Elucidation and modulation of active sites in holey graphene electrocatalysts for H2O2 production
Abstract Selective electrochemical oxygen reduction (ORR) toward a two‐electron (2e−) pathway is an eco‐friendly alternative method for H2O2 synthesis to replace the energy‐intensive anthraquinone oxidation process. Carbon‐based electrocatalysts (CBEs) show great potential for practical H2O2 synthes...
| Main Authors: | , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley
2023-01-01
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| Series: | EcoMat |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/eom2.12266 |
| _version_ | 1828114975677218816 |
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| author | Ki Hwan Koh Amir Hassan Bagherzadeh Mostaghimi Qiaowan Chang Yu Joong Kim Samira Siahrostami Tae Hee Han Zheng Chen |
| author_facet | Ki Hwan Koh Amir Hassan Bagherzadeh Mostaghimi Qiaowan Chang Yu Joong Kim Samira Siahrostami Tae Hee Han Zheng Chen |
| author_sort | Ki Hwan Koh |
| collection | DOAJ |
| description | Abstract Selective electrochemical oxygen reduction (ORR) toward a two‐electron (2e−) pathway is an eco‐friendly alternative method for H2O2 synthesis to replace the energy‐intensive anthraquinone oxidation process. Carbon‐based electrocatalysts (CBEs) show great potential for practical H2O2 synthesis. However, their complex structures make it challenging to determine the nature of active sites and to precisely control them. Herein, we show that precise modulation of the chemistry and structures of holey graphene with edge sites enriched by oxygen‐containing functional groups can facilitate 2e− ORR. These combined functionalities could improve ORR performance under various pH conditions, for example, resulting in an average of 95% H2O2 selectivity, ~97% Faraday efficiency, high productivity of 2360 mol kgcat−1 h−1 in alkaline media. Density functional theory calculations on the oxygen functional groups at the edge sites revealed the most active site for 2e− ORR is a synergy between ether (COC) and carbonyl (CO) functional groups with nearly zero overpotential. |
| first_indexed | 2024-04-11T12:33:39Z |
| format | Article |
| id | doaj.art-9f48510ea19e4f9bbe2d6b3bc37dc393 |
| institution | Directory Open Access Journal |
| issn | 2567-3173 |
| language | English |
| last_indexed | 2024-04-11T12:33:39Z |
| publishDate | 2023-01-01 |
| publisher | Wiley |
| record_format | Article |
| series | EcoMat |
| spelling | doaj.art-9f48510ea19e4f9bbe2d6b3bc37dc3932022-12-22T04:23:42ZengWileyEcoMat2567-31732023-01-0151n/an/a10.1002/eom2.12266Elucidation and modulation of active sites in holey graphene electrocatalysts for H2O2 productionKi Hwan Koh0Amir Hassan Bagherzadeh Mostaghimi1Qiaowan Chang2Yu Joong Kim3Samira Siahrostami4Tae Hee Han5Zheng Chen6Department of Nano Engineering University of California San Diego San Diego California USADepartment of Chemistry University of Calgary Calgary Alberta CanadaDepartment of Nano Engineering University of California San Diego San Diego California USADepartment of Organic and Nano Engineering, Human‐Tech Convergence Program Hanyang University Seoul Republic of KoreaDepartment of Chemistry University of Calgary Calgary Alberta CanadaDepartment of Organic and Nano Engineering, Human‐Tech Convergence Program Hanyang University Seoul Republic of KoreaDepartment of Nano Engineering University of California San Diego San Diego California USAAbstract Selective electrochemical oxygen reduction (ORR) toward a two‐electron (2e−) pathway is an eco‐friendly alternative method for H2O2 synthesis to replace the energy‐intensive anthraquinone oxidation process. Carbon‐based electrocatalysts (CBEs) show great potential for practical H2O2 synthesis. However, their complex structures make it challenging to determine the nature of active sites and to precisely control them. Herein, we show that precise modulation of the chemistry and structures of holey graphene with edge sites enriched by oxygen‐containing functional groups can facilitate 2e− ORR. These combined functionalities could improve ORR performance under various pH conditions, for example, resulting in an average of 95% H2O2 selectivity, ~97% Faraday efficiency, high productivity of 2360 mol kgcat−1 h−1 in alkaline media. Density functional theory calculations on the oxygen functional groups at the edge sites revealed the most active site for 2e− ORR is a synergy between ether (COC) and carbonyl (CO) functional groups with nearly zero overpotential.https://doi.org/10.1002/eom2.12266electrocatalystgraphenehydrogen peroxideoxygen reduction reaction |
| spellingShingle | Ki Hwan Koh Amir Hassan Bagherzadeh Mostaghimi Qiaowan Chang Yu Joong Kim Samira Siahrostami Tae Hee Han Zheng Chen Elucidation and modulation of active sites in holey graphene electrocatalysts for H2O2 production EcoMat electrocatalyst graphene hydrogen peroxide oxygen reduction reaction |
| title | Elucidation and modulation of active sites in holey graphene electrocatalysts for H2O2 production |
| title_full | Elucidation and modulation of active sites in holey graphene electrocatalysts for H2O2 production |
| title_fullStr | Elucidation and modulation of active sites in holey graphene electrocatalysts for H2O2 production |
| title_full_unstemmed | Elucidation and modulation of active sites in holey graphene electrocatalysts for H2O2 production |
| title_short | Elucidation and modulation of active sites in holey graphene electrocatalysts for H2O2 production |
| title_sort | elucidation and modulation of active sites in holey graphene electrocatalysts for h2o2 production |
| topic | electrocatalyst graphene hydrogen peroxide oxygen reduction reaction |
| url | https://doi.org/10.1002/eom2.12266 |
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