Abstract
The oxygen reduction reaction (ORR) is a corner stone for energy conversion techniques such as fuel cells and metal-air batteries[1]. The use of Pt unfortunately generate a number of obstacles including the high cost, scarcity and readily poisoning by impurity and the cross-over of fuel9. Shaped bimetallic nanocrystals (NCs) with precisely controlled structure and composition at the atomic level, e.g. PtxNi1−x alloy NCs[2], intermetallic PtCo core–shell nanoparticles[3] and Pt3Ni nanoframes[4], represent a class of exciting and promising ORR catalysts. Herein, we demonstrate a one-pot protocol for the controlled synthesis of icosahedral Pt3M nanocrystal with twenty active Pt3M (111) facets using glucosamine as both reducing and structure-directing agent. Among the investigated catalysts, the Pt3Ni icosahedral with nano-segregated Pt-skin displays the unexpected 32-fold enhancement in specific activity and 12-fold improvement in mass activity relative to state-of-the-art Pt/C catalyst. Besides, the catalyst was found ultra-robust during 20,000 potential cycling tests. The Pt3Ni icosahedral thus represents one class of the most efficient ORR electrocatalysts ever reported and demonstrates an effect technique in mimicing the active extended surface in nano-scale. Fig.1 (a) TEM image of the typical icosahedral Pt3Ni nanocrystal, (b) HRTEM micrograph showing the twin boundaries of five-fold symmetry, (c) the (111) and (200) planes, (d)cyclic voltammetry curves of Pt/C, Pt NI/C and Pt3Ni/C catalysts, (e) ORR polarization curves for Pt/C, Pt NI/C and Pt3Ni/C catalysts in O2-saturated 0.1M HClO4, (f) comparative ORR activities of Pt/C and Pt3Ni/C catalysts before and after 20,000 potential cycles. Acknowledgments The study was financed by the National Basic Research Program of China (973 Program, 2012CB215500), the National Natural Science Foundation of China (21373199, 21433003) and the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA09030104).
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