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

Abstract:

: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 Rnetwork, 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.

journal_name

Biomacromolecules

journal_title

Biomacromolecules

authors

Grossutti M,Dutcher JR

doi

10.1021/acs.biomac.0c01098

subject

Has Abstract

pub_date

2020-12-14 00:00:00

pages

4871-4877

issue

12

eissn

1525-7797

issn

1526-4602

journal_volume

21

pub_type

杂志文章
  • Analysis of the conserved N-terminal domains in major ampullate spider silk proteins.

    abstract::Major ampullate silk, also known as dragline silk, is one of the strongest biomaterials known. This silk is composed of two proteins, major ampullate spidroin 1 (MaSp1) and major ampullate spidroin 2 (MaSp2). Only partial cDNA sequences have been obtained for these proteins, and these sequences are toward the C-termin...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm050472b

    authors: Motriuk-Smith D,Smith A,Hayashi CY,Lewis RV

    更新日期:2005-11-01 00:00:00

  • Synthetic 3D PEG-Anisogel Tailored with Fibronectin Fragments Induce Aligned Nerve Extension.

    abstract::An enzymatically cross-linked polyethylene glycol (PEG)-based hydrogel was engineered to promote and align nerve cells in a three-dimensional manner. To render the injectable, otherwise bioinert, PEG-based material supportive for cell growth, its mechanical and biochemical properties were optimized. A recombinant fibr...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.9b00891

    authors: Licht C,Rose JC,Anarkoli AO,Blondel D,Roccio M,Haraszti T,Gehlen DB,Hubbell JA,Lutolf MP,De Laporte L

    更新日期:2019-11-11 00:00:00

  • Structure and mechanical properties of wet-spun fibers made from natural cellulose nanofibers.

    abstract::Cellulose nanofibers were prepared by TEMPO-mediated oxidation of wood pulp and tunicate cellulose. The cellulose nanofiber suspension in water was spun into an acetone coagulation bath. The spinning rate was varied from 0.1 to 100 m/min to align the nanofibers to the spun fibers. The fibers spun from the wood nanofib...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm101510r

    authors: Iwamoto S,Isogai A,Iwata T

    更新日期:2011-03-14 00:00:00

  • Influence of enzymatic specificity on the behavior of ephemeral gels.

    abstract::Ephemeral gels, called Enzgels, successively undergo sol-gel and then gel-sol transition under the action of two antagonistic enzymes, transglutaminase and protease. Molecular and macroscopic properties of Enzgels are directly dependent on the enzymatic activities and their ratios. This work studies the characteristic...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm700601n

    authors: Picard J,Giraudier S,Larreta-Garde V

    更新日期:2008-01-01 00:00:00

  • Well-defined homopolypeptides, copolypeptides, and hybrids of poly(l-proline).

    abstract::l-Proline is the only, out of 20 essential, amino acid that contains a cyclized substituted α-amino group (is formally an imino acid), which restricts its conformational shape. The synthesis of well-defined homo- and copolymers of l-proline has been plagued either by the low purity of the monomer or the inability of m...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm200495n

    authors: Gkikas M,Iatrou H,Thomaidis NS,Alexandridis P,Hadjichristidis N

    更新日期:2011-06-13 00:00:00

  • From In Silico to Experimental Validation: Tailoring Peptide Substrates for a Serine Protease.

    abstract::Smart nanocarriers for the transport of drugs to tumor cells are nowadays of great interest for treating cancer. The use of enzymatic stimuli to cleave peptide-based drug nanocapsules for the selective release of nanocapsule cargo in close proximity to tumor cells opens new possibilities in cancer research. In the pre...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.0c00240

    authors: Knaff PM,Kersten C,Willbold R,Champanhac C,Crespy D,Wittig R,Landfester K,Mailänder V

    更新日期:2020-04-13 00:00:00

  • Nanomaterials Derived from Fungal Sources-Is It the New Hype?

    abstract::Greener alternatives to synthetic polymers are constantly being investigated and sought after. Chitin is a natural polysaccharide that gives structural support to crustacean shells, insect exoskeletons, and fungal cell walls. Like cellulose, chitin resides in nanosized structural elements that can be isolated as nanof...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.9b01141

    authors: Nawawi WMFBW,Jones M,Murphy RJ,Lee KY,Kontturi E,Bismarck A

    更新日期:2020-01-13 00:00:00

  • Resilin-PEG Hybrid Hydrogels Yield Degradable Elastomeric Scaffolds with Heterogeneous Microstructure.

