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Title: Diphosphine-induced chiral propeller arrangement of gold nanoclusters for singlet oxygen photogeneration

Abstract

In this study, 1,2-bis(diphenylphosphino)ethane (dppe) ligands are used to synthesize gold nanoclusters with an icosahedral Au 13 core. The nanoclusters are characterized and formulated as [Au 13(dppe) 5Cl 2]Cl 3 using synchrotron radiation X-ray diffraction, UV/Vis absorption spectroscopy, electrospray ionization mass spectrometry, and density functional theory (DFT) calculations. The bidentate feature of dppe ligands and the positions of coordinating surface gold atoms induce a helical arrangement that forms a propeller-like structure, which reduces the symmetry of the gold nanocluster to C 1. Therefore, dppe ligands perform as a directing agent to create chiral an ansa metallamacrocycle [Au 13(dppe) 5Cl 2] 3+ nanocluster, as confirmed by simulated electronic circular dichroism spectrum. The highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) gap of the [Au 13(dppe) 5Cl 2] 3+ cluster is determined as approx. 1.9 eV, and further confirmed by ultraviolet photoemission spectroscopy analysis and DFT simulation. Furthermore, the photoactivity of [Au 13(dppe) 5Cl 2] 3+ is investigated, with the nanocluster shown to possess near-infrared photoluminescence properties, which can be employed for 1O 2 photogeneration. In conclusion, the quantum yield of 1O 2 photogeneration using the [Au 13(dppe) 5Cl 2] 3+ nanocluster is up to 0.71, which is considerably higher thanmore » those of anthracene (an organic dye), and Au 25 and Au 38 nanoclusters.« less

Authors:
 [1];  [2];  [1];  [3];  [4];  [5];  [1]
  1. Chinese Academy of Sciences, Dalian (China)
  2. Chinese Academy of Sciences, Dalian (China); Univ. of Chinese Academy of Sciences, Beijing (China)
  3. Stanford Univ., Stanford, CA (United States)
  4. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
  5. Peking Univ., Beijing (China)
Publication Date:
Research Org.:
National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States); National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States). In-house Research
Sponsoring Org.:
FE; USDOE
OSTI Identifier:
1509723
Alternate Identifier(s):
OSTI ID: 1477163
Report Number(s):
NETL-PUB-22331
Journal ID: ISSN 1998-0124
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Research
Additional Journal Information:
Journal Volume: 11; Journal Issue: 11; Journal ID: ISSN 1998-0124
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; gold nanoclusters; Au13; chirality; singlet oxygen; synchrotron radiation; X-ray diffraction (XRD); 36 MATERIALS SCIENCE; Catalyst development; nanomaterials; materials characterization; X-ray spectroscopy; photoluminescence

Citation Formats

Zhang, Jiangwei, Zhou, Yang, Zheng, Kai, Abroshan, Hadi, Kauffman, Douglas R., Sun, Junliang, and Li, Gao. Diphosphine-induced chiral propeller arrangement of gold nanoclusters for singlet oxygen photogeneration. United States: N. p., 2018. Web. doi:10.1007/s12274-017-1935-2.
Zhang, Jiangwei, Zhou, Yang, Zheng, Kai, Abroshan, Hadi, Kauffman, Douglas R., Sun, Junliang, & Li, Gao. Diphosphine-induced chiral propeller arrangement of gold nanoclusters for singlet oxygen photogeneration. United States. doi:10.1007/s12274-017-1935-2.
Zhang, Jiangwei, Zhou, Yang, Zheng, Kai, Abroshan, Hadi, Kauffman, Douglas R., Sun, Junliang, and Li, Gao. Mon . "Diphosphine-induced chiral propeller arrangement of gold nanoclusters for singlet oxygen photogeneration". United States. doi:10.1007/s12274-017-1935-2. https://www.osti.gov/servlets/purl/1509723.
@article{osti_1509723,
title = {Diphosphine-induced chiral propeller arrangement of gold nanoclusters for singlet oxygen photogeneration},
author = {Zhang, Jiangwei and Zhou, Yang and Zheng, Kai and Abroshan, Hadi and Kauffman, Douglas R. and Sun, Junliang and Li, Gao},
abstractNote = {In this study, 1,2-bis(diphenylphosphino)ethane (dppe) ligands are used to synthesize gold nanoclusters with an icosahedral Au13 core. The nanoclusters are characterized and formulated as [Au13(dppe)5Cl2]Cl3 using synchrotron radiation X-ray diffraction, UV/Vis absorption spectroscopy, electrospray ionization mass spectrometry, and density functional theory (DFT) calculations. The bidentate feature of dppe ligands and the positions of coordinating surface gold atoms induce a helical arrangement that forms a propeller-like structure, which reduces the symmetry of the gold nanocluster to C1. Therefore, dppe ligands perform as a directing agent to create chiral an ansa metallamacrocycle [Au13(dppe)5Cl2]3+ nanocluster, as confirmed by simulated electronic circular dichroism spectrum. The highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) gap of the [Au13(dppe)5Cl2]3+ cluster is determined as approx. 1.9 eV, and further confirmed by ultraviolet photoemission spectroscopy analysis and DFT simulation. Furthermore, the photoactivity of [Au13(dppe)5Cl2]3+ is investigated, with the nanocluster shown to possess near-infrared photoluminescence properties, which can be employed for 1O2 photogeneration. In conclusion, the quantum yield of 1O2 photogeneration using the [Au13(dppe)5Cl2]3+ nanocluster is up to 0.71, which is considerably higher than those of anthracene (an organic dye), and Au25 and Au38 nanoclusters.},
doi = {10.1007/s12274-017-1935-2},
journal = {Nano Research},
issn = {1998-0124},
number = 11,
volume = 11,
place = {United States},
year = {2018},
month = {11}
}

