覆盖层
催化作用
氧化物
钯
氧气
金属
密度泛函理论
材料科学
反应性(心理学)
吸附
化学工程
无机化学
化学
物理化学
冶金
计算化学
有机化学
医学
替代医学
病理
工程类
作者
Jingkun Chen,Yuetan Su,Qingjie Meng,Hehe Qian,Le Shi,Jawwad A. Darr,Zhongbiao Wu,Xiaole Weng
标识
DOI:10.1002/anie.202310191
摘要
The development of oxidation catalysts that are resistant to sulfur poisoning is crucial for extending the lifespan of catalysts in real-working conditions. Herein, we describe the design and synthesis of oxide-metal interaction (OMI) catalyst under oxidative atmospheres. By using organic coated TiO2 , an oxide/metal inverse catalyst with non-classical oxygen-saturated TiO2 overlayers were obtained at relatively low temperature. These catalysts were found to incorporate ultra-small Pd metal and support particles with exceptional reactivity and stability for CO oxidation (under 21 vol % O2 and 10 vol % H2 O). In particular, the core (Pd)-shell (TiO2 ) structured OMI catalyst exhibited excellent resistance to SO2 poisoning, yielding robust CO oxidation performance at 120 °C for 240 h (at 100 ppm SO2 and 10 vol % H2 O). The stability of this new OMI catalyst was explained through density functional theory (DFT) calculations that interfacial oxygen atoms at Pd-O-Ti sites (of oxygen-saturated overlayers) serve as non-metal active sites for low-temperature CO oxidation, and change the SO2 adsorption from metal(d)-to-SO2 (π*) back-bonding to much weaker σ(Ti-S) bonding.
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