Engineering Complex, Layered Metal Oxides: High-Performance Nickelate Oxide Nanostructures for Oxygen Exchange and Reduction

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• 作者：Xianfeng Ma ; Juliana S. A. Carneiro ; Xiang-Kui Gu ; Hao Qin ; Hongliang Xin ; Kai Sun ; Eranda Nikolla
• 刊名：ACS Catalysis
• 出版年：2015
• 出版时间：July 2, 2015
• 年：2015
• 卷：5
• 期：7
• 页码：4013-4019
• 全文大小：383K
• ISSN：2155-5435

文摘

Synthetically tuning the surface properties of many oxide catalysts to optimize their catalytic activity has been appreciably challenging, given their complex crystal structure. Nickelate oxides (e.g., La₂NiO_4+未) are among complex, layered oxides with great potential toward efficiently catalyzing chemical/electrochemical reactions involving oxygen (oxygen reduction, ammonia oxidation). Our theoretical calculations show that the surface structure of La₂NiO_4+未 plays a critical role in its activity, with the (001)-Ni oxide-terminated surface being the most active. This is demonstrated through the effect on the energetics associated with surface oxygen exchange, a key process in reactions involving oxygen on these oxides. Using a reverse microemulsion method, we have synthesized La₂NiO_4+未 nanorod-structured catalysts highly populated by (001)-Ni oxide-terminated surfaces. We show that these nanostructures exhibit superior catalytic activity toward oxygen exchange/reduction as compared with traditional catalysts while maintaining stability under reaction conditions. The findings reported here pave the way for engineering complex metal oxides with optimal activity.