卡宾桥接Ag-Cu位点: 促进*CO富集与*COCHO偶联, C2+选择性破80%

doi:10.1016/S1872-2067(25)64888-1

催化学报 ›› 2026, Vol. 82: 105-114.DOI: 10.1016/S1872-2067(25)64888-1

卡宾桥接Ag-Cu位点: 促进CO富集与COCHO偶联, C₂₊选择性破80%

张浩宇^a^,¹, 金鲁杰^b^,¹, 郑堂洪^a, 邱新然^a, 刘阳^a, 陈冬赟^a, 徐庆锋^a^,^*(), 李有勇^b^,^*(), 路建美^a^,^*()

^a苏州大学材料与化学化工学部, 江苏苏州 215123
^b苏州大学功能纳米与软材料研究院, 江苏苏州 215123

收稿日期:2025-07-30 接受日期:2025-09-11 出版日期:2026-03-18 发布日期:2026-03-05
通讯作者: * 电子信箱: xuqingfeng@suda.edu.cn (徐庆锋),yyli@suda.edu.cn (李有勇),lujm@suda.edu.cn (路建美).
作者简介:¹共同第一作者.
基金资助:
国家自然科学基金(22438009);国家自然科学基金(22578298);国家自然科学基金(U24A20535);江苏省基础研究计划重点项目(BK20243002);江苏省高等学校优势学科建设工程资助项目(PAPD);科技部智能纳米环保新材料与检测技术国际联合研究中心项目

Carbene dual-function bridging of Ag-Cu sites enables CO pooling for COCHO coupling with > 80% C₂₊ selectivity in CO₂ electroreduction

Haoyu Zhang^a^,¹, Lujie Jin^b^,¹, Tanghong Zheng^a, Xinran Qiu^a, Yang Liu^a, Dongyun Chen^a, Qingfeng Xu^a^,^*(), Youyong Li^b^,^*(), Jianmei Lu^a^,^*()

^aCollege of Chemistry, Chemical Engineering and Materials Science, Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou 215123, Jiangsu, China
^bInstitute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou 215123, Jiangsu, China

Received:2025-07-30 Accepted:2025-09-11 Online:2026-03-18 Published:2026-03-05
Contact: * E-mail: xuqingfeng@suda.edu.cn (Q. Xu),yyli@suda.edu.cn (Y. Li),lujm@suda.edu.cn (J. Lu).
About author:¹ Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(22438009);National Natural Science Foundation of China(22578298);National Natural Science Foundation of China(U24A20535);Basic Research Project of Leading Technology in Jiangsu Province(BK20243002);Priority Academic Program Development of Higher Education Institutions (PAPD) in Jiangsu;National Center for International Research on Intelligent Nano Materials and Detection Technology in Environmental Protection

摘要/Abstract

摘要：

随着全球对碳中和目标的日益关注, 电催化CO₂还原反应(CO₂RR)作为一种可持续的将CO₂转化为高附加值化学品和燃料的方法,已成为当前能源与环境领域的研究热点. 与C₁产物相比, 多碳(C₂₊)产物具有更高的能量密度和商业价值. 但是, 由于C-C偶联反应的选择性偏低且反应动力学迟缓, 因此在CO₂RR中高效合成C₂₊产物仍然是一个重大挑战. Cu表面与*CO关键中间体之间存在适当的结合强度, 能够促进C-C偶联反应, 因此Cu基催化剂被广泛研究. 然而, 由于*CO中间体的生成量不足以及C-C偶联活性有限, 单一的Cu催化剂合成C₂₊产物的法拉第效率仍然较低. 因此, 如何提供足量*CO以及保证*CO中间体加氢及偶联的顺畅进行, 是提高C₂₊产物选择性的关键.

本文提出了一种表面修饰的高效策略, 即通过卡宾双功能桥接Ag-Cu位点, 实现*CO富集并促进*COCHO偶联, 从而显著提高CO₂电还原过程中C₂₊产物的选择性. 实验结果表明, 卡宾修饰的Ag-Cu₂O催化剂在400 mA cm^-2的电流密度下实现了80.3%的C₂₊法拉第效率, 显著优于未修饰的Cu₂O和Ag-Cu₂O催化剂. 通过电化学产物分析和原位表面增强拉曼光谱技术, 观察到Ag位点可以产生CO中间体, 并通过“脱附-再吸附”的方式溢流到Cu位点表面, 从而增加Cu位点上的*CO覆盖度. 而卡宾的引入, 可以富集和活化CO₂, 为CO的生成提供了充足的反应物. 更重要的是, 结合拉曼特征峰以及密度泛函理论计算, 发现卡宾可以调节Cu的电子结构, 使Cu表面更易于重新吸附CO并稳定*CO中间体, 从而促进了后续的C-C偶联反应. 利用原位衰减全反射表面增强红外吸收光谱来监测反应中间体的动态变化, 发现修饰卡宾后, *CHO和*COCHO中间体的信号明显增强, 这表明卡宾降低了*CO在Cu表面氢化的能量势垒, 使得*CO更容易转化为*CHO中间体, 进而促进*COCHO中间体的形成. 晶体轨道哈密顿布居分析进一步解释了卡宾在活化*CO中的作用, 与在原始Cu表面上吸附的*CO相比, 在卡宾修饰的Cu表面上吸附的*CO在其反键态上展现出更高的占据和更低的能量水平, 表明其C-O键更弱, 更易被活化, 因此加氢反应的反应势垒更低. 由卡宾增强的串联协同效应源于两个因素: (1)卡宾修饰增强了*CO与Cu表面之间的相互作用, 从而强化了*CO从Ag到Cu的溢流效应, 提高了*CO的在Cu表面的覆盖度; (2)卡宾改变了Cu的电子结构, 降低了*CO加氢的能垒, 从而促进了更有效的C-C偶联反应.

