Catalysis Today最新文献_第7页

Evaluation of the performance and detection of the oxygen reduction reaction kinetics of metal doped imine framework in proton exchange membrane fuel cells 质子交换膜燃料电池中金属掺杂亚胺骨架的性能评价及氧还原反应动力学检测

IF 5.2 2区化学

Catalysis Today Pub Date : 2025-04-14 DOI: 10.1016/j.cattod.2025.115320

Álvaro Tolosana-Moranchel , Nicolas Bibent , José Luis Gómez de la Fuente , Moulay Tahar Sougrati , Frédéric Jaouen , Diego Gianolio , María Retuerto , Sergio Rojas

{"title":"Evaluation of the performance and detection of the oxygen reduction reaction kinetics of metal doped imine framework in proton exchange membrane fuel cells","authors":"Álvaro Tolosana-Moranchel , Nicolas Bibent , José Luis Gómez de la Fuente , Moulay Tahar Sougrati , Frédéric Jaouen , Diego Gianolio , María Retuerto , Sergio Rojas","doi":"10.1016/j.cattod.2025.115320","DOIUrl":"10.1016/j.cattod.2025.115320","url":null,"abstract":"<div><div>Fe/N/C based catalysts are the best positioned ones to replace the state-of-the-art Pt-based catalysts for the oxygen reduction reaction (ORR) in Proton Exchange Membrane Fuel Cells (PEMFCs). Here, a Fe/N/C catalyst characterized by a high N/C ratio, has been synthesized from the pyrolysis of a N-rich imine-based polymer. In acidic electrolyte (0.1 M HClO<sub>4</sub>) the catalyst demonstrates notable ORR activity with E<sub>onset</sub> and E<sub>1/2</sub> values of 1.09 and 0.77 V vs. RHE, respectively. Furthermore, the catalyst’s performance has been assessed in a single cell PEMFC setup. The optimization of the membrane electrode assembly (MEA) with the Fe/N/C catalyst entails examining various ionomer to catalyst ratios (I/C) as well as two coating methods: spray coating and drop casting. The optimized MEA achieved a cell performance of 725 mA cm<sup>−2</sup> at 0.3 V and a power density close to 220 mW cm<sup>−2</sup>. In order to understand the factors influencing PEMFC polarisation curves, electrochemical impedance spectroscopy (EIS) was performed under potentiostatic conditions. The effect of operational parameters, such as ionomer to catalyst ratios (I/C) and the use of either O<sub>2</sub> or air at the anode feed, has been investigated. EIS spectra allow the calculation of the distribution of relaxation times (DRT), providing insights into the rate and resistance of the ORR process occurring at the MEA. Notably, the cathode with an I/C= 2, prepared by drop casting, exhibited superior performance attributed to reduced ORR resistances. The current density and power density reached with the 25 cm<sup>2</sup> MEA are comparable to those obtained with the 5 cm<sup>2</sup> MEA using O<sub>2</sub> as cathode reactant.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"456 ","pages":"Article 115320"},"PeriodicalIF":5.2,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860440","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

Multifunctional CaBi LDH/Ag-gC3N4 catalytic composite for sustainable pollution remediation and photochemical conversion into usable derivatives 多功能 CaBi LDH/Ag-gC3N4 催化复合材料用于可持续污染修复和光化学转化为可用衍生物

IF 5.2 2区化学

Catalysis Today Pub Date : 2025-04-12 DOI: 10.1016/j.cattod.2025.115315

Prabagar Jijoe Samuel , Challaraj Emmanuel E S , Vinod Divya , Mohammad Khalid , Mohammed H. Alqarni , Harikaranahalli Puttaiah Shivaraju

