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Nitroarene Reduction by a Virus Protein Cage Based Nanoreactor
ACS Catalysis ( IF 11.3 ) Pub Date : 2016-04-14 00:00:00 , DOI: 10.1021/acscatal.6b00106 Aijie Liu 1 , Christoph H.-H. Traulsen 1 , Jeroen J. L. M. Cornelissen 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2016-04-14 00:00:00 , DOI: 10.1021/acscatal.6b00106 Aijie Liu 1 , Christoph H.-H. Traulsen 1 , Jeroen J. L. M. Cornelissen 1
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Gold nanoparticles have recently gained attention as heterogeneous catalysts in a variety of industrially relevant processes. The catalytic activity of the particles is directly related to the available surface area, which increases with decreasing particle size. However, their stability in solution decreases along with the size, and surface modifications have to be carried out to enable efficient catalysis also for elongated reaction times. To prolong catalyst lifetime and to study the substrate selectivity, we encapsulated colloidal gold nanoparticles in cowpea chlorotic mottle virus cages and catalyzed the reduction of nitroarenes with different substituents. The reduction mechanism has been investigated carefully, revealing the reduction sequence nitro → hydroxylamine → amine to take place. The reduction rate is slowed by the introduction of the diffusion barrier imposed by the virus cage, and a nonconventional relation between electronic effects and reduction rate constants is reported that originates from the limited pore sizes and charged exterior/interior of the virus cage. Finally, a significantly increased stability of the hybrid nanoreactors and their recyclability are demonstrated.
中文翻译：
基于病毒蛋白笼的纳米反应器还原亚硝基芳烃
金纳米颗粒作为各种工业相关方法中的非均相催化剂最近受到关注。颗粒的催化活性与有效表面积直接相关，可用表面积随粒径的减小而增加。然而，它们在溶液中的稳定性随着尺寸的增加而降低，并且必须进行表面改性以对于延长的反应时间也能够进行有效的催化。为了延长催化剂寿命并研究底物的选择性，我们将胶体金纳米颗粒封装在cow豆绿斑驳的斑驳病毒笼中，并催化了具有不同取代基的硝基芳烃的还原。仔细研究了还原机理，揭示了还原顺序为硝基→羟胺→胺。通过引入由病毒笼施加的扩散屏障减慢了还原速率，并且据报道，电子效应与还原速率常数之间的非常规关系源于有限的孔径和病毒笼的外部/内部带电。最后，证明了杂化纳米反应器的显着提高的稳定性及其可回收性。
更新日期：2016-04-14
中文翻译：
基于病毒蛋白笼的纳米反应器还原亚硝基芳烃
金纳米颗粒作为各种工业相关方法中的非均相催化剂最近受到关注。颗粒的催化活性与有效表面积直接相关，可用表面积随粒径的减小而增加。然而，它们在溶液中的稳定性随着尺寸的增加而降低，并且必须进行表面改性以对于延长的反应时间也能够进行有效的催化。为了延长催化剂寿命并研究底物的选择性，我们将胶体金纳米颗粒封装在cow豆绿斑驳的斑驳病毒笼中，并催化了具有不同取代基的硝基芳烃的还原。仔细研究了还原机理，揭示了还原顺序为硝基→羟胺→胺。通过引入由病毒笼施加的扩散屏障减慢了还原速率，并且据报道，电子效应与还原速率常数之间的非常规关系源于有限的孔径和病毒笼的外部/内部带电。最后，证明了杂化纳米反应器的显着提高的稳定性及其可回收性。
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