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Thioester Synthesis through Geoelectrochemical CO2 Fixation on Ni Sulfides

preprint
revised on 04.06.2020 and posted on 04.06.2020 by Norio Kitadai, Ryuhei Nakamura, Masahiro Yamamoto, Satoshi Okada, Wataru Takahagi, Yuko Nakano, Yoshio Takahashi, Ken Takai, Yoshi Oono
Thioester synthesis by CO dehydrogenase/acetyl-CoA synthase is among the most ancient autotrophic metabolisms. Although the preceding prebiotic CO2 fixation routes to thioesters are often suggested, none has any experimentally supported evidence. Here we demonstrate that, under an electrochemical condition realizable in early ocean hydrothermal systems, nickel sulfide (NiS) gradually reduces to Ni0, while accumulating surface-bound CO due to CO2 electroreduction. The resultant partially reduced NiS facilitates thioester (S-methyl thioacetate) formation from CO and methanethiol even at room temperature and neutral pH. This thioester formation can further be enhanced up to a selectivity of 56% by NiS coprecipitating with FeS or CoS. Considering the central role of Ni in the enzymatic process mentioned above, our demonstrated thioester synthesis with the partially reduced NiS could have a direct implication to the autotrophic origin of life.

Funding

JSPS KAKENHI

the Astrobiology Center Program of NINS

History

Email Address of Submitting Author

nkitadai@jamstec.go.jp

Institution

Japan Agency for Marine-Earth Science and Technology

Country

Japan

ORCID For Submitting Author

0000-0002-8767-4598

Declaration of Conflict of Interest

Authors declare no conflict of interest.

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