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Dual-Sites Tandem Catalysts for C–N Bond Formation via Electrocatalytic Coupling of CO2 and Nitrogenous Small Molecules
ACS Materials Letters ( IF 9.6 ) Pub Date : 2021-09-06 , DOI: 10.1021/acsmaterialslett.1c00375
Jiaju Fu 1 , Yan Yang 1, 2 , Jin-Song Hu 1, 2
Affiliation  

The electrocatalytic carbon dioxide reduction (ECR) to fuels and feedstocks driven by renewable energy is a promising approach to alleviate the environmental and energy crisis. Recently, high-performance ECR catalysts for producing simple products has been achieved. However, the producing of chemicals with high industrial significance still remains challenging. Coupling the reduction of CO2 and nitrogenous small molecules (N2, NO2, NH3 etc.) is one potential solution and is currently attracting increased interest. Here, we propose a rational perspective of constructing heterogeneous dual-active site catalysts (DACs) for the C–N coupling in ECR, which could provide isolated dual sites for coupling the C and N intermediates and thus improve the C–N coupling efficiency. In this Perspective, by investigating the possible pathway of C–N coupling reaction in the co-reduction process of CO2 with nitrogenous molecules and the reported strategies for building DACs, we discuss and project the potential strategies and challenges for the in-depth construction of C–N coupling tandem DACs systems. These insights may open up opportunities to develop high-efficiency DACs for diverse coupling electrocatalytic reactions and offer higher economic benefits and broader application prospects of electrocatalysis.

中文翻译:

通过 CO2 和含氮小分子的电催化偶联形成 C-N 键的双位点串联催化剂

由可再生能源驱动的燃料和原料的电催化二氧化碳还原 (ECR) 是缓解环境和能源危机的一种很有前景的方法。最近,已经实现了用于生产简单产品的高性能 ECR 催化剂。然而,具有高度工业意义的化学品的生产仍然具有挑战性。耦合还原 CO 2和含氮小分子(N 2、NO 2、NH 3等)是一种潜在的解决方案,目前正引起越来越多的兴趣。在这里,我们提出了一个合理的观点,即为 ECR 中的 C-N 偶联构建非均相双活性位点催化剂 (DAC),它可以为 C 和 N 中间体的偶联提供孤立的双位点,从而提高 C-N 偶联效率。在这个视角下,通过研究 CO 2共还原过程中 C-N 偶联反应的可能途径通过含氮分子和已报道的构建 DAC 的策略,我们讨论并预测了深入构建 C-N 耦合串联 DAC 系统的潜在策略和挑战。这些见解可能为开发用于多种耦合电催化反应的高效 DAC 提供机会,并提供更高的经济效益和更广泛的电催化应用前景。
更新日期:2021-10-04
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