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Integrated Two-in-one Strategy for Efficient Neutral Hydrogen Peroxide Electrosynthesis via Phosphorous Doping in 2D Mesoporous Carbon Carriers

delete2025-02-11
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DOI:10.1002/anie.202500177delete
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Abstract

Abstract

En 中文
Herein, we demonstrate a two-in-one strategy for efficient neutral electrosynthesis of H2O2 via two-electron oxygen reduction reaction (2e(-) ORR), achieved by synergistically fine-modulating both the local microenvironment and electronic structure of indium (In) single atom (SA) sites. Through a series of finite elemental simulations and experimental analysis, we highlight the significant impact of phosphorous (P) doping on an optimized 2D mesoporous carbon carrier, which fosters a favorable microenvironment by improving the mass transfer and O-2 enrichment, subsequently leading to an increased local pH levels. Consequently, an outstanding 2e(-) ORR performance is observed in neutral electrolytes, achieving over 95 % selectivity for H2O2 across a broad voltage range of 0.1 to 0.5 V vs RHE. In a flow cell, the production rate of H2O2 exceeds 22.54 mol g(cat)(-1) h(-1) while maintaining high stability at industrial-level current densities. These results are comparable to, if not better than, those achieved under alkaline conditions. Further analysis, both experimental and theoretical, indicates that the P dopant occupies the second coordination sphere of the In SA, which shows optimized OOH* binding strength for an enhanced 2e(-) ORR kinetic.
Keywords:
Heteroatoms
microenvironment
mesoporous nanosheets
neutral media
H2O2 production

Journal

Angewandte Chemie-International Edition cover
Angewandte Chemie-International Edition
IF:
16.9
Papers:
5.6W
Citations:
53.0W

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