Dual Lewis Acid-Base Sites Regulate Silver-Copper Bimetallic Oxide Nanowires for Highly Selective Photoreduction of Carbon Dioxide to Methane

Deng, Shimao1; Wang, Ranhao1; Feng, Xuezhen1; Zheng, Renji1; Gong, Shaokuan2; Chen, Xihan2; Shangguan, Yangzi1; Deng, Lili1; Tang, Huan1; Dai, Hao3,4; Duan, Lele3,4; Liu, Chengyuan5; Pan, Yang5; Chen, Hong1

2023-08-01

10.1002/anie.202309625

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   影响因子和分区

1433-7851

1521-3773

Highly selective photoreduction of CO2 to valuable hydrocarbons is of great importance to achieving a carbonneutral society. Precisely manipulating the formation of the Metal(1)center dot center dot center dot C=O center dot center dot center dot Metal(2) (M-1 center dot center dot center dot C=O center dot center dot center dot M-2) intermediate on the photocatalyst interface is the most critical step for regulating selectivity, while still a significant challenge. Herein, inspired by the polar electronic structure feature of CO2 molecule, we propose a strategy whereby the Lewis acid-base dual sites confined in a bimetallic catalyst surface are conducive to forming a M-1 center dot center dot center dot C=O center dot center dot center dot M-2 intermediate precisely, which can promote selectivity to hydrocarbon formation. Employing the Ag2Cu2O3 nanowires with abundant Cu center dot center dot center dot Ag Lewis acid-base dual sites on the preferred exposed {110} surface as a model catalyst, 100% selectivity toward photoreduction of CO2 into CH4 has been achieved. Subsequent surface-quenching experiments and density functional theory (DFT) calculations verify that the Cu center dot center dot center dot Ag Lewis acid-base dual sites do play a vital role in regulating the M-1 center dot center dot center dot C=O center dot center dot center dot M-2 intermediate formation that is considered to be prone to convert CO2 into hydrocarbons. This study reports a highly selective CO2 photocatalyst, which was designed on the basis of a newly proposed theory for precise regulation of reaction intermediates. Our findings will stimulate further research on dual-site catalyst design for CO2 reduction to hydrocarbons.

Ag center dot center dot center dot C=O center dot center dot center dot Cu Intermediate Lewis Acid-Base Dual Sites Methane Selective Reduction

SCI ; EI

英语

NI论文

第一 ; 通讯

Shenzhen Science and Technology Innovation Committee[KCXST20221021111208018] ; National Key Research and Development Program of China[2021YFA1202500] ; Natural Science Funds for Distinguished Young Scholar of Guangdong Province, China[2020B151502094] ; National Natural Science Foundation of China[21777045] ; Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials[ZDSYS20200421111401738] ; Foundation of Shenzhen Science, Technology and Innovation Commission (SSTIC)["JCYJ20200109141625078","JCYJ20190809144409460"] ; Guangdong Basic and Applied Basic Research Foundation[2020A1515110723]

Chemistry

Chemistry, Multidisciplinary

WOS:001050208300001

WILEY-V C H VERLAG GMBH

20233414604885

Carbon dioxide ; Catalyst selectivity ; Copper oxides ; Density functional theory ; Design for testability ; Electronic structure ; Nanowires ; Reaction intermediates ; Reduction

Nanotechnology:761 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4 ; Solid State Physics:933

CHEMISTRY

Web of Science

1.Southern Univ Sci & Technol, Sch Environm Sci & Engn, Shenzhen Key Lab Interfacial Sci & Engn Mat SKLISE, State Environm Protect Key Lab Integrated Surface, Shenzhen 518055, Peoples R China
2.Southern Univ Sci & Technol, SUSTech Energy Inst Carbon Neutral, Dept Mech & Energy Engn, Shenzhen 518055, Peoples R China
3.Southern Univ Sci & Technol, Shenzhen Grubbs Inst, Dept Chem, Shenzhen 518055, Peoples R China
4.Southern Univ Sci & Technol, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Peoples R China
5.Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China

Deng, Shimao,Wang, Ranhao,Feng, Xuezhen,et al. Dual Lewis Acid-Base Sites Regulate Silver-Copper Bimetallic Oxide Nanowires for Highly Selective Photoreduction of Carbon Dioxide to Methane[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2023,62(39).

Deng, Shimao.,Wang, Ranhao.,Feng, Xuezhen.,Zheng, Renji.,Gong, Shaokuan.,...&Chen, Hong.(2023).Dual Lewis Acid-Base Sites Regulate Silver-Copper Bimetallic Oxide Nanowires for Highly Selective Photoreduction of Carbon Dioxide to Methane.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,62(39).

Deng, Shimao,et al."Dual Lewis Acid-Base Sites Regulate Silver-Copper Bimetallic Oxide Nanowires for Highly Selective Photoreduction of Carbon Dioxide to Methane".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62.39(2023).