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Title: Understanding crystallization pathways leading to manganese oxide polymorph formation

Abstract

Hydrothermal synthesis is challenging in metal oxide systems with diverse polymorphism, as reaction products are often sensitive to subtle variations in synthesis parameters. This sensitivity is rooted in the non-equilibrium nature of low-Temperature crystallization, where competition between different metastable phases can lead to complex multistage crystallization pathways. Here, we propose an ab initio framework to predict how particle size and solution composition influence polymorph stability during nucleation and growth. We validate this framework using in situ X-ray scattering, by monitoring how the hydrothermal synthesis of MnO2 proceeds through different crystallization pathways under varying solution potassium ion concentrations ([K+] = 0, 0.2, and 0.33 M). We find that our computed size-dependent phase diagrams qualitatively capture which metastable polymorphs appear, the order of their appearance, and their relative lifetimes. In conclusion, our combined computational and experimental approach offers a rational and systematic paradigm for the aqueous synthesis of target metal oxides.

Authors:
 [1];  [2]; ORCiD logo [3];  [4];  [1];  [5];  [5];  [4]; ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  4. Colorado School of Mines, Golden, CO (United States)
  5. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials by Design: Incorporating Metastability (CNGMD); National Renewable Energy Laboratory (NREL), Golden, CO (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1457088
Alternate Identifier(s):
OSTI ID: 1461258; OSTI ID: 1462356; OSTI ID: 1506381
Report Number(s):
NREL/JA-5F00-71965
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
AC36-08GO28308; AC02-05CH11231; AC02-76SF00515
Resource Type:
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; computational chemistry; materials chemistry; materials for energy and catalysis

Citation Formats

Chen, Bor -Rong, Sun, Wenhao, Kitchaev, Daniil A., Mangum, John S., Thampy, Vivek, Garten, Lauren M., Ginley, David S., Gorman, Brian P., Stone, Kevin H., Ceder, Gerbrand, Toney, Michael F., and Schelhas, Laura T. Understanding crystallization pathways leading to manganese oxide polymorph formation. United States: N. p., 2018. Web. doi:10.1038/s41467-018-04917-y.
Chen, Bor -Rong, Sun, Wenhao, Kitchaev, Daniil A., Mangum, John S., Thampy, Vivek, Garten, Lauren M., Ginley, David S., Gorman, Brian P., Stone, Kevin H., Ceder, Gerbrand, Toney, Michael F., & Schelhas, Laura T. Understanding crystallization pathways leading to manganese oxide polymorph formation. United States. https://doi.org/10.1038/s41467-018-04917-y
Chen, Bor -Rong, Sun, Wenhao, Kitchaev, Daniil A., Mangum, John S., Thampy, Vivek, Garten, Lauren M., Ginley, David S., Gorman, Brian P., Stone, Kevin H., Ceder, Gerbrand, Toney, Michael F., and Schelhas, Laura T. Fri . "Understanding crystallization pathways leading to manganese oxide polymorph formation". United States. https://doi.org/10.1038/s41467-018-04917-y.
@article{osti_1457088,
title = {Understanding crystallization pathways leading to manganese oxide polymorph formation},
author = {Chen, Bor -Rong and Sun, Wenhao and Kitchaev, Daniil A. and Mangum, John S. and Thampy, Vivek and Garten, Lauren M. and Ginley, David S. and Gorman, Brian P. and Stone, Kevin H. and Ceder, Gerbrand and Toney, Michael F. and Schelhas, Laura T.},
abstractNote = {Hydrothermal synthesis is challenging in metal oxide systems with diverse polymorphism, as reaction products are often sensitive to subtle variations in synthesis parameters. This sensitivity is rooted in the non-equilibrium nature of low-Temperature crystallization, where competition between different metastable phases can lead to complex multistage crystallization pathways. Here, we propose an ab initio framework to predict how particle size and solution composition influence polymorph stability during nucleation and growth. We validate this framework using in situ X-ray scattering, by monitoring how the hydrothermal synthesis of MnO2 proceeds through different crystallization pathways under varying solution potassium ion concentrations ([K+] = 0, 0.2, and 0.33 M). We find that our computed size-dependent phase diagrams qualitatively capture which metastable polymorphs appear, the order of their appearance, and their relative lifetimes. In conclusion, our combined computational and experimental approach offers a rational and systematic paradigm for the aqueous synthesis of target metal oxides.},
doi = {10.1038/s41467-018-04917-y},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41467-018-04917-y

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Cited by: 90 works
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Works referencing / citing this record:

Annealing induced a well-ordered single crystal δ-MnO2 and its electrochemical performance in zinc-ion battery
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