催化作用
氧化物
化学工程
介孔材料
多相催化
铁
材料科学
烧结
铁质
吸附
金属
密度泛函理论
纳米技术
无机化学
化学
钯
过渡金属
纳米颗粒
贵金属
物理化学
计算化学
冶金
工程类
生物化学
作者
Jixing Liu,Lu Wang,Francis Okejiri,Jing Luo,Jiahua Zhao,Pengfei Zhang,Miaomiao Liu,Shize Yang,Zihao Zhang,Weiyu Song,Wenshuai Zhu,Zhen Zhao,Guodong Feng,Xu Chen,Sheng Dai
标识
DOI:10.1021/acscatal.0c01447
摘要
Tuning the atomic interface configuration of noble metals (NMs) and transition-metal oxides is an effective straightforward yet challenging strategy to modulate the activity and stability of heterogeneous catalysts. Herein, Pd supported on mesoporous Fe2O3 with a high specific surface area was rationally designed and chosen to construct the Pd/iron oxide interface. As a versatile model, the physicochemical environments of Pd nanoparticles (NPs) could be precisely controlled by taming the reduction temperature. The experimental and density functional theory calculation results unveiled that the catalyst in the support–metal interface confinement (SMIC) state showed significantly enhanced catalytic activity and sintering resistance for CO oxidation. The constructed Fe sites at the interfaces between FeOx overlayers and Pd NPs not only provided additional coordinative unsaturated ferrous sites for the adsorption and activation of O2, thereby facilitating the activation efficiency of O2, but also impressively changed the reaction pathway of CO oxidation. As a result, the catalyst followed the Pd/Fe dual-site mechanism instead of the classical Mars–van Krevelen mechanism. For the catalyst in the strong metal–support interaction (SMSI) state, its catalytic activity was seriously suppressed because of the excessive encapsulation of the active Pd sites by FeOx overlayers. The present study therefore provides detailed insights into the SMIC and SMSI in ferric oxide-supported Pd catalysts, which could guide the preparation of highly efficient supported catalysts for practical applications.
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