Article
Chemistry, Applied
Gabriel Luna-Lopez, Raquel Sainz, Ana M. Coito, Charlotte Pichon, Ana Iglesias-Juez, Ines A. C. Pereira, Antonio L. De Lacey, Marcos Pita
Summary: In order to tackle the challenge of diminishing the high potentials required for the reaction, a combination of a redox biocatalyst and an inorganic semiconductor has been studied. The system, based on a photocathode made of copper gallium sulfide and Desulfovibrio vulgaris Hildenborough NiFeSe-hydrogenase, can produce photoelectrochemical biocatalytic proton reduction to H2 without any sacrificial agent while providing an approximately 400 mV decrease of the applied potential.
Article
Biochemistry & Molecular Biology
Gabriel Luna-Lopez, Melisa del Barrio, Jennifer Fize, Vincent Artero, Ana Margarida Coito, Ines A. C. Pereira, Jose Carlos Conesa, Ana Iglesias-Juez, Antonio L. De Lacey, Marcos Pita
Summary: Clean energy vectors are required to achieve a fossil fuel-free society, reducing both greenhouse effect and pollution. Electrochemical water splitting provides a clean method to obtain green hydrogen, but efficient electrocatalysts are needed to avoid high overpotentials. The combination of inorganic semiconductors with biocatalysts offers an alternative approach for photoelectrochemical H2 production.
BIOELECTROCHEMISTRY
(2023)
Article
Multidisciplinary Sciences
Osvaldo Daniel Cortazar, Ana Megia-Macias, Sandra Moreno, Alejandro Brun, Eduardo Gomez-Casado
Summary: This study demonstrates the capability of Plasma Activated Media (PAM) to inactivate SARS-CoV-2 and PR8 H1N1 influenza virus without damaging healthy cells, acting through virus detachment and reduced replication. Furthermore, PAM treatment does not induce inflammation. These findings open up a new research avenue for the development of novel treatments for COVID-19, influenza, and other respiratory diseases using PAM.
SCIENTIFIC REPORTS
(2022)
Article
Chemistry, Multidisciplinary
Aurore Jacq-Bailly, Martino Benvenuti, Natalie Payne, Arlette Kpebe, Christina Felbek, Vincent Fourmond, Christophe Leger, Myriam Brugna, Carole Baffert
Summary: Hnd, a tetrameric enzyme from Desulfovibrio fructosovorans, is capable of flavin-based electron bifurcation. Despite its complexity, the enzyme can catalytically exchange electrons with an electrode and demonstrates unique high potential inactivation/reactivation kinetics. The catalytic properties of Hnd are comparable to standard hydrogenases, suggesting that the additional subunits necessary for electron bifurcation do not alter the enzyme's catalytic behavior at the active site.
FRONTIERS IN CHEMISTRY
(2021)
Article
Chemistry, Physical
A. A. Tsygankov, N. A. Zorin, A. S. Starodubov, M. Kh Khasimov, M. S. Melnikova, I. A. Doronin, R. G. Vasilov
Summary: The C-terminal domain of the HydS subunit of HydSL hydrogenase plays an important role in electron transfer with the transmembrane protein Isp1, and a simple method for immobilizing the hydrogenase on a hydrophobic carbon electrode has been developed. The resulting electrodes demonstrated high power and current in a fuel cell and maintained stability over a period of 49 days.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Multidisciplinary
Takeshi Hiromoto, Koji Nishikawa, Seiya Inoue, Hideaki Ogata, Yuta Hori, Katsuhiro Kusaka, Yu Hirano, Kazuo Kurihara, Yasuteru Shigeta, Taro Tamada, Yoshiki Higuchi
Summary: This study reports that [NiFe]-hydrogenase from Desulfovibrio vulgaris Miyazaki F can recover its catalytic activity by reacting with H2 under anaerobic conditions after being inactivated in the presence of O2. Neutron structure analysis revealed that a part of the Ni ion dissociates from the active site Ni-Fe complex and forms a new square-planar Ni complex, accompanied by rearrangement of the coordinated thiolate ligands. The analysis also found that the Cys17(S) thiolate forms an unusual hydrogen bond with the main-chain amide N atom of Gly19(S), providing insights into the redox reaction of the Fe-S cluster.
