Tensile Reinforcement of Silk Films by the Addition of Telechelic-Type Polyalanine.

Abstract:

:An appropriate modification technique for silk materials is needed to effectively improve their physical properties for specific applications. A telechelic-type polyalanine (T-polyA) was synthesized by papain-catalyzed polymerization as a novel reinforcing agent for silk materials. A silk fibroin obtained from Bombyx mori was homogeneously doped with T-polyA, and casting a solution of silk fibroin and T-polyA in 1,1,1,3,3,3-hexafluoro-2-propanol (HFIP) resulted in a robust and transparent film. Tensile deformation studies of the silk composite film containing T-polyA with prestretching revealed that the tensile strength and toughness were enhanced relative to those of a silk-only film. To determine the capability of T-polyA to reinforce the tensile property of silk films, the secondary structure in the silk composite film was characterized by wide-angle X-ray diffraction (WAXD) analysis. Antiparallel β-sheet structures of T-polyA and GAGAGS motifs of silk fibroin formed independently in the prestretched composite film. In addition, measuring the tensile deformation and performing WAXD analysis simultaneously demonstrated that the β-sheet structures of both T-polyA and the silk fibroin were aligned along the stretching direction and that T-polyA had no significant effect on the final morphology of the silk crystal domains. The silk film was toughened by the addition of T-polyA because of the generation of the T-polyA β-sheet in the amorphous region of the composite film. This work provides novel insight into the design and development of tough silk materials with controlled and aligned β-sheet structures.

journal_name

Biomacromolecules

journal_title

Biomacromolecules

authors

Tsuchiya K,Masunaga H,Numata K

doi

10.1021/acs.biomac.6b01891

subject

Has Abstract

pub_date

2017-03-13 00:00:00

pages

1002-1009

issue

3

eissn

1525-7797

issn

1526-4602

journal_volume

18

pub_type

杂志文章
  • A new model for the substitution patterns in the polymer chain of polysaccharide derivatives.

    abstract::A new mathematical model is presented for the analysis of the substituent distribution in the polymer chain of polysaccharide derivatives. For the first time, the influence of substitution on the reactivity of neighbored monomer units is taken into account. The model was applied to various cellulose and amylose ethers...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm000093c

    authors: Mischnick P,Hennig C

    更新日期:2001-04-01 00:00:00

  • Pore sizes in hydrated dextran microspheres.

    abstract::The average pore size of hydrated dextran microspheres is derived from rheological and protein release data. The microspheres were prepared by cross-linking an aqueous solution of methacrylated dextran emulsified in a continuous poly(ethylene glycol) phase. The rheological data were obtained using a novel micromanipul...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm005574a

    authors: Stenekes RJ,De Smedt SC,Demeester J,Sun G,Zhang Z,Hennink WE

    更新日期:2000-01-01 00:00:00

  • Molecular dynamics study of complexes of poly(glutamate) and dodecyltrimethylammonium.

    abstract::The supramolecular organization of self-assembled stoichiometric complexes formed by dodecyltrimethylammonium cations and ionized poly(gamma-glutamic) acid has been investigated in chloroform solution. Atomistic molecular dynamics simulations have been performed considering three different starting conformations for t...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm060927c

    authors: Zanuy D,Alemán C

    更新日期:2007-02-01 00:00:00

  • Characterization of resilin-based materials for tissue engineering applications.

    abstract::Modular proteins have emerged as powerful tools in tissue engineering because both the mechanical and biochemical properties can be precisely controlled through amino acid sequence. Resilin is an attractive candidate for use in modular proteins because it is well-known for having low stiffness, high fatigue lifetime, ...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm301129b

    authors: Renner JN,Cherry KM,Su RS,Liu JC

    更新日期:2012-11-12 00:00:00

  • Unraveling the Correlations between Conformation, Lubrication, and Chemical Stability of Bottlebrush Polymers at Interfaces.

    abstract::In the present study, we monitored the conformation and chemical stability of a hydrophilic bottlebrush (BB) polymer in pure water and buffered saline solutions. We correlated these parameters to lubricating and wear protecting properties. Using the surface forces apparatus (SFA), we show that the BB polymer partially...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.7b01063

    authors: Faivre J,Shrestha BR,Xie G,Delair T,David L,Matyjaszewski K,Banquy X

    更新日期:2017-12-11 00:00:00

  • pH-responsive polymeric micelle carriers for siRNA drugs.

    abstract::The ability of small interfering RNA (siRNA) to efficiently silence the expression of specific genes provides the basis for exciting new therapies based on RNA interference (RNAi). The efficient intracellular delivery of siRNA from cell uptake through the endosomal trafficking pathways into the cytoplasm remains a sig...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm100652w

    authors: Convertine AJ,Diab C,Prieve M,Paschal A,Hoffman AS,Johnson PH,Stayton PS

