Single, Self-Born RP-Au-PR Motif Boosts 19-Fold Photoluminescence Quantum Yield of Metal Nanocluster
Xu, Daolan1,2; Yang, Ying1,2; Fan, Wentao1,2,3; He, Zongbing1,2; Zou, Jiafeng1,2; Feng, Lei1,2; Li, Man-Bo1,2; Wu, Zhikun1,2
刊名ACTA CHIMICA SINICA
2022-01-15
卷号80
关键词metal nanocluster RP-Au-PR motif photoluminescence
ISSN号0567-7351
DOI10.6023/A21110499
通讯作者Li, Man-Bo(mbli@ahu.edu.cn)
英文摘要The study of phosphine-protected gold nanocluster can be dated back to 1969, however, the RP-Au-PR motif has not been reported until now. Meanwhile, its analogue RS-Au-SR motif was often reported in thiolated gold nanoclusters, being of multiple functions (e.g., enhancing the luminescence). Herein, we successfully synthesized a monodisperse gold-silver nanocluster: [Au10Ag4(Dppp)(5)Cl-4]Cl-2 (Au10Ag4 NC, where the Dppp represents 1,3-diphenylphosphine propane, and NC represents nanocluster) by introducing the reducing agent (NaBH4) in an dichloromethane-ethanol solution of chloroauric acid, silver nitrate and 1,3-diphenylphosphine propane. Hydrochloric acid was added to promote the nanocluster size-focusing. Au10Ag4 NC is unstable in dichloromethane and will be transformed into another nanocluster [Au9Ag4(Dppp)(4)Cl-4]Cl (Au9Ag4 NC). The structures and compositions of Au10Ag4 and Au9Ag4 NCs have been determined by single crystal X-ray crystallography and electrospray ionization mass spectrometry (ESI-MS). Au10Ag4 NC possesses an ico-sahedral Au9Ag4 core, which is protected by a special RP-Au-PR motif, diphosphine and halogen ligands; Au9Ag4 NC has an icosahedral Au9Ag4 metal core protected by bisphosphine and halogen ligands, thus the major structural difference between Au10Ag4 and Au9Ag4 NCs is the RP-Au-PR motif. The motif can be self-vanished in Au10Ag4 NC when dichloromethane acts as the solvent, resulting in the formation of Au9Ag4 NC as mentioned above; on the other hand, the motif can self-bear in Au9Ag4 NC when the solvent is ethanol instead of dichloromethane, resulting in the formation of Au10Ag4 NC. The two nanoclusters showed similar ultraviolet-visible-near infrared (UV/Vis/NIR) absorption spectra except for slight shift of the profile, indicating that the RP-Au-PR motif has no essential influence on the electronic structure of nanocluster, which was supported by density functional theory (DFT) calculations. However, the photoluminescence quantum yield of Au10Ag4 NC (10.32%) is 19 times higher than that of Au9Ag4 NC (0.52%), ascribing to the enhancement of charge transfer and structure rigidity induced by the motif. This work provides new views to the structure and photoluminescence of gold-silver nanocluster, has important implications for the structure-property understanding and the property improvement.
资助项目National Natural Science Foundation of China[92061110] ; National Natural Science Foundation of China[21925303] ; National Natural Science Foundation of China[21771186] ; National Natural Science Foundation of China[21829501] ; National Natural Science Foundation of China[21222301] ; National Natural Science Foundation of China[21171170] ; National Natural Science Foundation of China[21528303] ; Hefei National Laboratory for Physical Sciences at the Microscale[KF2020102] ; Anhui University[S020118002/113] ; CASHIPS Director's Fund[BJPY2019A02] ; Key Program of the 13th five-year plan, CASHIPS[KP-2017-16] ; Collaborative Innovation Program of Hefei Science Center, CAS[2020HSC-CIP005]
WOS关键词GOLD NANOCLUSTERS ; CLUSTERS ; NANOPARTICLES ; LUMINESCENT
WOS研究方向Chemistry
语种英语
出版者SCIENCE PRESS
WOS记录号WOS:000745689000001
资助机构National Natural Science Foundation of China ; Hefei National Laboratory for Physical Sciences at the Microscale ; Anhui University ; CASHIPS Director's Fund ; Key Program of the 13th five-year plan, CASHIPS ; Collaborative Innovation Program of Hefei Science Center, CAS
内容类型期刊论文
源URL[http://ir.hfcas.ac.cn:8080/handle/334002/127575]  
专题中国科学院合肥物质科学研究院
通讯作者Li, Man-Bo
作者单位1.Anhui Univ, Inst Phys Sci & Informat Technol, Hefei 230601, Peoples R China
2.Chinese Acad Sci, Anhui Key Lab Nanomat & Nanotechnol, CAS Ctr Excellence Nanosci, Key Lab Mat Phys,Inst Solid State Phys,Hefei Inst, Hefei 230031, Peoples R China
3.Univ Sci & Technol China, Hefei 230026, Peoples R China
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GB/T 7714
Xu, Daolan,Yang, Ying,Fan, Wentao,et al. Single, Self-Born RP-Au-PR Motif Boosts 19-Fold Photoluminescence Quantum Yield of Metal Nanocluster[J]. ACTA CHIMICA SINICA,2022,80.
APA Xu, Daolan.,Yang, Ying.,Fan, Wentao.,He, Zongbing.,Zou, Jiafeng.,...&Wu, Zhikun.(2022).Single, Self-Born RP-Au-PR Motif Boosts 19-Fold Photoluminescence Quantum Yield of Metal Nanocluster.ACTA CHIMICA SINICA,80.
MLA Xu, Daolan,et al."Single, Self-Born RP-Au-PR Motif Boosts 19-Fold Photoluminescence Quantum Yield of Metal Nanocluster".ACTA CHIMICA SINICA 80(2022).
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