Two-dimensional (2D) conductive metal-organic frameworks (MOFs), whose advanced electrical properties accompany their intrinsic structural characteristics, represent an exciting new class of 2D atomic crystals for the van der Waals integration of novel heterostructures and the development of novel nano/quantum devices. Guided by topology, we report two 2D MOFs (1 and 2) constructed via combination of [In(COO)₄]⁻ metal nodes and tetratopic tetrathiafulvalene (TTF)-based linkers, with ultrahigh proton conductivity (6.66 × 10⁻⁴ and 1.30 × 10⁻² S cm⁻¹ for 1 and 2, respectively). Additionally, high electrical conductivity was simultaneously achieved with the pure protonic nature of the 2D MOF 2. The electrical conduction at the MOF-metal interface is enabled by the redox-switchable behavior of the TTF-based ligands. This unique charge-transport mechanism, protonic/pseudo-capacitance coupling, offers a new strategy for utilizing the ionic conductivity from MOFs to construct functional electronic devices.

二维（2D）导电金属有机骨架（MOF）具有先进的电性能以及其固有的结构特征，代表了令人兴奋的新型2D原子晶体，可用于新型异质结构的范德华整合和新型纳米/量子设备。在拓扑学的指导下，我们报告了通过[In（COO）₄ ] ^-金属节点和基于四主题四硫富瓦烯（TTF）的连接基的组合构建的两个二维MOF（1 和 2），具有超高质子传导性（6.66×10 ^-4和1.30） ×10 ^-2小号厘米^-1为1和2， 分别）。另外，具有2D MOF 2的纯质子特性，同时实现了高电导率。通过基于TTF的配体的氧化还原可切换行为，可以在MOF-金属界面上实现导电。这种独特的电荷传输机制，质子/伪电容耦合，为利用MOF的离子传导性构建功能性电子设备提供了新的策略。