Design of PtZn nanoalloy catalysts for propane dehydrogenation through interface tailoring <i>via</i> atomic layer deposition

Ingale, Piyush; Knemeyer, Kristian; Preikschas, Phil; Ye, Mengyang; Geske, Michael; d’Alnoncourt, Raoul Naumann; Thomas, Arne; Rosowski, Frank

doi:10.1039/d0cy01528h

Cited by 48 publications

(47 citation statements)

References 56 publications

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“…Here, we assumed that when a lower-valent element with a higher reduction potential is used as a second metal, regular zeolite silanols can also be effective in promoting intermetallic alloy formation with Pt. We used mesoporous zeolite synthesized in a purely siliceous form as a support material and Zn as the second metal element, which has recently been reported as an effective second metal element to Pt in PDH reactions. ,− In accordance with our assumption, the PtZn species supported on the mesoporous zeolite were found to exist as finely dispersed Pt 1 Zn 1 intermetallic alloy nanoparticles, which exhibited outstanding PDH performance with high catalytic activity, selectivity, and durability. In comparison to the previously reported Pt-REE catalysts, the PtZn catalyst exhibited even higher durability, recording one of the highest among the previously reported PDH catalysts.…”

Section: Introductionmentioning

confidence: 64%

“…Under the same reaction condition, the 1 wt % Pt supported on mesoporous zeolite catalyst (hereafter denoted as “1Pt/MZ”) also showed a relatively high initial propane conversion of 28%, but the catalyst immediately deactivated to reach half conversion within only half a day. This agrees well with previous reports claiming that the addition of Zn to Pt can effectively boost the propane conversion as well as slow down the catalyst deactivation. − , Moreover, the effect of excessive Zn species has been investigated by examining the PDH performance of the 1 wt % Zn supported on mesoporous zeolite catalyst (hereafter denoted as “1Zn/MZ”) as shown in Figure S6. The 1Zn/MZ catalyst exhibited a propane conversion of 4%, which also includes contributions from the cracking reactions occurring on the zeolite surface and at the void space of the reactor.…”

Section: Resultsmentioning

confidence: 99%

“…This agrees well with previous reports claiming that the addition of Zn to Pt can effectively boost the propane conversion as well as slow down the catalyst deactivation. [22][23][24]31 Moreover, the effect of excessive Zn species has been investigated by examining the PDH performance of the 1 wt % Zn supported on mesoporous zeolite catalyst (hereafter denoted as "1Zn/MZ") as shown in Figure S6. The 1Zn/MZ catalyst exhibited a propane conversion of 4%, which also includes contributions from the cracking reactions occurring on the zeolite surface and at the void space of the reactor.…”

Section: Resultsmentioning

confidence: 99%

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PtZn Intermetallic Compound Nanoparticles in Mesoporous Zeolite Exhibiting High Catalyst Durability for Propane Dehydrogenation

et al. 2021

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A PtZn alloy nanoparticle catalyst for propane dehydrogenation was synthesized by simple coimpregnation of Pt(NH3)4(NO3)2 with Zn(NO3)2 onto a mesoporous material, which was built with siliceous MFI zeolite nanosheets. This mesoporous zeolite-supported PtZn catalyst exhibited high activity and selectivity with remarkably long catalytic lifetime compared with other PtZn catalysts loaded on γ-alumina, MCM-48 mesoporous silica, silica gel, and bulk MFI zeolite. When measured under a high-purity propane flow at 580 °C, the PtZn/mesoporous zeolite catalyst with metal loadings of 0.7 wt % Pt and 0.7 wt % Zn lasted for more than 20 days before the propane conversion decreased to half of its initial value. In comparison, other PtZn catalysts were deactivated almost completely within a few days. Atomic-resolution scanning transmission electron microscopic analysis revealed that the mesoporous zeolite contained finely dispersed Pt1Zn1 intermetallic compound-type alloy nanoparticles, which could effectively suppress catalyst deactivation. The mesoporous structure and the surface silanol groups of the MFI zeolite are suggested to play an important role in promoting the formation of intermetallic alloy nanoparticles.

