Essay: Improvement of specific heat capacity of drilling fluid using metal oxide nanoparticles

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Department of Petroleum Engineering, Faculty of Petroleum and Chemical Engineering,
Science and Research Branch, Islamic Azad University, Tehran, Iran

Abstract
Cooling drill bits is one of the major tasks of drilling fluids, especially under high-pressure high‐temperature (HPHT) conditions. Designing stable drilling fluids with proper thermal properties is a great challenge, but identifying appropriate additives for the drilling fluid can prevent drill-bit wear or breakdown caused by high temperature. The unique advantages of nanoparticles may enhance thermal properties of the standard base drilling fluids. In this study, the impacts of certain metal oxide nanoparticles on the specific heat capacity and rheological properties of water‐based drilling mud were experimentally investigated. Three types of nanofluids, respectively containing Al2O3, TiO2 and SiO2 in different volume concentrations, were prepared. Transmission Electron Microscopy (TEM), X-Ray Diffraction (XRD) were used to characterize the nanoparticle samples. A simple device was designed and constructed to measure the drilling fluid heat capacity. The experimental results showed that the heat capacity of the drilling fluid is enhanced by 35.8% in the presence of 0.5 wt% Al2O3. Furthermore, significant improvement was observed in the rheological properties such as the yield point, apparent viscosity, plastic viscosity, and gel strength of the drilling nanofluids compared to the base drilling fluid. The results reveal that the application of nanoparticles may reduce drill-bit exchange costs by improving the thermal and rheological properties of drilling fluid.

 

