Enhanced light harvesting and charge separation of carbon and oxygen co-doped carbon nitride as excellent photocatalyst for hydrogen evolution reaction

Yabin Jiang; Shaofan Fang; Chi Cao; Enna Hong; Lei Zeng; Wensheng Yang; Limin Huang; Chunzhen Yang

doi:10.1016/j.jcis.2021.12.077

Enhanced light harvesting and charge separation of carbon and oxygen co-doped carbon nitride as excellent photocatalyst for hydrogen evolution reaction

J Colloid Interface Sci. 2022 Apr 15:612:367-376. doi: 10.1016/j.jcis.2021.12.077. Epub 2021 Dec 22.

Authors

Yabin Jiang¹, Shaofan Fang², Chi Cao³, Enna Hong⁴, Lei Zeng⁵, Wensheng Yang⁶, Limin Huang⁷, Chunzhen Yang⁸

Affiliations

¹ School of Materials, Sun Yat-Sen University, Shenzhen 518107, PR China; Department of Chemistry, Southern University of Science and Technology, Shenzhen 518055, PR China.
² International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen 518060, PR China.
³ State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, PR China.
⁴ School of Materials, Sun Yat-Sen University, Shenzhen 518107, PR China.
⁵ Department of Chemistry, Southern University of Science and Technology, Shenzhen 518055, PR China. Electronic address: zl0613341@sina.com.
⁶ Institute of Molecular Plus, Tianjin University, Tianjin 300072, PR China.
⁷ Department of Chemistry, Southern University of Science and Technology, Shenzhen 518055, PR China. Electronic address: huanglm@sustech.edu.cn.
⁸ School of Materials, Sun Yat-Sen University, Shenzhen 518107, PR China. Electronic address: yangchzh6@mail.sysu.edu.cn.

PMID: 34998196
DOI: 10.1016/j.jcis.2021.12.077

Abstract

Solar-driven water splitting has been regarded as a promising strategy for renewable hydrogen production. Among many semiconductor photocatalysts, graphitic carbon nitride (g-C₃N₄) has received tremendous attention due to its two-dimensional structure, appropriate band gap and decent photocatalytic activity. However, it suffers severe charge recombination problems, affecting its practical performance. In this work, we demonstrated that dual heteroatoms (C and O) doped g-C₃N₄ can exhibit about 3 times higher catalytic performance for hydrogen evolution than that of the normal g-C₃N₄ with a hydrogen evolution rate reaching 2595.4 umol g^-1h^-1 and an apparent quantum efficiency at 420 nm of 16.6%. The heteroatoms (C and O) doped g-C₃N₄ photocatalyst also exhibited superior removal performance when removing Rhodamine B (RhB) . X-ray photoelectron spectroscopy (XPS), solid-state nuclear magnetic resonance (ssNMR) and X-ray absorption near-edge structure (XANES) spectroscopy reveal that the carbon and oxygen dopants replace the sp² nitrogen and bridging N atom, respectively. DFT calculations demonstrate the codoping of carbon and oxygen- induced the generation of mid-gap state, leading to the improvement of light harvesting and charge separation.

Keywords: C and O co-doped; Carbon nitride; Cyanobenzene; Hydrogen production.