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Lin CF, Qi Y, Gregorczyk K, et al. Nanoscale Protection Layers To Mitigate Degradation in High-Energy Electrochemical Energy Storage Systems. Acc Chem Res. 2018;51(1):97-106doi: 10.1021/acs.accounts.7b00524.
Lin, C. F., Qi, Y., Gregorczyk, K., Lee, S. B., & Rubloff, G. W. (2018). Nanoscale Protection Layers To Mitigate Degradation in High-Energy Electrochemical Energy Storage Systems. Accounts of chemical research, 51(1), 97-106. https://doi.org/10.1021/acs.accounts.7b00524
Lin, Chuan-Fu, et al. "Nanoscale Protection Layers To Mitigate Degradation in High-Energy Electrochemical Energy Storage Systems." Accounts of chemical research vol. 51,1 (2018): 97-106. doi: https://doi.org/10.1021/acs.accounts.7b00524
Lin CF, Qi Y, Gregorczyk K, Lee SB, Rubloff GW. Nanoscale Protection Layers To Mitigate Degradation in High-Energy Electrochemical Energy Storage Systems. Acc Chem Res. 2018 Jan 16;51(1):97-106. doi: 10.1021/acs.accounts.7b00524. Epub 2018 Jan 02. PMID: 29293316.
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Acc Chem Res. 2018 Jan 16;51(1):97-106. doi: 10.1021/acs.accounts.7b00524. Epub 2018 Jan 02.

Nanoscale Protection Layers To Mitigate Degradation in High-Energy Electrochemical Energy Storage Systems.

Accounts of chemical research

Chuan-Fu Lin, Yue Qi, Keith Gregorczyk, Sang Bok Lee, Gary W Rubloff

Affiliations

  1. Department of Materials Science and Engineering, University of Maryland , College Park, Maryland 20742, United States.
  2. Institute for Systems Research, University of Maryland , College Park, Maryland 20742, United States.
  3. Department of Chemical Engineering and Materials Science, Michigan State University , East Lansing, Michigan 48824, United States.
  4. Department of Chemistry and Biochemistry, University of Maryland , College Park, Maryland 20742, United States.

PMID: 29293316 DOI: 10.1021/acs.accounts.7b00524

Abstract

In the pursuit of energy storage devices with higher energy and power, new ion storage materials and high-voltage battery chemistries are of paramount importance. However, they invite-and often enhance-degradation mechanisms, which are reflected in capacity loss with charge/discharge cycling and sometimes in safety problems. Degradation mechanisms are often driven by fundamentals such as chemical and electrochemical reactions at electrode-electrolyte interfaces, volume expansion and stress associated with ion insertion and extraction, and profound inhomogeneity of electrochemical behavior. While it is important to identify and understand these mechanisms at some reasonable level, it is even more critical to design strategies to mitigate these degradation pathways and to develop means to implement and validate the strategies. A growing set of research highlights the mitigation benefits achievable by forming thin protection layers (PLs) intentionally created as artificial interphase regions at the electrode-electrolyte interface. These advances illustrate a promising-perhaps even generic-pathway for enabling higher-energy and higher-voltage battery configurations. In this Account, we summarize examples of such PLs that serve as mitigation strategies to avoid degradation in lithium metal anodes, conversion-type electrode materials, and alloy-type electrodes. Examples are chosen from a larger body of electrochemical degradation research carried out in Nanostructures for Electrical Energy Storage (NEES), our DOE Energy Frontier Research Center. Overall, we argue on the basis of experimental and theoretical evidence that PLs effectively stabilize the electrochemical interfaces to prevent parasitic chemical and electrochemical reactions and mitigate the structural, mechanical, and compositional degradation of the electrode materials at the electrode-electrolyte interfaces. The evidenced improvement in performance metrics is accomplished by (1) establishing a homogeneous interface for ion insertion and extraction, (2) providing mechanical constraints to maintain structural integrity and robust electronic and ionic conduction pathways, and (3) introducing spatial confinements on the electrode material matrix to alter the phase transformation (delaying the occurrence of the conversion reaction) upon Li insertion, which results in superior electrode performance, excellent capacity retention, and improved reversibility. Taken together, these examples portray a valuable role for thin protection layers synthesized over electrode surfaces, both for their benefit to cycle stability and for revealing insights into degradation and mitigation mechanisms. Furthermore, they underscore the impact of complex electrochemical behavior at nanoscale materials and nanostructure interfaces in modulating the behavior of energy storage devices at the mesoscale and macroscale.

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