8WZR

SFX structure of an Mn-carbonyl complex immobilized in hen egg white lysozyme microcrystals, 100 ns after photoexcitation at RT.

Summary for 8WZR

• Entry DOI: 10.2210/pdb8wzr/pdb
• Descriptor: Lysozyme C, CHLORIDE ION, SODIUM ION, ... (5 entities in total)
• Functional Keywords: hewl, mn-carbonyl comples, photoexcitation, hydrolase
• Biological source: Gallus gallus (chicken)
• Total number of polymer chains: 1
• Total formula weight: 14528.57

Authors

Maity, B.,Shoji, M.,Luo, F.,Nakane, T.,Abe, S.,Owada, S.,Kang, J.,Tono, K.,Tanaka, R.,Thuc, T.T.,Kojima, M.,Hishikawa, Y.,Tanaka, J.,Tian, J.,Noya, H.,Nakasuji, Y.,Asanuma, A.,Yao, X.,Iwata, S.,Shigeta, Y.,Nango, E.,Ueno, T. (deposition date: 2023-11-02, release date: 2024-09-04, Last modification date: 2024-10-23)

Primary citation

Maity, B.,Shoji, M.,Luo, F.,Nakane, T.,Abe, S.,Owada, S.,Kang, J.,Tono, K.,Tanaka, R.,Pham, T.T.,Kojima, M.,Hishikawa, Y.,Tanaka, J.,Tian, J.,Nagama, M.,Suzuki, T.,Noya, H.,Nakasuji, Y.,Asanuma, A.,Yao, X.,Iwata, S.,Shigeta, Y.,Nango, E.,Ueno, T.
Real-time observation of a metal complex-driven reaction intermediate using a porous protein crystal and serial femtosecond crystallography.
Nat Commun, 15:5518-5518, 2024

PubMed Abstract: Determining short-lived intermediate structures in chemical reactions is challenging. Although ultrafast spectroscopic methods can detect the formation of transient intermediates, real-space structures cannot be determined directly from such studies. Time-resolved serial femtosecond crystallography (TR-SFX) has recently proven to be a powerful method for capturing molecular changes in proteins on femtosecond timescales. However, the methodology has been mostly applied to natural proteins/enzymes and limited to reactions promoted by synthetic molecules due to structure determination challenges. This work demonstrates the applicability of TR-SFX for investigations of chemical reaction mechanisms of synthetic metal complexes. We fix a light-induced CO-releasing Mn(CO) reaction center in porous hen egg white lysozyme (HEWL) microcrystals. By controlling light exposure and time, we capture the real-time formation of Mn-carbonyl intermediates during the CO release reaction. The asymmetric protein environment is found to influence the order of CO release. The experimentally-observed reaction path agrees with quantum mechanical calculations. Therefore, our demonstration offers a new approach to visualize atomic-level reactions of small molecules using TR-SFX with real-space structure determination. This advance holds the potential to facilitate design of artificial metalloenzymes with precise mechanisms, empowering design, control and development of innovative reactions.

PubMed: 38951539
DOI: 10.1038/s41467-024-49814-9

Experimental method

X-RAY DIFFRACTION (1.6 Å)