The onion-like carbon (OLC) was prepared as adsorbent and tested for the removal of chromate ions from aqueous solutions. The OLC was thermally derived from nanodiamond by vacuum annealing at 1000-2000 degrees C. An investigation was conducted the chromate adsorption mechanism of OLC, by analysing the temperature-dependent evolution of the various oxygen-carbon bonds and the chemisorbed water by X-ray photo electron spectroscopy, as well as by the first principle calculation of the bond energies for relevant bond configurations. The present work demonstrated the importance of the carbon-oxygen bond type and carbon dangling bonds for chromate adsorption, as well as for other anionic heavy metals adsorbed from wastewater and sewage. (C) 2016 Elsevier B.V. All rights reserved.