CIESC Journal ›› 2021, Vol. 72 ›› Issue (5): 2604-2615.DOI: 10.11949/0438-1157.20201738
• Catalysis, kinetics and reactors • Previous Articles Next Articles
ZHANG Yuming1(),JI Dexin1,2,ZHU Hanwen1,2,WAN Lifeng1,2,ZHANG Wei1,WEN Hongyan1,2,YUE Junrong2()
Received:
2020-12-03
Revised:
2021-02-20
Online:
2021-05-05
Published:
2021-05-05
Contact:
ZHANG Yuming,YUE Junrong
张玉明1(),纪德馨1,2,朱翰文1,2,万利锋1,2,张炜1,温宏炎1,2,岳君容2()
通讯作者:
张玉明,岳君容
作者简介:
张玉明(1985—),男,博士,副教授,基金资助:
CLC Number:
ZHANG Yuming, JI Dexin, ZHU Hanwen, WAN Lifeng, ZHANG Wei, WEN Hongyan, YUE Junrong. Reaction kinetics of naphthalene cracking into small molecule gas in a micro fluidized bed[J]. CIESC Journal, 2021, 72(5): 2604-2615.
张玉明, 纪德馨, 朱翰文, 万利锋, 张炜, 温宏炎, 岳君容. 微型流化床中萘裂解生成小分子气体的反应动力学研究[J]. 化工学报, 2021, 72(5): 2604-2615.
样品 | 工业分析/%(质量分数) | 元素分析/%(质量分数) | |||||||
---|---|---|---|---|---|---|---|---|---|
Vad | Mad | Aad | FCad* | Nd | Cd | Hd | Sd | Od* | |
LC | 4.12 | 2.92 | 25.59 | 67.37 | 0.94 | 69.32 | 1.49 | 0.80 | 1.09 |
Table 1 Proximate and ultimate analysis of sample
样品 | 工业分析/%(质量分数) | 元素分析/%(质量分数) | |||||||
---|---|---|---|---|---|---|---|---|---|
Vad | Mad | Aad | FCad* | Nd | Cd | Hd | Sd | Od* | |
LC | 4.12 | 2.92 | 25.59 | 67.37 | 0.94 | 69.32 | 1.49 | 0.80 | 1.09 |
LC ash/%(质量分数) | ||||||||
---|---|---|---|---|---|---|---|---|
TiO2 | MgO | Al2O3 | SiO2 | SO3 | K2O | CaO | Fe2O3 | Others |
1.19 | 3.94 | 8.56 | 12.63 | 31.65 | 0.54 | 34.46 | 6.52 | 0.51 |
FCC-C/%(质量分数) | ||||||||
V2O5 | P2O5 | Al2O3 | SiO2 | Na2O | K2O | NiO | Fe2O3 | Others |
1.09 | 1.38 | 47.87 | 47.34 | 0.36 | 0.20 | 0.52 | 0.51 | 0.73 |
Table 2 XRF analysis of the LC ash and FCC catalyst
LC ash/%(质量分数) | ||||||||
---|---|---|---|---|---|---|---|---|
TiO2 | MgO | Al2O3 | SiO2 | SO3 | K2O | CaO | Fe2O3 | Others |
1.19 | 3.94 | 8.56 | 12.63 | 31.65 | 0.54 | 34.46 | 6.52 | 0.51 |
FCC-C/%(质量分数) | ||||||||
V2O5 | P2O5 | Al2O3 | SiO2 | Na2O | K2O | NiO | Fe2O3 | Others |
1.09 | 1.38 | 47.87 | 47.34 | 0.36 | 0.20 | 0.52 | 0.51 | 0.73 |
样品 | 比表面积/(m2/g) | 孔体积/(cm3/g) | 平均孔径Da/nm | ||||
---|---|---|---|---|---|---|---|
Atotal | Amicro | Ameso | Vtotal | Vmico | Vmeso | ||
LC | 214.0 | 175.5 | 38.5 | 0.5319 | 0.1043 | 0.4276 | 9.94 |
FCC-C | 106.8 | 64.6 | 42.2 | 0.5716 | 0.0432 | 0.5329 | 24.97 |
Table 3 Pore structure analysis of LC and FCC-C samples
样品 | 比表面积/(m2/g) | 孔体积/(cm3/g) | 平均孔径Da/nm | ||||
---|---|---|---|---|---|---|---|
Atotal | Amicro | Ameso | Vtotal | Vmico | Vmeso | ||
LC | 214.0 | 175.5 | 38.5 | 0.5319 | 0.1043 | 0.4276 | 9.94 |
FCC-C | 106.8 | 64.6 | 42.2 | 0.5716 | 0.0432 | 0.5329 | 24.97 |
函数 | 机理模型 | f(X) | G(X) |
---|---|---|---|
G(1) | 一维扩散 | 1/2X | X 2 |
G(2) | 二维扩散 | [-ln(1-X)]-1 | X+(1-X)ln(1-X) |
G(3) | 三维扩散(球形对称) | 3/2×(1-X)2/3[1-(1-X)1/3] -1 | [1-(1-X)1/3]2 |
G(4) | 三维扩散(圆柱形对称) | 3/2X[(1-X)-1/3-1] -1 | (1-2/3X)-(1-X)2/3 |
G(5) | 三维扩散 | 1.5(1+X)2/3[(1+X)1/3-1] -1 | [(1+X)1/3-1]2 |
G(6) | 成核与生长 (n =2/3) | 1.5(1-X)[-ln(1-X)]1/3 | [-ln(1-X)]2/3 |
G(7) | 成核与生长 (n =1/2) | 2(1-X)[-ln(1-X)]1/2 | [-ln(1-X)]1/2 |
G(8) | 成核与生长 (n =1/3) | 3(1-X)[-ln(1-X)]2/3 | [-ln(1-X)]1/3 |
G(9) | 成核与生长 (n =1/4) | 4(1-X)[-ln(1-X)]3/4 | [-ln(1-X)]1/4 |
G(10) | 自催化 | X(1-X) | ln[X/(1-X)] |
G(11) | Mampel power法则(n =1/2) | 2X1/2 | X1/2 |
G(12) | Mampel power法则(n =1/3) | 3X2/3 | X1/3 |
G(13) | Mampel power法则(n =1/4) | 4X3/4 | X1/4 |
G(14) | 化学反应(n =3) | (1-X)3 | [(1-X) -2-1]/2 |
G(15) | 化学反应(n =2) | (1-X)2 | (1-X) -1-1 |
G(16) | 化学反应(n=1) | 1-X | -ln(1-X) |
G(17) | 收缩几何形状(片状) | 1 | X |
G(18) | 收缩几何形状(球形对称) | 3(1-X)2/3 | 1-(1-X)1/3 |
G(19) | 收缩几何形状(圆柱形对称) | 2(1-X)1/2 | 1-(1-X)1/2 |
Table 4 Typical reaction mechanisms for heterogeneous solid-state reaction
函数 | 机理模型 | f(X) | G(X) |
---|---|---|---|
G(1) | 一维扩散 | 1/2X | X 2 |
G(2) | 二维扩散 | [-ln(1-X)]-1 | X+(1-X)ln(1-X) |
G(3) | 三维扩散(球形对称) | 3/2×(1-X)2/3[1-(1-X)1/3] -1 | [1-(1-X)1/3]2 |
G(4) | 三维扩散(圆柱形对称) | 3/2X[(1-X)-1/3-1] -1 | (1-2/3X)-(1-X)2/3 |
G(5) | 三维扩散 | 1.5(1+X)2/3[(1+X)1/3-1] -1 | [(1+X)1/3-1]2 |
G(6) | 成核与生长 (n =2/3) | 1.5(1-X)[-ln(1-X)]1/3 | [-ln(1-X)]2/3 |
G(7) | 成核与生长 (n =1/2) | 2(1-X)[-ln(1-X)]1/2 | [-ln(1-X)]1/2 |
G(8) | 成核与生长 (n =1/3) | 3(1-X)[-ln(1-X)]2/3 | [-ln(1-X)]1/3 |
G(9) | 成核与生长 (n =1/4) | 4(1-X)[-ln(1-X)]3/4 | [-ln(1-X)]1/4 |
G(10) | 自催化 | X(1-X) | ln[X/(1-X)] |
G(11) | Mampel power法则(n =1/2) | 2X1/2 | X1/2 |
G(12) | Mampel power法则(n =1/3) | 3X2/3 | X1/3 |
G(13) | Mampel power法则(n =1/4) | 4X3/4 | X1/4 |
G(14) | 化学反应(n =3) | (1-X)3 | [(1-X) -2-1]/2 |
G(15) | 化学反应(n =2) | (1-X)2 | (1-X) -1-1 |
G(16) | 化学反应(n=1) | 1-X | -ln(1-X) |
G(17) | 收缩几何形状(片状) | 1 | X |
G(18) | 收缩几何形状(球形对称) | 3(1-X)2/3 | 1-(1-X)1/3 |
G(19) | 收缩几何形状(圆柱形对称) | 2(1-X)1/2 | 1-(1-X)1/2 |
Conversion ratio of gas during cracking | H2 | CH4 | ||||||
---|---|---|---|---|---|---|---|---|
FCC-C | LC | FCC-C | LC | |||||
Ea/(kJ/mol) | R2 | Ea/(kJ/mol) | R2 | Ea/(kJ/mol) | R2 | Ea/(kJ/mol) | R2 | |
