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在NU-1000金属有机框架中稳定Cu-Oxo集群催化甲氧化成甲醇
Takaaki Ikuno1, Jian Zheng2, Aleksei Vjunov2
1Department of Chemistry and Catalysis Research Institute, Technische Universität München , 85748 Garching, Germany.
Journal of the American Chemical Society
|June 15, 2017
概括
在金属有机框架 (MOF) 中的氧化铜集群有效地将甲转化为甲醇. 这种基于MOF的催化剂在温和条件下有望选择性氧化甲.
科学领域:
- 催化剂
- 材料科学
- 化学工程
背景情况:
- 在化学中,选择性氧化甲以甲醇是一个关键的挑战.
- 金属有机框架 (MOF) 为催化应用提供可调节的结构.
- NU-1000是一个MOF,有可能容纳活跃的催化物种.
研究的目的:
- 在NU-1000上为甲氧化合成和描述氧化铜集群.
- 研究Cu-NU-1000催化系统中的结构活动关系.
- 评估以MOF为基础的甲转化催化剂的选择性和活性.
主要方法:
- 在NU-1000上合成氧化铜集群的原子层沉积 (ALD).
- 在现场X射线吸收光谱 (XAS) 探测铜物种.
- 密度函数理论 (DFT) 计算用于机械洞察.
- 化学反应性分析以确定产品的分布.
主要成果:
- 在NU-1000上成功固定了由几个铜原子组成的氧化铜集群.
- 在环境条件下,催化剂表现出Cu+和Cu2+氧化状态的混合物.
- 甲氧化导致Cu2+部分减少为Cu+.
- -NU-1000催化剂在甲醇生产中显示出45-60%的碳选择性.
- 产品在135°C时使用水/进行脱离.
结论:
- 在NU-1000框架内稳定的氧铜集群对选择性甲氧化具有活性.
- 这代表了第一代基于MOF的催化剂.
- 这项研究阐明了控制催化过程的结构活动关系.
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