Abstract
Moisture content in coal is an important factor affecting the coal seam gas extraction. It directly affects the storage and flow of gas in bituminous coal. In this paper, the cylindrical bituminous coal cores of Xutuan coal mine in Huaibei coal mine group were studied as experimental objects, using the laboratory self-designed experimental device
Introduction
Improvement of coal permeability and an efficient, safe gas extraction from coal seams is an actual research topic (Long et al., 2017; Zhu et al., 2017). Gas extraction intensity depends on many parameters such as its content and thermodynamic conditions, as well as adsorption and flow characteristics of coal (Li et al., 2017; Liu et al., 2018; Wu et al., 2014). Among them, moisture content is one of the important factors affecting gas adsorption. Therefore, this paper mainly studies the effect of moisture content on CH4 adsorption and deformation characteristics of bituminous coal.
Many research teams studied coal adsorption of CH4, CO2, N2, and other adsorptive gases (Bae and Bhatia, 2006; Meng and Li, 2017; Ottiger et al., 2008; Song et al., 2015). As a porous medium, coal adsorbs gas molecules through the Van der Waals intermolecular forces attraction, and coal gas adsorption is reversible. The gas adsorption of coal is usually indicated by the adsorption isotherm. Many experimental studies of isothermal adsorption of different coals have been carried out. Several methods for adsorption isotherm tests have been developed: the volumetric method (Chareonsuppanimit et al., 2012; Krooss et al., 2002; Meng et al., 2015; Mohammad et al., 2008; Shen et al., 2015), gravimetric method (Ottiger et al., 2008; Song et al., 2015), direct adsorption method (Hol et al., 2011), etc. The testing methods were compared and improved by Kudasik (2017) and Zhang et al. (2013).
The main factors affecting coal gas adsorption are the moisture content (Nie et al., 2015; Nie et al., 2016; Teng et al., 2017), temperature (Crosdale et al., 2008), gas pressure (Song et al., 2015), the particle size of coal (Yuan et al., 2017; Zhang et al., 2014b), coal rank (Nie et al., 2016; Shen et al., 2015), and ash content, cleat (Jing-Ming et al., 2008). Among them, moisture content is the main factor affecting gas adsorption and desorption (Crosdale et al., 2008; Guo and Guo, 2017; Wang et al., 2014). Water in coal presents in different states (chemically bonded, adsorption, capillary, and free, etc.), but the absorbed moisture influences most strongly on gas adsorption characteristics of coal (Zhang and Ma, 2008). The water vapor adsorption capacity of coal is much higher than the capacity for methane sorption. Obviously, the amount of coal-adsorbed gas decreases if the moisture content in coal is high (Bae and Bhatia, 2006). At the same time, the presence of adsorbed moisture leads to the decrease of pore connectivity of coal and influences the further adsorption of coal on gas (Cheng et al., 2017; Yang et al., 2016).
Philip and De Vries (1957) studied water transfer in porous media and derived equations to determine liquid vs. gaseous state of water. Joubert et al. (1973) believe that moisture beyond the critical point has no further effect on methane adsorption. Some researchers carried out laboratory experiments to find the relationship between the moisture content in coal and the amount of methane adsorbed. Liu et al. (2014) performed isothermal desorption experiment of drying coal sample, liquid water wetting coal sample, and high-pressure water injection into coal sample after methane adsorption, and found that the adsorption capacity of coal samples at high-pressure water injection was significantly higher than that of coal sample at liquid water wetting. He (2015) considered water displacement desorption and inhibiting desorption of gas adsorbed in coal. Wang et