层状核壳沸石上的Pt-Pd双金属纳米颗粒用于萘的深度加氢

IF 4.8 3区 材料科学 Q1 CHEMISTRY, APPLIED
Haiwei Li, Zhipeng Su, Xueyin Zhang, Tiehong Chen
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引用次数: 0

摘要

针对贵金属催化剂在多环芳烃(PAHs)深度加氢反应中传质受限和选择性低的问题,设计了分级核壳结构催化剂。随后,通过初始湿浸渍,将改性载体与Pt-Pd双金属纳米颗粒功能化,构建了高性能萘加氢催化剂。表征结果表明,碱处理产生了6 ~ 11 nm的介孔,但保留了原有的微孔结构,从而提高了传质效率。脱硅过程有效地调节了酸性位点的分布。均匀的Pt-Pd合金纳米颗粒(3-5 nm)表现出很强的电子协同作用,Pd三维结合能正偏移0.3 eV,这改善了氢的活化。在240℃条件下,0.75 wt% Pt-Pd/ h - β -73催化剂的萘转化率为99%,十氢萘选择性为68.6%,与单金属催化剂相比有了显著提高。而Pt-Pd合金与Brønsted酸位之间的相互作用则通过氢气溢出和底物吸附促进了深度加氢反应。本研究介绍了一种“介孔-酸-金属”优化策略,为开发将多环芳烃转化为高价值化学品的先进催化系统提供了新的见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Bimetallic Pt-Pd nanoparticles on hierarchical core-shell zeolite for deep hydrogenation of naphthalene
A hierarchical core-shell structured catalyst was designed to address the mass transfer limitations and low selectivity of noble metal catalysts in the deep hydrogenation of polycyclic aromatic hydrocarbons (PAHs). The modified support was subsequently functionalized with Pt-Pd bimetallic nanoparticles through incipient wetness impregnation to construct a high-performance naphthalene hydrogenation catalyst. Characterization revealed that mesopores (6–11 nm) were created by the alkaline treatment, while the original microporous structure was retained, resulting in enhanced mass transfer efficiency. The distribution of acidic sites was effectively modulated through the desilication process. Uniform Pt-Pd alloy nanoparticles (3–5 nm) were shown to exhibit strong electronic synergy, as evidenced by a 0.3 eV positive shift in the Pd 3d binding energy, which improved hydrogen activation. The 0.75 wt% Pt-Pd/H-Beta-73 catalyst achieved 99 % naphthalene conversion with 68.6 % decalin selectivity at 240 °C, representing a significant improvement over monometallic catalysts. The hierarchical pore structure facilitated both reactant diffusion and accessibility to acidic sites, while the interaction between Pt-Pd alloys and Brønsted acid sites promoted deep hydrogenation via hydrogen spillover and substrate adsorption. This research introduces a “mesopores-acid-metal” optimization strategy, providing new insights into the development of advanced catalytic systems for converting polycyclic aromatics into high-value chemicals.
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来源期刊
Microporous and Mesoporous Materials
Microporous and Mesoporous Materials 化学-材料科学:综合
CiteScore
10.70
自引率
5.80%
发文量
649
审稿时长
26 days
期刊介绍: Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.
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