Journal of Catalysis最新文献

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Efficient one-pot synthesis of 2,5-furandicarboxylic acid from fructose and 5-hydroxymethylfurfural using synergistically active Ce-Al composite catalyst under mild conditions 在温和条件下,采用协同活性Ce-Al复合催化剂,以果糖和5-羟甲基糠醛为原料,高效一锅合成2,5-呋喃二羧酸
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-07-01 DOI: 10.1016/j.jcat.2025.116310
Pratap M. Ganje , Chang-Gu Lee , Hern Kim
{"title":"Efficient one-pot synthesis of 2,5-furandicarboxylic acid from fructose and 5-hydroxymethylfurfural using synergistically active Ce-Al composite catalyst under mild conditions","authors":"Pratap M. Ganje ,&nbsp;Chang-Gu Lee ,&nbsp;Hern Kim","doi":"10.1016/j.jcat.2025.116310","DOIUrl":"10.1016/j.jcat.2025.116310","url":null,"abstract":"<div><div>Using <em>tert</em>-butyl hydroperoxide (TBHP) as a low-cost oxidant, we synthesized, characterized, and evaluated heterogeneous bifunctional oxide catalysts composed of the non-noble metals Ce and Al in specific molar ratios, supported on glucose-derived carbon, for the conversion of 5-hydroxymethylfurfural (5-HMF) to 2,5-furandicarboxylic acid (2,5-FDCA) in dimethyl sulfoxide (DMSO). TBHP offers two advantages: it functions as an oxidant and generates <em>tert</em>-butanol, a valuable industrial solvent. We fully investigated catalyst loading, temperature, 5-HMF:TBHP molar ratio, reaction time, and reuse impact on product yield while correlating with the catalyst’s textural and chemical properties. CAOC-1, the best catalyst, achieved 98 % conversion, 82.0 % yield, and 83.54 % selectivity of 2,5-FDCA in optimal conditions (5-HMF (1 mmol), TBHP (9 mmol), DMSO (5 gm), CAOC-1 (50 mg), Temp (120 °C), 24 h), with minimal yield reduction over five reuse cycles. We used the bifunctional CAOC-1 in a one-pot, two-step system to directly transform fructose to 2,5-FDCA under mild conditions (fructose (1 mmol), TBHP (9 mmol), DMSO (5 gm), CAOC-1 (50 mg), temp (120 °C), 26 h) with minimal process modifications. The yield and selectivity of 2,5-FDCA were 80.26 % and 83.94 %, respectively. We proposed mechanistic pathways for dehydration and oxidation reactions, highlighting the catalyst’s bifunctional nature in facilitating high 2,5-FDCA yields from fructose and 5-HMF. The formation of the distinct redox environment of Ce and Al on carbon, the various oxidation states, and the oxygen vacancies in the CAOC-1 catalyst—all of which most likely operate as base-free oxidation active sites. One-pot reaction processes involve bifunctional CAOC-1 catalysts, –OH, and redox active sites (Ce), which play a significant role in dehydration and oxidation reactions, respectively. 2,5-FDCA is crucial to produce polyethylene 2,5-furandicarboxylate (PEF), a sustainable bioplastic and alternative to PET.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116310"},"PeriodicalIF":6.5,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144533967","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}
引用次数: 0
In situ engineering carbon-coated hydrotalcite-derived ZnxAlOy-C catalysts for efficient catalytic transfer hydrogenation of furfural to furfuryl alcohol 原位工程碳包覆水滑石衍生的ZnxAlOy-C催化剂,用于糠醛高效催化转移加氢制糠醇
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-06-30 DOI: 10.1016/j.jcat.2025.116301
Junling Xie, Guyu Yin, Xiaoyu Niu, Yujun Zhu
