Ionic gel formation of a (pseudo)alginate characterised by an alternating MG sequence produced by epimerising mannuronan with AlgE4

被引:25
作者
Dentini, Mariella [1 ]
Rinaldi, Gianluca
Barbetta, Andrea
Risica, Daniela
Anselmi, Claudio
Skjak-Braek, Gudmund
机构
[1] Univ Roma La Sapienza, Dept Chem, I-00185 Rome, Italy
[2] Norwegian Univ Sci & Technol, Dept Biotechnol, N-7034 Trondheim, Norway
关键词
pseudo(alginates)/calcium gels; alternating mannuronic-guluronic sequences; rheology; circular dichroism; molecular dynamics;
D O I
10.1016/j.carbpol.2006.06.020
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The scope of this paper is the characterization, in terms of viscoelastic and mechanical properties, of ionic gels obtained from solutions of pseudoalginates characterized by a strictly alternating MG sequence (ALG(47%, 0%GG)) in the presence of calcium ions. ALG(47%, 0%GG) was obtained using a recombinantly produced mannuronan C-5 epimerase, named AlgE4 which catalyses the conversion of mannuronic residues into guluronic mannuronic (GM) blocks. It was established that the kinetics of gelation as well as the mechanical properties and degree of syneresis of the ensuing gels are markedly dependent on both polymer concentration and Ca2+ content. The molecular dynamic investigation was carried out on a comparative basis between poly(MG) vs. poly(G) and demonstrated that in the case of poly(MG) the structural unit composed by two calcium paired MG oligomer enjoy a higher degree of flexibility in comparison to the equivalent structure based on GG sequence. Furthermore, the electrostatic interaction between Ca2+ ions and carboxylate groups of M and G units is the main driving force to gel formation. (c) 2006 Elsevier Ltd. All rights reserved.
引用
收藏
页码:465 / 473
页数:9
相关论文
共 35 条
[1]   A WELL-BEHAVED ELECTROSTATIC POTENTIAL BASED METHOD USING CHARGE RESTRAINTS FOR DERIVING ATOMIC CHARGES - THE RESP MODEL [J].
BAYLY, CI ;
CIEPLAK, P ;
CORNELL, WD ;
KOLLMAN, PA .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (40) :10269-10280
[2]   Molecular basis of Ca2+-induced gelation in alginates and pectins:: The egg-box model revisited [J].
Braccini, I ;
Pérez, S .
BIOMACROMOLECULES, 2001, 2 (04) :1089-1096
[3]   Conformational and configurational features of acidic polysaccharides and their interactions with calcium ions:: a molecular modeling investigation [J].
Braccini, I ;
Grasso, RP ;
Pérez, S .
CARBOHYDRATE RESEARCH, 1999, 317 (1-4) :119-130
[4]  
Case D.A., 2002, AMBER 7
[5]   Rheology of kappa-carrageenan in mixtures of sodium and cesium iodide: Two types of gels [J].
Chronakis, IS ;
Piculell, L ;
Borgstrom, J .
CARBOHYDRATE POLYMERS, 1996, 31 (04) :215-225
[6]   A 2ND GENERATION FORCE-FIELD FOR THE SIMULATION OF PROTEINS, NUCLEIC-ACIDS, AND ORGANIC-MOLECULES [J].
CORNELL, WD ;
CIEPLAK, P ;
BAYLY, CI ;
GOULD, IR ;
MERZ, KM ;
FERGUSON, DM ;
SPELLMEYER, DC ;
FOX, T ;
CALDWELL, JW ;
KOLLMAN, PA .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1995, 117 (19) :5179-5197
[7]   Acid gel formation in (pseudo) alginates with and without G blocks produced by epimerising mannuronan with C5 epimerases [J].
Dentini, M ;
Rinaldi, G ;
Barbetta, A ;
Risica, D ;
Skjåk-Bræk, G .
CARBOHYDRATE POLYMERS, 2006, 63 (04) :519-526
[8]   Comparative studies on solution characteristics of mannuronan epimerized by C-5 epimerases [J].
Dentini, M ;
Rinaldi, G ;
Risica, D ;
Barbetta, A ;
Skjåk-Bræk, G .
CARBOHYDRATE POLYMERS, 2005, 59 (04) :489-499
[9]   New hypothesis on the role of alternating sequences in calcium-alginate gels [J].
Donati, I ;
Holtan, S ;
Morch, YA ;
Borgogna, M ;
Dentini, M ;
Skjåk-Bræk, G .
BIOMACROMOLECULES, 2005, 6 (02) :1031-1040
[10]   Alginate based new materials [J].
Draget, KI ;
SkjakBraek, G ;
Smidsrod, O .
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES, 1997, 21 (1-2) :47-55