Revealing isoelectronic size conversion dynamics of metal nanoclusters by a noncrystallization approach

Nature Communications
Qiaofeng YaoJianping Xie

Abstract

Atom-by-atom engineering of nanomaterials requires atomic-level knowledge of the size evolution mechanism of nanoparticles, which remains one of the greatest mysteries in nanochemistry. Here we reveal atomic-level dynamics of size evolution reaction of molecular-like nanoparticles, i.e., nanoclusters (NCs) by delicate mass spectrometry (MS) analyses. The model size-conversion reaction is [Au23(SR)16]- → [Au25(SR)18]- (SR = thiolate ligand). We demonstrate that such isoelectronic (valence electron count is 8 in both NCs) size-conversion occurs by a surface-motif-exchange-induced symmetry-breaking core structure transformation mechanism, surfacing as a definitive reaction of [Au23(SR)16]- + 2 [Au2(SR)3]- → [Au25(SR)18]- + 2 [Au(SR)2]-. The detailed tandem MS analyses further suggest the bond susceptibility hierarchies in feed and final Au NCs, shedding mechanistic light on cluster reaction dynamics at atomic level. The MS-based mechanistic approach developed in this study also opens a complementary avenue to X-ray crystallography to reveal size evolution kinetics and dynamics.

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Citations

Aug 18, 2018·Advanced Materials·Qiaofeng YaoJianping Xie
Oct 6, 2018·Angewandte Chemie·Shengli ZhuangZhikun Wu
Jun 19, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Xinyue DouJianping Xie
Jan 4, 2020·Chemical Communications : Chem Comm·Shubo TianJianping Xie
Mar 25, 2020·Nanoscale·Yuichi NegishiTokuhisa Kawawaki
Jun 20, 2020·Chemistry : a European Journal·Ying LvHaizhu Yu
Nov 1, 2020·Nature Communications·Yitao CaoJianping Xie
Mar 19, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Yu-Jie ZhongC W Liu
Apr 17, 2021·The Journal of Chemical Physics·Kiichirou Koyasu, Tatsuya Tsukuda
Jun 25, 2021·Chemical Science·Nan Xia, Zhikun Wu
Nov 11, 2020·Journal of the American Chemical Society·Yingwei LiRongchao Jin
Nov 7, 2018·Accounts of Chemical Research·Belén Nieto-Ortega, Thomas Bürgi
Nov 27, 2018·Langmuir : the ACS Journal of Surfaces and Colloids·Seyyedamirhossein HosseiniZhihai Li
Jun 11, 2020·Journal of the American Chemical Society·Nan XiaZhikun Wu
Oct 15, 2019·Journal of the American Chemical Society·Kaiyuan ZhengJianping Xie
Oct 9, 2018·Journal of the American Chemical Society·Yingwei LiRongchao Jin
Sep 14, 2021·Inorganic Chemistry·Xuejuan ZouManzhou Zhu
Nov 6, 2021·The Journal of Physical Chemistry Letters·Saniya GratiousSukhendu Mandal

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Methods Mentioned

BETA
surface plasmon resonance
X-ray

Software Mentioned

Turbomole

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