Unexpected Catalytic Performance in Silent Tantalum Oxide through Nitridation and Defect Chemistry

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• 作者：Yiguo Su ; Junyu Lang ; Liping Li ; Kai Guan ; Chunfang Du ; Liman Peng ; Dan Han ; Xiaojing Wang
• 刊名：The Journal of the American Chemical Society
• 出版年：2013
• 出版时间：August 7, 2013
• 年：2013
• 卷：135
• 期：31
• 页码：11433-11436
• 全文大小：310K
• 年卷期：v.135,no.31(August 7, 2013)
• ISSN：1520-5126

文摘

This work reports on the preparation of a noble-metal-free and highly active catalyst that proved to be an efficient and green reductant with renewable capacity. Nitridation of a silent Ta_1.1O_1.05 substrate led to the formation of a series of TaO_xN_y hollow nanocrystals that exhibited outstanding activity toward catalytic reduction of nitrobenzenes under ambient conditions. ESR and XPS results indicated that defective nitrogen species and oxygen vacancies at the surfaces of the TaO_xN_y nanocrystals may play synergetic roles in the reduction of nitrobenzenes. The underlying mechanism is completely different from those previously reported for metallic nanoparticles. This work may provide new possibilities for the development of novel defect-meditated catalytic systems and offer a strategy for tuning any catalysts from silent to highly reactive by carefully tailoring the chemical composition and surface defect chemistry.