基于二级双回流的变压吸附捕碳工艺研究

doi:10.11949/0438-1157.20240608

摘要/Abstract

摘要：

碳捕获、利用与封存是应对全球气候变化的关键技术，而火电厂烟气是工业碳排放主要来源之一。变压吸附是常用的烟气捕碳工艺之一，已有的研究表明常规真空变压吸附难以获得满足指标的二氧化碳产品，双回流变压吸附可获得两种高纯度和回收率的产品，但生产能力较低。对此，基于文献数据对组成为N₂/CO₂=85%/15%的烟气进行了二级耦合工艺的模拟，探究了进料位置，吸附时长，空塔气速和轻、重回流量对工艺的影响。结果表明，吸附压力为一级200 kPa，二级105 kPa，解吸压力为一级30 kPa，二级2 kPa，进料位置距塔底与塔高比0.4，吸附时长90 s，空塔气速0.07 m/s，轻回流量5.5×10^-3 mol/s，重回流量1.1×10^-2 mol/s时，能得到96.42%的CO₂和99.93%的N₂，回收率96.22%和99.47%。此外，与文献对比，提出的二级工艺具有高生产能力和较低能耗。

关键词: 双回流, 变压吸附, 二氧化碳捕集, 硅胶, 烟道气, 数值模拟

Abstract:

Carbon capture, utilization, and storage technology is a key technology for addressing global climate change, and flue gas from thermal power plants is one of the main sources of industrial carbon emissions. The pressure swing adsorption process is one of the commonly used flue gas carbon capture processes. Existing studies have shown that conventional vacuum pressure swing adsorption is difficult to obtain carbon dioxide products that meet the indicators. Double reflux pressure swing adsorption can obtain two products with high purity and recovery rate, but the production capacity is low. For this purpose, using silica gel as the adsorbent, a simulation study was conducted on a two-stage process coupling the dual reflux pressure adsorption process and conventional vacuum pressure swing adsorption process for flue gas with a feed composition of N₂/CO₂=85%/15% based on literature data. The effects of feed position, adsorption time, gas velocity, light component reflux rate, and heavy component reflux rate on performance were explored. The results showed that when the adsorption pressure was 200 kPa for the first stage and 105 kPa for the second stage, the desorption pressure was 30 kPa for the first stage and 2 kPa for the second stage, the feed position was 0.4 times higher than the bottom, the adsorption time was 90 s, the gas velocity was 0.07 m/s, the reflux flow rate of light components is 5.5×10^-3 mol/s and the reflux flow rate of heavy components is 1.1×10^-2 mol/s, 96.42% CO₂ and 99.93% N₂ can be obtained, with recovery rates of 96.22% and 99.47%, respectively. In addition, compared with existing research results in the literature, the proposed two-stage process has high productivity and low energy consumption.

Key words: dual-reflux, pressure swing adsorption, CO₂ capture, silica gel, flue gas, numerical simulation

中图分类号:

TQ 028.1

姚佳逸, 张东辉, 唐忠利, 李文彬. 基于二级双回流的变压吸附捕碳工艺研究[J]. 化工学报, 2025, 76(2): 744-754.

Jiayi YAO, Donghui ZHANG, Zhongli TANG, Wenbin LI. Research on carbon capture by pressure swing adsorption based on two-stage dual reflux[J]. CIESC Journal, 2025, 76(2): 744-754.

图/表 19

表1 二级双回流变压吸附时序

Table 1 The schedule of the two-stage dual-reflux PSA process

工艺		时间/s
工艺		90	10	45	90	10	45
一级	bed 1	AD	ED	VU	PU	ER	PR
一级	bed 2	PU	ER	PR	AD	ED	VU
二级	bed 3	AD	ED	VU	VU	ER	PR
二级	bed 4	VU	ER	PR	AD	ED	VU

图1 二级双回流变压吸附流程图

Fig.1 The diagram of the two-stage dual-reflux PSA process

表2 CO2、N2在硅胶上的扩展型Langmuir 2拟合参数［25］

Table 2 Fitting parameters of extended Langmuir 2 model for CO2/N2 adsorption on silica gel［25］

