Aerogel-Based Single-Ion Magnets: A Case Study of a Cobalt(II) Complex Immobilized in Silica

The chemical immobilization of cobalt(II) ions in a silica aerogel matrix enabled the synthesis of the first representative example of aerogel-based single-ion magnets. For the synthesis of the lyogels, methyl-trimethoxysilane and N-3-(trimethoxysilyl)propyl ethylenediamine were co-hydrolyzed, then...

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Published inMolecules (Basel, Switzerland) Vol. 28; no. 1; p. 418
Main Authors Kottsov, Sergey Yu, Shmelev, Maxim A, Baranchikov, Alexander E, Kiskin, Mikhail A, Sharipov, Alim U, Efimov, Nikolay N, Rubtsova, Irina K, Nikolaevskii, Stanislav A, Kopitsa, Gennady P, Khamova, Tamara V, Roslyakov, Ilya V, Eremenko, Igor L, Ivanov, Vladimir K
Format Journal Article
LanguageEnglish
Published Switzerland MDPI AG 01.01.2023
MDPI
Subjects
aerogel
Bulk density
Carbon dioxide
Case studies
chemical immobilization
Cobalt
Cobalt compounds
Diamines
Ethylenediamine
Immobilization
Information storage
Ions
Magnetic induction
Magnetic measurement
magnetic properties
Magnetic relaxation
Magnetization
Magnetization reversal
N-3-(trimethoxysilyl)propyl ethylenediamine
Nanoparticles
Porosity
Silica
Silica aerogels
Silicon dioxide
single-ion magnet
single-molecule magnet
United Kingdom
United States
Germany
Russia
magnetic properties
electron paramagnetic resonance
single-ion magnet
chemical immobilization
single-molecule magnet
Raman spectroscopy
aerogel
N-3-(trimethoxysilyl)propyl ethylenediamine
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Abstract The chemical immobilization of cobalt(II) ions in a silica aerogel matrix enabled the synthesis of the first representative example of aerogel-based single-ion magnets. For the synthesis of the lyogels, methyl-trimethoxysilane and N-3-(trimethoxysilyl)propyl ethylenediamine were co-hydrolyzed, then the ethylenediamine groups that were immobilized on the silica matrix enabled the subsequent binding of cobalt(II) ions. Lyogels with various amounts of ethylenediamine moieties (0.1-15 mol %) were soaked in isopropanol solutions of cobalt(II) nitrate and further supercritically dried in carbon dioxide to obtain aerogels with a specific surface area of 210-596 m ·g , an apparent density of 0.403-0.740 cm ·g and a porosity of 60-78%. The actual cobalt content in the aerogels was 0.01-1.50 mmol per 1 g of SiO , which could easily be tuned by the concentration of ethylenediamine moieties in the silica matrix. The introduction of cobalt(II) ions into the ethylenediamine-modified silica aerogel promoted the stability of the diamine moieties at the supercritical drying stage. The molecular prototype of the immobilized cobalt(II) complex, bearing one ethylenediamine ligand [Co(en)(MeCN)(NO ) ], was synthesized and structurally characterized. Using magnetometry in the DC mode, it was shown that cobalt(II)-modified silica aerogels exhibited slow magnetic relaxation in a nonzero field. A decrease in cobalt(II) concentration in aerogels from 1.5 mmol to 0.14 mmol per 1 g of SiO resulted in a weakening of inter-ion interactions; the magnetization reversal energy barrier likewise increased from 4 to 18 K.
AbstractList The chemical immobilization of cobalt(II) ions in a silica aerogel matrix enabled the synthesis of the first representative example of aerogel-based single-ion magnets. For the synthesis of the lyogels, methyl-trimethoxysilane and N-3-(trimethoxysilyl)propyl ethylenediamine were co-hydrolyzed, then the ethylenediamine groups that were immobilized on the silica matrix enabled the subsequent binding of cobalt(II) ions. Lyogels with various amounts of ethylenediamine moieties (0.1-15 mol %) were soaked in isopropanol solutions of cobalt(II) nitrate and further supercritically dried in carbon dioxide to obtain aerogels with a specific surface area of 210-596 m ·g , an apparent density of 0.403-0.740 cm ·g and a porosity of 60-78%. The actual cobalt content in the aerogels was 0.01-1.50 mmol per 1 g of SiO , which could easily be tuned by the concentration of ethylenediamine moieties in the silica matrix. The introduction of cobalt(II) ions into the ethylenediamine-modified silica aerogel promoted the stability of the diamine moieties at the supercritical drying stage. The molecular prototype of the immobilized cobalt(II) complex, bearing one ethylenediamine ligand [Co(en)(MeCN)(NO ) ], was synthesized and structurally characterized. Using magnetometry in the DC mode, it was shown that cobalt(II)-modified silica aerogels exhibited slow magnetic relaxation in a nonzero field. A decrease in cobalt(II) concentration in aerogels from 1.5 mmol to 0.14 mmol per 1 g of SiO resulted in a weakening of inter-ion interactions; the magnetization reversal energy barrier likewise increased from 4 to 18 K.