al. (2017) studied the effect of inherent moisture on hard coal adsorption–desorption characteristics, found that moisture occupies a certain space of the pore structure and reduces the density of gas adsorption sites in coal. Zhang and Ma (2008) studied the adsorption isotherm of different metamorphic coals with different moisture contents and deduced the correction coefficient of coal moisture effect on its methane adsorptive capacity. Gensterblum et al. (2013) studied sorption isotherms of Australian subbituminous, German high-volatile bituminous, and German anthracite coals in dry and moisture-equilibrated states and concluded that the sorption capacity of dry coals followed a parabolic function of the coal rank while the sorption capacity of moisturized coals depended linearly on it. Nie et al. (2016) performed experiments of sorption characteristics of methane in various rank coal samples at different moisture contents and concluded that the effect of moisture content on a low-rank coal was higher than that on a high-rank coal. Guo et al. (2015) made use of a new water injection and gas adsorption device to conduct isothermal adsorption experiments on low rank coal for different moisture contents and concluded that the inhibition degree of moisture on gas adsorption capacity increase with the increase of moisture content. Clarkson and Bustin (2000) carried out experiments on the effects of moisture content on the adsorption characteristics of a mixture of CH4 and CO2 and deduced that the moisture in a coal reduced the selectivity to CO2. Zhang et al. (2014a) used a modified indirect gravimetric method to test sorption isotherm and found that moisture in a coal affected more on the adsorption capacity of CH4 than on CO2 adsorption capacity. Teng et al. (2017) established a fully coupled multi physical model of coal deformation, gas flow and water loss, and got the water loss, which improved the porosity and permeability of coal.
In addition to studies of the influence of moisture content in coal on its gas adsorption characteristics, some researchers also analyzed the influence of the moisture content in coal on its volume. Among them, Fry et al. (2009) studied coal swell induced by water adsorption and found that the volume of adsorbed water is linearly related to the pore volume of coal. Van Bergen et al. (2009) believe that moisture is a competitor of gas adsorption. Thus, it affects the coalbed methane extraction.
But the influence of moisture content in coal on gas adsorption characteristics was studied mostly on crushed or briquette coal samples. It is difficult to measure adsorption characteristics of a coal seam. Therefore, in this paper, the bituminous coal of Xutuan coal mine was used as the object of study, employing the laboratory self-designed experimental device
Measurement of the moisture content in Xutuan coal mine bituminous coal
Occurrence characteristics of bituminous coal
The Xutuan coal mine belongs to Huaibei mining area (as shown in Figure 1(a)), and the main coal seams are 32, 71, 72, and 82 of Permian. The 32 coal seam is bituminous rank coal; it mainly includes metabituminous and 1/3 of coking coal. The main water filling source of 3237 working face is the coarse sandstone fissure of the top coal seam and the dynamic water of 3235 goaf in the upper section. Boreholes are arranged at the bottom of 3237 working face. By measuring the coalbed methane pressure and the coal seam gas content, the maximum original gas pressure of 0.53 MPa was found, and the maximum original gas content was 5.80 m3/t. The Xutuan coal mine location in China and the borehole diagram of the longwall face are shown in Figure 1. The industrial analysis results and the gas adsorption parameters of the coal samples from 3237 working face conveyor entry of 32 coal seam in Xutuan coal mine are shown in Table 1.

