Motif-mediated Au-25(SPh)(5)(PPh3)(10)X-2 nanorods with conjugated electron delocalization
文献类型：期刊论文
| 作者 | Li, Gao1; Zhao, Dan3; Zheng, Kai1,2; Zhang, Jiangwei1; Yang, Yong4; Li, Zhimin1,2 |
| 刊名 | NANO RESEARCH
 |
| 出版日期 | 2019-03-01 |
| 卷号 | 12期号:3页码:501-507 |
| 关键词 | gold clusters Au-25 nanorod synchrotron radiation X-ray diffraction (SRXRD) aerobic oxidation |
| ISSN号 | 1998-0124 |
| DOI | 10.1007/s12274-018-2147-0 |
| 通讯作者 | Li, Gao(gaoli@dicp.ac.cn) |
| 英文摘要 | We developed a general and effective strategy to afford rod-like [Au-25(SPh)(5)(PPh3)(10)X-2]X-2 (X = Cl/Br) nanoclusters, capped by conjugated delocalized p electron mediated ligands. The detailed atomic structure of these materials was resolved by synchrotron radiation X-ray diffraction (SRXRD) combined with electrospray ionization mass spectrometry (ESI-MS) and UV-vis analyses. The Au-17(SR)(3)(PPh3)(6)X(2)minimum asymmetric unit, with exposed Au atoms at the center, can serve as an important model to understand the transformation of homogold nanoclusters into alloy nanoclusters. The conjugated delocalized p electrons of the thiolate ligands can effectively tune the electronic properties of the Au-25 kernel, as qualitatively evidenced by the energy gaps measured by UV-vis experiments and density functional theory (DFT) calculations. The delocalized electrons distinctly flow to the orbitals of the Au-25 kernel via the S atoms of the aromatic thiolates. The ESI-MS analysis indicates that Au-3 clusters are formed during the etching reactions, which provide an opportunity to gain insight into the intriguing conversion pathway of the Au-n(PPh3)(m)X-y precursor to the final Au-25 nanorods. Finally, the thiophenol-protected Au-25 nanorods, immobilized on activated carbon, show good catalytic activity in the aerobic oxidation of glucose to gluconic acid (74% glucose conversion and 100% selectivity for gluconic acid), much higher than that of the aliphatic Au-25 analogue. The Au-25(SPh)(5)(PPh3)(10)X-2 catalyst yields a turnover frequency (TOF) of 13.5 s(-1), higher than that of commercial catalysts such as Pd/activated carbon (AC) and Pd-Bi/AC. The insight obtained from this study will support the development and design of efficient nanogold catalysts for special oxidation reactions. |
| WOS关键词 | AEROBIC OXIDATION ; CRYSTAL-STRUCTURE ; GOLD NANOCLUSTERS ; CLUSTERS ; NANOPARTICLES ; PHOTOCATALYST ; LIGANDS |
| 资助项目 | National Natural Science Foundation of China[21701168] ; Liaoning Natural Science Foundation[20170540897] ; open project Foundation of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University[201709] ; Shanxi Province Hundred Talent Project |
| WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics |
| 语种 | 英语 |
| WOS记录号 | WOS:000458992000003 |
| 出版者 | TSINGHUA UNIV PRESS |
| 资助机构 | National Natural Science Foundation of China ; National Natural Science Foundation of China ; Liaoning Natural Science Foundation ; Liaoning Natural Science Foundation ; open project Foundation of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University ; open project Foundation of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University ; Shanxi Province Hundred Talent Project ; Shanxi Province Hundred Talent Project ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Liaoning Natural Science Foundation ; Liaoning Natural Science Foundation ; open project Foundation of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University ; open project Foundation of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University ; Shanxi Province Hundred Talent Project ; Shanxi Province Hundred Talent Project ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Liaoning Natural Science Foundation ; Liaoning Natural Science Foundation ; open project Foundation of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University ; open project Foundation of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University ; Shanxi Province Hundred Talent Project ; Shanxi Province Hundred Talent Project ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Liaoning Natural Science Foundation ; Liaoning Natural Science Foundation ; open project Foundation of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University ; open project Foundation of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University ; Shanxi Province Hundred Talent Project ; Shanxi Province Hundred Talent Project |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/166010]  |
| 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 |
| 作者单位 | 1.Chinese Acad Sci, State Key Lab Catalysis, Dalian Inst Chem Phys, Dalian 116023, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Shenyang Normal Univ, Inst Catalysis Energy & Environm, Coll Chem & Chem Engn, Shenyang 110034, Liaoning, Peoples R China 4.Peking Univ, Dept Mat Sci & Engn, Coll Engn, Beijing 100871, Peoples R China |
| 推荐引用方式 GB/T 7714 | Li, Gao,Zhao, Dan,Zheng, Kai,et al. Motif-mediated Au-25(SPh)(5)(PPh3)(10)X-2 nanorods with conjugated electron delocalization[J]. NANO RESEARCH,2019,12(3):501-507. |
| APA | Li, Gao,Zhao, Dan,Zheng, Kai,Zhang, Jiangwei,Yang, Yong,&Li, Zhimin.(2019).Motif-mediated Au-25(SPh)(5)(PPh3)(10)X-2 nanorods with conjugated electron delocalization.NANO RESEARCH,12(3),501-507. |
| MLA | Li, Gao,et al."Motif-mediated Au-25(SPh)(5)(PPh3)(10)X-2 nanorods with conjugated electron delocalization".NANO RESEARCH 12.3(2019):501-507. |
入库方式： OAI收割
来源：大连化学物理研究所
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