- 學位論文
應用於水裂解反應產氫之 Ru/ (CuAg) XIn2XZn2(1-2X)S2光觸媒研究
Ru/ (CuAg) XIn2XZn2(1-2X)S2 Photocatalysts for Water-splitting Reaction to Produce Hydrogen
摘要
本研究是以熔鹽法製備(CuAg)xIn2xZn2(1-2x)S2光觸媒，藉由混合不同比例之Cu2S、 Ag2S 、 In2S3與ZnS作為前驅物並加入助熔劑Na2Sx中煅燒而得。此外所製備好之(CuAg)xIn2xZn2(1-2x)S2光觸媒再以含浸法負載共觸媒Ru於其上即得Ru/(CuAg)xIn2xZn2(1-2x)S2光觸媒。所製備之光觸媒以 XRD 、 UV-Vis與SEM測定其性質。由XRD結果可知製備溫度600℃時光觸媒擁有最佳晶體結構，(CuAg)xIn2xZn2(1-2x)S2光觸媒隨著x值增加，光觸媒結晶會由纖維鋅礦及閃鋅礦兩種混合晶相，轉變成黃銅礦結構。由UV-Vis結果可得知(CuAg)xIn2xZn2(1-2x)S2光觸媒在x=0.25時具有最佳吸光値，隨著x增加吸收峰會有紅平移的現象。由SEM結果得知600℃所製得光觸媒之顆粒有較小且均勻之粒徑，另外在600℃下所製得(CuAg)xIn2xZn2(1-2x)S2光觸媒之顆粒隨著x值增加而變大。 不同x值的Ru/ (CuAg)xIn2xZn2(1-2x)S2光觸媒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(0.5 wt%)/ (CuAg)0.25In0.5ZnS2光觸媒之水裂解反應活性最佳，其產氫速率可達到586μmole/h。
並列摘要
The purpose of this research is to prepare the (CuAg)xIn2xZn2(1-2x)S2 photocatalysts by the molten-salt method by mixing different proportions of Cu2S,Ag2S,In2S3 and ZnS as precursors and adding Na2Sx flux agent during the calcination. The prepared (CuAg)xIn2xZn2(1-2x)S2 photocatalysts followed by loading of Ru as co-catalyst to obtain Ru /(CuAg)xIn2xZn2(1-2x)S2. The properties of the prepared photocatalysts were investigated by means of UV-Vis , XRD and SEM. From UV-Vis results, it could be known that the (CuAg)xIn2xZn2(1-2x)S2 photocatalysts possessed the best absorption band-edge at x=0.25 with the increase of x, the absorption band edges of prepared photocatalysts would show the phenomenon of red shift. From XRD results, it could be known that with the increase of x, the structure of the (CuAg)xIn2xZn2(1-2x)S2 photocatalysts would transform from the mixture of two crystalline phases of wurtize structure and zinc-blend structure to the chalcopyrite structure. From SEM results, it could be seen that the photocatalysts prepared by 600℃ calcination possessed small practical diameters with uniform size. Also, with the increase of x in the (CuAg)xIn2xZn2(1-2x)S2 photocatalysts, the particle diameters of the prepared photocatalysts increased .The Ru /(CuAg)xIn2xZnS2 photocatalysts which were prepared with different x proportions, were put into a batch reactor to carry out the water splitting reaction to produce hydrogen under the irradiation of 450W metallic halogen lamp. The water splitting reaction results showed that the Ru /(CuAg)0.25In0.5ZnS2 photocatalysts which was prepared by 600℃ calcination,could reach to the hydrogen producing rate of 586 μmol/hr with the addition of Na2S(0.25M)/K2SO3(0.35M) sacrificial reagent into the water solustion.