Abstract
Advancements in many modern technologies rely on the continuous need for materials discovery. However, the design of synthesis routes leading to new and targeted solid-state materials requires understanding of reactivity patterns1–3. Advances in synthesis science are necessary to increase efficiency and accelerate materials discovery4–10. We present a highly effective methodology for the rational discovery of materials using high-temperature solutions or fluxes having tunable solubility. This methodology facilitates product selection by projecting the free-energy landscape into real synthetic variables: temperature and flux ratio. We demonstrate the effectiveness of this technique by synthesizing compounds in the chalcogenide system of A(Ba)-Cu-Q(O) (Q = S or Se; A = Na, K or Rb) using mixed AOH/AX (A = Li, Na, K or Rb; X = Cl or I) fluxes. We present 30 unreported compounds or compositions, including more than ten unique structural types, by systematically varying the temperature and flux ratios without requiring changing the proportions of starting materials. Also, we found that the structural dimensionality of the compounds decreases with increasing reactant solubility and temperature. This methodology serves as an effective general strategy for the rational discovery of inorganic solids.
Original language | English (US) |
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Pages (from-to) | 72-77 |
Number of pages | 6 |
Journal | Nature |
Volume | 612 |
Issue number | 7938 |
DOIs | |
State | Published - Dec 1 2022 |
Funding
This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. Work carried out at the Center for Nanoscale Materials (SEM, ACAT and Carbon high-performance computing cluster), a US Department of Energy (DOE) Office of Science User Facility, was supported by the US DOE Office of Basic Energy Sciences under contract no. DE-AC02-06CH11357. The computational work is supported by the US DOE Office of Science Scientific User Facilities AI/ML project titled 'A digital twin for spatiotemporally resolved experiments.' M.K.Y.C. acknowledges support from the BES SUFD Early Career award. Work at the beamlines 15-IDD and 17-BM at the Advanced Photon Source (APS) at Argonne National Laboratory was supported by the US DOE, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02-06CH11357. NSF’s ChemMatCARS Sector 15 is supported by the Divisions of Chemistry (CHE) and Materials Research (DMR), National Science Foundation, under grant no. NSF/CHE-1834750. This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. Work carried out at the Center for Nanoscale Materials (SEM, ACAT and Carbon high-performance computing cluster), a US Department of Energy (DOE) Office of Science User Facility, was supported by the US DOE Office of Basic Energy Sciences under contract no. DE-AC02-06CH11357. The computational work is supported by the US DOE Office of Science Scientific User Facilities AI/ML project titled 'A digital twin for spatiotemporally resolved experiments.' M.K.Y.C. acknowledges support from the BES SUFD Early Career award. Work at the beamlines 15-IDD and 17-BM at the Advanced Photon Source (APS) at Argonne National Laboratory was supported by the US DOE, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02-06CH11357. NSF’s ChemMatCARS Sector 15 is supported by the Divisions of Chemistry (CHE) and Materials Research (DMR), National Science Foundation, under grant no. NSF/CHE-1834750.
ASJC Scopus subject areas
- General
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CSD 2184426: Experimental Crystal Structure Determination
Zhou, X. (Contributor), Kolluru, V. S. C. (Contributor), Xu, W. (Contributor), Wang, L. (Contributor), Chang, T. (Contributor), Chen, Y.-S. (Contributor), Yu, L. (Contributor), Wen, J. (Contributor), Chan, M. K. Y. (Contributor), Chung, D. Y. (Contributor), Chung, D. Y. (Contributor) & Kanatzidis, M. G. (Contributor), FIZ Karlsruhe - Leibniz Institute for Information Infrastructure, 2022
DOI: 10.25505/fiz.icsd.cc2cb2c5, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.25505/fiz.icsd.cc2cb2c5&sid=DataCite
Dataset
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CSD 2184424: Experimental Crystal Structure Determination
Zhou, X. (Contributor), Kolluru, V. S. C. (Contributor), Xu, W. (Contributor), Wang, L. (Contributor), Chang, T. (Contributor), Chen, Y.-S. (Contributor), Yu, L. (Contributor), Wen, J. (Contributor), Chan, M. K. Y. (Contributor), Chung, D. Y. (Contributor), Chung, D. Y. (Contributor) & Kanatzidis, M. G. (Contributor), FIZ Karlsruhe - Leibniz Institute for Information Infrastructure, 2022
DOI: 10.25505/fiz.icsd.cc2cb293, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.25505/fiz.icsd.cc2cb293&sid=DataCite
Dataset
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CSD 2184433: Experimental Crystal Structure Determination
Zhou, X. (Contributor), Kolluru, V. S. C. (Contributor), Xu, W. (Contributor), Wang, L. (Contributor), Chang, T. (Contributor), Chen, Y.-S. (Contributor), Yu, L. (Contributor), Wen, J. (Contributor), Chan, M. K. Y. (Contributor), Chung, D. Y. (Contributor), Chung, D. Y. (Contributor) & Kanatzidis, M. G. (Contributor), FIZ Karlsruhe - Leibniz Institute for Information Infrastructure, 2022
DOI: 10.25505/fiz.icsd.cc2cb2ld, http://www.ccdc.cam.ac.uk/services/structure_request?id=doi:10.25505/fiz.icsd.cc2cb2ld&sid=DataCite
Dataset