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Two-step pyrolytic engineering of carbon-doped Mn3O4 with rich defects for efficient photothermal acetone oxidation 富缺陷碳掺杂Mn3O4光热丙酮高效氧化两步热解工程
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-05-05 DOI: 10.1016/j.cattod.2025.115355
Huiyang Mao , Yikui Zeng , Mingli Fu , Yun Hu
{"title":"Two-step pyrolytic engineering of carbon-doped Mn3O4 with rich defects for efficient photothermal acetone oxidation","authors":"Huiyang Mao ,&nbsp;Yikui Zeng ,&nbsp;Mingli Fu ,&nbsp;Yun Hu","doi":"10.1016/j.cattod.2025.115355","DOIUrl":"10.1016/j.cattod.2025.115355","url":null,"abstract":"<div><div>Efficient photothermal catalysts are crucial for effective light energy utilization and low-energy-driven catalytic oxidation reaction of oxygenated volatile organic compounds (OVOCs). Herein, defect-rich carbon-doped Mn<sub>3</sub>O<sub>4</sub> samples were successfully synthesized through a two-step calcination process of Mn-MIL-100 under various atmospheres. Among them, Mn<sub>3</sub>O<sub>4</sub>/C-N6A2 exhibited the optimal performance, achieving a 91 % CO<sub>2</sub> yield and a 92 % acetone conversion under the entire spectrum simulated sunlight while maintaining stability for at least 100 h. The high activity can be due to the beneficial synergies of carbon's photothermal-assisted properties, numerous oxygen vacancies, and Mn<sup>3+</sup> active sites. Additionally, carbon doping could also improve the catalytic performance of Mn<sub>3</sub>O<sub>4</sub> by enhancing light-absorbing capacity, charge transmission efficiency, and reactive oxygen species (ROS) formation. Furthermore, light-driven thermocatalysis, photoactivation, and photocatalysis coexist, ensuring an efficient and sustained photothermal catalytic acetone oxidation. Besides, oxygen vacancies accelerated the adsorption and activation of gaseous oxygen and promoted intermediates such as acetaldehyde and carboxylate, deep oxidation into CO<sub>2</sub> and H<sub>2</sub>O. Therefore, this study offers an innovative approach to designing and fabricating efficient carbon-doped metal oxide photothermal catalysts.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"457 ","pages":"Article 115355"},"PeriodicalIF":5.2,"publicationDate":"2025-05-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143921854","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
Formic acid dehydrogenation and use as H-donor in 5-hydroxymethylfurfural hydrodeoxygenation over Pd/C3N4 catalysts 甲酸脱氢并作为h给体在Pd/C3N4催化剂上进行5-羟甲基糠醛加氢脱氧
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-04-30 DOI: 10.1016/j.cattod.2025.115353
M. Achour , D. Álvarez-Hernández , C. Megías-Sayago , F. Ammari , M.A. Centeno , S. Ivanova
{"title":"Formic acid dehydrogenation and use as H-donor in 5-hydroxymethylfurfural hydrodeoxygenation over Pd/C3N4 catalysts","authors":"M. Achour ,&nbsp;D. Álvarez-Hernández ,&nbsp;C. Megías-Sayago ,&nbsp;F. Ammari ,&nbsp;M.A. Centeno ,&nbsp;S. Ivanova","doi":"10.1016/j.cattod.2025.115353","DOIUrl":"10.1016/j.cattod.2025.115353","url":null,"abstract":"<div><div>This work studies the behavior of a series of Pd/C<sub>3</sub>N<sub>4</sub> catalyst in the reaction of formic acid dehydrogenation and the use of the latter as H-donor for 2,5-hydroxymethyl furfural hydrodeoxygenation. Firstly, a series of supports have been synthesized from melamine and urea as a function of precursors ratio and temperature of their condensation. The different synthetic conditions resulted in materials with very different specific surface areas and N-containing groups on the surface which influenced Pd deposition. The resulting defects facilitated enhanced electron transfer from nitrogen to Pd due to the close positioning of Pd nanoparticles near nitrogen sites. Consequently, the physicochemical and catalytic properties of the materials were notably impacted.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"457 ","pages":"Article 115353"},"PeriodicalIF":5.2,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143908110","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
