Single copper sites dispersed on defective TiO2-xas a synergistic oxygen reduction reaction catalyst

Li，Minchan1; Qin，Ning1,2; Ji，Zongwei1,3; Gan，Qingmeng1; Wang，Zhenyu1; Li，Yingzhi1; Cao，Lujie1; Yuan，Huimin1; He，Dongsheng4; Chen，Zhenhua5; Luo，Guangfu1,3; Zhang，Kaili2; Lu，Zhouguang1

2021-01-21

10.1063/5.0030559

JOURNAL OF CHEMICAL PHYSICS   影响因子和分区

0021-9606

1089-7690

Catalysts containing isolated single atoms have attracted much interest due to their good catalytic behavior, bridging the gap between homogeneous and heterogeneous catalysts. Here, we report an efficient oxygen reduction reaction (ORR) catalyst that consists of atomically dispersed single copper sites confined by defective mixed-phased TiO2-x. This synergistic catalyst was produced by introducing Cu2+ to a metal organic framework (MOF) using the Mannich reaction, occurring between the carbonyl group in Cu(acac)2 and the amino group on the skeleton of the MOF. The embedding of single copper atoms was confirmed by atomic-resolution high-angle annular dark-field scanning transmission electron microscopy and x-ray absorption fine structure spectroscopy. Electronic structure modulation of the single copper sites coupling with oxygen vacancies was further established by electron paramagnetic resonance spectroscopy and first-principles calculations. Significantly enhanced ORR activity and stability were achieved on this special Cu single site. The promising application of this novel electrocatalyst was demonstrated in a prototype Zn-air battery. This strategy of the stabilization of single-atom active sites by optimization of the atomic and electronic structure on a mixed matrix support sheds light on the development of highly efficient electrocatalysts.

SCI ; EI

英语

第一 ; 通讯

Basic Research Project of the Science and Technology Innovation Commission of Shenzhen[JCYJ20190809115413414] ; Shenzhen Peacock Plan[KQTD2016022620054656] ; Guangdong-Hong Kong-Macao Joint Laboratory[2019B121205001] ; National Natural Science Foundation of China[21671096] ; Introduced Innovative R&D Team of Guangdong[2017ZT07C062] ; Guangdong Provincial Key Laboratory of Computational Science and Material Design[2019B030301001]

Chemistry ; Physics

Chemistry, Physical ; Physics, Atomic, Molecular & Chemical

WOS:000630465400002

AMER INST PHYSICS

20210509834112

Atoms ; Calculations ; Copper ; Defects ; Electrocatalysts ; Electrolytic reduction ; Electron spin resonance spectroscopy ; Electronic structure ; High resolution transmission electron microscopy ; Metal-Organic Frameworks ; Organometallics ; Oxide minerals ; Oxygen reduction reaction ; Oxygen vacancies ; Paramagnetic resonance ; Scanning electron microscopy ; Titanium dioxide ; X ray absorption ; X ray absorption fine structure spectroscopy ; Zinc air batteries

Minerals:482.2 ; Ore Treatment:533.1 ; Copper:544.1 ; Magnetism: Basic Concepts and Phenomena:701.2 ; Electromagnetic Waves:711 ; Optical Devices and Systems:741.3 ; Chemistry:801 ; Chemical Agents and Basic Industrial Chemicals:803 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2 ; Mathematics:921 ; Atomic and Molecular Physics:931.3 ; Crystalline Solids:933.1 ; Materials Science:951

CHEMISTRY

2-s2.0-85099772019

Scopus

1.Department of Materials Science and Engineering,Guangdong-Hong Kong-Macao Jt. Lab. for Photonic-Thermal-Electrical Energy Materials and Devices,Southern University of Science and Technology,Shenzhen,518055,China
2.Department of Mechanical Engineering,City University of Hong Kong,Kowloon, Hong Kong,83 Tat Chee Avenue,Hong Kong
3.Guangdong Provincial Key Laboratory of Computational Science and Material Design,Southern University of Science and Technology,Shenzhen,518055,China
4.Materials Characterization and Preparation Center,Southern University of Science and Technology,Shenzhen, Guangdong,518055,China
5.Shanghai Synchrotron Radiation Facility (SSRF),Shanghai Advanced Research Institute,Chinese Academy of Sciences,Shanghai,201800,China

Li，Minchan,Qin，Ning,Ji，Zongwei,et al. Single copper sites dispersed on defective TiO2-xas a synergistic oxygen reduction reaction catalyst[J]. JOURNAL OF CHEMICAL PHYSICS,2021,154(3).

Li，Minchan.,Qin，Ning.,Ji，Zongwei.,Gan，Qingmeng.,Wang，Zhenyu.,...&Lu，Zhouguang.(2021).Single copper sites dispersed on defective TiO2-xas a synergistic oxygen reduction reaction catalyst.JOURNAL OF CHEMICAL PHYSICS,154(3).

Li，Minchan,et al."Single copper sites dispersed on defective TiO2-xas a synergistic oxygen reduction reaction catalyst".JOURNAL OF CHEMICAL PHYSICS 154.3(2021).