Journal
MATTER
Volume 1, Issue 5, Pages 1354-1369Publisher
CELL PRESS
DOI: 10.1016/j.matt.2019.06.021
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Funding
- University of Zurich, Switzerland
- University Research Priority Program (URPP) for Solar Light to Chemical Energy Conversion (LightChEC)
- Swiss National Science Foundation, Switzerland (Sinergia grant) [CRSII2_160801/1]
- QAFCO
- Qatar National Research Foundation, Qatar [NPRP10-0125-170246]
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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.
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