Pub Date : 2025-02-13DOI: 10.1016/j.cattod.2025.115238
Javeria Sultana , Shomaila Noureen , Madeeha Rani , Iftikhar Ahmad , Chongqing Wang , Cui Li , Aiyeshah Alhodaib , Amir Waseem
In this study, the facile hydrothermal method was used to fabricate pristine LaNiO3 and LaNiO3/rGO composites. Three composites were prepared by altering small amount of rGO content in the composites. Various characterization techniques were utilized to investigate the physical properties of as-fabricated samples including Powder X-ray diffraction, Scanning electron microscopy, Energy-dispersive X-ray, Raman and Photoluminescence. Band gap energies calculated from UV–visible spectra using Tauc plots of LaNiO3, and LaNiO3/rGO were 2.4 eV, and 2.2 eV respectively. Photoluminescence spectrum of LaNiO3/rGO composite showed the lower peak intensity than pristine LaNiO3 and rGO, which indicates the enhanced charge separation in charge carriers. The photocatalytic performance of LaNiO3/rGO composite was evaluated by bisphenol A degradation and Cr(VI) reduction under visible light irradiation. Among all of the synthesized photocatalysts, it was proved that 15 % LaNiO3/rGO composite was an outstanding photocatalyst for BPA degradation and Cr(VI) reduction than the other reported photocatalysts. The photooxidation activity and stability of LaNiO3 was enhanced when rGO was incorporated in LaNiO3. Complete degradation of 20 ppm solution of bisphenol A and reduction of Cr(VI) solutions were achieved in 25 min and 30 min, respectively by using 40 mg of 15 % LaNiO3/rGO photocatalyst. BPA degradation and Cr(VI) reduction followed the pseudo first-order kinetics. The LaNiO3/rGO composite exhibited outstanding stability for up to five cycles.
{"title":"Visible-light-driven perovskite carbonaceous photocatalyst using LaNiO3/rGO composite for environmental remediation","authors":"Javeria Sultana , Shomaila Noureen , Madeeha Rani , Iftikhar Ahmad , Chongqing Wang , Cui Li , Aiyeshah Alhodaib , Amir Waseem","doi":"10.1016/j.cattod.2025.115238","DOIUrl":"10.1016/j.cattod.2025.115238","url":null,"abstract":"<div><div>In this study, the facile hydrothermal method was used to fabricate pristine LaNiO<sub>3</sub> and LaNiO<sub>3</sub>/rGO composites. Three composites were prepared by altering small amount of rGO content in the composites. Various characterization techniques were utilized to investigate the physical properties of as-fabricated samples including Powder X-ray diffraction, Scanning electron microscopy, Energy-dispersive X-ray, Raman and Photoluminescence. Band gap energies calculated from UV–visible spectra using Tauc plots of LaNiO<sub>3</sub>, and LaNiO<sub>3</sub>/rGO were 2.4 eV, and 2.2 eV respectively. Photoluminescence spectrum of LaNiO<sub>3</sub>/rGO composite showed the lower peak intensity than pristine LaNiO<sub>3</sub> and rGO, which indicates the enhanced charge separation in charge carriers. The photocatalytic performance of LaNiO<sub>3</sub>/rGO composite was evaluated by bisphenol A degradation and Cr(VI) reduction under visible light irradiation. Among all of the synthesized photocatalysts, it was proved that 15 % LaNiO<sub>3</sub>/rGO composite was an outstanding photocatalyst for BPA degradation and Cr(VI) reduction than the other reported photocatalysts. The photooxidation activity and stability of LaNiO<sub>3</sub> was enhanced when rGO was incorporated in LaNiO<sub>3</sub>. Complete degradation of 20 ppm solution of bisphenol A and reduction of Cr(VI) solutions were achieved in 25 min and 30 min, respectively by using 40 mg of 15 % LaNiO<sub>3</sub>/rGO photocatalyst. BPA degradation and Cr(VI) reduction followed the pseudo first-order kinetics. The LaNiO<sub>3</sub>/rGO composite exhibited outstanding stability for up to five cycles.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"451 ","pages":"Article 115238"},"PeriodicalIF":5.2,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143428653","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 pursuit of higher energy density for electrochemical energy storage systems has directed attention towards rechargeable metal-air battery chemistries, all of which function based on reversible oxygen redox, i.e., oxygen evolution and reduction reactions. This renders electrocatalyst an essential functional component, with the design/development of efficient-cum-stable electrocatalysts assuming enormous importance. However, these battery chemistries have challenges, such as the passivation of catalysts and dendrite growth at the metal anode. In this regard, after introducing the mechanistic aspects of metal-air battery chemistry, in general, the review discusses the chemistries in more specific terms, followed by highlighting the challenges and ways adopted to address them.
