Dual-Sites Tandem Catalysts for C–N Bond Formation via Electrocatalytic Coupling of CO2 and Nitrogenous Small Molecules,ACS Materials Letters

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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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