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Angew. Chem.-Int. Edit., Jun 04 2025, | https://doi.org/10.1002/anie.202508565
Fortification of FeS Clusters Reshapes Anaerobic CO Dehydrogenase into an Air-Viable Enzyme Through Multilayered Sealing of O2 Tunnels
Suk Min Kim+,*1 So Yeon Kong+2, Jingu Kang+3, Jeong Seok Ji2, Sung Heuck Kang3, Hye-Jin Yoon2, Hyunwoo Kim3, Jungki Ryu3, Hyung Ho Lee,*2 and Yong Hwan Kim*3,4
1Department of Biotechnology, The Catholic University of Korea, Bucheon, 14662, Republic of Korea.
2Department of Chemistry, College of Natural Sciences, Seoul National University, Seoul, 08826, Republic of Korea.
3School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 44919, Republic of Korea.
4Graduate School of Carbon Neutrality, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 44919, Republic of Korea.
+These authors contributed equally to this work.
Corresponding Authors: Prof. Dr. Suk Min Kim, Prof. Dr. Hyung Ho Lee, Prof. Dr. Yong Hwan Kim
1Department of Biotechnology, The Catholic University of Korea, Bucheon, 14662, Republic of Korea.
2Department of Chemistry, College of Natural Sciences, Seoul National University, Seoul, 08826, Republic of Korea.
3School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 44919, Republic of Korea.
4Graduate School of Carbon Neutrality, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 44919, Republic of Korea.
+These authors contributed equally to this work.
Corresponding Authors: Prof. Dr. Suk Min Kim, Prof. Dr. Hyung Ho Lee, Prof. Dr. Yong Hwan Kim
Abstract
The inherent O2 sensitivity of Ni─Fe carbon monoxide dehydrogenases (CODHs), crucial for rapid CO to CO2 interconversion, presents substantial challenges for industrial application. Transforming CO/CO2, a prevalent anthropogenic air pollutant, into valuable carbon chemicals either directly or through intermediate steps via biocatalytic methods offers a promising pathway to achieve net-zero emissions across industries and the environment. However, completely eliminating oxygen from industrial biotransformations, especially under ambient conditions, is exceedingly onerous. Here, we engineered variants of the CODH2 from Carboxydothermus hydrogenoformans (ChCODH2) with dual blocking at both the O2 entrance and near the active site, effectively sealing the tunnel against atmospheric O2 levels (20%). The O2-tunnel engineered A559W/V610H variant demonstrated a marked improvement in air stability, with a half-life of 24.6 h compared to the wild type's 2.4 h. Crystallographic snapshots of this air-viable variant after 24 h of exposure revealed the robust integrity of the fortified FeS and NiFeS clusters. Additionally, electro-enzymatic reactions corroborated its CO/CO2 conversion capability even in ubiquitous air. These findings, which address the O2 sensitivity of anaerobic enzymes caused by O2-induced metal cluster collapse, enhance their potential for biological CO/CO2 transformations in O2-rich environments, thereby broadening their industrial viability and applicability.
논문정보
- Research article
- 2025년 06월 (BRIC 등록일 2025-06-16)
- 국내 연구진
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