单原子Pd-基催化剂室温氧化甲醛的研究

Formaldehyde (HCHO), a major indoor air pollutant in airtight houses, is detrimental to human health. Supported noble metal (Pt, Au and Pd) catalysts exhibit excellent activity for catalytic oxidation of HCHO at low and even room temperature, but their high cost restricts their wide application. Compared with Pt and Au, Pd possess cost advantage. However, there still are some disadvantages for the Pd based catalyst that show excellent performance of HCHO oxidation at ambient temperature, that is, relatively high loading and poor dispersion of Pd. Based on our previous studies, the current work will exploit single atom Pd based catalyst through tuning morphology and concentration of oxygen vacancies on some oxide supports and combining relative synthesis and post treatment methods. Then, the interaction between single Pd atom and the supports will be investigated. In addition, multiple characterization methods will be used for establishing the structure-activity relationship of Pd-based catalysts in HCHO oxidation reaction and clarifying the reaction mechanism of HCHO oxidation，which will be helpful for the improvement of the catalysts. The current work will be meaningful and valuable to exploit new-typed, efficient and low-cost catalysts in the future.

甲醛是室内最典型的污染物之一，对人体健康具有严重危害。负载贵金属(Pt、Au、Pd)催化剂在室温下表现出优异的甲醛降解性能，然而高成本限制了其广泛应用。相对于Pt和Au，Pd具有成本优势，但目前具有室温降解甲醛能力的Pd-基催化剂Pd负载量较高且分散度较低。本项目拟在前期的研究基础上，通过调控氧化物载体表面氧空位的形态和浓度，并结合相应的制备方法和后处理方式，以期开发出可在室温下高效催化氧化甲醛的单原子Pd-基催化剂，明确单原子Pd与载体之间的作用方式，进一步阐明Pd-基催化剂的构效关系及其氧化甲醛反应机理，指导高性能催化剂的设计。本项目可为开发新型、高效、低成本的催化材料提供科学依据和技术储备，具有重要的科学价值和实际意义。

甲醛是室内最典型的污染物之一，对人体健康具有严重危害。负载贵金属(Pt、Au、Pd)催化剂在室温下表现出优异的甲醛降解性能，然而高成本限制了其广泛应用。因此，我们通过高温还原的方式处理Pd/TiO2催化剂，调控Pd与TiO2之间的强相互作用，提高了Pd的分散度，构筑了高效活化水和氧的活性中心。通过多种表征手段，阐明了高温还原处理的Pd/TiO2催化剂室温氧化甲醛的构效关系，并明确了甲醛在Pd/TiO2催化剂上的反应路径。进一步通过微观调控TiO2载体上的缺陷浓度，明确了载体缺陷在物理结构上具有稳定Pd颗粒的作用，在电子结构上具有电子传递作用，并能高效活化水和氧形成表面羟基。本项目可为开发新型、高效、低成本的催化材料提供科学依据和技术储备，具有重要的科学价值和实际意义。