{"title":"Multifunctional CaBi LDH/Ag-gC3N4 catalytic composite for sustainable pollution remediation and photochemical conversion into usable derivatives","authors":"Prabagar Jijoe Samuel , Challaraj Emmanuel E S , Vinod Divya , Mohammad Khalid , Mohammed H. Alqarni , Harikaranahalli Puttaiah Shivaraju","doi":"10.1016/j.cattod.2025.115315","DOIUrl":"10.1016/j.cattod.2025.115315","url":null,"abstract":"<div><div>A simple methodology was devised for synthesizing the CaBi LDH/Ag-gC<sub>3</sub>N<sub>4</sub> composite using eggshell-derived calcium. Composite is a potent catalyst for converting atmospheric gases into value-added derivatives and photocatalytic remediation with antimicrobial potential. An innovative CaBi LDH/Ag-gC<sub>3</sub>N<sub>4</sub> was effectively fabricated using solvothermal and hydrothermal techniques and was subjected to sophisticated characterizations. Enhanced crystallinity with the intact framework of Ag-gC<sub>3</sub>N<sub>4</sub> into CaBi LDH, agglomerated cloud-like structure, easy electron mobility transfer with extensive charge separation and high photocatalysis have been confirmed by characterization studies. The CaBi LDH/Ag-gC<sub>3</sub>N<sub>4</sub> composite further demonstrated photocatalytic conversion of N<sub>2</sub> and CO<sub>2</sub> into NH<sub>3</sub> (up to 84.02 µmol/L at 45 min) and functional hydrocarbon derivatives (C<sub>2</sub>H<sub>6</sub>O ∼350 μmol/L and CH<sub>3</sub>OH ∼118.2 μmol/L at 4 hr) respectively under visible light. The composite demonstrated superior photocatalytic remediation of ciprofloxacin (CPF) under visible spectrum and antibacterial efficacy against two pathogens, <em>Escherichia coli and Staphylococcus aureus</em>, supported by well suggested mechanism. The photoreduction mechanism of CaBi LDH/Ag-gC<sub>3</sub>N<sub>4</sub> is discussed, and the CB position of g-C<sub>3</sub>N<sub>4</sub> (-1.16 eV) showed comparatively having lesser value (negative) than CB of CaBi LDH (-0.73 eV). An intricate mechanism has been devised in each photocatalytic reaction to elucidate the general reactions in line with the intended reactions.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"455 ","pages":"Article 115315"},"PeriodicalIF":5.2,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143835374","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

Addressing the influence of alkaline compounds in 5-hydroxymethylfurfural oxidation and separation towards 2,5-furandicarboxylic acid 探讨碱性化合物对5-羟甲基糠醛氧化分离制备2,5-呋喃二羧酸的影响

IF 5.2 2区化学

Catalysis Today Pub Date : 2025-04-12 DOI: 10.1016/j.cattod.2025.115338

P. Díaz-Maizkurrena , J. Requies , A. Iriondo , M. Macías-Villasevil

{"title":"Addressing the influence of alkaline compounds in 5-hydroxymethylfurfural oxidation and separation towards 2,5-furandicarboxylic acid","authors":"P. Díaz-Maizkurrena , J. Requies , A. Iriondo , M. Macías-Villasevil","doi":"10.1016/j.cattod.2025.115338","DOIUrl":"10.1016/j.cattod.2025.115338","url":null,"abstract":"<div><div>The conversion of 5-hydroxymethylfurfural (HMF) into valuable chemicals is a critical challenge in biomass valorization. This study explores the degradation of HMF in the presence of various alkaline compounds (KOH, NaOH, Na<sub>2</sub>CO₃, and NaHCO<sub>3</sub>) without the use of a catalyst. The experiments showed that strong bases such as KOH and NaOH significantly accelerated HMF degradation, even under cold storage conditions, while weaker bases (Na<sub>2</sub>CO<sub>3</sub> and NaHCO<sub>3</sub>) exhibited slower degradation rates. Additionally, the aerobic oxidation of HMF to 2,5-furandicarboxylic acid (FDCA) was evaluated using a Pt-Bi/C catalyst under different alkaline conditions. Results indicated that the type and strength of the alkaline compound strongly influenced FDCA yield, with intermediate bases such as Na<sub>2</sub>CO<sub>3</sub> providing the highest yields (up to 99.3 %). The study also examined the post-reaction addition of alkaline compounds, revealing that this step is essential for dissolving FDCA, which may precipitate as a solid under acidic conditions. Two methods for FDCA separation and recovery were assessed: precipitation with HCl and dissolution in isopropanol. Both methods proved effective, with the HCl method yielding crystalline FDCA and isopropanol offering a more environmentally friendly alternative. These findings provide valuable insights into optimising reaction conditions for HMF valorization and improving FDCA recovery processes.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"456 ","pages":"Article 115338"},"PeriodicalIF":5.2,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143873399","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

