Alejandro Ayala-Cortés, Daniel Torres, E. Frecha, P. Arcelus-Arrillaga, H. Villafán-Vidales, Adriana Longoria, J. Pinilla, I. Suelves
Transition metal carbides have emerged as an attractive alternative to conventional catalysts in hydrodeoxygenation (HDO) reactions due to surface reactivity, catalytic activity, and thermodynamic stability similar to those of noble metals. In this study, the impact of varying Mo concentration in carbon nanofiber-supported catalysts for the supercritical ethanol-assisted HDO of bio-oils in an autoclave batch reactor is discussed. Raw bio-oils derived from agave bagasse and corncob through solar hydrothermal liquefaction were treated at 350 °C. Our findings indicate that the presence of Mo has a strong impact on both product yield and chemical properties. Thus, a Mo concentration of 10 wt.% is enough to obtain high deoxygenation values (69–72%), resulting in a yield of upgraded bio-oil ranging between 49.9 and 60.4%, depending on the feedstock used, with an energy content of around 35 MJ/kg. A further increase in the Mo loadings (20 and 30 wt.%) reduced the loss of carbon due to gasification and improved the bio-oil yields up to 62.6 and 67.4%, without compromising the product quality.
{"title":"Catalytic Hydrodeoxygenation of Solar Energy Produced Bio-Oil in Supercritical Ethanol with Mo2C/CNF Catalysts: Effect of Mo Concentration","authors":"Alejandro Ayala-Cortés, Daniel Torres, E. Frecha, P. Arcelus-Arrillaga, H. Villafán-Vidales, Adriana Longoria, J. Pinilla, I. Suelves","doi":"10.3390/catal13121500","DOIUrl":"https://doi.org/10.3390/catal13121500","url":null,"abstract":"Transition metal carbides have emerged as an attractive alternative to conventional catalysts in hydrodeoxygenation (HDO) reactions due to surface reactivity, catalytic activity, and thermodynamic stability similar to those of noble metals. In this study, the impact of varying Mo concentration in carbon nanofiber-supported catalysts for the supercritical ethanol-assisted HDO of bio-oils in an autoclave batch reactor is discussed. Raw bio-oils derived from agave bagasse and corncob through solar hydrothermal liquefaction were treated at 350 °C. Our findings indicate that the presence of Mo has a strong impact on both product yield and chemical properties. Thus, a Mo concentration of 10 wt.% is enough to obtain high deoxygenation values (69–72%), resulting in a yield of upgraded bio-oil ranging between 49.9 and 60.4%, depending on the feedstock used, with an energy content of around 35 MJ/kg. A further increase in the Mo loadings (20 and 30 wt.%) reduced the loss of carbon due to gasification and improved the bio-oil yields up to 62.6 and 67.4%, without compromising the product quality.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"31 16","pages":""},"PeriodicalIF":3.9,"publicationDate":"2023-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138589153","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Rotating packed beds (RPB) facilitate the mixing of heterogeneous substrates, and promote high mass transfer efficiency in heterogeneous reactions. For the enzymatic reactions, traditional porous particles with immobilized enzymes are sensitive to the strong sheer force of the RPB, thus limiting its application. This work offers a strategy for enzyme immobilization on the surface of stainless-steel fleece, to improve the shear strength resistance of immobilized enzymes. Lipase was applied to investigate and optimize the immobilization. Finally, a fatty acid hydratase (FAH) was applied for immobilization based on the optimized method, which was further applied for evaluating its performance in RPB. The results indicated that metal immobilized enzymes resist a higher shear force than their particle-immobilized alternatives. Operating at a centrifugal force factor (β) of 30, the hydration conversion rate of 96% is achieved after 8 h, which was from nearly 38% faster than in a stirrer tank reactor (hydration yield of 60%). The metal immobilization, moreover, efficiently improved the enzyme reusability, as demonstrated by a conversion rate remaining above 90% after 15 batches. These results indicated that a metal immobilization method combined with an RPB reactor significantly increases the efficiency of enzymatic reactions.
