<p>A central task in clean energy conversion involves designing highly efficient electrocatalysts based on non-precious metals for the hydrogen evolution reaction (HER). In this study, three dimeric metal (M = Co (<b>1</b>), Cu (<b>2</b>), Ga (<b>3</b>)) imidazole-functionalized corrole complexes were prepared as electrocatalysts for HER in organic and aqueous media. All three complexes displayed the appreciable HER catalytic activity, among which BPFIC-2Co (<b>1</b>) exhibited the best performance. When TFA or TsOH was used as the proton source, catalytic efficiency (C.E.) and turnover frequency (TOF) followed the sequence <b>1</b> &gt; <b>2</b> &gt; <b>3</b>. Furthermore, the HER processes of complexes <b>1–3</b> likely followed EECC, EECC, and ECEC pathways (E: electron transfer, C: proton coupling), respectively. In neutral aqueous media, complexes <b>1–3</b> achieved HER TOFs of 166.01, 125.60, and 109.12&#xa0;h<sup>−1</sup>. Under controlled-potential electrolysis at − 2.15&#xa0;V, complexes <b>1–3</b> all displayed H<sub>2</sub> Faradaic efficiencies above 80%. Moreover, all catalysts demonstrated excellent stability throughout the electrolysis in both organic and aqueous phase.</p> Graphical Abstract <p></p>

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Electrocatalytic Hydrogen Evolution by Dimeric Metal (M = Co, Cu, Ga) Imidazole-Functionalized Corrole Complexes

  • Hai-Xin Xu,
  • De-Yu Guo,
  • Feng Li,
  • Lei Shi,
  • Hao Zhang,
  • Li-Ping Si,
  • Xin-Yan Xiao,
  • Hai-Yang Liu

摘要

A central task in clean energy conversion involves designing highly efficient electrocatalysts based on non-precious metals for the hydrogen evolution reaction (HER). In this study, three dimeric metal (M = Co (1), Cu (2), Ga (3)) imidazole-functionalized corrole complexes were prepared as electrocatalysts for HER in organic and aqueous media. All three complexes displayed the appreciable HER catalytic activity, among which BPFIC-2Co (1) exhibited the best performance. When TFA or TsOH was used as the proton source, catalytic efficiency (C.E.) and turnover frequency (TOF) followed the sequence 1 > 2 > 3. Furthermore, the HER processes of complexes 1–3 likely followed EECC, EECC, and ECEC pathways (E: electron transfer, C: proton coupling), respectively. In neutral aqueous media, complexes 1–3 achieved HER TOFs of 166.01, 125.60, and 109.12 h−1. Under controlled-potential electrolysis at − 2.15 V, complexes 1–3 all displayed H2 Faradaic efficiencies above 80%. Moreover, all catalysts demonstrated excellent stability throughout the electrolysis in both organic and aqueous phase.

Graphical Abstract