The chemical immobilization of cobalt(II) ions in a silica aerogel matrix enabled the synthesis of the first representative example of aerogel-based single-ion magnets. For the synthesis of the lyogels, methyl-trimethoxysilane and N-3-(trimethoxysilyl)propyl ethylenediamine were co-hydrolyzed, then the ethylenediamine groups that were immobilized on the silica matrix enabled the subsequent binding of cobalt(II) ions. Lyogels with various amounts of ethylenediamine moieties (0.1–15 mol %) were soaked in isopropanol solutions of cobalt(II) nitrate and further supercritically dried in carbon dioxide to obtain aerogels with a specific surface area of 210–596 m2·g−1, an apparent density of 0.403–0.740 cm3·g−1 and a porosity of 60–78%. The actual cobalt content in the aerogels was 0.01–1.50 mmol per 1 g of SiO2, which could easily be tuned by the concentration of ethylenediamine moieties in the silica matrix. The introduction of cobalt(II) ions into the ethylenediamine-modified silica aerogel promoted the stability of the diamine moieties at the supercritical drying stage. The molecular prototype of the immobilized cobalt(II) complex, bearing one ethylenediamine ligand [Co(en)(MeCN)(NO3)2], was synthesized and structurally characterized. Using magnetometry in the DC mode, it was shown that cobalt(II)-modified silica aerogels exhibited slow magnetic relaxation in a nonzero field. A decrease in cobalt(II) concentration in aerogels from 1.5 mmol to 0.14 mmol per 1 g of SiO2 resulted in a weakening of inter-ion interactions; the magnetization reversal energy barrier likewise increased from 4 to 18 K.
The chemical immobilization of cobalt(II) ions in a silica aerogel matrix enabled the synthesis of the first representative example of aerogel-based single-ion magnets. For the synthesis of the lyogels, methyl-trimethoxysilane and N-3-(trimethoxysilyl)propyl ethylenediamine were co-hydrolyzed, then the ethylenediamine groups that were immobilized on the silica matrix enabled the subsequent binding of cobalt(II) ions. Lyogels with various amounts of ethylenediamine moieties (0.1–15 mol %) were soaked in isopropanol solutions of cobalt(II) nitrate and further supercritically dried in carbon dioxide to obtain aerogels with a specific surface area of 210–596 m 2 ·g −1 , an apparent density of 0.403–0.740 cm 3 ·g −1 and a porosity of 60–78%. The actual cobalt content in the aerogels was 0.01–1.50 mmol per 1 g of SiO 2 , which could easily be tuned by the concentration of ethylenediamine moieties in the silica matrix. The introduction of cobalt(II) ions into the ethylenediamine-modified silica aerogel promoted the stability of the diamine moieties at the supercritical drying stage. The molecular prototype of the immobilized cobalt(II) complex, bearing one ethylenediamine ligand [Co(en)(MeCN)(NO 3 ) 2 ], was synthesized and structurally characterized. Using magnetometry in the DC mode, it was shown that cobalt(II)-modified silica aerogels exhibited slow magnetic relaxation in a nonzero field. A decrease in cobalt(II) concentration in aerogels from 1.5 mmol to 0.14 mmol per 1 g of SiO 2 resulted in a weakening of inter-ion interactions; the magnetization reversal energy barrier likewise increased from 4 to 18 K.
The chemical immobilization of cobalt(II) ions in a silica aerogel matrix enabled the synthesis of the first representative example of aerogel-based single-ion magnets. For the synthesis of the lyogels, methyl-trimethoxysilane and N-3-(trimethoxysilyl)propyl ethylenediamine were co-hydrolyzed, then the ethylenediamine groups that were immobilized on the silica matrix enabled the subsequent binding of cobalt(II) ions. Lyogels with various amounts of ethylenediamine moieties (0.1-15 mol %) were soaked in isopropanol solutions of cobalt(II) nitrate and further supercritically dried in carbon dioxide to obtain aerogels with a specific surface area of 210-596 m[sup.2]·g[sup.−1], an apparent density of 0.403-0.740 cm[sup.3]·g[sup.−1] and a porosity of 60-78%. The actual cobalt content in the aerogels was 0.01-1.50 mmol per 1 g of SiO[sub.2], which could easily be tuned by the concentration of ethylenediamine moieties in the silica matrix. The introduction of cobalt(II) ions into the ethylenediamine-modified silica aerogel promoted the stability of the diamine moieties at the supercritical drying stage. The molecular prototype of the immobilized cobalt(II) complex, bearing one ethylenediamine ligand [Co(en)(MeCN)(NO[sub.3])[sub.2]], was synthesized and structurally characterized. Using magnetometry in the DC mode, it was shown that cobalt(II)-modified silica aerogels exhibited slow magnetic relaxation in a nonzero field. A decrease in cobalt(II) concentration in aerogels from 1.5 mmol to 0.14 mmol per 1 g of SiO[sub.2] resulted in a weakening of inter-ion interactions; the magnetization reversal energy barrier likewise increased from 4 to 18 K.