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Cited by: 8 works
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Works referenced in this record:

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    Works referencing / citing this record:

    A direct anchoring of Anderson-type polyoxometalates in aqueous media with tripodal ligands especially containing the carboxyl group
    journal, January 2014

    • Zhang, Jiangwei; Huang, Yichao; Zhang, Jin
    • Dalton Trans., Vol. 43, Issue 7
    • DOI: 10.1039/c3dt53034e

    Ylide–Metal Complexes. X. An X-Ray Photoelectron Spectroscopic Study of Triphenylmethylenephosphorane and Gold- and Copper–Phosphorane Complexes
    journal, May 1986

    • Yamamoto, Yoshihisa; Konno, Hidetaka
    • Bulletin of the Chemical Society of Japan, Vol. 59, Issue 5
    • DOI: 10.1246/bcsj.59.1327

    Density‐functional thermochemistry. III. The role of exact exchange
    journal, April 1993

    • Becke, Axel D.
    • The Journal of Chemical Physics, Vol. 98, Issue 7, p. 5648-5652
    • DOI: 10.1063/1.464913

    Atomically Precise Gold Nanoclusters as New Model Catalysts
    journal, March 2013

    • Li, Gao; Jin, Rongchao
    • Accounts of Chemical Research, Vol. 46, Issue 8
    • DOI: 10.1021/ar300213z

    The Chemistry of the Sulfur–Gold Interface: In Search of a Unified Model
    journal, March 2012

    • Pensa, Evangelina; Cortés, Emiliano; Corthey, Gastón
    • Accounts of Chemical Research, Vol. 45, Issue 8
    • DOI: 10.1021/ar200260p

    Superoxide Ion: Generation and Chemical Implications
    journal, February 2016


    Experimental and Theoretical Investigation of the Electronic and Geometrical Structures of the Au32 Cluster
    journal, November 2005

    • Ji, Min; Gu, Xiao; Li, Xi
    • Angewandte Chemie International Edition, Vol. 44, Issue 43
    • DOI: 10.1002/anie.200502795

    Evidence for s–d Hybridization in Au 38 Clusters
    journal, February 2012

    • Losovyj, Yaroslav B.; Li, Shao-Chun; Lozova, Natalia
    • The Journal of Physical Chemistry C, Vol. 116, Issue 9
    • DOI: 10.1021/jp3010508

    Structurally Similar Triphenylphosphine-Stabilized Undecagolds, Au 11 (PPh 3 ) 7 Cl 3 and [Au 11 (PPh 3 ) 8 Cl 2 ]Cl, Exhibit Distinct Ligand Exchange Pathways with Glutathione
    journal, September 2014

    • McKenzie, Lallie C.; Zaikova, Tatiana O.; Hutchison, James E.
    • Journal of the American Chemical Society, Vol. 136, Issue 38
    • DOI: 10.1021/ja5075689

    Emergence of hierarchical structural complexities in nanoparticles and their assembly
    journal, December 2016


    Chirality and Electronic Structure of the Thiolate-Protected Au 38 Nanocluster
    journal, June 2010

    • Lopez-Acevedo, Olga; Tsunoyama, Hironori; Tsukuda, Tatsuya
    • Journal of the American Chemical Society, Vol. 132, Issue 23
    • DOI: 10.1021/ja102934q

    Nonscalable Oxidation Catalysis of Gold Clusters
    journal, December 2013

    • Yamazoe, Seiji; Koyasu, Kiichirou; Tsukuda, Tatsuya
    • Accounts of Chemical Research, Vol. 47, Issue 3
    • DOI: 10.1021/ar400209a