{"title":"In situ engineering carbon-coated hydrotalcite-derived ZnxAlOy-C catalysts for efficient catalytic transfer hydrogenation of furfural to furfuryl alcohol","authors":"Junling Xie,&nbsp;Guyu Yin,&nbsp;Xiaoyu Niu,&nbsp;Yujun Zhu","doi":"10.1016/j.jcat.2025.116301","DOIUrl":"10.1016/j.jcat.2025.116301","url":null,"abstract":"<div><div>Catalytic Transfer Hydrogenation (CTH) has been widely reported as an efficient, safe and green method for catalytic hydrogenation of biomass-derived platform molecules in recent years. In this work, we fabricated tunable Zn/Al molar ratio carbon-coated hydrotalcite-derived Zn-Al oxide composites (Zn<sub>x</sub>AlO<sub>y</sub>-C), where Isopropanol (IPA) served dual roles as hydrogen donor and reaction medium, to achieve selective hydrogenation of Furfural (FAL) into Furfuryl Alcohol (FOL). Under mild reaction conditions, the conversion of FAL and the selectivity of FOL can reach 92.0% and 93.8% over Zn<sub>2</sub>AlO<sub>y</sub>-C, respectively. Through analysis, the reasons for the high yield of FOL are that the surface carbon material effectively increases the specific surface area of the catalyst, enhances the adsorption capacity of the catalyst to the reactants, and more effectively promotes the migration of the reactants from the solution to the Zn-O-Al active site, while by adjusting the Zn/Al ratio, a suitable acid/base ratio is found to reduce the occurrence of side reactions and improve the selectivity. The current synthesis method provides an effective way to design carbon-containing composite catalysts with controllable catalytic application performance.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116301"},"PeriodicalIF":6.5,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144516255","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}
引用次数: 0
Lowering the barrier to access information-rich transient kinetic data for machine learning methods 为机器学习方法降低访问信息丰富的瞬态动力学数据的障碍
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-06-28 DOI: 10.1016/j.jcat.2025.116306
B. Ariana Thompson , Shengguang Wang , Konstantinos Goulas , M. Ross Kunz , Rebecca Fushimi
{"title":"Lowering the barrier to access information-rich transient kinetic data for machine learning methods","authors":"B. Ariana Thompson ,&nbsp;Shengguang Wang ,&nbsp;Konstantinos Goulas ,&nbsp;M. Ross Kunz ,&nbsp;Rebecca Fushimi","doi":"10.1016/j.jcat.2025.116306","DOIUrl":"10.1016/j.jcat.2025.116306","url":null,"abstract":"<div><div>Transient kinetic data contain a wealth of information about intrinsic features of a catalyst as well as the reaction mechanism. Currently, high volume transient data is underutilized, and data science methods could increase the value of information that can be extracted from this data, integrate experimental with theoretical data sources, and accelerate the pace of catalyst technology advancement. Transient kinetic characterizations with simple probe molecules exhibiting reversible adsorption, irreversible adsorption and bulk-surface diffusion are presented as training components for similar experiments with more complex surface reactions. By increasing the availability and accessibility of transient kinetic data through details of its structure and acquisition, we aim to decrease the barrier for data scientists to apply machine learning methods to this valuable data source.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116306"},"PeriodicalIF":6.5,"publicationDate":"2025-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515499","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}
引用次数: 0
Synergistic regulation of oxygen vacancy and Lewis acid sites by Ru loading in LaMnOx catalysts for boosting 2-butanol production from levulinic acid and levulinates 负载Ru对LaMnOx催化剂中氧空位和路易斯酸位点的协同调节,促进乙酰丙酸和乙酰丙酸酯生产2-丁醇
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-06-28 DOI: 10.1016/j.jcat.2025.116302
Lingling Gao , Yiwei Long , Zhiguo Xiao , Lungang Chen , Guozhang Chang , Wenguang Zhou , Chenguang Wang , Yong Liu
