物理化学学报 >> 2017, Vol. 33 >> Issue (9): 1884-1890.doi: 10.3866/PKU.WHXB201705084

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无模板法水热合成CoTe及其可见光光催化还原CO2性能

周亮1,2,张雪华2,林琳2,3,李盼2,3,邵坤娟2,3,李春忠1,*(),贺涛2,3,*()   

  1. 1 华东理工大学材料科学与工程学院,上海200237
    2 中国科学院纳米系统与多级次制造重点实验室,中国科学院纳米科学卓越创新中心,国家纳米科学中心,北京100190
    3 中国科学院大学,北京100049
  • 收稿日期:2017-04-05 发布日期:2017-07-05
  • 通讯作者: 李春忠,贺涛 E-mail:czli@ecust.edu.cn;het@nanoctr.cn
  • 基金资助:
    科学技术部国家国际科技合作专项项目(2015DFG62610);国家自然科学基金(21673052)

Visible-Light Photocatalytic Reduction of CO2 by CoTe Prepared via a Template-Free Hydrothermal Method

Liang ZHOU1,2,Xue-Hua ZHANG2,Lin LIN2,3,Pan LI2,3,Kun-Juan SHAO2,3,Chun-Zhong LI1,*(),Tao HE2,3,*()   

  1. 1 School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, P. R. China
    2 CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, P. R. China
    3 University of Chinese Academy of Sciences, Beijing 100049, P. R. China
  • Received:2017-04-05 Published:2017-07-05
  • Contact: Chun-Zhong LI,Tao HE E-mail:czli@ecust.edu.cn;het@nanoctr.cn
  • Supported by:
    the National Special Project of International Cooperation in Science and Technology, Ministry of Science and Technology of China(2015DFG62610);National Natural Science Foundation of China(21673052)

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摘要：

本文利用无模版水热法合成了碲化钴（CoTe）纳米催化剂。为了避免引入残炭，所有的反应物均为无机化合物。利用X射线衍射（XRD）、扫描电子显微镜（SEM）、紫外-可见（UV-Vis）吸收光谱和X射线光电子能谱（XPS）等技术对所制备的CoTe纳米材料进行了表征。结果表明，所得产物为具有六方结构的海绵状CoTe，且具有可见光（λ > 420 nm）光催化活性。当以N, N-二甲基乙酰胺（DMA）或纯水为溶剂时，二氧化碳（CO2）均可被光催化还原为甲烷（CH4），但产率较低。而在催化体系中加入牺牲剂三乙醇胺（TEOA）后，产物由CH4变为一氧化碳（CO）。这些实验结果表明，溶剂和牺牲剂的引入均可影响CoTe纳米催化剂对CO2的光催化还原性能。

关键词: CoTe, CO2, 光催化还原, 有机溶剂, 牺牲剂

Abstract:

A CoTenanocatalyst has been successfully synthesized via a template-free hydrothermal method. Inorganic reactants were used so as not to introduce carbon residue contamination. The as-prepared sample was characterized by many techniques, including X-ray diffraction, scanning electron microscopy, ultraviolet-visible light absorption spectroscopy, and X-ray photoelectron spectroscopy. The obtained sample was found to be sponge-like CoTe with a hexagonal structure, which exhibited visible-light (λ > 420 nm) photocatalytic activity. Photoreduction of CO2 over CoTe is believed to have undergone via the carbene pathway. The CO2 was photocatalytically reduced into CH4 with a low yield when N, N-dimethylacetamide (DMA) or water was used as the solvent. When the sacrificial agent triethanolamine (TEOA) was introduced into the photocatalytic system, however, the product was CO instead. These results indicated that both the solvent and sacrificial agent can influence the photoreduction of CO2 over the CoTenanocatalyst. Usually, the solubility of CO2 in an organic solvent such as DMA is higher than that in the pure water, leading to a larger product yield. The presence of TEOA may change the adsorption characteristics of CO onto the surface of the CoTe catalyst, as well as enhance the separation efficiency of photogenerated charge carriers, resulting in a change in the activity and selectivity of CO2 photoreduction.

Key words: CoTe, CO2, Photocatalytic reduction, Organic solvent, Sacrificial agent