基于Keggin型多酸化合物的光催化产氢性质研究

发布时间：2018-11-04 08:49

【摘要】：在过去的几十年里,煤和石油产品这样的用来满足世界能源需求的典型能源被几乎耗尽。基于能源危机和环保的需求,替代燃料和可再生燃料的产出在世界范围内迅速的增长。氢能源是其中的典型能源发展趋势,氢气的制备及其储存被广泛的研究。太阳光和水是地球上最充足的,清洁的,可再生的自然资源。从太阳能到氢能的转移可以被描述为一种理想的减少化石燃料使用的解决方案。多酸作为一系列结构多样的金属氧簇,具有丰富的氧表面和一般阴离子所不具备的高的负电荷,并且具备能够容纳多个电子和可逆的氧化还原的性质,已被报道在电催化和光催化产氢方面具有优异的表现。本文主要由两部分组成,第一章总结了多酸化合物作为光催化分解水产氢催化剂的研究进展以及发展前景。第二章概括了自己在多酸光催化分解水方面所做的工作。作为被最广泛研究的多酸,Keggin型多酸已经被报道在近可见和紫外区具有光活性。为了对三个不同中心的Keggin型多酸的光催化分解水性质的研究,能够为调控电子结构,发现更加可行的(催化效率,选择性,稳定性)发现多酸水还原催化剂提供理论基础。我们设计合成了三个具有不同中心原子的无机有机杂化的Keggin型多酸,(HTEA)_2{[Na(TEA)_2]H[Si W_12O_40]}?5H_2O(1),(HTEA)_2{[Na(TEA)_2][PW_12O_40]}?4H_2O(2)and(HTEA)_2{[Na(TEA)_2]H[Ge W_12O_40]}?4H_2O(3)。并对三个化合物进行了表征,三个化合物展现出一维链状结构。另外我们对比了三个化合物及其相应的Keggin多酸的光催化还原水产氢性质。
[Abstract]:In the past few decades, typical sources of energy such as coal and petroleum products to meet the world's energy needs have been almost depleted. Because of the energy crisis and environmental demand, the output of alternative and renewable fuels is growing rapidly around the world. Hydrogen energy is a typical energy development trend, the preparation and storage of hydrogen have been widely studied. Sunlight and water are the most abundant, clean and renewable natural resources on earth. The transfer of solar energy to hydrogen energy can be described as an ideal solution to reduce fossil fuel use. Polyacids, as a series of metal oxygen clusters with various structures, have rich oxygen surfaces and high negative charges which are not possessed by general anions, and have the properties of accommodating multiple electrons and reversible redox. Excellent performance in electrocatalysis and photocatalytic hydrogen production has been reported. This paper consists of two parts. In the first chapter, the research progress and development prospect of polyacid compounds as photocatalytic catalysts for the decomposition of aquatic hydrogen are summarized. In the second chapter, we summarize our work in the photocatalytic decomposition of water. As the most widely studied polyacids, Keggin polyacids have been reported to have photoactivity in near visible and ultraviolet regions. In order to study the photocatalytic decomposition properties of Keggin polyacids with three different centers, it can provide a theoretical basis for regulating the electronic structure and finding more feasible (catalytic efficiency, selectivity, stability) for the discovery of polyacid water reduction catalysts. We have designed and synthesized three inorganic organic hybrid, (HTEA) _ 2 {[Na (TEA) _ 2] H [Si W_12O_40]}? 5H_2O (1) with different central atoms. (HTEA) _ 2 {[Na (TEA) _ 2] [PW_12O_40]}? 4H_2O (2) and (HTEA) _ 2 {[Na (TEA) _ 2] H [Ge W_12O_40]}? 4H_2O (3). Three compounds were characterized and showed one-dimensional chain structure. In addition, the photocatalytic reduction properties of three compounds and their corresponding Keggin polyacids were compared.
【学位授予单位】：东北师范大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：O643.36;TQ116.2

【相似文献】