原子铋替代稳定的4H/fcc多相界面AgBi单原子合金用于高效CO2还原

doi:10.1016/S1872-2067(26)65090-5

催化学报 ›› 2026, Vol. 86: 212-224.DOI: 10.1016/S1872-2067(26)65090-5

原子铋替代稳定的4H/fcc多相界面AgBi单原子合金用于高效CO₂还原

王文搏^a, 龚善和^a, 阚二军^b, 朱国兴^a^,^*(), 霍鹏伟^a, 关锦彤^c^,^*(), 吕晓萌^a^,^*()

^a 江苏大学化学化工学院, 江苏镇江 212013
^b 南京理工大学应用物理系, 能源与微结构研究院, 江苏南京 210094
^c 江苏大学材料科学与工程学院, 江苏镇江 212013

收稿日期:2025-11-05 接受日期:2026-01-26 出版日期:2026-07-05 发布日期:2026-06-12
通讯作者: ^*电子信箱: zhuguoxing@ujs.edu.cn (朱国兴),
guanjt1224@gmail.com (关锦彤),
lvxm@ujs.edu.cn (吕晓萌).
基金资助:
国家自然科学基金(21776115);镇江重点研发计划(GY2021004);江苏大学应急管理学院专项计划(JG-04-12);材料合成与加工新技术国家重点实验室计划(武汉理工大学);材料合成与加工新技术国家重点实验室计划(2024-KF-24);江苏省研究生科研创新实践计划(KYCX24_4005)

Atomic Bi substitution stabilized AgBi single-atom alloy with 4H/fcc heterophase interfaces for efficient CO₂ reduction

Wenbo Wang^a, Shanhe Gong^a, Erjun Kan^b, Guoxing Zhu^a^,^*(), Pengwei Huo^a, Jintong Guan^c^,^*(), Xiaomeng Lv^a^,^*()

^a School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu, China
^b Department of Applied Physics and Institution of Energy and Microstructure, Nanjing University of Science and Technology, Nanjing 210094, Jiangsu, China
^c School of Materials Science and Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu, China

Received:2025-11-05 Accepted:2026-01-26 Online:2026-07-05 Published:2026-06-12
Supported by:
National Natural Science Foundation of China(21776115);Key Research and Development Program of Zhenjiang(GY2021004);Special Program for School of Emergency Management in Jiangsu University(JG-04-12);Program of State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology);Program of State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(2024-KF-24);Innovative Program for Graduate Student Research Practice of Jiangsu Province(KYCX24_4005)

摘要/Abstract

摘要：

面对全球能源需求持续增长与气候变化的双重挑战, 电化学二氧化碳还原反应(CO₂RR)作为一种能够将CO₂转化为高附加值化学品的碳中和技术, 已受到广泛关注, 为实现碳循环和可持续能源存储提供了关键路径. 单原子合金(SAA)催化剂通过将活性金属原子级分散于主体金属中, 实现了电子结构的精确调控, 在优化反应路径、提高催化选择性与活性方面展现出巨大潜力. 然而, 当前SAA催化剂的设计大多基于热力学稳定的单一晶相, 忽略了不同晶相之间形成的界面结构可赋予独特催化性能. 特别是, 在原子尺度上构建稳定的多相界面, 并利用由此产生的晶格应变来进一步优化催化性能, 是一个极具吸引力但充满挑战的研究方向.

针对上述难题, 本研究创新性地提出了原子级替代策略, 以原子半径大于Ag的Bi作为掺杂元素, 利用其作为“界面触发器”, 实现两大目标: 一是稳定常规条件下难以存在的4H-Ag亚稳相, 二是精准构建4H/fcc-Ag多相界面并引入可控晶格应变. 密度泛函理论(DFT)计算从能量和动力学角度验证了该策略的可行性. 在此基础上, 成功合成了一系列不同Bi含量的AgBi SAA催化剂, 并系统评估了其CO₂RR性能. 最优的4H/fcc Ag₄₉Bi₁ SAA催化剂在碱性流动池中, 在200 mA cm⁻²的电流密度下, 实现了99.5%的CO法拉第效率(FE_CO)、70%的单程转换效率、45.6 mmol h⁻¹ cm⁻²的CO产率以及超过330 h的卓越耐久性. 在膜电极组件电解槽中, 在150 mA cm⁻²的电流密度下实现了98.6%的峰值FE_CO, 并在100 mA cm⁻²的电流密度下保持FE_CO > 80%达70 h. 在Zn-CO₂电池中进一步验证了4H/fcc Ag₄₉Bi₁ SAA催化剂的潜在应用, 其展示出0.86 mW cm⁻²的峰值功率密度和98.7%的FE_CO, 以及在2 mA cm⁻²的电流密度下140 h的循环稳定性. 原位拉曼光谱和DFT计算表明, 这种优异的性能源于*COOH生成能垒的降低以及4H/fcc-Ag的Ag-3d与C-2p轨道之间更强的轨道耦合作用.