    更新日期:2010-11-08 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

  • Polycarbonates with Potent and Selective Antimicrobial Activity toward Gram-Positive Bacteria.

    abstract::The resistance developed by life-threatening bacteria toward conventional antibiotics has become a major concern in public health. To combat antibiotic resistance, there has been a significant interest in the development of antimicrobial cationic polymers due to the ease of synthesis and low manufacturing cost compare...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.6b01385

    authors: Nimmagadda A,Liu X,Teng P,Su M,Li Y,Qiao Q,Khadka NK,Sun X,Pan J,Xu H,Li Q,Cai J

    更新日期:2017-01-09 00:00:00

  • Synthesis and characterization of core-shell star copolymers for in vivo PET imaging applications.

    abstract::The synthesis of core-shell star copolymers via living free radical polymerization provides a convenient route to three-dimensional nanostructures having a poly(ethylene glycol) outer shell, a hydrophilic inner shell bearing reactive functional groups, and a central hydrophobic core. By starting with well-defined line...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm7014152

    authors: Fukukawa K,Rossin R,Hagooly A,Pressly ED,Hunt JN,Messmore BW,Wooley KL,Welch MJ,Hawker CJ

    更新日期:2008-04-01 00:00:00

  • Collagenase-labile polyurethane urea synthesis and processing into hollow fiber membranes.

    abstract::As a means to stimulate wound healing, a hollow fiber membrane system might be placed within a wound bed to provide local and externally regulated controlled delivery of regenerative factors. After sufficient healing, it would be desirable to triggerably degrade these fibers as opposed to pulling them out. Accordingly...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm500552f

    authors: Fu HL,Hong Y,Little SR,Wagner WR

    更新日期:2014-08-11 00:00:00

  • Synthesis and characterizations of in situ cross-linkable gelatin and 4-arm-PPO-PEO hybrid hydrogels via enzymatic reaction for tissue regenerative medicine.

    abstract::In situ cross-linkable hybrid hydrogels composed of gelatin and 4-arm-polypropylene oxide-polyethylene oxide (Tetronic) was developed as an injectable scaffold for tissue regeneration. The gelatin was modified by hydroxyphenyl propionic acid (HPA) and the Tetronic was conjugated with tyramines (Tet-TA). The hydrogels ...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm201712z

    authors: Park KM,Lee Y,Son JY,Oh DH,Lee JS,Park KD

    更新日期:2012-03-12 00:00:00

  • Injectable Polypeptide Hydrogels with Tunable Microenvironment for 3D Spreading and Chondrogenic Differentiation of Bone-Marrow-Derived Mesenchymal Stem Cells.

    abstract::Bone-marrow-derived mesenchymal stem cells (BMSCs) possess vast potential for tissue engineering and regenerative medicine. In this study, an injectable hydrogel comprising poly(l-glutamic acid)-graft-tyramine (PLG-g-TA) with tunable microenvironment was developed via enzyme-catalyzed cross-linking and used as an arti...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.6b00884

    authors: Ren K,Cui H,Xu Q,He C,Li G,Chen X

    更新日期:2016-12-12 00:00:00

  • Copolymerization of 2-carboxyisopropylacrylamide with N-isopropylacrylamide accelerates cell detachment from grafted surfaces by reducing temperature.

    abstract::Acrylic acid (AAc) has been utilized to introduce reactive carboxyl groups to a temperature-responsive polymer, poly(N-isopropylacrylamide) (PIPAAm). However, AAc introduction shifts the copolymer phase transition temperatures higher and dampens the steep homopolymer phase transition with increasing AAc content. We pr...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm025692t

    authors: Ebara M,Yamato M,Hirose M,Aoyagi T,Kikuchi A,Sakai K,Okano T

    更新日期:2003-03-01 00:00:00

  • Chondroitin sulfate coatings display low platelet but high endothelial cell adhesive properties favorable for vascular implants.

    abstract::This study highlights the advantages of chondroitin sulfate (CS) as a sublayer combining selective low-fouling properties, low-platelet adhesion and pro-adhesive properties on endothelial cells, making CS promising for vascular graft applications. These properties were evaluated by comparing CS with well-known low-fou...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm5003762

    authors: Thalla PK,Fadlallah H,Liberelle B,Lequoy P,De Crescenzo G,Merhi Y,Lerouge S

    更新日期:2014-07-14 00:00:00

  • Secondary Structure Transition and Critical Stress for a Model of Spider Silk Assembly.

