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单层 HNb3O8 可见光响应选择性光催化氧化苄醇。

Monolayer HNb3O8 for selective photocatalytic oxidation of benzylic alcohols with visible light response.

机构信息

State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou 350002 (P.R. China).

出版信息

Angew Chem Int Ed Engl. 2014 Mar 10;53(11):2951-5. doi: 10.1002/anie.201311280. Epub 2014 Feb 12.

Abstract

Monolayer HNb3O8 2D nanosheets have been used as highly chemoselective and active photocatalysts for the selective oxidation of alcohols. The nanosheets exhibit improved photocatalytic activity over their layered counterparts. Results of in situ FTIR, DRS, ESR, and DFT calculations show the formation of surface complexes between the Lewis acid sites on HNb3O8 2D nanosheets and alcohols. These complexes play a key role in the photocatalytic activity of the material. Furthermore, the unique structural features of the nanosheets contributed to their high photocatalytic activity. An electron transition from the coordinated alcohol species to surface Nb atoms takes place and initiates the aerobic oxidation of alcohols with high product selectivity under visible light irradiation. This reaction process is distinct from that of classic semiconductor photocatalysis.

摘要

单层 HNb3O8 二维纳米片已被用作高度选择性和活性的光催化剂,用于醇的选择性氧化。纳米片表现出比层状对应物更高的光催化活性。原位 FTIR、DRS、ESR 和 DFT 计算结果表明,在 HNb3O8 二维纳米片的路易斯酸位和醇之间形成了表面配合物。这些配合物在材料的光催化活性中起着关键作用。此外,纳米片的独特结构特征有助于其具有高的光催化活性。电子从配位的醇物种向表面 Nb 原子跃迁,并在可见光照射下引发醇的有氧氧化,具有高的产物选择性。这个反应过程与经典半导体光催化不同。

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