Applied Catalysis A: General最新文献_第2页

Efficient and recyclable tetramethylguanidine-functionalized polyacrylonitrile fiber catalyst tailored for high-yield knoevenagel condensation 高效可回收的四甲基胍功能化聚丙烯腈纤维催化剂，专为高收率knoevenagel缩合而设计

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-07-22 DOI: 10.1016/j.apcata.2025.120456

Yanfei Zhang , Jinxin Liu , Xiaoting Li , Ning Ma , Minli Tao , Wenqin Zhang

{"title":"Efficient and recyclable tetramethylguanidine-functionalized polyacrylonitrile fiber catalyst tailored for high-yield knoevenagel condensation","authors":"Yanfei Zhang , Jinxin Liu , Xiaoting Li , Ning Ma , Minli Tao , Wenqin Zhang","doi":"10.1016/j.apcata.2025.120456","DOIUrl":"10.1016/j.apcata.2025.120456","url":null,"abstract":"<div><div>This work presents a novel and recyclable tetramethylguanidine-modified polyacrylonitrile fiber catalyst (PAN<sub>MG</sub>F), specifically designed for the Knoevenagel condensation reaction, which is a crucial method in organic synthesis for C<img>C bond formation. The PAN<sub>MG</sub>F was characterized through Fourier-transform infrared spectroscopy (FT-IR), elemental analysis (EA), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and mechanical performance analysis. These results collectively confirmed the successful grafting of dimethylcyanamide as a guanidine precursor, which was subsequently converted into tetramethylguanidine functionalities on the PAN<sub>MG</sub>F. Under mild conditions of 40 °C with H<sub>2</sub>O as the solvent for a 12-hour reaction, the PAN<sub>MG</sub>F exhibited superior catalytic performance, with a yield of 97 %. A thorough investigation of various benzaldehyde substrates revealed yields exceeding 90 % for both electron-withdrawing and electron-donating derivatives. These results demonstrate the remarkable substrate versatility and broad applicability of this catalyst. Moreover, when applied to other active methylene substrates, such as methyl cyanoacetate and malononitrile, the PAN<sub>MG</sub>F achieved yields of 97 % and 98 %, respectively. These results collectively underscore its broad substrate scope across 28 different substrates and exceptional stability, which maintained a yield of 91.1 % even after 14 cycles, with an 89.9 % yield observed in the 15th cycle. Additionally, gram-scale experiments yielded a high separation efficiency of 93.6 %, further reinforcing the significant potential of PAN<sub>MG</sub>F for practical applications in sustainable organic synthesis.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"705 ","pages":"Article 120456"},"PeriodicalIF":4.7,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144696531","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

Coordination number dependence of Pt catalysts for catalytic decomposition of aqueous hydroxylammonium nitrate (HAN) Pt催化剂催化分解硝酸羟铵配位数依赖性研究

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-07-21 DOI: 10.1016/j.apcata.2025.120457

Shu Liu , Yujia Han , Teng Zong , Chaojie Wang , Ming Tian , Lin Li , Wansheng Zhang , Wentao Wang , Xiaodong Wang

{"title":"Coordination number dependence of Pt catalysts for catalytic decomposition of aqueous hydroxylammonium nitrate (HAN)","authors":"Shu Liu , Yujia Han , Teng Zong , Chaojie Wang , Ming Tian , Lin Li , Wansheng Zhang , Wentao Wang , Xiaodong Wang","doi":"10.1016/j.apcata.2025.120457","DOIUrl":"10.1016/j.apcata.2025.120457","url":null,"abstract":"<div><div>To uncover the relation between active metals structure and the adsorption, activation as well as its decomposition performance of hydroxylamine nitrate (HAN) that has been considered to be a promising low-toxicity monopropellant for spacecrafts, the performance of xPt/Al<sub>2</sub>O<sub>3</sub> with various Pt loadings (x = 0.1, 0.5, 1 and 2, indicates the mass percentage of Pt) was evaluated in the aqueous HAN (10 wt%) decomposition. It was found that the both the NH<sub>3</sub>OH<sup>+</sup> conversion and the turnover frequency (TOF) enhanced as Pt loadings increased while NO<sub>3</sub><sup>-</sup> was hardly converted at the temperature of lower than 120 ℃ for xPt/Al<sub>2</sub>O<sub>3</sub>, and 2Pt/Al<sub>2</sub>O<sub>3</sub> exhibited the best activity with almost 100 % NH<sub>3</sub>OH<sup>+</sup> conversion, 20 % NH<sub>4</sub><sup>+</sup> selectivity and 80 % N<sub>2</sub>O selectivity at around 120 ℃, respectively. This originated from the increased Pt coordinated number of active sites with sufficiently continuous Pt sites caused by its enhanced particle size with loadings, which was beneficial to the cracking of N-O, O-H and N-H bonds together thus the activation and conversion of NH<sub>3</sub>OH<sup>+</sup> to NH<sub>4</sub><sup>+</sup> and N<sub>2</sub>O.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"705 ","pages":"Article 120457"},"PeriodicalIF":4.7,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144696557","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

