2021
DOI: 10.1038/s41467-021-24416-x
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Life and death of colloidal bonds control the rate-dependent rheology of gels

Abstract: Colloidal gels exhibit rich rheological responses under flowing conditions. A clear understanding of the coupling between the kinetics of the formation/rupture of colloidal bonds and the rheological response of attractive gels is lacking. In particular, for gels under different flow regimes, the correlation between the complex rheological response, the bond kinetics, microscopic forces, and an overall micromechanistic view is missing in previous works. Here, we report the bond dynamics in short-range attractiv… Show more

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Cited by 40 publications
(23 citation statements)
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References 58 publications
(74 reference statements)
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“…Decreasing K eq below ∼50 M –1 leads to a precipitous drop in p , which drives particle–particle contacts at rest, 24 , 29 , 36 as evidenced by the higher η r , shear thinning under steady shear, and solid-like SAOS response ( Figures 3 A, S17, and S18 ). 19 , 65 As unbonded surface thiol groups could potentially ionize, we note that the drop in p and transition from antithixotropy to shear thinning could also be related to an increase in particle surface charge, which alters nanoparticle dynamics 67 and stability within the homopolymer melt. The system would be expected to be in the concentrated polymer brush (CPB) regime from a minimum graft density of ∼0.07 chains/nm 2 to the maximum theoretical graft density of 0.5 chains/nm 2 set by the interfacial −SH density.…”
Section: Resultsmentioning
confidence: 96%
“…Decreasing K eq below ∼50 M –1 leads to a precipitous drop in p , which drives particle–particle contacts at rest, 24 , 29 , 36 as evidenced by the higher η r , shear thinning under steady shear, and solid-like SAOS response ( Figures 3 A, S17, and S18 ). 19 , 65 As unbonded surface thiol groups could potentially ionize, we note that the drop in p and transition from antithixotropy to shear thinning could also be related to an increase in particle surface charge, which alters nanoparticle dynamics 67 and stability within the homopolymer melt. The system would be expected to be in the concentrated polymer brush (CPB) regime from a minimum graft density of ∼0.07 chains/nm 2 to the maximum theoretical graft density of 0.5 chains/nm 2 set by the interfacial −SH density.…”
Section: Resultsmentioning
confidence: 96%
“…We think that our method will help quickly produce a wide variety of different DNA-coated colloids from a single feed-stock and optimize their designs so applications and experiments requiring many different DNA-coated colloids come within reach. Our method may also help expand the use of DNA-coated particles beyond crystallization and self-assembly to sub-fields of colloid science such as gelation and rheology [44,45,46].…”
Section: Discussionmentioning
confidence: 99%
“…Furthermore, the rheology of such colloidal gels can be rate-and history-dependent. This is especially important at low Mason numbers where the ratio of shearing forces to attractive forces is dominating over hydrodynamic effects [31].…”
Section: Capillary Force and Influence Of Bridge Shapementioning
confidence: 99%