催化学报 ›› 2014, Vol. 35 ›› Issue (10): 1591-1608.DOI: 10.1016/S1872-2067(14)60082-6

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负载氧化钒催化剂的多波长拉曼光谱研究:结构识别和定量

吴自力   

  1. 橡树岭国家实验室, 纳米材料科学中心和化学科学部, 美国田纳西州橡树岭
  • 收稿日期:2014-04-28 修回日期:2014-05-22 出版日期:2014-09-28 发布日期:2014-09-30
  • 通讯作者: 吴自力
  • 基金资助:

    本研究工作是在美国橡树岭国家实验室的纳米材料研究中心进行的,该中心由美国能源部下属的基础能源科学部的科学用户设施处资助. 其中纳米形状CeO2的合成工作是由能源部的科学办公室下属基础能源科学部的化学,地理和生物科学处资助的.

Multi-wavelength Raman spectroscopy study of supported vanadia catalysts:Structure identification and quantification

Zili Wu   

  1. Center for Nanophase Materials Sciences and Chemical Science Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
  • Received:2014-04-28 Revised:2014-05-22 Online:2014-09-28 Published:2014-09-30
  • Supported by:

    This research was conducted at the Center for Nanophase Materials Sciences, which is sponsored at Oak Ridge National Laboratory by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. Part of the work including the synthesis of ceria nanoshapes was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division.

摘要:

探究负载金属氧化物的结构是确立催化剂结构和催化性能之间相互关系的首要条件. 在众多表征技术中,多波长拉曼光谱结合了共振拉曼和由不同波长激发的非共振拉曼,不仅在识别负载金属氧化物团簇的结构,而且在定量方面已经成为强有力的工具. 本文以两个负载氧化钒体系(VOx/SiO2,VOx/CeO2)为例,阐述了如何利用该技术研究活性氧化物团簇的多相结构,并理解氧化物团簇和载体之间复杂的相互作用. 由多波长拉曼光谱得到的定性和定量信息能为设计更有效的负载金属氧化物催化剂提供基本的依据.

关键词: 多波长, 拉曼光谱, 共振拉曼, 氧化钒, 二氧化硅, 二氧化铈

Abstract:

Revealing the structure of supported metal oxide catalysts is a prerequisite for establishing the structure-catalysis relationship. Among a variety of characterization techniques, multi-wavelength Raman spectroscopy, combining resonance Raman and non-resonance Raman with different excitation wavelengths, has recently emerged as a particularly powerful tool in not only identifying but also quantifying the structure of supported metal oxide clusters. In this review, we make use of two supported vanadia systems, VOx/SiO2 and VOx/CeO2, as examples to showcase how one can employ this technique to investigate the heterogeneous structure of active oxide clusters and to understand the complex interaction between the oxide clusters and the support. The qualitative and quantitative structural information gained from the multi-wavelength Raman spectroscopy can be utilized to provide fundamental insights for designing more efficient supported metal oxide catalysts.

Key words: Multi-wavelength, Raman spectroscopy, Resonance Raman, Vanadia, Silica, Ceria