Progress and Perspective for In Situ Studies of CO2 Reduction
Progress and Perspective for In Situ Studies of CO2 Reduction
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DOI：
10.1021/jacs.0c02973
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发表时间：
2020-05-27
影响因子：
15
通讯作者：
Xie, Yi
中科院分区：
文献类型：
--
作者：
Li, Xiaodong;Wang, Shumin;Xie, Yi
通过光还原、电还原或热还原将CO2转化为化学燃料被认为是解决环境污染和能源短缺问题的最有效方法之一。然而，最近的研究表明，所涉及的催化剂可能在现实工作条件下进行连续重构，不幸的是，这引起了有关CO2还原活性位点和反应机制的争议结果。因此，虽然具有挑战性，但有必要在实验条件下通过原位技术实时监测催化剂和反应中间体的动态演化。在这个视角中，我们从各种原位表征技术的工作原理和检测模式开始。随后，我们系统总结了二氧化碳还原过程中催化剂演化的原位研究的最新进展。我们进一步关注监测反应中间体和催化产物的原位研究进展，其中我们还强调如何结合理论计算来详细揭示反应机理。最后，基于代表性研究成果，对未来CO2减排原位研究提出了一些展望和建议。
CO2 conversion to chemical fuels through photoreduction, electroreduction, or thermoreduction is considered as one of the most effective methods to solve environmental pollution and energy shortage problems. However, recent studies show that the involved catalysts may undergo continuous reconstruction under realistic working conditions, which unfortunately causes controversial results concerning the active sites and reaction mechanism of CO2 reduction. Thus, it is necessary, while challenging, to monitor in real time the dynamic evolution of the catalysts and reaction intermediates by in situ techniques under experimental conditions. In this Perspective, we start with the working principle and detection modes of various in situ characterization techniques. Subsequently, we systematically summarize the recent developments of in situ studies on probing the catalyst evolution during the CO2 reduction process. We further focus on the progress of in situ studies in monitoring the reaction intermediates and catalytic products, in which we also highlight how the theoretical calculations are combined to reveal the reaction mechanism in detail. Finally, based on the achievements in the representative studies, we present some prospects and suggestions for in situ studies of CO2 reduction in the future.