Chen Yu-Zhen, Gu Bingchuan, Uchida Takeyuki, Liu Jiandang, Liu Xianchun, Ye Bang-Jiao, Xu Qiang, Jiang Hai-Long
Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Soft Matter Chemistry, Department of Chemistry, Collaborative Innovation Center of Suzhou Nano Science and Technology, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
College of Chemistry and Chemical Engineering, Qingdao University, Qingdao, Shandong, 266071, P. R. China.
Nat Commun. 2019 Aug 1;10(1):3462. doi: 10.1038/s41467-019-11449-6.
Metal nanoparticles (NPs) stabilized by metal-organic frameworks (MOFs) have been intensively studied in recent decades, while investigations on the location of guest metal NPs relative to host MOF particles remain challenging and very rare. In this work, we have developed several characterization techniques, including high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) tomography, hyperpolarized Xe NMR spectroscopy and positron annihilation spectroscopy (PAS), which are able to determine the specific location of metal NPs relative to the MOF particle. The fine PdCu NPs confined inside MIL-101 exhibit excellent catalytic activity, absolute selectivity and satisfied recyclability in the aerobic oxidation of benzyl alcohol in pure water. As far as we know, the determination for the location of metal NPs relative to MOF particles and pore structure information of metal NPs/MOF composites by Xe NMR and PAS techniques has not yet been reported.
近几十年来，金属有机框架（MOF）稳定的金属纳米颗粒（NPs）受到了广泛研究，然而，关于客体金属NP相对于主体MOF颗粒的位置的研究仍然具有挑战性且非常罕见。在这项工作中，我们开发了几种表征技术，包括高角度环形暗场扫描透射电子显微镜（HAADF-STEM）断层扫描、超极化Xe核磁共振光谱和正电子湮没光谱（PAS），这些技术能够确定金属NP相对于MOF颗粒的具体位置。限制在MIL-101内部的精细PdCu NPs在纯水中苯甲醇的有氧氧化中表现出优异的催化活性、绝对选择性和良好的可回收性。据我们所知，尚未有通过Xe NMR和PAS技术确定金属NP相对于MOF颗粒的位置以及金属NP/MOF复合材料的孔结构信息的报道。
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