{"title":"Synergistic regulation of oxygen vacancy and Lewis acid sites by Ru loading in LaMnOx catalysts for boosting 2-butanol production from levulinic acid and levulinates","authors":"Lingling Gao ,&nbsp;Yiwei Long ,&nbsp;Zhiguo Xiao ,&nbsp;Lungang Chen ,&nbsp;Guozhang Chang ,&nbsp;Wenguang Zhou ,&nbsp;Chenguang Wang ,&nbsp;Yong Liu","doi":"10.1016/j.jcat.2025.116302","DOIUrl":"10.1016/j.jcat.2025.116302","url":null,"abstract":"<div><div>The conversion of biomass-derived levulinic acid (LA) into 2-butanol offers a promising route to produce valuable secondary alcohols under sustainable conditions. In this study, a series of Ru-LaMnOx catalysts with varied Ru loadings were synthesized and their structural, electronic, and acidic properties were systematically characterized. Increasing Ru loading enhanced the surface Ru<sup>0</sup>/Ru<sup>4+</sup> ratio and promoted the reduction of Mn species. These modifications led to an increased concentration of surface oxygen vacancies (Ov) and a higher density of Lewis acid sites, both of which are critical for the Meerwein–Ponndorf–Verley (MPV) reduction and subsequent hydrogenolysis of LA. Catalytic performance tests revealed that the optimized Ru<sub>3</sub>LaMnOx catalyst achieved a 2-butanol yield of 99.1 % at 200 °C under 5 MPa H<sub>2</sub> and 8 h, along with good recyclability. This study identified the ring-opening of γ-valerolactone as the rate-determining step, with Ru<sup>0</sup> sites and adjacent Ov facilitating hydrogen transfer and selective C–C bond cleavage. Density functional theory calculations confirmed that surface Ov enhanced LA and isopropanol adsorption and promote essential electron transfer processes. These findings demonstrate that tuning Ru loading to synergistically control electronic and acidic properties is a promising strategy for efficient biomass conversion.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116302"},"PeriodicalIF":6.5,"publicationDate":"2025-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515283","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}
引用次数: 0
Interfacial effect of CoZn-MOFs synergizes with In doping to notably improve efficiency of TaON photoanode photoelectrochemical water splitting cozn - mof的界面效应与In掺杂协同作用,显著提高了TaON光阳极的光电化学水分解效率
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-06-28 DOI: 10.1016/j.jcat.2025.116304
Shaomang Wang , Qiankun Deng , Chengye Huang , Zheng Shen , Yuan Guan , Zhongyu Li , Shicheng Yan , Zhigang Zou
{"title":"Interfacial effect of CoZn-MOFs synergizes with In doping to notably improve efficiency of TaON photoanode photoelectrochemical water splitting","authors":"Shaomang Wang ,&nbsp;Qiankun Deng ,&nbsp;Chengye Huang ,&nbsp;Zheng Shen ,&nbsp;Yuan Guan ,&nbsp;Zhongyu Li ,&nbsp;Shicheng Yan ,&nbsp;Zhigang Zou","doi":"10.1016/j.jcat.2025.116304","DOIUrl":"10.1016/j.jcat.2025.116304","url":null,"abstract":"<div><div>For photoelectrochemical hydrogen evolution by complete water splitting, the creation of strong and efficient photoanodes is essential. Herein, the In-TaON/CoZn-MOFs photoanode was developed by doping In ions into TaON, then compounded by CoZn-MOFs. The In-TaON/CoZn-MOFs exhibited remarkably improved performance after cyclic voltammetry (CV) treatment. The current density of In-TaON/CoZn-MOFs-CV was 2.63 mA cm<sup>−2</sup> at 1.23 V (vs RHE) under light irradiation (AM 1.5G), which was around 7.3 times that of TaON. After 10 h of running, the current density generated by In-TaON/CoZn-MOFs-CV could still reach about 2 mA cm<sup>−2</sup>. Compared to the ΔF<sub>max</sub> value of 1.77 eV for TaON, the ΔF<sub>max</sub> value of In-TaON/<strong><em>Co</em></strong>Zn-MOFs with Co<sup>2+</sup> as the active site was reduced to 0.38 eV. As a result, the In-TaON/CoZn-MOFs-CV produced a quantity of O<sub>2</sub> that was 17.7 times that of TaON.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116304"},"PeriodicalIF":6.5,"publicationDate":"2025-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515282","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}
引用次数: 0
Co-promoter interactions within silver-catalyzed propylene epoxidation by molecular oxygen 分子氧催化银催化丙烯环氧化过程中的共启动子相互作用
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-06-28 DOI: 10.1016/j.jcat.2025.116305
Joseph Esposito, Aditya Bhan
