Journal
CARBON
Volume 163, Issue -, Pages 154-161Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.carbon.2020.02.084
Keywords
-
Funding
- National Natural Science Foundation of China [51738013, 51978371, 51722811]
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Electrocatalytic two-electron oxygen reduction reaction (2e(-) ORR) is a promising strategy to achieve hydrogen peroxide (H2O2) production, which can replace the anthraquinone method in industrial processes. Nitrogen-doped carbon materials are active and selective electrocatalysts for 2e(-) ORR; however, it remains challenging to develop N-doped carbons for practical H2O2 production and pinpoint the exact role of nitrogen functionalities. Here, we examine covalent organic framework-derived nitrogen-doped carbons with well-defined porous structure and tunable N species for electrocatalytic H2O2 production. Electrochemical studies show their highest ORR activity and H2O2 selectivity of up to 75% in alkaline electrolyte. Notably, chronoamperometric bulk electrolysis achieves an unprecedented carbon-catalyzed H2O2 yield rate of 1286.9 mmol g(catalyst)(-1) h(-1) and a faradaic efficiency of 69.8% at pH 13. X-ray photoelectron spectroscopy analysis combined with control experiments reveals that graphitic N is responsible for H2O2 production from 2e(- )ORR on N-doped carbons. Our work provides insights into the rational development of heteroatom-doped carbon electrocatalysts for efficient H2O2 generation. (C) 2020 Elsevier Ltd. All rights reserved.
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