0.2 | 21.8 | 0.865 | 23.0 | 0.991 | 66.8 | 0.976 | 43.6 | 0.969 |
0.4 | 40.4 | 0.994 | 31.5 | 0.995 | 68.2 | 0.963 | 47.4 | 0.951 |
0.6 | 68.5 | 0.964 | 82.2 | 0.993 | 107.9 | 0.980 | 78.1 | 0.923 |
0.8 | 88.3 | 0.999 | 53.8 | 0.987 | 129.5 | 0.996 | 124.1 | 0.999 |
average | 54.8 | — | 47.6 | — | 93.1 | — | 73.3 | — |
Table 5 Activation energies by the Friedman method
Conversion ratio of gas during cracking | H2 | CH4 | ||||||
---|---|---|---|---|---|---|---|---|
FCC-C | LC | FCC-C | LC | |||||
Ea/(kJ/mol) | R2 | Ea/(kJ/mol) | R2 | Ea/(kJ/mol) | R2 | Ea/(kJ/mol) | R2 | |
0.2 | 21.8 | 0.865 | 23.0 | 0.991 | 66.8 | 0.976 | 43.6 | 0.969 |
0.4 | 40.4 | 0.994 | 31.5 | 0.995 | 68.2 | 0.963 | 47.4 | 0.951 |
0.6 | 68.5 | 0.964 | 82.2 | 0.993 | 107.9 | 0.980 | 78.1 | 0.923 |
0.8 | 88.3 | 0.999 | 53.8 | 0.987 | 129.5 | 0.996 | 124.1 | 0.999 |
average | 54.8 | — | 47.6 | — | 93.1 | — | 73.3 | — |
Temp./℃ | 参数 | H2 | CH4 | ||||
---|---|---|---|---|---|---|---|
G(2) | G(4) | G(19) | G(4) | G(16) | G(19) | ||
700 | k(T) | 0.0109 | 0.0034 | 0.0093 | 0.0033 | 0.0532 | 0.0086 |
lnk(T) | -4.519 | -5.687 | -4.678 | -5.711 | -2.934 | -4.756 | |
R2 | 0.996 | 0.982 | 0.989 | 0.972 | 0.834 | 0.878 | |
750 | k(T) | 0.0098 | 0.0032 | 0.0080 | 0.0060 | 0.0947 | 0.0158 |
lnk(T) | -4.625 | -5.745 | -4.828 | -5.121 | -2.357 | -4.151 | |
R2 | 0.922 | 0.969 | 0.877 | 0.958 | 0.960 | 0.873 | |
800 | k(T) | 0.0104 | 0.0034 | 0.0087 | 0.0148 | 0.2253 | 0.0443 |
lnk(T) | -4.566 | -5.678 | -4.744 | -4.213 | -1.490 | -3.116 | |
R2 | 0.885 | 0.946 | 0.852 | 0.945 | 0.877 | 0.983 | |
850 | k(T) | 0.0270 | 0.0086 | 0.0230 | 0.0160 | 0.2585 | 0.0462 |
lnk(T) | -3.612 | -4.756 | -3.772 | -4.135 | -1.353 | -3.075 | |
R2 | 0.968 | 0.988 | 0.959 | 0.962 | 0.899 | 0.979 | |
Ea/(kJ/mol) | 53.6 | 50.2 | 48.9 | 73.6 | 102.5 | 111.2 |
Table 6 Reaction models and kinetic parameters for H2 and CH4 in naphthalene pyrolysis using LC
Temp./℃ | 参数 | H2 | CH4 | ||||
---|---|---|---|---|---|---|---|
G(2) | G(4) | G(19) | G(4) | G(16) | G(19) | ||
700 | k(T) | 0.0109 | 0.0034 | 0.0093 | 0.0033 | 0.0532 | 0.0086 |
lnk(T) | -4.519 | -5.687 | -4.678 | -5.711 | -2.934 | -4.756 | |
R2 | 0.996 | 0.982 | 0.989 | 0.972 | 0.834 | 0.878 | |
750 | k(T) | 0.0098 | 0.0032 | 0.0080 | 0.0060 | 0.0947 | 0.0158 |
lnk(T) | -4.625 | -5.745 | -4.828 | -5.121 | -2.357 | -4.151 | |
R2 | 0.922 | 0.969 | 0.877 | 0.958 | 0.960 | 0.873 | |
800 | k(T) | 0.0104 | 0.0034 | 0.0087 | 0.0148 | 0.2253 | 0.0443 |
lnk(T) | -4.566 | -5.678 | -4.744 | -4.213 | -1.490 | -3.116 | |
R2 | 0.885 | 0.946 | 0.852 | 0.945 | 0.877 | 0.983 | |
850 | k(T) | 0.0270 | 0.0086 | 0.0230 | 0.0160 | 0.2585 | 0.0462 |
lnk(T) | -3.612 | -4.756 | -3.772 | -4.135 | -1.353 | -3.075 | |
R2 | 0.968 | 0.988 | 0.959 | 0.962 | 0.899 | 0.979 | |
Ea/(kJ/mol) | 53.6 | 50.2 | 48.9 | 73.6 | 102.5 | 111.2 |
Temp./℃ | 参数 | H2 | CH4 | ||||
---|---|---|---|---|---|---|---|
G(3) | G(6) | G(16) | G (6) | G (7) | G (16) | ||
700 | k(T) | — | — | — | 0.0897 | 0.0664 | 0.1504 |
lnk(T) | — | — | — | -2.4113 | -2.7121 | -1.8945 | |
R2 | — | — | — | 0.9420 | 0.9255 | 0.8934 | |
750 | k(T) | 0.0663 | 0.2571 | 0.4516 | 0.1555 | 0.1100 | 0.2876 |
lnk(T) | -2.7136 | -1.3583 | -0.7950 | -1.8611 | -2.2073 | -1.2462 | |
R2 | 0.989 | 0.975 | 0.923 | 0.9504 | 0.9205 | 0.9359 | |
800 | k(T) | 0.0638 | 0.2556 | 0.4646 | 0.3208 | 0.2294 | 0.5849 |
lnk(T) | -2.7520 | -1.3641 | -0.7666 | -1.1369 | -1.4723 | -0.5363 | |
R2 | 0.987 | 0.982 | 0.987 | 0.9931 | 0.9796 | 0.9757 | |
850 | k(T) | 0.1169 | 0.4615 | 0.8806 | 0.3871 | 0.2769 | 0.7475 |
lnk(T) | -2.1464 | -0.7733 | -0.1272 | -0.9491 | -1.2841 | -0.2910 | |
R2 | 0.973 | 0.986 | 0.963 | 0.9898 | 0.9830 | 0.9505 | |
Ea/(kJ/mol) | 53.2 | 57.0 | 62.8 | 93.3 | 91.6 | 100.8 |
Table 7 Reaction models and kinetic parameters for H2 and CH4 in naphthalene pyrolysis using FCC-C
Temp./℃ | 参数 | H2 | CH4 | ||||
---|---|---|---|---|---|---|---|
G(3) | G(6) | G(16) | G (6) | G (7) | G (16) | ||
700 | k(T) | — | — | — | 0.0897 | 0.0664 | 0.1504 |
lnk(T) | — | — | — | -2.4113 | -2.7121 | -1.8945 | |
R2 | — | — | — | 0.9420 | 0.9255 | 0.8934 | |
750 | k(T) | 0.0663 | 0.2571 | 0.4516 | 0.1555 | 0.1100 | 0.2876 |
lnk(T) | -2.7136 | -1.3583 | -0.7950 | -1.8611 | -2.2073 | -1.2462 | |
R2 | 0.989 | 0.975 | 0.923 | 0.9504 | 0.9205 | 0.9359 | |
800 | k(T) | 0.0638 | 0.2556 | 0.4646 | 0.3208 | 0.2294 | 0.5849 |
lnk(T) | -2.7520 | -1.3641 | -0.7666 | -1.1369 | -1.4723 | -0.5363 | |
R2 | 0.987 | 0.982 | 0.987 | 0.9931 | 0.9796 | 0.9757 | |
850 | k(T) | 0.1169 | 0.4615 | 0.8806 | 0.3871 | 0.2769 | 0.7475 |
lnk(T) | -2.1464 | -0.7733 | -0.1272 | -0.9491 | -1.2841 | -0.2910 | |
R2 | 0.973 | 0.986 | 0.963 | 0.9898 | 0.9830 | 0.9505 | |
Ea/(kJ/mol) | 53.2 | 57.0 | 62.8 | 93.3 | 91.6 | 100.8 |
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