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Electrocatalytic Hydrogen Evolution Using Cyano-Substituted Triaryl Corrole Antimony(III) Complexes
Yuan-Yuan Wang1, Ting-Long Wu1, De-Yu Guo1
1Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, China.
Researchers developed new antimony(III) corrole complexes for efficient hydrogen evolution reaction (HER) catalysis. Adding cyano groups enhanced catalytic activity, offering a pathway for designing improved HER electrocatalysts.
Area of Science:
- Inorganic Chemistry
- Materials Science
- Electrochemistry
Background:
- Developing efficient molecular electrocatalysts for the hydrogen evolution reaction (HER) is crucial for catalysis.
- Controllable and predictable properties of catalysts remain a significant challenge.
Purpose of the Study:
- To synthesize and investigate the effect of electron-withdrawing cyano substituents on Sb(III) corrole complexes for HER catalysis.
- To explore structure-activity relationships for designing enhanced Sb(III) corrole-based HER catalysts.
Main Methods:
- Synthesis and characterization of four Sb(III) corrole complexes using UV-vis, NMR, HRMS, and XPS.
- Electrocatalytic HER performance evaluation in organic and mixed aqueous-organic media.
- Density Functional Theory (DFT) calculations to rationalize experimental observations.
Main Results:
- Sb(III) corrole complexes with increasing numbers of cyano groups showed enhanced HER activity.
- Complex 4, with three cyano groups, exhibited the highest activity (TOF of 42.19 s⁻¹ at 895 mV overpotential) and 85.5% Faradaic efficiency.
- DFT calculations indicated ligand-centered reduction and supported an ECEC pathway for HER.
Conclusions:
- Cyano functionalization effectively modulates the electronic properties of Sb(III) corroles, enhancing their HER performance.
- The study provides insights into designing efficient Sb(III) corrole-based electrocatalysts for hydrogen production.
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