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Abstract:
Hydrogen peroxide (H2O2) electrosynthesis using metal-free carbon materials via the 2e(-) oxygen reduction pathway has sparked considerable research interest. However, the scalable preparation of carbon electrocatalysts to achieve satisfactory H2O2 yield in acidic media remains a grand challenge. Here, we present the design of a carbon nanoreactor series that integrates precise O/N codoping alongside well-regulated geometric structures targeting high-efficiency electrosynthesis of H2O2. Theoretical computations reveal that strategic N/O codoping facilitates partial electron transfer from C sites to O sites, realizing electronic rearrangement that optimizes C-site adsorption of *OOH. Concurrently, the O-O bond in *OOH is strengthened by charge transfer from antibonding to pi-orbitals, stabilizing the O-O bond and preventing its dissociation. The carbon nanoreactor with a hollow bowl geometry also facilitates the mass transport of O-2 and H2O2, achieving an H2O2 selectivity of 96% in acidic media. Furthermore, a flow cell integrated with the refined nanoreactor catalyst achieves an impressive H2O2 production rate of 2942.4 mg L-1 h(-1), coupled with stable operation of nearly 80 h, surpassing the state-of-the-art metal-free analogs. The feasibility of the electro-synthesized H2O2 is further demonstrated to be highly efficient in wastewater remediation.
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Source :
ENVIRONMENTAL SCIENCE & TECHNOLOGY
ISSN: 0013-936X
Year: 2024
Issue: 49
Volume: 58
Page: 21893-21903
1 1 . 4 0 0
JCR@2022
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ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
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30 Days PV: 14
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