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Most existing lithium batteries (LIBs) are integrated with graphite anodes, with a capacity of about 350 milliampere hours (mAh) per gram. The capacity of silicon anode is almost 10 times that of graphite anode (about 2800 milliampere hours per gram), so in theory, a more compact and lighter lithium battery can be developed.

Although silicon anode has higher capacity, so far, silicon anode cannot compete with graphite anode, because silicon will expand and contract during the operation of the battery, so the outer protective layer of the anode is easy to break when the battery is working. In a paper recently published in the journal NatureEnergy, researchers from the University of Maryland and the Army Research Laboratory proposed a new electrolyte design that can overcome the limitations of existing silicon anodes.

Si particles covered with LiF rich SEI layer

Silicon anode and its formed solid electrolyte interphase layer (SEI) protective layer are easier to be crushed during battery operation. Because SEI and Si are firmly combined, both have experienced a lot of changes, said Ji Chen, one of the important researchers conducting this research.

SEI is a protective layer, which will naturally form when positive particles directly contact with the electrolyte. The purpose of this protective layer is to prevent further reaction inside the battery and separate the anode and electrolyte.

If this protective layer is damaged during expansion or contraction of the Si anode particles, newly exposed anode particles will continuously react with the electrolyte until electrolyte runs out during battery cycle, said Oleg Borodin, senior chemist involved in research at Army Research Laboratory.

For more than ten years, research groups around the world have been working hard to overcome the problem that hinders the use of silicon anode in LIB. The important thing is to design flexible and organic SEI to expand with the anode. However, it turns out that most of the solutions developed by them are either completely ineffective or slightly effective, so they can only partially prevent SEI damage.

For a long time, the LIB research community has been trying to design and transfer the technology for the use of high-capacity anode such as Si, said Chung Wang, a professor in the Department of Chemical and Biomolecular Engineering at the University of Maryland (UMD), who is also the director of the UMD Extreme Battery Research Center. Most of these researchers conduct research on Si materials by introducing expensive nano manufacturing processes. We tried to solve this problem by designing electrolyte of high capacity anode and corresponding SEI, but we tried different methods.

Chen, Borodin, Wang and their colleagues have designed an electrolyte that can improve the performance of micro silicon anode in LIB and prevent its external protective layer from being damaged. Compared with the solution proposed previously, their method greatly reduces the degradation of electrolyte, thus greatly prolonging the cycle time before the battery loses its capacity.

The ultimate goal of researchers' research is to determine a universal plug and play solution to promote the development of high-capacity anode for lithium battery. In order to achieve this goal, they used the most advanced mixture of salt LiPF6 and ether solvent to design the electrolyte, forming a very solid SEI protective layer rich in LiF.

The special solvation structure (the mutual use between salt and solvent) and the huge gap between the reduction tendency of salt and solvent promote the formation of unique LiF rich SEI on Si, which is extremely beneficial to the battery recycling high capacity Si anode. Oleg explained. The electrolyte we designed provides the current LIB technology with a plug and play solution that can be realized without expensive processing technology, while maintaining an unprecedented high cycle stability.

The recent research of Chen, Borodin, Wang and their colleagues has proved that it is actually possible to achieve good circulation and high efficiency in LIB containing silicon anode, which can be achieved only by replacing the electrolyte inside the battery, which was previously considered impractical or completely unfeasible. The principle behind their electrolyte design can also be applied to all high-capacity alloy anodes theoretically. In the future, this design can create a lithium battery with better performance, which contains anodes made of materials other than graphite.

Our research results point out a new direction for electrolyte design, which can enable global research teams to have confidence in the application of high-capacity anode materials in LIB. Wang said. Our next step will be to improve the voltage range of electrolyte and try to license this technology to battery manufacturers.

The title of the paper is "Electrolytedesign for Li F richsolid– electrolyteinterface to enable high performance microsized lloyanodes for batteries".

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