Motif-mediated Au-25(SPh)(5)(PPh3)(10)X-2 nanorods with conjugated electron delocalization
Zheng Kai1; Zhang Jiangwei1; Zhao Dan3; Yang Yong4; Li Zhimin1; Li Gao1
Source PublicationNANO RESEARCH
AbstractWe developed a general and effective strategy to afford rod-like Au-25(SPh)(5)(PPh3)(10)X-2X-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.
KeywordAEROBIC OXIDATION CRYSTAL-STRUCTURE GOLD NANOCLUSTERS CLUSTERS NANOPARTICLES PHOTOCATALYST LIGANDS gold clusters Au-25 nanorod synchrotron radiation X-ray diffraction (SRXRD) aerobic oxidation
Indexed ByCSCD
Funding Project[National Natural Science Foundation of China] ; [Liaoning Natural Science Foundation] ; [open project Foundation of State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University] ; [Shanxi Province Hundred Talent Project]
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Cited Times:4[CSCD]   [CSCD Record]
Document Type期刊论文
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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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