Article
Chemistry, Physical
Ruizhe Gu, Tao Zhou, Zihao Wang, Zheng Chen, Junwen Tao, Zhewei Fan, Lingyun Guo, Yongsheng Liu
Summary: Designing high-efficiency catalysts for overall water splitting is crucial for reducing the cost of hydrogen fuel as a clean and renewable energy source. This study successfully synthesized Mo-, P-codoped NiFeSe catalysts on nickel foam, which exhibited efficient HER/OER performances with low overpotential and high stability. The catalysts required only 1.53 V to deliver a current density of 10 mA cm-2 in overall water splitting and maintained outstanding durability for 100 h.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Biotechnology & Applied Microbiology
Enrique Raga-Carbajal, Guadalupe Espin, Marcela Ayala, Julieta Rodriguez-Salazar, Liliana Pardo-Lopez
Summary: In this study, a LEA protein AvLEA1 was found to provide protection to enzymes and showed potential as a biological stabilizer reagent. AvLEA may act as a molecular chaperone or shield to prevent enzyme dissociation or aggregation, or function as a radical scavenger to prevent damage to enzymes under stress conditions.
APPLIED MICROBIOLOGY AND BIOTECHNOLOGY
(2022)
Article
Gastroenterology & Hepatology
Shuyang Cao, Yuanyuan Zhang, Ruoyu Bao, Tao Wang, Liqi Zhu, Quan Zhang
Summary: This study found that Helicobacter hepaticus produces a nickel-containing hydrogenase enzyme that promotes liver inflammation and fibrosis. However, the impact of a mutated form of this enzyme on liver fibrosis has not been explored.
Article
Chemistry, Physical
Yu Ma, Feng-Ge Wang, Ruo-Yao Fan, Hui-Ying Wang, Wen-Li Yu, Hai-Jun Liu, Jing-Qi Chi, Lei Wang, Yong-Ming Chai, Bin Dong
Summary: This study utilized nickel-iron selenide as a two-dimensional nanosheet structure OER electrocatalyst, achieving excellent basic OER electrocatalytic performance with the assistance of microwave, demonstrating potential for future applications.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Biochemistry & Molecular Biology
Petra Kosutova, Nikolett Nemcova, Maros Kolomaznik, Daniela Mokra, Andrea Calkovska, Pavol Mikolka
Summary: Aspirated meconium into a newborn's airways can induce oxidative stress and inflammation, which may affect the effectiveness of surfactant therapy. This study aimed to investigate the time course of oxidative stress marker production during meconium aspiration syndrome (MAS) and its relationship with leukocyte infiltration.
Article
Microbiology
Peter Walker, Aidan J. Taylor, Andrew Hitchcock, Joseph P. Webb, Jeffrey Green, Julia Weinstein, David J. Kelly
Summary: This study demonstrates that C. jejuni is highly susceptible to violet-blue light and identifies the regulatory networks involved in responding to photo-oxidative damage. The findings provide insights for the development of commercial applications of VB light-based technologies.
Article
Environmental Sciences
Shiquan Sun, Qingxin Tang, Hui Xu, Yang Gao, Wei Zhang, Lean Zhou, Yifu Li, Jinting Wang, Chuxuan Song
Summary: Harmful algae blooms (HABs) caused by eutrophication and extreme weather have worldwide distribution and pose threats to the environment and human health. Photocatalytic technology has shown potential in inhibiting HABs by damaging algae cells and degrading toxic metabolites. This study systematically reviews the progress in photocatalytic performance and algae removal efficiency, discusses the damage mechanisms of photocatalysts to algae cells, and explores the degradation rates and pathways of microcystins.
