Ni-Induced C-Al2O3-Framework (NiCAF) Supported Core–Multishell Catalysts for Efficient Catalytic Ozonation: A Structure-to-Performance Study

Wei, Kajia; Cao, Xun; Gu, Wancong; Liang, Peng; Huang, Xia; Zhang, Xiaoyuan

doi:10.1021/acs.est.8b07132

Cited by 115 publications

(38 citation statements)

References 34 publications

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“…Heterogeneous catalytic ozonation (HCO) has been widely studied as a promising approach for the removal of organic contaminants from wastewater. − Various earlier studies have reported that the O 3 concentrated on the catalyst surface reacts with active surface sites triggering the production of reactive oxygen species (ROS) such as hydroxyl radicals ( · OH) and/or other radicals which contribute to the oxidation of targeted organic contaminants. − For example, Bing et al suggested that by introducing different metal oxides into the structure of mesoporous SBA-15 silica, the decomposition of adsorbed O 3 on the catalyst surface can be manipulated with their results showing that Al 2 O 3 promoted surface atomic oxygen generation while Fe 2 O 3 favored surface · OH and superoxide (O 2 · – ) production. The formation of · OH was also reported to occur via the interaction of adsorbed O 3 with Fe sites in amorphous iron silicate and iron silicate loaded pumice , as well as at aluminum oxide and iron oxy-hydroxide surface sites in light-weight granular mixed-quartz sands .…”

Section: Introductionmentioning

confidence: 99%

Kinetic Modeling-Assisted Mechanistic Understanding of the Catalytic Ozonation Process Using Cu–Al Layered Double Hydroxides and Copper Oxide Catalysts

Yuan

Garg

et al. 2021

Environ. Sci. Technol.

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In this study, copper aluminum layered hydroxides (Cu–Al LDHs) and copper oxide (CuO) were utilized as catalysts for heterogeneous catalytic ozonation (HCO). Target compounds oxalate and formate were used with removal by adsorption and oxidation quantified to elucidate the role of the catalyst in contaminant removal. Oxidation of oxalate mostly occurred on the catalyst surface via interaction of surface oxalate complexes with surface-located oxidants. In contrast, the oxidation of formate occurred in the bulk solution as well as on the surface of the catalyst. Measurement of O3 decay kinetics coupled with fluorescence microscopy image analysis corresponding to 7-hydroxycoumarin formation indicates that while surface hydroxyl groups in Cu–Al LDHs facilitate slow decay of O3 resulting in the formation of hydroxyl radicals on the surface, CuO rapidly transforms O3 into surface-located hydroxyl radicals and/or other oxidants. Futile consumption of surface-located oxidants via interaction with the catalyst surface was minimal for Cu–Al-LDHs; however, it becomes significant in the presence of higher CuO dosages. A mechanistic kinetic model has been developed which adequately describes the experimental results obtained and can be used to optimize the process conditions for the application of HCO.

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Section: Introductionmentioning

confidence: 99%

Kinetic Modeling-Assisted Mechanistic Understanding of the Catalytic Ozonation Process Using Cu–Al Layered Double Hydroxides and Copper Oxide Catalysts

Yuan

Garg

et al. 2021

Environ. Sci. Technol.

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“…Commonly used advanced oxidation processes include ozone catalytic oxidation, Fenton/Fenton-like reaction, ultraviolet photocatalysis, and electrochemical oxidation (Hervy et al, 2018;Kou et al, 2018). The rapid development of ozone catalytic oxidation has become a powerful tool for the efficient treatment of refractory organics in advanced oxidation processes (Wei et al, 2019).…”

Section: Research Articlementioning

confidence: 99%

Ozone catalytic oxidation capacity of Ti‐Co@Al₂O₃ for the treatment of biochemical tailwater from the coal chemical industry

Sun

Zhou

Sun

et al. 2020

Water Environment Research

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A Ti‐Co@γ‐Al2O3 composite catalyst was prepared using impregnation and sol‐gel methods to degrade biochemical tailwater from the coal chemical industry, and its preparation conditions (active component doping ratio, load times, and calcination temperature) were optimized through single‐factor experiments. The surface properties of the Ti‐Co@γ‐Al2O3 composite catalyst and the crystal structure characteristics of the catalytically active components were characterized via scanning electron microscopy–energy dispersive spectrometry, X‐ray diffraction, and X‐ray fluorescence. The effects of reaction time, initial pH, ozone aeration, and catalyst dosage on degradation performance were investigated through an experiment on the catalytic ozonation degradation of biochemical tail water. Results showed that the optimal conditions were as follows: reaction time of 30 min, pH of 8.2, ozone aeration of 30 mg/min, and catalyst dosage of 20 g/L. The total phenol and total organic carbon removal rates for biochemical tailwater were 66.1% and 57.6%, respectively, in the catalytic system. The mechanism of degradation of organic pollutants by catalytic ozonation was investigated by adding tert‐butanol to the catalytic ozone oxidation system. The degradation of chemical oxygen demand in biochemical tailwater was caused primarily by the synergy between the Ti‐Co@γ‐Al2O3 catalyst and ozone. Practitioner points Ti‐Co/γ‐Al2O3 catalyst was prepared for the catalytic oxidation of biochemical tail water. The optimal removal rates of total phenol and TOC were 67.7% and 58.8%, respectively. The organic matter was degraded rapidly and efficiently after 5 min of ozone catalytic oxidation reaction. It provides theoretical guidance for the practical application of ozone catalytic oxidation.

