Oxygen Functional Groups Regulate Cobalt-Porphyrin Molecular Electrocatalyst for Acidic H₂O₂ Electrosynthesis at Industrial-Level Current

Chen, Yihe1,2; Zhen, Cheng3,4; Chen, Yubin2; Zhao, Hao2; Wang, Yuda2; Yue, Zhouying2; Wang, Qiansen1,2; Li, Jun2; Gu, M. Danny4; Cheng, Qingqing2; Yang, Hui1,2

2024-07-01

10.1002/anie.202407163

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   影响因子和分区

1433-7851

1521-3773

Electrosynthesis of hydrogen peroxide (H2O2) based on proton exchange membrane (PEM) reactor represents a promising approach to industrial-level H2O2 production, while it is hampered by the lack of high-efficiency electrocatalysts in acidic medium. Herein, we present a strategy for the specific oxygen functional group (OFG) regulation to promote the H2O2 selectivity up to 92 % in acid on cobalt-porphyrin molecular assembled with reduced graphene oxide. In situ X-ray adsorption spectroscopy, in situ Raman spectroscopy and Kelvin probe force microscopy combined with theoretical calculation unravel that different OFGs exert distinctive regulation effects on the electronic structure of Co center through either remote (carboxyl and epoxy) or vicinal (hydroxyl) interaction manners, thus leading to the opposite influences on the promotion in 2e(-) ORR selectivity. As a consequence, the PEM electrolyzer integrated with the optimized catalyst can continuously and stably produce the high-concentration of ca. 7 wt % pure H2O2 aqueous solution at 400 mA cm(-2) over 200 h with a cell voltage as low as ca. 2.1 V, suggesting the application potential in industrial-scale H2O2 electrosynthesis.

Local-environmental regulation Oxygen functional groups H2O2 electrosynthesis Molecular electrocatalyst PEM electrolyzer

SCI ; EI

英语

其他

National Key Research and Development Project["2021YFB4000200","2022YFA1503900"] ; Shanghai Science and Technology Innovation Action Plan["23ZR1471000","22511102500"]

Chemistry

Chemistry, Multidisciplinary

WOS:001282247200001

WILEY-V C H VERLAG GMBH

CHEMISTRY

Web of Science

1.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
2.Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
3.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Guangdong, Peoples R China
4.Eastern Inst Technol, Eastern Inst Adv Study, Ningbo 315200, Zhejiang, Peoples R China

Chen, Yihe,Zhen, Cheng,Chen, Yubin,et al. Oxygen Functional Groups Regulate Cobalt-Porphyrin Molecular Electrocatalyst for Acidic H₂O₂ Electrosynthesis at Industrial-Level Current[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2024.

Chen, Yihe.,Zhen, Cheng.,Chen, Yubin.,Zhao, Hao.,Wang, Yuda.,...&Yang, Hui.(2024).Oxygen Functional Groups Regulate Cobalt-Porphyrin Molecular Electrocatalyst for Acidic H₂O₂ Electrosynthesis at Industrial-Level Current.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION.

Chen, Yihe,et al."Oxygen Functional Groups Regulate Cobalt-Porphyrin Molecular Electrocatalyst for Acidic H₂O₂ Electrosynthesis at Industrial-Level Current".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2024).