{"title":"Enzyme Immobilization on Stainless Steel Fleece and Its Mass Transfer Enhancement of Enzymatic Catalysis in a Rotating Packed Bed Reactor","authors":"Ruiyi Yang, Juntao Xu, Jinglong Wu, Dong Lu, Fang Wang, Kaili Nie","doi":"10.3390/catal13121501","DOIUrl":"https://doi.org/10.3390/catal13121501","url":null,"abstract":"Rotating packed beds (RPB) facilitate the mixing of heterogeneous substrates, and promote high mass transfer efficiency in heterogeneous reactions. For the enzymatic reactions, traditional porous particles with immobilized enzymes are sensitive to the strong sheer force of the RPB, thus limiting its application. This work offers a strategy for enzyme immobilization on the surface of stainless-steel fleece, to improve the shear strength resistance of immobilized enzymes. Lipase was applied to investigate and optimize the immobilization. Finally, a fatty acid hydratase (FAH) was applied for immobilization based on the optimized method, which was further applied for evaluating its performance in RPB. The results indicated that metal immobilized enzymes resist a higher shear force than their particle-immobilized alternatives. Operating at a centrifugal force factor (β) of 30, the hydration conversion rate of 96% is achieved after 8 h, which was from nearly 38% faster than in a stirrer tank reactor (hydration yield of 60%). The metal immobilization, moreover, efficiently improved the enzyme reusability, as demonstrated by a conversion rate remaining above 90% after 15 batches. These results indicated that a metal immobilization method combined with an RPB reactor significantly increases the efficiency of enzymatic reactions.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"32 1","pages":""},"PeriodicalIF":3.9,"publicationDate":"2023-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138587505","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Marina Maddaloni, Ander Centeno-Pedrazo, Simone Avanzi, N. J. Mazumdar, H. Manyar, N. Artioli
The selective hydrogenation of CO2 for the production of net-zero fuels and essential chemical building blocks is a promising approach to combat climate change. Key to this endeavor is the development of catalysts with high activity and selectivity for desired hydrocarbon products in the C2–C5 range. The process involves a two-step reaction, starting with the reverse water–gas shift (RWGS) reaction and proceeding to the Fischer–Tropsch reactions under high pressure. Understanding the catalyst features that control the selectivity of these pathways is crucial for product formation, as well as identifying morphological changes in the catalysts during the reaction to optimize their performance. In this study, an innovative method for synthesizing iron–ruthenium bimetallic catalysts is introduced, capitalizing on the synergistic effects of these metals as active phases. This method leverages ionic liquids as solvents, allowing for the precise and uniform distribution of active metal phases. Advanced characterizations and extensive catalytic tests have demonstrated that the use of ionic liquids outperformed traditional colloid-based techniques, resulting in superior selectivity for target hydrocarbons. The success of this inventive approach not only advances the field of CO2 hydrogenation catalysis, but also represents a significant stride towards sustainable e-fuel production.
{"title":"Novel Ionic Liquid Synthesis of Bimetallic Fe–Ru Catalysts for the Direct Hydrogenation of CO2 to Short Chain Hydrocarbons","authors":"Marina Maddaloni, Ander Centeno-Pedrazo, Simone Avanzi, N. J. Mazumdar, H. Manyar, N. Artioli","doi":"10.3390/catal13121499","DOIUrl":"https://doi.org/10.3390/catal13121499","url":null,"abstract":"The selective hydrogenation of CO2 for the production of net-zero fuels and essential chemical building blocks is a promising approach to combat climate change. Key to this endeavor is the development of catalysts with high activity and selectivity for desired hydrocarbon products in the C2–C5 range. The process involves a two-step reaction, starting with the reverse water–gas shift (RWGS) reaction and proceeding to the Fischer–Tropsch reactions under high pressure. Understanding the catalyst features that control the selectivity of these pathways is crucial for product formation, as well as identifying morphological changes in the catalysts during the reaction to optimize their performance. In this study, an innovative method for synthesizing iron–ruthenium bimetallic catalysts is introduced, capitalizing on the synergistic effects of these metals as active phases. This method leverages ionic liquids as solvents, allowing for the precise and uniform distribution of active metal phases. Advanced characterizations and extensive catalytic tests have demonstrated that the use of ionic liquids outperformed traditional colloid-based techniques, resulting in superior selectivity for target hydrocarbons. The success of this inventive approach not only advances the field of CO2 hydrogenation catalysis, but also represents a significant stride towards sustainable e-fuel production.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"13 3","pages":""},"PeriodicalIF":3.9,"publicationDate":"2023-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138590996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Vincenzo Langellotti, Massimo Melchiorre, M. E. Cucciolito, Roberto Esposito, Domenico Grieco, Gabriella Pinto, F. Ruffo
This article presents an efficient iron(III) molecular catalyst for the production of biodiesel from waste vegetable oils. The approach involved an initial screening of eight salophen complexes with various substituents on the arene rings, leading to the selection of the simplest unsubstituted species as the most active catalyst. Under optimized conditions, this catalyst demonstrated the capability to achieve complete conversion of the oil at a low catalyst loading (0.10% mol/mol) and convenient conditions (160 °C, 20/1 MeOH/oil ratio).