参数	N₂	CO₂
IP₁/(kmol/(kg·kPa))	6.77×10^-10	6.07×10^-9
IP₂/K	2034.0	2435.0
IP₃/kPa^-1	2.01×10^-7	1.32×10^-6
IP₄/K	2034.0	2034.0
ΔH/(kJ/mol)	-17.08	-23.14

表3 吸附塔及吸附剂相关参数

Table 3 Parameters for column and adsorbent

参数	数值
H_b1/m	1.00
H_b2/m	0.52
D_b1/m	0.060
D_b2/m	0.025
W_t/m	0.002
r_p/m	0.002
ρ_b/(kg/m³)	785
k_w/(W/(m·K))	17
k_s/(W/(m·K))	0.3
k_g/(W/(m·K))	0.242
c_p_w/(kJ/(kg·K))	0.502
c_p_s/(kJ/(kg·K))	0.902
h_amb/(W/(m²·K))	60
ε_b	0.3125
ε_p	0.1429
ρ_w/(kg/m³)	7800
T_amb/K	298.15

表4 二级双回流变压吸附数学模型

Table 4 Mathematical models of the two-stage dual-reflux PSA process

模型方程		数学表达
质量平衡		$- ε_{b} D_{a x, i} \frac{\partial^{2} c_{i}}{\partial z^{2}} + \frac{\partial (v_{g} c_{i})}{\partial z} + [ε_{b} + (1 - ε_{b}) ε_{p}] \frac{\partial c_{i}}{\partial t} + ρ_{s} (1 - ε_{b}) \frac{\partial q_{i}}{\partial t} = 0$ $D_{a x, i} = 0.73 D_{m, i} + \frac{v_{g} r_{p}}{ε_{b} (1 + 9.49 \frac{ε_{b} D_{m, i}}{2 v_{g} r_{p}})}$	(1) (2)
能量平衡	气相	$- k_{g} \frac{\partial^{2} T_{g}}{\partial z^{2}} + c_{v g} v_{g} ρ_{g} \frac{\partial T_{g}}{\partial z} + ε_{b} c_{v g} ρ_{g} \frac{\partial T_{g}}{\partial t} + P \frac{\partial v_{g}}{\partial z} + h_{f} (T_{g} - T_{s}) + \frac{4 h_{w}}{D_{b}} (T_{g} - T_{0}) = 0$	(3)
	固相	$- k_{s} \frac{\partial^{2} T_{s}}{\partial z^{2}} + c_{p s} ρ_{s} \frac{\partial T_{s}}{\partial t} + ρ_{s} \sum_{i = 1}^{n} (c_{p a, i} q_{i}) \frac{\partial T_{s}}{\partial t} + ρ_{s} \sum_{i = 1}^{n} (Δ H_{i} \frac{\partial q_{i}}{\partial t}) - h_{f} (T_{g} - T_{s}) = 0$	(4)
	塔壁	$k_{w} \frac{\partial^{2} T_{w}}{\partial z^{2}} + c_{p w} ρ_{w} \frac{\partial T_{w}}{\partial z} - h_{w} \frac{4 D_{b}}{(D_{b} + W_{t})^{2} - D_{b}^{2}} (T_{g} - T_{w}) + h_{a m b} \frac{4 (D_{b} + W_{t})^{2}}{(D_{b} + W_{t})^{2} - D_{b}^{2}} (T_{w} - T_{a m b}) = 0$	(5)
动量平衡		$- \frac{\partial P}{\partial z} = \frac{150 μ (1 - ε_{b})^{2}}{ε_{b}^{3} (2 r_{p} {ψ)}^{2}} + 1.75 M \frac{(1 - ε_{b}) ρ_{g}}{2 r_{p} ψ ε_{b}^{3}} \|v_{g}\| v_{g}$	(6)
吸附平衡		$q_{i}^{*} = \frac{q_{m, i} b_{i} P_{i}}{1 + \sum_{i = 1}^{n} b_{i} P_{i}}$ ， $b_{i} = b_{0 i} e x p (- Δ H_{i} / R_{g} T)$ ， $- Δ H_{i} = R_{g} T {(\frac{\partial l n P_{i}}{\partial T})}_{q}$	(7)
吸附速率		$\frac{\partial q_{i}}{\partial t} = k_{L D F, i} (q_{i}^{} - q_{i}) = \frac{15 D_{e, i}}{r_{p}^{2}} (q_{i}^{} - q_{i})$ ， $D_{e, i} = \frac{ε_{p}}{τ} \times \frac{D_{k, i} D_{m, i}}{D_{k, i} + D_{m, i}}$ ， $D_{k, i} = 97.0 r_{p} \sqrt[]{(\frac{T}{M_{i}})}$	(8)
纯度		$Y_{i} = \frac{\int_{0}^{t_{c y c l e}} F_{o u t} y_{o u t, i} d t}{\int_{0}^{t_{c y c l e}} F_{o u t} d t}$	(9)
回收率		$R_{i} = \frac{\int_{0}^{t_{c y c l e}} F_{o u t} y_{o u t, i} d t}{\int_{0}^{t_{c y c l e}} F_{i n} {y_{i n}}_{, i} d t}$	(10)
生产能力		$p_{C O_{2}} = 3600 \frac{\int_{0}^{t_{c y c l e}} F_{o u t} y_{o u t, C O_{2}} d t}{t_{c y c l e} m_{a d s o r b e n t s}}$	(11)
电耗		$W = \frac{\int_{0}^{t_{c y c l e}} \frac{V_{i n} P_{o u t} γ}{η (γ + 1)} [{(P_{o u t} / P_{i n})}^{1 - (1 / γ)} - 1] d t}{\int_{0}^{t_{c y c l e}} V_{p r o d u c t} y_{p r o d u c t} d t}$	(12)
阀门		$F = C_{V} (P_{i n} - P_{o u t})$	(13)

表4 二级双回流变压吸附数学模型

Table 4 Mathematical models of the two-stage dual-reflux PSA process

模型方程		数学表达
质量平衡		$- ε_{b} D_{a x, i} \frac{\partial^{2} c_{i}}{\partial z^{2}} + \frac{\partial (v_{g} c_{i})}{\partial z} + [ε_{b} + (1 - ε_{b}) ε_{p}] \frac{\partial c_{i}}{\partial t} + ρ_{s} (1 - ε_{b}) \frac{\partial q_{i}}{\partial t} = 0$ $D_{a x, i} = 0.73 D_{m, i} + \frac{v_{g} r_{p}}{ε_{b} (1 + 9.49 \frac{ε_{b} D_{m, i}}{2 v_{g} r_{p}})}$	(1) (2)
能量平衡	气相	$- k_{g} \frac{\partial^{2} T_{g}}{\partial z^{2}} + c_{v g} v_{g} ρ_{g} \frac{\partial T_{g}}{\partial z} + ε_{b} c_{v g} ρ_{g} \frac{\partial T_{g}}{\partial t} + P \frac{\partial v_{g}}{\partial z} + h_{f} (T_{g} - T_{s}) + \frac{4 h_{w}}{D_{b}} (T_{g} - T_{0}) = 0$	(3)
	固相	$- k_{s} \frac{\partial^{2} T_{s}}{\partial z^{2}} + c_{p s} ρ_{s} \frac{\partial T_{s}}{\partial t} + ρ_{s} \sum_{i = 1}^{n} (c_{p a, i} q_{i}) \frac{\partial T_{s}}{\partial t} + ρ_{s} \sum_{i = 1}^{n} (Δ H_{i} \frac{\partial q_{i}}{\partial t}) - h_{f} (T_{g} - T_{s}) = 0$	(4)
	塔壁	$k_{w} \frac{\partial^{2} T_{w}}{\partial z^{2}} + c_{p w} ρ_{w} \frac{\partial T_{w}}{\partial z} - h_{w} \frac{4 D_{b}}{(D_{b} + W_{t})^{2} - D_{b}^{2}} (T_{g} - T_{w}) + h_{a m b} \frac{4 (D_{b} + W_{t})^{2}}{(D_{b} + W_{t})^{2} - D_{b}^{2}} (T_{w} - T_{a m b}) = 0$	(5)
动量平衡		$- \frac{\partial P}{\partial z} = \frac{150 μ (1 - ε_{b})^{2}}{ε_{b}^{3} (2 r_{p} {ψ)}^{2}} + 1.75 M \frac{(1 - ε_{b}) ρ_{g}}{2 r_{p} ψ ε_{b}^{3}} \|v_{g}\| v_{g}$	(6)
吸附平衡		$q_{i}^{*} = \frac{q_{m, i} b_{i} P_{i}}{1 + \sum_{i = 1}^{n} b_{i} P_{i}}$ ， $b_{i} = b_{0 i} e x p (- Δ H_{i} / R_{g} T)$ ， $- Δ H_{i} = R_{g} T {(\frac{\partial l n P_{i}}{\partial T})}_{q}$	(7)
吸附速率		$\frac{\partial q_{i}}{\partial t} = k_{L D F, i} (q_{i}^{} - q_{i}) = \frac{15 D_{e, i}}{r_{p}^{2}} (q_{i}^{} - q_{i})$ ， $D_{e, i} = \frac{ε_{p}}{τ} \times \frac{D_{k, i} D_{m, i}}{D_{k, i} + D_{m, i}}$ ， $D_{k, i} = 97.0 r_{p} \sqrt[]{(\frac{T}{M_{i}})}$	(8)
纯度		$Y_{i} = \frac{\int_{0}^{t_{c y c l e}} F_{o u t} y_{o u t, i} d t}{\int_{0}^{t_{c y c l e}} F_{o u t} d t}$	(9)
回收率		$R_{i} = \frac{\int_{0}^{t_{c y c l e}} F_{o u t} y_{o u t, i} d t}{\int_{0}^{t_{c y c l e}} F_{i n} {y_{i n}}_{, i} d t}$	(10)
生产能力		$p_{C O_{2}} = 3600 \frac{\int_{0}^{t_{c y c l e}} F_{o u t} y_{o u t, C O_{2}} d t}{t_{c y c l e} m_{a d s o r b e n t s}}$	(11)
电耗		$W = \frac{\int_{0}^{t_{c y c l e}} \frac{V_{i n} P_{o u t} γ}{η (γ + 1)} [{(P_{o u t} / P_{i n})}^{1 - (1 / γ)} - 1] d t}{\int_{0}^{t_{c y c l e}} V_{p r o d u c t} y_{p r o d u c t} d t}$	(12)
阀门		$F = C_{V} (P_{i n} - P_{o u t})$	(13)