Bimetallic palladium and copper single atoms catalyst boosting direct oxidation of methane to formaldehyde with 100 % selectivity at room temperature 双金属钯和铜单原子催化剂在室温下以100% %的选择性促进甲烷直接氧化成甲醛
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-04-29 DOI: 10.1016/j.cattod.2025.115354
Chuanhao Yao , Baiyang Yu , Wulin Li , Shoujie Zhang , Yun Guo , Xuan Tang , Yang Lou
{"title":"Bimetallic palladium and copper single atoms catalyst boosting direct oxidation of methane to formaldehyde with 100 % selectivity at room temperature","authors":"Chuanhao Yao ,&nbsp;Baiyang Yu ,&nbsp;Wulin Li ,&nbsp;Shoujie Zhang ,&nbsp;Yun Guo ,&nbsp;Xuan Tang ,&nbsp;Yang Lou","doi":"10.1016/j.cattod.2025.115354","DOIUrl":"10.1016/j.cattod.2025.115354","url":null,"abstract":"<div><div>Direct oxidation of methane (DOM) to sole value-added products (such as HCHO, etc.) at room temperature is of great importance for synthesis of commodity chemicals but still remains challenging. Herein, we design and construct ZSM-5 supported bimetallic palladium and copper single atoms catalysts (Pd<sub>1</sub>-Cu<sub>1</sub>/ZSM-5) via modified co-adsorption strategy to promote the DOM by using molecular oxygen (O<sub>2</sub>) with the assistance of hydrogen (H<sub>2</sub>) at room temperature. The Pd<sub>1</sub>-Cu<sub>1</sub>/ZSM-5 achieves a remarkable formaldehyde selectivity of 100 % (yield of 22.7 μmol·g<sub>cat</sub><sup>−1</sup>·h<sup>−1</sup>) at room temperature and the reaction atmosphere is out of the explosive limits of CH<sub>4</sub>/H<sub>2</sub>/O<sub>2</sub> systems. The characterization results demonstrate that the synergistic effect between palladium and copper facilitates the formation of highly reactive surface hydroxyl species to activate C-H bonds of CH<sub>4</sub>, which is the key for the high performance of DOM over Pd<sub>1</sub>-Cu<sub>1</sub>/ZSM-5 compared with that of sole Pd and Cu single atom catalysts (Pd<sub>1</sub>/ZSM-5 and Cu<sub>1</sub>/ZSM-5). This work provides a new direction for DOM to sole value-added products with O<sub>2</sub> at room temperature via designing single atom center catalysts.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"457 ","pages":"Article 115354"},"PeriodicalIF":5.2,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143908108","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
Catalytic CO2 methanation for biogas upgrading using a polytropic fixed bed reactor 用多向固定床反应器催化CO2甲烷化处理沼气
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-04-29 DOI: 10.1016/j.cattod.2025.115351
P. Aragüés-Aldea, R.G. Pizarro, P. Durán, V.D. Mercader, E. Francés, J.A. Peña, J. Herguido
{"title":"Catalytic CO2 methanation for biogas upgrading using a polytropic fixed bed reactor","authors":"P. Aragüés-Aldea,&nbsp;R.G. Pizarro,&nbsp;P. Durán,&nbsp;V.D. Mercader,&nbsp;E. Francés,&nbsp;J.A. Peña,&nbsp;J. Herguido","doi":"10.1016/j.cattod.2025.115351","DOIUrl":"10.1016/j.cattod.2025.115351","url":null,"abstract":"<div><div>The experiments of this study aim to determine the effect of distributed feeding of reactants throughout the many inlets of a polytropic fixed bed reactor. The effect of dosing either carbon dioxide or hydrogen, was analyzed on the <em>Sabatier</em> reaction (i.e., carbon dioxide methanation) using a Ni-Mn catalyst to carry out the biogas upgrading process. This work analyzes the influence of three feeding configurations (a conventional fixed bed, one with side distribution of biogas, and another with side distribution of hydrogen) and temperatures (350, 375, and 400 °C) for a wide <em>gas hourly space velocity</em> (<em>GHSV</em>) range from 30 × 10<sup>3</sup> (STP) mL g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup> to more than 200 × 10<sup>3</sup> (STP) mL g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup>. The molar ratios of reactants were always kept constant (H<sub>2</sub>:CH<sub>4</sub>:CO<sub>2</sub> = 12:7:3) simulating the hydrogenation of the CO<sub>2</sub> present in a biogas with a proportion of 70 <sup>v</sup>% of CH<sub>4</sub> and 30 <sup>v</sup>% of CO<sub>2</sub>.