Electrochemical oxygen activation driven by enamine-keto push-pull interactions in triazole-based covalent organic polymers

We have developed two triazole-based covalent organic polymers (COPs) with donor-acceptor motifs. The keto-enriched COP demonstrated exceptional oxygen activation via electrochemical stimuli, driven by strong push-pull interactions. In situ studies and DFT calculations confirmed the critical role of enamine carbon positive charges in enhancing performance, setting new benchmarks in COP design. Extended π-conjugated COPs has been synthesized, containing triazole-linked carbon as the active site accelerating ORR. The push-pull interactions mechanism of the ORR in alkaline medium is explored through the Pauling model and in situ FTIR study.