Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Elucidating the origin of the attractive force among hydrophilic macroions

Abstract

In this study, coarse-grained simulation approach is applied to provide a general understanding of various soluble, hydrophilic macroionic solutions, especially the strong attractions among the like-charged soluble macroions and the consequent spontaneous, reversible formation of blackberry structures with tunable sizes. This model captures essential molecular details of the macroions and their interactions in polar solvents. Results using this model provide consistent conclusions to the experimental observations, from the nature of the attractive force among macroions (counterion-mediated attraction), to the blackberry formation mechanism. The conclusions can be applied to various macroionic solutions from inorganic molecular clusters to dendrimers and biomacromolecules.

Authors:
 [1];  [1];  [1]
+ Show Author Affiliations
  1. Univ. of Akron, Akron, OH (United States). Dept. of Polymer Science
Publication Date:
Research Org.:
Univ. of Akron, Akron, OH (United States); Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1282008
Grant/Contract Number:  
SC0001089
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; molecular-dynamics simulations; aqueous-solution; dilute-solutions; keggin anions; counterions; nanostructures; macroanions; transition; vesicles; clusters

Citation Formats

Liu, Zhuonan, Liu, Tianbo, and Tsige, Mesfin. Elucidating the origin of the attractive force among hydrophilic macroions. United States: N. p., 2016. Web. doi:10.1038/srep26595.
Copy to clipboard
Liu, Zhuonan, Liu, Tianbo, & Tsige, Mesfin. Elucidating the origin of the attractive force among hydrophilic macroions. United States. https://doi.org/10.1038/srep26595
Copy to clipboard
Liu, Zhuonan, Liu, Tianbo, and Tsige, Mesfin. Tue . "Elucidating the origin of the attractive force among hydrophilic macroions". United States. https://doi.org/10.1038/srep26595. https://www.osti.gov/servlets/purl/1282008.
Copy to clipboard
@article{osti_1282008,
title = {Elucidating the origin of the attractive force among hydrophilic macroions},
author = {Liu, Zhuonan and Liu, Tianbo and Tsige, Mesfin},
abstractNote = {In this study, coarse-grained simulation approach is applied to provide a general understanding of various soluble, hydrophilic macroionic solutions, especially the strong attractions among the like-charged soluble macroions and the consequent spontaneous, reversible formation of blackberry structures with tunable sizes. This model captures essential molecular details of the macroions and their interactions in polar solvents. Results using this model provide consistent conclusions to the experimental observations, from the nature of the attractive force among macroions (counterion-mediated attraction), to the blackberry formation mechanism. The conclusions can be applied to various macroionic solutions from inorganic molecular clusters to dendrimers and biomacromolecules.},
doi = {10.1038/srep26595},
journal = {Scientific Reports},
number = ,
volume = 6,
place = {United States},
year = {Tue May 24 00:00:00 EDT 2016},
month = {Tue May 24 00:00:00 EDT 2016}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/srep26595
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 42 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Self-assembly in aqueous solution of wheel-shaped Mo154 oxide clusters into vesicles
journal, November 2003

  • Liu, Tianbo; Diemann, Ekkehard; Li, Huilin
  • Nature, Vol. 426, Issue 6962
  • DOI: 10.1038/nature02036

Polyoxometalates in Solution:  Molecular Dynamics Simulations on the α-PW 12 O 40 3- Keggin Anion in Aqueous Media
journal, February 2005

  • López, Xavier; Nieto-Draghi, Carlos; Bo, Carles
  • The Journal of Physical Chemistry A, Vol. 109, Issue 6
  • DOI: 10.1021/jp046862u

Sheet-like assemblies of spherical particles with point-symmetrical patches
journal, April 2012

  • Mani, Ethayaraja; Sanz, Eduardo; Roy, Soumyajit
  • The Journal of Chemical Physics, Vol. 136, Issue 14
  • DOI: 10.1063/1.3702203

Lag Periods During the Self-Assembly of {Mo 72 Fe 30 } Macroions: Connection to the Virus Capsid Formation Process
journal, October 2009

