Research Institute of Electrochemical Energy, National Institute of Advanced Industrial Science and Technology (AIST), 1-8-31 Midorigaoka, Ikeda, Osaka, 563-8577, Japan.
AIST-Kyoto University Chemical Energy Materials Open Innovation Laboratory (ChEM-OIL), Sakyo-ku, Kyoto, 606-8501, Japan.
Adv Sci (Weinh). 2023 Feb;10(6):e2204672. doi: 10.1002/advs.202204672. Epub 2022 Dec 27.
Honeycomb-layered oxides with monovalent or divalent, monolayered cationic lattices generally exhibit myriad crystalline features encompassing rich electrochemistry, geometries, and disorders, which particularly places them as attractive material candidates for next-generation energy storage applications. Herein, global honeycomb-layered oxide compositions, Ag M TeO ( .) exhibiting atom bilayers with sub-valent states within Ag-rich crystalline domains of Ag M TeO and -deficient domains of ( ). The -rich material characterized by aberration-corrected transmission electron microscopy reveals local atomic structural disorders characterized by aperiodic stacking and incoherency in the bilayer arrangement of atoms. Meanwhile, the global material not only displays high ionic conductivity but also manifests oxygen-hole electrochemistry during silver-ion extraction. Within the -rich domains, the bilayered structure, argentophilic interactions therein and the expected sub-valent states ( , etc.) are theoretically understood via spontaneous symmetry breaking of SU(2)× U(1) gauge symmetry interactions amongst 3 degenerate mass-less chiral fermion states, justified by electron occupancy of silver and 5s orbitals on a bifurcated honeycomb lattice. This implies that bilayered frameworks have research applications that go beyond the confines of energy storage.
具有单价或二价、单层阳离子晶格的蜂窝状层状氧化物通常表现出丰富的电化学、几何和无序特征，这使得它们特别成为下一代储能应用的有吸引力的材料候选物。本文报道了一种具有全球蜂窝层状氧化物组成的材料，AgMTeO（.），其中含有亚价态的 原子双层，存在于富含 Ag 的 AgMTeO 结晶域和 （ ）不足的域内。通过像差校正的透射电子显微镜对富含 的材料进行表征，揭示了局部原子结构的无序性，表现为双层排列的 原子的非周期性堆叠和非相干性。同时，这种全局材料不仅表现出高离子电导率，而且在银离子提取过程中还表现出氧空穴电化学。在富含 的区域内，通过 3 个简并无质量手性费米子状态之间的 SU(2)×U(1)规范对称性相互作用的自发对称破缺，从理论上理解了双层结构、其中的银亲合相互作用以及预期的亚价态（ 等），这是由银和分叉的蜂窝状晶格上的 5s 轨道上的电子占据所证明的。这意味着双层框架的研究应用超出了储能的范围。
