Tunable glycyrrhizic acid supramolecular hydrogels via metal ion complexation
Glycyrrhizic acid (GA) is a natural edible chiral triterpene saponin that can undergo hierarchical self-assembly in water to form supramolecular hydrogels. Customizing the properties of GA supramolecular hydrogels is crucial for their wide food and biomedical applications, and the incorporation of s...
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Elsevier
2024-03-01
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| Series: | Giant |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2666542524000055 |
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| author | Xinke Yu Mengyue Xu Jiyang Cai Qing Li Yunyi Yang Zhili Wan Xiaoquan Yang |
| author_facet | Xinke Yu Mengyue Xu Jiyang Cai Qing Li Yunyi Yang Zhili Wan Xiaoquan Yang |
| author_sort | Xinke Yu |
| collection | DOAJ |
| description | Glycyrrhizic acid (GA) is a natural edible chiral triterpene saponin that can undergo hierarchical self-assembly in water to form supramolecular hydrogels. Customizing the properties of GA supramolecular hydrogels is crucial for their wide food and biomedical applications, and the incorporation of specific metal ions can be an attractive way for this purpose. Herein, this study investigates the effects of metal ions with different valence states and concentrations on the linear and nonlinear rheological properties and network structures of GA supramolecular hydrogels. Monovalent metal ions (Na+ and K+), exhibiting weak binding affinity to GA, rely on the electrostatic screening effects at high concentrations (e.g., 50 mM) to enhance the GA interfibrillar interactions and thus the formation of a more compact and ordered gel network, which displays a pronounced nonlinear rheological behavior with a typical transition from elastic to viscous response. Polyvalent metal ions (Ca2+, Zn2+, and Al3+), owing to their greater charge density and stronger binding with GA, significantly enhance the network strength of the hydrogels at low concentrations (e.g., 5 mM). Nonetheless, at high ion concentrations (e.g., 50 mM), the GA-Mn+ forms discrete aggregated network structures due to excessively strong cation-carboxylate complexation, leading to the irregular nonlinear rheological responses and the lower resistance to large deformations. These findings can deepen our understanding of the highly tunable rheological behaviors and network structures of GA hydrogels, which demonstrates a new possibility for the design and development of responsive natural supramolecular hydrogels with controlled properties through the strategy of metal ion complexation. |
| first_indexed | 2024-03-08T11:42:56Z |
| format | Article |
| id | doaj.art-e400bb51d602405fada6355c50289412 |
| institution | Directory Open Access Journal |
| issn | 2666-5425 |
| language | English |
| last_indexed | 2024-04-24T20:12:32Z |
| publishDate | 2024-03-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Giant |
| spelling | doaj.art-e400bb51d602405fada6355c502894122024-03-23T06:26:12ZengElsevierGiant2666-54252024-03-0117100240Tunable glycyrrhizic acid supramolecular hydrogels via metal ion complexationXinke Yu0Mengyue Xu1Jiyang Cai2Qing Li3Yunyi Yang4Zhili Wan5Xiaoquan Yang6Laboratory of Food Proteins and Colloids, School of Food Science and Engineering, Guangdong Province Key Laboratory for Green Processing of Natural Products and Product Safety, South China University of Technology, Guangzhou 510640, PR ChinaLaboratory of Food Proteins and Colloids, School of Food Science and Engineering, Guangdong Province Key Laboratory for Green Processing of Natural Products and Product Safety, South China University of Technology, Guangzhou 510640, PR China; Laboratory of Physics and Physical Chemistry of Foods, Wageningen University, Bornse Weilanden 9, 6708WG Wageningen, The NetherlandsLaboratory of Food Proteins and Colloids, School of Food Science and Engineering, Guangdong Province Key Laboratory for Green Processing of Natural Products and Product Safety, South China University of Technology, Guangzhou 510640, PR ChinaLaboratory of Food Proteins and Colloids, School of Food Science and Engineering, Guangdong