本文選題：硫化鉬 + 非晶相��； 參考：《鄭州大學(xué)》2017年碩士論文

【摘要】：近年來,太陽能光催化分解水制氫成為研究的熱點(diǎn)之一。硫化鉬類材料由于優(yōu)異的析氫活性、價(jià)格低廉、無毒等優(yōu)點(diǎn)被廣泛認(rèn)為是最具潛力的能取代貴金屬的催化劑。然而,硫化鉬類材料的光生載流子易于復(fù)合,遷移率低,導(dǎo)電性差等缺點(diǎn)限制了其光催化活性。針對(duì)以上問題,本文從增大暴露的活性位點(diǎn)的數(shù)目、擴(kuò)展光譜響應(yīng)范圍、促進(jìn)載流子分離等方面展開研究,具體工作內(nèi)容如下:(1)通過簡單的一步反應(yīng)法在低溫環(huán)境下利用鹽酸羥胺還原(NH4)2MoS_4合成非晶相MoS_3,并利用X光電子能譜(XPS)、X射線衍射(XRD)、掃描電子顯微鏡(SEM)和透射電子顯微鏡(TEM)等手段對(duì)其進(jìn)行表征;進(jìn)而以藻紅B鈉鹽(Erythrosin B,簡寫為EB)為光敏劑,三乙醇胺(Triethanolamine,簡寫為TEOA)為犧牲劑,測(cè)得非晶相MoS_3在最優(yōu)條件下(10 vol%TEOA,5.0 mM EB,0.1 g MoS_3,pH 9.0)的最大產(chǎn)氫速率高達(dá)1190.0μmol·h-1。另外還深入探究了影響體系穩(wěn)定性的原因,結(jié)果表明:在光照過程中,非晶相MoS_3先轉(zhuǎn)變?yōu)榉蔷郙oS_2,然后非晶相MoS_2再轉(zhuǎn)變?yōu)榫郙oS_2;并證實(shí)了產(chǎn)氫的活性成分是生成的非晶相MoS_2;產(chǎn)氫活性下降的主要原因是光敏劑EB的快速降解和催化劑MoS_3表面活性位點(diǎn)被占據(jù)。(2)利用非晶相MoS_3為前驅(qū)體合成T-MoS_2+x(T為煅燒溫度),并對(duì)其作了全面的表征;進(jìn)而以EB為光敏劑,TEOA為犧牲劑構(gòu)建了基于MoS_2+x的光催化產(chǎn)氫體系。結(jié)果表明:隨著煅燒溫度的改變,催化劑的組成、形貌、結(jié)晶性、比表面積等均發(fā)生了改變;煅燒溫度對(duì)催化劑的產(chǎn)氫性能具有顯著影響;在相同測(cè)試條件下,300-MoS_2+x表現(xiàn)出極高的產(chǎn)氫活性;在10 vol%TEOA,7.5 mM EB,pH 9.0的最優(yōu)條件下,300-MoS_2+x的最大產(chǎn)氫速率為1923.5μmol/h,達(dá)到煅燒前非晶相MoS_3活性的近1.6倍;循環(huán)產(chǎn)氫測(cè)試表明催化劑活性的下降同樣歸因于光敏劑EB的快速降解和催化劑表面活性位點(diǎn)被占據(jù)。(3)通過三步水熱法成功制備了MoS_2-NiS/CdS三元復(fù)合光催化劑,并對(duì)其進(jìn)行一系列表征;利用CdS為固體光敏劑,MoS_2和NiS為雙助催化劑實(shí)現(xiàn)了可見光下的光催化產(chǎn)氫,詳細(xì)研究了MoS_2-NiS/CdS在乳酸溶液中的產(chǎn)氫性能和穩(wěn)定性。實(shí)驗(yàn)結(jié)果表明:MoS_2-NiS/CdS在最佳條件下(MoS_2的含量為7 wt%,NiS負(fù)載量為2 wt%,pH 3.0,乳酸體積為40%)的最大產(chǎn)氫速率可達(dá)2525.2μmol·h-1,達(dá)到純CdS的11.3倍;隨著循環(huán)次數(shù)的增加,產(chǎn)氫效率沒有出現(xiàn)顯著下降,說明所制備的MoS_2-NiS/CdS復(fù)合光催化劑具有良好的穩(wěn)定性。
[Abstract]:In recent years, photocatalytic decomposition of water for hydrogen production by solar energy has become one of the hotspots. Molybdenum sulphide is widely regarded as the most potential catalyst to replace precious metals because of its excellent hydrogen evolution activity, low price and non-toxicity. However, the photocatalytic activity of molybdenum sulfide materials is limited by the disadvantages of easy recombination of photogenerated carriers, low mobility and poor electrical conductivity. In order to solve the above problems, this paper studies on increasing the number of active sites exposed, expanding the spectral response range, promoting carrier separation, etc. The specific work is as follows: (1) Synthesis of amorphous MoS3 by a simple one-step reaction method using hydroxylamine hydrochloride to reduce NH _ 4N _ 2MoS _ 4 at low temperature, and X-ray photoelectron spectroscopy (XPS) X-ray diffraction, scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Tem) was used to characterize it. The maximum hydrogen production rate of amorphous MoS_3 was determined to be as high as 1190.0 渭 mol h-1 under the optimum conditions by using Erythrosin B (EB3) as Guang Min agent and triethanolamine as sacrificial agent. Under the optimum conditions, the maximum hydrogen production rate was 1190.0 渭 mol h-1.The