Significance Two-dimensional (2D) polyaniline (PANI) has been realized for the first time, to our knowledge, by direct solid-state reaction of organic single crystals. The 2D PANI framework consists of six nitrogen atoms that periodically surround a phenyl ring. Pristine 2D PANI (undoped) has electrical conductivity of 0.72 S/cm, which is 10 10 times higher than its linear analog (undoped, 6.28 × 10 −11 S/cm). When it is doped by hydrochloric acid (HCl), its conductivity jumps to almost 1,960 times (1.41 × 10 3 S/cm). Due to its highest conductivity among organic materials, we very strongly believe that this well-defined 2D PANI and its heterogeneity with C and N elements will open up a new research field of layered 2D materials beyond linear PANI and other organic/inorganic 2D materials.
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