Electrosynthesis of Hydrogen Peroxide Enabled by Exceptional Molecular Ni Sites in a Graphene-Supported Nickel Organic Framework

Yu，Dongxue1; Zhu，Peng3; Hu，Chunfeng1; Huang，Xiang4; Tang，Kangjian1; Wang，Jiong1,2

2023-12-14

10.1021/acs.jpclett.3c02774

Journal of Physical Chemistry Letters   影响因子和分区

1948-7185

Electrosynthesis of hydrogen peroxide (HO) from 2e transfer of the oxygen reduction reaction (2e-ORR) is a potential alternative to the traditional anthraquinone process. Two-dimensional (2D) metal-organic frameworks (MOFs) supported by carbon are frequently reported as promising 2e-ORR catalysts. Herein, a graphene-supported 2D MOF of Ni(2,3,6,7,10,11-hexahydrotriphenylene) is synthesized through a common hydrothermal method, which exhibits high 2e-ORR performance. It is discovered that except for emerging MOFs, exceptional molecularly dispersed Ni sites coexist in the synthesis that have the same coordination sphere of the NiOC moiety as the MOF. The molecular Ni sites are more catalytically active. The graphene support contains a suitable amount of residual oxygen groups, leading to the generation of those molecularly dispersed Ni sites. The oxygen groups exhibit a moderate electron-withdrawing effect at the outer sphere of Ni sites to slightly increase their oxidation state. This interaction decreases overpotentials and kinetically improves the selectivity of the 2e reaction pathway.

EI ; SCI

英语

NI论文

其他

20235015222118

Coordination reactions ; Electrolytic reduction ; Hydrogen peroxide ; Ketones ; Nickel ; Organic polymers ; Organometallics ; Oxidation ; Oxygen

Ore Treatment:533.1 ; Nickel:548.1 ; Nanotechnology:761 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2 ; Organic Polymers:815.1.1

2-s2.0-85179614300

Scopus

1.Innovation Center for Chemical Science,College of Chemistry,Chemical Engineering and Materials Science,Soochow University,Suzhou,215006,China
2.Jiangsu Key Laboratory of Advanced Negative Carbon Technologies,Soochow University,Suzhou,215123,China
3.Department of Chemistry,Tsinghua University,Beijing,100084,China
4.Department of Physics,Southern University of Science and Technology,Shenzhen,518055,China

Yu，Dongxue,Zhu，Peng,Hu，Chunfeng,et al. Electrosynthesis of Hydrogen Peroxide Enabled by Exceptional Molecular Ni Sites in a Graphene-Supported Nickel Organic Framework[J]. Journal of Physical Chemistry Letters,2023,14(49):10959-10966.

Yu，Dongxue,Zhu，Peng,Hu，Chunfeng,Huang，Xiang,Tang，Kangjian,&Wang，Jiong.(2023).Electrosynthesis of Hydrogen Peroxide Enabled by Exceptional Molecular Ni Sites in a Graphene-Supported Nickel Organic Framework.Journal of Physical Chemistry Letters,14(49),10959-10966.

Yu，Dongxue,et al."Electrosynthesis of Hydrogen Peroxide Enabled by Exceptional Molecular Ni Sites in a Graphene-Supported Nickel Organic Framework".Journal of Physical Chemistry Letters 14.49(2023):10959-10966.