{"title":"Biodiesel from Waste Cooking Oil: Highly Efficient Homogeneous Iron(III) Molecular Catalysts","authors":"Vincenzo Langellotti, Massimo Melchiorre, M. E. Cucciolito, Roberto Esposito, Domenico Grieco, Gabriella Pinto, F. Ruffo","doi":"10.3390/catal13121496","DOIUrl":"https://doi.org/10.3390/catal13121496","url":null,"abstract":"This article presents an efficient iron(III) molecular catalyst for the production of biodiesel from waste vegetable oils. The approach involved an initial screening of eight salophen complexes with various substituents on the arene rings, leading to the selection of the simplest unsubstituted species as the most active catalyst. Under optimized conditions, this catalyst demonstrated the capability to achieve complete conversion of the oil at a low catalyst loading (0.10% mol/mol) and convenient conditions (160 °C, 20/1 MeOH/oil ratio).","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"49 18","pages":""},"PeriodicalIF":3.9,"publicationDate":"2023-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138593784","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hydrogen has emerged as an important candidate for clean energy, owing to its environmentally friendly advantages. Electrolytic hydrogen production stands out as the most promising technology for hydrogen production. Therefore, the design of highly efficient electrocatalysts is significant to drive the application of hydrogen technologies. Platinum (Pt)-based catalysts are famous for their outstanding performance in the hydrogen evolution reaction (HER). However, the expensive cost limits its wide application. Ruthenium (Ru)-based catalysts have received extensive attention due to their relatively lower cost and HER performance similar to that of Pt. Nevertheless, the performance of Ru-based catalysts is still unable to meet industrial demands. Therefore, improving HER performance through the modification of Ru-based catalysts remains significant. In this review, the reaction mechanism of HER is analyzed and the latest research progress in the modification of Ru-based electrocatalysts is summarized. From the reaction mechanism perspective, addressing the adsorption of intermediates on the Ru-based electrocatalyst surface, the adsorption–activation of interface water molecules, and the behavior of interface water molecules and proposing solutions to enhance performance of Ru-based electrocatalyst are the main findings, ultimately contributing to promoting their application in the field of electrocatalysis.
{"title":"Recent Progress on Ruthenium-Based Electrocatalysts towards the Hydrogen Evolution Reaction","authors":"Lulu Li, Fenyang Tian, Long-Wu Qiu, Fengyu Wu, Weiwei Yang, Yongsheng Yu","doi":"10.3390/catal13121497","DOIUrl":"https://doi.org/10.3390/catal13121497","url":null,"abstract":"Hydrogen has emerged as an important candidate for clean energy, owing to its environmentally friendly advantages. Electrolytic hydrogen production stands out as the most promising technology for hydrogen production. Therefore, the design of highly efficient electrocatalysts is significant to drive the application of hydrogen technologies. Platinum (Pt)-based catalysts are famous for their outstanding performance in the hydrogen evolution reaction (HER). However, the expensive cost limits its wide application. Ruthenium (Ru)-based catalysts have received extensive attention due to their relatively lower cost and HER performance similar to that of Pt. Nevertheless, the performance of Ru-based catalysts is still unable to meet industrial demands. Therefore, improving HER performance through the modification of Ru-based catalysts remains significant. In this review, the reaction mechanism of HER is analyzed and the latest research progress in the modification of Ru-based electrocatalysts is summarized. From the reaction mechanism perspective, addressing the adsorption of intermediates on the Ru-based electrocatalyst surface, the adsorption–activation of interface water molecules, and the behavior of interface water molecules and proposing solutions to enhance performance of Ru-based electrocatalyst are the main findings, ultimately contributing to promoting their application in the field of electrocatalysis.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"31 7","pages":""},"PeriodicalIF":3.9,"publicationDate":"2023-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138591753","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kang Hoon Lee, Zafar Arshad, A. Dahshan, Mubark Alshareef, Q. Alsulami, A. Bibi, Eui-Jong Lee, Muddasir Nawaz, Usman Zubair, Amjed Javid
There was an error in the original publication [...]
原文中有个错误[…]
{"title":"Correction: Lee et al. Porous Aerogel Structures as Promising Materials for Photocatalysis, Thermal Insulation Textiles, and Technical Applications: A Review. Catalysts 2023, 13, 1286","authors":"Kang Hoon Lee, Zafar Arshad, A. Dahshan, Mubark Alshareef, Q. Alsulami, A. Bibi, Eui-Jong Lee, Muddasir Nawaz, Usman Zubair, Amjed Javid","doi":"10.3390/catal13121498","DOIUrl":"https://doi.org/10.3390/catal13121498","url":null,"abstract":"There was an error in the original publication [...]","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"41 14","pages":""},"PeriodicalIF":3.9,"publicationDate":"2023-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138593400","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In this work, Sn-Si mixed oxide microspheres with concave hollow morphologies were first synthesized by a simple aerosol method using the very common commercial surfactant cetyl trimethyl ammonium bromide (CTAB) as a template, and then highly interconnected mesoporous and hollow Sn-Si mixed oxide microspheres were synthesized via an alkali (NaOH) treatment in the presence of CTAB. The results show that CTAB plays a crucial role not only in forming hollow morphologies during the aerosol process, but also protecting the amorphous framework and thus preventing the excessive loss of Sn species during the NaOH treatment. More importantly, it widens mesoporous distribution and forms interconnected mesoporous channels. The catalytic performance of Baeyer–Villiger oxidation on the interconnected mesoporous and hollow Sn-Si mixed oxide microspheres with 2-adamantanone and hydrogen peroxide was 9.4 times higher than that of the sample synthesized without the addition of CTAB; 2.3 times that of the untreated parent, which was due to the excellent diffusion properties derived from the hollow and interconnected mesopore structure. This method is mild, simple, low-cost, and can be continuously produced, which has the prospect of industrial application. Furthermore, the fundamentals of this study provide new insights for the rational design and preparation of highly interlinked mesoporous and hollow metal-oxides with unique catalytic performances.
