Chen Xi, Li Songrong, Yang Peizhen, Chen Yunfeng, Xue Cheng, Long Yuhan, Han Jiayan, Su Jianming, Huang Wenli, Liu Dongfang
Key Laboratory of Pollution Process and Environmental Criteria, Ministry of Education, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China.
Tianjin Huabo Water Company Limited, Tianjin 300040, China.
J Colloid Interface Sci. 2022 Dec 15;628(Pt A):318-330. doi: 10.1016/j.jcis.2022.07.145. Epub 2022 Jul 28.
Peroxymonosulfate (PMS) heterogeneous catalysis dominated by nonradical pathway showed excellent adaptability for pollutant removal in complex water matrixes. Herein, ultra-small Fe-doped MoS nanosheets with N-doped carbon intercalation (CF-MoS) were synthesized via a one-step hydrothermal method to treat high salinity organic wastewater. CF-MoS exhibited an expanded interlayer spacing by 1.63 times and the specific surface area by 9 times compared with Fe-doped MoS (F-MoS), substantially increasing the active sites. Homogeneous Fe catalytic experiments confirmed that the promotion of carbon intercalated MoS (C-MoS) on Fe/Fe redox cycle was much higher than pure MoS. Besides, the considerable removal of tetracycline (TC) under high salinity conditions (0-7.1%) was attributed to the dominant role of PMS nonradical oxidation pathways, including O and surface-bound radicals. The catalytic sites included Fe/Fe, Mo/Mo/Mo, C=O, pyridine N, pyrrolic N and hydroxyl groups. Finally, density functional theory (DFT) was employed to get the radical electrophilic attack sites and nucleophile attack sites of TC, and the results were consistent with the TC degradation products determined by HPLC-MS. This work would broaden the application of MoS-based catalysts, especially for PMS catalytic removal of organic pollutants from high salinity wastewater.
由非自由基途径主导的过氧单硫酸盐(PMS)多相催化在复杂水基质中对污染物的去除表现出优异的适应性。在此,通过一步水热法合成了具有N掺杂碳插层的超小铁掺杂MoS纳米片(CF-MoS),用于处理高盐度有机废水。与铁掺杂MoS(F-MoS)相比,CF-MoS的层间距扩大了1.63倍,比表面积扩大了9倍,大大增加了活性位点。均相铁催化实验证实,碳插层MoS(C-MoS)对Fe/Fe氧化还原循环的促进作用远高于纯MoS。此外,在高盐度条件下(0-7.1%)对四环素(TC)的显著去除归因于PMS非自由基氧化途径的主导作用,包括O和表面结合自由基。催化位点包括Fe/Fe、Mo/Mo/Mo、C=O、吡啶N、吡咯N和羟基。最后,采用密度泛函理论(DFT)得到TC的自由基亲电攻击位点和亲核攻击位点,结果与HPLC-MS测定的TC降解产物一致。这项工作将拓宽基于MoS的催化剂的应用,特别是用于PMS催化去除高盐度废水中的有机污染物。