Exploring the bifunctional role of Pd/ZrO2-TiO2 in the production of secondary amines via reductive amination of furfural 探索Pd/ZrO2-TiO2在糠醛还原胺化生产仲胺中的双功能作用

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-07-18 DOI: 10.1016/j.apcata.2025.120455

Alex A. Fernández-Andrade , John A. Vergara , Daviel Gómez , Daniela González-Vera , Cristian H. Campos , Joan M. Rodríguez-Díaz , Luis E. Arteaga-Pérez

{"title":"Exploring the bifunctional role of Pd/ZrO2-TiO2 in the production of secondary amines via reductive amination of furfural","authors":"Alex A. Fernández-Andrade , John A. Vergara , Daviel Gómez , Daniela González-Vera , Cristian H. Campos , Joan M. Rodríguez-Díaz , Luis E. Arteaga-Pérez","doi":"10.1016/j.apcata.2025.120455","DOIUrl":"10.1016/j.apcata.2025.120455","url":null,"abstract":"<div><div>Environmental concerns and the pressing need for sustainable technologies have increased the interest in furfural (FUR) amination as an environmentally friendly alternative to current petroleum-based amination processes. Here we systematically investigate the bifunctional effect of Pd/ZrO<sub>2</sub>-TiO<sub>2</sub> for the one-pot reductive amination of FUR with aniline (ANI) using H<sub>2</sub> as the reducing agent. The structural characterization of Pd/ZrO<sub>2</sub>-TiO<sub>2</sub> indicated Ti atom substitutions by Zr, highly dispersed Zr sites, and modulated acidity. The Pd/ZrO<sub>2</sub>-TiO<sub>2</sub> catalyst was active and stable for converting FUR into N-furfurylaniline (FFA) following a sequential reaction map, involving the formation of an intermediate imine (IME), with subsequent hydrogenation. The water formed in the first reaction step does not interfere in the reaction performance as confirmed by FTIR-ATR <em>in situ</em> measurements. Finally, the effectiveness of the catalyst was explained by the presence of acid sites which enhance C<img>O and N = H activation, with subsequent hydrogenation promoted by Pd<sup>0</sup> sites.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"705 ","pages":"Article 120455"},"PeriodicalIF":4.7,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144663185","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

In-situ growth of NiFe-LDH/fluoride heterostructures on FeN4/C for bifunctional oxygen electrocatalysis 双功能氧电催化在FeN4/C上原位生长NiFe-LDH/氟化物异质结构

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-07-16 DOI: 10.1016/j.apcata.2025.120454

Jie Yang , Lixia Ma , Yuqi Zhang , Xuqian Zhao , Shouren Zhang , Luo Huang , Yunpeng Fang , Xiaojie Zhou , Jianghao Kang , Ruibin Jiang

