Applied Catalysis B: Environmental, volume 300, pages 120695

Ultrahigh surface density of Co-N2C single-atom-sites for boosting photocatalytic CO2 reduction to methanol

Minzhi Ma ¹

Zeai Huang ¹

Dmitry E. Doronkin ²

Wenjun Fa ³

Zhiqiang Rao ⁴

Yanzhao Zou ⁴

Rui Wang ⁴

Yunqian Zhong ⁴

Yuehan Cao ⁴

Ruiyang Zhang ⁴

Ying Zhou ¹

Hide authors affiliations Show authors affiliations: 4 affiliations

State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum university, Chengdu 610500, China |

Institute of Catalysis Research and Technology and Institute for Chemical Technology and Polymer Chemistry, Karlsruhe Institute of Technology, Karlsruhe 76131, Germany |

Key Laboratory of Micro-Nano Materials for Energy Storage and Conversion of Henan Province & College of Advanced Materials and Energy, Xuchang University, Henan 461000, China |

⁴

Institute of Carbon Neutrality & School of New Energy and Materials, Southwest Petroleum University, Chengdu 610500, China |

Publication type: Journal Article

Publication date: 2022-01-01

Elsevier

Journal: Applied Catalysis B: Environmental

Quartile SCImago

Quartile WOS

Impact factor: 22.1

ISSN: 09263373, 18733883

DOI: 10.1016/j.apcatb.2021.120695

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Catalysis

Process Chemistry and Technology

General Environmental Science

Abstract

Cobalt species as active sites for photocatalytic reduction of CO 2 to valuable products such as methanol have received increasing attention, however, it remains a huge challenge to achieve the high activity. Herein, a pyrolysis-induced-vaporization strategy was successfully employed to fabricate Co/g-C 3 N 4 single-atom catalysts (Co/g-C 3 N 4 SACs) with surface Co atom loading up to 24.6 wt%. Systematic investigation of Co/g-C 3 N 4 SACs formation process disclosed that concentrated-H 2 SO 4 exfoliation of g-C 3 N 4 nanosheets (g-C 3 N 4 NSs) as the substrate followed by a two-step calcination process is essential to achieve ultrahigh metal loading. It was found that the ultrahigh-density of Co single-atom sites were anchored on the g-C 3 N 4 substrate surface and coordinated with two nitrogen and one carbon atoms (Co-N 2 C). These single dispersed Co-N 2 C sites on the g-C 3 N 4 surface were found to act not only as electron gathering centers but also as the sites of CO 2 adsorption and activation, subsequently, boosting the photocatalytic methanol generation during light irradiation. As a result, the methanol formation rate at 4 h (941.9 μmol g −1 ) over Co/g-C 3 N 4 -0.2 SAC with 24.6 wt% surface Co loading was 13.4 and 2.2 times higher than those of g-C 3 N 4 (17.7 μmol g −1 ) and aggregated CoO x /g-C 3 N 4 -0.2 (423.9 μmol g −1 ), respectively. Simultaneously, H 2 (18.9 μmol g −1 h −1 ), CO (2.9 μmol g −1 h −1 ), CH 4 (3.4 μmol g −1 h −1 ), C 2 H 4 (1.1 μmol g −1 h −1 ), C 3 H 6 (1.4 μmol g −1 h −1 ), and CH 3 OCH 3 (3.3 μmol g −1 h −1 ) products were detected over Co/g-C 3 N 4 -0.2 SAC. Besides, the photocatalytic activity of the Co/g-C 3 N 4 -0.2 SAC for the reduction of CO 2 to methanol was stable within 12-cycle experiments (~48 h). This work paves a strategy to boost the photoreduction CO 2 activity via loading ultrahigh surface density single atomically dispersed cobalt active sites. • The two-step calcination process induced bulk cobalt nitrate vaporization to avoid the aggregation of Co atoms during the pyrolysis process. • The g-C 3 N 4 nanosheets as the substrate was proven to afford rich exposed N sites for anchoring single Co atoms. • Formed ultrahigh density Co-N 2 C single dispersed active sites boost the photoreduction CO 2 to methanol by localization of photogenerated electrons.

