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Title: Lithium assisted “dissolution–alloying” synthesis of nanoalloys from individual bulk metals

Here, we report new fundamental chemistry involved in the synthesis of bimetallic nanoalloys via dissolving the pure bulk transition metals in molten lithium. It is revealed at the atomic level that when two pure bulk transition metals such as Pd and Pt are placed in molten lithium (~200°C), they undergo a dissolution process in which the metal-metal bonds in pure bulk transition metals are completely ruptured, resulting in the existence of individual Pd and Pt atoms surrounded by lithium atoms, as is evident by synchrotron Xray adsorption techniques. Then, upon the conversion of metal lithium to LiOH in humid air, the Pd and Pt atoms undergo an alloying process, to aggregate into nanoalloys. This method was further expanded to include PdZn, which is notoriously difficult to prepare via traditional nanoalloy synthesis methods due to the easily oxidizable Zn component. The constantly reducing environment of metallic Li allowed for preparation of PdZn nanoalloys with minimal Zn oxidation via dissolution-alloying of individual bulk transition metals in molten lithium. Additionally, this lithium assisted “dissolutionalloying” method bypasses many complications intrinsic to conventional ion reductionbased nanoalloy synthesis including the necessity of ligated metal ions, the use of proper reducing agents and dispersing surfactants, and themore » presence of segregated phases due to different reduction potentials of the constituent metal ions.« less
Authors:
 [1] ;  [2] ;  [2] ;  [2] ;  [2] ;  [3] ;  [2] ;  [4]
  1. Northern Illinois Univ., DeKalb, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States); Purdue Univ., West Lafayette, IN (United States)
  4. Northern Illinois Univ., DeKalb, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 28; Journal Issue: 7; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1341436

Barkholtz, Heather M., Gallagher, James R., Li, Tao, Liu, Yuzi, Winans, Randall E., Miller, Jeffrey T., Liu, Di -Jia, and Xu, Tao. Lithium assisted “dissolution–alloying” synthesis of nanoalloys from individual bulk metals. United States: N. p., Web. doi:10.1021/acs.chemmater.6b00216.
Barkholtz, Heather M., Gallagher, James R., Li, Tao, Liu, Yuzi, Winans, Randall E., Miller, Jeffrey T., Liu, Di -Jia, & Xu, Tao. Lithium assisted “dissolution–alloying” synthesis of nanoalloys from individual bulk metals. United States. doi:10.1021/acs.chemmater.6b00216.
Barkholtz, Heather M., Gallagher, James R., Li, Tao, Liu, Yuzi, Winans, Randall E., Miller, Jeffrey T., Liu, Di -Jia, and Xu, Tao. 2016. "Lithium assisted “dissolution–alloying” synthesis of nanoalloys from individual bulk metals". United States. doi:10.1021/acs.chemmater.6b00216. https://www.osti.gov/servlets/purl/1341436.
@article{osti_1341436,
title = {Lithium assisted “dissolution–alloying” synthesis of nanoalloys from individual bulk metals},
author = {Barkholtz, Heather M. and Gallagher, James R. and Li, Tao and Liu, Yuzi and Winans, Randall E. and Miller, Jeffrey T. and Liu, Di -Jia and Xu, Tao},
abstractNote = {Here, we report new fundamental chemistry involved in the synthesis of bimetallic nanoalloys via dissolving the pure bulk transition metals in molten lithium. It is revealed at the atomic level that when two pure bulk transition metals such as Pd and Pt are placed in molten lithium (~200°C), they undergo a dissolution process in which the metal-metal bonds in pure bulk transition metals are completely ruptured, resulting in the existence of individual Pd and Pt atoms surrounded by lithium atoms, as is evident by synchrotron Xray adsorption techniques. Then, upon the conversion of metal lithium to LiOH in humid air, the Pd and Pt atoms undergo an alloying process, to aggregate into nanoalloys. This method was further expanded to include PdZn, which is notoriously difficult to prepare via traditional nanoalloy synthesis methods due to the easily oxidizable Zn component. The constantly reducing environment of metallic Li allowed for preparation of PdZn nanoalloys with minimal Zn oxidation via dissolution-alloying of individual bulk transition metals in molten lithium. Additionally, this lithium assisted “dissolutionalloying” method bypasses many complications intrinsic to conventional ion reductionbased nanoalloy synthesis including the necessity of ligated metal ions, the use of proper reducing agents and dispersing surfactants, and the presence of segregated phases due to different reduction potentials of the constituent metal ions.},
doi = {10.1021/acs.chemmater.6b00216},
journal = {Chemistry of Materials},
number = 7,
volume = 28,
place = {United States},
year = {2016},
month = {3}
}