Abstract Polypyrrole (PPy) represents an intriguing class of materials for high‐performance pseudocapacitor electrode due to their fast and reversible Faradaic redox reaction. However, these pseudocapacitors suffer from several disadvantages such as low capacitance and charge/discharge cycling instability, which can be attributed to the poor charge‐transfer capability and stability of PPy. Previously, it is found that charge hopping is more efficient in the crystalline domain of PPy, and thus higher charge‐transfer capability can be achieved from PPy with higher crystallinity. However, the polymerization of pyrrole monomers usually forms randomly entangled chains, which results in PPy with a high fraction of amorphous domains. Therefore, synthesis of PPy with higher crystallinity remains challenging. Here, air–water interface‐confined polymerization (ICP) strategy is introduced to synthesize PPy with enhanced crystallinity. Three kinds of crystalline PPy with different dopants (chlorion ion, 4‐[[4‐(dimethylamino)phenyl]diazenyl]benzenesulfonate anion, and β‐naphthalene sulfonate anion) are synthesized via ICP. The PPy synthesized from ICP is demonstrated to have an improved electrochemical performance. This work will shed light on the synthesis methods and mechanisms to form PPy with improved crystallinity and electrochemical performances.
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