The Xutuan coal mine location in China (a) and the borehole diagram (b) of the longwall face.
Industrial analysis results and adsorption constants of coal samples from 32 coal seam in Xutuan coal mine.
Note: BET (Brunauer-Emmett-Teller)
Preparation of coal samples with different moisture contents
In this paper, the preparation of coal samples with different moisture contents was made according to the method used by Pan and Yang (Pan et al., 2010; Yang et al., 2016). In general, the moisture content in coal means the adsorbed water that is the total moisture (
The air-drying base moisture (
The equilibrium moisture (
Table 1 shows that the
Moisture content (
First, we selected lump coal in the Xutuan coal mine then packed it in the sealed plastic bag, transported to the laboratory, and finally prepared coal samples of Φ50 × 50 mm sizes by drilling coal before the experiment. In this paper, HB3, HB4, HB5, and HB6 (HB represent Huaibei) coal samples were selected to investigate the influence of the moisture content on their gas adsorption characteristics. The individual parameters of the experimental coal samples are listed in Table 2. The samples are shown in Figure 2.
Parameters of coal samples.
HB: Huaibei.

Experimental coal samples. (1) HB3, (2) HB4, (3) HB5, (4) HB6.
For convenience, the samples were put into small steel bowls. After weighing the total mass of the sample and the bowl, both of them were put into a vacuum drying oven with a temperature of 100°C. With the certain period, the sample and the bowl were taken out for weighting and data record. When the sum of the mass of the two is no longer lowered for a long time, the drying was finished. After drying for more than 40 hours, coal samples were dry. The calculated original moisture content values are presented in Table 3. Table 3 shows that the original moisture content was 1.28–1.39% and the average value was about 1.3% (that is consistent with
Coal samples moisture content.
HB: Huaibei.

The original moisture content of coal samples as a function of time at heating in vacuum oven. (a) HB3, (b) HB4, (c) HB5, (d) HB6.
The fitting formula and the fitting precision for the moisture content decrease in coal samples.
HB: Huaibei.
Firstly, Dried coal samples were placed in a vacuum environment. After the temperature of samples dropped to room temperature, they were put into the vacuum dryer as shown in Figure 4 to speed up wetting and the water was soaked through the lower end of the samples. Finally, samples were weighed through the certain periods until the mass of each sample remained unchanged. Thus, the samples were water saturated after wetting for 250 hours. The saturated moisture content of coal samples was calculated, and the dates are listed in Table 5. It can be seen from Table 5 that the saturated moisture content of coal samples is 2.26–2.55% with an average value of about 2.4%. It can be seen from Figure 2 that HB3 sample is more fractured than the other three samples, so the saturated moisture content of HB3 was higher. The fitting analysis of the experimental data using Origin software provided the curve and the formula of moisture content increase along with the time (as shown in Figure 5 and Table 6), and the fitting precision parameter (R2) reached 0.99. From Figure 5 and equation (5), that the moisture content of coal samples at wetting increases as Exponential Association (Exp Assoc) function. A relation of the moisture content increase at wetting vs. time is obtained

Vacuum dryer.
Saturated moisture content of coal samples.
HB: Huaibei.

Raise curve of coal sample moisture content. (a) HB3, (b) HB4, (c) HB5, (d) HB6.
The fitting formula and the fitting precision for the moisture content increase in coal samples.
HB: Huaibei.
Using the above experimental method, we obtained bituminous coal samples with 0.0, 0.5, 1.0, 1.5, 2.0, and 2.4% moisture content. We used them for the study of effects of coal moisture content on gas adsorption characteristics.
Experimental system and experimental design
GASTA system
1. Composition of experimental system
The GASTA system mainly consists of the following components: the adsorption cavity system (including reference cylinder and sample cylinder) (withstand pressure 20 MPa), gas decompression system (test gases including CH4, N2, He, CO2), temperature control system (room temperature – 100 ± 0.1°C), vacuum system, acquisition control system, strain testing system, and other systems. Figure 6 is the physical map of GASTA system.

GASTA system.
2. Experimental principles
The experimental coal samples were placed in a sealed sample cylinder to measure the adsorption volume of CH4 and other gases when the adsorption equilibrium was reached under different gas pressure conditions (0–12 MPa). According to the Langmuir monolayer adsorption theory, the Langmuir volume (

Schematic diagram of GASTA system.

