International audienceHybrid materials based on layered double hydroxides (LDHs) exhibit great potential in diverse fields such as health care, polymer composites, environment, catalysis, and energy generation. Indeed, the compositional flexibility and the scalability of LDH structures, their low cost, and their ease of synthesis have made hybrid LDHs extremely attractive for constructing smart and high-performance multifunctional materials. This review provides a comprehensive and critical overview of the current research on multifunctional hybrid LDHs. Organic–inorganic hybrid LDHs, intercalated and surface-immobilized structures, are both specifically addressed. The new trends and strategies for hybrid LDH synthesis are first described, and then the potential of the latest hybrid LDHs, polymer LDH nanocomposites, and LDH bio-nanocomposites are presented. Significant achievements published from ≈2010, including authors' results, which employ hybrid LDH assemblies in materials science, medicine, polymer nanocomposites, cement chemistry, and environmental technologies, are specifically addressed. It is concluded with remarks on present challenges and future prospects

Tartrate and succinate anions have been intercalated in Zn(3)Al and Zn(2)Cr LDHs. The preparations using either coprecipitation, anion exchange, or reconstruction methods are described. In the case of tartrate-containing LDH, coprecipitation and reconstruction methods have proved to be very limited to lead to pure materials due to the particular reactivity of tartrate anions. Intercalation of both anions under room-temperature conditions gives rise to expanded LDH with similar basal spacing. Moderate thermal treatments lead in all cases to a reorientation of the anions in the interlayer domains associated with an interlayer contraction occurring around 80 degrees C. The structural characterization, the thermal evolution, and the chemical stability of all the phases are studied by PXRD, FTIR, TGA, and DTA.

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Bayerite was treated under hydrothermal conditions (120, 130, 140, and 150 °C) to prepare a series of layered double hydroxides (LDHs) with an ideal composition of ZnAl4(OH)12(SO4)0.5·nH2O (ZnAl4-LDHs). These products were investigated by both bulk techniques (powder X-ray diffraction (PXRD), transmission electron microscopy, and elemental analysis) and atomic-level techniques ((1)H and (27)Al solid-state NMR, IR, and Raman spectroscopy) to gain a detailed insight into the structure of ZnAl4-LDHs and sample composition. Four structural models (one stoichiometric and three different defect models) were investigated by Rietveld refinement of the PXRD data. These were assessed using the information obtained from other characterization techniques, which favored the ideal (nondefect) structural model for ZnAl4-LDH, as, for example, (27)Al magic-angle spinning NMR showed that excess Al was present as amorphous bayerite (Al(OH)3) and pseudoboehmite (AlOOH). Moreover, no evidence of cation mixing, that is, partial substitution of Zn(II) onto any of four Al sites, was observed. Altogether this study highlights the challenges involved to synthesize pure ZnAl4-LDHs and the necessity to use complementary techniques such as PXRD, elemental analysis, and solid-state NMR for the characterization of the local and extended structure of ZnAl4-LDHs.

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This review highlights the current research on the interactions between biological cells and Layered Double Hydroxides (LDH). The as-prepared biohybrid materials appear extremely attractive in diverse fields of application relating to health care, environment and energy production. We describe how thanks to the main features of biological cells and LDH layers, various strategies of assemblies can be carried out for constructing smart biofunctional materials. The interactions between the two components are described with a peculiar attention to the adsorption, biocompatibilization, LDH layer internalization, antifouling and antimicrobial properties. The most significant achievements including authors' results, involving biological cells and LDH assemblies in waste water treatment, bioremediation and bioenergy generation are specifically addressed.

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Layered double hydroxides (LDHs), especially (doped) with transition metals, as well as nanohybrid and 2D materials derived from these structures, are interesting materials due to their catalytic and electrochemical properties. Their reactivity is determined by the atomic level distribution of the transition metal in the LDH cation layer, which is essential to control the design of LDHs with optimized properties. However, low crystallinity, absence of long range order, and/or isoelectronic ions often prevent atomic level structural characterization. A series of poorly crystalline Mg2-xNixAl-NO3 LDH materials were investigated by ultrafast 27Al MAS NMR spectroscopy to determine the distribution of Ni2+ in these as well as possible superstructures and their miscibility gaps. Four Ni2Al-LDH samples with interlayer distances ranging from 7.6 to 17.5 Å were prepared to assess the contribution of inter- and intralayer magnetic interactions. The effects of the Ni2+ content and the atomic level distribution of Ni2+ were probed by ultrafast 27Al MAS NMR spectroscopy: the Al distribution can be modeled using a binomial distribution and neither a superstructure was identified for the MgNiAl-LDH sample nor a miscibility gap. The 27Al isotropic shift, δiso(27Al), is a very sensitive probe for a number of neighboring Ni2+ in the first metal ion sphere, but to a smaller degree it is also affected by the intercalated anion (interlayer distance). These results were used for detailed characterization of an exfoliated (2D)-restacked Mg1.83Ni0.17Al-LDH nanohybrid material and a Mg1.83Ni0.17Al-LDH-alginate nanohybrid material, in which 27Al MAS NMR showed how the structure and partial dissolution of the LDHs were retained. In contrast, both powder X-ray diffraction and vibrational spectroscopies (IR and Raman) reflected only the overall change in sample composition.