Soft Templating and Disorder in an Applied 1D Cobalt Coordination Polymer Electrocatalyst

Abstract

Disordered materials with resilient and soft-templated functional units bear thepotential to fill the pipeline of robust catalysts for renewable energy storage.However, for novel materials lacking long-range order, the ability to discernlocal structure with atomic resolution still pushes the boundaries of currentanalytical and modeling approaches. We introduce a two-pillar strategy tomonitor the formation and unravel the structure of the first disordered one-dimensional cobalt coordination polymer catalyst, Co-dppeO2.Thistargetmaterial excels through proven high performance in commercial alkalineelectrolyzers and organic transformations. We demonstrate that the key archi-tecture behind this activity is the unconventional embedding of hydrated{H2O-Co2(OH)2-OH2} edge-site motifs, nested into a flexible organic matrix ofhighly oxidized and bridging hydrophobic dppeO2ligands. Our combinationofin situspectroscopy and computational modeling of X-ray scattering andabsorption spectra, backed with complementary experimental techniques,holds the key to understanding the atomic-range structure of importantdisordered materials.