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Spontaneous water dissociation on intermetallic electride LaCu0.67Si1.33 enhances electrochemical methanization of CO2

Author

Listed:
  • Luming Zhang

    (Taiyuan University of Technology
    Huairou District
    Peking University)

  • Huan Ma

    (Huairou District
    Chinese Academy of Sciences
    No. 19A Yuquan Road)

  • Yongfang Sun

    (Chinese Academy of Sciences)

  • Yilin Zhao

    (Peking University)

  • Huiying Deng

    (199 Ren’ai Road)

  • Yuhang Wang

    (199 Ren’ai Road)

  • Fei Wang

    (Chinese Academy of Sciences)

  • Xiao-Dong Wen

    (Taiyuan University of Technology
    Huairou District
    Chinese Academy of Sciences
    No. 19A Yuquan Road)

  • Mingchuan Luo

    (Peking University)

Abstract

Renewable electricity driven CO2 electroreduction into methane offers a sustainable route to mitigate our dependence on natural gas. However, this route is now limited by the unsatisfied efficiency and short durability, which originates from a kinetic disparity between water dissociation (WD) and proton-coupled electron transfer on existing catalysts. Herein, we harness the exceptional WD capability of the intermetallic electride (IE) materials for the electrocatalytic methanization from CO2. Combinative experimental and theoretical approaches strongly evidence a spontaneous WD on an IE LaCu0.67Si1.33 catalyst due to its unique electronic structure (strongly modified charge states, reversible lattice hydride ions and anionic electrons). Consequently, this catalyst exhibits improved methanization performance in alkaline flow cells, achieving a methane Faraday efficiency of 72% at −1.21 V versus the reversible hydrogen electrode (vs. RHE) and peak partial current density of 476.7 mA cm−2 at −1.52 V vs. RHE. Energetic calculations further establish the mechanistic link between WD and methanization processes on our catalyst, on which a lowered free energy barrier for the key *CO to *CHO transformation step is observed. This work sheds light on the pivotal role of WD and expands the repertoire of materials for efficient electrocatalytic methanization from CO2.