{"title":"Co-promoter interactions within silver-catalyzed propylene epoxidation by molecular oxygen","authors":"Joseph Esposito,&nbsp;Aditya Bhan","doi":"10.1016/j.jcat.2025.116305","DOIUrl":"10.1016/j.jcat.2025.116305","url":null,"abstract":"<div><div>Propylene epoxidation on promoted Ag catalysts requires several promoters including gaseous co-feeds of allyl chloride (5–20 ppm), nitric oxide (100–1000 ppm), and carbon dioxide (2–10 vol%) on K-promoted Ag/CaCO<sub>3</sub>. Steady-state rate and selectivity trends with respect to individual promoter concentrations reveal, in addition to direct influence of promoters on oxidation intermediates, co-promoters significantly alter the nature and magnitude of the effect of other co-promoters. On K-promoted Ag/CaCO<sub>3</sub>, nitric oxide increases epoxidation selectivity at low concentrations (depending on K loading, up to ∼100 ppm NO) and decreases selectivity at higher concentrations (&gt;200 ppm NO). Co-promoting K concentrations significantly influence the concentrations of NO required for selective oxidation, evincing cooperative co-promotional effects of NO and K. At low levels of K/NO promotion, carbon dioxide (0.2–40 vol%) weakly inhibits O<sub>2</sub> activation rates (∼0.3 order inhibition) and inhibits selectivity while at high levels of K/NO promotion, co-fed CO<sub>2</sub> increases selectivity and reaches maximal order inhibition of rates (at ∼0.5 order inhibition). These results can be rationalized on the basis of selectivity-enhancing, competing alkali-stabilized NO<sub>x</sub> and/or CO<sub>x</sub> derived from co-fed NO and CO<sub>2</sub>. NO renders half-order promotion of steady-state rates on K-promoted catalysts, and transient experiments show NO slowly generates long-lived surface intermediates relevant to catalytic activity for both oxidation and chlorination—consistent either with NO generating an activity-enhancing, co-catalytic NO<sub>x</sub> intermediate or removing surface-poisoning, alkali-stabilized CO<sub>x</sub> species to promote catalytic activity. K promotion (&gt;0.05 mol K (mol Ag<sub>bulk</sub>)<sup>−1</sup>) is also shown to substantially alter the promoting action of co-fed allyl chloride, with K-bare catalysts featuring significantly weaker selectivity promotion by the organochloride. Insights into co-promoter interactions suggest selective propylene epoxidation occurs only on active sites covered in appropriate concentrations of alkali-stabilized chlorine and oxyanions derived from CO<sub>2</sub> and NO<sub>x</sub>.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116305"},"PeriodicalIF":6.5,"publicationDate":"2025-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515281","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}
引用次数: 0
Pre-treated carbon additive enables reduction of metal loading in CoNiFe oxide-based OER electrocatalysts while maintaining performance 预处理的碳添加剂可以在保持性能的同时减少CoNiFe氧化物基OER电催化剂中的金属负载
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-06-26 DOI: 10.1016/j.jcat.2025.116299
Trang Minh Pham, Na Liu, Stephan Bartling, Nils Rockstroh, Reinhard Eckelt, Wen Ju, Annette-Enrica Surkus, Robert Francke
{"title":"Pre-treated carbon additive enables reduction of metal loading in CoNiFe oxide-based OER electrocatalysts while maintaining performance","authors":"Trang Minh Pham,&nbsp;Na Liu,&nbsp;Stephan Bartling,&nbsp;Nils Rockstroh,&nbsp;Reinhard Eckelt,&nbsp;Wen Ju,&nbsp;Annette-Enrica Surkus,&nbsp;Robert Francke","doi":"10.1016/j.jcat.2025.116299","DOIUrl":"10.1016/j.jcat.2025.116299","url":null,"abstract":"<div><div>Mixed oxides (MO) of Co, Ni, and Fe have emerged as promising catalysts for the oxygen evolution reaction (OER) in alkaline water electrolysis (AWE). Although they are significantly cheaper than the precious metal catalysts used for proton exchange membrane (PEM) water splitting, the limited availability of Co and the exceptionally poor environmental footprint of Co and Ni mining remain challenges for scaling up AWE capacities. In this context, we present a promising approach toward reducing the metal content while preserving the catalytic performance. Based on a recent work on CoNiFeO<sub>x</sub> OER catalysts from our group, admixture of pre-treated Vulcan carbon XC-72R (VC) at different synthesis stages in various loadings was evaluated in view of material structure and electrocatalytic activity. Attractive performance characteristics were obtained for the optimized MO-VC composite material, <em>e.g.