Tuning metal encapsulation in zeolites: Impact of crystal downsizing on liquid-phase hydrogenation reactions

IF 14.2
Green Carbon Pub Date : 2026-06-01 Epub Date: 2026-03-14 DOI:10.1016/j.greenca.2025.11.007
Adrián Martínez Gómez-Aldaraví, Francisco Javier Escobar-Bedia, Raquel Simancas, Toru Wakihara, Cristina Martínez, Manuel Moliner
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Abstract

Pt- and Pd-encapsulated pure-silica MFI zeolites with tunable crystal sizes (80–350 nm) were synthesized by controlling the hydrothermal process temperature (80–175 °C). This approach enabled the systematic modulation of the textural and diffusional properties of the resulting materials. Comprehensive characterization confirmed the encapsulation of metals within the zeolite frameworks of varying crystal sizes. The impact of crystal size on catalytic behavior was evaluated through the selective liquid-phase hydrogenation of phenylacetylene, using it as a model reaction to assess diffusion constraints. Pd-MFI with smaller crystals exhibited markedly higher activity and selectivity toward styrene compared with its larger-crystal counterparts, underscoring the critical role of tailored textural and diffusional properties in catalyst design. However, nanocrystalline materials with larger external surfaces underwent partial metal sintering under liquid-phase conditions. Strategies to mitigate sintering, such as controlling structural defects or applying protective surface coatings, are essential for further improvements.
调整沸石中的金属包封:晶体缩小对液相氢化反应的影响
通过控制水热温度(80 ~ 175℃),合成了晶粒尺寸可调(80 ~ 350 nm)的Pt和pd包封纯二氧化硅MFI分子筛。这种方法能够系统地调制所得到的材料的纹理和扩散特性。综合表征证实了金属在不同晶体尺寸的沸石框架内的封装。通过苯乙炔的选择性液相加氢反应来评估晶体尺寸对催化行为的影响,并将其作为模型反应来评估扩散约束。与具有较大晶体的Pd-MFI相比,具有较小晶体的Pd-MFI对苯乙烯表现出明显更高的活性和选择性,强调了定制结构和扩散特性在催化剂设计中的关键作用。然而,具有较大外表面的纳米晶材料在液相条件下进行了部分金属烧结。减轻烧结的策略,如控制结构缺陷或应用保护性表面涂层,对进一步改进是必不可少的。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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