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Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

CN 11-5981/TQ

邮发代号 80-969

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Frontiers of Chemical Science and Engineering  2020, Vol. 14 Issue (2): 233-247   https://doi.org/10.1007/s11705-019-1893-1
  本期目录
Optimization of electrochemically synthesized Cu3(BTC)2 by Taguchi method for CO2/N2 separation and data validation through artificial neural network modeling
Kasra Pirzadeh, Ali Asghar Ghoreyshi(), Mostafa Rahimnejad, Maedeh Mohammadi
Chemical Engineering Department, Babol Noshirvani University of Technology, Babol, Iran
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Abstract：

Cu3(BTC)2, a common type of metal organic framework (MOF), was synthesized through electrochemical route for CO2 capture and its separation from N2. Taguchi method was employed for optimization of key parameters affecting the synthesis of Cu3(BTC)2. The results indicated that the optimum synthesis conditions with the highest CO2 selectivity can be obtained using 1 g of ligand, applied voltage of 25 V, synthesis time of 2 h, and electrode length of 3 cm. The single gas sorption capacity of the synthetized microstructure Cu3(BTC)2 for CO2 (at 298 K and 1 bar) was a considerable value of 4.40 mmol·g−1. The isosteric heat of adsorption of both gases was calculated by inserting temperature-dependent form of Langmuir isotherm model in the Clausius-Clapeyron equation. The adsorption of CO2/N2 binary mixture with a concentration ratio of 15/85 vol-% was also studied experimentally and the result was in a good agreement with the predicted value of IAST method. Moreover, Cu3(BTC)2 showed no considerable loss in CO2 adsorption after six sequential cycles. In addition, artificial neural networks (ANNs) were also applied to predict the separation behavior of CO2/N2 mixture by MOFs and the results revealed that ANNs could serve as an appropriate tool to predict the adsorptive selectivity of the binary gas mixture in the absence of experimental data.
Key words： Cu3(BTC)2 electrochemical synthesis    CO2 adsorption    Taguchi optimization    ANN modeling
收稿日期: 2019-04-28      出版日期: 2020-03-24
Corresponding Author(s): Ali Asghar Ghoreyshi   
 引用本文:   
. [J]. Frontiers of Chemical Science and Engineering, 2020, 14(2): 233-247.
Kasra Pirzadeh, Ali Asghar Ghoreyshi, Mostafa Rahimnejad, Maedeh Mohammadi. Optimization of electrochemically synthesized Cu3(BTC)2 by Taguchi method for CO2/N2 separation and data validation through artificial neural network modeling. Front. Chem. Sci. Eng., 2020, 14(2): 233-247.
 链接本文:  
https://academic.hep.com.cn/fcse/CN/10.1007/s11705-019-1893-1
https://academic.hep.com.cn/fcse/CN/Y2020/V14/I2/233
Fig.1  
Controlling factors Variables Levels
1 2 3 4
Ligand /g L 0.6 0.8 1 1.2
Voltage /V V 20 25 30 35
Time /h T 1 1.5 2 2.5
Electrode length /cm E 1.5 2 2.5 3
Tab.1  
Fig.2  
Set No. MOF structure BET
/(m2·g–1)		 Pore vol. /(m3·g–1) CO2 heat of adsorption
/(kJ·mol–1)		 N2 heat of adsorption
/(kJ·mol–1)		 Ads. Temp.
/K		 Ads. Press.
/bar		 15:85
CO2/N2
selectivity		 Ref.
