Heterobimetallic Metal-organic Framework Nanocages as Highly Efficient Catalysts for CO2 Conversion under Mild Conditions
Heterobimetallic Metal-organic Framework Nanocages as Highly Efficient Catalysts for CO2 Conversion under Mild Conditions
复制标题
异双金属金属有机框架纳米笼作为温和条件下二氧化碳转化的高效催化剂
DOI：
10.1039/c7ta09082j
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发表时间：
2018
影响因子：
11.9
通讯作者：
Jiang Zhongyi
中科院分区：
文献类型：
--
作者：
Tang Lei;Zhang Shengbo;Wu Qilong;Wang Xinru;Wu Hong;Jiang Zhongyi
设计和制造高活性、稳定的CO2转化催化剂具有重要意义。本文通过调控金属有机骨架（MOF）纳米晶体的结构演化，合成了一种新型多孔杂双金属催化剂。起始材料为同金属ZIF-8纳米颗粒，在溶液中通过与Au3+离子的阳离子交换转化为有利于活性位点增强的异质金属Au/Zn-MOF纳米笼。以正六面体（RH） ZIF-8和菱形十二面体（RD） ZIF-8纳米颗粒为模板，分别制备了壳厚可控的RH和RD型Au/Zn-MOF纳米笼。制备的Au/Zn-MOF纳米笼在温和的反应条件下催化CO2和环氧化物的环加成。由于Au/Zn-MOF两种金属组分的协同作用和独特的空心结构，其催化性能优于大多数mof基催化剂和均相Au催化剂，产率高达95-99%，且易于回收。令人印象深刻的是，即使在室温和常压下，这些Au/Zn-MOF纳米笼也表现出显著的二氧化碳转化催化活性。因此，这些纳米材料在制备方便、丰富的多活性位点以及增强的催化活性和稳定性方面，作为二氧化碳转化的催化剂具有很大的前景。
It is of critical importance to design and fabricate highly active and stable catalysts for CO2 conversion. Herein, we synthesize a kind of novel porous heterobimetallic catalyst by manipulating the structural evolution of metal–organic framework (MOF) nanocrystals. The starting material, homometallic ZIF-8 nanoparticles, transforms in solution by cation exchange with Au3+ ions into heterobimetallic Au/Zn-MOF nanocages that favor the enhancement of active sites. With the use of regular hexahedral (RH) ZIF-8 and rhombic dodecahedral (RD) ZIF-8 nanoparticles as the templates, we obtain RH and RD Au/Zn-MOF nanocages with controllable shell thickness, respectively. The resulting Au/Zn-MOF nanocages are employed to catalyze the cycloaddition of CO2 and epoxides under mild reaction conditions. The excellent catalytic performance is demonstrated by high yields of 95–99% along with easy recyclability of the Au/Zn-MOF nanocages, which outperform most of the reported MOF-based catalysts and a homogeneous Au catalyst due to the synergetic effect of the two metallic components and the unique hollow structures. Impressively, these Au/Zn-MOF nanocages exhibit remarkable catalytic activity for CO2 conversion even at room temperature and atmospheric pressure. These nanomaterials thus hold great promise as catalysts for CO2 conversion in terms of facile preparation, abundant multiple active sites, and enhanced catalytic activity and stability.