MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Yupeng Zhai,Jialin Yu,Lijuan Zhang,Yunshan Zhou,Yuxu Zhong,Ying Yang,Yong’An Wang
In this study, an α-Keggin-type polyoxometalate H 5 PV 2 Mo 10 O 40 was 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 H 5 PV 2 Mo 10 O 40 loading 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 ( t 1/2 ) and kinetic rate constant ( k ) of these two reactions were 27.77 min and −0.02496 min −1 and 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 to p -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.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL RESEARCH
·
2022
·
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
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Materials
·
2021
·Vol. 14
·期 9
·2419
·
IF 3.623
Mingfei Chen,Yingxue Tu,Songhai Wu
There is an urgent need to develop catalytic degradation technologies for chemical warfare agents (CWAs) that are environmentally friendly and do not require secondary treatment. UiO-66-NH2and other metal–organic frameworks (MOFs) based on zirconium have been shown to promote the catalytic degradation of CWAs. At the same time, MOFs have been studied, and they have shown interesting properties in CWA removal because of their ultrahigh surface area, tunable structures, and periodically distributed abundant catalytic sites. However, MOFs synthesized by conventional methods are mostly powdery crystals that are difficult to process and have poor mechanical stability, which largely limit the development of MOFs in practical applications. An emerging trend in MOF research is hybridization with flexible materials. Polymers possess a variety of unique attributes, such as flexibility, thermal and chemical stability, and process ability, and these properties can be combined with MOFs to make a low-cost and versatile material that also provides convenience for the subsequent integration of such MOFs into independent substrates or textiles. In this article, we used a green and simple method to coat the surface of UiO-66-NH2with polydopamine (PDA), PDA can promote the catalytic hydrolysis of UiO-66-NH2to DMNP (a simulant of chemical warfare agents). Additionally, it can adsorb the toxic hydrolysis product p-nitrophenol, avoiding the trouble of secondary treatment. The half-life of UiO-66-NH2coated with polydopamine (UiO-66-NH2@PDA) for catalytic hydrolysis is 8.9 min, and that of pure UiO-66-NH2is 20 min. We speculate that the surface coated with PDA can improve the diffusion of DMNP to the active sites of UiO-66-NH2.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2020
·
IF 4.3
Sanping Zhao,Yongbing Zhu,Hailing Xi,Mengwei Han,Daxue Li,Yang Li,Hongjie Zhao
To overcome the insufficient understanding of the detoxification mechanisms of Chemical Warfare Agents (CWAs) and simulants by a molybdate-activated hydrogen peroxide solution (MoO 4 2− -H 2 O 2 ), detoxification performances toward CWAs and simulants were tested. The detoxification efficacy toward mustard gas (HD), nerve agent GD and VX by using MoO 4 2− -H 2 O 2 was higher than that by using H 2 O 2 activated/modified by sodium hydroxide , ammonia, bicarbonate , and borates, but the vesicant mustard sulfone (HDO 2 ) was only formed when using MoO 4 2− -H 2 O 2 to detoxify HD. Although Reactive Oxygen Species (ROS) such as singlet oxygen ( 1 O 2 ), superoxide anion (O 2 − ), H 2 O 2 and peroxide anion (OOH − ) were detected by electron spin resonance (ESR) and chemiluminescence (CL) in the 0.1 M MoO 4 2− -1.0 M H 2 O 2 solution, 95 Mo NMR indicated that Mo(O 2 ) 4 2− was the dominant oxidant for the oxidation of sulfide to sulfoxide and then to sulfone. Oxidation of HD by Mo(O 2 ) 4 2− occurred on the HD-drop/water interface through a direct oxygen transfer mechanism without the participation of H 2 O molecules, and further oxidation of HD to HDO 2 was inevitable in an aqueous MoO 4 2− -H 2 O 2 solution. 18 O tracer experiments confirmed that OOH − -based perhydrolysis dominated the detoxification reaction of nerve agents in an alkaline H 2 O 2 solution. Considering the balance of oxidation/nucleophilic reactivity for a practical decontaminant, pH 10.5–11 range was recommended as the ideal for the MoO 4 2− -H 2 O 2 system to detoxify CWAs.
