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 journalArticle

6 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 Jan 1

Fingerprint

Monolayers
Aluminum Oxide
Irradiation
Photocatalysts
Nickel
Alumina
Wavelength
Photosensitizing Agents
Photosensitizers
Ruthenium
Energy barriers
Gibbs free energy
Carbon Monoxide
Electron energy levels
Tuning
Defects
Electrons
hydroxide ion

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)

Cite this

Tan, Ling ; Xu, Si Min ; Wang, Zelin ; Xu, Yanqi ; Wang, Xian ; Hao, Xiaojie ; Bai, Sha ; Ning, Chenjun ; Wang, Yu ; Zhang, Wenkai ; Jo, Yun Kyung ; Hwang, Seong Ju ; Cao, Xingzhong ; Zheng, Xusheng ; Yan, Hong ; Zhao, Yufei ; Duan, Haohong ; Song, Yu Fei. / Highly Selective Photoreduction of CO2 with Suppressing H2 Evolution over Monolayer Layered Double Hydroxide under Irradiation above 600 nm. In: Angewandte Chemie - International Edition. 2019 ; Vol. 58, No. 34. pp. 11860-11867.
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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).",
author = "Ling Tan and Xu, {Si Min} and Zelin Wang and Yanqi Xu and Xian Wang and Xiaojie Hao and Sha Bai and Chenjun Ning and Yu Wang and Wenkai Zhang and Jo, {Yun Kyung} and Hwang, {Seong Ju} and Xingzhong Cao and Xusheng Zheng and Hong Yan and Yufei Zhao and Haohong Duan and Song, {Yu Fei}",
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Tan, L, Xu, SM, Wang, Z, Xu, Y, Wang, X, Hao, X, Bai, S, Ning, C, Wang, Y, Zhang, W, Jo, YK, Hwang, SJ, Cao, X, Zheng, X, Yan, H, Zhao, Y, Duan, H & Song, YF 2019, 'Highly Selective Photoreduction of CO2 with Suppressing H2 Evolution over Monolayer Layered Double Hydroxide under Irradiation above 600 nm', Angewandte Chemie - International Edition, vol. 58, no. 34, pp. 11860-11867. https://doi.org/10.1002/anie.201904246

Highly Selective Photoreduction of CO2 with Suppressing H2 Evolution over Monolayer Layered Double Hydroxide under Irradiation above 600 nm. / Tan, Ling; Xu, Si Min; Wang, Zelin; Xu, Yanqi; Wang, Xian; Hao, Xiaojie; Bai, Sha; Ning, Chenjun; Wang, Yu; Zhang, Wenkai; Jo, Yun Kyung; Hwang, Seong Ju; Cao, Xingzhong; Zheng, Xusheng; Yan, Hong; Zhao, Yufei; Duan, Haohong; Song, Yu Fei.

In: Angewandte Chemie - International Edition, Vol. 58, No. 34, 01.01.2019, p. 11860-11867.

Research output: Contribution to journalArticle

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T1 - Highly Selective Photoreduction of CO2 with Suppressing H2 Evolution over Monolayer Layered Double Hydroxide under Irradiation above 600 nm

AU - Tan, Ling

AU - Xu, Si Min

AU - Wang, Zelin

AU - Xu, Yanqi

AU - Wang, Xian

AU - Hao, Xiaojie

AU - Bai, Sha

AU - Ning, Chenjun

AU - Wang, Yu

AU - Zhang, Wenkai

AU - Jo, Yun Kyung

AU - Hwang, Seong Ju

AU - Cao, Xingzhong

AU - Zheng, Xusheng

AU - Yan, Hong

AU - Zhao, Yufei

AU - Duan, Haohong

AU - Song, Yu Fei

PY - 2019/1/1

Y1 - 2019/1/1

N2 - 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).

AB - 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).

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