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<p>Electroconversion of acetylene towards polymer-grade ethylene (EAE) is recognized as a promising substitution for thermo-catalytic route. The excessive active-hydrogen supplies a high current density induces the conspicuous hydrogen evolution, reducing the ethylene Faradaic efficiency (FE). Here, we develop a Cu-Pd single atom alloy (SAA) catalyst, achieving a 90.5% FE with a large ethylene partial current density of −1.16 A cm<sup>−2</sup>, and maintain stability for 110 h at −0.2 A cm<sup>−2</sup> in the flow-cell system. In membrane electrode assembly, Cu-Pd SAA delivers a 90.1% ethylene FE and ~100 % conversion at −2.5 A (−0.1 A cm<sup>−2</sup>), along with 500 h stability for crude ethylene purification. Combined in-situ spectroscopy and DFT calculation reveal that the catalyst facilitates the direct hydrogenation of acetylene via Pd-H species rather than hydrogen spillover. This mechanism concurrently lowers the EAE energy barrier and suppresses the hydrogen evolution reaction. This work provides insights for designing high-efficiency electrocatalysts for hydrogenation electrosynthesis.</p>

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Ampere-level electroconversion of acetylene towards polymer grade ethylene via Pd-H mediated non-spillover hydrogenation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月29日

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  • Lei Bai,
  • Xiao Han,
  • Dingding Li,
  • Chuncai Kong,
  • Jingbo Shi,
  • Mengyao She,
  • Jintao Bai,
  • Jinbo Bai,
  • Kunyue Leng,
  • Yafei Zhao,
  • Yue Lin,
  • Lirong Zheng,
  • Yunteng Qu

摘要

Electroconversion of acetylene towards polymer-grade ethylene (EAE) is recognized as a promising substitution for thermo-catalytic route. The excessive active-hydrogen supplies a high current density induces the conspicuous hydrogen evolution, reducing the ethylene Faradaic efficiency (FE). Here, we develop a Cu-Pd single atom alloy (SAA) catalyst, achieving a 90.5% FE with a large ethylene partial current density of −1.16 A cm−2, and maintain stability for 110 h at −0.2 A cm−2 in the flow-cell system. In membrane electrode assembly, Cu-Pd SAA delivers a 90.1% ethylene FE and ~100 % conversion at −2.5 A (−0.1 A cm−2), along with 500 h stability for crude ethylene purification. Combined in-situ spectroscopy and DFT calculation reveal that the catalyst facilitates the direct hydrogenation of acetylene via Pd-H species rather than hydrogen spillover. This mechanism concurrently lowers the EAE energy barrier and suppresses the hydrogen evolution reaction. This work provides insights for designing high-efficiency electrocatalysts for hydrogenation electrosynthesis.