{"title":"In-situ growth of NiFe-LDH/fluoride heterostructures on FeN4/C for bifunctional oxygen electrocatalysis","authors":"Jie Yang , Lixia Ma , Yuqi Zhang , Xuqian Zhao , Shouren Zhang , Luo Huang , Yunpeng Fang , Xiaojie Zhou , Jianghao Kang , Ruibin Jiang","doi":"10.1016/j.apcata.2025.120454","DOIUrl":"10.1016/j.apcata.2025.120454","url":null,"abstract":"<div><div>The design of low-cost and highly efficient bifunctional electrocatalyst towards oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is challengeable, which limits the commercial application of rechargeable zinc-air battery. Herein, an efficient ORR and OER bifunctional electrocatalyst (NiFe-LDH/F<sub>x</sub>−FeN<sub>4</sub>/C) is composed of nickel/iron-based heterostructures sparsely grown on carbon black (CB) with single FeN<sub>4</sub> sites. The NiFe-LDH/F<sub>x</sub><strong>−</strong>FeN<sub>4</sub>/C electrocatalysts are prepared through the pyrolysis of hemin chloride adsorbed on CB, followed by in-situ hydrothermal growth of NiFe-LDH/F<sub>x</sub> heterostructures. The NiFe-LDH/F<sub>x</sub> heterostructures are composed of NiFe-LDH, (NH<sub>4</sub>)<sub>3</sub>FeF<sub>6</sub>, and NiF<sub>2</sub>. The elevated valence states of Fe and Ni in heterostructures significantly increase the OER activity. The mesopores and large pores of the NiFe-LDH/F<sub>x</sub><strong>−</strong>FeN<sub>4</sub>/C facilitate the exposure of active sites and enhance mass transfer. These features contribute to the outstanding bifunctional activity of NiFe-LDH/F<sub>x</sub><strong>−</strong>FeN<sub>4</sub>/C, achieving a half-wave potential of 0.906 V for the ORR, an OER overpotential of 246 mV at 10 mA cm<sup>−2</sup>, and an extremely small voltage gap of 0.57 V. Additionally, the NiFe-LDH/F<sub>x</sub><strong>−</strong>FeN<sub>4</sub>/C-based RZAB also exhibits a peak power density of 209 mW cm<sup>−2</sup> and charging/discharging cycling stability for 445 h. This work establishes a novel strategy for the preparation of highly efficient bifunctional electrocatalysts through in-situ growth and heterostructure engineering.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"705 ","pages":"Article 120454"},"PeriodicalIF":4.7,"publicationDate":"2025-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144655561","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

Cu-MOF-derived Cu/C catalysts via solvent polarity engineering with renewable ligand for efficient hydrogenation of levulinic acid to γ-valerolactone 基于可再生配体的Cu- mof衍生Cu/C催化剂的高效乙酰丙酸加氢制备γ-戊内酯

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-07-15 DOI: 10.1016/j.apcata.2025.120453

Weimeng Cai , Haojie Du , Erju Wang , Yuting Qiang , Kunhong Hu , Jianhua Guo

{"title":"Cu-MOF-derived Cu/C catalysts via solvent polarity engineering with renewable ligand for efficient hydrogenation of levulinic acid to γ-valerolactone","authors":"Weimeng Cai , Haojie Du , Erju Wang , Yuting Qiang , Kunhong Hu , Jianhua Guo","doi":"10.1016/j.apcata.2025.120453","DOIUrl":"10.1016/j.apcata.2025.120453","url":null,"abstract":"<div><div>The synthesis of value-added chemicals from renewable biomass is becoming increasingly important in the transition to a sustainable and low-carbon energy system. Herein, we demonstrate a solvent-polarity modulation strategy to engineer biomass-derived Cu-MOF using 2,5-furandicarboxylic acid (FDCA) as a renewable ligand, where tailored β/α ratios via Kamlet-Taft parameters balance nucleation-growth kinetics to optimize textural properties. Pyrolyzed Cu-MOF at 500 °C under a nitrogen atmosphere yield the Cu/C catalysts, which were subsequently employed in the selective hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). Among the various solvents used, the Cu-MOF precursor synthesized in a mixed solvent of methanol and N, N-dimethylformamide (DMF) demonstrated the highest catalytic performance, outperforming those synthesized in other solvents. This highlights the significant impact of solvent selection on the structure of Cu-MOF, which in turn affects their hydrogenation activity. Advanced characterization confirming that the uniform Cu dispersion (confirmed by HRTEM mapping) and Cu⁰/Cu⁺ electronic synergy (via Cu Auger analysis) enhanced hydrogenation performance. Additionally, the biomass-derived catalysts exhibited excellent durability. Overall, this research provides a promising approach to develop highly efficient catalysts using renewable ligands and demonstrates the potential of regulating catalyst properties through the strategic selection of solvents, as informed by Kamlet-Taft parameters.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"705 ","pages":"Article 120453"},"PeriodicalIF":4.7,"publicationDate":"2025-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144665524","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