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Citations by journals

	1 2 3 4 5 6 7 8
Chemical Engineering Journal	Chemical Engineering Journal, 8, 8.79% Chemical Engineering Journal 8 publications, 8.79%
Applied Catalysis B: Environmental	Applied Catalysis B: Environmental, 7, 7.69% Applied Catalysis B: Environmental 7 publications, 7.69%
Small	Small, 4, 4.4% Small 4 publications, 4.4%
Advanced Materials	Advanced Materials, 4, 4.4% Advanced Materials 4 publications, 4.4%
Nano Research	Nano Research, 3, 3.3% Nano Research 3 publications, 3.3%
Journal of Materials Chemistry A	Journal of Materials Chemistry A, 3, 3.3% Journal of Materials Chemistry A 3 publications, 3.3%
ACS Nano	ACS Nano, 2, 2.2% ACS Nano 2 publications, 2.2%
ACS Catalysis	ACS Catalysis, 2, 2.2% ACS Catalysis 2 publications, 2.2%
Small Structures	Small Structures, 2, 2.2% Small Structures 2 publications, 2.2%
Advanced Functional Materials	Advanced Functional Materials, 2, 2.2% Advanced Functional Materials 2 publications, 2.2%
Nanoscale	Nanoscale, 2, 2.2% Nanoscale 2 publications, 2.2%
Green Chemistry	Green Chemistry, 2, 2.2% Green Chemistry 2 publications, 2.2%
ChemPhysChem	ChemPhysChem, 2, 2.2% ChemPhysChem 2 publications, 2.2%
ACS applied materials & interfaces	ACS applied materials & interfaces, 2, 2.2% ACS applied materials & interfaces 2 publications, 2.2%
Advanced Energy Materials	Advanced Energy Materials, 2, 2.2% Advanced Energy Materials 2 publications, 2.2%
Energy Technology	Energy Technology, 2, 2.2% Energy Technology 2 publications, 2.2%
Catalysts	Catalysts, 1, 1.1% Catalysts 1 publication, 1.1%
Transactions of Tianjin University	Transactions of Tianjin University, 1, 1.1% Transactions of Tianjin University 1 publication, 1.1%
iScience	iScience, 1, 1.1% iScience 1 publication, 1.1%
Renewable Energy	Renewable Energy, 1, 1.1% Renewable Energy 1 publication, 1.1%
Current Opinion in Green and Sustainable Chemistry	Current Opinion in Green and Sustainable Chemistry, 1, 1.1% Current Opinion in Green and Sustainable Chemistry 1 publication, 1.1%
Coordination Chemistry Reviews	Coordination Chemistry Reviews, 1, 1.1% Coordination Chemistry Reviews 1 publication, 1.1%
Chemical Physics Letters	Chemical Physics Letters, 1, 1.1% Chemical Physics Letters 1 publication, 1.1%
Ceramics International	Ceramics International, 1, 1.1% Ceramics International 1 publication, 1.1%
Colloids and Surfaces A: Physicochemical and Engineering Aspects	Colloids and Surfaces A: Physicochemical and Engineering Aspects, 1, 1.1% Colloids and Surfaces A: Physicochemical and Engineering Aspects 1 publication, 1.1%
International Journal of Hydrogen Energy	International Journal of Hydrogen Energy, 1, 1.1% International Journal of Hydrogen Energy 1 publication, 1.1%
Progress in Energy and Combustion Science	Progress in Energy and Combustion Science, 1, 1.1% Progress in Energy and Combustion Science 1 publication, 1.1%
Journal of Environmental Chemical Engineering	Journal of Environmental Chemical Engineering, 1, 1.1% Journal of Environmental Chemical Engineering 1 publication, 1.1%
Carbon Energy	Carbon Energy, 1, 1.1% Carbon Energy 1 publication, 1.1%
Energy & Fuels	Energy & Fuels, 1, 1.1% Energy & Fuels 1 publication, 1.1%
	1 2 3 4 5 6 7 8

