How the Morphology of NiOx-Decorated CeO2 Nanostructures Affects Catalytic Properties in CO2 Methanation,Langmuir

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How the Morphology of NiOx-Decorated CeO2 Nanostructures Affects Catalytic Properties in CO2 Methanation
Langmuir ( IF 3.7 ) Pub Date : 2021-04-21 , DOI: 10.1021/acs.langmuir.1c00546
Naoki Hashimoto ₁ , Kohsuke Mori _{1,

2,

3} , Kohei Asahara ₁ , Shun Shibata ₁ , Hirotaka Jida ₁ , Yasutaka Kuwahara _{1,

2,

3,

4} , Hiromi Yamashita _{1,

2,

3}

Affiliation

Effects of morphology and exposed crystal planes of NiO_x-decorated CeO₂ (NiCeO₂) nanostructured catalysts on activity during CO₂ methanation were examined, using nanorod (NR), nanocube (NC), and nanooctahedron (NO) structures. The NiCeO₂ nanorods (NiCeO₂-NR) showed superior activity to NiCeO₂-NC and NiCeO₂-NO along with excellent selectivity for CH₄. This material also demonstrated exceptional durability, with no significant loss of catalytic activity or structural change after use. Comprehensive physicochemical characterization as well as density functional theory calculations determined that the high performance of the NiCeO₂-NR was closely related to the large quantity of surface oxygen vacancies and the high degree of reversibility associated with the Ce⁴⁺ ↔ Ce³⁺ redox cycle of the support. These effects originate from the enhanced reactivity of oxygen atoms on the (110) surfaces of the oxide compared with the (100) and (111) surfaces. This information is expected to assist in the rational design of practical catalysts for the activation of CO₂ molecules and other important transformations.

中文翻译：

NiO _x修饰的CeO ₂纳米结构的形貌如何影响CO ₂甲烷化中的催化性能

使用纳米棒（NR），纳米立方体（NC）和纳米八面体（NO）结构，研究了NiO _x修饰的CeO ₂（NiCeO ₂）纳米结构催化剂的形态和裸露晶面对CO ₂甲烷化活性的影响。NiCeO ₂纳米棒（NiCeO ₂ -NR）表现出优于NiCeO ₂ -NC和NiCeO ₂ -NO的活性，并且对CH ₄具有出色的选择性。。该材料还显示出卓越的耐久性，使用后不会显着降低催化活性或结构变化。综合理化特性和密度泛函理论计算确定，NiCeO ₂ -NR的高性能与大量的表面氧空位以及与Ce ⁴⁺ ↔Ce ³⁺氧化还原循环相关的高度可逆性密切相关的支持。这些效应源自与（100）和（111）表面相比，氧化物（110）表面上的氧原子增强的反应性。预计该信息将有助于合理设计用于CO ₂活化的实用催化剂分子和其他重要的转变。

更新日期：2021-05-04

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