| Motif-mediated au-25(sph)(5)(pph3)(10)x-2 nanorods with conjugated electron delocalization | |
| Zheng, Kai1,2; Zhang, Jiangwei1; Zhao, Dan3; Yang, Yong4; Li, Zhimin1,2; Li, Gao1 | |
| 刊名 | Nano research
 |
| 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 |
| WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics |
| WOS类目 | Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied |
| 语种 | 英语 |
| 出版者 | TSINGHUA UNIV PRESS |
| WOS记录号 | WOS:000458992000003 |
| 内容类型 | 期刊论文 |
| URI标识 | http://www.corc.org.cn/handle/1471x/2372774 |
| 专题 | 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 | Zheng, Kai,Zhang, Jiangwei,Zhao, Dan,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 | Zheng, Kai,Zhang, Jiangwei,Zhao, Dan,Yang, Yong,Li, Zhimin,&Li, Gao.(2019).Motif-mediated au-25(sph)(5)(pph3)(10)x-2 nanorods with conjugated electron delocalization.Nano research,12(3),501-507. |
| MLA | Zheng, Kai,et al."Motif-mediated au-25(sph)(5)(pph3)(10)x-2 nanorods with conjugated electron delocalization".Nano research 12.3(2019):501-507. |
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