Audience Academic
Author Khamova, Tamara V
Sharipov, Alim U
Kottsov, Sergey Yu
Shmelev, Maxim A
Kiskin, Mikhail A
Rubtsova, Irina K
Ivanov, Vladimir K
Efimov, Nikolay N
Roslyakov, Ilya V
Baranchikov, Alexander E
Eremenko, Igor L
Nikolaevskii, Stanislav A
Kopitsa, Gennady P
AuthorAffiliation 1 Kurnakov Institute of General and Inorganic Chemistry, Russian Academy of Sciences, Moscow 119991, Russia
2 Faculty of Technology of Inorganic Substances and High Temperature Materials, Mendeleev University of Chemical Technology of Russia, Moscow 125047, Russia
3 St.-Petersburg Nuclear Physics Institute, National Research Center “Kurchatov Institute”, Gatchina 188300, Russia
4 Grebenshchikov Institute of Silicate Chemistry, Russian Academy of Sciences, St.-Petersburg 199034, Russia
5 Department of Materials Science, Lomonosov Moscow State University, Moscow 119991, Russia
6 Faculty of Chemistry, National Research University Higher School of Economics, Moscow 109028, Russia
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– name: 4 Grebenshchikov Institute of Silicate Chemistry, Russian Academy of Sciences, St.-Petersburg 199034, Russia
– name: 5 Department of Materials Science, Lomonosov Moscow State University, Moscow 119991, Russia
– name: 6 Faculty of Chemistry, National Research University Higher School of Economics, Moscow 109028, Russia
– name: 3 St.-Petersburg Nuclear Physics Institute, National Research Center “Kurchatov Institute”, Gatchina 188300, Russia
– name: 2 Faculty of Technology of Inorganic Substances and High Temperature Materials, Mendeleev University of Chemical Technology of Russia, Moscow 125047, Russia
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  givenname: Sergey Yu
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  givenname: Stanislav A
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  givenname: Igor L
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  surname: Eremenko
  fullname: Eremenko, Igor L
  organization: Kurnakov Institute of General and Inorganic Chemistry, Russian Academy of Sciences, Moscow 119991, Russia
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  givenname: Vladimir K
  orcidid: 0000-0003-2343-2140
  surname: Ivanov
  fullname: Ivanov, Vladimir K
  organization: Faculty of Chemistry, National Research University Higher School of Economics, Moscow 109028, Russia
BackLink https://www.ncbi.nlm.nih.gov/pubmed/36615607$$D View this record in MEDLINE/PubMed
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Issue 1
Keywords magnetic properties
electron paramagnetic resonance
single-ion magnet
chemical immobilization
single-molecule magnet
Raman spectroscopy
aerogel
N-3-(trimethoxysilyl)propyl ethylenediamine
Language English
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Snippet The chemical immobilization of cobalt(II) ions in a silica aerogel matrix enabled the synthesis of the first representative example of aerogel-based single-ion...
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SubjectTerms aerogel
Bulk density
Carbon dioxide
Case studies
chemical immobilization
Cobalt
Cobalt compounds
Diamines
Ethylenediamine
Immobilization
Information storage
Ions
Magnetic induction
Magnetic measurement
magnetic properties
Magnetic relaxation
Magnetization
Magnetization reversal
N-3-(trimethoxysilyl)propyl ethylenediamine
Nanoparticles
Porosity
Silica
Silica aerogels
Silicon dioxide
single-ion magnet
single-molecule magnet
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Title Aerogel-Based Single-Ion Magnets: A Case Study of a Cobalt(II) Complex Immobilized in Silica
URI https://www.ncbi.nlm.nih.gov/pubmed/36615607
https://www.proquest.com/docview/2761196974
https://search.proquest.com/docview/2761984857
https://pubmed.ncbi.nlm.nih.gov/PMC9824035
https://doaj.org/article/0701f9b8ff734ea59f9043e17f979d72
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