Lithium-ion batteries are currently widely used in various portable electronic devices, and are expected to be used in large-scale applications in electric vehicles and smart grids. High-capacity, renewable, environmentally friendly, low-cost lithium battery cathode materials have become the current research hotspot. Organic electrode materials containing carbon, hydrogen, oxygen and other elements are considered to be very promising next-generation lithium-ion battery cathode materials due to their structural designability, environmental friendliness, and low cost. However, these materials still face problems such as low actual capacity (<600 mA h g-1) and easy dissolution in organic electrolytes, resulting in lower energy density and severe capacity decay. Therefore, how to design and synthesize an organic cathode material with ultra-high capacity and solve its dissolution problem in the electrolyte is of great significance.

Recently, the team of academician Chen Jun of Nankai University designed, synthesized and studied a kind of ultra-high capacity lithium ion battery cathode material-cyclohexanone. According to the molecular design (Figure 1a-c), among many organic carbonyl cathode materials, the cyclic ketone material composed only of carbonyl group does not have any non-electrochemically active structural unit, so it reflects the current highest theoretical specific capacity (957 mA h g-1).


Figure 1. Molecular design of high-capacity organic carbonyl cathode materials and the synthesis and reaction mechanism of cyclohexanone

First, the researchers synthesized cyclohexanone via dehydration (Figure 1d). The reaction mechanism of cyclohexanone was studied by infrared and Raman characterization methods. The results showed that the conversion of carbonyl and enol groups occurred during the charging and discharging process. And further use density functional theory to calculate the reaction process of cyclohexanone deintercalation of lithium (Figure 2). Next, the electrochemical performance of cyclohexanone in lithium-ion batteries was studied. The results showed that the discharge specific capacity of cyclohexanone could reach 902 mA h g-1, and the average discharge platform was about 1.7 V. In addition, due to the low solubility of cyclohexanone in ionic liquids with high polarity, it has better cycle performance in ionic liquid-based electrolytes. This work provides a new idea for the design, preparation and battery application of high-capacity organic electrode materials.


Figure 2. Theoretical calculation and simulation of the reaction mechanism of cyclohexanone

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