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Published March 24, 2020 | Version Published + Supplemental Material
Journal Article Open

High-throughput, combinatorial synthesis of multimetallic nanoclusters

Creators

  • 1. ROR icon University of Maryland, College Park
  • 2. ROR icon University of Illinois at Chicago
  • 3. ROR icon New York University
  • 4. ROR icon Johns Hopkins University
  • 5. ROR icon Joint Center for Artificial Photosynthesis
  • 6. ROR icon National Institute of Standards and Technology
  • 7. ROR icon United States Army Research Laboratory

Abstract

Multimetallic nanoclusters (MMNCs) offer unique and tailorable surface chemistries that hold great potential for numerous catalytic applications. The efficient exploration of this vast chemical space necessitates an accelerated discovery pipeline that supersedes traditional "trial-and-error" experimentation while guaranteeing uniform microstructures despite compositional complexity. Herein, we report the high-throughput synthesis of an extensive series of ultrafine and homogeneous alloy MMNCs, achieved by 1) a flexible compositional design by formulation in the precursor solution phase and 2) the ultrafast synthesis of alloy MMNCs using thermal shock heating (i.e., ∼1,650 K, ∼500 ms). This approach is remarkably facile and easily accessible compared to conventional vapor-phase deposition, and the particle size and structural uniformity enable comparative studies across compositionally different MMNCs. Rapid electrochemical screening is demonstrated by using a scanning droplet cell, enabling us to discover two promising electrocatalysts, which we subsequently validated using a rotating disk setup. This demonstrated high-throughput material discovery pipeline presents a paradigm for facile and accelerated exploration of MMNCs for a broad range of applications.

Additional Information

© 2020 the Author(s). Published by PNAS. This open access article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND). Edited by Catherine J. Murphy, University of Illinois Urbana–Champaign, Urbana, IL, and approved February 6, 2020 (received for review March 8, 2019). PNAS first published March 10, 2020. This work was supported by the Maryland Nanocenter, its Surface Analysis Center, and the AIMLab. R.S.-Y. was supported by NSF Division of Materials Research Award 1809439. R.J. thanks the Electrochemistry Branch, Combat Capabilities Development Command Army Research Laboratory for helpful collaboration in electrocatalysis. Y.L. and C.W. were supported by the Young Investigator Program of the Army Research Office (Grant W911 NF-15-1-0123). Scanning droplet cell measurements were supported by the Office of Science of the US Department of Energy under Award DE-SC0004993. Y.M. thanks Peter Z. Zavalij for his helpful discussion. This research used resources of the Advanced Photon Source, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract DE-AC02-06CH11357. The identification of any commercial product or trade name does not imply endorsement or recommendation by the National Institute of Standards and Technology. Data Availability: All data are available within the main text and SI Appendix. Author contributions: Y.Y. and L.H. designed research; Y.Y., Z.H., T.L., H.W., Y.L., Y.M., J.G., M.J., Q.D., P.X., H.X., S.D.L., and R.J. performed research; Z.H., H.S.S., Y.M., J.D., J.M.G., and R.S.-Y. contributed new reagents/analytic tools; Y.Y., T.L., H.W., Y.L., H.S.S., Y.M., J.G., M.J., Q.D., P.X., I.T., J.M.G., R.J., C.W., A.D.T., R.S.-Y., and L.H. analyzed data; Y.Y. and L.H. wrote the paper; and T.L., I.T., C.W., A.D.T., and R.S.-Y. revised the manuscript. Y.Y., Z.H., T.L., and H.W. contributed equally to this work. The authors declare no competing interest. This article is a PNAS Direct Submission. This article contains supporting information online at https://www.pnas.org/lookup/suppl/doi:10.1073/pnas.1903721117/-/DCSupplemental.

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Supplemental Material - pnas.1903721117.sapp.pdf

Supplemental Material - pnas.1903721117.sm01.mov

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Additional details

Identifiers

PMCID
PMC7104385
Eprint ID
101846
Resolver ID
CaltechAUTHORS:20200310-155236320

Funding

Maryland Nanocenter
NSF
DMR-1809439
Army Research Office (ARO)
W911NF-15-1-0123
Department of Energy (DOE)
DE-SC0004993
Department of Energy (DOE)
DE-AC02-06CH11357

Dates

Created
2020-03-10
Created from EPrint's datestamp field
Updated
2022-02-15
Created from EPrint's last_modified field

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