Catalytic decomposition of hydrous hydrazine (N2H4.H2O) has received considerable attention as a promising chemical hydrogen storage system. But the currently available N2H4.H2O decomposition catalysts always showed poor durability. In the present paper, we report an experimental study of the performance degradation of Ni-Pt/CeO2 catalyst using TPD-MS, FTIR, HRTEM techniques. Our study on the post-used Ni-Pt/CeO2 catalyst found that a predominant N-2 species and various reaction intermediates over-strongly bound on the catalyst surface. Furthermore, the amount of the bound N-2 species at Ni sites is approximately linearly correlated with the activity decay degree. These results provide a straightforward explanation of the performance degradation phenomenon and highlight the critical role of adsorbate/catalyst interaction in determination of the catalytic performance. (C) 2017 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.