Catalysis Today最新文献

{"title":"Defective TiO2 for CO2 photoreduction: Influence of alkaline agent and reduction temperature modulation","authors":"Rudolf Ricka ,&nbsp;Agnieszka Wanag ,&nbsp;Ewelina Kusiak-Nejman ,&nbsp;Miroslava Filip Edelmannová ,&nbsp;Martin Reli ,&nbsp;Marcin Łapinski ,&nbsp;Grzegorz Słowik ,&nbsp;Antoni W. Morawski ,&nbsp;Kamila Kočí","doi":"10.1016/j.cattod.2024.115162","DOIUrl":"10.1016/j.cattod.2024.115162","url":null,"abstract":"<div><div>This study investigates the synthesis and characterization of Black TiO₂ photocatalyst (TiO_2-x) through the sol-gel method combined with NaBH₄ reduction at different temperatures (350 °C, 500 °C, and 650 °C). The photocatalytic performance for CO₂ reduction was evaluated, revealing that TiO_2-x_500°C sample exhibited the highest efficiency. This enhanced performance is mainly attributed to a higher concentration of oxygen vacancies and successful nitrogen doping resulting from ammonia water addition during synthesis. Comprehensive characterization techniques, including Raman spectroscopy, and XPS confirmed the presence of defects and their correlation with increased photocatalytic activity. These findings confirm the importance of defect engineering and doping in optimizing TiO₂-based photocatalysts for CO₂ photoreduction.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"448 ","pages":"Article 115162"},"PeriodicalIF":5.2,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143093948","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}

{"title":"Visible-light-active Rh-doped SrTiO3: Effect of Rh doping on the structural characteristics contributing to outstanding photocatalytic activity","authors":"Tamás Gyulavári ,&nbsp;Fanni Bóka ,&nbsp;Milica Todea ,&nbsp;Áron Ágoston ,&nbsp;Ákos Kukovecz ,&nbsp;Zoltán Kónya ,&nbsp;Zsolt Pap","doi":"10.1016/j.cattod.2024.115161","DOIUrl":"10.1016/j.cattod.2024.115161","url":null,"abstract":"<div><div>Strontium titanate photocatalysts were doped with rhodium (0, 1, 5, 10, and 15 at%) via a hydrothermal method to enhance their visible light absorbance. The samples were characterized by X-ray diffractometry, X-ray photoelectron spectroscopy, infrared spectroscopy, nitrogen adsorption, scanning and transmission electron microscopy, diffuse reflectance spectroscopy, and photoluminescence measurements. Their photocatalytic activity was evaluated by the photocatalytic oxidation of phenol under visible light irradiation, using the non-Rh-containing sample as a reference. All the applied rhodium was successfully incorporated into the cubic crystal lattice. Rhodium doping resulted in significantly enhanced visible light absorption and suppressed charge recombination. The photocatalytic activity was enhanced to an exceptionally large degree: the best sample completely degraded phenol in 1 h under visible light. The optimal rhodium amount was found to be 5 at%. The high photocatalytic activity was attributed to the resultant effect of enhanced visible light absorbance, suppressed charge recombination, and high Rh³⁺/Rh⁴⁺ ratio.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"447 ","pages":"Article 115161"},"PeriodicalIF":5.2,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143180474","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}

{"title":"Special issue on advances in catalysis in aqueous media","authors":"Georgios Papadogianakis,&nbsp;Roger A. Sheldon,&nbsp;Bruce H. Lipshutz,&nbsp;Paul J. Dyson","doi":"10.1016/j.cattod.2024.115163","DOIUrl":"10.1016/j.cattod.2024.115163","url":null,"abstract":"","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"447 ","pages":"Article 115163"},"PeriodicalIF":5.2,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143180476","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}

{"title":"Dry reforming of methane over Ni catalysts supported on hierarchical ZSM-5 and USY zeolites","authors":"Amanda C.P. Guimarães ,&nbsp;Lícia R.F. Coelho ,&nbsp;Andressa A.A. Silva ,&nbsp;Yutao Xing ,&nbsp;Rita C. Colman ,&nbsp;Lisiane V. Mattos ,&nbsp;Cristiane A. Henriques","doi":"10.1016/j.cattod.2024.115159","DOIUrl":"10.1016/j.cattod.2024.115159","url":null,"abstract":"<div><div>In this study, 3 wt% of Ni supported on hierarchical ZSM-5 and USY zeolites were prepared using desilication and dealumination/desilication methods, respectively. These catalysts were used to produce syngas via dry reforming of methane. Mesoporosity was introduced in both zeolites, leading to increased initial values of CH₄ and CO₂ conversions, possibly attributable to higher Ni dispersion. The catalyst supported on hierarchical ZSM-5 exhibited a good NiO/Ni^2 + species distribution, an improved metal-support interface, and strong basicity. These aspects of the catalyst increased the number of accessible Ni active sites, resulting in higher stability, lower carbon formation, and reduced metal sintering. The inferior performance of the hierarchical USY-based catalyst could be ascribed to a greater quantity of trapped Ni²⁺ species within smaller pores, thus reducing their reducibility and hindering the accessibility of reagents to metal and basic sites.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"447 ","pages":"Article 115159"},"PeriodicalIF":5.2,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143180469","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}

