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

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...

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Veröffentlicht in:Advanced energy materials 2020-06, Vol.10 (21), p.n/a
Hauptverfasser: Li, Laiquan, Tang, Cheng, Zheng, Yao, Xia, Bingquan, Zhou, Xianlong, Xu, Haolan, Qiao, Shi‐Zhang
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container_issue 21
container_start_page
container_title Advanced energy materials
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creator Li, Laiquan
Tang, Cheng
Zheng, Yao
Xia, Bingquan
Zhou, Xianlong
Xu, Haolan
Qiao, Shi‐Zhang
description 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. A nitrogen‐rich few‐layered graphene material is designed for electrochemical H2O2 generation. A positive relationship between the H2O2 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 H2O2 generation with furfural oxidation is fabricated to simulate the practical application of the obtained electrocatalyst.
doi_str_mv 10.1002/aenm.202000789
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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. A nitrogen‐rich few‐layered graphene material is designed for electrochemical H2O2 generation. A positive relationship between the H2O2 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 H2O2 generation with furfural oxidation is fabricated to simulate the practical application of the obtained electrocatalyst.</description><identifier>ISSN: 1614-6832</identifier><identifier>EISSN: 1614-6840</identifier><identifier>DOI: 10.1002/aenm.202000789</identifier><language>eng</language><publisher>Weinheim: Wiley Subscription Services, Inc</publisher><subject>Adsorption ; Anodes ; Anthraquinones ; Cathodes ; Chemical reduction ; Configurations ; electrochemical H 2O 2 generation ; Furfural ; furfural oxidation ; Furoic acid ; Graphene ; Hydrogen peroxide ; Nitrogen ; nitrogen doped graphene ; Oxidation ; oxygen reduction reaction ; Selectivity</subject><ispartof>Advanced energy materials, 2020-06, Vol.10 (21), p.n/a</ispartof><rights>2020 WILEY‐VCH Verlag GmbH &amp; Co. 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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. A nitrogen‐rich few‐layered graphene material is designed for electrochemical H2O2 generation. A positive relationship between the H2O2 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 H2O2 generation with furfural oxidation is fabricated to simulate the practical application of the obtained electrocatalyst.</description><subject>Adsorption</subject><subject>Anodes</subject><subject>Anthraquinones</subject><subject>Cathodes</subject><subject>Chemical reduction</subject><subject>Configurations</subject><subject>electrochemical H 2O 2 generation</subject><subject>Furfural</subject><subject>furfural oxidation</subject><subject>Furoic acid</subject><subject>Graphene</subject><subject>Hydrogen peroxide</subject><subject>Nitrogen</subject><subject>nitrogen doped graphene</subject><subject>Oxidation</subject><subject>oxygen reduction reaction</subject><subject>Selectivity</subject><issn>1614-6832</issn><issn>1614-6840</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNqFkLFOwzAQhiMEElXpymyJOeViGyceq6q0SKVUosyW41yKqyQuTgpk4xF4Rp6ElKIyMt1_0vfdSX8QXEYwjADotcaqHFKgABAn8iToRSLioUg4nB4zo-fBoK43HQNcRsBYLyhX2hbO22pNHrFA09hX27TE5WSy37wzz1haowsyazPv1liRJXr3bjMkU6zQ68a6iqQtWe0qnRZIlq33rrDm6-NzYZsfpYtj7VNXXQRnuS5qHPzOfvB0O1mNZ-H8YXo3Hs1DwwXIkFGBQDFBkRnBaZ4xE-dGxCYCYSRIbkQep1HOJWOZ0B0rkkSkN0kqtGCJZv3g6nB3693LDutGbdzOV91LRTkkPJYMZEcND5Txrq495mrrbal9qyJQ-1bVvlV1bLUT5EF4swW2_9BqNFnc_7nfKSZ-xQ</recordid><startdate>20200601</startdate><enddate>20200601</enddate><creator>Li, Laiquan</creator><creator>Tang, Cheng</creator><creator>Zheng, Yao</creator><creator>Xia, Bingquan</creator><creator>Zhou, Xianlong</creator><creator>Xu, Haolan</creator><creator>Qiao, Shi‐Zhang</creator><general>Wiley Subscription Services, Inc</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SP</scope><scope>7TB</scope><scope>8FD</scope><scope>F28</scope><scope>FR3</scope><scope>H8D</scope><scope>L7M</scope><orcidid>https://orcid.org/0000-0002-4568-8422</orcidid></search><sort><creationdate>20200601</creationdate><title>Tailoring Selectivity of Electrochemical Hydrogen Peroxide Generation by Tunable Pyrrolic‐Nitrogen‐Carbon</title><author>Li, Laiquan ; Tang, Cheng ; Zheng, Yao ; Xia, Bingquan ; Zhou, Xianlong ; Xu, Haolan ; Qiao, Shi‐Zhang</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c4609-326e02e8e6dc642fd3c7fc67c106c9094c6f7b1f4933d6ae026886b58b6a638a3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>Adsorption</topic><topic>Anodes</topic><topic>Anthraquinones</topic><topic>Cathodes</topic><topic>Chemical reduction</topic><topic>Configurations</topic><topic>electrochemical H 2O 2 generation</topic><topic>Furfural</topic><topic>furfural oxidation</topic><topic>Furoic acid</topic><topic>Graphene</topic><topic>Hydrogen peroxide</topic><topic>Nitrogen</topic><topic>nitrogen doped graphene</topic><topic>Oxidation</topic><topic>oxygen reduction reaction</topic><topic>Selectivity</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Li, Laiquan</creatorcontrib><creatorcontrib>Tang, Cheng</creatorcontrib><creatorcontrib>Zheng, Yao</creatorcontrib><creatorcontrib>Xia, Bingquan</creatorcontrib><creatorcontrib>Zhou, Xianlong</creatorcontrib><creatorcontrib>Xu, Haolan</creatorcontrib><creatorcontrib>Qiao, Shi‐Zhang</creatorcontrib><collection>CrossRef</collection><collection>Electronics &amp; Communications Abstracts</collection><collection>Mechanical &amp; Transportation Engineering Abstracts</collection><collection>Technology Research Database</collection><collection>ANTE: Abstracts in New Technology &amp; Engineering</collection><collection>Engineering Research Database</collection><collection>Aerospace Database</collection><collection>Advanced Technologies Database with Aerospace</collection><jtitle>Advanced energy materials</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Li, Laiquan</au><au>Tang, Cheng</au><au>Zheng, Yao</au><au>Xia, Bingquan</au><au>Zhou, Xianlong</au><au>Xu, Haolan</au><au>Qiao, Shi‐Zhang</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Tailoring Selectivity of Electrochemical Hydrogen Peroxide Generation by Tunable Pyrrolic‐Nitrogen‐Carbon</atitle><jtitle>Advanced energy materials</jtitle><date>2020-06-01</date><risdate>2020</risdate><volume>10</volume><issue>21</issue><epage>n/a</epage><issn>1614-6832</issn><eissn>1614-6840</eissn><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. 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subjects Adsorption
Anodes
Anthraquinones
Cathodes
Chemical reduction
Configurations
electrochemical H 2O 2 generation
Furfural
furfural oxidation
Furoic acid
Graphene
Hydrogen peroxide
Nitrogen
nitrogen doped graphene
Oxidation
oxygen reduction reaction
Selectivity
title Tailoring Selectivity of Electrochemical Hydrogen Peroxide Generation by Tunable Pyrrolic‐Nitrogen‐Carbon
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