Abstract:
:Glycosaminoglycan (GAG)-protein binding governs critically important signaling events in living matter. Aiming at a quantitative analysis of the involved processes, we herein present a thermodynamic study of the interaction of the model GAG heparin and lysozyme in aqueous solution. Heparin is a highly charged linear polyelectrolyte with a charge parameter of 2.9 (37 °C). The binding constant Kb was determined by ITC as a function of the temperature and ionic strength adjusted through the concentration cs of added salt. The dependence on salt concentration cs was used to determine the net number of released counterions. Moreover, the binding constant at a reference salt concentration of 1 M Kb(1 M) was determined by extrapolation. The dependence on temperature of Kb was used to dissect the binding free energy ΔGb into the respective enthalpies ΔHb and entropies ΔSb together with the specific heat Δc p . A strong enthalpy-entropy cancelation was found similar to the results for many other systems. The binding free energy ΔGb could furthermore be split up into a part ΔGci due to counterion release and a residual part ΔGres. The latter quantity reflects specific contributions as, e.g., salt bridges, van der Waals interactions, or hydrogen bonds. The entire analysis shows that heparin-lysozyme interactions are mainly caused by counterion release; that is, ca. three counterions are being released upon binding one lysozyme molecule. Our reported approach of quantifying interactions between glycosaminoglycans and proteins is generally applicable and suitable to provide new insights in the physical modulation of biomolecular signals.
journal_name
Biomacromoleculesjournal_title
Biomacromoleculesauthors
Walkowiak JJ,Ballauff M,Zimmermann R,Freudenberg U,Werner Cdoi
10.1021/acs.biomac.0c00780subject
Has Abstractpub_date
2020-11-09 00:00:00pages
4615-4625issue
11eissn
1525-7797issn
1526-4602journal_volume
21pub_type
杂志文章abstract::Structures of three pectic arabinogalactans, one from Vernonia kotschyana (Vk2a) and two from Cochlospermum tinctorium (Ct50A1 and Ct50A2), and their complement fixation and induction of B cell proliferation in vitro were compared. The polysaccharide Vk2a expressed potent biological activity in both assays compared wi...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/bm050355g
更新日期:2006-01-01 00:00:00
abstract::Surface modification of biodegradable vascular grafts is an important strategy to improve the in situ endothelialization of tissue engineered vascular grafts (TEVGs) and prevent major complications associated with current synthetic grafts. Important strategies for improving endothelialization include increasing endoth...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/bm501853s
更新日期:2015-02-09 00:00:00
abstract::Biodegradable polyrotaxanes (PRXs) were synthesized from bis-amino-terminated poly(L-lactide) (PLLA) and alpha-cyclodextrin (alpha-CD), combined with capping by bulky end groups at the amino-termini of PLLA through enzymatically cleavable peptide linkages. The crystalline structure of the PRXs in the solid state was i...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/bm900440v
更新日期:2009-08-10 00:00:00
abstract::RNA interference (RNAi) requires the intracellular delivery of RNA molecules to initiate the neutralization of targeted mRNA molecules, inhibiting the expression or translation of the targeted gene. Current polymers and lipids that are used to deliver RNA molecules are generally required to be positively charged, to a...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/acs.biomac.8b01321
更新日期:2019-01-14 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::Covalently modified albumin (BSA) microparticles were developed for potential use as an adjuvant in mucosal vaccines against hepatitis B. To synthesize consistent protein particles, a covalent approach was proposed to modify BSA. Our strategy was to bond maleic anhydride (MA) molecules to BSA structure by nucleophilic...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/bm400859z
更新日期:2013-09-09 00:00:00
abstract::Recently antifreeze proteins (AFP) have been the subject of many structure-function relationship studies regarding their antifreeze activity. Attempts have been made to elucidate the structure-function relationship by various amino acid substitutions, but to our knowledge there has been no successful from first princi...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/bm000004w
更新日期:2000-07-01 00:00:00
abstract::Nanocoating of individual mammalian cells with polymer layers has been of increasing interest in biotechnology and biomedical engineering applications. Electrostatic layer-by-layer (LbL) deposition of polyelectrolytes on negatively charged cell surfaces has been utilized for cell nanocoatings using synthetic or natura...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/acs.biomac.0c00523
更新日期:2020-07-13 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 Vitamin E (vitE)-labeled PEIs (PEI-vitEn) were synthesized and showed excellent complexation ability with plasmid DNA (pDNA). The cellular uptake of PEI-vitEn/pDNA complexes was greatly enhanced with the increase of vitE labeling, which is much better than that of control PEI25 in three different cell line...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/acs.biomac.6b00776
更新日期:2016-10-10 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::Mechanically fibrillated cellulose nanofibrils (CNFs) have attracted special attention as building blocks for the development of advanced materials and composites. A correlation exists between CNF morphology and the properties of the materials they form. However, this correlation is often evaluated indirectly by proce...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/acs.biomac.9b00432
更新日期:2019-07-08 00:00:00
