Author's Accepted Manuscript

Hyperbolic rheological model with shear

stress limit for acrylamide polymer modified
bentonite drilling Muds
C. Vipulanandan, Ahmed Mohammed

www.elsevier.com/locate/petrol

PII: S0920-4105(14)00253-8
DOI: http://dx.doi.org/10.1016/j.petrol.2014.08.004
Reference: PETROL2758

To appear in: Journal of Petroleum Science and Engineering

Received date: 16 February 2014

Revised date: 22 July 2014
Accepted date: 5 August 2014

Cite this article as: C. Vipulanandan, Ahmed Mohammed, Hyperbolic

rheological model with shear stress limit for acrylamide polymer modified
bentonite drilling Muds, Journal of Petroleum Science and Engineering, http://dx.doi.
org/10.1016/j.petrol.2014.08.004

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 Hyperbolic Rheological Model with Shear Stress Limit for Acrylamide Polymer Modified
Bentonite Drilling Muds

C. Vipulanandan and Ahmed Mohammed

Abstract:

The effects of additives on the flow characteristics of the drilling muds used in various drilling

operations including oil and gas wells must be better quantified. In this study, acrylamide

polymer was used to modify the water based bentonite mud to reduce the yield point and

maximum shear stress produced by the mud during the drilling operation. The bentonite content

in the drilling mud was varied up to 6% (by weight). Based on the X-ray diffraction (XRD)

analyses the major constituents of the bentonite were montmorillonite (MMT,

(Na,Ca)0.33(Al,Mg)2(Si4O10)(OH)2·nH2O), feldspar (Albite, NaAlSi3O8), kaolinite

(Al2Si2O5(OH4)), Beidellite ((Na,Ca0.5)0.3Al2((Si,Al)4O10)(OH)2.nH2O) and quartz (SiO2). The

bentonite was modified using a water soluble polymer solution before using it in the drilling

mud. The rheological properties of bentonite were characterized from very low strain rate to

relatively high strain rate to determine the nonlinear behavior of the shear thinning drilling mud.

The polymer modification reduced the yield point by 26% to 66% based on the bentonite content

in the drilling mud. The polymer treatment also reduced the apparent viscosity of the drilling

muds. The shear thinning behavior of the bentonite drilling mud with and without polymer has

been quantified using the new hyperbolic model and compared with two other constitutive

models, Herschel-Bulkley and Casson models. While Casson model had two material parameters

the other two models had three parameters. The results showed that the hyperbolic model

predicated the shear thinning relationship between the shear stress and shear strain rate of the

polymer modified bentonite drilling mud very well. Also the hyperbolic model has a maximum

shear stress limit were as the other two models did not have a limit on the maximum shear stress.
Based on the hyperbolic model the maximum shear stresses produced by the 2%, 4% and 6%

bentonite drilling muds were 11 Pa, 18.5 Pa and 45.7 Pa respectively. The maximum shear stress

produced by 0.24% polymer treated 2%, 4% and 6% bentonite drilling muds were 10.4 Pa, 16 Pa

and 31 Pa respectively, hence a reduction of 5% to 33% in the maximum shear stress. Effects of

bentonite content and polymer content on the model parameters have been quantified using a

nonlinear model (NLM). The NLM quantified the effect of polymer treatment on all the model

parameters.

Keywords: Water-based drilling mud, Polymer solution, Bentonite, Maximum shear stress limit,

Yield stress, Modeling.

Introduction

Constructions of the oil and gas wells are very much influenced by the flow properties of

the drilling muds used for the operations. Wyoming bentonite has been used for decades as

drilling mud for performing the functions such as transporting rock cuttings to surface,

lubricating the drill bit, applying hydrostatic pressure in the well bore to ensure well safety,

minimizing fluid loss across permeable formations by forming a filter cake on the walls of the

well bore and enhancing the drilling operation by eroding the formation under the drilling tool.

The maximum shear stress that can be produced by the drilling mud will be a very good indicator

of the erodibility potential of the drilling mud. Also bentonite and many other additives are

added in drilling fluids to modify viscosity, yield stress and maximum shear stress to enhance the

drilling and aid in the transfer of cuttings from the bottom of the well to the surface in addition to

the above mentioned functions (Kelessidis et al. 2006). Based on 72 data collected from the

literature (CIGMAT data base) the amount of bentonite used in water based drilling muds varied
from 0.5 to 14% (by weight of water) as shown in Fig.1. Over 50% of the studies used between

1% to 8% of bentonite in water based drilling mud. Drilling mud properties such as shear stress

and shear strain rate relationship, yield stress (τo) and maximum shear stress play an important

role in designing and optimizing the performance of drilling fluids. Acrylamide polymer has

been used as an additive to improve the bentonite properties (Kelessidis et al. 2006). Non-

Newtonian fluids do not conform to direct proportionality between shear stress and shear strain

rate and there are limitations on the relationships that are being used to describe the rheological

properties of drilling fluids (Ochoa 2006). Drilling fluids may be water or oil based (diesel or

synthetic oils) although the latter are more expensive and there is more search for

environmentally friendly water-based fluids which should contain several additives so that it

could give the required properties similar to the properties of oil-based fluids while protecting

the environment (Kelessidis et al. 2013).

A polymer is made up of repeating chemical units known as monomers with relatively

high molecular weight. Polymer properties designed can modify the water based bentonite

drilling muds to modify the viscosity, control fluid loss and minimize the interaction with the

geological formations. Polymers can also be used as shear thinning agents to reduce viscosity

when the mud is under relatively large shear strain rate. The amount of shear stress and shear

strain rate needed to induce flow varies in different parts of the circulation system during the

drilling of oil/gas wells. For example the shear strain rate is high at the bottom of the hole but

lower in the annulus. So a mud that is shear thinning improves the drilling rate since the viscosity

is lower at the place where the bit is working while still maintaining the ability to move the

cutting up the annulus (Dyke 2000). Also drilling mud, for that matter any other material will

have its own maximum shear stress tolerance, which has not been quantified.
 There are two broad types of water soluble polymers such as polysaccharides

(biopolymers) and synthetic polymers (polyacrylamides). Polysaccharides are formed from the

polymerization of saccharide molecules from a process called bacterial fermentation and the

molecules are bonded through glycosides linkages and they are relatively non-ionic. The

synthetic polymers are where the molecular chains grow by polymerization. These polymers are

either viscoelastic or viscoplastic. Under static conditions the synthetic polymers exhibit not only

thixotropic but also non-Newtonian behavior. With the polymer addition drilling mud can be

designed to have selected viscosity with varying amount of bentonite. The shear thinning

characteristics of these muds makes it efficient for the borehole cleaning (Dyke 2000). Polymers

are becoming more popular for modify drilling muds due to their ability to modify rheological

properties of bentonite suspensions and their low impact on the environmental (Dolz et al. 2007).

