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Published on: December 6, 2021
Mesoporous N,S-Dual-Doped Carbon Nanoreactors via Entropy-Driven Interface Self-Assembly for Efficient H2O2
Fei Liu1, Xiaoqing Liu2, Rui Zhang1,3
1College of Chemistry and Chemical Engineering, Inner Mongolia Key Laboratory of Rare Earth Catalysis, Inner Mongolia University, Hohhot, China.
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The electrochemical two-electron oxygen reduction reaction (2e- ORR) offers a sustainable route for H2O2 production. Rational catalyst design is essential for achieving efficient H2O2 electrosynthesis, in which porous heteroatom-doped carbon-based materials hold tremendous potential. Nevertheless, the simultaneous realization of homogenized heteroatom doping and a precisely engineered porous structure in the carbon skeleton remains a significant challenge. Herein, we propose an entropy-driven interface self-assembly strategy to fabricate mesoporous N,S-dual-doped carbon-based nanoreactors with tunable geometries. The optimal sample shows exceptional performance in a flow cell, achieving H2O2 production rate of 17.38 molgcat -1 h-1 at -0.2 V versus reversible hydrogen electrode (RHE) with > 90% selectivity. DFT calculations and finite element analysis simulations reveal that the N,S-dual-doping configuration optimizes the *OOH adsorption energy, while the well‑defined mesoporous structure accelerates mass transport and promotes the enrichment of surface O2 concentration. This work provides a general principle for synergizing heteroatom doping and nanostructural engineering toward high-performance electrocatalysts for sustainable synthesis.
