한빛사논문
- 조회499
Suk Min Kim 1,4,5,*, Sung Heuck Kang 1,4, Jinhee Lee 1,4, Yoonyoung Heo 2,4, Eleni G. Poloniataki 1, Jingu Kang 1, Hye-Jin Yoon 2, So Yeon Kong 2, Yaejin Yun 2, Hyunwoo Kim 1, Jungki Ryu 1, Hyung Ho Lee 2,5,* & Yong Hwan Kim 1,3,5,*
1School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulsan 44919, Republic of Korea.
2Department of Chemistry, College of Natural Sciences, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 08826, Republic of Korea.
3Graduate School of Carbon Neutrality, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulsan 44919, Republic of Korea.
4These authors contributed equally: Suk Min Kim, Sung Heuck Kang, Jinhee Lee, Yoonyoung Heo.
5These authors jointly supervised this work: Suk Min Kim, Hyung Ho Lee, Yong Hwan Kim.
*Corresponding authors: correspondence to Suk Min Kim, Hyung Ho Lee or Yong Hwan Kim
Abstract
Fe‒S cluster-harboring enzymes, such as carbon monoxide dehydrogenases (CODH), employ sophisticated artificial electron mediators like viologens to serve as potent biocatalysts capable of cleaning-up industrial off-gases at stunning reaction rates. Unraveling the interplay between these enzymes and their associated mediators is essential for improving the efficiency of CODHs. Here we show the electron mediator-interaction site on ChCODHs (Ch, Carboxydothermus hydrogenoformans) using a systematic approach that leverages the viologen-reactive characteristics of superficial aromatic residues. By enhancing mediator-interaction (R57G/N59L) near the D-cluster, the strategically tailored variants exhibit a ten-fold increase in ethyl viologen affinity relative to the wild-type without sacrificing the turn-over rate (kcat). Viologen-complexed structures reveal the pivotal positions of surface phenylalanine residues, serving as external conduits for the D-cluster to/from viologen. One variant (R57G/N59L/A559W) can treat a broad spectrum of waste gases (from steel-process and plastic-gasification) containing O2. Decoding mediator interactions will facilitate the development of industrially high-efficient biocatalysts encompassing gas-utilizing enzymes.
논문정보
- Research article
- 2024년 03월 (BRIC 등록일 2024-03-29)
- 국내 연구진
- 생명과학 > 생물공학
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