Several types of the biopolymers have been used such as Carboxyl-menthy-cellulose (CMC),

polyanionic cellulose (PAC) and Xanthan gum (Iscan and Kok 2007). Also synthetic polymer

polyacrylamide has been used to stabilize shale in the wellbore because they are used as clay

extenders, flocculants and for encapsulating colloids (Caenn and Chillingar 1996). Kelessidis et

al. (2013) used four different percentage of bentonite water based drilling muds (2% up to 5%)

modified using five percentage of partially hydrolyzed polyacrylamide (PHPA) concentrations

up to 0.7%. PHPA increased the apparent viscosity and reduced the fluid loss and the shales

were stabilized in HPHT applications. By using SEM study, they concluded PHPA acted as

coating on cuttings preventing agglomeration, minimizing fluid loss and aiding cutting transport.

Drilling fluids, both aqueous and non-aqueous exhibit non-Newtonian rheological

behavior. The yield stress (τo) is a key rheological parameter that has been recognized as critical

for the performance of drillings fluids. Based on literature review, the yield stress for bentonite
based drilling muds varied from zero to 28 Pa as shown in Fig. 2. Borehole cleaning, surge of

pressures and several other important drilling issues are impacted directly by the yield stress

characteristics. The yield stress can best be described as the stress that must be applied to a

material to initiate flow and depends on the model selected to represent the drilling mud. Non-

Newtonian fluids are those fluids that do not conform to a linear proportionality between shear

stress and shear stain rate, and there is no single equation has been proved to describe the

rheogram of all such fluids. Bingham plastic model includes the yield stress (τo) that is a positive

shear stress at zero shear strain rate which most drilling fluids and cement slurries exhibit.

Conventional rheological models such as Bingham plastic, Power law and Newtonian models

have been used widely for the past half century in the oil industry (Ochoa 2006). None of these

models have a limit on the maximum shear stress for the drilling fluids, since no shear thinning

drilling fluid can tolerate infinite shear stress as shown in Fig. 4.

Principles of Flow Properties

Pumpabiliy of a drilling mud is better represented by yield stress (τo) since higher stress has to be

applied to move the fluid. The performance of rheological models usually varies with the test

geometries, gap between shearing surfaces and their friction capacity, which makes the

measurements even more complicated (Nehdi and Rahman 2004). Existing empirical and time-

independent rheological models (Power law, Bingham, Herschel- Buckley, Modified Bingham

and Casson model) allow fitting shear stress, shear strain rate and viscosity data to specific trends

using rheological data analysis. The estimated rheological properties can vary significantly based

on the models (Nehdi and Rahman 2004). The Bingham plastic model and the Power law model

are widely used in the petroleum industry to describe the rheological properties of drilling mud

and cement slurries (Guillot 2006).

 There is a limit on the maximum shear stress (shear strength) produced by the fluid based

on the composition. None of the current models can represent this phenomenon. Also the

maximum shear stress produced by the liquid will also represent the shear erosion potential of

the liquid when used in various applications.

Yield Stress (τo)

Drilling fluids are designed such that under static conditions they are capable of suspending the

drill cuttings. In order for this to be possible, drilling muds must exhibit yield stress behavior or a

very high zero shear strain rate viscosity. It has been the assumption in the drilling industry that

most drilling muds do in fact display yield stress characteristics even though this property is not

measured directly. More than 50 data on yield stress (τo) of water based drilling mud using

bentonite were collected from the literature and the minimum and maximum values varied from

0 and 28 Pa as shown in Fig. 2. The experimental results of yield stress of water based drilling

mud (using hyperbolic model) were compared with data from the literature as shown in Fig. 2.

Model Development

For shear thinning fluids the shear stress- shear strain rate relationship is nonlinear with a limit

on the maximum shear stress tolerance. Similar trends have been observed in many other

engineering and environmental applications and have been modelled using the hyperbolic

relationship. Vipulanandan et al. (1993) used hyperbolic relationship to predicate the amount of

phenol leached from a solidified cement matrix, containing an initial concentration of phenol

during Toxicity characteristic leaching procedure (TCLP) test with coefficient of determination

(R2) values ranged between 0.97 and 0.99. Ata et al. (1998) proposed hyperbolic model to

represent the change in grouted sand properties with curing time. Vipulanandan et al. (2007)

used hyperbolic relationship to represent the variation of in-situ vertical stress and logarithmic
undrained shear strength of the soft marine and deltaic clays. This relationship better represented

the marine clay as compared to the deltaic clay. Usluogullari et al. (2012) used hyperbolic

relationship to represent the compressive strength variation with curing time for cemented sand.

Similar trend was observed between curing time and elastic modulus. Non-linear relationships

were developed to represent the changes in properties with curing time and cement content.

Mohammed and Vipulanandan (2014) used the hyperbolic relationship to predicate the relation

between compressive and tensile strength of sulfate contaminated CL soils with and without

polymer treatment.

Objectives

The overall objective was to quantify the changes in the rheological properties of bentonite

drilling mud modified with an acrylamide polymer. The specific objectives are as follows:

(i) Investigate the rheological properties of drilling muds modified using a water soluble

polymer.

(ii) Quantify the shear stress - shear strain rate relationship of bentonite drilling mud

modified with varying amounts of polymer using the hyperbolic model and compare

it to the current nonlinear models.

