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Title

Evidence of multiple sorption modes in layered double hydroxides using Mo as structural probe

AuthorsMa, Bin; Fernandez-Martinez, Alejandro; Grangeon, Sylvain; Tournassat, Christophe; Findling, Nathaniel; Claret, Francis; Koishi, Ayumi; Marty, Nicolas C. M.; Tisserand, Delphine; Bureau, Sarah; Salas, Eduardo ; Elkaïm, Erik; Marini, Carlo; Charlet, Laurent
Issue Date16-May-2017
PublisherAmerican Chemical Society
CitationEnvironmental Science and Technology 51(10): 5531-5540 (2017)
AbstractLayered double hydroxides (LDHs) have been considered as effective phases for the remediation of aquatic environments, to remove anionic contaminants mainly through anion exchange mechanisms. Here, a combination of batch isotherm experiments and X-ray techniques was used to examine molybdate (MoO ) sorption mechanisms on CaAl LDHs with increasing loadings of molybdate. Advanced modeling of aqueous data shows that the sorption isotherm can be interpreted by three retention mechanisms, including two types of edge sites complexes, interlayer anion exchange, and CaMoO precipitation. Meanwhile, Mo geometry evolves from tetrahedral to octahedral on the edge, and back to tetrahedral coordination at higher Mo loadings, indicated by Mo K-edge X-ray absorption spectra. Moreover, an anion exchange process on both CaAl LDHs was followed by in situ time-resolved synchrotron-based X-ray diffraction, remarkably agreeing with the sorption isotherm. This detailed molecular view shows that different uptake mechanisms - edge sorption, interfacial dissolution-reprecipitation - are at play and control anion uptake under environmentally relevant conditions, which is contrast to the classical view of anion exchange as the primary retention mechanism. This work puts all these mechanisms in perspective, offering a new insight into the complex interplay of anion uptake mechanisms by LDH phases, by using changes in Mo geometry as powerful molecular-scale probe.
Publisher version (URL)https://doi.org/10.1021/acs.est.7b00946
URIhttp://hdl.handle.net/10261/188343
DOI10.1021/acs.est.7b00946
Identifiersdoi: 10.1021/acs.est.7b00946
e-issn: 1520-5851
issn: 0013-936X
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