Matching Bidentate Ligand Anchoring: an Accurate Control Strategy for Stable Single-Atom/ZIF Nanocatalysts,Advanced Materials

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Matching Bidentate Ligand Anchoring: an Accurate Control Strategy for Stable Single-Atom/ZIF Nanocatalysts
Advanced Materials ( IF 27.4 ) Pub Date : 2022-12-08 , DOI: 10.1002/adma.202209561
Yapei Yun ₁ , Haitao Zeng ₂ , Lin Li ₁ , Haifeng Li ₁ , Shen Cheng ₁ , Ningning Sun ₁ , Meng Li ₁ , Hongting Sheng ₁ , Shuxian Hu ₃ , Tao Yao ₂ , Manzhou Zhu ₁

Affiliation

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.

中文翻译：

匹配双齿配体锚定：稳定单原子/ZIF 纳米催化剂的精确控制策略

对于单原子催化剂 (SAC) 而言，提高金属负载量和控制配位环境并非易事且具有挑战性，因为单原子催化剂具有最高的原子效率和最多的界面位点。在这项研究中，设计了一种匹配的双齿配体 (MBL) 锚定策略来构建 CuN ₄具有可调协调环境的 SAC（Cu 负载范围从 0.4 到 15.4 wt.%）。获得的 Cu SA/ZIF 和 Cu SA/ZIF* （0.4 wt.%）（ZIF 和 ZIF* = 具有匹配双齿 N-配体的沸石咪唑酯骨架）纳米复合材料在光照射下苯乙炔的自偶联方面表现出优异的性能（TON = 580，选择性 > 99%），比 Cu SA/NC-800（NC = N 掺杂多孔碳）高 22 倍。实验和密度泛函理论计算证实，使用MBL锚定策略形成的特定Cu五元环是固定孤立Cu原子的关键。该策略为构建 M SA/MOF 提供了基础，有可能缩小实验催化和理论催化之间的差距，

更新日期：2022-12-08

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