</div><div>The empirical results highlight that side distribution of biogas yields improved results over those obtained in a conventional fixed bed reactor, or the one with side distribution of hydrogen. At temperatures of 375 and 400 °C, this feeding configuration brings higher conversions than the other two, while consistently shows greater selectivities to methane for all the conditions tested. As such, its optimal condition to conduct the process is extended to methane <em>space-time yields</em> (<em>STY</em>), for which the highest methane productions are obtained. In addition, the influence of contact time, or <em>GHSV</em>, was determined to be critical both on selectivities and flowrates of methane. It is shown that for a given conversion value, keeping constant all the other parameters, a longer contact time and lower temperature result in an improvement of selectivities to methane. On the other hand, it also affects <em>STY</em> values, where an optimum between the employed flows of reactants and reaction performances is reached at a value of 180 × 10<sup>3</sup> (STP) mL g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup>, independently of experimental conditions.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"457 ","pages":"Article 115351"},"PeriodicalIF":5.2,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143901979","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
Al/Cu-pillared clay catalyzes CO2 valorization driven by UV and Vis light 铝/铜柱粘土在紫外和可见光驱动下催化CO2增值
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-04-29 DOI: 10.1016/j.cattod.2025.115357
Rosaura Peña , Rubi Romero , Héctor Barrera , Armando Ramírez-Serrano , Eduardo Martín del Campo , Reyna Natividad
{"title":"Al/Cu-pillared clay catalyzes CO2 valorization driven by UV and Vis light","authors":"Rosaura Peña ,&nbsp;Rubi Romero ,&nbsp;Héctor Barrera ,&nbsp;Armando Ramírez-Serrano ,&nbsp;Eduardo Martín del Campo ,&nbsp;Reyna Natividad","doi":"10.1016/j.cattod.2025.115357","DOIUrl":"10.1016/j.cattod.2025.115357","url":null,"abstract":"<div><div>Pillared interlayer clay (PILC) is a low-cost material with great specific surface area, large pore volume and surface acidity that ensures its effectiveness in catalytic reactions. In this work, Al pillars and Cu ions were inserted between layers of a natural silicate clay mineral (bentonite) by cation exchange to constitute the PILC (Al/Cu-PILC) and characterized by atomic absorption spectrometry (AAS), X-ray diffraction (XRD), ammonia adsorption, infrared spectroscopy (IR), TEM, scanning electron microscopy and energy-dispersive spectrometry (SEM-EDS), N<sub>2</sub> adsorption–desorption and X-Ray photoelectron spectroscopy (XPS). Then Al/Cu-PILC was evaluated as photocatalyst for CO<sub>2</sub> reduction. The characterization results confirmed a successful pillaring process that increased the basal space and specific surface area of initial bentonite. The catalyst showed activity for CO<sub>2</sub> photoreduction. The reaction products were identified by gas and liquid chromatography and formic acid was identified as the major product. The studied variables were the effect of the catalyst loading, wavelength, and reactor type; for this purpose, four catalyst concentrations were tested (0.03, 0.055, 0.11 and 0.5 g L<sup>−1</sup>), UV light and visible light were also studied, the performance of a typical semi-batch stirred tank reactor (STR) and capillary reactor was compared. The highest specific productivity corresponded to the catalyst loading of 0.055 g L<sup>−1</sup> (3926 μmol⋅g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup>). The highly efficient photocatalytic activities of Al/Cu-PILC for the reduction process of CO<sub>2</sub> were ascribed to the synergistic effect by incorporation of copper ions and the use of a capillary reactor. By probe molecules addition, photo-generated holes and hydroxyl radicals were proven to exert an important positive effect over formic acid production.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"457 ","pages":"Article 115357"},"PeriodicalIF":5.2,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143895160","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
