Bo
Fan
ab,
Tivadar
Pongó
c,
Joshua A.
Dijksman
bd,
Jasper
van der Gucht
b and
Tamás
Börzsönyi
*a
aInstitute for Solid State Physics and Optics, HUN-REN Wigner Research Centre for Physics, Budapest H-1525, Hungary. E-mail: borzsonyi.tamas@wigner.hu
bPhysical Chemistry and Soft Matter, Wageningen University & Research, Wageningen 6700 HB, The Netherlands
cCollective Dynamics Lab, Division of Natural and Applied Sciences, Duke Kunshan University, Kunshan, China
dInstitute of Physics, University of Amsterdam, Amsterdam 1098 XH, The Netherlands
First published on 21st April 2025
The discharge of granular mixtures composed of hard frictional beads and soft low-friction beads was investigated in a cylindrical silo in experiments and numerical simulations. In the two limits, we find a fill height dependent flow rate for 100% low friction soft grains and a height independent flow rate for 100% hard frictional grains. When mixing the two types of grains, the transition between the two limiting cases occurs rather abruptly. Namely, adding only 20% of hard frictional grains to a sample of low friction soft grains changes the dependence of the flow rate on the discharged mass significantly, i.e. causes the slope of the curve to decrease by 50–70%. Our numerical simulations reveal that the main factor leading to the strong change in the flow rate behavior at low hard grain concentration is the high sensitivity of the stress conditions in the orifice region to the mixture composition. Since frictional dissipation can be an important factor influencing the flow rate, we also analyze the frictional properties of our samples in two additional experiments: (i) quasistatic shear tests in a split-bottom shear cell and (ii) drag force measurements on an object moved in the mixture. The mixtures show increasing dissipation as a function of increasing hard grain concentration in both of these measurements, but the increase is rather modest in the low concentration range, thus it does not explain the abrupt change in the silo discharge rate.
Hydrogel beads are excellent examples of soft particles with low surface friction. Their use becomes increasingly important in various applications in food industry (delivery of drugs, nutrients or probiotics in the gastronintestinal tract) or in agriculture and water purification (removal of dyes, metal ions, organic pollutants or bacteria) and various biomedical applications.11–14 The effect of particle softness on the rheology of a granulate has been investigated previously in shear flows numerically,15–17 and hydrogel beads proved to be very useful to gain experimental insight into the microscopic dynamics by sophisticated noninvasive 3-dimensional (3D) imaging techniques.18–20 The mechanical response of a mixture of soft and hard grains subjected to compression or shear was also investigated in recent studies.20–23
As mentioned above, the discharge of low friction soft particles out of a container is very different from the behavior of hard grains. Experiments in a 2-dimensional system allowed the observation of the flow at the level of individual particles.8,9,24,25 At small orifice sizes, temporary congestions occur which resolve after some time, unlike the permanent clogs observed for hard grains. Both the statistics of the temporary congestions for small orifice (in the intermittent flow regime), as well as the discharge rate for larger orifice (in the continuous flow regime) are filling height dependent. Investigations in a 3D silo also unveiled strong differences in the flow field between the cases of hard grains and low friction soft hydrogel beads26,27 and a strong dependence of the flow rate on the filling height for the latter.7 This is related to the fact that for hydrogel beads dynamic arch formation and Janssen screening is less pronounced. As a result of this, for low-friction soft grains (i) the local vertical stress σzz above the orifice decreases from a higher value, i.e. spans a wider range during the discharge process and (ii) the value of σzz has a stronger impact on the outflow rate than for hard grains.7
For a mixture of hard grains and hydrogel beads, a transition is expected to happen as a function of concentration between the two different behaviors described above. Interestingly, in a 2D silo, a recent work showed that adding a small amount (5 or 10%) of hard frictional grains to hydrogel beads strongly changes the flow.28 By adding only 10% of hard grains the constant flow rate was already recovered. The probability of the formation of clogging arches also strongly changed with the concentration of hard grains in 2D silo experiments.28–30 In view of the striking behavior of the 2D systems, it is also interesting to test how the flow characteristics of mixtures changes with concentration in 3-dimensional configurations, especially because the nature of force chain propagation and wall effects do not trivially generalize from two to three dimensions.
In the present work, we therefore investigate experimentally the flow of mixtures of hydrogel beads and plastic beads in a 3-D silo, exploring the full range (0–100%) of concentrations. We complement these laboratory experiments by numerical simulations using the discrete element model (DEM). Furthermore, our investigations on silo discharge are complemented with two further experimental tests: (i) quasistatic shearing in a split-bottom shear cell and (ii) measuring the drag force on an object moved horizontally in the granulate.