Materials and Methods

(i) XRD Analysis

An X-ray diffraction (XRD) analyses was performed in order to determine the chemical

composition of bentonite at 25°C. The XRD pattern of the particles was obtained by using

Siemens D5000 powder x-ray diffraction device (Jenkins and Snyder 1996). XRD analyses were

performed on bentonite passing sieve No. 200 (75 μm). The powder (≈2 g) was placed in an

acrylic sample holder (3 mm) depth. The sample was analyzed by using parallel beam optics
with CuKα radiation at 40 kV and 30 mA. The sample was scanned for reflections (2θ) from 0o

to 80o in steps of 0.02° and a 2 sec count time per step.

(ii) Viscosity Measurements

(a) Low Shear Strain Rate

Brookfield model LVF Rheometer was used to measure fluid parameters of shear stress and

viscosity at given shear strain rates. The principle of operation of the Model LVF is to drive a

spindle (which is immersed in the test fluid) using a calibrated spring. The viscous drag of the

fluid against the spindle was measured by the spring deflection. Spring deflection was measured

with a rotary transducer. The viscosity range for the Model LVF (centipoises (cP)) was

determined by the rotational speed of the spindle, the size and shape of the spindle, the container

in which the spindle was rotating and the full scale torque of the calibrated spring. Four spindles

were used for measurement of viscosity of modified bentonite. The Brookfield viscometer LVF

was calibrated using four standard liquids (standard liquid #1 with viscosity 1 cP, standard liquid

# 2 with viscosity 9.8 cP, standard liquid #3 with viscosity 445 cP and standard liquid # 4 with

viscosity 4800 cP). The tests were performed based on the ASTM D 2196 –99 specification. The

bentonite used for this work was Wyoming bentonite. The preparation of samples followed the

API 13A standard procedures. Bentonite was modified by first mixing with varying amounts of

polymer solution and then adding to the water and was mixed for five minutes using high speed

mixer. The bentonite drilling muds were cured for 16 hours at room temperature before testing.

Prior to the rheological measurements the samples were sheared for five minutes with a high

speed mixer (API 13D).

(b) High Shear Strain Rate

Drilling muds with bentonite content up to 6% were tested using a viscometer with the high

speed range up to 600 rpm (1024 s-1). The higher shear strain rate behavior data was used to

verify the predications using the model parameters developed from lower shear strain rate.

Behavior of the fluids at higher shearing rate is important to better model the drilling mud

behavior with the maximum shear stress tolerance.

(iii) Polymer Modification

Polymer solution was prepared by mixing 15% of acrylamide polymer powder (C3H5NO) with

0.5% of catalyst, 0.5% of activator and 84% of water. Hence the polymer solution had 15%

polymer dissolved in it. The pH of the polymer solution was 10. Hence, for example, if 20% of

polymer solution content was used to tread the bentonite (based on dry weight of bentonite) it

will have 3% of polymer addition (by weight) to the bentonite. When 6% of this polymer

modified bentonite was used in the drilling mud, the polymer content in the drilling mud will be

0.18%.

Modeling

The drilling muds showed non-linear shear thinning behavior with a yield stress. Based on the

test results, following conditions have to be satisfied for the model to represent the observed

behavior.

Hence the conditions are as follows:

τ = τ o When γ$ = 0

dτ
>0
d γ$
………… (1)

d 2τ
<0
d γ$ 2
………… (2)
γ$ → ∞ ⇒ τ = τ * ………… (3)

The rheological models used for predicating the shear thinning behavior of drilling mud are as

follows:

(i) Herschel-Bulkley Model

The Bingham plastic model includes both yield stress (τo) and a limiting viscosity (μp) at finite

shear rates, which the Power law model fails to consider. For a nonlinear flow relationship shear-

thinning or shear thickening behavior may be observed and the assumption of constant plastic

viscosity is not valid. The Herschel-Bulkley (Eqn. 4) model defines a fluid with three parameters

and can be represented mathematically as follows:

τ = τ o1 + k1γ$ n …….. (4)

Where τ , το1, γ$ , k1 and n represent the shear stress, yield stress, shear strain rate, correction

parameter and flow behavior index respectively. For τ < το the material remains rigid. The model

assumes that below the yield stress (το), the slurry behaves as a rigid solid, similar to the

Bingham plastic model. For τ > το the material flows as a Power law fluid. The exponent n

describes the shear thinning and shear thickening behavior. Slurries are considered as shear

thinning when n <1 and shear thickening when n >1. A fluid becomes shear thinning when the

apparent viscosity decreases with the increase in shear strain rate.

Hence the model should satisfy the following conditions (Eqns. (1), (2) and (3)).

dτ (n−1)
= k n * γ$ >0⇒k n>0
d γ$ 1 1 ……….. (5)

d 2τ (n−2)
= k n *(n − 1)* γ$ ⇒ k n *(n − 1) < 0
d γ$ 2
1 1 ……….. (6)
As shown in Eqns (5) and (6), one condition when both Eqns (1) and (2) will be satisfied only is

as follows:

0 < n < 1 and k1 > 0.

From the Eqn. (4)

When γ$ → ∞ ⇒ τ max.
=∞

Hence Herschel-Bulkley model doesn't satisfy the upper limit condition for the shear stress limit.

(ii) Casson Model

This two parameters model was originally developed for ink pigments but has been shown to

give a good match for some oil-based fluid systems (Ayeni 2003). The relationship is as follows:

τ = (τ o 2 ) + k2 * γ$ 2
1 1 1 1
2 2 2
………… (7)

Where:

k2: model constant ( γ$ = 0 when τ ≤ τ o ).

τ o 2 : yield stress (Pa).

γ$ : shear strain rate (s-1).

Hence by differentiating Eqn. (7) following first and second order differential relationships were
obtained.

( τ 2 )dτ = ( 1 (γ$ ) 2 *(k2 ) 2 )d γ$

1 −1 −1 1

2 2

dτ (k2 ) 2 * γ$
−1

= >0
1

d γ$
2

τ 2
−1
……………………… (8)

d 2τ 1 k 2 2 *τ o 2 2
= − )<0
1 1

d γ$ 2
(γ$ )
( 3
…………………….. (9)
2 2

Hence to satisfy the conditions in Eqns. (1) and (2), parameter k2 must be greater than zero (k2 >

0) in Eqns. (8) and (9).