Keywords: heat capacity, drilling fluid, nanofluid, metal oxide nanoparticle
1. Introduction
Cooling is one of the most important technical challenges facing various industries, including the drilling industry. Drilling fluids have this primary important task in oil and gas well drilling operations and help prevent the costly bit failures that occur with crushing rigid rocks, at high temperature, and at the great depth [1, 2]. Therefore, such fluids must be engineered so that they can perform efficiently in complex subsurface environments without damaging the formations. Drilling for oil and gas involves the drilling of a hole from surface to a reservoir that can be kilometers away. Drilling is achieved with the use of a drill bit connected to a drill pipe. The drilling fluid is pumped through the drill string and is continually introduced to the bottom of the bore hole from the drill bit nozzles. The circulating drilling fluid cools and lubricates the drill bit and helps to convey drill cuttings to the surface [3].
One of the major challenges in designing drilling fluid formulations is the requirement for the highest degree of thermal stability under high‐pressure high‐temperature (HPHT) conditions. To obtain the necessary stability and the best performance requires finding ways to improve the thermal and rheological properties of the drilling fluid, and nanotechnology offers a promising approach.
Nanofluids are defined as a mixture of nano sized particles suspended in a base fluid and usually stabilized by various methods. The presence of nanoparticles in a fluid enhances the rheological, mechanical, and thermal properties. Suspensions of nano-sized particles can augment fluid stability and reduce flow-passages blockage [4]. Nanoparticles, with high surface-to-volume ratio, possess enhanced physico-chemical properties compared to macro and micro-sized materials. Such properties make nanoparticles the best materials for the design of smart drilling fluids with desired properties and drilling performance.
Several factors affect the heat transfer properties of nanofluids, including their thermal conductivity, viscosity, heat capacity, density, and diffusion coefficient. Although several investigations have been conducted on drilling fluid thermal conductivity, studies on the effects of nanoparticles on drilling nanofluid heat capacity are scarce and little information is available. Nanofluids with higher heat capacities are necessary to enhance heat transfer efficiency at lower operating costs.
In the case of the thermal behavior of drilling fluids, enhancement of thermal conductivity through the addition of nanoparticles has been widely investigated. The presence of nanoparticles in nanofluids is known to enhance thermal conductivities [5-8], but studies on the effect of nanoparticles on the specific heat capacity of fluids, have not yielded consistent results [9-22]. William et al. investigated the influence of copper and zinc based nanoparticles in water-based drilling fluids. The results of their experiments showed up to 53% and 23% improvement in the thermal conductivities of the drilling fluids, respectively [16]. Hassani et al. conducted experiments on water-based drilling fluids in the presence of multiwall carbon nanotube, nano zinc oxide and silica nanoparticles, and reported 12%, 22% and 16.9% enhancement in the thermal conductivity of drilling nanofluid at a volume fraction of 2% CNT, ZnO and SiO2 , respectively [17]. Baghebanzadeh et al. synthesized spherical silica/multiwall carbon nanotube hybrid and prepared nanofluids to examine the thermal conductivity variations. They indicated that the nanoparticle concentration and amount in a hybrid, affect the thermal conductivity of the nanofluids [18].
In this present study undertaken to determine the effect of nanoparticle concentration on the enhancement of specific heat capacity of drilling nanofluids, three types of metal oxide nanoparticles were used to prepare drilling nanofluid. The nanoparticles were characterized by Transmission Electron Microscopy (TEM) and X-Ray Diffraction (XRD). Different concentrations of nanoparticles were stabilized in distillated water and homogenized in drilling fluid. Moreover, the rheological properties such as apparent viscosity, plastic viscosity, yield point, and gel strength were measured in the presence of nanoparticles in the base drilling fluid. It was found that the specific heat capacity for all the samples of drilling nanofluid is greater than that of the base drilling fluid, and improving the thermal conductivity and specific heat capacity simultaneously is necessary to improve the heat transfer characteristics of conventional drilling fluids.
2. Theory
As described in the literature, the ratio between the amount of applied heat to the unit mass of a substance, and the temperature change of that substance is called the specific heat capacity [19].
C = Q/(m.∆T) (1)
The specific heat capacity of a body is an intensive property and does not depend on the body’s mass. This thermal property shows the capacity of a body to absorb heat and depends on the temperature at which it is measured. A direct measure of specific heat capacity is not possible. The heat delivered to the body and its temperature should be measured, to make calculation of the heat capacity possible. According to Eq. (1), plotting the data on heat energy supplied to the body against the temperature variations results in a straight line. The specific heat capacity is calculated from the slope of that line. The rate of the convective heat transfer between a solid body and adjacent fluid is given by Newton–Richman’s law. The heat transfer rate is proportional to the heat transfer coefficient, surface area and temperature difference.
= ℎA( ‒ f ) (2)
According to Eq. (2), the heat transfer rate from a drill bit can be enhanced by increasing the temperature difference between the bit and drilling fluid. Therefore, designing a drilling fluid with high specific heat capacity leads to efficient cooling of the drill bit.
3. Experimental Procedure
3.1. Drilling nanofluid preparation
The analysis of a nanofluids thermal properties requires proper synthesis procedures that produce stable suspensions of nanoparticles in liquids. nanosilates are usually prepared by two steps: One-step procedure and two-step procedure. In the one-step procedure, in this method, nanoparticles are synthesized using base fluid by chemical methods. In the two-step procedure, nanoparticles are first prepared by chemical and physical Processes then suspended with a base fluid [21]. This method is more economical because of the production of nanoparticles at an industrial scale. Due to the tendency of nanoparticles to be agglomerated, the preparation of a stable nanosystem requires tools for controlling such as: a pH control or a prevent agglomeration tools [22].
The nanoparticles used in the research work were titania (TiO2), silica (SiO2), and alumina (Al2O3), selected for their excellent thermal properties compared to other nonmetallic and metallic solids. The physical properties of the nanoparticles are summarized in Table 1. Transmission electron microscopy and XRD analysis were used to verify the nanoparticles’ size, shape and purity.
The standard two-step method was used to prepare the nanofluid samples. Nanofluids were prepared by dispersing the nanoparticles in a certain concentration in distilled water. The colloidal fluid was then mixed completely using an ultrasonic disruptor for 20 min, resulting in homogeneous and stable nanofluids.
To prepare the drilling nanofluid, the nano suspensions were added to the base drilling fluid and stirred to produce uniform suspension. Drilling nanofluid samples were prepared in different concentrations of 0.01, 0.05, 0.1 and 0.5 wt%.
Water-based drilling fluid is usually prepared by mixing different minerals, dissolved salts, and organic compounds in water. The base drilling fluid was prepared on the basis of a formulation that is currently being used for drilling operations in an oilfield in the south of Iran. The formulation used in preparing the base drilling fluid is presented in Table 2. The chemical additives were slowly stirred into 350 ml tap water, then mixed well in a mixer.

Table 1. The properties of metal oxide nanoparticles
nanoparticle size (nm) purity specific heat capacity (J/kg.K)
Al2O3 30 99.8 % 955
TiO2 20 99 % 697
SiO2 30 99 % 730

 

Table 2. The formulation used in preparing the water‐based drilling fluid.
component weight (g) mixing duration (min)
Sodium Carbonate 0.18 3
Caustic Soda 0.1 3
Calcium Chloride 95 10
Potassium Chloride 10 8
Starch (C6 H10 O5) 10 8
Xunthun Gum 1 8
PAC LV 1 5
Barite 20 10

 