{"title":"A comprehensive review of metal-air batteries: Mechanistic aspects, advantages and challenges","authors":"Madhurima Barman , Manodip Pal , Rathindranath Biswas , Arnab Dutta","doi":"10.1016/j.cattod.2025.115229","DOIUrl":"10.1016/j.cattod.2025.115229","url":null,"abstract":"<div><div>The pursuit of higher energy density for electrochemical energy storage systems has directed attention towards rechargeable metal-air battery chemistries, all of which function based on reversible oxygen redox, i.e., oxygen evolution and reduction reactions. This renders electrocatalyst an essential functional component, with the design/development of efficient-cum-stable electrocatalysts assuming enormous importance. However, these battery chemistries have challenges, such as the passivation of catalysts and dendrite growth at the metal anode. In this regard, after introducing the mechanistic aspects of metal-air battery chemistry, in general, the review discusses the chemistries in more specific terms, followed by highlighting the challenges and ways adopted to address them.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"451 ","pages":"Article 115229"},"PeriodicalIF":5.2,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143422127","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}
Niobia catalysts dispersed in amorphous silica were synthesized using the Pechini method for the catalytic conversion of blonde glycerin into acrolein. The samples were calcined at 500°C and incorporated with different niobia contents: 10 %, 15 %, and 20 % by mass, designated as 10NbSi500, 15NbSi500, and 20NbSi500, respectively. The X-ray diffraction patterns revealed the formation of the TT-Nb2O5 phase, whose crystallinity depends on the calcination temperature and niobia content. FTIR spectra showed the presence of Nb-OH and Si-OH groups on the surface of the impregnated solids. Stain micrographs revealed a porous surface with Nb species, and their incorporation did not alter the silica matrix. The 15NbSi500 sample stood out with a high specific surface area (255.9 m².g⁻¹), larger pore distribution and volume (13 nm and 0.83 cm³.g⁻¹), a high concentration of acid sites (4.30 μmol.m⁻²), and a higher L/B ratio (FTIR-py results), which is crucial in reducing coke formation. The solids containing 15 % and 20 % niobia exhibited high catalytic performance after 180 min, with conversions of 96.02 % and 96.44 % and selectivity to acrolein of 76.25 % and 75.79 %, respectively. The high selectivity to acrolein was attributed to the conversion of LAS to BAS during the reaction. Catalytic tests over 600 min were conducted for 15NbSi500 and 20NbSi500. The superiority of the solid with 15 % niobia was attributed to its excellent acidic and textural properties, achieving 77 % conversion and 84 % selectivity to acrolein. After three reuse cycles, the catalyst maintained 62 % conversion and 75 % selectivity values, indicating its promise for near-industrial applications in enhancing the biodiesel production chain.