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Fig. 1 Experimental setups: (a) silo, (b) cylindrical split-bottom shear cell, (c) rheometer, (d) materials: hydrogel beads (HGB) on the left and airsoft beads (ASB) on the right. |
In the second experiment, the sample was exposed to shear deformation in a cylindrical split bottom device (see Fig. 1(b)). In this setup, the middle of the sample was slowly rotated with a time period of 13 s, while the outer part was stationary, so the region between them (denoted with red color in Fig. 1(b)) was constantly sheared with a typical shear rate of 3 s−1. In order to measure the resistance of the sample against shearing, we measured the torque needed for maintaining stationary rotation of the middle part.
In the third type of experiment, we moved an object horizontally in the mixture and measured the force needed to maintain stationary motion. Two objects were used: an airsoft bead (same as for making the mixtures; glued at the end of a stainless steel needle with diameter of 0.7 mm) or a vertical stainless steel cylinder with the diameter of 6 mm. For each experiment, a 50 mm thick layer of the sample was placed in a cylindrical container with the diameter of 150 mm. Then, the object was immersed at a depth of 22 mm and it was moved using a rheometer (Anton-Paar MCR-501) along a circular trajectory with the radius of 45 mm. The speed of the object was varied in the range of 0.47 cm s−1 ≤ v ≤ 7.54 cm s−1. We can estimate the corresponding shear rate range by dividing the velocity difference of the moving object and the static neighboring grains by the grain size, which results in 0.8 s−1 ≤ ≤ 13 s−1.
In the experiments presented here, we used airsoft beads (ASB) with the diameter of d = 5.95 ± 0.04 mm and hydrogel beads (HGB) with d = 6.4 ± 0.3 mm (for photographs of the beads see Fig. 1(c)). We have investigated 11 samples, spanning the whole concentration range 0–100 wt% (weight percent). The mass density of the two types of grains was identical ρ = 1035 ± 5 kg m−3, as both were slowly sinking/rising in salty water with salt concentrations of 3% or 4%, respectively.
For characterizing the shear resistance as a function of the concentration, we prepared samples with the same volume (V = 10.9 liters), i.e. all samples had the same fill height h = 5.6 cm in the shear cell. Since the HGB are deformable, their packing fraction depends on the pressure. For a layer with a thickness of h = 5.6 cm, the HGB packing fraction was about 0.7 while that of ASB was measured to be 0.62. Thus, increasing ASB concentration leads to slightly decreasing mass (and density) of the sample. The measured torque was normalized by the mass of the sample. For the silo measurements, the same samples were used. Fig. 2 shows the mass of the samples as well as the fill height in the silo as a function of the ASB concentration.
The gravity driven numerical setup included a cylindrical wall and a 1-mm thick bottom mesh wall including the circular orifice. The hard grains were modelled with a Young's modulus of Yhard = 0.5 GPa, the soft ones with Ysoft = 300 kPa. The latter value was chosen so that the numerical flow rate results are close to the experimental data. Here we note that this Young's modulus is higher than the usual ≈100 kPa, in order to account for the smaller forces due to the lack of a multi-contact interaction.33 For the hard grains we chose a Young's modulus that is common for plastics, due to this fact their deformation is negligible compared to the soft ones in our system. The Poissons's ratio of each type was set to ν = 0.45, while the coefficient of restitution was en = 0.9. Following the experiments, the diameter of the hard grains was 5.95 mm and 6.4 mm for soft particles. Due to the small degree of polydispersity of the ASB and softness of the hydrogel beads, we did not implement polydispersity in the numerical system. The mass density of the particles was ρ = 1030 kg m−3. The friction between two hard grains was set to μhard–hard = 0.4, between two soft grains μsoft–soft = 0.03, between the two different types it was μhard–soft = 0.1 or μhard–soft = 0.03. The friction coefficient between the wall and hydrogel was set lower, μsoft–wall = 0.03, to better match the experimental basal force. The time step of the integration was 10−6 s. At the initialization of the simulation, we used Fig. 2(a) for the total mass of the mixtures, to obtain comparable data. The initial packing was created by random insertion of the not overlapping particles, let to settle under gravity (g = 9.8 m s−2). The numerical results presented here were obtained in a system with equivalent size to the experimental one (Dc = 144 mm), but we mention that additional simulations were performed with Dc = 180 mm, which resulted in the same flow rate, i.e. confirmed the absence of finite size effects.
