Atomically Precise Preorganization of Open Metal Sites on Gold Nanoclusters with High Catalytic Performance,Angewandte Chemie International Edition

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Atomically Precise Preorganization of Open Metal Sites on Gold Nanoclusters with High Catalytic Performance
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-12-01 , DOI: 10.1002/anie.202012499
Shang‐Fu Yuan _{1,

2} , Zhen Lei ₁ , Zong‐Jie Guan ₁ , Quan‐Ming Wang _{1,

2}

Affiliation

Gold nanoclusters with surface open sites are crucial for practical applications in catalysis. We have developed a surface geometric mismatch strategy by using mixed ligands of different type of hindrance. When bulky phosphine Ph₃P and planar dipyridyl amine (Hdpa) are simultaneously used, steric repulsion between the ligands will reduce the ligand coverage of gold clusters. A well‐defined access granted gold nanocluster [Au₂₃(Ph₃P)₁₀(dpa)₂Cl](SO₃CF₃)₂ (Au₂₃, dpa=dipyridylamido) has been successfully synthesized. Single crystal structural determination reveals that Au₂₃ has eight uncoordinated gold atoms in the shape of a distorted bicapped triangular prism. The accessibility of the exposed Au atoms has been confirmed quantitatively by luminescent titration with 2‐naphthalenethiol. This cluster has excellent performance toward selective oxidation of benzyl alcohol to benzaldehyde and demonstrates excellent stability due to the protection of negatively charged multidentate ligand dpa.

中文翻译：

具有高催化性能的金纳米团簇上开放金属位点的原子精确预组织

具有表面开放位点的金纳米簇对于催化的实际应用至关重要。我们已经通过使用不同类型障碍的混合配体开发了表面几何失配策略。当同时使用庞大的膦Ph ₃ P和平面二吡啶胺（Hdpa）时，配体之间的空间排斥会降低金簇的配体覆盖率。已成功合成了定义明确的准入许可的金纳米簇[Au ₂₃（Ph ₃ P）₁₀（dpa）₂ Cl]（SO ₃ CF ₃）₂（Au ₂₃，dpa = dipyridylamido）。单晶结构测定表明金₂₃具有扭曲的二尖形三棱柱形状的八个未配位的金原子。暴露的金原子的可及性已经通过2-萘硫醇的发光滴定进行了定量确认。该簇具有优异的苯甲醇选择性氧化为苯甲醛的性能，并由于保护带负电荷的多齿配体dpa而显示出极好的稳定性。

更新日期：2020-12-01

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