Imperial College London

Emeritus ProfessorNigelGraham

Faculty of EngineeringDepartment of Civil and Environmental Engineering

Senior Research Investigator
 
 
 
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Contact

 

n.graham Website

 
 
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Assistant

 

Miss Judith Barritt +44 (0)20 7594 5967

 
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Location

 

406Skempton BuildingSouth Kensington Campus

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Summary

 

Publications

Citation

BibTex format

@article{Wan:2022:10.1016/j.jhazmat.2022.128223,
author = {Wan, Z and Xu, Z and Sun, Y and Zhang, Q and Hou, D and Gao, B and Khan, E and Graham, NJD and Tsang, DCW},
doi = {10.1016/j.jhazmat.2022.128223},
journal = {Journal of Hazardous Materials},
title = {Stoichiometric carbocatalysis via epoxide-like C-S-O configuration on sulfur-doped biochar for environmental remediation},
url = {http://dx.doi.org/10.1016/j.jhazmat.2022.128223},
volume = {428},
year = {2022}
}

RIS format (EndNote, RefMan)

TY  - JOUR
AB - Heteroatom doping is a promising technique to enhance biochar for effective environmental remediation. However, development of electroactive heteroatom-doped biochars, e.g., sulfur-doped biochar, has been hindered due to complex nature of non-stoichiometric biomass-derived carbon and changeable electrochemical state of dopants. Herein, we produced a series of wood waste-derived biochars with customized levels of minerals and redox-active moieties, aiming to unravel the crucial factors for sulfur doping. Calcium (Ca) in biochar was found to preferentially coordinate with sulfur to form inactive inorganic sulfur minerals (i.e., CaSO4 and CaS) with inferior catalytic reactivity. After diminishing the inherent Ca minerals beforehand, we could introduce surface phenoxyl-type radicals (C-O•) and vacancy defects on the biochar to develop an electrophilic C-S-O bonding configuration, which guaranteed a high affinity towards peroxymonosulfate (PMS, 2.08 mM g-1, 30 min) and efficient removal of bisphenol A (BPA, 91.1%, 30 min). Scavenging experiments and in-situ Raman analyses indicated that the epoxide-like C-S-O structure induced nucleophilic addition of PMS to generate surface-bound singlet oxygen (1O2, major) and hydroxyl radicals (•OH, minor) through a preservative and stoichiometric interfacial reaction. Overall, the proposed approach overcomes the major hurdles in science-informed fabrication of sulfur-doped biochar and advances its development for environmental remediation.
AU - Wan,Z
AU - Xu,Z
AU - Sun,Y
AU - Zhang,Q
AU - Hou,D
AU - Gao,B
AU - Khan,E
AU - Graham,NJD
AU - Tsang,DCW
DO - 10.1016/j.jhazmat.2022.128223
PY - 2022///
SN - 0304-3894
TI - Stoichiometric carbocatalysis via epoxide-like C-S-O configuration on sulfur-doped biochar for environmental remediation
T2 - Journal of Hazardous Materials
UR - http://dx.doi.org/10.1016/j.jhazmat.2022.128223
UR - https://www.ncbi.nlm.nih.gov/pubmed/35063837
UR - http://hdl.handle.net/10044/1/94067
VL - 428
ER -