Spontaneous chemical fixation of atmospheric CO2 by polydentate amine in Zinc(II) bound state

The activation of atmospheric CO2 and its chemical fixation as metal carbonate complexes are of continuous attention for the purpose of fundamental research but also in terms of potential application to reduce the concentration of this greenhouse gas. Carbon dioxide is slightly soluble water. In aqueous medium gaseous CO2 is in equilibrium with carbonic acid (H2CO3) through the following reactions:

CO2(g) ⇌ CO2(aq) CO2(aq) + H2O(l) ⇌ H2CO3(aq)

The equilibrium constant for the reaction at 25°C is Kh = 1.70×10−3. This means that most of the carbon dioxide remains as CO2 molecules, rather than being converted into carbonic acid.
It is well known that at pH ~ 6.0 carbonic acid is in equilibrium with bicarbonate anion and at pH ~ 10 bicarbonate anion is in equilibrium with carbonate anion (Scheme 1). This equilibrium suggests that in alkaline medium, solubility of CO2 increases and majorly exists as carbonate anion (CO32-).

Scheme 1 pH dependent equilibria of CO2 in water

This carbonate anion can act as monodentate and bidentate ligands binding a single metal ion or as a bridging ligand linking more than one metal ions through its various coordination modes (Scheme 2).

Scheme 2 Various coordination modes of carbonate anion

In this present endeavor, we have explored the coordination behavior of carbonate anion in alkaline medium for the spontaneous chemical fixation of atmospheric CO2 in the form of crystalline zinc(II) amine carbonate complex. In aqueous medium, we have taken zinc(II) perchlorate hexahydrate salt and a tailored tetradentate amine, N,N’-bis(3-aminopropyl)-1,2- ethanediamine (L, Scheme 3) in 1:1 molar ratio in a beaker and left undisturbed in an open air.

Scheme 3 Tetradentate amine, N,N’-bis(3-aminopropyl)-1,2-ethanediamine (L)

After 2-3 days colourless crystalline compounds appeared at the surface of the solution as well at the bottom of the beaker. This compound is then collected by filtration and dried in air-oven at 105 °C. The formation of zinc(II) amine carbonate complex has been established through FTIR spectrum of the isolated compound. In FTIR spectrum, ν(N–H) stretching frequencies of the –NH2 groups of L is observed at ~3230 cm-1. Several weak bands in the range 2880–2950 cm-1 assignable to aliphatic C–H stretching vibration are observed. The asymmetric stretching vibrations of carbonate are seen at 1480 and 1440 cm-1. The presence of perchlorate stretches at 1150, 1120, 1080 and 620 cm-1 are indicative of non-coordination to the metal centre. The formulation of the isolated complex as [Zn3(μ3-CO3)(L)3](ClO4)4 (1) is established by single crystal X-ray diffraction analysis (Scheme 4). Structural analyses show that the complex 1 consist of one trinuclear [Zn3(μ3-CO3)(L)3]4+ cation and four perchlorates as counter anions. The formation of carbonate complex 1 may presumably be due to intake of CO2 from atmosphere by the alkaline zinc(II) amine species that leads to transformation of CO2 into CO 2- anion at pH ~11 in aqueous solution followed by coordinating three metal centres [Zn(L)]2+ through tris(monodentate) bridging mode (Scheme 4).

Scheme 4 (a) Formation of carbonate complex and molecular structure of (b) [Zn3(μ3- CO3)(L)3](ClO4)4 (1) and (c) [Zn3(μ3-CO3)(L)3]4+ cation

This present work illustrates that Zinc (II) ion in combination with judiciously chosen polyamine creates suitable alkaline medium which triggers the fixation of atmospheric carbon dioxide into carbonate complex. We are now active to investigate such fixation of this greenhouse gas to some other metal ions such as Copper (II), Nickel(II), Cobalt(II) and Cadmium(II) in combination with L and other polydentate amines.

Contributed by Dr. Kishalay Bhar

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Spontaneous chemical fixation of atmospheric CO2 by polydentate amine in Zinc(II) bound state

Scheme 1 pH dependent equilibria of CO2 in water

Scheme 2 Various coordination modes of carbonate anion

Scheme 3 Tetradentate amine, N,N’-bis(3-aminopropyl)-1,2-ethanediamine (L)

Testimonial

Mitra S.K. have added value to our business process by effective inspection, strict quality control and timely response. It is a pleasant experience to work with “Team Mitra S.K.”. We hope the same service level will continue in the future too....

Sirsendu Mukherjee

Mitra SK Inspection Gulf LLC has been appointed by us and the services provided by them has been up to the mark and as per our expectations....

Ajay Mathur

Amar Singh Gohil

The Inspection services provided by Mitra S. K. Inspection Gulf has been prompt and accurate and has been in the line with our expectations....

Naser Bustami

We would like to express our high appreciation of the business association our company had with Mitra S. K. as a testing and inspection house for their quality of service, good documentation and reporting during the job ....

R. Jeyakumar

Tulus Situmeang

Their job was excellent and showed Mitra S.K. differential from others....

Geraldo Pimenta

Konstantin Gertsen

We’ve been pleased with the improvement we have seen in CIQ results, and Mitra S.K’s reports have certainly helped us to resolve any disputes with our customers in a more timely manner….....

Brian Mcdonald

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