Facet Engineering to Regulate Surface States of Topological Crystalline Insulator Bismuth Rhombic Dodecahedrons for Highly Energy Efficient Electrochemical CO2 Reduction

Xie, Huan1,2,3; Zhang, Tan4,5,6; Xie, Ruikuan1,2,3; Hou, Zhufeng1,2,3; Ji, Xuecong4,5,6; Pang, Yongyu1,2,3; Chen, Shaoqing7; Titirici, Maria-Magdalena8; Weng, Hongming4,5,6; Chai, Guoliang1,2,3

2021-06-01

10.1002/adma.202008373

ADVANCED MATERIALS   影响因子和分区

0935-9648

1521-4095

Bismuth (Bi) is a topological crystalline insulator (TCI), which has gapless topological surface states (TSSs) protected by a specific crystalline symmetry that strongly depends on the facet. Bi is also a promising electrochemical CO2 reduction reaction (ECO2RR) electrocatalyst for formate production. In this study, single-crystalline Bi rhombic dodecahedrons (RDs) exposed with (104) and (110) facets are developed. The Bi RDs demonstrate a very low overpotential and high selectivity for formate production (Faradic efficiency >92.2%) in a wide partial current density range from 9.8 to 290.1 mA cm(-2), leading to a remarkably high full-cell energy efficiency (69.5%) for ECO2RR. The significantly reduced overpotential is caused by the enhanced *OCHO adsorption on the Bi RDs. The high selectivity of formate can be ascribed to the TSSs and the trivial surface states opening small gaps in the bulk gap on Bi RDs, which strengthens and stabilizes the preferentially adsorbed *OCHO and mitigates the competing adsorption of *H during ECO2RR. This study describes a promising application of Bi RDs for high-rate formate production and high-efficiency energy storage of intermittent renewable electricity. Optimizing the geometry of TCIs is also proposed as an effective strategy to tune the TSSs of topological catalysts.

Bi rhombic dodecahedrons electrochemical CO (2) reduction high energy efficiency surface states topological crystalline insulators

SCI ; EI

英语

NI期刊

其他

China Postdoctoral Science Foundation[2019M662255] ; National Natural Science Foundation of China[21703248] ; National Key Research and Development Program of China["2017YFA0700103","2018YFA0704502"] ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDB20000000]

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

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

WOS:000666591700001

WILEY-V C H VERLAG GMBH

20212610574066

Carbon dioxide ; Electric energy storage ; Electrocatalysts ; Energy efficiency ; Surface states ; Topology

Energy Conservation:525.2 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Inorganic Compounds:804.2 ; Combinatorial Mathematics, Includes Graph Theory, Set Theory:921.4 ; Classical Physics; Quantum Theory; Relativity:931 ; High Energy Physics; Nuclear Physics; Plasma Physics:932

MATERIALS SCIENCE

Web of Science

1.Chinese Acad Sci, State Key Lab Struct Chem, Fujian Inst Res Struct Matter, Fuzhou 350002, Fujian, Peoples R China
2.Univ Chinese Acad Sci, Sch Chem Sci, Beijing 100049, Peoples R China
3.Fujian Sci & Technol Innovat Lab Optoelect Inform, Fuzhou 350108, Fujian, Peoples R China
4.Chinese Acad Sci, Inst Phys, Beijing Natl Res Ctr Condensed Matter Phys, Beijing 100190, Peoples R China
5.Univ Chinese Acad Sci, Sch Phys Sci, Beijing 100049, Peoples R China
6.Songshan Lake Mat Lab, Dongguan 523808, Guangdong, Peoples R China
7.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Guangdong, Peoples R China
8.Imperial Coll London, Dept Chem Engn, London SW7 2AZ, England

Xie, Huan,Zhang, Tan,Xie, Ruikuan,et al. Facet Engineering to Regulate Surface States of Topological Crystalline Insulator Bismuth Rhombic Dodecahedrons for Highly Energy Efficient Electrochemical CO2 Reduction[J]. ADVANCED MATERIALS,2021,33.

Xie, Huan.,Zhang, Tan.,Xie, Ruikuan.,Hou, Zhufeng.,Ji, Xuecong.,...&Chai, Guoliang.(2021).Facet Engineering to Regulate Surface States of Topological Crystalline Insulator Bismuth Rhombic Dodecahedrons for Highly Energy Efficient Electrochemical CO2 Reduction.ADVANCED MATERIALS,33.

Xie, Huan,et al."Facet Engineering to Regulate Surface States of Topological Crystalline Insulator Bismuth Rhombic Dodecahedrons for Highly Energy Efficient Electrochemical CO2 Reduction".ADVANCED MATERIALS 33(2021).