Black Phosphorous Mediates Surface Charge Redistribution of CoSe2 for Electrochemical H2O2 Production in Acidic Electrolytes

Zheng, Ya-Rong1,2; Hu, ShaoJin3; Zhang, Xiao-Long1; Ju, Huanxin4; Wang, Zhenbin5; Tan, Peng-Ju3; Wu, Rui1; Gao, Fei-Yue1; Zhuang, Taotao1; Zheng, Xiao3; Zhu, Junfa4; Gao, Min-Rui1; Yu, Shu-Hong1,6

2022-09-01

10.1002/adma.202205414

ADVANCED MATERIALS   Impact Factor & Quartile

0935-9648

1521-4095

Electrochemical generation of hydrogen peroxide (H2O2) by two-electron oxygen reduction offers a green method to mitigate the current dependence on the energy-intensive anthraquinone process, promising its on-site applications. Unfortunately, in alkaline environments, H2O2 is not stable and undergoes rapid decomposition. Making H2O2 in acidic electrolytes can prevent its decomposition, but choices of active, stable, and selective electrocatalysts are significantly limited. Here, the selective and efficient two-electron reduction of oxygen toward H2O2 in acid by a composite catalyst that is composed of black phosphorus (BP) nailed chemically on the metallic cobalt diselenide (CoSe2) surface is reported. It is found that this catalyst exhibits a 91% Faradic efficiency for H2O2 product at an overpotential of 300 mV. Moreover, it can mediate oxygen to H2O2 with a high production rate of approximate to 1530 mg L-1 h(-1) cm(-2) in a flow-cell reactor. Spectroscopic and computational studies together uncover a BP-induced surface charge redistribution in CoSe2, which leads to a favorable surface electronic structure that weakens the HOO* adsorption, thus enhancing the kinetics toward H2O2 formation.

acidic electrolytes electrocatalysis non-noble-metal electrocatalysts transition metal catalysts two-electron oxygen reduction

SCI

English

NI Journal Papers

Corresponding

National Natural Science Foundation of China["51732011","U1932213","21703228","21975237","51702312"] ; National Basic Research Program of China["2018YFA0702001","2021YFA0715700"] ; National Key Research and Development Program of China[2018YFE0202201] ; Science and Technology Major Project of Anhui Province[201903a05020003] ; University Synergy Innovation Program of Anhui Province[GXXT-2019028] ; China Postdoctoral Science Foundation[2016M592063]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000860638000001

WILEY-V C H VERLAG GMBH

MATERIALS SCIENCE

Web of Science

1.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Div Nanomat & Chem, Dept Chem,Inst Biomimet Mat & Chem,Anhui Engn Lab, Hefei 230026, Anhui, Peoples R China
2.Hefei Univ Technol, Anhui Prov Key Lab Adv Catalyt Mat & React Engn, Sch Chem & Chem Engn, Hefei 230009, Anhui, Peoples R China
3.Univ Sci & Technol China, Dept Chem Phys, Div Theoret & Computat Sci, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
4.Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230026, Anhui, Peoples R China
5.Tech Univ Denmark, Dept Phys, DK-2800 Lyngby, Denmark
6.Southern Univ Sci & Technol, Inst Innovat Mat, Dept Mat Sci & Engn, Dept Chem, Shenzhen 518055, Peoples R China

Zheng, Ya-Rong,Hu, ShaoJin,Zhang, Xiao-Long,et al. Black Phosphorous Mediates Surface Charge Redistribution of CoSe2 for Electrochemical H2O2 Production in Acidic Electrolytes[J]. ADVANCED MATERIALS,2022.

Zheng, Ya-Rong.,Hu, ShaoJin.,Zhang, Xiao-Long.,Ju, Huanxin.,Wang, Zhenbin.,...&Yu, Shu-Hong.(2022).Black Phosphorous Mediates Surface Charge Redistribution of CoSe2 for Electrochemical H2O2 Production in Acidic Electrolytes.ADVANCED MATERIALS.

Zheng, Ya-Rong,et al."Black Phosphorous Mediates Surface Charge Redistribution of CoSe2 for Electrochemical H2O2 Production in Acidic Electrolytes".ADVANCED MATERIALS (2022).