- 學位論文
應用於可見光水裂解反應產氫之 Ru/(AgIn)xZn2(1-x)S2光觸媒
Ru/(AgIn)xZn2(1-x)S2 Photocatalysts for Water-Splitting Reaction to Produce Hydrogen under Visible Light Irradiation
摘要
(AgIn)XZn2(1-X)S2光觸媒的製備是利用熔鹽法（Molten-Salt Method）混合不同比例之Ag2S、In2S3及ZnS，再加入Na2SX助熔劑以升溫速度1℃/min升至所需的製備溫度，並維持1小時後自然冷卻至室溫，經水洗過濾數次再真空乾燥後，即可獲得(AgIn)XZn2(1-X)S2之灰色光觸媒粉末。將共觸媒Ru(0.5wt%)利用含浸法負載於(AgIn)XZn2(1-X)S2後，即得Ru/(AgIn)XZn2(1-X)S2光觸媒。所製備之光觸媒分別利用X 光繞射分析儀（XRD）、紫外光-可見光光譜分析儀（UV-Vis）、掃瞄式電子顯微鏡( SEM)、能量散佈光譜儀( EDS)來分析光觸媒的特性。由XRD結果得知，製備溫度600℃時光觸媒擁有最佳晶體結構。從UV-Vis結果得知， (AgIn)XZn2(1-X)S2光觸媒之x值增加時臨界波長會有明顯的紅平移。由SEM結果得知，600℃所製得(AgIn)0.22Zn1.56S2光觸媒之顆粒有較小且均勻之粒徑。另外在600℃下所製得(AgIn)XZn2(1-X)S2光觸媒之顆粒隨著X值增加而變大。由EDS得知，光觸媒組成鑑定為(AgIn)xZn2(1-x)S2。光觸媒之水裂解產氫反應是在加入Na2S(0.25M)/K2SO3(0.35M)犧牲劑之批式反應器中以450W金屬鹵素燈照射下進行。由實驗結果得知，在600℃製備所得Ru(0.5wt%)/(AgIn)0.22Zn1.56S2光觸媒之水裂解反應活性最佳，其產氫速率可達到412.5μmole/h。
並列摘要
The (AgIn)xZn2(1-x)S2 photocatalyst were prepared by the molten-salt method via mixing the different proportions of Ag2S-In2S3 and ZnS as preaursors and adding of the Na2SX flux. Followed by calcination at the required preparation temperature with the temperature elevating rate of 1 ℃/min, and natural cooling to the room temperature after maintaining for 1 hour. The obtained samples were washed with distilled water and filtered for several times. Finally the gray-colored powders of (AgIn)xZn2(1-x)S2 photocatalysts were obtained after the vacuum drying. All the prepared catalysts were loading of with Ru(0.5%) co-catalyst to Ru/(AgIn)xZn2(1-x)S2 photocatalysts. The photocatalystic characterization of prepared photocatalysts were carried out with X-ray diffraction (XRD), UV - Visible spectrometer (UV-Vis), scanning electron microscope (SEM), energy dispersed spectrometer (EDS). From the XRD results, it could be known that the photocatalysts possessed the best crystalline structure at 600℃ calcination. From the UV-Vis results, it could be known that with the increase of in (AgIn)xZn2(1-x)S2 photocatalysts, the absorption band edges showed obvious red shift. From the SEM results, it could be known that the grains of prepared photocatalysts by 600℃ calcination possessed the smaller and average particle diameters. Besides, with the increasing of X in (AgIn)xZn2(1-x)S2 prepared under 600℃ calcination, the grain size of (AgIn)xZn2(1-x)S2 photocatalysts would become larger. From the EDS results, it could be known that the composition of the photocatalysts was identified as (AgIn)xZn2(1-x)S2. The water-splitting reaction with the photocatalysts for hydrogen production was carried out in a batch reactor with the addition of the Na2S(0.25M)/K2SO¬3(0.35M)sacrificial reagent under the irradiation of 450W metallic halogen lamp. From the experimental results, the highest photocatalystic reactivity for the water-splitting reaction was obtained by the Ru(0.5%)/(AgIn)0.22Zn1.56S2 photocatalyst prepared at 600℃ calcination which possessed the hydrogen evolution rate of 412.5 μmole/h . Keywords : Molten-Salt Method, Photocatalyst, ZnS, Water-Splitting,