{"title":"Constructing Interconnected Hollow Mesopore Sn-Si Mixed Oxide Microspheres by Aerosol-Assisted Alkali Treatment with Enhanced Catalytic Performance in Baeyer-Villiger Oxidation","authors":"Qingrun Meng, Xiaoxu Gao, Dezheng Li, Huimin Liu","doi":"10.3390/catal13121494","DOIUrl":"https://doi.org/10.3390/catal13121494","url":null,"abstract":"In this work, Sn-Si mixed oxide microspheres with concave hollow morphologies were first synthesized by a simple aerosol method using the very common commercial surfactant cetyl trimethyl ammonium bromide (CTAB) as a template, and then highly interconnected mesoporous and hollow Sn-Si mixed oxide microspheres were synthesized via an alkali (NaOH) treatment in the presence of CTAB. The results show that CTAB plays a crucial role not only in forming hollow morphologies during the aerosol process, but also protecting the amorphous framework and thus preventing the excessive loss of Sn species during the NaOH treatment. More importantly, it widens mesoporous distribution and forms interconnected mesoporous channels. The catalytic performance of Baeyer–Villiger oxidation on the interconnected mesoporous and hollow Sn-Si mixed oxide microspheres with 2-adamantanone and hydrogen peroxide was 9.4 times higher than that of the sample synthesized without the addition of CTAB; 2.3 times that of the untreated parent, which was due to the excellent diffusion properties derived from the hollow and interconnected mesopore structure. This method is mild, simple, low-cost, and can be continuously produced, which has the prospect of industrial application. Furthermore, the fundamentals of this study provide new insights for the rational design and preparation of highly interlinked mesoporous and hollow metal-oxides with unique catalytic performances.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"60 34","pages":""},"PeriodicalIF":3.9,"publicationDate":"2023-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138594721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Flavin-dependent monooxygenases (FMOs) have raised substantial interest as catalysts in monooxygenation reactions, impacting diverse fields such as drug metabolism, environmental studies, and natural product synthesis. Their application in biocatalysis boasts several advantages over conventional chemical catalysis, such as heightened selectivity, safety, sustainability, and eco-friendliness. In the realm of biomedicine, FMOs are pivotal in antibiotic research, significantly influencing the behavior of natural products, antimicrobial agents, and the pathways critical to drug synthesis They are also underscored as potential pharmaceutical targets, pivotal in opposing disease progression and viable for therapeutic intervention. Additionally, FMOs play a substantial role in environmental science, especially in pesticide processing and in preserving plant vitality. Their involvement in the biosynthesis of compounds like polyethers, tropolones, and ω-hydroxy fatty acids, with remarkable regio- and stereoselectivity, renders them indispensable in drug discovery and development. As our comprehension of FMOs’ catalytic mechanisms and structures advances, through the use of cutting-edge biotechnologies like computational design and directed evolution, FMOs are poised to occupy an increasingly significant role in both scientific exploration and industrial applications.
{"title":"Recent Applications of Flavin-Dependent Monooxygenases in Biosynthesis, Pharmaceutical Development, and Environmental Science","authors":"Yuze Guan, Xi Chen","doi":"10.3390/catal13121495","DOIUrl":"https://doi.org/10.3390/catal13121495","url":null,"abstract":"Flavin-dependent monooxygenases (FMOs) have raised substantial interest as catalysts in monooxygenation reactions, impacting diverse fields such as drug metabolism, environmental studies, and natural product synthesis. Their application in biocatalysis boasts several advantages over conventional chemical catalysis, such as heightened selectivity, safety, sustainability, and eco-friendliness. In the realm of biomedicine, FMOs are pivotal in antibiotic research, significantly influencing the behavior of natural products, antimicrobial agents, and the pathways critical to drug synthesis They are also underscored as potential pharmaceutical targets, pivotal in opposing disease progression and viable for therapeutic intervention. Additionally, FMOs play a substantial role in environmental science, especially in pesticide processing and in preserving plant vitality. Their involvement in the biosynthesis of compounds like polyethers, tropolones, and ω-hydroxy fatty acids, with remarkable regio- and stereoselectivity, renders them indispensable in drug discovery and development. As our comprehension of FMOs’ catalytic mechanisms and structures advances, through the use of cutting-edge biotechnologies like computational design and directed evolution, FMOs are poised to occupy an increasingly significant role in both scientific exploration and industrial applications.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"97 4","pages":""},"PeriodicalIF":3.9,"publicationDate":"2023-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138596092","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mengling Li, Ye Wang, Lin Liu, Yanan Gao, Zhanyun Gao, Liping Zhang
In this study, coal fly ash was functionalized, using a simple one-step process (loading with Al3+ and sulfonation), to yield a solid acid catalyst (S/Al-CFA) with strong acid sites. The catalyst was then used to produce furfural from xylose in a biphasic system (H2O(NaCl)/tetrahydrofuran). The furfural yield reached 82% at 180 °C–60 min with catalyst/xylose ratio of 0.2:1.0 (w/w). With the reaction completed, all of the components could be effectively separated, and the furfural was 97.6% pure. The cycle and regeneration of the catalyst were evaluated, and the catalyst deactivation mechanism was investigated.
