Control of the single atom/nanoparticle ratio in Pd/C catalysts to optimize the cooperative hydrogenation of alkenes

Rivera‐Cárcamo, Camila; Gerber, Iann C.; Rosal, Iker del; Guicheret, Boris; Contreras, Rosa; Vanoye, Laurent; Favre‐Réguillon, Alain; Machado, Bruno F.; Audevard, Jeremy; Bellefon, Claude de; Philippe, Régis; Serp, Philippe

doi:10.1039/d0cy01938k

Cited by 37 publications

(58 citation statements)

References 101 publications

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“…disappear almost completely upon catalyst preparation at 350 °C, and a Co(OOC-) interface is created for the four catalysts, associated to a narrow and intense peak characteristic of a catalytic decomposition between 427 and 448 °C, depending on the catalyst. This phenomenon has already been reported for Ru/CNT [55] and Pd/CNT [56] catalysts prepared on oxidized CNT.…”

Section: Effect Of Carbon Surface Chemistry On Catalyst Features and Hydrogen Spilloversupporting

confidence: 79%

Beyond confinement effects in Fischer-Tropsch Co/CNT catalysts

Ghogia

Machado

Cayez

et al. 2021

Journal of Catalysis

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Fischer-Tropsch catalyst preparation parameters, such as cobalt precursor and impregnation solvent, determine structure and in fine catalytic performances of Co-based catalysts. Co particles of 3-7 nm mean size were prepared by incipient wetness impregnation on surface-oxidized CNT. In this work the crucial impact of the chemistry operating between the Co precursor and the support during catalyst preparation on the catalyst properties is demonstrated and the influence of CNT surface chemistry on catalyst characteristics has been assessed. Very good correlations were found between: i) the reduction degree of the catalysts and the concentration of the Co(OOC-) surface species; ii) the Co hcp /Co fcc ratio and the amount of CO-releasing groups on the support surface; iii) the extent of hydrogen spillover and the concentration of quinone surface groups. The initial catalytic activity could only be correlated to a combination of catalyst features: percentage of Co hcp , Co confinement, hydrogen spillover, and surprisingly the inverse of the Co initial particle size. No significant differences in S C5+ selectivity were observed, in accordance with comparable final Co particle size. Finally, the stability of the catalyst can be correlated with the initial Co particle size and the percentage of Co hcp in the catalyst. These results confirm the significant impact of the precursor/support couple on the structure and performance of Co/CNT catalysts, and reveal for the first time an inverse correlation between Co particle size and activity, which is attributed to the confined Co hcp phase.

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Section: Effect Of Carbon Surface Chemistry On Catalyst Features and Hydrogen Spilloversupporting

confidence: 79%

Beyond confinement effects in Fischer-Tropsch Co/CNT catalysts

Ghogia

Machado

Cayez

et al. 2021

Journal of Catalysis

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“…To verify whether the ratio between Pd NP and Pd SA could also have an impact on 4-NP reduction, we prepared a series of Pd/O-CNT catalysts presenting similar Pd loading (1.2 % w/w) with different Pd SA /Pd NP ratio. [53] These catalysts present similar metal loadings (1.15 À 1.37 % w/w), Pd NP size ranging between 1 and 1.5 nm, and Pd SA /Pd NP ratio ranging between 3 and 60 (Figure S11). The catalytic performances for 4-NP reduction of this catalyst series is given on Table 3 and Figure 6.…”

Section: Chemcatchemmentioning

confidence: 92%

“…[52] Variation in the Pd ox /Pd (0) ratio could be associated to the presence in different proportion of Pd SA in addition to Pd NP . [46,53] Indeed, these Pd SA species, as well as Pd clusters of small nuclearity, are particularly sensitive to charge transfer. Thus, the higher Pd SA /Pd NP ratio measured for Pd/N-CNT could explain the fact that this catalyst is also the one that present the higher Pd ox /Pd (0) ratio and the stronger charge transfer, since SAs are more sensitive to charge transfer than metallic NPs.…”

Section: Materials Characterizationmentioning

confidence: 99%

“…[50] H-spillover could be operative on S-doped and O-doped CNTs, as recently reported for the Pd/O-CNT catalyzed hydrogenation of alkenes. [53] Another explanation of the difference of reactivity could arise from the presence of Pd SA in different proportion on the different supports. [77,78] Such species could be involved in 4-NP reduction, since it has been proposed that Pd SA are more active than Pd NP for 4-NP reduction with NaBH 4 .…”

Section: Chemcatchemmentioning

confidence: 99%

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Multifunctional Catalytic Properties of Pd/CNT Catalysts for 4‐Nitrophenol Reduction

et al. 2022

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Carbon nanotubes are arousing real interest in catalysis, either as catalyst support or as catalyst itself. In this work, the influence of CNT doping (O, N, S) on the catalytic performance of CNT and Pd/CNT catalysts have been investigated in the reduction of 4-nitrophenol both under H 2 or using NaBH 4 as a hydride source. The morphology, composition, particle size and crystallinity of the materials were investigated by various techniques including HRTEM, STEM, XPS, Raman spectroscopy and XRD. Among the CNT carbocatalysts, only N-CNT is active for 4-nitrophenol reduction at room temperature, and only in the presence of NaBH 4 . As far as supported Pd catalysts are concerned, the nature of the support influences the Pd nanoparticle location (confinement), the Pd nanoparticles/Pd single atoms ratio and the extent of H-spillover, three catalyst features that directly affect the catalytic activity. The best combination of Pd nanoparticles/Pd single atoms ratio, H-spillover and confinement for 4-nitrophenol reduction using NaBH 4 , is found in Pd/O-CNT catalysts, while for reactions performed under H 2 , Pd/N-CNT presents the best combination.

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“…The Pd/CNT (2% w/w) and Pd/FLG (2% w/w) catalysts were prepared according to this reference. 2 Characterization. IR spectra were recorded on a Perkin-Elmer 1710 Fourier Transform spectrophotometer on KBr solid pellet analysis.…”

Section: Methodsmentioning

confidence: 99%

Computational Design of Pd Nanoclusters and Pd Single-Atom Catalysts Supported on OFunctionalized Graphene

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Control of the single atom/nanoparticle ratio in Pd/C catalysts to optimize the cooperative hydrogenation of alkenes

Abstract: We recently reported (J. Catal., 2019, 372, 226-244) that a structure/activity correlation exists in Pd/C catalysts for myrcene hydrogenation, which integrates the Pd dispersion, and the surface concentration of oxygen...

Cited by 37 publications

References 101 publications

Beyond confinement effects in Fischer-Tropsch Co/CNT catalysts

Beyond confinement effects in Fischer-Tropsch Co/CNT catalysts

Multifunctional Catalytic Properties of Pd/CNT Catalysts for 4‐Nitrophenol Reduction

Computational Design of Pd Nanoclusters and Pd Single-Atom Catalysts Supported on OFunctionalized Graphene

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