{"title":"Conversion of blonde glycerin to acrolein using Nb2O5/SiO2 catalysts synthesized by the Pechini method","authors":"Antônio Marcelo Silva Lopes , Marcos Antônio do Nascimento Júnior , Antoninho Valentini , Sibele B.C. Pergher , Tiago Pinheiro Braga","doi":"10.1016/j.cattod.2025.115228","DOIUrl":"10.1016/j.cattod.2025.115228","url":null,"abstract":"<div><div>Niobia catalysts dispersed in amorphous silica were synthesized using the Pechini method for the catalytic conversion of blonde glycerin into acrolein. The samples were calcined at 500°C and incorporated with different niobia contents: 10 %, 15 %, and 20 % by mass, designated as 10NbSi500, 15NbSi500, and 20NbSi500, respectively. The X-ray diffraction patterns revealed the formation of the TT-Nb<sub>2</sub>O<sub>5</sub> phase, whose crystallinity depends on the calcination temperature and niobia content. FTIR spectra showed the presence of Nb-OH and Si-OH groups on the surface of the impregnated solids. Stain micrographs revealed a porous surface with Nb species, and their incorporation did not alter the silica matrix. The 15NbSi500 sample stood out with a high specific surface area (255.9 m².g⁻¹), larger pore distribution and volume (13 nm and 0.83 cm³.g⁻¹), a high concentration of acid sites (4.30 μmol.m⁻²), and a higher L/B ratio (FTIR-py results), which is crucial in reducing coke formation. The solids containing 15 % and 20 % niobia exhibited high catalytic performance after 180 min, with conversions of 96.02 % and 96.44 % and selectivity to acrolein of 76.25 % and 75.79 %, respectively. The high selectivity to acrolein was attributed to the conversion of LAS to BAS during the reaction. Catalytic tests over 600 min were conducted for 15NbSi500 and 20NbSi500. The superiority of the solid with 15 % niobia was attributed to its excellent acidic and textural properties, achieving 77 % conversion and 84 % selectivity to acrolein. After three reuse cycles, the catalyst maintained 62 % conversion and 75 % selectivity values, indicating its promise for near-industrial applications in enhancing the biodiesel production chain.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"451 ","pages":"Article 115228"},"PeriodicalIF":5.2,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143372346","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 : 2025-01-31DOI: 10.1016/j.cattod.2025.115207
James G. Highfield , Agnieszka M. Ruppert , Nicolas Keller
Simple energy-dense liquid oxygenates obtained directly from biomass e.g., fermentation ethanol, or “solar methanol”, synthesised from renewable hydrogen (via PV-driven water electrolysis) and recycled carbon dioxide, could provide the basis of an energy cycle that is climate-neutral and promotes long-term sustainability in industrial chemical processing. The development of new earth-abundant heterogeneous (photo-)catalysts and associated reaction engineering promoting hydrogen release (by steam-reforming) and insertion (by CO2 hydro-deoxygenation) under mild conditions will be pivotal to its success. This review anticipates the key methodologies involved in future bio-refineries and forecasts the increasing role therein of modular and portable low-power solar concentrators as renewable (photonic and thermal) resources. The techno-economic prospects for oxygenates like acetaldehyde, ethylene glycol, and glycerol, are also considered based on their reactivity (C2) and/or a pre-existent supply glut in need of valorisation (C3). Many examples highlighting the growing importance of computational (DFT and microkinetic) modelling in catalyst development are presented.
{"title":"Sustainable energy cycles based on liquid oxygenates as carbon-neutral hydrogen carriers: A holistic vision","authors":"James G. Highfield , Agnieszka M. Ruppert , Nicolas Keller","doi":"10.1016/j.cattod.2025.115207","DOIUrl":"10.1016/j.cattod.2025.115207","url":null,"abstract":"<div><div>Simple energy-dense liquid oxygenates obtained directly from biomass e.g., fermentation ethanol, or “solar methanol”, synthesised from renewable hydrogen (via PV-driven water electrolysis) and recycled carbon dioxide, could provide the basis of an energy cycle that is climate-neutral and promotes long-term sustainability in industrial chemical processing. The development of new earth-abundant heterogeneous (photo-)catalysts and associated reaction engineering promoting hydrogen release (by steam-reforming) and insertion (by CO<sub>2</sub> hydro-deoxygenation) under mild conditions will be pivotal to its success. This review anticipates the key methodologies involved in future bio-refineries and forecasts the increasing role therein of modular and portable low-power solar concentrators as renewable (photonic and thermal) resources. The techno-economic prospects for oxygenates like acetaldehyde, ethylene glycol, and glycerol, are also considered based on their reactivity (C<sub>2</sub>) and/or a pre-existent supply glut in need of valorisation (C<sub>3</sub>). Many examples highlighting the growing importance of computational (DFT and microkinetic) modelling in catalyst development are presented.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"451 ","pages":"Article 115207"},"PeriodicalIF":5.2,"publicationDate":"2025-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143279803","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}
A series of substituted La1-xSrxCoO3 perovskites, with XSr = 0.0, 0.05, 0.1, 0.2 were used as catalysts in the liquid hydrogenation of levulinic acid at 250 °C and 5.0 MPa of H2. The solids were analyzed by elemental chemical analysis, XRD, H2-TPR, N2 physisorption at 77 K, NH3-TPD, and XPS. The catalytic activity increased as Sr-substitution increased up to 10 % of Sr. A further increase in Sr-substitution produces a significant decrease in LA conversion. The higher catalytic activity correlated with the highest amount of Co2+ species, whereas the further reduction of the catalytic activity was attributed to segregated phases. Furthermore, it was found that Sr substitution in the A-site changes the reaction mechanism for forming the main reaction product gamma-valerolactone, demonstrating that the substitution of La3+ by Sr2+ modifies the Co3+/Co2+ ratio redox pair.
