Manifestation of Geometric and Electronic Shell Structures of Metal Clusters in Intercluster Reactions

ACS Nano
K R KrishnadasT Pradeep

Abstract

Monolayer protected clusters exhibit rich diversity in geometric and electronic structures. However, structure-reactivity relationships in these clusters are rarely explored. In this context, [Ag44(SR)30]4-, where -SR is an alkyl/aryl thiolate, is an interesting system due to its geometrically and electronically closed-shell structures and distinct charge states. We demonstrate that these structural features of [Ag44(SR)30]4- are distinctly manifested in its solution-state reaction with another cluster, [Au25(SR)18]-. Through this reaction, an alloy cluster anion, [Au12Ag32(SR)30]4-, evolves spontaneously as revealed by high-resolution electrospray ionization mass spectrometry. Ultraviolet-visible absorption spectroscopy and density functional theory calculations indicate that [Au12Ag32(SR)30]4- is formed by the substitution of all of the Ag atoms in the innermost icosahedral shell of [Ag44(SR)30]4- and the abundance is attributed to its higher stability due to closed geometric as well as electronic shell structure, similar to the reactant clusters. We further demonstrate that the substitution of metal atoms in the middle dodecahedral shell and the outermost mount sites are also possible, however such substitutions produce AuxA...Continue Reading

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Citations

Jul 21, 2017·Accounts of Chemical Research·K R KrishnadasThalappil Pradeep
Jun 7, 2018·Nanoscale·Xi KangManzhou Zhu
Aug 18, 2018·Advanced Materials·Qiaofeng YaoJianping Xie
Aug 8, 2020·Chemical Society Reviews·Xi KangRongchao Jin
Nov 12, 2020·Small·Ian D AndersonChristopher J Ackerson
Jan 19, 2021·ACS Omega·Esma Khatun, Thalappil Pradeep
Feb 5, 2021·Nature Communications·Danyu LiuManzhou Zhu
Mar 19, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Yu-Jie ZhongC W Liu
Nov 14, 2020·Small·Mohammad BodiuzzamanThalappil Pradeep
Nov 23, 2017·ACS Nano·Giovanni SalassaThomas Bürgi
Dec 7, 2018·Langmuir : the ACS Journal of Surfaces and Colloids·Kumaranchira Ramankutty KrishnadasThalappil Pradeep
Oct 12, 2018·Journal of the American Chemical Society·Abhijit NagThalappil Pradeep
Nov 27, 2018·Langmuir : the ACS Journal of Surfaces and Colloids·Seyyedamirhossein HosseiniZhihai Li
Dec 13, 2017·The Journal of Physical Chemistry Letters·Evangelina Pensa, Tim Albrecht
Oct 9, 2018·Journal of the American Chemical Society·Yingwei LiRongchao Jin

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