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Applied Energy 87 (2010) 2142–2147

Contents lists available at ScienceDirect

Applied Energy
journal homepage: www.elsevier.com/locate/apenergy

Coalbed methane liquefaction adopting a nitrogen expansion process


with propane pre-cooling
Ting Gao a, Wensheng Lin a,*, Anzhong Gu a, Min Gu b
a
Institute of Refrigeration and Cryogenics, Shanghai Jiao Tong University, Shanghai 200240, China
b
Department of Mining, Chongqing University, Chongqing 400044, China

a r t i c l e i n f o a b s t r a c t

Article history: Coalbed methane (CBM) is an important global energy resource and liquefaction is suggested to best uti-
Received 22 May 2009 lize it. Different from ordinary natural gas, CBM usually contains a high proportion of nitrogen, which
Received in revised form 21 November 2009 cannot be removed by purification procedures applied in ordinary natural gas liquefaction processes.
Accepted 13 December 2009
One approach for separating nitrogen from CBM is by distillation after liquefaction. In this way, nitrogen
Available online 8 January 2010
is liquefied together with methane, and the liquefaction system performance may change along with the
nitrogen content of CBM feed gas. The liquefaction process adopting nitrogen expansion with propane
Keywords:
pre-cooling is usually considered suitable for small-scale liquefaction plants due to its simplicity and
Coalbed methane (CBM)
Nitrogen content
is the focus of this paper. Taking the unit product liquefaction power consumption as the major index
Liquefaction process for analysis, optimum parameters of the liquefaction process for CBM feed gas containing different nitro-
Nitrogen expansion cycle gen contents are calculated. Based on the optimization results, the effects of nitrogen content as well as
Optimization the other two important technical indexes (liquefaction rate and methane recovery rate) on system per-
Power consumption formance are also investigated.
Ó 2009 Elsevier Ltd. All rights reserved.

1. Introduction uct from the producer to the consumer [4]. Unlike ordinary natural
gas, CBM usually contains a high level of nitrogen, which cannot be
Coalbed methane (CBM) is a valuable energy resource. Esti- removed by using the common purification technology used to
mates of global in situ CBM reserves now range between 99 and produce liquefied natural gas (LNG). Thus, nitrogen needs to be
212  1012 N m3, though not all reserves are technically recover- separated from the CBM to enrich its methane content. Such a pro-
able. Underground coal mines throughout the world, liberate an cess could be achieved by adsorption before liquefaction or by dis-
estimated 29–41  109 N m3 of methane annually, of which less tillation after liquefaction [4–7]. The CBM liquefaction–distillation
than 2.3  109 N m3 are used as fuel. The remaining methane is process is the focus of this paper. Distillation is an efficient separa-
vented to the atmosphere, representing a loss of the valuable en- tion technology. What demands attention is that for the liquefac-
ergy resource. China has the third largest CBM reserves in the tion–distillation process, nitrogen needs to be liquefied together
world (31  1012 N m3), an amount almost equal to its natural with methane, which may in turn increase the unit liquefaction
gas reserve, however, the CBM utilization rate in China is only power consumption of the system.
about 40%. Nonetheless though, CBM emissions can cause out- One typical liquefaction process used for natural gas is the
bursts and explosions. Worldwide, there have been thousands of nitrogen expansion liquefaction process, which is a good option
recorded fatalities from underground mine explosions in which for small-scale liquefaction plants because of its simple and com-
methane was a contributing factor. Furthermore, coal-related pact structure, thus it is also worth considering for CBM liquefac-
methane emissions contribute to global change, as methane is a tion. Adopting propane pre-cooling in this process, which is a
powerful greenhouse gas with a global warming potential (GWP) more efficient refrigeration method in the high temperature range,
of 21. Therefore, recovery of CBM is important not only for energy can consequently reduce power consumption efficiently [8–11].
utilization, but also for safety and environmental protection [1–3]. Taking unit product liquefaction power consumption as the ma-
As an efficient storage and transportation technology, liquefac- jor index for analysis, the optimum parameters of the liquefaction
tion of CBM provides a convenient means of getting the CBM prod- process at different nitrogen contents of CBM feed gas are calcu-
lated, and based on the optimization results, the effects of nitrogen
content as well as other two important technical indexes (liquefac-
* Corresponding author. Tel.: +86 21 34206533. tion rate and methane recovery rate) on the system performance
E-mail addresses: gtwgq@sjtu.edu.cn (T. Gao), linwsh@sjtu.edu.cn (W. Lin). are studied further.

