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<p>Renewable electricity driven CO<sub>2</sub> 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 CO<sub>2</sub>. Combinative experimental and theoretical approaches strongly evidence a spontaneous WD on an IE LaCu<sub>0.67</sub>Si<sub>1.33</sub> 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<sup>−2</sup> 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 CO<sub>2</sub>.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年5月30日

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  • Luming Zhang,
  • Huan Ma,
  • Yongfang Sun,
  • Yilin Zhao,
  • Huiying Deng,
  • Yuhang Wang,
  • Fei Wang,
  • Xiao-Dong Wen,
  • Mingchuan Luo

摘要

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.