Tuning Multi‐Active Sites in Cu Catalyst via Ag/Ni Doping for Enhanced CO2 Electroreduction to C2+ Products,Angewandte Chemie International Edition

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Tuning Multi‐Active Sites in Cu Catalyst via Ag/Ni Doping for Enhanced CO2 Electroreduction to C2+ Products
Angewandte Chemie International Edition ( IF 16.9 ) Pub Date : 2025-04-23 , DOI: 10.1002/anie.202501833
Shuaiqiang Jia _{1,

2} , Hailian Cheng _{1,

2} , Qinggong Zhu ₃ , Xiao Chen _{1,

2} , Cheng Xue _{1,

2} , Ting Deng _{1,

2} , Mengke Dong _{1,

2} , Zhanghui Xia _{1,

2} , Jiapeng Jiao _{1,

2} , Chunjun Chen _{1,

2} , Haihong Wu _{1,

2} , Mingyuan He _{1,

2} , Buxing Han _{1,

2,

3}

Affiliation

Electrochemical CO2 reduction (ECR) to C2+ products is a promising sustainable carbon conversion pathway, yet simultaneously achieving high Faradaic efficiency (FE) and current density remains a challenge. Herein, we found that creating Cu‐Ag‐Ni multi‐metal sites could effectively modulate the adsorption energies of *H and *CO on the catalyst surface, thereby achieving highly efficient ECR to synthesize C2+ products. In situ measurements coupling theoretical calculations indicated that by systematically altering the spatial arrangement and distribution of active sites in Cu‐Ag‐Ni catalysts, the electronic structure and the local *CO coverage on the Cu surface could be tuned, consequently steering the ECR to C2+ pathway. In particular, Cu‐Ag‐Ni catalyst with dispersed multi‐sites (CuxAgNi DNPs) could more effectively reduce the energy barrier for C─C coupling than Cu‐Ag‐Ni catalyst with phase‐separated multi‐sites (CuxAgNi PNPs). As a result, the Cu40AgNi DNPs catalyst with dispersed multi‐sites yielded C2+ products with a FE of 93.2% and a current density up to 818.1 mA cm−2 at −1.38 V versus reversible hydrogen electrode (vs. RHE), which are higher than most reported up to date for C2+ production. This work provides a methodology for designing robust multi‐metallic ECR catalysts with tailored multi‐active site configurations.

中文翻译：

通过 Ag/Ni 掺杂调整 Cu 催化剂中的多活性位点，以增强 CO2 电还原为 C2+ 产物

电化学 CO2 还原（ECR）制 C2+ 产物是一种很有前途的可持续碳转化途径，但同时实现高法拉第效率（FE）和电流密度仍然是一个挑战。在此，我们发现创建 Cu-Ag-Ni 多金属位点可以有效调节催化剂表面 *H 和 *CO 的吸附能，从而实现高效的 ECR 合成 C2+ 产物。原位测量耦合理论计算表明，通过系统地改变 Cu-Ag-Ni 催化剂中活性位点的空间排列和分布，可以调整 Cu 表面的电子结构和局部 *CO 覆盖率，从而将 ECR 引导到 C2+ 途径。特别是，与具有相分离多位点的 Cu-Ag-Ni 催化剂（CuxAgNi PNP）相比，具有分散多位点的 Cu-Ag-Ni 催化剂（CuxAgNi DNP）可以更有效地降低 C─C 耦合的能垒。结果，与可逆氢电极（相对于 RHE）相比，具有分散多位点的 Cu40AgNi DNPs 催化剂产生了 FE 为 93.2% 且电流密度高达 818.1 mA cm-2 的 C2+ 产物，与可逆氢电极（相对于 RHE）相比，这高于迄今为止报道的 C2+ 生产。这项工作提供了一种设计具有定制多活性位点配置的稳健多金属 ECR 催化剂的方法。

更新日期：2025-04-23

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