Song Youngdong, Budiyanto Eko, Kumar Ashwani, Landrot Gautier, Tüysüz Harun
Department of Heterogeneous Catalysis, Max-Planck-Institut für Kohlenforschung, Kaiser-Wilhelm-Platz 1, 45470, Mülheim an der Ruhr, Germany.
Synchrotron SOLEIL, L'Orme des Merisiers, Départementale 128, Saint-Aubin, 91190, France.
Angew Chem Int Ed Engl. 2025 Jun 2;64(23):e202503747. doi: 10.1002/anie.202503747. Epub 2025 Apr 21.
Submarine hydrothermal vents harbor diverse microbial communities and have long intrigued researchers studying the origin of life. Transition metals in these environments can be reduced by serpentinization, potentially forming zeolite-supported transition metal nanoparticles capable of driving prebiotic chemistry. This inorganic structure could catalyze biochemical reactions, including converting metabolically crucial pyruvate before the emergence of biological processes. This study explores the catalytic interconversion of pyruvate and lactate, mediated by lactate dehydrogenase in biochemical systems, using inorganic zeolite Y-supported Ni nanoparticles (Ni/Y) under mild hydrothermal vent conditions. Our results demonstrate that Ni/Y effectively catalyzes the hydrogenation of pyruvate in an inert environment, facilitated by the in situ generation of H₂ through an autocatalytic reaction between Ni/Y and H₂O. Post-reaction analysis by X-ray absorption spectroscopy (XAS) revealed structural transformations in the catalyst, including the formation of unique nickel oxide and hydroxide species, along with extra-framework aluminum from zeolite dealumination, resulting in a thin amorphous nickel oxide/hydroxide layer. Notably, Ni/Y also enables the oxidative reconversion of lactate to pyruvate under atmospheric conditions-an essential reaction catalyzed by lactate dehydrogenase in biological systems. These findings underscore the potential prebiotic role of Ni/Y, suggesting they may have catalyzed the synthesis of key metabolic intermediates.
海底热液喷口蕴藏着多样的微生物群落,长期以来一直吸引着研究生命起源的科研人员。在这些环境中,过渡金属可通过蛇纹石化作用被还原,有可能形成能够驱动生命起源前化学反应的沸石负载过渡金属纳米颗粒。这种无机结构可以催化生化反应,包括在生物过程出现之前催化代谢关键物质丙酮酸的转化。本研究在温和的热液喷口条件下,利用无机Y型沸石负载镍纳米颗粒(Ni/Y),探索了生化系统中由乳酸脱氢酶介导的丙酮酸和乳酸之间的催化相互转化。我们的结果表明,在惰性环境中,Ni/Y通过与水的自催化反应原位生成氢气,有效地催化了丙酮酸的氢化反应。通过X射线吸收光谱(XAS)进行的反应后分析揭示了催化剂的结构转变,包括形成独特的氧化镍和氢氧化镍物种,以及沸石脱铝产生的骨架外铝,从而形成了一层薄的非晶态氧化镍/氢氧化镍层。值得注意的是,Ni/Y还能在大气条件下使乳酸氧化再转化为丙酮酸,这是生物系统中乳酸脱氢酶催化的一个重要反应。这些发现强调了Ni/Y在生命起源前的潜在作用,表明它们可能催化了关键代谢中间体的合成。