钴基水氧化催化剂的制备和性能研究

发布时间：2018-02-24 13:49

本文关键词： 光催化水氧化非贵金属钴催化性能稳定性　出处：《新疆大学》2017年硕士论文　论文类型：学位论文

【摘要】：氢气作为一种可再生、燃烧值高的清洁能源,燃烧产物仅有水。模拟自然界光合作用实现水的分解产生氢气是最理想的能源转换途径。水分解包括两个半反应:水氧化和水还原,并且水氧化半反应更难以进行。所以水氧化是一直是制约水高效全分解的瓶颈。因此设计合成高效且稳定的水氧化催化剂是突破此瓶颈问题的关键。本文以三种钴基水氧化催化剂为研究对象,系统的研究了所制备催化剂的水氧化催化性能和稳定性,进一步拓展了钴基水氧化催化剂范围,为开发高效稳定的水氧化催化剂提供了有价值的参考。1、通过简单的一锅法水-甲苯两相界面反应方法合成了四种不同形貌的核壳结构Co@CoO催化剂,并且进一步研究了不同缓冲溶液体系、缓冲溶液pH、光敏剂种类以及催化剂用量对水氧化反应催化活性的影响。结合多种技术手段包括催化剂老化实验、DLS、LC-MS、XRD和XPS等测试对催化剂的水氧化稳定性进行了充分的考察。结果表明在Na_2S_2O_8/可见光/[Ru(bpy)3]2+光催化水氧化体系中,1表现出优异的催化性能和良好的稳定性。此研究对于设计核壳结构催化剂水氧化催化剂具有很好的指导作用。2、合成并表征了Co-MOF-74,考察了其催化水氧化活性。并且进一步研究了不同缓冲溶液体系、缓冲溶液pH、光敏剂种类以及催化剂用量对水氧化反应催化活性的影响。通过XRD、XPS和催化剂老化实验等测试对Co-MOF-74催化水氧化稳定性进行了充分的考察。结果表明,Co-MOF-74在水氧化条件下具有高度稳定性。此工作对于设计和合成MOFs类水氧化催化剂具有指导作用。3、制备了钴基多金属氧酸盐Na_7H_(10)[Co_6(H_2O)_2(PW_9O_(34))_2(PW_6O_(26))]·30H_2O,并将该催化剂应用于可见光驱动催化水氧化反应。并且进一步研究了不同缓冲溶液体系、缓冲溶液pH、光敏剂种类以及催化剂浓度对水氧化反应催化活性的影响。采用DLS、FT-IR、萃取实验结合AAS等实验等对催化剂的水氧化稳定性进行了深入研究。多种表征结果表明制备的催化剂在该反应体系中是高度稳定的。
[Abstract]:Hydrogen as a renewable, high-burning clean energy, Combustion products have only water. Simulating natural photosynthesis to decompose water to produce hydrogen is the ideal energy conversion approach. Water decomposition consists of two half-reactions: water oxidation and water reduction. Therefore, water oxidation is always the bottleneck restricting the total decomposition of water. Therefore, the design and synthesis of efficient and stable catalyst for water oxidation is the key to break through this bottleneck. Cobalt based water oxidation catalyst was studied. The catalytic performance and stability of the prepared catalysts for water oxidation have been systematically studied, and the range of cobalt based water oxidation catalysts has been further expanded. This paper provides a valuable reference for the development of high efficient and stable water oxidation catalyst. Four core-shell structure Co@CoO catalysts with different morphologies were synthesized by a simple one-pot water-toluene two-phase interfacial reaction. And further studied the different buffer solution system, The effects of pH of buffer solution, the type of Guang Min and the amount of catalyst on the catalytic activity of water oxidation reaction were studied. The stability of water oxidation of the catalyst was fully tested by various technical means, including catalyst aging test (DLSX) LC-MS XRD and XPS. The results show that Na-1 exhibits excellent catalytic performance and good stability in the water oxidation system of S _ 2S _ 2O _ 8 / visible-light / [Ru(bpy)3] _ 2 photocatalytic oxidation system. This study is useful for the design of core-shell structure catalysts for water oxidation. Co-MOF-74 was synthesized and characterized by .2.The catalytic water oxidation activity of Co-MOF-74 was investigated. The effects of pH of buffer solution, the type of Guang Min and the amount of catalyst on the catalytic activity of water oxidation reaction were studied. The stability of Co-MOF-74 catalytic water oxidation was investigated by XRDX XPS and catalyst aging experiments. This work has a high degree of stability under the condition of water oxidation. This work has a guiding effect on the design and synthesis of MOFs type water oxidation catalysts. 3. The preparation of Cobalt based polyoxometalates Na7HPO4 10). Reaction. And further study of different buffer solution system, The effects of pH of buffer solution, the type of Guang Min and the concentration of catalyst on the catalytic activity of water oxidation reaction were studied. The stability of water oxidation of the catalyst was studied by DLS- FT-IRR, extraction experiment and AAS. It is shown that the prepared catalyst is highly stable in the reaction system.
【学位授予单位】：新疆大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O643.36;TQ116.2

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