期刊
CELL REPORTS PHYSICAL SCIENCE
卷 2, 期 10, 页码 -出版社
CELL PRESS
DOI: 10.1016/j.xcrp.2021.100612
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资金
- Defense Threat Reduction Agency [HDTRA1-18-1-0003]
- Northwestern University
- Department of Defense (DoD) through the National Defense Science & Engineering Graduate (NDSEG) Fellowship Program
- Ryan Fellowship
- International Institute for Nanotechnology at Northwestern University
Zirconium-based metal-organic frameworks with tuned micropore environments by functional groups show significant catalytic activity for the degradation of nerve agent simulants. The control of functional group distribution and regulation of the environment across the micropore are important factors in heterogeneous catalysis. Zirconium MOFs with -Br, -CN, -I, and -NH2 functional groups demonstrate rapid degradation of dimethyl 4-nitrophenyl phosphate (DMNP) with catalytic half-lives of less than 3 minutes.
Protection from nerve agents is an important societal challenge requiring effective strategies for rapid degradation of these toxic chemicals. Here, we report a series of zirconium-based metal-organic frameworks (MOFs)-NU-912 and its derivatives-with a 4,8-connected scu topology. We explore their activity toward degradation of a nerve agent simulant, dimethyl 4-nitrophenyl phosphate (DMNP), to illustrate the virtues of controlling functional group distribution and regulating the environment across the micropore in heterogeneous catalysis. The micropore environments of these MOFs tuned by functional groups (-Br, -CN, -I, and -NH2) have significant influence on catalytic activity. NU-912-I, NU-912-CN, and NU-912-NH2 have half-lives (t(1/2)) of less than 3 min using only 3 mol % catalyst loading, which places them among the best zirconium (Zr)-MOF-based heterogeneous catalysts for hydrolysis of DMNP.
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