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- 2015
Pd/CeO2催化CO氧化活性对载体CeO2形貌的依赖效应
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Abstract:
摘要 Pd纳米颗粒的氧化还原性能对Pd/CeO2催化氧化反应的性能至关重要,且与Pd-CeO2的界面结构密切相关.我们发现Pd/CeO2的低温催化CO氧化活性高度依赖于载体CeO2的形貌和暴露晶面.利用胶体沉积法,得到Pd/CeO2八面体和Pd/CeO2立方块两种催化剂.结果表明暴露{111}晶面的CeO2八面体负载Pd催化剂的催化CO氧化活性远优于暴露{100}晶面的CeO2立方块负载Pd催化剂.DFT理论模拟计算结果表明,催化剂表面的Pd物种的氧化还原活性可能决定催化剂的可还原性和催化活性:钯从氧化态到金属态的循环更容易在CeO2(111)上进行,而这取决于Pd与载体CeO2之间的相互作用.我们的结果表明,催化剂表面活性Pd物种的氧化还原性能对Pd/CeO2的催化活性至关重要,可以通过调控载体暴露的晶面实现Pd与载体CeO2之间的相互作用,最终实现对催化剂可还原性和催化活性的可控调变.
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