N-B-OH Site-Activated Graphene Quantum Dots for Boosting Electrochemical Hydrogen Peroxide Production

Mengmeng Fan; Zeming Wang; Kang SunAo WangYuying ZhaoQixin YuanRuibin WangJithu RajJingjie WuJianchun JiangLiang Wang

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N-B-OH Site-Activated Graphene Quantum Dots for Boosting Electrochemical Hydrogen Peroxide Production

机译：N-B-OH Site-Activated Graphene Quantum Dots for Boosting Electrochemical Hydrogen Peroxide Production

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Carbon materials are considered promising 2/4 e~? oxygen reduction reaction(ORR) electrocatalysts for synthesizing H_2O_2/H_2O via regulating heteroatomdopants and functionalization. Here, various doped and functionalized graphenequantum dots (GQDs) are designed to reveal the crucial active sites ofcarbon materials for ORR to produce H_2O2. Density functional theory (DFT)calculations predict that the edge structure involving edge N, B dopant pairsand further OH functionalization to the B (N-B-OH) is an active center for2e~? ORR. To verify the above predication, GQDs with an enriched density ofN-B-OH (NBO-GQDs) are designed and synthesized by the hydrothermalreaction of -NH_2 edge-functionalized GQDs with H3BO3 forming sixmemberheterocycle containing the N-B-OH structure. When dispersed onconductive carbon substrates, the NBO-GQDs show H_2O_2 selectivity of over90% at 0.7 –0.8 V versus reversible hydrogen electrode in the alkaline solutionin a rotating ring-disk electrode setup. The selectivity retains 90% of theinitial value after 12 h stability test. In a flow cell setup, the H_2O_2 productionrate is up to 709 mmol gcatalyst~(?1) h~(?1), superior to most reported carbon- andmetal-based electrocatalysts. This work provides molecular insight into thedesign and formulation of highly efficient carbon-based catalysts for sustainableH_2O_2 production.

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来源
《Advanced Materials》 |2023年第17期|2209086.1-2209086.11|共11页
作者
Mengmeng Fan; Zeming Wang; Kang SunAo WangYuying ZhaoQixin YuanRuibin WangJithu RajJingjie WuJianchun JiangLiang Wang;
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作者单位

Key Lab of Biomass Energy and MaterialJiangsu ProvinceJiangsu Co-Innovation Center of Efficient Processing and Utilizationof Forest ResourcesInstitute of Chemical Industry of Forest ProductsChinese Academy of ForestryNanjing 210042, China;

Jiangsu Co-Innovation Center of Efficient Processing and Utilizationof Forest ResourcesInternational Innovation Center for Forest Chemicals and MaterialsCollege of Chemical EngineeringNanjing Forestry UniversityNanjing 210037, China;

Department of Chemical and Environmental EngineeringUniversity of CincinnatiCincinnati, OH 45221, USAJiangsu Co-Innovation Center of Efficient Processing and Utilizationof Forest ResourcesInternational Innovation Center for Forest Chemicals and MaterialsCollege of Chemical EngineeringNanjing Forestry UniversityNanjing 210037, China,Key Lab of Biomass EneInstitute of Nanochemistry and NanobiologySchool of Environmental and Chemical EngineeringShanghai UniversityShanghai 200444, China;

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正文语种英语
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2 e~? electrocatalysis; graphene quantum dots; hydrogen peroxide synthesis; N-B-OH sites; oxygen reduction reaction;

N-B-OH Site-Activated Graphene Quantum Dots for Boosting Electrochemical Hydrogen Peroxide Production

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