Article
Chemistry, Multidisciplinary
Armel F. T. Waffo, Christian Lorent, Sagie Katz, Janna Schoknecht, Oliver Lenz, Ingo Zebger, Giorgio Caserta
Summary: This study used cryogenic infrared and electron paramagnetic resonance spectroscopy to decipher the structural basis of the Ni-a-L intermediates in the regulatory [NiFe]-hydrogenase from Cupriavidus necator, revealing the importance of the protein scaffold in fine-tuning proton and electron dynamics.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Victoria Davis, Nina Heidary, Amandine Guiet, Khoa Hoang Ly, Maximilian Zerball, Claudia Schulz, Norbert Michael, Regine von Klitzing, Peter Hildebrandt, Stefan Frielingsdorf, Oliver Lenz, Ingo Zebger, Anna Fischer
Summary: The oxygen tolerance of membrane-bound [NiFe] hydrogenase (MBH) from Cupriavidus necator makes it an attractive electrocatalyst for hydrogen energy conversion devices. By immobilizing MBH with affinity tags on a tin-rich indium tin oxide (ITOTR) electrode, hydrogen oxidation and an unusually high proton reduction current were observed, suggesting bidirectionality in unidirectional [NiFe] hydrogenases. The favorable enzyme-semiconductor interactions contribute to this behavior.
Article
Chemistry, Multidisciplinary
Rhiannon M. Evans, Stephen E. Beaton, Patricia Rodriguez Macia, Yunjie Pang, Kin Long Wong, Leonie Kertess, William K. Myers, Ragnar Bjornsson, Philip A. Ash, Kylie A. Vincent, Stephen B. Carr, Fraser A. Armstrong
Summary: A variant of hydrogenase-2 from E. coli with a mutated arginine residue at its active site forms a tightly-bound diatomic ligand. This ligand is stabilized by hydrogen bonding and removal only occurs after reduction with H-2 and reduced methyl viologen. The R479K variant shows decreased rates in hydrogen oxidation and evolution compared to the native enzyme. Importance rating: 7/10.
Article
Chemistry, Physical
Manuel Antonio Ruiz-Rodriguez, Christopher D. Cooper, Walter Rocchia, Mose Casalegno, Yossef Lopez de los Santos, Guido Raos
Summary: This study uses computational methods to determine the possible orientations of [NiFe] hydrogenase on a planar electrode and finds that the solution's salinity and pH have significant effects on the orientation.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Multidisciplinary
Ravi Kumar, Matthias Stein
Summary: Recently, it was discovered that the oxygen tolerance of the [NiFe]-hydrogenase from H. thermoluteolus stems from an unusual coordination sphere of the active site nickel atom. In the oxidized state, a terminal cysteine residue is displaced by a bidentate coordinating nearby glutamate, resulting in its occupation of a third bridging position.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Biochemistry & Molecular Biology
Giorgio Caserta, Sven Hartmann, Casey Van Stappen, Chara Karafoulidi-Retsou, Christian Lorent, Stefan Yelin, Matthias Keck, Janna Schoknecht, Ilya Sergueev, Yoshitaka Yoda, Peter Hildebrandt, Christian Limberg, Serena DeBeer, Ingo Zebger, Stefan Frielingsdorf, Oliver Lenz
Summary: In this study, the maturation process of [NiFe]-hydrogenase was investigated using biochemical analysis and various spectroscopic techniques, providing detailed insights into its complex maturation mechanism.
NATURE CHEMICAL BIOLOGY
(2023)
Article
Chemistry, Physical
Yuanming Wang, Zepeng Kang, Lingling Zhang, Zhiguang Zhu
Summary: This study investigates the interactions between PfSHI and carbon nanotubes, revealing that electrostatic and hydrophobic interactions play a crucial role in the interaction between PfSHI and electrodes. Based on these findings, a high-performance biofuel cell was constructed, demonstrating an improved power output.
Article
Chemistry, Physical
Monica L. K. Sanchez, Seth Wiley, Edward Reijerse, Wolfgang Lubitz, James A. Birrell, R. Brian Dyer
Summary: The FeFe hydrogenases are efficient catalysts for hydrogen conversion, with a unique active site containing a [4Fe-4S] electron relay and a diiron cluster ligated by CO, CN-, and ADT ligands. The study using TRIR spectroscopy on the CrHydA1 hydrogenase revealed that a modification with PDT ligand inhibits the enzyme from proceeding through the catalytic cycle. The results suggest that the first electron transfer step is pH-independent, supporting a simple electron transfer mechanism rather than a proton-coupled event.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Microbiology
Pier Francesco Di Leonardo, Giacomo Antonicelli, Valeria Agostino, Angela Re
Summary: Understanding the organizational and functional properties of hydrogen metabolism is crucial for creating a framework to support a hydrogen-fueled low-carbon economy. This study investigated the genomes of several industrially relevant acetogens and identified their hydrogenases' repertoire. The findings provide valuable knowledge on the functional specificity and potential applications of hydrogenases in biotechnological processes.