{"title":"Effect of the Sr substitution in the A-site for La1-xSrxCoO3 perovskite catalysts for the valorization of levulinic acid to produce gamma-valerolactone","authors":"Dana Arias , Alejandro Karelovic , Catherine Sepulveda , Gina Pecchi , Carla Herrera","doi":"10.1016/j.cattod.2025.115210","DOIUrl":"10.1016/j.cattod.2025.115210","url":null,"abstract":"<div><div>A series of substituted La<sub>1-x</sub>Sr<sub>x</sub>CoO<sub>3</sub> perovskites, with X<sub>Sr</sub> = 0.0, 0.05, 0.1, 0.2 were used as catalysts in the liquid hydrogenation of levulinic acid at 250 °C and 5.0 MPa of H<sub>2</sub>. The solids were analyzed by elemental chemical analysis, XRD, H<sub>2</sub>-TPR, N<sub>2</sub> physisorption at 77 K, NH<sub>3</sub>-TPD, and XPS. The catalytic activity increased as Sr-substitution increased up to 10 % of Sr. A further increase in Sr-substitution produces a significant decrease in LA conversion. The higher catalytic activity correlated with the highest amount of Co<sup>2+</sup> species, whereas the further reduction of the catalytic activity was attributed to segregated phases. Furthermore, it was found that Sr substitution in the A-site changes the reaction mechanism for forming the main reaction product gamma-valerolactone, demonstrating that the substitution of La<sup>3+</sup> by Sr<sup>2+</sup> modifies the Co<sup>3+</sup>/Co<sup>2+</sup> ratio redox pair.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"450 ","pages":"Article 115210"},"PeriodicalIF":5.2,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143173704","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 : 2025-01-24DOI: 10.1016/j.cattod.2025.115208
Zhongyin Kang , Min Zhang , Yang Wang , Pengtao Yue , Jun Li , Xun Zhu , Qian Fu , Qiang Liao
Acidic electrolysis of CO2 has been considered as a promising route to inhibit carbonate formation, and enhances CO2 utilization efficiency. Suppressing hydrogen evolution reaction (HER) in the excessive H+ environment remains a considerable challenge, however, necessitating concerted efforts toward advanced catalysts and electrode designs to facilitate the CO2 diffusion. Herein, a Ni-N-C catalyst with a hydrophobic property (hydrophobic Ni-N-C) was synthesized as electrocatalyst for CO2 reduction, which showed a high faradaic efficiency of 98.9 % towards CO at 200 mA cm−2 compared to the hydrophilic Ni-N-C catalyst (77.8 %). Remarkably, when integrated into a gas diffusion electrode (GDE) in a flow cell, the hydrophobic Ni-N-C was capable of delivering carbon utilization up to 82.8 %, surpassing all of the other CO2 reduction electrocatalysts in alkaline electrolysis in the literature. Such outstanding performance could be contributed to the hydrophobic Ni-N-C with multiple three-phase interface, which provided superior gas-phase transfer channels for CO2 supply and impeded the H+-enriched on the catalyst surface, thus successfully suppressing the HER during the acidic CO2 electrolysis. This work may inspire further optimization of the wettability of catalyst electrode for electrochemical CO2 reduction and other gas consumption electrosynthesis in acidic electrolysis.
