Synergetic control of specific orientation and self-distribution of photoelectrons in micro-nano ZnIn2S4/black phosphorus quantum dots (BPQDs) heterojunction to enhance photocatalytic hydrogen evolution

Yanning Qu; Jie Ren; Dongfeng Sun; Yuan Yu

doi:10.1016/j.jcis.2023.03.148

Synergetic control of specific orientation and self-distribution of photoelectrons in micro-nano ZnIn₂S₄/black phosphorus quantum dots (BPQDs) heterojunction to enhance photocatalytic hydrogen evolution

J Colloid Interface Sci. 2023 Jul 15:642:204-215. doi: 10.1016/j.jcis.2023.03.148. Epub 2023 Mar 29.

Authors

Yanning Qu¹, Jie Ren², Dongfeng Sun³, Yuan Yu⁴

Affiliations

¹ The School of Chemistry and Chemical Engineering, Shaanxi University of Science and Technology, Xi'an 710021, China.
² Materials Institute of Atomic and Molecular Science, Shaanxi University of Science and Technology, Xi'an 710021, China; School of Materials Science & Engineering, Shaanxi University of Science and Technology, Xi'an 710021, China.
³ Materials Institute of Atomic and Molecular Science, Shaanxi University of Science and Technology, Xi'an 710021, China.
⁴ Materials Institute of Atomic and Molecular Science, Shaanxi University of Science and Technology, Xi'an 710021, China. Electronic address: yuyuan@sust.edu.cn.

PMID: 37004255
DOI: 10.1016/j.jcis.2023.03.148

Abstract

Black phosphorus quantum dots (BPQDs)-based materials possess excellent photocatalytic efficiency; however, they often present a loss of photo-induced carriers and random active sites in electron transfer of heterojunctions, thus restricting the enhancement of hydrogen (H₂) evolution and their potential application. In this study, a micro-nano ZnIn₂S₄/BPQDs (MN-ZISBP) composite is constructed to enable specific orientation and self-distribution of photoelectrons transferred from ZnIn₂S₄ (ZIS) to BPQDs. The relationship between photoelectron transfer and H₂ evolution efficiency is investigated via experiments and density functional theory (DFT) calculations. MN-ZISBP with a nanorod-like structure presents an H₂ evolution rate of 1207 μmol/g/h and is higher than that of the sheet-shaped (S-ZISBP, 1023 μmol/g/h) and flower-like composites (F-ZISBP, 744 μmol/g/h) under visible light irradiation. The MN-ZISBP composite with a lower conduction band level and larger specific surface area increases the number of active sites on BPQDs via "self-distribution" for H₂ evolution. Finally, the electron transfer direction and bonding orbitals of MN-ZISBP are calculated using the work function and density of states results to verify the above conclusions. The novel construction technique and photocatalytic mechanism of MN-ZISBP reported in this study provide significant insights into the BPQDs-based photocatalysts for H₂ evolution.

Keywords: BPQDs; Micro-nano; Photocatalytic H(2) evolution; Synergetic control; ZnIn(2)S(4).