Citations by publishers

	5 10 15 20 25 30 35
Elsevier	Elsevier, 34, 37.36% Elsevier 34 publications, 37.36%
Wiley	Wiley, 23, 25.27% Wiley 23 publications, 25.27%
American Chemical Society (ACS)	American Chemical Society (ACS), 13, 14.29% American Chemical Society (ACS) 13 publications, 14.29%
Royal Society of Chemistry (RSC)	Royal Society of Chemistry (RSC), 11, 12.09% Royal Society of Chemistry (RSC) 11 publications, 12.09%
Springer Nature	Springer Nature, 5, 5.49% Springer Nature 5 publications, 5.49%
Multidisciplinary Digital Publishing Institute (MDPI)	Multidisciplinary Digital Publishing Institute (MDPI), 1, 1.1% Multidisciplinary Digital Publishing Institute (MDPI) 1 publication, 1.1%
Tianjin Daxue/Tianjin University	Tianjin Daxue/Tianjin University, 1, 1.1% Tianjin Daxue/Tianjin University 1 publication, 1.1%
Hans Publishers	Hans Publishers, 1, 1.1% Hans Publishers 1 publication, 1.1%
Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii	Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii, 1, 1.1% Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii 1 publication, 1.1%
Proceedings of the National Academy of Sciences (PNAS)	Proceedings of the National Academy of Sciences (PNAS), 1, 1.1% Proceedings of the National Academy of Sciences (PNAS) 1 publication, 1.1%
	5 10 15 20 25 30 35

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Ma M. et al. Ultrahigh surface density of Co-N2C single-atom-sites for boosting photocatalytic CO2 reduction to methanol // Applied Catalysis B: Environmental. 2022. Vol. 300. p. 120695.

GOST all authors (up to 50) Copy

Ma M., Huang Z., Doronkin D. E., Fa W., Rao Z., Zou Y., Wang R., Zhong Y., Cao Y., Zhang R., Zhou Y. Ultrahigh surface density of Co-N2C single-atom-sites for boosting photocatalytic CO2 reduction to methanol // Applied Catalysis B: Environmental. 2022. Vol. 300. p. 120695.

RIS |

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RIS Copy

TY - JOUR

DO - 10.1016/j.apcatb.2021.120695

UR - https://doi.org/10.1016/j.apcatb.2021.120695

TI - Ultrahigh surface density of Co-N2C single-atom-sites for boosting photocatalytic CO2 reduction to methanol

T2 - Applied Catalysis B: Environmental

AU - Ma, Minzhi

AU - Huang, Zeai

AU - Rao, Zhiqiang

AU - Zou, Yanzhao

AU - Zhong, Yunqian

AU - Zhang, Ruiyang

AU - Zhou, Ying

AU - Doronkin, Dmitry E.

AU - Fa, Wenjun

AU - Wang, Rui

AU - Cao, Yuehan

PY - 2022

DA - 2022/01/01 00:00:00

PB - Elsevier

SP - 120695

VL - 300

SN - 0926-3373

SN - 1873-3883

ER -

BibTex

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BibTex Copy

@article{2022_Ma,

author = {Minzhi Ma and Zeai Huang and Zhiqiang Rao and Yanzhao Zou and Yunqian Zhong and Ruiyang Zhang and Ying Zhou and Dmitry E. Doronkin and Wenjun Fa and Rui Wang and Yuehan Cao},

title = {Ultrahigh surface density of Co-N2C single-atom-sites for boosting photocatalytic CO2 reduction to methanol},

journal = {Applied Catalysis B: Environmental},

year = {2022},

volume = {300},

publisher = {Elsevier},

month = {jan},

url = {https://doi.org/10.1016/j.apcatb.2021.120695},

pages = {120695},

doi = {10.1016/j.apcatb.2021.120695}

}

Found error?

Publisher

Elsevier

Journal

Applied Catalysis B: Environmental

Quartile SCImago

Quartile WOS

Impact factor

22.1

ISSN

09263373 (Print)
18733883 (Electronic)

Profiles

Zhou, Ying