Guo Yaoping, Huang Yaxiong, Li Yifan, Luo Yan, Xuan Keng, Guo Yadan, Jiang Hao, Fang Rui
School of Water Resources Environmental Engineering, East China University of Technology Nanchang 330013 China
School of Surveying and Mapping and Spatial Information Engineering, East China University of Technology Nanchang 330013 China.
RSC Adv. 2024 Apr 10;14(16):11470-11481. doi: 10.1039/d3ra08958d. eCollection 2024 Apr 3.
Sulfur-doped activated carbon has proved to be a promising metal-free catalyst for persulfate (PDS) catalytic activation for the oxidation of aqueous refractory organics. Herein, sulfur-doped porous carbon (ACS) catalysts with different pore structures and doped-S contents were prepared a template method using d(+)-glucose as the carbon source, sulfur as the sulfur source, and nano-MgO with different particle sizes as templates. Characterization results showed that the particle size of MgO significantly affects the pore structure and doped-S content of ACSs catalysts: a sample synthesized with 20 nm MgO as template (ACS-20) presented the highest content of doped-S and a mesoporous structure, which endowed it with superior adsorption and catalytic performance toward tetracycline (TC) removal. The effect of catalyst dosage, TC concentration, PDS concentration and solution pH on TC removal efficiency were evaluated. The reaction mechanism, investigated by combination of EPR, quenching experiments and LC-MS, indicated that the reactive species included HO·, SO˙, and O, but that O played the dominant role in TC oxidation through a non-radical oxidation pathway. In addition, the reusability and regeneration properties of the ACS-20 catalyst were also studied. This work provides a promising strategy and some theoretical basis for the design and preparation of activated carbon catalysts for advanced oxidation reactions from the viewpoint of pore structure design and S-doping.
硫掺杂活性炭已被证明是一种用于过硫酸盐（PDS）催化活化以氧化水中难降解有机物的有前景的无金属催化剂。在此，以d(+)-葡萄糖为碳源、硫为硫源、不同粒径的纳米MgO为模板，采用模板法制备了具有不同孔结构和硫掺杂量的硫掺杂多孔碳（ACS）催化剂。表征结果表明，MgO的粒径显著影响ACS催化剂的孔结构和硫掺杂量：以20 nm MgO为模板合成的样品（ACS-20）具有最高的硫掺杂量和介孔结构，这使其对四环素（TC）去除具有优异的吸附和催化性能。评估了催化剂用量、TC浓度、PDS浓度和溶液pH对TC去除效率的影响。通过电子顺磁共振（EPR）、猝灭实验和液相色谱-质谱联用（LC-MS）相结合的方法研究反应机理，结果表明活性物种包括羟基自由基（HO·）、硫酸根自由基（SO˙）和单线态氧（O），但单线态氧通过非自由基氧化途径在TC氧化中起主导作用。此外，还研究了ACS-20催化剂 的可重复使用性和再生性能。这项工作从孔结构设计和硫掺杂的角度为高级氧化反应活性炭催化剂的设计和制备提供了一种有前景的策略和一些理论依据。
