<p>Electrochemical CO<sub>2</sub> reduction to formic acid is a promising pathway for sustainable carbon utilization, but efficient and durable Sn-based catalysts remain limited. Here, an <i>in situ</i> electrochemical approach is employed to fabricate a porous Sn electrocatalyst via highly cathodic polarization of polycrystalline Sn in alkaline medium. The resulting catalyst features a hierarchical porous structure with a high density of grain boundaries. In CO<sub>2</sub>-saturated NaHCO<sub>3</sub> electrolyte, the <i>in situ</i> synthesized Sn exhibits an early onset potential and delivers a maximum formate Faradaic efficiency of 95% at −1.01&#xa0;V versus. reversible hydrogen electrode (RHE), significantly outperforming pristine Sn. The enhanced activity is attributed to increased active sites arising from grain boundary enrichment and porous morphology. The catalyst maintains structural integrity and achieves 92% formate selectivity over 12&#xa0;h of continuous electrolysis at 12&#xa0;mA&#xa0;cm<sup>−2</sup>. <i>In situ</i> Raman spectroscopy and density functional theory (DFT) calculations elucidate key reaction intermediates, demonstrating the potential of <i>in situ</i> engineered Sn catalysts for efficient CO<sub>2</sub>-to-liquid conversion.</p>

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Facile Synthesis of Highly Selective Porous Sn Electrocatalyst for Electrochemical CO2 Reduction to Formate

  • Samina Farid,
  • Ashi Rashid,
  • Aneela Anwar,
  • Muhammad Ahsan Khan

摘要

Electrochemical CO2 reduction to formic acid is a promising pathway for sustainable carbon utilization, but efficient and durable Sn-based catalysts remain limited. Here, an in situ electrochemical approach is employed to fabricate a porous Sn electrocatalyst via highly cathodic polarization of polycrystalline Sn in alkaline medium. The resulting catalyst features a hierarchical porous structure with a high density of grain boundaries. In CO2-saturated NaHCO3 electrolyte, the in situ synthesized Sn exhibits an early onset potential and delivers a maximum formate Faradaic efficiency of 95% at −1.01 V versus. reversible hydrogen electrode (RHE), significantly outperforming pristine Sn. The enhanced activity is attributed to increased active sites arising from grain boundary enrichment and porous morphology. The catalyst maintains structural integrity and achieves 92% formate selectivity over 12 h of continuous electrolysis at 12 mA cm−2. In situ Raman spectroscopy and density functional theory (DFT) calculations elucidate key reaction intermediates, demonstrating the potential of in situ engineered Sn catalysts for efficient CO2-to-liquid conversion.