JOURNAL OF CHEMICAL RESEARCH
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2022
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IF 1.097
Shaoxiong Wu,Lianyuan Wang,Haiyan Zhu,Jing Liang,Liang Ge,Cong Li,Ting Miao,Jian Li,Zhenxing Cheng
Chemical warfare agents, such as nerve agents (GD and VX) and blister agents (HD), have strong toxicities to mankind. In recent years, zirconium-based metal-organic frameworks have been found to be attractive materials for chemical warfare agent degradation. Among them, metal-organic framework-808 (MOF-808) and porous coordination network-222 (PCN-222) were the best. However, few papers pay attention to their practical application. In this work, we prepared MOF-808 and PCN-222 using water phase and organic solvothermal methods, respectively. Their performance for the catalytic degradation of chemical warfare agents under practical decontamination conditions was studied. The results showed that MOF-808 displayed a high potency for catalytic hydrolysis of VX (10,000 mg L−1) in unbuffered solution. PCN-222 exhibited weaker reactivity with a half-life (t1/2) of 28.8 min. Their different performances might stem from the different connectivity of the Zr6 nodes and framework structures. The results illustrated that the hydrolysis of high-concentration GD required a strong alkaline buffer to neutralize the hydrolysis product of hydrofluoric acid (HF) to avoid catalyst poisoning. When H2O2 was used as the oxidant instead of O2, both zirconium-based metal-organic frameworks performed with effective catalytic potency for HD degradation without any special lighting and so was suitable for practical application, whereas the products obtained from HD, such as HDO2 and V-HDO2, still possessed vesicant toxicity. Overall, MOF-808 prepared via a water-phase synthesis performed with effective catalysis for the degradation of high-concentration VX, GD, and HD with t1/2 of < 0.5, 3.1 and 2.2 min, respectively, exhibiting its potential for practical applications.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
RSC Advances
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2021
·Vol. 11
·期 56
·35245-35257
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IF 3.361
Xingqi Huang,Ting Zhao,Hongpeng Zhang,Chunxiao Yan,Jiulong Sha,Huamin Tang,Haiyan Zhu,Yue Wu
Traditional air filter papers can only filter toxic aerosols without the function of decontamination. If the poison stagnating in the paper is desorbed, it may pose a secondary threat to personnel and make it more difficult to dispose of the scrapped paper. Using an alkali-free glass fiber as the base material and zirconium hydroxide as the decontaminant, a self-decontaminating air filter paper that can degrade HD and VX simultaneously was successfully prepared by an intra-pulp addition method, with high filtration efficiency, low pressure drop and moderate tensile strength. The physicochemical properties were characterized by FE-SEM, EDX, XRD and TGA, and the results indicated that Zr(OH)4 was dispersed uniformly in the paper and filled in the interstices of the glass fiber. The preparation of the composite material had no impact on the structure of fibers and Zr(OH)4. The preparation technology of the self-decontaminating air filter paper was optimized. It was found that the paper with a fiber grammage of 50 g m−2, the adhesive of 2% and a Zr(OH)4 retention rate of 175.0 wt% could completely degrade HD and VX, whose conversion rate exceeded 99.0%, and had a tensile strength of 0.1193 kN m−1, a filtration efficiency of 99.995%, and a pressure drop of 313.6 Pa. Using GC-MS to detect the decontamination products, it was speculated that HD mainly underwent hydrolysis and elimination reactions, VX mainly underwent hydrolysis and polymerization reactions, and their products were non-toxic or low-toxic. The reaction kinetics of HD and VX on the paper was investigated and the half-lives were 2.6 h and 16.2 min, respectively, which demonstrated an outstanding degradation performance. This work manifested for the first time that the air filter paper can be optimized as an efficient self-decontaminating material, which will open up new possibilities for the design and manufacture of multifunctional protective materials.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
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2022
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IF 9.988
Yue Gao,Lifeng Yao,Shengzu Zhang,Qinyan Yue,Weiyan Yin