Province Key Laboratory for Green Processing of Natural Products and Product Safety, South China University of Technology, Guangzhou 510640, PR ChinaLaboratory of Food Proteins and Colloids, School of Food Science and Engineering, Guangdong Province Key Laboratory for Green Processing of Natural Products and Product Safety, South China University of Technology, Guangzhou 510640, PR ChinaLaboratory of Food Proteins and Colloids, School of Food Science and Engineering, Guangdong Province Key Laboratory for Green Processing of Natural Products and Product Safety, South China University of Technology, Guangzhou 510640, PR China; Overseas Expertise Introduction Center for Discipline Innovation of Food Nutrition and Human Health (111 Center), Guangzhou 510640, PR China; Corresponding author.Laboratory of Food Proteins and Colloids, School of Food Science and Engineering, Guangdong Province Key Laboratory for Green Processing of Natural Products and Product Safety, South China University of Technology, Guangzhou 510640, PR ChinaGlycyrrhizic acid (GA) is a natural edible chiral triterpene saponin that can undergo hierarchical self-assembly in water to form supramolecular hydrogels. Customizing the properties of GA supramolecular hydrogels is crucial for their wide food and biomedical applications, and the incorporation of specific metal ions can be an attractive way for this purpose. Herein, this study investigates the effects of metal ions with different valence states and concentrations on the linear and nonlinear rheological properties and network structures of GA supramolecular hydrogels. Monovalent metal ions (Na+ and K+), exhibiting weak binding affinity to GA, rely on the electrostatic screening effects at high concentrations (e.g., 50 mM) to enhance the GA interfibrillar interactions and thus the formation of a more compact and ordered gel network, which displays a pronounced nonlinear rheological behavior with a typical transition from elastic to viscous response. Polyvalent metal ions (Ca2+, Zn2+, and Al3+), owing to their greater charge density and stronger binding with GA, significantly enhance the network strength of the hydrogels at low concentrations (e.g., 5 mM). Nonetheless, at high ion concentrations (e.g., 50 mM), the GA-Mn+ forms discrete aggregated network structures due to excessively strong cation-carboxylate complexation, leading to the irregular nonlinear rheological responses and the lower resistance to large deformations. These findings can deepen our understanding of the highly tunable rheological behaviors and network structures of GA hydrogels, which demonstrates a new possibility for the design and development of responsive natural supramolecular hydrogels with controlled properties through the strategy of metal ion complexation.http://www.sciencedirect.com/science/article/pii/S2666542524000055Glycyrrhizic acidSupramolecular hydrogelsMetal ion complexationLarge amplitude oscillation shear (LAOS)Lissajous-Bowditch curvesGel networks |
| spellingShingle | Xinke Yu Mengyue Xu Jiyang Cai Qing Li Yunyi Yang Zhili Wan Xiaoquan Yang Tunable glycyrrhizic acid supramolecular hydrogels via metal ion complexation Giant Glycyrrhizic acid Supramolecular hydrogels Metal ion complexation Large amplitude oscillation shear (LAOS) Lissajous-Bowditch curves Gel networks |
| title | Tunable glycyrrhizic acid supramolecular hydrogels via metal ion complexation |
| title_full | Tunable glycyrrhizic acid supramolecular hydrogels via metal ion complexation |
| title_fullStr | Tunable glycyrrhizic acid supramolecular hydrogels via metal ion complexation |
| title_full_unstemmed | Tunable glycyrrhizic acid supramolecular hydrogels via metal ion complexation |
| title_short | Tunable glycyrrhizic acid supramolecular hydrogels via metal ion complexation |
| title_sort | tunable glycyrrhizic acid supramolecular hydrogels via metal ion complexation |
| topic | Glycyrrhizic acid Supramolecular hydrogels Metal ion complexation Large amplitude oscillation shear (LAOS) Lissajous-Bowditch curves Gel networks |
| url | http://www.sciencedirect.com/science/article/pii/S2666542524000055 |
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