Boosting intrinsic activity of electrocatalytic hydrogen peroxide production by tuning coordinative environment of monoatomic Pt site

Abstract

Single atom catalysts (SACs) was spotlighted due to their unique catalytic behavior and maximum atom efficiency especially in electrocatalysis. However, Fabricating the SACs with high metal contents have been considered to symbolic challenges because of insufficient metal-support interaction to prevent agglomeration of metal atoms. Herein, highly sulfur-doped zeolite templated carbon (HSC) with 17 wt% of S-contents was able to generate single atomic Pt site to fairly high metal contents of 10 wt% since sulfur ligands provide strong binding affinity to Pt. Electrocatalytic hydrogen peroxide production was performed for Pt/HSCs containing 1 to 10 wt%. The intrinsic catalytic activity of these catalysts was boosted by increasing Pt contents, maintaining high selectivity of hydrogen peroxide production >90%. In the insitu-XAFS analysis, oxidation state and Pt–S coordination number was increased along with increasing Pt loading and it is expected that electronic and geometric structure of active site affect to the intrinsic catalytic activity. the elucidation of effect of structure of single-atom active site on catalytic activity via operando tools will assist rational design of single atom catalyst.