Journal of Catalysis最新文献

{"title":"Selective hydrogenation of quinoline catalyzed by Ni/TiO2-Al2O3: role of TiO2 in promoting hydrogen spillover","authors":"Hong Zhao ,&nbsp;Tongtong Fan ,&nbsp;Chuang Liu ,&nbsp;Huaguang Tong ,&nbsp;Tong Li ,&nbsp;Jiantai Ma ,&nbsp;Zhengping Dong","doi":"10.1016/j.jcat.2026.116730","DOIUrl":"10.1016/j.jcat.2026.116730","url":null,"abstract":"<div><div>Efficient hydrogen activation and spillover remain critical challenges limiting the hydrogenation efficiency of heterogeneous catalytic systems. To address this limitation, we developed a TiO₂ modification strategy involving the in-situ formation of reducible TiO₂ on Al₂O₃, resulting in a Ni/TiO₂-Al₂O₃ catalyst with enhanced hydrogen spillover efficiency. The modified catalyst exhibits significantly improved activity for the selective hydrogenation of quinoline under identical reaction conditions. Comprehensive characterization and experimental results demonstrate that TiO₂ incorporation facilitates H₂ activation and generates abundant hydrogen migration pathways, thereby increasing the concentration of active hydrogen species on the Al₂O₃ surface. DFT calculations further confirm that the hydrogen migration barrier at the TiO₂-Al₂O₃ interface is lower than that of pure Al₂O₃, offering theoretical support for the enhanced spillover efficiency. Meanwhile, the spatial separation between quinoline adsorption sites, Lewis acid of Al₂O₃ and hydrogen activation sites, Ni nanoparticles, directly drive the enhanced hydrogenation performance. Furthermore, the use of an <em>i</em>-PrOH/ H₂O mixed solvent significantly enhances catalysis, as water mediates the spillover of active hydrogen species from the catalyst into the aqueous phase, where they participate in the reaction via a Grotthuss proton-hopping mechanism, as evidenced by NMR. Delayed feeding experiments demonstrate that hydrogen stored in the aqueous phase can still drive quinoline hydrogenation even after H₂ removal, highlighting the importance of both solid- and liquid-phase hydrogen transfer. This dual-phase spillover strategy offers a promising avenue for designing highly efficient heterogeneous catalytic hydrogenation systems.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"456 ","pages":"Article 116730"},"PeriodicalIF":6.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146129540","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Step-by-step elucidation of the role of platinum in a co-impregnated Co/SiO2 Fischer–Tropsch catalyst","authors":"Sandeeran Govender,&nbsp;Sinqobile V.L. Mahlaba,&nbsp;Eric van Steen","doi":"10.1016/j.jcat.2026.116757","DOIUrl":"10.1016/j.jcat.2026.116757","url":null,"abstract":"<div><div>Platinum is a well-known reduction promoter for cobalt-based catalysts resulting in a higher degree of reduction, and an improved activity. Here, the role of platinum in a co-impregnated Pt-Co/SiO₂ catalyst (Co-loading: 10 wt-%; Pt-loading: 0–0.44 wt-%) is investigated in depth. The addition of more platinum to the catalyst formulation results in an increased formation of Co₃O₄ in the calcined catalyst, progressively fewer reduction features in the TPR profiles, and yet a decreasing hydrogen uptake after peaking at 0.05 wt-% Pt. The metallic cobalt particle appears to become richer in smaller hcp-cobalt crystallites upon platinum incorporation. The calculated initial TOF increases strongly with increasing platinum loading possibly due to electronic promotion, however the cobalt time yield plateaus as a function of the platinum loading because of the decreasing metal dispersion. The intrinsic deactivation becomes stronger at high platinum loading which is postulated to be linked to increased carbon deposition. The product selectivity appears to be primarily affected by the conversion level rather than the level of platinum promotion.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"456 ","pages":"Article 116757"},"PeriodicalIF":6.