{"title":"Regulating CO2/H2O ratio of Ni-N-C single-atom catalysts through hydrophobicity engineering for acidic CO2 electroreduction","authors":"Zhongyin Kang , Min Zhang , Yang Wang , Pengtao Yue , Jun Li , Xun Zhu , Qian Fu , Qiang Liao","doi":"10.1016/j.cattod.2025.115208","DOIUrl":"10.1016/j.cattod.2025.115208","url":null,"abstract":"<div><div>Acidic electrolysis of CO<sub>2</sub> has been considered as a promising route to inhibit carbonate formation, and enhances CO<sub>2</sub> utilization efficiency. Suppressing hydrogen evolution reaction (HER) in the excessive H<sup>+</sup> environment remains a considerable challenge, however, necessitating concerted efforts toward advanced catalysts and electrode designs to facilitate the CO<sub>2</sub> diffusion. Herein, a Ni-N-C catalyst with a hydrophobic property (hydrophobic Ni-N-C) was synthesized as electrocatalyst for CO<sub>2</sub> reduction, which showed a high faradaic efficiency of 98.9 % towards CO at 200 mA cm<sup>−2</sup> compared to the hydrophilic Ni-N-C catalyst (77.8 %). Remarkably, when integrated into a gas diffusion electrode (GDE) in a flow cell, the hydrophobic Ni-N-C was capable of delivering carbon utilization up to 82.8 %, surpassing all of the other CO<sub>2</sub> reduction electrocatalysts in alkaline electrolysis in the literature. Such outstanding performance could be contributed to the hydrophobic Ni-N-C with multiple three-phase interface, which provided superior gas-phase transfer channels for CO<sub>2</sub> supply and impeded the H<sup>+</sup>-enriched on the catalyst surface, thus successfully suppressing the HER during the acidic CO<sub>2</sub> electrolysis. This work may inspire further optimization of the wettability of catalyst electrode for electrochemical CO<sub>2</sub> reduction and other gas consumption electrosynthesis in acidic electrolysis.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"450 ","pages":"Article 115208"},"PeriodicalIF":5.2,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143173702","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 : 2025-01-23DOI: 10.1016/j.cattod.2025.115211
Natalia Uricochea , Victor Uzquiano , Marta Paniagua , Gabriel Morales , Juan A. Melero
The high potential of using levulinic acid and furfural as platform molecules for the production of oxygenated adducts suitable as precursors for SAF synthesis is studied through the aldol condensation of both molecules. The research is the first-time demonstration of solventless acid-catalysed levulinic acid/furfural aldol condensation. The catalytic performance of a commercial H-USY zeolite and two post-synthetic variations thereof, with different dealumination degree and Zr loading, is analyzed, aiming at tuning the acid catalytic properties. The catalyst with an almost complete Al removal accompanied by the highest Zr wt% (Zr-USY-2) gave the best results in terms of selective conversion of furfural, pointing out to the Lewis acid sites as the main active sites to promote the aldol condensation reaction. An experimental design allowed to identify the optimal LA/FAL molar ratio (9/1) and reaction temperature (140 °C), while catalyst loading presented a minor significance. The optimization of the reaction parameters allowed to achieve a maximum furfural conversion of 88 %, combined with a yield towards the desired C10 adducts of 55 %. Furthermore, despite the catalytic performance of this material is slightly impaired in consecutive reaction cycles, it can be recovered with a thermal regeneration step, indicating a good reusability.