3.2. Heat Capacity measurement
A device was designed and constructed for measuring liquid samples’ heat capacity. This apparatus, shown in Fig. 1, consists of an insulated container with a stirrer, an internal thermocouple, and a heating element placed in the middle of the container.
The following procedure was done to gather the data required for the calculation of specific heat capacity. The insulated container was put on a digital balance, and after the calibration, 200 g of prepared drilling nanofluid was weighed to a precision of 1 mg. The initial temperature of the sample was recorded. The heat generated by the heating element caused the sample to increase in temperature. The stirrer inside the container homogenized the sample thermally. The temperature of the sample was registered at frequent time intervals.
The specific heat capacity of the prepared drilling fluid and different nanofluids were calculated based on Eq. (1) using the procedure explained previously. For each sample of the nanofluid concentration, measurements were taken three times, and the calculated specific heat capacities were then averaged to yield the final value.
To calibrate the device, a reference sample with a known heat capacity was selected. The calibration ensured that the measured value coincided with the reference one. Distilled water was used to calibrate the device. The distilled water sample was heated, temperature versus time data were gathered, and the heat capacity was calculated from the slope of the line plotted in Fig. 2. The specific heat capacity of water was found to be 4.21 J/g ºC, whereas the reference value in the literature is 4.18 J/g ºC. The discrepancy was 0.03 J/g ºC and the relative error was assessed as 0.7%.

Fig. 1. The experimental device.

Fig. 2. The measured data and the fitted straight line for distilled water used for device
calibration.

4. Results and discussion
Fig. 3 represents the TEM images of metal oxide nanoparticles. It can be seen that the nanoparticles are in spherical shape. The average sizes of Al2O3 , TiO2 , and SiO2 nanoparticles observed in the images are 34.7, 15.4, 28.2 nm, respectively.
The XRD pattern of nanoparticles shown in Fig.4 indicates the purity of nanoparticles. The characteristic peaks are consistent with the reference pattern for the nanoparticles.

Fig. 3. TEM image of (a) alumina, (b) titania, and (c) silica nanoparticles.

Fig. 4. XRD pattern of (a) alumina, (b) titania, and (c) silica nanoparticles.
4.1. Specific heat capacity
The accuracy of the experimental device developed for measuring specific heat capacity was initially evaluated using distillated water. To provide a baseline for comparing the drilling nanofluids data, the specific heat capacity of the base drilling fluid without nanoparticles was measured. The drilling nanofluids containing a type of nanoparticle i.e., alumina, titania, and silica at concentrations of 0.01, 0.05, 0.1 and 0.5 wt% were prepared and tested. The experimental results for the three types of drilling nanofluids that included 0.1 wt% nanoparticles are illustrated in Fig.5, with the base fluid for comparison. The specific heat capacities of the different samples were calculated from the slope of the straight line fitted on the data and reported in Table 3.

Fig. 5. The measured data and the fitted straight line for drilling fluid samples.
The specific heat capacity of the base drilling fluid was found to be 3.1598 J/gºC. The experimental results show that the addition of nanoparticles to this base drilling fluid enhances the specific heat capacity. The increase in heat capacity of the drilling fluid containing nanoparticles shows that drilling nanofluids can absorb more heat from the drill bit than conventional drilling fluids. The maximum heat capacity enhancement, 35.8%, was obtained with the addition of 0.5 wt% of alumina nanoparticles.

Table 3. The calculated specific heat capacity for drilling fluid samples.
Fluid sample Nanoparticle (wt%) Cp (J/g ºC) Cp enhancement (%)
Base drilling mud 0 3.1598 –
0.01 3.8917 23.16
Base mud + Al2O3 0.05 3.8334 21.31
0.1 4.1792 32.26
0.5 4.2918 35.82
0.01 3.3592 6.31
Base mud + TiO2 0.05 3.1952 1.12
0.1 3.4089 7.88
0.5 4.1219 30.45
0.01 3.5704 12.99
Base mud + SiO2 0.05 3.5002 10.77
0.1 3.9026 20.50
0.5 4.2722 35.20

