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

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

Abstract

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

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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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65090-5

https://www.cjcatal.com/EN/Y2026/V86/I7/212

Figures/Tables 7

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

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