研究领域:
化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Fan Liu,Wenbo Li,Junjie Yang,Dongxiao Ji,Yuan Liang,Hengtao Liang,Xiang Li,Pengju Han,Zupei Yuan,Jianxin He,Weili Shao
Highly efficient and reusable protective materials for chemical warfare agents (CWAs) are in high demand. Here, we used a surface modification technique to develop a material that provides chemical protection. Using an electrospun polyacrylonitrile (PAN) nanofiber membrane as the substrate, we modified the surface of the nanofiber with dopamine hydrochloride, which self-polymerized to form a polydopamine (PDA) surface layer, onto which we loaded metal–organic framework (MOF-808) particles. The presence of PDA on the surface of the PAN nanofibers significantly increased the breaking strength (2-fold increase) and elongation (9-fold increase) of the nanofiber membrane. Moreover, the PDA functionalities formed coordination sites to trigger the in situ growth of MOF-808 particles on the surface of the nanofiber membrane, thereby considerably increasing the growth rate and loading capacity. The surface of the nanofiber membrane was completely covered with MOF-808 particles following solvothermal treatment for 16 h. The MOF-808/PAN/PDA composite membrane could rapidly degrade 99.9% of dimethyl-4-nitrophenyl phosphate to p-nitrophenol within 8 min. After the membrane was used several times, the conversion rate stabilized at 95.9%, indicating that the MOF-808/PAN/PDA composite membrane has significant potential for application as protective clothing for CWAs.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Linna Song,Tianyu Zhao,Dongzhi Yang,Xuejiao Wang,Xinmin Hao,Yaxin Liu,Shiyi Zhang,Zhong-Zhen Yu
Lightweight and wearable fabrics with rapid self-detoxification functions are highly desired to resist chemical warfare agents (CWAs). Metal organic frameworks (MOFs) with high specific surface area and customizability are singularly attractive because of their ability to effectively capture and catalytically degrade CWAs. Herein, photothermal graphene-based nanocomposite fabrics are designed by wet-spinning and chemical reduction of graphene oxide fibers followed by in situ growth of UiO-66-NH 2 . The flexible graphene fabrics decorated with UiO-66-NH 2 nanoparticles exhibit an ultrafast photothermal catalytic decontamination of dimethyl 4-nitrophenyl phosphate (DMNP), a typical simulant of CWAs. The half-life of the degradation reaction decreases from 3.4 to 1.6 min under simulated solar light irradiation, a significant gain over the values reported in the literature. Furthermore, DMNP can be degraded in 20 min by the graphene/UiO-66-NH 2 fabric, and even after 5 cycles the degradation efficiency still retains more than 92 %. More importantly, the photothermal conversion of graphene and its instantaneous heat transfer to the UiO-66-NH 2 catalyst effectively accelerate the catalytic reaction kinetics, achieving the fast detoxification of DMNP. The combination of catalytic degradation of MOFs with photothermal conversion effect of graphene makes the lightweight and flexible fabrics promising for protection against CWAs and other pollutants.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY
·
2020
·Vol. 97
·期 1
·1-4
·
IF 2.008
Chen Wenming,Wang Haibo,Guo Xuan,Zhong Jinyi
Self-detoxifying materials for capturing and destructing chemical warfare agents (CWAs) have attracted intense attention in efficient personal protection and safe handling of contaminated materials. In this study, we reported an approach for synthesis of flexible Zr(OH) 4 -carbon fiber composite by sol–gel method. Activated carbon fibers serving as substrate carrier and adsorption conveyor could effectively make Zr(OH) 4 evenly distributed on the surface, which has excellent sorption properties and wide-ranging reactivity toward CWAs. The results demonstrated that the Zr(OH) 4 -carbon fiber composite could quickly remove (within 10 s) and 6-h degradation efficiency to 10-mg/mL sulfur mustard (HD) and O-ethyl S-(2-diisopropylamino)-ethyl methylphosphonothioate (VX) could reach 92.2 and 99.99%. In addition, it was found that Zr(OH) 4 -carbon fiber composite remained intact after adsorption, which could recollect resources and avoid Zr(OH) 4 leakage into waters. Therefore, the designed Zr(OH) 4 -carbon fiber composite will be a good potential application in precision equipment or skin decontamination equipment.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Processes
·
2025
·Vol. 13
·期 4
·973
·
IF 2.8
Saijie Li,Lei Wang,Jiayi Zhang,Yun Liang,Min Tang,Guilong Xu,Chunyu Wang