Two main macroscopic measurables were extracted in the simulations, the flow rate and the total force acting on the silo bottom by the grains, similarly to the experiments. Furthermore, we computed the average vertical stress σzz in the region above the orifice. To do this, firstly we employed a coarse-graining methodology34,35 that takes the discrete contact force data as input and produces a smooth macroscopic field of the stress tensor. The function used for smoothing the fields was a normalized 3D Gaussian with a standard deviation of w = 1.5 mm, approximately a quarter of the grain diameter. After the continuous field was obtained, the vertical stress was averaged in a cylindrical volume above the supposed free fall arch. A sketch about the position and dimensions of this averaging volume is shown in the inset of Fig. 5(b).
The results of the numerical simulations are presented in the bottom section of Fig. 3. We present data for one orifice size (D = 52 mm) and two values of the friction coefficient between the hard and soft grains μhard–soft = 0.1 or 0.03.
In order to quantify how the nature of the silo flow rate changes with the mixture concentration, we take the slope of the flow rate curve in the middle part of the discharge process which is free of the initial and final transients, and normalize it with the slope obtained for the pure hydrogel sample. The normalized slope is presented as a function of the percentage of ASB in Fig. 4. As we see, in the experiments the discharge characteristics changes stronger in the beginning of the curve (up to about 20–30% ASB), i.e. adding a small amount of hard grains has a strong effect on the behaviour of the sample. But the change is not so dramatic as it was in previous experiments in a 2-dimensional silo,28 where a constant discharge rate scenario was already reached at 10% ASB. In the present experiments we see a gradual change in the whole concentration range with a stronger dependence up to 20–30% ASB. Note, that the experimental curves obtained for different orifice sizes nicely overlap, when normalized by the flow rate obtained for pure hydrogel for the given orifice.
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Fig. 4 The slope of flow rate curve obtained by linear fitting between 0.2 < m/mtotal < 0.7 (see the two black dotted lines in Fig. 3) as a function of ASB concentration. The slope is normalized by the slope value obtained for 0% ASB. |
The data obtained from the numerical simulations shows a similar decreasing trend for the slope of the flow rate, and we see that using a friction coefficient μhard–soft = 0.1 results in a better match with the experimental data, than using μhard–soft = 0.03. This is similar to our observations in a 2-dimensional system,28 and probably it is related to the presence of capillary bridges between the grains. Namely, in our earlier work we measured the microscopic friction coefficient of lubricated hard grain–hard grain contacts, and we found that the friction coefficient was much smaller for large normal forces (where capillarity can be neglected) than for small normal forces, where capillary forces are comparable to the normal force.7 The contact angle of water on a hydrogel surface and on a plastic surface is different, therefore we think that this effect will play a stronger role for ASB–HGB contacts than HGB–HGB contacts, leading to μASB–HGB > μHGB–HGB. We also mention that in another recent work, a harmonic mean was used to estimate the friction coefficient between hydrogel beads and hard grains, which yields a value closer to the lower coefficient of friction.21
In the present case for the mixtures we have performed a similar analysis, the result of which can be seen in Fig. 5. First, we present the average pressure pb at the basal plane as well as the local stress σzz above the orifice as a function of the normalized mass of the granular material above these locations (see Fig. 5(a) and (b)). The local stress σzz above the orifice was measured in the region indicated with a red box in Fig. 5(b). The curves show a gradual transition from hydrostatic to Janssen-like behavior by increasing the concentration of hard frictional grains. We can quantify this by fitting the data with a Janssen formula:36–38
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The fitting parameters λ and p∞ are shown in Fig. 5(c) as a function of hard grain fraction normalized by the silo diameter Dc and ρbgDc, respectively, where ρb is the bulk density. As we see, the curve for the local stress σzz above the orifice changes significantly in the low concentration range, which is clearly represented by the change of the fitting parameters in the Janssen-formula (Fig. 5(b) and (c)). We can also note in Fig. 5(c) that the parameters describing pb (which is the average pressure calculated from the basal force) change less abruptly in the low concentration range, and this tendency can be described by a simple approximation. For example, taking the case of the characteristic length, it can be expressed as λ = Dc/4μwK based on the stress balance model,37 where μw is the particle-wall friction and K is the Janssen constant that characterizes the transmission of vertical to horizontal stress. As a simple model, we assume that both μw and K change linearly with the concentration of hard grains between the two limiting values, which are μw = 0.03; K = 1 at 0% and μw = 0.4; K = 0.484 at 100%. We estimate a perfectly hydrostatic condition for soft grains resulting in K = 1, while for the hard grains K was calculated from the angle of repose of ϕ = 20.5° (typical value for spheres39) using the K = (1 − sinϕ)/(1 + sin
ϕ)37 formula. This model leads to a characteristic length λ indicated with the dashed line in Fig. 5(c), which fits the parameter corresponding to the basal pressure (blue squares). However, this simple model does not work for the case of σzz, as it changes much more strongly in the low concentration range (blue circles).
