立方Nd2O3上过氧物种光诱导生成的18O同位素示踪考察

doi:10.1016/S1872-2067(14)60153-4

催化学报 ›› 2014, Vol. 35 ›› Issue (8): 1385-1393.DOI: 10.1016/S1872-2067(14)60153-4

立方Nd₂O₃上过氧物种光诱导生成的¹⁸O同位素示踪考察

景孝廉, 佘雯瑜, 翁维正, 李建梅, 夏文生, 万惠霖

厦门大学化学化工学院化学系, 固体表面物理化学国家重点实验室, 醇醚酯化工清洁生产国家工程实验室, 福建厦门 361005

收稿日期:2014-03-28 修回日期:2014-05-14 出版日期:2014-08-01 发布日期:2014-08-05
通讯作者: 翁维正, 万惠霖
基金资助:
国家重点基础研究发展计划（973计划，2010CB732303）；国家自然科学基金（21173173，21033006，21373169）；教育部创新团队项目（IRT1036）.

¹⁸O isotopic study of photo-induced formation of peroxide species on cubic Nd₂O₃

Xiaolian Jing, Wenyu She, Weizheng Weng, Jianmei Li, Wensheng Xia, Huilin Wan

State Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China

Received:2014-03-28 Revised:2014-05-14 Online:2014-08-01 Published:2014-08-05
Supported by:
This work was supported by the National Basic Research Program of China (973 Program, 2010CB732303), the National Natural Science Foundation of China (21173173, 21033006, 21373169), and the Program for Changjiang Scholars and Innovative Research Team in University (IRT1036).

摘要/Abstract

摘要：

采用原位显微Raman光谱和¹⁸O同位素示踪技术，以325 nm激光为激发光源，对立方Nd₂O₃上过氧物种的光诱导生成过程进行了详细表征，进一步证实过氧源于分子氧对晶格氧的氧化反应. 结果还表明，325 nm激光在室温下即可诱导过氧的生成，在实验条件下，生成的过氧物种可与Nd₂O₃的晶格氧发生快速的氧交换反应，位于Nd₂O₃体相的晶格氧也可迁移至样品表层进而参与过氧的生成. 325 nm激光照射有助于促进晶格氧的迁移以及晶格氧与分子氧之间的氧交换反应.

关键词: 分子氧活化, 过氧, 倍半氧化钕, 光诱导反应, ¹⁸O同位素研究, Raman光谱

Abstract:

Photo-induced formation of peroxide species on cubic Nd₂O₃ was studied by in situ microprobe Raman spectroscopy using ¹⁸O as a tracer and a 325-nm laser as an excitation source. The results confirmed that the peroxide ions were formed through photooxidation of the lattice oxygen species in neodymium sesquioxide by molecular oxygen species. Under UV excitation (λ = 325 nm), the reaction between O₂ and O^2- could take place at room temperature. A fast oxygen exchange between the peroxide ions and the lattice oxygen species in Nd₂O₃ took place under the experimental conditions studied. Also, bulk lattice oxygen species in Nd₂O₃ could migrate to the surface layer and participate in the formation of peroxide ions. The migration of lattice oxygen species and the oxygen exchange between lattice oxygen and peroxide ions were promoted by UV laser irradiation.

Key words: Oxygen activation, Peroxide, Neodymium sesquioxide, Photo-induced reaction, ¹⁸O isotopic study, Raman spectroscopy

景孝廉, 佘雯瑜, 翁维正, 李建梅, 夏文生, 万惠霖. 立方Nd₂O₃上过氧物种光诱导生成的¹⁸O同位素示踪考察[J]. 催化学报, 2014, 35(8): 1385-1393.

Xiaolian Jing, Wenyu She, Weizheng Weng, Jianmei Li, Wensheng Xia, Huilin Wan. ¹⁸O isotopic study of photo-induced formation of peroxide species on cubic Nd₂O₃[J]. Chinese Journal of Catalysis, 2014, 35(8): 1385-1393.

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立方Nd₂O₃上过氧物种光诱导生成的¹⁸O同位素示踪考察

¹⁸O isotopic study of photo-induced formation of peroxide species on cubic Nd₂O₃

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