邻近Ni-Cu双单原子位点调控界面水微环境促进CO2至CO电还原动力学研究

doi:10.1016/S1872-2067(26)65092-9

催化学报 ›› 2026, Vol. 87: 47-58.DOI: 10.1016/S1872-2067(26)65092-9

邻近Ni-Cu双单原子位点调控界面水微环境促进CO₂至CO电还原动力学研究

郝琦^a^,^b^,¹, 汤淇^c^,^d^,¹, 武俊秀^e, 刘剀^b^,^f^,^*(), 陆俊^e^,^*(), 吴天品^e^,^*()

^a 浙江大学材料科学与工程学院, 浙江杭州 310027
^b 西湖大学工学院, 浙江杭州 310030
^c 中国科学院长春应用化学研究所, 稀土资源利用国家重点实验室, 吉林长春 130022
^d 中国科学技术大学应用化学与工程学院, 安徽合肥 230026
^e 浙江大学化学工程与生物工程学院, 浙江杭州 310027
^f 西湖大学工学院, 浙江省海岸带环境与资源研究重点实验室, 浙江杭州 310030

收稿日期:2025-11-09 接受日期:2026-02-04 出版日期:2026-08-18 发布日期:2026-06-24
通讯作者: ^*电子信箱: liukai@westlake.edu.cn (刘剀),
junzoelu@zju.edu.cn (陆俊),
tianpinwu@zju.edu.cn (吴天品).
作者简介:¹共同第一作者.
基金资助:
西湖牧原合成生物研究院创新引导项目(N14116522401);西湖大学人才引进专项经费(103506022001);浙江省领军型创新创业项目(2023R01007)

Neighboring Ni-Cu dual single-atom sites regulate the local environment of interfacial water for promoting CO₂ electroreduction kinetics in CO₂-to-CO conversion

Qi Hao^a^,^b^,¹, Qi Tang^c^,^d^,¹, Junxiu Wu^e, Kai Liu^b^,^f^,^*(), Jun Lu^e^,^*(), Tianpin Wu^e^,^*()

^a School of Materials Science & Engineering, Zhejiang University, Hangzhou 310027, Zhejiang, China
^b School of Engineering, Westlake University, Hangzhou 310030, Zhejiang, China
^c State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China
^d School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, Anhui, China
^e College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, Zhejiang, China
^f Key Laboratory of Coastal Environment and Resources of Zhejiang Province, School of Engineering, Westlake University, Hangzhou 310030, Zhejiang, China

Received:2025-11-09 Accepted:2026-02-04 Online:2026-08-18 Published:2026-06-24
About author:¹Contributed equally to this work.
Supported by:
Westlake-Muyuan Institute of Synthetic Biology(N14116522401);Westlake Education Foundation(103506022001);Leading Innovative and Entrepreneurial Projects in Zhejiang Province(2023R01007)

摘要/Abstract

摘要：

电催化二氧化碳还原(ECO₂RR)是将CO₂转化为高附加值化学品、实现碳循环利用的关键途径之一. 其中, CO₂至CO的转化路径因产物分离简便, 且可作为合成气原料, 具有重要的工业化潜力. 单原子催化剂(SACs)因其明确的活性中心与极高的原子利用率, 在ECO₂RR中展现出优异的活性和选择性. 然而, 传统单金属SACs受限于中间体与产物吸附能的线性标度关系, 其整体反应动力学仍有待提升. 近年来, 异核双单原子催化剂(DSACs)通过相邻位点间的协同效应, 为突破上述限制提供了新思路. 值得注意的是, 以往研究多关注位点间的本征电子相互作用, 而对于活性中心与界面水分子之间的相互作用机制仍不清晰. 特别是在能够有效抑制碳酸盐生成、提升碳利用效率的酸性介质中, 如何通过调控界面水结构来促进CO₂还原并抑制竞争性析氢反应, 已成为一个关键的科学挑战.

