Evolutionary Steps in the Analytics of Primordial Metabolic Evolution
Experimental studies of primordial metabolic evolution are based on multi-component reactions which typically result in highly complex product mixtures. The detection and structural assignment of these products crucially depends on sensitive and selective analytical procedures. Progress in the instr...
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| Format: | Article |
| Language: | English |
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MDPI AG
2019-06-01
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| Series: | Life |
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| Online Access: | https://www.mdpi.com/2075-1729/9/2/50 |
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| author | Thomas Geisberger Philippe Diederich Thomas Steiner Wolfgang Eisenreich Philippe Schmitt-Kopplin Claudia Huber |
| author_facet | Thomas Geisberger Philippe Diederich Thomas Steiner Wolfgang Eisenreich Philippe Schmitt-Kopplin Claudia Huber |
| author_sort | Thomas Geisberger |
| collection | DOAJ |
| description | Experimental studies of primordial metabolic evolution are based on multi-component reactions which typically result in highly complex product mixtures. The detection and structural assignment of these products crucially depends on sensitive and selective analytical procedures. Progress in the instrumentation of these methods steadily lowered the detection limits to concentrations in the pico molar range. At the same time, conceptual improvements in chromatography, nuclear magnetic resonance (NMR) and mass spectrometry dramatically increased the resolution power as well as throughput, now, allowing the simultaneous detection and structural determination of hundreds to thousands of compounds in complex mixtures. In retrospective, the development of these analytical methods occurred stepwise in a kind of evolutionary process that is reminiscent of steps occurring in the evolution of metabolism under chemoautotrophic conditions. This can be nicely exemplified in the analytical procedures used in our own studies that are based on Wächtershäuser’s theory for metabolic evolution under Fe/Ni-catalyzed volcanic aqueous conditions. At the onset of these studies, gas chromatography (GC) and GC-MS (mass spectrometry) was optimized to detect specific low molecular weight products (<200 Da) in a targeted approach, e.g., methyl thioacetate, amino acids, hydroxy acids, and closely related molecules. Liquid chromatography mass spectrometry (LC-MS) was utilized for the detection of larger molecules including peptides exceeding a molecular weight of 200 Da. Although being less sensitive than GC-MS or LC-MS, NMR spectroscopy benefitted the structural determination of relevant products, such as intermediates involved in a putative primordial peptide cycle. In future, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) seems to develop as a complementary method to analyze the compositional space of the products and reaction clusters in a non-targeted approach at unprecedented sensitivity and mass resolution (700,000 for m/z 250). Stable isotope labeling was important to differentiate between reaction products and artifacts but also to reveal the mechanisms of product formation. In this review; we summarize some of the developmental steps and key improvements in analytical procedures mainly used in own studies of metabolic evolution. |
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| institution | Directory Open Access Journal |
| issn | 2075-1729 |
| language | English |
| last_indexed | 2024-04-11T13:40:32Z |
| publishDate | 2019-06-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Life |
| spelling | doaj.art-510afb31031949d5afcc84c670c6a8292022-12-22T04:21:16ZengMDPI AGLife2075-17292019-06-01925010.3390/life9020050life9020050Evolutionary Steps in the Analytics of Primordial Metabolic EvolutionThomas Geisberger0Philippe Diederich1Thomas Steiner2Wolfgang Eisenreich3Philippe Schmitt-Kopplin4Claudia Huber5Department of Biochemistry, Technical University of Munich, 80333 Munich, GermanyResearch Unit Analytical BioGeoChemistry, Helmholtz Zentrum München–German Research Center for Environmental Health, 85764 Neuherberg, GermanyDepartment of Biochemistry, Technical University of Munich, 80333 Munich, GermanyDepartment of Biochemistry, Technical University of Munich, 80333 Munich, GermanyResearch Unit Analytical BioGeoChemistry, Helmholtz Zentrum München–German Research Center for Environmental Health, 85764 Neuherberg, GermanyDepartment of Biochemistry, Technical University of Munich, 80333 Munich, GermanyExperimental studies of primordial metabolic evolution are based on multi-component reactions which typically result in highly complex product mixtures. The detection and structural assignment of these products crucially depends on sensitive and selective analytical procedures. Progress in the instrumentation of these methods steadily lowered the detection limits to concentrations in the pico molar range. At the same time, conceptual improvements in chromatography, nuclear magnetic resonance (NMR) and mass spectrometry dramatically increased the resolution power as well as throughput, now, allowing the simultaneous detection and structural determination of hundreds to thousands of compounds in complex mixtures. In retrospective, the development of these analytical methods occurred stepwise in a kind of evolutionary process that is reminiscent of steps occurring in the evolution of metabolism under chemoautotrophic conditions. This can be nicely exemplified in the analytical procedures used in our own studies that are based on Wächtershäuser’s theory for metabolic evolution under Fe/Ni-catalyzed volcanic aqueous conditions. At the onset of these studies, gas chromatography (GC) and GC-MS (mass spectrometry) was optimized to detect specific low molecular weight products (<200 Da) in a targeted approach, e.g., methyl thioacetate, amino acids, hydroxy acids, and closely related molecules. Liquid chromatography mass spectrometry (LC-MS) was utilized for the detection of larger molecules including peptides exceeding a molecular weight of 200 Da. Although being less sensitive than GC-MS or LC-MS, NMR spectroscopy benefitted the structural determination of relevant products, such as intermediates involved in a putative primordial peptide cycle. In future, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) seems to develop as a complementary method to analyze the compositional space of the products and reaction clusters in a non-targeted approach at unprecedented sensitivity and mass resolution (700,000 for m/z 250). Stable isotope labeling was important to differentiate between reaction products and artifacts but also to reveal the mechanisms of product formation. In this review; we summarize some of the developmental steps and key improvements in analytical procedures mainly used in own studies of metabolic evolution.https://www.mdpi.com/2075-1729/9/2/50origin of lifeGC-MSLC-MSNMRFT-ICRstable isotopesreaction network |
| spellingShingle | Thomas Geisberger Philippe Diederich Thomas Steiner Wolfgang Eisenreich Philippe Schmitt-Kopplin Claudia Huber Evolutionary Steps in the Analytics of Primordial Metabolic Evolution Life origin of life GC-MS LC-MS NMR FT-ICR stable isotopes reaction network |
| title | Evolutionary Steps in the Analytics of Primordial Metabolic Evolution |
| title_full | Evolutionary Steps in the Analytics of Primordial Metabolic Evolution |
| title_fullStr | Evolutionary Steps in the Analytics of Primordial Metabolic Evolution |
| title_full_unstemmed | Evolutionary Steps in the Analytics of Primordial Metabolic Evolution |
| title_short | Evolutionary Steps in the Analytics of Primordial Metabolic Evolution |
| title_sort | evolutionary steps in the analytics of primordial metabolic evolution |
| topic | origin of life GC-MS LC-MS NMR FT-ICR stable isotopes reaction network |
| url | https://www.mdpi.com/2075-1729/9/2/50 |
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