Prebiotic iron–sulfur peptide catalysts generate a pH gradient across model membranes of late protocells

Bonfio, Claudia; Godino, Elisa; Corsini, Maddalena; Biani, Fabrizia Fabrizi de; Guella, Graziano; Mansy, Sheref S.

doi:10.1038/s41929-018-0116-3

Cited by 89 publications

(109 citation statements)

References 53 publications

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“…Regeneration of NAD + was chemically driven in recent studies by Wang et al and Bonfia et al In the first example, NADH was encapsulated inside of lipid vesicles. Alike other mentioned examples where soluble redox mediators were used, in this contribution, the redox mediator was confined inside of the lipid membrane.…”

Section: Nad(h) Regenerationmentioning

confidence: 99%

Artificial Organelles for Energy Regeneration

et al. 2019

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cell's total energy budget. [2] The universal energy currency that is used for these purposes and can be found in all forms of life is adenosine triphosphate (ATP). A vast majority of the cellular energy demand is covered by either converting a large variety of energy-rich substrates into ATP in a process called oxidative phosphorylation, or by converting light (electromagnetic) energy into ATP in a process called photophosphorylation (or photosynthesis).These naturally existing energy conversions are valid in in the context of bottomup synthetic biology as well. In the latter, an artificial cell is envisioned as a compendium of functional modules, each hand-tailored to partially or entirely mimic one of the essential life processes, such as reproduction, growth, motility, etc. [3] Like their natural counterparts, all these reenvisioned synthetic processes are energy demanding, therefore, the deliberate design of synthetic cells should involve suitable energy management strategy, by, for example, continuous regeneration of ATP. Apart from the importance in the context of artificial cells, new energy conversion strategies can be considered as a standalone feature for enzymatic and cell-free biotechnology, wherein bottom-up synthetic biology might also deliver new and sustainable solutions.The notion of synthetic in terms of engineered and/or non-natural can be even expanded to other forms of energy (like electrical energy) and non-natural building blocks. The chemically driven ATP synthesis, as in oxidative phosphorylation, represents a spontaneous process, in which the electrons of a fuel (glucose, NADH) are transferred to an electron acceptor such as oxygen with the concomitant generation of proton gradient, which is afterwards stored again as chemical energy in ATP. In the realm of synthetic biology, other options might also be feasible, for example: can we use electrical energy and directly plug it in to drive biological processes [4,5] or make use of natural electron transfer mechanisms to produce electricity? [6] The Electron Transport Chain-a Natural Toolbox of Functional Parts for the Construction of Artificial OrganellesDuring the process of oxidative phosphorylation, electrons are passed from an electron donor ("fuel") with a more negative One of the critical steps in sustaining life-mimicking processes in synthetic cells is energy, i.e., adenosine triphosphate (ATP) regeneration. Previous studies have shown that the simple addition of ATP or ATP regeneration systems, which do not regenerate ATP directly from ADP and P i , have no or only limited success due to accumulation of ATP hydrolysis products. In general, ATP regeneration can be achieved by converting light or chemical energy into ATP, which may also involve redox transformations of cofactors. The present contribution provides an overview of the existing ATP regeneration strategies and the related nicotinamide adenine dinucleotide (NAD + ) redox cycling, with a focus on compartmentalized systems. Special attention is being paid to those approach...

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Section: Nad(h) Regenerationmentioning

confidence: 99%

Artificial Organelles for Energy Regeneration

et al. 2019

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“…Writing in Nature Catalysis, Mansy and colleagues demonstrate that simple iron-sulfur peptides catalyse electron transfer reactions ( Figure 1). 3 Although simple aqueous ferric (Fe(III)) ions oxidise NADH, the resulting acidic solution destroys the NAD + that forms. Increasing the pH would prevent NAD + degradation, but this leads to precipitation of inactive oxo-hydroxo iron complexes.…”

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confidence: 99%

“…When these iron-sulfur catalysts are encapsulated in POPC (model protocell) membranes with 0.5 mM NADH, stoichiometric hydrogen peroxide reduction establishes a trans-membrane pH-gradient (40 mV), with a similar magnitude to electrochemical gradients found across biological membranes. 3 Establishing a trans-membrane electrochemical gradient by membrane-localised redox catalysts lays the foundations to develop simple systems that exploit these gradients to drive anabolic reactions.…”

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“…However, maintaining an electrochemical gradient requires, in addition to a competent catalyst, feedstock reagents (nutrients) and a well-tuned semi-permeable membrane. Simpler (fatty acid) membranes could not harness this gradient, 3 outlining the need to simultaneously develop dynamic interactions amongst the constituent molecules of life from the outset. Functions must be balanced, and sealing a membrane to an ion gradient could, in principle, block essential nutrients (or reagents) accessing the cell.…”

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confidence: 99%

“…However, current methods for (short) prebiotic peptide synthesis remain ineffective for amino acids with functional side chains such as cysteine and serine, and the pronounced nucleophilicity of thiols renders cysteine incompatible with current methods for electrophilic activation of amino acids. Nevertheless, in a broader sense, the work of Bonfio et al 3,4 suggests that the activity of simple iron-sulfur peptides could have helped to couple catabolism with anabolism during early evolution, and exemplifies value accrued by uniting catalysis with compartmentalisation.…”

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confidence: 99%

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