Deoxyguanosine phosphate mediated sacrificial bonds promote synergistic mechanical properties in nacre-mimetic nanocomposites.

Abstract:

:We show that functionalizing polymer-coated colloidal nanoplatelets with guanosine groups allows synergistic increase of mechanical properties in nacre-mimetic lamellar self-assemblies. Anionic montmorillonite (MTM) was first coated using cationic poly(diallyldimethylammonium chloride) (PDADMAC) to prepare core-shell colloidal platelets, and subsequently the remaining chloride counterions allowed exchange to functional anionic 2'-deoxyguanosine 5'-monophosphate (dGMP) counterions, containing hydrogen bonding donors and acceptors. The compositions were studied using elemental analysis, scanning and transmission electron microscopy, wide-angle X-ray scattering, and tensile testing. The lamellar spacing between the clays increases from 1.85 to 2.14 nm upon addition of the dGMP. Adding dGMP increases the elastic modulus, tensile strength, and strain 33.0%, 40.9%, and 5.6%, respectively, to 13.5 GPa, 67 MPa, and 1.24%, at 50% relative humidity. This leads to an improved toughness seen as a ca. 50% increase of the work-to-failure. This is noteworthy, as previously it has been observed that connecting the core-shell nanoclay platelets covalently or ionically leads to increase of the stiffness but to reduced strain. We suggest that the dynamic supramolecular bonds allow slippage and sacrificial bonds between the self-assembling nanoplatelets, thus promoting toughness, still providing dynamic interactions between the platelets.

journal_name

Biomacromolecules

journal_title

Biomacromolecules

authors

Martikainen L,Walther A,Seitsonen J,Berglund L,Ikkala O

doi

10.1021/bm400056c

subject

Has Abstract

pub_date

2013-08-12 00:00:00

pages

2531-5

issue

8

eissn

1525-7797

issn

1526-4602

journal_volume

14

pub_type

杂志文章
  • Structural effects on the biodistribution and positron emission tomography (PET) imaging of well-defined (64)Cu-labeled nanoparticles comprised of amphiphilic block graft copolymers.

    abstract::The synthesis of poly(methyl methacrylate-co-methacryloxysuccinimide-graft-poly(ethylene glycol)) (PMMA-co-PMASI-g-PEG) via living free radical polymerization provides a convenient route to well-defined amphiphilic graft copolymers having a controllable number of reactive functional groups, variable length PEG grafts,...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm700541e

    authors: Pressly ED,Rossin R,Hagooly A,Fukukawa K,Messmore BW,Welch MJ,Wooley KL,Lamm MS,Hule RA,Pochan DJ,Hawker CJ

    更新日期:2007-10-01 00:00:00

  • Noninvasive in vivo monitoring of the biofate of 195 kDa poly(vinyl alcohol) by multispectral fluorescence imaging.

    abstract::A comprehensive knowledge of the in vivo fate of polymers is essential for their potential application in humans. In this study, the body distribution, accumulation, and elimination processes of intraperitoneally (ip) administered poly(vinyl alcohol) (PVA) in mice were investigated in detail. Two derivatives of PVA (1...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm200899h

    authors: Schädlich A,Naolou T,Amado E,Schöps R,Kressler J,Mäder K

    更新日期:2011-10-10 00:00:00

  • Effects of molecular size and surface hydrophobicity on oligonucleotide interfacial dynamics.

    abstract::Single-molecule total internal reflection fluorescence microscopy was used to observe the dynamic behavior of polycytosine single-stranded DNA (ssDNA) (1-50 nucleotides long) at the interface between aqueous solution and hydrophilic (oligoethylene glycol-modified fused silica, OEG) and hydrophobic (octadecyltriethoxys...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm301289n

    authors: Monserud JH,Schwartz DK

    更新日期:2012-12-10 00:00:00

  • Biologically Functionalized Expanded Polytetrafluoroethylene Blood Vessel Grafts.

