A few metal-organic frameworks (MOFs), which typically use strong acids as proton sources, display superprotonic conductivity (≈10 S cm ); however, they are rare due to the instability of MOFs in highly acidic conditions. For the first time, we report superprotonic conductivity using a moderately acidic guest, zwitterionic sulfamic acid (HSA), which is encapsulated in MOF-808 and MIL-101. HSA acts not only as a proton source but also as a proton-conducting medium due to its extensive hydrogen bonding ability and zwitterion effect. A new sustained concentration gradient method results in higher HSA encapsulation compared to conventional methods, producing 10HSA@MOF-808-(bSA) and 8HSA@MIL-101. These MOFs show impressive superprotonic conductivity of 2.47×10 and 3.06×10 S cm , respectively, at 85 °C and 98 % relative humidity, and maintain stability for 7 days.
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