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arxiv: 2605.12696 · v1 · submitted 2026-05-12 · ⚛️ physics.flu-dyn

Recognition: unknown

Time-Resolved Pore-Scale Imaging of Multiphase Dissolution during CO2-Saturated Brine Injection into a Carbonate: Competition between Hydrocarbon Mobilisation and Swelling

Branko Bijeljic, Martin J. Blunt, Qianqian Ma, Rukuan Chai, Yanghua Wang, Zhuangzhuang Ma

Authors on Pith no claims yet

Pith reviewed 2026-05-14 19:56 UTC · model grok-4.3

classification ⚛️ physics.flu-dyn
keywords multiphase dissolutioncarbonate rockCO2 injectionpore-scale imaginghydrocarbon mobilisationX-ray tomographyreaction rateadvective access
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0 comments X

The pith

Effective dissolution rates in residual-oil carbonate rock are controlled by the competition between hydrocarbon swelling and ganglion mobilisation.

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

The authors inject CO2-saturated brine into a water-wet Ketton limestone sample that still contains residual hydrocarbon and image the system repeatedly with 4D X-ray microtomography under reservoir pressure and temperature. They extract pore-network models at successive times to measure how pore geometry, fluid occupancy, interfacial areas, and the effective reaction rate evolve. The dissolution rate is not steady; it passes through an initial fast advection-dominated stage, a middle stage of strong suppression, and a later recovery stage. A sympathetic reader cares because the timing and extent of rock dissolution during CO2 injection determine both how much storage capacity is created and how residual oil is mobilised in real reservoirs.

Core claim

Time-resolved pore-scale experiments show that the dissolution rate of Ketton limestone by CO2-saturated brine in the presence of residual hydrocarbon is non-monotonic and proceeds through three regimes. In the first advection-dominated regime, pore-throat widening mobilises hydrocarbon ganglia and delivers acidic brine efficiently to reactive surfaces. The second dissolution-inhibited regime features up to two orders of magnitude reduction in effective reaction rate because swollen hydrocarbon ganglia persistently occupy the largest throats, reorganising the flow field into preferential paths and stagnant zones; the suppression is interpreted as arising mainly from path-dependent loss ofadv

What carries the argument

The competition between hydrocarbon swelling and ganglion mobilisation that governs advective access to reactive mineral surfaces.

If this is right

  • Pore-throat widening in the first regime produces efficient ganglion mobilisation and high initial dissolution rates.
  • Persistent occupation of the largest throats by swollen ganglia in the second regime reorganises flow and suppresses the effective reaction rate by up to two orders of magnitude.
  • Displacement of hydrocarbon from the largest throats in the third regime restores advective access and accelerates dissolution.
  • The overall effective dissolution rate therefore depends dynamically on the shifting balance between swelling and mobilisation.

Where Pith is reading between the lines

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

  • Field-scale models of CO2 injection into carbonate reservoirs may require time-dependent reaction rates that account for local residual-oil saturation and its effect on flow topology.
  • The same swelling-mobilisation competition could appear in other multiphase reactive transport problems, such as acid stimulation or contaminant dissolution, whenever a non-aqueous phase occupies pore throats.
  • Pre-flushing to reduce residual hydrocarbon saturation before CO2 injection could avoid the inhibited regime and maintain higher average dissolution rates.
  • Repeating the experiment on rocks with different pore-size distributions would test whether the three-regime pattern depends on the presence of a broad throat-size spectrum.

Load-bearing premise

The rate suppression is caused primarily by loss of advective access to surfaces as swollen ganglia block the largest throats, rather than by H+ depletion or mass-transfer limits, and that the three observed regimes generalise to other carbonates and conditions.

What would settle it

An otherwise identical experiment that prevents hydrocarbon swelling (for example by using a non-swelling fluid or by pre-flushing to remove residual oil) would produce a monotonic dissolution rate without the middle inhibited regime.

Figures

Figures reproduced from arXiv: 2605.12696 by Branko Bijeljic, Martin J. Blunt, Qianqian Ma, Rukuan Chai, Yanghua Wang, Zhuangzhuang Ma.

