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Title: Fast Charge‐Transfer Rates in Li‐CO 2 Batteries with a Coupled Cation‐Electron Transfer Process

Journal Article · · Advanced Energy Materials
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  1. Department of Mechanical and Industrial Engineering University of Illinois at Chicago Chicago IL 60607 United States
  2. Department of Chemical Engineering University of Illinois at Chicago Chicago IL 60608 United States
  3. Department of Chemistry University of Illinois at Chicago Chicago IL 60607 United States
  4. Department of Chemical Engineering University of Illinois at Chicago Chicago IL 60608 United States, Materials Science Division Argonne National Laboratory Lemont IL 60439 United States
  5. Department of Mechanical and Industrial Engineering University of Illinois at Chicago Chicago IL 60607 United States, Materials Science Division Argonne National Laboratory Lemont IL 60439 United States
  6. Materials Science Division Argonne National Laboratory Lemont IL 60439 United States

Abstract Li‐CO 2 batteries with a high theoretical energy density (1876 Wh kg −1 ) have unique benefits for reversible carbon fixation for energy storage systems. However, due to lack of stable and highly active catalysts, the long‐term operation of Li‐CO 2 batteries is limited to low current densities (mainly <0.2 mA cm −2 ) that are far from practical conditions. In this work, it is discovered that, with an ionic liquid‐based electrolyte, highly active and stable transition metal trichalcogenide alloy catalysts of Sb 0.67 Bi 1.33 X 3 (X = S, Te) enable operation of the Li‐CO 2 battery at a very high current rate of 1 mA cm −2 for up to 220 cycles. It is revealed that: i) the type of chalcogenide (Te vs S) significantly affects the electronic and catalytic properties of the catalysts, ii) a coupled cation‐electron charge transfer process facilitates the carbon dioxide reduction reaction (CO 2 RR) occurring during discharge, and iii) the concentration of ionic liquid in the electrolyte controls the number of participating CO 2 molecules in reactions. A combination of these key factors is found to be crucial for a successful operation of the Li‐CO 2 chemistry at high current rates. This work introduces a new class of catalysts with potential to fundamentally solve challenges of this type of batteries.

Sponsoring Organization:
USDOE
Grant/Contract Number:
NONE; EE0009651
OSTI ID:
2322599
Alternate ID(s):
OSTI ID: 2568523
Journal Information:
Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 15 Vol. 14; ISSN 1614-6832
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

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