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Within the framework of The Heterogeneous dust Evolution Model at the IaS(THEMIS) this work investigates in detail the surface processes and chemistryrelating to core/mantle interstellar and cometary grain structures and itsinfluence on the nature of these fascinating particles. It appears that arealistic consideration of the nature and chemical reactivity of interstellargrain surfaces could self-consistently and within a coherent framework explain:the anomalous oxygen depletion, the nature of the CO dark gas, the formation of'polar ice' mantles, the red wing on the 3 um water ice band, the basis for theO-rich chemistry observed in hot cores, the origin of organic nano-globules andthe \sim 3.2 um 'carbonyl' absorption band observed in comet reflectancespectra. It is proposed that the reaction of gas phase species withcarbonaceous a- C(:H) grain surfaces in the interstellar medium, in particularthe incorporation of atomic oxygen into grain surfaces in epoxide functionalgroups, is the key to explaining these observations. Thus, the chemistry ofcosmic dust is much more intimately related with that of the interstellar gasthan has previously been considered. The current models for interstellar gasand dust chemistry will therefore most likely need to be fundamentally modifiedto include these new grain surface processes.

Dust evolution, a global view: III. Core/mantle grains, organic nano-globules, comets and surface chemistry