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<p>Copper (Cu) has been widely recognized as a promising catalyst for electrocatalytic CO<sub>2</sub> reduction (CO<sub>2</sub>R) into value-added multi-carbon (C<sub>2+</sub>) chemicals. However, the limited selectivity of C<sub>2+</sub> products persists due to the inactivation of precisely designed active sites triggered by uncontrollable reconstruction. Herein, we report the successful synthesis of the electrocatalysts of Lewis-acidic aluminum (Al)-doped copper oxides (AlCuO<sub><i>x</i></sub>) with exposed abundant atomic-scale Al − O − Cu sites. The strong Al − O − Cu bridge bonds effectively suppress surface electrochemical reconstruction, and highly stable Cu<sup><i>δ</i>+</sup> species are obtained. The AlCuO<sub><i>x</i></sub> catalyst exhibits an excellent electrocatalytic CO<sub>2</sub>R performance, delivering a Faradaic efficiency (FE) for C<sub>2+</sub> products of 73.6% (ethylene 54.16% and ethanol 19.44%), at a current density of − 221.7&#xa0;mA/cm<sup>2</sup>. The analyses of in situ spectroscopy and theoretical calculations confirm that the high electron localization of Cu active sites in AlCuO<sub><i>x</i></sub> strengthens the interactions between Cu and linearly bonded *CO (*CO<sub>L</sub>) through p − d orbital hybridization, thus facilitating C − C coupling and steering the CO<sub>2</sub> electroreduction pathway toward C<sub>2+</sub> products. This work provides new insights into constructing reconstruction-resistant Cu-based catalysts that enable efficient and stable CO<sub>2</sub>-to-C<sub>2+</sub> conversion.</p>

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Highly Stable Cuδ+ Sites at Reconstruction-Resistant Al‒O‒Cu Bridge Bond for Boosting CO2 Electroreduction into Multi-Carbon Products

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月11日

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  • Zhiling Tang,
  • Yingli Wang,
  • Yuechang Wei,
  • Jing Xiong,
  • Jinqing Jiao,
  • Yunpeng Liu,
  • Zhen Zhao

摘要

Copper (Cu) has been widely recognized as a promising catalyst for electrocatalytic CO2 reduction (CO2R) into value-added multi-carbon (C2+) chemicals. However, the limited selectivity of C2+ products persists due to the inactivation of precisely designed active sites triggered by uncontrollable reconstruction. Herein, we report the successful synthesis of the electrocatalysts of Lewis-acidic aluminum (Al)-doped copper oxides (AlCuOx) with exposed abundant atomic-scale Al − O − Cu sites. The strong Al − O − Cu bridge bonds effectively suppress surface electrochemical reconstruction, and highly stable Cuδ+ species are obtained. The AlCuOx catalyst exhibits an excellent electrocatalytic CO2R performance, delivering a Faradaic efficiency (FE) for C2+ products of 73.6% (ethylene 54.16% and ethanol 19.44%), at a current density of − 221.7 mA/cm2. The analyses of in situ spectroscopy and theoretical calculations confirm that the high electron localization of Cu active sites in AlCuOx strengthens the interactions between Cu and linearly bonded *CO (*COL) through p − d orbital hybridization, thus facilitating C − C coupling and steering the CO2 electroreduction pathway toward C2+ products. This work provides new insights into constructing reconstruction-resistant Cu-based catalysts that enable efficient and stable CO2-to-C2+ conversion.