0306-2619/$ - see front matter Ó 2009 Elsevier Ltd. All rights reserved.
doi:10.1016/j.apenergy.2009.12.010
T. Gao et al. / Applied Energy 87 (2010) 2142–2147 2143

Nomenclature

COP coefficient of performance (–) x methane recovery rate (–)


p pressure (kPa or MPa) y liquefaction rate (–)
qn molar flow rate (kmol/h)
qv gas volume flow rate at standard state (N m3/h) Abbreviations
t temperature (°C) CBM coalbed methane
W power consumption (kW) GWP global warming potential
w unit product liquefaction power consumption (kW h/ LNG liquefied natural gas
N m3)

2. Simulation details 2.2. Known parameters in the flow process

The simulation calculations and optimization of processes are Initially, some parameters are set or assumed as the basis of the
performed with HYSYS software (AspenTech). The Peng-Robinson process analysis. In the CBM liquefaction process the temperature
(PR) equation of state is used. of the feed gas for t101 = 35 °C, the pressure for p101 = 101.325 kPa,
the molar flow rate for qn101 = 1 kmol/h, the temperature after pro-
2.1. Liquefaction process pane pre-cooling (t106) is set at 5 °C higher than the propane refrig-
erant temperature (t305), the pressure of the product LNG is
The nitrogen expansion liquefaction process with propane pre- p109 = 101.325 kPa; likewise the temperature of LNG is determined
cooling is shown in Fig. 1. The pre-treatment for CBM is similar to by the given liquefaction rate (or methane recovery rate); in the
traditional purification of natural gas, by which water and some cold energy recovering backflow of flashed gas, t111 = t305,
acidic gases are removed. To simplify the computation and t112 = 30 °C.
analysis, the process of pre-treatment is omitted here, and it is In the propane pre-cooling process the condensation tempera-
assumed that the CBM consists of methane and nitrogen only ture is t303 = 35 °C and the sub-cooling temperature is t304 = 30 °C.
(Fig. 1). In the nitrogen expansion process t206 = t106, t208 is set at 5 °C
As shown in Fig. 1, CBM undergoes two stages of compression lower than t107, which can be calculated with HYSYS; the molar
and cooling using water-coolers, and then it is pre-cooled with flow rate of nitrogen is adjusted to guarantee an appropriate min-
propane in HEX-101 and cooled further with nitrogen in HEX- imum heat transfer temperature difference of HEX-102, which is
102. Following this process the pressure of the CBM is reduced, set as 3 °C.
and finally the LNG product is separated out in a liquid–vapor sep- The temperature of each fluid after being cooled by the water-
arator (V-101). The flash gas from the separator is diverted succes- cooler is 35 °C; the adiabatic efficiency of each compressor is
sively into HEX-102 and HEX-101 to recover its cold energy. 85%, the adiabatic efficiency of each expander is 80%; and the pres-
The process of propane pre-cooling is a vapor compression sure drop of each water-cooler and heat exchanger is set to 0 kPa to
refrigeration cycle with regeneration and is also shown in Fig. 1. simplify the analysis.
In the nitrogen expansion cycle, nitrogen firstly undergoes two
stages of compression and cooling firstly by using water-coolers, 2.3. Calculation and optimization method
and then by propane pre-cooling in HEX-101. Afterwards it under-
goes two stages of expansion to a low pressure and produces cold With above parameters set, there are still several parameters
energy for HEX-102. that are integral to make the liquefaction process work. Some of

Q-301
301 302 303 304
VLV-301 110
propane WC-301
W-301 305
C-301 306
112

HEX-103
Q-101 Q-102 111
V-101
101 102 103 104 105 106 107 108
WC-101 VLV-101
CBM WC-102
W-101 W-102
C-101 C-102
HEX-101
Q-201 Q-202 205 208
109
201 202 203 206
204
nitrogen WC-201 HEX-102 LNG
WC-202
207
W-201 W-202 W-203
W-204
C-201 C-202 E-201
E-202

Fig. 1. The CBM nitrogen expansion liquefaction process with propane pre-cooling.
2144 T. Gao et al. / Applied Energy 87 (2010) 2142–2147

them need to be optimized, such as the CBM pressure after com-


pression p104; the propane refrigerant temperature t305, i.e. the
evaporation temperature, and the nitrogen pressure after compres-
sion p204; the other parameters, whose effects on the system per-
formance will be investigated, are the nitrogen content of CBM
feed gas, the liquefaction rate and the methane recovery rate.
All of the optimizations and investigations are performed on the
basis of the calculation of the unit product liquefaction power con-
sumption w (kW h/N m3), which is one of the most important fac-
tors of the system performance (Eq. (1)). It can be defined as:
W com  W exp
w¼ ; ð1Þ
qv 109

where Wcom (kW) is the sum of each compressor’s power consump-


tion, Wexp (kW) is the sum of each expander’s power generation,
qv109 (N m3/h) is the gas volume flow rate of LNG product in its
standard state. These parameters were computed from the HYSYS
program.

