香草醛氢脱氧负载钯金属镧有机骨架

IF 4.7 2区 化学 Q2 CHEMISTRY, PHYSICAL
Kavya Pradeepan , Shun Nishimura
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引用次数: 0

摘要

金属有机骨架(MOFs)作为一种有效的载体,在多相催化方面引起了人们的兴趣,特别是在多孔结构上稳定金属物种。本文合成了负载钯的镧基MOF (Pd/La-MOF)作为香兰素氢脱氧(HDO)的高效催化剂。通过透射电子显微镜(TEM)验证了钯纳米粒子在La-MOF载体上的成功结合,同时通过x射线衍射(XRD)分析验证了La-MOF后金属负载的结构完整性。热重分析(TGA)证实了催化剂在反应条件下的热稳定性。采用傅里叶变换红外光谱(FT-IR)、x射线光电子能谱(XPS)和N2吸附-解吸等温线对材料的官能团、氧化态、金属载体相互作用和比表面积进行了表征。考察了Pd/La-MOF催化剂对香兰素HDO的催化性能。在不同Pd负载(0.5、1.0和2.0 wt%)中,1.0 wt% Pd/La-MOF在1.0 MPa h₂压力下,在160°C下,6 h内的甲酚收率最高,为93 %。基于时间剖面分析,提出了反应机理。与其他负载pd载体的对比分析表明,La-MOF具有较好的催化效率。此外,中毒和浸出研究证实了酸性位点在甲酚形成中的作用,以及反应过程中Pd浸出的缺失。可回收性测试以及反应后的XRD和TEM分析证实了催化剂的结构稳定性和多次循环后钯纳米粒子的均匀分散。这些结果突出了La-MOF作为金属基催化剂的热稳定和有效载体的潜力,特别是在pd催化的HDO反应中。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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.
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
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.
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