Ambient temperature CO(2) fixation to pyruvate and subsequently to citramalate over iron and nickel nanoparticles.
Ambient temperature CO(2) fixation to pyruvate and subsequently to citramalate over iron and nickel nanoparticles.
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环境温度CO（2）固定在丙酮酸上，然后在铁和镍纳米颗粒上固定到柑橘酸盐。
DOI：
10.1038/s41467-023-36088-w
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发表时间：
2023-02-02
影响因子：
16.6
通讯作者：
Tueysuez, Harun
中科院分区：
文献类型：
--
作者：
Beyazay, Tugce;Belthle, Kendra S.;Fares, Christophe;Preiner, Martina;Moran, Joseph;Martin, William F.;Tueysuez, Harun
生命起源时，形成生命基石的化学反应需要催化剂，而催化剂的性质会影响积累的产物类型。最近的研究表明，在100 °C下，一种天然存在于蛇纹岩系统中的Ni 3Fe合金，是将CO2转化为甲酸盐、乙酸盐和丙酮酸盐的有效催化剂。这些产物与乙酰辅酶A途径的中间体和产物相同，乙酰辅酶A途径是最古老的CO2固定途径，也是H2依赖性自养微生物中碳代谢的骨架。在这里，我们表明，通过硬模板法制备的Ni 3Fe纳米颗粒催化H2和CO2在25 °C和25 bar下转化为甲酸盐、乙酸盐和丙酮酸盐。此外，13 C标记的丙酮酸盐可以在室温下在Ni、Fe和Ni 3Fe纳米颗粒上在1小时内进一步转化为乙酸盐、对丙酮酸盐和柠檬酸盐。这些发现强烈地表明，awaruite可以催化柠檬酸苹果酸的形成，在微生物碳代谢中丙酮酸与乙酰辅酶A缩合的C5产物，从丙酮酸和丙酮酸的形成，从CO2在非常温和的反应条件下，没有有机催化剂。这些结果与热液喷口条件下微生物代谢的自养起源理论吻合得很好。合成的Ni-Fe纳米颗粒已被证明是在较高温度下将CO2固定为甲酸盐、乙酸盐和丙酮酸盐的催化剂。在这里，作者表明这些可以在环境温度下将丙酮酸转化为柠檬酸，这与热液喷口条件下微生物代谢的起源一致。
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 Ni3Fe alloy that naturally occurs in serpentinizing systems, is an efficient catalyst for CO2 conversion to formate, acetate, and pyruvate. These products are identical with the intermediates and products of the acetyl-CoA pathway, the most ancient CO2 fixation pathway and the backbone of carbon metabolism in H2-dependent autotrophic microbes. Here, we show that Ni3Fe nanoparticles prepared via the hard-templating method catalyze the conversion of H2 and CO2 to formate, acetate and pyruvate at 25 °C under 25 bar. Furthermore, the 13C-labeled pyruvate can be further converted to acetate, parapyruvate, and citramalate over Ni, Fe, and Ni3Fe nanoparticles at room temperature within one hour. These findings strongly suggest that awaruite can catalyze both the formation of citramalate, the C5 product of pyruvate condensation with acetyl-CoA in microbial carbon metabolism, from pyruvate and the formation of pyruvate from CO2 at very moderate reaction conditions without organic catalysts. These results align well with theories for an autotrophic origin of microbial metabolism under hydrothermal vent conditions. Synthetic Ni-Fe nanoparticles have been demonstrated as catalysts for CO2 fixation to formate, acetate, and pyruvate at higher temperatures. Here, the authors show these can convert pyruvate to citramalate at the ambient temperature, in line with origin of microbial metabolism under hydrothermal vent conditions.
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影响因子：
3.9
作者：
Dekov, Vesselin
通讯作者：
Dekov, Vesselin
影响因子：
4.9
作者：
Adams, Ralph W.;Holroyd, Chloe M.;Morris, Gareth A.
通讯作者：
Morris, Gareth A.
DOI：
10.1073/pnas.1105715108
发表时间：
2011-08-23
影响因子：
11.1
作者：
Cooper, George;Reed, Chris;Wang, Yi
通讯作者：
Wang, Yi
影响因子：
5
作者：
Cody, GD;Boctor, NZ;Yoder, HS
通讯作者：
Yoder, HS
影响因子：
4.5
作者：
Garibello, C. Felipe;Simonov, Alexandr N.;Hocking, Rosalie K.
通讯作者：
Hocking, Rosalie K.