Micro-nano structured CoS: An efficient catalyst for peroxymonosulfate activation for removal of bisphenol A
Micro-nano structured CoS: An efficient catalyst for peroxymonosulfate activation for removal of bisphenol A
复制标题
微纳结构CoS：过一硫酸盐活化去除双酚A的高效催化剂
DOI：
10.1016/j.seppur.2019.116022
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发表时间：
2020-02-15
影响因子：
8.6
通讯作者：
Huang, Jia
中科院分区：
文献类型：
--
作者：
Ding, Yaobin;Hu, Yue;Huang, Jia
钴基催化剂表现出高性能的活化过一硫酸盐（PMS）。采用简单的溶剂热反应制备了微纳结构的CoS，系统研究了CoS中硫对PMS催化双酚A（BPA）分解的影响。结果表明，微纳结构的CoS在0.05 g L-1CoS和0.3 mmol L-1 PMS的条件下，25 ℃下10 min内对20 mg L-1BPA的去除率可达90%。该体系降解BPA的peso-first反应速率常数为0.37 min（-1），是表面硫改性Co_3O_4（S-Co_3 O_4）和纳米Co_3O_4催化剂的1.1和1.5倍。考察了初始pH（pH 0）、PMS和CoS投加量等因素对BPA降解的影响。随着反应液中双酚A的浓度从3提高到11，由于PMS分解和自由基产生的增加，BPA的去除率也随之提高。此外，通过电子顺磁共振（EPR）分析和淬灭实验，观察到当pH（0）从3变化到10时，SO 4中心点-转化为（OH）-O-中心点作为主要反应物种。根据降解中间产物的LC-MS分析结果，提出了CoS/PMS系统降解BPA的途径。最后，根据XPS谱图分析，提出了CoS活化PMS的可能机理。
Co-based catalysts demonstrated high performance for activating peroxymonosulfate (PMS). In the present study, micro-nano structured CoS was prepared by a simple solvothermal reaction and the influence of sulfur in CoS in the PMS activation for bisphenol A (BPA) decomposition was investigated systematically. It was found that micro-nano structured CoS exhibited remarkable catalytic activity with 90% removal of 20 mg L-1 BPA within 10 min under 0.05 g L-1 CoS and 0.3 mmol L-1 PMS at 25 degrees C. The peso-first reaction rate constant for BPA degradation in this system was 0.37 min(-1) , 1.1 and 1.5 times that by using surface sulfur modified Co3O4 (S-Co3O4) and Co3O4 nanoparticles as a catalyst. Factors influencing BPA degradation were also examined, including initial pH (pH(0)), dosages of PMS and CoS. The BPA removal was enhanced with the raise from 3 to 11 in the reaction solution due to enhanced PMS decomposition and free radicals production. Moreover, the conversion of SO4 center dot- to (OH)-O-center dot as the main reactive species was observed as pH(0) was varied from 3 to 10 through electron paramagnetic resonance (EPR) analysis and quenching experiments. BPA degradation pathways by CoS/PMS system were proposed based on LC-MS results of degradation intermediates. Finally, a possible mechanism for activation of PMS by CoS was proposed according to the surface evolution of CoS during the reaction process by XPS spectra.