Article
Biochemistry & Molecular Biology
Kady M. Oakley, Ryan L. Lehane, Ziyi Zhao, Eunsuk Kim
Summary: In this study, a biomimetic [4Fe-4S] complex was reported to react with oxygen in the presence of thiolate and convert to a [2Fe-2S] analogue. The cluster conversion could also be achieved by using disulfide as an oxidant. Oxygen was found to facilitate the [4Fe-4S] to [2Fe-2S] cluster conversion at a faster rate than disulfide, although disulfide reaction produced higher yields of the [2Fe-2S] analogue.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2022)
Article
Multidisciplinary Sciences
Jiashen Zhou, Lin Zhang, Liping Zeng, Lu Yu, Yuanyuan Duan, Siqi Shen, Jingyan Hu, Pan Zhang, Wenyan Song, Xiaoxue Ruan, Jing Jiang, Yinan Zhang, Lu Zhou, Jia Jia, Xudong Hang, Changlin Tian, Houwen Lin, Hong-Zhuan Chen, John E. Cronan, Hongkai Bi, Liang Zhang
Summary: The study presents the crystal structures of the essential UFA biosynthesis enzyme FabX in Helicobacter pylori, revealing a unique [4Fe-4S] cluster that potentiates FMN oxidation during dehydrogenase catalysis. This [4Fe-4S] cluster is crucial for unsaturated fatty acid synthesis and contributes to the pathogenic function of H. pylori in the corrosion of gastric mucosa.
NATURE COMMUNICATIONS
(2021)
Article
Biochemistry & Molecular Biology
Nisha He, Jingjing Zhou, Ornella Bimai, Jonathan Oltmanns, Jean-Luc Ravanat, Christophe Velours, Volker Schuenemann, Marc Fontecave, Beatrice Golinelli-Pimpaneau
Summary: This study identified the TtuI enzymes involved in the sulfuration of bacterial and archaeal tRNAs and proposed a mechanism involving the transfer of sulfur atoms through the assembly of a [4Fe-4S] cluster coordinated by the CXXC + C motif.
NUCLEIC ACIDS RESEARCH
(2022)
Article
Chemistry, Multidisciplinary
Giovanni Saudino, Simone Ciofi-Baffoni, Lucia Banci
Summary: In this study, it was discovered that NFU1 and ISCA1 in the mitochondrial iron-sulfur cluster assembly machinery play a crucial role in the insertion of a [4Fe-4S] cluster into LIAS by forming a heterodimeric complex. The C-domain of NFU1 drives the cluster to its final destination by exploiting a protein interaction affinity gradient.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Patricia R. Feliciano, Kate S. Carroll, Catherine L. Drennan
Summary: Tuberculosis is the deadliest infectious disease in the world. APS reductase plays a vital role in producing essential reduced-sulfur-containing metabolites in Mycobacterium tuberculosis, making it a potential target for therapeutic interventions. The crystal structure of MtbAPSR provides important information for structure-based drug design aimed at combating TB.
Article
Biology
Jonathan Fuchs, Rapolas Jamontas, Maren Hellen Hoock, Jonathan Oltmanns, Beatrice Golinelli-Pimpaneau, Volker Schuenemann, Antonio J. Pierik, Rolandas Meskys, Agota Aucynaite, Matthias Boll
Summary: This study reveals a new enzyme called TudS desulfidase in cells, which can desulfurize thiouracil and play a crucial role in recycling and detoxification of tRNA-derived 4-thiouridine monophosphate nucleosides for RNA synthesis.
COMMUNICATIONS BIOLOGY
(2023)
Article
Multidisciplinary Sciences
Ornella Bimai, Pierre Legrand, Jean-Luc Ravanat, Nadia Touati, Jingjing Zhou, Nisha He, Marine Lenon, Frederic Barras, Marc Fontecave, Beatrice Golinelli-Pimpaneau
Summary: Thiolation of uridine 34 in tRNAs is conserved in all three domains of life and is essential for accurate protein translation. The mechanism of U34-tRNA thiolation involves a [4Fe-4S] cluster, which is coordinated by conserved cysteine residues. The enzyme NcsA in archaea and the Ctu1/Ctu2 complex in eukaryotes play a crucial role in catalyzing U34-tRNA thiolation. The crystal structure of NcsA from Methanococcus maripaludis reveals the coordination of the [4Fe-4S] cluster and provides insights into the binding and activation of the sulfur donor.