abstract::In this work, we have analyzed the structural, topographical, and surface dilatational characteristics of pure beta-lactoglobulin adsorbed films and the effect of the self-assembly of monoglycerides (monopalmitin or monoolein) in beta-lactoglobulin films at the air-water interface. Measurements were performed in a sin...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/bm060144r
更新日期:2006-09-01 00:00:00
abstract::Silk fibroin (SF) protein, produced by silkworm Bombyx mori, is a promising biomaterial, while sophorolipid (SL) is an amphiphilic functional biosurfactant synthesized by nonpathogenic yeast Candida bombicola. SL is a mixture of two forms, acidic (ASL) and lactonic (LSL), which when added to SF results in accelerated ...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/acs.biomac.6b01069
更新日期:2016-10-10 00:00:00
abstract::Silk fibroin hydrogels with tunable properties could be obtained from aqueous fibroin solutions (4.2 w/v %) in a short period of time. This was achieved by the addition of ethylene glycol diglycidyl ether (EGDE) into the reaction solution. Introduction of EGDE cross-links between the fibroin molecules decreases the mo...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/bm300006r
更新日期:2012-04-09 00:00:00
abstract::Herein we present an innovative approach to produce biocompatible, degradable, and stealth polymeric nanoparticles based on poly(lipoic acid), stabilized by a PEG-ended surfactant. Taking advantage of the well-known thiol-induced polymerization of lipoic acid, a universal and nontoxic nanovector consisted of a solid c...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/acs.biomac.0c01321
更新日期:2020-12-21 00:00:00
abstract::Polymer conjugation increases an enzyme's circulation time and stability for use as a therapeutic agent, but this attachment indubitably affects its properties. Covalent attachment of multiple polyethylene glycol chains with sizes of either 2, 5, 10, or 20 kDa increases the molecular weight and hydrodynamic radius of ...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/bm1006954
更新日期:2010-12-13 00:00:00
abstract::Spider dragline silk exhibits an extraordinary toughness and is typically composed of two types of major ampullate spidroins (MaSp1 and MaSp2), differing in their proline content and hydrophobicity. In this paper, we recombinantly produced an unusual but naturally occurring short major ampullate spidroin (MaSp1s) as a...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/acs.biomac.7b00090
更新日期:2017-04-10 00:00:00
abstract::Control of the photoluminescence properties of cellulose is conducted by introduction of conducting polymers including fluorene (F) and 3-hexylthiophene (3HT) on cellulose surface through FeCl3 oxidative polymerization. The UV-vis absorption peak of cellulose grafted with the 3-hexylthiophene and fluorene copolymer wa...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/acs.biomac.7b01067
更新日期:2017-12-11 00:00:00
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
更新日期:2016-01-11 00:00:00
abstract::Nanoparticles with high aspect ratios have favorable attributes for drug delivery and bioimaging applications based on their enhanced tissue penetration and tumor homing properties. Here, we investigated a novel filamentous viral nanoparticle (VNP) based on the Pepino mosaic virus (PepMV), a relative of the establishe...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/acs.biomac.8b01365
更新日期:2019-01-14 00:00:00
abstract::Benefiting from their inherent localized and controlled release properties, hydrogels are ideal delivery systems for therapeutic drugs or nanoparticles. In particular, applications of hydrogels for the delivery and release of photoresponsive drugs or nanoparticles are receiving increasing attention. However, the effec...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/acs.biomac.7b00725
更新日期:2017-10-09 00:00:00
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
更新日期:2020-06-08 00:00:00
abstract::Despite recent advances in tumor treatment through cancer immunotherapy, the efficacy of this approach remains to be improved. Looking forward to high rates of objective clinical response, cancer immunotherapy combined with chemotherapy has gained increasing attention recently. Here, we constructed liposomes with matr...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/acs.biomac.8b01510
更新日期:2019-02-11 00:00:00
abstract::Chimeric DNA containing parallel (ps) and antiparallel (aps) duplex elements as well as poly-dC tracts were designed and synthesized. Oligonucleotide duplexes with ps chain orientation containing reverse Watson-Crick dA-dT base pairs and short d(C)2 tails are stabilized under slightly acidic conditions by hemiprotonat...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/bm301471d
更新日期:2012-12-10 00:00:00
abstract::Highly fluorescent N-substituted 1-cyanobenz[f]isoindole chitosans (CBI-CSs) with various degrees of N-substitution (DS) were synthesized by reacting chitosan (CS) with naphthalene-2,3-dicarboxaldehyde (NDA) in the presence of cyanide under mild acidic conditions. Introduction of 1-cyanobenz[f]isoindole moieties into ...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/bm5004459
更新日期:2014-08-11 00:00:00
abstract::A cellulose-chitin hybrid polysaccharide having alternatingly beta(1-->4)-linked D-glucose (Glc) and N-acetyl-d-glucosamine (GlcNAc) was synthesized via two modes of enzymatic polymerization. First, a sugar oxazoline monomer of Glcbeta(1-->4)GlcNAc (1) was designed as a transition-state analogue substrate (TSAS) monom...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/bm060094q
更新日期:2006-05-01 00:00:00
abstract::Restorative medicine has a constant need for improved scaffold materials. Degradable biopolymers often suffer from uncontrolled chemical or enzymatic hydrolysis by the host. The need for a second surgery on the other hand is a major drawback for nondegradable scaffold materials. In this paper we report the design and ...
journal_title:Biomacromolecules
pub_type: 杂志文章
doi:10.1021/bm800327s
更新日期:2008-09-01 00:00:00
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
更新日期:2020-12-14 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