ZIF-8浆液中试分离CO2/N2过程模拟及能耗分析

doi:10.11949/0438-1157.20211441

摘要/Abstract

摘要：

ZIF-8/2-甲基咪唑-乙二醇-水浆液(ZIF-8浆液)可以高效低耗能地分离CO₂。为了进一步评估ZIF-8浆液在填料塔中分离CO₂的塔效率及能耗，使用Peng-Robinson(PR)状态方程，求出CO₂和ZIF-8浆液的二元交互作用参数(k_CO2)，将二元交互作用参数和Aspen Plus软件进行关联，对CO₂/N₂多级吸收分离进行过程模拟。计算结果表明在中试填料塔中，ZIF-8浆液仅需要5块理论塔板即可将CO₂浓度由20%(mol)降低至2%(mol)以下，填料塔的塔板效率为25%。对中试分离CO₂/N₂进行能耗计算，结果表明当解吸条件为解吸温度333 K，解吸压力0.8 MPa和空气吹扫流量200 L/h时，CO₂捕集等效功最低可至0.474 GJ/t CO₂。在同样条件下使用ZIF-8浆液和MEA(30%(mass))水溶液进行碳捕集时，CO₂捕集等效功分别为0.507 GJ/t CO₂和0.957 GJ/t CO₂，ZIF-8浆液的CO₂捕集等效功仅为MEA水溶液的53%。

关键词: ZIF-8, 二氧化碳捕集, 填料塔, 过程模拟, 能耗分析

Abstract:

ZIF-8/2-methylimidazole-ethylene glycol-water slurry was used for separating CO₂ from CO₂/N₂ in a pilot-scale packed tower. In order to evaluate the tower efficiency and energy consumption of the packed tower in the CO₂ capture process, firstly, the binary interaction parameters k_CO2 of CO₂ and ZIF-8 slurry were fitted by Peng-Robinson equation of state. Then the binary interaction parameters were related to Aspen Plus to simulate the multi-stage absorption process of CO₂/N₂. The calculation results show that in the pilot-scale packed tower, with only 5 theoretical plates, ZIF-8 slurry could reduce the CO₂ concentration from 20%(mol) to less than 2%(mol), indicating the tray efficiency of the packed tower is 25%. About the energy consumption for the separation of CO₂/N₂ in the pilot plant, the results indicate that when desorption conditions were set at 333 K, 0.8 MPa, and 200 L/h, the CO₂ capture equivalent work can be as low as 0.474 GJ/t CO₂. When ZIF-8 slurry and MEA (30%(mass)) aqueous solution were used for CO₂ capture under the same conditions, the CO₂ capture equivalent work are 0.507 GJ/t CO₂ and 0.957 GJ/t CO₂, respectively. The CO₂ capture equivalent work of ZIF-8 slurry is only 53% of that of MEA aqueous solution.

Key words: ZIF-8, CO₂ capture, packed tower, process simulation, energy consumption analysis

中图分类号:

TQ 015.1

黄子轩, 陈欢, 李海, 王明龙, 陈光进, 刘蓓. ZIF-8浆液中试分离CO₂/N₂过程模拟及能耗分析[J]. 化工学报, 2022, 73(1): 322-331.

Zixuan HUANG, Huan CHEN, Hai LI, Minglong WANG, Guangjin CHEN, Bei LIU. Process simulation and energy consumption analysis of CO₂/N₂ pilot-scale separation using ZIF-8 slurry[J]. CIESC Journal, 2022, 73(1): 322-331.

图/表 17

图1 CO2-浆液的二元相互作用参数(kCO2)回归计算图

Fig.1 Calculation diagram for the regression of CO2-slurry binary interaction parameters

图2 吸收-吸附塔Aspen过程模拟流程图

Fig.2 Aspen simulation flow chart of absorption-adsorption column

图3 ZIF-8浆液脱碳系统能耗评价流程图1—compressor; 2—absorption tower; 3—lean liquid cooler; 4—heat exchanger; 5—metering pump; 6—desorption tower; 7—rich liquid heater; 8—vacuum pump; black—gas flow; blue—rich liquid flow; red—lean liquid flow

Fig.3 The flow chart for CO2 capture equivalent work evaluation of decarbonization system

图4 Wcompr计算模板: Aspen Plus软件中的气体压缩机模块(COMPR)；进入压缩机模块的原料气流(FEED-GAS)；压缩后的混合气流(COMPR-GAS)

Fig.4 Computation module of Wcompr： gas compression module in the Aspen Plus (COMPR); gas stream before compression (FEED-GAS); gas stream after compression (COMP-GAS)

图5 Wmet计算模板: Aspen Plus软件中的计量泵模块(MET-PUMP)；解吸塔底出来的贫液(SLU-IN)；贫液增压至吸收塔操作压力(SLU-OUT)

Fig.5 Computation module of Wmet： metering pump module in the Aspen Plus (MET-PUMP); lean slurry under desorption pressure (SLU-IN); lean slurry under sorption pressure (SLU-OUT)

