Formaldehyde dehydrogenase SzFaldDH: an indispensable bridge for relaying CO2 bioactivation and conversion†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry Pub Date : 2024-10-22 DOI:10.1039/d4gc03745f

Boxia Guo , Xiuling Ji , Yaju Xue , Yuhong Huang

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Abstract

Formaldehyde dehydrogenases (FaldDHs) are becoming attractive biocatalysts as an indispensable bridge for relaying CO₂ bioactivation and conversion by multi-enzyme cascade reactions (CO₂ → HCOOH → HCHO → C_n) in a green process. This study has discovered four novel FaldDHs using the effective bioinformatics tool Peptide Pattern Recognition (PPR), among which SzFaldDH was shown to have outstanding reducing activity 10-fold greater than the commercial PFaldDH. This new FaldDH achieved the highest catalytic efficiency among all free enzyme systems of CO₂ → HCHO at 0.496 μmol g_enzyme⁻¹ min⁻¹. The outstanding reducing capability was attributed to the enlarged substrate tunnel achieved by residue at the entrance and an extra loop, making it easier for the combination with the substrates. The Quantum Mechanics and Molecular Dynamic calculations revealed the facilitation of hydrogen transfer between formate and NADH as well as protonation of carbonyl oxygen also contributed to the high reducing activity. This discovery provided a novel effective biocatalyst for further promoting the conversion and utilization of CO₂.

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甲醛脱氢酶 SzFaldDH：连接二氧化碳生物活化和转化不可或缺的桥梁†。

甲醛脱氢酶（FaldDHs）作为多酶级联反应（CO2 → HCOOH → HCHO → Cn）中CO2生物活化和转化不可或缺的桥梁，正在成为一种绿色工艺中极具吸引力的生物催化剂。这项研究利用有效的生物信息学工具肽模式识别（PPR）发现了四种新型 FaldDH，其中 SzFaldDH 的还原活性比商用 PFaldDH 高出 10 倍。在所有自由酶系统中，这种新型 FaldDH 对 CO2 → HCHO 的催化效率最高，达到 0.496 μmol genzyme-1 min-1。这种出色的还原能力归功于入口处的残基和额外的环路扩大了底物隧道，使其更容易与底物结合。量子力学和分子动力学计算显示，促进甲酸盐和 NADH 之间的氢转移以及羰基氧的质子化也有助于提高还原活性。这一发现为进一步促进二氧化碳的转化和利用提供了一种新型有效的生物催化剂。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Green Chemistry 化学-化学综合

CiteScore

16.10

自引率

7.10%

发文量

677

审稿时长

1.4 months

期刊介绍： Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.