“…In this work we focus on the origin of adsorption-induced deformation of microporous carbons. Typically microporous materials, such as carbons or zeolites, exhibit a nonmonotonic adsorption-induced deformation: they contract at low stages of micropore filling and switch to expansion as adsorption progresses. − The extent of observed contraction and expansion depends on the structure of the adsorbent, , the adsorptive applied, ,,,− and the temperature. ,,, The first model for adsorption-induced deformation of microporous materials was proposed by Bangham, who considered the energy change of the adsorbate–adsorbent interface to be the sole source of stress within the porous structure . This concept was later implemented into the framework of Biot’s poromechanics by the use of the Gibbs adsorption equation. ,, However, the fundamental issue of this approach is that adsorption leads to a reduction of the interfacial energy, and thereby only expansion should be observed, in clear contradiction with experimental findings.…”