Pub Date : 2025-01-10DOI: 10.1016/j.cattod.2025.115185
Hannah K. Hennig , Jacob R. Schare , Reilly P. Lynch , Alex Bullock , Michael S. Baldwin , Mark E. Bussell
The CO2 hydrogenation (HYD) reaction was investigated over Ni phosphide (Ni3P, Ni12P5, Ni2P) catalysts to probe the effect of the NixPy phase on photo-thermal catalytic properties in comparison to Ni metal. The light absorption properties of 2.5 wt% NixPy/SiO2 catalysts differ substantially, with the extent of light absorption decreasing as the P/Ni molar ratio of the Ni phosphide phase increases. This finding directly impacts the photo-thermal catalytic properties as the photo-enhancement (light activity / dark activity) correlates linearly with the extent of light absorption. For comparison purposes, 2.5 wt% Ni/SiO2 catalysts were also investigated and showed high activity but suffered from low CO selectivity (57–68 %). A Ni3P/SiO2 catalyst was the most active of the Ni phosphides with high CO selectivity (>95 %), while Ni12P5/SiO2 and Ni2P/SiO2 catalysts had lower CO2 HYD activities but CO selectivities above 98 %. Upon light exposure, the NixPy/SiO2 (and Ni/SiO2) catalysts exhibited significant rises of temperature (∼200 K increase from room temperature), indicating the importance of photothermal heating in increasing the CO2 HYD rate. The findings highlight how a non-metal element (i.e., P) plays a crucial role in tailoring the photo-thermal catalytic properties of earth abundant nickel metal.
{"title":"Effect of nickel phosphide phase on the photo-thermal catalytic hydrogenation of carbon dioxide","authors":"Hannah K. Hennig , Jacob R. Schare , Reilly P. Lynch , Alex Bullock , Michael S. Baldwin , Mark E. Bussell","doi":"10.1016/j.cattod.2025.115185","DOIUrl":"10.1016/j.cattod.2025.115185","url":null,"abstract":"<div><div>The CO<sub>2</sub> hydrogenation (HYD) reaction was investigated over Ni phosphide (Ni<sub>3</sub>P, Ni<sub>12</sub>P<sub>5</sub>, Ni<sub>2</sub>P) catalysts to probe the effect of the Ni<sub>x</sub>P<sub>y</sub> phase on photo-thermal catalytic properties in comparison to Ni metal. The light absorption properties of 2.5 wt% Ni<sub>x</sub>P<sub>y</sub>/SiO<sub>2</sub> catalysts differ substantially, with the extent of light absorption decreasing as the P/Ni molar ratio of the Ni phosphide phase increases. This finding directly impacts the photo-thermal catalytic properties as the photo-enhancement (light activity / dark activity) correlates linearly with the extent of light absorption. For comparison purposes, 2.5 wt% Ni/SiO<sub>2</sub> catalysts were also investigated and showed high activity but suffered from low CO selectivity (57–68 %). A Ni<sub>3</sub>P/SiO<sub>2</sub> catalyst was the most active of the Ni phosphides with high CO selectivity (>95 %), while Ni<sub>12</sub>P<sub>5</sub>/SiO<sub>2</sub> and Ni<sub>2</sub>P/SiO<sub>2</sub> catalysts had lower CO<sub>2</sub> HYD activities but CO selectivities above 98 %. Upon light exposure, the Ni<sub>x</sub>P<sub>y</sub>/SiO<sub>2</sub> (and Ni/SiO<sub>2</sub>) catalysts exhibited significant rises of temperature (∼200 K increase from room temperature), indicating the importance of photothermal heating in increasing the CO<sub>2</sub> HYD rate. The findings highlight how a non-metal element (i.e., P) plays a crucial role in tailoring the photo-thermal catalytic properties of earth abundant nickel metal.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"449 ","pages":"Article 115185"},"PeriodicalIF":5.2,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143141446","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-07DOI: 10.1016/j.cattod.2025.115186
Francieli Martins Mayer , Mateus da Silva Carvalho , Amanda Ramos Mallmann , Ana Paula Stelzer de Oliveira , Dóris Ruiz , Ana Carla Specht Boeira , Dirléia dos Santos Lima , Maria do Carmo Rangel
The increasing demand for clean energy and for the environmental protection has driven the search for new technologies that minimize the impacts of the excessive consumption of fossil fuel. Catalytic pyrolysis emerges as a promising alternative route for producing energy and chemicals from biomass, because of its flexibility, low cost and simplicity. However, the process still requires active catalysts that can be tailored for each application. With this goal in mind, catalysts based on platinum (1 %) supported on beta zeolite with different SAR (30, 60 and 90) were evaluated in the fast pyrolysis of pre-treated medium density fiber (MDF) residues in this work. Beta zeolite was prepared using silica extracted from coal ash came from a thermoelectric plant. Non-oxygenated compounds, such as BTEX (benzene, toluene, ethylbenzene and xylenes), other monoaromatics (21.2–26.5 %), naphthalene derivatives (5–29.2 %), polyaromatics (0–6.1 %) and linear hydrocarbon (0.4–11.9 %), as well as oxygenates (1.0–11.8 %), were produced over the catalysts in contrast with oxygenates (80.2 %) and linear hydrocarbons (6.6 %) formed without any