Probing the catalytic activity of porous graphene oxide and the origin of this behaviour

Chenliang Su, Muge Acik, Kazuyuki Takai, Jiong Lu, Si-jia Hao, Yi Zheng, Pingping Wu, Qiaoliang Bao, Toshiaki Enoki, Yves J. Chabal and Kian Ping Loh ()
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Chenliang Su: Graphene Research Centre, National University of Singapore
Muge Acik: University of Texas at Dallas
Kazuyuki Takai: Tokyo Institute of Technology
Jiong Lu: Graphene Research Centre, National University of Singapore
Si-jia Hao: Tokyo Institute of Technology
Yi Zheng: Graphene Research Centre, National University of Singapore
Pingping Wu: Graphene Research Centre, National University of Singapore
Qiaoliang Bao: Graphene Research Centre, National University of Singapore
Toshiaki Enoki: Tokyo Institute of Technology
Yves J. Chabal: University of Texas at Dallas
Kian Ping Loh: Graphene Research Centre, National University of Singapore

Nature Communications, 2012, vol. 3, issue 1, 1-9

Abstract: Abstract Graphene oxide, a two-dimensional aromatic scaffold decorated by oxygen-containing functional groups, possesses rich chemical properties and may present a green alternative to precious metal catalysts. Graphene oxide-based carbocatalysis has recently been demonstrated for aerobic oxidative reactions. However, its widespread application is hindered by the need for high catalyst loadings. Here we report a simple chemical treatment that can create and enlarge the defects in graphene oxide and impart on it enhanced catalytic activities for the oxidative coupling of amines to imines (up to 98% yield at 5 wt% catalyst loading, under solvent-free, open-air conditions). This study examines the origin of the enhanced catalytic activity, which can be linked to the synergistic effect of carboxylic acid groups and unpaired electrons at the edge defects. The discovery of a simple chemical processing step to synthesize highly active graphene oxide allows the premise of industrial-scale carbocatalysis to be explored.

Date: 2012
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DOI: 10.1038/ncomms2315

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