{"title":"Bimetallic Pt-Pd nanoparticles on hierarchical core-shell zeolite for deep hydrogenation of naphthalene","authors":"Haiwei Li, Zhipeng Su, Xueyin Zhang, Tiehong Chen","doi":"10.1016/j.micromeso.2025.113686","DOIUrl":null,"url":null,"abstract":"<div><div>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.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"395 ","pages":"Article 113686"},"PeriodicalIF":4.8000,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Microporous and Mesoporous Materials","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1387181125002008","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
引用次数: 0
Abstract
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.
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.