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146676","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Insight into the crucial role of carbon in LaFeO3@C composites for liquid-phase aerobic oxidation of benzyl alcohol to benzaldehyde","authors":"Wenwen Xiao ,&nbsp;Joshua Gorimbo ,&nbsp;Qingye Zhao ,&nbsp;Zhiyan He ,&nbsp;Shuai Lyu ,&nbsp;Ping Xiao ,&nbsp;Yali Yao ,&nbsp;Junjiang Zhu","doi":"10.1016/j.jcat.2026.116747","DOIUrl":"10.1016/j.jcat.2026.116747","url":null,"abstract":"<div><div>Adsorption, reaction and desorption are three primary steps of a catalytic reaction, and a potential catalyst should thus have large surface area to adsorb reactants, efficient active sites to convert reactants and good ability to eliminate products. To achieve this goal, we herein report the fabrication of porous carbon-coated perovskite catalyst, LaFeO₃@C, for liquid-phase oxidation of benzyl alcohol (BzOH) to benzaldehyde (BzH) using O₂ as oxidant. The large surface area and rich pores of porous carbon facilitate the adsorption and transport of reactants (BzOH and O₂) from solution to the active sites of LaFeO₃, the oxygen vacancies of LaFeO₃ generated by carbon reduction improve the reaction rate between BzOH and O₂, and the hydrophobic surface oxygen functional groups (SOFGs) formed on the porous carbon promote the removal of by-product water from the active sites. Catalytic tests indicated that LaFeO₃ and carbon individually showed negligible activity for the reaction, while an abrupt increase in the activity was observed upon their integration, especially for LaFeO₃@C heated in air at 350 °C for 60 min (denoted as LFO@C-60), which showed a reaction rate of 0.57 mmol·g⁻¹·h⁻¹ after 3 h of reaction time, owing to its appropriate surface area, mesopores, oxygen vacancies and hydrophobic SOFGs. The results provide a novel strategy to fabricate perovskite oxide catalysts for liquid-phase reactions <em>via</em> porous carbon coating.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"456 ","pages":"Article 116747"},"PeriodicalIF":6.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146135420","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Layered double hydroxides enabled efficient electrocatalytic oxidative cleavage of C(OH)−C bonds","authors":"Yiyuan Zhang,&nbsp;Xianhong Wu,&nbsp;Jinjie Lin,&nbsp;Hanyang Chen,&nbsp;Run-Cang Sun","doi":"10.1016/j.jcat.2026.116728","DOIUrl":"10.1016/j.jcat.2026.116728","url":null,"abstract":"<div><div>The electrochemical oxidative cleavage of C(OH)-C bonds facilitates the conversion of lignin-derived secondary alcohols and ketones into valuable carboxylates in a mild and environmentally friendly manner. In this study, we present efficient and cost-effective FeNi layered double-hydroxide (LDH) nanosheets created through a one-step galvanostatic electrodeposition on nickel foam (NF). The FeNi-LDH/NF shows a high activity for α-phenethyl alcohol (α-PEA) electrooxidation reaction leading to low potential 1.489 V vs. RHE to reach a current density of 100 mA cm⁻², α-PEA was almost completely transformed, and the yield of benzoic acid (BA) was high (&gt; 95%). Both theory and experiments show that α-PEA is first oxidized to acetophenone and then to benzoic acid. The dehydrogenation and oxygenation of the C–H bond is the rate-limiting step of the reaction. In addition, an energy-saving and multifunctional flow electrolytic cell has been developed successfully, througn coupling α-PEA electrooxidation reaction with hydrogen evolution reaction, with FeNi-LDH/NF as dual-functional electrocatalyst. The flow electrolytic cell can operate stably for 200 h.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"456 ","pages":"Article 116728"},"PeriodicalIF":6.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146095952","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Alkaline oxide clusters inside zeolites catalyze the selective synthesis of ethyl methyl carbonate","authors":"Yongkun Zheng,&nbsp;Nacho Solá-Ferrer,&nbsp;Lluís Martínez-Belenguer,&nbsp;Belén Lerma-Berlanga,&nbsp;Antonio Leyva-Pérez","doi":"10.1016/j.jcat.2026.116729","DOIUrl":"10.1016/j.jcat.2026.116729","url":null,"abstract":"<div><div>Ethyl methyl carbonate (EMC), as the simplest asymmetric carbonate, is considered a unique green liquid organic compound for lithium batteries (electrolyte) and gasoline blending (octane enhancer additive), with properties between dimethyl and diethyl carbonate. In accordance, its chemical production is expected to boost during the coming years, despite green chemical syntheses