    abstract::Hydrogels derived from resilin-like polypeptides (RLPs) have shown outstanding mechanical resilience and cytocompatibility; expanding the versatility of RLP-based materials via conjugation with other polypeptides and polymers would offer great promise in the design of a range of materials. Here, we present an investig...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.5b01255

    authors: McGann CL,Akins RE,Kiick KL

    更新日期:2016-01-11 00:00:00

  • Combined effects of PEG hydrogel elasticity and cell-adhesive coating on fibroblast adhesion and persistent migration.

    abstract::The development and use of synthetic, cross-linked, macromolecular substrates with tunable elasticity has been instrumental in revealing the mechanisms by which cells sense and respond to their mechanical microenvironment. We here describe a hydrogel based on radical-free, cross-linked poly(ethylene glycol) to study t...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm4014827

    authors: Missirlis D,Spatz JP

    更新日期:2014-01-13 00:00:00

  • Dual MMP7-proximity-activated and folate receptor-targeted nanoparticles for siRNA delivery.

    abstract::A dual-targeted siRNA nanocarrier has been synthesized and validated that is selectively activated in environments where there is colocalization of two breast cancer hallmarks, elevated matrix metalloproteinase (MMP) activity and folate receptor overexpression. This siRNA nanocarrier is self-assembled from two polymer...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm501394m

    authors: Li H,Miteva M,Kirkbride KC,Cheng MJ,Nelson CE,Simpson EM,Gupta MK,Duvall CL,Giorgio TD

    更新日期:2015-01-12 00:00:00

  • Nanocarrier Composed of Magnetite Core Coated with Three Polymeric Shells Mediates LCS-1 Delivery for Synthetic Lethal Therapy of BLM-Defective Colorectal Cancer Cells.

    abstract::Synthetic lethality is a molecular-targeted therapy for selective killing of cancer cells. We exploited a lethal interaction between superoxide dismutase 1 inhibition and Bloom syndrome gene product (BLM) defect for the treatment of colorectal cancer (CRC) cells (HCT 116) with a customized lung cancer screen-1-loaded ...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.7b01607

    authors: Gupta A,Ahmad A,Singh H,Kaur S,K M N,Ansari MM,Jayamurugan G,Khan R

    更新日期:2018-03-12 00:00:00

  • Hydrogel-Based Bioinks for Cell Electrowriting of Well-Organized Living Structures with Micrometer-Scale Resolution.

    abstract::Bioprinting has become an important tool for fabricating regenerative implants and in vitro cell culture platforms. However, until today, extrusion-based bioprinting processes are limited to resolutions of hundreds of micrometers, which hamper the reproduction of intrinsic functions and morphologies of living tissues....

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.0c01577

    authors: Castilho M,Levato R,Bernal PN,de Ruijter M,Sheng CY,van Duijn J,Piluso S,Ito K,Malda J

    更新日期:2021-01-07 00:00:00

  • Long-circulating near-infrared fluorescence core-cross-linked polymeric micelles: synthesis, characterization, and dual nuclear/optical imaging.

    abstract::We report the synthesis of PEG-coated, core-cross-linked polymeric micelles (CCPMs) derived from an amine-terminated amphiphilic block copolymer, poly(PEG-methacrylate)-b-poly(triethoxysilyl propylmethacrylate). The block copolymer self-assembled to form micellar nanoparticles, and a Cy-7-like near-infrared fluorescen...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm7005399

    authors: Yang Z,Zheng S,Harrison WJ,Harder J,Wen X,Gelovani JG,Qiao A,Li C

    更新日期:2007-11-01 00:00:00

  • Morphology of artificial silica matrices formed via autosilification of a silaffin/protein polymer chimera.

    abstract::Protein polymers (long-chain proteins in which a specific amino acid sequence "monomer" is repeated through the molecule) are found widely in nature, and these materials exhibit a diverse array of physical properties. One class of self-assembling proteins is hydrophobic-polar (HP) protein polymers capable of self-asse...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm701131x

    authors: Marner WD 2nd,Shaikh AS,Muller SJ,Keasling JD

    更新日期:2008-01-01 00:00:00

  • Adhesion of Blood Plasma Proteins and Platelet-rich Plasma on l-Valine-Based Poly(ester urea).

