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

Ling Tan, Si Min Xu, Zelin Wang, Yanqi Xu, Xian Wang, Xiaojie Hao, Sha Bai, Chenjun Ning, Yu Wang, Wenkai Zhang, Yun Kyung Jo, Seong Ju Hwang, Xingzhong Cao, Xusheng Zheng, Hong Yan, Yufei Zhao, Haohong Duan, Yu Fei Song

Research output: Contribution to journalArticlepeer-review

70 Citations (Scopus)

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).

Original languageEnglish
Pages (from-to)11860-11867
Number of pages8
JournalAngewandte Chemie - International Edition
Volume58
Issue number34
DOIs
Publication statusPublished - 2019 Aug 19

Bibliographical note

Funding Information:
The authors are grateful for the financial support from the National Natural Science Foundation of China (U1707603, 21625101, 21521005, U1507102), Beijing Natural Science Foundation (2182047) and the Fundamental Research Funds for the Central Universities (XK1802-6, XK1902, 12060093063, ZY1709) and Young Elite Scientist Sponsorship Program by CAST (YESS), and the “Chemical Grid Project” of Beijing University of Chemical Technology. We acknowledge the National Supercomputing Center in Shenzhen for providing the computational resources and the materials studio (version 6.1, CASTEP). We would like to thank 1W1B beam line of Beijing Synchrotron Radiation Facility (BSRF), 10C beam line of Pohang Accelerator Laboratory (PAL) and the photoemission end-station at beamline BL10B in the National Synchrotron Radiation Laboratory (NSRL) in Hefei, China.

Funding Information:
The authors are grateful for the financial support from the National Natural Science Foundation of China (U1707603, 21625101, 21521005, U1507102), Beijing Natural Science Foundation (2182047) and the Fundamental Research Funds for the Central Universities (XK1802-6, XK1902, 12060093063, ZY1709) and Young Elite Scientist Sponsorship Program by CAST (YESS), and the ?Chemical Grid Project? of Beijing University of Chemical Technology. We acknowledge the National Supercomputing Center in Shenzhen for providing the computational resources and the materials studio (version 6.1, CASTEP). We would like to thank 1W1B beam line of Beijing Synchrotron Radiation Facility (BSRF), 10C beam line of Pohang Accelerator Laboratory (PAL) and the photoemission end-station at beamline BL10B in the National Synchrotron Radiation Laboratory (NSRL) in Hefei, China.

Publisher Copyright:
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)

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