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Section: Introductionmentioning

confidence: 64%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

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PtZn Intermetallic Compound Nanoparticles in Mesoporous Zeolite Exhibiting High Catalyst Durability for Propane Dehydrogenation

et al. 2021

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“…Atomic layer deposition (ALD) has been used to tailor the interface between Pt nanoparticles and the SiO 2 support [45]; the SiO 2 surface was modified by homogeneous deposition of a thin ZnO layer, and the resulting support was impregnated with platinum precursor. Reductive thermal treatment gave rise to a phase transformation to form Pt1Zn1 alloy nanoparticles.…”

Section: Bimetallic and Promoted Catalystsmentioning

confidence: 99%

Propylene Synthesis: Recent Advances in the Use of Pt-Based Catalysts for Propane Dehydrogenation Reaction

et al. 2021

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Propylene is one of the most important feedstocks in the chemical industry, as it is used in the production of widely diffused materials such as polypropylene. Conventionally, propylene is obtained by cracking petroleum-derived naphtha and is a by-product of ethylene production. To ensure adequate propylene production, an alternative is needed, and propane dehydrogenation is considered the most interesting process. In literature, the catalysts that have shown the best performance in the dehydrogenation reaction are Cr-based and Pt-based. Chromium has the non-negligible disadvantage of toxicity; on the other hand, platinum shows several advantages, such as a higher reaction rate and stability. This review article summarizes the latest published results on the use of platinum-based catalysts for the propane dehydrogenation reaction. The manuscript is based on relevant articles from the past three years and mainly focuses on how both promoters and supports may affect the catalytic activity. The published results clearly show the crucial importance of the choice of the support, as not only the use of promoters but also the use of supports with tuned acid/base properties and particular shape can suppress the formation of coke and prevent the deep dehydrogenation of propylene.

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“…The low reaction selectivity using monometallic Pt/C, Pd/C, and bimetallic Au–Pt, Au–Pd can be greatly enhanced when the Au nanoparticles are supported on TiO 2 or Fe 2 O 3 , mainly because the supports show high selective adsorption over the −NO 2 group. , Clearly, the adsorption modes and selective adsorption of the −NO 2 group greatly determine the selectivity of the hydrogenation for the functionalized nitroarene. Following this idea, many strategies, including the design of bimetallic catalysts such as Pt–Zn intermetallic nanoparticles, have been carried out to alter the electronic properties of the surfaces in order to obtain proper surface acidity/basicity for the potential catalysts. ,− …”

Section: Introductionmentioning

confidence: 99%

Mechanism of Selective Hydrogenation of 4-Nitrophenylacetylene Using Pt–Zn Intermetallic Nanoparticles: The Role of Hydrogen Coverage

et al. 2021

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Selective hydrogenation of the nitroaromatics containing other reducible functional groups is very important, but the mechanism still remains controversial. Inspired by recent work on the excellent transformation of 4nitrophenylacetylene into 4-aminophenylacetylene using the Pt−Zn intermetallic nanoparticles as catalysts (Nat. Commun. 2019, 10, 3787), theoretical investigations have been performed to unravel the mechanism. Both the positive Zn species and the moderate hydrogen coverage were found to profoundly affect the adsorption structures and the bonding strength of the functional groups, thus dramatically affecting the adsorption selectivity. In contrast to the bare surface that the hydrogenation of the −CC group competes with the −NO 2 group, the overall barrier for the hydrogenation of the −NO 2 group on the 12H−PtZn (022̅ ) model is 0.90 eV, much lower than those of the −CC group for various intermediates by at least 0.28 eV, well explaining the experimental observation of the very high selectivity and conversion. The computational results strongly support that the pre-adsorbed hydrogen greatly changes the adsorption modes of the reactants and alters the reaction mechanism and, therefore, should be carefully evaluated for the hydrogenation of nitroaromatics on metal surfaces.

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Design of PtZn nanoalloy catalysts for propane dehydrogenation through interface tailoring via atomic layer deposition

Abstract: Supported Pt nanoparticles are widely used for the catalytic dehydrogenation of propane to propylene. However, Pt nanoparticles suffer from strong deactivation under dehydrogenation conditions. In this study, we present a...

Cited by 48 publications

References 56 publications

PtZn Intermetallic Compound Nanoparticles in Mesoporous Zeolite Exhibiting High Catalyst Durability for Propane Dehydrogenation

PtZn Intermetallic Compound Nanoparticles in Mesoporous Zeolite Exhibiting High Catalyst Durability for Propane Dehydrogenation

Propylene Synthesis: Recent Advances in the Use of Pt-Based Catalysts for Propane Dehydrogenation Reaction

Mechanism of Selective Hydrogenation of 4-Nitrophenylacetylene Using Pt–Zn Intermetallic Nanoparticles: The Role of Hydrogen Coverage

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