高等学校化学学报 ›› 2018, Vol. 39 ›› Issue (3): 416-421.doi: 10.7503/cjcu20170497

• 研究论文: 无机化学 • 上一篇    下一篇

缺陷调控对钙钛矿结构锰酸镧催化性质的影响

蒋一兰, 袁龙, 王西阳, 黄科科(), 冯守华   

  1. 吉林大学化学学院, 无机合成与制备化学国家重点实验室, 长春 130012
  • 收稿日期:2017-07-21 出版日期:2018-03-10 发布日期:2018-01-23
  • 作者简介:联系人简介: 黄科科, 男, 博士, 副教授, 主要从事无机固体化学研究. E-mail:kkhuang@jlu.edu.cn
  • 基金资助:
    国家自然科学基金(批准号: 21427802, 21671076, 21621001)资助

Effect of Defect Tuning on the Catalytic Behavior of Perovskite Structure Lanthanum Manganite

JIANG Yilan, YUAN Long, WANG Xiyang, HUANG Keke*(), FENG Shouhua   

  1. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China
  • Received:2017-07-21 Online:2018-03-10 Published:2018-01-23
  • Contact: HUANG Keke E-mail:kkhuang@jlu.edu.cn
  • Supported by:
    † Supported by the National Natural Science Foundation of China(Nos.21427802, 21671076, 21621001)

摘要:

以钙钛矿结构锰酸镧为模型化合物, 通过制造A位缺陷调控LaxMnO3-δ中Mn的价态和氧缺陷, 并通过电催化析氧(OER)及热催化CO氧化等反应对缺陷与催化性质的关系进行评价. 所有样品均采用溶胶-凝胶法合成, 并通过ICP-OES分析确定A位缺陷, 再经过碘量法滴定确定Mn的价态, 根据电中性原则, 计算出氧缺陷(δ)值, 调控所得样品的化学式分别为La0.85MnO2.85, La0.80MnO2.81和La0.75MnO2.74. 分别利用X射线衍射仪(XRD)、 X射线光电子能谱仪(XPS)和扫描电子显微镜(SEM)等对样品的结构、 Mn结合能和形貌进行了表征, 并利用物理吸附仪测得样品的比表面积. 材料的电催化析氧和CO催化氧化性能测试结果表明, 氧缺陷对2种催化反应均表现了很大的影响, 氧缺陷的浓度与OER催化活性呈线性关系, 而对于CO催化, 则需要合适的氧缺陷浓度.

关键词: 氧缺陷, 锰酸镧, 电催化析氧反应, 一氧化碳催化氧化

Abstract:

In this paper, lanthanum manganite with perovskite structure was chosen as a model compound of which the valence of Mn and oxygen defects were tuned by introducing A-site defect. Electrochemical catalytic oxygen evolution reaction(OER) and catalytic oxidation of CO were performed to evaluate the relationship between the defects and catalytic properties. All the samples were prepared via a sol-gel method, and the composition was determined by ICP-OES. The valence of Mn was titrated by iodometric method. The oxygen defect(δ) was calculated according to the principle of neutrality. The chemical formulas of the samples were La0.85MnO2.85, La0.80MnO2.81 and La0.75MnO2.74, respectively. The structure, binding energy of Mn and morphology of the samples were characterized by X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS) and scanning electron microscopy(SEM). The specific surface area of the samples was determined by physical adsorption. The OER results indicated a linear relationship between the concentration of defect and OER property, while the La0.80MnO2.81 sample showed the best CO catalytic property.

Key words: Oxygen defect, lanthanum manganite, Oxygen evolution reaction(OER), Catalytic oxidation of CO

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