Catalytic acH may boost the generation otivation of percarbonate with synthesized carrollite for efficient decomposition of bisphenol S: Performance, degradation mechanism and toxicity assessment.
Catalytic acH may boost the generation otivation of percarbonate with synthesized carrollite for efficient decomposition of bisphenol S: Performance, degradation mechanism and toxicity assessment.
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DOI：
10.1016/j.jhazmat.2023.132719
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发表时间：
2023-10
影响因子：
13.6
通讯作者：
Shicheng Liu;Sitong Liu;Huabin Chen;Yujin Xing;Wenzhong Wang;Lijuan Wang;Yujie Liang;Junli Fu;Chen Zhang
中科院分区：
文献类型：
--
作者：
Shicheng Liu;Sitong Liu;Huabin Chen;Yujin Xing;Wenzhong Wang;Lijuan Wang;Yujie Liang;Junli Fu;Chen Zhang
研究了钙钛矿（CuCo 2S 4）在活化过碳酸钠（SPC）降解双酚S（BPS）中的新应用.考察了BPS浓度、CuCo 2S 4投加量、SPC浓度、反应温度、水基质、无机阴离子和pH值等因素对反应的影响。实验结果表明，CuCo 2S 4活化的SPC体系能有效地降解BPS，在pH= 6.9时降解率为88.52%.通过淬灭实验和电子自旋共振实验揭示了CuCo 2S 4活化的SPC体系降解BPS的机理，发现BPS的降解是由羟基自由基（· OH）、超氧自由基（·O2 −）、单线态氧超氧（1 O2）和碳酸根（· CO 3−）等多种活性氧自由基参与的.此外，S（-II）物种促进了Cu（I）/Cu（II）和Co（II）/Co（III）之间的快速氧化还原循环。CO 3-不仅直接与BPS分子反应，而且作为桥梁促进·O2-和1 O2的生成，从而加速BPS的降解。最后，采用UHPLC/Q-TOF-MS结合密度泛函理论（DFT）方法对BPS降解过程中的主要中间产物进行了分析，并对BPS降解过程中可能的反应途径进行了探讨。该研究为过渡金属硫化物与过碳酸盐的联用去除水中有机污染物提供了一种新的策略。
This study demonstrates the novel application of carrollite (CuCo 2 S 4) for the activation of sodium percarbonate (SPC) towards bisphenol S (BPS) degradation. The effect of several crucial factors like BPS concentration, CuCo 2 S 4 dosage, SPC concentration, reaction temperature, water matrices, inorganic anions, and pH value were investigated. Experimental results demonstrated that BPS could be efficiently degraded by CuCo 2 S 4-activated SPC system (88.52% at pH= 6.9). The mechanism of BPS degradation by CuCo 2 S 4-activated SPC system was uncovered by quenching and electron spin resonance experiments, discovering that a multiple reactive oxygen species process was involved in BPS degradation by hydroxyl radical (• OH), superoxide radical (• O 2−), singlet oxygen superoxide (1 O 2) and carbonate radical (• CO 3−). Furthermore, the S (-II) species facilitated rapid redox cycles between Cu (I)/Cu (II) and Co (II)/Co (III).• CO 3− was found to not only directly react with BPS molecules, but also act as a bridge to promote• O 2− and 1 O 2 generation, thereby accelerating BPS degradation. Finally, the combination of UHPLC/Q-TOF-MS test with density functional theory (DFT) method was employed to detect major degradation intermediates and thereby elucidate possible reaction pathways of BPS degradation. This study provides a novel strategy by integrating transition metal sulfides with percarbonate for the elimination of organic pollutants in water.