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作 者:吴朝军[1] 尹明彩[1] 张尚青 孙艺萌[1] 贾芳芳[1] 樊耀亭[1] WU Chaojun;YIN Mingcai;ZHANG Shangqing;SUN Yimeng;JIA Fangfang;FAN Yaoting(College of Chemistry and Molecular Engineering,Zhengzhou University,Zhengzhou 450001)
机构地区:[1]郑州大学化学与分子工程学院,郑州450001
出 处:《材料导报》2017年第A01期158-163,共6页Materials Reports
基 金:国家自然科学基金(21171147);郑州大学全国大学生创新创业训练计划(2015xjxm190)
摘 要: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-C_3N_4)的基础之上,采用简单的低温溶液反应法将二硫化钼(MoS_2)与石墨相氮化碳(g-C_3N_4)复合得到复合催化剂MoS_2/g-C_3N_4,并利用透射电子显微镜(TEM)、X射线衍射(XRD)、紫外-可见漫反射(DRS)、傅里叶变换红外光谱(FT-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MoS_2纳米颗粒负载到g-C_3N_4上可使g-C_3N_4的光催化产氢性能得到显著提高。当MoS_2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-C3N4)was prepared by using urea as starting material.Then,compo-site photocatalyst MoS2/g-C3N4 was synthesized by a simple low-temperature solution reaction method and characterized by transmission electron microscopy(TEM),X-ray diffraction(XRD),UV-vis diffuse reflectance spectroscopy(US-vis DRS),Fourier transform 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 MoS2 nanoparticles were successfully loaded onto g-C3N4 and the hydrogen production activity of the composite photocatalyst was significantly improved compared with that of pure g-C3N4.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 total H 2 produced reached 212.61μmol in 6 h under the optimized hydrogen production condition of pH 9.0,25 mL CdSe QDs.Finally,according to results of the fluorescence quenching,the mechanism of photocatalytic hydrogen evolution was proposed.
关 键 词:光催化产氢 CdSe量子点敏化 MoS2/g-C3N4
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