本文關(guān)鍵詞：具有電或光催化水分解性能的鈷、鐵和銅配合物的設(shè)計、合成與研究　出處：《華南理工大學(xué)》2016年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 配合物 分子催化劑 水還原和氧化 電催化和光催化產(chǎn)氫

【摘要】：21世紀(jì),是信息的時代,也是技術(shù)的時代。伴隨著科技的飛速發(fā)展,能源的需求量也是愈來愈大,但是全球的儲備量卻日漸減少,開發(fā)并利用新的能源成為當(dāng)下的難題。氫能成為21世紀(jì)最理想的能源。水的裂解是由水的氧化和還原兩部分構(gòu)成,需要113.38 kcal/mol(4.92 eV)的自由能。所以從熱力學(xué)的角度說,水是一個相對穩(wěn)定的分子。電解水可以得到純凈的氫氣和氧氣,但是得消耗一部分電能。所以我們試圖從化學(xué)角度上來降低電能的消耗,一個化學(xué)反應(yīng)加入合適的催化劑可以降低反應(yīng)所需的活化能。同理,尋找一種高效的催化劑,也可以減少電解水反應(yīng)所需要的電能。我們知道,微生物可以通過光合作用,在氫化酶的作用下,催化裂解水生成氫氣。雖然光合作用的生物環(huán)境是無法模擬的,但是這種現(xiàn)象使得科學(xué)家們對分子催化劑的研究有了更深層的思考:能否通過光催化的方法制取氫氣,這樣就可以減少電能的消耗。本研究旨在所以通過設(shè)計新型配體和不同類型過渡金屬配合物,以尋找新的水裂解催化劑。本論文包括:1)三種有機(jī)配體的合成:1-[(2-甲氧基)苯]-3-[(2-苯并噻唑)苯]三氮烯(HLa)、(N,N-二甲基)乙二胺-N,N-二(2-叔丁基-4-甲基苯酚)(H2Lb)、(2-氨甲基吡啶)-N-(2-亞甲基-4-乙基-6-叔丁基苯酚),N-(2-亞甲基-4-甲基-6-叔丁基苯酚)(H2Lc)。2)五種新型分子催化劑配合物[Co2(La)4]1、配合物[LbCoCl]2、配合物[LbCo(H2O)]3、配合物[LcFeCl]4、配合物[CuMe2(oxpn)Cu(OH)2]5的制備、結(jié)構(gòu)和光譜。3)一種新型配合物的電催化制氫和制氧性能研究:配合物[CuMe2(oxpn)Cu(OH)2]5同時具有水還原和水氧化的性能,水還原的TOF為654 h-1(pH 7.0),水氧化的TOF為2.56 s-1(pH 10.4)。4)兩種新型配合物的電催化和光催化性能研究:配合物[Co2(La)4]1、配合物[LbCoCl]2同時具有電催化和光催化制氫的性能,電解制氫的TOF依次為為223 h-1(pH 7.0)、162h-1(pH 7.0),光催化制氫的TON為4360、4125。5)催化機(jī)理的初步研究。
[Abstract]:Twenty-first Century is the era of information technology, but also the era. With the rapid development of science and technology, the demand of energy is increasing, but the global reserves are gradually reducing, the development and use of new energy has become the current problems. Hydrogen has become the ideal twenty-first Century energy. Water is cracking by oxidation of water and the reduction of two parts, 113.38 kcal/mol (4.92 eV) of the free energy. So from the point of view of thermodynamics, water is a relatively stable molecule. The electrolysis of water can be pure hydrogen and oxygen, but a part of the electric power consumption. So we try to reduce the consumption of electrical energy from chemical angle a chemical reaction, adding suitable catalyst can lower the activation energy required for the reaction. In the same way, looking for a highly efficient catalyst, can also reduce the water electrolysis reaction power. As we know, by microorganisms Photosynthesis, in the role of the hydrogenase, hydrogen generation catalytic pyrolysis of water. Although the photosynthesis biological environment can not be simulated, but this phenomenon allows scientists to study the molecular catalysts have deeper thinking: whether through the method of photocatalytic preparation of hydrogen gas, which can reduce the power consumption in this research. So to through the design of new ligands and transition metal complexes of different types, in order to find new water cracking catalyst. This thesis includes: 1) the synthesis of three kinds of organic ligands: 1-[(2- methoxy benzene]-3-[(2-) benzothiazoles) phenyl] three azene (HLa), (N, N- two methyl) Ethylenediamine -N (2-, N- two -4- methyl phenol tert Ding Ji (H2Lb) (2-), -N- (aminomethyl pyridine) 2- methylene -4- ethyl -6- TERT phenol, N- (Ding Ji) 2- methylene -4- methyl -6- tert Ding Ji phenol) (H2Lc).2) five new molecular catalyst complexes [Co2 (La 4]1) [LbC complexes OCl]2, [LbCo (H2O)]3 complexes, [LcFeCl]4 complexes, complexes of [CuMe2 (oxpn) Cu (OH) 2]5 preparation, structure and spectral.3) on Electrocatalytic hydrogen and oxygen production performance of a new type of complexes: complexes of [CuMe2 (oxpn) Cu (OH) 2]5 with water and reduction water oxidation performance, water reduction of TOF 654 H-1 (pH 7), water oxidation of TOF was 2.56 S-1 (pH 10.4).4) electro catalytic and photocatalytic properties of two new complexes: complexes of [Co2 (La) 4]1, and has performance of electro catalytic and photocatalytic hydrogen production [LbCoCl]2 with the electrolytic hydrogen production of TOF were followed by 223 H-1 (pH 7), 162h-1 (pH 7), photocatalytic TON 43604125.5) preliminary study on catalytic mechanism.

【學(xué)位授予單位】：華南理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2016
【分類號】：O641.4

【相似文獻(xiàn)】

相關(guān)期刊論文 前10條

1 周明華,吳祖成,汪大，

本文編號：1359385