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基于硅納米線(xiàn)陣列的光催化體系的構(gòu)建及其光催化還原水制氫性能

發(fā)布時(shí)間:2018-05-14 03:00

  本文選題:Si納米線(xiàn)陣列 + EDTA金屬配合物; 參考:《上海應(yīng)用技術(shù)學(xué)院》2015年碩士論文


【摘要】:硅納米線(xiàn)以其獨(dú)特的光電性能受到了越來(lái)越多的研究者的關(guān)注。隨著研究的深入,使用硅納米線(xiàn)(SiNWs)陣列作為光催化劑來(lái)制備氫氣也引起了人們的廣泛興趣,成為了目前光催化制氫領(lǐng)域的新熱點(diǎn)。為此,我們?cè)诒菊撐牡难芯恐?利用乙二胺四乙酸金屬配合物(EDTA-M, M=Ni、Co)同時(shí)作為光敏化劑和犧牲劑,設(shè)計(jì)并構(gòu)建了一系列基于SiNWs陣列的光催化體系,并在模擬太陽(yáng)光的照射下,考察了上述催化體系的光催化還原水制氫性能。具體研究?jī)?nèi)容如下:(1)在模擬太陽(yáng)光的條件下,使用EDTA-Ni作為光敏化劑和犧牲劑,構(gòu)建了EDTA-Ni敏化的SiNWs陣列,并考察了其光催化還原水制氫性能。此外,還通過(guò)光電化學(xué)手段對(duì)該催化體系的光催化還原水制氫機(jī)理進(jìn)行了初步探討。研究結(jié)果表明:EDTA-Ni敏化的SiNWs陣列是一個(gè)性能較為優(yōu)異的光催化制氫催化劑,其光催化制氫速率可達(dá)2.41 L.m2.h-1。在光催化還原水制氫過(guò)程中,EDTA-Ni既是敏化劑又是犧牲劑,起著非常重要的作用,可以顯著地提高SiNWs陣列對(duì)可見(jiàn)光的利用效率。當(dāng)使用EDTA-Ni替代EDTA-Na時(shí), SiNWs陣列對(duì)λ500 nm光的利用效率提高了5倍。另外,實(shí)驗(yàn)結(jié)果還表明EDTA-Ni敏化的SiNWs陣列具有良好的光穩(wěn)定性和可循環(huán)性能。(2)在上述研究的基礎(chǔ)上,使用EDTA-Ni/EDTA-Co混合配合物代替單一EDTA-Ni作為敏化劑和犧牲劑,構(gòu)建了EDTA-Ni/EDTA-Co共敏化的SiNWs陣列,并在模擬太陽(yáng)光的條件下,考察了其光催化還原水制氫性能。研究結(jié)果表明:利用EDTA-Ni/EDTA-Co的協(xié)同作用,可以進(jìn)一步提高SiNWs陣列的光催化制氫效率,其光催化制氫速率可達(dá)2.8 L.m2.h-1。此外,光電化學(xué)手段還表明,在光催化還原水制氫過(guò)程中,EDTA-Ni與EDTA-Co之間存在著明顯的協(xié)同作用。這導(dǎo)致SiNWs陣列工作波長(zhǎng)被進(jìn)一步拓寬。(3)通過(guò)在SiNWs陣列上接枝Ti02納米棒,構(gòu)建了TiO2-Si納米“森林”。隨后,使用EDTA-Ni作為光敏化劑和犧牲劑,考察了該納米“森林”的光催化還原水制氫性能,并通過(guò)光電化學(xué)手段對(duì)其光催化還原水制氫機(jī)理進(jìn)行了初步探討。研究結(jié)果表明:通過(guò)構(gòu)筑TiO2-Si納米“森林”復(fù)合光催化體系,納米Ti02的光催化還原水制氫性能得到了明顯改善。相比于在SiNWs陣列上簡(jiǎn)單涂覆的P25, TiO2-Si納米“森林”的光催化制氫速率是其近2倍。這意味著在固體基片上構(gòu)建TiO2-Si納米“森林”是一個(gè)很好的、Ti02納米材料的固定手段?捎行Ы鉀QTi02納米粒子固定化所帶來(lái)的光催化效率下降的問(wèn)題。
[Abstract]:Silicon nanowires have attracted more and more attention due to their unique photoelectric properties. With the development of research, the use of silicon nanowires (SiNWs) arrays as photocatalysts to produce hydrogen has attracted extensive interest and become a new hot spot in the field of photocatalytic hydrogen production. Therefore, in this thesis, a series of photocatalytic systems based on SiNWs arrays were designed and constructed by using EDTA-MMNICO as Guang Min agents and sacrificial agents, and under simulated solar irradiation, a series of photocatalytic systems based on SiNWs arrays were designed and constructed. The photocatalytic reduction of water for hydrogen production was investigated. The main contents of this study are as follows: (1) under the condition of simulated solar light, EDTA-Ni sensitized SiNWs array was constructed by using EDTA-Ni as Guang Min agent and sacrificial agent, and its photocatalytic reduction of water for hydrogen production was investigated. In addition, the mechanism of photocatalytic reduction of water for hydrogen production was also discussed by photochemical method. The results show that the SiNWs array sensitized by 1: EDTA-Ni is an excellent photocatalytic catalyst for hydrogen production, and the photocatalytic hydrogen production rate can reach 2.41 L 路m ~ (2. 