CeO2 纳米结构中氧空位在催化好氧环己烷氧化中的作用,ACS Applied Nano Materials

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CeO2 纳米结构中氧空位在催化好氧环己烷氧化中的作用
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2023-07-21 , DOI: 10.1021/acsanm.3c02147
Yingwei Li _{1,

2} , Hao Li _{1,

2} , Kexin Li _{1,

2} , Ruirui Wang _{1,

2} , Ruirui Zhang _{1,

2} , Ruixia Liu _{1,

2}

Affiliation

纳米结构铈基催化材料由于纳米晶体表面暴露出优异的活性位点，在氧化还原催化领域备受关注，其中典型模型纳米结构二氧化铈的氧空位（O V ）和晶面_效应（纳米CeO ₂ )被重点研究用于催化需氧环己烷氧化。特别是对于具有{100}面的CeO _{2纳米立方体、具有主导{111}面的CeO}₂纳米多面体和具有主导{110}面的CeO ₂纳米棒，O _V和酸性位点对环己烷的催化作用氧化作用进行了系统的研究。表面氧空位（Sur-O _V）和固有氧空位（Int-O _V），特别是在环己烷氧化特有的工作状态下发挥催化活性的活性Sur-O _V和活性Int-O _{V ，被准确识别和区分。}_{此外，还揭示了O V}位点将分子氧活化成活性氧物种（O _Active ）的活化能力，并对酸位点特性（包括酸度和酸位点类型）进行了探测和定量。具有暴露的{100}面的Nano-CeO ₂拥有最活跃的Sur-O _V，决定催化活性，具有最强的活化能力，有助于在极惰性条件下保持高反应活性。具有{110}主晶面的纳米CeO ₂具有最活跃的Int-O _V和丰富的酸位点，可以加速进一步氧化为己二酸；_{两个关键位点的影响特别通过α因子（=总酸度×活性Int-O V}量）来描述。最后，基于纳米CeO ₂催化体系推测了环己烷氧化的性能关系。

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Roles of Oxygen Vacancies in CeO2 Nanostructures for Catalytic Aerobic Cyclohexane Oxidation

Nanostructured cerium-based catalytic materials have attracted much attention in the field of redox catalysis, due to the excellent active sites exposed on the nanocrystal surface, and herein, the oxygen vacancy (O_V) and the crystal facet effect of typical model nanostructured ceria (Nano-CeO₂) were focused and investigated for the catalytic aerobic cyclohexane oxidation. Specifically for the CeO₂ nanocubes with a {100} facet, the CeO₂ nanopolyhedrons with a dominant {111} facet, and the CeO₂ nanorods with a dominant {110} facet, the catalytic roles of the O_V and acid sites toward cyclohexane oxidation were systematically investigated. Surface oxygen vacancy (Sur-O_V) and intrinsic oxygen vacancy (Int-O_V), and particularly the active Sur-O_V and active Int-O_V performing catalytic activity under a working state specific for cyclohexane oxidation, were accurately recognized and distinguished. Furthermore, the activation ability of the O_V sites for activating molecular oxygen into active oxygen species (O_Active) was also revealed, and the acid site properties, which include the acidity and the types of acid sites, were probed and quantified. The Nano-CeO₂ with an exposed {100} facet possesses the most active Sur-O_V, determining the catalytic activity, and has the strongest activation ability, contributing to a high reaction activity under extremely inert conditions. The Nano-CeO₂ with a {110} dominant facet with the most active Int-O_V and abundant acid sites could accelerate further oxidation to adipic acid; the effect of the two key sites was described particularly by the α factor (= Total Acidity × Amount of Active Int-O_V). Finally, the property–performance relationship toward cyclohexane oxidation was speculated based on the Nano-CeO₂ catalytic system.

更新日期：2023-07-21

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