163 research outputs found

    Preference-based Detailed Feedback Management for E-commerce Applications

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    A poster discussing feedback in consumer to consumer economic environments

    Recent advances in the catalytic oxidation of volatile organic compounds: a review based on pollutant sorts and sources

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    It is well known that urbanization and industrialization have resulted in the rapidly increasing emissions of volatile organic compounds (VOCs), which are a major contributor to the formation of secondary pollutants (e.g., tropospheric ozone, PAN (peroxyacetyl nitrate), and secondary organic aerosols) and photochemical smog. The emission of these pollutants has led to a large decline in air quality in numerous regions around the world, which has ultimately led to concerns regarding their impact on human health and general well-being. Catalytic oxidation is regarded as one of the most promising strategies for VOC removal from industrial waste streams. This Review systematically documents the progresses and developments made in the understanding and design of heterogeneous catalysts for VOC oxidation over the past two decades. It addresses in detail how catalytic performance is often drastically affected by the pollutant sources and reaction conditions. It also highlights the primary routes for catalyst deactivation and discusses protocols for their subsequent reactivation. Kinetic models and proposed oxidation mechanisms for representative VOCs are also provided. Typical catalytic reactors and oxidizers for industrial VOC destruction are further discussed. We believe that this Review will provide a great foundation and reference point for future design and development in this field

    Sphere-shaped Mn3O4 catalyst with remarkable low-temperature activity for Methyl-Ethyl-Ketone combustion

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    Mn3O4, FeMnOx, and FeOx catalysts synthesized via a solvothermal method were employed for catalytic oxidation of methyl−ethyl−ketone (MEK) at low temperature. Mn3O4 with sphere-like morphology exhibited the highest activity for MEK oxidation, over which MEK was completely oxidized to CO2 at 200 °C, and this result can be comparable to typical noble metal loaded catalysts. The activation energy of MEK over Mn3O4 (30.8 kJ/mol) was much lower than that of FeMnOx (41.5 kJ/mol) and FeOx (47.8 kJ/mol). The dominant planes, surface manganese species ratio, surface-absorbed oxygen, and redox capability played important roles in the catalytic activities of catalysts, while no significant correlation was found between specific surface area and MEK removal efficiency. Mn3O4 showed the highest activity, accounting for abundant oxygen vacancies, low content of surface Mn4+ and strong reducibility. The oxidation of MEK to CO2 via an intermediate of diacetyl is a reaction pathway on Mn3O4 catalyst. Due to high efficiency and low cost, sphere-shaped Mn3O4 is a promising catalyst for VOCs abatement

    Atomic-scale insights into the low-temperature oxidation of methanol over a single-atom Pt1-Co3O4 catalyst

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    Heterogeneous catalysts with single‐atom active sites offer a means of expanding the industrial application of noble metal catalysts. Herein, an atomically dispersed Pt1‐Co3O4 catalyst is presented, which exhibits an exceptionally high efficiency for the total oxidation of methanol. Experimental and theoretical investigations indicate that this catalyst consists of Pt sites with a large proportion of occupied high electronic states. These sites possess a strong affinity for inactive Co2+ sites and anchor over the surface of (111) crystal plane, which increases the metal–support interaction of the Pt1‐Co3O4 material and accelerates the rate of oxygen vacancies regeneration. In turn, this is determined to promote the coadsorption of the probe methanol molecule and O2. Density functional theory calculations confirm that the electron transfer over the oxygen vacancies reduces both the methanol adsorption energy and activation barriers for methanol oxidation, which is proposed to significantly enhance the dissociation of the CH bond in the methanol decomposition reaction. This investigation serves as a solid foundation for characterizing and understanding single‐atom catalysts for heterogeneous oxidation reactions

    Catalytic removal of 1,2-dichloroethane over LaSrMnCoO6/H-ZSM-5 composite: insights into synergistic effect and pollutant-destruction mechanism

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    LaxSr2−xMnCoO6 materials with different Sr contents were prepared by a coprecipitation method, with LaSrMnCoO6 found to be the best catalyst for 1,2-dichloroethane (DCE) destruction (T90 = 509 °C). As such, a series of LaSrMnCoO6/H-ZSM-5 composite materials were rationally synthesized to further improve the catalytic activity of LaSrMnCoO6. As expected, the introduction of H-ZSM-5 could remarkably enlarge the surface area, increase the number of Lewis acid sites, and enhance the mobility of the surface adsorbed oxygen species, which consequently improved the catalytic activity of LaSrMnCoO6. Among all the composite materials, 10 wt% LaSrMnCoO6/H-ZSM-5 possessed the highest catalytic activity, with 90% of 1,2-DCE destructed at 337 °C, which is a temperature reduction of more than 70 °C and 170 °C compared with that of H-ZSM-5 (T90 = 411 °C) and LaSrMnCoO6 (T90 = 509 °C), respectively. Online product analysis revealed that CO2, CO, HCl, and Cl2 were the primary products in the oxidation of 1,2-DCE, while several unfavorable reaction by-products, such as vinyl chloride, 1,1,2-trichloroethane, trichloroethylene, perchloroethylene, and acetaldehyde, were also formed via dechlorination and dehydrochlorination processes. Based on the above results, the reaction path and mechanism of 1,2-DCE decomposition are proposed