Cu-doped TiO2 porous discs: A novel photo-enzyme catalyst for enhanced antibacterial activity and oral ulcer treatment cu掺杂TiO2多孔片:一种增强抗菌活性和治疗口腔溃疡的新型光酶催化剂
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-04-24 DOI: 10.1016/j.cattod.2025.115352
Songbo Ma , Lei Shen , Qijie Shen , Chunhua Lv , Yujuan Mao , Qinqin Liu
{"title":"Cu-doped TiO2 porous discs: A novel photo-enzyme catalyst for enhanced antibacterial activity and oral ulcer treatment","authors":"Songbo Ma ,&nbsp;Lei Shen ,&nbsp;Qijie Shen ,&nbsp;Chunhua Lv ,&nbsp;Yujuan Mao ,&nbsp;Qinqin Liu","doi":"10.1016/j.cattod.2025.115352","DOIUrl":"10.1016/j.cattod.2025.115352","url":null,"abstract":"<div><div>The global challenge of bacterial infections and antibiotic resistance underscores the urgent need for innovative antimicrobial strategies, with emerging photodynamic therapy using photocatalysts and nanozyme technologies showing promise in addressing multidrug-resistant pathogens. However, limited research exists on synergistic systems integrating both photocatalysts and nanoenzymes, highlighting a vital gap requiring systematic exploration. This study addresses this void through the rational design of copper-doped titanium dioxide (Cu-TiO<sub>2</sub>) porous disc catalysts that synergistically combine photocatalytic activity with light-activated enzymatic activity. The optimized Cu doping strategy substantially improved charge separation efficiency and redox capacity, while the hierarchical porous architecture maximized reactive oxygen species (ROS) generation through exposing of abundant active sites and enhancing mass transport of reactants. Under Xe light irradiation, the engineered Cu-TiO<sub>2</sub> demonstrated exceptional antimicrobial efficacy, achieving 99.7 % eradication of ampicillin-resistant <em>Escherichia coli</em> (<em>AREC</em>) within 45 minutes and 97.5 % elimination of methicillin-resistant <em>Staphylococcus aureus</em> (<em>MRSA</em>) within 60 minutes. Notably, the integration with low-concentration H<sub>2</sub>O<sub>2</sub> under illumination activated photo-enhanced peroxidase-mimicking activity, enabling 99.3 % <em>MRSA</em> inactivation within 30 minutes. Practical validation through hydrogel-mediated treatment of oral ulcer infections confirmed accelerated wound healing and infection control. This bifunctional catalysts establishes a new paradigm for developing light-responsive antimicrobial agents, offering transformative potential for combating antibiotic-resistant infections in biomedical and environmental applications through ROS-mediated multimodal disinfection mechanisms.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"456 ","pages":"Article 115352"},"PeriodicalIF":5.2,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143881568","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
Production of high value-added phenolic compounds through lignin catalytic pyrolysis over ion-exchanged hierarchical ZSM-5 and Beta zeolites 离子交换ZSM-5和β分子筛上木质素催化热解生产高附加值酚类化合物
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-04-23 DOI: 10.1016/j.cattod.2025.115343
M.I. Ávila , M.M. Alonso-Doncel , J. Cueto , L. Briones , G. Gómez-Pozuelo , J.M. Escola , D.P. Serrano , A. Peral , J.A. Botas
{"title":"Production of high value-added phenolic compounds through lignin catalytic pyrolysis over ion-exchanged hierarchical ZSM-5 and Beta zeolites","authors":"M.I. Ávila ,&nbsp;M.M. Alonso-Doncel ,&nbsp;J. Cueto ,&nbsp;L. Briones ,&nbsp;G. Gómez-Pozuelo ,&nbsp;J.M. Escola ,&nbsp;D.P. Serrano ,&nbsp;A. Peral ,&nbsp;J.A. Botas","doi":"10.1016/j.cattod.2025.115343","DOIUrl":"10.1016/j.cattod.2025.115343","url":null,"abstract":"<div><div>Synthesised H-ZSM-5 and H-Beta zeolites with hierarchical porosity (h-H-ZSM-5 and h-H-Beta) have been ion-exchanged with alkali (Na<sup>+</sup> and K<sup>+</sup>) and alkaline-earth (Mg<sup>2+</sup>) metals