    abstract::Spiders spin their silk from an aqueous solution to a solid fiber in ambient conditions. However, to date, the assembly mechanism in the spider silk gland has not been satisfactorily explained. In this paper, we use molecular dynamics simulations to model Nephila clavipes MaSp1 dragline silk formation under shear flow...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.5b01246

    authors: Giesa T,Perry CC,Buehler MJ

    更新日期:2016-02-08 00:00:00

  • Characterization of methylprednisolone esters of hyaluronan in aqueous solution: conformation and aggregation behavior.

    abstract::Methylprednisolone steroid esters of hyaluronan differing in degree of functionalization and molecular weight were investigated in aqueous solution. Conformation and aggregation phenomena were elucidated by means of circular dichroism, viscometry, rheology, and nuclear magnetic resonance, mainly by (1)H pulsed field g...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm049221d

    authors: Taglienti A,Valentini M,Sequi P,Crescenzi V

    更新日期:2005-05-01 00:00:00

  • Modification of cellulose films by adsorption of CMC and chitosan for controlled attachment of biomolecules.

    abstract::The adsorption of human immunoglobulin G (hIgG) and bovine serum albumin (BSA) on cellulose supports were investigated. The dynamics and extent of related adsorption processes were monitored by surface plasmon resonance (SPR) and quartz crystal microbalance with dissipation monitoring (QCM-D). Amine groups were instal...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm201236a

    authors: Orelma H,Filpponen I,Johansson LS,Laine J,Rojas OJ

    更新日期:2011-12-12 00:00:00

  • Synthesis and properties of degradable poly(urethane urea)s to be used for ligament reconstructions.

    abstract::In the present study we describe the synthesis, wet spinning, mechanical testing, and degradation of poly(urethane urea)s (PUURs) intended for clinical use in anterior cruciate ligament (ACL) reconstruction. The effects of soft segment chemical composition and molar mass and the kind of diamine chain extender on the m...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm025535u

    authors: Gisselfält K,Edberg B,Flodin P

    更新日期:2002-09-01 00:00:00

  • Understanding Poly(vinyl alcohol)-Mediated Ice Recrystallization Inhibition through Ice Adsorption Measurement and pH Effects.

    abstract::The development of improved cryopreservative materials is necessary to enable complete recovery of living cells and tissue after frozen storage. Remarkably, poly(vinyl alcohol) (PVA) displays some of the same cryoprotective properties as many antifreeze proteins found in cold tolerant organisms. In particular, PVA is ...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.7b01502

    authors: Burkey AA,Riley CL,Wang LK,Hatridge TA,Lynd NA

    更新日期:2018-01-08 00:00:00

  • Polypeptide-based aerosol nanoparticles: self-assembly and control of conformation by solvent and thermal annealing.

    abstract::Nanoconfined self-assemblies within aerosol nanoparticles and control of the secondary structures are shown here upon ionically complexing poly(L-lysine) (PLL) with dodecylbenzenesulfonic acid (DBSA) surfactant and using solvents chloroform, 1-propanol, or dimethylformamide. Different solvent volatilities and drying t...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm500704e

    authors: Rahikkala A,Junnila S,Vartiainen V,Ruokolainen J,Ikkala O,Kauppinen E,Raula J

    更新日期:2014-07-14 00:00:00

  • Photoresponsive Micelle-Incorporated Doxorubicin for Chemo-Photodynamic Therapy to Achieve Synergistic Antitumor Effects.

    abstract::A combination of chemo-photodynamic therapy has been manifested as a promising strategy for efficient cancer treatment due to the enhanced therapeutic efficacy. Here, we designed doxorubicin (DOX)-loaded photoresponsive micelles (DPRMs) based on a combination of chlorin e6 (Ce6) and lipoic acid (LA) conjugated methoxy...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.8b00607

    authors: Kim DH,Hwang HS,Na K

    更新日期:2018-08-13 00:00:00

  • Identification of a marine benthic P(3HB)-degrading bacterium isolate and characterization of its P(3HB) depolymerase.

    abstract::A poly[(R)-3-hydroxybutyrate] (P(3HB))-degrading marine bacterium (strain NK-1, JCM10458) was isolated from the Pacific Ocean deep-sea floor (1165 m in depth) in Japan. The organism was a motile and Gram negative, aerobic, and rod-shaped bacterium, and its DNA had a guanine-plus-cytosine content of 57.7 mol%. On the b...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm9900186

    authors: Kasuya K,Mitomo H,Nakahara M,Akiba A,Kudo T,Doi Y

    更新日期:2000-07-01 00:00:00

  • Development of a hybrid dextrin hydrogel encapsulating dextrin nanogel as protein delivery system.