Also when γ$ → ∞ ⇒ τ max. = ∞

Hence Casson model doesn't satisfy the upper limit condition for the shear stress.

A plot of 1/2
versus τ 1/ 2 gives the intercept of (τo2)1/2 and a slope of k21/2 . The parameters of this
model were obtained using nonlinear regression analyses. This model combines the yield stress
with the nonlinear shear thinning behavior.
(iii) Hyperbolic Model

Relationship between shear stress with shear strain rate of polymer modified bentonite was

investigated. Based on the inspection of the test data following relationship is proposed:

γ$
τ − τ o3 =
A + D * γ$
………… (10)

Where:

τo3: yield stress (Pa).

A (Pa. s)-1 and D (Pa)-1: are model parameters.

γ$ : shear strain rate (s-1).

dτ ( A + Dγ$ ) − γ$ * D
= = >0⇒ A>0
d γ$ ( A + Dγ$ ) ( A + Dγ$ ) 2
A
2

d 2τ − AD
= <0⇒ D >0
d γ$ 2
( A + Dγ$ ) 4

Also when γ$ → ∞ ⇒ τ max. = +τo

1
……………. (11)
D

Hence this model has a limit on the maximum shear stress the fluid will produce at relatively

high rate of shear strains.

Comparison of Model Predictions

In order to determine the accuracy of the model predictions, both coefficient of

determination (R2) and the root mean square error (RMSE) in curve fitting as defined in Eqns.

(12) and (13) were quantified.

RMSE =
∑ ( yi − xi ) 2
n
i =1
…………………… (12)
N

⎛
R2 = ⎜
∑ i( xi − x )( yi − y ) ⎞
⎟
2

⎜
⎝ ∑ i( xi − x ) * ∑ i( yi − y ) ⎠
2 2 ⎟

…………………… (13)

Where yi= actual value; xi=calculated value from the model; y =mean of actual values; x =
mean of calculated values and N is the number of data points.
Nonlinear Model (NLM) Parameters

The model parameters τo1, τo2, τo3, k1, k2, n, A and D were influenced by the composition of the

drilling muds. It is being proposed to relate the model parameters to the independent variables

(bentonite content and polymer content) using a nonlinear power relationship as proposed by

Demircan et al. (2011).

The effect of bentonite and polymer were separated as follows:

Model Parameters (τo1, τo2, τo3, k 1 , k 2 ,券, A , D ) = a * ( B ) b + c * ( B ) d * ( P ) e ..............(14)

Where:

a, b, c, d and e are the nonlinear model parameters.

P: polymer content (%).

B: bentonite content (%).

The NLM parameters were obtained from multiple regression analyses using the least square

method. The NLM model parameters are summarized in Table 2.

Results and Analyses

XRD

The bentonite used in this study had montmorillonite (MMT) (hydrated sodium calcium

aluminum magnesium silicate hydroxide (Na,Ca)0.33(Al,Mg)2(Si4O10)(OH)2·nH2O) (2θ peaks at

7.51°, 28.12°, 35.10°, 48.02°, 52.31° and 76.20°), kaolinite (Al2Si2O5(OH4)) (2θ peak at 11.89°

and 42.12°), feldspar (Albite) (NaAlSi3O8) (2θ peaks at 9.81°, 14.32°, 21.03°, 29.40° and

30.01°), beidellite (Na, Ca0.5)0.3Al2((Si,Al)4O10)(OH)2.nH2O (2θ peak at 62.05° and 73.88o) and

quartz (SiO2) (2θ peaks at 32.09°, 50.10 and 68.20°) as shown in Fig. 3.

Apparent Viscosity

Based on the low shear strain rate results using the Brookfield model LVF Rheometer, the

apparent viscosities of the control drilling muds with 2%, 4% and 6% of bentonite contents were

4.6 cP, 9 cP and 24.1 cP respectively at a shear strain rate of 17.2 s-1 (30 rpm). When the 2%

bentonite was modified using varying amounts of polymer up to 0.24%, it decreased the apparent

viscosity at a shear strain rate of 17.2 s-1 (30 rpm) from 4% to 17% based on the polymer content.

When the 4% and 6% of bentonite were modified using varying amounts of polymer up to

0.24%, it decreased the apparent viscosity at a shear strain rate of 17.2 s-1 (30 rpm) from 9% to

35% based on the bentonite and polymer contents. The apparent viscosity of 2% and 6%

bentonite drilling muds were 112.6 cP and 450 cP at a shear strain rate of 170.2 s-1 (100 rpm), a

300 % increase in viscosity. At a shearing strain rate of 510 s-1 (300 rpm), the apparent viscosity

of 2% bentonite mud increased by 51% and 147% when the bentonite content was increased to

4% and 6% respectively.
CONSTITUTIVE MODELS

Shear stress – shear strain rate relationships were predicated using the hyperbolic model and

compared with other two models as shown in Fig. 5, Fig. 6 and Fig. 7.

(i) Herschel-Bulkley Model

(a) 2% Bentonite

The shear thinning behavior of 2% bentonite drilling mud with and without polymer treatment

was modeled using the Herschel-Bulkley model (Eqn. (4)) up to a shear strain rate of 35 s-1. The

coefficient of determination (R2) varied from 0.98 to 0.99 as summarized in Table 1. The root

mean square of error (RMSE) varied from 0.18 Pa to 0.27 Pa as summarized in Table 1.The yield

stresses (τo1) for the bentonite drilling mud without and with 0.24% polymer treatment (by dry

weight of bentonite) were 4.1 Pa and 2.2 Pa respectively, a 46% reduction. The model parameter

k1 for drilling mud without and with 0.24% polymer treatment were 0.8 Pa.sn and 1.27 Pa.sn, a

58% increase with polymer treatment. The model parameter n for the drilling mud decreased by

19% with 0.24% polymer treatment.

