Synergistic Effects of Silica-Supported Iron-Cobalt Catalysts for CO Reduction to Prebiotic Organics.

To test the ability of geochemical surfaces in serpentinizing hydrothermal systems to catalyze reactions from which metabolism arose, we investigated H-dependent CO reduction toward metabolic intermediates over silica-supported Co-Fe catalysts. Supported catalysts converted CO to various products at 180 °C and 2.0 MPa.

Materials Genes of CO Hydrogenation on Supported Cobalt Catalysts: An Artificial Intelligence Approach Integrating Theoretical and Experimental Data.

Designing materials for catalysis is challenging because the performance is governed by an intricate interplay of various multiscale phenomena, such as the chemical reactions on surfaces and the materials' restructuring during the catalytic process. In the case of supported catalysts, the role of the support material can be also crucial. Here, we address this intricacy challenge by a symbolic-regression artificial intelligence (AI) approach.

Influence of Composition of Nickel-Iron Nanoparticles for Abiotic CO Conversion to Early Prebiotic Organics.

Abiotic synthesis of formate and short hydrocarbons takes place in serpentinizing vents where some members of vent microbial communities live on abiotic formate as their main carbon source. To better understand the catalytic properties of Ni-Fe minerals that naturally exist in hydrothermal vents, we have investigated the ability of synthetic Ni-Fe based nanoparticular solids to catalyze the H -dependent reduction of CO , the first step required for the beginning of pre-biotic chemistry. Mono and bimetallic Ni-Fe nanoparticles with varied Ni-to-Fe ratios transform CO and H into intermediates and products of the acetyl-coenzyme A pathway-formate, acetate, and pyruvate-in mM range under mild hydrothermal conditions.

Ambient temperature CO fixation to pyruvate and subsequently to citramalate over iron and nickel nanoparticles.

The chemical reactions that formed the building blocks of life at origins required catalysts, whereby the nature of those catalysts influenced the type of products that accumulated. Recent investigations have shown that at 100 °C awaruite, a NiFe alloy that naturally occurs in serpentinizing systems, is an efficient catalyst for CO conversion to formate, acetate, and pyruvate. These products are identical with the intermediates and products of the acetyl-CoA pathway, the most ancient CO fixation pathway and the backbone of carbon metabolism in H-dependent autotrophic microbes.

Effects of Silica Modification (Mg, Al, Ca, Ti, and Zr) on Supported Cobalt Catalysts for H-Dependent CO Reduction to Metabolic Intermediates.

Serpentinizing hydrothermal systems generate H as a reductant and harbor catalysts conducive to geochemical CO conversion into reduced carbon compounds that form the core of microbial autotrophic metabolism. This study characterizes mineral catalysts at hydrothermal vents by investigating the interactions between catalytically active cobalt sites and silica-based support materials on H-dependent CO reduction. Heteroatom incorporated (Mg, Al, Ca, Ti, and Zr), ordered mesoporous silicas are applied as model support systems for the cobalt-based catalysts.