Volume 131, Issue 34 pp. 11986-11993
Forschungsartikel

Highly Selective Photoreduction of CO2 with Suppressing H2 Evolution over Monolayer Layered Double Hydroxide under Irradiation above 600 nm

Ling Tan

Ling Tan

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China

These authors contributed equally to this work.

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Dr. Si-Min Xu

Dr. Si-Min Xu

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China

These authors contributed equally to this work.

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Zelin Wang

Zelin Wang

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China

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Yanqi Xu

Yanqi Xu

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China

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Xian Wang

Xian Wang

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China

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Xiaojie Hao

Xiaojie Hao

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China

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Sha Bai

Sha Bai

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China

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Chenjun Ning

Chenjun Ning

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China

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Yu Wang

Yu Wang

Department of Physics, Beijing Normal University, Beijing, 100875 P. R. China

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Prof. Wenkai Zhang

Prof. Wenkai Zhang

Department of Physics, Beijing Normal University, Beijing, 100875 P. R. China

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Yun Kyung Jo

Yun Kyung Jo

Center for Hybrid Interfacial Chemical Structure (CICS), Department of Chemistry and Nanoscience, College of Natural Sciences, Ewha Womans University, Seoul, 03760 Republic of Korea

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Prof. Seong-Ju Hwang

Prof. Seong-Ju Hwang

Center for Hybrid Interfacial Chemical Structure (CICS), Department of Chemistry and Nanoscience, College of Natural Sciences, Ewha Womans University, Seoul, 03760 Republic of Korea

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Prof. Xingzhong Cao

Prof. Xingzhong Cao

Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049 P. R. China

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Dr. Xusheng Zheng

Dr. Xusheng Zheng

School of Chemistry and Materials Science, National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui, 230026 P. R. China

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Prof. Hong Yan

Prof. Hong Yan

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China

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Prof. Yufei Zhao

Corresponding Author

Prof. Yufei Zhao

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China

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Dr. Haohong Duan

Corresponding Author

Dr. Haohong Duan

Department of Chemistry, Tsinghua University, 30 Shuangqing Rd, Haidian Qu, Beijing Shi, 100084 China

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Prof. Yu-Fei Song

Corresponding Author

Prof. Yu-Fei Song

State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China

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First published: 10 June 2019
Citations: 57

Abstract

Although progress has been made to improve photocatalytic CO2 reduction under visible light (λ>400 nm), the development of photocatalysts that can work under a longer wavelength (λ>600 nm) remains a challenge. Now, a heterogeneous photocatalyst system consisting of a ruthenium complex and a monolayer nickel-alumina layered double hydroxide (NiAl-LDH), which act as light-harvesting and catalytic units for selective photoreduction of CO2 and H2O into CH4 and CO under irradiation with λ>400 nm. By precisely tuning the irradiation wavelength, the selectivity of CH4 can be improved to 70.3 %, and the H2 evolution reaction can be completely suppressed under irradiation with λ>600 nm. The photogenerated electrons matching the energy levels of photosensitizer and m-NiAl-LDH only localized at the defect state, providing a driving force of 0.313 eV to overcome the Gibbs free energy barrier of CO2 reduction to CH4 (0.127 eV), rather than that for H2 evolution (0.425 eV).

Conflict of interest

The authors declare no conflict of interest.

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