Abstract：
:Macromolecular dynamics in biological systems, which play a crucial role for biomolecular function and activity at ambient temperature, depend strongly on moisture content. Yet, a generally accepted quantitative model of hydration-dependent phenomena based on local relaxation and diffusive dynamics of both polymer and its adsorbed water is still missing. In this work, atomistic-scale spatial distributions of motional modes are calculated using molecular dynamics simulations of hydrated xyloglucan (XG). These are shown to reproduce experimental hydration-dependent 13C NMR longitudinal relaxation times ( T1) at room temperature, and relevant features of their broad distributions, which are indicative of locally heterogeneous polymer reorientational dynamics. At low hydration, the self-diffusion behavior of water shows that water molecules are confined to particular locations in the randomly aggregated XG network while the average polymer segmental mobility remains low. Upon increasing water content, the hydration network becomes mobile and fully accessible for individual water molecules, and the motion of hydrated XG segments becomes faster. Yet, the polymer network retains a heterogeneous gel-like structure even at the highest level of hydration. We show that the observed distribution of relaxations times arises from the spatial heterogeneity of chain mobility that in turn is a result of heterogeneous distribution of water-chain and chain-chain interactions. Our findings contribute to the picture of hydration-dependent dynamics in other macromolecules such as proteins, DNA, and synthetic polymers, and hold important implications for the mechanical properties of polysaccharide matrixes in plants and plant-based materials.
journal_name
Biomacromoleculesjournal_title
Biomacromoleculesauthors
Chen P,Terenzi C,Furó I,Berglund LA,Wohlert Jdoi
10.1021/acs.biomac.8b00191subject
Has Abstractpub_date
2018-07-09 00:00:00pages
2567-2579issue
7eissn
1525-7797issn
1526-4602journal_volume
19pub_type
杂志文章abstract：:The layer-by-layer technique has been used as a powerful method to produce multilayer thin films with tunable properties. When natural polymers are employed, complicated phenomena such as self-aggregation and fibrilogenesis can occur, making it more difficult to obtain and characterize high-quality films. The weak aci...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm5012135
更新日期：2015-01-12 00:00:00
abstract：:Biobased poly(γ-butyrolactone) (PγBL) as a fully biodegradable and bioabsorbable biomaterial has shown superior properties compared to those of other aliphatic polyesters. It is of great importance to prepare amphiphilic block copolymer containing PγBL block to make ordered nano-objects for biomedical applications suc...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/acs.biomac.8b01239
更新日期：2019-01-14 00:00:00
abstract：:The storage and transport of cells is a fundamental technology which underpins cell biology, biomaterials research, and emerging cell-based therapies. Inspired by antifreeze and ice-binding proteins in extremophiles, macromolecular (polymer) cryoprotectants are emerging as exciting biomaterials to enable the reduction...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/acs.biomac.0c00591
更新日期：2020-07-13 00:00:00
abstract：:Vaginal films featuring the pH-dependent release of tenofovir (TFV) were developed for the prevention of sexual transmission of human immunodeficiency syndrome (HIV). Films based on hydroxypropyl methylcellulose and zein were prepared incorporating different plasticizers [oleic acid, lactic acid, glycerol, and polyeth...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/acs.biomac.0c01609
更新日期：2021-01-06 00:00:00
abstract：:Ambidextrous supergelators are developed through structure-gelation screening of rationally designed cyclic dipeptides (CDPs). The organo- and hydrogels of CDPs were thoroughly characterized by their minimal gelation concentration (MGC) for organic and aqueous solvents, thermal stability (Tg), and viscoelastic propert...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/acs.biomac.7b00924
更新日期：2017-11-13 00:00:00
abstract：:Cocontinuous phase structures of immiscible polymers can be developed under appropriate melt-blending conditions. Because of the presence of interfacial tension, such cocontinuous structures start to coarsen when heated to a temperature higher than the melting/softening temperature of both phases. In this study, a met...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm900008d
更新日期：2009-05-11 00:00:00
