Establishing hierarchy: the chain of events leading to the formation of silicalite-1 nanosheets

Zhu, Xiaochun; Goesten, Maarten G.; Koekkoek, Arjan J. J.; Mezari, Brahim; Kosinov, Nikolay; Filonenko, Georgy A.; Friedrich, Heiner; Rohling, Roderigh; Szyja, Bartłomiej M.; Gascón, Jorge; Kapteijn, Freek; Hensen, Emiel J. M.

doi:10.1039/c6sc01295g

Cited by 21 publications

(30 citation statements)

References 41 publications

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“…To prevent the metal aggregation, the introduction of a mesoporous system into the microporous zeolite network can greatly improve the dispersion of metal species due to a large increasing number of defect sites [33]. With the benefits of mesoporous or hierarchical structures [34,35], an improved catalytic efficiency has been observed in some reactions, in particular the processes involving bulky molecules, such as hydroisomerization, aromatization and hydrodesulfurization, as compared to a conventional zeolite [36][37][38][39][40].…”

Section: Introductionmentioning

confidence: 99%

Dehydrogenation of Propane to Propylene Using Promoter-Free Hierarchical Pt/Silicalite-1 Nanosheets

et al. 2019

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Propane dehydrogenation (PDH) is the extensive pathway to produce propylene, which is as a very important chemical building block for the chemical industry. Various catalysts have been developed to increase the propylene yield over recent decades; however, an active site of monometallic Pt nanoparticles prevents them from achieving this, due to the interferences of side-reactions. In this context, we describe the use of promoter-free hierarchical Pt/silicalite-1 nanosheets in the PDH application. The Pt dispersion on weakly acidic supports can be improved due to an increase in the metal-support interaction of ultra-small metal nanoparticles and silanol defect sites of hierarchical structures. This behavior leads to highly selective propylene production, with more than 95% of propylene selectivity, due to the complete suppression of the side catalytic cracking. Moreover, the oligomerization as a side reaction is prevented in the presence of hierarchical structures due to the shortening of the diffusion path length.

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Section: Introductionmentioning

confidence: 99%

Dehydrogenation of Propane to Propylene Using Promoter-Free Hierarchical Pt/Silicalite-1 Nanosheets

et al. 2019

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“…The appearance of the quasi-Bragg peak, around q = 1.6 nm −1 , is typical for an assembly of stacked sheets-a paracrystalline system. [26] The line shape of the quasi Bragg peak, deviates from a Gaussian profile. It is broad, and sharpens toward the top.…”

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confidence: 99%

Nanosheets of Nonlayered Aluminum Metal–Organic Frameworks through a Surfactant‐Assisted Method

et al. 2018

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During the last decade, the synthesis and application of metal-organic framework (MOF) nanosheets has received growing interest, showing unique performances for different technological applications. Despite the potential of this type of nanolamellar materials, the synthetic routes developed so far are restricted to MOFs possessing layered structures, limiting further development in this field. Here, a bottom-up surfactant-assisted synthetic approach is presented for the fabrication of nanosheets of various nonlayered MOFs, broadening the scope of MOF nanosheets application. Surfactant-assisted preorganization of the metallic precursor prior to MOF synthesis enables the manufacture of nonlayered Al-containing MOF lamellae. These MOF nanosheets are shown to exhibit a superior performance over other crystal morphologies for both chemical sensing and gas separation. As revealed by electron microscopy and diffraction, this superior performance arises from the shorter diffusion pathway in the MOF nanosheets, whose 1D channels are oriented along the shortest particle dimension.

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“… 151 , 152 The possibility to rationally design the amphiphilic mesoporogens was recently outlined by Zhu et al, who studied the early stages of MFI nanosheet synthesis by operando small-angle X-ray scattering, complementary characterization techniques, and molecular modeling. 153 The authors found that the meso-order is established at the very beginning of synthesis and that amphiphilic SDA stabilizes pre-zeolitic species via a molecular-recognition-type mechanism, followed by the micro-ordering into zeolite nanosheets. It was also shown that the rational fine-tuning of the ammonium headgroup allows synthesis of different zeolite topologies (namely, MFI and MEL) and aspect ratios (nanosheets or needles).…”

Section: Engineering Well-defined Zeolite Catalystsmentioning

confidence: 99%

Engineering of Transition Metal Catalysts Confined in Zeolites

et al. 2018

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Transition metal–zeolite composites are versatile catalytic materials for a wide range of industrial and lab-scale processes. Significant advances in fabrication and characterization of well-defined metal centers confined in zeolite matrixes have greatly expanded the library of available materials and, accordingly, their catalytic utility. In this review, we summarize recent developments in the field from the perspective of materials chemistry, focusing on synthesis, postsynthesis modification, (operando) spectroscopy characterization, and computational modeling of transition metal–zeolite catalysts.

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Establishing hierarchy: the chain of events leading to the formation of silicalite-1 nanosheets

Abstract: In applying a multi-scale spectroscopic and computational approach, we demonstrate that the synthesis of stacked zeolite silicalite-1 nanosheets, in the presence of a long-tail diquaternary ammonium salt surfactant, proceeds through a pre-organised phase in the condensed state.

Cited by 21 publications

References 41 publications

Dehydrogenation of Propane to Propylene Using Promoter-Free Hierarchical Pt/Silicalite-1 Nanosheets

Dehydrogenation of Propane to Propylene Using Promoter-Free Hierarchical Pt/Silicalite-1 Nanosheets

Nanosheets of Nonlayered Aluminum Metal–Organic Frameworks through a Surfactant‐Assisted Method

Engineering of Transition Metal Catalysts Confined in Zeolites

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