{"title":"Zr-modified USY zeolite as an efficient catalyst for the production of bio-jet fuel precursors from levulinic acid and furfural in the absence of solvent","authors":"Natalia Uricochea , Victor Uzquiano , Marta Paniagua , Gabriel Morales , Juan A. Melero","doi":"10.1016/j.cattod.2025.115211","DOIUrl":"10.1016/j.cattod.2025.115211","url":null,"abstract":"<div><div>The high potential of using levulinic acid and furfural as platform molecules for the production of oxygenated adducts suitable as precursors for SAF synthesis is studied through the aldol condensation of both molecules. The research is the first-time demonstration of solventless acid-catalysed levulinic acid/furfural aldol condensation. The catalytic performance of a commercial H-USY zeolite and two post-synthetic variations thereof, with different dealumination degree and Zr loading, is analyzed, aiming at tuning the acid catalytic properties. The catalyst with an almost complete Al removal accompanied by the highest Zr wt% (Zr-USY-2) gave the best results in terms of selective conversion of furfural, pointing out to the Lewis acid sites as the main active sites to promote the aldol condensation reaction. An experimental design allowed to identify the optimal LA/FAL molar ratio (9/1) and reaction temperature (140 °C), while catalyst loading presented a minor significance. The optimization of the reaction parameters allowed to achieve a maximum furfural conversion of 88 %, combined with a yield towards the desired C10 adducts of 55 %. Furthermore, despite the catalytic performance of this material is slightly impaired in consecutive reaction cycles, it can be recovered with a thermal regeneration step, indicating a good reusability.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"450 ","pages":"Article 115211"},"PeriodicalIF":5.2,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143173707","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 : 2025-01-21DOI: 10.1016/j.cattod.2025.115209
Arisha Sharma, Prakash Biswas
Methane tri-reforming (MTR) is a promising approach for the utilization of anthropogenic greenhouse gases such as CH4 and CO2 to produce syngas. In this work, the activities of monometallic (Ru, Ni) and bimetallic (Ru-Ni) catalysts supported on the alumina derived from metal-organic framework (MOF) precursors were compared for MTR. The catalysts were synthesized by impregnation technique, and their activity was investigated in a packed bed-down flow tubular reactor over a temperature range of 600–800 °C at 1 atm. The catalyst structure-activity relationship was determined with the help of extensive catalyst characterization techniques, including N2 physisorption, X-ray diffraction (XRD), temperature-programmed reduction (TPR), and CO2 temperature-programmed desorption (CO2-TPD). Experimental results demonstrated that the bimetallic catalyst was more active as compared to monometallic one. Among the bimetallic catalysts, 0.65RuNAlM-53 catalyst demonstrated comparatively high CO2 conversion (36.1 %) and an almost complete conversion of CH4 (99.9 %) with an H2/CO ratio of 3.2 at 800 °C. The 0.65RuNAlM-53 catalyst showed consistent activity for a prolonged duration of > 125 h with no carbon deposition. Based on the experimental observation, a probable reaction mechanism is proposed for the MTR. The catalyst structure was intact even after 125 h of reaction, which suggested the MOF-derived Ru-Ni bimetallic catalyst developed is very promising for MTR.
{"title":"Methane tri-reforming over Ni, Ru monometallic and Ni-Ru bimetallic catalyst supported on MIL-53 metal-organic framework","authors":"Arisha Sharma, Prakash Biswas","doi":"10.1016/j.cattod.2025.115209","DOIUrl":"10.1016/j.cattod.2025.115209","url":null,"abstract":"<div><div>Methane tri-reforming (MTR) is a promising approach for the utilization of anthropogenic greenhouse gases such as CH<sub>4</sub> and CO<sub>2</sub> to produce syngas. In this work, the activities of monometallic (Ru, Ni) and bimetallic (Ru-Ni) catalysts supported on the alumina derived from metal-organic framework (MOF) precursors were compared for MTR. The catalysts were synthesized by impregnation technique, and their activity was investigated in a packed bed-down flow tubular reactor over a temperature range of 600–800 °C at 1 atm. The catalyst structure-activity relationship was determined with the help of extensive catalyst characterization techniques, including N<sub>2</sub> physisorption, X-ray diffraction (XRD), temperature-programmed