Amplifying Reactivity of Bio‐Inspired [FeFe]‐Hydrogenase Mimics by Organic Nanotubes

Abstract A bio‐inspired FeFe hydrogenase model which catalyses hydrogen evolution reaction (HER) in acidic solutions is immobilized in polyaniline (PANI)‐based nanotubes. A combination of analytical techniques reveals that this construct maintains both the molecular signatures of the bio‐inspired complex and the material properties of PANI. The amine and imine‐rich environment of the PANI chain amplifies the inherent HER activity of the bio‐inspired complex, allowing electrocatalytic HER at neutral pH, with lower overpotentials and higher current densities compared to the bio‐inspired complex alone. This construct retains the oxygen stability of the bio‐inspired complex and remains stable through several hours of aerobic electrolysis, producing only 6.5 % H₂O₂ from the competing oxygen reduction reaction (ORR).