Chinese Chemical Letters ( IF 9.4 ) Pub Date : 2022-08-19 , DOI: 10.1016/j.cclet.2022.107755 Feng Ye , Wei Sun , Kangfeng Pang , Wenchao Yang , Mengjie Pu , Qichun Zhang
Carbon-mediated persulfate advanced oxidation processes (PS-AOPs) are appealing in contaminant remediation. For the first time, S,B-co-doped carbon-based persulfate activators were synthesized through direct carbonization of sodium lignosulfonate and boric acid. By degrading sulfamethoxazole (SMX), CSB-750 obtained 98.7% removal and 81.4% mineralization within 30 min. In comparison with solo S or B doping, S and B co-doped carbon showed the coupling effect for enhanced catalysis. The rate constant (kobs) of 0.1679 min–1 was 22.38- and 279.83-fold higher than those of CS-750 (0.0075 min–1) and CB-750 (0.0006 min–1), respectively. The degradation was efficient at strong acidic and weak basic conditions (pH 3–9). Substantial inhibition effect was presented at strong basic condition (pH 10.95) and in presence of CO32–. The CO32–-caused inhibition was the combined result of the cooperation of pH and quenching O2·–. Thiophene sulfur, BC3, BC2O, and structural defects were identified as the active sites for PS activation. Radical and nonradical pathways were both involved in the CSB-750/PS/SMX system, where 1O2 dominated the degradation, SO4·–, ·OH and direct electron transfer played the subordinate role, and O2·– served as a precursor for the formation of partial 1O2. The toxicity of degradation system, the effect of real water matrix, and the reusability of carbocatalysts were comprehensively analyzed. Nine possible degradation pathways were proposed. This work focuses on the catalytic performance improvement through the coupling effect of S,B co-doping, and develops an advanced heteroatom doping system to fabricate carbonaceous persulfate activators.
中文翻译:
碳质材料中硫和硼的偶联以增强抗生素降解的过硫酸盐活化:活性位点、机理和毒性评估
碳介导的过硫酸盐高级氧化工艺 (PS-AOP) 在污染物修复中很有吸引力。首次通过木质素磺酸钠和硼酸直接碳化合成了S,B共掺杂碳基过硫酸盐活化剂。通过降解磺胺甲恶唑 (SMX),CSB-750 在 30 分钟内获得了 98.7% 的去除率和 81.4% 的矿化率。与单独的 S 或 B 掺杂相比,S 和 B 共掺杂碳显示出增强催化的偶联效应。0.1679 min –1的速率常数 ( k obs )比 CS-750 (0.0075 min –1 ) 和 CB-750 (0.0006 min –1 ) 高 22.38 倍和 279.83 倍), 分别。降解在强酸性和弱碱性条件下 (pH 3–9) 是有效的。在强碱性条件下(pH 10.95)和CO 3 2-存在时表现出明显的抑制作用。CO 3 2–引起的抑制是pH值和猝灭O 2 ·–共同作用的结果。噻吩硫、BC 3、BC 2 O和结构缺陷被确定为PS活化的活性位点。CSB-750/PS/SMX 系统中均涉及自由基和非自由基途径,其中1 O 2主导降解,SO 4 ·– , ·OH和直接电子转移起次要作用,O 2 ·–是部分1 O 2形成的前体。综合分析了降解体系的毒性、真实水基质的影响以及碳催化剂的可重复使用性。提出了九种可能的降解途径。本工作着重于通过 S,B 共掺杂的耦合效应提高催化性能,并开发了一种先进的杂原子掺杂体系来制备碳质过硫酸盐活化剂。