The urgent need for immediate personal protection against chemical warfare agents(CWAs)spurs the requirement on robust and highly efficient catalytic systems that can be conveniently integrated to wearable devices.Her...The urgent need for immediate personal protection against chemical warfare agents(CWAs)spurs the requirement on robust and highly efficient catalytic systems that can be conveniently integrated to wearable devices.Herein,as a new concept for CWA decontamination catalyst design,sub-nanoscale,catalytically active zirconium-oxo molecular clusters are covalently integrated in flexible polymer network as crosslinkers for the full exposure of catalytic sites as well as robust framework structures.The obtained membrane catalysts exhibit high swelling ratio with aqueous content as 84 wt%and therefore,demonstrate quasi-homogeneous catalytic activity toward the rapid hydrolysis of both CWA,soman(GD)(t_(1/2)=5.0 min)and CWA simulant,methyl paraoxon(DMNP)(t_(1/2)=8.9 min).Meanwhile,due to the covalent nature of cross-linkages and the high flexibility of polymer strands,the membranes possess promising mechanical strength and toughness that can stand the impact of high gas pressures and show high permeation for both CO_(2)and O_(2),enabling their extended applications in the field of collective/personal protective materials with body comfort.展开更多
基金the National Key Research and Development Program of China(No.2018YFB0704200)the Project of State Key Laboratory of NBC Protection for Civilian(No.ZKGSG-ZB-20194334)+1 种基金the National Natural Science Foundation of China(Nos.21961142018 and 51873067)Natural Science Foundation of Guangdong Province(Nos.2021A1515012024 and 2021A1515010271)。
文摘The urgent need for immediate personal protection against chemical warfare agents(CWAs)spurs the requirement on robust and highly efficient catalytic systems that can be conveniently integrated to wearable devices.Herein,as a new concept for CWA decontamination catalyst design,sub-nanoscale,catalytically active zirconium-oxo molecular clusters are covalently integrated in flexible polymer network as crosslinkers for the full exposure of catalytic sites as well as robust framework structures.The obtained membrane catalysts exhibit high swelling ratio with aqueous content as 84 wt%and therefore,demonstrate quasi-homogeneous catalytic activity toward the rapid hydrolysis of both CWA,soman(GD)(t_(1/2)=5.0 min)and CWA simulant,methyl paraoxon(DMNP)(t_(1/2)=8.9 min).Meanwhile,due to the covalent nature of cross-linkages and the high flexibility of polymer strands,the membranes possess promising mechanical strength and toughness that can stand the impact of high gas pressures and show high permeation for both CO_(2)and O_(2),enabling their extended applications in the field of collective/personal protective materials with body comfort.
