Energy Platform for Directed Charge Transfer in the Cascade Z-Scheme Heterojunction: CO2 Photoreduction without a Cocatalyst

Ji Bian; Ziqing Zhang; Jiannan Feng; Madasamy Thangamuthu; Fan Yang; Ling Sun; Zhijun Li; Yang Qu; Dongyan Tang; Zewei Lin; Fuquan Bai; Junwang Tang; Liqiang Jing

doi:10.1002/anie.202106929

Energy Platform for Directed Charge Transfer in the Cascade Z-Scheme Heterojunction: CO₂ Photoreduction without a Cocatalyst

Angew Chem Int Ed Engl. 2021 Sep 13;60(38):20906-20914. doi: 10.1002/anie.202106929. Epub 2021 Aug 13.

Authors

Ji Bian^{1

2}, Ziqing Zhang¹, Jiannan Feng¹, Madasamy Thangamuthu³, Fan Yang¹, Ling Sun¹, Zhijun Li¹, Yang Qu¹, Dongyan Tang², Zewei Lin², Fuquan Bai⁴, Junwang Tang³, Liqiang Jing¹

Affiliations

¹ Department Key Laboratory of Functional Inorganic Materials Chemistry (Ministry of Education), School of Chemistry and Materials Science, International Joint Research Center and Lab for Catalytic Technology, Heilongjiang University, Harbin, 150080, P. R. China.
² School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, P. R. China.
³ Department of Chemical Engineering, University College London, Torrington Place, London, WC1E 7JE, UK.
⁴ International Joint Research Laboratory of Nano-Micro Architecture Chemistry, Institute of Theoretical Chemistry and College of Chemistry, Jilin University, Changchun, 130021, P. R. China.

Abstract

A universal strategy is developed to construct a cascade Z-Scheme system, in which an effective energy platform is the core to direct charge transfer and separation, blocking the unexpected type-II charge transfer pathway. The dimension-matched (001)TiO₂ -g-C₃ N₄ /BiVO₄ nanosheet heterojunction (T-CN/BVNS) is the first such model. The optimized cascade Z-Scheme exhibits ≈19-fold photoactivity improvement for CO₂ reduction to CO in the absence of cocatalysts and costly sacrificial agents under visible-light irradiation, compared with BVNS, which is also superior to other reported Z-Scheme systems even with noble metals as mediators. The experimental results and DFT calculations based on van der Waals structural models on the ultrafast timescale reveal that the introduced T as the platform prolongs the lifetimes of spatially separated electrons and holes and does not compromise their reduction and oxidation potentials.

Keywords: Z-Scheme heterojunctions; charge lifetime; charge modulation; heterojunctions; photocatalysis.

Abstract

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