Insights into the Assembly and Conformation of Nanoparticle Organic Hybrid Materials (NOHMs) in Solution with Varying Grafting Type

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

doi:10.1021/acsapm.3c03219

Insights into the Assembly and Conformation of Nanoparticle Organic Hybrid Materials (NOHMs) in Solution with Varying Grafting Type

Journal Article · Wed Mar 13 00:00:00 EDT 2024 · ACS Applied Polymer Materials

DOI:https://doi.org/10.1021/acsapm.3c03219· OSTI ID:2333622

Haque, Md Ashraful ^[1]; Feric, Tony G. ^[2]; ^[2]; ^[2]; ^[3]

University of Tennessee, Knoxville, TN (United States); Case Western Reserve University
Columbia University, New York, NY (United States)
University of Tennessee, Knoxville, TN (United States)

Recently, nanoparticle organic hybrid materials (NOHMs) have been considered promising electrolytes for energy storage applications due to their unique combination of properties, which include high thermal stability, negligible vapor pressure, and easy synthesis. However, the structural features of NOHMs in electrochemical systems are not well understood. Hence, we investigate the impact of grafting type (ionic vs covalent) on the structure and performance of NOHMs that consist of a silica core and grafted HPE polymer (Jeffamine M2070) in aqueous solution with and without the presence of the supporting electrolyte (0.1 M KHCO₃) using small-angle neutron scattering. Careful analyses of the results indicate that even at low grafting density (0.8 chains nm^–2) and concentration (1–3 wt %), ionic NOHMs solutions contain a free polymer that may interact with the grafted polymer, altering the assembly of NOHMs in solution. Our investigation also elucidates that the covalent NOHM solutions consist of both aggregated and dispersed NOHMs in the solution. Moreover, the addition of the supporting electrolyte affects the assembly and structure of the polymer in the ionic NOHMs solution significantly, whereas only a slight change in the conformation of the grafted polymer is observed for covalent NOHMs. These conformational changes alter the performance of the NOHMs solution, resulting in a dramatic change in viscosity. Careful analysis shows that this significant alteration of solution viscosity in the ionic NOHMs can be traced back to the presence of the free polymer that interacts with the grafted layer and the attenuation of this interaction between the free and grafted polymers with the addition of salt. Furthermore, these studies elucidate the impact of grafting type on the overall structure, assembly, and performance of functionalized NOHMs in aqueous solution and explicitly correlate the structure and assembly of NOHMs to their transport properties and must be considered when designing functional systems that incorporate NOHMs.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: SC0019409

OSTI ID:: 2333622

Journal Information:: ACS Applied Polymer Materials, Journal Name: ACS Applied Polymer Materials Journal Issue: 6 Vol. 6; ISSN 2637-6105

Publisher:: ACS PublicationsCopyright Statement

Country of Publication:: United States

Language:: English

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