本文關(guān)鍵詞：基于金屬—有機(jī)骨架構(gòu)筑復(fù)合光催化材料及其可見光光催化制氫性能　出處：《安徽大學(xué)》2016年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 光催化材料 金屬有機(jī)骨架材料 染料敏化 UiO-66 g-C_3N_4

【摘要】：能源短缺和環(huán)境污染是困擾人類社會(huì)可持續(xù)發(fā)展的兩大問題,尋找和開發(fā)可再生、無(wú)污染、廉價(jià)易得的新能源是解決上述問題的重要途徑。氫氣具有燃燒值大、產(chǎn)物(H20)無(wú)污染、易儲(chǔ)存運(yùn)輸?shù)葍?yōu)點(diǎn),是驅(qū)動(dòng)人類社會(huì)發(fā)展的最有潛力的清潔能源。水是地球上最為豐富的資源,廉價(jià)易得,具有巨大的利用價(jià)值。直接利用太陽(yáng)能光催化分解水制取氫氣是制備清潔能源的一種重要技術(shù)。在眾多的已知材料中,半導(dǎo)體被廣泛用于光催化反應(yīng)中,很多半導(dǎo)體光催化材料由于帶隙太寬或容易光腐蝕等原因而影響了其光催化活性。因此,研究設(shè)計(jì)高效的光催化材料是光解水制氫技術(shù)發(fā)展的關(guān)鍵。近期,金屬-有機(jī)骨架(metal-organic frameworks, MOFs)材料作為一種新型的光催化材料受到研究者的廣泛關(guān)注。金屬-有機(jī)骨架材料具有比表面積大、結(jié)構(gòu)可設(shè)計(jì)、孔道可調(diào)控等突出優(yōu)勢(shì)。目前,MOFs材料的研究主要集中在其光催化環(huán)境凈化方面,而關(guān)于其可見光光催化制氫的研究相對(duì)較少。本論文主要基于MOFs材料構(gòu)筑復(fù)合光催化材料,并研究其可見光光催化制氫性能,具體研究?jī)?nèi)容如下：(1) CdS/UiO-66復(fù)合光催化的可見光光催化制氫性能：通過(guò)溶劑熱法合成出含鋯MOFs UiO-66,再利用原位合成法制備出復(fù)合光催化劑(CdS/UiO-66)。對(duì)制備的CdS/UiO-66系列催化劑進(jìn)行了XRD、SEM、TEM、UV-vis、PL等形貌、結(jié)構(gòu)和性質(zhì)的表征。以L-抗壞血酸為犧牲劑,檢測(cè)了CdS/UiO-66復(fù)合材料在可見光(λ≥420 nm)照射下的光解水制氫活性。實(shí)驗(yàn)結(jié)果顯示,制備的CdS/UiO-66復(fù)合型光催化劑具有較高的制氫活性和穩(wěn)定性,其光催化活性的提高可以歸結(jié)為光生電子-空穴對(duì)在CdS/UiO-66復(fù)合物界面之間能夠有效分離。當(dāng)CdS/UiO-66復(fù)合材料中CdS含量為16wt.%時(shí)光催化制氫活性達(dá)到最高。(2) UiO-66/g-C3N4復(fù)合光催化的可見光光催化制氫性能：采用煅燒法,將g-C3N4納米片層負(fù)載到UiO-66八面體上,得到UiO-66/g-C3N4光催化復(fù)合材料。在可見光(λ≥420 nm)照射下,以L-抗壞血酸為犧牲劑,檢測(cè)了UiO-66/g-C3N4的光解水制氫性能。測(cè)試結(jié)果表明, g-C3N4所占比例為50%時(shí)制氫速率為單一g-C3N4制氫速率的18倍之多。UiO-66和g-C3N4的結(jié)合能夠有效的提高光解水制氫活性,且催化劑穩(wěn)定性較好。由于g-C3N4本身對(duì)可見光有響應(yīng),UiO-66材料的介孔結(jié)構(gòu)加速光生電子的快速轉(zhuǎn)移,從而能夠大大提高制氫效率。(3)MIL-101(Cr)/Ni(dmgH)2非貴金屬助催化劑體系的可見光光催化制氫性能：在MIL-101(Cr)的基礎(chǔ)上,通過(guò)化學(xué)沉淀法在室溫下制得非貴金屬?gòu)?fù)合催化劑MIL-101(Cr)/Ni(dmgH)2。利用染料赤蘚紅B對(duì)MIL-101(Cr)/Ni(dmgH)2材料進(jìn)行敏化,在可見光的照射下,染料的加入可使MIL-101在15%體積分?jǐn)?shù)的三乙醇胺水溶液犧牲劑中光催化產(chǎn)氧,產(chǎn)氫速率可達(dá)45.9μmol·h-1。Ni(dmgH)2絡(luò)合物的加入可以代替了貴金屬作為助催化劑,染料的加入也擴(kuò)大了材料的光響應(yīng)范圍。
[Abstract]:Energy shortage and environmental pollution are two major problems that haunt the sustainable development of human society. Finding and developing renewable, pollution-free, cheap and easily available new energy is an important way to solve these problems. Hydrogen has a high combustion value. It is the most potential clean energy to drive the development of human society. Water is the most abundant resource on the earth, cheap and easy to obtain. Direct use of solar photocatalytic decomposition of water to produce hydrogen is an important technology for the preparation of clean energy. Semiconductor is widely used in photocatalytic reactions among many known materials. Many semiconductor photocatalytic materials affect their photocatalytic activity due to the wide band gap or easy photocorrosion. Therefore, the research and design of efficient photocatalytic materials is the key to the development of hydrophotolysis technology. Metal-organic frameworks. As a new type of photocatalytic materials, MOFs have been widely concerned by researchers. Metal-organic skeleton materials have many advantages, such as large specific surface area, structure design, pore control and so on. The research of MOFs materials is mainly focused on the photocatalytic environment purification, but the research on visible photocatalytic hydrogen production is relatively few. This paper mainly based on MOFs materials to construct composite photocatalytic materials. The catalytic properties of hydrogen production by visible light were studied. The main contents of this study are as follows: 1) the visible photocatalytic activity of CdS/UiO-66: MOFs UiO-66 containing zirconium was synthesized by solvothermal method. The composite photocatalyst, CDs / UiO-66, was prepared by in-situ synthesis. The CdS/UiO-66 series catalysts were prepared by XRDX SEMTEM. Characterization of morphology, structure and properties of UV-Vis PL. L- ascorbic acid was used as sacrificial agent. The photocatalytic activity of CdS/UiO-66 composites irradiated by visible light (位 鈮，

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