1 Q-MOF-1 140 0.07 15.3 10.5 298 1 17.2 [43]
2 Q-MOF-1 140 0.07 15.3 10.5 273 1 18.7 [43]
3 ZnDABCO 1863 0.67 19 14 294 1 9.3 [44]
4 NiDABCO 1904 0.98 19 17 294 1 7.2 [45]
5 CuDABCO 1415 0.72 19 13 294 1 7.2 [45]
6 MFM-300(Ga) 1175.77 0.39 40.03 17.37 298 1 100 [46]
7 MFM-300(Al) 1340.69 0.44 42.49 18.49 298 1 105 [46]
8 MFM-300(In-3N) 1174.54 0.39 35.92 15.71 298 1 50 [46]
9 mmen-CuBTTri 870 0.363 96 15 318 1 123 [47]
10 ZIF-8 1025 0.54 26 12.5 298 0.1 21 [48]
11 ZIF-8 1025 0.54 26 12.5 298 0.5 15 [48]
12 ZIF-8 1025 0.54 26 12.5 298 1 12 [48]
13 ZIF-8 1025 0.54 26 12.5 298 5 8 [48]
14 ZIF-8 1025 0.54 26 12.5 298 10 6 [48]
15 ZIF-8 1025 0.54 26 12.5 298 15 5 [48]
16 ED-ZIF-8 1428 0.75 33 11.5 298 0.1 37 [48]
17 ED-ZIF-8 1428 0.75 33 11.5 298 0.5 20 [48]
18 ED-ZIF-8 1428 0.75 33 11.5 298 1 15 [48]
19 ED-ZIF-8 1428 0.75 33 11.5 298 5 8 [48]
20 ED-ZIF-8 1428 0.75 33 11.5 298 10 7 [48]
21 ED-ZIF-8 1428 0.75 33 11.5 298 15 6.5 [48]
22 Mg-DOBDC 1800 0.5727 42 18 313 1 19 [49]
23 Mg-DOBDC 1800 0.5727 42 18 333 1 16 [49]
24 Mg-DOBDC 1800 0.5727 42 18 353 1 11 [49]
25 MIL-101 powder 2471 1.2 38.81 19.66 288 1 12.26 [50]
26 MIL-101 powder 2471 1.2 38.81 19.66 303 1 12.61 [50]
27 MIL-101 powder 2471 1.2 38.81 19.66 313 1 21.25 [50]
28 MIL-101 granular 1642 0.83 39.08 15.8 288 1 10.83 [50]
29 MIL-101 granular 1642 0.83 39.08 15.8 303 1 12 [50]
30 MIL-101 granular 1642 0.83 39.08 15.8 313 1 11.64 [50]
31 UIO-66 1105 0.55 24.8 12.8 298 0.5 30 [51]
32 UIO-66 1105 0.55 24.8 12.8 298 1 28 [51]
33 UIO-66 1105 0.55 24.8 12.8 298 1.5 27 [51]
34 UIO-66 1105 0.55 24.8 12.8 298 2 27 [51]
35 UIO-66 1105 0.55 24.8 12.8 298 2.5 27 [51]
36 UIO-66 1105 0.55 24.8 12.8 298 3 27 [51]
37 UIO-NH2 1123 0.52 28 16.2 298 0.5 58 [51]
38 UIO-NH2 1123 0.52 28 16.2 298 1 59 [51]
39 UIO-NH2 1123 0.52 28 16.2 298 1.5 60 [51]
40 UIO-NH2 1123 0.52 28 16.2 298 2 63 [51]
41 UIO-NH2 1123 0.52 28 16.2 298 2.5 65 [51]
42 UIO-NH2 1123 0.52 28 16.2 298 3 69 [51]
43 UIO-66 (Naphtyl) 757 0.42 26 16.6 298 0.5 30 [51]
44 UIO-66 (Naphtyl) 757 0.42 26 16.6 298 1 32 [51]
45 UIO-66 (Naphtyl) 757 0.42 26 16.6 298 1.5 33 [51]
46 UIO-66 (Naphtyl) 757 0.42 26 16.6 298 2 33 [51]
47 UIO-66 (Naphtyl) 757 0.42 26 16.6 298 2.5 33 [51]
48 UIO-66 (Naphtyl) 757 0.42 26 16.6 298 3 33 [51]
49 UIO-66 (NO2) 792 0.4 32 16 298 0.5 39 [51]
50 UIO-66 (NO2) 792 0.4 32 16 298 1 38 [51]
51 UIO-66 (NO2) 792 0.4 32 16 298 1.5 38 [51]
52 UIO-66 (NO2) 792 0.4 32 16 298 2 39 [51]
53 UIO-66 (NO22) 792 0.4 32 16 298 2.5 39 [51]
54 UIO-66 (NO2) 792 0.4 32 16 298 3 40 [51]
55 UIO-66 (Ome) 868 0.38 31.8 18.2 298 0.5 50 [51]
56 UIO-66 (Ome) 868 0.38 31.8 18.2 298 1 52 [51]
57 UIO-66 (Ome) 868 0.38 31.8 18.2 298 1.5 55 [51]
58 UIO-66 (Ome) 868 0.38 31.8 18.2 298 2 60 [51]
59 UIO-66 (Ome) 868 0.38 31.8 18.2 298 2.5 65 [51]
60 UIO-66 (Ome) 868 0.38 31.8 18.2 298 3 69 [51]
Tab.2  
No. Controlling factors Mean of CO2/N2 selectivity S/N ratios
Ligand /g Voltage /V Time /h Electrode /cm
1 0.6 20 1 1.5 29.96 29.53
2 0.6 25 1.5 2 29.31 29.34
3 0.6 30 2 2.5 28.68 29.09
4 0.6 35 2.5 3 28.48 28.90
5 0.8 20 1.5 2.5 32.21 30.15
6 0.8 25 1 3 31.86 30.06
7 0.8 30 2.5 1.5 28.11 28.97
8 0.8 35 2 2 28.05 28.95
9 1 20 2 3 31.12 29.86
10 1 25 2.5 2.5 31.37 30.20
11 1 30 1 2 30 29.54
12 1 35 1.5 1.5 27.52 28.79
13 1.2 20 2.5 2 31.79 29.76
14 1.2 25 2 1.5 31 29.82
15 1.2 30 1.5 3 31.97 30.04
16 1.2 35 1 2.5 29.85 29.49
Tab.3  
Level Ligand Voltage Time Electrode
1 28.13 29.62 28.71 29.27
2 29.21 29.85 29.58 26.39
3 29.83 29.41 29.65 29.51
4 28.66 27.08 27.75 29.73
Delta 1.70 2.77 1.90 3.34
Tab.4  
Source DoF Adj. SS Adj. MS F-value
Ligand 3 55.31 18.43 0.84
Voltage 3 143.54 47.84 2.18
Time 3 112.11 37.37 1.71
Electrode 3 265.81 88.60 4.07
Error 3 65.67 21.89
Total 15 642.44
Tab.5  
Fig.3  
Fig.4  
Sample SBET /(m2·g–1) Total pore volume /(cm3·g–1) Micropore volume
/(cm3·g–1)		 Mean pore diameter
/nm
Opt-Cu3(BTC)2 1627.4 0.69 0.67 1.69
Cu3(BTC)2 1474.1 0.62 0.59 1.68
Tab.6  
Fig.5  
Fig.6  
Constants CO2 N2
q0 /(mmol·g–1) 10.8851 2.7209
δ/K–1 0.0004 0.0008
KL0 /(L·mmol–1) 3.15× 10 −5 0.0053
Q /(kJ·mol–1) 34.1492 17.1850
Cost value 0.0161 0.0014
Tab.7  
Fig.7  
Fig.8  
Fig.9  
Fig.10  
MOF SBET /(m2·g–1) Vt /(cm3·g–1) T /K P /bar Synthesis time /h CO2 uptake /(mmol·g–1) CO2/N2 selectivity Ref.
Cu3(BTC)2 1571 0.79 298 1 24 3.80 20 [63]
Cu3(BTC)2 1922 0.80 273 1 24 7.32 22 [64]
Cu3(BTC)2 1202 0.59 298 1 12 4.07 16.8 [65]
Cu3(BTC)2 1326 0.58 303 1 12 3.00 N/A [66]
Cu3(BTC)2 1306 0.65 298 1 14 3.20 N/A [40]
Cu3(BTC)2 1370 0.57 298 1 24 3.20 N/A [67]
Cu3(BTC)2 1627 0.69 298 1 2 4.40 31 This study
Tab.8  
Fig.11  
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[1] FCE-19045-OF-PK_suppl_1 Download
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