Publications by authors named "Encarnacion Ruiz-Agudo"

Crystallization of monosodium urate monohydrate (MSU) leads to painful gouty arthritis. Despite extensive research it is still unknown how this pathological biomineralization occurs, which hampers its prevention. Here we show how inflammatory MSU crystals form after a non-inflammatory amorphous precursor (AMSU) that nucleates heterogeneously on collagen fibrils from damaged articular cartilage of gout patients.

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In this work, the potential of bio-inspired strategies for the synthesis of calcium sulfate (CaSO·nHO) materials for heritage conservation is explored. For this, a nonclassical multi-step crystallization mechanism to understand the effect of calcein- a fluorescent chelating agent with a high affinity for divalent cations- on the nucleation and growth of calcium sulfate phases is proposed. Moving from the nano- to the macro-scale, this strategy sets the basis for the design and production of fluorescent nano-bassanite (NB-C; CaSO·0.

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Ancient Maya produced some of the most durable lime plasters on Earth, yet how this was achieved remains a secret. Here, we show that ancient Maya plasters from Copan (Honduras) include organics and have a calcite cement with meso-to-nanostructural features matching those of calcite biominerals (e.g.

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The relatively recent development of nanolimes (i.e., alcoholic dispersions of Ca(OH) nanoparticles) has paved the way for new approaches to the conservation of important art works.

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Bacteria play crucial roles in the biogeochemical cycle of arsenic (As) and selenium (Se) as these elements are metabolized via detoxification, energy generation (anaerobic respiration) and biosynthesis (e.g. selenocysteine) strategies.

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We report a novel solvothermal route for the production of bassanite (CaSO·0.5HO) nanoparticles using amorphous Ca-ethoxide as a precursor. Bassanite nanorods, 120-200 nm in length, with the highest specific surface area reported so far (54 m g) and enhanced reactivity, are obtained at 78 °C and 1 atm.

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Article Synopsis
  • The mineralization of hydroxylapatite (HAp), crucial for bone formation, occurs through nontraditional routes influenced by organic compounds, particularly the small organic molecule citrate.
  • Research shows that citrate stabilizes both prenucleation species and a liquid-like calcium phosphate precursor, which may enhance the mineralization process within collagen fibrils before any solid structure forms.
  • The study reveals that HAp formed from amorphous calcium phosphate in the presence of citrate results in unique nanoplate structures similar to natural bone, suggesting that citrate plays a significant role in the mineralization process and challenges existing theories about HAp formation.
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In this work, calcium oxalate (CaOx) precursors were stabilized by poly(acrylic acid) (PAA) as an additive under in vitro crystallization assays involving the formation of pre-nucleation clusters of CaOx via a non-classical crystallization (NCC) pathway. The in vitro crystallization of CaOx was carried out in the presence of 10, 50 and 100 mg/L PAA by using automatic calcium potentiometric titration experiments at a constant pH of 6.7 at 20 °C.

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To overcome the limitations of traditional conservation treatments used for protection and consolidation of stone and lime mortars and plasters, mostly based on polymers or alkoxysilanes, a novel treatment based on the activation of indigenous carbonatogenic bacteria has been recently proposed and applied both in the laboratory and . Despite very positive results, little is known regarding its effect on the evolution of the indigenous bacterial communities, specially under hot and humid tropical conditions where proliferation of microorganisms is favored, as it is the case of the Maya area. Here, we studied changes in bacterial diversity of severely degraded tuff stone and lime plaster at the archeological Maya site of Copan (Honduras) after treatment with the patented sterile M-3P nutritional solution.

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Although calcium oxalates are relevant biominerals, their formation mechanisms remain largely unresolved. Here, we investigate the early stages of calcium oxalate formation in pure and citrate-bearing solutions. Citrate is used as a well-known oxalate precipitation inhibitor; moreover, it resembles the functional domains of the biomolecules that modulate biomineralization.

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Hydrated lime (Ca(OH)) is a vernacular art and building material produced following slaking of CaO in water. If excess water is used, a slurry, called lime putty, forms, which has been the preferred craftsman selection for formulating lime mortars since Roman times. A variety of natural additives were traditionally added to the lime putty to improve its quality.

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Enhanced salt weathering resulting from global warming and increasing environmental pollution is endangering the survival of stone monuments and artworks. To mitigate the effects of these deleterious processes, numerous conservation treatments have been applied that, however, show limited efficacy. Here we present a novel, environmentally friendly, bacterial self-inoculation approach for the conservation of stone, based on the isolation of an indigenous community of carbonatogenic bacteria from salt damaged stone, followed by their culture and re-application back onto the same stone.

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In order to evaluate the organic phosphorus (OP) and pyrophosphate (PyroP) cycle and their fate in the environment, it is critical to understand the effects of mineral interfaces on the reactivity of adsorption and precipitation of OP and PyroP. Here, in situ atomic force microscopy (AFM) is used to directly observe the kinetics of coupled dissolution-precipitation on cleaved (001) surfaces of brucite [Mg(OH)] in the presence of phytate, glucose-6-phosphate (G6P) and pyrophosphate, respectively. AFM results show that the relative order of contribution to mineral surface adsorption and precipitation is phytate > pyrophosphate > G6P under the same solution conditions and can be quantified by the induction time of OP/PyroP-Mg nucleation in a boundary layer at the brucite-water interface.

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Recent research has shown that biominerals and their biomimetics (i) typically form via an amorphous precursor phase, and (ii) commonly display a nanogranular texture. Apparently, these two key features are closely related, underlining the fact that the formation of biominerals and their biomimetics does not necessarily follow classical crystallization routes, and leaves a characteristic nanotextural imprint which may help to disclose their origins and formation mechanisms. Here we present a general overview of the current theories and models of nonclassical crystallization and their applicability for the advance of our current understanding of biomineralization and biomimetic mineralization.

