Nanocluster superstructures assembled via surface ligand switching at high temperature

Johnson, Grayson; Yang, Moon Young; Liu, Chang; Zhou, Hua; Zuo, Xiaobing; Dickie, Diane A.; Wang, Sihan; Gao, Wenpei; Anaclet, Bukuru; Perras, Frédéric A.; Ma, Fuyan; Zeng, Chenjie; Wang, Da; Bals, Sara; Dai, Sheng; Xu, Zhen; Liu, Guoliang; Goddard, III, William A.; Zhang, Sen

doi:10.1038/s44160-023-00304-8

Title: Nanocluster superstructures assembled via surface ligand switching at high temperature

Journal Article · 01 May 2023 · Nature Synthesis

DOI: https://doi.org/10.1038/s44160-023-00304-8 · OSTI ID:2000555

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University of Virginia, Charlottesville, VA (United States)
California Institute of Technology (CalTech), Pasadena, CA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)
North Carolina State University, Raleigh, NC (United States)
Iowa State University, Ames, IA (United States)
University of Florida, Gainesville, FL (United States)
University of Antwerp (Belgium)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)

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. Here, this synthetic approach, and the accurate mechanistic understanding, are promising for the preparation of superstructures for use in electronics, plasmonics, magnetics and catalysis.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Alfred P. Sloan Foundation; European Research Council (ERC); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Graduate Student Research (SCGSR) Program; USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS)

Grant/Contract Number:: AC02-06CH11357; SC0014664

OSTI ID:: 2000555

Journal Information:: Nature Synthesis, Journal Name: Nature Synthesis Journal Issue: 9 Vol. 2; ISSN 2731-0582

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Nanocluster superstructures assembled via surface ligand switching at high temperature

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