catalyst. The catalysts changed the products distribution, the amount varying according to SAR and platinum. The platinum-containing catalysts with SAR 30 and 60 produced the highest amount of BTEX (41.1 and 42.0 %, respectively), the most valuable compounds among the products and formed negligible amounts of polyaromatics (0.3 %), the main coke precursor. They also produced low amounts of oxygenates (5.3: SAR 30 and 1.4 %: SAR 60). Among the BTEX compounds, the catalyst with SAR 30 produced more benzene, toluene and xylenes than that with SAR 60 which in turn formed more ethylbenzene. The catalyst with SAR 90 was the least selective to BTEX. This work showed that platinum supported on beta zeolites (SAR 30 and 60) are promising options to produce BTEX from MDF fast pyrolysis, with the advantage of tailoring the catalysts to obtain high yields of benzene, toluene, xylenes and ethylbenzene. Moreover, the process used two kinds of residues (MDF and coal ash), contributing to environmental protection.
{"title":"Catalytic pyrolysis of MDF wastes over beta zeolite-supported platinum","authors":"Francieli Martins Mayer , Mateus da Silva Carvalho , Amanda Ramos Mallmann , Ana Paula Stelzer de Oliveira , Dóris Ruiz , Ana Carla Specht Boeira , Dirléia dos Santos Lima , Maria do Carmo Rangel","doi":"10.1016/j.cattod.2025.115186","DOIUrl":"10.1016/j.cattod.2025.115186","url":null,"abstract":"<div><div>The increasing demand for clean energy and for the environmental protection has driven the search for new technologies that minimize the impacts of the excessive consumption of fossil fuel. Catalytic pyrolysis emerges as a promising alternative route for producing energy and chemicals from biomass, because of its flexibility, low cost and simplicity. However, the process still requires active catalysts that can be tailored for each application. With this goal in mind, catalysts based on platinum (1 %) supported on beta zeolite with different SAR (30, 60 and 90) were evaluated in the fast pyrolysis of pre-treated medium density fiber (MDF) residues in this work. Beta zeolite was prepared using silica extracted from coal ash came from a thermoelectric plant. Non-oxygenated compounds, such as BTEX (benzene, toluene, ethylbenzene and xylenes), other monoaromatics (21.2–26.5 %), naphthalene derivatives (5–29.2 %), polyaromatics (0–6.1 %) and linear hydrocarbon (0.4–11.9 %), as well as oxygenates (1.0–11.8 %), were produced over the catalysts in contrast with oxygenates (80.2 %) and linear hydrocarbons (6.6 %) formed without any catalyst. The catalysts changed the products distribution, the amount varying according to SAR and platinum. The platinum-containing catalysts with SAR 30 and 60 produced the highest amount of BTEX (41.1 and 42.0 %, respectively), the most valuable compounds among the products and formed negligible amounts of polyaromatics (0.3 %), the main coke precursor. They also produced low amounts of oxygenates (5.3: SAR 30 and 1.4 %: SAR 60). Among the BTEX compounds, the catalyst with SAR 30 produced more benzene, toluene and xylenes than that with SAR 60 which in turn formed more ethylbenzene. The catalyst with SAR 90 was the least selective to BTEX. This work showed that platinum supported on beta zeolites (SAR 30 and 60) are promising options to produce BTEX from MDF fast pyrolysis, with the advantage of tailoring the catalysts to obtain high yields of benzene, toluene, xylenes and ethylbenzene. Moreover, the process used two kinds of residues (MDF and coal ash), contributing to environmental protection.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"449 ","pages":"Article 115186"},"PeriodicalIF":5.2,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143141447","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-07DOI: 10.1016/j.cattod.2025.115189
M.V. Morales , J.M. Conesa , A. Guerrero-Ruiz , I. Rodríguez-Ramos
2,5-Dimethylfuran (DMF), which is one of the most promising liquid biofuels, has garnered significant attention due to its potential to develop the utilization of biomass energy. In this work, its synthesis through the hydrodeoxygenation reaction (HDO) of 5-hydroxymethylfurfural (HMF) has been studied on Ni catalysts supported on various metal oxides and a high surface graphite (HSAG), in a batch reactor, using 1-butanol as a solvent. At 180 °C and under 30 bar H2, the catalytic activity and the predominant reaction route were found to be strongly conditioned by the nature of the support, as well as by the presence of impurities depending on the commercial HMF feedstock employed. The HSAG support turned out to be the most suitable for the HDO of HMF leading to the formation of DMF, via rupture of the C-O bonds. Additionally, the catalytic performance of Co and Cu supported on this graphitic material was studied, being Cu the one that offers the best yields to DMF (95 %), even in the absence of external hydrogen (84 %), confirming that butanol acts as a hydrogen donor in addition of solvent.
