加氢制取烯烃(CTO)是缓解化石能源的消耗及温室效应的有效方法之一。铁基催化剂因其优异的催化反应性能,被视为该反应最具应用前景的催化剂之一;但铁基催化剂烯烃选择性仍有待进一步提高。本文综述了铁基催化剂CTO反应研究进展,包括反应热力学分析、理论模型、催化剂设计与开发(助剂和载体对催化剂结构及性能的影响)、反应机理、构-效关系、失活机理等;提出未来催化研究方向,即借助Operando技术聚焦反应过程中催化剂活性相的动态结构变化规律,探究外界因素引起的催化材料表界面的作用机制,为工业催化剂的理性设计提供思路。

关键词: 二氧化碳, 加氢, 催化剂, 选择性, 失活, 稳定性

Abstract:

The concentration of CO2 in the atmosphere is increasing year by year, and high value utilization of CO2 is an important path to reduce the carbon emissions. Low-carbon olefins are important chemical raw materials, and CO2 as a carbon source hydrogenation to olefins (CTO) is one of the most promising CO2 utilization technologies that can potentially mitigate the global greenhouse gas emission and reduce the dependence of chemical production on fossil fuels. The Fe-based catalysts are recognized as a promising candidate in CTO due to their low cost and excellent performance. However, the selectivity to lower olefins and the activity of the Fe-based catalysts currently haven’t met the industrial requirements, and the mechanism of CTO reaction remains unclear. This article reviews the research progress of the iron-based catalysts for CTO reaction, including the reaction thermodynamic analysis, theoretical model, catalyst design and development (the influence of additives and supports on the structure and performance of catalysts), reaction mechanism, structure-activity relationship, and deactivation mechanism. Future research direction of catalysis was put forward. With the help of Operando technology, the dynamic structure evolution of active phases could be focused during the reaction process, and the mechanism of the catalytic material surface and interface caused by external factors could be explored. Based on the principle, which could provide ideas for the rational design of industrial catalysts.

Key words: carbon dioxide, hydrogenation, catalyst, selectivity, deactivation, stability

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