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<p>Cu-based metal–organic frameworks (MOFs) have demonstrated promising potential for electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) toward CH<sub>4</sub> production. However, achieving high CH<sub>4</sub> selectivity under industrial-level current densities remains challenging. Although high-valent Cu species are favorable for CH<sub>4</sub> generation, the reduction of Cu during the CO<sub>2</sub>RR process is inevitable. In this work, an Al-doped CuAl-BTC catalyst was successfully synthesized by incorporating the strongly oxyphilic metal Al. X-ray photoelectron spectroscopy (XPS) results reveal that the introduction of Al effectively suppresses the reduction of Cu, preserving more Cu<sup>2+</sup> sites and enhancing the adsorption of the *CO intermediate. At 500&#xa0;mA cm<sup>−2</sup>, the as-prepared CuAl-BTC catalyst exhibits a faradaic efficiency (FE) of 79.1% for methane, which is 1.5 times higher than that of Cu-BTC. In situ Raman and infrared spectroscopy analyses further demonstrate that the stronger adsorption of the *CO intermediate on the CuAl-BTC catalyst accelerated its protonation process, which in turn promoted the conversion of CO<sub>2</sub> to CH<sub>4</sub>. These findings propose a strategy of stabilizing high-valent Cu sites via oxyphilic metals to enhance key intermediate adsorption, offering a new avenue for efficient electrocatalytic CO₂ reduction to CH<sub>4</sub>.</p>

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Stabilizing Cu2+ species by Al doping with enhanced *CO adsorption for highly efficient electrochemical CO2 reduction to CH4

  • 期刊论文

  • 发表日期：

    2026年2月24日

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  • Yunpeng Zhan,
  • Jinrong Jia,
  • Jingbo Shi,
  • Guanghui Lei,
  • Yi Wang,
  • Kunyue Leng,
  • Yunteng Qu

摘要

Cu-based metal–organic frameworks (MOFs) have demonstrated promising potential for electrochemical CO2 reduction reaction (CO2RR) toward CH4 production. However, achieving high CH4 selectivity under industrial-level current densities remains challenging. Although high-valent Cu species are favorable for CH4 generation, the reduction of Cu during the CO2RR process is inevitable. In this work, an Al-doped CuAl-BTC catalyst was successfully synthesized by incorporating the strongly oxyphilic metal Al. X-ray photoelectron spectroscopy (XPS) results reveal that the introduction of Al effectively suppresses the reduction of Cu, preserving more Cu2+ sites and enhancing the adsorption of the *CO intermediate. At 500 mA cm−2, the as-prepared CuAl-BTC catalyst exhibits a faradaic efficiency (FE) of 79.1% for methane, which is 1.5 times higher than that of Cu-BTC. In situ Raman and infrared spectroscopy analyses further demonstrate that the stronger adsorption of the *CO intermediate on the CuAl-BTC catalyst accelerated its protonation process, which in turn promoted the conversion of CO2 to CH4. These findings propose a strategy of stabilizing high-valent Cu sites via oxyphilic metals to enhance key intermediate adsorption, offering a new avenue for efficient electrocatalytic CO₂ reduction to CH4.