Anhydrous Amorphous Calcium Oxalate Nanoparticles from Ionic Liquids: Stable Crystallization Intermediates in the Formation of Whewellite

Gehl, Aaron; Dietzsch, Michael; Mondeshki, Mihail; Bach, Sven; Häger, Tobias; Panthöfer, Martin; Barton, Bastian; Kolb, Ute; Tremel, Wolfgang

doi:10.1002/chem.201502229

Cited by 20 publications

(34 citation statements)

References 108 publications

(193 reference statements)

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“…It represents more than 80% of the dry weight of some plants and is the main component of pathological biominerals such as kidney stones. Some researchers (Qiu et al, 2004;Hajir et al, 2014;Gehl et al, 2015;Kolbach-Mandel et al, 2015) identified that the amorphous phase existed before the nucleation of calcium oxalate. However, the nature of this pre-nucleation amorphous phase remains unclear.…”

Section: Organic Biomineralsmentioning

confidence: 99%

Liquid-Liquid Phase Separation in Nucleation Process of Biomineralization

Qin

Zhang

2022

Front. Chem.

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Biomineralization is a typical interdisciplinary subject attracting biologists, chemists, and geologists to figure out its potential mechanism. A mounting number of studies have revealed that the classical nucleation theory is not suitable for all nucleation process of biominerals, and phase-separated structures such as polymer-induced liquid precursors (PILPs) play essential roles in the non-classical nucleation processes. These structures are able to play diverse roles biologically or pathologically, and could also give inspiring clues to bionic applications. However, a lot of confusion and dispute occurred due to the intricacy and interdisciplinary nature of liquid precursors. Researchers in different fields may have different opinions because the terminology and current state of understanding is not common knowledge. As a result, our team reviewed the most recent articles focusing on the nucleation processes of various biominerals to clarify the state-of-the-art understanding of some essential concepts and guide the newcomers to enter this intricate but charming field.

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Section: Organic Biomineralsmentioning

confidence: 99%

Liquid-Liquid Phase Separation in Nucleation Process of Biomineralization

Qin

Zhang

2022

Front. Chem.

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“…H2O (whewellite, COM) and dihydrate CaC2O4 . 2H2O (weddellite, COD) species, although amorphous calcium oxalate can also be observed (Gehl et al, 2015;Ruiz-Agudo et al, 2017). The trihydrate form, CaC2O4 .…”

Section: Introductionmentioning

confidence: 99%

A novel multinuclear solid state NMR approach for the characterization of kidney stones

Leroy¹,

Bonhomme-Coury²,

Gervais³

et al. 2021

Preprint

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Abstract. The spectroscopic study of pathological calcifications (including kidney stones) is extremely rich and helps to improve the understanding of the physical and chemical processes associated with their formation. While FTIR imaging and optical/electron microscopies are routine techniques in hospitals, there has been a dearth of solid state NMR studies introduced into this area of medical research, probably due to the scarcity of this analytical technique in hospital facilities. This work introduces effective multinuclear and multi-dimensional solid state NMR methodologies to study the complex chemical and structural properties characterising kidney stone composition. As a basis for comparison three hydrates (n = 1, 2 and 3) of calcium oxalate are examined along with nine representative kidney stones. The multinuclear MAS NMR approach adopted investigates the 1H, 13C, 31P and 43Ca nuclei, with the 1H and 13C MAS NMR data able to be readily deconvoluted into the constituent elements associated with the different oxalates and organics present. For the first time, the full interpretation of highly resolved 1H NMR spectra is presented for the three hydrates, based on structure and local dynamics. The corresponding 31P MAS NMR data indicates the presence of low-level inorganic phosphate species, however the complexity of these data make the precise identification of the phases difficult to assign. This work provides physicians, urologists and nephrologists with additional avenues of spectroscopic investigation to interrogate this complex medical dilemma that requires real multi technique approaches to generate effective outcomes.

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“…[4][5][6][7][8][9][10][11][12][13][14] 4,6,[15][16][17][18][19][20] As in the case of calcium carbonate, an amorphous phase has also been detected for calcium oxalate, with a degree of hydration close to 1 molecule of water per formula unit. 21,22 On the other hand, understanding the structure and polymorphism of anhydrous calcium oxalate (COA) directly from experiment is a challenge due to the fact that it is highly hygroscopic and therefore little work has been done so far on these phases.…”

Section: Introductionmentioning

confidence: 99%

Anhydrous Calcium Oxalate Polymorphism: A Combined Computational and Synchrotron X-ray Diffraction Study

Zhao¹,

Sharma

Jones³

et al. 2016

Crystal Growth & Design

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Four possible models for anhydrous calcium oxalate (COA) polymorphs have been investigated through ab initio quantum mechanical methods. Their structural properties, IR and Raman spectra, and thermodynamic stability in the range of 0-800 K have been analyzed and compared. Along with the known β-COA structures, two models turn out to be possible candidates for the α-and γ-polymorphs that 2 were observed during dehydration of weddellite (calcium oxalate dihydrate, COD) by Walter-Lévy and Laniepce (C. R. Acad. Sc. Paris, 259, 4685, 1964). While the calculated vibrational frequencies show that the four COA models correspond to minimum energy structures, β-COA is the thermodynamically favored phase over the range of temperatures examined in the present study. Despite the fact that computed vibrational spectra and XRD patterns of these polymorphs exhibit some different features, a definitive assignment of the structures based on computational results is not possible due to the lack of accurate experimental data. In an effort to improve comparative experimental data, the structural evolution of whewellite (calcium oxalate monohydrate, COM) has been probed using time-resolved synchrotron X-ray diffraction, in order to correlate the calculated structures to the observed structures. The evolution has been shown to go through at least 4 phases identified as COM, α-COA (corresponding to one of the models proposed by computation), β-COA, and CaCO 3. The reactions are predominantly two-phase reactions and at 140 °C evidence of three-phase coexistence has been noted between COM, α-COA, and β-COA. The time-resolved XRD data allow estimation of the kinetics of the reactions; these indicate second order reactions between COM and α-COA and zeroth order reactions between α-COA and β-COA.

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Anhydrous Amorphous Calcium Oxalate Nanoparticles from Ionic Liquids: Stable Crystallization Intermediates in the Formation of Whewellite

Cited by 20 publications

References 108 publications

Liquid-Liquid Phase Separation in Nucleation Process of Biomineralization

Liquid-Liquid Phase Separation in Nucleation Process of Biomineralization

A novel multinuclear solid state NMR approach for the characterization of kidney stones

Anhydrous Calcium Oxalate Polymorphism: A Combined Computational and Synchrotron X-ray Diffraction Study

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