Structure and Dispersion of Free and Grafted Polymer in Nanoparticle Organic Hybrid Materials-Based Solutions by Small-Angle Neutron Scattering

Haque, Md. Ashraful; Feric, Tony G.; Hamilton, Sara T.; Park, Ah-Hyung Alissa; Dadmun, Mark D.

doi:10.1021/acs.jpcc.0c10790

Title: Structure and Dispersion of Free and Grafted Polymer in Nanoparticle Organic Hybrid Materials-Based Solutions by Small-Angle Neutron Scattering

Journal Article · Mon Mar 01 00:00:00 EST 2021 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c10790· OSTI ID:1808451

Haque, Md. Ashraful ^[1]; Feric, Tony G. ^[2]; Hamilton, Sara T. ^[2]; Park, Ah-Hyung Alissa ^[2];

^[3]

Univ. of Tennessee, Knoxville, TN (United States)
Columbia Univ., New York, NY (United States)
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Liquid-like Nanoscale Organic Hybrid Materials or NOHMs consisting of polymer grafted nanoparticles have shown great promise in applications, such as electrochemistry and gas separation, due to their enhanced conductivity, tunability, and negligible vapor pressure. Recently, NOHMs are considered to be used as novel electrolytes in Redox Flow Batteries (RFBs). However, to employ NOHMs in redox flow batteries as electrolytes, it is important to understand the conformation and dispersion of NOHMs in the electrochemical milieu. In this work, we report the use of small-angle neutron scattering to probe the structure and dispersion of Jeffamine M2070 polymer grafted to a SiO₂ nanoparticle in an aqueous solution with and without the presence of a supporting electrolyte. Our results indicate that, in the aqueous environment, there exists a large amount of free polymer in the solution that is not grafted to the functionalized nanoparticles. These protonated free polymers, dispersed in the aqueous solvent, may also strongly interact with the grafted polymer layer and greatly affect the neat structure of NOHMs. Thus, there also exist polymers identified as “interacting” polymers to distinguish them from tethered or truly free polymers in the fluid system. The presence of supporting electrolyte shows a greater effect on the structure of NOHMs-based fluid as it not only alters the structure of the free polymer but also hinders the interaction of the polymer with the functionalized nanoparticles. Moreover, the change in the interaction of the Jeffamine M2070 with the functionalized nanoparticles due to the addition of supporting electrolyte has revealed a drastic change in the viscosities of NOHM solutions. Overall, the dispersion of the free polymer, the interaction of the interacting polymer with grafted polymer, and the change in conformation of free polymer and grafted layers with the addition of supporting electrolyte provide valuable insight into the overall scenario of the electrochemical environment of NOHMs. These results can be applied to fine-tune the structure of liquid-like NOHMs and will aid in a better understanding of their performance as potential electrolytes in RFBs.

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Research Organization:: Case Western Reserve Univ., Cleveland, OH (United States)

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

Grant/Contract Number:: SC0019409

OSTI ID:: 1808451

Journal Information:: Journal of Physical Chemistry. C, Vol. 125, Issue 9; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Structure and Dispersion of Free and Grafted Polymer in Nanoparticle Organic Hybrid Materials-Based Solutions by Small-Angle Neutron Scattering

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