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

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