高效石墨烯基复合光催化材料可控构建及其光催化性能的构效关系研究

The conversion of solar energy into chemical fuels or high value-added fine chemicals can not only alleviate the energy crisis caused by the shortage of fossil fuels resources, but also provide organic raw materials for the petrochemical industry and its derivative industries, which is of great significance for both of the development of petrochemical industry and the implementation of our national sustainable development strategy. Design and synthesis of graphene-based semiconductor nanocomposite photocatalysts offers a new opportunity for the achievement of solar energy conversion. However, thus far, the knowledge regarding how to controllably optimize and prepare the graphene-semiconductor nanocomposite systems and how to microscopically tune the structure-activity relationship of these photocatalysts is still lacking. This project will launch in-depth study on some key issues, including the controlled preparation and systems optimization of the efficient and stable graphene-based nanocomposite photocatalysts, the improvement of their photocatalytic performance and so forth. We will focus on understanding the structure of materials, reaction mechanism and their relationship with the photocatalytic performance, in order to establish the controllable and scalable synthesis approaches of novel, efficient and stable graphene-based composite photocatalysts from the concept of systems materials engineering, and clarify the structure-activity relationship and the regulative laws for the photocatalysts. The as-prepared graphene-semiconductor nanocomposite photocatalysts will be utilized for photocatalytic hydrogen evolution from water, photocatalytic reduction of carbon dioxide and photocatalytic selective organic transformations, realizing the applications of graphene-based composite materials in the field of petrochemical industry.

将太阳能转化为化学燃料或高附加值的精细化学品，既可缓解因化石燃料资源短缺引起的能源危机，又能为石油化工及其衍生产业提供有机原料，对于石油化工的发展及实现我国可持续发展战略都具有重大意义。设计合成碳基石墨烯-半导体化合物复合型光催化材料为实现太阳能转化提供了新机遇。然而，目前对石墨烯-半导体化合物复合型材料的系统可控优化制备和光催化构效关系的微观调控还很缺乏。本项目拟针对高效稳定型碳基石墨烯复合光催化材料的系统可控优化制备及其光催化反应性能调控等关键问题进行系统深入的研究。亟待从材料结构、反应机理和光催化性能之间的关联等基本科学问题着手，建立基于系统化工程设计理念的新型高效稳定的石墨烯基复合光催化材料的可控规模化制备方法，阐明构效关系和调控规律，并将该类复合材料应用于光解水制氢，光催化还原二氧化碳及光催化选择性有机合成，实现该类碳基石墨烯复合材料在石油化工领域的应用。

该项目旨在对高效石墨烯基复合光催化材料的可控合成、改性及其规模化制备方法展开研究，探究充分发挥石墨烯在复合材料体系中导电特性的策略，阐明光催化剂的微观结构和光催化反应性能的内在构效关系，建立基于石墨烯-半导体复合材料的新型高效光催化反应，并将该类复合材料应用于光催化降解污染物，光解水制氢，光催化还原二氧化碳及选择性有机合成等与石油化工相关的领域中。在该项目的支持下，项目组围绕如何有效利用石墨烯的结构和电子特性，合理挖掘石墨烯的潜力，以及深入探究如何使石墨烯和半导体界面处的电荷分离转移与利用效率达到最优化等关键问题展开。取得的主要进展如下：(1)利用石墨烯独特的二维结构和表面特性，对复合材料的微观结构和形貌进行调控，实现了石墨烯基复合光催化材料的可控合成；(2)通过调节石墨烯材料的尺寸大小，表面性质，前躯体种类等多种策略来提高石墨烯材料的导电性，实现了对复合材料性能的优化；(3)设计构建了三维宏观结构的石墨烯基复合材料，增强其对载流子的分离效率和复合材料的回收利用性能；(4)探究了石墨烯在提升复合材料性能中的作用机制，揭示了石墨烯对复合材料吸附性能，光吸收性质以及传质方面的综合影响；(5)拓展和研究了石墨烯的其他特性，如通过元素掺杂的策略赋予其半导体特性，理论计算与实验相结合揭示了石墨烯作为光敏剂的作用机制，并提出有效提高其光敏化效率的方法。.在项目执行期间，项目组已在Nature Photonics, Nature Communications, Angewandte Chemie, Chemical Reviews, Chemical Society Reviews, Chem, ACS Nano, Chemical Science, Materials Horizons, Nano Today, Small, Journal of Catalysis，Applied Catalysis B, Nanoscale等国际学术期刊上发表SCI论文共计61篇，其中7篇入选Web of Science ESI 0.1%热点论文，16篇入选ESI高被引论文，22篇论文作为杂志封面论文发表，申请中国发明专利18项，其中已授权5项。此外项目负责人徐艺军教授作为主编编写丛书一部，参加国内外学术会议12次，做邀请报告7场，主题报告4场，口头报告1场。

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