Aggregation of heteropolyanions in aqueous solutions exhibiting short-range attractions and long-range repulsions

Bera, Mrinal K.; Qiao, Baofu; Seifert, Soenke; Burton-Pye, Benjamin P.; Antonio, Mark R.

doi:10.1021/acs.jpcc.5b10609

Title: Aggregation of heteropolyanions in aqueous solutions exhibiting short-range attractions and long-range repulsions

Journal Article · Tue Dec 15 00:00:00 EST 2015 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.5b10609· OSTI ID:1238111

Bera, Mrinal K. ^[1]; Qiao, Baofu ^[1]; Seifert, Soenke ^[1]; Burton-Pye, Benjamin P. ^[2]; Antonio, Mark R. ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States)
Lehman College of the City Univ. of New York, Bronx, NY (United States); The Graduate Center of the City Univ. of New York, New York, NY (United States)

Charged colloids and proteins in aqueous solutions interact via short-range attractions and long-range repulsions (SALR) and exhibit complex structural phases. These include homogeneously dispersed monomers, percolated monomers, clusters, and percolated clusters. We report the structural architectures of simple charged systems in the form of spherical, Keggin-type heteropolyanions (HPAs) by small-angle X-ray scattering (SAXS) and molecular dynamics (MD) simulations. Structure factors obtained from the SAXS measurements show that the HPAs interact via SALR. Concentration and temperature dependences of the structure factors for HPAs with –3e (e is the charge of an electron) charge are consistent with a mixture of nonassociated monomers and associated randomly percolated monomers, whereas those for HPAs with –4e and –5e charges exhibit only nonassociated monomers in aqueous solutions. Our experiments show that the increase in magnitude of the charge of the HPAs increases their repulsive interactions and inhibits their aggregation in aqueous solutions. MD simulations were done to reveal the atomistic scale origins of SALR between HPAs. As a result, the short-range attractions result from water or proton-mediated hydrogen bonds between neighboring HPAs, whereas the long-range repulsions are due to the distributions of ions surrounding the HPAs.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0000989

OSTI ID:: 1238111

Journal Information:: Journal of Physical Chemistry. C, Vol. 120, Issue 2; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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pH-Dependent Interactions between Keggin Heteropolyanions in Dilute Solutions: pH-Dependent Interactions between Keggin Heteropolyanions in Dilute Solutions Antonio, Mark R.; Bera, Mrinal K. European Journal of Inorganic Chemistry, Vol. 2019, Issue 3-4 https://doi.org/10.1002/ejic.201801165	journal	December 2018
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