Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal–Organic Framework,Journal of the American Chemical Society

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Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal–Organic Framework
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2017-07-17 , DOI: 10.1021/jacs.7b02936
Takaaki Ikuno ₁ , Jian Zheng ₂ , Aleksei Vjunov ₂ , Maricruz Sanchez-Sanchez ₁ , Manuel A. Ortuño ₃ , Dale R. Pahls ₃ , John L. Fulton ₂ , Donald M. Camaioni ₂ , Zhanyong Li ₄ , Debmalya Ray ₃ , B. Layla Mehdi ₂ , Nigel D. Browning _{2,

5} , Omar K. Farha _{4,

6} , Joseph T. Hupp ₄ , Christopher J. Cramer ₃ , Laura Gagliardi ₃ , Johannes A. Lercher _{1,

2}

Affiliation

Copper oxide clusters synthesized via atomic layer deposition on the nodes of the metal-organic framework (MOF) NU-1000 are active for oxidation of methane to methanol under mild reaction conditions. Analysis of chemical reactivity, in situ X-ray absorption spectroscopy, and density functional theory calculations are used to determine structure/activity relations in the Cu-NU-1000 catalytic system. The Cu-loaded MOF contained Cu-oxo clusters of a few Cu atoms. The Cu was present under ambient conditions as a mixture of ∼15% Cu+ and ∼85% Cu2+. The oxidation of methane on Cu-NU-1000 was accompanied by the reduction of 9% of the Cu in the catalyst from Cu2+ to Cu+. The products, methanol, dimethyl ether, and CO2, were desorbed with the passage of 10% water/He at 135 °C, giving a carbon selectivity for methane to methanol of 45-60%. Cu oxo clusters stabilized in NU-1000 provide an active, first generation MOF-based, selective methane oxidation catalyst.

中文翻译：

由稳定在 NU-1000 金属-有机框架中的 Cu-Oxo 簇催化甲烷氧化为甲醇

通过在金属有机框架 (MOF) NU-1000 节点上的原子层沉积合成的氧化铜簇在温和的反应条件下对甲烷氧化为甲醇具有活性。化学反应性分析、原位 X 射线吸收光谱和密度泛函理论计算用于确定 Cu-NU-1000 催化体系中的结构/活性关系。负载铜的 MOF 包含几个铜原子的铜氧簇。在环境条件下，Cu 以~15% Cu+ 和~85% Cu2+ 的混合物形式存在。甲烷在 Cu-NU-1000 上的氧化伴随着催化剂中 9% 的 Cu 从 Cu2+ 还原为 Cu+。产物甲醇、二甲醚和 CO2 在 135°C 下通过 10% 的水/He 解吸，使甲烷对甲醇的碳选择性为 45-60%。

更新日期：2017-07-17

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