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According to foreign media reports, the international team led by the Institute of Superconductivity and Electronic Materials of the University of Wollongong has confirmed that the structural stability of lithium battery cathode materials can be improved by introducing new molecular orbital interactions.

(: University of Wollongong)

For the electric vehicle industry, it is one of the important challenges to produce better cathode materials for high-performance lithium batteries. In this study, researchers used the facilities and technology of the Australian Nuclear Science and Technology Organization (ANSTO) to prove that doping germanium in the promising cathode material LiNi0.5Mn1.5O4 (LNMO) can significantly enhance the mutual use of 4s-2p orbitals between oxygen and metal cations. Relatively speaking, 4s-2p orbits are not common. However, researchers have found a compound in the literature, in which the valence state of germanium is+3, making the electronic configuration ([Ar] 3d104s1) possible, in which the 4s transition metal orbital electrons can be used with unpaired electrons on the oxygen 2p orbital, resulting in the hybrid 4s-2p orbital.

In LNMO materials, 4s-2p orbital can achieve structural stability. This can be determined through the synchrotron and neutron experiments of the Australian Synchrotron of ANSTO and the Australian Center for Neutron Scattering, as well as other methods.

The team used neutron and (laboratory based) X-ray powder diffraction, as well as microscope, to confirm the doped germanium in LNMO structure (with Fd3 ̅ M space group symmetry). The valence state of germanium dopant is very important for research. Therefore, researchers conducted experimental X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS) measurements at the Australian synchrotron. The results show that the average valence state of germanium dopant is+3.56, and the valence states of germanium at 16c and 16d sites are+3 and+4, respectively. This observation is supported by the density functional theory (DFT) calculation results.

Researchers evaluated the electrochemical performance of the battery containing LNMO and compared it with the LNMO battery containing 4s-2p orbital hybridization (called 4s-LNMO). The evaluation found that doping 2% germanium can help to achieve better structural stability, reduce the voltage polarization of the battery, and improve the energy density and high voltage output. Researcher Dr. GemengLiang said: Researchers want to understand the diffusion kinetics of lithium in the two materials. The results show that lithium diffuses faster in the material and can be charged faster after introducing germanium into the system.

After completing the performance test, Dr. Liang used the near-edge X-ray absorption spectrum (NEXAFS) based on synchrotron on the soft X-ray beam line to obtain more detailed information about the electronic structure of active substances during the cycle. The spectral data under the open-circuit voltage of the battery showed that the peak intensity of 4s-LNMO material increased significantly at the corresponding position of 4s-2p orbital hybridization, which further verified the successful introduction of the new 4s-LNMO orbital interaction. Dr. Bruce Cowie, one of the researchers and instrument scientist, said: Researchers can see the unfilled orbit and connect it with the filled orbit in a unique but complex way. On this basis, the chemical properties of the system can be better described by quantum mechanical calculation or comparison with similar materials.

NEXAFS data also help to evaluate the behavior of manganese in materials. Dr. Liang said that preventing the dissolution of manganese into the electrolyte can prevent the formation of Mn+2 and+3 in the structure, which is helpful to prevent the degradation of the structure. NEXAFS results show that there is only a small amount of Mn3+in 4s-LNMO, but no obvious Mn2+, which further improves the structural stability of the material.

In situ experiments conducted on the powder diffraction beam line of the Australian synchrotron, researchers explored the material structure behavior during the battery cycle. Using these data, the team confirmed that the adverse two-phase reaction in 4s-LNMO was suppressed under high operating voltage. The researchers said that orbital hybridization is a quite new concept in battery research, and has great prospects in solving battery performance problems. It is worth mentioning that this method can be extended to other battery materials.

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