Strain-promoted conductive metal-benzenhexathiolate frameworks for overall water splitting

Designing efficient catalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is a desirable strategy for overall water splitting and the generation of clean and renewable energies. Herein, the electrocatalytic HER and OER activity of the conductive metal-benzenhexathiolate (M-BHT) frameworks has been evaluated utilizing first-principles calculations. The in-plane π-d conjugation of M-BHT guarantees fast electron transfer during electrocatalytic reactions. Notably, Rh-BHT holds the promise of bifunctional HER/OER activity with the overpotentials of 0.07/0.36 V. Furthermore, the application of strain engineering tailors the adsorption of intermediates and promotes the overall water splitting performance. Rh-BHT with the +1% tensile strain shows the HER/OER overpotential of 0.02/0.37 V. This work not only demonstrates the prospects of conductive metal-organic frameworks in electrocatalysis but also offers new insights into designing efficient catalysts by strain engineering.