本文選題：釕配合物 + 染料敏化TiO2�。� 參考：《鄭州大學(xué)》2015年碩士論文

【摘要】：光催化分解水制氫作為一種清潔、可持續(xù)的產(chǎn)氫方法,備受科學(xué)家的關(guān)注。本文構(gòu)建了兩種光分解水催化產(chǎn)氫體系:基于聯(lián)吡啶釕配合物敏化二氧化鈦的非均相光催化產(chǎn)氫體系和基于鈷催化劑的均相光催化產(chǎn)氫體系。合成了兩種聯(lián)吡啶釕類光敏配合物(PS1、PS2),并通過質(zhì)譜、元素分析、紅外、核磁、紫外-可見光譜以及循環(huán)伏安圖譜等進(jìn)行表征。然后,將兩種聯(lián)吡啶釕類光敏配合物敏化到Pt-Ti O2的固體表面得到相應(yīng)的復(fù)合光敏催化劑,以抗壞血酸為電子給體,在純水溶劑里構(gòu)建非均相光催化產(chǎn)氫體系。研究表明,優(yōu)化的反應(yīng)條件下,以20mg PS1敏化的Pt負(fù)載Ti O2作為復(fù)合光敏催化劑,犧牲劑為抗壞血酸(1.0g),反應(yīng)液p H值為5.3,可見光照射5h下,在水體系中獲得了375.8μmol的最大累積產(chǎn)氫量,3h內(nèi)產(chǎn)氫速率為11903.3μmol/g/h。循環(huán)實(shí)驗(yàn)表明復(fù)合光敏催化劑具有較好的穩(wěn)定性,對反應(yīng)體系失活原因的初步研究表明釕配合物光敏染料從Ti O2表面的脫附是主要原因。合成了三種基于鈷的光催化劑(C1、C2、C3),并通過紅外、核磁、單晶衍射、紫外-可見光譜和循環(huán)伏安圖譜等進(jìn)行了表征。以三種鈷配合物為光催化劑,曙紅Y為光敏劑,TEA或TEOA為電子給體,在乙腈/水混合溶劑里構(gòu)建均相產(chǎn)氫體系,并對反應(yīng)條件進(jìn)行了優(yōu)化。研究表明,催化劑C1濃度為2×10-5M,曙紅Y濃度為1×10-4M,TEA體積分?jǐn)?shù)為10%,p H=10.0,乙腈/水(v/v)=1:1,可見光照射3h后,體系相對于催化劑的TON最高,可以達(dá)到352。
[Abstract]:Photocatalytic decomposition of water for hydrogen production as a clean and sustainable method of hydrogen production has attracted the attention of scientists. In this paper, two kinds of photocatalytic hydrogen production systems were constructed: heterogeneous photocatalytic hydrogen production system based on bipyridine ruthenium complex sensitized titanium dioxide and homogeneous photocatalytic hydrogen production system based on cobalt catalyst. Two kinds of bipyridine ruthenium Guang Min complexes were synthesized and characterized by mass spectrometry, elemental analysis, IR, NMR, UV-Vis spectra and cyclic voltammetry. Then, two kinds of bipyridine ruthenium Guang Min complexes were sensitized to the solid surface of Pt-Ti O 2 to obtain the corresponding composite Guang Min catalyst. Using ascorbic acid as the electron donor, the heterogeneous photocatalytic hydrogen production system was constructed in pure water solvent. The results showed that under the optimized reaction conditions, the Pt / TIO _ 2 supported on 20mg PS1 was used as the composite Guang Min catalyst, the sacrificial agent was ascorbic acid (1.0 g), the pH value of the reaction solution was 5.3, and the visible light irradiation was 5 h. The maximum cumulative hydrogen production rate of 375.8 渭 mol is 11903.3 渭 mol / g / h within 3 h. The cycling experiment showed that the composite Guang Min catalyst had good stability, and the primary study on the deactivation of the reaction system showed that the desorption of the ruthenium complex Guang Min dye from the surface of TIO 2 was the main reason. Three kinds of cobalt based photocatalysts were synthesized and characterized by IR, NMR, single crystal diffraction, UV-Vis spectra and cyclic voltammetry. Using three cobalt complexes as photocatalyst, eosin Y as Guang Min agent tea or TEOA as electron donor, homogeneous hydrogen production system was constructed in acetonitrile / water mixed solvent, and the reaction conditions were optimized. The results show that the catalyst C1 concentration is 2 脳 10 ~ (-5) M, eosin Y concentration is 1 脳 10 ~ (-4) M ~ (-1) tea volume fraction is 10 脳 10 ~ (-4) M ~ (-1), acetonitrile / water v / v ~ (-1) 1: 1, and visible light irradiation for 3 h, the TON of the catalyst is the highest, which can reach 352.
【學(xué)位授予單位】：鄭州大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：TQ116.2;O643.36

【參考文獻(xiàn)】

相關(guān)期刊論文 前1條

1 楊朋舉;王劍;趙江紅;朱珍平;;羅丹明B敏化TiO_2可見光分解水產(chǎn)氫研究[J];燃料化學(xué)學(xué)報(bào);2013年06期

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本文編號：1818127