Coal samples with strain gauges.
3. Operation process of experimental system
Set the water bath temperature and paste the axial and hoop strain gauges on the coal sample (as shown in Figure 8) and perform zero calibration on the system; Use N2 to test the pressure resistance of the system and check the hermeticity of the experimental system; Vacuum the system and install the coal sample, connect the interface of strain gauge; The He was used to measure the void space of the sample cylinder under the pressure of 2.0, 3.0, and 4.0 MPa, and the average value was calculated as the void space of sample cylinder; Vacuum the system and test gas adsorption and adsorption deformation under different pressures; Vent gas and remove the coal sample.
Experiment principle analysis of coal adsorption
According to the gas pressure and temperature in the reference and sample cylinders before and after adsorption equilibrium, the gas adsorption capacity and saturation under different gas equilibrium pressures were calculated. The adsorption experiments were carried out and the influence of moisture content on coal gas adsorption characteristics is characterized.
Firstly, we measured the pressure in the reference and sample cylinders before and after the same equilibrium pressure at a temperature of
The gas equation is as follows
The most fundamental operational procedure to quantify gas adsorption is the Gibbs approach. Thus, on the basis of previous studies, this paper decides to adopt Gibbs approach (Gensterblum et al., 2013; Krooss et al., 2002; Zhang et al., 2014c).
The number of moles of the total gas (
The amount-of-substance of gas in the void space (
The molar number of the gas adsorbed (
The total volume of adsorption gas (
The related gas adsorption capacity (
The coal adsorption isotherms are usually used to determine the coal adsorption capacity in a laboratory. We applied the Langmuir model in this study. Comparing the adsorption capacity of CH4 in different moisture content coals, we obtained the influence of bituminous coal moisture content on gas adsorption characteristics. The Langmuir equation is the following
According to the ratio of gas adsorption equilibrium pressure to the related adsorption capacity (
The relation between
The coal gas adsorption saturation is the ratio of the adsorbed gas amount to the maximum adsorbed gas amount. According to equation (12), the maximum adsorbed gas amount is
The effect of coal moisture on its gas adsorption mainly depends on adsorption strength of coal to different gases (equation (17)). Since the adsorption capacity of coal to H2O exceeds that to CH4 (Bae and Bhatia, 2006), the influence of coal moisture content on gas adsorption was studied.
Coal samples deformed during the process of gas adsorption (Van et al., 2009). In the experiment, the axial and hoop strain gauges were pasted on coal samples, and the deformations of samples with different moisture contents were monitored during the process of gas adsorption. The volumetric strain of the coal samples was calculated by equation (18).
Experiment scheme of adsorption
Experiment scheme for adsorption of CH4 by bituminous coal
The water bath temperature was set at 30°C. Before the experiment, the system withstood pressure test with N2, and then the free volume of the sample cylinder was measured by helium. The initial pressure in the reference cylinder was 1 MPa, while the initial pressure in the sample cylinder was 0.1 MPa. After 24 hours of CH4 adsorption, the equilibrium pressure was obtained, and the gas compressibility coefficient, SRK molar volume, and gas adsorption capacity at different gas pressures were calculated. The above procedures were repeated under the conditions of the initial pressure in the reference cylinder of 1.5, 3.0, 4.0, 5.0, and 6.0 MPa, respectively, and the gas adsorption capacity, isothermal adsorption curve, and adsorption parameters were obtained under the conditions of different gas equilibrium pressures. The strain data of coal samples were recorded every 30 minutes. Figure 9 shows the adsorption pressure path.

The adsorption pressure path.
Experiment scheme for studies of the moisture content influence on CH4 adsorption characteristics of bituminous coals
Through the analysis of measurements of bituminous coal moisture content, the maximum moisture content investigated in this paper was about 2.4%. Taking sample HB6, we studied the influence of the moisture content on gas adsorption characteristics at six values of the content: 0.0, 0.5, 1.0, 1.5, 2.0, and 2.4%. The selected moisture content for the adsorption experiments and the related actual moisture content in the samples are listed in Table 7. During the experiment, in order to ignore the macroscopic flow velocity of the gas in the reference cylinder as it enters the sample cylinder, we slowly open the connection valve between the two cylinders. And because it is not the gas seepage experiment, therefore, the macroscopic flow velocity of the gas in the sample cylinder is negligible. Thus, the changes of moisture content in the experiment are negligible.
Designed and actual moisture content for adsorption experiments.
Experimental results and analysis of the coal gas adsorption
Experimental results and analysis of coal adsorption under the same moisture content
Isothermal gas adsorption curve
By equations (7) to (12), the gas adsorption mole number, gas adsorption volume, and gas adsorption capacity of coal samples with different moisture content under different equilibrium gas pressures were obtained. The

P–P/V diagram of coal samples with different moisture contents.
Linear fitting equation parameters and correlation coefficient of P/V–P diagram.
The slope and the intercept of the obtained linear equation were substituted into equations (13) and (14), and the Langmuir volume (
Gas adsorption parameters.

