Coordination tuning of cobalt phosphates towards efficient water oxidation catalyst.,Nature Communications

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Coordination tuning of cobalt phosphates towards efficient water oxidation catalyst.
Nature Communications ( IF 14.7 ) Pub Date : 2015-Sep-14 , DOI: 10.1038/ncomms9253
Hyunah Kim ₁ , Jimin Park _{1,

2} , Inchul Park ₁ , Kyoungsuk Jin ₁ , Sung Eun Jerng ₃ , Sun Hee Kim ₃ , Ki Tae Nam ₁ , Kisuk Kang _{1,

4}

Affiliation

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.

中文翻译：

磷酸钴的配位调整以实现高效的水氧化催化剂。

开发高效稳定的水氧化催化剂对于实现实际可行的水分解系统是必要的。尽管广泛的研究集中在金属氧化物催化剂上，但金属配位对催化能力的影响仍然难以捉摸。在这里，我们选择了四种具有不同钴基团和磷酸基团配位的钴基磷酸盐催化剂作为平台，以更好地了解钴基材料的催化活性。尽管它们在水氧化过程中表现出各种催化活性和稳定性，但具有扭曲的钴四面体几何形状的Na2CoP2O7在中性条件下表现出与无定形磷酸钴相当的高活性，以及高结构稳定性。第一性原理计算表明，焦磷酸配体的表面重组会产生高度扭曲的四面体几何形状，其中水分子可以有利地结合，从而产生较低的过电势（~0.42 eV）。我们的研究结果强调了局部钴配位在催化中的重要性，并表明聚阴离子对水氧化化学的可能影响。

更新日期：2015-09-17

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