图2 单周期内一级吸附塔压力变化

Fig.2 Pressure curves of the first stage for one cycle

图3 单周期内二级吸附塔压力变化

Fig.3 Pressure curves of the second stage for one cycle

图4 一级吸附塔内温度随时间和轴向距离分布曲线

Fig.4 Temperature distribution curves of the first stage with time and axial distance

图5 二级吸附塔内温度随时间和轴向距离分布曲线

Fig.5 Temperature distribution curves of the second stage with time and axial distance

图6 一级CO2气相浓度分布

Fig.6 Concentration distribution of CO2 on gas phase of the first stage

图7 二级CO2气相浓度分布

Fig.7 Concentration distribution of CO2 on gas phase of the second stage

图8 一级CO2固相浓度分布

Fig.8 Concentration distribution of CO2 on solid phase of the first stage

图9 二级CO2固相浓度分布

Fig.9 Concentration distribution of CO2 on solid phase of the second stage

图10 进料位置对CO2、N2纯度和回收率的影响

Fig.10 Effect of feed position on purity and recovery of CO2 and N2

图11 吸附时间对CO2、N2纯度和回收率的影响

Fig.11 Effect of adsorption time on purity and recovery of CO2 and N2

图12 气体流速对CO2、N2纯度和回收率影响

Fig.12 Effect of gas velocity on purity and recovery of CO2 and N2

图13 轻组分回流量对CO2、N2纯度和回收率影响

Fig.13 Effect of light component reflux flow on purity and recovery of CO2 and N2

图14 重组分回流量对CO2、N2纯度和回收率影响

Fig.14 Effect of heavy component reflux flow on purity and recovery of CO2 and N2

表5 不同PSA捕碳工艺对比

Table 5 Comparison of different PSA processes for carbon capture

工艺	CO₂纯度/%	CO₂回收率/%	N₂纯度/%	N₂回收率/%	生产能力/( $m o l_{C O_{2}}$ /(h·kg_吸附剂))	能耗/（ $G J / t_{C O_{2}}$ ）
二级DR-PSA	96.42	96.22	99.93	99.47	1.05	1.69
二床六步DR-PSA^[25]	95.6	96.8	>98	>98	0.32	2.5
二床六步DR-PSA^[29]	95.55	96.81	—	—	0.89	2.5
三床七步VPSA^[30]	80.94	90.61	—	—	0.52	1.0

