Silica-pillared and non-pillared H2Ti4O9 samples were doped with nitrogen from urea as a nitrogen precursor for visible light photocatalysis The photocatalytic activities of the nitrogen-doped samples were evaluated for hydrogen evolution from aqueous methanol solution Techniques such as XRD FT-IR TG-DSC SEM XPS and UV-visible diffuse reflectance spectroscopy were adopted to explore the characteristics of the materials The silica-pillared H2Ti4O9 sample is more stable than the non-pillared one and its layered structure was retained well at temperatures up to 500 degrees C The interlayer spacing of H2Ti4O9 was expanded from 2 7 angstrom to 7 2 angstrom after being pillared with silica Silica pillaring could have a profound impact on nitrogen doping and the resultant photocatalytic activity The interlayer spacing of the silicapillared H2Ti4O9 did not change after nitrogen doping in contrast that of the non-pillared H2Ti4O9 was reduced by 44% after the same doping process despite the fact that the non-pillared sample showed better nitrogen doping properties With expanded interlayer spicing and better retained layered structure the silica-pillared and nitrogen-doped H2Ti4O9 performed much better than the non-pillared counterpart for hydrogen evolution under visible light irradiation (C) 2010 Elsevier B V All rights reserved