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Oxidative Dehydration of Glycerol to Acrylic Acid over Vanadium-Substituted Cesium Salts of Keggin-Type Heteropolyacids
ACS Catalysis ( IF 11.3 ) Pub Date : 2016-03-28 00:00:00 , DOI: 10.1021/acscatal.6b00213 Xiukai Li 1 , Yugen Zhang 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2016-03-28 00:00:00 , DOI: 10.1021/acscatal.6b00213 Xiukai Li 1 , Yugen Zhang 1
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Acrylic acid is one of the most desired products from bioglycerol. In this work, we demonstrated that Keggin-type heteropoly compounds (HPCs) act as efficient bifunctional catalysts for the one-step conversion of glycerol to acrylic acid in gas phase. This is the first example of HPCs as catalysts for selective conversion of glycerol to acrylic acid. It was found that introduction of vanadium species into the secondary structure of the cesium salts of H3PMo12O40 and H3PW12O40 heteropolyacids is beneficial for acrylic acid formation. The combination of H0.1Cs2.5(VO)0.2PMo12O40 and H0.1Cs2.5(VO)0.2PW12O40 as solid solutions resulted in variations in the oxidization ability and surface acidity of the catalysts and, consequently, notably improved selectivity for acrylic acid. Up to 60% yield to acrylic acid was achieved over the catalyst with the formula of H0.1Cs2.5(VO)0.2(PMo12O40)0.25(PW12O40)0.75. The catalyst also showed good resistance to coke deposition and long-term stability due to the salt feature. It is deduced that the synergism between the Keggin anions and the cesium/vanadium entities at the secondary structure determined the overall catalyst performance.
中文翻译：
Keggin型杂多酸的钒取代铯盐将甘油氧化脱水为丙烯酸
丙烯酸是生物甘油最需要的产品之一。在这项工作中，我们证明了Keggin型杂多化合物（HPC）可以作为气相中甘油一步转化为丙烯酸的有效双功能催化剂。这是HPC作为将甘油选择性转化为丙烯酸的催化剂的第一个例子。发现将钒物种引入H 3 PMo 12 O 40和H 3 PW 12 O 40杂多酸铯盐的二级结构中对丙烯酸的形成是有利的。H 0.1 Cs 2.5（VO）0.2 PMo 12 O的组合40和H 0.1 Cs 2.5（VO）0.2 PW 12 O 40固溶体导致催化剂的氧化能力和表面酸度变化，因此，对丙烯酸的选择性显着提高。在分子式为H 0.1 Cs 2.5（VO）0.2（PMo 12 O 40）0.25（PW 12 O 40）0.75的催化剂上，丙烯酸的收率高达60％。由于盐的特征，该催化剂还显示出良好的抗焦炭沉积性和长期稳定性。可以推断，在二级结构中，Keggin阴离子与铯/钒实体之间的协同作用决定了催化剂的整体性能。
更新日期：2016-03-28
中文翻译：
Keggin型杂多酸的钒取代铯盐将甘油氧化脱水为丙烯酸
丙烯酸是生物甘油最需要的产品之一。在这项工作中，我们证明了Keggin型杂多化合物（HPC）可以作为气相中甘油一步转化为丙烯酸的有效双功能催化剂。这是HPC作为将甘油选择性转化为丙烯酸的催化剂的第一个例子。发现将钒物种引入H 3 PMo 12 O 40和H 3 PW 12 O 40杂多酸铯盐的二级结构中对丙烯酸的形成是有利的。H 0.1 Cs 2.5（VO）0.2 PMo 12 O的组合40和H 0.1 Cs 2.5（VO）0.2 PW 12 O 40固溶体导致催化剂的氧化能力和表面酸度变化，因此，对丙烯酸的选择性显着提高。在分子式为H 0.1 Cs 2.5（VO）0.2（PMo 12 O 40）0.25（PW 12 O 40）0.75的催化剂上，丙烯酸的收率高达60％。由于盐的特征，该催化剂还显示出良好的抗焦炭沉积性和长期稳定性。可以推断，在二级结构中，Keggin阴离子与铯/钒实体之间的协同作用决定了催化剂的整体性能。
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