Wettability-Driven Palladium Catalysis for Enhanced Dehydrogenative Coupling of Organosilanes

Lin, Jiandong; Bi, Qingyuan; Tao, Lei; Jiang, Tongying; Liu, Yongmei; He, Heyong; Cao, Yong; Wang, Yangdong

doi:10.1021/acscatal.6b03233

Cited by 48 publications

(25 citation statements)

References 83 publications

(24 reference statements)

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“…More and more reports exhibited that the activity could be enhanced after hydrophobicity modification when nonpolar or low polar molecules were used as substrate in the reaction. [25][26][27][28][29][30][31][32][33][34][35][36][37] The reason was simply ascribed to the accumulation of more hydrophobic substrates on the hydrophobic surface during reactions. However, the precise and deep mechanism for this widespread improvement in catalytic activity had very little reports.…”

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confidence: 99%

Fabrication of Pd/SiO₂ with Controllable Wettability for Enhanced Catalytic Hydrogenation Activity at Ambient H₂ Pressure

et al. 2019

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The wettability had great influence on the catalytic performance of heterogeneous catalyst. In this manuscript, relationship between wettability and catalytic performance was studied by the preparation of Pd/SiO2 with controllable wettability employing surface‐bonded vinyl as the reductant. The surface‐bonded vinyl ensured the reduction of PdCl2 on the hydrophobic surface of SiO2 to afford the hydrophobic Pd/SiO2. The wettability of the catalysts could be adjusted by changing the content of phenyl on the surface. The catalysts were characterized by solid‐state CP/MAS NMR, TEM, HRTEM, XPS, XRD and ICP‐AES as well as water droplet contact angles. The catalysts showed zero‐order kinetics for the hydrogenation of styrene under mild conditions. The activation energy for this reaction was measured by the Arrhenius formula. The wettability was proved to influence the reaction activity by changing the activation energy. The increase in hydrophobicity led to higher activity by decreasing the activation energy for hydrogenation of styrene to ethylbenzene.

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confidence: 99%

Fabrication of Pd/SiO₂ with Controllable Wettability for Enhanced Catalytic Hydrogenation Activity at Ambient H₂ Pressure

et al. 2019

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“…This as‐synthesized PtPd/C sample shows high efficiency for oxygen reduction reaction (ORR) . Similarly, the underlying supports modified with the hydrophobic characteristics could boost the efficiency of Pd NPs catalysed dehydrogenative coupling of organosilanes . For another case, in the molten carbonate fuel cell, the support materials are always designed to have low wettability (considered as a generalised hydrophobic) to prevent the reforming catalyst from poisoning, and the catalyst can act as its maximum effects on the catalysis .…”

Section: The Effect Of Wettability On the Catalytic Performancementioning

confidence: 99%

The Effect of Surface Wettability and Coalescence Dynamics in Catalytic Performance and Catalyst Preparation: A Review

Wang

et al. 2019

ChemCatChem

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The interactions between the reactants and catalysts surfaces play a significant role in heterogeneous catalysis, thus to tune the interfacial properties between them has emerged as an important topic. This review has summarised some recent advances about the effects of wettability on the catalytic reactions, including hydrophilicity, hydrophobicity, and dewetting properties. In addition, the effect of coalescence dynamics among the catalyst particles is also discussed based on a series of investigations. Although the researchers have realised the importance of wettability, the ability to tune the wettability in their work needs to be further enhanced. Therefore, we finally highlighted considerable useful approaches to achieve controllable wettability and coalescence. It is expected that in the future design of catalysts, researchers should pay more attention to tuning the interfacial structure to achieve the enhanced catalysts behaviours.[a] T.

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“…In addition, the strategy for adjusting catalyst wettability is extended to prepare supported metal nanoparticle catalysts and metal-organic frameworks (MOFs) [28][29][30][31]. Cao and co-workers [28] developed hydrophobic carbon supported Pd nanoparticles, showing higher activities for the dehydrogenative coupling of organosilanes with alcohols and amines than those of the existing catalysts.…”

Section: Enrichment Of Reactants For Increasing Catalytic Activitymentioning

confidence: 99%

“…Cao and co-workers [28] developed hydrophobic carbon supported Pd nanoparticles, showing higher activities for the dehydrogenative coupling of organosilanes with alcohols and amines than those of the existing catalysts. Jiang and co-workers [29] developed a polydimethylsiloxane coating for a Pd/MOF composite, realizing significantly enhanced catalytic performance in nitroarene hydrogenation by enriching the molecules.…”

Section: Enrichment Of Reactants For Increasing Catalytic Activitymentioning

confidence: 99%

A significant enhancement of catalytic performance by adjusting catalyst wettability

Wang

Xiao

2018

Sci. China Mater.

