Glycerol is a highly versatile molecule because of its three hydroxyl groups and can be transformed to a plethora of different value-added fine chemicals and products. It is an important byproduct in biodiesel production and, hence, produced in high amounts, which resulted in a high surplus flooding the market over the last decades. Thus, glycerol is regarded as a potential platform chemical, and many research efforts were devoted to find active catalysts to transform glycerol to various products via different catalytic processes. The selective oxidation reaction is one of the most promising reaction pathways to produce valuable fine chemicals used in the chemical and pharmaceutical industry. This Review describes the recent developments in selective glycerol oxidation to value-added products over heterogeneous catalysts. Particular emphasis is placed not only on newly developed catalysts based on supported noble-metal nanoparticles but also on catalysts containing nonprecious metals. The idea of using cost-efficient non-noble metals for glycerol oxidation is appealing from an economic point of view. Numerous parameters can influence the catalytic performance of the materials, which can be tuned by various synthetic approaches. The reasons for enhancements in activity are critically examined and put into perspective among the various studies. Moreover, during the past decade, many research groups also reported photocatalytic and, more scarcely, electrocatalytic pathways for glycerol oxidation, which are also described in detail herein and have otherwise found little attention in other reviews.
Halide perovskites have prompted the evolution of the photovoltaic field and simultaneously demonstrated their great potential for application in other optoelectronic devices. A fundamental understanding of their structure-property relationship is essential to fabricate novel materials and high-performance devices. This review gives a perspective on different synthetic methodologies for the preparation of halide perovskites and highlights the effects of structural factors such as crystal structure, grain size, nanoscale dimensionality, patterned arrangement, and hierarchical structure on their optoelectronic properties. The main emphasis is given to 0D, 1D and 2D nanostructured materials including their common synthesis methods and key structural properties. Structural factors should be precisely controlled during the material preparation and device fabrication to improve the performance of targeted applications.
Halide perovskites have attracted great attention in the fields of photovoltaics, LEDs, lasers, and most recently photocatalysis, owing to their unique optoelectronic properties. The all-inorganic halide perovskite CsPbBr /TiO composite material catalyzes selective benzyl alcohol oxidation to benzaldehyde under visible-light illumination. The catalyst, which is prepared by a facile wet-impregnation method, shows very good selectivity towards benzaldehyde (>99 % at 50 % conversion). Action spectra and electron spin resonance (ESR) studies reveal that photoexcited electrons formed within CsPbBr upon visible-light illumination take part in the reaction via reduction of oxygen to form superoxide radicals. The detailed post-catalysis characterization by UV/Vis and X-ray photoelectron spectroscopy, X-ray diffraction, and high-angle annular dark-field scanning transmission electron microscopy studies further demonstrated the good stability of CsPbBr in terms of morphology and crystal structure under the reaction conditions. This study sheds light on promising new photocatalytic applications of halide perovskites.
We use intensity-modulated photovoltage spectroscopy (IMVS) and intensitymodulated photocurrent spectroscopy (IMPS) to characterize carrier dynamics in titania (TiO 2 ) aerogels under photocatalytic conditions. By systematically increasing the weight fraction of the sol-gel precursor during TiO 2 sol-gel synthesis, we are able to impart drastic changes in carrier transport/trapping and improve the photocatalytic activity of TiO 2 aerogels for two mechanistically divergent photochemical reactions-reductive water splitting (H 2 generation) and oxidative degradation of dichloroacetate (DCA). The lifetimes of photogenerated electrons increase in going from lowest-to-highest precursor concentrations, as measured by IMVS, indicating increasing site density for electron traps, a trend that correlates with an 8× improvement for photocatalytic H 2 generation. Electron mobility in the aerogel films, as measured by IMPS, decreases with increasing trap density, further implicating the trapping sites as reactive sites. In contrast, photocatalytic DCA degradation-driven primarily by direct hole transfer to adsorbed DCA-depends only weakly on the electron dynamics in the film. Transient infrared spectroscopy shows no difference in carrier decay amongst the aerogel samples on picosecond timescales, indicating that changes in carrier dynamics within these networked nanomaterials are only observable at timescales measured by IMPV and IMPS. Correlating holemediated and electron-mediated photocatalytic activity with direct measurement of electron dynamics under photocatalytically relevant conditions and timescales comprises a powerful approach to determine how synthetic modifications to networked nanostructured photocatalysts affect the relevant physicochemical phenomena underlying their photocatalytic performance.
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