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Organomagnesia: Reversibly High Carbon Dioxide Uptake by Magnesium Pyrazolates.

ABSTRACT: A series of new pyrazolate and mixed pyrazolate/pyrazole magnesium complexes is described and their reactivity toward carbon dioxide is examined. The dimeric complex [Mg(pz^t ^Bu, ^t ^Bu)₂]₂ inserts CO₂ instantly and quantitatively forming the tetrameric complex [Mg(CO₂·pz^t ^Bu, ^t ^Bu)₂]₄ and monomeric donor-stabilized [Mg(CO₂·pz^t ^Bu, ^t ^Bu)₂(thf)₂]. Complexes of the type [Mg_x(pz^R,R)₂ _x(Hpz^R,R)_y]_n (R = iPr, tBu) engage in similar insertion reactions involving dissociation of the carbamic acid HOOCpz^R,R. Even solid polymeric derivatives [Mg(pz^R,R)₂]_n (R = Me, H) react instantaneously and exhaustively with CO₂, the resulting [Mg(CO₂·pz)₂]_m featuring a CO₂ capacity of 35.7 wt% (8.2 mmol g^-1). All described magnesium pyrazolates display completely reversible CO₂ uptake in solution and in the solid state, respectively, as monitored via VT ¹H NMR and in situ FTIR spectroscopy as well as thermogravimetric analysis. Fluorinated [Mg₂(pz^CF3,CF3)₄(thf)₃] does not yield any isolable CO₂ insertion product but exhibits the highest activity in the catalytic transformation of epoxides and CO₂ to cyclic carbonates.

SUBMITTER: Kracht F

PROVIDER: S-EPMC11348227 | biostudies-literature | 2024 Aug

REPOSITORIES: biostudies-literature

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Organomagnesia: Reversibly High Carbon Dioxide Uptake by Magnesium Pyrazolates.

Kracht Felix F Rolser Philipp P Preisenberger Paul P Maichle-Mössmer Cäcilia C Anwander Reiner R

Advanced science (Weinheim, Baden-Wurttemberg, Germany) 20240621 32

A series of new pyrazolate and mixed pyrazolate/pyrazole magnesium complexes is described and their reactivity toward carbon dioxide is examined. The dimeric complex [Mg(pzt Bu, t Bu)2]2 inserts CO2 instantly and quantitatively forming the tetrameric complex [Mg(CO2·pzt Bu, t Bu)2]4 and monomeric donor-stabilized [Mg(CO2·pzt</su ...[more]

PMID: 39189457

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Project description:Physiological effects of carbon dioxide and impact on genome-wide transcript profiles were analysed in chemostat cultures of Saccharomyces cerevisiae. In anaerobic, glucose-limited chemostat cultures grown at atmospheric pressure, cultivation under CO2-saturated conditions had only a marginal (<10%) impact on the biomass yield. Conversely, a 25% decrease of the biomass yield was found in aerobic, glucose-limited chemostat cultures aerated with a mixture of 79% CO2 and 21% O2. This observation indicated that respiratory metabolism is more sensitive to CO2 than fermentative metabolism. Consistent with the more pronounced physiological effects of CO2 in respiratory cultures, the number of CO2-responsive transcripts was higher in aerobic cultures than in anaerobic cultures. Many genes involved in mitochondrial functions showed a transcriptional response to elevated CO2 concentrations. This is consistent with an uncoupling effect of CO2 and/or intracellular bicarbonate on the mitochondrial inner membrane. Other transcripts that showed a significant transcriptional response to elevated CO2 included NCE103 (probably encoding carbonic anhydrase), PCK1 (encoding PEP carboxykinase) and members of the IMD gene family (encoding isozymes of inosine monophosphate dehydrogenase Experiment Overall Design: Knowledge on the genome-wide transcriptional response of S. cerevisiae to high CO2 concentrations may provide a deeper insight into the molecular mechanisms of CO2 stress. Such insight is essential to develop metabolic-engineering strategies for improving CO2 tolerance. Furthermore, identification of âsignature transcriptsâ that uniquely respond to CO2 stress may be applicable for diagnosing the CO2 status of industrial fermentations. It has recently been demonstrated that the combination of chemostat cultivation with DNA-microarray-based transcriptome analysis offers a powerful and reproducible approach to identify the transcriptional responses of yeasts to environmental parameters For this reason, in the present study we used chemostat cultures of S. cerevisiae to quantify the effect of CO2 on respiring and fermenting cells, and to determine the genome-wide transcriptional responses of this yeast to high CO2 concentrations.

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Organomagnesia: Reversibly High Carbon Dioxide Uptake by Magnesium Pyrazolates.

Publications

Organomagnesia: Reversibly High Carbon Dioxide Uptake by Magnesium Pyrazolates.

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