  • Zhang, Jie; Li, Dong; Liu, Guang
  • Journal of the American Chemical Society, Vol. 131, Issue 42
  • DOI: 10.1021/ja903548m

Self-Assembly of Discrete Cyclic Nanostructures Mediated by Transition Metals
journal, March 2000

  • Leininger, Stefan; Olenyuk, Bogdan; Stang, Peter J.
  • Chemical Reviews, Vol. 100, Issue 3
  • DOI: 10.1021/cr9601324

Polyoxometalates in Solution:  Molecular Dynamics Simulations on the α-PW 12 O 40 3- Keggin Anion in Aqueous Media
journal, February 2005

  • López, Xavier; Nieto-Draghi, Carlos; Bo, Carles
  • The Journal of Physical Chemistry A, Vol. 109, Issue 6
  • DOI: 10.1021/jp046862u

Molecular Structure Encodes Nanoscale Assemblies: Understanding Driving Forces in Electrostatic Self-Assembly
journal, December 2011

  • Willerich, Immanuel; Gröhn, Franziska
  • Journal of the American Chemical Society, Vol. 133, Issue 50
  • DOI: 10.1021/ja207565m

Spontaneous Self-Assembly of γ-Cyclodextrins in Dilute Solutions with Tunable Sizes and Thermodynamic Stability
journal, May 2015

  • Zhou, Jing; Yin, Panchao; Gao, Yunyi
  • Chemistry - A European Journal, Vol. 21, Issue 26
  • DOI: 10.1002/chem.201501115

An Unusually Slow Self-Assembly of Inorganic Ions in Dilute Aqueous Solution
journal, January 2003

  • Liu, Tianbo
  • Journal of the American Chemical Society, Vol. 125, Issue 2
  • DOI: 10.1021/ja028933d

Lag Periods During the Self-Assembly of {Mo 72 Fe 30 } Macroions: Connection to the Virus Capsid Formation Process
journal, October 2009

  • Zhang, Jie; Li, Dong; Liu, Guang
  • Journal of the American Chemical Society, Vol. 131, Issue 42
  • DOI: 10.1021/ja903548m

Interactions between solvent molecules and the reduced or unreduced forms of silico-molybdic acid studied by ESR and NMR spectroscopies and molecular modelling
journal, January 2000

Self-assembly of ten molecules into nanometre-sized organic host frameworks
journal, November 1995

  • Fujita, Makoto; Oguro, Daichi; Miyazawa, Mayumi
  • Nature, Vol. 378, Issue 6556, p. 469-471
  • DOI: 10.1038/378469a0

Self-diffusion in normal and heavy water in the range 1-45.deg.
journal, March 1973

Introduction to the Dendritic State
book, December 2001

Polyoxometalate Chemistry: An Old Field with New Dimensions in Several Disciplines
journal, January 1991

  • Pope, Michael T.; Müller, Achim
  • Angewandte Chemie International Edition in English, Vol. 30, Issue 1
  • DOI: 10.1002/anie.199100341

Self-Assembly of Discrete Cyclic Nanostructures Mediated by Transition Metals
journal, March 2000

  • Leininger, Stefan; Olenyuk, Bogdan; Stang, Peter J.
  • Chemical Reviews, Vol. 100, Issue 3
  • DOI: 10.1021/cr9601324

Crystal Structure and Dynamics of 12-Heteropoly Compounds as Investigated by Molecular Dynamics
journal, December 1995

Spontaneous Self-Assembly of Metal−Organic Cationic Nanocages to Form Monodisperse Hollow Vesicles in Dilute Solutions
journal, April 2008

  • Li, Dong; Zhang, Jie; Landskron, Kai
  • Journal of the American Chemical Society, Vol. 130, Issue 13
  • DOI: 10.1021/ja710820a

Keggin Polyoxoanions in Aqueous Solution: Ion Pairing and Its Effect on Dynamic Properties by Molecular Dynamics Simulations
journal, July 2008