Figure 1
Figure 1. Figure 1: The experimental apparatus including the flow loop and micro-CT scanner. [PITH_FULL_IMAGE:figures/full_fig_p004_1.png] view at source ↗
Figure 2
Figure 2. Figure 2: Temporal evolution of porosity, oil saturation, and oil content during reactive flooding. Each CT scan is labelled by the [PITH_FULL_IMAGE:figures/full_fig_p009_2.png] view at source ↗
Figure 3
Figure 3. Figure 3: Greyscale image observations and oil ganglion evolution. (a) Greyscale images depicting the temporal evolution of [PITH_FULL_IMAGE:figures/full_fig_p010_3.png] view at source ↗
Figure 4
Figure 4. Figure 4: Pressure response over the entire experiment, displayed in three panels corresponding to the three evolutionary stages identified from [PITH_FULL_IMAGE:figures/full_fig_p011_4.png] view at source ↗
Figure 5
Figure 5. Figure 5: Temporal evolution of topological and geometric characteristics of the pore network. The entire evolution process is divided into three [PITH_FULL_IMAGE:figures/full_fig_p013_5.png] view at source ↗
Figure 6
Figure 6. Figure 6: Volume-weighted oil and brine occupancy as a function of pore radius (top rows) and throat radius (bottom rows) at successive scan [PITH_FULL_IMAGE:figures/full_fig_p014_6.png] view at source ↗
Figure 7
Figure 7. Figure 7: Interfacial areas, phase surface areas, and e [PITH_FULL_IMAGE:figures/full_fig_p016_7.png] view at source ↗
Figure 8
Figure 8. Figure 8: Co-evolution of oil occupancy in large throats and the e [PITH_FULL_IMAGE:figures/full_fig_p018_8.png] view at source ↗
Figure 9
Figure 9. Figure 9: Pore-scale streamlines coloured by velocity magnitude [PITH_FULL_IMAGE:figures/full_fig_p019_9.png] view at source ↗
read the original abstract

We present time-resolved pore-scale experiments in which CO2-saturated brine was injected into a water-wet Ketton limestone sample containing residual hydrocarbon under reservoir conditions (8 MPa, 50 {\deg}C) and monitored by 4D X-ray microtomography. Equivalent pore-network models were extracted at each scan time to track pore geometry, topology, and fluid occupancy, while fluid-fluid and fluid-rock interfacial areas and the effective reaction rate were determined from segmented images. The dissolution rate is non-monotonic in time and proceeds through three regimes, consistent with a shifting balance between hydrocarbon swelling and ganglion mobilisation, which control advective access to reactive surfaces. In the initial advection-dominated regime, pore-throat widening leads to ganglia mobilisation and efficient acidic brine delivery to reactive surfaces. The second, dissolution-inhibited regime is marked by up to two orders of magnitude reduction in effective reaction rate. Pore-network analysis shows that swollen hydrocarbon ganglia persistently occupy the largest throats throughout this regime. This occupancy is associated with a reorganisation of the advective flow field into preferential flow paths and stagnant zones. We interpret the rate suppression as primarily reflecting a path-dependent loss of advective access to reactive surfaces, with subordinate contributions from localised H+ depletion near ganglia and reduced near-wall mass transfer in widened flow paths. The inhibited state persists until hydrocarbon is displaced from the largest throats, after which, in the third stage, advective access improves and rock dissolution accelerates. These results show that the effective dissolution rate in residual-hydrocarbon-bearing carbonate depends dynamically on the competition between hydrocarbon swelling and ganglion mobilisation, governing advective access to surfaces.

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.

Referee Report

1 major / 1 minor

Summary. The paper reports time-resolved 4D X-ray microtomography experiments injecting CO2-saturated brine into a water-wet Ketton limestone sample containing residual hydrocarbon at reservoir conditions (8 MPa, 50°C). Equivalent pore networks are extracted at successive scan times to track geometry, topology, and fluid occupancy; interfacial areas and effective reaction rates are computed from segmented images. The dissolution rate is shown to be non-monotonic, progressing through three regimes governed by the competition between hydrocarbon swelling and ganglion mobilisation that controls advective access to reactive surfaces.

