Chem. J. Chinese Universities ›› 2016, Vol. 37 ›› Issue (1): 134.doi: 10.7503/cjcu20150389
• Physical Chemistry • Previous Articles Next Articles
JI Keming, MENG Fanhui, GAO Yuan, LI Zhong*()
Received:
2015-05-14
Online:
2016-01-10
Published:
2015-12-20
Contact:
LI Zhong
E-mail:lizhong@tyut.edu.cn
Supported by:
CLC Number:
TrendMD:
JI Keming, MENG Fanhui, GAO Yuan, LI Zhong. Effect of Fuel on Structure and Catalytic Performance for Slurry Methanation over Ni-Al2O3 Catalysts Prepared by Combustion Method†[J]. Chem. J. Chinese Universities, 2016, 37(1): 134.
Sample | Specific surface area/(m2·g-1) | Pore volume/(cm3·g-1) | Average pore diameter/nm |
---|---|---|---|
γ-Al2O3 | 191 | 0.38 | 5.8 |
NiAl-IU | 162 | 0.30 | 5.5 |
NiAl-IG | 153 | 0.29 | 5.2 |
NiAl-IE | 147 | 0.24 | 4.9 |
NiAl-CU | 468 | 0.28 | 2.4 |
NiAl-CG | 158 | 0.41 | 10.1 |
NiAl-CE | 51 | 0.05 | 3.6 |
Table 1 Textural properties of Al2O3 support and the catalysts
Sample | Specific surface area/(m2·g-1) | Pore volume/(cm3·g-1) | Average pore diameter/nm |
---|---|---|---|
γ-Al2O3 | 191 | 0.38 | 5.8 |
NiAl-IU | 162 | 0.30 | 5.5 |
NiAl-IG | 153 | 0.29 | 5.2 |
NiAl-IE | 147 | 0.24 | 4.9 |
NiAl-CU | 468 | 0.28 | 2.4 |
NiAl-CG | 158 | 0.41 | 10.1 |
NiAl-CE | 51 | 0.05 | 3.6 |
Catalyst | Ni crystallite size/nm | Ni dispersion(%) | Metal surface area/(m2·g-1) |
---|---|---|---|
NiAl-IU | 6.9 | 7.7 | 10.3 |
NiAl-IG | 7.0 | 7.2 | 9.6 |
NiAl-IE | 7.3 | 6.9 | 9.2 |
NiAl-CU | 6.3 | 7.9 | 10.5 |
NiAl-CG | 7.6 | 6.2 | 8.3 |
NiAl-CE | 12.5 | 3.5 | 4.8 |
Table 2 XRD and H2 chemisorption analytic results for the catalysts
Catalyst | Ni crystallite size/nm | Ni dispersion(%) | Metal surface area/(m2·g-1) |
---|---|---|---|
NiAl-IU | 6.9 | 7.7 | 10.3 |
NiAl-IG | 7.0 | 7.2 | 9.6 |
NiAl-IE | 7.3 | 6.9 | 9.2 |
NiAl-CU | 6.3 | 7.9 | 10.5 |
NiAl-CG | 7.6 | 6.2 | 8.3 |
NiAl-CE | 12.5 | 3.5 | 4.8 |
Fig.4 TEM images of NiAl-IU(A, A'), NiAl-IG(B, B'), NiAl-IE(C, C'), NiAl-CU(D, D'), NiAl-CG(E, E') and NiAl-CE(F, F') catalysts before(A—F) and after(A'—F') reduction
Catalyst | Relative content, w(%)(reduction temperature/℃) | /(mmol·g-1) | ||||
---|---|---|---|---|---|---|
Ni2O3 | α-NiO | β1-NiO | β2-NiO | γ-NiO | ||
NiAl-IU | 11(220) | 5(268) | 36(321) | 37(439) | 11(499) | 2.70 |
NiAl-IG | 8(232) | 5(279) | 30(323) | 46(412) | 11(504) | 2.14 |
NiAl-IE | 2(214) | 5(275) | 38(321) | 46(462) | 9(566) | 1.96 |
NiAl-CU | ___ | 27(280) | 35(459) | 31(543) | 7(709) | 2.76 |
NiAl-CG | ___ | 39(373) | 14(448) | 33(509) | 14(646) | 2.04 |
NiAl-CE | ___ | 83(345) | 3(430) | 3(499) | 11(600) | 1.91 |
Table 3 Gaussian fitting analysis of H2-TPR profiles of the Ni-based catalysts
Catalyst | Relative content, w(%)(reduction temperature/℃) | /(mmol·g-1) | ||||
---|---|---|---|---|---|---|
Ni2O3 | α-NiO | β1-NiO | β2-NiO | γ-NiO | ||
NiAl-IU | 11(220) | 5(268) | 36(321) | 37(439) | 11(499) | 2.70 |
NiAl-IG | 8(232) | 5(279) | 30(323) | 46(412) | 11(504) | 2.14 |
NiAl-IE | 2(214) | 5(275) | 38(321) | 46(462) | 9(566) | 1.96 |
NiAl-CU | ___ | 27(280) | 35(459) | 31(543) | 7(709) | 2.76 |
NiAl-CG | ___ | 39(373) | 14(448) | 33(509) | 14(646) | 2.04 |
NiAl-CE | ___ | 83(345) | 3(430) | 3(499) | 11(600) | 1.91 |
Fig.6 Catalytic stability of Ni-Al2O3 catalysts for slurry CO methanation ^Reaction conditions: 260 ℃, 1.0 MPa, V(H2)∶V(CO)=3∶1, space velocity: 3000 mL·g-1·h-1.
Catalyst | Conversion of CO(%) | Selectivity(%) | Yield for CH4(%) | ||
---|---|---|---|---|---|
CH4 | C2—C4 | CO2 | |||
NiAl-IU | 83.5 | 90.1 | 4.6 | 5.3 | 75.2 |
NiAl-IG | 81.3 | 89.4 | 5.2 | 5.4 | 72.7 |
NiAl-IE | 80.1 | 88.3 | 5.8 | 5.9 | 70.7 |
NiAl-CU | 84.7 | 91.1 | 4.4 | 4.5 | 77.2 |
NiAl-CG | 63.2 | 87.8 | 6.2 | 6.0 | 55.5 |
NiAl-CE | 43.1 | 81.6 | 7.1 | 11.3 | 35.2 |
Table 4 Catalytic performance of Ni-Al2O3 catalysts for slurry CO methanation*
Catalyst | Conversion of CO(%) | Selectivity(%) | Yield for CH4(%) | ||
---|---|---|---|---|---|
CH4 | C2—C4 | CO2 | |||
NiAl-IU | 83.5 | 90.1 | 4.6 | 5.3 | 75.2 |
NiAl-IG | 81.3 | 89.4 | 5.2 | 5.4 | 72.7 |
NiAl-IE | 80.1 | 88.3 | 5.8 | 5.9 | 70.7 |
NiAl-CU | 84.7 | 91.1 | 4.4 | 4.5 | 77.2 |
NiAl-CG | 63.2 | 87.8 | 6.2 | 6.0 | 55.5 |
NiAl-CE | 43.1 | 81.6 | 7.1 | 11.3 | 35.2 |
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