Ethane ODH with CO2 over alumina-supported Fe-Ni-O mixed oxides catalysts 乙烷ODH与CO2在氧化铝负载的Fe-Ni-O混合氧化物催化剂上的反应

IF 5.2 2区化学

Catalysis Today Pub Date : 2025-04-11 DOI: 10.1016/j.cattod.2025.115317

Gustavo do N. Franceschini , Patricia Concepcion , Marcio Schwaab , Joaquín Martínez-Triguero , José M. Lopez Nieto

{"title":"Ethane ODH with CO2 over alumina-supported Fe-Ni-O mixed oxides catalysts","authors":"Gustavo do N. Franceschini , Patricia Concepcion , Marcio Schwaab , Joaquín Martínez-Triguero , José M. Lopez Nieto","doi":"10.1016/j.cattod.2025.115317","DOIUrl":"10.1016/j.cattod.2025.115317","url":null,"abstract":"<div><div>The dehydrogenation of ethane in the presence of CO<sub>2</sub> on alumina supported Fe-Ni-O catalysts was studied. The Fe/Ni ratio in catalysts strongly influences both the conversion of ethane and CO<sub>2</sub> and the nature of reaction products. Iron species, linked to the hematite phase (α-Fe<sub>3</sub>O<sub>4</sub>), favors ethane ODH but also the RWGS and dry reforming reactions (as parallel reactions). Nickel oxide has a high catalytic activity due to its capacity to break both C-H and C<img>C bonds in a non-selective way, facilitating the generation of CO. Characterization results show changes in catalysts during the reaction. The H<sub>2</sub>-TPR patterns of catalysts suggest a low interaction between the support and the iron particles, and a parallelism between the reducibility of iron particles and the conversion of reactants. In addition, all catalysts suffer important restructuration under reaction conditions, with iron oxide segregates to the catalyst surface together with a partial reduction of Fe<sup>3</sup><sup>+</sup> to Fe<sup>2+</sup> (as determined by XPS). These changes could be confirmed by XRD, Raman, XPS and UV–vis spectroscopy analyses. Temperature programmed surface reactions (TPSR), under different experimental conditions, indicate an important role of nickel in the bimetallic catalysts, avoiding severe reduction of the catalyst and stabilizing different types of iron oxide species with different selectivity to products.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"455 ","pages":"Article 115317"},"PeriodicalIF":5.2,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143843702","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

Influence of CO2 presence on propane conversion routes over Cr- and Ga-doped PtCe/Al2O3 catalysts CO2存在对Cr和ga掺杂PtCe/Al2O3催化剂丙烷转化路线的影响

IF 5.2 2区化学

Catalysis Today Pub Date : 2025-04-11 DOI: 10.1016/j.cattod.2025.115318

D. Ballesteros-Plata , I. Barroso-Martín , J.A. Cecilia , P. Concepción , J.M. López Nieto , E. Rodríguez-Castellón , A. Infantes-Molina

