Electrochemically
active covalent organic frameworks (COFs) are
promising electrode materials for Li-ion batteries. However, improving
the specific capacities of COF-based electrodes requires materials
with increased conductivity and a higher concentration of redox-active
groups. Here, we designed a series of pyrene-4,5,9,10-tetraone COF
(PT-COF) and carbon nanotube (CNT) composites (denoted as PT-COFX,
where
X
= 10, 30, and 50 wt % of CNT) to address
these challenges. Among the composites, PT-COF50 achieved a capacity
of up to 280 mAh g
–1
as normalized to the active
COF material at a current density of 200 mA g
–1
,
which is the highest capacity reported for a COF-based composite cathode
electrode to date. Furthermore, PT-COF50 exhibited excellent rate
performance, delivering a capacity of 229 mAh g
–1
at 5000 mA g
–1
(18.5C). Using
operando
Raman microscopy the reversible transformation of the redox-active
carbonyl groups of PT-COF was determined, which rationalizes an overall
4 e
–
/4 Li
+
redox process per pyrene-4,5,9,10-tetraone
unit, accounting for its superior performance as a Li-ion battery
electrode.
low specific capacity of 73 mAh g −1 at 500 mA g −1 in a Li-ion cell. However, the electrochemical performance was greatly enhanced by forming the tube-type core-shell structure of the composites (DAPQ-COFX). Using this approach, we achieved specific capacities of up to 162 mAh g −1 at 500 mA g −1 . By varying the composition of the DAPQ-COFX composite, it was found that DAPQ-COF50, which contained 50 wt% of CNT, exhibited the highest utilization of the redox-active sites (95%). Notably, the DAPQ-COF50 composite presents the best rate performance in COF-based electrode materials reported so far, facilitating ultrafast charge/discharge rates as high as 50 A g −1 -this means that the device can be fully charged in just 11 s.
This paper reports on the solubility and diffusivity of dissolved oxygen in a series of ionic liquids (ILs) based on the bis{(trifluoromethyl)sulfonyl}imide anion with a range of related alkyl and ether functionalised cyclic alkylammonium cations. Cyclic voltammetry has been used to observe the reduction of oxygen in ILs at a microdisk electrode and chronoamperometric measurements have then been applied to simultaneously determine both the concentration and the diffusion coefficient of oxygen in different ILs. The viscosity of the ILs and the calculated molar volume and free volume are also reported. It is found that, within this class of ILs, the oxygen diffusivity generally increases with decreasing viscosity of the neat IL. An inverse relationship between oxygen solubility and IL free volume is reported for the two IL families implying that oxygen is not simply occupying the available empty space. In addition, it is reported that the introduction of an ether-group into the IL cation structure promotes the diffusivity of dissolved oxygen but reduces the solubility of the gas.
During this work, a novel series of hydrophobic room temperature ionic liquids (ILs) based on five ether functionalized sulfonium cations bearing the bis{(trifluoromethyl)sulfonyl}imide, [NTf2]− anion were synthesized and characterized. Their physicochemical properties, such as density, viscosity and ionic conductivity, electrochemical window, along with thermal properties including phase transition behavior and decomposition temperature, have been measured. All of these ILs showed large liquid range temperature, low viscosity, and good conductivity. Additionally, by combining DFT calculations along with electrochemical characterization it appears that these novel ILs show good electrochemical stability windows, suitable for the potential application as electrolyte materials in electrochemical energy storage devices.
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