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首页> 外文期刊>Journal of Materials Research >Mechanism of the interfacial reaction between cation-deficient La_(0.56)Li_(0.33)TiO_3 and metallic lithium at room temperature
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Mechanism of the interfacial reaction between cation-deficient La_(0.56)Li_(0.33)TiO_3 and metallic lithium at room temperature

机译：室温下缺阳离子的La_（0.56）Li_（0.33）TiO_3与金属锂的界面反应机理

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摘要

We used x-ray diffractometry (XRD), x-ray photoelectron spectrometry (XPS), and secondary-ion mass spectrometry (SIMS) to investigate the mechanism of the interfacial room-temperature (RT) chemical reaction between cation-deficient La_(0.56)Li_(0.33)TiO_3 solid electrolytes and metallic lithium anodes in all-solid-state lithium batteries. A stoichiometric mixture of La_2O_3, Li_2CO_3, and TiO_2 powders was calcined at 1250 ℃ for 8 h to obtain a single perovskite structure of La_(0.56)Li_(0.33)TiO_3. When this La_(0.56)Li_(0.33)TiO_3 sample and lithium were placed in contact at room temperature for 24 h, the phase of the La_(0.56)Li_(0.33)TiO_3 remained unchanged. The XPS results indicate that 12% of the tetravalent Ti~(4+) ions were converted into trivalent Ti~(3+) ions. The valence conversion and degree of conversion were limited by the structural rigidity of the host crystal. Our SIMS analysis suggests the existence of a local electric field near the contact surface and indicates that the~6Li~+ isotope ions were inserted into the specimen through the effect of this field. The change in the electrical properties of La_(0.56)Li_(0.33)TiO_3 supports this mechanism for the interfacial reaction. The ionic conductivities of the grain and total grain boundary decreased and increased, respectively, after the insertion of Li~+, and the total electronic conductivity increased as a result of the presence of intervalence electron hopping between mixed Ti~(3+)/Ti~(4+) states. The mechanism of the lithium-activated RT interfacial reaction is associated with the reduction of Ti~(4+) transition metal ions from tetravalent to trivalent states and the local-electric-field-induced Li~+ insertion into La~(3+)/Li~+-site vacancies of La_(0.56)Li_(0.33)TiO_3.
机译：我们使用x射线衍射（XRD），x射线光电子能谱（XPS）和二次离子质谱（SIMS）来研究阳离子不足的La_（0.56）之间的界面室温（RT）化学反应的机理全固态锂电池中的Li_（0.33）TiO_3固体电解质和金属锂阳极。将La_2O_3，Li_2CO_3和TiO_2粉末的化学计量混合物在1250℃下煅烧8小时，以获得La_（0.56）Li_（0.33）TiO_3的单一钙钛矿结构。当此La_（0.56）Li_（0.33）TiO_3样品与锂在室温下接触24小时时，La_（0.56）Li_（0.33）TiO_3的相保持不变。 XPS结果表明12％的四价Ti〜（4+）离子被转化为三价Ti〜（3+）离子。化合价和转化度受基质晶体的结构刚度限制。我们的SIMS分析表明在接触表面附近存在局部电场，并表明〜6Li〜+同位素离子通过该电场的作用被插入样品中。 La_（0.56）Li_（0.33）TiO_3的电学性质的变化支持了这种界面反应机理。插入Li〜+后，晶粒的离子电导率和总晶界的离子电导率分别降低和增加，并且由于混合的Ti〜（3 +）/ Ti之间存在间隔电子跳跃，总电子电导率增加〜（4+）个状态。锂激活的RT界面反应的机理与Ti〜（4+）过渡金属离子从四价态还原为三价态以及局部电场诱导的Li〜+插入La〜（3+）有关La_（0.56）Li_（0.33）TiO_3的/ Li〜+位空位。

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