Jianhua Liu, Diru Liu, Qi An, Tingxu Chen, Yunbo Yu, Guangyan Xu, Hong He
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引用次数: 0
摘要
汽车和发电厂排放的氨引起了严重的环境问题。本文研究了不同还原性氧化物负载的铂和铱催化剂在氨选择性催化氧化中的作用。弱金属-载体相互作用(MSI)导致不可还原Al2O3上形成金属纳米颗粒,而强金属-载体相互作用(SMSI)诱导可还原CeO2上形成单原子金属。值得注意的是,MSI对Pt基催化剂(Pt/Al2O3∶Pt/TiO2 >;Pt/CeO2)和Ir基催化剂(Ir/CeO2 >;Ir/TiO2 > Ir/Al2O3)。Pt/Al2O3表面的金属Pt纳米粒子活化了气态O2,促进了低温NH3氧化。相反,在Ir/CeO2催化剂上,单原子Ir- o - ce位点以极低的能垒对NH3裂解表现出很高的反应活性,从而具有优异的低温活性。本研究提供了控制MSI效应来调节负载型催化剂活性位点的结构,从而提高其催化性能的见解。
Reverse effect of metal-support interaction on platinum and iridium catalysts in ammonia selective oxidation
Ammonia emissions from vehicles and power plants cause significant environmental concerns. Here, a range of platinum and iridium catalysts supported on oxides with various levels of reducibility were investigated in ammonia selective catalytic oxidation. Weak metal-support interaction (MSI) led to the formation of metal nanoparticles on irreducible Al2O3, whereas strong MSI (SMSI) induced the generation of single-atom metals on reducible CeO2. Notably, MSI demonstrated opposite effects on the catalytic performance of Pt-based catalysts (Pt/Al2O3 ≫ Pt/TiO2 > Pt/CeO2) and Ir-based catalysts (Ir/CeO2 > Ir/TiO2 ≫ Ir/Al2O3). Metallic Pt nanoparticles on Pt/Al2O3 activated gaseous O2 and promoted the low-temperature NH3 oxidation. Conversely, on Ir/CeO2 catalysts, the single-atom Ir-O-Ce site demonstrated high reactivity for NH3 cleavage with an extremely low energy barrier, contributing to the superior low-temperature activity. This study provides insights into governing the MSI effect to regulate the structure on active sites of supported catalysts, thereby enhancing their catalytic performance.
期刊介绍:
Chem Catalysis is a monthly journal that publishes innovative research on fundamental and applied catalysis, providing a platform for researchers across chemistry, chemical engineering, and related fields. It serves as a premier resource for scientists and engineers in academia and industry, covering heterogeneous, homogeneous, and biocatalysis. Emphasizing transformative methods and technologies, the journal aims to advance understanding, introduce novel catalysts, and connect fundamental insights to real-world applications for societal benefit.