Not yet reviewed by Pith; the record is open.

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, we report global honeycomb layered oxide compositions, ${\rm Ag_2}M_2{\rm TeO_6}$ ($M = \rm Ni, Mg, \textit{etc}.$) exhibiting $\rm Ag$ atom bilayers with sub-valent states within Ag-rich crystalline domains of ${\rm Ag_6}M_2{\rm TeO_6}$ and $\rm Ag$-deficient domains of ${\rm Ag}_{2 - x}\rm Ni_2TeO_6$ ($0 < x < 2$). The $\rm Ag$-rich material characterised by aberration-corrected transmission electron microscopy reveals local atomic structural disorders characterised by aperiodic stacking and incoherency in the bilayer arrangement of $\rm Ag$ atoms. Meanwhile, the global material not only displays high ionic conductivity, but also manifests oxygen-hole electrochemistry during silver-ion extraction. Within the $\rm Ag$-rich domains, the bilayered structure, argentophilic interactions therein and the expected $\rm Ag$ sub-valent states ($1/2+, 2/3+, \textit{etc}.$) are theoretically understood via spontaneous symmetry breaking of SU($2$)$\times$U($1$) gauge symmetry interactions amongst $3$ degenerate mass-less chiral fermion states, justified by electron occupancy of silver $4d_{z^2}$ and $5s$ orbitals on a bifurcated honeycomb lattice. This implies that bilayered frameworks have research applications that go beyond the confines of energy storage.