    Low-temperature direct dehydrogenation of propane over binary oxide catalysts: insights into geometric effects and active sites

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    Binary ZnZrxOy catalysts were prepared and employed to catalyze propane dehydrogenation at relatively low temperatures. The evaluation of these materials for propane dehydrogenation was supplemented by material characterization and density functional theory calculations, to provide molecular insights into the nature of the catalytic active sites. Combined, these experiments suggested that coordinatively unsaturated Zn cations (Zncus) in Zncus–O–Zrcus were the active sites for the first step of propane dehydrogenation, and coordinatively unsaturated Zr cations (Zrcus) in Zncus–O–Zrcus were active sites for the second step. This synergistic effect, derived from both these components, led to significant enhancements in activity. Furthermore, the combination of Zn and Zr species resulted in notable changes to the structure of the catalysts, leading to both the formation of the Zrcus active site and improved oxygen mobility. ZnZr2 exhibited relatively high activity

    Understanding the promotional effect of Mn2O3 on micro-/mesoporous hybrid silica nanocubic-supported Pt catalysts for the low-temperature destruction of methyl ethyl ketone: An experimental and theoretical study

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    Pt0.3Mnx/SiO2 nanocubic (nc) micro-/mesoporous composite catalysts with varied Mn contents were synthesized and tested for the oxidation of methyl ethyl ketone (MEK). Results show that MEK can be efficiently decomposed over synthesized Pt0.3Mnx/SiO2-nc materials with a reaction rate and turnover frequency respectively higher than 12.7 mmol gPt–1 s–1 and 4.7 s–1 at 100 °C. Among these materials, the Pt0.3Mn5/SiO2-nc catalyst can completely oxidize MEK at just 163 °C under a high space velocity of 42600 mL g–1 h–1. The remarkable performance of these catalysts is attributed to a synergistic effect between the Pt nanoparticles and Mn2O3. NH3-TPD and NH3-FT-IR experiments revealed that exposed Mn2O3 (222) facets enhance the quantity of Brønsted acid sites in the catalyst, which are considered to be responsible for promoting the desorption of surface-adsorbed O2 and CO2. It is suggested that the desorption of these species liberates active sites for MEK molecules to adsorb and react. 18O2 isotopic labeling experiments revealed that the presence of a Pt–O–Mn moiety weakens the Mn–O bonding interactions, which ultimately promotes the mobility of lattice oxygen in the Mn2O3 system. It was determined that the Mn4+/Mn3+ redox cycle in Mn2O3 allows for the donation of electrons to the Pt nanoparticles, enhancing the proportion of Pt0/Pt2+ and in turn increasing the activity and stability of catalyst. In situ DRIFTS, online FT-IR, and DFT studies revealed that acetone and acetaldehyde are the main intermediate species formed during the activation of MEK over the Pt0.3Mn5/SiO2-nc catalyst. Both intermediates were found to partake in sequential reactions resulting in the formation of H2O and CO2 via formaldehyde

    Catalytic oxidation of 1,2-dichloroethane over three-dimensional ordered meso-macroporous Co 3 O 4 /La 0.7 Sr 0.3 Fe 0.5 Co 0.5 O 3 : destruction route and mechanism

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    Three-dimensional ordered meso-macroporous La0.7Sr0.3Fe0.5Co0.5O3 (3DOM LSFCO)-supported Co3O4 catalysts were designed and prepared via a PMMA-templating strategy for the total oxidation of 1,2-dichloroethane (1,2-DCE). The physicochemical properties of all synthesized samples were characterized by XRD, FE-SEM, TEM, HAADF-STEM, low-temperature N2 sorption, XPS, H2-TPR, and in situ FT-IR. The introduction of Co3O4 increases the generation rate of oxygen vacancy, playing a crucial role in adsorption and activation of oxygen species. The special 3DOM structure of perovskite-type oxide promotes 1,2-DCE molecules to effectively and intimately contact with the surface adsorbed oxygen over supported catalysts and further accelerates the redox process. Compared with pure LSFCO, all the Co3O4 supported catalysts show superior catalytic performance with reaction rate increases from 5.53 × 10−12 to 2.29 × 10−11 mol g−1 s−1 and Ea decreases from 74.7 to 22.6 KJ mol−1. Amongst, the 10Co3O4/3DOM LSFCO catalyst exhibits the best catalytic activity, highest resistance to chlorine poisoning and lowest by-products concentration because of the largest amount of surface adsorbed oxygen. CO2, CO, HCl, and Cl2 are the main oxidation productions, while some typical reaction intermediates such as vinyl chloride, 1,1,2-trichloroethane and trichloroethylene are also observed, especially over the 3DOM LSFCO sample. Furthermore, the reaction mechanism of 1,2-DCE oxidation over obtained catalysts was proposed based on the results of gas chromatography, in situ FT-IR, and on-line MS. It is believed that the Co3O4/3DOM LSFCO are promising catalysts for the total removal of chlorinated volatile organic compounds
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