Synthesis of Nanocrystalline Gd2O2NCN from a Versatile Single-source Precursor

Emanuel Ionescu, Wenjie Li, Leonore Wiehl, Gabriela Mera, Ralf Riedel

Research output: Contribution to journalArticle

Abstract

Nanocrystalline Gd2O2NCN (P3m1, crystallite size 30–40 nm) was synthesized upon ammonolysis of bis[[(N-carboxymethyl,N-carboxy-κO-methyl)amino-κN]-ethyl]-glycinato(3-)-κN,κO]gadolinium(III) (diethylenetriamine pentaacetic acid gadolinium(III) dihydrogen salt or gadopentetic acid, Gd-H2DTPA hereafter) at 900 °C. The conversion of Gd-H2DTPA into Gd2O2NCN takes place in several steps, probably via transient formation of iminodiacetate-, glycinate-, and carbamate-containing complexes of Gd. Thermal treatment in air of Gd-H2DTPA at 750 and 1300 °C delivers nanocrystalline bixbyite-type Gd2O3 (Ia3, crystallite size 30–70 nm); in an argon or nitrogen atmosphere the formation of monoclinic Gd2O3 (C2/m) was observed at 1300 °C. The synthesized Gd2O2NCN converts upon thermal treatment in air, nitrogen, or argon atmosphere into monoclinic Gd2O3 (C2/m). In ammonia atmosphere, Gd2O2NCN seems to be stable against decomposition, even upon prolonged exposure to 1000 °C. This study indicates that Gd-H2DTPA may be a robust, low-cost, and flexible precursor for nanoscaled Gd-based nanopowders. Moreover, precursor approaches based on metal complexes using H5DTPA as a ligand are suggested as promising access pathways towards nanocrystalline materials in the M/O/C/N system.

Original languageEnglish (US)
Pages (from-to)1681-1691
Number of pages11
JournalZeitschrift fur Anorganische und Allgemeine Chemie
Volume643
Issue number21
DOIs
StatePublished - Nov 17 2017

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Argon
Gadolinium
Crystallite size
Nitrogen
Heat treatment
Nanocrystalline materials
Pentetic Acid
Gadolinium DTPA
Carbamates
Coordination Complexes
Air
Ammonia
Salts
Ligands
Decomposition
Costs

All Science Journal Classification (ASJC) codes

  • Inorganic Chemistry

Cite this

Ionescu, Emanuel ; Li, Wenjie ; Wiehl, Leonore ; Mera, Gabriela ; Riedel, Ralf. / Synthesis of Nanocrystalline Gd2O2NCN from a Versatile Single-source Precursor. In: Zeitschrift fur Anorganische und Allgemeine Chemie. 2017 ; Vol. 643, No. 21. pp. 1681-1691.
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Synthesis of Nanocrystalline Gd2O2NCN from a Versatile Single-source Precursor. / Ionescu, Emanuel; Li, Wenjie; Wiehl, Leonore; Mera, Gabriela; Riedel, Ralf.

In: Zeitschrift fur Anorganische und Allgemeine Chemie, Vol. 643, No. 21, 17.11.2017, p. 1681-1691.

Research output: Contribution to journalArticle

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T1 - Synthesis of Nanocrystalline Gd2O2NCN from a Versatile Single-source Precursor

AU - Ionescu, Emanuel

AU - Li, Wenjie

AU - Wiehl, Leonore

AU - Mera, Gabriela

AU - Riedel, Ralf

PY - 2017/11/17

Y1 - 2017/11/17

N2 - Nanocrystalline Gd2O2NCN (P3m1, crystallite size 30–40 nm) was synthesized upon ammonolysis of bis[[(N-carboxymethyl,N-carboxy-κO-methyl)amino-κN]-ethyl]-glycinato(3-)-κN,κO]gadolinium(III) (diethylenetriamine pentaacetic acid gadolinium(III) dihydrogen salt or gadopentetic acid, Gd-H2DTPA hereafter) at 900 °C. The conversion of Gd-H2DTPA into Gd2O2NCN takes place in several steps, probably via transient formation of iminodiacetate-, glycinate-, and carbamate-containing complexes of Gd. Thermal treatment in air of Gd-H2DTPA at 750 and 1300 °C delivers nanocrystalline bixbyite-type Gd2O3 (Ia3, crystallite size 30–70 nm); in an argon or nitrogen atmosphere the formation of monoclinic Gd2O3 (C2/m) was observed at 1300 °C. The synthesized Gd2O2NCN converts upon thermal treatment in air, nitrogen, or argon atmosphere into monoclinic Gd2O3 (C2/m). In ammonia atmosphere, Gd2O2NCN seems to be stable against decomposition, even upon prolonged exposure to 1000 °C. This study indicates that Gd-H2DTPA may be a robust, low-cost, and flexible precursor for nanoscaled Gd-based nanopowders. Moreover, precursor approaches based on metal complexes using H5DTPA as a ligand are suggested as promising access pathways towards nanocrystalline materials in the M/O/C/N system.

AB - Nanocrystalline Gd2O2NCN (P3m1, crystallite size 30–40 nm) was synthesized upon ammonolysis of bis[[(N-carboxymethyl,N-carboxy-κO-methyl)amino-κN]-ethyl]-glycinato(3-)-κN,κO]gadolinium(III) (diethylenetriamine pentaacetic acid gadolinium(III) dihydrogen salt or gadopentetic acid, Gd-H2DTPA hereafter) at 900 °C. The conversion of Gd-H2DTPA into Gd2O2NCN takes place in several steps, probably via transient formation of iminodiacetate-, glycinate-, and carbamate-containing complexes of Gd. Thermal treatment in air of Gd-H2DTPA at 750 and 1300 °C delivers nanocrystalline bixbyite-type Gd2O3 (Ia3, crystallite size 30–70 nm); in an argon or nitrogen atmosphere the formation of monoclinic Gd2O3 (C2/m) was observed at 1300 °C. The synthesized Gd2O2NCN converts upon thermal treatment in air, nitrogen, or argon atmosphere into monoclinic Gd2O3 (C2/m). In ammonia atmosphere, Gd2O2NCN seems to be stable against decomposition, even upon prolonged exposure to 1000 °C. This study indicates that Gd-H2DTPA may be a robust, low-cost, and flexible precursor for nanoscaled Gd-based nanopowders. Moreover, precursor approaches based on metal complexes using H5DTPA as a ligand are suggested as promising access pathways towards nanocrystalline materials in the M/O/C/N system.

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