图6 Wvac计算模板： Aspen Plus软件中的真空泵模块(VACUUM)；常压下气体流体(DE)；解吸压力下的气体流体(NOL)

Fig.6 Computation module of Wvac： vacuum pump module in the Aspen Plus (VACUUM); gas stream under normal pressure (DE); gas stream under desorption pressure (NOL)

图7 Qheat计算模板： Aspen Plus软件中的热交换器模块(HEATX)；AspenPlus软件中的加热器模块(RICH-H)；从解吸塔塔底流入热交换器的贫液(LEAN-IN)；从热交换器流向吸收塔塔顶的贫液(LEAN-OUT)；从吸收塔塔底流向热交换器的富液(RICH-IN)；从热交换器流向加热器模块的富液(RICH-OUT)；从加热器流向解吸塔塔顶的富液(RICH)

Fig.7 Computation module of Qheat: heat exchanger module in the Aspen Plus (HEATX); lean slurry from desorption tower to heat exchanger (LEAN-IN); lean slurry from heat exchanger to sorption tower (LEAN-OUT); rich slurry from the sorption tower to heat exchanger (RICH-IN); rich slurry from heat exchanger to heater (RICH-OUT); rich slurry from heater to desorption tower (RICH)

图8 CO2在新鲜ZIF-8浆液(a)和从中试解吸塔底(解吸温度、解吸压力和空气吹扫流速分别设定为333.15 K、0.08 MPa和200 L/h)获得的ZIF-8浆液(b)中的溶解度曲线(303.15 K)；N2在新鲜ZIF-8浆液中的溶解度曲线(303.15 K)(c)[33]

Fig.8 Sorption isotherms of CO2 at 303.15 K in fresh ZIF-8 slurry (a), the ZIF-8 slurry obtained from the desorption packed tower(desorption condition: the desorption temperature, pressure, and air-purge flow rate were fixed at 333.15 K, 0.08 MPa, and 200 L/h)(b); Sorption isotherm of N2 at 303.15 K in fresh ZIF-8 slurry (c)[33]

表1 CO2和ZIF-8浆液的二元交互作用参数kCO2与温度、压力的函数关系

Table 1 The relationship between temperature， pressure， and the binary interaction parameter kCO2 of CO2 and ZIF-8 slurry

ZIF-8浆液	k_CO2=(mT+n)p+MT+N
ZIF-8浆液	m	n	M	N
新鲜ZIF-8浆液	-0.01148	4.20695	0.00029	-0.54962
从中试解吸塔底获得的ZIF-8浆液^①	-0.01776	5.82127	0.00156	-0.88403

表2 新鲜ZIF-8浆液吸收CO2气体相平衡实验数据与模拟结果

Table 2 Experimental and simulated phase equilibrium data of CO2 absorption by fresh ZIF-8 slurry

T/K	k_CO2	p_E/MPa	x_cal	x_exp	AADx/%
293.15	-0.4596	0.007	0.0067	0.0078	13.40
293.15	-0.4503	0.018	0.0145	0.0137	5.24
293.15	-0.4352	0.036	0.0223	0.0203	9.66
293.15	-0.4032	0.074	0.0281	0.0265	6.15
303.15	-0.4575	0.007	0.0046	0.0054	13.52
303.15	-0.4495	0.018	0.0104	0.0103	0.55
303.15	-0.4292	0.046	0.0191	0.0179	6.82
303.15	-0.4045	0.08	0.0233	0.0230	1.30
303.15	-0.3870	0.104	0.0237	0.0262	9.40
313.15	-0.4530	0.011	0.0050	0.0050	1.15
313.15	-0.4444	0.025	0.0098	0.0098	0.18
313.15	-0.4334	0.043	0.0143	0.0144	0.75
313.15	-0.4114	0.079	0.0193	0.0187	3.01
313.15	-0.3906	0.113	0.0209	0.0215	3.03
总AADx					5.30

表3 从中试解吸塔底获得的ZIF-8浆液吸收CO2气体相平衡实验数据与模拟结果

Table 3 Experimental and simulated phase equilibrium data of CO2 absorption by ZIF-8 slurry obtained from the desorption packed tower

T/K	k_CO2	p_E/MPa	x_cal	x_exp	AADx/%
293.15	-0.4224	0.007	0.0039	0.0044	12.75
293.15	-0.4113	0.025	0.0113	0.0096	17.46
293.15	-0.3990	0.045	0.0166	0.0154	8.32
293.15	-0.3751	0.084	0.0215	0.0207	3.65
293.15	-0.3615	0.106	0.0222	0.0227	2.38
303.15	-0.4067	0.01	0.0032	0.0035	7.90
303.15	-0.3997	0.026	0.0074	0.0072	1.95
303.15	-0.3932	0.041	0.0105	0.0112	5.88
303.15	-0.3809	0.069	0.0147	0.0157	6.37
303.15	-0.3648	0.106	0.0179	0.0190	5.77
313.15	-0.3911	0.017	0.0033	0.0033	1.10
313.15	-0.3875	0.031	0.0057	0.0054	4.66
313.15	-0.3838	0.045	0.0078	0.0076	2.91
313.15	-0.3797	0.061	0.0099	0.0098	1.65
313.15	-0.3724	0.089	0.0131	0.0127	3.19
313.15	-0.3690	0.102	0.0143	0.0141	1.56
总AADx					5.47

