太阳能光催化分解水制氢被认为是从根本上解决能源与环境问题较为理想的途径之一。在以尿素为原料制得石墨相氮化碳(g-C3N4)的基础之上,采用简单的低温溶液反应法将二硫化钼(MoS2)与石墨相氮化碳(g-C3N4)复合得到复合催化剂MoS2/g-GN4,并利用透射电子显微镜(TEM)、X射线衍射(XRD)、紫外一可见漫反射(DRS)、傅里叶变换红外光谱(Fr_IR)和荧光光谱等对该复合光催化剂的组成、形貌和光物理性能进行了表征;进而以CdSe量子点为光敏剂,三乙醇胺(TEOA)为牺牲剂,构建了不含贵金属的三组分光催化产氢体系,并对体系pH值、CdSe量子点浓度等对产氢性能的影响进行了研究。结果表明:将MoS2纳米颗粒负载到g-CsN4上可使手GN4的光催化产氢性能得到显著提高。当Mos2负载量为7%(质量比)时,在最佳的条件下(pH=9.0,CdSe量子点的体积为25mL),最大产氢速率达到了141.74μmol·h^-1,6h的产氢总量达到了212.61μmol。最后,结合荧光猝灭实验,推测了该体系的产氢机理。
Solar hydrogen production by water splitting has been considered as an ideal route to solve the problems of energy and environment. Herein, firstly, graphitic carbon nitride (g-Ca N4 ) was prepared by using urea as starting material. Then, compo- site photocatalyst MoS2/g-CaN4 was synthesized by a simple low-temperature solution reaction method and characterized by transmis- sion electron microscopy (TEM), X-ray diffraction (XRD), UV-vis diffuse reflectance spectroscopy (US-vis DRS), Fourier trans- form infrared (FT-IR) spectroscopy and photoluminescence (PL) spectroscopy to obtain its composition, morphology and photophy- sical properties. Furthermore, a noble-metal-free hydrogen evolution system was constructed by using CdSe quantum dots (QDs) as photosensitizer and triethanolamine (TEOA) as sacrificial agent, and the reaction parameters, such as pH value of the system and CdSe QDs concentration were optimized. The results showed that MoSv nanoparticles were successfully loaded onto g-Ca N4 and the hydrogen production activity of the composite photoeatalyst was significantly improved compared with that of pure g-C3 N4. When the loading amount of MoS2 was 7% (mass ratio), the maximal hydrogen evolution rate reached high up to 141.74μmol·h 1 and the to- tal H2 produced reached 212. 61μmol in 6 h under the optimized hydrogen production condition of pH 9.0, 25 mL CdSe QDs. Final- ly, according to results of the fluorescence quenching, the mechanism of photocatalytic hydrogen evolution was proposed.