maximum hydrogen production rate was as high as 1190.0 渭 mol h-1. In addition, the reasons that affect the stability of the system are also deeply explored. The results show that: in the process of illumination, The amorphous phase MoS_3 was transformed into amorphous phase MoS _ 2, and then amorphous phase MoS_2 was transformed to crystalline phase MoS _ 2. It was confirmed that the active component of hydrogen production was formed amorphous phase MoS _ 2; the main reason for the decrease of hydrogen-producing activity was the rapid degradation of Guang Min agent EB and the catalyst MoS_3. The surface active site was occupied. (2) the amorphous phase MoS_3 was used as the precursor to synthesize T-MoS_2 XT as calcining temperature, and it was characterized comprehensively. Furthermore, the photocatalytic hydrogen production system based on MoS_2 x was constructed with EB as Guang Min agent and TEOA as sacrificial agent. The results showed that the composition, morphology, crystallinity and specific surface area of the catalyst changed with the change of calcination temperature, and the calcination temperature had a significant effect on the hydrogen production performance of the catalyst. The maximum hydrogen production rate of 300-MoS2x is 1923.5 渭 mol / h under the optimum conditions of 10 vola 7.5 mm EBN pH 9.0, which is about 1.6 times of the MoS_3 activity of the amorphous phase before calcination, and the maximum hydrogen production rate of 300-MoS2x is about 1923.5 渭 mol / h under the same test conditions, and the maximum hydrogen production rate of 300-MoS2x is 1923.5 渭 mol / h under the optimum conditions of 10 volta 7.5 mm EBN pH 9.0. Cyclic hydrogen production test showed that the decrease of catalyst activity was also attributed to the rapid degradation of Guang Min agent EB and the occupation of catalyst surface activity sites. The MoS_2-NiS/CdS ternary photocatalyst was successfully prepared by three-step hydrothermal method and characterized by a series of characteristics. Photocatalytic hydrogen production under visible light was realized by using CdS as solid Guang Min agent MoS _ 2 and NiS as double catalyst. The hydrogen production performance and stability of MoS_2-NiS/CdS in lactic acid solution were studied in detail. The results showed that under the optimum conditions, the maximum hydrogen production rate of mol / CDs reached 2525.2 渭 mol h-1, 11.3 times higher than that of pure CdS, with the maximum hydrogen production rate of 2525.2 渭 mol h-1, which was 11.3 times higher than that of pure CdS, when the load of NiS was 7 wtand the load of NiS was 3.0, and the efficiency of hydrogen production did not decrease significantly with the increase of cycle times. The results show that the prepared MoS_2-NiS/CdS composite photocatalyst has good stability.
【學(xué)位授予單位】：鄭州大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O643.36;TQ116.2

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