Materials Synthesis and Catalysis in Microfluidic Devices: Prebiotic Chemistry in Mineral Membranes

Wang, Qingpu; Steinbock, Oliver

doi:10.1002/cctc.201901495

Cited by 32 publications

(31 citation statements)

References 106 publications

(123 reference statements)

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“…S28 and accompanying text in SI Appendix ). Our results show that a system of size similar to our 300-µm-wide reactor would indeed lead to the type of microfluidic confluence of reagents that we have shown here and elsewhere ( 30 , 31 , 42 ). Notably, such an effect is not limited to submarine alkaline vents and will likely occur within porous hydrothermal systems at any location and depth, lending itself to multiple geochemical scenarios for the emergence of life.…”

Section: Discussionsupporting

confidence: 68%

CO ₂ reduction driven by a pH gradient

Hudson

Graaf

Rodin

et al. 2020

Proc. Natl. Acad. Sci. U.S.A.

110

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All life on Earth is built of organic molecules, so the primordial sources of reduced carbon remain a major open question in studies of the origin of life. A variant of the alkaline-hydrothermal-vent theory for life’s emergence suggests that organics could have been produced by the reduction of CO2 via H2 oxidation, facilitated by geologically sustained pH gradients. The process would be an abiotic analog—and proposed evolutionary predecessor—of the Wood–Ljungdahl acetyl-CoA pathway of modern archaea and bacteria. The first energetic bottleneck of the pathway involves the endergonic reduction of CO2 with H2 to formate (HCOO–), which has proven elusive in mild abiotic settings. Here we show the reduction of CO2 with H2 at room temperature under moderate pressures (1.5 bar), driven by microfluidic pH gradients across inorganic Fe(Ni)S precipitates. Isotopic labeling with 13C confirmed formate production. Separately, deuterium (2H) labeling indicated that electron transfer to CO2 does not occur via direct hydrogenation with H2 but instead, freshly deposited Fe(Ni)S precipitates appear to facilitate electron transfer in an electrochemical-cell mechanism with two distinct half-reactions. Decreasing the pH gradient significantly, removing H2, or eliminating the precipitate yielded no detectable product. Our work demonstrates the feasibility of spatially separated yet electrically coupled geochemical reactions as drivers of otherwise endergonic processes. Beyond corroborating the ability of early-Earth alkaline hydrothermal systems to couple carbon reduction to hydrogen oxidation through biologically relevant mechanisms, these results may also be of significance for industrial and environmental applications, where other redox reactions could be facilitated using similarly mild approaches.

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Section: Discussionsupporting

confidence: 68%

CO ₂ reduction driven by a pH gradient

Hudson

Graaf

Rodin

et al. 2020

Proc. Natl. Acad. Sci. U.S.A.

110

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“…It should be noted, however, that these experiments were performed using synthetic devices specifically designed for these experiments. Recent progress in generating inorganic precipitate membranes that resemble those at hydrothermal vents [123] would allow us to explore whether the above findings are applicable to natural geochemical structures.…”

Section: Porous Structures Of Hydrothermal Ventsmentioning

confidence: 99%

Primitive Compartmentalization for the Sustainable Replication of Genetic Molecules

Mizuuchi

Ichihashi

2021

Life

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Sustainable replication and evolution of genetic molecules such as RNA are likely requisites for the emergence of life; however, these processes are easily affected by the appearance of parasitic molecules that replicate by relying on the function of other molecules, while not contributing to their replication. A possible mechanism to repress parasite amplification is compartmentalization that segregates parasitic molecules and limits their access to functional genetic molecules. Although extent cells encapsulate genomes within lipid-based membranes, more primitive materials or simple geological processes could have provided compartmentalization on early Earth. In this review, we summarize the current understanding of the types and roles of primitive compartmentalization regarding sustainable replication of genetic molecules, especially from the perspective of the prevention of parasite replication. In addition, we also describe the ability of several environments to selectively accumulate longer genetic molecules, which could also have helped select functional genetic molecules rather than fast-replicating short parasitic molecules.

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“…Either way, many of the research challenges for the hypothesized role(s) of fougerite—dosed with various trace elements and anions—are similar. Such research addressing the submarine acid v. alkaline milieu calls for the further employment of tried-and-tested microfluidic and nano-crystallographic techniques [ 192 , 201 , 202 , 203 , 204 , 205 , 206 , 207 , 224 , 254 , 296 , 297 , 298 , 299 , 300 , 301 , 302 , 310 , 327 , 328 , 329 , 330 , 331 , 332 , 333 , 334 , 335 , 336 , 337 , 338 ]. We enumerate some possible developments from, expectations of, and tests for, the AVT below:…”

Section: What’s Next For the Avt?mentioning

confidence: 99%

The “Water Problem”(sic), the Illusory Pond and Life’s Submarine Emergence—A Review

Russell

2021

Life

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The assumption that there was a “water problem” at the emergence of life—that the Hadean Ocean was simply too wet and salty for life to have emerged in it—is here subjected to geological and experimental “reality checks”. The “warm little pond” that would take the place of the submarine alkaline vent theory (AVT), as recently extolled in the journal Nature, flies in the face of decades of geological, microbiological and evolutionary research and reasoning. To the present author, the evidence refuting the warm little pond scheme is overwhelming given the facts that (i) the early Earth was a water world, (ii) its all-enveloping ocean was never less than 4 km deep, (iii) there were no figurative “Icelands” or “Hawaiis”, nor even an “Ontong Java” then because (iv) the solidifying magma ocean beneath was still too mushy to support such salient loadings on the oceanic crust. In place of the supposed warm little pond, we offer a well-protected mineral mound precipitated at a submarine alkaline vent as life’s womb: in place of lipid membranes, we suggest peptides; we replace poisonous cyanide with ammonium and hydrazine; instead of deleterious radiation we have the appropriate life-giving redox and pH disequilibria; and in place of messy chemistry we offer the potential for life’s emergence from the simplest of geochemically available molecules and ions focused at a submarine alkaline vent in the Hadean—specifically within the nano-confined flexible and redox active interlayer walls of the mixed-valent double layer oxyhydroxide mineral, fougerite/green rust comprising much of that mound.

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Materials Synthesis and Catalysis in Microfluidic Devices: Prebiotic Chemistry in Mineral Membranes

Cited by 32 publications

References 106 publications

CO ₂ reduction driven by a pH gradient

CO ₂ reduction driven by a pH gradient

Primitive Compartmentalization for the Sustainable Replication of Genetic Molecules

The “Water Problem”(sic), the Illusory Pond and Life’s Submarine Emergence—A Review

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Materials Synthesis and Catalysis in Microfluidic Devices: Prebiotic Chemistry in Mineral Membranes

Cited by 32 publications

References 106 publications

CO 2 reduction driven by a pH gradient

CO 2 reduction driven by a pH gradient

Primitive Compartmentalization for the Sustainable Replication of Genetic Molecules

The “Water Problem”(sic), the Illusory Pond and Life’s Submarine Emergence—A Review

Contact Info

Product

Resources

About

CO ₂ reduction driven by a pH gradient

CO ₂ reduction driven by a pH gradient