Suggested Citation

  • Luming Zhang & Huan Ma & Yongfang Sun & Yilin Zhao & Huiying Deng & Yuhang Wang & Fei Wang & Xiao-Dong Wen & Mingchuan Luo, 2025. "Spontaneous water dissociation on intermetallic electride LaCu0.67Si1.33 enhances electrochemical methanization of CO2," Nature Communications, Nature, vol. 16(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-60353-9
    DOI: 10.1038/s41467-025-60353-9
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    as
    1. Wensheng Fang & Wei Guo & Ruihu Lu & Ya Yan & Xiaokang Liu & Dan Wu & Fu Min Li & Yansong Zhou & Chaohui He & Chenfeng Xia & Huiting Niu & Sicong Wang & Youwen Liu & Yu Mao & Chengyi Zhang & Bo You & , 2024. "Publisher Correction: Durable CO2 conversion in the proton-exchange membrane system," Nature, Nature, vol. 627(8005), pages 13-13, March.
    2. Zishan Han & Daliang Han & Zhe Chen & Jiachen Gao & Guangyi Jiang & Xinyu Wang & Shuaishuai Lyu & Yong Guo & Chuannan Geng & Lichang Yin & Zhe Weng & Quan-Hong Yang, 2022. "Author Correction: Steering surface reconstruction of copper with electrolyte additives for CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-1, December.
    3. Weiwei Fu & Jin Wan & Huijuan Zhang & Jian Li & Weigen Chen & Yuke Li & Zaiping Guo & Yu Wang, 2022. "Photoinduced loading of electron-rich Cu single atoms by moderate coordination for hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    4. Yao Yang & Sheena Louisia & Sunmoon Yu & Jianbo Jin & Inwhan Roh & Chubai Chen & Maria V. Fonseca Guzman & Julian Feijóo & Peng-Cheng Chen & Hongsen Wang & Christopher J. Pollock & Xin Huang & Yu-Tsun, 2023. "Operando studies reveal active Cu nanograins for CO2 electroreduction," Nature, Nature, vol. 614(7947), pages 262-269, February.
    5. Hong-Jing Zhu & Duan-Hui Si & Hui Guo & Ziao Chen & Rong Cao & Yuan-Biao Huang, 2024. "Oxygen-tolerant CO2 electroreduction over covalent organic frameworks via photoswitching control oxygen passivation strategy," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    6. Xinyan Liu & Jianping Xiao & Hongjie Peng & Xin Hong & Karen Chan & Jens K. Nørskov, 2017. "Understanding trends in electrochemical carbon dioxide reduction rates," Nature Communications, Nature, vol. 8(1), pages 1-7, August.
    7. Qiubo Zhang & Zhigang Song & Xianhu Sun & Yang Liu & Jiawei Wan & Sophia B. Betzler & Qi Zheng & Junyi Shangguan & Karen C. Bustillo & Peter Ercius & Prineha Narang & Yu Huang & Haimei Zheng, 2024. "Atomic dynamics of electrified solid–liquid interfaces in liquid-cell TEM," Nature, Nature, vol. 630(8017), pages 643-647, June.
    8. Jiqing Jiao & Qing Yuan & Meijie Tan & Xiaoqian Han & Mingbin Gao & Chao Zhang & Xuan Yang & Zhaolin Shi & Yanbin Ma & Hai Xiao & Jiangwei Zhang & Tongbu Lu, 2023. "Constructing asymmetric double-atomic sites for synergistic catalysis of electrochemical CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    9. Yizhou Dai & Huan Li & Chuanhao Wang & Weiqing Xue & Menglu Zhang & Donghao Zhao & Jing Xue & Jiawei Li & Laihao Luo & Chunxiao Liu & Xu Li & Peixin Cui & Qiu Jiang & Tingting Zheng & Songqi Gu & Yao , 2023. "Manipulating local coordination of copper single atom catalyst enables efficient CO2-to-CH4 conversion," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    10. Wensheng Fang & Wei Guo & Ruihu Lu & Ya Yan & Xiaokang Liu & Dan Wu & Fu Min Li & Yansong Zhou & Chaohui He & Chenfeng Xia & Huiting Niu & Sicong Wang & Youwen Liu & Yu Mao & Chengyi Zhang & Bo You & , 2024. "Durable CO2 conversion in the proton-exchange membrane system," Nature, Nature, vol. 626(7997), pages 86-91, February.
    11. Zishan Han & Daliang Han & Zhe Chen & Jiachen Gao & Guangyi Jiang & Xinyu Wang & Shuaishuai Lyu & Yong Guo & Chuannan Geng & Lichang Yin & Zhe Weng & Quan-Hong Yang, 2022. "Steering surface reconstruction of copper with electrolyte additives for CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    12. Mingchuan Luo & Ziyun Wang & Yuguang C. Li & Jun Li & Fengwang Li & Yanwei Lum & Dae-Hyun Nam & Bin Chen & Joshua Wicks & Aoni Xu & Taotao Zhuang & Wan Ru Leow & Xue Wang & Cao-Thang Dinh & Ying Wang , 2019. "Hydroxide promotes carbon dioxide electroreduction to ethanol on copper via tuning of adsorbed hydrogen," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    13. Yu Zhang & Long-Zhang Dong & Shan Li & Xin Huang & Jia-Nan Chang & Jian-Hui Wang & Jie Zhou & Shun-Li Li & Ya-Qian Lan, 2021. "Coordination environment dependent selectivity of single-site-Cu enriched crystalline porous catalysts in CO2 reduction to CH4," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    14. Yuhang Li & Aoni Xu & Yanwei Lum & Xue Wang & Sung-Fu Hung & Bin Chen & Ziyun Wang & Yi Xu & Fengwang Li & Jehad Abed & Jianan Erick Huang & Armin Sedighian Rasouli & Joshua Wicks & Laxmi Kishore Saga, 2020. "Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    15. Zhenhua Zhang & Sha-Sha Wang & Rui Song & Tian Cao & Liangfeng Luo & Xuanye Chen & Yuxian Gao & Jiqing Lu & Wei-Xue Li & Weixin Huang, 2017. "The most active Cu facet for low-temperature water gas shift reaction," Nature Communications, Nature, vol. 8(1), pages 1-10, December.
    16. Huali Wu & Lingqi Huang & Janis Timoshenko & Kun Qi & Wensen Wang & Jiefeng Liu & Yang Zhang & Shaokang Yang & Eddy Petit & Valérie Flaud & Ji Li & Chrystelle Salameh & Philippe Miele & Luc Lajaunie &, 2024. "Selective and energy-efficient electrosynthesis of ethylene from CO2 by tuning the valence of Cu catalysts through aryl diazonium functionalization," Nature Energy, Nature, vol. 9(4), pages 422-433, April.
    17. Cao-Thang Dinh & Ankit Jain & F. Pelayo García Arquer & Phil De Luna & Jun Li & Ning Wang & Xueli Zheng & Jun Cai & Benjamin Z. Gregory & Oleksandr Voznyy & Bo Zhang & Min Liu & David Sinton & Ethan J, 2019. "Multi-site electrocatalysts for hydrogen evolution in neutral media by destabilization of water molecules," Nature Energy, Nature, vol. 4(2), pages 107-114, February.
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