dc.contributor.author | Vasiliadou, Rafaela | |
dc.contributor.author | Dimov, Nikolay | |
dc.contributor.author | Szita, Nicolas | |
dc.contributor.author | Jordan, Sean F. | |
dc.contributor.author | Lane, Nick | |
dc.date.accessioned | 2019-12-19T01:07:05Z | |
dc.date.available | 2019-12-19T01:07:05Z | |
dc.date.issued | 2019-10-18 | |
dc.identifier.citation | Vasiliadou , R , Dimov , N , Szita , N , Jordan , S F & Lane , N 2019 , ' Possible mechanisms of CO2 reduction by H2 via prebiotic vectorial electrochemistry ' , Interface Focus , vol. 9 , no. 6 , pp. 1-11 . https://doi.org/10.1098/rsfs.2019.0073 | |
dc.identifier.issn | 2042-8901 | |
dc.identifier.other | PURE: 17332968 | |
dc.identifier.other | PURE UUID: 3c3cb5ff-b23c-4bf5-a4e1-ad915b5686f3 | |
dc.identifier.other | ORCID: /0000-0002-2873-1505/work/66369098 | |
dc.identifier.other | Scopus: 85074580375 | |
dc.identifier.other | PubMed: 31641439 | |
dc.identifier.uri | http://hdl.handle.net/2299/22019 | |
dc.description | © 2019 The Authors.Published by the Royal Society under the terms of the Creative Commons Attribution License http://creativecommons.org/licenses/by/4.0/, which permits unrestricted use, provided the original author and source are credited. | |
dc.description.abstract | Methanogens are putatively ancestral autotrophs that reduce CO 2 with H 2 to form biomass using a membrane-bound, proton-motive Fe(Ni)S protein called the energy-converting hydrogenase (Ech). At the origin of life, geologically sustained H+ gradients across inorganic barriers containing Fe(Ni)S minerals could theoretically have driven CO 2 reduction by H 2 through vectorial chemistry in a similar way to Ech. pH modulation of the redox potentials of H 2, CO 2 and Fe(Ni)S minerals could in principle enable an otherwise endergonic reaction. Here, we analysewhether vectorial electrochemistry can facilitate the reduction of CO 2 by H 2 under alkaline hydrothermal conditions using a microfluidic reactor. We present pilot data showing that steep pH gradients of approximately 5 pH units can be sustained over greater than 5 h across Fe(Ni)S barriers, with H+-flux across the barrier about two million-fold faster than OH-flux. This high flux produces a calculated 3-pH unit-gradient (equating to 180 mV) across single approximately 25-nm Fe(Ni)S nanocrystals, which is close to that required to reduce CO 2. However, the poor solubility of H2 at atmospheric pressure limits CO 2 reduction by H 2, explaining why organic synthesis has so far proved elusive in our reactor. Higher H 2 concentration will be needed in future to facilitate CO 2 reduction through prebiotic vectorial electrochemistry. | en |
dc.format.extent | 11 | |
dc.language.iso | eng | |
dc.relation.ispartof | Interface Focus | |
dc.subject | CO2 reduction, origin of life, Energy-converting hydrogenase, alkaline hydrothermal vents, microfluidic reactor | |
dc.subject | CO reduction | |
dc.subject | Alkaline hydrothermal vents | |
dc.subject | Microfluidic reactor | |
dc.subject | Vectorial chemistry | |
dc.subject | Origin of life | |
dc.subject | Energy-converting hydrogenase | |
dc.subject | Bioengineering | |
dc.subject | Biophysics | |
dc.subject | Biochemistry | |
dc.subject | Biotechnology | |
dc.subject | Biomedical Engineering | |
dc.subject | Biomaterials | |
dc.title | Possible mechanisms of CO2 reduction by H2 via prebiotic vectorial electrochemistry | en |
dc.contributor.institution | School of Physics, Engineering & Computer Science | |
dc.description.status | Peer reviewed | |
dc.identifier.url | http://www.scopus.com/inward/record.url?scp=85074580375&partnerID=8YFLogxK | |
rioxxterms.version | VoR | |
rioxxterms.versionofrecord | https://doi.org/10.1098/rsfs.2019.0073 | |
rioxxterms.type | Journal Article/Review | |
herts.preservation.rarelyaccessed | true | |