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

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.%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.