The “Origin-of-Life Reactor” and Reduction of CO2 by H2 in Inorganic Precipitates

Letter to the Editor


It has been suggested that inorganic membranes were forerunners of organic membranes at the origin of life. Such membranes, interposed between alkaline fluid in submarine vents and the more acidic Hadean ocean, were thought to house inorganic molecular machines. H+ flowed down the pH gradient (ΔpH) from ocean to vent through the molecular machines to drive metabolic reactions for early life. A set of experiments was performed by Herschy et al. (J Mol Evol 79:213–227, 2014) who followed earlier work to construct inorganic precipitate membranes which, they argued, would be transected by a ΔpH. They supposed that inorganic molecular machines might assemble by chance in the precipitate membranes, and be capable of using the ΔpH to drive unfavourable reduction of CO2 by H2 to formate and formaldehyde. Indeed, these workers detected both of these compounds in their origin-of-life reaction vessel and contend this was proof of principle for their hypothesis. However, it is shown here by a straightforward calculation that the formate produced was only that which reached on approach to equilibrium without any driving force from ΔpH. We conclude that the reaction was facilitated by isotropic catalysts in the precipitate membrane but not by an anisotropic ΔpH-driven molecular machine.


Inorganic membranes Natural pH gradient Hydrothermal vents Chemiosmotic theory Origin of life 