Adsorption isotherms for different moisture contents.
2. Adsorption saturation
According to equation (16), the gas adsorption saturation is the ratio of the gas adsorption capacity to the adsorption capacity limit. When the adsorption constant

Relationship between the adsorption saturation and gas pressure at fixed moisture content.
According to equation (16), the gas adsorption saturation depends on the adsorption constant 3. Variation of strains at gas adsorption
In the experiment, the tensile strain was positive while the compressive strain was negative. According to the axial and hoop strain values monitored in the experiment, the corresponding volume strain was calculated by equation (18). We chose bituminous coal samples with the moisture content of 0.5% to draw the curves of its axial, hoop, and volume strains at different gas pressure condition (Figure 13).

Adsorption strain curve of coal sample.
As illustrated in Figure 13, at the fixed gas pressure, the variation trends of the axial and hoop strains are basically the same, and they increase with the increase of adsorption time. The strain growth rate decreases gradually, and the strain tends to a certain value. The results show that the coal possesses swelling deformation while adsorbing gas, but the expansion slows down gradually with the decrease of adsorption rate. The hoop strain is larger than the axial strain (
Experimental results and analysis of gas adsorption of coal samples with different moisture contents
Gas adsorption curve
The adsorption capacity and the moisture content under the same gas pressure condition are plotted in Figure 14. And the curve fitting of the scatter plot also carried out as shown in Figure 14. The parameters of the fitting equation were adjusted, so that the fitting formula describes the actual relationship between the gas adsorption capacity and the moisture content. The fitting of the experimental relation between the gas adsorption and the moisture content satisfies the single exponential attenuation function (equation (19)). The curve fitting formula parameters and the correlation coefficient of the moisture content are shown in Table 10. Using the fitting formula parameters in Table 10, the maximum moisture content corresponding to the minimum gas adsorption capacity of 0.001 ml/g was obtained as shown in Table 11.

Relationship between the adsorption capacity and moisture content under fixed gas pressure.
The fitting formula coefficients of adsorption capacity and moisture content under fixed gas pressure.
Adsorption amount limit and the related moisture content.
It can be seen from Figure 14, with the moisture content increase, the gas adsorption capacity and its rate gradually decreased. The adsorption capacity in dry condition is the maximum adsorption capacity under the certain gas pressure. When the moisture content increases to a certain magnitude, the gas adsorption capacity tends to 0, and the decrease rate approaches to 1. All the adsorption sites in coal are occupied by water in this case. As illustrated in Table 11, with the gas pressure increase, the maximum moisture content related to the minimum gas adsorption capacity increases (the default minimum order is 10−3 ml/g). When the gas pressure was 0.5 MPa, the maximum moisture content was 8%, while at the gas pressure of 5 MPa, the maximum moisture content increased to 18%.
The fitting formula for the gas adsorption capacity and the relative moisture content is
The Langmuir volume and Langmuir pressure of the coal samples with different moisture content are presented in Table 9. The variation trends of the Langmuir volume and Langmuir pressure were analyzed with the increase of moisture content as shown in Figure 15. It can be seen from Figure 15, the Langmuir volume is almost insensitive to the moisture content increase (that is, the maximum gas adsorption capacity is unchanged), while the Langmuir pressure increases linearly with the moisture content increase.

Relationship between
Linear fits of parameters

Relationship between parameter
2. Adsorption saturation
The dependencies of the gas adsorption saturation on moisture content at different gas pressures are shown in Figure 17. As illustrated in Figure 17, with the increase of the moisture content, the gas adsorption saturation and its rate decrease. The gas adsorption saturation is the largest at zero moisture content.