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“…can improve the catalytic performance dramatically, ,,, while the carbon structure may lose the structural integrity in the process of frictions and collisions between catalysts. In order to promote the mechanical strength, the Ni-induced C–Al 2 O 3 framework (CAF) was proposed . Its graphitized carbon out-shell decorated with bimetal elements of Cu–Co increased the active sites, reaction routines, and surface mass-transfer efficiency.…”

Section: Introductionmentioning

confidence: 99%

“…Meanwhile, the rigid Al 2 O 3 core maintained its mechanical stability. However, Ni has high catalytic graphitization ability while it exhibits limited catalytic performance in the CAF structure . There are other metals that possess both catalytic graphitization ability and high catalytic ozonation performance such as Fe, which has not been studied for CAF yet.…”

Section: Introductionmentioning

confidence: 99%

Bifunctional Fe for Induced Graphitization and Catalytic Ozonation Based on a Fe/N-Doped Carbon–Al₂O₃ Framework: Theoretical Calculations Guided Catalyst Design and Optimization

Ouyang

Wei

Huang

et al. 2021

Environ. Sci. Technol.

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Heterogeneous catalytic ozonation is regarded as a feasible technology in advanced wastewater treatment. Catalytic performance, mass transfer, and mechanical strength are the key elements for large-scale applications of catalysts. To optimize those elements, Fe was selected for its dual role in graphitization and catalytic ozonation. A Fe/N-doped micron-scale carbon−Al 2 O 3 framework (CAF) was designed and applied to a fluidized catalytic process for the treatment of secondary effluent from coal gasification. The chemical oxygen demand removal rate constant and the hydroxyl radical generation efficiency (R ct ) of the Fe/Ndoped CAF were 190% and 429% higher than those of pure ozone, respectively. Theoretical calculations revealed that higher Fe valence promoted ozone decomposition, which implied increasing Fe III content for further catalyst optimization. The rate constant and R ct with a higher Fe III -proportion catalyst were increased by 13% and 16%, respectively, compared to those with the lower one. Molecular dynamics and density functional theory calculations were performed to analyze the reaction kinetics qualitatively and quantitatively. The energy barrier corresponding to Fe III configuration was 1.32 kcal mol −1 , 27% lower than that for Fe II configuration. These theoretical calculations guided the catalyst optimization and provided a novel solution for designing ozonation catalysts. The Fe/N-doped CAF demonstrated a great potential for practical applications.

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Ni-Induced C-Al₂O₃-Framework (_NiCAF) Supported Core–Multishell Catalysts for Efficient Catalytic Ozonation: A Structure-to-Performance Study

Cited by 115 publications

References 34 publications

Kinetic Modeling-Assisted Mechanistic Understanding of the Catalytic Ozonation Process Using Cu–Al Layered Double Hydroxides and Copper Oxide Catalysts

Kinetic Modeling-Assisted Mechanistic Understanding of the Catalytic Ozonation Process Using Cu–Al Layered Double Hydroxides and Copper Oxide Catalysts

Ozone catalytic oxidation capacity of Ti‐Co@Al₂O₃ for the treatment of biochemical tailwater from the coal chemical industry

Bifunctional Fe for Induced Graphitization and Catalytic Ozonation Based on a Fe/N-Doped Carbon–Al₂O₃ Framework: Theoretical Calculations Guided Catalyst Design and Optimization

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Ni-Induced C-Al2O3-Framework (NiCAF) Supported Core–Multishell Catalysts for Efficient Catalytic Ozonation: A Structure-to-Performance Study

Cited by 115 publications

References 34 publications

Kinetic Modeling-Assisted Mechanistic Understanding of the Catalytic Ozonation Process Using Cu–Al Layered Double Hydroxides and Copper Oxide Catalysts

Kinetic Modeling-Assisted Mechanistic Understanding of the Catalytic Ozonation Process Using Cu–Al Layered Double Hydroxides and Copper Oxide Catalysts

Ozone catalytic oxidation capacity of Ti‐Co@Al2O3 for the treatment of biochemical tailwater from the coal chemical industry

Bifunctional Fe for Induced Graphitization and Catalytic Ozonation Based on a Fe/N-Doped Carbon–Al2O3 Framework: Theoretical Calculations Guided Catalyst Design and Optimization

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Ni-Induced C-Al₂O₃-Framework (_NiCAF) Supported Core–Multishell Catalysts for Efficient Catalytic Ozonation: A Structure-to-Performance Study

Ozone catalytic oxidation capacity of Ti‐Co@Al₂O₃ for the treatment of biochemical tailwater from the coal chemical industry

Bifunctional Fe for Induced Graphitization and Catalytic Ozonation Based on a Fe/N-Doped Carbon–Al₂O₃ Framework: Theoretical Calculations Guided Catalyst Design and Optimization