abstract：:Incorporating charged amino acid side chains in polypeptide polymer backbones to improve solubility usually leads to reduced secondary structuring. Here we show that highly water soluble (>15 mg.mL-1) β-sheets can be obtained via nucleotide monophosphate grafting onto simple poly(γ-propargyl- L-glutamate) backbone. Th...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/acs.biomac.8b01084
更新日期：2018-10-08 00:00:00
abstract：:Presently there is great interest in the construction of nanostructures from DNA fragments. Here we report the preparation of much larger helical textures with different shapes from pure DNA fragments. We have observed them while preparing crystals of the dodecamer d(AAAAAATTTTTT), which only contains adenine and thym...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm700994v
更新日期：2008-01-01 00:00:00
abstract：:The dynamics of silk protein in the presence and absence of water has been investigated by dielectric relaxation spectroscopy (DRS). The silk fibroin film cast from its water solution contains 4-7 wt % bound water molecules, which can be removed by dehydration at 165 °C. Temperature and frequency scans were performed ...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm1008316
更新日期：2010-10-11 00:00:00
abstract：:Electrospinning of cellulose nanocrystals (CNC)/poly(lactic acid) (PLA) emulsions has been demonstrated to be an effective dispersion and alignment method to control assembly of CNC into continuous composite ultrafine fibers. CNC-PLA nanocomposite random-fiber mats and aligned-fiber yarns were prepared by emulsion ele...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm400540v
更新日期：2013-11-11 00:00:00
abstract：:Mammalian synovial joints are extremely efficient lubrication systems reaching friction coefficient μ as low as 0.001 at high pressures (up to 100 atm) and shear rates (up to 10(6) to 10(7) Hz); however, despite much previous work, the exact mechanism responsible for this behavior is still unknown. In this work, we st...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm2004912
更新日期：2011-10-10 00:00:00
abstract：:Although composed simply of glucose polymers, the starch granule is a complex, semicrystalline structure. Much of this complexity arises from the fact that the two primary enzymes of synthesis-starch synthase and starch-branching enzyme-exist as multiple isoforms. Each form has distinct properties and plays a unique r...
journal_title：Biomacromolecules
pub_type： 杂志文章,评审
doi：10.1021/bm000133c
更新日期：2001-07-01 00:00:00
abstract：:This work demonstrates that hydrogen peroxide (H2O2) is generated in weak polyacrylamide hydrogels due to mechanochemical reactions to osmotic swelling. Hydrogels are important tools and materials for many biomedical applications, particularly for growth of stem cells. However, swollen gels are under constant tension,...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/acs.biomac.8b00743
更新日期：2018-08-13 00:00:00
abstract：:A polyethylene glycol (PEG) retinylamine (Ret-NH2) conjugate PEG-GFL-NH-Ret with a glycine-phenylalanine-leucine (GFL) spacer was synthesized for controlled oral delivery of Ret-NH2 to treat retinal degenerative diseases, including Stargardt disease (STGD) and age-related macular degeneration (AMD). The peptide spacer...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm501352s
更新日期：2014-12-08 00:00:00
abstract：:Chemotherapy faces challenges, including poor aqueous solubility of the drugs, and cardiotoxicity. Micellar drug delivery systems (DDS) are used to encapsulate anticancer drugs for better therapeutic effects, however, with poor loading content. Herein, we synthesized a micellar DDS using γ-benzyloxy substituted poly(ε...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/acs.biomac.9b01742
更新日期：2020-04-13 00:00:00
abstract：:In the present study, novel bionanocomposite materials with tunable properties were successfully prepared using a poly(lactic acid) (PLA) matrix and acetylated microfibrillated cellulose (MFC) as reinforcing agent. The acetylation of MFC was confirmed by FTIR and (13)C CP-MAS NMR spectroscopies. The grafting of acetyl...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm901186u
更新日期：2010-02-08 00:00:00
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
更新日期：2014-01-13 00:00:00
abstract：:In this work, biodegradable branched polycationic polymers were synthesized by Michael addition polymerization from different amine monomers and the triacrylate monomer trimethylolpropane triacrylate. The polymers varied in the number of amines that dissociate in different pH ranges, which are considered to be benefic...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm901147k
更新日期：2010-03-08 00:00:00
