Prebiotic Interconversion of Pyruvate and Lactate over Zeolite-Supported Ni Catalyst

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-03-28 DOI:10.1002/anie.202503747
Dr. Youngdong Song, Dr. Eko Budiyanto, Dr. Ashwani Kumar, Dr. Gautier Landrot, Prof. Dr. habil. Harun Tüysüz
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Abstract

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.

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丙酮酸和乳酸在沸石负载镍催化剂上的益生元相互转化
海底热液喷口孕育着多种微生物群落,长期以来一直吸引着研究生命起源的研究人员。在这些环境中,过渡金属可以通过蛇纹石化而减少,可能形成沸石支撑的过渡金属纳米颗粒,能够驱动益生元化学。这种无机结构可以催化生物化学反应,包括在生物过程出现之前转化代谢至关重要的丙酮酸。本研究探讨了在温和热液喷口条件下,利用无机沸石Y-负载Ni纳米颗粒(Ni/Y)在生化系统中乳酸脱氢酶介导的丙酮酸和乳酸的催化相互转化。我们的研究结果表明,Ni/Y在惰性环境中有效地催化丙酮酸的加氢,通过Ni/Y和H₂O之间的自催化反应原位生成H₂。反应后的x射线吸收光谱分析揭示了催化剂的结构变化,包括独特的氧化镍和氢氧化物的形成,以及沸石脱铝产生的框架外铝,导致薄的无定形氧化镍/氢氧化物层。值得注意的是,Ni/Y还可以使乳酸盐在大气条件下氧化再转化为丙酮酸盐,这是生物系统中由乳酸脱氢酶催化的重要反应。这些发现强调了Ni/Y的潜在益生元作用,表明它们可能催化了关键代谢中间体的合成。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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