MICROBIOLOGY SPECTRUM
(2022)
Article
Chemistry, Multidisciplinary
Andrea Schmidt, Jacqueline Kalms, Christian Teutloff, Sagie Katz, Stefan Frielingsdorf, Rhiannon M. Evans, Johannes Fritsch, Elisabeth Siebert, Christian Teutloff, Fraser A. Armstrong, Ingo Zebger, Oliver Lenz, Patrick Scheerer
Summary: The membrane-bound [NiFe]-hydrogenase of Cupriavidus necator is an O-2-tolerant hydrogenase with a unique Cys(6)[4Fe-3S] cluster. Replacing two additional cysteines in the cluster led to structural changes and decreased O-2 tolerance. Formation of a hydroxy ligand in the active site under electron-deficient conditions can protect the enzyme from O-2 binding.
Article
Chemistry, Multidisciplinary
Cejun Hu, Yanfang Hu, Chenghao Fan, Ling Yang, Yutong Zhang, Haixia Li, Wei Xie
Summary: In this study, label-free surface-enhanced Raman spectroscopy was used to monitor the oxygen evolution reaction process on Ni3FeOx nanoparticles, revealing that Fe atoms are responsible for the initial OH- to O-O- oxidation, and the O-O- species undergo further oxidation between neighboring Fe and Ni sites.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Roman Rohac, Lydie Martin, Liang Liu, Debashis Basu, Lizhi Tao, R. David Britt, Thomas B. Rauchfuss, Yvain Nicolet
Summary: FeFe-hydrogenases use a unique H cluster to convert H-2 into protons and low-potential electrons. The [2Fe](H) center is where the reaction occurs and is built stepwise by maturating enzymes, with HydE performing complex modifications of complex-B to produce a precursor to the [2Fe](H) center.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Inorganic & Nuclear
Debashis Basu, Danielle L. Gray, Toby J. Woods, Thomas B. Rauchfuss, Federica Arrigoni, Giuseppe Zampella
Summary: In the field of bioorganometallic chemistry, progress has been made in studying mimics of the active sites of [NiFe]-hydrogenases, with challenges arising in the conversion and misassignment when using Ni(N2S2) derivatives.
Article
Chemistry, Multidisciplinary
Lei Zhao, Junhui Yan, Haojie Huang, Xing Du, Hui Chen, Xuan He, Weixin Li, Wei Fang, Daheng Wang, Xianghui Zeng, Jichen Dong, Yunqi Liu
Summary: Recently, conductive metal-organic frameworks (c-MOFs) have gained significant attention for their excellent conductivity and highly accessible active sites in the application of oxygen evolution reaction (OER). This study reports a method to prepare bimetallic c-MOFs with optimal electronic structures and adsorption capacity to intermediates by adjusting the ratio of Ni/Fe. The Ni0.5Fe0.5-THQ catalyst exhibits superior catalytic performances for OER, surpassing commercial RuO2, traditional MOFs, and even some monometallic conductive MOFs.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Haruhiko Teramoto, Tetsu Shimizu, Masako Suda, Masayuki Inui
Summary: This study explored the genetic engineering of Escherichia coli for hydrogen production. The introduction of exogenous hydrogenase and inactivation of endogenous hydrogenases resulted in both hydrogen production and uptake. Disabling the pathways for ethanol, lactate, and succinate production significantly increased hydrogen production. Unexpectedly, high expression of exogenous hydrogenase completely repressed hydrogen production, and the introduction of heterologous enzyme repressed the endogenous hydrogen production ability.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Biochemistry & Molecular Biology
S. Wilkening, F. -J. Schmitt, O. Lenz, I. Zebger, M. Horch, T. Friedrich
BIOCHIMICA ET BIOPHYSICA ACTA-BIOENERGETICS
(2019)
Article
Chemistry, Multidisciplinary
Anne-Christine Schulz, Stefan Frielingsdorf, Phillip Pommerening, Lars Lauterbach, Giovanni Bistoni, Frank Neese, Martin Oestreich, Oliver Lenz
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Multidisciplinary Sciences
J. S. Rowbotham, M. A. Ramirez, O. Lenz, H. A. Reeve, K. A. Vincent
NATURE COMMUNICATIONS
(2020)
Article
