期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 115, 期 31, 页码 7890-7895出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1800284115
关键词
Materials by Design; in situ X-ray studies; electronic structure calculations
资金
- Welch Foundation [A-1890-20160319]
- US Department of Energy (DOE), Office of Basic Energy Sciences [DEAC0298CH1088]
- DOE Office of Science by Argonne National Laboratory [DE-AC02-06CH11357]
- DOE Office of Science by Brookhaven National Laboratory [DE-SC0012704]
The lack of a mechanistic framework for chemical reactions forming inorganic extended solids presents a challenge to accelerated materials discovery. We demonstrate here a combined computational and experimental methodology to tackle this problem, in which in situ X-ray diffraction measurements monitor solid-state reactions and deduce reaction pathways, while theoretical computations rationalize reaction energetics. The method has been applied to the La2CuO4-xSx (0 <= x <= 4) quaternary system, following an earlier prediction that enhanced superconductivity could be found in these new lanthanum copper(II) oxysulfide compounds. In situ diffraction measurements show that reactants containing Cu(II) and S(2-) ions undergo redox reactions, leaving their ions in oxidation states that are incompatible with forming the desired new compounds. Computations of the reaction energies confirm that the observed synthetic pathways are indeed favored over those that would hypothetically form the suggested compounds. The consistency between computation and experiment in the La2CuO4-xSx system suggests a role for predictive theory: to identify and to explicate new synthetic routes for forming predicted compounds.
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