Zhou Chuan, Li Li, Qin Haojie, Wu Qiong, Wang Liying, Lin Changxu, Yang Bo, Tao Cheng-An, Zhang Shouxin
State Key Laboratory of NBC Protection for Civilian, Beijing 102205, PR China.
College of Mechanical and Electrical Engineering, Beijing University of Chemical Technology, Beijing 100029, PR China.
ACS Appl Mater Interfaces. 2023 Nov 29;15(47):54582-54589. doi: 10.1021/acsami.3c14297. Epub 2023 Nov 17.
Zirconium-based metal-organic frameworks have emerged as promising materials for detoxifying chemical warfare agents (CWAs) due to their remarkable stability and porosity. However, their practical application is hindered by issues with their powder form and poor catalytic performance in solid-phase degradation. To address these challenges, herein, a granular MOF-808 metal-organic gel (G808) is prepared under optimized conditions for catalytic degradation of the simulant 2-chloroethyl ethyl sulfide (2-CEES), a sulfide blister agent, in a neat state under different humidity conditions. The detoxification performance of G808 toward 2-CEES is significantly enhanced as the content of water present increases. The half-life of 2-CEES decontaminated by G808 can be shortened to 816 s, surpassing those of many other benchmark materials. To confirm the mechanism of catalytic degradation, we used gas chromatography, gas chromatography-mass spectrometry, and theoretical calculations. The findings revealed that hydrolysis was the predominant route. Additionally, granular G808 was reusable and adaptable to high-moisture environments, making it an excellent protective material with practical potential.
基于锆的金属有机框架因其卓越的稳定性和孔隙率,已成为用于解毒化学战剂(CWA)的有前景的材料。然而,其粉末形式的问题以及在固相降解中较差的催化性能阻碍了它们的实际应用。为应对这些挑战,本文在优化条件下制备了颗粒状MOF-808金属有机凝胶(G808),用于在不同湿度条件下对模拟剂2-氯乙基乙基硫醚(2-CEES,一种硫化物起泡剂)进行纯态催化降解。随着含水量的增加,G808对2-CEES的解毒性能显著增强。G808净化的2-CEES的半衰期可缩短至816秒,超过了许多其他基准材料。为确认催化降解的机制,我们使用了气相色谱、气相色谱-质谱联用以及理论计算。研究结果表明水解是主要途径。此外,颗粒状G808可重复使用且适用于高湿度环境,使其成为具有实际潜力的优异防护材料。