Fabrication of nitrogen-modified annealed nanodiamond with improved catalytic activity.

Abstract

Annealed ultradispersed nanodiamond (ADD) with sp(2) curved concentric graphitic shells is an interesting hybrid material consisting of the remarkable surface properties of graphene-based nanomaterials and the intrinsic properties of a diamond core. In this case, based on its specific properties and surface oxygen functional groups, nitrogen-modified ADD powders have been tunably synthesized via three different preparation methods in a calcination treatment process. The detailed formation and dynamic behaviors of the nitrogen species on the modified ADD during the preparation process are revealed by elemental analysis, X-ray photoelectron spectroscopy (XPS) and temperature-programmed desorption. Moreover, we study the catalytic performance on the metal-free nitrogen-modified ADD catalysts by means of selective oxidation of benzylic alcohols as a probe reaction. The results indicate that the modified ADD catalysts exhibit a higher catalytic activity than pristine ADD. By correlating XPS data with catalytic measurements, we conclude that the pyridinic nitrogen species plays a pivotal role in the catalytic reaction. Our work provides valuable information on the design of modified carbon materials with more excellent properties.