在尖晶石 Co3O4 的几何位依赖水氧化活性的原位鉴定。
In Operando Identification of Geometrical-Site-Dependent Water Oxidation Activity of Spinel Co3O4.
机构信息
School of Chemical and Biomedical Engineering, Nanyang Technological University , Block N1.2, 62 Nanyang Drive, Singapore 637459, Singapore.
Department of Chemistry, National Taiwan University , Taipei, 106, Taiwan, Republic of China.
出版信息
J Am Chem Soc. 2016 Jan 13;138(1):36-9. doi: 10.1021/jacs.5b10525. Epub 2015 Dec 31.
Spinel Co3O4, comprising two types of cobalt ions: one Co(2+) in the tetrahedral site (Co(2+)(Td)) and the other two Co(3+) in the octahedral site (Co(3+)(Oh)), has been widely explored as a promising oxygen evolution reaction (OER) catalyst for water electrolysis. However, the roles of two geometrical cobalt ions toward the OER have remained elusive. Here, we investigated the geometrical-site-dependent OER activity of Co3O4 catalyst by substituting Co(2+)(Td) and Co(3+)(Oh) with inactive Zn(2+) and Al(3+), respectively. Following a thorough in operando analysis by electrochemical impedance spectroscopy and X-ray absorption spectroscopy, it was revealed that Co(2+)Td site is responsible for the formation of cobalt oxyhydroxide (CoOOH), which acted as the active site for water oxidation.
尖晶石 Co3O4 由两种类型的钴离子组成：一种位于四面体位置的 Co(2+)（Co(2+)(Td)），另一种位于八面体位置的 Co(3+)（Co(3+)(Oh)）。它已被广泛探索作为一种有前途的析氧反应 (OER) 催化剂用于水电解。然而，两种几何钴离子对 OER 的作用仍然难以捉摸。在这里，我们通过分别用非活性 Zn(2+)和 Al(3+)取代 Co(2+)(Td)和 Co(3+)(Oh)，研究了 Co3O4 催化剂的几何位依赖性 OER 活性。通过电化学阻抗谱和 X 射线吸收光谱的深入原位分析，揭示了 Co(2+)Td 位负责形成钴氧氢氧化物 (CoOOH)，它作为水氧化的活性位点。
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