▎ 摘　　要

To elucidate the usage of graphene oxide (GO) as a photocatalysis material, we have studied the effect of epoxy and hydroxyl functionalization on the electronic structure, work function, CBM/VBM position, and optical absorption spectra of GO using density functional theory calculations. By varying the coverage and relative ratio of the surface epoxy (-O-) and hydroxyl (-OH) groups, both band gap and work function of the GO materials can be tuned to meet the requirement of photocatalyst. Interestingly, the electronic structures of GO materials with 40-50% (33-67%) coverage and OH:O ratio of 2:1(1:1) are suitable for both reduction and oxidation reactions for water splitting. Among of these systems, the GO composition with 50% coverage and OH:O (1:1) ratio can be very promising materials for visible-light-driven photocatalyst. Our results not only explain the recent experimental observations about 2-D graphene oxide as promising visible-light-driven photocatalyst materials but can also be very helpful in designing the optimal composition for higher performance. (C) 2012 Elsevier Inc. All rights reserved.