arxiv: 2605.14130 · v1 · submitted 2026-05-13 · ❄️ cond-mat.soft

Recognition: 2 theorem links

· Lean Theorem

The Role of Hydrogen Bridging Bonds in the Shear-Thickening and Jamming of Dense Suspensions

Hojin Kim , Samantha M. Livermore , Yongjin Shin , Heinrich M. Jaeger

Authors on Pith no claims yet

Pith reviewed 2026-05-15 01:41 UTC · model grok-4.3

classification ❄️ cond-mat.soft

keywords shear thickeninghydrogen bondingdense suspensionsjammingsolvent effectscornstarchrheologyfriction

0 comments

The pith

Solvent chain length flips dense suspensions from shear thickening to thinning.

A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.

Dense suspensions like cornstarch in liquid thicken sharply under shear because particles are pushed into frictional contact. The paper demonstrates that solvent molecules can form hydrogen bridges linking hydroxyl groups on neighboring particle surfaces, which strengthens that friction and promotes thickening or jamming. By lengthening the carbon backbone of the solvent from water and ethylene glycol to propanediol and butanediol, the bridging weakens and the same particle concentration switches to shear thinning. This shows solvent molecular structure can be used to control interparticle forces and flow behavior without changing the particles themselves.

Core claim

Experiments with cornstarch suspensions show that friction is enhanced by molecular bridging when hydrogen atoms at the ends of solvent molecules bond with hydroxyl groups on the surfaces of adjacent particles. Systematically varying the hydrogen bonding propensity by increasing the size of the backbone of the solvent molecule, from water to diols with up to 4 carbon atoms, produces a sudden transition from strong shear thickening in water and ethylene glycol to shear thinning in propanediol and butanediol at fixed particle weight fraction. Rheology data, density functional theory simulations, and fixed-rate pull tests together indicate that changes in solvent molecular structure affect both

What carries the argument

Hydrogen bridging bonds between solvent molecule ends and particle surface hydroxyl groups that increase interparticle friction under shear.

If this is right

Solvent choice alone can switch a fixed-concentration suspension between strong shear thickening and shear thinning.
Weaker bridging from larger solvent backbones eliminates the frictional contacts needed for jamming.
Both particle-solvent and solvent-solvent hydrogen bonds are altered by the solvent's molecular structure.
Rheological response can be tuned by solvent selection without modifying particle shape or surface chemistry.

Where Pith is reading between the lines

These are editorial extensions of the paper, not claims the author makes directly.

The same bridging strategy could be adapted to other particle-solvent pairs to engineer custom flow behavior in industrial slurries.
Natural suspensions in biological fluids might exhibit analogous solvent-dependent jamming based on molecular size and bonding.
Testing the transition in solvents with controlled bonding sites but different chain lengths would isolate the role of backbone size.
Extending the approach to non-hydroxyl particles would require identifying alternative bridging chemistries.

Load-bearing premise

The switch from thickening to thinning is caused mainly by changes in the solvent's hydrogen-bonding ability rather than its viscosity, dielectric constant, or other properties.

What would settle it

A set of solvents with matched viscosity and dielectric constant but systematically varied hydrogen-bonding strength that still produces the same thickening-to-thinning transition would support the bridging claim; failure to observe the transition would falsify it.

read the original abstract

Strong shear thickening and jamming in dense suspensions are driven by friction as particles are sheared into contact. Control over these frictional interactions can be achieved via particle shape and roughness, and also via the particles' surface chemistry and interactions with the surrounding solvent. We report on experiments with cornstarch suspensions where friction is enhanced by molecular bridging when hydrogen atoms at the ends of solvent molecules bond with hydroxyl groups on the surfaces of adjacent particles. We systematically vary the hydrogen bonding propensity by increasing the size of the backbone of the solvent molecule, from water to diols with up to 4 carbon atoms. For a fixed particle weight fraction, we find a sudden transition from strong shear thickening (in water and ethylene glycol) to shear thinning (in propanediol and butanediol). Combining data from rheology, density functional theory simulations, and fixed-rate pull tests, our results show how changes in the solvent's molecular structure affect both particle-solvent and solvent-solvent interactions, and how this can be used to tailor the shear thickening and jamming behavior of suspensions.

Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, simulated authors' rebuttal, and a circularity audit. Tearing a paper down is the easy half of reading it; the pith above is the substance, this is the friction.

