A bifunctional composite H5PV2Mo10O40@MOF-808(Ce): Preparation, characterization, and performance in the decontamination of chemical warfare agent surrogates CEES and DMNP
A bifunctional composite H5PV2Mo10O40@MOF-808(Ce): Preparation, characterization, and performance in the decontamination of chemical warfare agent surrogates CEES and DMNP
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DOI：
10.1016/j.micromeso.2021.111163
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发表时间：
2021-07
影响因子：
5.2
通讯作者：
Yupeng Zhai;Jialin Yu;Lijuan Zhang;Yunshan Zhou;Yuxu Zhong;Yingli Yang;Yong’an Wang
中科院分区：
文献类型：
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作者：
Yupeng Zhai;Jialin Yu;Lijuan Zhang;Yunshan Zhou;Yuxu Zhong;Yingli Yang;Yong’an Wang
采用浸渍法将α-Keggin型聚氧乙烯酸盐H5 PV 2 Mo 10 O 40负载到MOF-808（Ce）的金刚烷笼（18 μ m）中，制备了不同聚氧乙烯酸盐负载量的复合材料。考察了H5 PV 2 Mo 10 O 40负载量、反应时间、复合材料用量对2-氯乙基乙基硫醚（CEES）去污效果的影响，确定了CEES的最佳催化条件。使用40 mg优化的复合物，120 min内对4 μL CEES的去污率达到93.91%;使用5 mg复合物，25 min内对160 μL神经毒剂替代品甲基对氧磷（DMNP）的去污率达到100%。复合材料对CEES和DMNP的去污符合一级反应动力学。这两个反应的半衰期（t1/2）和动力学速率常数（k）分别为27.77 min和−0.02496 min− 1和1.895 min和−0.36569 min−1。该复合材料在四次重复实验后表现出良好的去污性能。结果表明，该复合物可将CEES氧化为CEESO，DMNP水解为对硝基苯酚和膦酸二甲酯，是一种有效的双功能催化剂，可用于化学战剂替代物的选择性氧化和水解.
In this study, an α-Keggin-type polyoxometalate H5PV2Mo10O40was loaded into the adamantane cage (18 Å) of MOF-808(Ce) by an immersion method to obtain composites with different polyoxometalate loadings. The effects of the H5PV2Mo10O40loading in the composite, the reaction time, and the quantity of the composite during the decontamination of the erosive agent surrogate, 2-chloroethyl ethyl sulfide (CEES) were investigated, and the optimized catalytic conditions for CEES were determined. The decontamination rate of 4 μL CEES reached 93.91% in 120 min using 40 mg of optimized composite, and the decontamination rate of 160 μL of the nerve agent surrogate, methyl paraoxon (DMNP) reached 100% in 25 min using 5 mg of the composite. Decontamination of CEES and DMNP by the composite followed first-order reaction kinetics. The half-life (t1/2) and kinetic rate constant (k) of these two reactions were 27.77 min and −0.02496 min−1and 1.895 min and −0.36569 min−1, respectively. The composite exhibited good decontamination performance after four replicate experiments. The results showed that CEES was oxidized to CEESO, while DMNP was hydrolyzed top-nitrophenol and dimethyl phosphonate in the presence of the composite, showing that the proposed composite is an effective bifunctional catalyst for the selective oxidation and hydrolysis of chemical warfare agent surrogates.