Premium
A Nano‐Fibrillated Mesoporous Carbon as an Effective Support for Palladium Nanoparticles in the Aerobic Oxidation of Alcohols “on Pure Water”
Author(s) -
Karimi Babak,
Behzadnia Hesam,
Bostina Mihnea,
Vali Hojatollah
Publication year - 2012
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201200373
Subject(s) - catalysis , x ray photoelectron spectroscopy , mesoporous material , heteroatom , carbonization , alcohol oxidation , carbon fibers , palladium , chemical engineering , materials science , nanoparticle , chemistry , adsorption , inorganic chemistry , organic chemistry , nanotechnology , composite material , ring (chemistry) , composite number , engineering
A novel nano‐fibrillated mesoporous carbon (IFMC) was successfully prepared via carbonization of the ionic liquid 1‐methyl‐3‐phenethyl‐1 H ‐imidazolium hydrogen sulfate ( 1 ) in the presence of SBA‐15. The material was shown to be an efficient and unique support for the palladium nanoparticle (PdNP) catalyst Pd@IFMC ( 2 ) in aerobic oxidation of heterocyclic, benzylic, and heteroatom containing alcohols on pure water at temperatures as low as 40 °C for the first time and giving almost consistent activities and selectivities within more than six reaction runs. The catalyst has also been employed as an effective catalyst for the selective oxidation of aliphatic and allylic alcohols at 70–80 °C. The materials were characterized by X‐ray photoelectron spectroscopy (XPS), N 2 adsorption–desorption analysis, transmission electron microscopy (TEM), and electron tomography (ET). Our compelling XPS and ET studies showed that higher activity of 2 compared to Pd@CMK‐3 and Pd/C in the aerobic oxidation of alcohols on water might be due to the presence of nitrogen functionalities inside the carbon structure and also the fibrous nature of our materials. The presence of a nitrogen heteroatom in the carboneous framework might also be responsible for the relatively uniform and nearly atomic‐scale distribution of PdNPs throughout the mesoporous structure and the inhibition of Pd agglomeration during the reaction, resulting in high durability, high stability, and recycling characteristics of 2 . This effect was clearly confirmed by comparing the TEM images of the recovered 2 and Pd@CMK‐3.