催化学报

催化学报 ›› 2020, Vol. 41 ›› Issue (8): 1208-1216.DOI: 10.1016/S1872-2067(19)63511-4

• 论文 • 上一篇    下一篇

一步法制备TiO2/石墨烯复合多孔薄膜应用于增强光催化活性及光伏性能

郭俊雄a, 李奕奕a, 李尚栋a, 崔旭梅b, 刘宇c, 黄文a, 毛琳娜a, 魏雄邦a, 张晓升a   

  1. a 电子科技大学电子薄膜与集成器件国家重点实验室, 电子科学与工程学院(示范性微电子学院), 四川成都 610054;
    b 成都信息工程大学光电工程学院, 四川成都 610225;
    c 清华大学微电子学研究所, 清华信息科学与技术国家实验室, 北京 100084
  • 收稿日期:2019-10-11 修回日期:2019-11-16 出版日期:2020-08-18 发布日期:2020-08-08
  • 通讯作者: 郭俊雄, 崔旭梅, 刘宇
  • 基金资助:
    国家自然科学基金（61804023，61971108）；四川省重点研发项目（2018GZ0527）；四川省科技创新研究团队建设项目（2015TD00008）；四川省科技厅重点项目（2017JY0038）.

One-step fabrication of TiO2/graphene hybrid mesoporous film with enhanced photocatalytic activity and photovoltaic performance

Junxiong Guoa, Yiyi Lia, Shangdong Lia, Xumei Cuib, Yu Liuc, Wen Huanga, Linna Maoa, Xiongbang Weia, Xiaosheng Zhanga   

  1. a State Key Laboratory of Electronic Thin Films and Integrated Devices, School of Electronic Science and Engineering(National Exemplary School of Microelectronics), University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China;
    b College of Optoelectronic Engineering, Chengdu University of Information Technology, Chengdu 610225, Sichuan, China;
    c Institute of Microelectronics, Tsinghua National Laboratory for Information Science and Technology(TNList), Tsinghua University, Beijing 100084, China
  • Received:2019-10-11 Revised:2019-11-16 Online:2020-08-18 Published:2020-08-08
  • Supported by:
    The authors acknowledge the financial supports of this work by the National Natural Science Foundation of China (61804023, 61971108), the Key R&D Program of Sichuan Province (2018GZ0527), the Science and Technology Innovation Research Team Construction Project of Sichuan Province (2015TD00008) and the Key Projects of Science and Technology Department of Sichuan Province (2017JY0038).

PDF

212

摘要： 纳米二氧化钛具有制备简单、成本低、化学稳定性好及光响应度高等诸多优势，因而广泛应用于光催化及太阳能转化等诸多领域中.然而，传统TiO2纳米材料受限于较高光电子空穴复合率，导致其光催化活性及光电转化效率较低.为解决这一问题，研究者采用多种方法用以改善纳米TiO2的结构，包括化学掺杂、半导体材料插层、碳材料杂化等；另一方面则关注材料结构的设计，例如将合成的纳米材料进一步加工为多孔薄膜，以增大材料比表面积及器件稳定性，以增强其器件性能.其中，将石墨烯引入纳米TiO2中，形成复合纳米材料，以提升材料本身的光电子传输效率，降低光生载流子复合率，为制备高性能光催化剂及光伏器件开辟了一条可行之路.然而，目前制备的纳米TiO2/石墨烯复合材料的性能仍不理想，其中常见的问题为合成的材料团聚严重，导致光生载流子在界面传输阻力及复合率都十分高，限制其实际应用.此外，当前大多数关于纳米TiO2/石墨烯的制备方法仍为溶胶凝胶法、水热法等，所得材料需要进一步进行微纳加工方能形成介孔结构；这些加工方式往往需要二次退火处理，这会进一步加重纳米材料的团聚现象，导致孔隙率分布混乱、材料界面缺陷增多等不良结果.
因此，本文采用一步法-蒸汽热法成功制备了TiO2/石墨烯复合多孔薄膜，无需二次热处理.实验结果表明，所制TiO2/石墨烯复合物（VTH）的形貌为二维结构，其比表面积高达260m2 g-1，获得的多孔薄膜无明显团聚且孔隙分布集中.当复合物中还原氧化石墨烯含量为5.0 wt%时，其光催化活性最高，高于单一的TiO2薄膜近3倍；将还原氧化石墨烯含量为0.75 wt%的复合物用于染料敏化太阳能电池的光阳极时，光电转化效率达到7.58%，明显高于传统方法制备的单一TiO2的（4.38%）.

关键词: TiO2-石墨烯复合物, 光催化活性, 光阳极, 蒸汽热法, 介孔薄膜

Abstract: We synthesized a mesoporous film based on TiO2-reduced graphene oxide (RGO) hybrids using a one-step vapor-thermal method without the need for an additional annealing process. The vapor-thermally prepared TiO2-graphene hybrid (VTH) features unique structures with an ultra-large specific surface area of ~260 m2 g-1 and low aggregation, giving rise to enhanced light harvesting and increased charge generation and separation efficiency. It was observed that a mesoporous film with uniform pore distribution is simultaneously obtained during the VTH growth process. When a 5.0 wt% RGO VTH film was used as the active layer in photocatalysis, the highest photocatalytic activity for degradation of methyl orange was achieved. For another, when a 0.75 wt% RGO VTH film was used as the photoanode in a dye-sensitized solar cell, the power conversion efficiency reached 7.58%, which represents an increase of 73.1% compared to a solar cell using an a photoanode of pure TiO2 synthesized by a traditional solvothermal method. It is expected that this facile method for the synthesis of TiO2/graphene hybrid mesoporous films will be useful in practical applications for preparing other metal oxide/graphene hybrids with ultra-high photocatalytic activity and photovoltaic performance.

Key words: TiO2-graphene hybrid, Catalytic activity, Photoanode, Vapor-thermal method, Mesoporous film