and have been evaluated as catalysts to produce high value-added products through catalytic pyrolysis of lignin. In comparison with the thermal test, hierarchical zeolites in acid form are effective catalysts for lignin pyrolysis, favouring the production of valuable light compounds although reducing bio-oil* yield and increasing gas and coke formation. In this way, h-H-ZSM-5 zeolite promotes the formation of oxygenated aromatics, being guaiacols and syringols the major products. Alkali-exchanged variants of this zeolite enhance demethylation reactions improving the selectivity towards 2-methoxy-phenol and syringol, by modifying acid site properties. On the other hand, h-H-Beta zeolite, with larger pore size and stronger acidity, leads to higher concentration of oxygenated aromatics for both parent and ion-exchanged catalysts. Specifically, h-KH-Beta promotes the production of 2-methoxy-phenol and syringol. Besides, h-MgH-Beta stands out for its greater selectivity towards phenol and alkylphenols, such as dimethylphenol. Overall, the combination of accessibility, provided by the hierarchical porosity, with the different nature and strength of the acid sites, induced by the ion-exchange with alkali and alkaline-earth metals, allows tailoring the lignin catalytic pyrolysis process to selectively produce high value-added compounds.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"456 ","pages":"Article 115343"},"PeriodicalIF":5.2,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143888049","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
Efficient recycling of polyamide 6 to ε-caprolactam under mild conditions 在温和条件下聚酰胺6高效回收制备ε-己内酰胺
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-04-21 DOI: 10.1016/j.cattod.2025.115344
Yukai Jiang, Bo Feng, Yingxiu Gao, Xiaohui Liu, Yanqin Wang
{"title":"Efficient recycling of polyamide 6 to ε-caprolactam under mild conditions","authors":"Yukai Jiang,&nbsp;Bo Feng,&nbsp;Yingxiu Gao,&nbsp;Xiaohui Liu,&nbsp;Yanqin Wang","doi":"10.1016/j.cattod.2025.115344","DOIUrl":"10.1016/j.cattod.2025.115344","url":null,"abstract":"<div><div>Polyamide 6 (PA6) is a kind of engineering plastic containing N atoms, the low activity of amide linkage makes it hard to recycle under mild conditions. In this work, a solid acid catalyst, L-Nb<sub>2</sub>O<sub>5</sub> is applied to convert PA6 into ε-caprolactam and as high as 82.2 % yield was achieved at 260°C, a relatively low temperature with THF as solvent. The catalyst can be used for 5 times with little decline of catalytic activity, and can be regenerated through calcination. Catalytic mechanism investigation reveals that Lewis acidity rather than acid concentration plays a decisive role in depolymerization, whereas Brönsted acid sites exhibit an inhibitory effect on the process. Enhanced specific surface area facilitates the exposure of more acidic sites, thereby promoting depolymerization efficiency. Systematic cyclic stability assessments and scaled-up experiments confirm the system's robustness and practical viability for industrial implementation. This study ultimately establishes a facile and efficient methodology for achieving closed-loop recycling of polyamide 6 (PA6) to ε-caprolactam (CPL) through rational catalyst design.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"456 ","pages":"Article 115344"},"PeriodicalIF":5.2,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860429","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
Operando spectroscopic studies of alcohol to hydrocarbon process over HSSZ-13 with the aid of MCR-ALS analysis for active species identification 基于MCR-ALS分析的HSSZ-13上醇制烃过程的操作光谱研究
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-04-19 DOI: 10.1016/j.cattod.2025.115339
Anna Walczyk, Karolina A. Tarach, Agata Kordek, Agata Olszewska, Oliwia Rogala, Kinga Góra-Marek
