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Abstract
In this work, we investigate the dissociation behavior of natural gas hydrate in a closed system with microwave (MW) heating and hot
water heating. The hydrate was formed at temperatures of 14 C and pressures of 4.55.5 MPa. It was found that the gas hydrate dis-
sociated more rapidly with microwave than with hot water heating. The rate of hydrate dissociation increased with increasing microwave
power, and it was a function of microwave power. Furthermore, the temperature of the hydrate increased linearly with time during the
microwave radiation.
2008 Elsevier Ltd. All rights reserved.
0196-8904/$ - see front matter 2008 Elsevier Ltd. All rights reserved.
doi:10.1016/j.enconman.2008.01.031
2208 D.-L. Li et al. / Energy Conversion and Management 49 (2008) 22072213
Fig. 2. Variation of the pressure and temperature with time during hydrate formation.
3.1. The procedure of hydrate formation Fig. 3 illustrates the change of pressure and temperature
with time during the natural gas hydrate dissociation pro-
The temperature in the water bath and solution and the cedure under microwave irradiation.
pressure in the cell during the hydrate formation procedure Point a represents the time of microwave injection. The
were measured and are given in Fig. 2. As seen in Fig. 2, at hydrate begins to dissociate at point b. The temperature
around 6 h, the temperature increased and the pressure increased but the pressure did not change from a to b. At
decreased sharply, which indicated the formation. point c, the hydrate was dissociated completely. The
Fig. 3. Variation of the pressure and temperature with time during hydrate dissociation.
2210 D.-L. Li et al. / Energy Conversion and Management 49 (2008) 22072213
temperature increased linearly with time during the micro- about 60 W. The power input of microwave power is
wave radiation from b to c. The time from a to b varied in 150 W, and 60% of the power was reected by the cell bot-
the dierent tests, so we discuss the process from b to c. tom because the sample was too small to absorb the total
Here, the total time of hydrate dissociation was dened microwave power. The value of the reected power can
from b to c, which characterized the rate of hydrate be indicated by directional couplers. The results show that
dissociation. the pressure decreased slightly after microwave injection or
bath heating. The pressure decrease may be because part of
3.3. Eects of dierent power of microwave on the methane the free water was transformed into gas hydrate. In this
hydrate dissociation test, the total time of hydrate dissociation was 30 min
equation: 70
b
t kw 1
60
Here, k is 687.07 and b is 0.5132 by tting the experi-
mental data. The related coecient R2 is 0.99. 50
Fig. 6. The process of microwave irradiation and water bath heating: (a) microwave irradiation and (b) water bath heating.
under microwave irradiation. However, the time required study, but it illustrates that microwave heating can speed
under water bath heating was 50 min. up hydrate dissociation relative to bath heating.
Energy ratio comparisons of microwave irradiation and
water bath heating are described in Table 2. Here, the nom-
inal heating value of the gas was 37,250 kJ/m3, and the heat Table 2
Energy eciency comparisons of microwave and hot water heating
capacities of stainless steel and quartz glass are 0.05 J/g K
and 0.772 J/g K, respectively. In the cell, the weight of Microwave Water-bath
heating heating
stainless steel is 7443 g and the weight of quartz glass is
1022 g. By preliminary calculation, the energy ratio of Evolving water of the sample (g) 50 50
Heating power (W) 60 60
microwave heating is 3.17. It is greater than that of water Gas content (V/V) 150 150
bath heating, but it is lower than the value of thermal stim- Total time of hydrate dissociation (min) 30 50
ulation production reported by Tang et al. [13]. Temperature rise of the cell during the 18 10
Because of the laboratory condition, the system was not hydrate dissociation (K)
in thermal insulation and much of the heat was lost. The Absorption heat of cell (kJ) 19.98 11.61
Energy ratio 3.17 1.66
energy ratio described in Table 2 is only a preliminary
2212 D.-L. Li et al. / Energy Conversion and Management 49 (2008) 22072213
3.5. Microwave energy conversion of the medium; and f is the electromagnetic wave
frequency.