</em>, a mass activity of 370 A <span><math><mrow><msubsup><mi>g</mi><mrow><mi>C</mi><mi>o</mi><mi>N</mi><mi>i</mi><mi>F</mi><mi>e</mi></mrow><mrow><mo>-</mo><mn>1</mn></mrow></msubsup></mrow></math></span> at 1.56 V vs. RHE and a Tafel slope of 39.0 mV dec<sup>−1</sup>. Stable long-term performance under practical AWE conditions was confirmed in an anion exchange membrane (AEM) electrolyzer. An understanding of the effect of carbon admixture was achieved by combining <em>in situ</em> X-ray absorption spectroscopy, analysis of the electrochemically active surface area, as well as electrochemical impedance spectroscopy. The results point toward a benign impact of carbon admixture on the electronic structure of the MO domains under potential bias.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116299"},"PeriodicalIF":6.5,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144515285","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}
引用次数: 0
Spatiotemporal investigation of the regeneration of a shaped zeolite catalyst extrudate using operando powder X-ray diffraction computed tomography 利用operando粉末x射线衍射计算机断层扫描研究异型沸石催化剂挤出物再生的时空
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-06-25 DOI: 10.1016/j.jcat.2025.116300
Izar Capel Berdiell , Lars F. Lundegaard , Pablo Beato , Marco Di Michiel , David S. Wragg , Stian Svelle
{"title":"Spatiotemporal investigation of the regeneration of a shaped zeolite catalyst extrudate using operando powder X-ray diffraction computed tomography","authors":"Izar Capel Berdiell ,&nbsp;Lars F. Lundegaard ,&nbsp;Pablo Beato ,&nbsp;Marco Di Michiel ,&nbsp;David S. Wragg ,&nbsp;Stian Svelle","doi":"10.1016/j.jcat.2025.116300","DOIUrl":"10.1016/j.jcat.2025.116300","url":null,"abstract":"<div><div>We have used <em>operando</em> powder X-ray diffraction computed tomography (PXRD-CT) analysed by parametric Rietveld refinements to monitor the regeneration of a deactivated ZSM-5 zeolite based extrudate employed as a catalyst in the methanol-to-hydrocarbon reaction. This investigation thus advances beyond previous studies of pure, powdered zeolites. We follow the coke oxidation by monitoring three XRD based descriptors. Lattice relaxation, monitored as the difference in length of the <em>a</em>- and <em>b</em>-lattice parameters (<em>a-b</em>), occurs first at the core of the extrudate and progresses towards the outer surface. This demonstrates a radial distribution of different coke species, wherein the heaviest, more oxidation resistant coke is matured near the external surface of the extrudate. In contrast, the total <em>non-framework species mass</em> (<em>NFSM</em>) decreased more uniformly throughout the extrudate, suggesting that chemical transformations of the coke species can occur prior to full oxidation. This notion is supported by in situ temperature programmed oxidation, which demonstrates that the regeneration of the ZSM-5/binder composite occurs in two distinct steps. We also observe that irreversible (hydro)thermal damage occurs in the severely coked regions of the extrudate during regeneration. Additionally, we demonstrate that the three different XRD based descriptors carry slightly different and complementary information. The (<em>a-b</em>) descriptor describes lattice distortion induced by rigid coke species. The total <em>non-framework species mass</em> (<em>NFSM</em>) and the <em>unit cell volume (UCV)</em>, in contrast, capture all guest species, including volatile compounds and water. However, as a drawback, the <em>UCV</em> is strongly influenced also by thermal effects, whereas the (<em>NFSM</em>) is virtually unaffected by temperature.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116300"},"PeriodicalIF":6.5,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144479634","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}