reduction (TPR), and CO<sub>2</sub> temperature-programmed desorption (CO<sub>2</sub>-TPD). Experimental results demonstrated that the bimetallic catalyst was more active as compared to monometallic one. Among the bimetallic catalysts, 0.65RuNAl<sub>M-53</sub> catalyst demonstrated comparatively high CO<sub>2</sub> conversion (36.1 %) and an almost complete conversion of CH<sub>4</sub> (99.9 %) with an H<sub>2</sub>/CO ratio of 3.2 at 800 °C. The 0.65RuNAl<sub>M-53</sub> catalyst showed consistent activity for a prolonged duration of > 125 h with no carbon deposition. Based on the experimental observation, a probable reaction mechanism is proposed for the MTR. The catalyst structure was intact even after 125 h of reaction, which suggested the MOF-derived Ru-Ni bimetallic catalyst developed is very promising for MTR.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"450 ","pages":"Article 115209"},"PeriodicalIF":5.2,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143173705","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 : 2025-01-18DOI: 10.1016/j.cattod.2025.115201
Houssam-Eddine Nemamcha , Nhu-Nang Vu , Jaspal Singh , Dinh Son Tran , Cédrik Boisvert , Phuong Nguyen-Tri
Novel Carbon nanospheres@graphitic-carbon nitride nanocomposites were successfully synthesized by a simple, inexpensive and ecofriendly chemical method (hydrothermal). The as-prepared materials Carbon nanospheres (CNS), pure g-C3N4, CNS@g-C3N4 and heat treated (HT)CNS@g-C3N4 were characterized by FTIR, Raman spectroscopy, XPS, XRD, TEM, EDX and N2-adsorption desorption, UV-Visible DRS, and Photoluminescence (PL). The photodegradation of bisphenol A (a typical endocrine disruptor) using photocatalysts was followed by HPLC-UV technique. The results show that (HT)CNS@g-C3N4 exhibits high photocatalytic efficiency for BPA degradation (99 %), which is 45 and 8.5 times greater than that of pure g-C3N4 and CNS@g-C3N4, respectively. Additionally, the (HT)CNS@g-C3N4 photocatalyst displays a high constant rate of apparent pseudo-first-order (kapp = 94.78 × 10−3 min–1) and low electrical energy per order consumption (EEO = 0.24 kWh/m3). These excellent abilities of (HT)CNS@g-C3N4 were attributed to its excellent morphological, structural and optical properties induced during the heat treatment: (i) The presence of CNS reduces the bad gap and consequently enhances the absorption of visible light and promotes the charge carriers separation, (ii) the high specific surface area and porosity and therefore availability of a high number of active sites to interact with BPA, (iii) high presence of different functional groups on the catalyst surface that enhance the interaction between the surface and BPA molecules, and (iv) The heterojunction interface created between CNS and g-C3N4 constitutes an efficient structure that enhances interfacial charge transfer and prevents direct recombination of charge carriers originating from g-C3N4. Based on the identification of the products and intermediates of the BPA photodegradation reaction, by HPLC−MS, a plausible mechanism of photocatalytic degradation of BPA using the prepared photocatalysts was proposed.
{"title":"Facile green synthesis of highly efficient carbon nanospheres@g-C3N4 catalysts for photodegradation of Bisphenol A","authors":"Houssam-Eddine Nemamcha , Nhu-Nang Vu , Jaspal Singh , Dinh Son Tran , Cédrik Boisvert , Phuong Nguyen-Tri","doi":"10.1016/j.cattod.2025.115201","DOIUrl":"10.1016/j.cattod.2025.115201","url":null,"abstract":"<div><div>Novel Carbon nanospheres@graphitic-carbon nitride nanocomposites were successfully synthesized by a simple, inexpensive and ecofriendly chemical method (hydrothermal). The as-prepared materials Carbon nanospheres (CNS), pure g-C<sub>3</sub>N<sub>4</sub>, CNS@g-C<sub>3</sub>N<sub>4</sub> and heat treated (HT)CNS@g-C<sub>3</sub>N<sub>4</sub> were characterized by FTIR, Raman spectroscopy, XPS, XRD, TEM, EDX and N<sub>2</sub>-adsorption desorption, UV-Visible DRS, and Photoluminescence (PL). The photodegradation of bisphenol A (a typical endocrine disruptor) using photocatalysts was followed by HPLC-UV technique. The results show that (HT)CNS@g-C<sub>3</sub>N<sub>4</sub> exhibits high photocatalytic efficiency for BPA degradation (99 %), which is 45 and 8.5 times greater than that of pure g-C<sub>3</sub>N<sub>4</sub> and CNS@g-C<sub>3</sub>N<sub>4</sub>, respectively. Additionally, the (HT)CNS@g-C<sub>3</sub>N<sub>4</sub> photocatalyst displays a high constant rate of apparent