Zinc Promotion of Platinum for Catalytic Light Alkane Dehydrogenation: Insights into Geometric and Electronic Effects

Cybulskis, Viktor J.; Bukowski, Brandon C.; Tseng, Han-Ting; Gallagher, James R.; Wu, Zhenwei; Wegener, Evan C.; Kropf, A. Jeremy; Ravel, Bruce; Ribeiro, Fabio H.; Greeley, Jeffrey; Miller, Jeffrey T.

doi:10.1021/acscatal.6b03603

Cited by 207 publications

(222 citation statements)

References 60 publications

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“…Upon formation of Pt 3 Fe, there is a small shift in the valence states, followed by a slightly larger shift in PtFe, and finally the largest change in PtFe 3 . The decrease in the energy of the filled Pt 5d orbitals in these PtFe IMC's, however, is significantly smaller than those for the Pt 1 Zn 1 . The DFT RIXS planes calculated from the projected DOS of Pt show a similar trend to the experimental results.…”

Section: Resultssupporting

confidence: 64%

Intermetallic Compounds as an Alternative to Single‐atom Alloy Catalysts: Geometric and Electronic Structures from Advanced X‐ray Spectroscopies and Computational Studies

et al. 2020

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Pt−Fe intermetallic compound (IMC) catalysts, including Pt3Fe, PtFe and PtFe3, are shown to have advantageous catalytic properties similar to those reported for single‐atom alloy catalysts. Suppresion of the Pt ensembles responsible for hydrogenolysis results in high olefin selectivity during propane dehydrogenation. In situ resonant inelastic X‐ray scattering (RIXS) results and density functional theory calculations show that these changes are associated with a decrease in the average energy of the filled 5d states of Pt in the Pt−Fe intermetallic compound structures compared to monometallic Pt, accompanied by an increase in the average energy of the unfilled valence bands. The decrease in energy of the filled Pt 5d orbitals increases with increasing Fe content in the IMC, i.e. PtFe3>PtFe>Pt3Fe. These results demonstrate that by altering the stoichiometry of IMC catalysts it is possible to control both the ensemble size and electronic properties of active sites, which affords another mechanism for tuning catalytic properties, in addition to changing promoter metals. The present study demonstrates the potential of ordered intermetallic compounds as an alternative to traditional solid‐solution single‐atom alloys to serve as catalysts with well‐defined and uniform active sites.

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Section: Resultssupporting

confidence: 64%

Intermetallic Compounds as an Alternative to Single‐atom Alloy Catalysts: Geometric and Electronic Structures from Advanced X‐ray Spectroscopies and Computational Studies

et al. 2020

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“…For catalytic dehydrogenation, the ethane is assumed to be converted to ethylene with 100% selectivity and the conversion of ethane is 45% according to reported experimental results; for steam cracking, the conversion of ethane is 67% and selectivity towards ethylene is 81% [20,28]. The catalytic dehydrogenation reactor and steam cracker are both operated at 900 K and 3.5 bar.…”

Section: Thermodynamic Analysis Of the Ngl-to-liquid Pathwaysmentioning

confidence: 99%

“…Using PtSn/Al 2 O 3 catalyst, propane is dehydrogenated at 1.4 barg and 873 K. The dehydrogenation of ethane is usually achieved through steam cracking [26]. Ethane conversion of 45% with selectivity of 99% toward ethylene has been reported at 873 K using PtZn/SiO 2 catalyst [20].…”

Section: Dehydrogenationmentioning

confidence: 99%

“…Some retained hydrogen in the retenate stream is desirable to ensure the stability of the dehydrogenation and oligomerization catalyst [20]. In Aspen Plus, the membrane was simulated using a separator and calculator block.…”

Section: Hydrogen Recoverymentioning

confidence: 99%

“…The catalytic dehydrogenation of light alkanes has been widely studied as an alternative process for producing olefins [19][20][21][22][23][24][25]. However, for olefins production, there are only a few reports on process synthesis and design for the production of olefins through the oxidative and non-oxidative catalytic dehydrogenation of light alkanes [22,24,25].…”

Section: Introductionmentioning

confidence: 99%

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Valorization of Shale Gas Condensate to Liquid Hydrocarbons through Catalytic Dehydrogenation and Oligomerization

Ridha

Gençer

et al. 2018

Processes

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Abstract:The recent shale gas boom has transformed the energy landscape of the United States. Compared to natural gas, shale resources contain a substantial amount of condensate and natural gas liquids (NGLs). Many shale basin regions located in remote areas are lacking the infrastructure to distribute the extracted NGLs to other regions-particularly the Gulf Coast, a major gas processing region. Here we present a shale gas transformation process that converts NGLs in shale resources into liquid hydrocarbons, which are easier to transport from these remote basins than NGL or its constituents. This process involves catalytic dehydrogenation followed by catalytic oligomerization. Thermodynamic process analysis shows that this process has the potential to be more energy efficient than existing NGL-to-liquid fuel (NTL) technologies. In addition, our estimated payback period for this process is within the average lifetime of shale gas wells. The proposed process holds the promise to be an energy efficient and economically attractive step to valorize condensate in remote shale basins.

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PtZn intermetallic nanoalloy encapsulated in silicalite‐1 for propane dehydrogenation

Zhang

Zhai

et al. 2021

AIChE Journal

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Propane dehydrogenation (PDH) is one of the most effective methods to produce propylene. But the industrial Pt‐based catalysts often suffer from short‐term stability under the high temperature reaction environment (500–700°C) via sintering and coke deposition. Herein, stable PDH reaction in high propylene yield has been achieved by the confinement of Pt–Zn intermetallic alloys (IMAs) in the channels of silicalite‐1. Single‐site Zn in the MFI framework was found to play a key role on assisting and stabilizing the PtZn IMAs for efficient PDH. By the cooperative action of the spatial confined PtZn IMAs and the lattice confined framework Zn, high propylene selectivity (>99%) without obvious deactivation was realized on the as‐developed catalyst (PtZn@S‐1) under 600°C even after 90 h. The low deactivation constant (0.003 h−1) was 6 times lower than that of the industrial PtSn catalyst.

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Zinc Promotion of Platinum for Catalytic Light Alkane Dehydrogenation: Insights into Geometric and Electronic Effects

Cited by 207 publications

References 60 publications

Intermetallic Compounds as an Alternative to Single‐atom Alloy Catalysts: Geometric and Electronic Structures from Advanced X‐ray Spectroscopies and Computational Studies

Intermetallic Compounds as an Alternative to Single‐atom Alloy Catalysts: Geometric and Electronic Structures from Advanced X‐ray Spectroscopies and Computational Studies

Valorization of Shale Gas Condensate to Liquid Hydrocarbons through Catalytic Dehydrogenation and Oligomerization

PtZn intermetallic nanoalloy encapsulated in silicalite‐1 for propane dehydrogenation

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