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Porous crystalline metal-organic frameworks (MOFs) or porous coordination polymers (PCPs) are emerging as a new class of proton conductors with numerous investigations. Some of the MOFs exhibit an excellent proton-conducting performance (higher than 10 -2 S cm -1 ) originating from the interesting hydrogen(H)-bonding networks with guest molecules, where the conducting medium plays a crucial role. In the overwhelming majority of MOFs, the conducting medium is H 2 O because of its degenerate conjugate acid-base system (H3O + + H 2 O ⇔ H 2 O + H 3 O + or OH - + H 2 O ⇔ H 2 O + OH - ) and the efficient H-bonding ability through two proton donor and two acceptor sites with a tetrahedral geometry. Considering the systematic molecular similarity to water, ammonia (NH 3 ; NH 4  + + NH 3 ⇔ NH 3 + NH 4  + ) is promising as the next proton-conducting medium. In addition, there are few reports on NH 3 -mediated proton conductivity in MOFs. In this perspective, we provide overviews of the degenerate water (hydronium or hydroxide)- or ammonia (ammonium)-mediated proton conduction system, the design strategies for proton-conductive MOFs, and the conduction mechanisms.

Proton transfer in hydrogen-bonded degenerate systems of water and ammonia in metal–organic frameworks