2D/2D层状复合直接Z型产氢光催化材料的静电自组装制备

To solve the critical environmental and energy issues, as well as advance sustainable human development, hydrogen generation through photocatalytic water splitting is vital. The single photocatalytic material is confronted with low activity, rapid recombination of photogenerated electron-hole pairs and suppressed oxidation and reduction abilities. This project aims to construct stable photocatalytic composite materials with high efficiency via employing self-assembly fabrication protocol and designing 2D/2D layered structures. This material can solve the limited contact area and sluggish charge transfer confronted by the composite with other kinds of dimensions. It can also overcome the drawbacks faced by traditional Type-II heterojunction, namely, the weak oxidation and reduction abilities of the photogenerated holes and electrons. This research will center on the preparation method and design principle, as well as the generation, separation, transportation and photocatalytic behavior of the electrostatic self-assembly composite material. Moreover, the effect of the type of material, thickness of the 2D layer and the ratio of the two components on the efficiency of the photocatalytic materials will be investigated. The relationship between surface area, pore structure, morphology and the hydrogen generation performance will be revealed. Therefore, the mechanism of the enhancement by this 2D/2D layered composite material is elucidated. This project can drive the practical application of photocatalytic materials, and hopefully world-class innovative results will be obtained.

光催化分解水产氢在解决日益严重的能源环境问题和促进人类可持续发展等方面均至关重要。针对单一光催化材料活性不高，光生空穴和电子易于复合、且氧化还原能力较弱的关键科学问题。项目拟通过静电自组装方法制备2D/2D层状复合直接Z型光催化产氢材料，该层状复合材料具有接触面积大和电子空穴传输迁移速率快等优点，可以克服纳米颗粒或纳米线相互复合接触面积小，电荷迁移受阻的瓶颈，以及传统II型异质结空穴电子氧化还原能力弱的缺陷。重点研究该复合材料的静电自组装制备方法与设计原理，光生空穴电子产生、分离、传输与催化行为；探索2D光催化材料厚度、种类、比例对复合直接Z型光催化材料产氢性能的影响规律；揭示2D/2D层状复合材料的比表面积、孔结构、形貌与产氢性能的关系；阐明2D/2D层状复合直接Z型光催化材料性能增强机理。推动光催化产氢材料的实际应用，取得具有国际水准的创新性研究成果。

项目执行期间通过静电纺丝法、水热模板法和原位生长等方法制备了直接Z型（后改为S型）异质结光催化材料；研究了材料组分和结构等因素与光催化产氢、产双氧水和二氧化碳还原性能的内在关系；揭示调控组分结构、优化合成方法的有效措施，阐明光生电荷分离和迁移的内在机理和影响规律。结合原位光照XPS测试、原位光照AFM测试和材料计算，本项目为材料合成和实现“双碳目标”等领域提供实验理论基础和思路，在该项目执行期间，共计45篇研究论文标注了本资助项目，发表在多种国内外权威刊物上，包括：Advanced Materials、Nature Communications、Chem、Small、Applied Catalysis B。其中与项目直接相关的论文26篇，ESI高被引论文14篇，热点论文4篇，论文总他引次数4000余次。项目执行期间共毕业了3位博士研究生和3位硕士研究生。项目期间，项目负责人张留洋总共参加国内外学术交流9次，并作邀请报告8次，参与建立了较为广泛的国际学术交流与合作关系。项目负责人张留洋2019年入选湖北省高层次人才计划，2022年入选了科睿唯安全球高被引科学家，并聘任为中国地质大学（武汉）材料与化学学院教授；项目期间被聘为国内期刊《物理化学学报》的编委。