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Author |
Johnson, G.; Yang, M.Y.; Liu, C.; Zhou, H.; Zuo, X.; Dickie, D.A.; Wang, S.; Gao, W.; Anaclet, B.; Perras, F.A.; Ma, F.; Zeng, C.; Wang, D.; Bals, S.; Dai, S.; Xu, Z.; Liu, G.; Goddard III, W.A.; Zhang, S. |
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Title |
Nanocluster superstructures assembled via surface ligand switching at high temperature |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Nature synthesis |
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Volume |
2 |
Issue |
9 |
Pages |
828-837 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Superstructures with nanoscale building blocks, when coupled with precise control of the constituent units, open opportunities in rationally designing and manufacturing desired functional materials. Yet, synthetic strategies for the large-scale production of superstructures are scarce. We report a scalable and generalized approach to synthesizing superstructures assembled from atomically precise Ce24O28(OH)8 and other rare-earth metal-oxide nanoclusters alongside a detailed description of the self-assembly mechanism. Combining operando small-angle X-ray scattering, ex situ molecular and structural characterizations, and molecular dynamics simulations indicates that a high-temperature ligand-switching mechanism, from oleate to benzoate, governs the formation of the nanocluster assembly. The chemical tuning of surface ligands controls superstructure disassembly and reassembly, and furthermore, enables the synthesis of multicomponent superstructures. This synthetic approach, and the accurate mechanistic understanding, are promising for the preparation of superstructures for use in electronics, plasmonics, magnetics and catalysis. Synthesizing superstructures with precisely controlled nanoscale building blocks is challenging. Here the assembly of superstructures is reported from atomically precise Ce24O28(OH)8 and other rare-earth metal-oxide nanoclusters and their multicomponent combinations. A high-temperature ligand-switching mechanism controls the self-assembly. |
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Wos |
001124824000001 |
Publication Date |
2023-05-01 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Times cited |
2 |
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Not_Open_Access |
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Notes |
This work was supported by the US National Science Foundation (CBET-2004808) and the Sloan Research Fellowship. We acknowledge UVA's Nanoscale Material Characterization Facility (NMCF) for use of the XPS and SCXRD acquired under NSF MRI award DMR-1626201 and CHE-20188780, respectively. G.J. acknowledges support from the US Department of Energy (DOE), Office of Science, Office of Workforce Development for Teachers and Scientists, Office of Science Graduate Student Research (SCGSR) programme. The SCGSR programme is administered by the Oak Ridge Institute for Science and Education for the DOE under contract number DE-SC0014664. This work benefited from the use of the SasView application, originally developed under NSF Award DMR-0520547. SasView also contains code developed with funding from the EU Horizon 2020 programme under the SINE2020 project grant number 654000. This research used resources of the Advanced Photon Source, a US DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory, under contract number DE-AC02-06CH11357. D.W. acknowledges an Individual Fellowship funded by the Marie Sk & lstrok;odowska-Curie Actions (MSCA) in the Horizon 2020 programme (grant 894254 SuprAtom). S.B. acknowledges support from the European Research Council (grant number 815128-REALNANO). The electron microscopy work was performed in part at the Analytical Instrumentation Facility (AIF) at North Carolina State University, which is supported by the State of North Carolina and the National Science Foundation (award number ECCS-2025064). The AIF is a member of the North Carolina Research Triangle Nanotechnology Network (RTNN), a site in the National Nanotechnology Coordinated Infrastructure (NNCI). G.L. gratefully acknowledges funding support by US NSF (DMR-1752611) and the Dean's Discovery Fund at Virginia Tech. S.D. acknowledges support from the US DOE, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. P. Bean at the University of Virginia is acknowledged for his SEM contributions measuring the HEASS. We thank T. B. Gunnoe (University of Virginia), J. Elena (University of Virginia), D. E. Jiang (University of California, Riverside) and C. B. Murray (University of Pennsylvania) for project discussions. |
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Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:202180 |
Serial |
9060 |
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