Ivet Pafian, Jorge Noé Díaz de León, Juan Seguel, Néstor Escalona, Gina Pecchi, Carla Herrera, Catherine Sepulveda
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引用次数: 0
摘要
合成了负载在碳纳米管(CNTs)上的过渡金属氮化物(MxNy,其中M = Mo, Ni或Co),并对其作为乙酰丙酸在250℃和50 bar H2条件下转化的催化剂进行了评价。采用N2物理吸附、XRD、TEM、FT-IR、H2-TPR、NH3-TPD、2-丙醇转化、XPS等手段对催化剂进行了表征。其中,Mo2N/CNT催化剂表现出更强的金属-载体相互作用、更小的粒径和更明显的碳纳米管结构约束。这是由于与Ni-N和Co-N相比,Mo-N的键强度更高,这也影响了表面酸位的密度和强度。相比之下,Ni3N/CNT催化剂表现出最高的催化活性,并且与位于碳纳米管外部表面的较小氮化物颗粒相关。Co4N/CNT催化剂表现出中间行为。产物的选择性主要取决于表面氮化物和氮氧化物的存在,而不是过渡金属的特定性质。这些发现强调了金属支撑相互作用和活性相分散在设计稳定的非贵金属催化剂用于生物质衍生的平台分子转化中的作用。
Carbon Nanotube-Supported Mo, Ni, and Co Nitrides as Stable Catalysts for Levulinic Acid Conversion: Influence of Metal-Nitrogen Interactions and Confinement Effects.
Transition metal nitrides (MxNy, where M = Mo, Ni, or Co) supported on carbon nanotubes (CNTs) are synthesized and evaluated as catalysts for the conversion of levulinic acid at 250 °C and 50 bar H2. The catalysts are extensively characterized by N2 physisorption, XRD, TEM, FT-IR, H2-TPR, NH3-TPD, 2-propanol conversion, and XPS. Among the series, the Mo2N/CNT catalyst exhibits stronger metal-support interaction, smaller particle size, and more pronounced confinement within the CNT structure. This is attributed to the higher Mo-N bond strength compared to Ni-N and Co-N, which also influence the density and strength of surface acid sites. In contrast, the Ni3N/CNT catalyst displays the highest catalytic activity and is associated with smaller nitride particles located on the external CNT surface. The Co4N/CNT catalyst shows intermediate behavior. Product selectivity is primarily governed by the presence of surface nitride and oxynitride species, rather than the specific nature of the transition metal. These findings highlight the role of metal-support interactions and active phase dispersion in the design of stable, nonnoble metal catalysts for biomass-derived platform molecule conversions.
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