Microbiology
Sven Hartmann, Stefan Frielingsdorf, Giorgio Caserta, Oliver Lenz
Editorial Material
Energy & Fuels
Oliver Lenz
Article
Chemistry, Physical
Janina Preissler, Holly A. Reeve, Tianze Zhu, Jake Nicholson, Kouji Urata, Lars Lauterbach, Luet L. Wong, Kylie A. Vincent, Oliver Lenz
Review
Biochemistry & Molecular Biology
Qin Fan, Peter Neubauer, Oliver Lenz, Matthias Gimpel
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2020)
Article
Multidisciplinary Sciences
Nico J. Claassens, Giovanni Scarinci, Axel Fischer, Avi I. Flamholz, William Newell, Stefan Frielingsdorf, Oliver Lenz, Arren Bar-Even
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2020)
Article
Chemistry, Physical
Giorgio Caserta, Christian Lorent, Vladimir Pelmenschikov, Janna Schoknecht, Yoshitaka Yoda, Peter Hildebrandt, Stephen P. Cramer, Ingo Zebger, Oliver Lenz
Article
Electrochemistry
Tomos G. A. A. Harris, Nina Heidary, Stefan Frielingsdorf, Sander Rauwerdink, Abbes Tahraoui, Oliver Lenz, Ingo Zebger, Anna Fischer
Summary: This work demonstrates the control and optimization of biocompatible interfaces on transparent conducting oxide indium tin oxide (ITO) using diazonium electrografting to achieve low charge transfer resistance and efficient electron transfer to immobilized enzymes. Radical scavenger enables interface thickness control, maximizing direct electron transfer processes. Electrografting is proposed as an alternative approach for the functional immobilization of redox-active enzymes on TCO electrodes.
Article
Chemistry, Multidisciplinary
Christian Lorent, Vladimir Pelmenschikov, Stefan Frielingsdorf, Janna Schoknecht, Giorgio Caserta, Yoshitaka Yoda, Hongxin Wang, Kenji Tamasaku, Oliver Lenz, Stephen P. Cramer, Marius Horch, Lars Lauterbach, Ingo Zebger
Summary: A new experimental setup was developed to study metalloenzymes in detail, allowing the controlled preparation and characterization of catalytic intermediates using various spectroscopic techniques. By investigating two O-2-tolerant [NiFe]-hydrogenases as model systems, detailed insights into the catalytic mechanisms and vibrational fingerprints were revealed. Additionally, the study highlighted the importance of complementing X-ray crystallographic data with spectroscopic analyses.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Microbiology
Qin Fan, Giorgio Caserta, Christian Lorent, Oliver Lenz, Peter Neubauer, Matthias Gimpel
Summary: Hydrogenases are important metalloenzymes that have witnessed significant progress in recent years, albeit with difficulties in low production yields. By heterologously expressing the hydrogenase RH, its yield was substantially increased and single subunits were successfully overproduced, offering a new strategy for bioprocess development and structural studies.
Article
Chemistry, Multidisciplinary
Armel F. T. Waffo, Christian Lorent, Sagie Katz, Janna Schoknecht, Oliver Lenz, Ingo Zebger, Giorgio Caserta
Summary: This study used cryogenic infrared and electron paramagnetic resonance spectroscopy to decipher the structural basis of the Ni-a-L intermediates in the regulatory [NiFe]-hydrogenase from Cupriavidus necator, revealing the importance of the protein scaffold in fine-tuning proton and electron dynamics.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Holly A. Reeve, Jake Nicholson, Farieha Altaf, Thomas H. Lonsdale, Janina Preissler, Lars Lauterbach, Oliver Lenz, Silke Leimkuehler, Frank Hollmann, Caroline E. Paul, Kylie A. Vincent
Summary: We present a recycling system utilizing a soluble hydrogenase for synthetic nicotinamide cofactor analogues. With the coupling of an ene reductase, we achieved quantitative conversion of N-ethylmaleimide to N-ethylsuccinimide. The biocatalyst system retained over 50% activity after 7 hours.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Marius Horch, Janna Schoknecht, Solomon L. D. Wrathall, Gregory M. Greetham, Oliver Lenz, Neil T. Hunt