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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
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2021-09-20 , DOI: 10.1016/j.jhazmat.2021.127270
Kangfeng Pang 1 , Wei Sun 1 , Feng Ye 1 , Lihui Yang 1 , Mengjie Pu 1 , Cao Yang 1 , Qichun Zhang 2 , Junfeng Niu 1
Affiliation  

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. SO4·- 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.



中文翻译:

硫改性壳聚糖衍生的 N,S 共掺杂碳作为双功能材料用于过硫酸盐吸附和催化降解磺胺甲恶唑

首次通过硫改性壳聚糖的煅烧合成了 N,S 共掺杂碳,并作为过硫酸盐活化剂用于水中磺胺甲恶唑 (SMX) 修复。壳聚糖和磺酰氯经过一步磺酰化反应生成S-修饰壳聚糖。催化剂 NSC-3 表现出优异的吸附和催化氧化效率,在 90 分钟内相应的去除率为 98.62%,矿化率为 81.34%。速率常数(k obs)高达0.0578 min -1,比无硫催化剂NC(7.6580×10 -4 min -1高75.60倍))。N和S的协同作用有助于提高去除效率。吸附和氧化性能高度依赖于 S/N 原子比。在信噪比为 0.18 时,获得了最大的吸附和氧化能力。NSC-3/PS体系在3.07至9.28的宽pH范围内表现出优异的适应性,而抑制作用发生在强碱性条件(pH = 11.01)。噻吩硫和结构缺陷被确定为活化 PS 的催化位点。自由基和非自由基途径都对降解过程负责,其中1 O 2起主要作用,SO 4 ·-起次要作用,O 2 ·-作为产生1 O 2的前体。SO 4 ·- 1 O 2的另一个来源被指定用于通过结构缺陷激活PS。该工作表明,最佳S/N原子比的N,S共掺杂碳可有效催化过硫酸盐,为构建吸附氧化双功能碳材料提供了一种创新方法。

更新日期:2021-09-21
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