  2D materials (2DM) and their heterostructures (2D + nD, n = 0,1,2,3) hold
significant promise for applications in Electrochemical Energy Storage Systems
(EESS), such as batteries. 2DM can serve as van der Waals (vdW) slick interface
between conventional active materials (e.g., Silicon) and current collectors,
modifying interfacial adhesion and preventing stress-induced fractures.
Additionally, 2DM can replace traditional polymer binders (e.g., MXenes). This
arrangement also underscores the critical role of interfacial mechanics between
2DM and active materials. Furthermore, 2DM can be designed to function as an
electrode itself. For instance, a porous graphene network has been reported to
possesses approximately five times the capacity of a traditional graphite
anode. Consequently, gaining a comprehensive understanding of the mechanical
properties of 2DM in EESS is paramount. However, modeling 2DM in EESS poses
significant challenges due to the intricate coupling of mechanics and
electrochemistry. For instance, defective graphene tends to favor adatom
adsorption (e.g., Li+) during charging. In cases of strong adsorption, adatoms
may not readily detach from electrodes during discharging. As a result, in such
scenarios, adsorption-desorption (charge-discharge) processes govern the
mechanical properties of 2DM when used as binders and current collectors.
Regrettably, most existing studies on the mechanical properties of 2DM in EESS
have failed to adequately address these critical issues. This perspective paper
aims to provide a comprehensive overview of recent progress in the
chemo-mechanics of 2DM's mechanical properties. A wide spectrum of multiscale
modeling approaches, including atomistic/molecular simulations, continuum
modeling, and machine learning, are discussed.
