Structure, Hydration, and Interactions of Native and Hydrophobically Modified Phytoglycogen Nanoparticles

Simmons, John V.; Nickels, Jonathan D.; Michalski, Michelle M.; Grossutti, Michael; Shamana, Hurmiz; Stanley, Christopher B.; Schwan, Adrian L.; Katsaras, John; Dutcher, John

doi:10.1021/acs.biomac.0c00870

Cited by 26 publications

(81 citation statements)

References 25 publications

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“…Phytoglycogen is a highly branched polysaccharide nanoparticle (44 nm diameter) produced by certain varieties of plants such as sweet corn. − It consists of linear chains of α(1,4)-linked anhydroglucose units (AGUs) with α(1,6) branching every 10–12 monomers. , The dendrimer architecture of phytoglycogen nanoparticles distinguishes it from other biopolymers and makes it an attractive platform for biomedical applications . Chemical modification of phytoglycogen can be performed via the polysaccharide hydroxyl groups, where simple chemistry can be used to attach diverse functional groups.…”

Section: Introductionmentioning

confidence: 99%

Hydration Water Structure, Hydration Forces, and Mechanical Properties of Polysaccharide Films

Grossutti

Dutcher

2020

Biomacromolecules

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The interaction of polysaccharides with water has a critical impact on their biological function as well as their technological applications. We performed ellipsometry experiments at different relative humidities (RH) to measure the equilibrium swelling of ultrathin films of different polysaccharides: native and modified phytoglycogen (PG) nanoparticles, dextran, and hyaluronic acid. For RH > 70%, the swelling of hydrophilic polymers with increases in RH is described by hydration forces that are characterized by an exponential decay length λ. Our analysis of the high RH swelling regime allowed us to determine λ and the bulk modulus K of the films of different polysaccharides. We also probed the high RH swelling regime using attenuated total reflection infrared (ATR-IR) spectroscopy, which allowed us to determine the degree of hydrogen bonding of the hydration water within the polysaccharide films. Combining the ellipsometry and ATR-IR spectroscopy results, we find that increases in the order of the hydrogen bond network of the hydration water, as specified by the ATR-IR parameter R network , lead to linear increases in K and corresponding inverse changes in λ. These measurements help to elucidate the intimate relationships between the degree of ordering of hydration water, hydration forces, and the mechanical stiffness of polysaccharides. For phytoglycogen, the addition of chemical groups, both cationic and anionic, produced significant increases in its water holding capacity and mechanical properties, suggesting that chemical modification can be used to tune the properties of phytoglycogen for different applications.

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Section: Introductionmentioning

confidence: 99%

Hydration Water Structure, Hydration Forces, and Mechanical Properties of Polysaccharide Films

Grossutti

Dutcher

2020

Biomacromolecules

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“…This hydration capacity is significantly high when compared to other mono-, di-, oligo-, and polysaccharides, such as glucose, sucrose, , maltodextrin, cellulose ethers, and branched polyglycerols, in all of which two to four water molecules are associated with each hydroxyl group. Using SANS analysis, the density of polymer branches in PhG NPs was found to be uniform, due to the folding back of the flexible glucose chains into the center of the NPs . Rheological characterization indicates that dispersion of these NPs undergo liquid-to-gel transition at ∼29 wt % polymer concentration, which is equivalent to the concentration of polymer in a single PhG NP. ,, Above this concentration, an increase in the osmotic pressure induces NP dehydration and causes an increase in NP bulk modulus .…”

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confidence: 99%

“…Using SANS analysis, the density of polymer branches in PhG NPs was found to be uniform, due to the folding back of the flexible glucose chains into the center of the NPs . Rheological characterization indicates that dispersion of these NPs undergo liquid-to-gel transition at ∼29 wt % polymer concentration, which is equivalent to the concentration of polymer in a single PhG NP. ,, Above this concentration, an increase in the osmotic pressure induces NP dehydration and causes an increase in NP bulk modulus . The physiochemical properties of PhG NPs have been recently reviewed …”