综上, 本工作不仅为高性能CO₂RR催化剂的设计提供了新范式, 也深化了对SAA催化剂中界面应变效应的理解.

关键词: 单原子合金, 原子级替代, 多相界面, 局域晶格应变, 耐久性

Abstract:

The pressing need to address global energy demand and climate change has positioned electrochemical CO₂ reduction into high-value chemicals as a crucial technology for carbon cycling and sustainable energy storage. However, precise control over the interfacial structure of active sites in single-atom alloy (SAA) remains a considerable challenge, significantly restricting their catalytic performance. In this study, we propose an atomic-level substitution strategy, integrating large atomic radius of Bi atoms into the Ag lattice to trigger and stabilize a 4H/fcc-Ag heterophase interfaces. Theoretical and experimental analyses reveal that the induced lattice strain stabilizes the metastable 4H phase and optimizes the geometric/electronic configuration of active sites, thereby enhancing the orbital overlap between Ag-3d and C-2p orbitals and lowering the energy barrier for *COOH formation. The optimal 4H/fcc Ag₄₉Bi₁ SAA catalyst, comprising approximately 3% 4H-Ag and 97% fcc-Ag, achieves CO Faraday efficiency (FE_CO) of 99.5%, single-pass conversion efficiency of 70%, CO yield of 45.6 mmol h⁻¹ cm⁻² and superior durability over 330 h under 200 mA cm⁻² in an alkaline flow cell. A membrane electrode assembly electrolyzer incorporating the catalyst reached a peak FE_CO of 98.6% at 150 mA cm⁻² and maintaining FE_CO >80% for 70 h under 100 mA cm⁻² without decay. When applied in a customized Zn-CO₂ battery, it delivered a peak power density of 0.86 mW cm⁻², along with 140 h cycling stability at 2 mA cm⁻². This work underscores the potential of atomic-level substitution for precise interface engineering, providing a novel strain-engineering strategy for designing high-performance SAA catalysts.

Key words: Single-atom alloy, Atomic-level substitution, Heterophase interfaces, Local lattice strain, Durability

王文搏, 龚善和, 阚二军, 朱国兴, 霍鹏伟, 关锦彤, 吕晓萌. 原子铋替代稳定的4H/fcc多相界面AgBi单原子合金用于高效CO₂还原[J]. 催化学报, 2026, 86: 212-224.

Wenbo Wang, Shanhe Gong, Erjun Kan, Guoxing Zhu, Pengwei Huo, Jintong Guan, Xiaomeng Lv. Atomic Bi substitution stabilized AgBi single-atom alloy with 4H/fcc heterophase interfaces for efficient CO₂ reduction[J]. Chinese Journal of Catalysis, 2026, 86: 212-224.

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Fig. 1. Theoretical simulation of the 4H-Ag metastable phase. (a) Schematic of several structures for Bi substitution fcc-Ag and 4H-Ag. Structural system energies of one Bi atom in the first or second layer of fcc-Ag and 4H-Ag (b) and four Bi atoms in the first layer of fcc-Ag or 4H-Ag (c). (d) Strategy diagram for increasing the phase transition energy barrier from 4H-Ag to fcc-Ag.

