基于罗丹明6G席夫碱非贵金属配合物的合成、结构和可见光催化产氢性质研究
发布时间:2018-04-28 03:45
本文选题:罗丹明6G + Schiff碱 ; 参考:《郑州大学》2015年硕士论文
【摘要】:伴随着工业和经济的发展,全球面临着一个重要问题:能源缺失。开发新的可循环利用的清洁能源迫在眉睫,将太阳能转化为化学能并有效的储存起来有着广阔的研究前景。氢能源是公认的清洁能源,作为低碳和零碳能源正在脱颖而出。氢气具有高热值,且燃烧后无污染的优点,被认为终将取代化石燃料而成为未来新能源。全球的科学家们正在努力解决降低产氢成本和实现产氢工业化的问题。利用太阳光催化分解水产氢是一个重要的研究方向,关键在于找到一种合适的催化剂。因此,制备出廉价而且高效的催化剂是多年来化学工作者们从事光催化制氢研究需要解决的一个重要问题。在本论文中,我们设计并且合成了两种基于罗丹明6G的Schiff碱类配体L1、L2,之后利用溶剂热的方法得到了一系列基于非贵金属(钴、铜、镉、铝)的有机金属配合物:[Co(L1)2Cl]?DMF(1)、[Co3(L1)2]?DMF(2)、[Co12(L1)6(OH)6(Ac)6]?2DMF?8H2O(3)、[Cu(L2)]?H2O}n(4)、[Co(L2)2]?2H2O(5)、{[Cd(L2)(DMF)(H2O)]?2H2O}n(6)、[Al(L2)2]?Cl?2H2O(7),并通过X-射线单晶衍射分析、元素分析、X-射线粉末衍射、红外、热分析等测试手段对该系列配合物的结构和性能进行了表征。我们主要研究了配合物[Co3(L1)2]?DMF(2)和配合物{Cu(Ⅱ)L2}n(4)在可见光条件下分解水产氢中的催化性能。以配合物{Co3(L1)2?DMF}(2)作为催化剂,曙红Y(EY2-)作为光敏剂,三乙胺(TEA)为电子给体(牺牲剂)构建了三组分非均相光催化产氢体系。并且成功实现了可见光催化水分解制氢,同时对构建的产氢体系进行了一系列产氢条件优化实验,最大产氢量达到6983μmol/g,体系的产氢寿命达到3个小时。用配合物{Cu(Ⅱ)L2}n(4)作为体系的光催化剂,曙红Y作光敏剂,三乙醇胺(TEOA)作为电子给体构建三组分产氢体系,是首次用金属铜配合物作光催化产氢体系的催化剂,实现了光催化分解水产氢,通过对产氢条件的优化,经过5小时光照后,最大产氢量达到197.37μmol,通过一系列实验证明了铜配合物催化剂的稳定性。
[Abstract]:With the development of industry and economy, the world is facing an important problem: energy shortage. It is urgent to develop new clean energy which can be recycled. It has a broad research prospect to convert solar energy into chemical energy and store it effectively. Hydrogen energy is recognized as a clean energy, as low-carbon and zero-carbon energy is emerging. Hydrogen has the advantages of high calorific value and no pollution after combustion. It is considered that hydrogen will eventually replace fossil fuels as a new energy source in the future. Scientists around the world are trying to reduce the cost of hydrogen production and industrialize it. Catalytic decomposition of aquatic hydrogen by solar light is an important research direction, the key is to find a suitable catalyst. Therefore, the preparation of cheap and efficient catalysts has been an important problem for many years in the research of photocatalytic hydrogen production. In this thesis, we have designed and synthesized two Schiff base ligands based on Rhodamine 6G, and then obtained a series of non-precious metals (cobalt, copper, cadmium) by solvothermal method. 閾,
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