Article
Chemistry, Physical
Umberto Contaldo, Bruno Guigliarelli, Julien Perard, Clara Rinaldi, Alan Le Goff, Christine Cavazza
Summary: A highly stable and active recombinant RrCODH was developed, showing impressive CO oxidation activity and selective CO2/CO interconversion capability. This functional device, with turnover number reaching at least 800,000, performs close to the best metal-based and molecular-based catalysts, setting a new benchmark for bioelectrocatalysis of reversible CO2 conversion.
Article
Microbiology
Shiho Nishida, Kimiho Omae, Masao Inoue, Yoshihiko Sako, Ryoma Kamikawa, Takashi Yoshida
Summary: Despite its toxicity, some prokaryotes can utilize carbon monoxide (CO) through the action of carbon monoxide dehydrogenase (CODH) and energy-converting hydrogenase (ECH). This study detected high-quality metagenome assembled genomes (MAGs) from potential hydrogenogenic CO utilizers through anaerobic CO-enrichment cultures. These MAGs contained novel CODH gene clusters, expanding the CODH database.
ARCHIVES OF MICROBIOLOGY
(2023)
Article
Biotechnology & Applied Microbiology
Yoshinari Imaura, Shunsuke Okamoto, Taiki Hino, Yusuke Ogami, