Diffusion-Controllable Biomineralization Conducted In Situ in Hydrogels Based on Reversibly Cross-Linked Hyperbranched Polyglycidol

被引:21
作者
Gosecki, Mateusz [1 ]
Kazmierski, Slawomir [1 ]
Gosecka, Monika [1 ]
机构
[1] Polish Acad Sci, Ctr Mol & Macromol Studies, Ul Sienkiewicza 112, PL-90363 Lodz, Poland
关键词
THERMORESPONSIVE HYDROGELS; ALKALINE-PHOSPHATASE; CALCIUM-CARBONATE; MESH SIZE; ACID; STABILITY; ENZYMES; MINERALIZATION; TEMPERATURE; ADSORPTION;
D O I
10.1021/acs.biomac.7b01071
中图分类号
Q5 [生物化学]; Q7 [分子生物学];
学科分类号
071010 ; 081704 ;
摘要
We present biocompatible hydrogel systems suitable for biomineralization processes based on hyperbranched polyglycidol cross-linked with acrylamide copolymer bearing carbonyl coordinated boronic acid. At neutral pH, diol functional groups of HbPGL react with boronic acid of polyacrylamide to generate 3D network in water by the formation of boronic ester cross-links. The dynamic associative/dissociative characteristics of the cross-links makes the network reversible. The presented hydrogels display self healing properties and are injectable, facilitating gap filing of bone tissue. The H-1 HR MAS DOSY NMR studies reveal that acrylamide copolymer plays the role of the network framework, whereas HbPGL macromolecules, due to their compact structure, move between reactive sites of the copolymer. The influence of the copolymer macromolecules entanglements and overall polymer concentrations on macromolecules mobility and stress relaxation processes is investigated. The process of hydrogel biomineralization results from hydrolysis of 1-naphthyl phosphate calcium salt catalyzed by encapsulation in hydrogel alkaline phosphatase. The environment of the hydrogel is entirely neutral toward the enzyme. However, the activity of alkaline phosphatase encapsulated within the hydrogel structure is diffusion-limited. In this article, based on the detailed characteristics of three model hydrogel systems, we demonstrate the influence of the hydrogel permeability on the encapsulated enzyme activity and calcium phosphate formation rate. The Ill HR MAS DOSY NMR is used to monitor diffusion low-molecular weight compound within hydrogels, whereas P-31 HR MAS NMR facilitates monitoring of the progress of biomineralization in situ within hydrogels. The results show a direct correlation between low molecular diffusivity in hydrogels and network dynamics. We demonstrate that the morphology of in situ-generated calcium phosphate within three model HbPGL/poly(AM-ran-APBA) hydrogels of different low molecular permeability varies substantially from sparsely deployed large, well-defined crystals to an even distribution within the polymers polycrystalline continuous network.
引用
收藏
页码:3418 / 3431
页数:14
相关论文
共 36 条
[1]   Enzymatically Cross-Linked Hyperbranched Polyglycerol Hydrogels as Scaffolds for Living Cells [J].
Wu, Changzhu ;
Strehmel, Christine ;
Achazi, Katharina ;
Chiapisi, Leonardo ;
Dernedde, Jens ;
Lensen, Marga C. ;
Gradzielski, Michael ;
Ansorge-Schumacher, Marion B. ;
Haag, Rainer .
BIOMACROMOLECULES, 2014, 15 (11) :3881-3890
[2]   Bioinspired Reversibly Cross-linked Hydrogels Comprising Polypeptide Micelles Exhibit Enhanced Mechanical Properties [J].
Ghoorchian, Ali ;
Simon, Joseph R. ;
Bharti, Bhuvnesh ;
Han, Wei ;
Zhao, Xuanhe ;
Chilkoti, Ashutosh ;
Lopez, Gabriel P. .
ADVANCED FUNCTIONAL MATERIALS, 2015, 25 (21) :3122-3130
[3]   Tough and stretchy double-network hydrogels based on in situ interpenetration of polyacrylamide and physically cross-linked polyurethane [J].
Wu, Feng ;
Chen, Lei ;
Wang, Yidi ;
Fei, Bin .
JOURNAL OF MATERIALS SCIENCE, 2019, 54 (18) :12131-12144
[4]   PREPARATION AND PROPERTIES OF ANTIBACTERIAL mZnO/PAAm NANOCOPOSITE HYDROGELS WITH CONTROLLABLE PHYSICAL/CHEMICAL DOUBLE CROSS-LINKED STRUCTURE [J].
Liu, Sheng ;
Xia, Meng-ge ;
Zhang, Yan ;
Jiang, Xiao-ze ;
Meng, Zhou-qi ;
Wu, Yong-tao ;
Cheng, Yan-hua ;
Zhu, Mei-fang .
ACTA POLYMERICA SINICA, 2013, (10) :1270-1276
[5]   Novel Gelatin-based Eco-friendly Adhesive with a Hyperbranched Cross-linked Structure [J].
Wang, Xuechuan ;
Zhu, Jingbo ;
Liu, Xinhua ;
Zhang, Hui Jie ;
Zhu, Xing .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2020, 59 (13) :5500-5511
[6]   Synthesis and properties of biodegradable hydrogels based on cross-linked natural rubber and cassava starch [J].
Vudjung, Chaiwute ;
Saengsuwan, Sayant .
JOURNAL OF ELASTOMERS AND PLASTICS, 2017, 49 (07) :574-594
[7]   Hydrogels with high mechanical strength cross-linked by a rosin-based cross-linking agent [J].
Zhang, Haibo ;
Huang, Xin ;
Jiang, Jianxin ;
Shang, Shibin ;
Song, Zhanqian .
RSC ADVANCES, 2017, 7 (67) :42541-42548
[8]   Evaluation of solute diffusion and polymer relaxation in cross-linked hyaluronic acid hydrogels: experimental measurement and relaxation modeling [J].
Kodavaty, Jagadeeshwar ;
Deshpande, Abhijit P. .
POLYMER BULLETIN, 2021, 78 (05) :2605-2626
[9]   Evaluation of solute diffusion and polymer relaxation in cross-linked hyaluronic acid hydrogels: experimental measurement and relaxation modeling [J].
Jagadeeshwar Kodavaty ;
Abhijit P. Deshpande .
Polymer Bulletin, 2021, 78 :2605-2626
[10]   Fabrication and Properties of in Situ Cross-Linked Supramolecular Gel Based on Host-Guest Interaction [J].
Shao, Minglu ;
Gong, Jing ;
Cheng, Mengjie ;
Fu, Lipei ;
Liao, Kaili ;
Chang, Ailian .
CHEMISTRYSELECT, 2024, 9 (37)