    abstract::Cardiovascular diseases plague human health because of the lack of transplantable small-diameter blood vessel (SDBV) grafts. Although expanded polytetrafluoroethylene (ePTFE) has the potential to be used as a biocompatible material for SDBV grafts, long-term patency is still the biggest challenge. As discussed in this...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.0c00897

    authors: Wang D,Xu Y,Lin YJ,Yilmaz G,Zhang J,Schmidt G,Li Q,Thomson JA,Turng LS

    更新日期:2020-09-14 00:00:00

  • Compatible ternary blends of chitosan/poly(vinyl alcohol)/poly(lactic acid) produced by oil-in-water emulsion processing.

    abstract::Ternary compatible blends of chitosan, poly(vinyl alcohol), and poly(lactic acid) were prepared by an oil-in-water (O/W) emulsion process. Solutions of chitosan in aqueous acetic acid, poly(vinyl alcohol) (PVA) in water, and poly(lactic acid) (PLA) in chloroform were blended with a high-shear mixer. PVA was used as an...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm101227q

    authors: Grande R,Carvalho AJ

    更新日期:2011-04-11 00:00:00

  • Efficient manipulation of nanoparticle-bound DNA via restriction endonuclease.

    abstract::As a programmable biopolymer, DNA has shown great potential in the fabrication and construction of nanometer-scale assemblies and devices. In this report, we described a strategy for efficient manipulation of gold nanoparticle-bound DNA using restriction endonuclease. The digestion efficiency of this restriction enzym...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm060517o

    authors: Qin WJ,Yung LY

    更新日期:2006-11-01 00:00:00

  • Effect of chitosan chain architecture on gene delivery: comparison of self-branched and linear chitosans.

    abstract::Chitosan possesses many characteristics of an ideal gene delivery system. However, the transfection efficiency of conventional chitosans is generally found to be low. In this study, we investigated the self-branching of chitosans as a strategy to improve its gene transfer properties without compromising its safety pro...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm1013525

    authors: Malmo J,Vårum KM,Strand SP

    更新日期:2011-03-14 00:00:00

  • Nonwoven Carboxylated Agarose-Based Fiber Meshes with Antimicrobial Properties.

    abstract::Hydrogel forming polysaccharides, such as the seaweed derived agarose, are well suited for wound dressing applications as they have excellent cell and soft tissue compatibility. For wound dressings, fibrous structure is desirable as the high surface area can favor adsorption of wound exudate and promote drug delivery....

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.6b01401

    authors: Forget A,Arya N,Randriantsilefisoa R,Miessmer F,Buck M,Ahmadi V,Jonas D,Blencowe A,Shastri VP

    更新日期:2016-12-12 00:00:00

  • Modular Polymer Antigens To Optimize Immunity.

    abstract::Subunit vaccines can have excellent safety profiles, but their ability to give rise to robust immune responses is often compromised. For glycan-based vaccines, insufficient understanding of B and T cell epitope combinations that yield optimal immune activation hinders optimization. To determine which antigen features ...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.9b01049

    authors: Bennett NR,Jarvis CM,Alam MM,Zwick DB,Olson JM,Nguyen HV,Johnson JA,Cook ME,Kiessling LL

    更新日期:2019-12-09 00:00:00

  • Development of a sialic acid-containing hydrogel of poly[N-(2-hydroxypropyl) methacrylamide]: characterization and implantation study.

    abstract::This study describes the preparation and the characterization of poly[ N-(2-hydroxypropyl methacrylamide)] hydrogel with bulk-modified saccharidic portion of ganglioside GM 3 (Neu5Ac-alpha2,3-Gal-beta1,4-Glc). The 3'-sialyllactose is a bioactive epitope recognized by many cell surface receptors on viruses, bacteria, a...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm800234r

    authors: Woerly S,Fort S,Pignot-Paintrand I,Cottet C,Carcenac C,Savasta M

    更新日期:2008-09-01 00:00:00

  • Engineered Polymeric Micelles for Combinational Oxidation Anticancer Therapy through Concurrent HO-1 Inhibition and ROS Generation.

    abstract::Cancer cells have a large amount of ROS (reactive oxygen species) because of disturbed ROS homeostasis. Cancer cells therefore undertake redox adaptation to drive proliferation in tumor environments and even survive during anticancer treatment by upregulating endogenous antioxidants. As one of antioxidant defense syst...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.8b01802

    authors: Noh J,Jung E,Lee J,Hyun H,Hong S,Lee D

    更新日期:2019-02-11 00:00:00

  • Polymers and Composites Derived from Castor Oil as Sustainable Materials and Degradable Biomaterials: Current Status and Emerging Trends.

