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Conversion of blonde glycerin to acrolein using Nb2O5/SiO2 catalysts synthesized by the Pechini method
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-02-07 DOI: 10.1016/j.cattod.2025.115228
Antônio Marcelo Silva Lopes , Marcos Antônio do Nascimento Júnior , Antoninho Valentini , Sibele B.C. Pergher , Tiago Pinheiro Braga
{"title":"Conversion of blonde glycerin to acrolein using Nb2O5/SiO2 catalysts synthesized by the Pechini method","authors":"Antônio Marcelo Silva Lopes ,&nbsp;Marcos Antônio do Nascimento Júnior ,&nbsp;Antoninho Valentini ,&nbsp;Sibele B.C. Pergher ,&nbsp;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}
引用次数: 0
Sustainable energy cycles based on liquid oxygenates as carbon-neutral hydrogen carriers: A holistic vision
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-01-31 DOI: 10.1016/j.cattod.2025.115207
James G. Highfield , Agnieszka M. Ruppert , Nicolas Keller
{"title":"Sustainable energy cycles based on liquid oxygenates as carbon-neutral hydrogen carriers: A holistic vision","authors":"James G. Highfield ,&nbsp;Agnieszka M. Ruppert ,&nbsp;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}
引用次数: 0
Effect of the Sr substitution in the A-site for La1-xSrxCoO3 perovskite catalysts for the valorization of levulinic acid to produce gamma-valerolactone
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-01-27 DOI: 10.1016/j.cattod.2025.115210
Dana Arias , Alejandro Karelovic , Catherine Sepulveda , Gina Pecchi , Carla Herrera
{"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 ,&nbsp;Alejandro Karelovic ,&nbsp;Catherine Sepulveda ,&nbsp;Gina Pecchi ,&nbsp;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}
引用次数: 0
Regulating CO2/H2O ratio of Ni-N-C single-atom catalysts through hydrophobicity engineering for acidic CO2 electroreduction
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-01-24 DOI: 10.1016/j.cattod.2025.115208
Zhongyin Kang , Min Zhang , Yang Wang , Pengtao Yue , Jun Li , Xun Zhu , Qian Fu , Qiang Liao
{"title":"Regulating CO2/H2O ratio of Ni-N-C single-atom catalysts through hydrophobicity engineering for acidic CO2 electroreduction","authors":"Zhongyin Kang ,&nbsp;Min Zhang ,&nbsp;Yang Wang ,&nbsp;Pengtao Yue ,&nbsp;Jun Li ,&nbsp;Xun Zhu ,&nbsp;Qian Fu ,&nbsp;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}
引用次数: 0
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
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-01-23 DOI: 10.1016/j.cattod.2025.115211
Natalia Uricochea , Victor Uzquiano , Marta Paniagua , Gabriel Morales , Juan A. Melero
{"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 ,&nbsp;Victor Uzquiano ,&nbsp;Marta Paniagua ,&nbsp;Gabriel Morales ,&nbsp;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}
引用次数: 0
Methane tri-reforming over Ni, Ru monometallic and Ni-Ru bimetallic catalyst supported on MIL-53 metal-organic framework
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-01-21 DOI: 10.1016/j.cattod.2025.115209
Arisha Sharma, Prakash Biswas
{"title":"Methane tri-reforming over Ni, Ru monometallic and Ni-Ru bimetallic catalyst supported on MIL-53 metal-organic framework","authors":"Arisha Sharma,&nbsp;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 &gt; 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}
引用次数: 0
Facile green synthesis of highly efficient carbon nanospheres@g-C3N4 catalysts for photodegradation of Bisphenol A
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-01-18 DOI: 10.1016/j.cattod.2025.115201
Houssam-Eddine Nemamcha , Nhu-Nang Vu , Jaspal Singh , Dinh Son Tran , Cédrik Boisvert , Phuong Nguyen-Tri
{"title":"Facile green synthesis of highly efficient carbon nanospheres@g-C3N4 catalysts for photodegradation of Bisphenol A","authors":"Houssam-Eddine Nemamcha ,&nbsp;Nhu-Nang Vu ,&nbsp;Jaspal Singh ,&nbsp;Dinh Son Tran ,&nbsp;Cédrik Boisvert ,&nbsp;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}
引用次数: 0
Photoelectrocatalytic advanced oxidation of perfluoroalkyl substances in groundwaters of the Veneto Region, Italy
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-01-17 DOI: 10.1016/j.cattod.2025.115205
Alessandro Pietro Tucci , Sapia Murgolo , Cristina De Ceglie , Giuseppe Mascolo , Massimo Carmagnani , Paolo Ronco , Massimiliano Bestetti , Silvia Franz
{"title":"Photoelectrocatalytic advanced oxidation of perfluoroalkyl substances in groundwaters of the Veneto Region, Italy","authors":"Alessandro Pietro Tucci ,&nbsp;Sapia Murgolo ,&nbsp;Cristina De Ceglie ,&nbsp;Giuseppe Mascolo ,&nbsp;Massimo Carmagnani ,&nbsp;Paolo Ronco ,&nbsp;Massimiliano Bestetti ,&nbsp;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&gt;PFHpA&gt;PFHxA≈PFPeA&gt;PFBA and PFOS&gt;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}
