000859966 001__ 859966 000859966 005__ 20240619092117.0 000859966 0247_ $$2doi$$a10.1021/acs.langmuir.8b00492 000859966 0247_ $$2ISSN$$a0743-7463 000859966 0247_ $$2ISSN$$a1520-5827 000859966 0247_ $$2pmid$$apmid:29924623 000859966 0247_ $$2WOS$$aWOS:000439398100009 000859966 037__ $$aFZJ-2019-00772 000859966 082__ $$a540 000859966 1001_ $$0P:(DE-HGF)0$$aDaab, Matthias$$b0$$eCorresponding author 000859966 245__ $$aOnset of Osmotic Swelling in Highly Charged Clay Minerals 000859966 260__ $$aWashington, DC$$bACS Publ.$$c2018 000859966 3367_ $$2DRIVER$$aarticle 000859966 3367_ $$2DataCite$$aOutput Types/Journal article 000859966 3367_ $$0PUB:(DE-HGF)16$$2PUB:(DE-HGF)$$aJournal Article$$bjournal$$mjournal$$s1554104582_30322 000859966 3367_ $$2BibTeX$$aARTICLE 000859966 3367_ $$2ORCID$$aJOURNAL_ARTICLE 000859966 3367_ $$00$$2EndNote$$aJournal Article 000859966 520__ $$aDelamination by osmotic swelling of layered materials is generally thought to become increasingly difficult, if not impossible, with increasing layer charge density because of strong Coulomb interactions. Nevertheless, for the class of 2:1 layered silicates, very few examples of delaminating organo-vermiculites were reported in literature. We propose a mechanism for this repulsive osmotic swelling of highly charged vermiculites based on repulsive counterion translational entropy that dominates the interaction of adjacent layers above a certain threshold separation. Based on this mechanistic insight, we were able to identify several organic interlayer cations appropriate to delaminate highly charged, vermiculite-type clay minerals. 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