{"title":"Carbon-supported non-noble metal catalysts for efficient synthesis of the biofuel 2,5-dimethylfurfural from 5‑hydroxymethylfurfural in 1-butanol under mild conditions","authors":"M.V. Morales , J.M. Conesa , A. Guerrero-Ruiz , I. Rodríguez-Ramos","doi":"10.1016/j.cattod.2025.115189","DOIUrl":"10.1016/j.cattod.2025.115189","url":null,"abstract":"<div><div>2,5-Dimethylfuran (DMF), which is one of the most promising liquid biofuels, has garnered significant attention due to its potential to develop the utilization of biomass energy. In this work, its synthesis through the hydrodeoxygenation reaction (HDO) of 5-hydroxymethylfurfural (HMF) has been studied on Ni catalysts supported on various metal oxides and a high surface graphite (HSAG), in a batch reactor, using 1-butanol as a solvent. At 180 °C and under 30 bar H<sub>2</sub>, the catalytic activity and the predominant reaction route were found to be strongly conditioned by the nature of the support, as well as by the presence of impurities depending on the commercial HMF feedstock employed. The HSAG support turned out to be the most suitable for the HDO of HMF leading to the formation of DMF, via rupture of the C-O bonds. Additionally, the catalytic performance of Co and Cu supported on this graphitic material was studied, being Cu the one that offers the best yields to DMF (95 %), even in the absence of external hydrogen (84 %), confirming that butanol acts as a hydrogen donor in addition of solvent.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"449 ","pages":"Article 115189"},"PeriodicalIF":5.2,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143141445","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-04DOI: 10.1016/j.cattod.2025.115188
Fangwei Liu , Yilin Zhao , Kunkun Wei , Jingbo Hu , Chengyuan Liu , Yang Pan , Jianzhou Wu , Xutao Chen , Shihui Zou , Jie Fan
Methyl radicals (·CH3) are crucial intermediates in the oxidative coupling of methane (OCM) reaction mechanism, involving both heterogeneous and homogeneous processes. We quantitatively determined the concentrations of desorbed ·CH3 from meticulously synthesized Er2O3 catalysts using in situ synchrotron-based vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS). Our findings corroborate that the generation capacity of ·CH3 serves as a robust metric for describing the catalytic performance of OCM. This investigation revealed that the modulation of reactive oxygen species (O- and O2-) on the surface of various Er2O3 catalysts significantly influences the generation capability of ·CH3 radicals. Notably, the ratio of these reactive oxygen species demonstrates a positive correlation with both the concentration of ·CH3 radicals and the C2 yield. Consequently, the generation potential of ·CH3 serves as a critical linkage between the reaction performance of OCM and the surface structure of the catalyst, thereby enriching our comprehension of the intrinsic relationship between structure and performance in catalysts based on metal oxide during the OCM reaction.
