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Mesoporous Core–Shell Nanostructures Bridging Metal and Biocatalyst for Highly Efficient Cascade Reactions
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-01-03 , DOI: 10.1021/acscatal.9b04877
Shiqi Gao 1 , Zihan Wang 1 , Li Ma 1 , Yunting Liu 1 , Jing Gao 1 , Yanjun Jiang 1, 2
Affiliation  

Mesoporous core–shell structured nanocatalysts with a PdPt bimetallic core and enzyme-immobilized polydopamine (PDA) shell were designed, in which the PDA shell worked as a barrier to position the bimetallic core and enzyme in separated locations. The accessible mesoporous structures of both the core and shell significantly facilitate mass transfer and catalyst utilization, improving the synergistic catalytic abilities in cascade reactions. The obtained bifunctional nanocatalysts enabled efficient two-step one-pot cascade reactions of different types: dynamic kinetic resolution of primary amines in organic solvent with high yield and enantioselectivity (up to 99% yield and 98% ee) and degradation of organophosphate nerve agent in aqueous solution with high rate constant and turnover frequency number values (0.8 min–1 and 20 min–1, respectively).

中文翻译:

介孔核-壳纳米结构架桥金属和生物催化剂的高效级联反应

设计了具有PdPt双金属核和固定有酶的聚多巴胺(PDA)壳的介孔核-壳结构纳米催化剂,其中PDA壳用作将双金属核和酶置于分离位置的屏障。核和壳的可及的介孔结构显着促进了传质和催化剂的利用,提高了级联反应中的协同催化能力。所获得的双功能纳米催化剂实现了不同类型的有效的两步式一锅级联反应:伯胺在有机溶剂中的动态动力学拆分,具有高收率和对映选择性(高达99%的收率和98%ee),以及降解有机磷神经毒剂。高速率常数和周转频率数值(0.8分钟–1和20 min –1分别)。
更新日期:2020-01-04
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