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Creators/Authors contains: "Song, Hocheol"

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  1. Current synthesis techniques for metal oxide (MOx)-supported catalysts have certain limitations of undesired target loading, ineffective dispersion of active species over the surface, uncontrolled particle size of active species, and complicated synthesis steps. We developed a one-pot chemical vapor deposition (OP-CVD) methodology; by using which a solid metal precursor forms a vapor in a controlled condition and gets supported over the surrounding matrix. The theoretical stability followed by experimental validation using TGA is crucial for selecting the metal precursors. Three simple steps viz. premixing, dispersion, and rapid fixation by calcination are involved in the catalyst development via the OP-CVD approach. This study solely focused on the synthesis of 3d transition MOx over ceria support. The physicochemical characterizations of the prepared catalysts were performed by XRD, ICP-OES, SEM-EDX, CO pulse chemisorption, XANES, and EXAFS analyses to understand the crystal structure of involved species, target metal loading, dispersion, and particle size and prove the feasibility and viability of OP-CVD. The prepared catalysts were further tested for reverse water gas shift (RWGS) reaction to link their structural information with activity. The RWGS reaction data showed that the CO activity and CO selectivity were metal - and metal precursor-dependent. Higher CO activity of > 0.1 mol/h g-cat was observed for Cu and Co-based catalysts, with CO selectivity of ~100 %. This study provides an opportunity to produce effcient supported catalysts in a convenient way, providing effective catalytic activity. 
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  2. NiOx/CeO2catalysts were synthesized under various pretreatment conditions. Different pretreatment conditions significantly influenced the activity of the NO reduction by CO reaction. 
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  3. Although cerium oxide (CeO2) is widely used as a catalyst support, its limited defect sites and surface oxygen vacancy/mobility should be improved. The incorporation of zirconium (Zr) in the cerium (Ce) lattice is shown to increase the number of oxygen vacancies and improve catalytic activity. Using a fixed surface density (SD) of copper (∼2.3 Cu atoms per nm2) as a surface species, the role of the support (CeyZr1−yO2 (y = 1.0, 0.9, 0.6, 0.5, and 0.0)) and defect site effects in the CO oxidation reaction was investigated. Spectroscopic (e.g., Raman, XRD, XPS) and microscopic (e.g., SEM-EDX, HR-TEM) characterization techniques were applied to evaluate the defect sites, crystallite size, lattice parameters, chemical composition, oxidation states of elements and microstructure of the catalysts. The CO oxidation reaction with varied CO:O2 ratios (1 : 5, 1 : 1, and 1 :0.5 (stoichiometric)) was used as a model reaction to describe the relationship between the structure and the catalytic performance of each catalyst. Based on the characterization results of CeyZr1−yO2 materials, the addition of Zr causes physical and chemical changes to the overall material. The inclusion of Zr into the structure of CeO2 decreased the overall lattice parameter of the catalyst and increased the number of defect sites. The prepared catalysts were able to reach complete CO conversion (∼100%) at low temperature conditions (<200 °C), each showing varied reaction activity. The difference in CO oxidation activity was then analyzed and related to the structure, wherein Cu loading, surface oxygen vacancies, reduction–oxidation ability, CuOx–support interaction and oxygen mobility in the catalyst were the crucial descriptors. 
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