材料科学
纳米材料基催化剂
沸石咪唑盐骨架
催化作用
配体(生物化学)
齿合度
纳米技术
Atom(片上系统)
密度泛函理论
金属有机骨架
结晶学
物理化学
吸附
计算化学
金属
有机化学
计算机科学
冶金
嵌入式系统
受体
生物化学
化学
作者
Yapei Yun,Haitao Zeng,Lin Li,Haifeng Li,Cheng Shen,Ningning Sun,Meng Li,Hongting Sheng,Shu‐Xian Hu,Tao Yao,Manzhou Zhu
标识
DOI:10.1002/adma.202209561
摘要
Improving metal loading and controlling the coordination environment is nontrivial and challenging for single-atom catalysts (SACs), which have the greatest atomic efficiency and largest number of interface sites. In this study, a matching bidentate ligand (MBL) anchoring strategy is designed for the construction of CuN4 SACs with tunable coordination environments (Cu loading range from 0.4 to15.4 wt.%). The obtained Cu SA/ZIF and Cu SA/ZIF* (0.4 wt.%) (ZIF and ZIF* = Zeolitic imidazolate framework with Matching bidentate N-ligands) nanocomposites exhibit superior performance in homo-coupling of phenyl acetylene under light irradiation (TON = 580, selectivity > 99%), which is 22 times higher than that of Cu SA/NC-800 (NC = N-doped porous carbon). Experiments and density functional theory calculations confirmed that the specific Cu five-membered ring formed using the MBL anchoring strategy is the key to the immobilization of isolated Cu atoms. This strategy provides a basis for the construction of M SA/MOF, which has the potential to narrow the gap between experimental and theoretical catalysis, as further confirmed by the successful preparation of Fe SA/ZIF and Ni SA/ZIF.
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