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Integrating Two Highly Active Components into One for Decontaminating Sulfur Mustard and Sarin
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2021-09-24 , DOI: 10.1021/acs.iecr.1c02434
Fangsheng Tao 1 , Jialin Yu 1 , Lijuan Zhang 1 , Yunshan Zhou 1 , Yuxu Zhong 2 , Chengcheng Huang 1 , Yong’An Wang 2
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A composite H5PV2Mo10O40@UiO-67(Zr) is synthesized via the one-step in situ encapsulation of Keggin-type H5PV2Mo10O40 (12 Å) polyoxometalate molecules in the octahedral metal–organic framework UiO-67(Zr) (18–23 Å). The effects of H5PV2Mo10O40 content in UiO-67(Zr), reaction time, and decontaminant dosage on the decontamination of sulfur mustard (HD) and nerve agent sarin (GB) were evaluated to determine the optimal conditions. The results showed that the decontamination rates of HD (4 μL) and GB (4 μL) by the composite (40 mg) with 21.52 wt % H5PV2Mo10O40 content under ambient conditions were 95.61% (120 min) and 96.53% (30 min), respectively. The decomposition processes followed first-order reaction kinetics. The half-life and kinetic constant were 33.65 min and 0.0206 min–1 for HD and 8.61 min and 0.08055 min–1 for GB. The oxidation product sulfoxide 2-chloroethyl ethyl sulfoxide and the hydrolysate p-nitrophenol were detected in the decontamination products of the HD simulant 2-chloroethyl ethyl sulfide (CEES) and the GB simulant methyl paraoxon (DMNP), respectively. These results indicated that CEES and HD decontamination followed the catalytic-oxidative mechanism, whereas DMNP and GB decontamination followed the catalytic-hydrolytic mechanism. The composite is a highly active dual-functional heterogeneous catalyst that can perform both the catalytic oxidation of HD by H5PV2Mo10O40 and the catalytic hydrolysis of GB by UiO-67(Zr).

中文翻译:

将两种高活性成分合二为一以净化硫芥和沙林

通过一步原位封装Keggin型H 5 PV 2 Mo 10 O 40 (12 Å)多金属氧酸盐分子在八面体金属中合成了一种复合材料H 5 PV 2 Mo 10 O 40 @UiO-67(Zr)–有机骨架 UiO-67(Zr) (18–23 Å)。H 5 PV 2 Mo 10 O 40 的影响对UiO-67(Zr)的含量、反应时间和去污剂用量对硫芥(HD)和神经毒剂沙林(GB)的去污进行了评估,以确定最佳条件。结果表明,在环境条件下,H 5 PV 2 Mo 10 O 40含量为21.52 wt%的复合材料(40 mg)对HD(4 μL)和GB(4 μL)的去污率为95.61%(120 min)和分别为 96.53%(30 分钟)。分解过程遵循一级反应动力学。半衰期和动力学常数分别为33.65分和0.0206分钟-1 HD和8.61分钟和0.08055分钟-1为GB。氧化产物亚砜2-氯乙基乙基亚砜和水解产物p分别在 HD 模拟物 2-氯乙基乙基硫醚 (CEES) 和 GB 模拟物甲基对氧磷 (DMNP) 的去污产物中检测到 -硝基苯酚。这些结果表明 CEES 和 HD 去污遵循催化氧化机制,而 DMNP 和 GB 去污遵循催化水解机制。该复合材料是一种高活性的双功能多相催化剂,既可以通过 H 5 PV 2 Mo 10 O 40催化氧化 HD,也可以通过 UiO-67(Zr) 催化水解 GB。
更新日期:2021-10-06
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