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<p>Acidic electrochemical CO<sub>2</sub> conversion is a promising alternative to overcome the low CO<sub>2</sub> utilization. However, over-reliance on highly concentrated K<sup>+</sup> to inhibit the hydrogen evolution reaction also causes (bi)carbonate precipitation to interfere with catalytic performance. In this work, under the screening and guidance of computational simulations, we present a carbon coated tip-like In<sub>2</sub>O<sub>3</sub> electrocatalyst for stable and efficient acidic CO<sub>2</sub> conversion to synthesize formic acid (HCOOH) with low K<sup>+</sup> concentration. The carbon layer protects the oxidized In species with higher intrinsic activity from reductive corrosion, and also peripherally formulates a tip-induced electric field to regulate the adverse H<sup>+</sup> attraction and desirable K<sup>+</sup> enrichment. In an acidic electrolyte at pH 0.94, only 0.1 M low K<sup>+</sup> is required to achieve a Faradaic efficiency (FE) of 98.9% at 300 mA cm<sup>−2</sup> for HCOOH and a long-time stability of over100 h. By up-scaling the electrode into a 25 cm<sup>2</sup> electrolyzer setup, a total current of 7 A is recorded to sustain a durable HCOOH production of 291.6 mmol L<sup>−1</sup> h<sup>−1</sup>.</p>

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Tip carbon encapsulation customizes cationic enrichment and valence stabilization for low K+ acidic CO2 electroreduction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年2月19日

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  • Zhitong Wang,
  • Dongyu Liu,
  • Chenfeng Xia,
  • Xiaodong Shi,
  • Yansong Zhou,
  • Qiuwen Liu,
  • Jiangtao Huang,
  • Haiyan Wu,
  • Deyu Zhu,
  • Shuyu Zhang,
  • Jing Li,
  • Peilin Deng,
  • Andrey S. Vasenko,
  • Bao Yu Xia,
  • Xinlong Tian

摘要

Acidic electrochemical CO2 conversion is a promising alternative to overcome the low CO2 utilization. However, over-reliance on highly concentrated K+ to inhibit the hydrogen evolution reaction also causes (bi)carbonate precipitation to interfere with catalytic performance. In this work, under the screening and guidance of computational simulations, we present a carbon coated tip-like In2O3 electrocatalyst for stable and efficient acidic CO2 conversion to synthesize formic acid (HCOOH) with low K+ concentration. The carbon layer protects the oxidized In species with higher intrinsic activity from reductive corrosion, and also peripherally formulates a tip-induced electric field to regulate the adverse H+ attraction and desirable K+ enrichment. In an acidic electrolyte at pH 0.94, only 0.1 M low K+ is required to achieve a Faradaic efficiency (FE) of 98.9% at 300 mA cm−2 for HCOOH and a long-time stability of over100 h. By up-scaling the electrode into a 25 cm2 electrolyzer setup, a total current of 7 A is recorded to sustain a durable HCOOH production of 291.6 mmol L−1 h−1.