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


Triana, Carlos A; Moré, René; Bloomfield, Aaron J; Petrović, Predrag V; Ferrón, Sara Goberna; Stanley, George; Zarić, Snežana D; Fox, Thomas; Brothers, Edward N; Sheehan, Stafford W; Anastas, Paul T; Patzke, Greta R (2019). Soft Templating and Disorder in an Applied 1D Cobalt Coordination Polymer Electrocatalyst. Matter, 1(5):1354-1369.

Abstract

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-dppeO2. 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-Co2(OH)2-OH2} edge-site motifs, nested into a flexible organic matrix of highly oxidized and bridging hydrophobic dppeO2 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.

Abstract

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-dppeO2. 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-Co2(OH)2-OH2} edge-site motifs, nested into a flexible organic matrix of highly oxidized and bridging hydrophobic dppeO2 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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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
08 Research Priority Programs > Solar Light to Chemical Energy Conversion
Dewey Decimal Classification:540 Chemistry
Language:English
Date:1 November 2019
Deposited On:14 Feb 2020 09:22
Last Modified:14 Feb 2020 09:24
Publisher:Cell Press (Elsevier)
ISSN:2590-2393
OA Status:Green
Publisher DOI:https://doi.org/10.1016/j.matt.2019.06.021
Project Information:
  • : FunderSNSF
  • : Grant IDCRSII2_160801
  • : Project TitlePhotocatalytic Processes at Solvated Interfaces
  • : FunderQatar National Research Foundations
  • : Grant IDNPRP10-0125-170246
  • : Project Title

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