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通过金属有机框架实现增强催化,在调节的微环境中清洁表面的纳米集群

He Wang¹, Xiyuan Liu¹, Weijie Yang²

¹Department of Chemistry, University of Science and Technology of China, Hefei, Anhui230026, P. R. China.

Journal of the American Chemical Society

|November 21, 2022

概括

在金属有机框架 (MOF) 中稳定的表面纯金纳米集群 (Au25NCs) 显示出增强的催化活性和furfural氧化稳定性. 在MOF孔壁上的功能组调整集群电子,优化性能.

科学领域:

材料科学
催化剂
纳米技术

背景情况:

由于其精确的原子结构,金属纳米集群 (NC) 是有前途的催化剂.
挑战包括NC聚合和配体干扰,限制它们的催化应用.

研究的目的:

使用金属有机框架 (MOF) 稳定表面清洁的金纳米集群 (Au25NC).
在furfural的氧化化中研究这些稳定NC的催化性能.
了解MOF功能组如何影响NC电子状态和催化活性.

主要方法:

封装Au25NCs成异构型MOF (UiO-66-X,其中X=H,NH2,OH,NO2).
从封装的Au25NC中去除表面连接物.
在furfural氧化化的催化活性和稳定性的评估.
实验和理论研究 (例如,DFT) 来分析电子结构和吸附能量.

主要成果:

与原始Au25NC相比,封装在MOF中的表面清洁Au25NC具有更高的活性和稳定性.
在UiO-66-X孔壁上的功能组调节了Au25NC的电子状态.
催化活性与电子密度和基质吸附能量相关,遵循趋势:Au25@UiO-66-NH2 > Au25@UiO-66-OH > Au25@UiO-66 > Au25@UiO-66-NO2.

结论:

MOF的空间限制有效地稳定了表面清洁的金属NC,防止聚合.
MOF的孔壁工程提供了一种多功能策略,用于调整封装NC的电子特性,以增强催化作用.
这种方法为设计高活性和稳定的NC基催化剂提供了新的途径.

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