{"title":"Regulating surface reactive oxygen species to promote ·CH3 generation on Er2O3 catalysts","authors":"Fangwei Liu , Yilin Zhao , Kunkun Wei , Jingbo Hu , Chengyuan Liu , Yang Pan , Jianzhou Wu , Xutao Chen , Shihui Zou , Jie Fan","doi":"10.1016/j.cattod.2025.115188","DOIUrl":"10.1016/j.cattod.2025.115188","url":null,"abstract":"<div><div>Methyl radicals (·CH<sub>3</sub>) are crucial intermediates in the oxidative coupling of methane (OCM) reaction mechanism, involving both heterogeneous and homogeneous processes. We quantitatively determined the concentrations of desorbed ·CH<sub>3</sub> from meticulously synthesized Er<sub>2</sub>O<sub>3</sub> catalysts using in situ synchrotron-based vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS). Our findings corroborate that the generation capacity of ·CH<sub>3</sub> serves as a robust metric for describing the catalytic performance of OCM. This investigation revealed that the modulation of reactive oxygen species (O<sup>-</sup> and O<sub>2</sub><sup>-</sup>) on the surface of various Er<sub>2</sub>O<sub>3</sub> catalysts significantly influences the generation capability of ·CH<sub>3</sub> radicals. Notably, the ratio of these reactive oxygen species demonstrates a positive correlation with both the concentration of ·CH<sub>3</sub> radicals and the C<sub>2</sub> yield. Consequently, the generation potential of ·CH<sub>3</sub> serves as a critical linkage between the reaction performance of OCM and the surface structure of the catalyst, thereby enriching our comprehension of the intrinsic relationship between structure and performance in catalysts based on metal oxide during the OCM reaction.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"449 ","pages":"Article 115188"},"PeriodicalIF":5.2,"publicationDate":"2025-01-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143097919","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-04DOI: 10.1016/j.cattod.2024.115178
Sounak Roy , Benjaram M. Reddy , Jennifer Strunk
{"title":"Preface: Catalysis for circular economy towards sustainable energy (Indo-German conference on catalysis, BITS Pilani – Hyderabad, 20–23 September 2023)","authors":"Sounak Roy , Benjaram M. Reddy , Jennifer Strunk","doi":"10.1016/j.cattod.2024.115178","DOIUrl":"10.1016/j.cattod.2024.115178","url":null,"abstract":"","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"449 ","pages":"Article 115178"},"PeriodicalIF":5.2,"publicationDate":"2025-01-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143097461","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-03DOI: 10.1016/j.cattod.2024.115181
Duc D. La , Duy Van Lai , D. Nguyen , D. Duc Nguyen
This study uses a straightforward, surfactant-free, non-covalent self-assembly method to present the controlled synthesis of tetrakis(4-carboxyphenyl) porphyrin (TCPP) nanofibers on ZnO nanoplates. The resulting ZnO/TCPP nanocomposites were meticulously characterized using SEM, XRD, EDS, UV–vis, FTIR, and BET spectroscopy, revealing a coral-like ZnO nanosheet structure embedded within a TCPP nanofiber matrix. These nanocomposites exhibit enhanced photocatalytic degradation of Rhodamine B in aqueous solutions, significantly outperforming individual ZnO nanoplates and TCPP nanofibers. The composite material benefits from synergistic photocatalytic activity, with reduced bandgap energies of 2.20 eV for TCPP and 2.68 eV for ZnO. Under simulated sunlight, the ZnO/TCPP catalyst achieved an impressive 99.02 % Rhodamine B removal within 90 minutes. Additionally, a detailed mechanism for the photocatalytic degradation process was proposed, highlighting the potential of this novel hybrid material for environmental remediation applications.
