N-heterocyclic carbene-functionalized magic-number gold nanoclusters

N-heterocyclic carbene-functionalized magic-number gold nanoclusters
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DOI:
10.1038/s41557-019-0246-5
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发表时间:
2019-05-01
期刊:
影响因子:
21.8
通讯作者:
Crudden, Cathleen M.
Crudden, Cathleen M.
中科院分区:
化学1区
文献类型:
--
作者:
Narouz, Mina R.;Osten, Kimberly M.;Crudden, Cathleen M.

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魔数金纳米团簇是原子上精确的纳米材料,在纳米科学中对结构-性质关系的研究是前所未有的。硫酸盐是最常见的配体,通过一个只有中心金原子处于金属状态的主基序结合到簇上。缺乏其他具有不同键合模式的纳米簇强结合配体是该领域的重大限制。在这里,我们报道了一种以前未知的金(0)纳米簇的配体——n -杂环碳烯(NHCs)——它具有强大的金属-碳单键,并赋予相应的金簇高稳定性。在金纳米团簇中加入单个NHC可显著改善其稳定性和电催化还原CO2的催化性能。通过改变NHC的条件,性质和等价物的数量,主要或完全单取代NHC功能化簇的结果。群集也可以获得多达五个国家卫生保健中心,作为物种的混合物。
Magic-number gold nanoclusters are atomically precise nanomaterials that have enabled unprecedented insight into structure-property relationships in nanoscience. Thiolates are the most common ligand, binding to the cluster via a staple motif in which only central gold atoms are in the metallic state. The lack of other strongly bound ligands for nanoclusters with different bonding modes has been a significant limitation in the field. Here, we report a previously unknown ligand for gold(0) nanoclusters-N-heterocyclic carbenes (NHCs)-which feature a robust metal-carbon single bond and impart high stability to the corresponding gold cluster. The addition of a single NHC to gold nanoclusters results in significantly improved stability and catalytic properties in the electrocatalytic reduction of CO2. By varying the conditions, nature and number of equivalents of the NHC, predominantly or exclusively monosubstituted NHC-functionalized clusters result. Clusters can also be obtained with up to five NHCs, as a mixture of species.