Asymmetrically coordinated cobalt single atom on carbon nitride for highly selective photocatalytic oxidation of CH4 to CH3OH

Jie Ding; Zhenyuan Teng; Xiaozhi Su; Kosaku Kato; Yuhang Liu; Ting Xiao; Wei Liu; Lingyue Liu; Qiao Zhang; Xinyi Ren; Jincheng Zhang; Zhaoyang Chen; Ohno Teruhisa; Akira Yamakata; Hongbin Yang; Yanqiang Huang; Bin Liu; Yueming Zhai

doi:10.1016/j.chempr.2023.02.011

Author(s)

Jie Ding
Zhenyuan Teng
Xiaozhi Su
Kosaku Kato
Yuhang Liu
Ting Xiao
Wei Liu
Lingyue Liu
Qiao Zhang
Xinyi Ren
Jincheng Zhang
Zhaoyang Chen
Ohno Teruhisa
Akira Yamakata
Hongbin Yang
Yanqiang Huang
Yueming Zhai

Related Research Unit(s)

Department of Materials Science and Engineering

Detail(s)

Original language	English
Pages (from-to)	1017-1035
Journal / Publication	Chem
Volume	9
Issue number	4
Online published	13 Mar 2023
Publication status	Published - 13 Apr 2023

Link(s)

DOI	DOI https://doi.org/10.1016/j.chempr.2023.02.011 Final Published version
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Link to Scopus	https://www.scopus.com/record/display.uri?eid=2-s2.0-85151553424&origin=recordpage
Permanent Link	https://scholars.cityu.edu.hk/en/publications/publication(1c2dfa8a-61fe-4a9f-a816-3f97398cda04).html

Abstract

By breaking structural symmetry of the single atomic active site, the photocatalytic water oxidation pathway is tuned for highly selective oxidation of CH₄ to CH₃OH in an aqueous solution. The water oxidation ability and its influence on photocatalytic oxidation of CH₄ over symmetrically coordinated cobalt single atom (Co-4N) on carbon nitride (SC-Co₁/PCN) and asymmetrically coordinated cobalt single atom (Co-C2N2) on carbon nitride (AC-Co₁/PCN_KOH) photocatalysts are systematically investigated. A super selectivity of 87.22% for photocatalytic oxidation of CH₄ to CH₃OH is realized on AC-Co₁/PCN_KOH, which is only 45% on SC-Co₁/PCN. Moreover, a CH₄ conversion of 2.42% and a CH₃OH yield of 2.11% are achieved over AC-Co₁/PCN_KOH (200 mg). Combining multiple in-situ characterizations and time-dependent density functional theory calculations, it is revealed that AC-Co₁/PCN_KOH possesses a desired electronic configuration for single-electron transfer water oxidation reaction during photocatalysis, leading to a notably promoted selectivity for CH₄ oxidation to CH₃OH under illumination. © 2023 Elsevier Inc.

Research Area(s)

asymmetrically coordinated cobalt single atom, one electron transfer, photocatalytic oxidation, SDG7: Affordable and clean energy, water oxidation reaction

SDG 7 - Affordable and Clean Energy

Citation Format(s)

[ RIS ] [ BibTeX ]

Asymmetrically coordinated cobalt single atom on carbon nitride for highly selective photocatalytic oxidation of CH₄ to CH₃OH. / Ding, Jie; Teng, Zhenyuan; Su, Xiaozhi et al.
In: Chem, Vol. 9, No. 4, 13.04.2023, p. 1017-1035.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

Ding, J, Teng, Z, Su, X, Kato, K, Liu, Y, Xiao, T, Liu, W, Liu, L, Zhang, Q, Ren, X, Zhang, J, Chen, Z, Teruhisa, O, Yamakata, A, Yang, H, Huang, Y, Liu, B & Zhai, Y 2023, 'Asymmetrically coordinated cobalt single atom on carbon nitride for highly selective photocatalytic oxidation of CH₄ to CH₃OH', Chem, vol. 9, no. 4, pp. 1017-1035. https://doi.org/10.1016/j.chempr.2023.02.011

Ding, J., Teng, Z., Su, X., Kato, K., Liu, Y., Xiao, T., Liu, W., Liu, L., Zhang, Q., Ren, X., Zhang, J., Chen, Z., Teruhisa, O., Yamakata, A., Yang, H., Huang, Y., Liu, B., & Zhai, Y. (2023). Asymmetrically coordinated cobalt single atom on carbon nitride for highly selective photocatalytic oxidation of CH₄ to CH₃OH. Chem, 9(4), 1017-1035. https://doi.org/10.1016/j.chempr.2023.02.011

Ding J, Teng Z, Su X, Kato K, Liu Y, Xiao T et al. Asymmetrically coordinated cobalt single atom on carbon nitride for highly selective photocatalytic oxidation of CH₄ to CH₃OH. Chem. 2023 Apr 13;9(4):1017-1035. Epub 2023 Mar 13. doi: 10.1016/j.chempr.2023.02.011

Ding, Jie ; Teng, Zhenyuan ; Su, Xiaozhi et al. / Asymmetrically coordinated cobalt single atom on carbon nitride for highly selective photocatalytic oxidation of CH₄ to CH₃OH. In: Chem. 2023 ; Vol. 9, No. 4. pp. 1017-1035.