High-temperature treatment to engineer the single-atom Pt coordination environment towards highly efficient hydrogen evolution

Abstract

The coordination environment of Pt is regulated through appropriate high-temperature treatment to further improve the HER performance of the single-atom Pt-catalyst. • High-t emperature induces new coordination environment for Pt single atom catalyst. • The obtained Pt 0.8 @CN-1000 shows superior HER performances to the pristine Pt 0.8 @CN. • The optimized Pt electronic state accounts for the enhanced HER performances. Development of high-performance and cost-effective catalysts for electrocatalytic hydrogen evolution reaction (HER) play crucial role in the growing hydrogen economy. Recently, the atomically dispersed metal catalysts have attracted increasing attention due to their ultimate atom utilization and great potential for highly cost-effective and high-efficiency HER electrocatalyst. Herein, we propose a high-temperature treatment strategy to furtherly improve the HER performance of atomically dispersed Pt-based catalyst. Interestingly, after appropriate high-temperature treatment on the atomically dispersed Pt 0.8 @CN, the Pt species on the designed N-doped porous carbon substrate with rich defect sites can be re-dispersed to single atom state with new coordination environment. The obtained Pt 0.8 @CN-1000 shows superior HER performance with overpotential of 13 mV at 10 mA cm −2 and mass activity of 11,284 mA/mg Pt at −0.1 V, much higher than that of the pristine Pt 0.8 @CN and commercial Pt/C catalyst. The experimental and theoretical investigations indicate that the high-temperature treatment induces the restructuring of coordination environment and then the optimized Pt electronic state leads to the enhanced HER performances. This work affords new strategy and insights to develop the atomically dispersed high-efficiency catalysts.