Relationship between adsorption saturation and moisture content at different gas pressures.
At fixed gas pressure value, the adsorption saturation decreases with the moisture increase from a dry state to lower moisture content state. For example, when the moisture content increases from dry to 0.5% the adsorption saturation decreases by nearly 50%. But with the increase of gas pressure, the decrease in adsorption saturation slightly reduces. Therefore, the influence of the moisture content on the gas adsorption reduces if the gas pressure is high.
3. Variation of strains at gas adsorption
As illustrated in Figure 13, the variation trends of axial and hoop strains are the same. Therefore, in this work, we studied the influence of moisture content on the adsorption strain by investigation of variation trend of the axial strain of bituminous coal samples with different moisture contents under fixed gas pressure. The axial strain curve of samples with different moisture contents under the gas pressure of 0.5 MPa is drawn in Figure 18. Since the strain gauges were pasted on coal samples before the experiment, the initial volume of coal samples differs, and it increases with the moisture content increase. The initial strain of samples at the beginning of the experiment was different. The scatter diagram of the initial axial strain of samples with different moisture contents is plotted in Figure 19.

Axial strain curves of coal with different moisture contents.

Initial axial strain of coal with different moisture contents.
As illustrated in Figure 18, the axial strain curves of coal samples with different moisture contents have the same trend for an increase with the adsorption time increase, while strain increase rate reduces with the adsorption time. At fixed adsorption time, the axial strain value of coal sample decreases with the increase of moisture content, that is, with the moisture content increase the adsorption capacity of coal samples decreases, and the expansion deformation decreases gradually. That result is consistent with the conclusions from Figure 14. As shown in Figure 19, the initial axial strain of the coal sample is larger if the moisture content is higher. Thus, the initial compression deformation decreases with the moisture content increase. Therefore, it can be concluded that the adsorption deformation of bituminous coal is strongly related to the moisture content. When the moisture content is high, the adsorption capacity and adsorption deformation of bituminous coal are less.
Conclusions
The average original moisture content and average saturated moisture content of coal samples from the Xutuan coal mine are 1.3 and 2.4%, respectively. At drying the original moisture content decreased following the exponential decay function of time, while at wetting the moisture content rose up according to Exp Assoc function. Using the designed GASTA With the moisture content increase, the gas adsorption capacity, as well as the adsorption saturation, reduced and their decrease rates gradually lowered. The swell deformation decreased gradually as well. The gas adsorption capacity and the moisture content followed the single exponential decay function. The gas adsorption capacity and saturation under fixed gas pressure were the largest in the dry condition. When the moisture content increases to a certain magnitude the gas adsorption capacity tends to zero, and the reduction rate approaches 1. With the gas pressure increase, the moisture content related the minimum gas adsorption capacity increased. At high gas pressure, the influence of moisture content on gas absorption was less. The adsorption deformation of bituminous coal is closely related to the moisture content. At high moisture content, the adsorption deformation of bituminous coal is less.
Footnotes
Declaration of Conflicting Interests
The author(s) declared no potential conflicts of interest with respect to the research, authorship, and/or publication of this article.
Funding
The author(s) disclosed receipt of the following financial support for the research, authorship and/or publication of this article: This research is supported by National Natural Science Foundation of China (51704274, 51704278, 51502339), Beijing Natural Science Foundation (8184082), the Young Talent Lifting Project from CAST, the Open Projects of State Key Laboratory of Coal Resources and Safe Mining CUMT (SKLCRSM16KF10, SKLCRSM16KF06), the State Key Laboratory Cultivation Base for Gas Geology and Gas Control (Henan Polytechnic University) (WS2017B02), Key Laboratory of Coal-based CO2 Capture and Geological Storage, Jiangsu Province CUMT (NO: 2016B09), and the Priority Academic Programme Development of Higher Education Institutions in Jiangsu Province, Postgraduate Research & Practice Innovation Program of Jiangsu Province (SJZZ16_0272).
