负载型双金属金钯纳米颗粒作为硝基芳烃选择性加氢的催化剂

Supported Bimetallic AuPd Nanoparticles as a Catalyst for the Selective Hydrogenation of Nitroarenes.

作者信息

Qu Ruiyang, Macino Margherita, Iqbal Sarwat, Gao Xiang, He Qian, Hutchings Graham John, Sankar Meenakshisundaram

机构信息

Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK.

State Key Laboratory of Clean Energy Utilization, College of Energy Engineering, Zhejiang University, Hangzhou 310027, China.

出版信息

Nanomaterials (Basel). 2018 Sep 5;8(9):690. doi: 10.3390/nano8090690.

DOI:10.3390/nano8090690

PMID:30189685

原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6165381/

Abstract

The solvent-free selective hydrogenation of nitrobenzene was carried out using a supported AuPd nanoparticles catalyst, prepared by the modified impregnation method (M), as efficient catalyst >99% yield of aniline (AN) was obtained after 15 h at 90 °C, 3 bar H₂ that can be used without any further purification or separation, therefore reducing cost and energy input. Supported AuPd nanoparticles catalyst, prepared by M, was found to be active and stable even after four recycle experiments, whereas the same catalyst prepared by S was deactivated during the recycle experiments. The most effective catalyst was tested for the chemoselective hydrogenation of 4-chloronitrobenzene (CNB) to 4-chloroaniline (CAN). The activation energy of CNB to CAN was found to be 25 kJ mol, while that of CNB to AN was found to be 31 kJ mol. Based on this, the yield of CAN was maximized (92%) by the lowering the reaction temperature to 25 °C.

摘要

使用通过改进浸渍法（M）制备的负载型金钯纳米颗粒催化剂进行硝基苯的无溶剂选择性氢化反应，该催化剂作为高效催化剂，在90℃、3巴氢气条件下反应15小时后，可获得>99%产率的苯胺（AN），所得苯胺无需进一步纯化或分离即可使用，从而降低了成本和能源投入。通过改进浸渍法（M）制备的负载型金钯纳米颗粒催化剂即使在四次循环实验后仍具有活性和稳定性，而通过常规浸渍法（S）制备的相同催化剂在循环实验中失活。对最有效的催化剂进行了4-氯硝基苯（CNB）化学选择性氢化为4-氯苯胺（CAN）的测试。发现CNB氢化为CAN的活化能为25 kJ/mol-1，而CNB氢化为AN的活化能为31 kJ/mol-1。基于此，通过将反应温度降至25℃，CAN的产率最大化（92%）。