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We demonstrate that (NH 4 ) 2 Si 0.5 Ti 0.5 P 4 O 13 is an excellent proton conductor. The crystallographic information concerning the hydrogen positions is unraveled from neutron-powder-diffraction (NPD) data for the first time. This study shows that all the hydrogen atoms are connected though H bonds, establishing a two-dimensional path between the [(Si 0.5 Ti 0.5 )P 4 O 13  2- ] n layers for proton diffusion across the crystal structure by breaking and reconstructing intermediate H-O═P bonds. This transient species probably reduces the potential energy of the H jump from an ammonium unit to the next neighboring NH 4  + unit. Both theoretical and experimental results support an interstitial-proton-conduction mechanism. The proton conductivities of (NH 4 ) 2 Si 0.5 Ti 0.5 P 4 O 13 reach 0.0061 and 0.024 S cm -1 in humid air at 125 and 250 °C, respectively. This finding demonstrates that (NH 4 ) 2 Si 0.5 Ti 0.5 P 4 O 13 is a promising electrolyte material operating at 150-250 °C. This work opens up a new avenue for designing and fabricating high-performance inorganic electrolytes.

inorganic chemistry

Visualization of the Diffusion Pathway of Protons in (NH4)2Si0.5Ti0.5P4O13 as an Electrolyte for Intermediate-Temperature Fuel Cells