Unveiling spin magnetic effect of TM doped SnS2 nanosheet with enhanced hydrogen evolution reaction

Abstract

Photoelectrochemical hydrogen evolution reaction (HER) is taken into account as an alternative to effective hydrogen production, emphasizing the importance of catalysts. The magnetism of catalysts could modulate the adsorption of the H atom and further enhance the HER activity. Herein, doping the double transition metal atoms on SnS2 nanosheet (TM2@SnS2) to form the efficient magnetic catalyst is proposed to explore the spin magnetic effect on the HER performance. By performing first-principles calculations, nonmagnetic V2@SnS2 is proved to be the candidate of the HER catalyst; nevertheless, the HER activities of antiferromagnetic and ferromagnetic V2@SnS2 are relatively inferior due to the spin-induced charge redistribution. Meanwhile, machine learning analysis shows the absolute importance of the electronic structure of TM dopants and surrounding S ligands, and the HER activity could be predicted by the modified band centers of S-3pz and TM-d. Furthermore, the proof-of-concept experiment has substantiated the above theoretical predictions by significantly increasing photocurrent with applied magnetic field. This work provides a new avenue for uncovering the spin catalytic mechanism and the exploration and design of efficient HER catalysts.