Publication

Disordered materials with resilient and soft-templated functional units bear the potential to fill the pipeline of robust catalysts for renewable energy storage. However, for novel materials lacking long-range order, the ability to discern local structure with atomic resolution still pushes the boundaries of current analytical and modeling approaches. We introduce a two-pillar strategy to monitor the formation and unravel the structure of the first disordered one-dimensional cobalt coordination polymer catalyst, Co-dppeO(2). This target material excels through proven high performance in commercial alkaline electrolyzers and organic transformations. We demonstrate that the key architecture behind this activity is the unconventional embedding of hydrated {H2O-Co-2(OH)(2)-OH2} edge-site motifs, nested into a flexible organic matrix of highly oxidized and bridging hydrophobic dppeO(2) ligands. Our combination of in situ spectroscopy and computational modeling of X-ray scattering and absorption spectra, backed with complementary experimental techniques, holds the key to understanding the atomic-range structure of important disordered materials.