{"title":"Surface tuning of a highly crystalline Ni/LaAlO3 perovskite catalyst obtained from aluminum saline slags using various synthesis methods for the dry reforming of methane","authors":"H.J. Muñoz,&nbsp;S.A. Korili,&nbsp;A. Gil","doi":"10.1016/j.cattod.2024.115158","DOIUrl":"10.1016/j.cattod.2024.115158","url":null,"abstract":"&lt;div&gt;&lt;div&gt;This research presents the first synthesis of nickel-modified lanthanum aluminate (Ni/LaAlO&lt;sub&gt;3&lt;/sub&gt;) perovskite from aluminum (Al) saline slag waste involving acid extraction. Two methods were employed to extract Al: a 2 M HCl aqueous solution (AH) and various citric acid (CA) aqueous solutions (0.5, 1.0, or 2.0 M). Three preparation methods (Pechini, modified citrate, and metal–organic gel) were evaluated to obtain the pure lanthanum aluminate (LaAlO&lt;sub&gt;3&lt;/sub&gt;) phase. This study also investigated the effects of several factors, with some variations being observed depending on the methodology used. The factors analyzed were: &lt;em&gt;(i)&lt;/em&gt; preparation method; &lt;em&gt;(ii)&lt;/em&gt; type of Al precursor solution (either extracted using HCl or CA); &lt;em&gt;(iii)&lt;/em&gt; ligand/cations molar ratio (La&lt;sup&gt;3 +&lt;/sup&gt; + Al&lt;sup&gt;3+&lt;/sup&gt;), ranging from 0.3 to 3.0; &lt;em&gt;(iv)&lt;/em&gt; CA concentration; &lt;em&gt;(v)&lt;/em&gt; molar ratio (La/Al), between 0.5 and 1.0; &lt;em&gt;(vi)&lt;/em&gt; calcination temperature; and &lt;em&gt;(vii)&lt;/em&gt; acid etching of the final materials with aqueous dilute nitric acid (HNO&lt;sub&gt;3&lt;/sub&gt;). The results indicated that it is possible to obtain LaAlO&lt;sub&gt;3&lt;/sub&gt; perovskite using all three methodologies and the Al extracted from saline slags. For the Pechini and metal–organic gel methods, ligand/cations molar ratios (La&lt;sup&gt;3+&lt;/sup&gt; + Al&lt;sup&gt;3+&lt;/sup&gt;) of 3.0 and between 0.3 (with CA) and 1.5 (with AH), respectively, were obtained, while a CA concentration of 1.0 M was used for the modified citrate method. The optimal molar ratio (La/Al) for obtaining the perovskite was 1.0 in all three methods. The perovskite was synthesized at low temperatures, starting from 650 °C, and was obtained in a completely pure form at between 950 and 1050 °C. Treatment with aqueous dilute acid had a marked effect, especially on the materials obtained when using the initial solution extracted with 2.0 M HCl. This treatment was particularly beneficial for the material prepared using the Pechini method, which induced a 2.5-fold increase in the specific surface area and total pore volume without affecting the crystalline structure, and allowed the specificity of the nickel (Ni) active sites incorporated to be directed, particularly towards a higher proportion of &lt;em&gt;β&lt;/em&gt;&lt;sub&gt;&lt;em&gt;1&lt;/em&gt;&lt;/sub&gt; reducible species. This result improved the catalytic performance in the dry reforming of methane (DRM) reaction, achieving conversions of up to 73 % in CO&lt;sub&gt;2&lt;/sub&gt; and up to 70 % in CH&lt;sub&gt;4&lt;/sub&gt;, with average selectivity of 0.93 after 20 h of reaction. These outcomes even surpassed the reference catalyst, which was entirely prepared using commercial-grade reagents. Factors such as the presence of other metals in the slag and the versatility of cationic substitution contributed to enhancing the physicochemical properties of the catalysts. Ultimately, all of this led to suppression of the formation of double-walled filamentous carbon deposits, which tend to deactivate the catalyst due to sint","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"447 ","pages":"Article 115158"},"PeriodicalIF":5.2,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143180282","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}

