Cooperative Stabilization of the Pyridinium-CO-Co Adduct on a Metal-Organic Layer Enhances Electrocatalytic CO Reduction.

08:00 EDT 11th October 2019 | BioPortfolio

Summary of "Cooperative Stabilization of the Pyridinium-CO-Co Adduct on a Metal-Organic Layer Enhances Electrocatalytic CO Reduction."

Pyridinium has been shown as a co-catalyst for electrochemical reduction of CO on metal and semiconductor electrodes but its exact role has been difficult to elucidate. In this work, we create cooperative cobalt-protoporphyrin (CoPP) and pyridinium (pyH) catalytic sites on metal-organic layers (MOLs) for electrocatalytic CO reduction reaction (CORR). Constructed from [Hf(µ-O)(µ-OH)(HCO)] secondary building units (SBUs) and terpyridine-based tricarboxylate ligands, the MOL was post-synthetically functionalized with CoPP via carboxylate exchange with formate capping groups. The CoPP group and the pyridinium (pyH) moiety on the MOL coactivate CO by forming the [pyH-OC-CoPP] adduct, which enhances CORR and suppresses hydrogen evolution to afford a high CO/H selectivity of 11.8. Cooperative stabilization of the [pyH-OC-CoPP] intermediate led to a catalytic current density of 1314 mA/mgCo for CO production at -0.86 V, which corresponds to a turnover frequency of 0.4 s.


Journal Details

This article was published in the following journal.

Name: Journal of the American Chemical Society
ISSN: 1520-5126


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