表5 不同PSA捕碳工艺对比

Table 5 Comparison of different PSA processes for carbon capture

工艺	CO₂纯度/%	CO₂回收率/%	N₂纯度/%	N₂回收率/%	生产能力/( $m o l_{C O_{2}}$ /(h·kg_吸附剂))	能耗/（ $G J / t_{C O_{2}}$ ）
二级DR-PSA	96.42	96.22	99.93	99.47	1.05	1.69
二床六步DR-PSA^[25]	95.6	96.8	>98	>98	0.32	2.5
二床六步DR-PSA^[29]	95.55	96.81	—	—	0.89	2.5
三床七步VPSA^[30]	80.94	90.61	—	—	0.52	1.0

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次数	20	74
比例	21%	79%

[1]	张珂, 任维杰, 王梦娜, 范凯锋, 常丽萍, 李佳斌, 马涛, 田晋平. Bunsen反应产物在微通道中的液-液两相混合特性[J]. 化工学报, 2025, 76(2): 623-636.
[2]	何传超, 周静红, 曹约强, 施尧, 周兴贵. Ag/SiO₂催化草酸酯加氢制乙醇酸甲酯的床层-颗粒双尺度耦合模拟研究[J]. 化工学报, 2025, 76(2): 654-666.
[3]	杨晋宁, 王卫凡, 徐冬, 刘毅, 翁小涵, 原野, 王志. 工业烟道气碳捕集膜技术放大研究进展[J]. 化工学报, 2025, 76(2): 504-518.
[4]	李舒月, 王欢, 周少强, 毛志宏, 张永民, 王军武, 吴秀花. 重质颗粒流态化研究现状与展望[J]. 化工学报, 2025, 76(2): 466-483.
[5]	贾晶宇, 孔德齐, 沈圆辉, 张东辉, 李文彬, 唐忠利. 合成氨反应器尾气变压吸附氨分离工艺的模拟与分析[J]. 化工学报, 2025, 76(2): 718-730.
[6]	韩启沃, 刘永峰, 裴普成, 张璐, 姚圣卓. 工作温度对PEMFC水分布、质子传输及性能影响分析[J]. 化工学报, 2025, 76(1): 374-384.
[7]	邓志诚, 杨欢, 王斯民, 王家瑞. 微混燃烧器中微管结构对氢燃料掺混效果与燃烧性能影响[J]. 化工学报, 2025, 76(1): 335-347.
[8]	王瀚彬, 胡帅, 毕丰雷, 李隽森, 贺来宾. 新型波纹翅片金属氢化物反应器的放氢性能有限元分析[J]. 化工学报, 2025, 76(1): 221-230.
[9]	高羡明, 杨汶轩, 卢少辉, 任晓松, 卢方财. 双槽道结构对超疏水表面液滴合并弹跳的影响[J]. 化工学报, 2025, 76(1): 208-220.
[10]	刘萍, 邱雨生, 李世婧, 孙瑞奇, 申晨. 微通道内纳米流体传热流动特性[J]. 化工学报, 2025, 76(1): 184-197.
[11]	韩志敏, 周相宇, 张宏宇, 徐志明. 不同粗糙元结构下CaCO₃污垢局部沉积特性[J]. 化工学报, 2025, 76(1): 151-160.
[12]	董新宇, 边龙飞, 杨怡怡, 张宇轩, 刘璐, 王腾. 冷却条件下倾斜上升管S-CO₂流动与传热特性研究[J]. 化工学报, 2024, 75(S1): 195-205.
[13]	郭骐瑞, 任丽媛, 陈康, 黄翔宇, 马卫华, 肖乐勤, 周伟良. 用于HTPB推进剂浆料的静态混合管数值模拟[J]. 化工学报, 2024, 75(S1): 206-216.
[14]	李匡奚, 于佩潜, 王江云, 魏浩然, 郑志刚, 冯留海. 微气泡旋流气浮装置内流动分析与结构优化[J]. 化工学报, 2024, 75(S1): 223-234.
[15]	汪张洲, 唐天琪, 夏嘉俊, 何玉荣. 基于复合相变材料的电池热管理性能模拟[J]. 化工学报, 2024, 75(S1): 329-338.