Second, we investigate the effect of σzz on the discharge rate (Fig. 5(d)). We find that the curves overlap for mixtures with concentrations of up to 25% hard frictional grains, and we only see a gradual decrease of the slope above 25% (Fig. 5(d)). This means that the two factors i.e. the slope of stress vs. discharged mass curves (blue data in Fig. 5(e)) and the slope of discharge rate vs. stress curves (orange data in Fig. 5(e)) contribute unequally to the change in flow rate slope vs. concentration curves. The major contribution comes from the dependence of the local stress on the discharged mass, as this quantity changes strongly in the low concentration range (blue data in Fig. 5(e)), while the other quantity (slope of flow rate vs. σzz curves) does not change significantly in the low concentration range.
Finally, in Fig. 5(f) we visualize the slope of the flow rate directly obtained from the simulation data as well as the product of the above described two quantities. As we expect, the two curves nicely overlap. Note, that the quantities in Fig. 5(e) and (f) present data averaged in the 0.2 < m/mtotal < 0.7 interval, which is denoted by a tilde sign.
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Fig. 6 Shear resistance per mass as a function of the of ASB concentration. The shear resistance data are normalized by the value of the first 13 s of the curve at 0% ASB. |
Another important observation regarding the samples' shear resistance is that even if the microscopic surface friction of common hard grains is more than 1 order of magnitude larger than the value of HGB (μ = 0.3–0.4 vs. μ = 0.02–0.037), we see in Fig. 6 that the shear resistance (effective friction) of the sample increases only by about a factor of 2 when going from 0% ASB to 100% ASB. This is perfectly consistent with the result of earlier numerical simulations41 and work on frictional hydrogel experiments,42 and again shows the importance of the geometrical origin of the effective friction of a sheared granulate.43
We also mention that shearing the mixture might also lead to segregation. If segregation is present, it would also result in a separation of the two curves presented in Fig. 6. As described above, during shearing we have clearly seen the development of ordering, but we did not see signs of segregation during the course of experiments (see ESI† for photographs). In any case, the curve obtained in the first 13 s of the measurement represents the behaviour of the random sample, and has the same trend as the curve obtained at later stages, i.e. shear resistance was less sensitive to mixture composition at low ASB concentration than in ASB rich samples.
First, as we see in Fig. 7(a) and (b) the drag force changes with the mixture concentration in a very similar way as the shear torque changed under quasistatic shear in the split bottom shear cell. Generally, the force increases with ASB concentration, and the rate of change is much larger in ASB rich samples than at low ASB concentrations. Thus, similarly to the shear experiments, these data do not provide a reason for the strong change in the slope of the silo discharge rate at low concentration either. The drag force is about 2.5–3 times larger in ASB rich samples than at small concentrations. Naturally, we get a larger drag force for a cylinder than for a single ASB. Second, the shear rate dependence of the drag force appears to be minor, as the data values are very similar even if the shear rate is increased by a factor of 16. In order to better visualize the weak shear rate dependence, we present the data in a normalized form in Fig. 7(c). For high ASB concentration, the data obtained for low and high shear rates are very similar within the uncertainty of the measurement which is about 10%. Decreasing the ASB concentration the curves clearly split up showing a 20–30% difference in the drag force in between the cases with the smallest and largest shear rate. Thus, the drag force on an object in a hydrogel rich sample is increasing with shear rate, similarly to viscous liquids or colloids, but here the magnitude of change is small.
Our complementary numerical simulations reveal that the main factor leading to the strong change in the flow rate behavior at low concentration of hard frictional grains is the high sensitivity of the of the stress conditions in the orifice region on the mixture composition. Namely, the slope of the vertical stress above the orifice vs. discharged mass curves changes significantly at low concentration of hard frictional grains, while it depends less on the concentration in samples rich in hard frictional grains. Our additional measurements show, that frictional dissipation also increases when increasing the ASB concentration but the dependence is less strong in the low concentration range compared to the trend of the slope of the silo discharge rate.
Footnote |
† Electronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d5sm00354g |
This journal is © The Royal Society of Chemistry 2025 |