{"title":"Influence of CO2 presence on propane conversion routes over Cr- and Ga-doped PtCe/Al2O3 catalysts","authors":"D. Ballesteros-Plata , I. Barroso-Martín , J.A. Cecilia , P. Concepción , J.M. López Nieto , E. Rodríguez-Castellón , A. Infantes-Molina","doi":"10.1016/j.cattod.2025.115318","DOIUrl":"10.1016/j.cattod.2025.115318","url":null,"abstract":"<div><div>A set of catalysts containing Cr- or Ga-doped Pt-CeO<sub>2</sub> supported on alumina (PCA, Cr-PCA and Ga-PCA) were synthesized by incipient wetness impregnation and tested in propane conversion processes. The catalysts were studied in the propane conversion process with or without CO<sub>2</sub> in the feed. In all cases, an enhancement in stability was found when CO<sub>2</sub> was present in the reaction medium despite the lower catalytic activity. As well, all catalysts presented a higher propylene selectivity in the absence of CO<sub>2</sub>, indicating that the direct dehydrogenation of propane is the main reaction route. Moreover, CO<sub>2</sub>-assisted propane cracking to ethylene is favoured over propane reforming or direct cracking, given the minimal selectivity to other products like methane. With regards to the catalyst composition, Cr-PCA catalyst was the most active catalyst both in the absence and presence of CO<sub>2</sub>, due to the presence of weak acidity and coexistence of Cr<sup>3 +</sup> and Cr<sup>6+</sup> redox species, as evidenced by XPS analysis. Ga-PCA catalyst was more selective to propylene, indicating that higher acidity of weak-to-medium nature along with formation of low coordinated Ga<sup>3+</sup> species is beneficial for the CO<sub>2</sub>-ODH process. Raman, DTG and XPS analyses after reaction with CO<sub>2</sub> showed that the deactivation of the catalysts was mainly due to carbon deposits of amorphous and graphitic nature on the surface of the catalysts.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"455 ","pages":"Article 115318"},"PeriodicalIF":5.2,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143835372","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

Improved productivity in direct dimethyl ether synthesis and sorption enhanced DME synthesis using tungstosilicic acid as the acidic function 提高了直接二甲醚的合成效率，并以钨硅酸为酸性功能，吸附增强了二甲醚的合成

IF 5.2 2区化学

Catalysis Today Pub Date : 2025-04-11 DOI: 10.1016/j.cattod.2025.115319

Cristina Peinado , Dalia Liuzzi , Jurriaan Boon , Sergio Rojas

{"title":"Improved productivity in direct dimethyl ether synthesis and sorption enhanced DME synthesis using tungstosilicic acid as the acidic function","authors":"Cristina Peinado , Dalia Liuzzi , Jurriaan Boon , Sergio Rojas","doi":"10.1016/j.cattod.2025.115319","DOIUrl":"10.1016/j.cattod.2025.115319","url":null,"abstract":"<div><div>Renewable dimethyl ether (DME) can reduce the carbon footprint in LPG and transportation sectors. The direct synthesis of DME (DDMES) is attracting a great deal of attention because it is possible to increase the productivity of DME. However, DDMES is hindered by the formation of a high amount of water, which promotes the deactivation of both catalytic phases used in the DDMES, namely Cu/ZnO/Al<sub>2</sub>O<sub>3</sub> and γ-Al<sub>2</sub>O<sub>3</sub>. This is particularly relevant when CO<sub>2</sub>-rich syngas is used, since it leads to a higher production of H<sub>2</sub>O. In this work we show that heteropolyacids such as HSiW are a suitable alternative to state-of-the-art γ-Al<sub>2</sub>O<sub>3</sub> for the dehydration of methanol during the DDMES. This is because HSiW is not deactivated by the presence of water in the reaction medium. Thus, catalytic beds with HSiW reach up to four times higher DME productivity than those containing γ-Al<sub>2</sub>O<sub>3</sub>. This feature is further exacerbated when water is removed from the reactor by means of a sorbent, i.e., during the sorption enhanced direct DME synthesis (SEDMES). Thus, the total carbon conversion is higher for SEDMES than for DDMES regardless of the actual nature of the acid catalyst.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"455 ","pages":"Article 115319"},"PeriodicalIF":5.2,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143829756","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

Experimental study and statistical analysis of hydrogen yield in methane steam reforming over a hydroxyapatite-supported nickel catalyst 羟基磷灰石负载镍催化剂甲烷蒸汽重整产氢率的实验研究与统计分析

IF 5.2 2区化学

Catalysis Today Pub Date : 2025-04-11 DOI: 10.1016/j.cattod.2025.115322

Sabrina B. Karakache, Maroua Rouabah, Ryan Gosselin, Nicolas Abatzoglou, Inès E. Achouri

