Lanthanide single-atom catalysts for efficient CO2-to-CO electroreduction

Abstract Single-atom catalysts (SACs) have received increasing attention due to their 100% atomic utilization efficiency. The electrochemical CO2 reduction reaction (CO2RR) to CO using SAC offers a promising approach for CO2 utilization, but achieving facile CO2 adsorption and CO desorption remains...

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Main Authors: Qiyou Wang, Tao Luo, Xueying Cao, Yujie Gong, Yuxiang Liu, Yusen Xiao, Hongmei Li, Franz Gröbmeyer, Ying-Rui Lu, Ting-Shan Chan, Chao Ma, Kang Liu, Junwei Fu, Shiguo Zhang, Changxu Liu, Zhang Lin, Liyuan Chai, Emiliano Cortes, Min Liu
Format: Article
Language:English
Published: Nature Portfolio 2025-03-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-57464-8
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author Qiyou Wang
Tao Luo
Xueying Cao
Yujie Gong
Yuxiang Liu
Yusen Xiao
Hongmei Li
Franz Gröbmeyer
Ying-Rui Lu
Ting-Shan Chan
Chao Ma
Kang Liu
Junwei Fu
Shiguo Zhang
Changxu Liu
Zhang Lin
Liyuan Chai
Emiliano Cortes
Min Liu
author_facet Qiyou Wang
Tao Luo
Xueying Cao
Yujie Gong
Yuxiang Liu
Yusen Xiao
Hongmei Li
Franz Gröbmeyer
Ying-Rui Lu
Ting-Shan Chan
Chao Ma
Kang Liu
Junwei Fu
Shiguo Zhang
Changxu Liu
Zhang Lin
Liyuan Chai
Emiliano Cortes
Min Liu
author_sort Qiyou Wang
collection DOAJ
description Abstract Single-atom catalysts (SACs) have received increasing attention due to their 100% atomic utilization efficiency. The electrochemical CO2 reduction reaction (CO2RR) to CO using SAC offers a promising approach for CO2 utilization, but achieving facile CO2 adsorption and CO desorption remains challenging for traditional SACs. Instead of singling out specific atoms, we propose a strategy utilizing atoms from the entire lanthanide (Ln) group to facilitate the CO2RR. Density functional theory calculations, operando spectroscopy, and X-ray absorption spectroscopy elucidate the bridging adsorption mechanism for a representative erbium (Er) single-atom catalyst. As a result, we realize a series of Ln SACs spanning 14 elements that exhibit CO Faradaic efficiencies exceeding 90%. The Er catalyst achieves a high turnover frequency of ~130,000 h− 1 at 500 mA cm− 2. Moreover, 34.7% full-cell energy efficiency and 70.4% single-pass CO2 conversion efficiency are obtained at 200 mA cm− 2 with acidic electrolyte. This catalytic platform leverages the collective potential of the lanthanide group, introducing new possibilities for efficient CO2-to-CO conversion and beyond through the exploration of unique bonding motifs in single-atom catalysts.
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spelling doaj-art-cbc77dc813b14a74906a5b525bb933fb2025-08-20T02:49:25ZengNature PortfolioNature Communications2041-17232025-03-0116111010.1038/s41467-025-57464-8Lanthanide single-atom catalysts for efficient CO2-to-CO electroreductionQiyou Wang0Tao Luo1Xueying Cao2Yujie Gong3Yuxiang Liu4Yusen Xiao5Hongmei Li6Franz Gröbmeyer7Ying-Rui Lu8Ting-Shan Chan9Chao Ma10Kang Liu11Junwei Fu12Shiguo Zhang13Changxu Liu14Zhang Lin15Liyuan Chai16Emiliano Cortes17Min Liu18Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityCollege of Materials Science and Engineering, Linyi UniversitySchool of Electrical Engineering, University of South ChinaHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityNanoinstitute Munich, Faculty of Physics, Ludwig-Maximilians-Universität (LMU)National Synchrotron Radiation Research Center, 300National Synchrotron Radiation Research Center, 300College of Materials Science and Engineering, Hunan UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityHunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityCollege of Materials Science and Engineering, Hunan UniversityCentre for Metamaterial Research & Innovation, Department of Engineering, University of ExeterSchool of Metallurgy and Environment, Central South UniversitySchool of Metallurgy and Environment, Central South UniversityNanoinstitute Munich, Faculty of Physics, Ludwig-Maximilians-Universität (LMU)Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, State Key Laboratory of Powder Metallurgy, School of Physics, Central South UniversityAbstract Single-atom catalysts (SACs) have received increasing attention due to their 100% atomic utilization efficiency. The electrochemical CO2 reduction reaction (CO2RR) to CO using SAC offers a promising approach for CO2 utilization, but achieving facile CO2 adsorption and CO desorption remains challenging for traditional SACs. Instead of singling out specific atoms, we propose a strategy utilizing atoms from the entire lanthanide (Ln) group to facilitate the CO2RR. Density functional theory calculations, operando spectroscopy, and X-ray absorption spectroscopy elucidate the bridging adsorption mechanism for a representative erbium (Er) single-atom catalyst. As a result, we realize a series of Ln SACs spanning 14 elements that exhibit CO Faradaic efficiencies exceeding 90%. The Er catalyst achieves a high turnover frequency of ~130,000 h− 1 at 500 mA cm− 2. Moreover, 34.7% full-cell energy efficiency and 70.4% single-pass CO2 conversion efficiency are obtained at 200 mA cm− 2 with acidic electrolyte. This catalytic platform leverages the collective potential of the lanthanide group, introducing new possibilities for efficient CO2-to-CO conversion and beyond through the exploration of unique bonding motifs in single-atom catalysts.https://doi.org/10.1038/s41467-025-57464-8
spellingShingle Qiyou Wang
Tao Luo
Xueying Cao
Yujie Gong
Yuxiang Liu
Yusen Xiao
Hongmei Li
Franz Gröbmeyer
Ying-Rui Lu
Ting-Shan Chan
Chao Ma
Kang Liu
Junwei Fu
Shiguo Zhang
Changxu Liu
Zhang Lin
Liyuan Chai
Emiliano Cortes
Min Liu
Lanthanide single-atom catalysts for efficient CO2-to-CO electroreduction
Nature Communications
title Lanthanide single-atom catalysts for efficient CO2-to-CO electroreduction
title_full Lanthanide single-atom catalysts for efficient CO2-to-CO electroreduction
title_fullStr Lanthanide single-atom catalysts for efficient CO2-to-CO electroreduction
title_full_unstemmed Lanthanide single-atom catalysts for efficient CO2-to-CO electroreduction
title_short Lanthanide single-atom catalysts for efficient CO2-to-CO electroreduction
title_sort lanthanide single atom catalysts for efficient co2 to co electroreduction
url https://doi.org/10.1038/s41467-025-57464-8
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