Influence of support acidity on the performance of size-confined Pt nanoparticles in the chemoselective hydrogenation of acetophenone

Wang, Zichun; Kim, Kyungduk; Zhou, Chengxin; Chen, Mengmeng; Maeda, Nobutaka; Liu, Zongwen; Jun, Shi; Baiker, Alfons; Hunger, Michael; Huang, Jun

doi:10.1039/c5cy00214a

Cited by 30 publications

(35 citation statements)

References 78 publications

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“…γ-Al 2 O 3 was a typical Lewis acidic catalyst, [38] and thus, the peak at 205°C observed with Pd/Al 2 O 3 catalysts has been assigned to ammonia adsorbed on LAS on alumina support. [14] In this work, Pd particles exhibit similar electronic properties over support with different acidic properties as indicated by NH 3 -TPD. Often, the relative strength of the acid sites can be scaled by their Tm, for instance the higher Tm the higher acid strength.…”

Section: Resultsmentioning

confidence: 64%

“…These Pd particles can sustain their morphology even after loading on different support materials (Figure 1 and S3-4). [14] The weak diffraction peaks at 42°and 48°w ere assigned to Pd (111) and Pd (200) on Pd nanocatalysts, respectively. BET surface areas of Pd catalysts on different supports were determined by nitrogen adsorption-desorption isotherm and summarized in Table 1.…”

Section: Resultsmentioning

confidence: 99%

“…[33,36,37] Since the metal-support interaction induced by acidic support (e. g. alumina and silica-alumina) can strongly influence the catalytic performance of Pd catalysts, [3,9,19] the surface acidity of supported Pd catalysts are characterized by the temperature programmed desorption of ammonia (NH 3 -TPD) experiments. [1,9,14,19] Often, the surface electronic properties of the Pd nanoparticles can be determined by XPS. Broad strong peaks were observed for both Pd/ SA and Pd/Al 2 O 3 catalysts with desorption maximum peak (Tm) cantered at 240°C and 205°C, respectively, indicating a significant amount of acid sites generated on the supports.…”

Section: Resultsmentioning

confidence: 99%

“…[14,19] Moreover, it demonstrates that the various functional groups (neutral for Pd/SiO 2 , Lewis acid sites for Pd/ Al 2 O 3 and Brønsted acid sites for Pd/SA catalyst) and different densities/strengths of acid sites on the supports, cannot significantly influence the chemoselectivity of Pd catalysts in hydrogenation reaction. The performance of the obtained Pd catalysts was tested in the hydrogenation of acetophenone (Aph), benzaldehyde (BA) and butyrophenone (Bph), and the proposed reaction pathway are described in Scheme S1.…”

Section: Resultsmentioning

confidence: 99%

“…[9][10][11][12][13] The metal-support interaction can be generated through the acidic sites withdrawing electrons from the metal surface, which results in ionic effects and tunes the surface electronic properties of metal particles. [3,9,14] With increase the support acidity, the XPS binding energy and Fermi level of Pd supported on zeolite LTL increases, leading to increase the difference in energy between the PdÀ H antibonding orbital, which enhance the activity of Pd catalysts in neopentane hydrogenolysis reaction. [15] Moreover, extensive works focus on the preparation of Pd particle with uniform size to control their catalytic performance.…”

Section: Introductionmentioning

confidence: 99%

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The Comparative Effect of Particle Size and Support Acidity on Hydrogenation of Aromatic Ketones

et al. 2019

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A comparative study was reported for both the effects of shape-confined cubic Pd particle size (8, 13, and 21 nm) and surface property of most commonly used supports (SiO 2 , Al 2 O 3 , and silica-alumina) on catalytic performance in the chemoselective hydrogenation of three model bio-oil chemicals (benzaldehyde, acetophenone, and butyrophenone). The results showed that the size of Pd particles could be more associated with the hydrogenation reaction than acidities of the supports. Smaller size of Pd particles, regardless of the type of the support, provided the higher catalytic performance. XPS data showed that the electronic properties of Pd particles were similar, therefore, the possible reasons were the higher fraction of Pd atoms on corner in smaller particles, the lower accessibility of hydrogen atom to reactant on bigger particles, and the more low-coordinated sites in the small-size particles due to the short-range ordering. In addition, Pd/SA catalysts (Brønsted acid sites on the support) showed the highest conversion and TOF compared to Pd/Al 2 O 3 and Pd/SiO 2 catalysts. This might be due to the enhanced the diffusion rates of the chemicals on the surface of the catalysts although they could not induce the ionic effect from the metal surface. Pd/ SiO 2 catalysts performed better than Pd/Al 2 O 3 catalysts (Lewis acid sites on the support). The flexible SiOH groups on surface made the easy interaction with the metal particles and promote the reaction.[a] Dr.

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Section: Resultsmentioning

confidence: 64%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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The Comparative Effect of Particle Size and Support Acidity on Hydrogenation of Aromatic Ketones

et al. 2019

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Metal Nanoparticles Supported on Perfluorinated Superacid Polymers: A Family of Bifunctional Catalysts for the Selective, One‐Pot Conversion of Vegetable Substrates in Water

et al. 2017

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We describe the rational design of a new versatile family of bifunctional catalytic materials based on the combination of supported metal nanoparticles (Pd, Rh, Ru) and the superacid, perfluorinated Aquivion® PFSA polymer. The heterogeneous catalysts were tested in the multi‐step valorisation of representative plant derivatives to high‐added‐value chemicals. Particularly, the conversion of (+)‐citronellal to (‐)‐menthol and levulinic acid to γ‐valerolactone was achieved in one pot and in one stage in the water phase and shows full selectivity at a high conversion level under mild reaction conditions. The results are discussed in terms of the catalyst micro‐structure.

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Selective Hydrogenation of Aromatic Ketone over Pt@Y Zeolite through Restricted Adsorption Conformation of Reactants by Zeolitic Micropores

et al. 2020

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With thermodynamically favorable prevailing flat‐lying adsorption of aromatic ketone molecules on Pt/Y catalyst via π‐electron interaction, the 100 % selective hydrogenation toward aromatic alcohols is hardly achieved because of competitive hydrogenation on benzene rings. Here we developed a general method to prepare encapsulated Pt nanoparticles into Y Zeolite (Pt@Y), which provided a novel method to retard hydrogenation of benzene rings via thermodynamically unfavorable end‐on adsorption conformation for almost 100 % selectivity from aromatic ketones to aromatic alcohols even at conversion close to 100 %.

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Influence of support acidity on the performance of size-confined Pt nanoparticles in the chemoselective hydrogenation of acetophenone

Abstract: Chemoselectivity of hydrogenation depends on strength of the covered BAS, whereas the free BAS enhance the rate.

Cited by 30 publications

References 78 publications

The Comparative Effect of Particle Size and Support Acidity on Hydrogenation of Aromatic Ketones

The Comparative Effect of Particle Size and Support Acidity on Hydrogenation of Aromatic Ketones

Metal Nanoparticles Supported on Perfluorinated Superacid Polymers: A Family of Bifunctional Catalysts for the Selective, One‐Pot Conversion of Vegetable Substrates in Water

Selective Hydrogenation of Aromatic Ketone over Pt@Y Zeolite through Restricted Adsorption Conformation of Reactants by Zeolitic Micropores

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