Decomposition of formic acid (FA) to hydrogen and carbon dioxide through catalysis holds great promise for clean energy in fuel cells designed for portable use, but the selective and efficient dehydrogenation of FA by a robust heterogeneous catalyst under ambient conditions remains a major challenge. We report herein that a new FA dehydrogenation system comprising liquid FA and amines with high boiling point as hydrogen storage material can be efficiently decomposed for ultrapure H-2 release under mild reaction conditions. Of significant importance is that a high turnover frequency (TOF) of up to 1166 h(-1) can be readily attained at 60 degrees C in FA-dimethylethanolamine system using gold nano particles supported on amphoteric zirconia (Au/ZrO2). The amine acts as a proton scavenger can facilitate the O-H bond cleavage in the key step of FA deprotonation in Au-ZrO2 interface resulting in high catalytic activity. The versatile gold catalyst displayed excellent stability for dimethylethanolamine-assisted FA dehydrogenation as well as a typical particle-size-dependent effect. (C) 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.