The observed polarity transitions that occur upon PS adsorption on both goethite and the diamond surface can be explained by the results of 2D-COS analyses. Polysaccharide adsorption at both surfaces results in increases in WCA since, as shown by concentration-dependent 2D-COS analysis, hydroneutral and hydrophobic residues interact causing the PS to self-associate at the surface. Therefore, with increasing PS surface loading, hydrophobic pockets form at the goethite and diamond surfaces that eventually lead to greater hydrophobicity (Figure ). Hence, results from WCA measurements suggest the polysaccharide chains undergo structural rearrangement once adsorbed at the mineral surfaces, and that this structural rearrangement or self-association is dependent on the polarity of the bare surface which dictates the initial mechanism of interaction between the PS and the surface. for adsorption (Figure ). We posit the introduction of background electrolyte to organo-mineral associations during desorption causes conformational disruptions, which increase the hydrophilic character of the surface by disturbing hydrophobic pockets and increasing water adsorption within organic associations (i.e., surface rehydration, Figure ). Overall, desorption of PS molecular fragments from the organic coating results in decreased WCA and surface hydrophobicity of the PS-mineral surfaces regardless of the hydrophobic nature of the initial mineral surface (Figure ). Water contact angle measurements support our 2D-COS analyses and interpretation.