Sequential Assembly of Mutually-Interactive Supramolecular Hydrogels and Fabrication of Multi-Domain Materials

TY - JOUR

T1 - Sequential Assembly of Mutually-Interactive Supramolecular Hydrogels and Fabrication of Multi-Domain Materials

AU - Piras, Carmen Cristina

AU - Smith, David Kelham

N1 - © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy. Further copying may not be permitted; contact the publisher for details.

PY - 2019/8

Y1 - 2019/8

N2 - We report a two-component self-sorting hydrogel based on acylhydrazide and carboxylic acid derivatives of 1,3:2,4-dibenzylidene-D-sorbitol (DBS-CONHNH2 and DBS-COOH). A heat-cool cycle induces the self-assembly of DBS-CONHNH2, followed by the self-assembly of DBS-COOH induced by decreasing pH. Although the networks are formed sequentially, there is spectroscopic evidence of interactions between them, which impact on the mechanical properties and significantly enhance the ability of these low-molecular-weight gelators (LMWGs) to form gels when mixed. The DBS-COOH network can be switched ‘off’ and ‘on’ within the two-component gel via a pH change. Using a photoacid generator, the two-component gel can be prepared combining the thermal trigger with photo-irradiation. Photopatterned self-assembly of DBS-COOH within a pre-formed DBS-CONHNH2 gel under a mask yields spatially-controlled multi-domain gels. Different gel domains can have different functions, for example controlling the rate of release of heparin incorporated into the gel, or directing gold nanoparticle assembly. Such photo-patterned multi-component hydrogels have potential applications in regenerative medicine or bio-nano-electronics.

AB - We report a two-component self-sorting hydrogel based on acylhydrazide and carboxylic acid derivatives of 1,3:2,4-dibenzylidene-D-sorbitol (DBS-CONHNH2 and DBS-COOH). A heat-cool cycle induces the self-assembly of DBS-CONHNH2, followed by the self-assembly of DBS-COOH induced by decreasing pH. Although the networks are formed sequentially, there is spectroscopic evidence of interactions between them, which impact on the mechanical properties and significantly enhance the ability of these low-molecular-weight gelators (LMWGs) to form gels when mixed. The DBS-COOH network can be switched ‘off’ and ‘on’ within the two-component gel via a pH change. Using a photoacid generator, the two-component gel can be prepared combining the thermal trigger with photo-irradiation. Photopatterned self-assembly of DBS-COOH within a pre-formed DBS-CONHNH2 gel under a mask yields spatially-controlled multi-domain gels. Different gel domains can have different functions, for example controlling the rate of release of heparin incorporated into the gel, or directing gold nanoparticle assembly. Such photo-patterned multi-component hydrogels have potential applications in regenerative medicine or bio-nano-electronics.

KW - gels

KW - self-assembly

KW - supramolecular chemistry

UR - http://www.scopus.com/inward/record.url?scp=85070068278&partnerID=8YFLogxK

U2 - 10.1002/chem.201902158

DO - 10.1002/chem.201902158

M3 - Article

SN - 0947-6539

VL - 25

SP - 11318

EP - 11326

JO - Chemistry : A European Journal

JF - Chemistry : A European Journal

IS - 48

ER -