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| 三维介孔氨基三亚甲基膦酸锆的合成及其担载铁催化剂的甲醛催化氧化活性 | |
| 引用本文： | 贾云洁,李明磊,崔纪利,刘亮,王润伟,义建军,徐庆红.三维介孔氨基三亚甲基膦酸锆的合成及其担载铁催化剂的甲醛催化氧化活性[J].无机化学学报,2013,29(3):465-473. |
| 作者姓名： | 贾云洁 李明磊 崔纪利 刘亮 王润伟 义建军 徐庆红 |
| 作者单位： | 1. 北京化工大学化工资源有效利用国家重点实验室,北京,100029 2. 吉林大学无机合成与制备化学国家重点实验室,长春,130012 3. 中国石油天然气集团公司石油化工研究院,北京,100083 |
| 基金项目： | 国家自然科学基金(No.50602004)、吉林大学无机合成与制备化学国家重点实验室开放课题基金、北京化工大学大学生科技训练计划资 助项目。 |
| 摘 要： | 以氧氯化锆和氨基三亚甲基膦酸(ATMP)为原料合成了一种新型介孔材料氨基三亚甲基膦酸锆(NTAZP)。使用XRD、FTIR、TG-DTA和SEM等手段对所合成的介孔材料进行了结构表征和形貌分析。然后以NTAZP为载体,用Fe(NO3)3水溶液处理,得到担载Fe3+的氨基三亚甲基膦酸锆。研究结果表明,Fe3+被吸附到载体孔道中后,NTAZP结构未被破坏,Fe3+离子与NTAZP孔壁骨架上的N发生了配位作用。铁担载NTAZP(NTAZP-Fe3+)对甲醛氧化具有良好的催化活性,催化反应条件温和,催化剂稳定性良好。以载体NTAZP担载铁还避免了Fe3+进入水体,催化剂得以回收利用,避免造成二次污染。NTAZP-Fe3+是一种高效绿色的新型小分子醛类化合物氧化催化剂。 |
| 关 键 词： | 催化 催化剂 催化剂制备 催化剂载体 有机膦酸锆 介孔 配位负载 氧化 |
| 收稿时间： | 2012/7/12 0:00:00 |
| 修稿时间： | 2012/10/7 0:00:00 |
3D-Mesoporous Zirconium Phosphonate NTAZP: Synthesis and Formaldehyde Oxidation by Its Supported Fe3+ Catalyst |
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| JIA Yun-Jie,LI Ming-Lei,CUI Ji-Li,LIU Liang,WANG Run-Wei,YI Jian-Jun and XU Qing-Hong.3D-Mesoporous Zirconium Phosphonate NTAZP: Synthesis and Formaldehyde Oxidation by Its Supported Fe3+ Catalyst[J].Chinese Journal of Inorganic Chemistry,2013,29(3):465-473. | |
| Authors: | JIA Yun-Jie LI Ming-Lei CUI Ji-Li LIU Liang WANG Run-Wei YI Jian-Jun and XU Qing-Hong |
| Institution: | State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin university, Changchun 130012, China;Petrochemical Research Institute, PetroChina Company Limited, Beijing 100083, China;State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China |
| Abstract: | A new mesoporous zirconium phosphonate(NTAZP) was synthesized by using nitrilotris(methylene)-triphosphonic acid (ATMP) and zirconium dichloride oxide octahydrate. The as-prepared mesoporous materials were characterized by XRD, FTIR, TG-DTA and SEM techniques. Fe3+-based aminotrialkylene zirconium phosphonate catalyst was obtained by using NTAZP as the support and by treating the support with an aqueous solution of Fe(NO3)3. The results indicate that the structure and morphology of NTAZP are not changed after loading, and ferric species are mainly anchored on NTAZP via the coordinative interactions between Fe3+ and N atoms inside the mesoporous channel. The supported ferric species NTAZP (NTAZP-Fe3+) with a good thermal stability are highly catalytic active for formaldehyde oxidation in relatively mild reaction conditions. The Fe-based catalyst can prevent Fe3+ from dissolving into the water, and can be recycled to avoid secondary pollution. NTAZP-Fe3+ is a high-efficient and green catalyst in small-molecule aldehydes oxidation. |
| Keywords: | catalysis catalyst catalyst preparation coordination load zirconium phosphonates mesoporous coordination loading oxidation |
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