Electrocatalytic Hydrogen Evolution Using Cyano-Substituted Triaryl Corrole Antimony(III) Complexes
Yuan-Yuan Wang, Ting-Long Wu, De-Yu Guo, Hao Zhang, Yan-Mei Sun, Li-Ping Si, Hai-Yang Liu
TL;DR
Scientists developed new antimony-based catalysts with cyano groups that improve hydrogen production efficiency through electrocatalysis.
Contribution
New Sb(III) corrole complexes with cyano groups are shown to enhance hydrogen evolution reaction performance through electronic modulation.
Findings
Complex 4 achieved a turnover frequency of 42.19 s−1 at 895 mV overpotential in DMF.
Faradaic efficiency of 85.5% was observed for complex 4 in mixed aqueous-organic media.
Cyano groups increase HER activity by modulating electronic properties, supported by DFT calculations.
Abstract
Developing molecular electrocatalysts with controllable and predictable properties remains a central challenge in hydrogen evolution reaction (HER) catalysis. Herein, four Sb(III) corrole complexes (1–4) bearing zero to three p-cyano-substituted meso-phenyl groups (-CN Ph) were synthesized to investigate the effect of electron-withdrawing substituents on their catalytic HER performance, in which complexes 2–4 are newly reported. All prepared complexes were well characterized via UV–vis, NMR, HRMS, and XPS. SEM–EDS and UV–vis analyses indicated their uniform dispersion and excellent stability under organic and neutral aqueous solvent electrolysis conditions. When using TsOH as the proton source in DMF, complex 4 exhibited the highest activity with a TOF of 42.19 s−1 at an overpotential of 895 mV. In mixed aqueous–organic media, the Faradaic efficiency of complex 4 reached 85.5%. The HER…
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Taxonomy
TopicsMetalloenzymes and iron-sulfur proteins · Electrocatalysts for Energy Conversion · Porphyrin and Phthalocyanine Chemistry