Article
Chemistry, Multidisciplinary
Rakesh Ruchel Khanikar, Monalisa Kalita, Parismita Kalita, Bhaswati Kashyap, Santanu Das, Mojibur R. Khan, Heremba Bailung, Kamatchi Sankaranarayanan
Summary: This study demonstrates that cold atmospheric pressure plasma treatment can deactivate the SARS-CoV-2 spike protein and degrade the RNA of the virus. The deactivation of spike protein binding is correlated with the higher concentration of hydrogen peroxide formation due to the interaction with reactive oxygen species in the plasma. This green process, using noble gases to generate reactive oxygen species, shows potential for designing disinfection systems and biomedical applications.
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
Chemistry, Multidisciplinary
Marta Meneghello, Alexandre Uzel, Marianne Broc, Rita R. Manuel, Axel Magalon, Christophe Leger, Ines A. C. Pereira, Anne Walburger, Vincent Fourmond
Summary: Metal-based formate dehydrogenases are enzymes that require molybdenum or tungsten ions to catalyze the conversion between formate and CO2. The coordination of the metal ion in the active form prevents direct binding of formate to the metal. The study's findings provide strong evidence for the hypothesis that the oxidation of formate occurs in the second coordination sphere of the metal.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Microbiology
Delfim Ferreira, Sofia S. S. Venceslau, Raquel Bernardino, Andre Preto, Lichun Zhang, Jacob R. R. Waldbauer, William D. D. Leavitt, Ines A. C. Pereira
Summary: DsrC is a crucial protein in dissimilatory sulfur metabolism, serving as a co-substrate of the dissimilatory sulfite reductase DsrAB. It has been found to have additional functions beyond sulfite reduction. In this study, the role of DsrC in fermentative growth of Desulfovibrio vulgaris Hildenborough was investigated, and it was found that impairment of DsrC function led to reduced growth and a shift towards more fermentative metabolism.
ENVIRONMENTAL MICROBIOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Vladimir Pelmenschikov, Delfim Ferreira, Sofia S. Venceslau, Peter Hildebrandt, Ines A. . C. Pereira, Smilja Todorovic, Smilja Todorovic
Summary: In this study, resonance Raman spectroscopy and density functional theory calculations were used to investigate the structural, electronic, and vibrational properties of the noncubane [4Fe-4S] cluster in heterodisulfide reductase (HdrB). Homology modeling was employed to predict the protein environment of the neighboring clusters in DvHdrB. The results showed that the oxidized [4Fe-4S](3+) cluster adopts a closed conformation in the absence of substrate, but transitions to an open structure upon substrate coordination, accompanied by a ligand switch. This study provides valuable insights for future research on enzymes with this unconventional cofactor.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Andreas Rutz, Chandan K. Das, Andrea Fasano, Jan Jaenecke, Shanika Yadav, Ulf-Peter Apfel, Vera Engelbrecht, Vincent Fourmond, Christophe Leger, Lars Schaefer, Thomas Happe
Summary: The active site of [FeFe]-hydrogenases degrades upon contact with oxygen, but the protein structure of a certain hydrogenase (CbA5H) allows its active site to be protected, reducing degradation caused by oxygen. By modifying the surface residue, the hydrogenase's resistance to oxygen can be increased.