    abstract::The competitive absorption of blood plasma components including fibrinogen (FG), bovine serum albumin (BSA), and platelet-rich plasma (PRP) on l-valine-based poly(ester urea) (PEU) surfaces were investigated. Using four different PEU polymers, possessing compositionally dependent trends in thermal, mechanical, and cri...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.6b01195

    authors: Childers EP,Peterson GI,Ellenberger AB,Domino K,Seifert GV,Becker ML

    更新日期:2016-10-10 00:00:00

  • Binding between proteins and cationic spherical polyelectrolyte brushes: effect of pH, ionic strength, and stoichiometry.

    abstract::Cationic spherical polyelectrolyte brushes (SPBs) were synthesized by photoemulsion polymerization, consisting of a polystyrene core with a diameter around 80 nm and a poly(2-aminoethylmethacrylate hydrochloride) (PAEMH) shell with a thickness from 10 to 50 nm densely grafted on the core surface. The binding of variou...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm301865g

    authors: Wang S,Chen K,Li L,Guo X

    更新日期:2013-03-11 00:00:00

  • Mutational analysis and allosteric effects in the HIV-1 capsid protein carboxyl-terminal dimerization domain.

    abstract::The carboxyl-terminal domain (CTD, residues 146-231) of the HIV-1 capsid (CA) protein plays an important role in the CA-CA dimerization and viral assembly of the human immunodeficiency virus type 1. Disrupting the native conformation of the CA is essential for blocking viral capsid formation and viral replication. Thu...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm801151r

    authors: Yu X,Wang Q,Yang JC,Buch I,Tsai CJ,Ma B,Cheng SZ,Nussinov R,Zheng J

    更新日期:2009-02-09 00:00:00

  • Polymersome nanoreactors for enzymatic ring-opening polymerization.

    abstract::Polystyrene-polyisocyanopeptide (PS-PIAT) polymersomes containing CALB in two different locations, one in the aqueous inner compartment and one in the bilayer, were investigated for enzymatic ring-opening polymerization of lactones in water. It is shown that the monomers 8-octanolactone and dodecalactone yield oligome...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm7005938

    authors: Nallani M,de Hoog HP,Cornelissen JJ,Palmans AR,van Hest JC,Nolte RJ

    更新日期:2007-12-01 00:00:00

  • Reconstruction of surfaces from mixed hydrocarbon and PEG components in water: responsive surfaces aid fouling release.

    abstract::Coatings derived from surface active block copolymers (SABCs) having a combination of hydrophobic aliphatic (linear hydrocarbon or propylene oxide-derived groups) and hydrophilic poly(ethlyene glycol) (PEG) side chains have been developed. The coatings demonstrate superior performance against protein adsorption as wel...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm300363g

    authors: Cho Y,Sundaram HS,Finlay JA,Dimitriou MD,Callow ME,Callow JA,Kramer EJ,Ober CK

    更新日期:2012-06-11 00:00:00

  • Mechanistic studies on the degradation and protein release characteristics of poly(lactic-co-glycolic-co-hydroxymethylglycolic acid) nanospheres.

    abstract::The purpose of this study was to gain mechanistic insights into the effect of different formulation parameters on the degradation and release behavior of protein-loaded nanoparticulate carrier systems based on an aliphatic polyester with pendant hydroxyl groups, poly(lactic-co-glycolic-hydroxymethyl glycolic acid) (pL...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm301900t

    authors: Samadi N,van Nostrum CF,Vermonden T,Amidi M,Hennink WE

    更新日期:2013-04-08 00:00:00

  • Pretreatment of amphiphilic comb polymer surfaces dramatically affects protein adsorption.

    abstract::New applications in regenerative biotechnology require the ability to understand and control protein-surface interactions on micrometer and submicrometer length scales. Evidence presented here shows that micropatterned amphiphilic comb polymer films exhibit a pretreatment-dependent behavior with respect to protein ads...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm050446d

    authors: Zhang Z,Ma H,Hausner DB,Chilkoti A,Beebe TP Jr

    更新日期:2005-11-01 00:00:00

  • Coating formation during drying of β-lactoglobulin: gradual and sudden changes.

    abstract::The drying dynamics of protein coatings is of importance for many applications. The main focus of research so far was to investigate macroscopic properties of protein coatings, leaving drying dynamics virtually unexplored. A unique combination of techniques is used to monitor drying of a coating containing the protein...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm501549b

    authors: Bouman J,de Vries R,Venema P,Belton P,Baukh V,Huinink HP,van der Linden E

    更新日期:2015-01-12 00:00:00

  • Type, density, and presentation of grafted adhesion peptides on polysaccharide-based hydrogels control preosteoblast behavior and differentiation.