The results in Table 3 also show the enhancement of specific heat capacity as a function of the nanoparticles’ weight fraction in the different drilling nanofluids. It is apparent that the specific heat capacity of drilling nanofluids increases nonlinearly with an increase in the nanoparticles concentration. It can be observed from the experimental data that the addition of more than 0.05 wt% of nanoparticles to the base drilling fluid causes the specific heat capacity to increase.
The trend of heat capacity increase with rising nanoparticle concentration clearly indicates that the enhancement rate of the heat capacity of the drilling nanofluid prepared by adding titania nanoparticles is faster than that of the other samples. This behavior can be attributed to the smaller sized titania nanoparticles. The enhanced heat capacity in nanofluids with smaller nanoparticles is due to the larger thermal vibrational energies of the particles’ surface atoms. The results show that the surface area to volume ratio for nanoparticles significantly affects the specific heat capacity of nanofluids. As the particles’ surface area to volume ratio increase, the number of surface atoms are increased. Thus, more heat is required to raise the temperature of surface atoms by one degree, and therefore the heat capacity is higher. [23]
One of the mechanisms considered for the increase of the specific heat capacity in nanofluids is the enhanced specific heat capacity of nanoparticles due to their higher specific surface energy compared with bulk material. Moreover, additional thermal storage mechanisms due to the high specific surface area of the nanoparticles, and the interfacial interactions between nanoparticles and fluid molecules, affect the nanofluid thermal properties. Another proposed mechanism is the formation of a solid-like nanolayer on the surface of the nanoparticles, which is likely to enhance specific heat capacity due to the smaller intermolecular spacing compared to the higher intermolecular spacing in the bulk liquid [24].
The enhancement of nanofluid thermal conductivity have been interpreted by different mechanisms based on the Brownian motion of nanoparticles [25], aggregation of nanoparticles [26], and formation of a nanolayer [27,28]. Among these mechanisms, the nanolayer effect is declared to be the most important factor affecting the specific heat capacity of nanofluids [28]. However, a molecular theory explaining the interfacial thermal characteristics and the effects of nanoparticles on the specific heat capacity of these fluids does not yet exist.
4.2. Rheological properties
The rheological behavior of any fluid is explained in terms of the relationship between shear stress (τ) and shear rate (γ ̇). The ratio of shear stress to shear rate is defined as viscosity which is a measure of resistance between the fluid’s adjacent layers during flow [29].
The rheological properties of the base drilling fluid with and without nanoparticles were measured and compared. To perform rheological analysis, the drilling fluid’s properties including the Apparent Viscosity (AV), Plastic Viscosity (PV), Yield Point (YP), and Gel Strength (GS) were investigated. The measurements were carried out according to API standards [30]. The rheological properties of the drilling fluid samples were measured using a Fann rotational viscometer, model 35A.
Several mathematical models that describe the behavior of non-Newtonian fluids are available. To determine which model is most appropriate to the drilling fluid samples, the shear stress over a range of shear rates were measured. The results for drilling nanofluid samples that included 0.1 wt% nanoparticles are shown in Fig. 6.

Fig. 6. Comparison of shear stress versus shear rate for the drilling nanofluids.
It is obvious that adding the nanoparticles to the drilling fluid increases the shear stress. The experimental data shows that for all drilling fluid samples the variation of shear stress with shear rate is not linear and exhibits viscoplastic shear thinning behavior. The Herschel-Bulkley model is found to be the best model.
The experimental results for yield point, apparent viscosity and plastic viscosity for the different drilling nanofluid samples are shown in Table 4. The apparent viscosity and the plastic viscosity for the base drilling fluid in the absence of nanoparticles were 42.5 and 24 cP, respectively. The experimental measurements show that the apparent viscosity and the plastic viscosity for the base drilling fluid increases with the addition of nanoparticles. Moreover, the AV and PV values of the drilling nanofluids rise with an increasing concentration of nanoparticles. As can be seen in Table 4, for the titania nanoparticles, an irregular reduction is observed after increasing the concentration from 0.01 to 0.05 wt%. However, further increase in titania nanoparticles causes the AV and PV values to increase. The increase of drilling nanofluid viscosity can be attributed to the increase in friction between fluid layers in the presence of nanoparticles [29].

Table 4. The rheological properties of drilling fluid samples.
Fluid sample Nanoparticle (wt%) YP (lb/100 ft2) AV (cP) PV (cP)
0.01 39 47.5 28
Base mud + Al2O3 0.05 42 49.5 28
0.1 44 50 29
0.5 47 52.5 30
0.01 38 46 27
Base mud + TiO2 0.05 35 42.5 25
0.1 39 47 28
0.5 40 47.5 32
0.01 41 47.5 27
Base mud + SiO2 0.05 48 51 27
0.1 49 51.5 27.5
0.5 60 65.5 28

The ability of a drilling fluid to carry drill cuttings out of the annulus is evaluated by the value of the yield point, which should be high enough for proper cuttings transport. However, large yield point values generate extra pump pressure that must be inhibited. The yield point is dependent on the electro-chemical charges in the drilling fluid under flowing conditions. The predominance of the attractive forces between the particles leads to a high yield point value. In contrast, when repulsive forces prevail, a decrease in yield point value is observed. However, the yield point value can be adjusted using various chemical additives [31].
The measured yield point value for the base drilling fluid was 37 cP. Table 4 shows that the addition of nanoparticles to the base drilling fluid increases the YP value. Moreover, the YP of drilling nanofluids increases when a greater concentration of nanoparticles is added. The maximum value of YP (i.e., 60 lb/100 ft2) was obtained with silica nanoparticles in a concentration of 0.5 wt%.
The rheological properties of the base drilling fluid have been compared with drilling nanofluids in Fig. 7. It is obvious that the drilling nanofluids prepared by addition of different nanoparticles exhibit better rheological properties than the base drilling fluid [32, 33].