    A linear scaling method for Hartree–Fock exchange calculations of large molecules
    journal, November 1996

    • Burant, John C.; Scuseria, Gustavo E.; Frisch, Michael J.
    • The Journal of Chemical Physics, Vol. 105, Issue 19
    • DOI: 10.1063/1.472627

    Tailoring the Electronic and Catalytic Properties of Au 25 Nanoclusters via Ligand Engineering
    journal, July 2016


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    journal, March 2014

    • Crasto, David; Malola, Sami; Brosofsky, Grace
    • Journal of the American Chemical Society, Vol. 136, Issue 13
    • DOI: 10.1021/ja412141j

    Ligand-Stabilized and Atomically Precise Gold Nanocluster Catalysis: A Case Study for Correlating Fundamental Electronic Properties with Catalysis
    journal, June 2013

    • Liu, Jing; Krishna, Katla Sai; Losovyj, Yaroslav B.
    • Chemistry - A European Journal, Vol. 19, Issue 31
    • DOI: 10.1002/chem.201300600

    Atomically Precise Colloidal Metal Nanoclusters and Nanoparticles: Fundamentals and Opportunities
    journal, September 2016


    Chiral Au 25 Nanospheres and Nanorods: Synthesis and Insight into the Origin of Chirality
    journal, September 2011

    • Zhu, Manzhou; Qian, Huifeng; Meng, Xiangming
    • Nano Letters, Vol. 11, Issue 9
    • DOI: 10.1021/nl202288j

    First enantioseparation and circular dichroism spectra of Au38 clusters protected by achiral ligands
    journal, January 2012

    • Dolamic, Igor; Knoppe, Stefan; Dass, Amala
    • Nature Communications, Vol. 3, Issue 1
    • DOI: 10.1038/ncomms1802

    Absolute structure and absolute configuration
    journal, September 1999

    • Flack, H. D.; Bernardinelli, G.
    • Acta Crystallographica Section A Foundations of Crystallography, Vol. 55, Issue 5
    • DOI: 10.1107/s0108767399004262

    Total Structure Determination of Thiolate-Protected Au 38 Nanoparticles
    journal, June 2010

    • Qian, Huifeng; Eckenhoff, William T.; Zhu, Yan
    • Journal of the American Chemical Society, Vol. 132, Issue 24
    • DOI: 10.1021/ja103592z

    Amplification of the Optical Activity of Gold Clusters by the Proximity of BINAP
    journal, November 2016


    Synthesis, Stability, and Photoluminescence Properties of PdAu10(PPh3)8Cl2 Clusters
    journal, January 2012


    Transition metal-mediated catalytic properties of gold nanoclusters in aerobic alcohol oxidation
    journal, March 2018


    Facile synthesis and optical properties of magic-number Au13 clusters
    journal, January 2012

    • Shichibu, Yukatsu; Suzuki, Kai; Konishi, Katsuaki
    • Nanoscale, Vol. 4, Issue 14
    • DOI: 10.1039/c2nr30675a

    Asymmetric Synthesis of Chiral Bimetallic [Ag 28 Cu 12 (SR) 24 ] 4– Nanoclusters via Ion Pairing
    journal, September 2016

    • Yan, Juanzhu; Su, Haifeng; Yang, Huayan
    • Journal of the American Chemical Society, Vol. 138, Issue 39
    • DOI: 10.1021/jacs.6b08100

    OLEX2 : a complete structure solution, refinement and analysis program
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    • Dolomanov, Oleg V.; Bourhis, Luc J.; Gildea, Richard J.
    • Journal of Applied Crystallography, Vol. 42, Issue 2
    • DOI: 10.1107/s0021889808042726

    Surface Coordination Chemistry of Metal Nanomaterials
    journal, January 2017

    • Liu, Pengxin; Qin, Ruixuan; Fu, Gang
    • Journal of the American Chemical Society, Vol. 139, Issue 6
    • DOI: 10.1021/jacs.6b10978

    Recent advances in the synthesis and catalytic applications of ligand-protected, atomically precise metal nanoclusters
    journal, September 2016


    Au 38 S 2 (SAdm) 20 Photocatalyst for One-Step Selective Aerobic Oxidations
    journal, April 2017


    Chiral 38-Gold-Atom Nanoclusters: Synthesis and Chiroptical Properties
    journal, October 2013


    Cluster–π electronic interaction in a superatomic Au 13 cluster bearing σ-bonded acetylide ligands
    journal, January 2015

    • Sugiuchi, Mizuho; Shichibu, Yukatsu; Nakanishi, Takayuki
    • Chemical Communications, Vol. 51, Issue 70
    • DOI: 10.1039/c5cc04312c

    Motif-mediated Au25(SPh)5(PPh3)10X2 nanorods with conjugated electron delocalization
    journal, August 2018