2) h ~ (-1). In the process of photocatalytic reduction of hydrogen from water, EDTA-Ni is both a sensitizer and a sacrificial agent, which plays a very important role in improving the efficiency of visible light utilization of SiNWs arrays. When EDTA-Na was replaced by EDTA-Ni, the utilization efficiency of 位 500nm light in SiNWs array was increased by 5 times. In addition, the experimental results also show that the SiNWs array sensitized by EDTA-Ni has good photostability and reproducibility. (2) on the basis of the above research, the mixed EDTA-Ni/EDTA-Co complex is used instead of a single EDTA-Ni as sensitizer and sacrificial agent. A EDTA-Ni/EDTA-Co co-sensitized SiNWs array was constructed and its photocatalytic reduction of water for hydrogen production was investigated under simulated solar light. The results show that the photocatalytic hydrogen production efficiency of SiNWs arrays can be further improved by using the synergistic effect of EDTA-Ni/EDTA-Co, and the photocatalytic hydrogen production rate can reach 2.8 L 路m ~ (2. 2) h ~ (-1). In addition, the photochemical method also shows that there is an obvious synergism between EDTA-Ni and EDTA-Co in the process of photocatalytic reduction of hydrogen from water. As a result, the working wavelengths of SiNWs arrays were further broadened. (3) by grafting Ti02 nanorods onto SiNWs arrays, the "forest" of TiO2-Si nanocrystals was constructed. Then, EDTA-Ni was used as Guang Min agent and sacrificial agent to investigate the photocatalytic reduction of water for hydrogen production. The mechanism of photocatalytic reduction of water for hydrogen production was preliminarily discussed by photochemical means. The results show that the photocatalytic reduction of water for hydrogen production by TiO2-Si nanocrystalline "forest" composite photocatalytic system has been improved obviously. Compared with P25 coated on SiNWs arrays, the photocatalytic hydrogen production rate of TiO2-Si nano-" forest "is nearly twice as high as that of P25. This means that the construction of TiO2-Si nanoscale "forest" on solid substrates is a good immobilization method for Ti02 nanomaterials. It can effectively solve the problem of decreasing photocatalytic efficiency caused by immobilization of Ti02 nanoparticles.
【學(xué)位授予單位】:上海應(yīng)用技術(shù)學(xué)院
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2015
【分類(lèi)號(hào)】:O643.36;TQ116.2

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