In a previous study, we used transmission electron microscopy and electron energy-loss (EEL) spectroscopy to investigate dehydrogenation of AlH₃ particles. In the present study, we systematically examine differences in the chemical bonding states of Al-containing compounds (including AlH₃) by comparing their Al-L2,3 EEL spectra. The spectral chemical shift and the fine peak structure of the spe...

We characterize a novel orthorhombic phase (gamma) of NaAlH4, discovered using first-principles molecular dynamics, and discuss its relevance to the dehydrogenation mechanism. This phase is close in energy to the known low-temperature structure and becomes the stabler phase above 320 K, thanks to a larger vibrational entropy associated with AlH4 rotational modes. The structural similarity of ga...

In this work, we present a mild method for direct conversion of primary alcohols into carboxylic acids with the use of water as an oxygen source. Applying a ruthenium dihydrogen based dehydrogenation catalyst for this cause, we investigated the effect of water on the catalytic dehydrogenation process of alcohols. Using 1 mol% of the catalyst we report up to high yields. Moreover, we isolated ke...

We have developed an infrared imaging setup enabling in situ infrared images to be acquired, and expanded on capabilities of an infrared imaging as a high-throughput screening technique, determination of a critical thickness of a Pd capping layer which significantly blocks infrared emission from below, enhancement of sensitivity to hydrogenation and dehydrogenation by normalizing raw infrared i...

In the solvent free oxidation of benzyl alcohol, using supported gold-palladium nanoalloys, toluene is often one of major by-products and it is formed by the disproportionation of benzyl alcohol. Gold-palladium catalysts on acidic supports promote both the disproportionation of benzyl alcohol and oxidative dehydrogenation to form benzaldehyde. Basic supports completely switch off disproportiona...

A repetitive control technique which is based on a time-varying stochastic state space model obtained by cycle-to-cycle linearization of a nonlinear fundamental process model around the operation trajectories in the previous cycle is introduced. The control technique was applied to two repetitive chemical processes: simulated moving bed, a continuous chromatograph separation process, and CATOFI...

Abstract Acceptorless dehydrogenation into carbonyls and molecular hydrogen is an attractive strategy to valorize (biobased) alcohols. Using 2-octanol as benchmark reaction in a continuous reactor, library of metal-supported catalysts tested validate the predictive level catalytic activity for combined DFT micro-kinetic modeling. Based on series transition metals, scaling relations are determin...

One-pot reactions leading to highly functionalized coumarins have been developed via a Pd(II)-catalyzed dehydrogenation-oxidative Heck-cyclization process.

An unexpected coupling reaction of arene carboxylic acid with nitroethane via a combination of decarboxylation and dehydrogenation is described. The method provides exclusively (E)-beta-nitrostyrenes.