Tailoring Electrocatalytic Hydrogen Evolution Activity in Topological Triangular Metal-Organic Frameworks

Gao, Yixuan1; Tao, Lei2,3,4; Yin, Yiyang2,3,4; Wang, Han5; Ge, Yiyao1

2024-10-01

10.1002/adsu.202400622

ADVANCED SUSTAINABLE SYSTEMS   影响因子和分区

2366-7486

["Metal-organic frameworks (MOFs) have attracted considerable attention in catalysis due to their exceptional structural and chemical tunability. However, high electrical conductivity is rare in MOFs, hindering their practical applications toward catalytic reactions. Recently, 2D topological MOFs stand out for the unique topologically nontrivial electronic structures. Particularly, their high electrical conductivity and chemical tunability make them promising candidates as high-performance catalysts. In this study, theoretical investigations are conducted into the intrinsic electronic properties and chemical activity of a 2D topological Cu-1,3,5-tris(pyridyl)benzene (Cu-TPyB) framework. It is found that the coordination environment of Cu with pyridyl groups plays a crucial role in modulating the electron density around the Fermi level, thereby enhancing the catalytic activity of Cu-TPyB toward electrochemical hydrogen evolution reaction (HER). Furthermore, substituting the single embedded Cu atom with Cu3 and Cu4Bi3 clusters further increases the electron density around the Fermi level. Specifically, the Cu4Bi3-TPyB framework exhibits superior HER activity, which is attributed to its high electron density contributed by the p orbitals of Bi and the d orbitals of Cu. This work introduces a novel approach for optimizing the catalytic activity of 2D MOFs and developing high-performance catalysts.","In this work, the intrinsic electronic properties and catalytic activity of a 2D topological Cu-TPyB framework are theoretically investigated. It is found that the coordination environment and central metal clusters play crucial roles in modulating the electron density around the Fermi level, thereby enhancing the catalytic activity of Cu-TPyB toward electrochemical hydrogen evolution reaction. image"]

2D organic topological insulators first-principles calculations hydrogen evolution reaction metal-organic frameworks

SCI

英语

其他

Fundamental Research Funds for the Central Universities[FRF-TP-24-055A] ; University of Science and Technology Beijing[00007838] ; null[52350322] ; null[52201231]

Science & Technology - Other Topics ; Materials Science

Green & Sustainable Science & Technology ; Materials Science, Multidisciplinary

WOS:001327436200001

WILEY-V C H VERLAG GMBH

Web of Science

1.Univ Sci & Technol Beijing, State Key Lab Adv Met & Mat, Beijing 100083, Peoples R China
2.Chinese Acad Sci, Beijing Natl Ctr Condensed Matter Phys, Beijing 100190, Peoples R China
3.Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China
4.Univ Chinese Acad Sci, Sch Phys Sci, Beijing 100190, Peoples R China
5.Southern Univ Sci & Technol, Dept Elect & Elect Engn, Shenzhen 518055, Peoples R China

Gao, Yixuan,Tao, Lei,Yin, Yiyang,et al. Tailoring Electrocatalytic Hydrogen Evolution Activity in Topological Triangular Metal-Organic Frameworks[J]. ADVANCED SUSTAINABLE SYSTEMS,2024.

Gao, Yixuan,Tao, Lei,Yin, Yiyang,Wang, Han,&Ge, Yiyao.(2024).Tailoring Electrocatalytic Hydrogen Evolution Activity in Topological Triangular Metal-Organic Frameworks.ADVANCED SUSTAINABLE SYSTEMS.

Gao, Yixuan,et al."Tailoring Electrocatalytic Hydrogen Evolution Activity in Topological Triangular Metal-Organic Frameworks".ADVANCED SUSTAINABLE SYSTEMS (2024).