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Self-Exfoliated Synthesis of Transition Metal Phosphate Nanolayers for Selective Aerobic Oxidation of Ethyl Lactate to Ethyl Pyruvate.

ABSTRACT: Two-dimensional (2D) transition metal nanosheets are promising catalysts because of the enhanced exposure of the active species compared to their 3D counterparts. Here, we report a simple, scalable, and reproducible strategy to prepare 2D phosphate nanosheets by forming a layered structure in situ from phytic acid (PTA) and transition metal precursors. Controlled combustion of the organic groups of PTA results in interlayer carbon, which keeps the layers apart during the formation of phosphate, and the removal of this carbon results in ultrathin nanosheets with controllable layers. Applying this concept to vanadyl phosphate synthesis, we show that the method yields 2D ultrathin nanosheets of the orthorhombic ?-form, exposing abundant V4+/V5+ redox sites and oxygen vacancies. We demonstrate the high catalytic activity of this material in the vapor-phase aerobic oxidation of ethyl lactate to ethyl pyruvate. Importantly, these ?-VOPO4 compounds do not get hydrated, thereby reducing the competing hydrolysis reaction by water byproducts. The result has superior selectivity to ethyl pyruvate compared to analogous vanadyl phosphates. The catalysts are highly stable, maintaining a steady-state conversion of ?90% (with >80% selectivity) for at least 80 h on stream. This "self-exfoliated" synthesis protocol opens opportunities for preparing structurally diverse metal phosphates for catalysis and other applications.

SUBMITTER: Zhang W

PROVIDER: S-EPMC7493282 | biostudies-literature | 2020 Apr

REPOSITORIES: biostudies-literature

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Self-Exfoliated Synthesis of Transition Metal Phosphate Nanolayers for Selective Aerobic Oxidation of Ethyl Lactate to Ethyl Pyruvate.

Zhang Wei W Oulego Paula P Sharma Sandeep K SK Yang Xiu-Lin XL Li Lain-Jong LJ Rothenberg Gadi G Shiju N Raveendran NR

ACS catalysis 20200219 7

Two-dimensional (2D) transition metal nanosheets are promising catalysts because of the enhanced exposure of the active species compared to their 3D counterparts. Here, we report a simple, scalable, and reproducible strategy to prepare 2D phosphate nanosheets by forming a layered structure in situ from phytic acid (PTA) and transition metal precursors. Controlled combustion of the organic groups of PTA results in interlayer carbon, which keeps the layers apart during the formation of phosphate, ...[more]

PMID: 32953234

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Project description:In order to obtain a global view of energy metabolism pathways of the sulfate-reducer Desulfovibrio vulgaris Hildenborough and the proteins involved therein whole-genome microarrays were used to compare the transcriptional response of cells grown with hydrogen/sulfate, pyruvate/sulfate, lactate/thiosulfate, and pyruvate with limiting sulfate, relative to growth in standard lactate/sulfate condition. Growth with hydrogen/sulfate showed the largest number of differently expressed genes and the largest changes in expression levels. The most up-regulated energy metabolism genes were those coding for the periplasmic [NiFeSe] hydrogenase, followed by the Ech hydrogenase, and the most down-regulated were genes coding for the Coo hydrogenase. The results point to the involvement of formate cycling and the ethanol pathway during growth on hydrogen, whereas there is evidence for CO cycling during growth on lactate and pyruvate, but not on H2. Growth with thiosulfate showed the hallmarks of a reduced energy status of the cells with down regulation of the ATP synthase and the Qmo and Dsr complexes., whereas growth with pyruvate showed the smallest differences but an increased role for the Ech hydrogenase.that in this case functions in reverse from the case of growth with H2. The multiple periplasmic hydrogenases and formate dehydrogenases, do not display the same regulation pattern showing that their metabolic roles are not totally interchangeable. This result together with the observation that several genes coding for proteins that have not been biochemically characterised were considerably affected in this study, reveals a more complex energy metabolism than previously considered and provides guidance for further studies. Keywords: Growth protocol Desulfovibrio vulgaris from our laboratory culture collection was cultured at 37°C with pyruvate as the only substrate (without sulfate as the electron acceptor) to mid-log phase. Cultures were also cultivated similarly in Lactate-Sulfate medium to mid-log phase. Gene expression profiles of cultures grown under pyruvate fermentation were compared with those of the cultures grown via sulfate reduction. Total RNA was harvested from four replicate cultures for microarray analysis. RNA extraction, purification, and labeling were performed independently on each cell sample.Two samples of each total RNA preparation were labeled, one with Cy3-dUTP and another with Cy5-dUTP for microarray hybridization.

Dataset Information

Self-Exfoliated Synthesis of Transition Metal Phosphate Nanolayers for Selective Aerobic Oxidation of Ethyl Lactate to Ethyl Pyruvate.

Publications

Self-Exfoliated Synthesis of Transition Metal Phosphate Nanolayers for Selective Aerobic Oxidation of Ethyl Lactate to Ethyl Pyruvate.

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