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Heterogeneous catalysts have played a crucial role in upgrading fuels, transforming biomass [1][2][3], removing pollutants [4][5][6], harvesting solar energy [7][8][9], and producing fine chemicals [10,11]. Compared with homogeneous catalysts, the heterogeneous catalysts have obvious advantages in easy separation and regeneration from the reaction systems [12][13][14][15], but still have unsatisfactory activity and/or selectivity. These issues are reasonably assigned to the limited molecular diffusion on the heterogeneous catalysts. Therefore, it is in great demand to improve the catalytic performances of these catalysts by increasing mass transfer in the reactions, which is always a challenge in the heterogeneous catalysis.For a general reaction from A and B reactants to C and D products, the rate of a chemical reaction is sensitive to the concentration of the reactants and products, as shown in Equation (1) Therefore, it is reasonable to improve the reaction rate by increasing the concentration of reactants and reducing the concentration of products close to the active centers. Normally, a heterogeneous catalysis [16] mainly includes the adsorption of reactant, reactant transfer on the catalyst surface, reactant conversion from reactants to products, product transfer on the catalyst surface, and desorption of products, as presented in Scheme 1. In these steps, four steps are related to the molecular diffusion in the reaction.It is well known that the molecular diffusion is strongly influenced by catalyst wettability. The recent results have demonstrated that the adjustment of catalyst wettability would lead to (i) enrichment of the reactants for accelerating the reaction, (ii) fast diffusion of the products for shifting the reaction balance, (iii) formation of new reaction intermediates, (iv) isolation of undesired molecules for hindering the side reactions, and (v) stabilization of the catalyst structure. Enrichment of reactants for increasing catalytic activityAs illustrated in Equation (1), enhancement of reactant concentration should effectively increase the reaction rate. In the beginning, it was focused on the zeolite catalysts. One typical example is the industrial TS-1 zeolite with hydrophobic framework, which is not favorable for adsorption of H 2 O 2 in the oxidations of organic compounds with H 2 O 2 because the H 2 O 2 is polar and hydrophilic [17][18][19][20]. Obviously, the TS-1 zeolite with more hydrophilicity might be helpful to enrich the H 2 O 2 , leading to improvement of the catalytic activities. As expected, Wang et al. [21] synthesized hydrophilic TS-1 zeolite by employing organosilicon as precursor, followed by calcination to transform the organic groups into silanol groups. The TS-1 zeolite with more hydrophilic silanol groups exhibits much higher reaction rate (4.9 mmol L −1 min) in the oxidation of 1-hexene with H 2 O 2 , because the hydrophilic zeolite can effectively enrich the concentration of H 2 O 2 reactant in the zeolite micropores, as confirmed by the molecule adsorption and...

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Wettability-Driven Palladium Catalysis for Enhanced Dehydrogenative Coupling of Organosilanes

Cited by 48 publications

References 83 publications

Fabrication of Pd/SiO₂ with Controllable Wettability for Enhanced Catalytic Hydrogenation Activity at Ambient H₂ Pressure

Fabrication of Pd/SiO₂ with Controllable Wettability for Enhanced Catalytic Hydrogenation Activity at Ambient H₂ Pressure

The Effect of Surface Wettability and Coalescence Dynamics in Catalytic Performance and Catalyst Preparation: A Review

A significant enhancement of catalytic performance by adjusting catalyst wettability

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Wettability-Driven Palladium Catalysis for Enhanced Dehydrogenative Coupling of Organosilanes

Cited by 48 publications

References 83 publications

Fabrication of Pd/SiO2 with Controllable Wettability for Enhanced Catalytic Hydrogenation Activity at Ambient H2 Pressure

Fabrication of Pd/SiO2 with Controllable Wettability for Enhanced Catalytic Hydrogenation Activity at Ambient H2 Pressure

The Effect of Surface Wettability and Coalescence Dynamics in Catalytic Performance and Catalyst Preparation: A Review

A significant enhancement of catalytic performance by adjusting catalyst wettability

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Fabrication of Pd/SiO₂ with Controllable Wettability for Enhanced Catalytic Hydrogenation Activity at Ambient H₂ Pressure

Fabrication of Pd/SiO₂ with Controllable Wettability for Enhanced Catalytic Hydrogenation Activity at Ambient H₂ Pressure