Nitrogen-doped biochar as peroxymonosulfate activator to degrade 2,4-dichlorophenol: Preparation, properties and structure-activity relationship

Yang Jingjing; Wang Jinling; Li Hong; Deng Yurong; Yang Chen; Zhao Qing; Dang Zhi

doi:10.1016/j.jhazmat.2021.127743

Nitrogen-doped biochar as peroxymonosulfate activator to degrade 2,4-dichlorophenol: Preparation, properties and structure-activity relationship

J Hazard Mater. 2022 Feb 15;424(Pt D):127743. doi: 10.1016/j.jhazmat.2021.127743. Epub 2021 Nov 19.

Authors

Yang Jingjing¹, Wang Jinling², Li Hong³, Deng Yurong², Yang Chen⁴, Zhao Qing⁵, Dang Zhi⁴

Affiliations

¹ Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and Management, Institute of Eco-environmental and Soil Sciences, Guangdong Academy of Sciences, Guangzhou 510650, China; National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in South China, Guangzhou 510650, China; School of Environment and Energy, South China University of Technology, Guangzhou 510006, China.
² School of Environment and Energy, South China University of Technology, Guangzhou 510006, China.
³ Wenzhou Vocational College of Science and Technology, Wenzhou 325000, China.
⁴ School of Environment and Energy, South China University of Technology, Guangzhou 510006, China; The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, Guangzhou 510006, China.
⁵ Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and Management, Institute of Eco-environmental and Soil Sciences, Guangdong Academy of Sciences, Guangzhou 510650, China; National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in South China, Guangzhou 510650, China; Institute of Applied Ecology, Chinese Academy of Sciences, Shenyang 110016, China. Electronic address: zhaoqing@iae.ac.cn.

PMID: 34863564
DOI: 10.1016/j.jhazmat.2021.127743

Abstract

Nitrogen-doped biochar (NCMs) has shown great potential as metal-free catalysts for persulfates. To understand the evolution law of properties of NCMs with preparation conditions, eleven NCMs were prepared and characterized by EA, BET, Raman, XPS, and conductivity. Surface area and conductivity can be improved by higher pyrolysis temperature and longer retention time. Distribution of nitrogen species of NCMs was greatly influenced by pyrolysis temperature. Subsequently, these NCMs were applied to activate peroxymonosulfate to degrade 2,4-dichlorophenol. A linear correlation of the initial apparent degradation rate constant (k_obs) of 2,4-dichlorophenol with conductivity and ratio of graphitic N was newly established, revealing that conductivity and graphitic N of NCMs would be the key property deciding degradation efficiency of 2,4-dichlorophenol. Positive effect of conductivity can be ascribed to the mediated electron-transfer mechanism. Electron-transfer mechanism is also proved by quenching experiments and solvent deuterium isotope effect experiment. Graphitic N would be the main active site for PMS activation. Understanding the evolvement rule of properties of NCMs with preparation conditions combined with the correlations between reactivity and properties of NCMs is meaningful for preparation of nitrogen-doped biochar as well as the development of carbonaceous materials with high performance in persulfates-based advanced oxidation processes.

Keywords: Correlation; Degradation; Mechanism; Nitrogen-doped biochar; Peroxymonosulfate.

Publication types

Research Support, Non-U.S. Gov't

MeSH terms

Charcoal
Chlorophenols
Nitrogen*
Peroxides*
Structure-Activity Relationship

Substances

Chlorophenols
Peroxides
biochar
Charcoal
peroxymonosulfate
Nitrogen
2,4-dichlorophenol