for EMC are still to be developed. Here we show the selective synthesis of EMC from DMC and ethanol with one of the cheapest commercially available solids, i.e. zeolites, as a heterogeneous catalyst for the reaction, surpassing most of the current soluble catalysts employed for this reaction. While a pristine commercial zeolite such as NaX already shows a significant catalytic activity (65% conversion, 91% selectivity to EMC) without any pre-activation treatment, is recoverable and reusable, and can be implemented in batch and in flow, the incorporation of alkaline oxide clusters inside the zeolitic framework, i.e. K₂O, boosts the catalytic activity not only for the NaX zeolite but also for the parent H-USY and NaY zeolites, otherwise barely catalytically active for the reaction, to give yields up to &gt;99% and ≈80% selectivity to EMC. These results bring a sustainable and cheap catalytic system for the production of EMC.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"456 ","pages":"Article 116729"},"PeriodicalIF":6.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098234","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Direct synthesis of phenyl isocyanate by carbonylation of nitrobenzene, catalyzed by palladium/phenanthroline complexes: promoting effect of phosphorus acids","authors":"Doaa R. Ramadan ,&nbsp;Manar Ahmed Fouad ,&nbsp;Francesco Ferretti ,&nbsp;Alessandro Gardelli ,&nbsp;Artur Brotons Rufes ,&nbsp;Chiara Costabile ,&nbsp;Fabio Ragaini","doi":"10.1016/j.jcat.2026.116753","DOIUrl":"10.1016/j.jcat.2026.116753","url":null,"abstract":"<div><div>The synthesis of aryl isocyanates by direct carbonylation of nitroarenes is the most straightforward alternative to the current technology, which involves the use of very toxic phosgene at one stage of the process. However, it faces several problems and has been little investigated in recent years. By taking advantage of our previous studies on the related carbonylation reaction yielding carbamates, we herein report that the use of phosphorus acids, diphenylphosphinic acid in particular, as promoters for the palladium/phenanthroline catalytic system, allows an improvement in activity and turnover number of almost one order of magnitude with respect to the best results previously reported. The effect of several experimental variables was investigated. Mechanistic investigations indicates that the enhanced activity is not associated with pathways involving water-assisted processes or aniline intermediates.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"456 ","pages":"Article 116753"},"PeriodicalIF":6.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146677","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Realize the non-radical selective dehydrogenation of amine on TiO2 photoanode with uniformly coated Ni(OH)2 nano-layer","authors":"Shaohua He ,&nbsp;Jie Yang ,&nbsp;Ge Tian ,&nbsp;Sipeng Yang ,&nbsp;Mengyu Duan ,&nbsp;Shaorui Jian ,&nbsp;Shirong Kang ,&nbsp;Jianjiang Lu ,&nbsp;Chuncheng Chen","doi":"10.1016/j.jcat.2026.116735","DOIUrl":"10.1016/j.jcat.2026.116735","url":null,"abstract":"<div><div>The photoelectrocatalytic (PEC) oxidation represents an efficient route for the degradation of organic pollutants and transformation of organic chemicals. However, the PEC direct oxidation on TiO₂ photoanode suffers from low current efficiency and poor selectivity because of the intrinsic radical characteristics. We realize the high-efficient and selective oxidation of organic amine to nitrile by covering the TiO₂ photoanode with a uniform Ni(OH)₂ nano-layer. It is found that on bare TiO₂ photoanode, the oxidation of model substrate benzylamine leads to the formation of benzaldehyde as the main products with a selectivity of 35% and a Faradaic efficiency (FE) of only 7%. By contrast, on the Ni(OH)₂-covered TiO₂, the selective dehydrogenation of benzylamine to benzonitrile becomes the dominant process with a selectivity of &gt; 99% and FE value exceeding 80%. The detailed experiments by operando EPR, XPS, UV–vis, and Raman spectroscopy reveals that the presence of Ni(OH)₂ nano-layer on the surface of TiO₂ successfully shifts the reaction pathway from traditional radical-driven oxidation to a predominantly non-radical mechanism. The high-valent Ni species (NiOOH), rather than radical, is the key reactive intermediate for the selective dehydrogenation of amine. This work provides a new strategy for PEC valorization of wastewater pollutants, achieving simultaneous pollutants highly selective conversion and chemical energy recovery.