Effect of citric acid addition on MoO3/CeO2-Al2O3 catalyst for sulfur-resistant methanation
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摘要: 将柠檬酸（CA）作为络合剂添加至CeO2-Al2O3复合载体中，并考察了CA对MoO3/CeO2-Al2O3催化剂耐硫甲烷化性能的影响。活性评价结果显示，催化剂活性随柠檬酸添加量的增大而增大，当n（CA）/n（Ce）为3时，CO转化率可达60%。催化剂BET、XRD、H2-TPR及XPS等表征结果表明，在CeO2-Al2O3复合载体中加入CA，可以增大载体及催化剂的比表面积，使Mo物种分散性提高。同时，CA对Ce物种起络合作用，致使催化剂表面Ce元素含量明显增加，进而减弱了活性组分Mo物种与载体间相互作用力，并最终导致了催化剂活性的提升。Abstract: Citric acid hold great promise to improve the Mo-based catalyst performance for hydrogenation reaction applications. MoO3/CeO2-Al2O3 catalysts were prepared by impregnation method with adding citric acid into CeO2-Al2O3 composite supports and tested for sulfur resistant methanation. The syngas methanation activity increased with the increase of citric acid additive amount, and CO conversion could reach up 60% when the molar ratio of citric acid to Ce was 3. The prepared catalysts were characterized by BET, H2-TPR, XRD and XPS. The increased catalytic performance was mainly attributed to the increased amount of Ce species on the surface of catalysts which could decreased the interaction force between MoO3 and CeO2-Al2O3 supports. Additionally, the increased specific surface of CeO2-Al2O3 composite support was also in favor of catalytic performance.
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Key words:
- synthetic natural gas /
- methanation /
- CeO2 /
- citric acid
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Figure 4 CO methanation activity of Mo-based catalyst samples (a): CO conversion; (b): CH4 selectivity
■: CA/Ce=0; ●: CA/Ce=0.5; ▲: CA/Ce=1; : CA/Ce=3
Table 1 Textural properties of CeAl supports with/without the addition of citric acid and their corresponding catalysts
Support BET surface area
A/(m2·g-1)Pore size d/nm CeO2 diameter
D/nmCatalyst BET surface area
A/(m2·g-1)Pore size d/nm CeAl 97 13.6 7.7 Mo/CeAl 76 13.0 CeAl-1CA 117 9.6 7.5 Mo/CeAl-1CA 89 10.2 
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