Desk Editor's Note private letter to a colleague

The paper reports a clear switch from strong shear thickening to shear thinning in cornstarch as diol chain length increases, attributed to weaker hydrogen bridging, but the fixed-weight-fraction design leaves volume fraction and viscosity unmatched.

read the letter

The main thing to know is that this work finds a sharp transition in cornstarch suspensions: strong shear thickening holds in water and ethylene glycol but flips to shear thinning in propanediol and butanediol at fixed particle weight fraction. The authors link the change to reduced hydrogen bridging as the solvent backbone lengthens, supported by DFT calculations of bond energies and fixed-rate pull tests showing lower adhesion forces. That multi-method approach is the clearest strength; it gives a direct chemical handle on the frictional contacts that drive thickening and jamming. The observation itself looks new for this solvent family and could matter for anyone trying to tune suspension flow with solvent choice. The soft spot is the experimental design. Solvent densities and viscosities vary enough across the series that volume fractions differ by several percent and the hydrodynamic Peclet number shifts substantially. Those changes alone can move the shear rate where contacts dominate, independent of bonding strength. The abstract gives no sign of viscosity-matched or volume-fraction-normalized controls, so the attribution to hydrogen bridging rests on the assumption that hydrodynamic confounds are secondary. If the full paper has those checks, the claim strengthens; otherwise it needs them. This is for soft-matter groups working on dense suspensions and frictional rheology. Readers who need practical levers for suppressing jamming will get the most out of it. The core result and the supporting calculations are solid enough to warrant peer review, though the authors should expect requests for the missing controls or a clearer separation of hydrodynamic and bonding effects.

Referee Report

2 major / 2 minor

Summary. The paper claims that hydrogen bridging bonds formed by solvent molecules (water to C4 diols) between hydroxyl groups on cornstarch particles control frictional interactions, leading to a sharp transition from strong shear thickening and jamming (in water and ethylene glycol) to shear thinning (in propanediol and butanediol) at fixed particle weight fraction. This is supported by rheological data, DFT simulations of particle-solvent interactions, and fixed-rate pull tests.

Significance. If the attribution to hydrogen-bond bridging holds after controlling for hydrodynamic variables, the work provides a molecular route to tune shear thickening and jamming via solvent structure, complementing existing approaches based on particle roughness or shape. The multi-method approach (rheology + DFT + mechanical tests) is a strength and could enable predictive design of suspension rheology.

major comments (2)

[Abstract and experimental rheology] Abstract and § on experimental rheology: the transition is reported exclusively at fixed particle weight fraction. Solvent densities differ substantially (water 0.998 g cm⁻³, EG 1.113 g cm⁻³, 1,3-propanediol 1.036 g cm⁻³, 1,4-butanediol 1.017 g cm⁻³), producing up to ~5 % variation in particle volume fraction at typical loadings. This volume-fraction mismatch alters the proximity to jamming and the shear rate for contact formation independently of H-bond strength.
[Results and discussion] Results and discussion sections: solvent viscosities increase sharply across the series (water ~1 mPa s to butanediol ~71 mPa s at 25 °C), changing the hydrodynamic Peclet number and the shear-rate window where frictional contacts dominate. No viscosity-matched or volume-fraction-normalized control experiments are described that would isolate the H-bonding contribution from these hydrodynamic confounds. DFT and pull-test data address only the bonding term.

minor comments (2)

[Figures and methods] Figure captions and methods: specify the exact particle weight fractions used, the range of shear rates probed for each solvent, and whether raw torque or stress data are shown with error bars.
[Introduction] Notation: clarify whether 'hydrogen bridging bonds' refers to a distinct mechanism or simply to conventional H-bonds between solvent ends and particle surfaces; add a short schematic if possible.

Simulated Author's Rebuttal

2 responses · 0 unresolved

We thank the referee for their thorough review and valuable feedback on our manuscript. We address the major comments point-by-point below, providing clarifications on the experimental design and noting revisions to strengthen the manuscript by explicitly discussing potential hydrodynamic effects.

read point-by-point responses

Referee: [Abstract and experimental rheology] Abstract and § on experimental rheology: the transition is reported exclusively at fixed particle weight fraction. Solvent densities differ substantially (water 0.998 g cm⁻³, EG 1.113 g cm⁻³, 1,3-propanediol 1.036 g cm⁻³, 1,4-butanediol 1.017 g cm⁻³), producing up to ~5 % variation in particle volume fraction at typical loadings. This volume-fraction mismatch alters the proximity to jamming and the shear rate for contact formation independently of H-bond strength.

