Pt/BN催化剂表面Pt物种的指认及其丙烷完全氧化性能和反应机理研究

Catalytic combustion is a promising technology for the abatement of volatile organic compounds, and the understanding of reaction mechanism is crucial for the development of highly efficient catalyst systems. It was found that supported Pt/BN catalysts were very effective for catalytic combustion of propane. However, key issues such as active species and reaction mechanism need to be clarified. Therefore, in this project, we plan to design a series of Pt/BN catalysts for propane combustion. With detailed characterizations such as XPS and HRTEM, surface Pt species (e.g. Pt0, Ptn+, Pt0-Ptn+) could be distinguished and their contributions in the reaction could be illustrated, which is helpful to clarify the active sites for the reaction. In addition, we plan to distinguish the nature of the Pt species on different locations of BN support (e.g. surface and edge) and their relation with the catalytic behaviors, as well as investigations on reaction intermediates and reaction pathways, which is helpful to establish a clear picture on the structure - performance correlation. The findings of this project may provide useful information for the development of high performance catalysts for propane combustion, and thus have great academic and practical value. Also, the rich academic backgroud and the early research results of the applicant ensure the successful completion of this project.

催化燃烧是一种处理VOCs的高效净化技术，认识催化剂的VOCs完全氧化作用机制，是研发高性能催化剂的关键。研究发现Pt/BN催化剂具有很高的丙烷氧化活性，但是对催化反应活性位、反应机理都缺乏完整的认识。本项目通过设计、制备系列Pt/BN催化剂，结合XPS、HRTEM等表征，指认和区分催化剂表面Pt粒子的Pt0、Ptn+（Pt2+、Pt4+）和Pt0-Ptn+物种，及其对丙烷完全氧化反应的贡献，明确Pt/BN催化剂的反应活性中心；研究BN纳米片表面、棱边上Pt粒子和Pt物种差异与催化性能之间的关系，结合丙烷氧化过程中间产物、吸附态、反应历程等问题的研究，建立清晰全面的表面Pt物种与催化性能的关系，认识影响反应行为的关键因素和反应机理，为进一步提高催化性能提供实验和理论支撑。申请者丰富的研究积累和前期探索性研究，为本项目的顺利完成提供了扎实的基础。

VOCs包含烃类、芳烃、酯类、酮类、醇类等有机物。在VOCs体系中，烷烃化学性质最稳定，是最难催化燃烧的一类有机物，也是VOCs催化燃烧中最具代表性的物质。含烷烃的VOCs存在于涂料、油气加工、柴油机尾气、F-T合成尾气等领域。因此，催化燃烧是处理VOCs的高效净化技术，认识VOCs催化剂作用机制，是研发高性能催化剂的关键。.本项目通过对系列Pt/BN、Pt-V/BN、Pt-W/BN表征和丙烷氧化反应活性测试，指认Pt/BN催化剂表面Pt存在形式，区分Pt0、Ptn+（Pt2+、Pt4+）物种对丙烷氧化反应的贡献，确认Pt0/Ptn+比例与反应活性（TOF）的关系，明确Pt粒子尺寸对表面Pt0-Ptn+物种比例及丙烷氧化活性（TOFPt）的影响。还开展了Pt-MoO3、Pt-WO3、Pt-NbOx界面和表面酸性对催化剂丙烷氧化性能的影响。结合丙烷氧化过程中间产物、吸附态、反应历程等问题的研究，建立清晰全面的Pt表面物种状态与催化性能的关系。明确了Pt0/Ptn+物种比例与催化剂表面酸性与催化剂的丙烷氧化活性之间的关系。为VOCs中的烷烃催化燃烧奠定了基础。.项目完成研究论文16，授权专利2件，还有2件发明专利在审理中。培养研究生6名。