    abstract::In this work, cell-responsive polysaccharide hydrogels were prepared by a simple procedure based on the sequential bioconjugation and cross-linking of the polysaccharide backbone with bioactive peptides and poly(ethylene glycol)-bis(thiol) (PEG-(SH)2), respectively. Using thiol-ene reactions, we successfully functiona...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm501613u

    authors: Jing J,Fournier A,Szarpak-Jankowska A,Block MR,Auzély-Velty R

    更新日期:2015-03-09 00:00:00

  • Inhibition of ice crystal growth by synthetic glycopolymers: implications for the rational design of antifreeze glycoprotein mimics.

    abstract::A series of structurally diverse polymers, containing either peptide or vinyl-derived backbones, was tested for ice recrystallization inhibition activity, which is commonly associated with antifreeze (glyco)proteins. It was revealed that only polymers bearing hydroxyl groups in the side chain could inhibit ice growth....

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm801069x

    authors: Gibson MI,Barker CA,Spain SG,Albertin L,Cameron NR

    更新日期:2009-02-09 00:00:00

  • Structural effects of terminal groups on nonenzymatic and enzymatic degradations of end-capped poly(L-lactide).

    abstract::Poly(L-lactide) (PLLA) with various alkyl ester chain end groups were synthesized by ring-opening polymerization of L-lactide in the presence of zinc alkoxide as a catalyst. The structural effect of chain end groups on the rate of enzymatic and nonenzymatic degradations for amorphous films of PLLA were investigated at...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm701259r

    authors: Kurokawa K,Yamashita K,Doi Y,Abe H

    更新日期:2008-03-01 00:00:00

  • Swelling and mechanical properties of biopolymer hydrogels containing chitosan and bovine serum albumin.

    abstract::Experimental and theoretical investigations of the swelling and mechanical properties of hydrogels formed from chitosan, bovine serum albumin (BSA), and chitosan/BSA mixtures cross-linked with genipin were performed. The properties of cross-linked chitosan hydrogels were explained in terms of its polyelectrolyte behav...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm060133y

    authors: Butler MF,Clark AH,Adams S

    更新日期:2006-11-01 00:00:00

  • Structural and Mechanical Roles for the C-Terminal Nonrepetitive Domain Become Apparent in Recombinant Spider Aciniform Silk.

    abstract::Spider aciniform (or wrapping) silk is the toughest of the seven types of spider silks/glue due to a combination of high elasticity and strength. Like most spider silk proteins (spidroins), aciniform spidroin (AcSp1) has a large core repetitive domain flanked by relatively short N- and C-terminal nonrepetitive domains...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.7b01057

    authors: Xu L,Lefèvre T,Orrell KE,Meng Q,Auger M,Liu XQ,Rainey JK

    更新日期:2017-11-13 00:00:00

  • Glucose-responsive vehicles containing phenylborate ester for controlled insulin release at neutral pH.

    abstract::This study is devoted to developing amphiphilic block polymers based on phenylborate ester, which can self-assemble to form nanoparticles, as a glucose-sensitive drug carrier. Poly(ethylene glycol)-block-poly[(2-phenylboronic esters-1,3-dioxane-5-ethyl) methylacrylate] (MPEG5000-block-PBDEMA) was fabricated with MPEG5...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm3003286

    authors: Yao Y,Zhao L,Yang J,Yang J

    更新日期:2012-06-11 00:00:00

  • Solution structures of two structural isoforms of CMrVIA chi/lambda-conotoxin.

    abstract::alpha-Conotoxins possess a conserved four-cysteine framework and disulfide linkages (C(1)(-)(3), C(2)(-)(4)) that fold toward the globular conformation with absolute fidelity. Despite the presence of a similar conserved set of cysteine framework, chi/lambda-conotoxins adopt an alternate disulfide-pairing (C(1)(-)(4), ...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm060269w

    authors: Kang TS,Jois SD,Kini RM

    更新日期:2006-08-01 00:00:00

  • In Situ Synthesis of Magnetic Field-Responsive Hemicellulose Hydrogels for Drug Delivery.

    abstract::A one-pot synthetic methodology for fabricating stimuli-responsive hemicellulose-based hydrogels was developed that consists of the in situ formation of magnetic iron oxide (Fe3O4) nanoparticles during the covalent cross-linking of O-acetyl-galactoglucomannan (AcGGM). The Fe3O4 nanoparticle content controlled the ther...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.5b00801

    authors: Zhao W,Odelius K,Edlund U,Zhao C,Albertsson AC

    更新日期:2015-08-10 00:00:00