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Slow and Sustained Release of Carbonate Ions from Amino Acids for Controlled Hydrothermal Growth of Alkaline-Earth Carbonate Single Crystals.

ABSTRACT: Alkaline-earth metal carbonate materials have attracted wide interest because of their high value in many applications. Various sources of carbonate ions (CO₃ ^2-), such as CO₂ gas, alkaline-metal carbonate salts, and urea, have been reported for the synthesis of metal carbonate crystals, yet a slow and sustained CO₃ ^2- release approach for controlled crystal growth is much desired. In this paper, we demonstrate a new chemical approach toward slow and sustained CO₃ ^2- release for hydrothermal growth of large alkaline-earth metal carbonate single crystals. Such an approach is enabled by the multiple hydrolysis of a small basic amino acid (arginine, Arg). Namely, the amino groups of Arg hydrolyze to form OH^- ions, making the solution basic, and the hydrolysis of the guanidyl group of Arg is hydrothermally triggered to produce urea and ammonia, followed by the hydrolysis of urea to produce CO₂ and ammonia and then the release of CO₃ ^2- because of the reaction between CO₂ and the OH^- ions hydrolyzed from ammonia. Such a CO₃ ^2- release behavior enables the slow and controlled growth of various carbonate single crystals over a wide range of pH values. The growth of uniform rhombohedron MgCO₃ single crystals with variable morphologies and crystal sizes is studied in detail. The influences of reaction temperature, solution pH, precursor type, and concentration on the morphology and size of the resulting MgCO₃ crystals are elucidated. The crystal evolution mechanism is also proposed and discussed with various supportive data.

SUBMITTER: Xia H

PROVIDER: S-EPMC7301596 | biostudies-literature | 2020 Jun

REPOSITORIES: biostudies-literature

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Slow and Sustained Release of Carbonate Ions from Amino Acids for Controlled Hydrothermal Growth of Alkaline-Earth Carbonate Single Crystals.

Xia Huayao H Zhou Mengyuan M Wei Xiangru X Zhang Xiangcheng X Wu Zhangxiong Z

ACS omega 20200601 23

Alkaline-earth metal carbonate materials have attracted wide interest because of their high value in many applications. Various sources of carbonate ions (CO3 2-), such as CO2 gas, alkaline-metal carbonate salts, and urea, have been reported for the synthesis of metal carbonate crystals, yet a slow and sustained CO3 2- release approach for controlled crystal growth is much desired. In this paper, we demonstrate a new chemical approach toward ...[more]

PMID: 32566880

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Project description:Bond-length distributions have been examined for 55 configurations of alkali-metal ions and 29 configurations of alkaline-earth-metal ions bonded to oxygen, for 4859 coordination polyhedra and 38?594 bond distances (alkali metals), and for 3038 coordination polyhedra and 24?487 bond distances (alkaline-earth metals). Bond lengths generally show a positively skewed Gaussian distribution that originates from the variation in Born repulsion and Coulomb attraction as a function of interatomic distance. The skewness and kurtosis of these distributions generally decrease with increasing coordination number of the central cation, a result of decreasing Born repulsion with increasing coordination number. We confirm the following minimum coordination numbers: ([3])Li(+), ([3])Na(+), ([4])K(+), ([4])Rb(+), ([6])Cs(+), ([3])Be(2+), ([4])Mg(2+), ([6])Ca(2+), ([6])Sr(2+) and ([6])Ba(2+), but note that some reported examples are the result of extensive dynamic and/or positional short-range disorder and are not ordered arrangements. Some distributions of bond lengths are distinctly multi-modal. This is commonly due to the occurrence of large numbers of structure refinements of a particular structure type in which a particular cation is always present, leading to an over-representation of a specific range of bond lengths. Outliers in the distributions of mean bond lengths are often associated with anomalous values of atomic displacement of the constituent cations and/or anions. For a sample of ([6])Na(+), the ratio Ueq(Na)/Ueq(bonded anions) is partially correlated with ?([6])Na(+)-O(2-)? (R(2) = 0.57), suggesting that the mean bond length is correlated with vibrational/displacement characteristics of the constituent ions for a fixed coordination number. Mean bond lengths also show a weak correlation with bond-length distortion from the mean value in general, although some coordination numbers show the widest variation in mean bond length for zero distortion, e.g. Li(+) in [4]- and [6]-coordination, Na(+) in [4]- and [6]-coordination. For alkali-metal and alkaline-earth-metal ions, there is a positive correlation between cation coordination number and the grand mean incident bond-valence sum at the central cation, the values varying from 0.84?v.u. for ([5])K(+) to 1.06?v.u. for ([8])Li(+), and from 1.76?v.u. for ([7])Ba(2+) to 2.10?v.u. for ([12])Sr(2+). Bond-valence arguments suggest coordination numbers higher than [12] for K(+), Rb(+), Cs(+) and Ba(2+).

Dataset Information

Slow and Sustained Release of Carbonate Ions from Amino Acids for Controlled Hydrothermal Growth of Alkaline-Earth Carbonate Single Crystals.

Publications

Slow and Sustained Release of Carbonate Ions from Amino Acids for Controlled Hydrothermal Growth of Alkaline-Earth Carbonate Single Crystals.

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