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Cooperative Catalysis of Methane Oxidation through Modulating the Stabilization of PdO and Electronic Properties over Ti-Doped Alumina-Supported Palladium Catalysts

机译:通过调节PDO和电子性质在Ti掺杂氧化铝支持的钯催化剂中的稳定化的协同催化

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Poor low-temperature catalytic activity and durability are the main drawbacks of palladium-based catalysts for methane combustion. Herein, stable and active PdO particles are constructed by incorporating Ti into an alumina support, which makes the catalysts exhibit satisfactory methane combustion activity. The results of comprehensive characterization reveal that an appropriate amount of Ti doping induces the optimization of electron transfer and distribution, thus contributing to the construction and stabilization of active PdO lattices. The reactive oxygen mobility is improved and the optimal PdO/Pd0 combination is achieved, thanks to the amplified PdO–support interaction. In addition, the acid–base properties are regulated and Br?nsted acid sites are generated by virtue of the adjustment of electronic properties, which facilitate stabilization of PdO as well. Hence, the Ti-containing catalyst exhibits superior activity for methane oxidation at low temperatures. Notably, the activity and cyclic performance of the catalyst can be further enhanced when undergoing long-term and isothermal heat treatment under the reactant stream and methane, and it demonstrates a high performance with 90% CH4 conversion at 340 °C.
机译:低温催化活性和耐久性差是甲烷燃烧的钯基催化剂的主要缺点。这里,通过将Ti掺入氧化铝载体中构建稳定和活性的PDO颗粒,这使得催化剂表现出令人满意的甲烷燃烧活性。全面表征的结果表明,适量的Ti掺杂诱导电子转移和分布的优化,从而有助于施工和稳定性的活性PDO格子。由于扩增的PDO - 载体相互作用,改善了活性氧迁移率,并且达到了最佳PDO / PD0组合。此外,酸碱性质是调节的,并且通过调节电子性质的调节产生Brαnsted酸部位,这促进了PDO的稳定性。因此,含Ti的催化剂在低温下表现出甲烷氧化的优异活性。值得注意的是,当在反应物流和甲烷下经历长期和等温热处理时,可以进一步提高催化剂的活性和循环性能,并在340℃下表明具有90%CH 4转化率的高性能。

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