Dual Metal Active Sites in an Ir-1/FeOx Single-Atom Catalyst: A Redox Mechanism for the Water-Gas Shift Reaction

Liang, Jin-Xia1; Lin, Jian2; Liu, Jingyue3; Wang, Xiaodong2; Zhang, Tao2; Li, Jun4,5,6

2020-05-20

10.1002/anie.201914867

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   影响因子和分区

1433-7851

1521-3773

Herein, we report a theoretical and experimental study of the water-gas shift (WGS) reaction on Ir-1/FeOx single-atom catalysts. Water dissociates to OH* on the Ir-1 single atom and H* on the first-neighbour O atom bonded with a Fe site. The adsorbed CO on Ir-1 reacts with another adjacent O atom to produce CO2, yielding an oxygen vacancy (O-vac). Then, the formation of H-2 becomes feasible due to migration of H from adsorbed OH* toward Ir-1 and its subsequent reaction with another H*. The interaction of Ir-1 and the second-neighbouring Fe species demonstrates a new WGS pathway featured by electron transfer at the active site from Fe3+-O...Ir2+-O-vac to Fe2+-O-vac...Ir3+-O with the involvement of O-vac. The redox mechanism for WGS reaction through a dual metal active site (DMAS) is different from the conventional associative mechanism with the formation of formate or carboxyl intermediates. The proposed new reaction mechanism is corroborated by the experimental results with Ir-1/FeOx for sequential production of CO2 and H-2.

active sites density functional theory redox mechanism single-atom catalysts water-gas shift reaction

SCI ; EI

英语

NI论文

通讯

National Science Foundation of China[21763006][21878283][21576251][91645203][21590792] ; Natural Science Foundation of the Department of Education of Guizhou Province[QJTD[2015]55] ; Youth Innovation Promotion Association CAS[2017223] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002]

Chemistry

Chemistry, Multidisciplinary

WOS:000534635700001

WILEY-V C H VERLAG GMBH

20202108696826

Atoms ; Chemical shift ; Iridium compounds ; Water gas shift ; Carbon dioxide ; Reaction intermediates ; Catalyst activity ; Iron ; Iron compounds

Iron:545.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

CHEMISTRY

Web of Science

1.Guizhou Educ Univ, Guizhou Prov Key Lab Computat Nanomat Sci, Guiyang 550018, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
3.Arizona State Univ, Dept Phys, Tempe, AZ 85287 USA
4.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
5.Tsinghua Univ, Minist Educ, Key Lab Organ Optoelect & Mol Engn, Beijing 100084, Peoples R China
6.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China

Liang, Jin-Xia,Lin, Jian,Liu, Jingyue,et al. Dual Metal Active Sites in an Ir-1/FeOx Single-Atom Catalyst: A Redox Mechanism for the Water-Gas Shift Reaction[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2020,59(31):12868-12875.

Liang, Jin-Xia,Lin, Jian,Liu, Jingyue,Wang, Xiaodong,Zhang, Tao,&Li, Jun.(2020).Dual Metal Active Sites in an Ir-1/FeOx Single-Atom Catalyst: A Redox Mechanism for the Water-Gas Shift Reaction.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,59(31),12868-12875.

Liang, Jin-Xia,et al."Dual Metal Active Sites in an Ir-1/FeOx Single-Atom Catalyst: A Redox Mechanism for the Water-Gas Shift Reaction".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 59.31(2020):12868-12875.