  1. Barge LM, Doloboff IJ, White LM, Stucky GD, Russell MJ, Kanik I (2012) Characterization of iron-phosphate-silicate chemical garden structures. Langmuir 28:3714–3721CrossRefPubMedGoogle Scholar
  2. Barge LM, Branscomb E, Brucato JR, Cardoso SSS, Cartwright JHE, Danielache SO, Galante D, Kee TP, Miguel Y, Mojzsis S, Robinson KJ, Russell MJ, Simoncini E, Sobron P (2017) Thermodynamics, disequilibrium, evolution: far from equilibrium geological and chemical considerations for origin of life research. Orig Life Evol Biosph. doi:10.1007/s11084-016-9508-z PubMedGoogle Scholar
  3. Borowska Z, Mauzerall D (1988) Photoreduction of carbon dioxide by aqueous ferrous ion: an alternative to the strongly reducing atmosphere for the chemical origin of life. Proc Natl Acad Sci USA 85:6577–6580CrossRefPubMedPubMedCentralGoogle Scholar
  4. Borowska Z, Mauzerall D (1991) Retraction. Proc Natl Acad Sci USA 88:4564Google Scholar
  5. Coatman RD, Thomas NL, Double DD (1980) Studies of the growth of “silicate gardens” and related phenomena. J Mater Sci 15:2017–2026CrossRefGoogle Scholar
  6. Deamer D (2017) Conjecture and hypothesis: the importance of reality checks. Beilstein J Org Chem 13:620–624CrossRefPubMedPubMedCentralGoogle Scholar
  7. Filtness MJ, Butler IB, Rickard D (2003) The origin of life: the properties of iron sulphide membranes. Trans Inst Min Metall B 112:171–172Google Scholar
  8. Gilbert W (1986) The RNA world. Nature 319:618CrossRefGoogle Scholar
  9. Herschy B, Whicher A, Camprubi E, Watson C, Dartnell L, Ward J, Evans JRG, Lane N (2014) An origin of life reactor to simulate alkaline hydrothermal vents. J Mol Evol 79:213–227CrossRefPubMedPubMedCentralGoogle Scholar
  10. Jackson JB (2016) Natural pH gradients in hydrothermal alkali vents were unlikely to have played a role in the origin of life. J Mol Evol 83:1–11CrossRefPubMedPubMedCentralGoogle Scholar
  11. Lane N (2014) Bioenergetic constraints on the evolution of complex life. Cold Spring Harb Perspect Biol 6(a801):5982Google Scholar
  12. Lane N (2017) Proton gradients at the origin of life. BioEssays. doi:10.1002/bies.201600217 PubMedGoogle Scholar
  13. Lane N, Martin WF (2012) The origin of membrane bioenergetics. Cell 151:1406–1416CrossRefPubMedGoogle Scholar
  14. Lane N, Allen JF, Martin W (2010) How did LUCA make a living? Chemiosmosis in the origin of life. BioEssays 32:271–280CrossRefPubMedGoogle Scholar
  15. Martin W, Russell MJ (2007) On the origin of biochemistry at an alkaline hydrothermal vent. Philos Trans R Soc Lond B 362:1887–1925CrossRefGoogle Scholar
  16. Mauzerall D, Borowska Z, Zielinski I (1993) Photo and thermal reactions of ferrous hydroxide. Orig Life Evol Biosph 23:105–114CrossRefGoogle Scholar
  17. McCollom TM (2016) Abiotic methane formation during experimental serpentinization of olivine. Proc Natl Acad Sci USA 113:13965–13970CrossRefPubMedPubMedCentralGoogle Scholar
  18. Mielke RE, Robinson KJ, White LM, McGlynn SE, McEachern K, Bhartia R, Kanik I, Russell MJ (2011) Iron-sulfide-bearing chimneys as potential catalytic energy traps at life’s emergence. Astrobiology 11:1–18CrossRefGoogle Scholar
  19. Miller SL (1953) A production of amino acids under possible primitive earth conditions. Science 117:528–529CrossRefPubMedGoogle Scholar
  20. Mitchell P (1966) Chemiosmotic coupling in oxidative and photophosphorylation. Glynn Research, BodminGoogle Scholar
  21. Mitchell P (1968) Chemiosmotic coupling and energy transduction. Glynn Research, BodminGoogle Scholar
  22. Nicholls DG, Ferguson SJ (2013) Bioenergetics, vol 4. Elsevier, AmsterdamGoogle Scholar
  23. Nitschke W, Russell MJ (2009) Hydrothermal focussing of chemical and chemiosmotic energy supported by delivery of catalytic Fe, Ni, Mo/W Co, Se, S forced life to emerge. J Mol Evol 69:481–496CrossRefPubMedGoogle Scholar
  24. Nitschke W, Russell MJ (2010) Just like the universe the emergence of life had high enthalpy and low entropy beginnings. J Mol Cosmol 10:3200–3216Google Scholar
  25. Nitschke W, McGlynn SE, Milner-White EJ, Russell MJ (2013) On the antiquity of metalloenzymes and their substrates in bioenergetics. Biochim Biophys Acta 1827:871–881CrossRefPubMedGoogle Scholar
  26. Orgel LE (2008) The implausibility of metabolic cycles on the prebiotic earth. PLoS Biol 6(1):e18CrossRefPubMedPubMedCentralGoogle Scholar
  27. Powner MW, Gerland B, Sutherland JD (2009) Synthesis of activated pyrimidine ribonucleotides in prebiotically plausible conditions. Nature 459:239–242CrossRefPubMedGoogle Scholar
  28. Reda T, Plugge PM, Abram NJ, Hirst J (2008) Reversible interconversion of carbon dioxide and formate by an electroactive enzyme. Proc Natl Acad Sci USA 105:10654–10658CrossRefPubMedPubMedCentralGoogle Scholar
  29. Roldan A, Hollingsworth N, Roffey A, Islam Y-U, Goodall JBM, Catlow CRA, Darr JA, Bras W, Sankar G, Holt KB, Hogarth G, de Leeuw NH (2015) Bio-inspired CO2 conversion by iron sulfide catalysts under sustainable conditions. Chem Commun 51:7501–7504CrossRefGoogle Scholar
  30. Russell MJ, Nitschke W, Branscomb E (2013) The inevitable journal to being. Philos Trans R Soc 368:20120254CrossRefGoogle Scholar
  31. Russell MJ (2007) The alkaline solution to the emergence of life: energy, entropy and early evolution. Acta Biotheor 55:133–179CrossRefPubMedGoogle Scholar
  32. Russell MJ (2010) Abiogenesis and the origins of life. J Cosmol 10:1008–3417Google Scholar
  33. Russell ML, Hall AJ (1997) The emergence of life from iron monosulphide bubbles at a submarine redox and pH front. J Geol Soc 154:377–402CrossRefGoogle Scholar
  34. Russell MJ, Hall AJ, Turner D (1989) In vitro growth of iron sulphide chimneys: possible culture chambers for origin-of-life experiments. Terra Nova 1:238–241CrossRefGoogle Scholar
  35. Russell MJ, Barge LM, Bhartia R, Bocanegra D, Bracher PJ, Branscomb E, Kidd R, McGlynn S, Meier DH, Nitschke W, Shibuya T, Vance S, White L, Kanik I (2014) The drive to life on wet and icy worlds. Astrobiology 14:308–343CrossRefPubMedPubMedCentralGoogle Scholar
  36. Sojo V, Pomiankowski A, Lane N (2014) A bioenergetics basis for membrane divergence in archaea and bacteria. PLoS Biol 12:e1001926CrossRefPubMedPubMedCentralGoogle Scholar
  37. Sojo V, Herschy B, Whicher A, Camprubi A, Lane N (2016) The origin of life in alkaline hydrothermal vents. Astrobiology 16:181–197CrossRefPubMedGoogle Scholar
  38. Sousa FL, Thiergart T, Landan G, Nelson-Sathi S, Ines ACP, Allen JF, Lane N, Martin W (2013) Early bioenergetic evolution. Philos Trans R Soc Lond B 368:20130088CrossRefGoogle Scholar
  39. Sutherland JD (2016) The origin of life—out of the blue. Angew Chem Int Ed 55:104–121CrossRefGoogle Scholar
  40. Urey HC (1952) The planets: their origin and development. Yale University Press, Newhaven. Chapter 4Google Scholar
  41. Vladimirov MG, Ryzhkov YF, Alekseev VA, Bogdanovskaya VA, Otroshchenko VA, Kritsky MS (2004) Electrochemical reduction of carbon dioxide on pyrite as a pathway for abiogenic formation of organic molecules. Orig Life Evol Biosph 34:347–360CrossRefPubMedGoogle Scholar
  42. Wächtershäuser G (2006) From volcanic origins of chemoautotrophic life to Bacteria, Archaea and Eukarya. Philos Trans R Soc Lond B 361:1787–1808CrossRefGoogle Scholar
  43. Wächtershäuser G (2016) In praise of error. J Mol Evol 82:75–80CrossRefPubMedGoogle Scholar
  44. Yamaguchi A, Yamamoto M, Takai K, Ishii T, Hashimoto K, Nakamura R (2014) Electrochemical CO2 reduction by Ni-containing iron sulphides: how is CO2 electrochemically reduced at bisulfide-bearing deep-sea hydrothermal precipitates? Electrochim Acta 141:311–318CrossRefGoogle Scholar

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© Springer Science+Business Media, LLC 2017

Authors and Affiliations

  1. 1.School of BiosciencesUniversity of BirminghamBirminghamUK

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