Abstract

The key to designing and fabricating highly efficient mixed protonic-electronic conductors materials (MPECs) is to integrate the mixed conductive active sites into a single structure, to break through the shortcomings of traditional physical blending. Herein, based on the host-guest interaction, an MPEC is consisted of 2D metal-organic layers and hydrogen-bonded inorganic layers by the assembly methods of layered intercalation. Noticeably, the 2D intercalated materials (≈1.3nm) exhibit the proton conductivity and electron conductivity, which are 2.02 × 10-5 and 3.84 × 10-4 S cm-1 at 100°C and 99% relative humidity, much higher than these of pure 2D metal-organic layers (>>1.0 × 10-10 and 2.01×10-8 S cm-1 ), respectively. Furthermore, combining accurate structural information and theoretical calculations reveals that the inserted hydrogen-bonded inorganic layers provide the proton source and a networks of hydrogen-bonds leading to efficient proton transport, meanwhile reducing the bandgap of hybrid architecture and increasing the band electron delocalization of the metal-organic layer to greatly elevate the electron transport of intrinsic 2D metal-organic frameworks.

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