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Title: High-Pressure Synthesis: A New Frontier in the Search for Next-Generation Intermetallic Compounds

Abstract

The application of high pressure adds an additional dimension to chemical phase space, opening up an unexplored expanse bearing tremendous potential for discovery. Our continuing mission is to explore this new frontier, to seek out new intermetallic compounds and new solid-state bonding. Simple binary elemental systems, specifically those composed of pairs of elements that do not form compounds under ambient pressures, can yield novel crystalline phases under compression. Thus, high-pressure synthesis can provide access to solid-state compounds that cannot be formed with traditional thermodynamic methods. An emerging approach for the rapid exploration of composition–pressure–temperature phase space is the use of hand-held high-pressure devices known as diamond anvil cells (DACs). These devices were originally developed by geologists as a way to study minerals under conditions relevant to the earth’s interior, but they possess a host of capabilities that make them ideal for high-pressure solid-state synthesis. Of particular importance, they offer the capability for in situ spectroscopic and diffraction measurements, thereby enabling continuous reaction monitoring—a powerful capability for solid-state synthesis. Here, we offer an overview of this approach in the context of research we have performed in the pursuit of new intermetallic compounds. We start with a discussion of pressure as amore » fundamental experimental variable that enables the formation of intermetallic compounds that cannot be isolated under ambient conditions. We then introduce the DAC apparatus and explain how it can be repurposed for use as a synthetic vessel with which to explore this phase space, going to extremes of pressure where no chemist has gone before. The remainder of the Account is devoted to discussions of recent experiments we have performed with this approach that have led to the discovery of novel intermetallic compounds in the Fe–Bi, Cu–Bi, and Ni–Bi systems, with a focus on the cutting-edge methods that made these experiments possible. We review the use of in situ laser heating at high pressure, which led to the discovery of FeBi2, the first binary intermetallic compound in the Fe–Bi system. Our work in the Cu–Bi system is described in the context of in situ experiments carried out in the DAC to map its high-pressure phase space, which revealed two intermetallic phases (Cu11Bi7 and CuBi). Finally, we review the discovery of β-NiBi, a novel high-pressure phase in the Ni–Bi system. We hope that this Account will inspire the next generation of solid-state chemists to boldly explore high-pressure phase space.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]
  1. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States); Carnegie Inst. of Science, Washington, DC (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE National Nuclear Security Administration (NNSA); US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)
OSTI Identifier:
1596767
Grant/Contract Number:  
SC0018092; AC02-06CH11357; FG02-94ER14466; NA0001974; FG02-99ER45775; FA9550-14-1-0358; FA9550-17-1-0247; EAR-1634415
Resource Type:
Accepted Manuscript
Journal Name:
Accounts of Chemical Research
Additional Journal Information:
Journal Volume: 51; Journal Issue: 6; Journal ID: ISSN 0001-4842
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Physical and chemical processes; Carbon; Bismuth; Lasers; Intermetallics

Citation Formats

Walsh, James P. S., and Freedman, Danna E. High-Pressure Synthesis: A New Frontier in the Search for Next-Generation Intermetallic Compounds. United States: N. p., 2018. Web. doi:10.1021/acs.accounts.8b00143.
Walsh, James P. S., & Freedman, Danna E. High-Pressure Synthesis: A New Frontier in the Search for Next-Generation Intermetallic Compounds. United States. doi:10.1021/acs.accounts.8b00143.
Walsh, James P. S., and Freedman, Danna E. Tue . "High-Pressure Synthesis: A New Frontier in the Search for Next-Generation Intermetallic Compounds". United States. doi:10.1021/acs.accounts.8b00143. https://www.osti.gov/servlets/purl/1596767.
@article{osti_1596767,
title = {High-Pressure Synthesis: A New Frontier in the Search for Next-Generation Intermetallic Compounds},
author = {Walsh, James P. S. and Freedman, Danna E.},
abstractNote = {The application of high pressure adds an additional dimension to chemical phase space, opening up an unexplored expanse bearing tremendous potential for discovery. Our continuing mission is to explore this new frontier, to seek out new intermetallic compounds and new solid-state bonding. Simple binary elemental systems, specifically those composed of pairs of elements that do not form compounds under ambient pressures, can yield novel crystalline phases under compression. Thus, high-pressure synthesis can provide access to solid-state compounds that cannot be formed with traditional thermodynamic methods. An emerging approach for the rapid exploration of composition–pressure–temperature phase space is the use of hand-held high-pressure devices known as diamond anvil cells (DACs). These devices were originally developed by geologists as a way to study minerals under conditions relevant to the earth’s interior, but they possess a host of capabilities that make them ideal for high-pressure solid-state synthesis. Of particular importance, they offer the capability for in situ spectroscopic and diffraction measurements, thereby enabling continuous reaction monitoring—a powerful capability for solid-state synthesis. Here, we offer an overview of this approach in the context of research we have performed in the pursuit of new intermetallic compounds. We start with a discussion of pressure as a fundamental experimental variable that enables the formation of intermetallic compounds that cannot be isolated under ambient conditions. We then introduce the DAC apparatus and explain how it can be repurposed for use as a synthetic vessel with which to explore this phase space, going to extremes of pressure where no chemist has gone before. The remainder of the Account is devoted to discussions of recent experiments we have performed with this approach that have led to the discovery of novel intermetallic compounds in the Fe–Bi, Cu–Bi, and Ni–Bi systems, with a focus on the cutting-edge methods that made these experiments possible. We review the use of in situ laser heating at high pressure, which led to the discovery of FeBi2, the first binary intermetallic compound in the Fe–Bi system. Our work in the Cu–Bi system is described in the context of in situ experiments carried out in the DAC to map its high-pressure phase space, which revealed two intermetallic phases (Cu11Bi7 and CuBi). Finally, we review the discovery of β-NiBi, a novel high-pressure phase in the Ni–Bi system. We hope that this Account will inspire the next generation of solid-state chemists to boldly explore high-pressure phase space.},
doi = {10.1021/acs.accounts.8b00143},
journal = {Accounts of Chemical Research},
number = 6,
volume = 51,
place = {United States},
year = {2018},
month = {5}
}

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