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confidence: 99%

“…Using SANS analysis, the density of polymer branches in PhG NPs was found to be uniform, due to the folding back of the flexible glucose chains into the center of the NPs. 34 Rheological characterization indicates that dispersion of these NPs undergo liquid-to-gel transition at ∼29 wt % polymer concentration, 35 which is equivalent to the concentration of polymer in a single PhG NP. 27,34,36 Above this concentration, an increase in the osmotic pressure induces NP dehydration and causes an increase in NP bulk modulus.…”

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confidence: 99%

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Phytoglycogen Nanoparticles: Nature-Derived Superlubricants

Adibnia

Halimi

et al. 2021

ACS Nano

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Phytoglycogen nanoparticles (PhG NPs), a single-molecule highly branched polysaccharide, exhibit excellent water retention, due to the abundance of close-packed hydroxyl groups forming hydrogen bonds with water. Here we report lubrication properties of close-packed adsorbed monolayers of PhG NPs acting as boundary lubricants. Using direct surface force measurements, we show that the hydrated nature of the NP layer results in its striking lubrication performance, with two distinct confinement-controlled friction coefficients. In the weak-to moderate-confinement regime, when the NP layer is compressed down to 8% of its original thickness under a normal pressure of up to 2.4 MPa, the NPs lubricate the surface with a friction coefficient of 10 −3 . In the strong-confinement regime, with 6.5% of the original layer thickness under a normal pressure of up to 8.1 MPa, the friction coefficient was 10 −2 . Analysis of the water content and energy dissipation in the confined NP film reveals that the lubrication is governed by synergistic contributions of unbound and bound water molecules, with the former contributing to lubrication properties in the weak-to moderate-confinement regime and the latter being responsible for the lubrication in the strong-confinement regime. These results unravel mechanistic insights that are essential for the design of lubricating systems based on strongly hydrated NPs.

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“…Neutron scattering data suggest that there are 66,660 anhydroglucose units per phytoglycogen NP (Simmons et al. 2020); thus, a degree of substitution of 0.03 would result in 2,000 IMP molecules per NP.…”

Section: Methodsmentioning

confidence: 99%

In Vitro and in Vivo Characterization of Inosine Monophosphate Delivered by a Nanoparticle in Rainbow Trout

et al. 2022

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Rainbow Trout Oncorhynchus mykiss are a commonly farmed fish worldwide and, as such, are of economic importance in many countries. Inosine monophosphate (IMP) has been shown to have a positive effect on Rainbow Trout growth performance and overall health. The aim of the current study was to test whether a novel phytoglycogen nanoparticle (NP) was nontoxic and if it could enhance the positive effects of IMP on Rainbow Trout health at the cellular and whole-animal level. The NP used in this study is derived from sweet corn and can act as a carrier, delivering its payload to the cell. The NP was chemically modified to covalently bind IMP. The effects of four experimental groups were tested on Rainbow Trout at the in vitro and in vivo level: untreated control, NP alone, IMP alone, and IMP covalently conjugated to the NP (IMP-NP). The effects of the four experimental groups were measured at the cellular level using a Rainbow Trout intestinal epithelial cell line (RTgutGC). Cellular metabolism was significantly increased in RTgutGC when treated with IMP-NP for 24 and 48 h compared with NP or IMP alone. These treatments did not result in a compromised cell membrane, with the exception of minimal membrane integrity loss at 48 h with the higher doses of IMP-NP. During the 48-h time frame, enhanced metabolism did not result in enhanced cell proliferation. A pilot study was performed in Rainbow Trout to test the safety of the NP to fish. Over an 8-week feeding trial, no mortalities were observed. Additionally, intestinal villi density increased with IMP-NP and NP treatments, while villus height and width were unaffected. This study introduces the use of a phytoglycogen-based NP as a novel delivery system for IMP that is able to increase metabolism at the cellular level and is nontoxic in Rainbow Trout.

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Structure, Hydration, and Interactions of Native and Hydrophobically Modified Phytoglycogen Nanoparticles

Cited by 26 publications

References 25 publications

Hydration Water Structure, Hydration Forces, and Mechanical Properties of Polysaccharide Films

Hydration Water Structure, Hydration Forces, and Mechanical Properties of Polysaccharide Films

Phytoglycogen Nanoparticles: Nature-Derived Superlubricants

In Vitro and in Vivo Characterization of Inosine Monophosphate Delivered by a Nanoparticle in Rainbow Trout

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