Naphthalene Diimide‐Based Hydrogen‐Bonded Organic Framework for High Electrical Conductivity and Ammonia Sensor Applications

While metal‐organic frameworks (MOFs) and covalent organic frameworks (COFs) have been widely investigated as porous conductive materials, the research on the electrical properties of HOF materials has been limited. Moreover, the electrical conductivity of HOF materials is typically several orders of magnitude lower than that of MOFs and COFs. In this work, a HOF material based on naphthalene diimide is designed and achieved a remarkable electrical conductivity of 2.9 × 10−2 S cm−1 after hydrazine doping, which represents the highest value reported in the HOF system to date. In addition, this material exhibits a reversible change of its electrical conductivity under exposure to ammonia which is promising for gas‐sensor applications. The demonstration reveals a new dimension of HOFs as conductive materials and opens up possibilities for new HOF‐based devices. In recent years, porous materials have gained significant interest as functional materials. This study introduces a novel hydrogen‐bonded organic framework (HOF) based on naphthalene diimide, which, following chemical reduction, exhibits the highest electrical conductivity reported among HOF systems to date. Additionally, this framework demonstrates electrical reversibility during repeated ammonia doping and de‐doping cycles, suggesting its potential as a gas sensor.