{"title":"Operando spectroscopic studies of alcohol to hydrocarbon process over HSSZ-13 with the aid of MCR-ALS analysis for active species identification","authors":"Anna Walczyk,&nbsp;Karolina A. Tarach,&nbsp;Agata Kordek,&nbsp;Agata Olszewska,&nbsp;Oliwia Rogala,&nbsp;Kinga Góra-Marek","doi":"10.1016/j.cattod.2025.115339","DOIUrl":"10.1016/j.cattod.2025.115339","url":null,"abstract":"<div><div>This research examines the conversion of C<sub>1</sub> and C<sub>2</sub> alcohols to higher olefins utilizing protonic chabazite (HSSZ-13, SiAl = 11) zeolite. The study employs advanced <em>operando</em> spectroscopy techniques, including FT-IR and UV–vis, while simultaneously using mass spectrometry and gas chromatography to analyze the products. By applying identical amounts of C<sub>1</sub> and C<sub>2</sub> alcohols, the research can effectively examine the intermediates formed and coke production. Further, the same zeolite structure aids a more comprehensive understanding of reaction pathways. The <em>operando</em> FT-IR and UV–vis studies supplemented by mass spectrometry and gas chromatography results for products released from the catalyst surface provide significant information on the key intermediates involved. The similarities and discrepancies between the transformation of ethanol and methanol into olefins, according to the established hydrocarbon pool process, are noted. MCR-ALS analysis is employed for the <em>operando</em> FT-IR and UV–vis results, providing significant insights into the findings. Additionally, the research is supported by chromatographic examinations of the coke species obtained from spent catalysts.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"456 ","pages":"Article 115339"},"PeriodicalIF":5.2,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143873400","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
Enhanced ammonia synthesis over barium cerate-supported cobalt catalyst by rare-earth element doping 通过掺杂稀土元素提高钡铈支撑钴催化剂的氨合成能力
IF 5.2 2区 化学
Catalysis Today Pub Date : 2025-04-17 DOI: 10.1016/j.cattod.2025.115342
Hubert Ronduda , Małgorzata Lemańska , Urszula Ulkowska , Wojciech Patkowski , Andrzej Ostrowski , Kamil Sobczak , Wioletta Raróg-Pilecka
{"title":"Enhanced ammonia synthesis over barium cerate-supported cobalt catalyst by rare-earth element doping","authors":"Hubert Ronduda ,&nbsp;Małgorzata Lemańska ,&nbsp;Urszula Ulkowska ,&nbsp;Wojciech Patkowski ,&nbsp;Andrzej Ostrowski ,&nbsp;Kamil Sobczak ,&nbsp;Wioletta Raróg-Pilecka","doi":"10.1016/j.cattod.2025.115342","DOIUrl":"10.1016/j.cattod.2025.115342","url":null,"abstract":"<div><div>A series of BaCeO<sub>3</sub> doped with various rare-earth elements (REE = Nd, Sm, Gd) were synthesised and used as the supports for cobalt catalysts for ammonia synthesis. The effects of rare-earth dopant type and concentration on the physicochemical properties and catalytic activities were studied using, e.g., XRD, STEM-EDX, and TPD techniques. Catalyst testing revealed that the optimal doping concentration was 10 mol%, regardless of the rare-earth ion. Samarium was identified as the most effective dopant, followed by gadolinium and neodymium. The superior performance of the Co/BaCe<sub>0.9</sub>REE<sub>0.1</sub>O<sub>3–</sub><sub>δ</sub> catalysts was due to the incorporation of REE dopant into the BaCeO<sub>3</sub> structure, which increased the electron density, enabling efficient electron transfer from the support to the Co surface. This, in turn, facilitated the N<sub>2</sub> dissociative adsorption, recognised as the rate-determining step (RDS) of ammonia synthesis. In addition, the catalysts were characterised by favourable hydrogen adsorption properties (co-existence of weak and strong adsorption sites), contributing to the effective hydrogen activation under the reaction conditions. This study provides an effective approach for designing cobalt catalysts supported on perovskites, demonstrating their great potential as next-generation catalysts for ammonia synthesis.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"456 ","pages":"Article 115342"},"PeriodicalIF":5.2,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143851536","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}
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