Tailoring Selectivity of Electrochemical Hydrogen Peroxide Generation by Tunable Pyrrolic‐Nitrogen‐Carbon. Issue 21 (17th April 2020)

• Record Type: Journal Article
• Authors: Li, Laiquan; Tang, Cheng; Zheng, Yao; Xia, Bingquan; Zhou, Xianlong; Xu, Haolan; Qiao, Shi‐Zhang
• Is Part Of: Advanced energy materials. Volume 10:Issue 21(2020)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2020-04-17
• Subjects: electrochemical H 2O 2 generation -- furfural oxidation -- nitrogen doped graphene -- oxygen reduction reaction; Energy harvesting -- Materials -- Periodicals; Energy conversion -- Materials -- Periodicals; Energy storage -- Materials -- Periodicals; Photovoltaics -- Periodicals; Fuel cells -- Periodicals; Thermoelectric materials -- Periodicals; 621.31
• DOI: 10.1002/aenm.202000789
• Languages: English
• ISSNs: 1614-6832

Abstract

Abstract: The electrochemical reduction of O2 via a two‐electron reaction pathway to H2 O2 provides a possibility for replacing the current anthraquinone process, enabling sustainable and decentralized H2 O2 production. Here, a nitrogen‐rich few‐layered graphene (N‐FLG) with a tunable nitrogen configuration is developed for electrochemical H2 O2 generation. A positive correlation between the content of pyrrolic‐N and the H2 O2 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 H2 O2 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 H2 O2 generation and furfural oxidation is assembled, simultaneously enabling a high yield rate of H2 O2 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. Abstract : A nitrogen‐rich few‐layered graphene material is designed for electrochemical H2 O2 generation. A positive relationship between the H2 O2 selectivity and the atomic content of pyrrolic‐N is observed, the mechanism is unraveled by X‐ray adsorption near edge structure (XANES) spectra. A device combining H2 O2 generation with furfural oxidation is fabricated to simulate the practical application of the obtained electrocatalyst.