SCIENTIFIC REPORTS
(2023)
Article
Biochemistry & Molecular Biology
Masato Ishizaka, Minghao Chen, Shun Narai, Yoshikazu Tanaka, Toyoyuki Ose, Masaki Horitani, Min Yao
Summary: Iron-sulfur (Fe-S) clusters play a vital role in enzyme activity. This study focuses on the relationship between the Fe-S cluster type and the catalytic activity of a tRNA-thiolation enzyme (TtuA). The researchers observed that [3Fe-4S]-TtuA spontaneously transforms into [4Fe-4S]-TtuA within minutes to an hour, and [3Fe-4S]-TtuA is highly inactive and unstable. These findings provide insights into the Fe-S cluster type used by the tRNA-thiolation enzyme.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Chemistry, Physical
Xuan Zhang, Zikuan Wang, Zhen Li, Sason Shaik, Binju Wang
Summary: This study reveals that the proximal [4Fe-4S] cluster in the reductive dehalogenase PceA can facilitate a proton-coupled electron transfer process to quench the substrate radical. The participation of [4Fe-4S] in mediating a PCET process in RDases is unexpected, although it is well known in reducing Co(II). The Arg305 residue acts as an efficient proton donor for the PCET reactions in RDases.
Review
Biochemistry & Molecular Biology
Francesca Camponeschi, Simone Ciofi-Baffoni, Vito Calderone, Lucia Banci
Summary: The review provides a structural and molecular overview of rare diseases associated with the genes encoding for the accessory proteins of the ISC machinery. It describes the impact of disease-related missense mutations on the specific activity/function of these accessory proteins in the biogenesis of mitochondrial [4Fe-4S] proteins.
Article
Biochemistry & Molecular Biology
Isabelle Fix, Lorenz Heidinger, Thorsten Friedrich, Gunhild Layer
Summary: In archaea and sulfate-reducing bacteria, heme is synthesized via the siroheme-dependent pathway. The Radical SAM enzyme AhbD catalyzes the last step of this pathway, converting iron-coproporphyrin III into heme. Amino acid sequence analysis and structural modeling suggested that some AhbD proteins may contain two auxiliary iron-sulfur clusters. Study on AhbD from Methanosarcina barkeri confirmed the presence of two auxiliary [4Fe-4S] clusters, and the clusters likely participate in the heme synthase activity.
Article
Biochemistry & Molecular Biology
Dafne Suraci, Giovanni Saudino, Veronica Nasta, Simone Ciofi-Baffoni, Lucia Banci
Summary: The study reveals the coordinated mechanism of ISCA1, ISCA2, and NFU1 in the maturation process of mitochondrial [4Fe-4S] proteins. ISCA1 plays a key role in promoting the interaction between NFU1 and ISCA2, leading to the formation of a transient ISCA1-ISCA2-NFU1 ternary complex. This mechanism ensures the safe transfer of [4Fe-4S] clusters from the assembly site on the ISCA1-ISCA2 complex to NFU1, making them available for mitochondrial apo proteins that require NFU1.
JOURNAL OF MOLECULAR BIOLOGY
(2021)
Article
Chemistry, Physical
Wenjin Li, Yanxin Gao, Xuan Sun, Lei Wan, Haishuo Ji, Hang Luo, Yao Tian, Hao Song, Geng Wu, Liyun Zhang
Summary: In this study, the adsorption characteristics and catalytic properties of formate dehydrogenase from Clostridium ljungdahlii (ClFDH) on electrodes were investigated. The electrochemical signals observed on the electrodes were attributed to the reduction and oxidation potential of the [4Fe-4S](2+/+) cluster. Upon adding substrates, the signals transformed into a specific redox center that catalytically engages in electron transport and promotes the rapid and efficient reversible interconversion between CO2 and formate. The results provide valuable insights into the understanding of the catalytic mechanism of FDH and the design of synthetic catalysts.
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
Biochemistry & Molecular Biology
Takashi Fujishiro, Miho Ooi, Kyosei Takaoka
Summary: The study revealed that the structure of class II HCP differs from other HCP classes, with a [4Fe-4S] cluster similar to class I HCPs. The protrusion of the Cys-rich region in class II HCP serves as a binding site for HCR, suggesting its importance in maturation of HCP and orienting HCR for electron transfer in the HCP-HCR complex.
