Issue 12, 2023

Metal-free amorphous carbon nitride with N-vacancies for efficient photocatalytic decontamination: a case of peroxydisulfate-based nonradical oxidation mechanism

Abstract

Peroxydisulfate-based nonradical oxidation processes (PDS-NOPs) are appealing for wastewater purification due to their high efficiency and environmental friendliness. Herein, we design and synthesize metal-free amorphous carbon nitride (ACN) with N3C-site vacancies for the photoactivation of PDS to eliminate pharmaceuticals and personal care products in wastewater. Integrated with electron paramagnetic resonance and radical scavenging tests, the nature of the nonradical pathways in PDS activation is unveiled to be an electron-transfer regime. The in situ Raman spectrum analysis and electrochemical test show that PDS molecules combine with positively charged nitrogen vacancies to form a metastable complex (i.e., ACN–PDS*) with high chemical potential. Then, the complex selectively extracts electrons from coexisting organic pollutants to trigger the oxidation reaction. In addition, the introduction of nitrogen vacancies not only enhances the surface affinity between the catalyst and PDS but also accelerates the transfer efficiency of photoinduced electrons. As a result, the ACN/PDS system shows high photocatalytic degradation efficiency of diclofenac (DCF) in the pH range of 4 to 10 with degradation rate constants in the range of 0.18 to 0.21 min−1. In a variety of practical aqueous matrices, DCF can be entirely removed within 5 minutes when exposed to sunlight. Toxicity evaluation experiments show that the toxicity of DCF could be efficiently removed in the can/PDS system.

Graphical abstract: Metal-free amorphous carbon nitride with N-vacancies for efficient photocatalytic decontamination: a case of peroxydisulfate-based nonradical oxidation mechanism

Supplementary files

Article information

Article type
Paper
Submitted
05 ספט 2023
Accepted
03 נוב 2023
First published
03 נוב 2023

Environ. Sci.: Nano, 2023,10, 3450-3461

Metal-free amorphous carbon nitride with N-vacancies for efficient photocatalytic decontamination: a case of peroxydisulfate-based nonradical oxidation mechanism

D. Wei, Y. Wang, L. Wu, D. Liu, Z. Fang, P. Chen, H. Liu, W. Lv and G. Liu, Environ. Sci.: Nano, 2023, 10, 3450 DOI: 10.1039/D3EN00614J

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements