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摘要: 使用溶胶-凝胶法制备了LaCoO3催化剂，采用XRD、BET和XPS等方式对催化剂进行了表征，考察了该催化剂制备过程中煅烧温度、表面活性剂PEG-6000和PEG-20000含量对其H2S选择氧化制硫磺反应催化活性的影响。结果表明，表面活性剂PEG-6000及PEG-20000的添加能明显提高LaCoO3的催化活性。0.02 mol La（NO3）3+0.02mol Co（NO3）2溶液中添加0.30 g PEG-20000、煅烧温度为650℃时所制备的LaCoO3催化活性最好；在最佳反应温度260℃下，H2S的转化率达到96.10%，硫选择性为93.77%。Abstract: A series of LaCoO3 catalysts were prepared by sol-gel method and characterized by XRD, BET and XPS; the effect of calcination temperature and content of surfactant PEG-6000 and PEG-20000 on the catalytic activity of LaCoO3 in the selective oxidation of H2S to sulfur was investigated. The results illustrated that adding surfactant PEG-6000 and PEG-20000 can significantly improve the catalytic activity of LaCoO3 in H2S oxidation; the LaCoO3 catalyst prepared by adding 0.30 g PEG-20000 in the solution of 0.02 mol La(NO3)3 + 0.02 mol Co(NO3)2 and calcination at 650 ℃ exhibits the highest activity in H2S oxidation. Over this catalyst and under the optimum reaction temperature of 260 ℃, the conversion of H2S reaches 96.10%, with a selectivity of 93.77% to sulfur.
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Key words:
- LaCoO3 /
- H2S /
- selective oxidation
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图 1 煅烧温度对LaCoO3催化剂的H2S选择性氧化活性的影响
Figure 1 Effect of calcination temperature on the activity of LaCoO3 catalysts in the selective oxidation of H2S
: H2S conversion; : sulfur selectivity; : sulfur yield
图 2 PEG-6000含量对LaCoO3催化剂的H2S选择性氧化活性的影响
Figure 2 Effect of surfactant PEG-6000 contents on the activity of LaCoO3 catalysts in the selective oxidation of H2S
: H2S conversion; : sulfur selectivity; : sulfur yield
图 3 PEG-20000含量对LaCoO3催化剂的H2S选择性氧化活性的影响
Figure 3 Effect of PEG-20000 contents on the activity of LaCoO3 catalysts in the selective oxidation of H2S
: H2S conversion; : sulfur selectivity; : sulfur yield
图 4 反应温度对LaCoO3催化剂H2S选择性氧化活性的影响
Figure 4 Effect of reaction temperature on the selective oxidation of H2S over the LaCoO3 catalysts
: H2S conversion; : sulfur selectivity; : sulfur yield
图 5 LaCoO3催化剂的稳定性能
Figure 5 Stability of the LaCoO3 catalyst in the selective oxidation of H2S
图 6 不同煅烧温度下LaCoO3的XRD谱图
Figure 6 XRD patterns of the LaCoO3 catalysts obtained at different calcination temperatures
图 7 不同PEG-20000含量下催化剂的XRD谱图
Figure 7 XRD patterns of the LaCoO3 catalysts obtained with different PEG-20000 surfactant contents
图 8 LaCoO3催化剂的XPS谱图
Figure 8 XPS spectra of the LaCoO3 catalyst
(a): overview; (b): La 3d; (c): Co 2p; (d): O 1s
表 1 LaCoO3催化剂的制备条件
Table 1 Preparation conditions of LaCoO3 catalysts
Entry Calcination temperature t/℃ PEG-6000 content m/g PEG-20000 content m/g 1 600 - - 2 650 - - 3 700 - - 4 750 - - 5 650 0.15 - 6 650 0.3 - 7 650 0.45 - 8 650 0.6 - 9 650 - 0.15 10 650 - 0.3 11 650 - 0.45 12 650 - 0.6 
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表 2 催化剂的比表面积以及平均粒径
Table 2 Specific surface area and average particle size of the LaCoO3 catalysts obtained with different surfactant contents
Surfactant content Calcination temperature t/℃ ABET /(m2·g-1) dP/nm vP/(cm3·g-1) - 650 7.495 7.396 1.941×10-2 0.45 g PEG-6000 650 8.543 9.276 1.981×10-2 0.30 g PEG-20000 650 9.626 8.413 2.025×10-2
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