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A distinct nanogranular fine structure is shared by a wealth of biominerals from several species, classes and taxa. This nanoscopic organization affects the properties and behavior of the biogenic ceramic material and confers on them attributes that are essential to their function. We present a set of structure-relationship properties that are rooted in the nanogranular organization and we propose that they rest on a common pathway of formation, a colloid-driven and hence nonclassical mode of crystallization.

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Nanolimes are alcohol dispersions of Ca(OH)2 nanoparticles used in the conservation of cultural heritage. Although it was believed that Ca(OH)2 particles were inert when dispersed in short-chain alcohols, it has been recently shown that they can undergo transformation into calcium alkoxides. Little is known, however, about the mechanism and kinetics of such a phase transformation as well as its effect on the performance of nanolimes.

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Esters of phosphoric acid constitute a large fraction of the total organic phosphorus (OP) in the soil environment and, thus, play an important role in the global phosphorus cycle. These esters, such as glucose-6-phosphate (G6P), exhibit unusual reactivity toward various mineral particles in soils, especially those containing calcite. Many important processes of OP transformation, including adsorption, hydrolysis, and precipitation, occur primarily at mineral-fluid interfaces, which ultimately governs the fate of organophosphates in the environment.

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Adsorption and subsequent immobilization of orthophosphate on iron oxides is of considerable importance in soil fertility and eutrophication studies. Here, in situ atomic force microscopy (AFM) has been used to probe the interaction of phosphate-bearing solutions with goethite, α-FeOOH, (010) cleavage surfaces. During the dissolution of goethite we observed simultaneous nucleation of nanoparticles (1.

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Classical molecular dynamics simulations of several aqueous alkali halide salt solutions have been used to determine the effect of electrolytes on the structure of water and the hydration properties of calcium ions. Compared with the simulations of Ca(2+) ions in pure liquid water, the frequency of water exchange in the first hydration shell of calcium, which is a fundamental process in controlling the reactivity of calcium(ii) aqua-ions, is drastically reduced in the presence of other electrolytes in solution. The strong stabilization of the hydration shell of Ca(2+) occurs not only when the halide anions are directly coordinated to calcium, but also when the alkali and halide ions are placed at or outside the second coordination shell of Ca(2+), suggesting that the reactivity of the first solvation shell of the calcium ion can be influenced by the specific affinity of other ions in solution for the water molecules coordinated to Ca(2+).

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In situ atomic force microscopy (AFM) has been used to study the interaction of phosphate-bearing solutions with cerussite, PbCO3, (010) surfaces. During the dissolution of cerussite we observed simultaneous growth of needle-shaped or spherical pyromorphite phases. This occurred at two different pH values and ionic strengths relevant to soil solution conditions.

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Calcite, a widespread natural mineral at the Earth's surface, is well-known for its capacity to sequester various elements within its structure. Among these elements, selenium is important because of its high toxicity in natural systems and for human health. In the form of selenite (Se((IV))), selenium can be incorporated into calcite during growth.

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Alcohol dispersions of Ca(OH)2 nanoparticles, the so-called nanolimes, are emerging as an effective conservation material for the consolidation of stone, mortars, and plasters present in old masonry and/or mural paintings. To better understand how this treatment operates, to optimize its performance and broaden its applications, here we study the nano and microstructural characteristics, carbonation behavior, and consolidation efficacy of colloidal alcohol dispersions of Ca(OH)2 nanoparticles produced by both homogeneous (commercial nanolime) and heterogeneous phase synthesis (aged slaked lime and carbide lime putties). We observe that the alcohol not only provides a high colloidal stability to Ca(OH)2 particles, but also affects the kinetics of carbonation and CaCO3 polymorph selection.

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The dissolution and carbonation of portlandite (Ca(OH)2) single crystals was studied by a combination of in situ Atomic Force Microscopy, Scanning Electron Microscopy, and two-dimensional X-ray diffraction. The dissolution of portlandite {0001} surfaces in water proceeds by the formation and expansion of pseudohexagonal etch pits, with edges parallel to ⟨100⟩ directions. Etch pits on {010} surfaces are elongated along ⟨001⟩, with edges parallel to ⟨101⟩.

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Pressure exerted by crystallization of salts within porous materials contributes to damage in historic and modern construction. By unequivocally identifying the precipitating phase(s) while simultaneously determining solution supersaturation and associated crystallization pressure in subsurface pores, we show that the formation of a thermodynamically metastable salt phase (heptahydrate; Na2SO4·7H2O) and the resulting transition to a less soluble stable phase (mirabilite; Na2SO4·10H2O) is largely responsible for the high supersaturation and crystallization pressure developed during evaporative crystallization of sodium sulfate, the most damaging salt known. These results help to explain why salts with various (stable and metastable) hydrated phases are the most damaging.

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The influence of mineral substrate composition and structure on bacterial calcium carbonate productivity and polymorph selection was studied. Bacterial calcium carbonate precipitation occurred on calcitic (Iceland spar single crystals, marble, and porous limestone) and silicate (glass coverslips, porous sintered glass, and quartz sandstone) substrates following culturing in liquid medium (M-3P) inoculated with different types of bacteria (Myxococcus xanthus, Brevundimonas diminuta, and a carbonatogenic bacterial community isolated from porous calcarenite stone in a historical building) and direct application of sterile M-3P medium to limestone and sandstone with their own bacterial communities. Field emission scanning electron microscopy (FESEM), atomic force microscopy (AFM), powder X-ray diffraction (XRD), and 2-dimensional XRD (2D-XRD) analyses revealed that abundant highly oriented calcite crystals formed homoepitaxially on the calcitic substrates, irrespective of the bacterial type.

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