{"title":"Cu(II) nano-MOF catalyzed synthesis of 4H-Chromene derivatives as cholinesterase inhibitors","authors":"Soumyabrata Goswami ,&nbsp;Bandita Datta ,&nbsp;Sudeep Das ,&nbsp;Shreya Taran ,&nbsp;Partha Pratim Ghosh ,&nbsp;Saumya Dasgupta ,&nbsp;Sumi Ganguly","doi":"10.1016/j.cattod.2024.115156","DOIUrl":"10.1016/j.cattod.2024.115156","url":null,"abstract":"<div><div>Nanoscale metal–organic frameworks have attracted a lot of attention lately for use in heterogeneous catalytic applications, considering their strong catalytic activity. In this research article, a new Cu(II) nano-MOF is synthesized, that functions as an efficient heterogeneous and recyclable catalyst in the synthesis of 4<em>H</em>-chromene derivatives. The distinctive features of the presented synthetic strategy include high yield of the products, shorter reaction time compared to already reported methods, mild and environmentally friendly reaction conditions. Additionally, the potential of the synthesized 4<em>H</em>-chromene derivatives to elegantly inhibit two crucial target enzymes, acetylcholinesterase and butyrylcholinesterase, in the quest to combat the relentless progression of Alzheimer's disease (AD) is explored.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"447 ","pages":"Article 115156"},"PeriodicalIF":5.2,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143180471","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}

{"title":"Predicting active, selective and stable Mo2C–based bimetallic carbides for direct deoxygenation and hydrogenation reactions: A computational screening","authors":"Sagar Bathla ,&nbsp;Ryan Wei Jie Tan ,&nbsp;Samir H. Mushrif","doi":"10.1016/j.cattod.2024.115155","DOIUrl":"10.1016/j.cattod.2024.115155","url":null,"abstract":"<div><div>Transition metal carbides (TMCs), especially molybdenum carbide (Mo₂C), represent an economical and attractive alternative to precious noble metal catalysts for processes involving hydrogenation (HYD) and direct deoxygenation (DDO) reactions such as hydrodeoxygenation (HDO). Although Mo₂C has good activity for DDO, it is not selective as it displays similar activity towards HYD as well. Moreover, stability against oxygen poisoning is a critical issue as it is the major reason of catalyst deactivation. Herein, using model compounds with different oxygen functionalities (phenol, guaiacol, and 5-HMF), we employed density functional theory (DFT) calculations to investigate three key reactions (C-O dissociation, oxygen removal and ring hydrogenation) representing activity, stability and selectivity which are critical to the HDO process on 45 Mo₂C-based bimetallic carbide catalysts (Co, Cr, Fe, Mn, Nb, Ni, Ti and Zr) obtained from the Materials Project database. Among these catalysts, different dopants, stoichiometric ratios and terminations were considered. First, reaction energies of oxygen removal were used to identify stable catalysts. Subsequently, with the energy barriers of DDO and HYD for activity and their differences for selectivity, best candidates for DDO (Mo-terminated Fe₃Mo₃C, Mn-terminated Mn₃Mo₃C and Ni-terminated Ni₃Mo₃C) and HYD (triclinic Mo-terminated Fe₁₁MoC₄ and Ni-terminated Ni₆Mo₆C) were identified. Since strong oxygen binding favors DDO but hinders oxygen removal, an optimal range of oxygen binding energy (OBE) between −100 kJ/mol to −200 kJ/mol has been proposed. In addition, a parameter encompassing the three critical aspects (activity, stability, and selectivity) of a catalyst was proposed. Using OBEas a descriptor and the proposed parameter, a qualitative trend was obtained which can be used for preliminary screening of large databases of catalysts, including TMCs other than Mo₂C-based, for processes involving DDO and HYD reactions.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"447 ","pages":"Article 115155"},"PeriodicalIF":5.2,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143180472","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}