4% Bentonite

The relationships between shear stress with shear strain rate for 4% bentonite drilling mud with

and without polymer treatment was modeled using the Herschel-Bulkley model (Eqn. (4)). The

coefficient of determination (R2) varied from 0.97 to 0.99 as summarized in Table 1. The root

mean square of error (RMSE) varied from 0.16 Pa to 0.68 Pa as summarized in Table 1. The

yield stresses (τo1) for the bentonite drilling mud without and with 0.24% polymer treatment (by

dry weight of bentonite) were 7.53 Pa and 3.1 Pa respectively, a 60% reduction and the trend was

similar to what was observed with 2% bentonite drilling mud. The model parameter k1 for
drilling mud without and with 0.24% polymer treatment were 3.5 Pa.sn and 2 Pa.sn respectively,

a 43% reduction. The model parameter n for the drilling mud increased by 30% with 0.24%

polymer treatment. The variation of on parameters k1 and n due to polymer treatment were

opposite to what was observed with 2% bentonite.

(c) 6% Bentonite

Using the Herschel-Bulkley model (Eqn. (4)), the relationships between shear stress with shear

strain rate of 6% bentonite drilling mud with and without polymer treatment was modeled. The

coefficient of determination (R2) varied from 0.95 to 0.98 as summarized in Table 1. The root

mean square of error (RMSE) varied from 1.42 Pa to 2.41 Pa as summarized in Table 1. The

yield stress (τo1) was higher than 4% bentonite drilling mud. The yield stresses (τo1) for the

bentonite drilling mud without and with 0.24% (by dry weight of bentonite) polymer treatment

were 11.2 Pa and 3.9 Pa respectively, a 65% reduction, similar to what was observed with 2%

and 4% bentonite drilling muds. The model parameter k1 for drilling mud without and with

0.24% polymer treatment were 11.19 Pa.sn and 8.9 Pa.sn respectively, a 21% reduction, similar to

the trend observed with 4% bentonite. The model parameter n for the drilling mud decreased by

8% with 0.24% polymer treatment.

The effect of bentonite and polymer on the model parameters were quantified using Eqn. (14)

where the effect of bentonite and polymer were separated.

Parameter τo1

Based on the nonlinear model parameter a (Eqn. (14)), bentonite content had the highest effect

on increasing the yield stress compared to parameters n and k1. NLM parameter c indicated that

addition of polymer had the highest effect on reducing the yield stress compared to parameter k1

and n as summarized in Table 2.

Parameter k1

Based on the nonlinear model parameter a (Eqn. (14)), bentonite content had the least effect on

parameter k1 compared to yield stress and parameter n. NLM parameter c indicated that addition

of polymer had the second highest effect on reducing the parameter k1 compared to the yield

stress and parameter n as summarized in Table 2.

Parameter n

Of the three model parameters, bentonite content (parameter a) had the second highest influence

on parameter n. Based on the NLM parameter c, addition of polymer had the highest effect on

increasing the parameter n.

(ii) Casson Model

(a) 2% Bentonite

The shear thinning behavior of 2% bentonite drilling mud with and without polymer treatment

was modeled using the Casson model (Eqn. (7)). The coefficient of determination (R2) varied

from 0.97 to 0.98 as summarized in Table 1. The root mean square of error (RMSE) varied from

0.26 Pa to 0.33 Pa as summarized in Table 1. The yield stresses (τo2) for the bentonite drilling

mud without and with 0.24% (by dry weight of bentonite) polymer treatments were 4.14 Pa and

2.85 Pa respectively, a 31% reduction. The model parameter k2 for drilling mud without and with

0.24% polymer treatment were 0.031 Pa.s-1 and 0.041 Pa.s-1 respectively, a 32% increase. The

effect of bentonite and polymer on the model parameters were quantified using Eqn. (14).

(b) 4% Bentonite

The relationships between shear stress with shear strain rate of 4% bentonite drilling mud with

and without polymer treatment was modeled using the Casson model (Eqn. (7)). The coefficient
of determination (R2) was varied from 0.85 to 0.99 as summarized in Table 1. The root mean

square of error (RMSE) varied from 0.35 Pa to 1.19 Pa as summarized in Table 1. The yield

stresses (τo2) for the bentonite drilling mud without and with 0.24% polymer treatment (by dry

weight of bentonite) were 9 Pa and 3.9 Pa respectively, a 56% reduction. The model parameter

k2 for drilling mud without and with 0.24% polymer treatment were 0.058 Pa.s-1 and 0.039 Pa.s-1

respectively, a 33% reduction and the trend was opposite to what was observed with 2%

bentonite drilling mud.

(c) 6% Bentonite

Using Casson model (Eqn. (7)), the relationships between shear stress with shear strain rate of

6% bentonite drilling mud with and without polymer treatment was modeled. The coefficient of

determination (R2) varied from 0.83 to 0.90 as summarized in Table 1. The root mean square of

error (RMSE) varied from 2.47 Pa to 3.70 Pa as summarized in Table 1. The yield stresses (τo2)

for the bentonite drilling mud without and with 0.24% (by dry weight of bentonite) polymer

treatment was 15.9 Pa and 6.3 Pa respectively, a 60% reduction. The model parameter k2 for

drilling mud without and with 0.24% polymer treatment were 0.477 Pa.s-1 and 0.570 Pa.s-1

respectively, a 19% increasing, the trend was similar to what was observed with 2% bentonite.

Parameter τo2

Based on the nonlinear model parameter a (Eqn. (14)), bentonite content had the highest effect

on increasing the yield stress compared to parameters k2. NLM parameter c indicated that

addition of polymer had the highest effect on reducing the yield stress compared to parameter k2

as summarized in Table 2.
Parameter k2

Based on parameter a, bentonite content had the least effect on parameter k2 compared to yield

stress. Additional of polymer increased the parameter k2 as summarized in Table 2.

(iii) Hyperbolic Model

(a) 2% Bentonite

The shear thinning behavior of 2% bentonite drilling mud with and without polymer treatment

was modeled using the Hyperbolic model (Eqn. (10)). The coefficient of determination (R2) was

0.99 as summarized in Table 1. The root mean square of error (RMSE) varied from 0.11 Pa to

0.19 Pa as summarized in Table 1. The yield stresses (τo3) for the bentonite drilling mud without

and with 0.24% (by dry weight of bentonite) polymer treatment was 3.9 Pa and 2.9 Pa

respectively, a 26% reduction. The model parameter A for drilling mud without and with 0.24%

polymer treatment was 1.41 (Pa.s)-1 and 2.45 (Pa.s)-1 respectively, a 74% increasing. The model

parameter D for drilling mud without and with 0.24% polymer treatment was 0.14 Pa-1 and 0.13

Pa-1 respectively, a 8% reduction.

