Thiol-Stabilized Atomically Precise, Superatomic Silver Nanoparticles for Catalyzing Cycloisomerization of Alkynyl Amines
Yan, J., Zhang, J., Chen, X., Malola, S., Zhou, B., Selenius, E., Zhang, X., Yuan, P., Deng, G., Liu, K., Su, H., Teo, B. K., Häkkinen, H., Zheng, L., & Zheng, N. (2018). Thiol-Stabilized Atomically Precise, Superatomic Silver Nanoparticles for Catalyzing Cycloisomerization of Alkynyl Amines. National Science Review, 5(5), 694-702. https://doi.org/10.1093/nsr/nwy034
Published inNational Science Review
Zhou, Bo |
© The Authors, 2018. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd.
Both the electronic and surface structures of metal nanomaterials play critical roles in determining their chemical properties. However, the non-molecular nature of conventional nanoparticles makes it extremely challenging to understand the molecular mechanism behind many of their unique electronic and surface properties. In this work, we report the synthesis, molecular and electronic structures of an atomically precise nanoparticle, [Ag206L72]q (L = thiolate, halide; q = charge). With a four-shell Ag7@Ag32@Ag77@Ag90 Ino-decahedral structure having a nearly perfect D5h symmetry, the metal core of the nanoparticle is co-stabilized by 68 thiolate and 4 halide ligands. Both electrochemistry and plasmonic absorption reveal the metallic nature of the nanoparticles, which is explained by density functional theory calculations. Electronically, the nanoparticle can be considered as a superatom, just short of a major electron shell closing of 138 electrons (q = –4). More importantly, many of ligands capping on the nanoparticle are labile due to their low-coordination modes, leading to high surface reactivity for catalysing the synthesis of indoles from 2-ethynylaniline derivatives. The results exemplify the power of the atomic-precision nanocluster approach to catalysis in probing reaction mechanisms and in revealing the interplay of heterogeneous reactivities, electronic and surface structural dynamics, thereby providing ways for optimization. ...
PublisherOxford University Press on behalf of China Science Publishing & Media Ltd
ISSN Search the Publication Forum2095-5138
Publication in research information system
MetadataShow full item record
Related funder(s)Academy of Finland
Funding program(s)Academy Project, AoF
Additional information about fundingWe thank the National Key R&D Program of China (2017YFA0207302) and the National Natural Science Foundation of China (21731005, 21420102001, 21333008, 21390390) for financial support. The financial support from iChEM, Xiamen University (to B.T.) and from National Innovation and Intelligence Introduction Base Program (to H.H.) is gratefully acknowledged. The work in the University of Jyväskylä was supported by the Academy of Finland (266492 and Academy Professorship to H.H.). ...
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