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Magnesium Polymer Electrolytes Based on the Polycarbonate Poly(2-butyl-2-ethyltrimethylene-carbonate).

David A SundermannBumjun ParkValerian HirschbergJennifer L SchaeferPatrick Theato
Published in: ACS omega (2023)
Magnesium electrolytes based on a polycarbonate with either magnesium tetrakis(hexafluoroisopropyloxy) borate (Mg(B(HFIP) 4 ) 2 ) or magnesium bis(trifluoromethanesulfonyl)imide (Mg(TFSI) 2 ) for magnesium batteries were prepared and characterized. The side-chain-containing polycarbonate, poly(2-butyl-2-ethyltrimethylene carbonate) (P(BEC)), was synthesized by ring opening polymerization (ROP) of 5-ethyl-5-butylpropane oxirane ether carbonate (BEC) and mixed with Mg(B(HFIP) 4 ) 2 or Mg(TFSI) 2 to form low- and high-salt-concentration polymer electrolytes (PEs). The PEs were characterized by impedance spectroscopy, differential scanning calorimetry (DSC), rheology, linear sweep voltammetry, cyclic voltammetry, and Raman spectroscopy. A transition from classical salt-in-polymer electrolytes to polymer-in-salt electrolytes was indicated by a significant change in glass transition temperature as well as storage and loss moduli. Ionic conductivity measurements indicated the formation of polymer-in-salt electrolytes for the PEs with 40 mol % Mg(B(HFIP) 4 ) 2 ( HFIP40 ). In contrast, the 40 mol % Mg(TFSI) 2 PEs showed mainly the classical behavior. HFIP40 was further found to have an oxidative stability window greater than 6 V vs Mg/Mg 2+ , but showed no reversible stripping-plating behavior in an Mg||SS cell.
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