(b) 4% Bentonite

The relationships between shear stress with shear strain rate of 4% bentonite drilling mud with

and without polymer treatment was modeled using the Hyperbolic model (Eqn.(10)). The

coefficient of determination (R2) varied from 0.98 to 0.99 as summarized in Table 1. The root

mean square of error (RMSE) varied from 0.01 Pa to 0.48 Pa as summarized in Table 1. The

yield stresses (τo3) for the bentonite drilling mud without and with 0.24% polymer treatment

were 8.9 Pa and 4.1 Pa respectively, a 54% reduction. The model parameter A for drilling mud

without and with 0.24% polymer treatment was 0.52 (Pa.s)-1 and 1.29 (Pa.s)-1 respectively, a
148% increase. The model parameters D for the drilling mud without and with 0.24% polymer

treatment were 0.104 Pa-1 and 0.084 Pa-1 respectively, a 19% reduction.

(c) 6% Bentonite

Using the Hyperbolic model (Eqn. (10)), the relationships between shear stress with shear strain

rate of 6% bentonite drilling mud with and without polymer treatment was modeled. The

coefficients of determination (R2) were greater than 0.97. The root mean square of error (RMSE)

varied from 0.74 Pa to 1.34 Pa as summarized in Table 1. The yield stresses (τo3) for the

bentonite drilling mud without and with 0.24% polymer treatment were 12.4 Pa and 5.8 Pa

respectively, a 53% reduction. The model parameter A for drilling mud without and with 0.24%

polymer treatment was 0.06 (Pa.s)-1 and 0.11 (Pa.s)-1 respectively, a 83% increasing as

summarized in Table 1. The model parameter D for the drilling mud without and with 0.24%

polymer treatment was 0.03 Pa-1 and 0.04 Pa-1 respectively, a 33% increase.

Parameter τo3

Based on the nonlinear model parameter a (Eqn. (14)), bentonite content had the second highest

effect on increasing the yield stress compared to parameters A and D. NLM parameter c

indicated that addition of polymer had the lowest effect on reducing the yield stress compared to

parameters A and D as summarized in Table 2.

Parameter A

Based on the nonlinear model parameter a (Eqn. (14)), bentonite content had highest effect on

this parameter compared to parameters τo3 and D. NLM parameter c indicated that addition of

polymer had increased the parameter A compared to the yield stress and parameter D as

summarized in Table 2.

Parameter D

Based on the nonlinear model parameter a (Eqn. (14)), bentonite content had least effect on this

parameter. NLM parameter c indicated that addition of polymer had the highest effect on

reducing the parameter D compared to the yield stress as summarized in Table 2.

High Shear Strain Rate

Drilling muds with bentonite content 2%, 4% and 6% were tested using a viscometer with

highest rotating speed of 600 rpm. The higher shear strain rate behavior data was used to verify

the prediction using the model parameters developed from lower shear strain rate (Table 1). The

root mean square of error (RMSE) for 2% drilling mud using the Herschel-Bulkley, Casson and

Hyperbolic models were 6.62 Pa, 6.42 Pa and 3.91 Pa respectively as shown in Fig.10 (a). The

root mean square of error (RMSE) for 4% drilling mud using the Herschel-Bulkley, Casson and

Hyperbolic models were 6.73 Pa, 27.37 Pa and 6.60 Pa respectively as shown in Fig.10 (b). The

root mean square of error (RMSE) for 6% drilling mud using the Herschel-Bulkley, Casson and

Hyperbolic models were 79.24 Pa, 9.77 Pa and 5.05 Pa respectively as shown in Fig.10 (c).
Clearly the hyperbolic model predicated the higher shear strain rate conditions very well and had

the minimum root mean square error (RMSE) of all the three constitutive models.

Maximum Shear Stress (τmax.)

Based on Eqn.14 the hyperbolic model has a limit on the maximum shear stress the fluid will

produce at relatively high rate of shear strains. The τmax for drilling mud with 2%, 4% and 6%

were 11 Pa, 18.5 Pa and 45.7 Pa respectively as shown in Fig. 9. Addition of 0.24% polymer

reduced the maximum shear stress of drilling mud with 2% of bentonite to 10.4 Pa, a 5%

reduction. Addition of 0.24% polymer also reduced the τmax for drilling muds with 4% and 6% of

bentonite to 16 Pa and 31 Pa respectively, reduction of 14% and 33% as shown in Fig. 9.

Conclusions

In this study, rheological properties including yield stress and maximum shear stress tolerance

(new concept) of acrylamide polymer modified bentonite drilling mud was investigated. Based

on X-ray diffraction (XRD) analyses the bentonite had kaolinite, feldspar (Albite) (NaAlSi3O8),

montmorillonite, beidellite (Na,Ca0.5)0.3Al2((Si, Al)4O10)(OH)2.nH2O and quartz (SiO2). The

bentonite was modified using up to 0.24% acrylamide polymer (by weight). Based on the

experimental study and modeling following conclusions are advanced:

 1. Additional of acrylamide polymer up to 0.24% modified the yield stress, shear thinning

behavior and ultimate shear stress tolerance of the drilling muds. The amounts of changes

in the properties were influenced by the bentonite and polymer contents in the drilling

muds and have been quantified using a nonlinear model.

2. The hyperbolic model predicted the maximum shear stress tolerance of each drilling mud.

Other two models predicated infinite shear stress tolerance for the drilling mud.

3. Based on the hyperbolic model the maximum shear stress produced by the 2% bentonite

drilling muds increased from 11 Pa to 18.5 Pa and 45.7 Pa when the bentonite content

was increased to 4% and 6% respectively. The ultimate shear stress produced by the

polymer treated bentonite reduced by 5% to 33% based on the bentonite content.

4. Polymer modified bentonite decreased the apparent viscosity of the drilling mud at low

and high shear strain rates.

5. Based on the constitutive models the yield stress increased with increasing the bentonite

content and decreased with increasing the polymer content.