引用次数: 0
Facile preparation of alkali metal-doped Ru/MgO catalysts for ammonia decomposition via one-pot dry ball milling: structural and electronic promoting effect of K, Rb, and Cs 一锅干球磨法制备碱金属掺杂Ru/MgO氨分解催化剂:K、Rb、Cs的结构和电子促进作用
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-06-25 DOI: 10.1016/j.jcat.2025.116298
Hongyang Huang, Haifan Deng, Yuyin Ji, Dalin Li, Chongqi Chen, Huihuang Fang, Yu Luo, Lilong Jiang
{"title":"Facile preparation of alkali metal-doped Ru/MgO catalysts for ammonia decomposition via one-pot dry ball milling: structural and electronic promoting effect of K, Rb, and Cs","authors":"Hongyang Huang,&nbsp;Haifan Deng,&nbsp;Yuyin Ji,&nbsp;Dalin Li,&nbsp;Chongqi Chen,&nbsp;Huihuang Fang,&nbsp;Yu Luo,&nbsp;Lilong Jiang","doi":"10.1016/j.jcat.2025.116298","DOIUrl":"10.1016/j.jcat.2025.116298","url":null,"abstract":"<div><div>Ammonia decomposition is a promising method for on-site hydrogen generation for fuel cells. Ruthenium is the most active catalyst for this process, and modulation of its geometric and electronic properties is essential for achieving high catalytic performance. This study developed a facile approach for synthesizing alkali metal-doped Ru/MgO catalysts using a one-pot dry ball milling method with acetates as precursors. Characterization results indicate that K, Rb, and Cs act as effective structural and electronic promoters. Notably, the presence of alkali metals significantly inhibits the aggregation of bulk-like RuO<sub>2</sub>, leading to the formation of well-dispersed RuO<em><sub>x</sub></em>, which, upon reduction, produces small Ru nanoparticles. The average Ru particle size is about 2–3 nm, aligning with the theoretical optimal size for maximizing B<sub>5</sub> sites. XAS and DRIFTS analyses confirm that Ru species are stabilized due to the strong metal-promoter interaction between ruthenium and alkali metals via oxygen bonding. The resulting alkali metal-promoted Ru nanoparticles exhibit superior low-temperature activity for ammonia decomposition. The 2 K-3 %Ru/MgO catalyst achieves a high reaction rate of 11.5 mmol-NH<sub>3</sub> g<sub>cat</sub><sup>−1</sup> min<sup>−1</sup> at 400 °C under 30,000 mL g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup>, demonstrating one of the highest performances among Ru catalysts. Furthermore, this catalyst maintains high activity at 475 °C for 50 h without significant deactivation. The enhanced catalytic performance is attributed to the structural and electronic promotion effects of alkali metals, which facilitate the formation of B<sub>5</sub> site-rich and electron-rich Ru nanoparticles. These findings offer valuable insights into the role of alkali metals and provide helpful guidance for designing efficient alkali metal-promoted ruthenium catalysts for practical applications.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"450 ","pages":"Article 116298"},"PeriodicalIF":6.5,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144488568","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}
引用次数: 0
Montmorillonite-mediated cobalt-doped Fe-MOF composites: a route to efficient photo-driven benzene hydroxylation 蒙脱石介导的钴掺杂Fe-MOF复合材料:光驱动苯羟基化的有效途径
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-06-25 DOI: 10.1016/j.jcat.2025.116297
Xu Jia , Jiaqi Zhang , Jiaolong Qiao , Zhiqi Song , Xuetong Xu , Liuxue Zhang , Xiulian Wang , Genxing Zhu , Shuyan Jiao
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