Volume 20, Issue 43 2403322
Research Article

An Organic–Inorganic Hydrogel with Exceptional Mechanical Properties via Anion-Induced Synergistic Toughening for Accelerating Osteogenic Differentiation

Hongmei Luo

Hongmei Luo

College of Polymer Science and Engineering, Sichuan University, Chengdu, 610065 China

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Qifeng Mu

Qifeng Mu

RIKEN Center for Emergent Matter Science, 2-1 Hirosawa, Wako, Saitama, 351-0198 Japan

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Ruijie Zhu

Ruijie Zhu

Faculty of Engineering, Hokkaido University, Sapporo, 060–8628 Japan

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Min Li

Min Li

College of Polymer Science and Engineering, Sichuan University, Chengdu, 610065 China

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Huanwei Shen

Huanwei Shen

College of Polymer Science and Engineering, Sichuan University, Chengdu, 610065 China

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Honglang Lu

Honglang Lu

College of Polymer Science and Engineering, Sichuan University, Chengdu, 610065 China

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Longyu Hu

Longyu Hu

College of Polymer Science and Engineering, Sichuan University, Chengdu, 610065 China

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Jiajun Tian

Jiajun Tian

College of Polymer Science and Engineering, Sichuan University, Chengdu, 610065 China

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Wei Cui

Corresponding Author

Wei Cui

College of Polymer Science and Engineering, Sichuan University, Chengdu, 610065 China

E-mail: [email protected]; [email protected]

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Rong Ran

Corresponding Author

Rong Ran

College of Polymer Science and Engineering, Sichuan University, Chengdu, 610065 China

E-mail: [email protected]; [email protected]

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First published: 19 June 2024
Citations: 4

Abstract

Mineralized bio-tissues achieve exceptional mechanical properties through the assembly of rigid inorganic minerals and soft organic matrices, providing abundant inspiration for synthetic materials. Hydrogels, serving as an ideal candidate to mimic the organic matrix in bio-tissues, can be strengthened by the direct introduction of minerals. However, this enhancement often comes at the expense of toughness due to interfacial mismatch. This study reveals that extreme toughening of hydrogels can be realized through simultaneous in situ mineralization and salting-out, without the need for special chemical modification or additional reinforcements. The key to this strategy lies in harnessing the kosmotropic and precipitation behavior of specific anions as they penetrate a hydrogel system containing both anion-sensitive polymers and multivalent cations. The resulting mineralized hydrogels demonstrate significant improvements in fracture stress, fracture energy, and fatigue threshold due to a multiscale energy dissipation mechanism, with optimal values reaching 12 MPa, 49 kJ m−2, and 2.98 kJ m−2. This simple strategy also proves to be generalizable to other anions, resulting in tough hydrogels with osteoconductivity for promoting in vitro mineralization of human adipose-derived mesenchymal stem cells. This work introduces a universal route to toughen hydrogels without compromising other parameters, holding promise for biological applications demanding integrated mechanical properties.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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