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HPMoVO/CN-SBA-15催化下甲基丙烯醛选择性氧化制甲基丙烯酸

Selective oxidation of methacrolein to methacrylic acid over HPMoVO/CN-SBA-15.

作者信息

Zhou Lilong, Zhang Shanshan, Li Zhengjie, Scott Jason, Zhang Zhikun, Liu Runjing, Yun Jimmy

机构信息

College of Chemical and Pharmaceutical Engineering, Hebei University of Science and Technology Shijiazhuang Hebei province 050018 P. R. China

School of Chemical Engineering, The University of New South Wales Sydney NSW 2052 Australia

出版信息

RSC Adv. 2019 Oct 23;9(58):34065-34075. doi: 10.1039/c9ra06021a. eCollection 2019 Oct 18.

DOI:10.1039/c9ra06021a
PMID:35528902
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9073591/
Abstract

Molybdovanadylphosphoric acid (HPMV) was supported on a carbon nitride-modified SBA-15 (CN-SBA-15) molecular sieve to enhance its catalytic performance for oxidation of methacrolein (MAL) to methacrylic acid (MAA). HPMV/CN-SBA exhibited increased catalytic activity (20%) and five times greater MAA selectivity (98.9%) compared to bulk HPMV. HPMV supported on CN-SBA-15 exhibited much better catalytic performance as compared to that on other supports, such as KIT-6, HY zeolite, TiO, AlO, SiO, CNTs, and NH-modified CNTs. The supported HPMV was well characterized by FT-IR, XRD, SEM, N physical desorption, TG-DTA, NH-TPD, CO-TPD, XPS, and solid-state NMR. The CN minimized the interaction between the silica support and HPMV. HPMV was successfully separated from SBA-15, which was restricted by CN to increase stability and prevent interaction between the catalysts and support that would lead to decomposition of the catalysts during calcination and reaction. HPMV reacted with amino groups on the CN, which improved MAA selectivity and enhanced the thermal stability of the supported heteropoly acid (HPA) catalysts. This work identifies a new approach to preparing highly efficient and stable supported HPA catalysts for oxidation reactions.

摘要

将钒钼磷酸（HPMV）负载于氮化碳改性的SBA-15（CN-SBA-15）分子筛上，以提高其催化甲基丙烯醛（MAL）氧化为甲基丙烯酸（MAA）的性能。与块状HPMV相比，HPMV/CN-SBA的催化活性提高了20%，MAA选择性提高了5倍（98.9%）。与负载于其他载体（如KIT-6、HY沸石、TiO、AlO、SiO、碳纳米管和NH改性碳纳米管）上的HPMV相比，负载于CN-SBA-15上的HPMV表现出更好的催化性能。通过傅里叶变换红外光谱（FT-IR）、X射线衍射（XRD）、扫描电子显微镜（SEM）、N物理吸附、热重-差示热分析（TG-DTA）、氨程序升温脱附（NH-TPD）、一氧化碳程序升温脱附（CO-TPD）、X射线光电子能谱（XPS）和固体核磁共振（NMR）对负载型HPMV进行了很好的表征。CN使二氧化硅载体与HPMV之间的相互作用最小化。HPMV成功地从SBA-15中分离出来，CN限制了HPMV与SBA-15的相互作用，从而提高了稳定性，并防止催化剂与载体之间发生相互作用，而这种相互作用会导致催化剂在煅烧和反应过程中分解。HPMV与CN上的氨基发生反应，提高了MAA的选择性，增强了负载型杂多酸（HPA）催化剂的热稳定性。这项工作为制备用于氧化反应的高效稳定负载型HPA催化剂确定了一种新方法。

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