Article
Biotechnology & Applied Microbiology
Shams T. A. Islam, Jie Zhang, Fabio Tonin, Renske Hinderks, Yanthi N. Deurloo, Vlada B. Urlacher, Peter-Leon Hagedoorn
Summary: Lignin valorization through laccase catalysis can release aromatic products, but different enzymes exhibit significant variations in conversion efficiency and rate. Trametes versicolor laccase follows Michaelis-Menten kinetics in converting Kraft lignin, with specific thermodynamic and kinetic parameters, making it a promising tool for guiding enzymatic lignin valorization strategies.
BIOTECHNOLOGY AND BIOENGINEERING
(2022)
Article
Engineering, Environmental
Daria Kowalczykiewicz, Daria Kowalczykiewicz, Marta Przypis, Marta Przypis, Luuk Mestrom, Luuk Mestrom, Antje Kumpf, Antje Kumpf, Dirk Tischler, Dirk Tischler, Peter-Leon Hagedoorn, Peter-Leon Hagedoorn, Ulf Hanefeld, Ulf Hanefeld, Andrzej Jarzebski, Andrzej Jarzebski, Katarzyna Szymanska, Katarzyna Szymanska
Summary: In this study, a two-step continuous flow enzymatic synthesis process was demonstrated using basic sugars as substrates in monolithic microreactors. Immobilisation of the enzymes on functionalised silica supports was found to be most effective through covalent bonding by amino groups using a glutaraldehyde linker. The process allows for the continuous in flow synthesis of natural and non-natural trehalose analogues and disaccharides, with high space-time-yield values achieved for UDP-glucose pyrophosphorylase and trehalose transferase catalysed reactions.
CHEMICAL ENGINEERING JOURNAL
(2022)
Review
Chemistry, Multidisciplinary
Kourosh Honarmand Ebrahimi, Simone Ciofi-Baffoni, Peter-Leon Hagedoorn, Yvain Nicolet, Nick E. Le Brun, Wilfred R. Hagen, Fraser A. Armstrong
Summary: Viruses utilize host cellular machinery to replicate, while the innate immune system activates, supports, and regulates iron-sulfur [FeS] cluster-containing proteins to restrict viral infections. Some of these proteins also support viral replication. This Review discusses the functions of these proteins and the role of [FeS] clusters in modulating the immune response, proposing models for their function.
Article
Chemistry, Physical
Jose Coloma, Lidwien Teeuwisse, Muhammad Afendi, Peter-Leon Hagedoorn, Ulf Hanefeld
Summary: The Granulicella tundricola hydroxynitrile lyase (GtHNL) can catalyze the synthesis of chiral (R)-cyanohydrins and (R)-beta-nitro alcohols. In this study, the GtHNL-3V variant was immobilized on Celite R-633 and used in batch and continuous flow systems for the synthesis of (R)-2-nitro-1-phenylethanol. The batch system showed higher yield and productivity compared to the flow system, indicating that the batch system is superior for the synthesis of (R)-NPE.
Article
Biochemistry & Molecular Biology
Romina Fernandez Varela, Ana Laura Valino, Eman Abdelraheem, Rosario Medici, Melisa Saye, Claudio A. Pereira, Peter-Leon Hagedoorn, Ulf Hanefeld, Adolfo Iribarren, Elizabeth Lewkowicz
Summary: The utility of different variants of DERA enzyme in synthesizing drug side chains and industrial applications was analyzed. One variant was found to efficiently produce the desired products under optimized conditions and exhibited tolerance to high acetaldehyde concentrations.
Article
Biochemistry & Molecular Biology
Hirotoshi Matsumura, Abayomi S. Faponle, Peter-Leon Hagedoorn, Takehiko Tosha, Sam P. de Visser, Pierre Moenne-Loccoz
Summary: In this study, low-temperature FTIR photolysis experiments were conducted to investigate the mechanism of substrate inhibition in cytochrome-c dependent denitrifying NO reductases (cNORs). The results confirmed that substrate inhibition is caused by a radical combination reaction between the diferric mu-oxo group and an NO molecule, forming a heme Fe(III)-nitrito-FeB(II) inhibitory complex.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2022)
Article
Biochemistry & Molecular Biology
Hongshan San, Marianne Paresoglou, Michelle Minneboo, Ingmar A. J. van Hengel, Aytac Yilmaz, Yaiza Gonzalez-Garcia, Ad C. Fluit, Peter-Leon Hagedoorn, Lidy E. Fratila-Apachitei, Iulian Apachitei, Amir A. Zadpoor
Summary: In this study, the authors incorporated reduced graphene oxide (rGO) and silver (Ag) nanoparticles onto 3D-printed titanium implants using plasma electrolytic oxidation (PEO), which showed enhanced antibacterial activity and stimulated the differentiation of preosteoblast cells. These findings suggest that these multifunctional surfaces have high clinical potential.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Engineering, Environmental
Jie Zhang, Lirong Tan, Peter-Leon Hagedoorn, Ruiqi Wang, Li Wen, Siwei Wu, Xuemei Tan, Hui Xu, Xing Zhou
Summary: This study introduces a novel hybrid technique of micro-nano bubbles assisted laccase (MNB-Lac) for the degradation of bisphenols in water. The results showed that MNB-Lac exhibited higher degradation efficiency and removal efficiency compared to other treatment methods. It was also successfully used for treating different types of bisphenols contaminants. This research could provide new insights into the enhancement of oxidizing enzyme performance using MNB technology.
