Loading cocatalysts on semiconductor-based photocatalysts to create active reaction sites is a preferable method to enhance photocatalytic activity and a widely adopted strategy to achieve effective photocatalytic applications. Although theoretical calculations suggest that the broad density of states of noble metal cocatalysts, such as Pt, act as a recombination center, this has never been experimentally demonstrated. Herein, we employed pico-nano and nano-micro second transient absorption spectroscopy to investigate the often overlooked photogenerated holes, instead of the widely studied electrons on Pt- and Ni-loaded SrTiO to evaluate the effects of cocatalysts as a recombination center.
View Article and Find Full Text PDFThe structure and configuration of reaction centers, which dominantly govern the catalytic behaviors, often undergo dynamic transformations under reaction conditions, yet little is known about how to exploit these features to favor the catalytic functions. Here, we demonstrate a facile light activation strategy over a TiO-supported Cu catalyst to regulate the dynamic restructuring of Cu active sites during low-temperature methanol steam reforming. Under illumination, the thermally deactivated Cu/TiO undergoes structural restoration from inoperative CuO to the originally active metallic Cu caused by photoexcited charge carriers from TiO, thereby leading to substantially enhanced activity and stability.
View Article and Find Full Text PDFThe composites of a high-capacity cathode material in lithium-ion batteries, LiCoO (LCO) and an oxide-based solid electrolyte, LiAlTi(PO) (LATP), were sintered at various temperatures and their reaction products were subsequently identified by X-ray diffraction (XRD) and X-ray absorption near edge structure (XANES). Rietveld analysis of XRD and the linear combination fitting of XANES showed that the reaction of LCO and LATP proceeds three major steps; from 300 °C to 500 °C, LCO and LATP react with each other to form CoO, amorphous TiO and LiPO; from 500 °C at which crystalline LCO is completely decomposed, LATP reacts not only with remaining amorphous/low crystalline LCO but also with CoO to form LiCoPO and TiO; from 700 °C to 750 °C, CoO and TiO react with each other to form CoTiO. The final products at 900 °C are LiCoPO, CoTiO, TiO, and LiPO.
View Article and Find Full Text PDFThe utilization of appropriate supports for constructing single-atom-catalysts is of vital importance to achieve high catalytic performances, as the strong mutual interactions between the atomically dispersed metal atoms and supports significantly influence their electronic properties. Herein, it is reported that atomic cobalt species (ACS) anchored 2D tellurium nanosheets (Te NS) can act as a highly active single-atom cocatalyst for boosting photocatalytic H production and CO reduction reactions under visible light irradiation, wherein Te NS serves as the ideal support material to bridge the light absorbers and ACS catalytic sites for efficient electron transfer. X-ray absorption near-edge structure spectroscopy reveals that the ACS are built by a Co center coordinated with five CoO bonding, which are anchored on Te NS through one CoTe bonding.
View Article and Find Full Text PDFPhotoreduction of CO to fuels offers a promising strategy for managing the global carbon balance using renewable solar energy. But the decisive process of oriented photogenerated electron delivery presents a considerable challenge. Here, we report the construction of intermolecular cascaded π-conjugation channels for powering CO photoreduction by modifying both intramolecular and intermolecular conjugation of conjugated polymers (CPs).
View Article and Find Full Text PDFGenerally, exfoliation is an efficient strategy to create more edge site so as to expose more active sites on molybdenum disulphide (MoS ). However, the lateral sizes of the resultant MoS monolayers are relatively large (≈50-500 nm), which retain great potential to release more active sites. To further enhance the catalytic performance of MoS , a facile cascade centrifugation-assisted liquid phase exfoliation method is introduced here to fabricate monolayer enriched MoS nanosheets with nanoscale lateral sizes.
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