    abstract::Dextrin, a glucose polymer with low molecular weight, was used to develop a fully resorbable hydrogel, without using chemical initiators. Dextrin was first oxidized (oDex) with sodium periodate and then cross-linked with adipic acid dihidrazide, a nontoxic cross-linking molecule. Furthermore, a new bidimensional compo...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm2015834

    authors: Molinos M,Carvalho V,Silva DM,Gama FM

    更新日期:2012-02-13 00:00:00

  • Two types of hydrophobic aggregates in aqueous solutions of chitosan and its hydrophobic derivative.

    abstract::The aggregation phenomena in aqueous solutions of hydrophobically modified (HM) chitosan, containing 4 mol % of n-dodecyl side chains, were studied by viscometry and fluorescence spectroscopy with pyrene as a probe. The results are compared with those for unmodified chitosan. Surprisingly, fluorescence data reveal the...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm005649a

    authors: Philippova OE,Volkov EV,Sitnikova NL,Khokhlov AR,Desbrieres J,Rinaudo M

    更新日期:2001-07-01 00:00:00

  • Preparation of lactose-modified cellulose films by a nonaqueous enzymatic reaction and their biofunctional characteristics as a scaffold for cell culture.

    abstract::Enzymatic glyco-modification of transparent cellulose films with lactose was achieved by nonaqueous biocatalysis, and rat hepatocyte attachment behavior to the lactose-modified cellulose films was investigated. Regenerated cellulose films were incubated with lactose using a surfactant-enveloped cellulase in lithium ch...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm900089j

    authors: Esaki K,Yokota S,Egusa S,Okutani Y,Ogawa Y,Kitaoka T,Goto M,Wariishi H

    更新日期:2009-05-11 00:00:00

  • Design and synthesis of water-soluble glycopolymers bearing breast tumor marker and enhanced lipophilicity for solid-phase assays.

    abstract::Water-soluble T-antigen containing glycopolymers [Gal beta(1,3)-GalNAc alpha) having a high degree of lipophilicity were synthesized from poly[N-(acryloxy)succinimide] (6-10) by amidation with an amine-ending T-antigen derivative (3) and various amines of increasing alkyl chain length (ammonia and methyl-, ethyl-, and...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm005593k

    authors: Baek MG,Roy R

    更新日期:2000-01-01 00:00:00

  • Ionic Hydrogel Based on Chitosan Cross-Linked with 6-Phosphogluconic Trisodium Salt as a Drug Delivery System.

    abstract::In this work, 6-phosphogluconic trisodium salt (6-PG-Na+) is introduced as a new aqueous and nontoxic cross-linking agent to obtain ionic hydrogels. Here, it is shown the formation of hydrogels based on chitosan cross-linked with 6-PG-Na+. This formulation is obtained by ionic interaction of cationic groups of polymer...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.8b00108

    authors: Martínez-Martínez M,Rodríguez-Berna G,Gonzalez-Alvarez I,Hernández MJ,Corma A,Bermejo M,Merino V,Gonzalez-Alvarez M

    更新日期:2018-04-09 00:00:00

  • Biocompatibility of plasma enhanced chemical vapor deposited poly(2-hydroxyethyl methacrylate) films for biomimetic replication of the intestinal basement membrane.

    abstract::It is recognized that topographical features such as ridges and grooves can dramatically influence cell phenotype, motivating the development of substrates with precisely biomimetic topography for study of the influence on cultured cells. Intestinal basement membrane topography has been precisely replicated using plas...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm100209b

    authors: Pfluger CA,Burkey DD,Wang L,Sun B,Ziemer KS,Carrier RL

    更新日期:2010-06-14 00:00:00

  • Factors controlling the deposition of silk fibroin nanofibrils during layer-by-layer assembly.

    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

    authors: de Moraes MA,Crouzier T,Rubner M,Beppu MM

    更新日期:2015-01-12 00:00:00

  • Imaging of homeostatic, neoplastic, and injured tissues by HA-based probes.

    abstract::An increase in hyaluronan (HA) synthesis, cellular uptake, and metabolism occurs during the remodeling of tissue microenvironments following injury and during disease processes such as cancer. We hypothesized that multimodality HA-based probes selectively target and detectably accumulate at sites of high HA metabolism...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm201143c

    authors: Veiseh M,Breadner D,Ma J,Akentieva N,Savani RC,Harrison R,Mikilus D,Collis L,Gustafson S,Lee TY,Koropatnick J,Luyt LG,Bissell MJ,Turley EA

    更新日期:2012-01-09 00:00:00