无额外供氢体下负载型MoFeO_x催化剂催化甘油制丙烯醇
发布时间：2019-01-28 21:26
【摘要】：采用浸渍法制备MoFe/X(X=SnO_2,ZrO_2,CeO_2,TiO_2,CNTs,MgO)以及MoFe氧化物催化剂用于甘油气-固相催化转化制丙烯醇。通过XRD、BET、XPS、H_2-TPR和NH_3-TPD表征,MoFe主要由晶相Fe_2O_3和Fe_2(MoO_4)_3组成而MoFe/X主要为高分散态的Fe、Mo氧化物(Fe~(3+)、Mo~(6+)),其表面均只存在弱酸中心;所采用载体由于自身性质(比表面积和酸碱性)差异与Mo、Fe氧化物之间存在不同的相互作用,进而有效地调控了MoFe/X的表面弱酸强度、酸浓度和可还原性能。所制备催化剂对甘油制丙烯醇的催化性能(收率)依次为:MoFe/TiO_2MoFe/CeO_2MoFe/ZrO_2MoFe/CNTsMoFe/SnO_2MoFeMoFe/MgO。340°C时,MoFe/TiO_2上甘油的转化率达到83.4%,丙烯醇的选择性和收率分别达到26.7%和22.3%;同时其展现出优于MoFe/CeO_2、MoFe/ZrO_2和MoFe/CNTs的稳定性。甘油转化率与催化剂表面弱酸中心浓度呈正相关性,而丙烯醇的生成则与氧化中心(非酸中心)密切相关。甘油转化率和丙烯醇选择性在MoFe/X上随反应温度变化而呈现相悖的变化趋势。
[Abstract]:MoFe/X was prepared by impregnation method, and MoFe oxide catalyst was used to catalyze the conversion of glycerol to allyl alcohol by gas-solid phase catalytic conversion of glycerol. XRD,BET,XPS,H_2-TPR and NH_3-TPD showed that MoFe was mainly composed of crystalline Fe_2O_3 and Fe_2 (MoO_4) _ 3, while MoFe/X was mainly highly dispersed Fe,Mo oxide (Fe~ (3), Mo~ (6),). There are only weak acid sites on the surface. Due to the differences of their own properties (specific surface area and acid-base) and the different interactions between the Mo,Fe oxides, the surface weak acid strength, acid concentration and reducibility of MoFe/X were effectively regulated. The catalytic activity (yield) of the prepared catalyst for glycerol to propanol was as follows: at MoFe/TiO_2MoFe/CeO_2MoFe/ZrO_2MoFe/CNTsMoFe/SnO_2MoFeMoFe/MgO.340 掳C, the conversion of glycerol on MoFe/TiO_2 was 83.4%. The selectivity and yield of allyl alcohol were 26.7% and 22.3%, respectively. At the same time, it shows better stability than MoFe/CeO_2,MoFe/ZrO_2 and MoFe/CNTs. The conversion rate of glycerol was positively correlated with the concentration of weak acid sites on the surface of the catalyst, while the formation of propanol was closely related to the oxidation center (non-acid center). The conversion of glycerol and the selectivity of allyl alcohol in MoFe/X showed a contrary trend with the change of reaction temperature.
【作者单位】： 中国科学院成都有机化学研究所;中国科学院大学;重庆工商大学环境与资源学院材料科学与工程系催化与功能有机分子重庆市重点实验室;
【基金】：中国科学院“西部之光”项目~~
【分类号】：O643.36;TQ223.14
本文编号：2417333
[Abstract]:MoFe/X was prepared by impregnation method, and MoFe oxide catalyst was used to catalyze the conversion of glycerol to allyl alcohol by gas-solid phase catalytic conversion of glycerol. XRD,BET,XPS,H_2-TPR and NH_3-TPD showed that MoFe was mainly composed of crystalline Fe_2O_3 and Fe_2 (MoO_4) _ 3, while MoFe/X was mainly highly dispersed Fe,Mo oxide (Fe~ (3), Mo~ (6),). There are only weak acid sites on the surface. Due to the differences of their own properties (specific surface area and acid-base) and the different interactions between the Mo,Fe oxides, the surface weak acid strength, acid concentration and reducibility of MoFe/X were effectively regulated. The catalytic activity (yield) of the prepared catalyst for glycerol to propanol was as follows: at MoFe/TiO_2MoFe/CeO_2MoFe/ZrO_2MoFe/CNTsMoFe/SnO_2MoFeMoFe/MgO.340 掳C, the conversion of glycerol on MoFe/TiO_2 was 83.4%. The selectivity and yield of allyl alcohol were 26.7% and 22.3%, respectively. At the same time, it shows better stability than MoFe/CeO_2,MoFe/ZrO_2 and MoFe/CNTs. The conversion rate of glycerol was positively correlated with the concentration of weak acid sites on the surface of the catalyst, while the formation of propanol was closely related to the oxidation center (non-acid center). The conversion of glycerol and the selectivity of allyl alcohol in MoFe/X showed a contrary trend with the change of reaction temperature.
【作者单位】： 中国科学院成都有机化学研究所;中国科学院大学;重庆工商大学环境与资源学院材料科学与工程系催化与功能有机分子重庆市重点实验室;
【基金】：中国科学院“西部之光”项目~~
【分类号】：O643.36;TQ223.14
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