图9 不同温度下ZIF-8浆液的CO2溶解度曲线

Fig.9 Sorption isotherms of CO2 at different temperatures

图10 ZIF-8浆液的解吸热：新鲜ZIF-8浆液(a)；从中试解吸塔底获得的ZIF-8浆液(解吸温度333.15 K、解吸压力0.08 MPa、空气吹扫流速200 L/h)(b)

Fig.10 Sorption heat of ZIF-8 slurry in fresh ZIF-8 slurry (a) and the ZIF-8 slurry obtained from the desorption packed tower (the desorption temperature, pressure, and air-purge flow rate were fixed at 333.15 K, 0.08 MPa, and 200 L/h) (b)

表4 新鲜ZIF-8浆液多级吸收CO2的过程模拟结果

Table 4 The simulation results of multi-stage CO2 absorption by fresh ZIF-8 slurry

理论塔板级数	气相中CO₂浓度，y/%	液相中CO₂浓度，x/%	气相中CO₂分压，p/MPa	平衡级温度，T/K	CO₂-浆液二元交互作用参数，k_CO2
塔顶(净化气/贫液)	0	0	0	303.15	-0.4626
2	0.0001	0	0	303.15	-0.4626
3	0.0005	0	0	303.15	-0.4626
4	0.0034	0.0002	0	303.15	-0.4626
5	0.0235	0.0015	0.0001	303.16	-0.4625
6	0.1612	0.0105	0.001	303.22	-0.4619
7	1.078	0.0706	0.0065	303.6	-0.4578
8	6.2328	0.4297	0.0374	305.9	-0.4358
塔底(原料气/富液)	20	1.5859	0.12	313.3	-0.3865

表5 中试解吸后的ZIF-8浆液多级吸收CO2的过程模拟结果

Table 5 The simulation results of multi-stage CO2 absorption by ZIF-8 slurry obtained from the desorption packed tower

理论塔板级数	气相中CO₂浓度，y/%	液相中CO₂浓度，x/%	气相中CO₂分压，p/MPa	平衡级温度，T/K	CO₂-浆液二元交互作用参数，k_CO2
塔顶(净化气/贫液)	0.0429	0	0.0003	303.15	-0.411
2	0.1794	0.0089	0.0011	303.2	-0.4106
3	0.6083	0.0369	0.0036	303.38	-0.4092
4	1.894	0.1223	0.0114	303.93	-0.4051
5	5.2582	0.3561	0.0315	305.42	-0.395
6	11.503	0.8351	0.069	308.49	-0.3791
7	17.4369	1.3552	0.1046	311.81	-0.3679
8	19.5741	1.5612	0.1174	313.13	-0.365
塔底(原料气/富液)	20	1.5832	0.12	313.27	-0.3644

表6 ZIF-8浆液在中试填料塔中运行时不同操作条件对CO2捕集等效功的影响

Table 6 Effect of different operating conditions of ZIF-8 slurry on the CO2 capture equivalent work in the packed tower

Test No.	T_de/K	p_de/MPa	V_de-air/(L/h)	p_ab/MPa	V_in-mixgas/(L/h)	φ	C_out-CO2/% (mol)	ΔS_V/(mol/L)	η_CO2/%	w_total/(GJ/t CO₂)
S₁	298	0.08	200	0.6	300	18	3.07	0.12	84.6	0.680
S₂	298	0.08	600	0.6	720	42	5.82	0.26	69.1	0.609
S₃	313	0.08	600	0.6	720	42	3.08	0.32	84.1	0.649
S₄	333	0.08	200	0.6	720	90	1.42	0.75	93.0	0.507
S₅	333	0.08	200	0.6	720	80	0.92	0.68	95.0	0.509
S₆	333	0.08	200	0.5	720	80	2.02	0.64	89.9	0.474
S_MEA	333	0.08	200	0.6	720	90	3.39	0.66	82.5	0.957

表7 不同操作条件下CO2捕集等效功的构成

Table 7 The composition of CO2 capture equivalent work in different operating conditions

Test No.	w_compr/(GJ/t CO₂)	w_heat/(GJ/t CO₂)	w_pump/(GJ/t CO₂)	w_total/(GJ/t CO₂)
S₁	0.477	0.000	0.203	0.680
S₂	0.478	0.000	0.131	0.609
S₃	0.412	0.119	0.117	0.649
S₄	0.382	0.081	0.045	0.507
S₅	0.374	0.084	0.051	0.509
S₆	0.343	0.086	0.045	0.474
S_MEA	0.418	0.177	0.052	0.957

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ZIF-8浆液中试分离CO₂/N₂过程模拟及能耗分析

Process simulation and energy consumption analysis of CO₂/N₂ pilot-scale separation using ZIF-8 slurry

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