A New Class of Heteroatom‐Doped Porous Carbon Materials with Unprecedented High Volumetric Capacitive Performance

The design of simultaneously high mass density and large porosity carbon‐based materials has always been a challenging goal to fulfill the demands of next generation of high volumetric performance supercapacitors and other electrochemical devices. Here, we report a new class of high‐density heteroatom‐doped porous carbon as aqueous‐based supercapacitor materials via an in‐situ dehalogenation reaction between halogenated conjugated diene and nitrogen‐containing nucleophiles. Under reaction conditions, pyridinium salts with conjugated double bonds could continue to experience the dehalogenation reaction only if there is a trace amount of residue water from the starting materials. The as‐obtained carbon materials are highly doped by varied heteroatoms, which render high densities and endow abundant multimodal pores, leading to excellent volumetric capacitive performance. N, P, O‐tri‐doped porous carbon exhibits a high packing density (2.13 g cm‐3) and an exceptional volumetric energy density (36.8 Wh L‐1) in alkaline electrolytes, making it competitive to even some Ni‐MH cells.

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