Nanocarbon-Based Catalytic Ozonation for Aqueous Oxidation: Engineering Defects for Active Sites and Tunable Reaction Pathways

ACS Catalysis ◽  
2020 ◽  
Vol 10 (22) ◽  
pp. 13383-13414
Author(s):  
Yuxian Wang ◽  
Xiaoguang Duan ◽  
Yongbing Xie ◽  
Hongqi Sun ◽  
Shaobin Wang
Keyword(s):  
Active Sites ◽  
Catalytic Ozonation ◽  
Reaction Pathways ◽  
Aqueous Oxidation

scholarly journals Enhanced catalytic ozonation of ibuprofen using a 3D structured catalyst with MnO2 nanosheets on carbon microfibers

2021 ◽  
Vol 11 (1) ◽  
Author(s):  
Guhankumar Ponnusamy ◽  
Hajar Farzaneh ◽  
Yongfeng Tong ◽  
Jenny Lawler ◽  
Zhaoyang Liu ◽  
...  
Keyword(s):  
Removal Efficiency ◽  
Active Sites ◽  
Low Cost ◽  
Three Dimensional ◽  
Industrial Applications ◽  
Catalytic Ozonation ◽  
Heterogeneous Catalytic ◽  
Structured Catalyst ◽  
Dimensional Network ◽  
Carbon Microfibers

AbstractHeterogeneous catalytic ozonation is an effective approach to degrade refractory organic pollutants in water. However, ozonation catalysts with combined merits of high activity, good reusability and low cost for practical industrial applications are still rare. This study aims to develop an efficient, stable and economic ozonation catalyst for the degradation of Ibuprofen, a pharmaceutical compound frequently detected as a refractory pollutant in treated wastewaters. The novel three-dimensional network-structured catalyst, comprising of δ-MnO2 nanosheets grown on woven carbon microfibers (MnO2 nanosheets/carbon microfiber), was synthesized via a facile hydrothermal approach. Catalytic ozonation performance of Ibuprofen removal in water using the new catalyst proves a significant enhancement, where Ibuprofen removal efficiency of close to 90% was achieved with a catalyst loading of 1% (w/v). In contrast, conventional ozonation was only able to achieve 65% removal efficiency under the same operating condition. The enhanced performance with the new catalyst could be attributed to its significantly increased available surface active sites and improved mass transfer of reaction media, as a result of the special surface and structure properties of this new three-dimensional network-structured catalyst. Moreover, the new catalyst displays excellent stability and reusability for ibuprofen degradation over successive reaction cycles. The facile synthesis method and low-cost materials render the new catalyst high potential for industrial scaling up. With the combined advantages of high efficiency, high stability, and low cost, this study sheds new light for industrial applications of ozonation catalysts.

scholarly journals Computational Investigation of the Role of Active Site Heterogeneity for a Supported Organovanadium(III) Hydrogenation Catalyst

2021 ◽  
Author(s):  
Prajay Patel ◽  
Robert Wells ◽  
David Kaphan ◽  
Massimiliano Delferro ◽  
Rex T. Skodje ◽  
...  
Keyword(s):  
Active Site ◽  
Active Sites ◽  
Density Functional ◽  
Computational Models ◽  
Surface Heterogeneity ◽  
Reaction Pathways ◽  
Spectroscopic Techniques ◽  
Organometallic Catalysts ◽  
Heterolytic Cleavage ◽  
Styrene Hydrogenation

