解锁立方相石榴石固体电解质中隐藏的化学空间，用于高效准全固态锂电池,Nature Communications

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解锁立方相石榴石固体电解质中隐藏的化学空间，用于高效准全固态锂电池
Nature Communications ( IF 14.7 ) Pub Date : 2022-12-10 , DOI: 10.1038/s41467-022-35287-1
Sung-Kyun Jung _{1,

2} , Hyeokjo Gwon ₁ , Hyungsub Kim ₃ , Gabin Yoon ₁ , Dongki Shin ₄ , Jihyun Hong ₄ , Changhoon Jung ₅ , Ju-Sik Kim ₁

Affiliation

石榴石型 Li ₇ La ₃ Zr ₂ O ₁₂ (LLZO) 固体电解质 (SE) 展示了对全固态锂金属电池应用具有吸引力的离子电导率特性。然而，LLZO 在与锂金属电极接触时的（电）化学稳定性对于开发实用电池而言并不令人满意。为了避免这个问题，我们报告了各种掺杂的立方相 LLZO SE 的制备，没有空位形成（即 Li = 7.0，例如 Li ₇ La ₃ Zr _0.5 Hf _0.5 Sc _0.5 Nb _0.5 O ₁₂和 Li ₇ La ₃ Zr _0.4Hf _0.4 Sn _0.4 Sc _0.4 Ta _0.4 O ₁₂ )。熵驱动合成方法允许进入立方相石榴石中隐藏的化学空间，并随着立方相成核从 750 °C 降至 400 °C 降低固态合成温度。我们证明，与具有低锂含量和相同原子种类的 SE（即 Li = 6.6，例如 Li _6.6 La ₃ Zr _0.4 Hf _0.4 Sn _0.4 Sc _0.2 Ta _0.6 O ）相比，Li = 7.0 的 SE 对锂金属显示出更好的还原稳定性₁₂ ). 此外，当 Li ₇La ₃ Zr _0.4 Hf _0.4 Sn _0.4 Sc _0.4 Ta _0.4 O ₁₂丸粒在 60 °C 下在纽扣电池配置中进行测试，该配置具有锂金属负极、LiNi _1/3 Co _1/3 Mn _1/3 O ₂基正极电极和基于离子液体的电解质在阴极|SE 界面，在 0.8 mA/cm ²和 60 °C 下经过 700 次循环后，放电容量保持率约为 92% 。

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Unlocking the hidden chemical space in cubic-phase garnet solid electrolyte for efficient quasi-all-solid-state lithium batteries

Garnet-type Li₇La₃Zr₂O₁₂ (LLZO) solid electrolytes (SE) demonstrates appealing ionic conductivity properties for all-solid-state lithium metal battery applications. However, LLZO (electro)chemical stability in contact with the lithium metal electrode is not satisfactory for developing practical batteries. To circumvent this issue, we report the preparation of various doped cubic-phase LLZO SEs without vacancy formation (i.e., Li = 7.0 such as Li₇La₃Zr_0.5Hf_0.5Sc_0.5Nb_0.5O₁₂ and Li₇La₃Zr_0.4Hf_0.4Sn_0.4Sc_0.4Ta_0.4O₁₂). The entropy-driven synthetic approach allows access to hidden chemical space in cubic-phase garnet and enables lower solid-state synthesis temperature as the cubic-phase nucleation decreases from 750 to 400 °C. We demonstrate that the SEs with Li = 7.0 show better reduction stability against lithium metal compared to SE with low lithium contents and identical atomic species (i.e., Li = 6.6 such as Li_6.6La₃Zr_0.4Hf_0.4Sn_0.4Sc_0.2Ta_0.6O₁₂). Moreover, when a Li₇La₃Zr_0.4Hf_0.4Sn_0.4Sc_0.4Ta_0.4O₁₂ pellet is tested at 60 °C in coin cell configuration with a Li metal negative electrode, a LiNi_1/3Co_1/3Mn_1/3O₂-based positive electrode and an ionic liquid-based electrolyte at the cathode|SE interface, discharge capacity retention of about 92% is delivered after 700 cycles at 0.8 mA/cm² and 60 °C.

更新日期：2022-12-10

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