  • Leroy, Frédéric; Miró, Pere; Poblet, Josep Maria
  • The Journal of Physical Chemistry B, Vol. 112, Issue 29
  • DOI: 10.1021/jp077098p

Keggin Polyoxoanions in Aqueous Solution: Ion Pairing and Its Effect on Dynamic Properties by Molecular Dynamics Simulations
journal, July 2008

  • Leroy, Frédéric; Miró, Pere; Poblet, Josep Maria
  • The Journal of Physical Chemistry B, Vol. 112, Issue 29
  • DOI: 10.1021/jp077098p

Archimedean Synthesis and Magic Numbers: “Sizing” Giant Molybdenum-Oxide-Based Molecular Spheres of the Keplerate Type
journal, November 1999

Deprotonations and Charges of Well-Defined {Mo 72 Fe 30 } Nanoacids Simply Stepwise Tuned by pH Allow Control/Variation of Related Self-Assembly Processes
journal, December 2006

  • Liu, Tianbo; Imber, Brandon; Diemann, Ekkehard
  • Journal of the American Chemical Society, Vol. 128, Issue 49
  • DOI: 10.1021/ja066133n

Counterion Distribution around Hydrophilic Molecular Macroanions: The Source of the Attractive Force in Self-Assembly
journal, August 2009

  • Pigga, Joseph M.; Kistler, Melissa L.; Shew, Chwen-Yang
  • Angewandte Chemie International Edition, Vol. 48, Issue 35
  • DOI: 10.1002/anie.200902050

An Unusually Slow Self-Assembly of Inorganic Ions in Dilute Aqueous Solution.
journal, May 2003

Polyoxometalate clusters, nanostructures and materials: From self assembly to designer materials and devices
journal, January 2007

  • Long, De-Liang; Burkholder, Eric; Cronin, Leroy
  • Chem. Soc. Rev., Vol. 36, Issue 1
  • DOI: 10.1039/B502666K

Deprotonations and Charges of Well-Defined {Mo 72 Fe 30 } Nanoacids Simply Stepwise Tuned by pH Allow Control/Variation of Related Self-Assembly Processes
journal, December 2006

  • Liu, Tianbo; Imber, Brandon; Diemann, Ekkehard
  • Journal of the American Chemical Society, Vol. 128, Issue 49
  • DOI: 10.1021/ja066133n

Supramolecular Assembly of Poly(propyleneimine) Dendrimers Driven By Simple Monovalent Counterions
journal, November 2015

  • Eghtesadi, Seyed Ali; Haso, Fadi; Kashfipour, Marjan Alsadat
  • Chemistry - A European Journal, Vol. 21, Issue 51
  • DOI: 10.1002/chem.201502852

Coarse Grained Model for Semiquantitative Lipid Simulations
journal, January 2004

  • Marrink, Siewert J.; de Vries, Alex H.; Mark, Alan E.
  • The Journal of Physical Chemistry B, Vol. 108, Issue 2
  • DOI: 10.1021/jp036508g

A Complete Macroion−“Blackberry” Assembly−Macroion Transition with Continuously Adjustable Assembly Sizes in {Mo 132 } Water/Acetone Systems
journal, May 2007

  • Kistler, Melissa L.; Bhatt, Anish; Liu, Guang
  • Journal of the American Chemical Society, Vol. 129, Issue 20
  • DOI: 10.1021/ja0685809

Counterion Distribution around Hydrophilic Molecular Macroanions: The Source of the Attractive Force in Self-Assembly
journal, August 2009

  • Pigga, Joseph M.; Kistler, Melissa L.; Shew, Chwen-Yang
  • Angewandte Chemie International Edition, Vol. 48, Issue 35
  • DOI: 10.1002/anie.200902050

Spontaneous Self-Assembly of Metal−Organic Cationic Nanocages to Form Monodisperse Hollow Vesicles in Dilute Solutions
journal, April 2008

  • Li, Dong; Zhang, Jie; Landskron, Kai
  • Journal of the American Chemical Society, Vol. 130, Issue 13
  • DOI: 10.1021/ja710820a