Article
Chemistry, Inorganic & Nuclear
Cheriehan Hessin, Jules Schleinitz, Nolwenn Le Breton, Sylvie Choua, Laurence Grimaud, Vincent Fourmond, Marine Desage-El Murr, Christophe Leger
Summary: Potential inversion refers to the phenomenon where the second electron transfer is easier than the first, and it is significant for understanding enzyme catalysis and developing efficient catalysts. Currently, there is a lack of analytical predictions to interpret voltammetric peak potentials when potential inversion occurs, and cyclic voltammograms are often analyzed without considering overfitting or estimating error. In this study, a theory for voltammetry of two-electron redox species in the irreversible limit is formulated and applied to analyze the voltammetry of a nickel complex with redox-active ligands, highlighting the intrinsic underdetermination of the model. Characterizing the thermodynamics of two-electron electron-transfer reactions is crucial for catalyst design.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Raphael J. Labidi, Bruno Faivre, Philippe Carpentier, Giulia Veronesi, Albert Solei-Daura, Ragnar Bjornsson, Christophe Leïger, Philipp Gotico, Yun Li, Mohamed Atta, Marc Fontecave
Summary: In this study, the performance of the orange protein (Orp) as a catalyst for photocatalytic reduction of protons into H-2 under visible light irradiation was investigated. It was found that Orp exhibited excellent photocatalytic activity in the presence of ascorbate as the sacrificial electron donor and [Ru(bpy)(3)]Cl-2 as the photosensitizer. Density functional theory (DFT) calculations were used to propose a consistent reaction mechanism.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Correction
Chemistry, Multidisciplinary
Vincent Fourmond, Carole Baffert, Kateryna Sybirna, Thomas Lautier, Abbas Abou Hamdan, Sebastien Dementin, Philippe Soucaille, Isabelle Meynial-Salles, Herve Bottin, Christophe Leger
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Ecology
Sinje Neukirchen, Ines A. C. Pereira, Filipa L. Sousa
Summary: Microbial dissimilatory sulfur metabolism plays a significant role in Earth's biochemical sulfur cycle. Comparative genomics and phylogenetic analyses indicate an archaeal origin of the minimal DsrABCMK(N) protein set, with sulfite reduction as its primordial function. The acquisition of additional Dsr proteins increased the complexity of the Dsr pathway. Further discoveries of two types of Qmo complexes allowed microorganisms to use sulfate as an electron acceptor. Chlorobi and Proteobacteria evolved the ability to use the Dsr pathway for sulfur oxidation independently.
Article
Chemistry, Multidisciplinary
Andrea Fasano, Chloe Guendon, Aurore Jacq-Bailly, Arlette Kpebe, Jeremy Wozniak, Carole Baffert, Melisa del Barrio, Vincent Fourmond, Myriam Brugna, Christophe Leger
Summary: The observation that some homologous enzymes have the same active site but very different catalytic properties demonstrates the importance of long-range effects in enzyme catalysis. In this study, the catalytic bias and sensitivity of hydrogenase 1 (Hyd 1) were found to be determined by the catalytic subunit rather than the electron transfer chain, and the proximal cluster was confirmed to play a role in the enzyme's resistance to long-term exposure to O-2. This research provides insights into the structure-function relationships of hydrogenases and offers possibilities for engineering useful hydrogenases with desired properties.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Correction
Chemistry, Multidisciplinary
Vincent Fourmond, Carole Baffert, Kateryna Sybirna, Thomas Lautier, Abbas Abou Hamdan, Philippe Soucaille, Isabelle Meynial-Salles, Christophe Leger
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Review
Chemistry, Multidisciplinary
Dan He, Yawen Li, Fuwen Zhao, Yuze Lin
Summary: High trap density in organic solar cells leads to localized charge carriers and reduced carrier lifetime, limiting device efficiency. This feature article summarizes the recent advances of trap suppression by material design and device engineering.