The dielectric properties of gas hydrates in combination As energy is absorbed within the material, the electric
with the applied electromagnetic elds result in the conver- eld decreases as a function of the distance from the sur-
sion of electromagnetic energy to heat. The power that is face of the material. Therefore, Eq. (4) is valid for only very
transmitted to an object can be determined by the use of thin materials. The penetration depth is dened as the dis-
the Poynting vector theorem [14], which can be derived tance from the sample surface where the absorbed power is
from the Maxwell equations. The power that is transmitted 1/e of the absorbed power at the surface. Beyond this
across the surface, S, of a volume, V, is given by the real depth, volumetric heating due to microwave energy is neg-
portion of the following equation: ligible. Assuming the dielectric constant of free space is e0,
I the penetration depth is given by the following equation:
1
W E H dS 2
2 s ce0
d 5
Here, W is the density of heat sources. E H* is the Poyn- 2pf e00
ting vector and the *, in this case, denotes the complex con- The penetration depth and knowledge of how the elec-
jugate. Using the divergence theorem, Maxwell equations tric eld decreases from the surface are particularly impor-
and by assuming the hydrates properties for the volume, tant in processing thick materials. If the penetration depth
the following equation can be obtained for the real portion of the microwave is much less than the thickness of the
of the Poynting power theorem material, only the surface is heated. The dielectric proper-
Z ties of gas hydrate are unknown. It is generally agreed that
1
W xlH H xe00 E E rE E dV 3 the dielectric constant of gas hydrate is 58 [15]. It is also
2
reported that the average dielectric constant of the hydrate
Here, l represents the imaginary component of the mag- zones is 9, ranging from 5 to 20 in the Mallik 5L-38 Well in
netic permeability and r is the conductance. In dielectric the Mackenzie Delta, Canada [16]. Generally, the dielectric
materials, the magnetic permeability is usually small, and constant of ice is 94 and the penetration depth is 70 cm.
the rst term can be neglected. In addition, xl can be con- When the microwave frequency is 2.45 GHz, therefore,
sidered as an equivalent conductance. If the electric eld is the penetration depth of gas hydrate is more than 70 cm,
assumed to be uniform throughout the volume, the follow- so we think the microwave eld is uniform throughout
ing simplied equation for the power, W, absorbed per unit the volume in this test. The velocity of the temperature
volume can be obtained from Eq. (4) increase is given by the following equation:
e00 Qh M C p T T 0
W pf e0 e0 tan dE2 ; tan d 4 w 6
e0 t t
Here, e0 is the permittivity of vacuum; e0 and e00 denote the During the test, the microwave power is invariable, and
real and imaginary parts of the permittivity of the medium, Cp is considered a constant at a small temperature varia-
respectively; tand is the tangent of the dielectric loss angle tion. The rate of hydrate dissociation increased with
Fig. 7. The scheme for gas recovery from in situ hydrate use microwave heating: (1) microwave generator, (2) microwave transducer, (3) transmission line
on ground, (4) gas storage equipment, (5) gas ow line, (6) platform surface, (7) exterior pipe, (8) sleeve, (9) interior pipe (transmission line in well), and
(10) receiving antenna.
D.-L. Li et al. / Energy Conversion and Management 49 (2008) 22072213 2213
increasing microwave power, and the temperature pose of recovering natural gas from in situ hydrate
increased linearly with time during the microwave radia- reservoirs.
tion (Fig. 4).
On dierent powers of microwave radiation, the end Acknowledgements
temperature at complete dissociation of the gas hydrate is
related to the microwave power. The relation can be writ- This work was supported by The National Natural Sci-
ten as follows: ence Foundation of China (50676097) and the Guangdong
T /W 7 Natural Science Foundation (05200113).
In accordance with Eq. (6), the total time of hydrate dis- References
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