銻鉛氧化物及其複合氧化石墨烯及石墨相氮化碳光觸媒的合成、特性、活性及降解機制之研究

近年來研究發現，由於鉛銻系化合物的特殊片狀結構以及高活性，可做為良好的可見光光催化劑，且可使用在鈣鈦礦太陽能電池材料的研究領域。本研究以高壓水熱法合成鉛銻氧化合物找出最佳條件之觸媒後，並且複合重量百分比不同之石墨相氮化碳(Graphitic-like carbon nitride, g-C3N4)以及複合克數不同氧化石墨烯(Graphene Oxide, GO) 並置入高壓釜(Autoclave)設備中進行反應，合成複合材料之光觸媒，並對結晶紫(Crystal Violet，簡稱CV)染料及水楊酸(2-hydroxybenzoic acid，簡稱2-HBA)照射可見光，進行光催化降解。 合成之樣品需經過分析鑑定，利用X射線粉末繞射儀(XRD)、場發射槍掃描式電子顯微鏡附能量分散光譜儀(FE-SEM-EDS)、場發式穿透式電子顯微鏡附能量分散光譜儀(FE-TEM-EDS) 、高解析X光光電子能譜儀(HR-XPS)、擴散反射光譜儀(DRS)、比表面積分析儀(BET)、螢光光譜儀(PL)、紫外光光電子能譜儀(UPS)及電磁共振光譜儀(EPR)等儀器鑑定其產物分子元素之組成、能帶間隙大小及化合物的結構及氧化態各種資料，在不同條件的觸媒下，進行光催化降解CV及2-HBA效率之影響，藉此得知其降解的反應速率，進而比較一系列光觸媒的光催化活性。 經由儀器的分析後，可以得知對CV降解而言，在P3SO-250-13-12 (PbSb2O6/Sb2O5)效果最好的k值中為0.0359 h−1，而在複合重量百分比為30%之g-C3N4後，P3SO-250-13-12/g-C3N4 (PbSb2O6/Sb2O5/g-C3N4)其k值提升為0.0579 h−1 ，降解效果明顯提升1.6倍之多。當複合0.1 g的GO後，P3SO-250-13-12/0.1g GO (PbSb2O6/Sb2O5/GO)其k值提升為0.0619 h−1。由PL鑑定中可得知電子電洞的再結合率明顯降低，使其增強光催化活性，改善鉛銻氧化合物在光催化領域中的限制，故可以確認複合GO可以使其純相光觸媒提高光催化效率。

Research in past years discovered that the special blocky structure and high activity of lead/antimony compounds could be good visible light photocatalysts and be used in the research on perovskite solar cell materials. High-pressure hydrothermal method is used in this study for synthesizing lead/antimony oxide to find out the optimal catalyst. Graphitic carbon nitride (g-C3N4) with different compound weight percentage and graphene oxide (GO) with distinct compound gram are placed in the autoclave equipment for reaction to synthesize composite photocatalysts. Crystal violet (CV) dye and 2-hydroxybenzoic acid (2-HBA) are further irradiated visible light for photocatalytic degradation.The synthesized samples should be analyzed and tested. X-ray powder diffractometer (XRD), field emission scanning electron microscope energy dispersive X-ray spectrometer (FE-SEM-EDS), field emission gun transmission microscope energy dispersive X-ray spectrometer (FE-TEM-EDS), high-resolution X-ray photoelectron spectroscopy (HR-XPS), diffuse reflectance spectroscopy (DRS), specific surface area analyzer (BET), photoluminescene spectrometer (PL), ultraviolet photoelectron spectroscopy (UPS), and electron paramagnetic resonance (EPR) are utilized for testing the composition of molecule element, band gap, and compound structure of products as well as oxidation state. Under catalysts with different conditions, the effect on photocatalytic degradation CV and 2-HBA efficiency is preceded for acquiring the reaction speed of degradation. The photocatalytic activity of the series of photocatalysts is further compared.After the analyses, the best effect of CV degradation on P3SO-250-13-12 (PbSb2O6/Sb2O5) appears on k= 0.0359 h−1; and, after g-C3N4 with the compound weight percentage 30%, k of P3SO-250-13-12/g-C3N4 (PbSb2O6/Sb2O5/g-C3N4) increases to 0.0579 h−1, with the degradation effect obviously enhancing 1.6 times. After compounding 0.1 g GO, k of P3SO-250-13-12/0.1g GO (PbSb2O6/Sb2O5/GO) increases to 0.0619 h−1. The PL test shows obvious reducing recombination rate of electron hole to enhance the photocatalytic activity and improve the limit of lead/antimony oxide in photocatalysis. As a result, it is confirmed that compound GO could enhance the photocatalysis effect of the pure phase photocatalyst.