3. Results and analysis

3.1. Parameters optimization

Unit product liquefaction power consumption w, is the main


function for the optimization process. The objective is to determine
what optimal parameters reduce w to a minimum. The optimal
parameters will be different for CBM with different nitrogen con-
tents. The calculations and analysis are performed with a liquefac-
tion rate assumed to be 95%.

3.1.1. Optimization of the CBM pressure after compression p104


The CBM should be compressed to a higher pressure which is
nearby its critical pressure, to gain better flow and heat transfer
characteristics. This is because the continuous cooling process
without phase transition of the supercritical CBM and the continu-
ous heating process of the nitrogen gas make their temperature
difference match well. Consequently the unit power consumption
is lowered down.
Take CBM with 50% of nitrogen content for instance, whose crit-
ical pressure is 5079 kPa, the change in unit power consumption w
along with p104 is shown in Fig. 2, and the heat exchange load var-
iation as a function of temperature of the pipelines in HEX-102
when p104 is 2.5 MPa, 4.5 MPa, and 6.5 MPa, respectively, are
shown in Fig. 3.
Fig. 2 shows that w decreases along with p104 increasing, how- Fig. 3. Heat exchange load in HEX-102.
ever the decreasing rate declines. Fig. 3 shows that, when p104 in-
creases, the heat exchange curves match better, and the maximum
temperature difference reduces. These results confirm that com- pression of CBM to a high pressure before cooling can improve
its heat transfer performance and consequently reduce the unit
power consumption. On the other hand, if the CBM pressure is
too high, the equipment cost of the plant will be very high. As a re-
0.82
sult, 4.5 MPa is chosen as the CBM liquefaction pressure, which is
0.80 also the usual liquefaction pressure for natural gas. This is a mod-
0.78 erate pressure close to its critical pressure, under which the harm-
w [kWh/Nm3]

ful effect of phase transition on the heat transfer performance is


0.76
limited.
0.74

0.72 3.1.2. Optimization of the propane refrigerant temperature t305


The lower t305 is, the more refrigerating load is reduced for the
0.70
nitrogen expansion cycle, therefore the power consumption in the
0.68 nitrogen expansion cycle will be reduced. However, the COP (coef-
2 3 4 5 6 7 8 9 ficient of performance) of the propane refrigeration cycle then de-
p104 [MPa] creases, so the power consumption in the propane cycle will
increase rapidly. As a result, there should be an optimal propane
Fig. 2. Change in unit power consumption w along with p104. refrigeration temperature.
T. Gao et al. / Applied Energy 87 (2010) 2142–2147 2145

0.90 the nitrogen pressure after compression (p204) at different nitrogen


contents (N2 %) are shown in Fig. 5.
0.85
Fig. 5 shows that the unit power consumption decreases rapidly
0.80 along with increasing p204. Correspondingly, the optimal pressure
N2%=0 of the nitrogen after compression can be set to its upper limit,
w[kWh/Nm3]

0.75 N2%=10 10 MPa.


N2%=20
0.70
N2%=30 3.1.4. Optimization result
0.65 N2%=40 Some types of thermodynamic diagrams, such as T–s or p–h dia-
gram, are good for demonstrating thermodynamic processes
N2%=50
0.60 clearly [12]. Taking the case when the nitrogen content is 10%,
N2%=60
and the liquefaction rate is 95% for instance, the temperature–en-
0.55 N2%=70 tropy diagram for the optimized process is shown in Fig. 6 to rep-
0.50 resent the optimization results.
-60 -50 -40 -30 -20

