A surface chemical approach of different pyrite size fraction is developed in this paper in the prospect of addressing the well-known coarse pyrite flotation challenge for environmental purposes. This work aims at exploring the effect of particle size on pyrite surface chemistry through the study of three pyrite size fractions up to 425 pm. Pyrite surface evolution was investigated through dry crushing, air oxidation and aqueous conditioning using X-ray photoelectron spectroscopy (XPS) and diffuse reflectance infrared spectroscopy (DRIFT) as complementary surface characterization tools. XPS, which characterized the outmost surface (about 40 angstrom depth), indicated that pyrite size fraction did not impact its surface chemistry after crushing. However, DRIFT which characterizes the whole oxidation layer, led to the conclusion that ferric sulfate was more abundant in the finer fraction than in the two coarser fractions. Those two surface characterization tools allowed a thorough insight into the three-dimensional oxidation product structures of pyrite from different size fractions. The surface evolution of coarse fractions had the same surface evolution trend when submitted to aging and conditioning processes than the fine pyrite size fraction, studied in previous works, in terms of surface species speciation and their relative proportion. Those results led to a better understanding of particle size impacts on pyrite surface chemistry. (C) 2012 Elsevier B.V. All rights reserved.