CHEMICAL COMMUNICATIONS
(2024)
Review
Chemistry, Multidisciplinary
Olivier Monfort, Arshitha Madhusudhan, Martin Motola
Summary: This article presents the advantages of coupling photocatalysis and Fenton-based processes for environmental remediation and discusses their synergy. It critically examines the simultaneous triggering of these two processes and provides insights into research approaches. The study aims to enhance understanding of this complex process and highlight the potential integration of new catalysts in current wastewater treatment technology.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Manideepa Dhar, Chittaranjan Mishra, Avijit Das, Uttam Manna
Summary: An approach of 'polymerization of monomers in its aggregated form' has been introduced to tailor the water wettability of fibrous and porous substrates, achieving hydrophobicity to superhydrophobicity transition, as well as patterned wettability. This facile chemical method provides a durable coating with adjustable and patterned wettability for various potential applications.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Saswat Ranjan Bhoi, Chhanda Debnath, Shikha Gandhi
Summary: In this article, a novel catalytic reaction using Pd(0) and Bronsted acid is reported for the synthesis of biologically important imidazolidinone-fused N-heterocycles through redox-neutral intramolecular N-allylation of indoles and pyrroles with alkynes. This atom-economical method is applicable to a wide range of substrates and eliminates the need for leaving groups or oxidizing agents commonly used in traditional allylation reactions.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Longkun Chen, Mingshuai Zhang, Meichen Liu, Zhuoyuan Liu, Yuetong Qiu, Zhilai Zhang, Fuchao Yu, Jiuzhong Huang
Summary: In this study, an efficient Rh(III)-catalyzed selective mono- and dual-C-H bond functionalization/cyclization with iodonium ylide as the sole coupling partner was demonstrated. Fused benzodiazepine skeletons were obtained in excellent yields, providing an improved approach to dual C-H unsymmetrical functionalization.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Alice Kennett, Sven Epple, Gabriella van der Valk, Irene Georgiou, Evelyne Gout, Romain R. Vives, Angela J. Russell
Summary: This study presents the design and synthesis of sulfated disaccharide inhibitors based on IdoA(2S)-GlcNS(6S), which showed potent inhibition of Sulf-2. The results suggest that IdoA(2S)-GlcNS(6S) is the shortest fragment size required for effective inhibition of Sulfs, and a trisulfated disaccharide is identified as the minimal fragment size of heparan sulfate for effective endosulfatase inhibition.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Mauro Garbini, Andrea Brunetti, Riccardo Pedrazzani, Magda Monari, Massimo Marcaccio, Giulio Bertuzzi, Marco Bandini
Summary: The self-adaptability of galvanostatic electrolysis was found to be helpful in a multistage chemo- and diastereoselective electrochemically promoted cyclodimerization of chalcones. Through a series of reductive events, densely functionalized cyclopentanes with five contiguous stereocenters were obtained (25 examples, yields up to 95%, dr values up to >20:1). Further experimental and electrochemical investigations indicated the crucial role of dynamic kinetic resolution of the aldol intermediate in the reaction mechanism.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Dhananjay S. Nipate, Neha Meena, Prakash N. Swami, Krishnan Rangan, Anil Kumar
Summary: In this study, the synthesis of functionalized benzo[a]phenazines and indazolo[2,3-a]quinolines was achieved through Rh(III)-catalyzed oxidative annulation of 2-arylquinoxalines and 2-aryl-2H-indazoles with allyl alcohols. The method showed a wide substrate scope, excellent functional group tolerance, good to high yields of annulated products, and the capability for scaled-up synthesis. A tentative mechanism of the annulation reaction was proposed based on a preliminary mechanistic investigation.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Ruonan Zhang, Abudukadi Tudi, Xia Yang, Xuping Wang, Zhihua Yang, Shujuan Han, Shilie Pan
Summary: A new lead tellurium borate material with a unique fundamental building block [B4O10] was synthesized and found to exhibit high birefringence. The structure-property relationship was discussed using first-principles calculations.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Amresh Kumar Singh, Baishali Thakurta, Anupam Giri, Monalisa Pal
Summary: This study introduces three key concepts for the quick synthesis of large-scale high-quality 2D materials films and their utilization in device fabrication.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Reina Hagiwara, Shun Nishimura, Kosuke Okeyoshi
Summary: A copolymer-conjugated nanocatalytic system has been developed to improve electron transfer and enhance photoinduced H2 generation.
CHEMICAL COMMUNICATIONS
(2024)
