Isotope and Hydrogen-Bond Effects on the Self-Assembly of Macroions in Dilute Solution

Hui Li; Yidan Shen; Peng Yang; Jennifer E.S. Szymanowski; Jiahui Chen; Yunyi Gao; Peter C. Burns; Ulrich Kortz; Tianbo Liu

doi:10.1002/chem.201902444

Isotope and Hydrogen-Bond Effects on the Self-Assembly of Macroions in Dilute Solution

Hui Li
, Yidan Shen
, Peng Yang
, Jennifer E.S. Szymanowski
, Jiahui Chen
, Yunyi Gao
, Peter C. Burns
, Ulrich Kortz
, Tianbo Liu

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

9 Scopus citations

Abstract

We report on the disparity in the assembly behavior of four types of nano-sized macroions induced by isotopic substitution of protium (H) to deuterium (D) in solvents. Macroions with modest charge density can self-assemble into single-layer, hollow, spherical “blackberry”-type structures, with larger assembly sizes representing stronger attractions among the macroions. Kinetically, all assembly processes become slower in D₂O than in H₂O. Thermodynamically, the polyoxometalate {SrPd₁₂}, the uranium cage {U₆₀} with alkali metal counterions, and the metal–organic cationic cage {Pd₁₂L₂₄} demonstrate similar assembly sizes in both H₂O and D₂O, whereas the metal oxide cluster {Mo₇₂Fe₃₀} as a weak acid shows an unusually large assembly size in H₂O—suggesting a stronger contribution from the hydrogen bonding in the last case.

Original language	English
Pages (from-to)	16288-16293
Number of pages	6
Journal	Chemistry - A European Journal
Volume	25
Issue number	71
DOIs	https://doi.org/10.1002/chem.201902444
State	Published - Dec 18 2019
Externally published	Yes

Funding

T.L. acknowledges support from the National Science foundation NSF (CHE1607138) and the University of Akron. U.K. thanks the German Science Foundation (DFG-KO-2288/20-1 and DFG-KO-2288/16-1), the Jacobs University, and CMST COST Action CM1203 (PoCheMoN) for support. T.L. and P.B. 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 that funded the synthesis and measurements for the uranium clusters. P.Y. sincerely acknowledges CSC (China Scholarship Council) for a doctoral fellowship.

Keywords

hydrogen bonds
isotope effects
macroions
self-assembly
solution behavior

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10.1002/chem.201902444

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title = "Isotope and Hydrogen-Bond Effects on the Self-Assembly of Macroions in Dilute Solution",

abstract = "We report on the disparity in the assembly behavior of four types of nano-sized macroions induced by isotopic substitution of protium (H) to deuterium (D) in solvents. Macroions with modest charge density can self-assemble into single-layer, hollow, spherical “blackberry”-type structures, with larger assembly sizes representing stronger attractions among the macroions. Kinetically, all assembly processes become slower in D2O than in H2O. Thermodynamically, the polyoxometalate \{SrPd12\}, the uranium cage \{U60\} with alkali metal counterions, and the metal–organic cationic cage \{Pd12L24\} demonstrate similar assembly sizes in both H2O and D2O, whereas the metal oxide cluster \{Mo72Fe30\} as a weak acid shows an unusually large assembly size in H2O—suggesting a stronger contribution from the hydrogen bonding in the last case.",

keywords = "hydrogen bonds, isotope effects, macroions, self-assembly, solution behavior",

author = "Hui Li and Yidan Shen and Peng Yang and Szymanowski, \{Jennifer E.S.\} and Jiahui Chen and Yunyi Gao and Burns, \{Peter C.\} and Ulrich Kortz and Tianbo Liu",

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year = "2019",

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doi = "10.1002/chem.201902444",

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AU - Li, Hui

AU - Shen, Yidan

AU - Yang, Peng

AU - Szymanowski, Jennifer E.S.

AU - Chen, Jiahui

AU - Gao, Yunyi

AU - Burns, Peter C.

AU - Kortz, Ulrich

AU - Liu, Tianbo

PY - 2019/12/18

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N2 - We report on the disparity in the assembly behavior of four types of nano-sized macroions induced by isotopic substitution of protium (H) to deuterium (D) in solvents. Macroions with modest charge density can self-assemble into single-layer, hollow, spherical “blackberry”-type structures, with larger assembly sizes representing stronger attractions among the macroions. Kinetically, all assembly processes become slower in D2O than in H2O. Thermodynamically, the polyoxometalate {SrPd12}, the uranium cage {U60} with alkali metal counterions, and the metal–organic cationic cage {Pd12L24} demonstrate similar assembly sizes in both H2O and D2O, whereas the metal oxide cluster {Mo72Fe30} as a weak acid shows an unusually large assembly size in H2O—suggesting a stronger contribution from the hydrogen bonding in the last case.

AB - We report on the disparity in the assembly behavior of four types of nano-sized macroions induced by isotopic substitution of protium (H) to deuterium (D) in solvents. Macroions with modest charge density can self-assemble into single-layer, hollow, spherical “blackberry”-type structures, with larger assembly sizes representing stronger attractions among the macroions. Kinetically, all assembly processes become slower in D2O than in H2O. Thermodynamically, the polyoxometalate {SrPd12}, the uranium cage {U60} with alkali metal counterions, and the metal–organic cationic cage {Pd12L24} demonstrate similar assembly sizes in both H2O and D2O, whereas the metal oxide cluster {Mo72Fe30} as a weak acid shows an unusually large assembly size in H2O—suggesting a stronger contribution from the hydrogen bonding in the last case.

KW - hydrogen bonds

KW - isotope effects

KW - macroions

KW - self-assembly

KW - solution behavior

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M3 - Article

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AN - SCOPUS:85075448695

SN - 0947-6539

VL - 25

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EP - 16293

JO - Chemistry - A European Journal

JF - Chemistry - A European Journal

IS - 71

ER -

Isotope and Hydrogen-Bond Effects on the Self-Assembly of Macroions in Dilute Solution

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Keywords

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