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Issue 25, 2019
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An FeIII dinuclear metallacycle complex as a size-selective adsorbent for nitrogenous compounds and a potentially effective ammonia storage material

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Abstract

Ammonia has a large volume energy density and consequently high potential for application as a fuel and energy reservoir in the future. In this study, the dinuclear FeIII metallacycle complex [Fe2(H2opba)2Cl2(dmso)2]·2CH2Cl2·2dmso (1) with excellent capacity to selectively adsorb ammonia (11.3 mmol g−1) was investigated, demonstrating a strong preference for nitrogenous compounds, especially short-chain amines. The adsorption results suggest that the cavity in the structure of 1 has an essential role in the adsorption mechanism i.e. it is the responsible for size selectivity of 1 during the adsorption process. To better understand the adsorption mechanism of ammonia, 1 was fully characterized before and after adsorption. Thermogravimetric-mass spectrometry (TG-MS) and ammonia isotherm experiments revealed that 8 ammonia molecules were physisorbed by the complex cavity (free ammonia) and 4 ammonia molecules were chemisorbed (coordinated ammonia) per dinuclear metallacycle unit. Further characterization also confirmed the proposed adsorption mechanism, corroborating the structural modification of the compound after its interaction with ammonia; in addition, reuse tests showed that despite a small loss of efficiency, the compound was capable of desorbing most of the ammonia and could be used consecutively for at least three cycles. Thus, 1 is a potential ammonia storage material and adsorbent for the removal of ammonia from effluents.

Graphical abstract: An FeIII dinuclear metallacycle complex as a size-selective adsorbent for nitrogenous compounds and a potentially effective ammonia storage material

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Supplementary files

Article information


Submitted
10 Oct 2018
Accepted
22 May 2019
First published
23 May 2019

J. Mater. Chem. A, 2019,7, 15225-15232
Article type
Paper

An FeIII dinuclear metallacycle complex as a size-selective adsorbent for nitrogenous compounds and a potentially effective ammonia storage material

I. F. Silva, I. F. Teixeira, W. P. Barros, C. B. Pinheiro, J. D. Ardisson, G. M. do Nascimento, N. A. Pradie, A. P. C. Teixeira and H. O. Stumpf, J. Mater. Chem. A, 2019, 7, 15225
DOI: 10.1039/C8TA09786K

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