Short-lived intermediate in N 2 O generation by P450 NO reductase captured by time-resolved IR spectroscopy and XFEL crystallography

Takashi Nomura 1, 2
Tetsunari Kimura 2, 3
Yusuke Kanematsu 4
Daichi Yamada 1
Keitaro Yamashita 2
Kunio Hirata 2
Go Ueno 2
Hironori Murakami 5
Tamao Hisano 2
Raika Yamagiwa 1, 2
Hanae Takeda 1, 2
Chai Gopalasingam 1, 2
Ryota Kousaka 1
Sachiko Yanagisawa 1
Osami Shoji 6, 7
Takashi KUMASAKA 5
MASAKI YAMAMOTO 2
Yu Takano 4
Hiroshi Sugimoto 2, 7
Takehiko Tosha 2
Minoru Kubo 1, 7
Yoshitsugu Shiro 1
Publication typeJournal Article
Publication date2021-05-17
scimago Q1
wos Q1
SJR3.414
CiteScore16.5
Impact factor9.1
ISSN00278424, 10916490
Multidisciplinary
Abstract
Significance

The short-lived intermediate formed during the reduction of nitric oxide (NO) to nitrous oxide (N 2 O) in denitrification, microbial anaerobic respiration, is a key state for understanding the generation mechanism of N 2 O, known not only as a greenhouse gas but also as an ozone-depleting substance on the global level. This paper combined state-of-the-art, time-resolved techniques, such as flow-flash infrared spectroscopy and X-ray free electron laser-based crystallography, and captured the intermediate of a P450-type NO reductase at the atomic and electronic levels. The intermediate was identified as a singly protonated Fe 3+ –NHO •− radical, offering insights into a radical–radical coupling mechanism for the N–N bond formation in N 2 O generation.

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GOST Copy
Nomura T. et al. Short-lived intermediate in N 2 O generation by P450 NO reductase captured by time-resolved IR spectroscopy and XFEL crystallography // Proceedings of the National Academy of Sciences of the United States of America. 2021. Vol. 118. No. 21.
GOST all authors (up to 50) Copy
Nomura T., Kimura T., Kanematsu Y., Yamada D., Yamashita K., Hirata K., Ueno G., Murakami H., Hisano T., Yamagiwa R., Takeda H., Gopalasingam C., Kousaka R., Yanagisawa S., Shoji O., KUMASAKA T., YAMAMOTO M., Takano Yu., Sugimoto H., Tosha T., Kubo M., Shiro Y. Short-lived intermediate in N 2 O generation by P450 NO reductase captured by time-resolved IR spectroscopy and XFEL crystallography // Proceedings of the National Academy of Sciences of the United States of America. 2021. Vol. 118. No. 21.
RIS |
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RIS Copy
TY - JOUR
DO - 10.1073/pnas.2101481118
UR - https://doi.org/10.1073/pnas.2101481118
TI - Short-lived intermediate in N 2 O generation by P450 NO reductase captured by time-resolved IR spectroscopy and XFEL crystallography
T2 - Proceedings of the National Academy of Sciences of the United States of America
AU - Nomura, Takashi
AU - Kimura, Tetsunari
AU - Kanematsu, Yusuke
AU - Yamada, Daichi
AU - Yamashita, Keitaro
AU - Hirata, Kunio
AU - Ueno, Go
AU - Murakami, Hironori
AU - Hisano, Tamao
AU - Yamagiwa, Raika
AU - Takeda, Hanae
AU - Gopalasingam, Chai
AU - Kousaka, Ryota
AU - Yanagisawa, Sachiko
AU - Shoji, Osami
AU - KUMASAKA, Takashi
AU - YAMAMOTO, MASAKI
AU - Takano, Yu
AU - Sugimoto, Hiroshi
AU - Tosha, Takehiko
AU - Kubo, Minoru
AU - Shiro, Yoshitsugu
PY - 2021
DA - 2021/05/17
PB - Proceedings of the National Academy of Sciences (PNAS)
IS - 21
VL - 118
PMID - 34001620
SN - 0027-8424
SN - 1091-6490
ER -
BibTex
Cite this
BibTex (up to 50 authors) Copy
@article{2021_Nomura,
author = {Takashi Nomura and Tetsunari Kimura and Yusuke Kanematsu and Daichi Yamada and Keitaro Yamashita and Kunio Hirata and Go Ueno and Hironori Murakami and Tamao Hisano and Raika Yamagiwa and Hanae Takeda and Chai Gopalasingam and Ryota Kousaka and Sachiko Yanagisawa and Osami Shoji and Takashi KUMASAKA and MASAKI YAMAMOTO and Yu Takano and Hiroshi Sugimoto and Takehiko Tosha and Minoru Kubo and Yoshitsugu Shiro},
title = {Short-lived intermediate in N 2 O generation by P450 NO reductase captured by time-resolved IR spectroscopy and XFEL crystallography},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
year = {2021},
volume = {118},
publisher = {Proceedings of the National Academy of Sciences (PNAS)},
month = {may},
url = {https://doi.org/10.1073/pnas.2101481118},
number = {21},
doi = {10.1073/pnas.2101481118}
}