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石墨相氮化碳改性及其光催化性能研究

發(fā)布時(shí)間:2018-08-07 19:37
【摘要】:近年來,氮化碳由于價(jià)格低廉、環(huán)境友好、合成簡(jiǎn)單和性質(zhì)穩(wěn)定等原因,成為了金屬材料的良好替代品而引起廣泛關(guān)注。尤其是石墨相氮化碳,在能源利用方面表現(xiàn)出良好的性質(zhì),比如光催化降解有機(jī)污染物、光電池和光電解應(yīng)用。盡管石墨相氮化碳作為光催化劑已趨于成熟,但其電子設(shè)備的利用率仍然處于初期階段。因此,本文通過將g-C_3N_4質(zhì)子化改善其溶解性,再通過負(fù)載、接枝共軛配體來提高其光催化性能。(1)通過熱分解雙氰胺制備g-C_3N_4,將g-C_3N_4在濃硫酸下剝層實(shí)現(xiàn)質(zhì)子化,得到p-g-C_3N_4。通過XRD和BET對(duì)其進(jìn)行表征及性質(zhì)研究。結(jié)果顯示,剝層前后的g-C_3N_4結(jié)構(gòu)沒有發(fā)生變化,但由于類石墨層的分離,比表面積由原來的7.14 m~2·g~(-1)增加到17.64m~2·g~(-1)。同時(shí),g-C_3N_4質(zhì)子化后的溶解性能也發(fā)生了變化,其可以溶解在DMSO和乙二醇中,且隨著溶液溫度的升高溶解度增大;(2)以三聚氯氰為橋聯(lián)劑,將p-g-C_3N_4負(fù)載到纖維素包裹的Fe_3O_4磁性微球上,制備得到了p-g-C_3N_4/Fe_3O_4催化劑。通過XRD、IR、VSM、TG等對(duì)其進(jìn)行一系列表征及性質(zhì)研究。結(jié)果顯示p-g-C_3N_4/Fe_3O_4具有超順磁性,可通過外加磁場(chǎng)快速回收。并通過在紫外光下對(duì)甲基紅的降解效果來研究其催化性能。結(jié)果表明,p-g-C_3N_4/Fe_3O_4在90min后甲基紅的降解率達(dá)到84.26%;(3)以Fe~(3+)為中心離子,咪唑和p-g-C_3N_4為配位體,通過機(jī)械研磨的方式制備得到類似于夾心面包的p-g-C_3N_4/Fe_2(SO_4)_3/C_3H_4N_2催化劑。通過XRD、IR、TG等對(duì)其進(jìn)行一系列表征及性質(zhì)研究。并通過在紫外光下對(duì)甲基紅的降解效果來研究其催化性能。結(jié)果表明,p-g-C_3N_4/Fe_2(SO_4)_3/C_3H_4N_2在90 min后甲基紅的降解率達(dá)到98.1%.
[Abstract]:In recent years, carbon nitride has become a good substitute for metal materials because of its low price, environmental friendliness, simple synthesis and stable properties. Especially, graphite phase carbon nitride shows good properties in energy utilization, such as photocatalytic degradation of organic pollutants, photocell and photoelectrolysis. Although graphite phase carbon nitride has become mature as photocatalyst, the utilization rate of its electronic equipment is still in its initial stage. In this paper, the solubility of g-C_3N_4 was improved by protonation, and its photocatalytic activity was improved by grafting conjugated ligand. (1) g-C3N _ 4 was prepared by thermal decomposition of dicyandiamide, and g-C_3N_4 was protonated under concentrated sulfuric acid to obtain p-g-C _ 3N _ 4. Their characterization and properties were studied by XRD and BET. The results show that the structure of g-C_3N_4 does not change before and after stripping, but due to the separation of graphite-like layer, the specific surface area increases from 7.14 mg-1 to 17.64m~2 g-1. At the same time, the solubility of tit _ g-C _ 3N _ 4 after protonation also changed, which could be dissolved in DMSO and ethylene glycol, and the solubility increased with the increase of solution temperature. (2) p-g-C_3N_4 was loaded on the Fe_3O_4 magnetic microspheres wrapped in cellulose with cyanuric chloride as bridging agent. P-g-C_3N_4/Fe_3O_4 catalyst was prepared. A series of characterization and properties were carried out by XRDX IR VSMTG and so on. The results show that p-g-C_3N_4/Fe_3O_4 is superparamagnetic and can be recovered quickly by external magnetic field. The catalytic activity of methyl red was studied by the degradation of methyl red under ultraviolet light. The results showed that the degradation rate of methyl-red reached 84.26 after 90min; (3) the p-g-C_3N_4/Fe_2 (SO_4) 3 / C3H4N2 catalyst similar to sandwich bread was prepared by mechanical grinding with Fe3 as the central ion and imidazole and p-g-C_3N_4 as the ligand. A series of characterization and properties were carried out by means of XRD IR TG and so on. The catalytic activity of methyl red was studied by the degradation of methyl red under ultraviolet light. The results showed that the degradation rate of methyl-red reached 98.1 after 90 min.
【學(xué)位授予單位】:天津理工大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2017
【分類號(hào)】:O643.36

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