t305 [°C] 3.2. Study of system performance

Fig. 4. Changes in w with respect to t305 at different nitrogen contents. High nitrogen content is the main difference between CBM and
ordinary natural gas, thus the effect of nitrogen content on the sys-
tem performance is one of the most important aspects for study in
The changes of unit power consumption (w) along with the pro- the CBM liquefaction process. Equally important is consideration of
pane refrigeration temperature (t305) at different nitrogen content the liquefaction rate and the methane recovery rate which are also
(N2 %) are shown in Fig. 4. crucial technical indexes of the liquefaction process.
From Fig. 4, we can see that the optimum propane refrigeration In this section, the research is done on the basis of the above
temperature (which makes the unit power consumption mini- optimization results (see Section 3.1), i.e. t305 = 40 °C, p204 =
mum) decreases when the nitrogen content of the CBM increases. 10 MPa.
However, most optimum temperatures are lower than the pro-
pane’s normal boiling point (42 °C). This could cause two prob-
3.2.1. Effect of nitrogen content
lems: Firstly, the system needs to stay at a partly high pressure
The nitrogen content of the CBM has two effects on the liquefac-
state and partly in a vacuum pressure state, making it difficult to
tion systems power consumption. Firstly, nitrogen has a lower liq-
prevent leakages. The other issue is, along with the decreasing of
uefaction temperature than methane for its lower boiling point,
the evaporation temperature, the vapor density at the inlet of the
and this leads to more refrigeration power consumption for the
compressor will decrease rapidly, and the unit volume refrigera-
same cold energy demand. Therefore the liquefaction of CBM with
tion capacity of refrigerant will decrease accordingly. Therefore,
higher nitrogen content may consume more power. Secondly,
the size of the compressor has to be enlarged to an economically
nitrogen has a lower specific heat capacity than methane, thus
unacceptable scale to attain the needed refrigeration capacity.
the cold energy needed for gas cooling is lower. Also, the latent
Considering the calculated results and the practical consider-
heat of vaporization for nitrogen is lower than that of methane,
ations mentioned above, it is reasonable to make the optimal
which leads to less cold energy required for condensation. There-
refrigeration temperature a little higher than propane’s normal
fore, the liquefaction of CBM with a higher nitrogen content may
boiling point, i.e. 40 °C.
need less energy input. As a result, the changes of unit power con-
sumption with nitrogen content may not be monotonic.
3.1.3. Optimization of the nitrogen pressure after compression p204 The results of unit power consumption at different nitrogen
Considering the technical and commercial availability of com- contents when the liquefaction rate is assumed to be 100%, 95%,
pressors, the nitrogen pressure after compression can be no higher 90%, 85% and 80% respectively are shown in Fig. 7. When the lique-
than 10 MPa, thus only pressures between 4 and 10 MPa are con- faction rate is 100% and the nitrogen content is relatively high, the
sidered. The changes of unit power consumption (w) along with
300

0.80 250 204

200 104 102


Temperture [ºC]

0.75 150

N2%=0 100 202


w[kWh/Nm3]

302
0.70 N2%=10 50 303
N2%=20 304 205 203 105 103 101
0
N2%=30 206 106
0.65 -50 305 301
N2%=40 201 306
-100
N2%=50 207
0.60 -150
N2%=60 107
108 208
N2%=70 -200
0.55 0 50 100 150 200
4 5 6 7 8 9 10 Molar entropy [kJ kmol-1 ºC-1]
CBM nitrogen
propane bubble point and dew point line of CBM
p204 [MPa] saturation line of propane

Fig. 5. Changes in w with respect to p204 at different nitrogen contents. Fig. 6. Temperature–entropy diagram.
2146 T. Gao et al. / Applied Energy 87 (2010) 2142–2147

0.75 content increases, the optimal liquefaction rate firstly decreases


and then increases.
0.70
3.2.3. Effect of methane recovery rate
In practice, the most important outcome is whether or not the
w[kWh/Nm3]

0.65
y=0.80 methane can be recovered. Therefore, the methane recovery rate
y=0.85 (x), that is the molar flow rate ratio of the methane in the LNG
0.60 y=0.90 product to that of methane in the CBM feed gas, can be an impor-
y=0.95
tant index to calculate.
The changes of w with x at different nitrogen contents are
0.55 y=1.00
shown in Fig. 9. Because low methane recovery rates together with
high nitrogen content may result in very low liquefaction rates and
0.50 consequently very high unit power consumption, only nitrogen
0 20 40 60 80 contents of 0–30% for CBM are considered here.
N2 [mol%] As shown in Fig. 9, there is an optimal methane recovery rate
which makes the unit power consumption reduce to a minimum,
Fig. 7. Changes in w with respect to N2 % at different liquefaction rates. and the optimal methane recovery rate increases along with
increasing nitrogen content.
liquefaction temperature is too low for nitrogen expansion cycle to Furthermore, the liquefaction rate decreases rapidly with
attain, so only nitrogen contents between 0% and 30% are increasing nitrogen content at the same methane recovery rate,
considered. as shown in Fig. 10 (where x = 95%). For example, when the nitro-
Fig. 7 shows that, w monotonically increases with increasing gen content is 50%, only 60% of the liquefaction rate is needed to
nitrogen content, although the rate of the increase drops when reach 95% of methane recovery rate. Therefore, for the purpose of
nitrogen content becomes high. That means that the effect of boil- methane recovery, a high liquefaction rate for CBM with high
ing point differences between nitrogen and methane may be great- nitrogen content is not required.
er than that of the specific heat capacity and the vaporization
latent heat differences. Furthermore, the propane refrigerant tem- 3.2.4. Methane enrichment
peratures are different from the optimal values for some of the Despite the fact that CBM has a high nitrogen content, methane
nitrogen levels tested, which also makes w increase along with may be enriched during CBM liquefaction process. Fig. 11 shows
increasing nitrogen content. the changes in methane content between CBM feed gas and the
LNG product at different nitrogen contents and liquefaction rate.
It is evident from Fig. 11 that the methane content of CBM in-
3.2.2. Effect of liquefaction rate
creases after liquefaction, or the purity of methane can be im-
Liquefaction rate (y) is the molar flow rate ratio of LNG product
proved by liquefaction. Furthermore, the lower the liquefaction
to CBM feed gas, which is one of the major technical indexes of the
rate is, the more the methane content increases. When the nitro-
LNG process.
gen content increases, the difference in methane content between
Liquefaction rate y also has two effects. Firstly, when the lique-
the CBM feed gas and LNG product firstly increases and then de-
faction rate increases, the liquefaction temperature will decrease,
creases. For example, the methane content can be improved from
which causes an increase in unit power consumption; secondly,
80% to greater than 90% at a liquefaction rate of 85%, and from
the increased liquefaction rate will also result in a decrease in
70% to almost 90% at a liquefaction rate of 75%. That means that
methane content of the LNG, which means more nitrogen partici-
liquefaction itself can produce high quality LNG from CBM without
pates in the process of heat exchange and condensation, thus
requiring adsorption or distillation.
decreasing unit power consumption.
The result described in the preceding paragraph indicates that
The changes of w with y at different nitrogen content are shown
when the liquefaction rate is lower, the purity of methane is im-
in Fig. 8.
proved; however, this sacrifices the methane recovery rate to a cer-
As shown in Fig. 8, there is an optimal liquefaction rate which
tain extent and results in higher unit power consumption.
reduces power consumption to a minimum. When the nitrogen

0.75 0.75

0.70 0.70

N2%=0
w[kWh/Nm3]

N2%=0
w[kWh/Nm3]

0.65 N2%=10 0.65


N2%=5
N2%=20
N2%=10
0.60
N2%=30
0.60
N2%=15
N2%=40
N2%=20
N2%=50
0.55 0.55 N2%=25
N2%=60
N2%=30
N2%=70
0.50 0.50
0.70 0.75 0.80 0.85 0.90 0.95 1.00 0.80 0.85 0.90 0.95 1.00

y x

Fig. 8. Changes in w with respect to y at different nitrogen contents. Fig. 9. Changes in w with respect to x at different nitrogen contents.
T. Gao et al. / Applied Energy 87 (2010) 2142–2147 2147

1.00 On the basis of the process optimization, the effects of some


0.90 important indexes on the system performance are further studied.
0.80
The CBM pressure after compression is set as 4.5 MPa, with consid-
eration from both sides of efficiency and equipment cost. The
0.70
refrigeration temperature of the propane pre-cooling cycle is set
0.60 as 40 °C. The high pressure in the nitrogen Brayton cycle is set
0.50 as 10 MPa. The system unit power consumption increases along
y

0.40 with increasing nitrogen content, but the increasing rate of unit
power consumption becomes very small when the nitrogen con-
0.30
tent is more than 30%. Optimal values for the liquefaction rate
0.20
and the methane recovery rate are found to reduce power con-
0.10 sumption to a minimum.
0.00 For CBM with high nitrogen content, a high methane recovery
0 10 20 30 40 50 60 rate can be achieved at a reasonably low liquefaction rate, avoiding
N2 [mol%] large energy consumption at a high liquefaction rate. For example,
when the nitrogen content is 50%, only 60% of the liquefaction rate
Fig. 10. Changes in y with respect to N2 % when x = 95%. is needed to reach 95% of methane recovery rate.
It was also found that, the methane content can be improved
significantly after liquefaction, if a lower methane recovery rate
100 is acceptable. The methane content can be improved from 80% to
90
greater than 90% at a liquefaction rate of 85%, and from 70% to al-
most 90% at a liquefaction rate of 75%.
80

70 Acknowledgment
CH4 [mol%]

60
NG The authors are grateful to the support of China’s National High
50
Technology Research and Development Program (863 Program)
LNG/y=95%
40 (No. 2006AA06Z234).
LNG/y=85%
30
LNG/y=75% References
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