Journal
JOURNAL OF CATALYSIS
Volume 307, Issue -, Pages 246-253Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2013.07.026
Keywords
Photocatalysis; Graphitic carbon nitride; Urea; Phenylurea; Water splitting
Categories
Funding
- National Basic Research Program of China (973 Program) [2013CB632405]
- National Natural Science Foundation of China [21173043, 21033003]
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Phenylurea has been integrated into the traditional polymerization route of carbon nitride (CN) precursors (e.g., urea, thiourea, dicyandiamide, and ammonium thiocyanide) in a facile one-pot approach, to modify the chemical composition, electronic structure, and catalytic performance of graphitic CN (g-CN). Results revealed that the co-polymerization of phenylurea with urea dramatically modifies the optical and electronic properties of g-CN, leading to a remarkable improvement by a factor of 9 in the photocatalytic activity of g-CN (when coupled with Pt as a co-catalyst) in an assay of hydrogen evolution reaction, while still keeping a high catalytic stability during pre-longed operations. The active catalyst is eventually a hybrid organocatalyst that is a heterogeneous Pt catalyst supported on a urea-based polymer. The promotional effect of phenylurea as the co-monomer for urea on the activity and stability of Pt/g-CN-could be related to the-extension-of delocalized pi-conjugated system of CN heterocycles, as a result of the fusion of phenyl motifs in the CN framework. The thus created surface dyadic structure favors the separation and migration of charge-carriers photoexcited upon light illumination. This work highlights a wide accessibility of chemical protocols for the design and synthesis of functional CN photocatalysts at molecular levels by applying suitable CN precursors and co-monomers. (C) 2013 Elsevier Inc. All rights reserved.
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