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<p>1,3-Butadiene (C<sub>4</sub>H<sub>6</sub>), the main raw material for producing important chemicals (nylon, synthetic resin, rubber), relies on petroleum cracking with intensive carbon emissions. The electrocatalytic dimeric hydrogenation of natural gas/coal-derived C<sub>2</sub>H<sub>2</sub> to C<sub>4</sub>H<sub>6</sub> provides a nonpetroleum pathway. However, C<sub>4</sub>H<sub>6</sub>, as a byproduct of C<sub>2</sub>H<sub>2</sub> hydrogenation, is usually neglected because of its very low Faradaic efficiency. Here, we theoretically and experimentally report a mechanism comprising acetylene dimerization and subsequent hydrogenation. The first dimerization process can be accelerated under appropriate coverage of acetylene and water. A ligand-modifying strategy is subsequently proposed to regulate the wettability of Cu nanoarrays to enable suitable coverages. The optimized 1-dodecanethiol-modified Cu nanoarrays deliver a 65.3% C<sub>4</sub>H<sub>6</sub> Faradaic efficiency at 100 mA cm<sup>−2</sup>. The C<sub>4</sub>H<sub>6</sub> formation kinetics become sluggish at the two ends of the surface C<sub>2</sub>H<sub>2</sub>/H<sub>2</sub>O ratios, and moderate C<sub>2</sub>H<sub>2</sub>/H<sub>2</sub>O coverage accelerates the C‒C coupling process to promote C<sub>4</sub>H<sub>6</sub> production. Moreover, life cycle assessment demonstrates its sustainability.</p>

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Selective electrosynthesis of 1,3-butadiene by tailoring the coverage of acetylene and water

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月1日

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  • Chuanqi Cheng,
  • Jiajun Wang,
  • Fanpeng Chen,
  • Yanran Han,
  • Yichen He,
  • Bin Zhang,
  • Bo-Hang Zhao

摘要

1,3-Butadiene (C4H6), the main raw material for producing important chemicals (nylon, synthetic resin, rubber), relies on petroleum cracking with intensive carbon emissions. The electrocatalytic dimeric hydrogenation of natural gas/coal-derived C2H2 to C4H6 provides a nonpetroleum pathway. However, C4H6, as a byproduct of C2H2 hydrogenation, is usually neglected because of its very low Faradaic efficiency. Here, we theoretically and experimentally report a mechanism comprising acetylene dimerization and subsequent hydrogenation. The first dimerization process can be accelerated under appropriate coverage of acetylene and water. A ligand-modifying strategy is subsequently proposed to regulate the wettability of Cu nanoarrays to enable suitable coverages. The optimized 1-dodecanethiol-modified Cu nanoarrays deliver a 65.3% C4H6 Faradaic efficiency at 100 mA cm−2. The C4H6 formation kinetics become sluggish at the two ends of the surface C2H2/H2O ratios, and moderate C2H2/H2O coverage accelerates the C‒C coupling process to promote C4H6 production. Moreover, life cycle assessment demonstrates its sustainability.