本文设计并构建了一种氯掺杂的Ni-Cu双单原子催化剂(Cl-Ni₁Cu₁-C), 旨在揭示双单原子位点对界面微环境的调控机制. 多维度结构表征证实, Ni与Cu物种均以单原子形式分散于氯掺杂的碳载体上, 并成功构筑了平均距离约为4.1 Å的相邻Ni-Cu双原子位点. 系统的电化学性能测试表明, 该催化剂在H型电解池中表现出优异的ECO₂RR活性, 其CO分电流密度显著优于对应的单金属催化剂. 进一步地, 在模拟工业应用的流动池测试中, Cl-Ni₁Cu₁-C在强酸(pH = 1)与强碱(pH = 13)介质中均展现出卓越的适应性和稳定性. 具体而言, 在50至400 mA cm⁻²的宽电流密度范围内, CO法拉第效率始终接近100%; 尤其在酸性条件下, 得益于对碳酸盐生成的抑制, 其在200 mA cm⁻²下的CO单程碳效率高达67.3%. 此外, Cl-Ni₁Cu₁-C在强酸中连续电解超过170 h后, 性能衰减不足10%, 展现了出色的运行稳定性. 为深入揭示Cl-Ni₁Cu₁-C高性能的微观起源, 结合原位谱学分析与理论计算, 对反应机理进行了深入探究. 结果表明, 相邻的Ni-Cu双单原子位点能够协同调控界面水分子的构型与氢键网络, 有效削弱其刚性, 从而显著增加界面水区域中易于解离的水物种比例. 这种优化的水微环境为CO₂质子化生成关键*COOH中间体的步骤提供了更高效的质子源, 进而加速了整体反应动力学. 理论计算进一步阐明, Ni位点与Cu位点间的电子协同效应优化了Ni活性中心对反应中间体的吸附能, 同时有效抑制了析氢副反应路径. 这两种机制的协同作用, 共同保障了催化剂在全pH范围内的高活性、高选择性与高稳定性.

综上, 本工作不仅成功开发出一种适用于工业级电流密度且性能优异的双单原子催化剂, 更重要的是, 通过多角度机理研究, 揭示了双原子位点通过协同调控界面水微环境以优化反应动力学的新机制. 该发现深化了对电催化界面复杂相互作用的理解, 为未来通过理性设计“活性中心-溶剂微环境”来定向提升催化性能提供了新的理论框架和设计思路.

关键词: CO₂电还原, 邻近协同效应, 微环境调控, 优化CO₂质子化动力学, 工业级电流密度

Abstract:

We develop a Ni-Cu dual single-atom catalyst (DSAC) as a model catalyst to investigate the neighboring synergy in dual single-atom sites for promoting the electrocatalytic carbon dioxide reduction reaction (ECO₂RR) kinetics. Through detailed electrochemical tests, in situ spectroscopic observations and theoretical calculations, we found that during ECO₂RR, the neighboring Ni-Cu dual single-atom sites synergistically weaken the rigidity of the hydrogen-bond networks of interfacial water and optimize the spatial configuration of water molecules surrounding the Ni-Cu dual single-atom sites, which increases the proportion of easily dissociated water species in the interfacial water, thus accelerating the CO₂ protonation kinetics during the conversion of CO₂ to CO. As a result, Ni-Cu DSAC exhibits a 1.5-fold increase and a 15-fold increase in ECO₂RR activity compared to Ni SAC and Cu SAC, respectively. In flow cell electrolyzer, Ni-Cu DSAC achieves almost 100% Faradaic efficiency for CO production (FE_CO) from applied current density of 50 to 400 mA cm⁻², with the optimal full-cell energy efficiency of 61.1% for CO production, reflecting the excellent catalytic performance of neighboring Ni-Cu dual single-atom sites for selective conversion of CO₂ to CO. Benefiting from the efficient suppression of carbonates formation in acidic media, Ni-Cu DSAC achieves an outstanding single-pass carbon efficiency of 67.3% for CO₂-to-CO conversion at 200 mA cm⁻². Additionally, Ni-Cu DSAC also exhibits excellent long-term stability, with less than 10% decay of FE_CO throughout a 170-h continuous electrolysis in strong acid (pH = 1, j = 200 mA cm⁻²).

Key words: CO₂ electroreduction, Neighboring synergistic effect, Microenvironment regulation, Optimized CO₂ protonation kinetics, Industrial-level current densities

郝琦, 汤淇, 武俊秀, 刘剀, 陆俊, 吴天品. 邻近Ni-Cu双单原子位点调控界面水微环境促进CO₂至CO电还原动力学研究[J]. 催化学报, 2026, 87: 47-58.