The MARTINI Force Field:  Coarse Grained Model for Biomolecular Simulations
journal, July 2007

  • Marrink, Siewert J.; Risselada, H. Jelger; Yefimov, Serge
  • The Journal of Physical Chemistry B, Vol. 111, Issue 27
  • DOI: 10.1021/jp071097f

Molecular Structure Encodes Nanoscale Assemblies: Understanding Driving Forces in Electrostatic Self-Assembly
journal, December 2011

  • Willerich, Immanuel; Gröhn, Franziska
  • Journal of the American Chemical Society, Vol. 133, Issue 50
  • DOI: 10.1021/ja207565m

A Complete Macroion−“Blackberry” Assembly−Macroion Transition with Continuously Adjustable Assembly Sizes in {Mo 132 } Water/Acetone Systems
journal, May 2007

  • Kistler, Melissa L.; Bhatt, Anish; Liu, Guang
  • Journal of the American Chemical Society, Vol. 129, Issue 20
  • DOI: 10.1021/ja0685809

Self-Assembly Driven Crystallization in Keplarate-Type Polyoxometalates
journal, March 2014

  • Goutham, Kaparapu; Mani, Ethayaraja
  • Journal of Molecular and Engineering Materials, Vol. 02, Issue 01
  • DOI: 10.1142/S225123731440005X

Supramolecular Assembly of Poly(propyleneimine) Dendrimers Driven By Simple Monovalent Counterions
journal, November 2015

  • Eghtesadi, Seyed Ali; Haso, Fadi; Kashfipour, Marjan Alsadat
  • Chemistry - A European Journal, Vol. 21, Issue 51
  • DOI: 10.1002/chem.201502852

Sheet-like assemblies of spherical particles with point-symmetrical patches
journal, April 2012

  • Mani, Ethayaraja; Sanz, Eduardo; Roy, Soumyajit
  • The Journal of Chemical Physics, Vol. 136, Issue 14
  • DOI: 10.1063/1.3702203

Computer Simulation Using Particles
book, January 1988

    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation
    journal, August 2018

    Tuning the Intercage Distance in Charge‐Regulated Blackberry‐Type Assemblies through Host–Guest Chemistry
    journal, March 2019

    • Li, Hui; Wang, Ruifu; Hong, You‐lee
    • Chemistry – A European Journal, Vol. 25, Issue 22
    • DOI: 10.1002/chem.201900800

    Isotope and Hydrogen‐Bond Effects on the Self‐Assembly of Macroions in Dilute Solution
    journal, November 2019

    • Li, Hui; Shen, Yidan; Yang, Peng
    • Chemistry – A European Journal, Vol. 25, Issue 71
    • DOI: 10.1002/chem.201902444

    Cation Translocation around Single Polyoxometalate-Organic Hybrid Cluster Regulated by Electrostatic and Cation-π Interactions
    journal, February 2017

    • Li, Dong; Liu, Zhuonan; Song, Jie
    • Angewandte Chemie International Edition, Vol. 56, Issue 12
    • DOI: 10.1002/anie.201612008

    Self-assembly study of nanometric spheres from polyoxometalate-phenylalanine hybrids, an experimental and theoretical approach
    journal, January 2018

    • Nikoloudakis, Emmanouil; Karikis, Kostas; Laurans, Maxime
    • Dalton Transactions, Vol. 47, Issue 18
    • DOI: 10.1039/c8dt00380g

    The applications of small-angle X-ray scattering in studying nano-scaled polyoxometalate clusters in solutions
    journal, April 2018

    Unique Symmetry-Breaking Phenomenon during the Self-assembly of Macroions Elucidated by Simulation
    journal, August 2018

    Cation Translocation around Single Polyoxometalate-Organic Hybrid Cluster Regulated by Electrostatic and Cation-π Interactions
    journal, February 2017

      Sort by:
      [ × clear filter / sort ]

      Similar Records in DOE PAGES and OSTI.GOV collections: