ZIF-8浆液法分离CH4/N2的双吸收-吸附塔工艺流程建模与模拟

doi:10.11949/0438-1157.20221488

摘要/Abstract

摘要：

由于ZIF-8浆液独特的可流动性，可以借鉴传统的吸收-解吸工艺，实现煤层气中甲烷的多级连续高效富集。在单吸收-吸附塔工艺的基础上，为了进一步降低能耗，提出了高低压双吸收-吸附塔新型分离工艺，并对该工艺进行了全流程建模及模拟。采用平衡级法，建立了工艺流程中各单元传质设备的数学模型，包括吸收-吸附塔、闪蒸罐、解吸塔。此外，还进行了灵敏度分析，探究了平衡级数、进料位置、气液比、解吸压力等因素对产品气中甲烷浓度以及回收率等工艺性能的影响。模拟结果表明，当产品气中甲烷浓度达到90.13%（mol）时，回收率为90.25%。并且单位原料气能耗为0.445 kW·h∙m^-3（原料气），低于单塔能耗（0.510 kW·h∙m^-3）。由此，改进的双塔工艺在满足甲烷纯度和回收率的同时，相较于单塔工艺进一步降低了能耗。

关键词: ZIF-8, 煤层气, 甲烷, 氮气, 吸附

Abstract:

Due to the unique flowability of ZIF-8 slurry, the traditional absorption-desorption process can be used for reference to realize the multi-stage continuous high-efficiency enrichment of methane in coalbed methane. In this paper, based on the single absorption-adsorption column process, a new process with two absorption-adsorption columns operated at high and low pressures is proposed aiming to reduce the energy consumption. The whole process modeling and simulation of the process was conducted. Using the equilibrium stage method, the mathematical model of each mass transfer unit in the process was established, including absorption-adsorption column, flash tank, and desorption column. Moreover, sensitivity analysis was carried out to explore the effects of equilibrium stages, feed stage, gas-slurry ratio, and desorption pressure on process performance, such as methane concentration in product gas and recovery ratio. The simulation results show that the recovery rate is 90.25% when the methane concentration reaches 90.13%(mol). In addition, the energy consumption per unit feed is 0.445 kW·h·m^-3 (feed gas), which is lower than the energy consumption of the process with a single column (0.510 kW·h·m^-3). The results show that compared with the single-column process, the improved double-column process can further reduce energy consumption while fulfilling the requirements of methane purity and recovery ratio.

Key words: ZIF-8, coalbed methane, methane, nitrogen, adsorption

中图分类号:

TQ 028.8

彭晓婉, 郭笑楠, 邓春, 刘蓓, 孙长宇, 陈光进. ZIF-8浆液法分离CH₄/N₂的双吸收-吸附塔工艺流程建模与模拟[J]. 化工学报, 2023, 74(2): 784-795.

Xiaowan PENG, Xiaonan GUO, Chun DENG, Bei LIU, Changyu SUN, Guangjin CHEN. Modeling and simulation of CH₄/N₂ separation process with two absorption-adsorption columns using ZIF-8 slurry[J]. CIESC Journal, 2023, 74(2): 784-795.

图/表 12

图1 ZIF-8浆液吸收-吸附分离CH4/N2的双塔工艺流程图C101、C102—吸收-吸附塔；D101—闪蒸罐；C103—解吸塔;K101、K102—气体压缩机；P101、P102—循环泵；P103—真空泵；T101、T102—透平；V101、V102、V103—阀；E101, E102, E103—换热器

Fig.1 Schematic diagram of twin columns of ZIF-8 slurry absorption-adsorption separation of CH4/N2 C101, C102—absorption-adsorption column; D101—flash tank; C103—desorber; K101, K102—gas compressor; P101, P102—circulation slurry pump; P103—vacuum pump; T101、T102—turbine; V101, V102, V103—valve; E101, E102, E103—heat exchanger

图2 吸收-吸附塔平衡级数对解吸塔塔顶气相中甲烷摩尔分数和甲烷回收率的影响

Fig.2 Effect of equilibrium stage numbers of absorption-adsorption column on methane mole fraction in the product gas stream and the methane recovery ratio

表1 吸收-吸附塔C102取不同气液比的模拟计算结果

Table 1 Simulation results of different gas-slurry ratios of C102

气液比	吸收-吸附塔塔顶气相流量（C102）/(kmol∙h^-1)	吸收-吸附塔塔顶气相中甲烷摩尔分数（C102）/%	产品气流量/ （kmol∙h^-1）	产品气中甲烷摩尔分数/%	甲烷回收率/%
12	0.4080	3.520	0.3117	87.66	91.08
14	0.4190	3.974	0.3004	90.13	90.25
16	0.4279	4.511	0.2914	91.98	89.34

表2 吸收-吸附塔C101取不同气液比的模拟计算结果

Table 2 Simulation results of different gas-slurry ratios of C101

气液比	吸收-吸附塔塔顶气相流量（C101）/(kmol∙h^-1)	吸收-吸附塔塔顶气相中甲烷摩尔分数（C101）/%	产品气流量/ (kmol∙h^-1)	产品气中甲烷摩尔分数/%	甲烷回收率/%
17	0.1706	3.409	0.3075	88.10	90.30
20	0.2806	4.486	0.3004	90.13	90.25
23	0.3624	5.867	0.2917	91.19	88.67

表3 不同解吸压力下的模拟计算结果

Table 3 Simulation results under different desorption pressures

内蒸

压力/MPa

吸收-吸附塔（C101）塔顶LV₁中甲烷

吸附量/

(mol∙L^-1)

吸收-吸附塔（C102）塔顶 $L V N 1 + 1$ 中甲烷

吸附量/

(mol∙L^-1)

贫液 $L V N 2 + 2$ 中甲烷

吸附量/(mol∙L^-1)

贫液 $L V N 2 + 2$ 中气体

流量/

(kmol∙h^-1)

贫液 $L V N 2 + 2$ 中甲烷

摩尔

分数/%

浆液

L V N 2 + 1

中甲烷摩尔分数/%

吸收-

吸附塔（C101）

塔顶气流流量/(kmol∙h^-1)

吸收-

吸附塔（C101）

塔顶气流中甲烷摩尔分数/%

吸收-

吸附塔（C102）

塔顶气流流量/(kmol∙h^-1)

吸收-

吸附塔（C102）塔顶气流中甲烷摩尔分数/%

产品气流量/(kmol∙h^-1)

产品气中甲烷摩尔

分数/%

甲烷

回收率/

表3 不同解吸压力下的模拟计算结果

Table 3 Simulation results under different desorption pressures

内蒸

压力/MPa

吸收-吸附塔（C101）塔顶LV₁中甲烷

吸附量/

(mol∙L^-1)

吸收-吸附塔（C102）塔顶 $L V N 1 + 1$ 中甲烷

吸附量/

(mol∙L^-1)

贫液 $L V N 2 + 2$ 中甲烷

吸附量/(mol∙L^-1)

贫液 $L V N 2 + 2$ 中气体

流量/

(kmol∙h^-1)

贫液 $L V N 2 + 2$ 中甲烷

摩尔

分数/%

浆液

L V N 2 + 1

中甲烷摩尔分数/%

吸收-

吸附塔（C101）

塔顶气流流量/(kmol∙h^-1)

吸收-

吸附塔（C101）

塔顶气流中甲烷摩尔分数/%

吸收-

吸附塔（C102）

塔顶气流流量/(kmol∙h^-1)

吸收-

吸附塔（C102）塔顶气流中甲烷摩尔分数/%

产品气流量/(kmol∙h^-1)

产品气中甲烷摩尔

分数/%

甲烷

回收率/

0.01

0.0459

0.0326

0.0100

0.0279

97.56

90.76

0.2806

4.486

0.4190

3.973

0.3004

90.13

90.25

0.03

0.0808

0.0686

0.0303

0.0842

97.95

93.13

0.2986

7.618

0.4368

7.980

0.2646

91.59

80.78

0.05

0.1148

0.1032

0.0513

0.1417

98.43

95.34

0.3168

10.48

0.4536

11.52

0.2296

93.43

71.51

图3 净吸附量在平衡级上的分布

Fig.3 Distribution of the net adsorption amounts along with the equilibrium stages

图4 气相和浆液相中的气体流量在平衡级上的分布

Fig.4 Distribution of the gas flow rates in gas and slurry phase (dry basis) along with the equilibrium stages

图5 各平衡级气、液相干基甲烷质量分数实验值与模拟值

Fig.5 Calculated and experimental values of dry methane mole fraction in gas and slurry phases at each equilibrium stages

表4 能耗计算结果汇总

Table 4 Summary of energy consumption calculation results

项目		入口压力/MPa	出口压力/MPa	流量	有效功率/kW	电功率/kW
合计						9.9786
压缩机	原料气	0.12	2	1 kmol·h^-1	2.3827	3.5299
	闪蒸循环气	0.15	1.5	1.5191 kmol·h^-1	2.6058	3.8604
	产品气	0.01	0.11	0.3004 kmol·h^-1	0.5418	0.8027
压缩机电功率合计						8.1930
浆液循环泵P101		0.01	2	1.12 m³·h^-1	0.8258	0.9176
浆液循环泵P102		0.01	1.5	1.60 m³·h^-1	0.8834	0.9815
泵电功率合计						1.8991
氮气透平T101		2	0.1	0.281 kmol·h^-1	-0.4559	-0.3077
氮气透平T102		1.5	0.1	0.419 kmol·h^-1	-0.6246	-0.4216
透平回收膨胀功合计						-0.7293
		入口温度/K	出口温度/K	流量	热负荷/kW	折合电功率/kW
冷却器	原料气	323.15	273.15	1 kmol·h^-1	0.4320	0.2160
	闪蒸循环气	323.15	273.15	1.5191 kmol·h^-1	0.7108	0.3554
	产品气	323.15	293.15	0.3004 kmol·h^-1	0.0888	0.0444
冷却器折合电功率合计						0.6158

图6 设备的能耗对比

Fig.6 Comparison of energy consumption for different units

表5 不同工艺流程下模拟计算结果对比

Table 5 Comparison of simulation results under different processes

项目		单吸收-吸附塔工艺	双吸收-吸附塔工艺（C101/C102）
吸收-吸附塔操作条件	平衡级数	13	7/13
	进料级	11	7/11
	全塔温度/K	273.15	273.15/273.15
	压力/MPa	2	2/1.5
闪蒸罐操作条件	温度/K	273.15	273.15
闪蒸罐操作条件	压力/MPa	0.15	0.15
解吸塔操作条件	温度/K	273.15	273.15
解吸塔操作条件	压力/MPa	0.01	0.01
原料气流量/(kmol∙h^-1)		1	1
原料气中甲烷的摩尔分数/%		30	30
循环浆液量/(m³·h^-1)		2.24	2.72
产品气摩尔分数/%		95.46	90.13
甲烷回收率/%		90.74	90.25

表6 不同工艺流程下能耗计算结果对比

Table 6 Comparison of energy consumption under different processes

项目		单吸收-吸附塔工艺	双吸收-吸附塔工艺（C101/C102）
压缩机/kW	原料气	3.5299	3.5299
	闪蒸循环气	5.3728	3.8604
	产品气	0.7621	0.8027
浆液循环泵合计/kW		1.8353	1.8991
冷却器/kW	原料气	0.2160	0.2160
	闪蒸循环气	0.4412	0.3554
	产品气	0.0418	0.0444
氮气回收合计/kW		-0.7840	-0.7293
合计/kW		11.4151	9.9786
单位原料气能耗/(kW·h∙m^-3)		0.510	0.445

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ZIF-8浆液法分离CH₄/N₂的双吸收-吸附塔工艺流程建模与模拟

Modeling and simulation of CH₄/N₂ separation process with two absorption-adsorption columns using ZIF-8 slurry

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