The decontamination of chemical warfare agents (CWAs) from contaminated surfaces is of critical importance due to the severe threats posed by CWAs to human health and the environment, particularly given the persistent threat of chemical weapons since World War I. In this study, a novel UiO-66-NH2crosslinked hyaluronic acid (HA) hydrogel was developed in the presence of polyvinyl alcohol under ambient conditions, leveraging the dual functionality of the amino-substituted zirconium-based metal–organic framework (Zr-MOF) as both a crosslinker and a catalytic site. The hydrogel demonstrated exceptional catalytic performance, achieving a degradation efficiency of over 90% for the chemical warfare agent simulant dimethyl 4-nitrophenyl phosphate (DMNP) within 1 h. Furthermore, the hydrogel demonstrated adequate mechanical and tensile strength for practical use, enabling easy peel-off from various contaminated surfaces without leaving residues. This peelable property, combined with its decontamination capabilities, highlights its significant potential for practical applications in the field of CWA decontamination.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 56
·35245-35257
·
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
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Nan Jiang,Hongyan Liu,Guodong Zhao,Heyi Li,Shuo Yang,Xianlin Xu,Xupin Zhuang,Bowen Cheng
Protective fabrics containing Zr-Based Metal-Organic Frameworks (Zr-MOFs) show great potential in the detoxification of chemical warfare agents (CWAs). However, the current studies still face the challenges of complicated fabrication processes, limited MOF loading mass, and insufficient protection. Herein, we developed a lightweight, flexible and mechanical robust aerogel by in situ growth of UiO-66-NH 2 onto aramid nanofibers (ANFs) and assembly of UiO-66-NH 2 loaded ANFs (UiO-66-NH 2 @ANFs) into 3D hierarchically porous architecture. The UiO-66-NH 2 @ANF aerogels feature high MOF loading of 261 %, high surface area of 589.349 m 2 g −1 , open and interconnected cellular structure, which provide efficient transfer channels and promote catalytic degradation of CWAs. As a result, the UiO-66-NH 2 @ANF aerogels demonstrate high 2-chloroethyl ethyl thioether (CEES) removal rate at 98.9 % and a short half-life of 8.15 min. Moreover, the aerogels present good mechanical stability (recovery rate of 93.3 % after 100 cycles under 30 % strain), low thermal conductivity (λ of 25.66 mW m −1 K −1 ), high flame resistance (LOI of 32 %) and good wearing comfortableness, indicating promising potential in multifunctional protection against CWAs.
研究领域:
材料科学
·
防护技术
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2020
·Vol. 49
·期 24
·8122-8135
·
IF 4.174
Jialin Yu,Qi Gao,Lijuan Zhang,Yunshan Zhou,Yuxu Zhong,Jianbo Yin,Yuanyuan Zhou,Fangsheng Tao,Yong'an Wang
ε-[Al13O4(OH)24(H2O)12]7+, which shares similarity with the phosphotriesterase active site ZnII–OH–ZnII, was specially chosen to interact with the cluster α-PMo10V2O405− to form a new three-dimensional intercluster, which crystallized in the monoclinic space group P21/m with Z = 2, for the decontamination of chemical warfare agents. The experimental results showed that 50 mg of the compound decontaminated 96.4% (within 120 min) and 99.5% (within 40 min) of sulfur mustard (HD) (4 μL) and soman (GD) (4 μL), respectively, in ambient conditions. The decontamination processes followed first-order reaction kinetics with a rate constant and half-life of 0.01234 min−1 and 56.15 min for HD and 0.1198 min−1 and 5.78 min for GD, respectively. It was concluded that the α-PMo10V2O405− moiety was responsible for the catalytic oxidation of HD into non-toxic sulfoxide, while the ε-[Al13O4(OH)24(H2O)12]7+ moiety was responsible for the catalytic hydrolysis of HD and GD into nontoxic hydrolysates. Besides, the compound showed notable efficacy for the decontamination of HD on guinea pig skin and of GD on Kunming mouse skin, indicating high potential for use in human skin protection and treatment.
研究领域:
化学
·
生物学
·
医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2024
·
IF 6.7
Suhui Wang,Yi Wang,Tengxiao Guo,Shuya Cao
In this work, a long-wave infrared (LWIR) quantum dot (QD) spectrometer was constructed for the first time by integrating a 255-element HgSe QD filter array with an LWIR array detector. The filter array was fabricated using a combination inkjet printing strategy with eight types of T-dodecyl mercaptan-terminated HgSe QD inks. The stability and morphology of the QDs were improved by optimizing the purification methodology and ligand modification. Combined with the compressive-sensing-based least-squares linear regression (CS-LS) algorithm, the LWIR QD spectrometer achieved a spectral resolution of 5.4 cm–1 over a wide spectral range of 8 to 14 μm, enabling the detection of the chemical warfare agent simulant dimethyl methylphosphonate. This technology is expected to facilitate the development of smaller volumes and more accurate identification of various targets in the future. This paper offers an approach to fabricating low-cost LWIR spectrometers and promoting the scale-up applications of QD devices.
研究领域:
光学
·
材料科学
·
光谱学
·
化学传感
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）