Electronic reconfiguration induced by anchoring orbital interaction onto asymmetric FeIn2S4 surface for hydrogen evolution reaction

Abstract

The catalytic activity is strongly related with the anchoring reactive sites on the catalyst surface, because the electronic occupation at these anchored metal sites can be changed by their orbital interaction. Herein, the FeIn2S4 monolayer can demonstrate two asymmetric surfaces that can be decorated by anchoring Fe atoms, which makes some valence electrons transfer to the pristine surfaces and leads to an electronic reconfiguration for anchored Fe atoms. First-principles calculations disclose that additional Fe atoms more prefer to anchor at a particular site of FeIn2S4 surface and more 3d electrons can be localized at this anchored Fe atom. More interestingly, the hydrogen evolution reaction can be effectively enhanced by this intriguing electronic reconfiguration, especially for the In–S terminated surface. This work provides a new insight into designing new-type catalysts by anchoring special atoms with catalytic activity.