无模板法合成介孔棒状钴酸锰及其苯乙烯环氧化反应性能
Template-Free Synthesis and Boosting Catalytic Activity in Styrene Epoxidation of Mesoporous Rod-like MnCo2O4
作者单位E-mail
徐蔓 南京工业大学化工学院, 材料化学工程国家重点实验室, 南京 211800  
苏航 南京工业大学化工学院, 材料化学工程国家重点实验室, 南京 211800  
邵波 南京工业大学化工学院, 材料化学工程国家重点实验室, 南京 211800  
王芸 南京工业大学化工学院, 材料化学工程国家重点实验室, 南京 211800  
周诗健 南京工业大学化工学院, 材料化学工程国家重点实验室, 南京 211800 zshijian@njtech.edu.cn 
孔岩 南京工业大学化工学院, 材料化学工程国家重点实验室, 南京 211800 kongy36@njtech.edu.cn 
摘要: 通过简单的无模板水热法及煅烧处理成功合成了介孔棒状钴酸锰。采用X射线衍射(XRD)、场发射扫描电镜(FE-SEM)、透射电镜(TEM)、氮气吸附-脱附和X射线光电子能谱(XPS)等手段对材料的晶体结构、表面形貌、孔结构和表面化学组成进行了表征。结果表明,目标产物钴酸锰样品介孔结构形成良好,孔径分布在6 nm。此外,钴酸锰的棒状形貌直径为100~200 nm,长度为2~3 μm。相比于其他Co基、Mn基催化剂,钴酸锰被首次应用在苯乙烯环氧化反应中,表现出了极高的催化活性,苯乙烯的转化率达到95.8%,对氧化苯乙烯的选择性为58.2%。而且,在5次循环试验后,催化活性并没有发生明显的改变,进一步证明了催化剂的稳定性。同时,系统研究了主要反应参数(反应时间、反应温度、苯乙烯/叔丁基过氧化氢(TBHP)的物质的量比值)对介孔棒状钴酸锰催化活性的影响。
关键词: 钴酸锰  棒状形貌  水热合成  介孔结构  环氧化
基金项目: 国家自然科学基金(No.21476108,21276125,21776129,21706121)、江苏省自然科学基金(No.BK20170995)、江苏省高校自然科学研究项目(No.16KJB530003)和江苏省高等教育机构重点学科建设项目(PAPD)资助
Abstract: Mesoporous rod-like MnCo2O4 was fabricated via a facile template-free hydrothermal method and subsequent calcination. The crystal structure, surface morphology, pore structure and surface chemical composition were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), N2 adsorption-desorption and X-ray photoelectron spectra (XPS). Characterization results revealed that, in the target MnCo2O4 sample, the mesoporous structure was well-formed, and the pore size distribution was defined in 6 nm. Also, the particular rod-like morphology was obtained in MnCo2O4 with diameters of 100~200 nm and a length of 2~3 μm. Based on these, the MnCo2O4 sample was firstly used as a heterogeneous catalyst in the epoxidation of styrene. Compared with other Co-based and Mn-based catalysts, it exhibited relatively high catalytic activity, the conversion rate of styrene was 95.8%, and the selectivity of styrene oxide was 58.2%. Moreover, after five cycles, the catalytic activity did not change significantly, further confirming the stability of MnCo2O4. Meanwhile, the effects of main reaction parameters (reaction time, reaction temperature, the molar ratio of styrene to tert-butyl hydroperoxide (TBHP)) on the catalytic activity of mesoporous rod-like MnCo2O4 were systematically investigated.
Keywords: MnCo2O4  rod-like morphology  hydrothermal synthesis  mesoporous structure  epoxidation
投稿时间:2019-02-21 修订日期:2019-05-07
摘要点击次数:  288
全文下载次数:  216
徐蔓,苏航,邵波,王芸,周诗健,孔岩.无模板法合成介孔棒状钴酸锰及其苯乙烯环氧化反应性能[J].无机化学学报,2019,35(7):1121-1129.
查看全文  查看/发表评论  下载PDF阅读器
Support information: