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Influence of Nanoscale Intimacy and Zeolite Micropore Size on the Performance of Bifunctional Catalysts for n-Heptane Hydroisomerization.

ABSTRACT: In this study, Pt nanoparticles on zeolite/?-Al₂O₃ composites (50/50 wt) were located either in the zeolite or on the ?-Al₂O₃ binder, hereby varying the average distance (intimacy) between zeolite acid sites and metal sites from "closest" to "nanoscale". The catalytic performance of these catalysts was compared to physical mixtures of zeolite and Pt/?-Al₂O₃ powders, which provide a "microscale" distance between sites. Several beneficial effects on catalytic activity and selectivity for n-heptane hydroisomerization were observed when Pt nanoparticles are located on the ?-Al₂O₃ binder in nanoscale proximity with zeolite acid sites, as opposed to Pt nanoparticles located inside zeolite crystals. On ZSM-5-based catalysts, mostly monobranched isomers were produced, and the isomer selectivity of these catalysts was almost unaffected with an intimacy ranging from closest to microscale, which can be attributed to the high diffusional barriers of branched isomers within ZSM-5 micropores. For composite catalysts based on large-pore zeolites (zeolite Beta and zeolite Y), the activity and selectivity benefitted from the nanoscale intimacy with Pt, compared to both the closest and microscale intimacies. Intracrystalline gradients of heptenes as reaction intermediates are likely contributors to differences in activity and selectivity. This paper aims to provide insights into the influence of the metal-acid intimacy in bifunctional catalysts based on zeolites with different framework topologies.

SUBMITTER: Oenema J

PROVIDER: S-EPMC7723304 | biostudies-literature | 2020 Dec

REPOSITORIES: biostudies-literature

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Influence of Nanoscale Intimacy and Zeolite Micropore Size on the Performance of Bifunctional Catalysts for n-Heptane Hydroisomerization.

Oenema Jogchum J Harmel Justine J Vélez Roxana Pérez RP Meijerink Mark J MJ Eijsvogel Willem W Poursaeidesfahani Ali A Vlugt Thijs J H TJH Zečević Jovana J de Jong Krijn P KP

ACS catalysis 20201121 23

In this study, Pt nanoparticles on zeolite/γ-Al2O3 composites (50/50 wt) were located either in the zeolite or on the γ-Al2O3 binder, hereby varying the average distance (intimacy) between zeolite acid sites and metal sites from "closest" to "nanoscale". The catalytic performance of these catalysts was compared to physical mixtures of zeolite and Pt/γ-Al2O3 powders, which provide a "microscale" distance between sites ...[more]

PMID: 33312750

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Project description:The preparation of zeolite-based bifunctional catalysts with low noble metal loadings while maintaining optimal performance has been studied. We have deposited 0.03 to 1.0 wt % Pt on zeolite H-USY (Si/Al ∼ 30 at./at.) using either platinum(II) tetraammine nitrate (PTA, Pt(NH3)4(NO3)2) or hexachloroplatinic(IV) acid (CPA, H2PtCl6·6H2O) and studied the nanoscale Pt loading heterogeneities and global hydroconversion performance of the resulting Pt/Y catalysts. Pt/Y samples prepared with PTA and a global Pt loading as low as 0.3 wt % Pt (n Pt/n A = 0.08 mol/mol, where nPt is the number of Pt surface sites and n A is the number of acid sites) maintained catalytic performance during n-heptane (T = 210-350 °C, P = 10 bar) as well as n-hexadecane (T = 170-280 °C, P = 5 bar) hydroisomerization similar to a 1.0 wt % Pt sample. For Pt/Y catalysts prepared with CPA, a loading of 0.3 wt % Pt (n Pt/n A = 0.08 mol/mol) sufficed for n-heptane hydroisomerization, whereas a detrimental effect on n-hexadecane hydroisomerization was observed, in particular undesired secondary cracking occurred to a significant extent. The differences between PTA and CPA are explained by differences in Pt loading per zeolite Y crystal (size ∼ 500 nm), shown from extensive transmission electron microscopy energy-dispersive X-ray spectroscopy experiments, whereby crystal-based n Pt/n A ratios could be determined. From earlier studies, it is known that the Al content per crystal of USY varied tremendously and that PTA preferentially is deposited on crystals with higher Al content due to ion-exchange with zeolite protons. Here, we show that this preferential deposition of PTA on Al-rich crystals led to a more constant value of n Pt/n A ratio from one zeolite crystal to another, which was beneficial for catalytic performance. Use of CPA led to a large variation of Pt loading independent of Al content, giving rise to larger variations of n Pt/n A ratio from crystal to crystal that negatively affected the catalytic performance. This study thus shows the impact of local metal loading variations at the zeolite crystal scale (nanoscale) caused by different interactions of metal precursors with the zeolite, which are essential to design and synthesize optimal catalysts, in particular at low noble metal loadings.

Dataset Information

Influence of Nanoscale Intimacy and Zeolite Micropore Size on the Performance of Bifunctional Catalysts for n-Heptane Hydroisomerization.

Publications

Influence of Nanoscale Intimacy and Zeolite Micropore Size on the Performance of Bifunctional Catalysts for <i>n</i>-Heptane Hydroisomerization.

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