Fig. 2. Synthesis and characterization of 4H/fcc Ag49Bi1. Schematic synthesis (a) and HRTEM image (b) of 4H/fcc Ag49Bi1. The high-magnification STEM images and FFT patterns of the corresponding 4H (c) and fcc (d) areas of the 4H/fcc Ag49Bi1 in (b). (e) HAADF-STEM image of 4H/fcc Ag49Bi1 and corresponding EDX elemental mapping. (f) A representative high-resolution HAADF-STEM image of 4H/fcc Ag49Bi1. The 4H/fcc heterophase interfaces are marked with yellow lines. (g-j) The high-magnification HAADF-STEM images taken from the corresponding areas in (f). (k) AC-HAADF-STEM image of 4H/fcc Ag49Bi1. (l-n) ADF-STEM image and corresponding atomic level EDX elemental mapping of 4H/fcc Ag49Bi1.

Fig. 3. X-ray spectral analysis of Ag and 4H/fcc AgBi. Ag 3d (a) and Bi 4f (b) XPS spectra. Bi L3-edge XAFS spectra (c), FT-EXAFS spectra (d), and Wavelet transform of the EXAFS signal (e) of Bi foil, Bi2O3 and 4H/fcc Ag49Bi1, respectively.

Fig. 4. Activity evaluation of electrochemical CO2RR in H-cell. LSV curves (a), product Faraday efficiency (FE) (b), CO partial current densities (jCO) (c) of Ag, 4H/fcc Ag49Bi1, and 4H/fcc Ag9Bi1. (d) Stability test of 4H/fcc Ag49Bi1 in H-type cell for 12 h at -0.8 V vs. RHE. ECSA value (e) and Tafel slopes (f) of Ag, 4H/fcc Ag49Bi1, and 4H/fcc Ag9Bi1.

Fig. 5. Activity evaluation of electrochemical CO2RR in flow cell. (a) Schematic diagram of the flow cell. (b) LSV curves and (c) CO and H2 FE of Ag and 4H/fcc Ag49Bi1 in flow cell. (d) CO yield at different current density for 4H/fcc Ag49Bi1 SAA. Durability test of 4H/fcc Ag49Bi1 at 200 mA cm−2 for 330 h (e) and durability comparisons with other Ag-based catalysts in the flow cell (f). Single-pass conversion efficiency at (g) 100 and (h) 200 mA cm−2.

Fig. 6. In-situ characterizations and DFT calculations analysis. In-situ surface-enhanced Raman spectra under different potentials over Ag (a) and 4H/fcc Ag49Bi1 (b). In-situ infrared spectroscopy under different potentials over Ag (c) and 4H/fcc Ag49Bi1 (d). (e) Structural modeling of adsorption of *COOH and *CO on 4H/fcc Ag49Bi1. (f) Free energy profiles for electrocatalytic CO2 reduction on fcc-Ag, 4H-Ag and 4H/fcc-Ag. (g) PDOS for *COOH adsorption on fcc-Ag and 4H/fcc-Ag. The dotted line represents the Fermi energy level. (h) Charge density difference of *COOH adsorption on 4H/fcc-Ag and fcc-Ag. Yellow and blue regions stand for the accumulation and dissipation of charges, respectively. The isosurface level is 0.003 au.

Fig. 7. Electrochemical CO2RR in MEA electrolyzer and Zn-CO2 battery. (a) Schematic diagram of the MEA. (b) LSV curves of Ag and 4H/fcc Ag49Bi1 in MEA. (c) FECO of Ag and 4H/fcc Ag49Bi1 at different current densities and the corresponding cell voltages. (d) Stability test of 4H/fcc Ag49Bi1||Ni foam at 100 mA cm−2. (e) Schematic diagram of the Zn-CO2 battery. (f) Charge-discharge polarization curve. Inset is the power density curve. (g) Galvanostatic discharge curves at different current densities and the corresponding FECO. (h) Galvanostatic discharge-charge cycling plots of 4H/fcc Ag49Bi1-based ZCB for 140 h at 2 mA cm−2.

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原子铋替代稳定的4H/fcc多相界面AgBi单原子合金用于高效CO₂还原

Atomic Bi substitution stabilized AgBi single-atom alloy with 4H/fcc heterophase interfaces for efficient CO₂ reduction

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[6]	Maria Flytzani-Stephanopoulos. 视角:单原子尺度的负载型金属催化剂[J]. 催化学报, 2017, 38(9): 1432-1442.