Significance of Site Proximity in Cu Single-Atomic Site Catalysts for Electrocatalytic Synthesis of Alanine

IF 8.6 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Materials Letters Pub Date : 2026-09-07 Epub Date: 2026-08-17 DOI:10.1021/acsmaterialslett.6c00477

Ziheng Chen, Zhiming Li, Yuanyuan Ye, Sisi Yue, Weichao Niu, Fanglei Yao, Jin Wang

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Abstract

Synthesis of amino acids via electrocatalytic C−N coupling is considered a promising and green approach. Whether C−N coupling relies on cooperative sites (bonded or nonbonded) is an open question and is crucial for the development of highly efficient catalysts. Here, Cu single-atomic site (SAS) catalysts with different site densities were synthesized via an ion exchange approach, and the impact of site proximity on Faradaic efficiency of alanine (FE_alanine) was probed. The FE_alanine is positively correlated with Cu SAS loadings. An FE_alanine of 42% can be achieved at 15 wt % loading. Remarkably, it is revealed that fully isolated Cu SASs (at 1 wt % loading) do not result in alanine. This suggests that the presence of adjacent-site configurations is probably essential for the C−N coupling. It is speculated that fully isolated Cu SASs prefer to adsorb pyruvic acid rather than nitrate, thus failing to form the key intermediate hydroxylamine.

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铜单原子位点催化剂中位点邻近性对电催化合成丙氨酸的意义

电催化C - N偶联法合成氨基酸被认为是一种很有前途的绿色方法。C−N耦合是否依赖于合作位点（键合或非键合）是一个悬而未决的问题，对于高效催化剂的开发至关重要。本文采用离子交换法合成了不同位点密度的Cu单原子位点（SAS）催化剂，并探讨了位点邻近度对丙氨酸（FEalanine）法拉第效率的影响。茶氨酸与Cu SAS负荷呈正相关。在15 wt %的负载下可以达到42%的茶氨酸。值得注意的是，完全分离的Cu SASs（负载为1wt %）不会产生丙氨酸。这表明邻接位点结构的存在可能是C - N耦合所必需的。推测完全分离的Cu SASs更倾向于吸附丙酮酸而不是硝酸盐，因此不能形成关键的中间体羟胺。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

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