Unveiling the critical role of active site interaction in single atom catalyst towards hydrogen evolution catalysis. (March 2022)

• Record Type: Journal Article
• Authors: Li, Feng; Han, Gao-Feng; Bu, Yunfei; Chen, Shanshan; Ahmad, Ishfaq; Jeong, Hu Young; Fu, Zhengping; Lu, Yalin; Baek, Jong-Beom
• Is Part Of: Nano energy. Volume 93(2022)
• Publication Date: 2022-03
• Subjects: Active site interaction -- Electronic configuration -- Acidic media -- Hydrogen evolution catalysis -- Density functional theory; Nanoscience -- Periodicals; Nanotechnology -- Periodicals; Nanostructured materials -- Periodicals; Power resources -- Technological innovations -- Periodicals; Nanoscience; Nanostructured materials; Nanotechnology; Power resources -- Technological innovations; Periodicals; 621.042
• DOI: 10.1016/j.nanoen.2021.106819
• Languages: English
• ISSNs: 2211-2855

Abstract

Abstract: Single atom catalysts (SACs) with efficient active sites are considered as valuable candidates to replace traditional catalysts. Fundamental insights into the interaction between single atom active sites, and its effect on the catalytic performance are still rare. Herein, we demonstrate the critical role of active site interaction in the intrinsic activity of SACs during acidic hydrogen evolution catalysis. Different amounts of platinum (Pt) atoms were atomically dispersed on graphitic carbon supports (PtSACs) to vary the spatial distance and thus the interaction between active sites. Remarkably, the PtSAC with improved active site interaction exhibited significantly enhanced intrinsic activity towards acidic hydrogen evolution (e.g., a high turnover frequency of 8.01 H2 s −1 at 20 mV), surpassing commercial Pt/C and other reported outstanding catalysts. Theoretical calculations further revealed that the increasing interaction between single atom active sites can largely modify their electronic configurations and result in more favored hydrogen adsorption/desorption behaviors, which is responsible for the enhanced intrinsic activity towards hydrogen evolution catalysis. Graphical Abstract: ga1 Highlights: Demonstrated the active site interaction plays a critical role in the intrinsic activity towards hydrogen evolution. Achieved significantly enhanced catalytic performance towards hydrogen evolution. Provided a fundamental insight into how active site interaction contributes to high intrinsic activity.