综上, 本研究提出了一种通过表面修饰增强多催化位点协同效应的新策略, 为CO₂电还原催化剂的设计提供了新的思路, 不仅充分展示了卡宾修饰在提高C₂₊产物选择性方面的巨大潜力, 还为设计更高效的CO₂RR催化剂奠定了坚实的实验和理论基础.

关键词: 二氧化碳, 多碳产物, 电催化, 卡宾修饰, 双功能桥接

Abstract:

The electrocatalytic CO₂ reduction reaction (CO₂RR) offers a promising sustainable route for producing high-value C₂₊ chemicals and fuels by using renewable electricity. However, boosting C₂₊ product yields has been significantly hindered by insufficient *CO intermediate generation in confined spaces and limited activity of sites for subsequent hydrogenation and C-C coupling processes. Herein, we introduce an efficient strategy that involves carbene dual-function bridging of Ag-Cu sites to enable *CO pooling and facilitate *COCHO coupling. As a result, a remarkable C₂₊ Faradaic efficiency of 80.3% at 400 mA cm^-2 was achieved. In-situ surface-enhanced Raman spectroscopy, in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy, and density functional theory calculations collectively uncover the underlying mechanism. Carbene facilitates CO spillover from Ag to Cu sites, modulates the electronic structure of Cu, stabilizes CO intermediates, and reduces the energy barrier for CO hydrogenation. These effects synergistically enhance C-C coupling, thereby improving the Faradaic efficiency for C₂₊ product formation.

Key words: Carbon dioxide, C₂₊ products, Electrolysis, Carbene modification, Dual-function bridging

张浩宇, 金鲁杰, 郑堂洪, 邱新然, 刘阳, 陈冬赟, 徐庆锋, 李有勇, 路建美. 卡宾桥接Ag-Cu位点: 促进*CO富集与*COCHO偶联, C₂₊选择性破80%[J]. 催化学报, 2026, 82: 105-114.

Haoyu Zhang, Lujie Jin, Tanghong Zheng, Xinran Qiu, Yang Liu, Dongyun Chen, Qingfeng Xu, Youyong Li, Jianmei Lu. Carbene dual-function bridging of Ag-Cu sites enables *CO pooling for *COCHO coupling with > 80% C₂₊ selectivity in CO₂ electroreduction[J]. Chinese Journal of Catalysis, 2026, 82: 105-114.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64888-1

https://www.cjcatal.com/CN/Y2026/V82/I3/105

图/表 5

Fig. 1. (a) Schematic illustration of the synthesis of Ag-Cu2O-carbene. TEM (b), HRTEM (c) HAADF-STEM images and corresponding elemental mapping, (d) of Ag-Cu2O-carbene. High-resolution Ag 3d (e) and N 1s (f) XPS spectra, and FTIR spectra (g) of Cu2O, Ag-Cu2O, and Ag-Cu2O-carbene.

Fig. 2. (a) LSV curves of the different electrodes under Ar or CO2 atmosphere. Faradaic efficiency of C1 (b) and C2+ (c) products for the three electrodes at different current densities. Faradaic efficiencies of various products for the Cu2O (d), Ag-Cu2O (e) and Ag-Cu2O-carbene (f) electrode at different current densities. (g) Comparison of Ag-Cu2O-carbene with other reported electrocatalysts. (h) Long-term stability of the Ag-Cu2O-carbene electrode at a current density of 400 mA cm-2.

Fig. 3. In-situ SERS of the Cu2O electrode (a), the Ag-Cu2O electrode (b) and Ag-Cu2O-carbene electrode (c). (d) Schematic illustration of the *CO coverage and the “desorption-re-adsorption” process on the surfaces of the three materials.

Fig. 4. (a) In-situ ATR-SEIRAS of the Cu2O electrode. (b) In-situ ATR-SEIRAS of the Ag-Cu2O electrode. (c) In-situ ATR-SEIRAS of the Ag-Cu2O-carbene electrode. Integrated peak areas of the *CHO (d) and *COCHO (e) signals on the surfaces of the three materials.

Fig. 5. (a) Adsorption energies of *CO intermediates on the surfaces of Ag, Cu, and Cu-carbene. (b) The projected density of states of the d orbital of Cu and p orbital of C atom on Cu and Cu-carbene, respectively. (c) Gibbs free energy profiles for the *CO → *COCHO reaction pathway. (d) The pCOHP for *CO adsorption on pristine Cu surface and Cu surface with carbene, respectively. (e) Schematic illustration of carbene dual-function bridging of Ag-Cu sites for enhancing *CO spillover and *COCHO coupling.

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卡宾桥接Ag-Cu位点: 促进CO富集与COCHO偶联, C₂₊选择性破80%

Carbene dual-function bridging of Ag-Cu sites enables CO pooling for COCHO coupling with > 80% C₂₊ selectivity in CO₂ electroreduction

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