铁基催化剂Fe_2P/C的设计合成及其温和条件下对硝基化合物的选择性催化加氢性能研究

The Design and Synthesis of Fe-based Catalyst Fe_2P/C with High Chemoselectivity of Hydrogenation of Nitro Compounds at Mild Conditions

调节金属纳米颗粒的催化活性及选择性是催化领域的一个长期课题.本文利用细菌(ATCC 19367)为含磷前驱体通过不同的金属/细菌比例及热解温度设计合成了一种新型铁基催化剂.过X-射线粉末衍射、场发扫描电子显微镜、透射电子显微镜、X-射线光电子能谱、电感耦合等离子体原子发射光谱仪等手段对所得化合物进行了结构及物相表征.本文针对不同热解时间,热解温度及金属比例系统的研究了催化剂的合成过程,通过分析表明,随着热解温度从600℃升到900℃,催化剂由单一的多孔碳逐渐到Fe_2P及Fe_2O_3转化.通过电子显微镜可以看出,金属纳米颗粒均匀的分布在多孔碳上.该铁基磷化物对硝基化合物具有较好的加氢还原催化功能,通过对比不同官能团取代的硝基催化加氢可以看出,常温常压下,该催化剂可以选择性的对硝基化合物的硝基进行加氢.通过循环实验证明,该催化剂具有很好的稳定性及可回收性.

Tuning the activity and selectivity of metal nanoparticles (NPs) is a long-term pursuit in the field of catalysis.Herein,a novel supported Fe-based catalyst was designed and synthesized by pyrolying the metal and the bacteria (ATCC 19367) within different temperature.The catalyst was characterized by powder X-ray diffraction,SEM,TEM,XPS and ICP.Interestingly,the materials will convert to C,Fe 2 P and Fe 2 O 3 step by step,due to the temperature up to 900 ℃ from 600 ℃.The EM images show Fe 2 P nanoparticles are well dispersed on porous carbon.The Fe-based catalyst is preferntially activate -NO 2 bond over other functional groups in water with hydrazine hydrate (HH).The experimental assessment of these hydrogenation of nitro compounds unveil that different size of Fe-based catalysts with different activity and selectivity with hydrogenation of the substrate.Moreover,this catalytic system is environmentally friendly because of its green solvent and harmless byproducts,and the catalyst shows outstanding stability and recyclability.