{"title":"Self-assembled porphyrin on coral-like ZnO nanoplates: A novel hybrid for enhanced photocatalytic degradation of organic pollutants under simulated sunlight","authors":"Duc D. La , Duy Van Lai , D. Nguyen , D. Duc Nguyen","doi":"10.1016/j.cattod.2024.115181","DOIUrl":"10.1016/j.cattod.2024.115181","url":null,"abstract":"<div><div>This study uses a straightforward, surfactant-free, non-covalent self-assembly method to present the controlled synthesis of tetrakis(4-carboxyphenyl) porphyrin (TCPP) nanofibers on ZnO nanoplates. The resulting ZnO/TCPP nanocomposites were meticulously characterized using SEM, XRD, EDS, UV–vis, FTIR, and BET spectroscopy, revealing a coral-like ZnO nanosheet structure embedded within a TCPP nanofiber matrix. These nanocomposites exhibit enhanced photocatalytic degradation of Rhodamine B in aqueous solutions, significantly outperforming individual ZnO nanoplates and TCPP nanofibers. The composite material benefits from synergistic photocatalytic activity, with reduced bandgap energies of 2.20 eV for TCPP and 2.68 eV for ZnO. Under simulated sunlight, the ZnO/TCPP catalyst achieved an impressive 99.02 % Rhodamine B removal within 90 minutes. Additionally, a detailed mechanism for the photocatalytic degradation process was proposed, highlighting the potential of this novel hybrid material for environmental remediation applications.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"449 ","pages":"Article 115181"},"PeriodicalIF":5.2,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143141084","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-03DOI: 10.1016/j.cattod.2025.115184
K. Jori , M. Mizrahi , L.J. Giovanetti , J.M. Ramallo-López , D. Buceta , I.R. Arias , J.M. Blanco Trillo , M.A.López Quintela , F.G. Requejo
To produce an impact in the reduction of sulfur derivatives on the environment it is essential to further eliminate the sulfur content in fuels. Although oxidative desulfurization using low temperatures and atmospheric pressure is a very appealing alternative to the currently used, and highly energy demanding, hydrodesulfurization method, it suffers from the use of high amounts of oxidizing agents such as NO2, H2O2, and tert-butyl-hydro-peroxide, especially for the oxidation of highly oxidation-resistant compounds as thiophens. Using X-ray absorption near edge structure (XANES) spectroscopy, we show that Ag clusters of 5 atoms (Ag5) have high catalytic activities to achieve the complete oxidation (S−2 to S+6) of highly oxidation-resistant compounds, such as dibenzothiophene, tetraphenyl thiophene and asphaltene, under ambient conditions in a simple and efficient process. Additionally, an analysis regarding the effect of Ag5 concentration for possible oxidation routes for dibenzothiophene is shown. These results can open a new avenue to face the challenge of reducing the presence of sulfur compounds in fuels using simple and green approaches.
{"title":"Room temperature aerobic oxidation of thiophenes catalyzed by silver 5-atoms clusters","authors":"K. Jori , M. Mizrahi , L.J. Giovanetti , J.M. Ramallo-López , D. Buceta , I.R. Arias , J.M. Blanco Trillo , M.A.López Quintela , F.G. Requejo","doi":"10.1016/j.cattod.2025.115184","DOIUrl":"10.1016/j.cattod.2025.115184","url":null,"abstract":"<div><div>To produce an impact in the reduction of sulfur derivatives on the environment it is essential to further eliminate the sulfur content in fuels. Although oxidative desulfurization using low temperatures and atmospheric pressure is a very appealing alternative to the currently used, and highly energy demanding, hydrodesulfurization method, it suffers from the use of high amounts of oxidizing agents such as NO<sub>2</sub>, H<sub>2</sub>O<sub>2</sub>, and tert-butyl-hydro-peroxide, especially for the oxidation of highly oxidation-resistant compounds as thiophens. Using X-ray absorption near edge structure (XANES) spectroscopy, we show that Ag clusters of 5 atoms (Ag5) have high catalytic activities to achieve the complete oxidation (S<sup>−2</sup> to S<sup>+6</sup>) of highly oxidation-resistant compounds, such as dibenzothiophene, tetraphenyl thiophene and asphaltene, under ambient conditions in a simple and efficient process. Additionally, an analysis regarding the effect of Ag5 concentration for possible oxidation routes for dibenzothiophene is shown. These results can open a new avenue to face the challenge of reducing the presence of sulfur compounds in fuels using simple and green approaches.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"449 ","pages":"Article 115184"},"PeriodicalIF":5.2,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143141449","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-03DOI: 10.1016/j.cattod.2025.115183
Jianbo Wang , Jianteng Yan , Qingyan Cui , Tiesen Li , Jie Shi , Tinghai Wang , Yuanyuan Yue , Xiaojun Bao
In order to gain insight into the influence of SiO2 support particle size on the vacuum residue (VR) slurry-phase hydrocracking performance of Fe-based catalysts, a series of FeZn/SiO2 catalysts with varying SiO2 particle sizes were prepared. Characterization results show that the surface area and pore volume of the FeZn/SiO2 catalysts increase with the reduction of SiO2 particle sizes. The metals Fe and Zn species on FeZn/SiO2-S catalyst are more readily reducible via H2-TPR analysis. Notably, FeZn/SiO2-S catalyst presents higher metal dispersion and a greater degree of sulfurization compared to the other catalysts by XRD and XPS. Hydrocracking results demonstrate that the FeZn/SiO2-S catalyst achieves the lowest coke and gas yields (11.9 wt% and 0.4 wt%), respectively, and the highest VR conversion among these catalysts. The superior performance of the FeZn/SiO2-S catalyst in VR slurry-phase hydrocracking is ascribed to its enhanced hydrogenation activity, deriving from the higher dispersion and sulfurization of metals species. This suppresses the aggregation of polycyclic aromatic hydrocarbons in VR and the over-cracking of intermediate products. Additionally, the increased mesopore associated with smaller SiO2 particles facilitates to the diffusion of large VR molecules, further promoting the hydrocracking reaction.
