Exploration of the synergistic regulatory mechanism of hydroxide and fluoride modification on the photocatalytic activity of 2D g-C3N4

Abstract

Exfoliation and hetero-element doping are common procedures for band gap engineering and enhancing the photocatalytic properties of g-C3N4. A novel and facile strategy for simultaneous exfoliation and hetero-element doping is still in high demand. Herein, we prepared hydroxide and fluoride doped ultrathin g-C3N4 nanosheets through the single-step solvothermal exfoliation of bulk g-C3N4 (BCN) using varying concentrations of ethanol and hydrofluoric acid (HF). The microscopic and spectroscopic analysis confirmed the doping of hydroxide groups and fluoride groups (HO/F groups) into g-C3N4 nanosheets (HF-CNS). The HO groups are primarily located at the terminal amino groups of the heptazine rings in HF-CNS, while the F groups are likely incorporated into the g-C3N4 lattice by forming C–F bonds. The UV-vis absorption spectra and DFT calculations showed that the electronic band structure, and hence charge carrier recombination, can be tuned by varying the HF amount during the exfoliation process. BET-specific surface area was increased from 18.65 m2 g−1 for BCN to 159.87 m2 g−1 for HF-CNS. The transient photocurrent increased from 5 μA to 20 μA. HF-CNS significantly improved the photocatalytic degradation of tetracycline, achieving 99% removal in 50 minutes, compared to 20% for BCN. Tetracycline degradation followed pseudo-first-order kinetics, with apparent rate constants (K) increasing from 0.0028 min−1 for BCN to 0.0793 min−1 for HF-CNS, a 30-fold enhancement. The photocatalytic hydrogen evolution for HF-CNS was 11 times higher than that of BCN. The HF-CNS exhibited remarkable stability and reusability, indicating its potential as a promising photocatalyst for green hydrogen production and degradation of organic pollutants.

Graphical abstract: Exploration of the synergistic regulatory mechanism of hydroxide and fluoride modification on the photocatalytic activity of 2D g-C3N4

Supplementary files

Article information

Article type
Paper
Submitted
08 Aug 2024
Accepted
30 Sep 2024
First published
18 Oct 2024

Catal. Sci. Technol., 2024, Advance Article

Exploration of the synergistic regulatory mechanism of hydroxide and fluoride modification on the photocatalytic activity of 2D g-C3N4

Q. Shang, H. Wang, C. Kan, R. Ding, Y. Li, S. Pandeya, Z. Li and M. K. Joshi, Catal. Sci. Technol., 2024, Advance Article , DOI: 10.1039/D4CY00971A

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