Engineering substitutional AgZn3 on penetration electrodes via in-situ reconstruction for ampere-level CO2 electroreduction

doi:10.1016/S1872-2067(26)65046-2

Chinese Journal of Catalysis ›› 2026, Vol. 86: 201-211.DOI: 10.1016/S1872-2067(26)65046-2

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Engineering substitutional AgZn₃ on penetration electrodes via in-situ reconstruction for ampere-level CO₂ electroreduction

Xiaohu Liu^a^,¹, Shoujie Li^a^,¹, Jianing Mao^a^,^c^,¹, Aohui Chen^a, Xiao Dong^a^,^*(), Yiheng Wei^a, Jiayu Xia^a^,^b, Huanyi Zhu^a^,^b, Xiaotong Wang^a^,^b, Ziran Xu^a^,^b^,^c, Guihua Li^a, Yanfang Song^a, Wei Wei^a^,^b^,^*(), Wei Chen^a^,^b^,^*()

^a Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China
^b University of Chinese Academy of Sciences, Beijing 100049, China
^c Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China

Received:2025-10-30 Accepted:2025-12-18 Online:2026-07-18 Published:2026-06-12
Contact: *E-mail: dongx@sari.ac.cn (X. Dong), weiwei@sari.ac.cn (W. Wei), chenw@sari.ac.cn (W. Chen).
About author:¹Contributed equally to this work.
Supported by:
Strategic Priority Research Program of the Chinese Academy of Sciences(XDB1500302);Strategic Priority Research Program of the Chinese Academy of Sciences(XDA0390402);National Key R&D Program of China(2022YFA1504604);National Natural Science Foundation of China(22478408);National Natural Science Foundation of China(22479156);National Natural Science Foundation of China(22302223);Major Project of the Science and Technology Department of Inner Mongolia(2021ZD0020);Special Project for Innovation in Modern Steel Industry of Hebei Province(252G4001D);Science and Technology Innovation Plan of Shanghai Science and Technology Commission(23DZ1202600);Science and Technology Innovation Plan of Shanghai Science and Technology Commission(23DZ1201804);Program of Shanghai Academic/Technology Research Leader(23XD1404400);Shanghai Sailing Program(23YF1453300);Youth Innovation Promotion Association of Chinese Academy of Sciences(E224301401);Outstanding Young Talent Project of Shanghai Advanced Research Institute, Chinese Academy of Sciences(E254991ZZ1)

Abstract

Abstract:

The electrochemical reduction of CO₂ to CO offers a promising route for mitigating carbon emissions and producing sustainable feedstocks. Although noble metals like Ag exhibit high CO selectivity, their high cost and scarcity hinder scalability. Earth-abundant Zn catalysts suffer from intrinsic activity limitations, while alloying with trace Ag would modulate electronic structures for tuning its CO₂ electroreduction activity. Herein, a surface-alloyed Ag-Zn hollow-fiber penetration electrode (HPE) is constructed via an electrochemically induced reconfiguration process that transforms the initial phase-separated Ag clusters on ZnO substrate into a homogeneously dispersed Ag-Zn alloy (AgZn₃). The resulting Ag-Zn HPE achieves 91% faradaic efficiency for CO at 1.2 A cm⁻² and demonstrates long-term electrolysis over 150 hours, as well as promising cost-effectiveness for industrial applications. Combined with the penetration effect that effectively mitigates CO₂ mass transport limitations, the HPE enables high-rate CO production even at large current densities. Mechanistic investigations reveal that alloying modifies the d-band center of Zn, strengthens *COOH adsorption and facilitates *CO desorption to boost CO formation while suppressing hydrogen evolution reaction. This work provides fundamental insights into the role of surface alloying in enhancing CO₂ reduction kinetics and presents a scalable electrode architecture with significant potential for sustainable CO₂ conversion.

Key words: CO₂ electroreduction, Structural reconfiguration, Electrocatalyst, Hollow-fiber penetration electrode, Ag-Zn alloy

Xiaohu Liu, Shoujie Li, Jianing Mao, Aohui Chen, Xiao Dong, Yiheng Wei, Jiayu Xia, Huanyi Zhu, Xiaotong Wang, Ziran Xu, Guihua Li, Yanfang Song, Wei Wei, Wei Chen. Engineering substitutional AgZn₃ on penetration electrodes via in-situ reconstruction for ampere-level CO₂ electroreduction[J]. Chinese Journal of Catalysis, 2026, 86: 201-211.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65046-2

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Figures/Tables 5

Fig. 1. (a) Diagrammatic presentation of synthesis procedures for Ag-Zn HPE. The SEM images of outer surface Ag-ZnO HFT (b1) and Ag-Zn HPE (c1). HRTEM image and EDS element mapping image of Ag-ZnO HFT (b2-b4) and Ag-Zn HPE (c2-c4). Spatial distribution of Zn/Ag overlay on Ag-ZnO HFT (b5) and Ag-Zn HPE (c5) detected by ToF-SIMS. (d) XRD patterns. (e) Ag 3d XPS spectra. (f) Operando Raman spectroscopy spectra of Ag-ZnO HFT electrochemical reduction to Ag-Zn HPE and ZnO HFT electrochemical reduction to Zn HPE.

Fig. 2. Normalized Zn K-edge (a) and Ag K-edge (c) XANES spectra. Fourier-transform Zn K-edge (b) and Ag K-edge (d) EXAFS spectra of different samples. EXAFS wavelet transforms (WT) at the Ag K-edge for Ag foil (e), Ag-ZnO HFT (f), and Ag-Zn HPE (g).

Fig. 3. (a) Faradaic efficiency of eCO2RR products at varying current densities from 0.1 to 1.8 A?cm?2 over Ag-Zn HPE and Zn HPE. (b) Partial current densities of eCO2RR products over Ag-Zn HPE and Zn HPE at different potentials. (c) CO formation rate (yield rate), CO partial current density, and CO faradaic/energy efficiency of Ag-Zn HPE. (d) Long-term electrolysis eCO2RR performance of Ag-Zn HPE at 1.2 A cm?2. Comparison of eCO2RR performances (e) and critical cost parameters (f) of Ag-Zn HPE with those of recently reported representative electrocatalysts for CO production.

Fig. 4. Schematic diagrams of the eCO2RR mechanism over Ag-Zn HPE in penetration (a) and nonpenetration (b) modes. (c) LSV responses under CO2 and Ar atmospheres for both modes. (d) Experimental CO partial current densities under penetration and nonpenetration conditions compared with theoretical current densities across various CO2 flow rates. (e) Experimental Tafel plots derived for both modes at different CO2 flow rates. (f) EIS measured under CO2 and Ar for both modes.

Fig. 5. (a) In-situ ATR-FTIR of eCO2RR over Ag-Zn HPE and Zn HPE (at same absorbance scale). (b) The PDOS of metal-d orbitals for the AgZn3(101) and Zn(101) models. Free energy diagrams of eCO2RR (c) and HER (d) on the AgZn3(101) and Zn(101) models.

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Engineering substitutional AgZn₃ on penetration electrodes via in-situ reconstruction for ampere-level CO₂ electroreduction

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