Filler-induced strengthening is ubiquitous in materials science and is particularly well-established in polymeric nanocomposites. Despite having similar constituents, colloidal gels with solid filling exhibit distinct rheology, which is of practical interest to industry (e.g., lithium-ion batteries) yet remains poorly understood. We show, using experiments and simulations, that filling monotonically enhances the yield stress (i.e., strength) of colloidal gels while the elastic modulus (i.e., stiffness) first increases and then decreases. The latter softening effect results from a frustrated gel matrix at dense filling, evidenced by a growing interphase pressure. This structural frustration is, however, not detrimental to yielding resistance. Instead, fillers offer additional mechanical support to the gel backbone via percolating force chains, decreasing the yield strain at the same time. We develop a mechanistic picture of this phenomenology that leads us to a novel “filler-removal protocol,” making possible individual control over the strength and brittleness of a composite gel.
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January 2025
Research Article|
January 02 2025
Filled colloidal gel rheology: Strengthening, stiffening, and tunability
Yujie Jiang
;
Yujie Jiang
a)
1
Wenzhou Key Laboratory of Biomaterials and Engineering, Wenzhou Institute, University of Chinese Academy of Sciences
, Wenzhou, Zhejiang 325000, China
2
School of Mathematics and Physics, University of Science and Technology Beijing
, Beijing 100083, China
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Yang Cui;
Yang Cui
1
Wenzhou Key Laboratory of Biomaterials and Engineering, Wenzhou Institute, University of Chinese Academy of Sciences
, Wenzhou, Zhejiang 325000, China
3
School of Engineering, The University of Edinburgh
, King’s Buildings, Edinburgh EH9 3FG, United Kingdom
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Yankai Li;
Yankai Li
1
Wenzhou Key Laboratory of Biomaterials and Engineering, Wenzhou Institute, University of Chinese Academy of Sciences
, Wenzhou, Zhejiang 325000, China
3
School of Engineering, The University of Edinburgh
, King’s Buildings, Edinburgh EH9 3FG, United Kingdom
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Zhiwei Liu
;
Zhiwei Liu
1
Wenzhou Key Laboratory of Biomaterials and Engineering, Wenzhou Institute, University of Chinese Academy of Sciences
, Wenzhou, Zhejiang 325000, China
4
Oujiang Laboratory (Zhejiang Lab for Regenerative Medicine, Vision and Brain Health)
, Wenzhou, Zhejiang 325000, China
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Christopher Ness
;
Christopher Ness
b)
3
School of Engineering, The University of Edinburgh
, King’s Buildings, Edinburgh EH9 3FG, United Kingdom
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Ryohei Seto
Ryohei Seto
c)
1
Wenzhou Key Laboratory of Biomaterials and Engineering, Wenzhou Institute, University of Chinese Academy of Sciences
, Wenzhou, Zhejiang 325000, China
4
Oujiang Laboratory (Zhejiang Lab for Regenerative Medicine, Vision and Brain Health)
, Wenzhou, Zhejiang 325000, China
5
Graduate School of Information Science, University of Hyogo
, Kobe, Hyogo 650-0047, Japan
c)Author to whom correspondence should be addressed; electronic mail: [email protected]
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c)Author to whom correspondence should be addressed; electronic mail: [email protected]
a)
Electronic mail: [email protected]
b)
Electronic mail: [email protected]
J. Rheol. 69, 35–44 (2025)
Article history
Received:
May 12 2024
Accepted:
November 17 2024
Connected Content
A companion article has been published:
Counterintuitive finding shows that fillers can change composite materials strength and stiffness non-monotonically
Citation
Yujie Jiang, Yang Cui, Yankai Li, Zhiwei Liu, Christopher Ness, Ryohei Seto; Filled colloidal gel rheology: Strengthening, stiffening, and tunability. J. Rheol. 1 January 2025; 69 (1): 35–44. https://doi.org/10.1122/8.0000878
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