Octa-ion pair-functionalized POSS bridging homogeneous catalysis and heterogeneous recycle for fixation of CO2 八离子对功能化POSS桥接均相催化和非均相循环固定CO2

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-07-15 DOI: 10.1016/j.apcata.2025.120452

Xin Yuan , Ziqi Liu , Zhenjiang Li , Jiahui Ma , Yanqi Shi , Min Zhang , Yujia Wang , Xin Zou , Sha Li , Kai Guo

{"title":"Octa-ion pair-functionalized POSS bridging homogeneous catalysis and heterogeneous recycle for fixation of CO2","authors":"Xin Yuan , Ziqi Liu , Zhenjiang Li , Jiahui Ma , Yanqi Shi , Min Zhang , Yujia Wang , Xin Zou , Sha Li , Kai Guo","doi":"10.1016/j.apcata.2025.120452","DOIUrl":"10.1016/j.apcata.2025.120452","url":null,"abstract":"<div><div>Bridging the gap of the exact molecular design of homogenous catalyst and the recyclability of heterogenous catalyst was a challenge, especially for the cycloaddition of carbon dioxide to epoxide (CCE) reactions due to the high boiling points of the product cyclic carbonates that exclude evaporation separations. We introduce octa-ion pair-functionalized polyhedral oligomeric silsesquioxanes (IP-POSS) nanoparticle catalyst featured homogenous catalysis and heterogenous recycle for catalytic CCE reactions. Guanidinium phenolate ion pairs covalently anchored on cubic POSS. A typical IP-POSS catalyst bearing 4-pyridinolate (4-OP⁻) and 1,5,7-triazabicyclo[4.4.0]dec-5-enium (TBDH⁺) ion pair, <strong>POSS-4-OP⁻·TBDH</strong><sup><strong>+</strong></sup>, was evaluated in CCE reactions by catalyst loading of 0.20 mol% at 120 °C and 1.0 MPa (CO<sub>2</sub>); high yield (97 %) and quantitative selectivity (99 %) was achieved by 24 h with a turnover number of 490. The high catalytic performance of the IP-POSS was attributed to the proximity effect. Bifunctional catalytic mechanism was proposed where pyridinolate attacked CO<sub>2</sub> and TBDH⁺ activated epoxide and validated by NMR titrations. The IP-POSS catalyst worked homogenously in CCE reaction mixtures at 120 °C, it aggregated spontaneously as the CO<sub>2</sub> vented and the temperature lowered to ambient by the end of the transformation. The precipitated IP-POSS was simply filtrated and recycled for 7 times with robust recovery (96–98 % yields, 99 % selectivity). A reversible homogenous catalysis to and fro heterogenous recycle of IP-POSS in a closed-loop was explained by the inter-nanoparticle bridging by dimeric ion paring, that aggregated and precipitated the IP-POSS. This work unveiled a practical strategy for developing nanoparticle organocatalysts that worked in homogeneous solvents and recycled in heterogeneous precipitation.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"705 ","pages":"Article 120452"},"PeriodicalIF":4.7,"publicationDate":"2025-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144696562","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

Efficient desulfurization of model diesel fuel using an amphiphilic bimetallic synergistic catalyst Mo/Zn-EG-K 两亲性双金属催化剂Mo/Zn-EG-K对模型柴油的高效脱硫研究

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-07-14 DOI: 10.1016/j.apcata.2025.120445

