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Development of oxygen vacancies enriched CoAl hydroxide@hydroxysulfide hollow flowers for peroxymonosulfate activation: A highly efficient singlet oxygen-dominated oxidation process for sulfamethoxazole degradation.
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2020-06-24 , DOI: 10.1016/j.jhazmat.2020.123297
Hanxuan Zeng 1 , Lin Deng 1 , Haojie Zhang 1 , Chan Zhou 1 , Zhou Shi 1
Affiliation  

In this study, oxygen vacancies enriched cobalt aluminum hydroxide@hydroxysulfide (CoAl-LDH@CoSx) hollow flowers was synthesized by in-situ etching of CoAl-LDH using sodium sulfide solution. The analysis of SEM, EDS, XRD, and XPS were used to characterize the samples. The as-synthesized 0.2CoAl-LDH@CoSx displayed higher catalysis performance of sulfamethoxazole (SMX) degradation via the activation of PMS than the pristine CoAl-LDH. 98.5 % of SMX (40 μM) was eliminated with 0.1 g/L 0.2CoAl-LDH@CoSx and 0.3 mM PMS at pH 6.0 in 4 min. The degradation fitted with the pseudo-first-order reaction kinetics well with rate constant of 0.89 min−1 for 0.2CoAl-LDH@CoSx/PMS system and 0.55 min−1 for CoAl-LDH/PMS system. Singlet oxygen (1O2) was verified as dominant reactive oxygen species responsible for SMX degradation via quenching tests. Mechanism investigation suggested that the oxygen vacancies, redox cycles of Co(II)/Co(III) and S22−/(S2− and sulfate species) on the surface of 0.2CoAl-LDH@CoSx were crucial for PMS activation. In addition, the plausible degradation pathways of SMX were proposed by analysis of the SMX degradation intermediates. This study not only reveals that 0.2CoAl-LDH@CoSx is an efficient catalyst to activate PMS for SMX degradation, but also shed a novel insight into development of heterogeneous catalysts with oxygen vacancies.



中文翻译:

富氧空缺的CoAl氢氧化物@羟基硫化物空心花的开发,用于过氧单硫酸盐的活化:一种高效的单线态氧主导的氧化过程,用于磺胺甲恶唑的降解。

在这项研究中,通过硫化钠溶液原位蚀刻CoAl-LDH合成了富氧空位的氢氧化铝氢氧化铝(CoAl-LDH @ CoS x)。SEM,EDS,XRD和XPS的分析用于表征样品。合成后的0.2CoAl-LDH@CoS x与原始CoAl-LDH相比,通过PMS活化显示出更高的磺胺甲恶唑(SMX)降解催化性能。在4分钟内用0.1 g / L 0.2CoAl-LDH@CoS x和0.3 mM PMS去除了98.5%的SMX(40μM)。对于0.2CoAl-LDH@CoS x / PMS系统,降解与拟一级反应动力学拟合得很好,速率常数为0.89 min -1和0.55 min -1用于CoAl-LDH / PMS系统。通过猝灭测试,单重态氧(1 O 2)被证实是造成SMX降解的主要活性氧。机理研究表明,0.2CoAl-LDH @ CoS x表面上的氧空位,Co(II)/ Co(III)和S 2 2- /(S 2-和硫酸盐物种)的氧化还原循环对于PMS活化至关重要。此外,通过对SMX降解中间体的分析,提出了SMX可能的降解途径。这项研究不仅揭示了0.2CoAl-LDH@CoS x是激活PMS降解SMX的有效催化剂,而且为开发具有氧空位的多相催化剂提供了新的见识。

更新日期:2020-06-24
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