Synthesis of a hybrid Pd0/Pd-carbide/carbon catalyst material with high selectivity for hydrogenation reactions

García‐Ortiz, Andrea; Vidal, Juan D.; Iborra, Sara; Climent, María J.; Cored, Jorge; Ruano, Daniel; Pérez-Dieste, Virgínia; Concepción, Patricia; Corma, Avelino

doi:10.1016/j.jcat.2020.06.036

Cited by 25 publications

(9 citation statements)

References 45 publications

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“…Although it is difficult to know the exact nature of the carbon Except for H2-C2H2-C2H4, the permeable carbon layer also formed from H2-C2H2 mixtures but not from H2-C2H4 in the absence of acetylene since the hydrogenation of C2H4 molecules need to be suppressed in the reaction of selective hydrogenation of C2H2 to C2H4. Also, based on existing reports 19,[23][24][25]29 , we believe that in situ adsorbate induction method can be extended to the other generally adopted active metal such as Ni, Co Rh, Ru, Pt, PtGa, NiZn, PdGa as the ideal candidates, which locally modifies the reactivity of the underlying metal nanoparticle surface. This further research and discussion on the properties of carbon layer derived by different treatment gases and the extension of this methodology to other metals will be performed in the future work.…”

Section: Discussionmentioning

confidence: 92%

“…This interpretation has become less popular in recent years as our understanding of how a Pd-carbide phase can form under operational conditions has been improved. Numerous studies (both experimental and theoretical in nature) , have shown that this metastable Pd-carbide phase may influence selectivity, which has led to a more contemporary belief that the interplay between Pd-hydride and carbide phases holds the key to controlling product distribution. Meanwhile, the spectator surface carbon species can also be employed to decorate/tune reaction behavior by modifying electronic and geometric structures .…”

Section: Introductionmentioning

confidence: 99%

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Adsorbate-Induced Structural Evolution of Pd Catalyst for Selective Hydrogenation of Acetylene

Liu

McCue

et al. 2020

ACS Catal.

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This work describes the transformation of Pd species under reaction condition to control the reactivity of heterogeneous catalysts, in which the real active sites for hydrogenation differ from simple Pd sites on a carbon nanofiber. Specifically, in the presence of C2H2/C2H4/H2 reaction mixtures, a permeable amorphous hydrocarbon overlayer is formed with simultaneous insertion of carbon atoms into Pd lattice that drives the formation of low coordinated Pd-carbide, thus providing more reactive Pd-Csub@Clayer sites (Csub: subsurface carbon; Clayer: carbon layer on the surface). The combination of these surface and subsurface effects hinders Pd-hydride, weakens ethylene adsorption confirmed by density functional theory (DFT) calculation, and thus improve catalytic behaviour for selective hydrogenation of acetylene (93% ethylene selectivity @ 100% conversion) with long-term stability. In the absence of hydrogen, a denser more crystalline overlayer is formed with severely restricted permeability, resulting in significantly lower activity. Moreover, by X-ray absorption 2 spectroscopy (XAS) and in-situ X-ray diffraction (XRD), it is demonstrated that different active sites dominate this catalytic reaction depending on choice of adsorbate and exposure temperature. This work represents an alternative and arguably simpler manner to design more reactive catalytic sites with the characteristics of long-term stability and facile preparation which would enable promising industrial application.

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Section: Discussionmentioning

confidence: 92%

Section: Introductionmentioning

confidence: 99%

Adsorbate-Induced Structural Evolution of Pd Catalyst for Selective Hydrogenation of Acetylene

Liu

McCue

et al. 2020

ACS Catal.

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“…On the other hand, our group has promoted a selective and active catalytic system for the onepot cascade type reactions, which avoids the isolation and purification of intermediates. 32 For instance, the reductive amination of carbonyl groups with a primary amine using Pd/C [33][34][35][36] offers a direct and selective way to secondary amines. Thus, recently, the development of efficient and selective methods through transition metal-catalyzed reductive amination has been actively explored.…”

Section: Scheme 1 Hydrogenation Of Nitroarenes Over Cobalt-based Hete...mentioning

confidence: 99%

Cobalt nanoclusters coated with N-doped carbon for chemoselective nitroarene hydrogenation and tandem reactions in water

et al. 2021

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“…through the Boudouard reaction and restored by CH4 through its dissociation. The present idea for the control of interstitial carbon atoms can be extended to incorporating other atoms, which shall further pave the way for other reforming reactions, such as steam reforming and partial oxidation as well as selective hydrogenation reactions [28,29] .…”

Section: Discussionmentioning

confidence: 99%

Reaction-induced Ni-based interstitial carbon atoms for coke-free dry reforming of methane

Wang¹,

Wu²,

Li³

et al. 2021

Preprint

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Dry reforming of methane on Ni-based catalyst offers an environmentally and economically viable and pivotal route to produce synthesis gas. The accumulation and polymerization of carbon atoms on the surface of Ni eventually deactivate the catalyst because of coke deposition. Here, we establish a reaction-induced method to isolate carbon atoms into the interstitial position of nickel octahedral sites (O-sites) under reaction condition, which can avoid the C−C bond formation. Al2O3 encapsulated Ni3Zn provides expanded space volume of O-sites in nickel to accommodate carbon atoms, and the further transformation to Ni3ZnC0.7 with superstructure feature was achieved under CH4/CO2 reaction. Ni3ZnC0.7/Al2O3 exhibits excellent activity and stability below 600°C with variable CH4/CO2 ratio (1/4−2/1). These active carbon atoms can be replenished and cycled in Ni3ZnC0.7 interior structure rather than depositing as coke on the surface during the reaction as revealed by in situ experiments.

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Synthesis of a hybrid Pd0/Pd-carbide/carbon catalyst material with high selectivity for hydrogenation reactions

Cited by 25 publications

References 45 publications

Adsorbate-Induced Structural Evolution of Pd Catalyst for Selective Hydrogenation of Acetylene

Adsorbate-Induced Structural Evolution of Pd Catalyst for Selective Hydrogenation of Acetylene

Cobalt nanoclusters coated with N-doped carbon for chemoselective nitroarene hydrogenation and tandem reactions in water

Reaction-induced Ni-based interstitial carbon atoms for coke-free dry reforming of methane

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