    abstract::Recent years have seen rapid growth in utilizing vegetable oils to derive a wide variety of polymers to replace petroleum-based polymers for minimizing environmental impact. Nonedible castor oil (CO) can be extracted from castor plants that grow easily, even in an arid land. CO is a promising source for developing sev...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.0c01291

    authors: Chakraborty I,Chatterjee K

    更新日期:2020-12-14 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

  • Intracellular trafficking and subcellular distribution of a large array of HPMA copolymers.

    abstract::The basic physicochemical properties that determine the distribution and fate of synthetic macromolecules in living cells were characterized using fluorescently labeled HPMA (N-(2-hydroxypropyl)methacrylamide) copolymers. Twelve different classes of water-soluble copolymers were created by incorporating eight differen...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm801514x

    authors: Callahan J,Kopečkov P,Kopeček J

    更新日期:2009-07-13 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

  • Low-fouling, biospecific films prepared by the continuous assembly of polymers.

    abstract::We report that the continuous assembly of polymers (CAP) approach, mediated by ring-opening metathesis polymerization (ROMP), is a facile and versatile technology to prepare engineered nanocoatings for various biomedical applications. Low-fouling coatings on particles were obtained by the formation of multicomposition...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm400680d

    authors: Guntari SN,Wong EH,Goh TK,Chandrawati R,Blencowe A,Caruso F,Qiao GG

    更新日期:2013-08-12 00:00:00

  • Polymeric surfactants based on inulin, a polysaccharide extracted from chicory. 1. Synthesis and interfacial properties.

    abstract::Inulin, the polydisperse reserve polysaccharide from chicory, has been modified by carbamoylation in organic solvents. The reaction of inulin with a range of alkyl isocyanates resulted, after crystalization, in a variety of carbamoylated inulins from which the interfacial properties were determined. The medium and lon...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm015570l

    authors: Stevens CV,Meriggi A,Peristeropoulou M,Christov PP,Booten K,Levecke B,Vandamme A,Pittevils N,Tadros TF

    更新日期:2001-01-01 00:00:00

  • Agarose hydrogels embedded with pH-responsive diblock copolymer micelles for triggered release of substances.

    abstract::Hybrid agarose hydrogels embedded with pH-responsive diblock copolymers micelles were developed to achieve functional hydrogels capable of stimulus-triggered drug release. Specifically, a well-defined poly(ethylene oxide) (PEO)-based diblock copolymer, PEO-b-poly(2-(N,N-diisopropylamino)ethyl methacrylate) (PEO(113)-b...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm4005639

    authors: Jin N,Morin EA,Henn DM,Cao Y,Woodcock JW,Tang S,He W,Zhao B

    更新日期:2013-08-12 00:00:00

  • Quantitatively Fine-Tuning the Physicochemical and Biological Properties of Peptidic Polymers through Monodisperse PEGylation.

    abstract::In biomedicine, PEGylation is one of the most successful strategies to modify the physicochemical and biological properties of peptides, proteins, and other biomacromolecules. Because of the polydisperse nature of regular PEGs and limited PEGylation strategies, it is challenging to quantitatively fine-tune and accurat...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.9b01425

    authors: Wang X,Li Y,Wu T,Yang Z,Zheng X,Chen S,Zhou X,Jiang ZX

    更新日期:2020-02-10 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

  • Exploration of Blood Coagulation of N-Alkyl Chitosan Nanofiber Membrane in Vitro.

    abstract::N-Alkylated chitosan (NACS) may improve the blood clotting efficiency of chitosan (CS). To study its blood coagulation capability, a series of NACSs with various carbon chain lengths and degrees of substitution (DS) of alkyl groups were synthesized and characterized by FTIR, NMR, elemental analysis, and X-ray diffract...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.7b01492

    authors: Wang X,Guan J,Zhuang X,Li Z,Huang S,Yang J,Liu C,Li F,Tian F,Wu J,Shu Z

    更新日期:2018-03-12 00:00:00

  • Direct amidation of poly(gamma-glutamic acid) with benzylamine in dimethyl sulfoxide.

