Machine Learning Derived Blueprint for Rational Design of the Effective Single-Atom Cathode Catalyst of the Lithium–Sulfur Battery

The "shuttle effect" and sluggish kinetics at cathode significantly hinder the further improvements of the lithium-sulfur (Li-S) battery, a candidate of next generation energy storage technology. Herein, machine learning based on high-throughput density functional theory calculations is employed to establish the pattern of polysulfides adsorption and screen the supported single-atom catalyst (SAC). The adsorptions are classified as two categories which successfully distinguish S-S bond breaking from the others. Moreover, a general trend of polysulfides adsorption was established regarding of both kind of metal and the nitrogen configurations on support. The regression model has a mean absolute error of 0.14 eV which exhibited a faithful predictive ability. Based on adsorption energy of soluble polysulfides and overpotential, the most promising SAC was proposed, and a volcano curve was found. In the end, a reactivity map is supplied to guide SAC design of the Li-S battery.