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. 2023 Jun 27;6(13):7250-7257.
doi: 10.1021/acsaem.3c00969. eCollection 2023 Jul 10.

Polyimides as Promising Cathodes for Metal-Organic Batteries: A Comparison between Divalent (Ca2+, Mg2+) and Monovalent (Li+, Na+) Cations

Damien Monti  1 , Nagaraj Patil  2 , Ashley P Black  1 , Dionysios Raptis  3 , Andreas Mavrandonakis  2 , George E Froudakis  3 , Ibraheem Yousef  4 , Nicolas Goujon  5   6 , David Mecerreyes  5 , Rebeca Marcilla  2 , Alexandre Ponrouch  1   7
Affiliations

Polyimides as Promising Cathodes for Metal-Organic Batteries: A Comparison between Divalent (Ca2+, Mg2+) and Monovalent (Li+, Na+) Cations

Damien Monti et al. ACS Appl Energy Mater. .

Abstract

Ca- and Mg-based batteries represent a more sustainable alternative to Li-ion batteries. However, multivalent cation technologies suffer from poor cation mass transport. In addition, the development of positive electrodes enabling reversible charge storage currently represents one of the major challenges. Organic positive electrodes, in addition to being the most sustainable and potentially low-cost candidates, compared with their inorganic counterparts, currently present the best electrochemical performances in Ca and Mg cells. Unfortunately, organic positive electrodes suffer from relatively low capacity retention upon cycling, the origin of which is not yet fully understood. Here, 1,4,5,8-naphthalenetetracarboxylic dianhydride-derived polyimide was tested in Li, Na, Mg, and Ca cells for the sake of comparison in terms of redox potential, gravimetric capacities, capacity retention, and rate capability. The redox mechanisms were also investigated by means of operando IR experiments, and a parameter affecting most figures of merit has been identified: the presence of contact ion-pairs in the electrolyte.

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Conflict of interest statement

The authors declare no competing financial interest.

Figures

Figure 1
Figure 1
(a) Proposed charge/discharge mechanism of PNTCDA; Mn+ = Li+ or Ca2+. The GCPL profiles of PNTCDA at C/10 in 1 M LiTFSI in EC:PC (b) and in 0.5 M Ca(TFSI)2 in EC:PC (c) with their corresponding IR spectra in the 2000–1000 cm–1 (operando measurements).
Figure 2
Figure 2
GCPL potential (vs Ag/Ag2S) vs capacity curves of PNTCDA in 1 M (a) LiTFSI and (b) NaTFSI and 0.5 M (c) Mg(TFSI)2 and (d) Ca(TFSI)2 in EC:PC for the last cycles at 1C, C/2, C/10, and C/20 rates and (e, h) CVs (cycles 1, 5, 10, 20, and 30 at 5 mV/s) obtained using the same electrolytes.
Figure 3
Figure 3
Charge (red) and discharge (black) capacities vs cycle number of PNTCDA for 1 M (a) LiTFSI and (b) NaTFSI and 0.5 M (c) Mg(TFSI)2 and (d) Ca(TFSI)2 in EC:PC with their respective Coulombic efficiencies (blue) scanned at 1C, C/2, C/10, and C/20 rates.
Figure 4
Figure 4
(a) Normalized voltage versus capacity profiles (third cycle) and (b) discharge capacities vs cycle number (Coulombic efficiencies in empty squares) of PNTCDA electrodes in (blue) 0.05 M, (red) 0.1 M, and (black) 0.5 M Mg(TFSI)2 in EC:PC.
Figure 5
Figure 5
SEM images of PNTCDA electrodes as prepared (pristine) or stopped after 50 cycles (end of reduction) in 0.05, 0.1, or 0.5 M Mg(TFSI)2 in EC:PC.
See this image and copyright information in PMC

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