Mingyan Chen , Haiqiong Wang , Dehua Zhang , Yucheng Liu

{"title":"Efficient desulfurization of model diesel fuel using an amphiphilic bimetallic synergistic catalyst Mo/Zn-EG-K","authors":"Mingyan Chen , Haiqiong Wang , Dehua Zhang , Yucheng Liu","doi":"10.1016/j.apcata.2025.120445","DOIUrl":"10.1016/j.apcata.2025.120445","url":null,"abstract":"<div><div>Carbon-based materials, particularly expanded graphite (EG), serve as excellent catalyst supports due to their high surface area, mechanical stability, and defect-rich structure. This study developed an amphiphilic Mo/Zn-EG-K catalyst by anchoring Zn/Mo oxides on EG and modifying it with KH550 silane, balancing lipophilic (methoxy) and hydrophilic (amino) properties to enhance oxidative desulfurization (ODS) efficiency. Characterization (TEM, Py-IR, etc.) confirmed the catalyst’s structure and amphiphilicity. Under optimized conditions (60 °C, O/S=10, 60 min), 99.12 % dibenzothiophene (DBT) conversion was achieved, reducing sulfur content below 10 ppm—outperforming most Mo-based catalysts. The reaction followed first-order kinetics, and the catalyst retained 95 % activity after five cycles. Mechanistic studies revealed that Zn enhances surface electrophilicity, promoting H₂O₂ activation to generate •O₂⁻ radicals, which form reactive Mo(O₂) species. These intermediates selectively oxidize DBT into polar sulfoxides/sulfones, subsequently extracted by acetonitrile. The catalyst demonstrated strong performance in real diesel and continuous-flow systems, highlighting its industrial potential for ultra-deep desulfurization.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"705 ","pages":"Article 120445"},"PeriodicalIF":4.7,"publicationDate":"2025-07-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144702300","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

Superb three-dimensional porous-structured metal foam-supported Ni/Ce/Al-CF ensemble as an active structured catalyst for hydrogen production via methanol decomposition 极好的三维多孔结构金属泡沫支撑Ni/Ce/Al-CF系综作为甲醇分解制氢的活性结构催化剂

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-07-13 DOI: 10.1016/j.apcata.2025.120450

Lijie Fu , Yong Men , Shuya Wu , Shuyi Xu , Guohong Wang , Chongchong Kong , Jinguo Wang , Feng Shi , Zhenrong Yan , Xuelong Miao

{"title":"Superb three-dimensional porous-structured metal foam-supported Ni/Ce/Al-CF ensemble as an active structured catalyst for hydrogen production via methanol decomposition","authors":"Lijie Fu , Yong Men , Shuya Wu , Shuyi Xu , Guohong Wang , Chongchong Kong , Jinguo Wang , Feng Shi , Zhenrong Yan , Xuelong Miao","doi":"10.1016/j.apcata.2025.120450","DOIUrl":"10.1016/j.apcata.2025.120450","url":null,"abstract":"<div><div>A series of metal foam-supported Ni-based catalysts-monometallic Ni-CF, bimetallic Ni/Ce-CF, Ni/Al-CF and trimetallic Ni/Ce/Al-CF-were prepared by modified wet chemical etching (MWCE) and employed for hydrogen production via methanol decomposition (MD) in the temperature range of 200–325 ℃. Among those catalysts, the 2Ni/3Ce/3Al-Cu foam (CF) catalyst shows the superior catalytic performance for hydrogen production, achieving a remarkable activity of almost complete methanol conversion (99.3 %) and high H<sub>2</sub> selectivity of 91.8 % at 300 ℃. Moreover, the performance of 2Ni/3Ce/3Al-CF catalyst remained stable during the stability test for up to 40 h at 275 ℃. SEM and BET characterization show that etched copper foam can remarkably enlarge the specific surface area of the structured catalyst, provide more active sites, and enhance its catalytic activity. The strong interaction among Ni, Ce and Al induce the synergistic effect by creating abundant oxygen vacancies in the trimetallic system as evidenced by XPS. H<sub>2</sub>-TPR and XPS further revealed a crucial balance between reducibility and metal-support interactions: Al-containing catalysts like 2Ni/3Ce/3Al-CF exhibit higher reduction thresholds and confirming the role of Al in stabilizing oxidized Ni species via strong metal-support interactions. And CH<sub>3</sub>OH-TPD analysis indicated the catalyst had much higher low-temperature hydrogen production than other catalysts because of the synergistic effect of three metals, consistent with the catalyst activity test results. The developed strategy may provide insights into the development of the design principles for high-performance structured catalysts for hydrogen production via methanol decomposition.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"705 ","pages":"Article 120450"},"PeriodicalIF":4.7,"publicationDate":"2025-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144632318","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

