Catalysis TodayPub Date : 2025-04-30DOI: 10.1016/j.cattod.2025.115356
Daniela Ramírez Espinosa , Laura Martí Montaner , Alicia Monleón-Ventura
{"title":"Layered double hydroxides as alternative catalysts for furan-based polyesters synthesis","authors":"Daniela Ramírez Espinosa , Laura Martí Montaner , Alicia Monleón-Ventura","doi":"10.1016/j.cattod.2025.115356","DOIUrl":"10.1016/j.cattod.2025.115356","url":null,"abstract":"<div><div>The development of alternative systems for the synthesis of furan-based polyesters is essential for enabling sustainable and biobased polymer production. In this work, layered double hydroxides (LDHs) containing alternative divalent (Zn<sup>2 +</sup>, Sn<sup>2+</sup>), trivalent (Sb<sup>3+</sup>) and tetravalent (Ti<sup>4+</sup>) metals to the traditional Mg<sup>2+</sup> and Al<sup>3+</sup> were synthesized and employed as catalysts for the production of poly(ethylene furanoate) (PEF) through a two-stage melt polymerization process. The X-ray diffraction data of the LDHs indicate the correct formation of crystalline structure. The catalytic performance of the LDHs was evaluated and compared to that of conventional metal catalysts. Zn/Sn/Al- and Mg/Al/Ti-based LDHs were efficient catalysts in the polymerization reaction. Interestingly, commercially available Mg/Al-based hydrotalcite afforded PEF with the highest molecular weight. Thermal properties of PEF were determined by thermogravimetric analysis and differential scanning calorimetry. All the synthesised polyesters are amorphous, exhibiting high Tg (83–87 ºC). The scalability and versatility of LDH-based catalysts were demonstrated by producing furan-based polyesters at different scales and with varying diol chain lengths from 4 to 6 carbons. The formation of poly(butylene furanoate) (PBF), poly(pentylene furanoate) (PPeB), and poly(hexylene furanoate) (PHF) was confirmed by IR and <sup>1</sup>H NMR. These results underscore the potential of LDHs as sustainable catalysts for advancing greener polymerization technologies.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"457 ","pages":"Article 115356"},"PeriodicalIF":5.2,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143935838","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}
Catalysis TodayPub Date : 2025-04-29DOI: 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 , Baiyang Yu , Wulin Li , Shoujie Zhang , Yun Guo , Xuan Tang , 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}
Catalysis TodayPub Date : 2025-04-29DOI: 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, R.G. Pizarro, P. Durán, V.D. Mercader, E. Francés, J.A. Peña, 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}
Catalysis TodayPub Date : 2025-04-29DOI: 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 , Rubi Romero , Héctor Barrera , Armando Ramírez-Serrano , Eduardo Martín del Campo , 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}
Catalysis TodayPub Date : 2025-04-24DOI: 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 , Lei Shen , Qijie Shen , Chunhua Lv , Yujuan Mao , 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}
Catalysis TodayPub Date : 2025-04-23DOI: 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 , M.M. Alonso-Doncel , J. Cueto , L. Briones , G. Gómez-Pozuelo , J.M. Escola , D.P. Serrano , A. Peral , 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}
Catalysis TodayPub Date : 2025-04-21DOI: 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, Bo Feng, Yingxiu Gao, Xiaohui Liu, 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}
Catalysis TodayPub Date : 2025-04-19DOI: 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, Karolina A. Tarach, Agata Kordek, Agata Olszewska, Oliwia Rogala, 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}
Catalysis TodayPub Date : 2025-04-17DOI: 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 , Małgorzata Lemańska , Urszula Ulkowska , Wojciech Patkowski , Andrzej Ostrowski , Kamil Sobczak , 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}
Catalysis TodayPub Date : 2025-04-17DOI: 10.1016/j.cattod.2025.115340
Raúl Murciano, M. Teresa Navarro, Agustín Martínez
{"title":"One-pass conversion of syngas to BTX/para-xylene aromatics over tandem oxide-zeolite catalysts based on large crystal size HZSM-5","authors":"Raúl Murciano, M. Teresa Navarro, Agustín Martínez","doi":"10.1016/j.cattod.2025.115340","DOIUrl":"10.1016/j.cattod.2025.115340","url":null,"abstract":"<div><div>The one-pass conversion of renewable syngas into aromatics, particularly to BTX (benzene, toluene, xylenes) and <em>para</em>-xylene (PX), represents a promising approach to produce high-value sustainable chemicals from non-fossil resources. In this work, a systematic study of the modification of HZSM-5 zeolite by surface silylation and incorporation of MgO was performed aiming at maximising the BTX and PX selectivity in the syngas-to-aromatics (STA) reaction using tandem Zn-ZrO<sub>2</sub>+HZSM-5 catalysts following the methanol route. A zeolite with unusually large crystal size was purposedly used to intensify the <em>shape selectivity</em> effect. This zeolite exhibited high BTX selectivity (53.0 % in aromatics) albeit poor stability with TOS. Generation of a proper amount of mesopores via controlled desilication improved the catalyst stability and the aromatics selectivity (from 59.2 % up to 73.2 %) at the cost of lowering the BTX selectivity. Effective passivation of the external Brønsted acid sites was reached by submitting the mesoporous zeolite to four silylation cycles with TEOS. The silylation treatment significantly raised the BTX selectivity to 52.1 % while maintaining high selectivity of total aromatics (67.9 %), but had only a moderate positive effect on PX selectivity. Incorporation of Mg species in the silylated zeolite produced the largest impact on PX selectivity, attaining an outstanding value of 76.8 % in xylenes (41.2 % in aromatics) upon loading 3 wt% Mg.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"456 ","pages":"Article 115340"},"PeriodicalIF":5.2,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860441","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}