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Title: Discovery of Calcium-Metal Alloy Anodes for Reversible Ca-Ion Batteries

Abstract

Ca-ion batteries (CIBs) show promise to achieve the high energy density required by emerging applications like electric vehicles because of their potentially improved capacities and high operating voltages. The development of CIBs is hindered by the failure of traditional graphite and calcium metal anodes due to the intercalation difficulty and the lack of efficient electrolytes. Recently, a high voltage (4.45 V) CIB cell using Sn as the anode has been reported to achieve a remarkable cyclability (>300 cycles). The calciation of Sn is observed to end at Ca 7Sn 6, which is surprising, since higher Ca-content compounds are known (e.g., Ca 2Sn). Here, the Sn electrochemical calciation reaction process is investigated computationally and the reaction driving force as a function of Ca content is explored using density functional theory (DFT) calculations. This exploration allows the identification of threshold voltages which govern the limits of the calciation process. This information is then used to design a four-step screening strategy and high-throughput DFT is utilized to search for anode materials with higher properties. Many metalloids (Si, Sb, Ge), (post-)transition metals (Al, Pb, Cu, Cd, CdCu 2) are predicted to be promising inexpensive anode candidates and warrant further experimental investigations.

Authors:
ORCiD logo [1];  [2];  [3];  [2]
  1. Department of Chemistry and Chemical Biology, Harvard University, 12 Oxford Street Cambridge MA 02138 USA; Department of Materials Science and Engineering, Northwestern University, 2220 Campus Drive Evanston IL 60208 USA
  2. Department of Materials Science and Engineering, Northwestern University, 2220 Campus Drive Evanston IL 60208 USA
  3. Department of Chemistry and Chemical Biology, Harvard University, 12 Oxford Street Cambridge MA 02138 USA; Department of Chemistry and Department of Computer Science, University of Toronto, Toronto Ontario M5S 3H6 Canada; Vector Institute for Artificial Intelligence, Toronto Ontario M5S 1M1 Canada; Canadian Institute for Advanced Research (CIFAR) Senior Fellow, Toronto Ontario M5S 1M1 Canada
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Electrical Energy Storage (CEES); Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1530588
Grant/Contract Number:  
SC0008688; AC02-06CH11357; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 9; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English

Citation Formats

Yao, Zhenpeng, Hegde, Vinay I., Aspuru-Guzik, Alán, and Wolverton, Chris. Discovery of Calcium-Metal Alloy Anodes for Reversible Ca-Ion Batteries. United States: N. p., 2019. Web. doi:10.1002/aenm.201802994.
Yao, Zhenpeng, Hegde, Vinay I., Aspuru-Guzik, Alán, & Wolverton, Chris. Discovery of Calcium-Metal Alloy Anodes for Reversible Ca-Ion Batteries. United States. doi:10.1002/aenm.201802994.
Yao, Zhenpeng, Hegde, Vinay I., Aspuru-Guzik, Alán, and Wolverton, Chris. Fri . "Discovery of Calcium-Metal Alloy Anodes for Reversible Ca-Ion Batteries". United States. doi:10.1002/aenm.201802994.
@article{osti_1530588,
title = {Discovery of Calcium-Metal Alloy Anodes for Reversible Ca-Ion Batteries},
author = {Yao, Zhenpeng and Hegde, Vinay I. and Aspuru-Guzik, Alán and Wolverton, Chris},
abstractNote = {Ca-ion batteries (CIBs) show promise to achieve the high energy density required by emerging applications like electric vehicles because of their potentially improved capacities and high operating voltages. The development of CIBs is hindered by the failure of traditional graphite and calcium metal anodes due to the intercalation difficulty and the lack of efficient electrolytes. Recently, a high voltage (4.45 V) CIB cell using Sn as the anode has been reported to achieve a remarkable cyclability (>300 cycles). The calciation of Sn is observed to end at Ca7Sn6, which is surprising, since higher Ca-content compounds are known (e.g., Ca2Sn). Here, the Sn electrochemical calciation reaction process is investigated computationally and the reaction driving force as a function of Ca content is explored using density functional theory (DFT) calculations. This exploration allows the identification of threshold voltages which govern the limits of the calciation process. This information is then used to design a four-step screening strategy and high-throughput DFT is utilized to search for anode materials with higher properties. Many metalloids (Si, Sb, Ge), (post-)transition metals (Al, Pb, Cu, Cd, CdCu2) are predicted to be promising inexpensive anode candidates and warrant further experimental investigations.},
doi = {10.1002/aenm.201802994},
journal = {Advanced Energy Materials},
number = 9,
volume = 9,
place = {United States},
year = {2019},
month = {1}
}

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