TiO2/graphene/NiFe-layered double hydroxide nanorod array photoanodes for efficient photoelectrochemical water splittingElectronic supplementary information (ESI) available: Experimental and computational details and supplementary figures and tables are included. See DOI: 10.1039/c6ee01092j

The ever-increasing demand for renewable and clean power sources has triggered the development of novel materials for photoelectrochemical (PEC) water splitting, but how to improve the solar conversion efficiency remains a big challenge. In this work, we report a conceptual strategy in a ternary material system to simultaneously enhance the charge separation and water oxidation efficiency of photoanodes by introducing reduced graphite oxide (rGO) and NiFe-layered double hydroxide (LDH) on TiO 2 nanorod arrays (NAs). An experimental-computational combination study reveals that rGO with a high work function and superior electron mobility accepts photogenerated electrons from TiO 2 and enables fast electron transportation; while NiFe-LDH acts as a cocatalyst which accelerates the surface water oxidation reaction. This synergistic effect in this ternary TiO 2 /rGO/NiFe-LDH photoanode gives rise to a largely enhanced photoconversion efficiency (0.58% at 0.13 V) and photocurrent density (1.74 mA cm −2 at 0.6 V). It is worth mentioning that the photocurrent density of TiO 2 /rGO/NiFe-LDH, to the best of our knowledge, is superior to previously reported TiO 2 -based photoanodes in benign and neutral media. In addition, the method presented here can be extended to the preparation of other efficient photoanodes (WO 3 /rGO/NiFe-LDH and α-Fe 2 O 3 /rGO/NiFe-LDH) toward high level PEC performance. TiO 2 /graphene/NiFe-layered double hydroxide nanorod arrays were fabricated as highly efficient photoanodes for photoelectrochemical water splitting with simultaneously enhanced charge separation and water oxidation efficiency.