Coordination tuning of cobalt phosphates towards efficient water oxidation catalyst

Hyunah Kim, Jimin Park, Inchul Park, Kyoungsuk Jin, Sung Eun Jerng, Sun Hee Kim, Ki Tae Nam () and Kisuk Kang ()
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Hyunah Kim: Research Institute of Advanced Materials (RIAM), Seoul National University
Jimin Park: Research Institute of Advanced Materials (RIAM), Seoul National University
Inchul Park: Research Institute of Advanced Materials (RIAM), Seoul National University
Kyoungsuk Jin: Research Institute of Advanced Materials (RIAM), Seoul National University
Sung Eun Jerng: Western Seoul Center, Korea Basic Science Institute (KBSI)
Sun Hee Kim: Western Seoul Center, Korea Basic Science Institute (KBSI)
Ki Tae Nam: Research Institute of Advanced Materials (RIAM), Seoul National University
Kisuk Kang: Research Institute of Advanced Materials (RIAM), Seoul National University

Nature Communications, 2015, vol. 6, issue 1, 1-11

Abstract: Abstract The development of efficient and stable water oxidation catalysts is necessary for the realization of practically viable water-splitting systems. Although extensive studies have focused on the metal-oxide catalysts, the effect of metal coordination on the catalytic ability remains still elusive. Here we select four cobalt-based phosphate catalysts with various cobalt- and phosphate-group coordination as a platform to better understand the catalytic activity of cobalt-based materials. Although they exhibit various catalytic activities and stabilities during water oxidation, Na2CoP2O7 with distorted cobalt tetrahedral geometry shows high activity comparable to that of amorphous cobalt phosphate under neutral conditions, along with high structural stability. First-principles calculations suggest that the surface reorganization by the pyrophosphate ligand induces a highly distorted tetrahedral geometry, where water molecules can favourably bind, resulting in a low overpotential (∼0.42 eV). Our findings emphasize the importance of local cobalt coordination in the catalysis and suggest the possible effect of polyanions on the water oxidation chemistry.

Date: 2015
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DOI: 10.1038/ncomms9253

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