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Project A1

Electron-driven protonation dynamics in cytochrome c oxidase

Principal Investigators: Prof. Dr. Joachim Heberle (FU), Prof. Dr. Inez Weidinger (TU)

The A1 project aims at the comprehensive monitoring of electron-driven proton translocations in oxidases (cytochrome c and ubiquinol oxidases) by time-resolved infrared (IR) and resonance Raman spectroscopy. Novel techniques will be developed and applied to initiate and monitor protonation dynamics: Microfluidic flow-flash setup for triggering the reaction by a short laser pulse as well as electrochemical electron injection to solid-supported oxidase in combination with surface-enhanced IR and resonance Raman spectroscopies. By these means, the reaction sequence, the rate-limiting steps and the key residues in CcO will be identified.

Publications

2017-2019

Kielb, P., Utesch, T., Kozuch, J., Jeoung, J.-H., Dobbek, H., Mroginski, M.A., Hildebrandt, P., and Weidinger, I. (2017). Switchable Redox Chemistry of the Hexameric Tyrosine-Coordinated Heme Protein. Journal of Physical Chemistry B 121, 3955-3964.

Kottke, T., Lórenz-Fonfría V.A., and Heberle J. (2017). The Grateful Infrared – Sequential Protein Structural Changes Resolved by IR Difference Spectroscopy. Journal of Physical Chemistry B 121, 335-350. [Link to news section.]

Senger, M., Eichmann, V., Laun, K., Duan, J., Wittkamp, F., Knör, G., Apfel, U.-P., Happe, T., Winkler, M., Heberle, J., Stripp, S. T. (2019). How [FeFe]-Hydrogenase Facilitates Bidirectional Proton Transfer. J. Am. Chem. Soc. 141 (43), 17394-17403; doi.org/10.1021/jacs.9b09225.

Schultz, B.-J., Mohrmann, H., Lórenz-Fonfría, V.A., and Heberle J. (2018). Protein dynamics observed by tunable mid-IR quantum cascade lasers across the time range from 10 ns to 1 s. Spectrochimica Acta A 188, 666-674.

Sezer, M., Woelke, A.-L., Knapp, E.W., Schlesinger, R., Mroginski, M.A., Weidinger, I.M. (2017). Redox induced protonation of heme propionates in cytochrome c oxidase: Insights from surface enhanced resonance Raman spectroscopy and QM/MM calculations. Biochimica et Biophysica Acta (BBA) - Bioenergetics 1858, 103-108.


2013-2016

Ataka, K., Stripp, S.T., and Heberle, J. (2013). Surface-enhanced infrared absorption spectroscopy (SEIRAS) to probe monolayers of membrane proteins. Biochimica et Biophysica Acta (BBA) - Biomembranes 1828, 2283-2293.

Kielb, P., Sezer, M., Katz, S., Lopez, F., Schulz, C., Gorton, L., Ludwig, R., Wollenberger, U., Zebger, I., and Weidinger, I.M. (2015). Spectroscopic Observation of Calcium-Induced Reorientation of Cellobiose Dehydrogenase Immobilized on Electrodes and its Effect on Electrocatalytic Activity. ChemPhysChem 16, 1960-1968.

Kozuch, J., von der Hocht, I., Hilbers, F., Michel, H., and Weidinger, I.M. (2013). Resonance Raman Characterization of the Ammonia-Generated Oxo Intermediate of Cytochrome c Oxidase from Paracoccus denitrificans. Biochemistry 52, 6197-6202.

Ly, H.K., Wrzolek, P., Heidary, N., Gotz, R., Horch, M., Kozuch, J., Schwalbe, M., and Weidinger, I.M. (2015). 2nd coordination sphere controlled electron transfer of iron hangman complexes on electrodes probed by surface enhanced vibrational spectroscopy. Chem. Sci. 6, 6999-7007.

Mohrmann, H., Kube, I., Lórenz-Fonfría, V.A., Engelhard, M., and Heberle, J. (2016). Transient Conformational Changes of Sensory Rhodopsin II Investigated by Vibrational Stark Effect Probes. Journal of Physical Chemistry B 120, 4383-4387.

Sezer, M., Kielb, P., Kuhlmann, U., Mohrmann, H., Schulz, C., Heinrich, D., Schlesinger, R., Heberle, J., and Weidinger, I.M. (2015). Surface Enhanced Resonance Raman Spectroscopy Reveals Potential Induced Redox and Conformational Changes of Cytochrome c Oxidase on Electrodes. Journal of Physical Chemistry B 119, 9586-9591.

Süss, B., Ringleb, F., and Heberle, J. (2016). New ultrarapid-scanning interferometer for FT-IR spectroscopy with microsecond time-resolution. Review of Scientific Instruments 87, 063113.

Weidinger, I.M. (2015). Analysis of structure–function relationships in cytochrome c oxidase and its biomimetic analogs via resonance Raman and surface enhanced resonance Raman spectroscopies. Biochimica et Biophysica Acta (BBA) - Bioenergetics 1847, 119-125.

Woelke, A.L., Galstyan, G., Galstyan, A., Meyer, T., Heberle, J., and Knapp, E.-W. (2013). Exploring the Possible Role of Glu286 in CcO by Electrostatic Energy Computations Combined with Molecular Dynamics. Journal of Physical Chemistry B 117, 12432-12441.