Authors: We acknowledge the referee's point that using fixed weight fraction leads to slight variations in volume fraction due to differing solvent densities. However, these variations are small (approximately 2-5% as noted), and the observed transition from shear thickening to thinning is abrupt between ethylene glycol and 1,3-propanediol, where the density difference is modest (1.113 vs 1.036 g/cm³). Our DFT simulations quantify the hydrogen bond strengths independently of hydrodynamics, showing a clear drop in bridging energy for larger diols. The fixed-rate pull tests further confirm reduced friction in larger solvents without flow. In revision, we will add a paragraph in the results section calculating the effective volume fractions for each suspension and argue that the small phi differences cannot account for the qualitative change in rheology, as similar phi variations in water-based suspensions do not eliminate thickening. This will be supported by referencing literature on jamming in cornstarch. revision: yes
Referee: [Results and discussion] Results and discussion sections: solvent viscosities increase sharply across the series (water ~1 mPa s to butanediol ~71 mPa s at 25 °C), changing the hydrodynamic Peclet number and the shear-rate window where frictional contacts dominate. No viscosity-matched or volume-fraction-normalized control experiments are described that would isolate the H-bonding contribution from these hydrodynamic confounds. DFT and pull-test data address only the bonding term.

Authors: The referee correctly identifies that viscosity differences affect the Peclet number. We did not perform viscosity-matched controls, as matching viscosity while varying molecular size is challenging without additives that might interfere with H-bonding. However, the data show that despite higher viscosity in butanediol (which should promote contacts at lower shear rates), the suspension shear thins rather than thickens, opposite to what hydrodynamics alone would predict. This supports the dominance of reduced H-bridging friction. We will revise the discussion to include estimates of Pe for each solvent at the onset shear rates and explain why the H-bonding effect overrides the hydrodynamic changes. The combination with DFT and pull tests provides orthogonal evidence for the molecular mechanism. revision: partial

Circularity Check

0 steps flagged

No circularity: results are direct experimental and simulation observations without self-referential reduction

full rationale

The paper's central claim rests on measured rheological transitions (shear thickening to thinning) across solvents at fixed particle weight fraction, combined with independent DFT calculations of hydrogen bonding and fixed-rate pull tests. No equations, fitted parameters renamed as predictions, or self-citation chains appear in the provided text that would make any result equivalent to its inputs by construction. The derivation chain is self-contained through direct data collection rather than internal fitting or imported uniqueness theorems.

Axiom & Free-Parameter Ledger

0 free parameters · 1 axioms · 0 invented entities

The central claim rests on standard experimental assumptions in rheology and DFT; no free parameters, new entities, or ad-hoc axioms are introduced in the abstract.

axioms (1)

domain assumption Standard assumptions of continuum rheology for dense suspensions hold (no wall slip, uniform shear rate).
Implicit in all reported viscosity measurements.

pith-pipeline@v0.9.0 · 5496 in / 1122 out tokens · 29270 ms · 2026-05-15T01:41:32.865338+00:00 · methodology

discussion (0)

Lean theorems connected to this paper

Citations machine-checked in the Pith Canon. Every link opens the source theorem in the public Lean library.

IndisputableMonolith/Foundation/AbsoluteFloorClosure.lean reality_from_one_distinction unclear

?

unclear
Relation between the paper passage and the cited Recognition theorem.

For a fixed particle weight fraction, we find a sudden transition from strong shear thickening (in water and ethylene glycol) to shear thinning (in propanediol and butanediol).
IndisputableMonolith/Cost/FunctionalEquation.lean washburn_uniqueness_aczel unclear

?

unclear
Relation between the paper passage and the cited Recognition theorem.

Density functional theory simulations reveal that increasing the length of the solvent molecule unlocks additional conformational complexity, where EG, PD, and BD molecules can form rings and dimers.

What do these tags mean?

matches: The paper's claim is directly supported by a theorem in the formal canon.
supports: The theorem supports part of the paper's argument, but the paper may add assumptions or extra steps.
extends: The paper goes beyond the formal theorem; the theorem is a base layer rather than the whole result.
uses: The paper appears to rely on the theorem as machinery.
contradicts: The paper's claim conflicts with a theorem or certificate in the canon.
unclear: Pith found a possible connection, but the passage is too broad, indirect, or ambiguous to say the theorem truly supports the claim.

Reference graph

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