Sustainable and Highly Reactive Nerve-Agent Simulant Detoxification: Effective Amine Buffers for Metal-Organic Framework Catalysts

被引:13
作者
Seo, Jin Young [2 ,5 ]
Lee, Jung-Hyun [5 ]
Cho, Kie Yong [6 ]
Jeong, Keunhong [1 ]
Baek, Kyung-Youl [1 ,2 ,3 ,4 ]
机构
[1] Korea Mil Acad, Dept Chem, Seoul 01805, South Korea
[2] Korea Inst Sci & Technol, Ctr Mat Architecturing, Seoul 02792, South Korea
[3] Korea Univ Sci & Technol, KIST Sch, Div Nano & Informat Technol, Seoul 02792, South Korea
[4] Kyung Hee Univ, KHU KIST Dept Converging Sci & Technol, Seoul 02447, South Korea
[5] Korea Univ, Dept Chem & Biol Engn, Seoul 02481, South Korea
[6] Pukyong Natl Univ, Dept Ind Chem, Busan 48513, South Korea
基金
新加坡国家研究基金会;
关键词
DESTRUCTION; DEGRADATION; HYDROLYSIS; UIO-66;
D O I
10.1021/acs.chemmater.2c03185
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The appropriate treatment of chemical warfare agents (CWAs) is essential because of their toxicity and lethality. Metal-organic framework (MOF) catalysts, with the assistance of a volatile small molecule buffer, have been reported to be effective for the destruction of CWAs. However, employing small molecular volatile buffers not only contaminates the catalysts and causes them to lose their activity but also prevents their practical application. In this study, we report a novel polymeric buffer that can enhance the catalytic ability of MOFs without contamination of the catalyst. The macromolecular chain can provide non-flowability to buffer, as well as inhibit catalyst contamination by steric hindrance while maintaining activity as a buffer. The optimized polymer buffer [P(MEMA)(43)] can effectively degrade nerve-agent simulants (7.7 min of t(1/2)) in the presence of UiO-66 and preserve its catalytic activity by more than 90% even after three cycles. In addition, the polymeric composite with MOFs coated on a cotton substrate shows excellent detoxification performance in humidified conditions (RH 99%). This fundamental study on a sustainable CWA destruction catalytic system is anticipated to be promising for developing chemical protective textiles against CWAs.
引用
收藏
页码:1624 / 1632
页数:9
相关论文
共 41 条
[1]   Steric hindrance classified: treatment of isothiocyanatoallene with secondary amines bearing bulky substituents to generate 2-aminothiazoles [J].
Banert, Klaus ;
Seifert, Jennifer .
ORGANIC CHEMISTRY FRONTIERS, 2019, 6 (20) :3517-3522
[2]   The Effect of Surface Hydroxylation on MOF Formation on ALD Metal Oxides: MOF-525 on TiO2/Polypropylene for Catalytic Hydrolysis of Chemical Warfare Agent Simulants [J].
Barton, Heather F. ;
Davis, Alexandra K. ;
Parsons, Gregory N. .
ACS APPLIED MATERIALS & INTERFACES, 2020, 12 (13) :14690-14701
[3]   Toward Base Heterogenization: A Zirconium Metal-Organic Framework/Dendrimer or Polymer Mixture for Rapid Hydrolysis of a Nerve-Agent Simulant [J].
Chen, Zhijie ;
Islamoglu, Timur ;
Farha, Omar K. .
ACS APPLIED NANO MATERIALS, 2019, 2 (02) :1005-1008
[4]   Facile control of defect site density and particle size of UiO-66 for enhanced hydrolysis rates: insights into feasibility of Zr(IV)-based metal-organic framework (MOF) catalysts [J].
Cho, Kie Yong ;
Seo, Jin Young ;
Kim, Hyun-Ji ;
Pai, Sung Jin ;
Do, Xuan Huy ;
Yoon, Ho Gyu ;
Hwang, Seung Sang ;
Han, Sang Soo ;
Baek, Kyung-Youl .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2019, 245 :635-647
[5]   Buffer-Induced Acceleration and Inhibition in Polyoxometalate-Catalyzed Organophosphorus Ester Hydrolysis [J].
Collins-Wildman, Daniel L. ;
Kim, Mooeung ;
Sullivan, Kevin P. ;
Plonka, Anna M. ;
Frenkel, Anatoly I. ;
Musaev, Djamaladdin G. ;
Hill, Craig L. .
ACS CATALYSIS, 2018, 8 (08) :7068-7076
[6]   Room-Temperature Synthesis of UiO-66 and Thermal Modulation of Densities of Defect Sites [J].
DeStefano, Matthew R. ;
Islamoglu, Timur ;
Hupp, Joseph T. ;
Farha, Omar K. .
CHEMISTRY OF MATERIALS, 2017, 29 (03) :1357-1361
[7]   A Polyoxoniobate-Polyoxovanadate Double-Anion Catalyst for Simultaneous Oxidative and Hydrolytic Decontamination of Chemical Warfare Agent Simulants [J].
Dong, Jing ;
Hu, Jufang ;
Chi, Yingnan ;
Lin, Zhengguo ;
Zou, Bo ;
Yang, Song ;
Hill, Craig L. ;
Hu, Changwen .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (16) :4473-4477
[8]  
Dwyer D. B., 2018, ACS APPL MATER INTER
[9]   Aqueous Solutions of Poly[2-(N-morpholino)ethyl methacrylate]: Learning about Macromolecular Aggregation Processes from a Peculiar Three-Step Thermoresponsive Behavior [J].
Eggers, Steffen ;
Fischer, Birgit ;
Abetz, Volker .
MACROMOLECULAR CHEMISTRY AND PHYSICS, 2016, 217 (06) :735-747
[10]   Technological advancements for the detection of and protection against biological and chemical warfare agents [J].
Eubanks, Lisa M. ;
Dickerson, Tobin J. ;
Janda, Kim D. .
CHEMICAL SOCIETY REVIEWS, 2007, 36 (03) :458-470