<div> <div> <p></p><p><a>A crucial consideration for supported heterogeneous catalysts is the non-uniformity of the active sites, particularly for Supported Organometallic Catalysts (SOMCs). Standard spectroscopic techniques, such as X-ray absorption spectroscopy (XAS), reflect the nature of the most populated sites, which are often intrinsically structurally distinct from the most catalytically active sites. With computational models, often only a few representative structures are used to depict catalytic active sites on a surface, even though there are numerous observable factors of surface heterogeneity that contribute to the kinetically favorable active species. A previously reported study on the mechanism of a surface organovanadium(III) catalyst [(SiO)V<sup>III</sup>(Mes)(THF)] for styrene hydrogenation yielded two possible mechanisms: heterolytic cleavage and redox cycling. These two mechanistic scenarios are challenging to differentiate experimentally based on the kinetic readouts of the catalyst are identical. To showcase the importance of modeling surface heterogeneity and its effect on catalytic activity, density functional theory (DFT) computational models of a series of potential active sites of [(SiO)V<sup>III</sup>(Mes)(THF)] for the reaction pathways are applied in combination with kinetic Monte Carlo (kMC) simulations. Computed results were t then compared to the previously reported experimental kinetic study</a><a>.: 1) DFT free energy reaction pathways indicated the likely active site and pathway for styrene hydrogenation; a heterolytic cleavage pathway requiring a bare tripodal vanadium site. 2) From the kMC simulations, a mixture of the different bond lengths from the support oxygen to the metal center was required to qualitatively describe the experimentally observed kinetic aspects of a supported organovanadium(III) catalyst for olefin hydrogenation. </a>This work underscores the importance of modeling surface heterogeneity in computational catalysis.</p><p></p></div></div>

scholarly journals Computational Investigation of the Role of Active Site Heterogeneity for a Supported Organovanadium(III) Hydrogenation Catalyst

2021 ◽  
Author(s):  
Prajay Patel ◽  
Robert Wells ◽  
David Kaphan ◽  
Massimiliano Delferro ◽  
Rex T. Skodje ◽  
...  
Keyword(s):  
Active Site ◽  
Active Sites ◽  
Density Functional ◽  
Computational Models ◽  
Surface Heterogeneity ◽  
Reaction Pathways ◽  
Spectroscopic Techniques ◽  
Organometallic Catalysts ◽  
Heterolytic Cleavage ◽  
Styrene Hydrogenation

<div> <div> <p></p><p><a>A crucial consideration for supported heterogeneous catalysts is the non-uniformity of the active sites, particularly for Supported Organometallic Catalysts (SOMCs). Standard spectroscopic techniques, such as X-ray absorption spectroscopy (XAS), reflect the nature of the most populated sites, which are often intrinsically structurally distinct from the most catalytically active sites. With computational models, often only a few representative structures are used to depict catalytic active sites on a surface, even though there are numerous observable factors of surface heterogeneity that contribute to the kinetically favorable active species. A previously reported study on the mechanism of a surface organovanadium(III) catalyst [(SiO)V<sup>III</sup>(Mes)(THF)] for styrene hydrogenation yielded two possible mechanisms: heterolytic cleavage and redox cycling. These two mechanistic scenarios are challenging to differentiate experimentally based on the kinetic readouts of the catalyst are identical. To showcase the importance of modeling surface heterogeneity and its effect on catalytic activity, density functional theory (DFT) computational models of a series of potential active sites of [(SiO)V<sup>III</sup>(Mes)(THF)] for the reaction pathways are applied in combination with kinetic Monte Carlo (kMC) simulations. Computed results were t then compared to the previously reported experimental kinetic study</a><a>.: 1) DFT free energy reaction pathways indicated the likely active site and pathway for styrene hydrogenation; a heterolytic cleavage pathway requiring a bare tripodal vanadium site. 2) From the kMC simulations, a mixture of the different bond lengths from the support oxygen to the metal center was required to qualitatively describe the experimentally observed kinetic aspects of a supported organovanadium(III) catalyst for olefin hydrogenation. </a>This work underscores the importance of modeling surface heterogeneity in computational catalysis.</p><p></p></div></div>

New insights in understanding plasma-catalysis reaction pathways: study of the catalytic ozonation of an acetaldehyde saturated Ag/TiO2/SiO2catalyst

2015 ◽  
Vol 71 (2) ◽  
pp. 20805 ◽  
Author(s):  
Sonia Sauce ◽  
Arlette Vega-González ◽  
Zixian Jia ◽  
Sylvain Touchard ◽  
Khaled Hassouni ◽  
...  
Keyword(s):  
Catalytic Ozonation ◽  
Reaction Pathways ◽  
Plasma Catalysis
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