{"title":"Synthesis of TiO2-g-C3N4 for efficient photocatalytic degradation of Congo Red dye","authors":"Muhammad Saeed ,&nbsp;Humaira Asghar ,&nbsp;Iltaf Khan ,&nbsp;Nadia Akram ,&nbsp;Muhammad Usman","doi":"10.1016/j.cattod.2024.115154","DOIUrl":"10.1016/j.cattod.2024.115154","url":null,"abstract":"<div><div>Heterogeneous photocatalysis is an efficient, cost effective and promising approach for pollution control and environmental remediation, however, the fast recombination of excitons inhibits the practical applications of photocatalysis. The construction of heterojunction is a viable solution that reduces the recombination of excitons by transfer of charge carriers resulting in improved catalytic performance. Here, the fabrication of a sunlight-active TiO₂-g-C₃N₄ photocatalyst by the hydrothermal process for the degradation of Congo red dye is reported. After characterization, TiO₂-g-C₃N₄ heterojunction was employed as a photocatalyst for the sunlight-light-assisted photodegradation of Congo red dye. The fabricated g-C₃N₄ and TiO₂-g-C₃N₄ exhibited 52 % and 100 % photodegradation of 50 mL (100 mg/L) of Congo red dye by irradiation in sunlight for 180 min, respectively. The hydroxyl radicals were major species involved in the photodegradation of Congo red dye.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"447 ","pages":"Article 115154"},"PeriodicalIF":5.2,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143180473","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}

{"title":"A detailed DFT theoretical investigation of the mechanism of quinoline hydrogenation catalyzed by a (1,5-cyclooctadiene)rhodium(I) complex","authors":"Merlín Rosales ,&nbsp;Federico Arrieta ,&nbsp;Pablo Baricelli ,&nbsp;Angymileth Colina ,&nbsp;Rodolfo Izquierdo","doi":"10.1016/j.cattod.2024.115160","DOIUrl":"10.1016/j.cattod.2024.115160","url":null,"abstract":"<div><div>A detailed catalytic cycle for the hydrogenation of quinoline (<strong>Q</strong>) to 1,2,3,4-tetrahydroquinoline (<strong>THQ</strong>) catalyzed by a cationic rhodium complex containing a 1,5-cyclooctadiene (<strong>COD</strong>) ligand was computationally investigated by using DFT. It was found that the catalytically active species was [Rh(COD)(<em>κN</em>-Q)]⁺ and that the addition of each of the two dihydrogen molecules occurs through the initial coordination of dihydrogen forming <em>η</em>^<em>2</em>-H₂ intermediates, followed by the subsequent hydride transfer to <strong>Q</strong> and <strong>DHQ</strong> ligands (<em>i.e.</em>, migratory insertion and reductive elimination), respectively. Except the reductive elimination of the <strong>THQ</strong> product, all of the elementary steps of the catalytic cycle were reversible, which is an important point in connection with the hydrogen storage models. Our theoretical DFT calculations are consistent with the experimental results previously reported, but additionally provides important information that allows us to have a deeper insight into the reaction mechanism and, therefore, to present a more detailed catalytic cycle for this reaction.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"447 ","pages":"Article 115160"},"PeriodicalIF":5.2,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143180470","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}

{"title":"Transesterification of methyl oleate for biolubricant production over K2CO3/activated carbon catalyst under conventional and microwave heating","authors":"Xu Gao,&nbsp;Huiyun Zhu,&nbsp;Zhaohui Shen,&nbsp;Shuang Ou,&nbsp;Tongbo Pan,&nbsp;Ying Duan,&nbsp;Xiaojiang Liang,&nbsp;Weirong Ji,&nbsp;Qinglong Xie,&nbsp;Yong Nie","doi":"10.1016/j.cattod.2024.115157","DOIUrl":"10.1016/j.cattod.2024.115157","url":null,"abstract":"<div><div>Trimethylolpropane fatty acid triester (TFATE) as an environmentally friendly biolubricant is a promising alternative to mineral-based lubricants. However, the synthesis of TFATE by transesterification reaction has the issues of difficult catalyst recovery and slow reaction rate. In this work, K₂CO₃/activated carbon (AC) catalyst was prepared and used in the transesterification of methyl oleate (MO) with trimethylolpropane (TMP) for TFATE production. Reaction conditions including agitation speed, N₂ flow rate, catalyst amount, catalyst loading, MO to TMP molar ratio, and temperature were optimized, with the highest TFATE selectivity of 93.7% obtained. To further increase the reaction rate, microwave heating was employed to intensify the process. The kinetic study demonstrated that the rate constants of the three consecutive transesterification reactions for TFATE synthesis were enhanced by the microwave irradiation, which was mainly attributed to the “hot spot effect” of the microwave heating. Moreover, the K₂CO₃/AC catalyst was recycled and reused for five times, with no significant change in catalyst performance was observed.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"447 ","pages":"Article 115157"},"PeriodicalIF":5.2,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143180283","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}