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Sulfur-modified chitosan derived N,S-co-doped carbon as a bifunctional material for adsorption and catalytic degradation sulfamethoxazole by persulfate

过硫酸盐 化学 催化作用 吸附 煅烧 双功能 壳聚糖 硫黄 无机化学 反应速率常数 核化学 有机化学 动力学 量子力学 物理
作者
Kangfeng Pang,Wei Sun,Feng Ye,Lihui Yang,Mengjie Pu,Yang Cao,Qichun Zhang,Junfeng Niu
出处
期刊:Journal of Hazardous Materials [Elsevier BV]
卷期号:424 (Pt A): 127270-127270 被引量:159
标识
DOI:10.1016/j.jhazmat.2021.127270
摘要

N,S-co-doped carbons were synthesized through the calcination of sulfur-modified chitosan for the first time, and utilized as persulfate activators for sulfamethoxazole (SMX) remediation in water. The chitosan and sulfonyl chloride underwent one-step sulfonylation reaction to generate S-modified chitosan. The catalyst NSC-3 showed both excellent adsorption and catalytic oxidation efficiency, corresponding 98.62% removal and 81.34% mineralization rate within 90 min. The rate constant (kobs) was up to 0.0578 min-1, with 75.60-folders higher than that of sulfur-free catalyst NC (7.6580 ×10-4 min-1). The synergy of N and S contributed to the improvement of removal efficiency. The adsorption and oxidation performance were highly depended on the S/N atomic ratio. At the S/N ratio of 0.18, the maximum adsorption and oxidation capability were obtained. The NSC-3/PS system exhibited outstanding adaptability at the wide pH range from 3.07 to 9.28, while the inhibitory effect occurred at strong basic conditions (pH = 11.01). The thiophene sulfur and structural defects were identified as the catalytic sites in activating PS. Both radical and non-radical pathways were responsible for degradation process, where 1O2 played a major role, SO4·-exerted a minor contribution, and O2·- acts as the precursor for the production of 1O2. Another source of 1O2 was assigned to the activation of PS by structure defects. This work indicates that N,S-co-doped carbon at an optimal S/N atomic ratio effectively catalyzes persulfate, and provides an innovative method to construct bifunctional carbon materials of adsorption and oxidization.
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