Fig. 7: Comparison of the rheological properties of the base drilling fluid with samples
containing 0.5 wt% nanoparticles.

The gel strength (GS) of a fluid is a measure of the minimum shearing stress necessary to produce slip-wise movement in fluids and is generally obtained in two ways: measurement immediately after preparation of the drilling fluid (10 s GS) and measurement after the mud in the cup has rested for 10 min (10 min GS) [34, 35].
The measured 10 s GS and 10 min GS of the base drilling fluid were 7 (lb/100 ft2) and 8 (lb/100 ft2), respectively. The gel strengths of the drilling fluid samples prepared with the addition of nanoparticles (Table 5) show that GS values for drilling nanofluid samples change according to the concentrations of nanoparticles. The variations of the GS values with nanofluid concentrations do not follow a specific trend; in fact for some of the nanoparticle concentrations, there is no change in the values of 10 s either the 10 min GS. These values for the alumina nanoparticles do increase when the concentration is increased. The GS values of the titania nanoparticles decline when the concentration drops from 0.01 to 0.05 wt%. The maximum GS values (i.e., 11 lb/100 ft2 after 10 s and 12 lb/100 ft2 after 10 min) were obtained for silica nanoparticles in a concentration of 0.5 wt%. The GS of the base drilling fluid and samples containing 0.5 wt% of the different nanoparticles are compared in Fig. 8.
Table 5. The gel strength for drilling fluid samples at various nanoparticle concentrations.
Nanofluid sample Nanoparticle (wt%) 10 s GS
(lb/100 ft2) 10 min GS
(lb/100 ft2)
0.01 7 9
Base mud + Al2O3 0.05 8 9
0.1 9 10
0.5 9 11
0.01 9 10
Base mud + TiO2 0.05 7 8
0.1 9 10
0.5 9 10
0.01 9 10
Base mud + SiO2 0.05 11 12
0.1 10 11
0.5 11 12

Fig. 8. Comparison of the gel strength of the base drilling fluid with samples containing 0.5 wt%
nanoparticles.

5. Conclusion
Considering the importance of efficient drill bit cooling by the drilling fluid, especially in deep drilling operations, the variations of the specific heat capacity of water-based drilling fluids in the presence of nanoparticles were investigated experimentally. A base drilling fluid prepared on the basis of industrial formulation was augmented with various concentrations of alumina, titania and silica nanoparticles to produce drilling nanofluids.
The experimental results show that the addition of these nanoparticles to the base drilling fluid enhances the specific heat capacity nonlinearly. A maximum value of 35.8% increase in the specific heat capacity compared to the base drilling fluid was observed with the addition of alumina nanoparticles with a weight fraction of 0.5%. The observed enhancements are attributed to the high surface area of the nanoparticles per unit volume, which leads to high specific surface energies. The rate of heat capacity increase of the drilling nanofluids varied with the nanoparticle concentration and type of nanoparticle. The experimental measurements showed that the enhancement rate of heat capacity with the addition of titania nanoparticles is faster than that with the other nanoparticles, which can be attributed to the smaller sized titania nanoparticles.
In addition, the effect of metal oxide nanoparticles on the rheological properties of the base drilling fluid was studied. The variation of shear stress with shear rate for all drilling fluid samples showed viscoplastic shear thinning behavior, and the best fitted model was found to be the Herschel-Bulkley model. The results revealed that the AV, PV, and YP of the base drilling fluid increased with increasing concentration of the added nanoparticles, except for the titania nanoparticles, for which a reduction was observed when the concentration was raised from 0.01 to 0.05 wt%. The maximum increase in rheological properties were obtained with titania nanoparticles in YP and silica nanoparticles in PV, both at a concentration of 0.5%wt. There is no direct relationship between the concentration of nanoparticles and the increase of gel strength in the limit of concentrations in this study.
This study has clearly confirmed that the addition of nanoparticles to drilling fluid favorably changes the thermal as well as rheological properties of the base drilling fluid and so should be thoroughly investigated for future industrial applications.

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