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Effect of surface acidity on the catalytic activity and deactivation of supported sulfonic acids during dehydration of methanol to DME
New Journal of Chemistry ( IF 2.7 ) Pub Date : 2020-09-09 , DOI: 10.1039/d0nj00229a Rosanna Viscardi 1, 2, 3, 4, 5 , Vincenzo Barbarossa 1, 2, 3, 4, 5 , Daniele Mirabile Gattia 1, 2, 3, 4, 5 , Raimondo Maggi 5, 6, 7, 8 , Giovanni Maestri 5, 6, 7, 8 , Francesco Pancrazzi 5, 6, 7, 8
New Journal of Chemistry ( IF 2.7 ) Pub Date : 2020-09-09 , DOI: 10.1039/d0nj00229a Rosanna Viscardi 1, 2, 3, 4, 5 , Vincenzo Barbarossa 1, 2, 3, 4, 5 , Daniele Mirabile Gattia 1, 2, 3, 4, 5 , Raimondo Maggi 5, 6, 7, 8 , Giovanni Maestri 5, 6, 7, 8 , Francesco Pancrazzi 5, 6, 7, 8
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The influence of a catalyst's surface acidity on the catalytic activity and deactivation in the dehydration of methanol to DME was investigated. Different materials including propylsulfonic acid functionalized silica with different Brønsted acidities, silica–alumina, and propyl and phenylsulfonic acid functionalized silica–alumina catalysts were prepared. All the samples were characterized by XRD, TGA, XPS, N2-sorption, ICP-OES and SEM analysis. It was found that the Brønsted and Lewis acidity of the SiO2/Al2O3-PhSO3H catalyst played a critical role in the performance of methanol to DME transformation. The grafting of sulfonic acid groups on silica–alumina enhanced the surface Brønsted acidity and also the reaction activity and selectivity for the dehydration of methanol to DME. In addition, the phenylsulfonic acid functionalized silica–alumina catalyst exhibited the highest activity and stability for the dehydration reaction at relatively low temperatures at which the γ-Al2O3 catalyst, commercial reference, displayed low dehydration activity. The effect of water was also investigated because in the indirect process to produce DME using acidic γ-alumina, it had the most important effect on catalyst deactivation. As a result, water had a positive effect on methanol dehydration over the SiO2/Al2O3-PhSO3H catalyst in contrast to γ-Al2O3 which was rapidly deactivated. Thus, Brønsted and Lewis acid sites with suitable strength may be responsible for the effective conversion of methanol to DME with high stability and selectivity.
中文翻译：
甲醇脱水制二甲醚过程中表面酸度对负载型磺酸催化活性和失活的影响
研究了催化剂的表面酸度对甲醇脱水生成二甲醚的催化活性和失活的影响。制备了不同的材料，包括具有不同布朗斯台德酸度的丙基磺酸官能化二氧化硅，二氧化硅-氧化铝以及丙基和苯磺酸官能化二氧化硅-氧化铝催化剂。通过XRD，TGA，XPS，N 2吸附，ICP-OES和SEM分析对所有样品进行表征。发现SiO 2 / Al 2 O 3 -PhSO 3的布朗斯台德和路易斯酸度H催化剂在甲醇向DME的转化中起着关键作用。二氧化硅-氧化铝上的磺酸基接枝提高了表面布朗斯台德酸度，并提高了甲醇脱水成二甲醚的反应活性和选择性。此外，苯基磺酸官能化的二氧化硅-氧化铝催化剂具有用于脱水反应的最高的活性和稳定性在相对低的温度下在其中的γ-Al 2 ö 3催化剂，商业参考，显示低脱水活性。还研究了水的影响，因为在使用酸性γ-氧化铝间接生产DME的过程中，水对催化剂的失活具有最重要的影响。结果，水对SiO2上的甲醇脱水有积极作用2 / Al的2 ö 3 -PhSO 3相反ħ催化剂的γ-Al 2 ö 3将其迅速失活。因此，具有合适强度的布朗斯台德和路易斯酸位点可以负责以高稳定性和选择性将甲醇有效地转化为二甲醚。
更新日期：2020-10-15
中文翻译：
甲醇脱水制二甲醚过程中表面酸度对负载型磺酸催化活性和失活的影响
研究了催化剂的表面酸度对甲醇脱水生成二甲醚的催化活性和失活的影响。制备了不同的材料，包括具有不同布朗斯台德酸度的丙基磺酸官能化二氧化硅，二氧化硅-氧化铝以及丙基和苯磺酸官能化二氧化硅-氧化铝催化剂。通过XRD，TGA，XPS，N 2吸附，ICP-OES和SEM分析对所有样品进行表征。发现SiO 2 / Al 2 O 3 -PhSO 3的布朗斯台德和路易斯酸度H催化剂在甲醇向DME的转化中起着关键作用。二氧化硅-氧化铝上的磺酸基接枝提高了表面布朗斯台德酸度，并提高了甲醇脱水成二甲醚的反应活性和选择性。此外，苯基磺酸官能化的二氧化硅-氧化铝催化剂具有用于脱水反应的最高的活性和稳定性在相对低的温度下在其中的γ-Al 2 ö 3催化剂，商业参考，显示低脱水活性。还研究了水的影响，因为在使用酸性γ-氧化铝间接生产DME的过程中，水对催化剂的失活具有最重要的影响。结果，水对SiO2上的甲醇脱水有积极作用2 / Al的2 ö 3 -PhSO 3相反ħ催化剂的γ-Al 2 ö 3将其迅速失活。因此，具有合适强度的布朗斯台德和路易斯酸位点可以负责以高稳定性和选择性将甲醇有效地转化为二甲醚。
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