New hydrogen bonded supramolecular hydrogels were formed through simultaneously gelating two isomeric building units, 4-oxo-4-(2-pyridinylamino)butanoic acid (G1) and 4-oxo-4-(3-pyridinylamino)butanoic acid (G2...New hydrogen bonded supramolecular hydrogels were formed through simultaneously gelating two isomeric building units, 4-oxo-4-(2-pyridinylamino)butanoic acid (G1) and 4-oxo-4-(3-pyridinylamino)butanoic acid (G2) at various molar ratios in water.展开更多
New supramolecular hydrogels with the maximal sol-gel transition temperature (Tgel) of 95 ℃ were obtained by using gelators formed from 1,3,5-benzenetricarboxylic acid (BTA) and para-hydroxyl pyridine (PHP) or ...New supramolecular hydrogels with the maximal sol-gel transition temperature (Tgel) of 95 ℃ were obtained by using gelators formed from 1,3,5-benzenetricarboxylic acid (BTA) and para-hydroxyl pyridine (PHP) or meta-hydroxyl pyridine (MHP). The single crystal structure of the complex formed from BTA and ortho-hydroxyl pyridine (OHP) indicated that the molecules assembled into superstructure via both hydrogen bonds and π--π stacking interaction.展开更多
A new hydrogelator,2,6-di[N-(carboxypropylcarbonyl)amino] pyridine (defined as DPAP) was synthesized from 2,6-diaminopyridine and glutaric anhydride by a one-step procedure.Self-supporting supramolecular hyrogels were...A new hydrogelator,2,6-di[N-(carboxypropylcarbonyl)amino] pyridine (defined as DPAP) was synthesized from 2,6-diaminopyridine and glutaric anhydride by a one-step procedure.Self-supporting supramolecular hyrogels were formed through cooling DPAP aqueous solution and DPAP mixed solution of 1,4-dioxane and water with 1,4-dioxane content no more than 15 wt%.However,only fiber-like crystals were obtained in pure 1,4-dioxane system.SEM observation of the xerogels indicated that the gelator molecules assembled into large sized sheet-like aggregates.The powder XRD diagrams indicated that the xerogel samples possess onset diffraction at 5.6°(2θ),corresponding to a d spacing of 1.580 nm.Such a length corresponded well with DPAP molecular length of 1.895 nm if considering the aggregating chain tilting with respect to the normal to the layer plane.So the hydrogen bonded molecular chain direction represents the main aggregating direction.Meanwhile,the xerogel samples have another preferred diffraction at 16.64°(2θ) due to the preferred arrangement of molecules under the help of hydrophobic association,therefore resulting in two-dimensional aggregating structure.展开更多
Supramolecular nanofiber peptide assemblies had been used to construct functional hydrogel biomaterials and achieved great progress.Here,a new class of biphenyl-tripeptides with different C-terminal amino acids sequen...Supramolecular nanofiber peptide assemblies had been used to construct functional hydrogel biomaterials and achieved great progress.Here,a new class of biphenyl-tripeptides with different C-terminal amino acids sequences transposition were developed,which could self-assemble to form robust supramolecular nanofiber hydrogels from 0.7 to 13.8 kPa at ultra-low weight percent(about 0.27 wt%).Using molecular dynamics simulations to interrogate the physicochemical properties of designed biphenyl-tripeptide sequences in atomic detail,reasonable hydrogen bond interactions and“FF”brick(phenylalanine-phenylalanine)promoted the formation of supramolecular fibrous hydrogels.The biomechanical properties and intermolecular interactions were also analyzed by rheology and spectroscopy analysis to optimize amino acid sequence.Enhanced L929 cells adhesion and proliferation demonstrated good biocompatibility of the hydrogels.The storage modulus of BPAA-AFF with 10 nm nanofibers self-assembling was around 13.8 kPa,and the morphology was similar to natural extracellular matrix.These supramolecular nanofiber hydrogels could effectively support chondrocytes spreading and proliferation,and specifically enhance chondrogenic related genes expression and chondrogenic matrix secretion.Such biomimetic supramolecular short peptide biomaterials hold great potential in regenerative medicine as promising innovative matrices because of their simple and regular molecular structure and excellent biological performance.展开更多
基金The financial support from the National Natural Science Foundation of China (No. 20574041) is gratefully acknowledged.
