Thermodynamic control of Cu-I nanotopologies enables solar-driven CO <sub>2</sub> -to-multicarbon conversion

Solar-driven electrochemical CO 2 reduction to multicarbon (C 2+ ) products presents a promising avenue for artificial photosynthesis, yet remains constrained by high overpotentials and limited conversion efficiency. Here, we developed an alkaline environment-modulated prereduction strategy that capitalizes on the divergent thermodynamic stabilities of precursors, enabling the precise synthesis of iodine-doped copper nanotopologies (Cu-I NTs). Featuring tunable under-coordination defects and stabilized high-energy adsorption sites, the Cu-I NTs achieve an onset potential of only −0.37 V versus the reversible hydrogen electrode for C 2+ formation. Operando Raman measurement and density functional theory calculation reveal that the tailored surface topologies favor Cu-CO rotation adsorption, enabling dynamic reorientation from bridge- to atop-binding configurations, which collectively lowers the barrier for CO-CO coupling. Impressively, powering the electrolyzer by a perovskite/silicon tandem together with a single-junction silicon photovoltaic device, the system delivers a photocurrent of 12.34 mA cm −2 at 2.17 V under standard AM 1.5 illumination, achieving a solar-to-C 2+ conversion efficiency of 8.64%.

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Publication Details

Journal
Science Advances
Published
2026-07-17
DOI
https://doi.org/10.1126/sciadv.aec6434
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
Field-Weighted Citation Impact
0.00

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article

Thermodynamic control of Cu-I nanotopologies enables solar-driven CO 2 -to-multicarbon conversion

Xixiang Xu, Zhenguo Li, Q Zhang, Xiaobing Gu et al.
Science Advances
CO2 Reduction Techniques and Catalysts
article

Thermodynamic control of Cu-I nanotopologies enables solar-driven CO 2 -to-multicarbon conversion

Xixiang Xu, Zhenguo Li, Q Zhang, Xiaobing Gu, Ying Yang, Guanlan Chen, Han He, Jing Gao, Yajun Gao, Xiaodan Zhang, Lijun Zhang, Hong Zhang, Li M, Bo He, Y.H. He, Yuanzhang Zhao, Xingfei Chen
article en

Abstract

Solar-driven electrochemical CO 2 reduction to multicarbon (C 2+ ) products presents a promising avenue for artificial photosynthesis, yet remains constrained by high overpotentials and limited conversion efficiency. Here, we developed an alkaline environment-modulated prereduction strategy that capitalizes on the divergent thermodynamic stabilities of precursors, enabling the precise synthesis of iodine-doped copper nanotopologies (Cu-I NTs). Featuring tunable under-coordination defects and stabilized high-energy adsorption sites, the Cu-I NTs achieve an onset potential of only −0.37 V versus the reversible hydrogen electrode for C 2+ formation. Operando Raman measurement and density functional theory calculation reveal that the tailored surface topologies favor Cu-CO rotation adsorption, enabling dynamic reorientation from bridge- to atop-binding configurations, which collectively lowers the barrier for CO-CO coupling. Impressively, powering the electrolyzer by a perovskite/silicon tandem together with a single-junction silicon photovoltaic device, the system delivers a photocurrent of 12.34 mA cm −2 at 2.17 V under standard AM 1.5 illumination, achieving a solar-to-C 2+ conversion efficiency of 8.64%.

Science AdvancesVol. 12(29)
Nankai University (CN), State Key Laboratory on Integrated Optoelectronics (CN), Green Technology (US), Unité Matériaux et Transformations (FR), École Polytechnique Fédérale de Lausanne (CH), Xi'an Jiaotong University (CN), Nanjing University of Aeronautics and Astronautics (CN)
National Natural Science Foundation of China, Natural Science Foundation of Tianjin City
Affordable and clean energy
Openalex Percentile: Top 23%
CO2 Reduction Techniques and Catalysts
DOIOpen Access PDFOpenAlex
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