稀土钼酸盐类石墨烯结构可控制备与催化氧化性能研究

Fabricating graphene-like inorganic materials and applying them in proper fields is one of the most attractive topics of materials research, while there are very few reports about the graphene-like lanthanide molybdates. It will offer a kind of high active catalysts to develop the graphene-like lanthanide molybdates which have high surface area. As a result, in this proposal, we plan to fabricate graphene-like lanthanide molybdates by ultrasonic exfoliation after a hydrothermal reaction step. The reaction parameters will be carefully tuned to obtain the graphene-like materials with high yields, unique thickness (layers) and low defects. Furthermore, the morphology and compositions of graphene-like lanthanide molybdates will be extensively modulated and series of products with different lateral size /morphology, thickness (layers) and compositions will be obtained. From these work, a simple and reliable method for high quality and tunable fabrication of graphene-like lanthanide molybdates will be summarized. Then, catalytic oxidation properties of graphene-like lanthanide molybdates will be studied, and the reaction of methanol selective oxidation to formaldehyde will be chosen as the model system. During this process, the relationship between structural and composition parameters of graphene-like materials and their catalytic properties such as conversion, selectivity, TOF and lifetime etc. will be carefully studied and summarized, besides that, several kinds of graphene-like lanthanide molybdates with high catalytic activity will be selected. Based on studies referred above, this proposal will be beneficial for development of novel graphene-like inorganic materials and their applications for catalysis.

无机类石墨烯结构材料的合成与应用是当前材料领域的研究热点,但有关稀土钼酸盐类石墨烯结构材料的合成与性质研究极为少见。研发高比表面积稀土钼酸盐类石墨烯结构材料有望提供一类较高活性的催化材料。本项目拟通过水热反应与超声剥离相结合的方法，优化各类反应参数，制备产率高、厚度（层数）均一、缺陷少的稀土钼酸盐类石墨烯结构材料。并实现所得材料结构和组成的有效调变，获得一系列具有不同截面尺寸和形貌、厚度（层数）以及组成的稀土钼酸盐类石墨烯结构材料。总结一套简便、可靠的稀土钼酸盐类石墨烯结构高质量可控制备方法。进而以甲醇选择性氧化制甲醛为模型反应，研究所得各种稀土钼酸盐类石墨烯结构的催化氧化性能，总结其结构和组成参数与催化反应转化率、选择性、TOF和催化剂寿命等参数的关联规律，筛选出几种具有较高催化活性的稀土钼酸盐类石墨烯结构材料。为新型无机类石墨烯结构材料的研发及其在催化领域的应用提供科学依据。

无机类石墨烯结构材料的合成与应用是当前材料领域的研究热点。本项目通过水热反应与超声剥离相结合的方法，优化各类反应参数，制备了镧、铈、镨、钕等系列稀土钼酸盐层状结构前驱体材料和类石墨烯结构材料。发现了氨基酸水热过程控制层状结构前驱体形貌和微观结构的内在规律。并实现所得材料结构和组成的有效调变，总结了一套较为简便、可靠的稀土钼酸盐类石墨烯结构可控制备方法。以钼酸镨为例,研究制备了氧化铝/氧化钛负载的类石墨烯结构钼酸镨复合材料,并初步研究其催化氧化性能。在上述工作研究思想启发下，进一步发展了多种层状结构、类石墨烯结构等相关材料制备及其在光催化氧化、光催化还原、光电催化氧化等方面的应用，包括：制备了层状结构结晶单质红磷及其复合材料，首次发现了该类材料的高效光催化氧化和还原反应性能，总结了该材料结构-性能的关联规律；认识并发展了超薄涂层材料和纳米级界面薄层在光电催化氧化中的应用，获得优异的光电化学增强效果；首次制备了类石墨烯氮化碳负载钒酸盐量子点复合光催化材料以及层状埃络石负载二氧化钛材料，研究并总结了其光催化氧化等性能；研究制备了稀土配位聚合物等二维结纳米结构材料的制备及其在电催化氧化等领域的应用。本项目所研发的一系列材料体系、制备工艺和学术成果，具有较高的创新性和启发性。部分研究成果发表在相关领域国际顶级和一流权威期刊上，获得同行广泛好评。为新型无机类石墨烯结构材料的研发及其在催化领域的应用提供科学依据。