{"title":"Experimental study and statistical analysis of hydrogen yield in methane steam reforming over a hydroxyapatite-supported nickel catalyst","authors":"Sabrina B. Karakache, Maroua Rouabah, Ryan Gosselin, Nicolas Abatzoglou, Inès E. Achouri","doi":"10.1016/j.cattod.2025.115322","DOIUrl":"10.1016/j.cattod.2025.115322","url":null,"abstract":"<div><div>This study aimed to investigate the use of hydroxyapatite (HAp) as a catalyst support for the methane steam reforming (MSR) process. Catalysts were prepared via incipient wetness impregnation using nickel as the active metal and characterized by N<sub>2</sub> physisorption analysis, X-ray diffraction, H<sub>2</sub> temperature-programmed reduction, and transmission electron microscopy. The effects of four key parameters in hydrogen production—nickel loading (Ni wt%), inlet steam-to-methane (H<sub>2</sub>O/CH<sub>4</sub>) ratio, space velocity (SV), and temperature (T)—were evaluated via a statistical analysis. Thermodynamic calculations were also used to compare the catalyst activity results with the equilibrium conditions. The findings confirmed the effectiveness and stability of HAp as a support, exhibiting high thermal stability, coke resistance, and a mesoporous structure with an average specific surface area of 65 m<sup>2</sup>·g<sup>−1</sup>. The calcined Ni/HAp catalyst mainly comprised crystalline NiO and displayed a higher surface area of 54 m<sup>2</sup>·g<sup>−1</sup> and superior dispersion at loadings of 5 and 10 wt% Ni compared to 15 wt% Ni. The temperature, SV, and inlet reactant ratio significantly influenced the process. A long-term stability test carried out under optimal conditions over 98 h demonstrated the consistent activity and stability of the 10 wt%Ni/HAp catalyst, maintaining a high methane conversion of 99 % and yielding 90 % hydrogen, 80 % carbon monoxide, and 20 % carbon dioxide, with no observed carbon deposition on the catalyst surface.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"456 ","pages":"Article 115322"},"PeriodicalIF":5.2,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143847579","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

Specific selectivity of simple oxides towards CH4 activation 简单氧化物对CH4活化的选择性

IF 5.2 2区化学

Catalysis Today Pub Date : 2025-04-11 DOI: 10.1016/j.cattod.2025.115337

Donato Pinto , Atsushi Urakawa

{"title":"Specific selectivity of simple oxides towards CH4 activation","authors":"Donato Pinto , Atsushi Urakawa","doi":"10.1016/j.cattod.2025.115337","DOIUrl":"10.1016/j.cattod.2025.115337","url":null,"abstract":"<div><div>Simple metal oxides exhibit noticeable catalytic activity in methane conversion reactions. However, their catalytic role in the selective activation of CH<sub>4</sub> to more valuable products (CO, H<sub>2</sub>, olefins) is often masked by the highly oxidative reaction conditions and by complex catalyst formulations. Transient studies of the direct interaction of CH<sub>4</sub> with simple catalytic systems, including rare-earth (La<sub>2</sub>O<sub>3</sub>, Nd<sub>2</sub>O<sub>3</sub>, Y<sub>2</sub>O<sub>3</sub>), alkali-earth (MgO) and reducible (TiO<sub>2</sub>), reveal peculiar selectivity for different monometallic oxides. Rare-earth metal oxides show high initial activity towards partial oxidation products (CO, H<sub>2</sub>), while MgO possesses unique selectivity towards coupling products (C<sub>2</sub>H<sub>6</sub> and C<sub>2</sub>H<sub>4</sub>) with remarkable activity in dehydrogenation reactions. A continuous supply of lattice oxygen species for the selective oxidation of CH<sub>4</sub> to CO is provided by TiO<sub>2</sub>, which can effectively prevent accumulation of C deposits. The results indicate the roles played by the metal oxide materials and provide a basis for rational design of catalysts and reaction conditions for the selective conversion of CH<sub>4</sub>.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"455 ","pages":"Article 115337"},"PeriodicalIF":5.2,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143838489","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