    abstract::Partially benzylamidated, amphipathic poly(gamma-glutamic acid) (BzPGA) was synthesized from poly(gamma-glutamic acid) (PGA) and benzylamine by direct amidation in dimethyl sulfoxide (DMSO). Benzylamine and PGA were heated in DMSO for 1 to 26 h at temperatures between 110 and 130 degrees C, producing derivatives of va...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm0612182

    authors: Novak L,Banyai I,Fleischer-Radu JE,Borbély J

    更新日期:2007-05-01 00:00:00

  • EGFR-Targeted Polymeric Mixed Micelles Carrying Gemcitabine for Treating Pancreatic Cancer.

    abstract::The objective of this study was to design GE11 peptide (YHWYGYTPQNVI) linked micelles of poly(ethylene glycol)-block-poly(2-methyl-2-carboxyl-propylene carbonate-graft-gemcitabine-graft-dodecanol (PEG-b-PCC-g-GEM-g-DC) for enhanced stability and target specificity of gemcitabine (GEM) to EGFR-positive pancreatic cance...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.5b01419

    authors: Mondal G,Kumar V,Shukla SK,Singh PK,Mahato RI

    更新日期:2016-01-11 00:00:00

  • Heterofunctional supports in enzyme immobilization: from traditional immobilization protocols to opportunities in tuning enzyme properties.

    abstract::A heterofunctional support for enzyme immobilization may be defined as that which possesses several distinct functionalities on its surface able to interact with a protein. We will focus on those supports in which a final covalent attachment between the enzyme and the support is achieved. Heterofunctionality sometimes...

    journal_title:Biomacromolecules

    pub_type: 杂志文章,评审

    doi:10.1021/bm400762h

    authors: Barbosa O,Torres R,Ortiz C,Berenguer-Murcia A,Rodrigues RC,Fernandez-Lafuente R

    更新日期:2013-08-12 00:00:00

  • Caspofungin Functionalized Polymethacrylates with Antifungal Properties.

    abstract::We describe the synthesis of hydrophilic poly(poly(ethylene glycol) methyl ether methacrylate) (PmPEGMA) and hydrophobic poly(methyl methacrylate) (PMMA) caspofungin conjugates by a post-polymerization modification of copolymers containing 10 mol % pentafluorophenyl methacrylate (PFPMA), which were obtained via revers...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/acs.biomac.0c00096

    authors: Alex J,González K,Kindel T,Bellstedt P,Weber C,Heinekamp T,Orasch T,Guerrero-Sanchez C,Schubert US,Brakhage AA

    更新日期:2020-06-08 00:00:00

  • Formation of a lamellar compound by reaction of acrylic acid crystallosolvated in highly crystalline beta-chitin.

    abstract::A lamellar compound resulted from reaction of acrylic acid inside crystalline beta-chitin and the structure was investigated. Beta-chitin acts like a layered crystal, having stacked molecular sheets composed of parallel chains bound in one direction by intermolecular amide hydrogen bonding. Small guest molecules can b...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm060643s

    authors: Saito Y,Tomotake Y,Shida S

    更新日期:2007-04-01 00:00:00

  • Decomposable hollow biopolymer-based capsules.

    abstract::Decomposable hollow capsules based on deoxyribonucleic acid (DNA) and a low molecular weight organic molecule, a naturally occurring polyamine, spermidine (SP), were formed by applying the layer-by-layer adsorption strategy to colloid particles, viz., assembling DNA/SP multilayers on colloids and subsequently removing...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm010052w

    authors: Schüler C,Caruso F

    更新日期:2001-10-01 00:00:00

  • Synthesis and characterization of biocompatible thermo-responsive gelators based on ABA triblock copolymers.

    abstract::The synthesis of biocompatible, thermo-responsive ABA triblock copolymers in which the outer A blocks comprise poly(N-isopropylacrylamide) and the central B block is poly(2-methacryloyloxyethyl phosphorylcholine) is achieved using atom transfer radical polymerization with a commercially available bifunctional initiato...

    journal_title:Biomacromolecules

    pub_type: 杂志文章

    doi:10.1021/bm049331k

    authors: Li C,Tang Y,Armes SP,Morris CJ,Rose SF,Lloyd AW,Lewis AL

    更新日期:2005-03-01 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

  • 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