{"title":"Effect of SiO2 support particle sizes on the performance of FeZn catalysts in VR slurry-phase hydrocracking","authors":"Jianbo Wang , Jianteng Yan , Qingyan Cui , Tiesen Li , Jie Shi , Tinghai Wang , Yuanyuan Yue , Xiaojun Bao","doi":"10.1016/j.cattod.2025.115183","DOIUrl":"10.1016/j.cattod.2025.115183","url":null,"abstract":"<div><div>In order to gain insight into the influence of SiO<sub>2</sub> support particle size on the vacuum residue (VR) slurry-phase hydrocracking performance of Fe-based catalysts, a series of FeZn/SiO<sub>2</sub> catalysts with varying SiO<sub>2</sub> particle sizes were prepared. Characterization results show that the surface area and pore volume of the FeZn/SiO<sub>2</sub> catalysts increase with the reduction of SiO<sub>2</sub> particle sizes. The metals Fe and Zn species on FeZn/SiO<sub>2</sub>-S catalyst are more readily reducible via H<sub>2</sub>-TPR analysis. Notably, FeZn/SiO<sub>2</sub>-S catalyst presents higher metal dispersion and a greater degree of sulfurization compared to the other catalysts by XRD and XPS. Hydrocracking results demonstrate that the FeZn/SiO<sub>2</sub>-S catalyst achieves the lowest coke and gas yields (11.9 wt% and 0.4 wt%), respectively, and the highest VR conversion among these catalysts. The superior performance of the FeZn/SiO<sub>2</sub>-S catalyst in VR slurry-phase hydrocracking is ascribed to its enhanced hydrogenation activity, deriving from the higher dispersion and sulfurization of metals species. This suppresses the aggregation of polycyclic aromatic hydrocarbons in VR and the over-cracking of intermediate products. Additionally, the increased mesopore associated with smaller SiO<sub>2</sub> particles facilitates to the diffusion of large VR molecules, further promoting the hydrocracking reaction.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"449 ","pages":"Article 115183"},"PeriodicalIF":5.2,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143097925","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The photothermo-catalysis is a combined multicatalytic approach that allows to overcome some drawbacks of the respective single catalytic processes as the thermocatalysis and the photocatalysis. In this work, to efficiently exploit the potentiality of the solar photothermo-catalysis, SiC/hydrotalcites-derived catalysts were prepared with a simple hydrothermal method to exploit both the thermocatalytic properties of the formed multifunctional mixed oxides and the photo(thermo)-catalytic features of the silicon carbide. Two different hydrotalcite-derived catalysts were prepared, one with Mg-Co ions and another with Zn-Co ions. This latter sample, after the addition of SiC, showed the best performance in the CO2 methanation reaction, with a CH4 selectivity maximum of 71 % in the photothermal conditions at 250 °C, strongly improving the performance of the thermocatalysis (36 % at 350 °C). The presence of SiC permitted to increase the harvesting of the solar light, to modify the basic sites of the hydrotalcite-derived catalysts, allowing an efficient CO2 activation, and to generate self-heating effects that enhanced the photo-driven thermocatalysis. Moreover, the formation of photocatalytic active species as the ZnO and the ZnAl2O4 after the calcination of the corresponding hydrotalcite precursor, led to exploit additional photocatalytic contributions to further increase the catalytic activity in the photo-promoted thermocatalytic CO2 conversion into methane. The high versatility and the several synergisms generated by the application of this hybrid catalysis with these peculiar SiC/hydrotalcite-derived catalysts can be a sustainable strategy to efficiently valorise the carbon dioxide.
