Crystalline Lattice-Confined Atomic Pt in Metal Carbides to Match Electronic Structures and Hydrogen Evolution Behaviors of Platinum

Ma, Tian1; Cao, Hao2,3; Li, Shuang1,4; Cao, Sujiao1; Zhao, Zhenyang1; Wu, Zihe1; Yan, Rui1; Yang, Chengdong1; Wang, Yi5; van Aken, Peter A.6; Qiu, Li1; Wang, Yang-Gang2,3; Cheng, Chong1

2022-09-01

10.1002/adma.202206368

ADVANCED MATERIALS   Impact Factor & Quartile

0935-9648

1521-4095

Platinum-based catalysts occupy a pivotal position in diverse catalytic applications in hydrogen chemistry and electrochemistry, for instance, the hydrogen evolution reactions (HER). While adsorbed Pt atoms on supports often cause severe mismatching on electronic structures and HER behaviors from metallic Pt due to the different energy level distribution of electron orbitals. Here, the design of crystalline lattice-confined atomic Pt in metal carbides using the Pt-centered polyoxometalate frameworks with strong Pt-O-metal covalent bonds is reported. Remarkably, the lattice-confined atomic Pt in the tungsten carbides (Pt-doped@WCx, both Pt and W have atomic radii of 1.3 angstrom) exhibit near-zero valence states and similar electronic structures as metallic Pt, thus delivering matched energy level distributions of the Pt 5d(z)2 and H 1s orbitals and similar acidic hydrogen evolution behaviors. In alkaline conditions, the Pt-doped@WCx exhibits 40 times greater mass activity (49.5 A mg(Pt)(-1) at eta = 150 mV) than the Pt@C because of the favorable water dissociation and H* transport. These findings offer a universal pathway to construct urgently needed atomic-scale catalysts for broad catalytic reactions.

atomic catalysts electrocatalysts hydrogen evolution reaction metal carbides water splitting

SCI ; EI

English

NI Journal Papers

Corresponding

National Natural Science Foundation of China["52161145402","52173133","81971622"] ; National Key R&D Program of China["2021YFE0205000","2019YFA0110600"] ; Science and Technology Project of Sichuan Province["2021YFH0135","2021YJ0554"] ; NSFC of China[22022504] ; Guangdong "Pearl River" Talent Plan[2019QN01L353] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002] ; State Key Laboratory of Polymer Materials Engineering["sklpme2022-3-07","sklpme2021-4-02"] ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)[LI 3545/1-1] ; European Union[823717 - ESTEEM3]

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

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

WOS:000849560000001

WILEY-V C H VERLAG GMBH

20223712716243

Alkalinity ; Atoms ; Electrocatalysis ; Electronic structure ; Metals ; Platinum compounds ; Tungsten carbide

Chemistry, General:801.1 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3

MATERIALS SCIENCE

Web of Science

1.Sichuan Univ, West China Hosp, Coll Polymer Sci & Engn, Dept Ultrasound,State Key Lab Polymer Mat Engn, Chengdu 610041, Peoples R China
2.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
3.Southern Univ Sci & Technol, Guangdong Prov Key Lab Catalyt Chem, Shenzhen 518055, Guangdong, Peoples R China
4.Tech Univ Berlin, Dept Chem, Hardenbergstr 40, D-10623 Berlin, Germany
5.Nanjing Univ Aeronaut & Astronaut, Ctr Microscopy & Anal, Nanjing 210016, Peoples R China
6.Max Planck Inst Solid State Res, Stuttgart Ctr Electron Microscopy, Heisenbergstr 1, D-70569 Stuttgart, Germany

Ma, Tian,Cao, Hao,Li, Shuang,et al. Crystalline Lattice-Confined Atomic Pt in Metal Carbides to Match Electronic Structures and Hydrogen Evolution Behaviors of Platinum[J]. ADVANCED MATERIALS,2022.

Ma, Tian.,Cao, Hao.,Li, Shuang.,Cao, Sujiao.,Zhao, Zhenyang.,...&Cheng, Chong.(2022).Crystalline Lattice-Confined Atomic Pt in Metal Carbides to Match Electronic Structures and Hydrogen Evolution Behaviors of Platinum.ADVANCED MATERIALS.

Ma, Tian,et al."Crystalline Lattice-Confined Atomic Pt in Metal Carbides to Match Electronic Structures and Hydrogen Evolution Behaviors of Platinum".ADVANCED MATERIALS (2022).