6. The hyperbolic model was effective in predicting the shear stress- shear strain rate shear

thinning behavior and was better than Herschel-Bulkley and Casson models based on the

coefficient of determination and root mean square of error (RMSE).

7. Using nonlinear relationship the model parameters were related to the composition of the

drilling mud. Nonlinear model was effective in identifying contribution of each

constituent (bentonite and polymer).

Acknowledgments

This study was supported by the Center for Innovative Grouting Materials and Technology

(CIGMAT) at the University of Houston, Houston, Texas with funding from various industries.
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Table 1.Herschel-Bulkley, Casson and Hyperbolic Models Parameter for Polymer Modified Drilling Mud

Herschel-Bulkley Model Casson Model Hyperbolic Model

Eqn.(4) Eqn.(7) Eqn.(10)
τo τo τo
Bent Poly
k2 A D
onite mer k1
1 RMS R 2 RMS R 3 (Pa (P RMS R
(Pa n 2 (P 2 -
(P E (Pa) (P E (Pa) (P .s) a)- E (Pa) 2
(%) (%) .sn) a.s 1 1
a) a) -1 a)
)
0. 0. 0. 0.
4. 0.8 4. 0.0 3. 1.4 0.1
0 5 0.27 9 0.33 9 0.12 9
1 0 2 31 9 1 4
3 8 7 9
0. 0. 0. 0.
3. 0.9 3. 0.0 3. 2.0 0.1
0.12 5 0.21 9 0.26 9 0.19 9
2 4 4 39 3 2 4
1 9 8 9
2
0. 0. 0. 0.
3. 0.9 3. 0.0 3. 2.4 0.1
0.18 4 0.18 9 0.28 9 0.15 9
0 2 1 41 2 1 3
5 9 7 9
0. 0. 0. 0.
2. 1.2 2. 0.0 2. 2.4 0.1
0.24 4 0.18 9 0.26 9 0.11 9
2 7 9 41 9 5 3
3 9 8 9
0. 0. 0. 0.
7. 3.5 9. 0.0 8. 0.5 0.1
0 3 0.39 9 1.08 8 0.01 9
5 0 0 58 9 2 0
1 8 5 9
0. 0. 0. 0.
4. 3.3 7. 0.0 5. 0.5 0.0
0.12 3 0.68 9 1.19 8 0.48 9
6 2 1 58 9 2 9
7 7 9 8
4
0. 0. 0. 0.
4. 2.3 5. 0.0 5. 1.1 0.0
0.18 3 0.16 9 0.35 9 0.12 9
1 3 4 57 1 7 8
9 8 7 9
0. 0. 0. 0.
3. 3. 0.0 4. 1.2 0.0
0.24 2.0 4 0.36 9 0.51 9 0.14 9
1 9 39 1 9 8
4 9 9 9
0. 0. 0. 0.
11 11. 15 0.4 12 0.0 0.0
0 4 2.02 9 3.34 9 0.74 9
.2 19 .9 77 .4 6 3
0 6 0 9
0. 0. 0. 0.
6. 10. 11 0.5 7. 0.0 0.0
0.12 3 2.41 9 3.70 8 1.34 9
6 56 .1 48 6 7 3
9 5 8 9
6
0. 0. 0. 0.
6. 8.8 8. 0.5 6. 0.0 0.0
0.18 3 1.85 9 3.59 8 1.15 9
5 9 1 81 3 8 4
8 6 3 8
0. 0. 0. 0.
3. 8.9 6. 0.5 5. 0.1 0.0
0.24 3 1.42 9 2.47 8 1.29 9
9 0 3 70 8 1 4
7 8 8 7
 Table 2. Nonlinear Model Parameters for Polymer Modified Drilling Mud

Model No. of
a b c d e R2 RMSE
Parameters Data
τo1 (Pa) 2.5 0.85 -2.1 0.95 0.39 11 0.95 0.58
n 0.46 -0.1 7.1 -13.3 -2.5 11 0.82 0.03
k1 (Pa.sn) 0.03 3.23 -0.1 4.8 2.03 11 0.98 0.55
τo2 (Pa) 1.98 1.2 -1.45 1.50 0.56 11 0.99 0.34
k2 (Pa.s-1) 0.06 5.2 0.71 -0.65 4.66 11 0.93 0.08
τo3 (Pa) 2.23 0.96 -1.23 1.39 0.52 11 0.99 0.25
A (Pa.s)-1 15.5 -3.4 21.8 15.1 21.6 11 0.88 0.25
D (Pa)-1 0.32 -1.1 -67.2 -11.6 -0.17 11 0.91 0.01
 Highlights
• Polymer treated bentonite drilling mud had reduced rheological properties.

• New Hyperbolic Model was developed to predict the shear thinning behavior.

• Maximum shear stresses produced by the drilling muds have been quantified.
 16
15

14 Maximum=14%
Minium=0.5%
12 11 Average=5%
Frequency 10 No.of Data=72
8 8
8
6
6
4 4
4 3 3 3
2 2 2
2 1

0
0.5 2 3 4 5 6 7 8 9 10 11 12 13 14 14+
Bentonite (%)

Figure 1. Histogram of the Composition of Bentonite Drilling Muds

30
Maximum=28 Pa
Minium=0.0 Pa
25
Average=6.6 Pa
No.of Data=56
Yield Stress (τo) (Pa)

20

15
Previous Studies
10
Current Study
(Hyperbolic Model)
5

0
0 2 4 6 8 10 12 14 16
Bentonite (%)

Figure 2. Variation of Yield Stress with Percent of

Bentonite Content in the Drilling Mud
 MMT: Montmorillonite
(Na, Ca) 0.33(Al, Mg) 2(Si4O10) (OH)
2·nH2O

Figure 3. XRD Pattern of the Wyoming Bentonite

∞ ∞
80

70

τmax.
60
Shear Stress,τ

50

40

τ
30
Herschel‐Bulkey Model
ο
20
Casson Model
10 Hyperbolic Model

0 ∞

Shear Strain Rate, γ$

0 50 100 150 200 250

Figure 4. Flow Curves for the Shear Thinning Fluids Using the
Herschel-Bulkley, Casson and Hyperbolic Models
 10
10
9 Bentonite=2%
a 9
8 P=0.12%
8
7
Shear Stress, τ (Pa)

