Department of Heterogeneous Catalysis, Max-Planck-Institut für Kohlenforschung, Kaiser-Wilhelm-Platz 1, 45470, Mülheim an der Ruhr, Germany.
Institute of Molecular Evolution, University of Düsseldorf, 40225, Düsseldorf, Germany.
Angew Chem Int Ed Engl. 2023 May 22;62(22):e202218189. doi: 10.1002/anie.202218189. Epub 2023 Apr 19.
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. Furthermore, Ni-Fe catalysts converted CO to similar products without molecular H by using water as a hydrogen source. Both CO chemisorption analysis and post-reaction characterization of materials indicate that Ni and Fe metals play complementary roles for CO fixation.
在蛇纹石化喷口处发生非生物合成的甲酸盐和短链烃，其中一些喷口微生物群落的成员以非生物合成的甲酸盐作为主要碳源。为了更好地了解自然存在于热液喷口的 Ni-Fe 矿物的催化特性，我们研究了合成的 Ni-Fe 基纳米颗粒固体催化 H 依赖性还原 CO 的能力，这是前生物化学开始所需的第一步。具有不同 Ni 与 Fe 比例的单金属和双金属 Ni-Fe 纳米颗粒在温和的水热条件下将 CO 和 H 转化为乙酰辅酶 A 途径的中间体和产物-甲酸盐、乙酸盐和丙酮酸-在 mM 范围内。此外，Ni-Fe 催化剂通过使用水作为氢源，在没有分子 H 的情况下将 CO 转化为类似的产物。CO 化学吸附分析和反应后材料表征均表明，Ni 和 Fe 金属在 CO 固定中起互补作用。
