Tailoring the Electronic and Catalytic Properties of Au-25 Nanoclusters via Ligand Engineering
文献类型：期刊论文
| 作者 | Li, Gao2; Abroshan, Hadi3; Liu, Chong1; Zhuo, Shuo3; Li, Zhimin2; Xie, Yan2; Kim, Hyung J.3,4; Ros, Nathaniel L.1; Jin, Rongchao3 |
| 刊名 | ACS NANO
 |
| 出版日期 | 2016-08-01 |
| 卷号 | 10期号:8页码:7998-8005 |
| 关键词 | Gold Nanoclusters Au-25 Ligand Effects Ullmann Coupling |
| ISSN号 | 1936-0851 |
| DOI | 10.1021/acsnano.6b03964 |
| 文献子类 | Article |
| 英文摘要 | To explore the electronic and catalytic properties of nanoclusters, here we report an aromatic-thiolate-protected gold nanocluster, [Au-25(SNap)(18)](-) [TOA](+), where SNap = 1-naphthalenethiolate and TOA = tetraoctylammonium. It exhibits distinct differences in electronic and catalytic properties in comparison with the previously reported [Au-25(SCH2CH2Ph)(18)](-), albeit their skeletons (i.e., Au25S18 framework) are similar. A red shift by similar to 10 nm in the HOMO-LUMO electronic absorption peak wavelength is observed for the aromatic-thiolate-protected nanocluster, which is attributed to its dilated Au-13 kernel. The unsupported [Au-25(SNap)(18)](-) nanoclusters show high thermal and antioxidation stabilities (e.g., at 80 degrees C in the present of O-2, excess H2O2, or TBHP) due to the effects of aromatic ligands on stabilization of the nanocluster's frontier orbitals (HOMO and LUMO). Furthermore, the catalytic activity of the supported Au-25(SR)(18)/CeO2 (R = Nap, Ph, CH2CH2Ph, and n-C6H13) is examined in the Ullmann heterocoupling reaction between 4-methyl-iodobenzene and 4-nitro-iodobenzene. Results show that the activity and selectivity of the catalysts are largely influenced by the chemical nature of the protecting thiolate ligands. This study highlights that the aromatic ligands not only lead to a higher conversion in catalytic reaction but also markedly increase the yield of the heterocoupling product (4-methyl-4'-nitro-1,1'-biphenyl). Through a combined approach of experiment and theory, this study sheds light on the structure activity relationships of the Au-25 nanoclusters and also offers guidelines for tailoring nanocluster properties by ligand engineering for specific applications. |
| WOS关键词 | CRYSTAL-STRUCTURE ; AU-25(SCH2CH2PH)(18) NANOCLUSTERS ; AU-25(SR)(18) CLUSTER ; OPTICAL-PROPERTIES ; OXIDATION ; HYDROGENATION ; EXCHANGE ; PSEUDOPOTENTIALS ; APPROXIMATION ; POLARIZATION |
| WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science |
| 语种 | 英语 |
| WOS记录号 | WOS:000381959100085 |
| 出版者 | AMER CHEMICAL SOC |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/170284]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 通讯作者 | Li, Gao; Jin, Rongchao |
| 作者单位 | 1.Univ Pittsburgh, Dept Chem, Pittsburgh, PA 15213 USA 2.Chinese Acad Sci, Dalian Inst Chem Phys, Gold Catalysis Res Ctr, State Key Lab Catalysis, Dalian 116023, Peoples R China 3.Carnegie Mellon Univ, Dept Chem, Pittsburgh, PA 15213 USA 4.Korea Inst Adv Study, Sch Computat Sci, Seoul 02455, South Korea |
| 推荐引用方式 GB/T 7714 | Li, Gao,Abroshan, Hadi,Liu, Chong,et al. Tailoring the Electronic and Catalytic Properties of Au-25 Nanoclusters via Ligand Engineering[J]. ACS NANO,2016,10(8):7998-8005. |
| APA | Li, Gao.,Abroshan, Hadi.,Liu, Chong.,Zhuo, Shuo.,Li, Zhimin.,...&Jin, Rongchao.(2016).Tailoring the Electronic and Catalytic Properties of Au-25 Nanoclusters via Ligand Engineering.ACS NANO,10(8),7998-8005. |
| MLA | Li, Gao,et al."Tailoring the Electronic and Catalytic Properties of Au-25 Nanoclusters via Ligand Engineering".ACS NANO 10.8(2016):7998-8005. |
入库方式： OAI收割
来源：大连化学物理研究所
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