(H3dien)[Ni(NO3)(C2O4)2].2H2O: Synthesis, crystal structure, catalytic activity and magnetic study

doi:10.1016/j.cdc.2022.100969

Chemical Data Collections

Volume 42, December 2022, 100969

https://doi.org/10.1016/j.cdc.2022.100969 Get rights and content

Highlights

•
The hybrid material (H₃dien)[Ni(NO₃)(C₂O₄)₂].2H₂O was synthesized using a soft chemistry route.
•
The crystal structure has been determined by X-ray single crystal diffraction.
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Thermal behavior of title compound has been studied by TGA/DTA analysis.
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The new compound turned to be an effective catalyst for the reduction reaction of the three nitrophenol isomers.
•
The negative Curie-Weiss temperature reveals antiferromagnetic coupling between the spin holders.

Abstract

The complex (H₃dien)[Ni(NO₃)(C₂O₄)₂].2H₂O, with (dien) is the diethylenetriamine (NH₂CH₂CH₂)₂NH, and was synthesized in solution. It was characterized using single-crystal X-ray diffraction, Infrared (FT-IR) and UV-Visible spectroscopies, and TG-DTA thermal analysis. FT-IR confirmed the characteristic bands of diethylenetriamine, nitrate and oxalate groups. (H₃dien)[Ni(NO₃)(C₂O₄)₂].2H₂O crystallizes into the monoclinic system (P2₁/c). Nickel has a square-based pyramidal NiO5 coordination. O-H...O and N-H...O H-bonds connect ionic entities and water molecules into bc-plane-parallel slabs. The UV-Visible spectrum shows absorption bands compatible with a six-coordinated high-spin octahedral Ni(II). Magnetization and a.c. susceptibility measurements were measured. The catalytic efficiency of the title compound in the reduction by NaBH4 of three nitrophenol isomers to their corresponding aminophenols was tested.

Graphical abstract

Section snippets

Specifications table

Subject area	Chemical Engineering.
Compounds	(H3dien)[Ni(NO3)(C2O4)2].2H2O: diethylenetriammonium nitrato-bis(oxalato)nickelate(II)dihydrate
Data category	Synthesis, crystallography, physico-chemistry studies.
Data acquisition format	Raw and simulated.
Data type	XRD, IR, UV-Visible, ATG-ATD, Magnetization and susceptibility, efficiency parameters.
Procedure	Wet chemistry synthesis, single and powder X-Rays characterizations, Infrared spectroscopy (FT-IR), UV-Visible spectroscopy and thermal stability

Rationale

During the last decades, the synthesis of hybrid materials has attracted considerable interest due to their new structural topologies, applications in the fields of catalysis, ion exchange and biochemistry [1], [2], [3], [4], [5], [6], and interesting magnetic properties [7,8]. Among these, a large number of open-framework compounds are based on metal phosphates [9]. Carboxylates ligands are versatile owing to the various modes of coordination such as monodentate, bidendate, or tetradentate

Synthesis of complex 1

Single crystals of complex 1 were synthesized by a wet chemistry method. The reaction mixture of Ni(NO₃)₂.6H₂O (0.34 g, 1.41 mmol) dissolved in distilled water (10 mL) was added dropwise to an aqueous solution (15 mL) of oxalic acid (0.52 g, 2.82 mmol) at room temperature with continuous stirring. Diethylenetriamine (1.7 mL, 15.60 mmol) dissolved in distilled water (15 mL) was dropwise added. This solution was allowed to evaporate slowly until blue single-crystals were formed. These crystals

Description of the structure

The crystal structure of (H₃dien)[Ni(NO₃)(C₂O₄)₂].2H₂O is made up of [Ni(C2O4)2(NO3)]3- anions, diethylenetriammonium cations (H3dien)3+, and water molecules. The asymmetric unit contains 26 non-hydrogen atoms (Fig. 1), and it is isostructural with diethylenetriammonium bis(oxalato)cuprate(II) reported by Savel'eva et al.

One nitrate and two oxalate ions coordinate the Ni²⁺, respectively in monodentate, via the O8, and bidentate, through the couples (O5, O12) and (O10, O11) forming the square

Conclusion

A new diethylenetriammonium nitrato-bis(oxalato)nickelate(II) dihydrate (H₃dien)[Ni(NO₃)(C₂O₄)₂].2H₂O was successfully synthesized using a soft chemistry route. The title compound was characterized by single-crystal X-ray diffraction, Infrared spectroscopy (FT-IR) and thermal stability analysis (TG-DTA). FT-IR confirmed the presence of the characteristic bands of diethylenetriamine, nitrate and oxalate groups. The complex crystallizes in the monoclinic system, space group P2₁/c and its

Declaration of Competing Interest

The authors declare no conflict of interest.

Acknowledgment

M. Lachkar is thanking the support of the University Sidi Mohamed ben Abdellah. The crystallographic part was supported by the project 18-10504S of the Czech Science Foundation using instruments of the CzechNanoLab Research Infrastructure supported by MEYS CR (LM2018110).

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Data Article(H3dien)[Ni(NO3)(C2O4)2].2H2O: Synthesis, crystal structure, catalytic activity and magnetic study

Highlights

Abstract

Graphical abstract

Section snippets

Specifications table

Rationale

Synthesis of complex 1

Description of the structure

Conclusion

Declaration of Competing Interest

Acknowledgment

Polyhedron

J. Solid State Chem.

Chem. Data Collect.

Inorg. Chem. Commun.

J. Mol. Struct.

Acta Cryst.

Inorg. Chem. Commun.

Polyhedron

Spectrochim. Acta A

J. Solid State Chem.

Inorg. Chem. Commun.

Phys. B Condens. Matter

Polyhedron

J. Mol. Struct.

J. Anal. Appl. Pyrolysis

Phys. B Condens. Matter

Acta Cryst.

Cambridge Crystallographic Data Centre

Acta A Mol. Biomol. Spectrosc.

Inorg. Chem.

J. Solid. State Chem.

Thermochim. Acta

Colloids Surf. B

J. Mol. Struct.

Spectrochim. Acta A

J. Photochem. Photobiol. A

Chem. Eur.

J. Phys. Chem. A

Molecules

Appl. Catal. B Environ.

Molecules

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Automotive fuels and internal combustion engines: a chemical perspective

Chem. Soc. Rev.

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J. Coord. Chem.

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Inorg. Chem. Front.

Luminescent and magnetic properties of lanthanide-thiophene-2, 5-dicarboxylate hybrid materials

Cryst. Growth Des.

Porous Zn (II)-based metal-organic frameworks decorated with carboxylate groups exhibiting high gas adsorption and separation of organic dyes

Cryst. Growth Des.

Data Article
(H₃dien)[Ni(NO₃)(C₂O₄)₂].2H₂O: Synthesis, crystal structure, catalytic activity and magnetic study