Promotion of Pd nanoparticles by Fe and formation of a Pd3Fe intermetallic alloy for propane dehydrogenation

Yang, Ce; Wu, Zhenwei; Zhang, Guanghui; Sheng, Huaping; Tian, Jun; Duan, Zhengli; Sohn, Hyuntae; Kropf, A. Jeremy; Wu, Tianpin; Krause, Theodore; Miller, Jeffrey T.

doi:10.1016/j.cattod.2018.07.043

Cited by 47 publications

(35 citation statements)

References 39 publications

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“…Further evidence for that can be found by comparison of the reduced 0.1 %Pd-ZnO-ZrO 2 catalyst with aPd-SiO 2 standard;the edge is shifted by about 0.7 eV,consistent with alloying. [18] Moreover,there is afeature approximately 15 eV above the edge position similar to that reported by Te we tal. for the bonding of Pd and H; [19] this suggests bonding between Pd and ah eteroatom, in this case Zn, with the shift corresponding to charge transfer of the Pd-Zn alloy.F urthermore,t he XANES spectra showed no changes under the presence of CO,i ndicating weak CO binding characteristics that differ from bulk Pd.…”

Section: Methodssupporting

confidence: 80%

Direct Catalytic Conversion of Ethanol to C₅₊ Ketones: Role of Pd–Zn Alloy on Catalytic Activity and Stability

et al. 2020

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Ethanol can be used as a platform molecule for synthesizing valuable chemicals and fuel precursors. Direct synthesis of C5+ ketones, building blocks for lubricants and hydrocarbon fuels, from ethanol was achieved over a stable Pd‐promoted ZnO‐ZrO2 catalyst. The sequence of reaction steps involved in the C5+ ketone formation from ethanol was determined. The key reaction steps were found to be the in situ generation of the acetone intermediate and the cross‐aldol condensation between the reaction intermediates acetaldehyde and acetone. The formation of a Pd–Zn alloy in situ was identified to be the critical factor in maintaining high yield to the C5+ ketones and the stability of the catalyst. A yield of >70 % to C5+ ketones was achieved over a 0.1 % Pd‐ZnO‐ZrO2 mixed oxide catalyst, and the catalyst was demonstrated to be stable beyond 2000 hours on stream without any catalyst deactivation.

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Section: Methodssupporting

confidence: 80%

Direct Catalytic Conversion of Ethanol to C₅₊ Ketones: Role of Pd–Zn Alloy on Catalytic Activity and Stability

et al. 2020

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“…The increased olefin selectivities observed for the PtÀ Fe catalysts are consistent with previously reported IMC alkane dehydrogenation catalysts. [43][44][45][46][47][48][49][50][51] It has been proposed that the increased olefin selectivity arises from the elimination of large active-metal ensembles by incorporation of the noncatalytic promoter metals into the active surface. Segregation of the active atoms reduces hydrogenolysis, which is thought to require ensemble active sites.…”

Section: Resultsmentioning

confidence: 99%

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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“…28 Nonetheless, a few recent reports have also shown that alloys of Pd can have dehydrogenation selectivities comparable to Pt alloys. 29,30 The ability of promoter metals to suppress hydrogenolysis in alloys in a way seemingly independent of the active metal's intrinsic hydrogenolysis activity motivates systematic study of alloy selectivity not only in Pt alloys, but also in other less selective metals such as Pd. This strategy should give insight into the salient features of alloying that lead to improved selectivity, independent of the behavior of the active metal, and ultimately open up a larger space of catalyst compositions and structures for use as dehydrogenation catalysts.…”

Section: Introductionmentioning

confidence: 99%

Structural trends in the dehydrogenation selectivity of palladium alloys

et al. 2020

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Promotion of Pd nanoparticles by Fe and formation of a Pd3Fe intermetallic alloy for propane dehydrogenation

Cited by 47 publications

References 39 publications

Direct Catalytic Conversion of Ethanol to C₅₊ Ketones: Role of Pd–Zn Alloy on Catalytic Activity and Stability

Direct Catalytic Conversion of Ethanol to C₅₊ Ketones: Role of Pd–Zn Alloy on Catalytic Activity and Stability

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

Structural trends in the dehydrogenation selectivity of palladium alloys

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Promotion of Pd nanoparticles by Fe and formation of a Pd3Fe intermetallic alloy for propane dehydrogenation

Cited by 47 publications

References 39 publications

Direct Catalytic Conversion of Ethanol to C5+ Ketones: Role of Pd–Zn Alloy on Catalytic Activity and Stability

Direct Catalytic Conversion of Ethanol to C5+ Ketones: Role of Pd–Zn Alloy on Catalytic Activity and Stability

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

Structural trends in the dehydrogenation selectivity of palladium alloys

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Direct Catalytic Conversion of Ethanol to C₅₊ Ketones: Role of Pd–Zn Alloy on Catalytic Activity and Stability

Direct Catalytic Conversion of Ethanol to C₅₊ Ketones: Role of Pd–Zn Alloy on Catalytic Activity and Stability