Computational Screening of Transition Metal-Doped CdS for Photocatalytic Hydrogen Production.

Abstract A novel computational screening study of single transition metal (TM), TM-doped (TM@CdS), and dual TMs-doped (TM1-TM2@CdS) on CdS (110) surfaces via DFT calculations is presented, focusing on their stability and catalytic activity, searching for efficient photocatalysts for hydrogen production. Criteria based on key performance descriptors allowed to fine-tune the selection. Results indicate that TM dopants can reduce the energy band gap and enhance impurity d-states. Pt, Rh and Pd were found to be the best dopant in TM@CdS, since their |ΔGH| is 80% smaller compared to the pristine CdS surface. Moreover, TM1-TM2@CdS catalysts show better performance than TM@CdS for the hydrogen evolution reaction (HER) due to synergistic effects of the two TM, where Co-Pt, Pd-Pt and Co-Rh@CdS significantly reduced |ΔGH| to less than 0.1 eV. Results point out four promising novel catalysts (i.e., Co@CdS, Co-Pt@CdS, Co-Rh@CdS, Rh-Ag@CdS) with very good performance in HER, to be further explored in experimental studies.