The metal-organic frameworks/cotton fabric composites (MOFs/CFCs) have emerged as a new type of prospective materials for environmental cleanup , due to their convenient recyclability and high removal efficiency towards hazardous pollutants . However, their practical applications are limited by complicated synthetic conditions, insufficient interface bonding and poor adsorption capacity. Herein, for the first time, a robust ethylenediaminetetraacetic acid (EDTA)-functionalized MOFs/CFC is prepared based on UiO-66-NH 2 crystals by using EDTA dianhydride as the cross-linking agent, and applied for simultaneous removal of heavy metals and dyes, as well as degradation of chemical warfare agents. The as-prepared EDTA-UiO-66-NH 2 /CFC shows extraordinary monocomponent adsorption performance with maximum adsorption capacity of 158.7, 126.2, 131.5, 117.4 and 104.5 mg/g for Cd(II), Cu(II), methylene blue , crystal violet and safranin O, respectively. Interestingly, in metal-dyes binary system, the uptake of Cu(II) by EDTA-UiO-66-NH 2 /CFC increases significantly when co-existing high concentration of dyes. The results indicate that the synergistic and simultaneous removal of both dyes and metal from complex systems can be realized by EDTA-UiO-66-NH 2 /CFC via multiple mechanisms. The EDTA-UiO-66-NH 2 /CFC also exhibits an outstanding catalytic performance for degrading dimethyl 4-nitrophenylphosphate. Besides, it can be reused for several times without obvious decrease of its adsorption and catalysis efficiencies. More impressively, the cross-linking reaction approach can not only anchor UiO-66-NH 2 crystals firmly onto cotton fabric, but also facilitate in-situ formation of abundant adsorption sties on the adsorbent surface. Therefore, this work offers a simple and versatile synthetic strategy to develop high-performance environmental material for multiple pollutants remediation.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2019
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IF 3.131
Haibin Li,Li Ma,Liya Zhou,Jing Gao,Zhihong Huang,Ying He,Yanjun Jiang
The combination of metal nanoparticle-catalysts and biocatalysts to perform cascade catalytic strategy is a powerful platform for synthesis or degradation of complex molecules. In this work, an integrated nanoreactor (INR) was successfully prepared via immobilizing organophosphorus hydrolase (OPH) onto porous carbon materials containing Co nanoparticles (C/Co). The C/Co was synthesized conveniently by pyrolysis of a metal-organic framework (MOF) named ZIF-67. This INR can reduce the toxicity of organophosphate nerve agent up to 208-fold by cascade degradation route. In this INR, C/Co not only acts as chemocatalyst but also serves as support for OPH, which allows an easy separation and reuse due to its magnetic properties. Moreover, this INR shows outstanding universal applicability, reusability and stability. With this proof-of-concept, it is foreseeable that the future metal nanoparticles that formed by pyrolyzing MOF will combine more other biocatalysts for perspective applications in more fields.
研究领域:
生物化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
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2012
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IF 4.531
Pingjing Li,Bin Hu,Xiaoyong Li
In this study, a sensitive, selective and reliable analytical method by combining zirconia (ZrO 2 ) coated stir bar sorptive extraction (SBSE) with large volume sample stacking capillary electrophoresis-indirect ultraviolet (LVSS-CE/indirect UV) was developed for the direct analysis of chemical warfare agent degradation products of alkyl alkylphosphonic acids (AAPAs) (including ethyl methylphosphonic acid (EMPA) and pinacolyl methylphosphonate (PMPA)) and methylphosphonic acid (MPA) in environmental waters. ZrO 2 coated stir bar was prepared by adhering nanometer-sized ZrO 2 particles onto the surface of stir bar with commercial PDMS sol as adhesion agent. Due to the high affinity of ZrO 2 to the electronegative phosphonate group, ZrO 2 coated stir bars could selectively extract the strongly polar AAPAs and MPA. After systematically optimizing the extraction conditions of ZrO 2 -SBSE, the analytical performance of ZrO 2 -SBSE-CE/indirect UV and ZrO 2 -SBSE-LVSS-CE/indirect UV was assessed. The limits of detection (LODs, at a signal-to-noise ratio of 3) obtained by ZrO 2 -SBSE-CE/indirect UV were 13.4–15.9 μg/L for PMPA, EMPA and MPA. The relative standard deviations (RSDs, n = 7, c = 200 μg/L) of the corrected peak area for the target analytes were in the range of 6.4–8.8%. Enhancement factors (EFs) in terms of LODs were found to be from 112- to 145-fold. By combining ZrO 2 coating SBSE with LVSS as a dual preconcentration strategy, the EFs were magnified up to 1583-fold, and the LODs of ZrO 2 -SBSE-LVSS-CE/indirect UV were 1.4, 1.2 and 3.1 μg/L for PMPA, EMPA, and MPA, respectively. The RSDs ( n = 7, c = 20 μg/L) were found to be in the range of 9.0–11.8%. The developed ZrO 2 -SBSE-LVSS-CE/indirect UV method has been successfully applied to the analysis of PMPA, EMPA, and MPA in different environmental water samples, and the recoveries for the spiked water samples were found to be in the range of 93.8–105.3%.
研究领域:
分析化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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