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<p>Cobalt phthalocyanine (CoPc) is recognized for catalysing electrochemical CO<sub>2</sub> reduction into methanol at high Faradaic efficiency but is subject to deactivation. Cobalt tetraaminophthalocyanine (CoPc-NH<sub>2</sub>) shows improved stability, but its methanol Faradaic efficiency is below 30%. This study addresses these limitations in selectivity, reactivity and stability by rationally designing a dual-site cascade catalyst. Here we quantify the local concentration of CO, a key intermediate of the reaction, near a working CoPc-NH<sub>2</sub> catalyst and show that co-loading nickel tetramethoxyphthalocyanine (NiPc-OCH<sub>3</sub>) with CoPc-NH<sub>2</sub> on multiwalled carbon nanotubes increases the generation and local concentration of CO. This dual-site cascade catalyst exhibits substantially higher performance than the original single-site CoPc-NH<sub>2</sub>/carbon nanotube catalyst, reaching a partial current density of 150 mA cm<sup>−2</sup> and a Faradaic efficiency of 50% for methanol production. Kinetic analysis and in situ sum-frequency generation vibrational spectroscopy attribute this notable performance improvement to molecular-scale CO spillover from NiPc-OCH<sub>3</sub> sites to methanol-active CoPc-NH<sub>2</sub> sites.</p>

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Molecular-scale CO spillover on a dual-site electrocatalyst enhances methanol production from CO2 reduction

  • 期刊论文

  • 发表日期：

    2025年2月18日

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  • Jing Li,
  • Quansong Zhu,
  • Alvin Chang,
  • Seonjeong Cheon,
  • Yuanzuo Gao,
  • Bo Shang,
  • Huan Li,
  • Conor L. Rooney,
  • Longtao Ren,
  • Zhan Jiang,
  • Yongye Liang,
  • Zhenxing Feng,
  • Shize Yang,
  • L. Robert Baker,
  • Hailiang Wang

摘要

Cobalt phthalocyanine (CoPc) is recognized for catalysing electrochemical CO2 reduction into methanol at high Faradaic efficiency but is subject to deactivation. Cobalt tetraaminophthalocyanine (CoPc-NH2) shows improved stability, but its methanol Faradaic efficiency is below 30%. This study addresses these limitations in selectivity, reactivity and stability by rationally designing a dual-site cascade catalyst. Here we quantify the local concentration of CO, a key intermediate of the reaction, near a working CoPc-NH2 catalyst and show that co-loading nickel tetramethoxyphthalocyanine (NiPc-OCH3) with CoPc-NH2 on multiwalled carbon nanotubes increases the generation and local concentration of CO. This dual-site cascade catalyst exhibits substantially higher performance than the original single-site CoPc-NH2/carbon nanotube catalyst, reaching a partial current density of 150 mA cm−2 and a Faradaic efficiency of 50% for methanol production. Kinetic analysis and in situ sum-frequency generation vibrational spectroscopy attribute this notable performance improvement to molecular-scale CO spillover from NiPc-OCH3 sites to methanol-active CoPc-NH2 sites.