Selective carboxylation of alkenes with CO2 to form unsaturated carboxylic acid on Sc-exchanged MFI zeolite 碳交换MFI沸石上烯烃与CO2选择性羧化生成不饱和羧酸的研究

IF 5.2 2区化学

Catalysis Today Pub Date : 2025-04-11 DOI: 10.1016/j.cattod.2025.115321

Zaheer Masood , Bin Wang

{"title":"Selective carboxylation of alkenes with CO2 to form unsaturated carboxylic acid on Sc-exchanged MFI zeolite","authors":"Zaheer Masood , Bin Wang","doi":"10.1016/j.cattod.2025.115321","DOIUrl":"10.1016/j.cattod.2025.115321","url":null,"abstract":"<div><div>Utilization of CO<sub>2</sub> in chemical synthesis as C1 carbon feedstock to introduce a carboxylic group into alkene is valuable for producing unsaturated carboxylic acids. Selective carboxylation of alkenes at targeted positions can be used to regulate the production of such specific unsaturated carboxylic acids or functionalize hydrocarbon plastics that possess residual C<img>C double bonds. In this study, we investigated the carboxylation of 1-butene and 2-butene (as representative alkene) with CO<sub>2</sub> on Sc-exchanged MFI zeolites using density functional theory calculations. We find that similar to ethylene, the carboxylation of butene is also rate-limited by the β─H transfer. We examined carboxylation at the C1 and C2 positions of 1-butene and cis and trans isomers for 2-butene. Based on activation barriers of the β─H transfer, our results demonstrate that Sc-MFI zeolite preferably carboxylates at the terminal position of butene. In the case of 2-butene, carboxylation of the trans isomer is more favorable than the cis isomer. Furthermore, We show that the energy of degenerate orbitals of C, O and H atoms (involved in the β─H transfer) in the metallalactone ring regulates the activation energy of the β─H transfer.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"455 ","pages":"Article 115321"},"PeriodicalIF":5.2,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826213","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 oxygen mobility in NiAg alloy catalysts for methane dry reforming: The role of AgO nanoparticles 甲烷干重整NiAg合金催化剂中氧迁移率的增强：AgO纳米颗粒的作用

IF 5.2 2区化学

Catalysis Today Pub Date : 2025-04-10 DOI: 10.1016/j.cattod.2025.115316

Alberth Renne Gonzalez Caranton , Ananda Vallezi Paladino Lino , Calazans Macchiutti , Jilder Dandy Peña serna , Noemi Raquel Checca Huaman , Fernando stavale , Emilia Annese , José Mansur Assaf

{"title":"Enhanced oxygen mobility in NiAg alloy catalysts for methane dry reforming: The role of AgO nanoparticles","authors":"Alberth Renne Gonzalez Caranton , Ananda Vallezi Paladino Lino , Calazans Macchiutti , Jilder Dandy Peña serna , Noemi Raquel Checca Huaman , Fernando stavale , Emilia Annese , José Mansur Assaf","doi":"10.1016/j.cattod.2025.115316","DOIUrl":"10.1016/j.cattod.2025.115316","url":null,"abstract":"<div><div>This study investigates the effect of AgO nanoparticles on oxygen mobility and catalytic performance in NiAg bimetallic alloy catalysts during the dry reforming of methane (DMR). Using sol-gel synthesized NiAgMgAl hydrotalcite precursors, the resulting catalysts were evaluated at 800 °C and 1 atm. AgO species were found to prevent sintering and protect nickel active sites under high-temperature conditions. Characterization techniques such as Near Ambient Pressure X-ray Photoelectron Spectroscopy (NAP-XPS) and Electron paramagnetic resonance (EPR) spectroscopy revealed distinct electrochemical properties related to oxygen vacancies, critical for methane and CO₂ activation. Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) confirmed efficient CH₄ and CO₂ activation, showcasing silver’s role in improving catalytic turnover frequency and preventing coke formation. The findings demonstrate that the NiAg alloy’s oxygen vacancies and nanoconfinement effects significantly enhance DRM performance, offering a promising strategy for syngas production.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"455 ","pages":"Article 115316"},"PeriodicalIF":5.2,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143824332","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