發(fā)布時(shí)間：2018-05-14 18:50

  本文選題：光催化產(chǎn)氫 + 鈷配合物��； 參考：《鄭州大學(xué)》2015年碩士論文

【摘要】：本文基于非貴金屬鈷,設(shè)計(jì)合成了四個(gè)鈷配合物,并將其作為光催化產(chǎn)氫反應(yīng)中的析氫催化劑,以半導(dǎo)體材料作為主催化劑,以有機(jī)染料作為光敏劑,三乙胺作為電子給體犧牲劑,構(gòu)建了完全不含貴金屬的非均相光催化產(chǎn)氫體系。具體研究內(nèi)容如下:1.以Co Cl2·6H2O、水楊酸和1,10-鄰菲Up琳為起始原料,設(shè)計(jì)并制備了4個(gè)具有析氫活性的分子催化劑,即[Co(phen)2(L)](用Co L1-Co L4表示),并通過元素分析、紅外光譜和核磁共振氫譜(1H NMR)等手段對其進(jìn)行了表征。2.將上述四個(gè)鈷配合物負(fù)載于Ti O2上得到Co L/Ti O2并以其作為催化劑,以有機(jī)氧雜蒽醌類染料作為光敏劑,三乙胺為電子給體構(gòu)建了非均相光催化產(chǎn)氫體系。產(chǎn)氫測定結(jié)果表明,4個(gè)配合物中,Co L2具有最高析氫活性;且在最佳條件下(4μmol EY2-(醇溶),5%(v/v)TEA,p H為11),催化劑2wt%Co L2/Ti O2(50 mg)6h內(nèi)產(chǎn)氫量達(dá)到了91μmol。此外,體系失活的主要原因?yàn)楣饷魟┑慕到夂虲o L從Ti O2表面的脫附。3.將上述四種鈷配合物負(fù)載于g-C3N4表面作為析氫催化劑,類似地,以EY2-(醇溶)作為光敏劑,三乙胺作為電子給體構(gòu)建了產(chǎn)氫體系,并對各析氫條件進(jìn)行了優(yōu)化。結(jié)果表明:Co L3具有最佳析氫活性。在最佳條件下(50 mg催化劑,6μmol EY2-,7.5%(v/v)TEA,p H=11),2wt%Co L3/g-C3N4 2.5h內(nèi)的產(chǎn)氫量達(dá)到72μmol。此外,同樣地,該體系光照2.5h失活的主要原因源自敏化劑的光解和Co L的部分脫附。
[Abstract]:In this paper, four cobalt complexes were designed and synthesized based on non-noble metal cobalt, and they were used as catalysts for hydrogen evolution in photocatalytic hydrogen production reactions. Semiconductor materials were used as main catalysts and organic dyes as Guang Min agents. A heterogeneous photocatalytic hydrogen production system without noble metals was constructed by triethylamine as an electron donor sacrificial agent. The specific contents of the study are as follows: 1. Using Co Cl2 6H _ 2O, salicylic acid and 1-10-phenanthroline as starting materials, four molecular catalysts with hydrogen evolution activity, namely [Cochlein 2L] (expressed by Co L1-Co L4), were designed and prepared by elemental analysis. It was characterized by IR and 1H NMRs. Co L/Ti O 2 was prepared by loading the above four cobalt complexes on TIO 2. The heterogeneous photocatalytic hydrogen production system was constructed using organic oxygen heteranthracene quinone dyes as Guang Min agent and triethylamine as electron donor. The results of hydrogen production showed that L2 had the highest hydrogen evolution activity in the four complexes, and under the optimum conditions, 4 渭 mol EY2-H was obtained, and the hydrogen production of the catalyst 2wt%Co L2/Ti O _ 2O _ (50) mg)6h was 91 渭 mol / h. In addition, the main reasons for the deactivation of the system are the degradation of Guang Min and the desorption of Co L from the surface of TIO 2. 3. The above four cobalt complexes were loaded on the surface of g-C3N4 as catalyst for hydrogen evolution. Similarly, EY2-( alcohol-soluble) was used as Guang Min agent, triethylamine as electron donor to construct the hydrogen production system, and the conditions of hydrogen evolution were optimized. The results show that: (1) Co L _ 3 has the best hydrogen evolution activity. Under the optimum conditions, the hydrogen production of 6 渭 mol EY2-5 / v / v / Similarly, the main reason for the inactivation of the system at 2.5 h is the photolysis of the sensitizer and the partial desorption of Co L.
【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】：O643.36;TQ116.2

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