A Spontaneous Structural Transition of {U24Pp12} Clusters Triggered by Alkali Counterion Replacement in Dilute Solution

Yunyi Gao; Mateusz Dembowski; Jennifer E.S. Szymanowski; Wenbin Yin; Steven S.C. Chuang; Peter C. Burns; Tianbo Liu

doi:10.1002/chem.201701972

A Spontaneous Structural Transition of {U₂₄Pp₁₂} Clusters Triggered by Alkali Counterion Replacement in Dilute Solution

Yunyi Gao
, Mateusz Dembowski
, Jennifer E.S. Szymanowski
, Wenbin Yin
, Steven S.C. Chuang
, Peter C. Burns
, Tianbo Liu

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

A transition between two isomeric clusters involving the change of the main skeleton structure of a well-defined, rigid molecular cluster [(UO₂)₂₄(O₂)₂₄(P₂O₇)₁₂]⁴⁸⁻, {U₂₄Pp₁₂}, is achieved by simply introducing proper alkali cations into its dilute aqueous solution. While the unique structural transition can be triggered by introducing any of the Na⁺/K⁺/Rb⁺/Cs⁺ alkali ions, the two isomers, Li/Na-{U₂₄Pp₁₂} and Na/K-{U₂₄Pp₁₂}, as typical macroions, can accurately choose among different alkali counter-cations based on their hydrated sizes, and the ion selectivity process clearly showed endothermic features. The preferred K⁺ and Rb⁺ ions have suitable sizes to be incorporated into the proper windows on {U₂₄Pp₁₂} nanocapsules, as supported by the transition points in both ITC studies and IR measurements.

Original language	English
Pages (from-to)	7915-7919
Number of pages	5
Journal	Chemistry - A European Journal
Volume	23
Issue number	33
DOIs	https://doi.org/10.1002/chem.201701972
State	Published - Jun 12 2017
Externally published	Yes

Funding

We acknowledge support from the Materials Science of Actinides Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001089.

Keywords

actinides
ion selectivity
isomerism
structural transition
uranyl peroxide cluster

Access to Document

10.1002/chem.201701972

Cite this

@article{a128e97d3cc1499c848e43b36520c207,

title = "A Spontaneous Structural Transition of \{U24Pp12\} Clusters Triggered by Alkali Counterion Replacement in Dilute Solution",

abstract = "A transition between two isomeric clusters involving the change of the main skeleton structure of a well-defined, rigid molecular cluster [(UO2)24(O2)24(P2O7)12]48−, \{U24Pp12\}, is achieved by simply introducing proper alkali cations into its dilute aqueous solution. While the unique structural transition can be triggered by introducing any of the Na+/K+/Rb+/Cs+ alkali ions, the two isomers, Li/Na-\{U24Pp12\} and Na/K-\{U24Pp12\}, as typical macroions, can accurately choose among different alkali counter-cations based on their hydrated sizes, and the ion selectivity process clearly showed endothermic features. The preferred K+ and Rb+ ions have suitable sizes to be incorporated into the proper windows on \{U24Pp12\} nanocapsules, as supported by the transition points in both ITC studies and IR measurements.",

keywords = "actinides, ion selectivity, isomerism, structural transition, uranyl peroxide cluster",

author = "Yunyi Gao and Mateusz Dembowski and Szymanowski, \{Jennifer E.S.\} and Wenbin Yin and Chuang, \{Steven S.C.\} and Burns, \{Peter C.\} and Tianbo Liu",

note = "Publisher Copyright: {\textcopyright} 2017 Wiley-VCH Verlag GmbH \& Co. KGaA, Weinheim",

year = "2017",

month = jun,

day = "12",

doi = "10.1002/chem.201701972",

language = "English",

volume = "23",

pages = "7915--7919",

journal = "Chemistry - A European Journal",

issn = "0947-6539",

publisher = "wiley",

number = "33",

}

TY - JOUR

T1 - A Spontaneous Structural Transition of {U24Pp12} Clusters Triggered by Alkali Counterion Replacement in Dilute Solution

AU - Gao, Yunyi

AU - Dembowski, Mateusz

AU - Szymanowski, Jennifer E.S.

AU - Yin, Wenbin

AU - Chuang, Steven S.C.

AU - Burns, Peter C.

AU - Liu, Tianbo

PY - 2017/6/12

Y1 - 2017/6/12

N2 - A transition between two isomeric clusters involving the change of the main skeleton structure of a well-defined, rigid molecular cluster [(UO2)24(O2)24(P2O7)12]48−, {U24Pp12}, is achieved by simply introducing proper alkali cations into its dilute aqueous solution. While the unique structural transition can be triggered by introducing any of the Na+/K+/Rb+/Cs+ alkali ions, the two isomers, Li/Na-{U24Pp12} and Na/K-{U24Pp12}, as typical macroions, can accurately choose among different alkali counter-cations based on their hydrated sizes, and the ion selectivity process clearly showed endothermic features. The preferred K+ and Rb+ ions have suitable sizes to be incorporated into the proper windows on {U24Pp12} nanocapsules, as supported by the transition points in both ITC studies and IR measurements.

AB - A transition between two isomeric clusters involving the change of the main skeleton structure of a well-defined, rigid molecular cluster [(UO2)24(O2)24(P2O7)12]48−, {U24Pp12}, is achieved by simply introducing proper alkali cations into its dilute aqueous solution. While the unique structural transition can be triggered by introducing any of the Na+/K+/Rb+/Cs+ alkali ions, the two isomers, Li/Na-{U24Pp12} and Na/K-{U24Pp12}, as typical macroions, can accurately choose among different alkali counter-cations based on their hydrated sizes, and the ion selectivity process clearly showed endothermic features. The preferred K+ and Rb+ ions have suitable sizes to be incorporated into the proper windows on {U24Pp12} nanocapsules, as supported by the transition points in both ITC studies and IR measurements.

KW - actinides

KW - ion selectivity

KW - isomerism

KW - structural transition

KW - uranyl peroxide cluster

UR - https://www.scopus.com/pages/publications/85020684830

U2 - 10.1002/chem.201701972

DO - 10.1002/chem.201701972

M3 - Article

C2 - 28477394

AN - SCOPUS:85020684830

SN - 0947-6539

VL - 23

SP - 7915

EP - 7919

JO - Chemistry - A European Journal

JF - Chemistry - A European Journal

IS - 33

ER -