Experimental visualization of lithium diffusion in LixFePO4

Chemical energy storage using batteries will become increasingly important for future environmentally friendly ('green') societies. The lithium-ion battery is the most advanced energy storage system, but its application has been limited to portable electronics devices owing to cost and safety issues(1). State-of-the-art LiFePO4 technology as a new cathode material with surprisingly high charge-discharge rate capability has opened the door for large-scale application of lithium-ion batteries such as in plug-in hybrid vehicles(2-5). The scientific community has raised the important question of why a facile redox reaction is possible in the insulating material(6-14). Geometric information on lithium diffusion is essential to understand the facile electrode reaction of LixFePO4 (0 < x < 1), but previous approaches have been limited to computational predictions(15,16). Here, we provide long-awaited experimental evidence for a curved one-dimensional chain for lithium motion. By combining high-temperature powder neutron diffraction and the maximum entropy method, lithium distribution along the [010] direction was clearly visualized.