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Synergistic Effect Between Ca4V4O14 and Vanadium-Substituted Hydroxyapatite in the Oxidative Dehydrogenation of Propane
ChemCatChem ( IF 3.8 ) Pub Date : 2021-07-13 , DOI: 10.1002/cctc.202100807 Guylene Costentin 1 , Sarah Petit 2 , Cyril Thomas 3 , Yannick Millot 4 , Frederic Averseng 4 , Dalil Brouri 5 , Jean-Marc Kraftt 2 , Stanislaw Dzwigaj 3 , Gwenaelle Rousse 6 , Christel Laberty-Robert 7
ChemCatChem ( IF 3.8 ) Pub Date : 2021-07-13 , DOI: 10.1002/cctc.202100807 Guylene Costentin 1 , Sarah Petit 2 , Cyril Thomas 3 , Yannick Millot 4 , Frederic Averseng 4 , Dalil Brouri 5 , Jean-Marc Kraftt 2 , Stanislaw Dzwigaj 3 , Gwenaelle Rousse 6 , Christel Laberty-Robert 7
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The present work reports on a new type of V-based catalysts, namely V-substituted hydroxyapatites, and the influence of the synthesis conditions on their catalytic performance in the oxidative dehydrogenation of propane (ODHP) reaction. Vx-substituted hydroxyapatite materials prepared with the periodic addition of ammonia during the maturation step (Vx-HAp-pH-per) were shown to exhibit a Ca4V4O14 phase in addition to the V-substituted hydroxyapatite phase for x greater than or equal to 3.5. TEM characterization of the biphasic samples allowed us to demonstrate that the Ca4V4O14 phase was grown epitaxially on the Vx-HAp nanorods. The close intimacy between the two phases was confirmed by NMR suggesting the involvement of V4+ species. Consistently EPR data of the fresh and spent samples showed that V4+ species may be stabilized at the boundaries of these two phases. The strong promotion of the oxidative dehydrogenation reaction to propene observed from 723 K for the V4-HAp-pH-per composition is attributed to a synergistic effect between the Vx-HAp nanorods that enable the activation of propane and the Ca4V4O14 phase that helps the redox exchanges. This synergy may be attributed to an easier electron delocalization on the V4O14 units located at the phases’ boundaries.
中文翻译：
Ca4V4O14与钒取代羟基磷灰石在丙烷氧化脱氢中的协同作用
目前的工作报告了一种新型的 V 基催化剂，即 V 取代的羟基磷灰石，以及合成条件对其在丙烷氧化脱氢 (ODHP) 反应中的催化性能的影响。在成熟步骤 (V x -HAp-pH-per)期间通过定期添加氨制备的V x - 取代的羟基磷灰石材料显示除了x的 V-取代的羟基磷灰石相之外还表现出 Ca 4 V 4 O 14相大于或等于 3.5。双相样品的 TEM 表征使我们能够证明 Ca 4 V 4 O 14相在 V x -HAp 纳米棒上外延生长。NMR证实了两相之间的密切关系，表明V 4+物种的参与。新鲜和废样品的一致 EPR 数据表明，V 4+物质可能稳定在这两个相的边界处。对于 V 4 -HAp-pH-per 组合物，从 723 K 观察到的丙烯氧化脱氢反应的强烈促进归因于能够活化丙烷的 V x -HAp 纳米棒和 Ca 4 V 4之间的协同效应Ø 14有助于氧化还原交换的相。这种协同作用可能归因于位于相边界的 V 4 O 14单元上更容易的电子离域。
更新日期：2021-09-17
中文翻译：
Ca4V4O14与钒取代羟基磷灰石在丙烷氧化脱氢中的协同作用
目前的工作报告了一种新型的 V 基催化剂，即 V 取代的羟基磷灰石，以及合成条件对其在丙烷氧化脱氢 (ODHP) 反应中的催化性能的影响。在成熟步骤 (V x -HAp-pH-per)期间通过定期添加氨制备的V x - 取代的羟基磷灰石材料显示除了x的 V-取代的羟基磷灰石相之外还表现出 Ca 4 V 4 O 14相大于或等于 3.5。双相样品的 TEM 表征使我们能够证明 Ca 4 V 4 O 14相在 V x -HAp 纳米棒上外延生长。NMR证实了两相之间的密切关系，表明V 4+物种的参与。新鲜和废样品的一致 EPR 数据表明，V 4+物质可能稳定在这两个相的边界处。对于 V 4 -HAp-pH-per 组合物，从 723 K 观察到的丙烯氧化脱氢反应的强烈促进归因于能够活化丙烷的 V x -HAp 纳米棒和 Ca 4 V 4之间的协同效应Ø 14有助于氧化还原交换的相。这种协同作用可能归因于位于相边界的 V 4 O 14单元上更容易的电子离域。
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