4.5 Article

Dynamic Mixing Behaviors of Ionically Tethered Polymer Canopy of Nanoscale Hybrid Materials in Fluids of Varying Physical and Chemical Properties

Journal

JOURNAL OF PHYSICAL CHEMISTRY B
Volume 125, Issue 32, Pages 9223-9234

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcb.1c00935

Keywords

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Funding

  1. Breakthrough Electrolytes for Energy Storage (BEES), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DESC0019409]
  2. Shell's New Energy Research and Technology (NERT) Program

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A new area of sustainable energy and environmental research focuses on developing novel electrolytes to enhance the solubility of target species and improve reaction performance, particularly in flow batteries and CO2 conversion. Liquid-like nanoparticle organic hybrid materials (NOHMs) show promise for electrolyte applications due to their enhanced conductivity, although high viscosity is a challenge. This study investigated the impact of different secondary fluids on the transport behaviors of NOHMs, with findings on how secondary fluids affect transport properties and the conformation of polymer in NOHMs.
An emerging area of sustainable energy and environmental research is focused on the development of novel electrolytes that can increase the solubility of target species and improve subsequent reaction performance. Electrolytes with chemical and structural tunability have allowed for significant advancements in flow batteries and CO2 conversion integrated with CO2 capture. Liquid-like nanoparticle organic hybrid materials (NOHMs) are nanoscale fluids that are composed of inorganic nanocores and an ionically tethered polymeric canopy. NOHMs have been shown to exhibit enhanced conductivity making them promising for electrolyte applications, though they are often challenged by high viscosity in the neat state. In this study, a series of binary mixtures of NOHM-I-HPE with five different secondary fluids, water, chloroform, toluene, acetonitrile, and ethyl acetate, were prepared to reduce the fluid viscosity and investigate the effects of secondary fluid properties (e.g., hydrogen bonding ability, polarity, and molar volume) on their transport behaviors, including viscosity and diffusivity. Our results revealed that the molecular ratio of secondary fluid to the ether groups of Jeffamine M2070 (lambda(SF)) was able to describe the effect that secondary fluid has on transport properties. Our findings also suggest that in solution, the Jeffamine M2070 molecules exist in different nanoscale environments, where some are more strongly associated with the nanoparticle surface than others, and the conformation of the polymer canopy was dependent on the secondary fluid. This understanding of the polymer conformation in NOHMs can allow for the better design of an electrolyte capable of capturing and releasing small gaseous or ionic species.

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