Ce3+-incorporated HZSM-5 as efficient catalysts with rich-strong Brønsted acid sites for cyclohexene hydration Ce3+-掺入HZSM-5作为环己烯水化的高效催化剂，具有丰富的强Brønsted酸位

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-07-13 DOI: 10.1016/j.apcata.2025.120451

Hefang Wang , Shijiao Hao , Hui Jiang, Xiaofei Ma, Hashim Khan, Jingwei Liu, Weiqian Qi

{"title":"Ce3+-incorporated HZSM-5 as efficient catalysts with rich-strong Brønsted acid sites for cyclohexene hydration","authors":"Hefang Wang , Shijiao Hao , Hui Jiang, Xiaofei Ma, Hashim Khan, Jingwei Liu, Weiqian Qi","doi":"10.1016/j.apcata.2025.120451","DOIUrl":"10.1016/j.apcata.2025.120451","url":null,"abstract":"<div><div>A series of Ce<sup>3+</sup> incorporated HZSM-5 catalysts were prepared by wet impregnation method for cyclohexene hydration. XRD, Vacuum-IR, XPS, and <sup>29</sup>Si NMR confirmed the successful incorporation of Ce<sup>3+</sup> into the HZSM-5. NH<sub>3</sub>-TPD and Py-IR analyses revealed that Ce-HZSM-5 catalyst significantly increased strong Brønsted acid density compared to HZSM-5. Further, the strong Brønsted/Lewis acid ratio of 3.0Ce-HZSM-5 is 4-fold higher than that of HZSM-5 (9.2 vs 2.3). As a result, the catalyst exhibited excellent activity with 12.7 % conversion of cyclohexene and 99.9 % selectivity to cyclohexanol and maintained high catalytic performance after five cycles. In situ FTIR was used to investigate the cyclohexene hydration reaction mechanism. The results showed that Ce<sup>3+</sup> interacts with Si–OH to form a new strong Bronsted acid site (Si–OH–Ce). This site can effectively promote the activation of cyclohexene and significantly enhance the catalytic hydration performance.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"705 ","pages":"Article 120451"},"PeriodicalIF":4.7,"publicationDate":"2025-07-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144663186","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

Solvent-induced one-pot catalytic conversion of xylose to high yield γ-valerolactone over Zr-Beta zeolite 溶剂诱导木糖在Zr-Beta沸石上一锅催化转化为高产γ-戊内酯

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-07-12 DOI: 10.1016/j.apcata.2025.120449

Tinghao Han , Zhongdi Liu , Lincai Peng , Weipeng Song , Huai Liu , Wenlong Jia , Rui Zhang

{"title":"Solvent-induced one-pot catalytic conversion of xylose to high yield γ-valerolactone over Zr-Beta zeolite","authors":"Tinghao Han , Zhongdi Liu , Lincai Peng , Weipeng Song , Huai Liu , Wenlong Jia , Rui Zhang","doi":"10.1016/j.apcata.2025.120449","DOIUrl":"10.1016/j.apcata.2025.120449","url":null,"abstract":"<div><div>The efficient production of γ-valerolactone (GVL) with high yield directly from xylose is of particular interest but remains a great challenge due to the long reaction path. We herein developed a facile catalytic system to directly convert xylose to GVL with a record-high yield of 54.3 %, employing β-zeolite supported Zr-based catalyst in 1,4-dioxane/isopropanol co-solvent. Using Zr(NO<sub>3</sub>)<sub>4</sub>·5 H<sub>2</sub>O as the Zr sources resulting in well-retained β-zeolite structure, larger surface area and pore volume and better dispersion of Zr species, as well as balanced acidic sites where higher amount of Brønsted acid sites promoted the ring-opening of furfural alcohol for this cascade reaction. Notably, the introduction of 1,4-dioxane facilitated the <em>in situ</em> formation of furfural (i.e. yield-determining step) by diluting the competitive adsorption behavior between isopropanol and xylose, allowing more xylose molecules to access the active center, thus promoting the sequential production of GVL with unexpectedly high yield. The present work provides a efficient and straightforward preparation of GVL from xylose, paving the pathway towards higher atom economy.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"705 ","pages":"Article 120449"},"PeriodicalIF":4.7,"publicationDate":"2025-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144632368","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}

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