Electronic and energy level structural engineering of graphitic carbon nitride nanotubes with B and S co-doping for photocatalytic hydrogen evolution

Zhao Mo; Zhihuan Miao; Pengcheng Yan; Peipei Sun; Guanyu Wu; Xingwang Zhu; Cheng Ding; Qiang Zhu; Yucheng Lei; Hui Xu

doi:10.1016/j.jcis.2023.04.123

Electronic and energy level structural engineering of graphitic carbon nitride nanotubes with B and S co-doping for photocatalytic hydrogen evolution

J Colloid Interface Sci. 2023 Sep:645:525-532. doi: 10.1016/j.jcis.2023.04.123. Epub 2023 Apr 27.

Authors

Zhao Mo¹, Zhihuan Miao¹, Pengcheng Yan¹, Peipei Sun¹, Guanyu Wu¹, Xingwang Zhu², Cheng Ding³, Qiang Zhu¹, Yucheng Lei¹, Hui Xu⁴

Affiliations

¹ School of Materials Science & Engineering, Institute for Energy Research, Jiangsu University, Zhenjiang 212013, PR China.
² College of Environmental Science and Engineering, Yangzhou University, Yangzhou, Jiangsu 225009, PR China. Electronic address: zxw@yzu.edu.cn.
³ School of Environmental Science & Engineering, Yancheng Institute of Technology, Yancheng 224051, PR China.
⁴ School of Materials Science & Engineering, Institute for Energy Research, Jiangsu University, Zhenjiang 212013, PR China. Electronic address: xh@ujs.edu.cn.

PMID: 37159994
DOI: 10.1016/j.jcis.2023.04.123

Abstract

The ideal photocatalyst used for photocatalytic water splitting requires strong light absorption, fast charge separation/transfer ability and abundant active sites. Heteroatom doping offers a promising and rational approach to optimize the photocatalytic activity. However, achieving high photocatalytic performance remains challenging if just relying on single-element doping. Herein, Boron (B) and sulfur (S) dopants are simultaneously introduced into graphitic carbon nitride (g-C₃N₄) nanotubes by supramolecular self-assembly strategy. The developed B and S co-doped g-C₃N₄ nanotubes (B,S-TCN) exhibited an outstanding photocatalytic performance in the conversion of H₂O into H₂ (9.321 mmol g^-1h^-1), and the corresponding external quantum efficiency (EQE) reached 5.3% under the irradiation of λ = 420 nm. It is well evidenced by the closely combined experimental and (density functional theory) DFT calculations: (1) the introduction of B dopants can facilitate H₂O adsorption and drive interatomic electron transfer, leading to efficient water splitting reaction. (2) S dopants can stretch the VB position to promote the oxidation ability of g-C₃N₄, which can accelerate the consumption of holes and thus inhibit the recombination with electrons. (3) the simultaneous introduction of B and S can engineer the electronic and energy level structural of g-C₃N₄ for optimizing interior charge transfer. Finally, the purpose of maximizing photocatalytic performance is achieved.

Keywords: Carbon nitride; Heteroatom doping; Hydrogen evolution; Photocatalysis.