Engineering Cu‐In Dual‐Site Catalysts by Dynamic Reconstruction of Cu‐In‐S Quantum Dots for Efficient Electrochemical CO2 Conversion to Formate,Advanced Functional Materials

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Engineering Cu‐In Dual‐Site Catalysts by Dynamic Reconstruction of Cu‐In‐S Quantum Dots for Efficient Electrochemical CO2 Conversion to Formate
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2025-02-03 , DOI: 10.1002/adfm.202425606
Bo Zhang _{1,

2} , Yuan Chang ₃ , Junfeng Gao ₃ , Jungang Hou ₂

Affiliation

With the increasing consumption of fossil fuels emitting a large amount of CO2, electrocatalytic CO2 reduction (CO2RR) has become a promising way to reduce carbon emissions. Dual‐site catalysts have been identified as attractive materials for CO2RR, however, suffering from low selectivity and activity. Herein, Cu‐In‐S quantum dots have undergone in situ dynamic restructuring to construct Cu‐In dual‐site catalysts (Cu0.15In0.85 NPs) with highly catalytic activity toward CO2 electrochemical conversion. Cu0.15In0.85 NPs achieved a high Faraday efficiency of 92.3% for formate production at −1.45 V versus RHE, and a high formate partial current density of 245.4 mA cm−2 at −1.82 V versus RHE in a flow cell. In situ ATR‐SEIRAS spectroscopy and theoretical calculations indicated Cu dopants induced the charge transfer from Cu to In atoms to form the Cu‐In synergistic active sites, thus decreasing the formation energy of OCHO* and HCOOH* intermediates, as well as inhibiting the dissociation of water molecules. This work elucidates the optimization mechanism of the electronic structure for dual‐site catalysts and guides the fabrication of highly efficient electrocatalysts for formate production.

中文翻译：

通过动态重构 Cu-In-S 量子点来设计 Cu-In 双位点催化剂，以实现高效的电化学 CO2 转化为甲酸盐

随着排放大量 CO2 的化石燃料消耗量的增加，电催化 CO2 还原（CO2RR）已成为一种很有前途的减少碳排放的方法。双位点催化剂已被确定为有吸引力的 CO2RR 材料，但选择性和活性较低。在此，Cu-In-S 量子点经历了原位动力学重组，构建了对 CO2 电化学转化具有高度催化活性的 Cu-In 双位催化剂（Cu0.15In0.85 NPs）。Cu0.15In0.85 NPs 在流通池中的 -1.45 V 下实现了 92.3% 的甲酸盐生产法拉第效率，在 -1.82 V 下实现了 245.4 mA cm-2 的高甲酸盐部分电流密度。原位 ATR-SEIRAS 光谱和理论计算表明，Cu 掺杂剂诱导电荷从 Cu 转移到 In 原子，形成 Cu-In 协同活性位点，从而降低 OCHO* 和 HCOOH* 中间体的形成能，并抑制水分子的解离。这项工作阐明了双位点催化剂电子结构的优化机制，并指导了用于甲酸盐生产的高效电催化剂的制备。

更新日期：2025-02-03

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