{"title":"Functionalized Coal Fly Ash Is an Efficient Catalyst for Synthesizing Furfural from Xylose at a Low Catalyst Load","authors":"Mengling Li, Ye Wang, Lin Liu, Yanan Gao, Zhanyun Gao, Liping Zhang","doi":"10.3390/catal13121492","DOIUrl":"https://doi.org/10.3390/catal13121492","url":null,"abstract":"In this study, coal fly ash was functionalized, using a simple one-step process (loading with Al3+ and sulfonation), to yield a solid acid catalyst (S/Al-CFA) with strong acid sites. The catalyst was then used to produce furfural from xylose in a biphasic system (H2O(NaCl)/tetrahydrofuran). The furfural yield reached 82% at 180 °C–60 min with catalyst/xylose ratio of 0.2:1.0 (w/w). With the reaction completed, all of the components could be effectively separated, and the furfural was 97.6% pure. The cycle and regeneration of the catalyst were evaluated, and the catalyst deactivation mechanism was investigated.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"141 12","pages":""},"PeriodicalIF":3.9,"publicationDate":"2023-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138598681","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalytic ozonation, with enhanced efficiency and reduced byproduct formation at lower temperatures, proved to be efficient in ethyl acetate (EA) degradation. In this work, MMn2O4 (M = Cu, Co, Ni, Mg) catalysts were prepared via a redox-precipitation method to explore the catalytic ozonation mechanism of EA. Among all the catalysts, CuMn exhibited superior catalytic activity at 120 °C, achieving nearly 100% EA conversion and above 90% CO2 selectivity with an O3/EA molar ratio of 10. Many characterizations were conducted, such as SEM, BET and XPS, for revealing the properties of the catalysts. Plentiful active sites, abundant oxygen vacancies, more acid sites and higher reduction ability contributed to the excellent performance of CuMn. Moreover, the addition of NO induced a degree of inhibition to EA conversion due to its competition for ozone. H2O had little effect on the catalytic ozonation of CuMn, as the conversion of EA could reach a stable platform at ~89% even with 5.0 vol.% of H2O. The presence of SO2 usually caused catalyst deactivation. However, the conversion could gradually recover once SO2 was discontinued due to the reactivation of ozone. A detailed reaction mechanism for catalytic ozonation was proposed via in situ DRIFTS measurements and DFT calculations.
{"title":"Catalytic Ozonation of Ethyl Acetate with Assistance of MMn2O4 (M = Cu, Co, Ni and Mg) Catalysts through In Situ DRIFTS Experiments and Density Functional Theory Calculations","authors":"Yulin Sun, Peixi Liu, Yiwei Zhang, Yong He, Yanqun Zhu, Zhihua Wang","doi":"10.3390/catal13121491","DOIUrl":"https://doi.org/10.3390/catal13121491","url":null,"abstract":"Catalytic ozonation, with enhanced efficiency and reduced byproduct formation at lower temperatures, proved to be efficient in ethyl acetate (EA) degradation. In this work, MMn2O4 (M = Cu, Co, Ni, Mg) catalysts were prepared via a redox-precipitation method to explore the catalytic ozonation mechanism of EA. Among all the catalysts, CuMn exhibited superior catalytic activity at 120 °C, achieving nearly 100% EA conversion and above 90% CO2 selectivity with an O3/EA molar ratio of 10. Many characterizations were conducted, such as SEM, BET and XPS, for revealing the properties of the catalysts. Plentiful active sites, abundant oxygen vacancies, more acid sites and higher reduction ability contributed to the excellent performance of CuMn. Moreover, the addition of NO induced a degree of inhibition to EA conversion due to its competition for ozone. H2O had little effect on the catalytic ozonation of CuMn, as the conversion of EA could reach a stable platform at ~89% even with 5.0 vol.% of H2O. The presence of SO2 usually caused catalyst deactivation. However, the conversion could gradually recover once SO2 was discontinued due to the reactivation of ozone. A detailed reaction mechanism for catalytic ozonation was proposed via in situ DRIFTS measurements and DFT calculations.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"80 12","pages":""},"PeriodicalIF":3.9,"publicationDate":"2023-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138606010","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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