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<p>Cu-based electrocatalysts are promising for the electrocatalytic CO<sub>2</sub> reduction reaction (eCO<sub>2</sub>RR) to realize valuable chemicals production. Here, a Mg-doped Cu based electrocatalysts via transient CO<sub>2</sub> pulsed laser (L<sub>4</sub>-Mg/Cu<sub><i>x</i></sub>O) was synthesized for highly selective eCO<sub>2</sub>RR to ethanol (C<sub>2</sub>H<sub>5</sub>OH). The synergistic effect of Mg-doping and transient CO<sub>2</sub> pulsed laser irradiation enables excellent eCO<sub>2</sub>RR performance, realizing Faradaic efficiencies (FE) of 52.2% and 74.1% for C<sub>2</sub>H<sub>5</sub>OH and C<sub>2</sub> products under a high current density of 298.9 mA cm<sup>−2</sup>, respectively. Operando Raman spectroscopy and DFT simulations results confirm that Mg-doping strategy suppresses the hydrogen evolution reaction (HER), enhances CO adsorption, elevates local pH and accelerates H<sub>2</sub>O dissociation, which could be beneficial for promoting OC–CO coupling and proton supply in eCO<sub>2</sub>RR. Furthermore, Mg incorporation induces electron delocalization in which electron accumulation on the C atom of *CHCOH intermediate and its enhanced p-d orbital coupling with Cu interface, which stabilizes the C–O bond from breakage and selectively favours the C<sub>2</sub>H<sub>5</sub>OH pathway, thus decoupling the selectivity between C<sub>2</sub>H<sub>5</sub>OH and ethylene. When employed in Li-CO<sub>2</sub> batteries, L<sub>4</sub>-Mg/Cu<sub><i>x</i></sub>O delivers 20480 mAh g<sup>−1</sup> discharge capacity and cycling stability over 187 cycles. This work presents a universal strategy for regulating eCO<sub>2</sub>RR selectivity through precise laser energy delivery, demonstrating significant potential for renewable energy conversion and storage.</p>

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Transient pulsed laser synthesis: boosting CO2-ethanol conversion and Li-CO2 batteries performance by p-d orbital hybridization and electron delocalization

  • 期刊论文

  • 发表日期：

    2026年3月9日

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  • Nan Wang,
  • Tinghui An,
  • Jiaqi Li,
  • Yuhao Wang,
  • Dong Xiang,
  • Kedi Cai

摘要

Cu-based electrocatalysts are promising for the electrocatalytic CO2 reduction reaction (eCO2RR) to realize valuable chemicals production. Here, a Mg-doped Cu based electrocatalysts via transient CO2 pulsed laser (L4-Mg/CuxO) was synthesized for highly selective eCO2RR to ethanol (C2H5OH). The synergistic effect of Mg-doping and transient CO2 pulsed laser irradiation enables excellent eCO2RR performance, realizing Faradaic efficiencies (FE) of 52.2% and 74.1% for C2H5OH and C2 products under a high current density of 298.9 mA cm−2, respectively. Operando Raman spectroscopy and DFT simulations results confirm that Mg-doping strategy suppresses the hydrogen evolution reaction (HER), enhances CO adsorption, elevates local pH and accelerates H2O dissociation, which could be beneficial for promoting OC–CO coupling and proton supply in eCO2RR. Furthermore, Mg incorporation induces electron delocalization in which electron accumulation on the C atom of *CHCOH intermediate and its enhanced p-d orbital coupling with Cu interface, which stabilizes the C–O bond from breakage and selectively favours the C2H5OH pathway, thus decoupling the selectivity between C2H5OH and ethylene. When employed in Li-CO2 batteries, L4-Mg/CuxO delivers 20480 mAh g−1 discharge capacity and cycling stability over 187 cycles. This work presents a universal strategy for regulating eCO2RR selectivity through precise laser energy delivery, demonstrating significant potential for renewable energy conversion and storage.