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<p>The development of efficient acidic CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) to high value-added chemical HCOOH at high current density (&gt;1 A cm<sup>-2</sup>) is crucial. However, addressing high potential, low Faradaic efficiency (FE), and poor stability simultaneously under acidic conditions remains challenging. Here, we construct small PdC<sub>x</sub> interstitial compounds and engineer the interstitial atoms to modulate the catalyst’s soft acid strength, thereby overcoming the triple challenge of “low overpotential-high current density-high stability” in acidic CO₂RR to HCOOH. Density functional theory (DFT) calculations and experimental characterization reveal that interstitial carbon infusion modulates Pd’s soft acid strength and weakens the Pd-O bond energy to form and desorb HCOOH, circumventing CO poisoning of the catalyst. Meanwhile, interstitial carbon infusion optimizes electronic structures, enhancing OCHO intermediate coverage as well as the effective retention and utilization of *H. This effect suppresses hydrogen evolution reaction (HER) while enhancing HCOOH selectivity. The optimized PdC<sub>0.13</sub>/CNT achieves &gt;95% FE<sub>HCOOH</sub> and demonstrates stability in a proton exchange membrane (PEM) electrolyzer, maintaining 1000 mA cm<sup>-2</sup> operation for 500 hours at 1.8 V cell voltage.</p>

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Small PdCx interstitial compound for efficient acidic CO2 electroreduction to formic acid

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月26日

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  • Yaodong Yu,
  • Zuochao Wang,
  • Weizhou Wang,
  • Jiani Han,
  • Tian Dong,
  • Guangzhe Jin,
  • Hongdong Li,
  • Qingliang Lv,
  • Alexander V. Kutchin,
  • Jianping Lai,
  • Lei Wang

摘要

The development of efficient acidic CO2 reduction reaction (CO2RR) to high value-added chemical HCOOH at high current density (>1 A cm-2) is crucial. However, addressing high potential, low Faradaic efficiency (FE), and poor stability simultaneously under acidic conditions remains challenging. Here, we construct small PdCx interstitial compounds and engineer the interstitial atoms to modulate the catalyst’s soft acid strength, thereby overcoming the triple challenge of “low overpotential-high current density-high stability” in acidic CO₂RR to HCOOH. Density functional theory (DFT) calculations and experimental characterization reveal that interstitial carbon infusion modulates Pd’s soft acid strength and weakens the Pd-O bond energy to form and desorb HCOOH, circumventing CO poisoning of the catalyst. Meanwhile, interstitial carbon infusion optimizes electronic structures, enhancing OCHO intermediate coverage as well as the effective retention and utilization of *H. This effect suppresses hydrogen evolution reaction (HER) while enhancing HCOOH selectivity. The optimized PdC0.13/CNT achieves >95% FEHCOOH and demonstrates stability in a proton exchange membrane (PEM) electrolyzer, maintaining 1000 mA cm-2 operation for 500 hours at 1.8 V cell voltage.