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"456 ","pages":"Article 116735"},"PeriodicalIF":6.5,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146110689","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Unraveling the evolution of oxygen species and its role in adjusting catalytic performance over LaAlO3-based catalysts in oxidative coupling of methane","authors":"Yaqian Zhang ,&nbsp;Xingxu Wang ,&nbsp;Bingying Han ,&nbsp;Lixia Ling ,&nbsp;Baojun Wang ,&nbsp;Maohong Fan ,&nbsp;Riguang Zhang","doi":"10.1016/j.jcat.2026.116695","DOIUrl":"10.1016/j.jcat.2026.116695","url":null,"abstract":"<div><div>The oxidative coupling of methane (OCM) reaction is hindered by fundamental scientific challenges including the difficulty in CH₄ activation and the inability to inhibit deep oxidation. In this study, the LaAlO₃ catalyst, which exhibits excellent low-temperature activity and thermal stability, was selected. The structure–activity relationship among the catalyst surface structure, surface oxygen species, and reaction performance was systematically explored using DFT calculations and microkinetic modeling. The results indicate that different surface terminations (LaO- and AlO₂-terminations) of LaAlO₃ catalyst exhibit distinct oxygen species. The evolution pathway of oxygen species on the LaO-termination surface proceeds as O^2–→O₂^–→O₂^2–→O^2–, while on the AlO₂-termination surface it follows O^2–→O₂^2–→O^2–. Among these oxygen species, O^2– plays a dominant role in CH₄ dissociation. The LaO-termination demonstrates three major advantages: higher CH₄ dissociation activity, superior C₂H₄ production activity, and enhanced selectivity, establishing it as the dominant active termination. Doping the LaO-termination catalysts with alkaline earth metals (Mg, Ca, Sr) do not alter the types of oxygen species but significantly modulate reaction characteristics. Bader charge of surface O^2– serves as an effective descriptor for predicting CH₄ dissociation capability of M/LaO-p-O^2– catalysts. Under realistic conditions, due to fewer surface free sites, Ca/LaO-p-O^2– exhibits a lower C₂H₄ formation rate than Sr/LaO-p-O^2–.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"455 ","pages":"Article 116695"},"PeriodicalIF":6.5,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145956885","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A tandem visible-light/heterogeneous-alumina catalytic platform for sustainable transition-metal-free cyclobutene synthesis","authors":"Zhe Wang ,&nbsp;Jie Huang ,&nbsp;Min Zhou,&nbsp;Lin Ma,&nbsp;Min Zhang","doi":"10.1016/j.jcat.2026.116726","DOIUrl":"10.1016/j.jcat.2026.116726","url":null,"abstract":"<div><div>A highly efficient one-pot synthesis of cyclobutenes is developed through a visible-light-driven [2 + 2] cycloaddition of 4-chlorocoumarin with benzofuran, followed by a basic alumina-mediated cascade sequence involving hydrolysis, decarboxylation, and elimination of HCl. This transition-metal-free protocol proceeds under mild conditions using readily available substrates, offering a green and practical approach to cyclobutene construction.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"455 ","pages":"Article 116726"},"PeriodicalIF":6.5,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146071915","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Corrigendum to “Robust rGO-supported α-FeOOH/Fe2O3 nanorods catalyst: Unveiling the role of χ-Fe5C2 phase and rGO for exceptional stability in Fischer–Tropsch synthesis”. [J. Catal. 453 (2026) 116584]","authors":"Juan Zhang ,&nbsp;Mohamed Abbas ,&nbsp;Weibin Fan ,&nbsp;Jiangang Chen","doi":"10.1016/j.jcat.2025.116666","DOIUrl":"10.1016/j.jcat.2025.116666","url":null,"abstract":"","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"455 ","pages":"Article 116666"},"PeriodicalIF":6.5,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145920100","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}