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Abstract
Developing efficient electrocatalysts for acidic electrosynthesis of hydrogen peroxide (H2O2) holds considerable significance, while the selectivity and stability of most materials are compromised under acidic conditions. Herein, we demonstrate that constructing amorphous platinum–selenium (Pt–Se) shells on crystalline Pt cores can manipulate the oxygen reduction reaction (ORR) pathway to efficiently catalyze the electrosynthesis of H2O2 in acids. The Se2‒Pt nanoparticles, with optimized shell thickness, exhibit over 95% selectivity for H2O2 production, while suppressing its decomposition. In flow cell reactor, Se2‒Pt nanoparticles maintain current density of 250 mA cm−2 for 400 h, yielding a H2O2 concentration of 113.2 g L−1 with productivity of 4160.3 mmol gcat−1 h−1 for effective organic dye degradation. The constructed amorphous Pt–Se shell leads to desirable O2 adsorption mode for increased selectivity and induces strain for optimized OOH* binding, accelerating the reaction kinetics. This selenization approach is generalizable to other noble metals for tuning 2e‒ ORR pathway.
Developing efficient catalysts for acidic electrosynthesis of H2O2 is desirable, while most materials are compromised in acidic conditions. Here, the authors report that constructing amorphous Pt–Se shells on crystalline Pt cores can regulate the reaction pathway to efficiently produce H2O2 in acid.
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1 Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen, China (GRID:grid.12955.3a) (ISNI:0000 0001 2264 7233)
2 Ministry of Education, Key Laboratory of Material Chemistry for Energy Conversion and Storage, Wuhan, China (GRID:grid.419897.a) (ISNI:0000 0004 0369 313X); Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica, Wuhan, China (GRID:grid.419897.a); Huazhong University of Science and Technology, School of Chemistry and Chemical Engineering, Wuhan, China (GRID:grid.33199.31) (ISNI:0000 0004 0368 7223)
3 Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen, China (GRID:grid.510968.3)
4 Southwest University, School of Materials and Energy, Chongqing, China (GRID:grid.263906.8) (ISNI:0000 0001 0362 4044)
5 Max Planck Institute for Chemical Physics of Solids, Dresden, Germany (GRID:grid.419507.e) (ISNI:0000 0004 0491 351X)
6 National Synchrotron Radiation Research Center, Hsinchu, Taiwan (GRID:grid.410766.2) (ISNI:0000 0001 0749 1496)
7 Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen, China (GRID:grid.12955.3a) (ISNI:0000 0001 2264 7233); Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen, China (GRID:grid.510968.3)