Strain engineering in single-atom catalysts: GaPS 4 for bifunctional oxygen reduction and evolution

• Published in: Inorganic chemistry frontiers Vol. 9; no. 16; pp. 4272 - 4280
• Main Authors: Liu, Xuefei, Liu, Tianyun, Xiao, Wenjun, Wang, Wentao, Zhang, Yuefei, Wang, Gang, Luo, Zijiang, Liu, Jin-Cheng
• Format: Journal Article
• Language: English
• Published: 09.08.2022
• ISSN: 2052-1553; 2052-1553
• DOI: 10.1039/D2QI01047J

We report here a theoretical study on 34 transition metal doped two-dimensional GaPS 4 catalysts, denoted as transition metal transition metal@V S -GaPS 4 . Among them, the Pt@V S1 -GaPS 4 single-atom catalyst is found to be stable with an ORR/OER overpotential of 0.59/0.41 V. Under the guidance of a volcano map, further biaxial strain engineering is adopted to tune the activity of Pt@V S1 -GaPS 4 to the top of the volcano. The overpotentials of the OER/ORR are decreased to 0.37/0.33 V by applying a 3% tensile strain. Our results prove that Pt@V S1 -GaPS 4 is an excellent candidate for OER/ORR bifunctional electrocatalysis. Moreover, bond angles and the highest occupied orbitals of the doped transition metal atoms can be used as descriptors to explain the underlying strain tunability mechanism. The machine learning method further predicts that the number of d electrons, the bond length and electronegativity are three main descriptors to determine the catalytic activity.