abstract：:In this study, we demonstrate for the first time the fabrication of carboxylated chitosan nanocrystals (ChsNC) with high degree of deacetylation (DDA) at >80% and narrow size distribution. We also studied its application as a sustainable support material for metal-based catalysts. Carboxylated chitin nanocrystals (ChN...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/acs.biomac.0c00201
更新日期：2020-06-08 00:00:00
abstract：:The application of nanoparticles comprising amphiphilic block copolymers for the delivery of drugs is a subject of great interest as they hold promise for more effective and selective therapies. In order to achieve this ambition, it is of critical importance to develop our understanding of the self-assembly mechanisms...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/acs.biomac.0c00169
更新日期：2020-06-08 00:00:00
abstract：:A series of well-defined thermoresponsive diblock copolymers (PEO45-b-PtNEAn, n=22, 44, 63, 91, 172) were prepared by the atom transfer radical polymerization of trans-N-(2-ethoxy-1,3-dioxan-5-yl) acrylamide (tNEA) using a poly(ethylene oxide) (PEO45) macroinitiator. All copolymers are water-soluble at low temperature...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm400180n
更新日期：2013-05-13 00:00:00
abstract：:Molecular orientation distributions in the crystalline and amorphous regions of a biaxially oriented poly(L-lactic acid) film were analyzed fully by polarized Raman spectroscopy. Raman bands at 926 and 875 cm(-1) were chosen for the determination of the most probable molecular orientation distribution functions for th...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm060326l
更新日期：2006-09-01 00:00:00
abstract：:We present a synthetic approach toward soft, glycooligomer-functionalized microgel particles mimicking carbohydrate presenting cell surfaces and analyze their specific binding to a model lectin (Concanavalin A, ConA). Focusing on multivalent presentation, a series of sequence-controlled glycooligomers with varying spa...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/acs.biomac.8b00790
更新日期：2018-08-13 00:00:00
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
更新日期：2005-11-01 00:00:00
abstract：:The copper(II) complex formation equilibria of N-(2-carboxyethyl)chitosans with three different degrees of substitution (DS = 0.42, 0.92, and 1.61) were studied in aqueous solution by pH-potentiometric and UV-spectrophotometric techniques. It was demonstrated that the complexation model of CE-chitosans depends on DS: ...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm049597r
更新日期：2005-01-01 00:00:00
abstract：:We study the fibrillation pathway of ovalbumin protein and report the simultaneous formation of several types of fibrils, with clear structural and physical differences. We compare the fibrillation mechanisms at low pH with and without salt, and follow the kinetics of fibrils growth by atomic force microscopy (AFM), s...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm301481v
更新日期：2012-12-10 00:00:00
abstract：:Eosinophil cationic protein (ECP) is an antimicrobial protein belonging to the superfamily of RNase A. ECP exhibits a broad spectrum of action against bacteria and, at higher concentrations, displays cytotoxic activity to eukaryotic cells. Recently, a powerful aggregation activity for lipid vesicles and for the gram-n...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm100334u
更新日期：2010-08-09 00:00:00
abstract：:Natural silk spinning offers several advantages over the synthetic fiber spinning, although the underlying mechanisms of this process are yet to be fully elucidated. Silkworm silks, specifically B. mori, comprise two main proteins: fibroin, which forms the fiber, and sericin, a coextruded coating that acts as a matrix...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/acs.biomac.7b00549
更新日期：2017-08-14 00:00:00
abstract：:Bovine serum albumin (BSA) and poly(diallyldimethylammonium chloride) (PDADMAC) spontaneously form, over a range of ionic strength I and pH, dense fluids rich in both macroions. To study their nanostructure, these coacervates were prepared at low I and high pH (strong interaction) or at high I and lower pH (weaker int...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm049174p
更新日期：2005-05-01 00:00:00
abstract：:Well-defined linear poly(acryloyl glucosamine) (PAGA) exhibiting molar masses ranging from 3 to 120 K and low polydispersities have been prepared via reversible addition-fragmentation chain transfer polymerization (RAFT) in aqueous solution without recourse to protecting group chemistry. The livingness of the process ...
journal_title：Biomacromolecules
pub_type： 杂志文章
doi：10.1021/bm0506086
更新日期：2006-01-01 00:00:00