引用次数: 0
Photoelectrochemical generation of H2O2 using hematite (α-Fe2O3) and gas diffusion electrode (GDE)
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-01-16 DOI: 10.1016/j.cattod.2025.115206
T. Imrich , T. Nakata , T. Ohno , J. Krýsa
{"title":"Photoelectrochemical generation of H2O2 using hematite (α-Fe2O3) and gas diffusion electrode (GDE)","authors":"T. Imrich ,&nbsp;T. Nakata ,&nbsp;T. Ohno ,&nbsp;J. Krýsa","doi":"10.1016/j.cattod.2025.115206","DOIUrl":"10.1016/j.cattod.2025.115206","url":null,"abstract":"<div><div>In contrast to the industrial-scale production of H<sub>2</sub>O<sub>2</sub>, electrochemical or photoelectrochemical synthesis is an environmentally friendly alternative. In this study, the photoelectrochemical generation of H<sub>2</sub>O<sub>2</sub> was investigated using a hematite (α-Fe<sub>2</sub>O<sub>3</sub>/FTO/glass) photoanode in combination with a gas diffusion electrode (GDE) modified by the incorporation of tin(II) phthalocyanine (SnPc) in its hydrophilic layer. The experiments were conducted in a photoelectrochemical cell with two compartments separated by a proton exchange membrane, under an applied bias and AM1.5 irradiation (100 mW/cm<sup>2</sup>). The amount of H<sub>2</sub>O<sub>2</sub> generated was quantified through chemical analysis using visible light spectrophotometry of the electrolyte. To assess the process efficiency, the Faradaic efficiency (<em>FE</em>) was calculated. The optimal configuration employed air as the inlet gas for the GDE and phosphate buffer (pH 6.4) as the electrolyte in the cathodic compartment. The combination of the hematite photoanode and the GDE modified with SnPc was the most effective for H<sub>2</sub>O<sub>2</sub> photoelectrochemical generation. The highest <em>FE</em> values achieved were 52.4 % for the GDE (O<sub>2</sub> reduction to H<sub>2</sub>O<sub>2</sub>) and 0.4 % for the hematite photoanode (H<sub>2</sub>O oxidation to H<sub>2</sub>O<sub>2</sub>).</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"450 ","pages":"Article 115206"},"PeriodicalIF":5.2,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143173703","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}
引用次数: 0
Effect of Ce:Ti ratio and cerium salts on the properties of mesoporous Ti-Ce oxides and their photocatalytic activity
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-01-16 DOI: 10.1016/j.cattod.2025.115204
Peter Nadrah , Mateja Knap , Tatiparthi Vikram Sagar , Andrijana Sever Škapin , Urška Lavrenčič Štangar
{"title":"Effect of Ce:Ti ratio and cerium salts on the properties of mesoporous Ti-Ce oxides and their photocatalytic activity","authors":"Peter Nadrah ,&nbsp;Mateja Knap ,&nbsp;Tatiparthi Vikram Sagar ,&nbsp;Andrijana Sever Škapin ,&nbsp;Urška Lavrenčič Štangar","doi":"10.1016/j.cattod.2025.115204","DOIUrl":"10.1016/j.cattod.2025.115204","url":null,"abstract":"<div><div>To investigate the influence of different CeO<sub>2</sub> precursors and Ce:Ti ratios, we have synthesised 8 mesoporous Ti-Ce oxides via the evaporation-induced self-assembly (EISA) method with Ce:Ti ratios between 0.2 and 20 mol%. The materials exhibited type IV isotherms and a specific surface area of 140–180 m<sup>2</sup>·g<sup>−</sup><sup>1</sup> with pore diameters in range of 3–20 nm. The crystalline phases of materials comprised predominantly anatase with a significant decrease in overall crystalline content with increasing Ce:Ti ratio. Materials with higher Ce:Ti ratio showed an increased light absorption in the visible region. Although crystalline CeO<sub>2</sub> was not detected, the presence of Ce(IV) was confirmed by X-ray photoelectron spectroscopy. For the photocatalytic experiments, we compared these materials with the TiO<sub>2</sub>-CeO<sub>2</sub> composites of our previously published syntheses to yield 16 samples synthesized via three synthesis approaches: (1) concurrent synthesis from titanium alkoxide and cerium salts in one pot, (2) synthesis of TiO<sub>2</sub> in the presence of previously-synthesised CeO<sub>2</sub> and (3) physical mixing of separately-synthesised TiO<sub>2</sub> and CeO<sub>2</sub>. Samples produced by physically mixing the separately-synthesised TiO<sub>2</sub> and CeO<sub>2</sub> showed the best photocatalytic activity towards gaseous isopropanol degradation, while the samples with TiO<sub>2</sub> synthesised in the presence of CeO<sub>2</sub> showed the best photocatalytic stability.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"449 ","pages":"Article 115204"},"PeriodicalIF":5.2,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143097918","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}
引用次数: 0
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