發(fā)布時(shí)間：2018-04-28 21:02

  本文選題：人工光合作用 + 光敏劑��； 參考：《大連理工大學(xué)》2015年碩士論文

【摘要】：隨著社會(huì)的不斷發(fā)展,煤、石油等能源的消耗逐年增加。傳統(tǒng)化石能源的日益枯竭和環(huán)境污染的日益嚴(yán)重,使得人類不得不尋求更加清潔的可持續(xù)能源。自然光系統(tǒng)II能通過分解水將太陽能轉(zhuǎn)化為化學(xué)能儲(chǔ)存起來,因此人工模擬光合作用是解決能源危機(jī)的有效方法。其中光解水制氫被認(rèn)為是一條非常具有前景的途徑,而光解水制氫過程中的關(guān)鍵步驟是光解水產(chǎn)生氧氣和質(zhì)子。光驅(qū)動(dòng)水氧化反應(yīng)體系中存在的技術(shù)難題是如何設(shè)計(jì)和合成具有較長激發(fā)態(tài)壽命、較好的電荷分離態(tài)、較高氧化電位的光敏劑,從而構(gòu)建高效的光驅(qū)動(dòng)水氧化反應(yīng)體系。本論文針對(duì)上述科學(xué)難題,嘗試做了兩部分工作。通過對(duì)[Ru(bpy)3]2+母體進(jìn)行修飾,設(shè)計(jì)合成了基于四吡啶吩嗪配體的單核釕光敏劑[RuⅡ(bpy)2(tpphz)](PF6)2(PS1)和雙核釕光敏劑[RuⅡ(bpy)2(tpphz) RuⅡ(bpy)2] (PF6)4(PS2)(bpy=2,2’-聯(lián)吡啶,tpphz=四吡啶吩嗪)。在含10%乙腈的pH=6.8的磷酸緩沖溶液中,以PS 1或PS 2作為光敏劑,以Ru(bda)(pic)2(Ru 1; H2bda=2,2’-聯(lián)吡啶-6,6’-二羧酸,pic=4-甲基吡啶)作為催化劑,以Na2S2O8作為電子受體組成三組分體系。研究結(jié)果表明,以PS 1為光敏劑時(shí)三組分體系的光驅(qū)動(dòng)水氧化反應(yīng)的活性比以PS 2和[RuⅡ(bpy)3] (PF6)2為光敏劑時(shí)體系的光驅(qū)動(dòng)水氧化反應(yīng)的活性都有較為顯著的提高。在光敏劑PS 1的基礎(chǔ)上設(shè)計(jì)合成了超分子催化劑RuⅡ(bpy)2(tpphz)RuⅡL(bpy)(pic)] (PF6)4 (SM; L=2,6-吡啶二甲酸)。研究結(jié)果表明,在相同條件下,含有超分子催化劑SM的超分子體系的光驅(qū)動(dòng)催化水氧化反應(yīng)的活性是三組分體系的兩倍,其原因可能是超分子體系有利于電子在光敏劑和催化劑之間的傳遞。
[Abstract]:With the continuous development of society, the consumption of coal, petroleum and other energy sources is increasing year by year. With the depletion of traditional fossil energy and the increasingly serious environmental pollution, human beings have to seek cleaner and more sustainable energy. Natural light system II can convert solar energy into chemical energy by decomposing water, so artificial simulation of photosynthesis is an effective method to solve energy crisis. The photolysis of water to produce hydrogen is considered to be a promising approach, and the key step in the process of photolysis is the production of oxygen and protons by photolysis of water. The technical problem in dynamic water oxidation reaction system of optical drive is how to design and synthesize Guang Min agent with long excited state life, better charge separation state and higher oxidation potential, so as to construct an efficient photo-driven water oxidation reaction system. In view of the above scientific problems, this paper tries to do two parts of the work. Based on the modification of [Ru(bpy)3] 2 matrix, the mononuclear ruthenium Guang Min (Ru 鈪，

本文編號(hào)：1816849