JOURNAL OF WATER PROCESS ENGINEERING
(2022)
Review
Biochemistry & Molecular Biology
Wilfred R. R. Hagen
Summary: The development of tungsten biochemistry is discussed, with a focus on personal involvement. A comprehensive catalog of genes, enzymes, and reactions related to tungsten has been compiled. EPR spectroscopy has played a significant role in understanding tungstopterin-based catalysis. However, the lack of pre-steady-state data remains a challenge. Tungstate transport systems and biosynthetic machinery for tungstopterin enzymes have been studied, revealing their specificity for tungsten and additional selectivity. Metallomics analysis of Pyrococcus furiosus has provided a comprehensive inventory of tungsten proteins.
Article
Chemistry, Physical
Carola S. Seelmann, Simona G. Huwiler, Martin Culka, Marc J. F. Strampraad, Till Biskup, Stefan Weber, G. Matthias Ullmann, Volker Schunemann, Peter-Leon Hagedoorn, Antonio J. Pierik, Matthias Boll
Summary: In anaerobic aromatic compound degrading microbes, class II benzoyl-coenzyme A (CoA) reductases (BCRs) reduce benzoyl-CoA to cyclohexa-1,5-diene-1-carboxyl-CoA (1,5-dienoyl-CoA) through a tungsten-bis-metallopterin (MPT) cofactor. This study provides experimental evidence for the Birch-like reduction mechanism via W(V)/radical intermediates and reveals the unique tetrahydro state of MPT cofactors essential for the reversibility of enzymatic Birch reduction.
Article
Chemistry, Physical
Josei Coloma, Peter-Leon Hagedoorn, Isabel Bento, Ulf Hanefeld
Summary: GtHNL is a manganese dependent cupin enzyme that can catalyze the enantioselective synthesis of cyanohydrins. It also has the ability to catalyze the oxidative cleavage of α-methyl styrene. The introduction of variants like H96A and H96F can enhance its catalytic activity towards oxidative cleavage of styrenes.
Article
Biochemistry & Molecular Biology
Wilfred R. Hagen, Ricardo O. Louro
Summary: Distances between Fe ions in multiheme cytochromes are short, allowing for intramolecular dipole-dipole interactions. Previous analysis of cytochrome EPR data has ignored this interaction. In this study, a low-frequency broadband EPR spectrometer was used to investigate the dipolar interaction in two cytochromes and identify limitations in analysis.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Chemistry, Inorganic & Nuclear
Radoslaw Kotuniak, Paulina Szczerba, Dobromila Sudzik, Marc J. F. Strampraad, Peter-Leon Hagedoorn, Wojciech Bal
Summary: We investigated the kinetics of Cu(ii) binding to ACTUN peptides using modified/substituted GGH analogues. Rules for rate modulation by 1(st) and 2(nd) sphere interactions were established, providing crucial insight into the elucidation of the reaction mechanism and its contribution to biological copper transport.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Physical
Wilfred R. Hagen, Randell L. Mills
Summary: The study explores the transition of the hydrogen atom between stable ground state and excited states, as well as the possible existence of lower-energy hydrino states with unique quantum properties. Experimental results show that molecular hydrino exhibits specific characteristics in both gas phase and polymers, consistent with theoretical models.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Biochemistry & Molecular Biology
Wilfred R. Hagen
Summary: Belief in a specific scientific claim can gain unfounded authority through citation bias, amplification, and invention. This phenomenon is not limited to specific fields of science, as evidenced by a case study in the field of metallomics.