The development of safe and efficient H2 generation/storage materials toward a fuel-cell-based H2 economy as a long-term solution has recently received much attention.
Bimetallic AuPt nanoparticles with different Au:Pt ratios (molar ratio: 9-1, 8-2, 6-4, 2-8, 1-9) and the corresponding Au and Pt monometallic ones were prepared by sol immobilization and immobilized on commercial TiO 2 (P25). The catalytic activity was evaluated in the liquid phase glycerol oxidation in presence and absence of a base (NaOH). It was found that the Au:Pt molar ratio and reaction conditions strongly influence the catalytic performance. In the presence of NaOH, Au-rich catalysts were more active than Pt-rich ones, with the highest activity observed for Au 9 Pt 1 /TiO 2 (6575 h −1 ). In absence of a base, a higher content of Pt is needed to produce the most active catalyst (Au 6 Pt 4 /TiO 2 , 301 h −1 ). In terms of selectivity, in presence of NaOH, Au-rich catalysts showed a high selectivity to C3 products (63-72%) whereas Pt-rich catalysts promote the formation of formic and glycolic acids. The opposite trend was observed in absence of a base with Pt-rich catalysts showing higher selectivity to C3 products (83-88%).
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Phosphorylated carbons have been reported to be effective catalysts in dehydration reactions for biomass valorization. The amount and the nature of P groups are a key parameter affecting the catalytic performances of functionalized materials. Herein, we investigate the role of structural and surface properties of carbon-based materials, specifically carbon nanofibers, in determining the amount of P-functionalities. In order to incorporate P groups on carbon surfaces, various carbon nanofibers (CNFs) with different graphitization degrees have been functionalized through treatment with a H 3 PO 4 -HNO 3 mixture at 150 • C. The pristine materials, as well as the functionalization protocol, were properly selected to achieve an effective functionalization without drastically altering the morphology of the samples. Surface and structural properties of the synthesized functionalized materials have been investigated by means of transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy. The catalytic behavior of phosphorylated carbon nanofibers has been evaluated in the selective dehydration of fructose to hydroxymethylfurfural (HMF) to elucidate structure-activity relationships.
Herein, we reported the utilization of pre-formed Au–Pt nanoparticles deposited on phosphorus functionalized carbons as effective catalysts for the oxidation of 5-hydroxymethylfurfural (HMF) to furandicarboxylic acid (FDCA). Au–Pt nanoparticles have been prepared by a two-step methodology using polyvinyl alcohol (PVA) as protective agent and a combination of NaBH4 and H2 as reducing agents. Three carbon nanofibers (CNFs) with different graphitization degrees have been functionalized through treatment with an H3PO4–HNO3 mixture at 150 °C, in order to incorporate P groups on carbon surface. Surface and structural properties of the synthesized functionalized materials have been investigated by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy. The structural and surface properties of carbon nanofibers determine the amount of P-functionalities, which is a key parameter affecting the catalytic performances of Au–Pt. Indeed, the highest activity and stability has been achieved for Au–Pt deposited on the sample, which showed the largest amount of P-groups on the surface.
This paper studies the cooperative effect of Au nanoparticles deposited on vanadyl pyrophosphate oxide (VPO) in the liquid phase oxidation of benzyl alcohol. VPO was prepared using the classical method by thermally treating VOHPO4·0.5H2O precursor in reacting atmosphere at 420 °C for a period of 72 h. Au nanoparticles were deposited by incipient wetness method. The catalysts were characterized by means of XRD, TEM, XPS and Raman. The bulk VPO catalyst contains vanadyl pyrophosphate phase ((VO)2P2O7), and a small amount of VOPO4. The catalytic system exhibits a high activity in the base-free liquid phase oxidation of alcohols compared to Au on activated carbon, classic catalyst used for this type of reaction. Au/VPO showed a high peculiar selectivity to benzyl benzoate (76%), an important product used in the pharmaceutical and perfume industries. This behavior might be ascribed to the presence of strong acid sites of VPO, as determined by liquid phase titration. Stability tests performed on Au/VPO showed a deactivation of 10% after the first run, but a constant conversion along the following five cycles. This phenomenon can be attributed to the increase of mean Au particle size (from 19.1 to 23.4 nm) after recycling tests as well as the partial leaching of Au and V in the reaction media. Moreover, XRD evidenced a modification in the VPO structure with the partial formation of VOHPO4·0.5H2O phase.
The increasing demand of energy requires the development of sufficient and sustainable energy sources. However, the upcoming hydrogen economy is suffering from challenges which need to be solved. In this context, the search for liquid hydrogen storage materials and successful utilisation is crucial due to the high gravimetric and volumetric hydrogen densities, easy recharging, low capital investment, and low potential risks. In this review, we survey the progress made in hydrogen generation from carbon-based liquid-phase chemical hydrogen storage materials, focusing mainly on the catalytic decomposition of formic acid for hydrogen production.
In this study, carbon nanofiber-supported Pd nanoparticles were used in the hydrogenation of cinnamaldehyde and in the dehydrogenation of cinnamyl alcohol. The different graphitisation of the surface of the nanofibers and the amount of oxygen functionalisation significantly affected both activity and selectivity to the various reaction products. In particular, a decrease in nanoparticle dimensions and oxygen content resulted in an increase in overall activity for both of the studied reactions. Moreover, the selectivity to hydrocinnamaldehyde enhanced with increasing surface oxygen content in the cinnamaldehyde hydrogenation, while the selectivity to cinnamaldehyde was higher with low-functionalised nanofibers in the cinnamyl alcohol dehydrogenation. Finally, the most active catalyst proved also to be stable in consecutive runs.
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