Qi Hao, Qi Tang, Junxiu Wu, Kai Liu, Jun Lu, Tianpin Wu. Neighboring Ni-Cu dual single-atom sites regulate the local environment of interfacial water for promoting CO₂ electroreduction kinetics in CO₂-to-CO conversion[J]. Chinese Journal of Catalysis, 2026, 87: 47-58.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65092-9

https://www.cjcatal.com/CN/Y2026/V87/I8/47

图/表 5

Fig. 1. (a) XRD patterns of Cl-Ni1-C, Cl-Cu1-C, and Cl-Ni1Cu1-C. (b) EPR spectra of Cl-Ni1-C, Cl-Cu1-C, and Cl-Ni1Cu1-C. (c) Raman spectra of Cl-Ni1-C, Cl-Cu1-C, and Cl-Ni1Cu1-C. (d) Low-resolution HAADF-STEM image of Cl-Ni1Cu1-C. (e,f) High-resolution HAADF-STEM images of Cl-Ni1Cu1-C. (g) The 3D fitting maps of dual single-atom sites in Cl-Ni1Cu1-C based on Area 1 and Area 2. (h) Atomic distance statistics based on Figs. 1(e) and Figs. 1(f). Low-resolution HAADF-STEM image (i) and the corresponding EDS mapping (j) of Cl-Ni1Cu1-C.

Fig. 2. (a) Ni K-edge XANES spectra of standard references (Ni foil, NiO and NiPc), Cl-Ni1-C and Cl-Ni1Cu1-C. (b) Ni K-edge FT-EXAFS spectra of standard references (Ni foil, NiO and NiPc), Cl-Ni1-C and Cl-Ni1Cu1-C. (c) Ni K-edge experimental and fiited FT-EXAFS spectra of standard references (Ni foil, NiO and NiPc), Cl-Ni1-C and Cl-Ni1Cu1-C. (d) Cu K-edge XANES spectra of standard references (Cu foil, CuO and CuPc,), Cl-Cu1-C and Cl-Ni1Cu1-C. (e) Cu K-edge FT-EXAFS spectra of standard references (Cu foil, CuO and CuPc,), Cl-Cu1-C and Cl-Ni1Cu1-C. (f) Cu K-edge experimental and fiited FT-EXAFS spectra of standard references (Cu foil, CuO and CuPc,), Cl-Cu1-C and Cl-Ni1Cu1-C. (g,h) Ni K-edge wavelet transform spectra of Cl-Ni1-C (g) and Cl-Ni1Cu1-C (h). (i,j) Cu K-edge wavelet transform spectra of Cl-Cu1-C (i) and Cl-Ni1Cu1-C (j).

Fig. 3. (a) LSV curves of Cl-Cu1-C, Cl-Ni1-C, and Cl-Ni1Cu1-C under CO2 atmosphere. Scan rate, 10 mV s−1. (b) FECOs of Cl-Cu1-C, Cl-Ni1-C, and Cl-Ni1Cu1-C under different potentials. (c) jCOs of Cl-Cu1-C, Cl-Ni1-C, and Cl-Ni1Cu1-C under different potentials. (d) The recorded Ecells for ECO2RR with using Cl-Ni1Cu1-C as the electrocatalyst in flow cell electrolyzers. (e) FECOs at different current densities (f) SPCE comparisons of Cl-Ni1Cu1-C with other recently reported electrocatalysts [8,38-46]. (g) Long-term stability test of Cl-Ni1Cu1-C in strong acid (j = 200 mA cm−2).

Fig. 4. The potential-dependent IR spectra on Cl-Ni1Cu1-C (a), Cl-Ni1-C (b), and Cl-Cu1-C (c) during ECO2RR. The fitted bands of potential-dependent O-H stretching vibrations on Cl-Ni1Cu1-C (d), Cl-Ni1-C (e), and Cl-Cu1-C (f) during ECO2RR. The normalized peak area of 4-HB water and 2-HB water on Cl-Ni1Cu1-C (g), Cl-Ni1-C (h), and Cl-Cu1-C (i) during ECO2RR under different potentials.

Fig. 5. AIMD simulations of the interactions between the interfacial water and single-atom Ni site (a), single-atom Cu site (b), and Ni-Cu dual single-atom sites (c). (d) The adsorption energy of water molecule on various atomic sites. (e) The calculated free energies for CO2-to-CO conversion on various atomic sites. (f) The calculated free energies for HER-Volmer step on various atomic sites. The gray, yellow, blue, cyan, white, and red spheres represent C, Ni, Cu, Cl, H and O atoms, respectively.

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邻近Ni-Cu双单原子位点调控界面水微环境促进CO₂至CO电还原动力学研究

Neighboring Ni-Cu dual single-atom sites regulate the local environment of interfacial water for promoting CO₂ electroreduction kinetics in CO₂-to-CO conversion

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