期刊
CHEMCATCHEM
卷 13, 期 20, 页码 4372-4383出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.202100805
关键词
Electrocatalysis; Graphene derivative; Hydrogen peroxide; Oxygen reduction reaction; Renewable energy
资金
- Operational Programme Research, Development and Education - European Regional Development Fund [CZ.02.1.01/0.0/0.0/15_003/0000416]
- Czech Science Foundation, Project GA CR - EXPRO [19-27454X]
- ERDF/ESF project Nano4Future [CZ.02.1.01/0.0/0.0/16_019/0000754]
- Research Infrastructure NanoEnviCz - Ministry of Education, Youth and Sports of the Czech Republic [LM2018124]
- University of Trieste
- MUR-PRIN2020 project
- ERC [683024]
Carbon-based materials, such as N-GA with selectively installed carboxyl groups, exhibit high catalytic activity for 2e(-) ORR, resulting in efficient production of H2O2 with high Faradaic efficiency.
Practical-scale on-site production of hydrogen peroxide (H2O2) via two-electron (2e(-)) oxygen reduction reaction (ORR) relies on efficient, robust, and selective electrocatalysts. Among them, carbon-based materials are cheap, abundant, durable, and their surface properties can be tuned to favor the 2e(-) ORR pathways, resulting in higher efficiency and facilitating possible scale-up towards commercially appealing levels. Here, we demonstrate that the selective installment of carboxyl groups on the surface of N-doped graphene yielding a material named graphene acid (N-GA) promotes the catalytic 2e(-) ORR, achieving a H2O2 faradaic efficiency (FE) as high as 70 % in acidic media (pH=0.96) and a H2O2 productivity in long term bulk electrolysis that could reach 107.8 mmol g(catalyst)(-1) h(-1) under optimized conditions. Extended XPS analysis and density functional theory (DFT) calculations revealed that surface carboxylic acid functional groups play a significant role in achieving the high activity of N-GA for 2e(-) ORR.
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