Shear Stress, τ (Pa)

6
6
5
5
4 Expermintal Data
4
Expermintal Data Herschel‐Bulkley Model
3
Herschel‐Bulkley Model 3
Casson Model
2 Bentonite=2% Casson Model 2
b Hyperbolic Model
1 P=0% Hyperbolic Model 1

γ$
0

Shear Strain Rate, γ$ (1/s)

0
0 5 10 15 20 25 30 35 40
0 5 10 15 20 25 30 35 40
Shear Strain Rate, (1/s)

10
9
9 Bentonite=2%
c 8
8 P=0.24%
7
7
Shear Stress, τ (Pa)

Shear Stress, τ (pa)

6
6
5
5
Expermintal Data 4
4 Expermintal Data
Herschel‐Bulkley Model
3 3 Herschel‐Bulkley Model
Casson Model
Casson Model
2 Hyperbolic Model 2
Bentonite=2% Hyperbolic Model
1
P=0.18% 1 d
0

Shear Strain Rate, γ$ (1/s)

Shear Strain Rate, γ$ (1/s)
0
0 5 10 15 20 25 30 35 40
0 5 10 15 20 25 30 35 40

Figure 5. Predicted and Measured Shear Stress - Shear Strain Rate Relationship for
2% Bentonite Mud Modified with Different Percentage of Polymer (P) (a) P=0%
(b) P=0.12 % (c) P=0.18 % and (d) P=0.24%
 25
18

a 16
Bentonite=4%
20 P=0.12%
14
Shear Stress, τ (Pa)

Shear Stress, τ (Pa)

12
15
10

Expermintal Data 8 Expermintal Study

10
Herschel‐Bulkley Model 6 Herschel‐Bulkley Model
Casson Model Casson Model
4
5
Bentonite=4% Hyperbolic Model b Hyperbolic Model
2
P=0%

Shear Strain Rate, γ$ (1/s)

0

γ$ (1/s)
0
0 5 10 15 20 25 30 35 40 0 5 10 15 20 25 30 35 40

Shear Strain Rate,

14 16
b
Betonite=4% Bentonite=4%
14
12 P=0.18% P=0.24%
12
10
Shear Stress, τ (Pa)

a
Shear Stress, τ (Pa)

10
8
8
6 Expermintal Data Expermintal Data
Herschel‐Bulkley Model 6 Herschel‐Bulkley Model
4 Casson Model Casson Model
4
Hyperbolic Model Hyperbolic Model
2
c d
2

γ$
0

γ$
0 5 10 15 20 25 30 35 40 0
0 5 10 15 20 25 30 35 40
Shear Strain Rate, (1/s)
Shear Strain Rate, (1/s)

Figure 6. Predicted and Measured Shear Stress - Shear Strain Rate Relationship for
4% Bentonite Mud Modified with Different Percentage of Polymer (P) (a) P=0%
(b) P=0.12 % (c) P=0.18 % and (d) P=0.24%
 50 45

45 Bentonite=6% Bentonite=6%
40
P=0% P=0.12%
40
35
35
Shear Stress, τ (Pa)

Shear Stress, τ (Pa)

30
30
25
25
Expermintal Data 20 Expermintal Data
20
Herschel‐Bulkley Model Herschel‐Bulkley Model
15 15
Casson Model
Casson Model
10 Hyperbolic Model 10
a b Hyperbolic Model
5 5

γ$ (1/s) γ$
0 0
0 2 4 6 8 10 12 14 16 18 0 2 4 6 8 10 12 14 16 18
Shear Strain Rate, Shear Strain Rate, (1/s)

40 35

35 Bentonite=6% Bentonite=6%
30
P=0.18% P=0.24%
30
Shear Stress, τ (Pa)

25
Shear Stress, τ (Pa)

25

20
20
Expermintal Data
15 15 Expermintal Data
Herschel‐Bulkley Model
Casson Model Herschel‐Bulkley Model
10
10 Casson Model
c Hyperbolic Model
5 Hyperbolic Model
5
d
γ$
0
0 2 4 6 8 10 12 14 16 18

γ$ (1/s)
0
Shear Strain Rate, (1/s) 0 2 4 6 8 10 12 14 16 18
Shear Strain Rate,

Figure 7. Predicted and Measured Shear Stress - Shear Strain Rate Relationship for 6% Bentonite
Mud Modified with Different Percentage of Polymer (P) (a) P=0% (b) P=0.12 %
(c) P=0.18 % and (d) P=0.24%
 14

12
Bentonite=2%
Bentonite=4%

Yield Stress, τo (Pa)

10
Bentonite=6%
8

0
0 0.05 0.1 0.15 0.2 0.25 0.3
Polymer (%)
Figure 8. Variation of Yield Stress with Polymer Content Predicated Using the
Hyperbolic Model

50
45
Shear Stress Limit, τmax. (Pa)

40
35 Bentonite=2%
30 Bentonite=4%
25 Bentonite=6%
20
15
10
5
0
0 0.05 0.1 0.15 0.2 0.25 0.3
Polymer (%)

Figure 9. Variation of Shear Stress Limit with Polymer Content Predicated

Using the Hyperbolic Model
 70
Expermintal Data
60 Herschel‐Bulkley Model
Casson Model
50 Hyperbolic Model

Shear Stress, τ (Pa)

40
‐a‐
30

20

10

Shear Strain Rate, γ$ (1/s)

0 200 400 600 800 1000 1200

100
Expermintal Data
90
Herschel‐Bulkley Model
80 Casson Model
70 Hyperbolic Model
Shear Stress, τ (Pa)

60
‐b‐
50

40

30

20

10

Shear Strain Rate, γ$ (1/s)

0 200 400 600 800 1000 1200

800
Expermintal Data
700 Herschel‐Bulkley Model
Casson Model
600
Hyperbolic Model
Shear Stress, τ (Pa)

500
‐c‐
400

300

200

100

Shear Strain Rate, γ$ (1/s)

0 200 400 600 800 1000 1200

Figure 10. Predicted and Measured Shear Stress with High Shear Strain Rate
Relationship for (a) 2% of Bentonite (b) 4% of Bentonite and (c) 6% of Bentonite