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Tailoring Selectivity of Electrochemical Hydrogen Peroxide Generation by Tunable Pyrrolic‐Nitrogen‐Carbon

Tailoring Selectivity of Electrochemical Hydrogen Peroxide Generation by Tunable... The electrochemical reduction of O2 via a two‐electron reaction pathway to H2O2 provides a possibility for replacing the current anthraquinone process, enabling sustainable and decentralized H2O2 production. Here, a nitrogen‐rich few‐layered graphene (N‐FLG) with a tunable nitrogen configuration is developed for electrochemical H2O2 generation. A positive correlation between the content of pyrrolic‐N and the H2O2 selectivity is experimentally observed. The critical role of pyrrolic‐N is elucidated by the variable intermediate adsorption profiles as well as the dependent negative shifts of the pyrrolic‐N peak on X‐ray adsorption near edge structure spectra. By virtue of the optimized N doping configuration and the unique porous structure, the as‐fabricated N‐FLG electrocatalyst exhibits high selectivity toward electrochemical H2O2 synthesis as well as superior long‐term stability. To achieve high‐value products on both the anode and cathode with optimized energy efficiency, a practical device coupling electrochemical H2O2 generation and furfural oxidation is assembled, simultaneously enabling a high yield rate of H2O2 at the cathode (9.66 mol h−1 gcat−1) and 2‐furoic acid at the anode (2.076 mol m−2 h−1) under a small cell voltage of 1.8 V. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Advanced Energy Materials Wiley

Tailoring Selectivity of Electrochemical Hydrogen Peroxide Generation by Tunable Pyrrolic‐Nitrogen‐Carbon

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Publisher
Wiley
Copyright
© 2020 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim
ISSN
1614-6832
eISSN
1614-6840
DOI
10.1002/aenm.202000789
Publisher site
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Abstract

The electrochemical reduction of O2 via a two‐electron reaction pathway to H2O2 provides a possibility for replacing the current anthraquinone process, enabling sustainable and decentralized H2O2 production. Here, a nitrogen‐rich few‐layered graphene (N‐FLG) with a tunable nitrogen configuration is developed for electrochemical H2O2 generation. A positive correlation between the content of pyrrolic‐N and the H2O2 selectivity is experimentally observed. The critical role of pyrrolic‐N is elucidated by the variable intermediate adsorption profiles as well as the dependent negative shifts of the pyrrolic‐N peak on X‐ray adsorption near edge structure spectra. By virtue of the optimized N doping configuration and the unique porous structure, the as‐fabricated N‐FLG electrocatalyst exhibits high selectivity toward electrochemical H2O2 synthesis as well as superior long‐term stability. To achieve high‐value products on both the anode and cathode with optimized energy efficiency, a practical device coupling electrochemical H2O2 generation and furfural oxidation is assembled, simultaneously enabling a high yield rate of H2O2 at the cathode (9.66 mol h−1 gcat−1) and 2‐furoic acid at the anode (2.076 mol m−2 h−1) under a small cell voltage of 1.8 V.

Journal

Advanced Energy Materials – Wiley

Published: Jun 1, 2020

Keywords: ; ; ;

References