{"title":"Solar-promoted photo-thermal CO2 methanation on SiC/hydrotalcites-derived catalysts","authors":"Roberto Fiorenza , Luca Calantropo , Eleonora La Greca , Leonarda Francesca Liotta , Antonino Gulino , Angelo Ferlazzo , Maria Grazia Musumeci , Giuseppe Proietto Salanitri , Sabrina Carola Carroccio , Giusy Dativo , Maria Teresa Armeli Iapichino , Salvatore Scirè , Giuliana Impellizzeri","doi":"10.1016/j.cattod.2024.115182","DOIUrl":"10.1016/j.cattod.2024.115182","url":null,"abstract":"<div><div>The photothermo-catalysis is a combined multicatalytic approach that allows to overcome some drawbacks of the respective single catalytic processes as the thermocatalysis and the photocatalysis. In this work, to efficiently exploit the potentiality of the solar photothermo-catalysis, SiC/hydrotalcites-derived catalysts were prepared with a simple hydrothermal method to exploit both the thermocatalytic properties of the formed multifunctional mixed oxides and the photo(thermo)-catalytic features of the silicon carbide. Two different hydrotalcite-derived catalysts were prepared, one with Mg-Co ions and another with Zn-Co ions. This latter sample, after the addition of SiC, showed the best performance in the CO<sub>2</sub> methanation reaction, with a CH<sub>4</sub> selectivity maximum of 71 % in the photothermal conditions at 250 °C, strongly improving the performance of the thermocatalysis (36 % at 350 °C). The presence of SiC permitted to increase the harvesting of the solar light, to modify the basic sites of the hydrotalcite-derived catalysts, allowing an efficient CO<sub>2</sub> activation, and to generate self-heating effects that enhanced the photo-driven thermocatalysis. Moreover, the formation of photocatalytic active species as the ZnO and the ZnAl<sub>2</sub>O<sub>4</sub> after the calcination of the corresponding hydrotalcite precursor, led to exploit additional photocatalytic contributions to further increase the catalytic activity in the photo-promoted thermocatalytic CO<sub>2</sub> conversion into methane. The high versatility and the several synergisms generated by the application of this hybrid catalysis with these peculiar SiC/hydrotalcite-derived catalysts can be a sustainable strategy to efficiently valorise the carbon dioxide.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"449 ","pages":"Article 115182"},"PeriodicalIF":5.2,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143141448","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A new magnetically recoverable polypyrrole supported copper based nanocatalyst was synthesized, characterized with various analytical techniques like Fourier-transform infrared spectroscopy (FTIR), Field Emission Scanning Electron Microscopy (FESEM), Energy Dispersive X-ray analysis (EDX), High Resolution Transmission Electron Microscopy (HRTEM), Thermogravimetric analysis (TGA), Vibrating Sample Magnetometry (VSM), and Inductively coupled plasma atomic emission spectroscopy (ICP-AES) analysis. The loading of copper on the surface of the catalyst was found to be 4.23 wt%. The application of the synthesized nanocatalyst was checked for the N-arylation of imidazoles. Excellent catalytic performance was obtained with easy recoverability and reusability upto six cycles. The current green protocol makes it environmentally beneficial for scale-up industries.
{"title":"Nano-architectured polypyrrole based magnetic nanocatalyst for the N- arylation of imidazoles and fused imidazoles","authors":"Sumanth Hegde, Sajin Surendran, Ajesh Vijayan, Aatika Nizam","doi":"10.1016/j.cattod.2024.115180","DOIUrl":"10.1016/j.cattod.2024.115180","url":null,"abstract":"<div><div>A new magnetically recoverable polypyrrole supported copper based nanocatalyst was synthesized, characterized with various analytical techniques like Fourier-transform infrared spectroscopy (FTIR), Field Emission Scanning Electron Microscopy (FESEM), Energy Dispersive X-ray analysis (EDX), High Resolution Transmission Electron Microscopy (HRTEM), Thermogravimetric analysis (TGA), Vibrating Sample Magnetometry (VSM), and Inductively coupled plasma atomic emission spectroscopy (ICP-AES) analysis. The loading of copper on the surface of the catalyst was found to be 4.23 wt%. The application of the synthesized nanocatalyst was checked for the <em>N-</em>arylation of imidazoles. Excellent catalytic performance was obtained with easy recoverability and reusability upto six cycles. The current green protocol makes it environmentally beneficial for scale-up industries.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"449 ","pages":"Article 115180"},"PeriodicalIF":5.2,"publicationDate":"2024-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143141081","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
扫码关注我们
求助内容：
应助结果提醒方式：
京公网安备 11010802042870号