Significance. If the interpretation holds, the results establish that residual hydrocarbons can suppress effective dissolution rates by up to two orders of magnitude through dynamic flow-field reorganization, with direct implications for reactive transport modeling in CO2 storage and EOR. The time-resolved imaging plus network extraction approach supplies observational evidence of regime transitions that is stronger than steady-state bulk measurements.

major comments (1)
  1. [Results (pore-network analysis and rate interpretation)] The central claim that rate suppression in the inhibited regime is primarily caused by path-dependent loss of advective access (via swollen ganglia occupying largest throats) rests on qualitative correlation between throat occupancy and observed rate drop. No single-phase flow simulations (Stokes or Darcy) on the extracted pore networks are reported to compute local velocity fields, flux-weighted reactive-surface fractions, or stagnant-zone volumes, leaving the causal link unquantified and difficult to separate from subordinate mechanisms such as local H+ depletion or reduced near-wall mass transfer.
minor comments (1)
  1. [Abstract] The abstract states that the inhibited state persists 'until hydrocarbon is displaced from the largest throats,' but the corresponding time series or occupancy statistics are not referenced to a specific figure or table.

Simulated Author's Rebuttal

1 responses · 0 unresolved

We thank the referee for their constructive and detailed review. The major comment highlights an important opportunity to strengthen the quantitative support for our interpretation of advective-access control. We address the point directly below and will revise the manuscript accordingly.

read point-by-point responses

  1. Referee: [Results (pore-network analysis and rate interpretation)] The central claim that rate suppression in the inhibited regime is primarily caused by path-dependent loss of advective access (via swollen ganglia occupying largest throats) rests on qualitative correlation between throat occupancy and observed rate drop. No single-phase flow simulations (Stokes or Darcy) on the extracted pore networks are reported to compute local velocity fields, flux-weighted reactive-surface fractions, or stagnant-zone volumes, leaving the causal link unquantified and difficult to separate from subordinate mechanisms such as local H+ depletion or reduced near-wall mass transfer.

    Authors: We agree that the original manuscript presents the link between swollen-ganglia occupancy of the largest throats and the observed rate drop as a correlation derived from the time-resolved pore-network extractions. While the network data directly document the topological changes and persistent occupancy that accompany the transition into the inhibited regime, we did not perform single-phase flow simulations. In the revised manuscript we will add Stokes-flow simulations on the extracted networks at representative time points within each regime. These simulations will compute local velocity fields, identify stagnant-zone volumes, and estimate flux-weighted fractions of reactive surface area, thereby providing a quantitative measure of advective-access loss and allowing clearer separation from the subordinate mechanisms (local H+ depletion and reduced near-wall mass transfer) that we already acknowledge in the text. revision: yes

Circularity Check

0 steps flagged

No significant circularity: purely observational experimental study with direct image-based measurements

full rationale

The manuscript reports time-resolved 4D X-ray microtomography experiments on Ketton limestone under reservoir conditions. Pore-network models are extracted at each time step, and interfacial areas plus effective reaction rates are computed directly from segmented images. The three regimes and rate suppression are identified from observed non-monotonic dissolution behavior and fluid occupancy changes. No equations, fitted parameters, or predictions are presented that reduce to inputs by construction. No self-citations are invoked as load-bearing uniqueness theorems or ansatzes. The central interpretation (advective-access loss due to swollen ganglia) is qualitative inference from imaging data rather than a mathematical reduction. The study is self-contained as direct experimental observation against external benchmarks.

Axiom & Free-Parameter Ledger

0 free parameters · 1 axioms · 0 invented entities

The paper is observational and relies on standard domain techniques in porous-media imaging without introducing new free parameters or postulated entities.

axioms (1)
  • domain assumption Segmented X-ray images and derived pore-network models accurately capture fluid occupancies, pore geometry, and interfacial areas at each time step
    This assumption underpins all quantitative claims about dissolution rates, regime identification, and flow-field reorganisation.

pith-pipeline@v0.9.0 · 5634 in / 1439 out tokens · 84405 ms · 2026-05-14T19:56:53.853116+00:00 · methodology

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