pseudo-first-order (k<sub>app</sub> = 94.78 × 10<sup>−3</sup> min<sup>–1</sup>) and low electrical energy per order consumption (EEO = 0.24 kWh/m<sup>3</sup>). These excellent abilities of (HT)CNS@g-C<sub>3</sub>N<sub>4</sub> were attributed to its excellent morphological, structural and optical properties induced during the heat treatment: (<em>i</em>) The presence of CNS reduces the bad gap and consequently enhances the absorption of visible light and promotes the charge carriers separation, <em>(ii)</em> the high specific surface area and porosity and therefore availability of a high number of active sites to interact with BPA, (<em>iii</em>) high presence of different functional groups on the catalyst surface that enhance the interaction between the surface and BPA molecules, and (<em>iv</em>) The heterojunction interface created between CNS and g-C<sub>3</sub>N<sub>4</sub> constitutes an efficient structure that enhances interfacial charge transfer and prevents direct recombination of charge carriers originating from g-C<sub>3</sub>N<sub>4</sub>. Based on the identification of the products and intermediates of the BPA photodegradation reaction, by HPLC−MS, a plausible mechanism of photocatalytic degradation of BPA using the prepared photocatalysts was proposed.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"450 ","pages":"Article 115201"},"PeriodicalIF":5.2,"publicationDate":"2025-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143173706","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}
Pub Date : 2025-01-17DOI: 10.1016/j.cattod.2025.115205
Alessandro Pietro Tucci , Sapia Murgolo , Cristina De Ceglie , Giuseppe Mascolo , Massimo Carmagnani , Paolo Ronco , Massimiliano Bestetti , Silvia Franz
Photoelectrocatalysis (PEC) was applied for the degradation of PFASs in natural groundwater collected from two wells located in the Veneto Region (Italy) where a massive contamination of the aquifer was discovered. Out of 48 monitored species, up to 9 PFASs were detected. On average, the degradation rate followed the order: PFOA>PFHpA>PFHxA≈PFPeA>PFBA and PFOS>PFHpS; the concentration of PFBS and PFHxS did not change during the tests. The overall PFASs concentration decreased by 63 % in well 1 and by 65 % in well 2. PEC tests of PFOA solutions ([PFOA] = 2 μg/l; [K2SO4] = 4 mM] induced the transient formation of PFHpA, followed by PFHxA, PFPeA and PFBA, confirming the reaction pathway consisting of decarboxylation followed by a stepwise losing of CF2 units, transiently forming shorter chain intermediates. PEC efficiency was compared to photolysis. According to electrical energy per order of magnitude, PEC outperforms conventional photolysis and most of the other advanced oxidation processes reported in literature.
{"title":"Photoelectrocatalytic advanced oxidation of perfluoroalkyl substances in groundwaters of the Veneto Region, Italy","authors":"Alessandro Pietro Tucci , Sapia Murgolo , Cristina De Ceglie , Giuseppe Mascolo , Massimo Carmagnani , Paolo Ronco , Massimiliano Bestetti , Silvia Franz","doi":"10.1016/j.cattod.2025.115205","DOIUrl":"10.1016/j.cattod.2025.115205","url":null,"abstract":"<div><div>Photoelectrocatalysis (PEC) was applied for the degradation of PFASs in natural groundwater collected from two wells located in the Veneto Region (Italy) where a massive contamination of the aquifer was discovered. Out of 48 monitored species, up to 9 PFASs were detected. On average, the degradation rate followed the order: PFOA>PFHpA>PFHxA≈PFPeA>PFBA and PFOS>PFHpS; the concentration of PFBS and PFHxS did not change during the tests. The overall PFASs concentration decreased by 63 % in well 1 and by 65 % in well 2. PEC tests of PFOA solutions ([PFOA] = 2 μg/l; [K<sub><em>2</em></sub>SO<sub>4</sub>] = 4 mM] induced the transient formation of PFHpA, followed by PFHxA, PFPeA and PFBA, confirming the reaction pathway consisting of decarboxylation followed by a stepwise losing of CF<sub>2</sub> units, transiently forming shorter chain intermediates. PEC efficiency was compared to photolysis. According to electrical energy per order of magnitude, PEC outperforms conventional photolysis and most of the other advanced oxidation processes reported in literature.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"450 ","pages":"Article 115205"},"PeriodicalIF":5.2,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143172956","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}
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