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Structure-controlled graphene electrocatalysts for high-performance H_2O_2 production

机译:Structure-controlled graphene electrocatalysts for high-performance H_2O_2 production

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摘要

Metal-free carbon materials have emerged as cost-effective and high-performance catalysts for the production of hydrogen peroxide (H2O2) through the two-electron oxygen reduction reaction (ORR). Here, we show that 3D crumpled graphene with controlled oxygen and defect configurations significantly improves the electrocatalytic production of H2O2. The crumpled graphene electrocatalyst with optimal defect structures and oxygen functional groups exhibits outstanding H2O2 selectivity of 92-100% in a wide potential window of 0.05-0.7 V vs. reversible hydrogen electrode (RHE) and a high mass activity of 158 A g(-1) at 0.65 V vs. RHE in alkaline media. In addition, the crumpled graphene catalyst showed an excellent H2O2 production rate of 473.9 mmol gcat(-1) h(-1) and stability over 46 h at 0.4 V vs. RHE. Moreover, density functional theory calculations revealed the role of the functional groups and defect sites in the two-electron ORR pathway through the scaling relation between OOH and O adsorption strengths. These results establish a structure-mechanism-performance relationship of functionalized carbon catalysts for the effective production of H2O2.

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  • 来源
    《Energy & environmental science: EES》 |2022年第7期|2858-2866|共9页
  • 作者单位

    Georgia Inst Technol, George W Woodruff Sch Mech Engn, Atlanta, GA 30332 USA;

    Korea Inst Sci & Technol KIST, Ctr Hydrogen Fuel Cell Res, Hwarang Ro 14 Gil 5, Seoul 02792, South Korea;

    Inha Univ, Dept Mech Engn, 100 Inha Ro Michuhol Gu, Incheon 22212, South KoreaKorea Inst Energy Res, Hydrogen Res Dept, 152 Gajeong Ro, Daejeon 34129, South KoreaKorea Inst Energy Res, Computat Sci Engn Lab, 152 Gajeong Ro, Daejeon 34129, South KoreaKorea Inst Energy Res, Computat Sci Engn Lab, 152 Gajeong Ro, Daejeon 34129, South Korea|Pusan Natl Univ, Dept Nanoenergy Engn, 2 Busandaehak Ro 63beon Gil, Busan 46241, South Korea;

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