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