    Chirality in Gold Nanoclusters Probed by NMR Spectroscopy
    journal, October 2011

    • Qian, Huifeng; Zhu, Manzhou; Gayathri, Chakicherla
    • ACS Nano, Vol. 5, Issue 11
    • DOI: 10.1021/nn203113j

    Visible Light Gold Nanocluster Photocatalyst: Selective Aerobic Oxidation of Amines to Imines
    journal, April 2017


    Identification of a Highly Luminescent Au 22 (SG) 18 Nanocluster
    journal, January 2014

    • Yu, Yong; Luo, Zhentao; Chevrier, Daniel M.
    • Journal of the American Chemical Society, Vol. 136, Issue 4
    • DOI: 10.1021/ja411643u

    Hexane-Driven Icosahedral to Cuboctahedral Structure Transformation of Gold Nanoclusters
    journal, October 2012

    • Li, Yuanyuan; Cheng, Hao; Yao, Tao
    • Journal of the American Chemical Society, Vol. 134, Issue 43
    • DOI: 10.1021/ja306923a

    Efficient Aerobic Oxidation of Glucose to Gluconic Acid over Activated Carbon‐Supported Gold Clusters
    journal, April 2017


    Generation of Singlet Oxygen by Photoexcited Au 25 (SR) 18 Clusters
    journal, April 2014

    • Kawasaki, Hideya; Kumar, Santosh; Li, Gao
    • Chemistry of Materials, Vol. 26, Issue 9
    • DOI: 10.1021/cm500260z

    Structurally Well-Defined Sigmoidal Gold Clusters: Probing the Correlation between Metal Atom Arrangement and Chiroptical Response
    journal, April 2016

    • He, Xin; Wang, Yuechao; Jiang, Hong
    • Journal of the American Chemical Society, Vol. 138, Issue 17
    • DOI: 10.1021/jacs.6b01658

    Chirality transfer from gold nanocluster to adsorbate evidenced by vibrational circular dichroism
    journal, May 2015

    • Dolamic, Igor; Varnholt, Birte; Bürgi, Thomas
    • Nature Communications, Vol. 6, Issue 1
    • DOI: 10.1038/ncomms8117

    Controlling Gold Nanoclusters by Diphospine Ligands
    journal, December 2013

    • Chen, Jing; Zhang, Qian-Fan; Bonaccorso, Timary A.
    • Journal of the American Chemical Society, Vol. 136, Issue 1
    • DOI: 10.1021/ja411061e

    A Chiral Gold Nanocluster Au 20 Protected by Tetradentate Phosphine Ligands
    journal, February 2014

    • Wan, Xian-Kai; Yuan, Shang-Fu; Lin, Zhi-Wei
    • Angewandte Chemie International Edition, Vol. 53, Issue 11
    • DOI: 10.1002/anie.201308599

    Step-by-Step Strategy from Achiral Precursors to Polyoxometalates-Based Chiral Organic–Inorganic Hybrids
    journal, February 2015

    • Zhang, Jiangwei; Luo, Jianhui; Wang, Pingmei
    • Inorganic Chemistry, Vol. 54, Issue 6
    • DOI: 10.1021/ic502622k

    Density-functional exchange-energy approximation with correct asymptotic behavior
    journal, September 1988


    A Missing Link in Undecagold Cluster Chemistry: Single-Crystal X-ray Analysis of [Au 11 (PPh 3 ) 7 Cl 3 ]
    journal, March 2013

    • Gutrath, Benjamin S.; Englert, Ulli; Wang, Yutian
    • European Journal of Inorganic Chemistry, Vol. 2013, Issue 12
    • DOI: 10.1002/ejic.201300148

    Chirality in Au 9 clusters protected by chiral/achiral mixed bidentate phosphine ligands: influence of the metal core and ligand array
    journal, January 2019

    • Sato, Yasuhiko; Mitani, Masaki; Yao, Hiroshi
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 27
    • DOI: 10.1039/c9cp02341k

    Motif-mediated Au25(SPh)5(PPh3)10X2 nanorods with conjugated electron delocalization
    journal, August 2018


    Chirality in Au 9 clusters protected by chiral/achiral mixed bidentate phosphine ligands: influence of the metal core and ligand array
    journal, January 2019

    • Sato, Yasuhiko; Mitani, Masaki; Yao, Hiroshi
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 27
    • DOI: 10.1039/c9cp02341k

    Heterogeneous Cross-Coupling over Gold Nanoclusters
    journal, June 2019

    • Shi, Quanquan; Qin, Zhaoxian; Xu, Hui
    • Nanomaterials, Vol. 9, Issue 6
    • DOI: 10.3390/nano9060838