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Title: Tuning of Polyoxopalladate Macroanionic Hydration Shell via Countercation Interaction

Three types of macroanion-countercation interactions in dilute solution, decided by the strength of electrostatic attraction and the change of hydration shells are reported: minor interaction between macroanions [MO 8Pd 12(SeO 3) 8] 6- (M = Zn 2+ or Ni 2+) and monovalent cations (Na +, K +, Rb +, Cs +), leaving their hydration shells intact (solvent-separated ion-pairs); strong binding between macroanions and divalent cations (Sr 2+, Ba 2+) to form solvent-shared ion-pairs with partial dehydration; very strong electrostatic attraction between macroanions and Y 3+ ion with contact ion-pairs formation by severely breaking their original hydration shells and forming new ones. Additionally, divalent cations can help the macroanions self-assemble into hollow spherical blackberry structures through counterion-mediated attraction, whereas macroanions with mono- or trivalent cations only stay as discrete ions due to either weak interaction or a small number of bound countercations.
Authors:
 [1] ; ORCiD logo [1] ;  [2] ;  [1] ;  [1] ;  [3] ;  [2] ; ORCiD logo [1]
  1. The Univ. of Akron, Akron, OH (United States)
  2. Jacobs Univ., Bremen (Germany)
  3. Northern Illinois Univ., DeKalb, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Chemistry - A European Journal
Additional Journal Information:
Journal Volume: 24; Journal Issue: 12; Journal ID: ISSN 0947-6539
Publisher:
ChemPubSoc Europe
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
University of Akron; National Science Foundation (NSF); German Research Foundation (DFG); Jacobs University Bremen gGmbH; USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; hydration shell; ion pair; macroion; polypalladate; thermodynamics
OSTI Identifier:
1471520
Alternate Identifier(s):
OSTI ID: 1418418

He, Jiazhi, Li, Hui, Yang, Peng, Haso, Fadi, Wu, Jiayingzi, Li, Tao, Kortz, Ulrich, and Liu, Tianbo. Tuning of Polyoxopalladate Macroanionic Hydration Shell via Countercation Interaction. United States: N. p., Web. doi:10.1002/chem.201705873.
He, Jiazhi, Li, Hui, Yang, Peng, Haso, Fadi, Wu, Jiayingzi, Li, Tao, Kortz, Ulrich, & Liu, Tianbo. Tuning of Polyoxopalladate Macroanionic Hydration Shell via Countercation Interaction. United States. doi:10.1002/chem.201705873.
He, Jiazhi, Li, Hui, Yang, Peng, Haso, Fadi, Wu, Jiayingzi, Li, Tao, Kortz, Ulrich, and Liu, Tianbo. 2017. "Tuning of Polyoxopalladate Macroanionic Hydration Shell via Countercation Interaction". United States. doi:10.1002/chem.201705873.
@article{osti_1471520,
title = {Tuning of Polyoxopalladate Macroanionic Hydration Shell via Countercation Interaction},
author = {He, Jiazhi and Li, Hui and Yang, Peng and Haso, Fadi and Wu, Jiayingzi and Li, Tao and Kortz, Ulrich and Liu, Tianbo},
abstractNote = {Three types of macroanion-countercation interactions in dilute solution, decided by the strength of electrostatic attraction and the change of hydration shells are reported: minor interaction between macroanions [MO8Pd12(SeO3)8]6- (M = Zn2+ or Ni2+) and monovalent cations (Na+, K+, Rb+, Cs+), leaving their hydration shells intact (solvent-separated ion-pairs); strong binding between macroanions and divalent cations (Sr2+, Ba2+) to form solvent-shared ion-pairs with partial dehydration; very strong electrostatic attraction between macroanions and Y3+ ion with contact ion-pairs formation by severely breaking their original hydration shells and forming new ones. Additionally, divalent cations can help the macroanions self-assemble into hollow spherical blackberry structures through counterion-mediated attraction, whereas macroanions with mono- or trivalent cations only stay as discrete ions due to either weak interaction or a small number of bound countercations.},
doi = {10.1002/chem.201705873},
journal = {Chemistry - A European Journal},
number = 12,
volume = 24,
place = {United States},
year = {2017},
month = {12}
}