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

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.