Combining Quinone Cathode and Ionic Liquid Electrolyte for Organic Sodium-Ion Batteries

Abstract

Coupling quinone cathode with ionic liquid electrolyte is demonstrated to build high-energy and long-life sodium-ion batteries. Computational and spectroscopic studies reveal that the inhibitory effect of ionic liquid on dissolution of quinone correlates with the strong polarity, weak electron donor ability, and low interaction energy. The calix[4]quinone and 5,7,12,14-pentacenetetrone cathodes exhibit significantly improved cycling performance in N-methyl-N-propylpyrrolidinium bis(trifluoromethanesulfonyl)amide than in ether electrolyte. These results would enlighten the design and application of ionic liquid and quinones for organic batteries. HIGHLIGHTSA facile strategy is proposed to suppress the dissolution of quinone electrodes Inhibitory effect of ILs correlates to polarity, donor number, and binding energy [PY13][TFSI] markedly inhibits quinone dissolution C4Q and PT cathodes exhibit better capacity retention in ILs than in ether Wang et al., Chem 5, 364-375 February 14, SUMMARYQuinone-based sodium-ion batteries (SIBs) are highly desirable electrochemical devices with high capacity and low cost but suffer from poor cycle life and low practical energy because of quinone dissolution in aprotic electrolyte. Herein, we report a facile strategy of using ionic liquid (IL) to tackle the dissolution of quinone electrodes. The inhibitory effect of ILs on quinone dissolution correlates with their polarity, donor number, and interaction energy, as revealed by combined density functional theory and spectroscopy studies. Particularly, in N-methyl-N-propylpyrrolidinium bis(trifluoromethanesulfonyl)amide ([PY13] [TFSI]) electrolyte with weak donor ability and large polarity, calix[4]quinone cathode exhibits high capacity (>400 mAh g À1 ) and superior capacity retention ($99.7% at 130 mA g À1 for 300 cycles), significantly outperforming that in etherbased electrolyte. Moreover, the remarkable cyclability and considerable rate capability of 5,7,12,14-pentacenetetrone in [PY13][TFSI] render it a promising sodium-storage material. This work would promote the development of highperformance SIBs with quinone electrodes and IL electrolyte.

A Calcium Organic Salt/rGO composite with Low Solubility and High Conductivity as a Sustainable Anode for Sodium‐Ion Batteries

“…Over the past few years, more and more researchers have focused on these materials. In spite of above advantages, the high solubility in organic electrolytes and poor electronic conductivity of organic materials hinder their electrochemical performance . Therefore, rational design from both a molecular and a materials level to solve these problems would advance the application of sustainable SIBs based on organic electrodes.…”

Cyclohexanehexone with Ultrahigh Capacity as Cathode Materials for Lithium‐Ion Batteries

“…Themethod can be seen in Figure 1a-c. First, we use DFT calculations to investigate several C n O n (n = 4, 5, 6,7,8,9) which have the potential to exhibit the highest theoretical capacity (957 mA hg À1 )a mong all carbonyl-based organic cathode materials based on the formula in Figure 1a. Compared with other cyclic ketones (C n O n , n = 4, 5,7,8,9), C 6 O 6 shows the highest theoretical working voltage (Figure 1b and Figure S1 in the Supporting Information).…”

“…TheT EM elemental mappings ( Figure S8) indicate that Cand Oare distributed uniformly in the C 6 O 6 sample.A dditionally,w ea lso investigated the thermal stability of C 6 O 6 .Asshown in the thermogravimetric curve ( Figure S9), there is no weight loss before 208 8 8C, implying the good thermal stability of C 6 O 6 ,w hich would be acceptable for practical applications concerning the safety issue. [8] After confirming the structure of C 6 O 6 ,w es tudied its electrochemical behavior in lithium batteries.A ccording to our previous work, [9] we selected 0.3 m LiTFSI-[PY13]-[TFSI] (N-methyl-N-propylpyrrolidinium bis(trifluoromethanesulfonyl)imide) as the electrolyte.W ef irst optimized the operating temperature and selected 70 8 8Casthe optimal one ( Figure S10). Note that in this work all the batteries operate at 70 8 8Cunless otherwise noted.…”

“…[11] In addition, ap revious work has revealed that the activity and structural evolution of aC 6 O 6 analogue (Na 2 C 6 O 6 )i ss ensitive to the selection of electrolyte. b) Calculated average working voltage and energy gap between HOMO and LUMO of C n O n (n = 4, 5, 6,7,8,9). a) The formula to calculate the theoreticalcapacity of different electrode materials.…”

Natural Compounds Gallic Acid Derivatives for Long‐Life Li/Na Organic Batteries

“…As so far, various organic materials such as free radical‐, quinine carbonyl‐ (C=O), organosulfur‐, imine‐ (C=N) and azo‐ (N=N) compounds have been applied in LIBs and SIBs . The double bonds are reduced by Li and Na in wide potential window, enabling them working as the anode and cathode materials in LIBs and SIBs.…”