Redox-active nitroxyl-containing polymers are promising candidates as possible replacements for inorganic based energy-storage materials, due to their high energy density and fast redox kinetics. One challenge towards the implementation of such a system is the insufficient electrical conductivity, impeding the charge collection even with highly conductive additives. Herein, the first implementation of a polymeric bis(salicylideniminato) nickel (NiSalen) conductive backbone as an active charge-collecting wire is reported. NiSalen simultaneously serves as a charge collector for nitroxyl pendants and supports the redox capacity of the material. This novel polymer exhibits a specific capacity of up to 91.5 mAh g−1, retaining 87 % of its theoretical capacity at 800 C and more than 30 % at as high as 3000 C (66 % capacity retention after 2000 cycles). The properties of the new material upon operation was studied by means of operando electrochemical methods, UV-Vis, and electron paramagnetic resonance spectroscopy.
