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High-throughput, combinatorial synthesis of multimetallic nanoclusters

Yao, Yonggang and Huang, Zhennan and Li, Tangyuan and Wang, Hang and Liu, Yifan and Stein, Helge S. and Mao, Yimin and Gao, Jinlong and Jiao, Miaolun and Dong, Qi and Dai, Jiaqi and Xie, Pengfei and Xie, Hua and Lacey, Steven D. and Takeuchi, Ichiro and Gregoire, John M. and Jiang, Rongzhong and Wang, Chao and Taylor, Andre D. and Shahbazian-Yassar, Reza and Hu, Liangbing (2020) High-throughput, combinatorial synthesis of multimetallic nanoclusters. Proceedings of the National Academy of Sciences of the United States of America, 117 (12). pp. 6316-6322. ISSN 0027-8424. PMCID PMC7104385. https://resolver.caltech.edu/CaltechAUTHORS:20200310-155236320

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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.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1073/pnas.1903721117DOIArticle
https://www.pnas.org/content/suppl/2020/03/09/1903721117.DCSupplementalPublisherSupporting Information
http://www.ncbi.nlm.nih.gov/pmc/articles/pmc7104385/PubMed CentralArticle
ORCID:
AuthorORCID
Stein, Helge S.0000-0002-3461-0232
Gregoire, John M.0000-0002-2863-5265
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.
Group:JCAP
Funders:
Funding AgencyGrant Number
Maryland NanocenterUNSPECIFIED
NSFDMR-1809439
Army Research Office (ARO)W911NF-15-1-0123
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-AC02-06CH11357
Subject Keywords:combinatorial; high-throughput synthesis; multimetallic nanoclusters; thermal shock; oxygen reduction reaction
Issue or Number:12
PubMed Central ID:PMC7104385
Record Number:CaltechAUTHORS:20200310-155236320
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200310-155236320
Official Citation:High-throughput, combinatorial synthesis of multimetallic nanoclusters. Yonggang Yao, Zhennan Huang, Tangyuan Li, Hang Wang, Yifan Liu, Helge S. Stein, Yimin Mao, Jinlong Gao, Miaolun Jiao, Qi Dong, Jiaqi Dai, Pengfei Xie, Hua Xie, Steven D. Lacey, Ichiro Takeuchi, John M. Gregoire, Rongzhong Jiang, Chao Wang, Andre D. Taylor, Reza Shahbazian-Yassar, Liangbing Hu. Proceedings of the National Academy of Sciences Mar 2020, 117 (12) 6316-6322; DOI: 10.1073/pnas.1903721117
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:101846
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:10 Mar 2020 23:04
Last Modified:06 Apr 2020 19:04

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