文摘New hydrogen bonded supramolecular hydrogels were formed through simultaneously gelating two isomeric building units, 4-oxo-4-(2-pyridinylamino)butanoic acid (G1) and 4-oxo-4-(3-pyridinylamino)butanoic acid (G2) at various molar ratios in water.
基金support from the National Natural Science Foundation of China(Nos.20574041,20874055)
文摘New supramolecular hydrogels with the maximal sol-gel transition temperature (Tgel) of 95 ℃ were obtained by using gelators formed from 1,3,5-benzenetricarboxylic acid (BTA) and para-hydroxyl pyridine (PHP) or meta-hydroxyl pyridine (MHP). The single crystal structure of the complex formed from BTA and ortho-hydroxyl pyridine (OHP) indicated that the molecules assembled into superstructure via both hydrogen bonds and π--π stacking interaction.
文摘A new hydrogelator,2,6-di[N-(carboxypropylcarbonyl)amino] pyridine (defined as DPAP) was synthesized from 2,6-diaminopyridine and glutaric anhydride by a one-step procedure.Self-supporting supramolecular hyrogels were formed through cooling DPAP aqueous solution and DPAP mixed solution of 1,4-dioxane and water with 1,4-dioxane content no more than 15 wt%.However,only fiber-like crystals were obtained in pure 1,4-dioxane system.SEM observation of the xerogels indicated that the gelator molecules assembled into large sized sheet-like aggregates.The powder XRD diagrams indicated that the xerogel samples possess onset diffraction at 5.6°(2θ),corresponding to a d spacing of 1.580 nm.Such a length corresponded well with DPAP molecular length of 1.895 nm if considering the aggregating chain tilting with respect to the normal to the layer plane.So the hydrogen bonded molecular chain direction represents the main aggregating direction.Meanwhile,the xerogel samples have another preferred diffraction at 16.64°(2θ) due to the preferred arrangement of molecules under the help of hydrophobic association,therefore resulting in two-dimensional aggregating structure.
基金sponsored by National Key R&D Program of China(Grant No.2018YFC1105900)National Natural Science Foundation of China(32071352)+1 种基金Sichuan Province Key R&D Program(2019YFS0007)Sichuan university Innovation Spark Project(2018SCUH0089).
文摘Supramolecular nanofiber peptide assemblies had been used to construct functional hydrogel biomaterials and achieved great progress.Here,a new class of biphenyl-tripeptides with different C-terminal amino acids sequences transposition were developed,which could self-assemble to form robust supramolecular nanofiber hydrogels from 0.7 to 13.8 kPa at ultra-low weight percent(about 0.27 wt%).Using molecular dynamics simulations to interrogate the physicochemical properties of designed biphenyl-tripeptide sequences in atomic detail,reasonable hydrogen bond interactions and“FF”brick(phenylalanine-phenylalanine)promoted the formation of supramolecular fibrous hydrogels.The biomechanical properties and intermolecular interactions were also analyzed by rheology and spectroscopy analysis to optimize amino acid sequence.Enhanced L929 cells adhesion and proliferation demonstrated good biocompatibility of the hydrogels.The storage modulus of BPAA-AFF with 10 nm nanofibers self-assembling was around 13.8 kPa,and the morphology was similar to natural extracellular matrix.These supramolecular nanofiber hydrogels could effectively support chondrocytes spreading and proliferation,and specifically enhance chondrogenic related genes expression and chondrogenic matrix secretion.Such biomimetic supramolecular short peptide biomaterials hold great potential in regenerative medicine as promising innovative matrices because of their simple and regular molecular structure and excellent biological performance.