Regioselective encapsulation of Pd clusters in hollow polycrystalline shell

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2024-10-22 DOI:10.1016/j.micromeso.2024.113389

Hongyan Wang , Xinyue Sun , Jingpei Cao , Yajie Tian , Bofeng Zhang

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Abstract

Zeolite catalysts have been widely applied in petroleum and chemical industries. Nano/hierarchical structure could improve the utilization efficiency of active sites, especially for metal species encapsulated in zeolites. However, the uniformity of zeolite surface and crystallinity would decrease, leading to low stabilization effect. Herein, we developed a seed-directed method to prepare Pd clusters (∼1.3 nm) regioselectively encapsulated in hollow polycrystalline shell of Silicalite-1 zeolite. In nitrobenzene hydrogenation reaction, the optimized Pd@S-1-hp showed a high conversion of 92.2 % at 110 °C, which is 40 % higher than that of Pd clusters in bulk zeolite. Sub-nano Pd species in polycrystalline shell could significantly shorten the diffusion length on the basis of strong microporous confinement effect. Catalytic hydrogenation activity remained stable after six cycles. This structure could be extended to heterogeneous reactions suffering from diffusion limitation.

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在空心多晶壳中对钯团簇进行区域选择性封装

沸石催化剂已广泛应用于石油和化学工业。纳米/层状结构可提高活性位点的利用效率，尤其是对沸石中包覆的金属物种。然而，沸石表面的均匀性和结晶度会降低，导致稳定效果不佳。在此，我们开发了一种种子定向方法，制备出区域选择性封装在 Silicalite-1 沸石空心多晶壳中的 Pd 簇（∼1.3 nm）。在硝基苯加氢反应中，优化的 Pd@S-1-hp 在 110 ℃ 时的转化率高达 92.2%，比块状沸石中的 Pd 簇群高出 40%。基于强大的微孔约束效应，多晶壳中的亚纳米 Pd 物种可显著缩短扩散长度。催化加氢活性在六个循环后保持稳定。这种结构可以推广到受到扩散限制的异质反应中。

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来源期刊

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.