{"title":"香草醛氢脱氧负载钯金属镧有机骨架","authors":"Kavya Pradeepan , Shun Nishimura","doi":"10.1016/j.apcata.2025.120442","DOIUrl":null,"url":null,"abstract":"<div><div>Metal organic frameworks (MOFs) as effective supports have attracted interest in heterogeneous catalysis, especially for stabilizing metal species on the porous structure. Herein, we synthesize palladium-loaded lanthanum-based MOF (Pd/La-MOF) as an efficient catalyst for vanillin hydrodeoxygenation (HDO). The successful incorporation of Pd nanoparticles onto the La-MOF support was confirmed by a transmission electron microscopy (TEM), while the structural integrity of the La-MOF post-metal loading was verified through X-ray diffraction (XRD) analysis. Thermogravimetric analysis (TGA) demonstrated the thermal stability of the catalyst under reaction conditions. Fourier-transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS) and N<sub>2</sub> adsorption–desorption isotherms were employed to evaluate the functional groups, oxidation state, metal support interaction and specific surface area of the material. Catalytic performance of as-prepared Pd/La-MOF catalysts was evaluated for vanillin HDO. Among the different Pd loadings (0.5, 1.0, and 2.0 wt%), the 1.0 wt% Pd/La-MOF exhibited the highest creosol yield of 93 % within 6 h at 160°C under 1.0 MPa H₂ pressure. The reaction mechanism was proposed based on time-profile analysis. Comparative analysis with other Pd-loaded supports demonstrated the superior catalytic efficiency of La-MOF. Additionally, poisoning and leaching studies confirmed the role of acidic sites in creosol formation and the absence of Pd leaching during the reaction. Recyclability tests, along with post-reaction XRD and TEM analyses, confirmed the structural stability of the catalyst and uniform dispersion of Pd nanoparticles after multiple cycles. These results highlight the potential of La-MOF as a thermally stable and effective support for metal-based catalysts, particularly in the Pd-catalyzed HDO reactions.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"705 ","pages":"Article 120442"},"PeriodicalIF":4.7000,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Palladium-loaded lanthanum metal organic framework for vanillin hydrodeoxygenation\",\"authors\":\"Kavya Pradeepan , Shun Nishimura\",\"doi\":\"10.1016/j.apcata.2025.120442\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Metal organic frameworks (MOFs) as effective supports have attracted interest in heterogeneous catalysis, especially for stabilizing metal species on the porous structure. Herein, we synthesize palladium-loaded lanthanum-based MOF (Pd/La-MOF) as an efficient catalyst for vanillin hydrodeoxygenation (HDO). The successful incorporation of Pd nanoparticles onto the La-MOF support was confirmed by a transmission electron microscopy (TEM), while the structural integrity of the La-MOF post-metal loading was verified through X-ray diffraction (XRD) analysis. Thermogravimetric analysis (TGA) demonstrated the thermal stability of the catalyst under reaction conditions. Fourier-transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS) and N<sub>2</sub> adsorption–desorption isotherms were employed to evaluate the functional groups, oxidation state, metal support interaction and specific surface area of the material. Catalytic performance of as-prepared Pd/La-MOF catalysts was evaluated for vanillin HDO. Among the different Pd loadings (0.5, 1.0, and 2.0 wt%), the 1.0 wt% Pd/La-MOF exhibited the highest creosol yield of 93 % within 6 h at 160°C under 1.0 MPa H₂ pressure. The reaction mechanism was proposed based on time-profile analysis. Comparative analysis with other Pd-loaded supports demonstrated the superior catalytic efficiency of La-MOF. Additionally, poisoning and leaching studies confirmed the role of acidic sites in creosol formation and the absence of Pd leaching during the reaction. Recyclability tests, along with post-reaction XRD and TEM analyses, confirmed the structural stability of the catalyst and uniform dispersion of Pd nanoparticles after multiple cycles. These results highlight the potential of La-MOF as a thermally stable and effective support for metal-based catalysts, particularly in the Pd-catalyzed HDO reactions.</div></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":\"705 \",\"pages\":\"Article 120442\"},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2025-07-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis A: General\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926860X25003436\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis A: General","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926860X25003436","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Palladium-loaded lanthanum metal organic framework for vanillin hydrodeoxygenation
Metal organic frameworks (MOFs) as effective supports have attracted interest in heterogeneous catalysis, especially for stabilizing metal species on the porous structure. Herein, we synthesize palladium-loaded lanthanum-based MOF (Pd/La-MOF) as an efficient catalyst for vanillin hydrodeoxygenation (HDO). The successful incorporation of Pd nanoparticles onto the La-MOF support was confirmed by a transmission electron microscopy (TEM), while the structural integrity of the La-MOF post-metal loading was verified through X-ray diffraction (XRD) analysis. Thermogravimetric analysis (TGA) demonstrated the thermal stability of the catalyst under reaction conditions. Fourier-transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS) and N2 adsorption–desorption isotherms were employed to evaluate the functional groups, oxidation state, metal support interaction and specific surface area of the material. Catalytic performance of as-prepared Pd/La-MOF catalysts was evaluated for vanillin HDO. Among the different Pd loadings (0.5, 1.0, and 2.0 wt%), the 1.0 wt% Pd/La-MOF exhibited the highest creosol yield of 93 % within 6 h at 160°C under 1.0 MPa H₂ pressure. The reaction mechanism was proposed based on time-profile analysis. Comparative analysis with other Pd-loaded supports demonstrated the superior catalytic efficiency of La-MOF. Additionally, poisoning and leaching studies confirmed the role of acidic sites in creosol formation and the absence of Pd leaching during the reaction. Recyclability tests, along with post-reaction XRD and TEM analyses, confirmed the structural stability of the catalyst and uniform dispersion of Pd nanoparticles after multiple cycles. These results highlight the potential of La-MOF as a thermally stable and effective support for metal-based catalysts, particularly in the Pd-catalyzed HDO reactions.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.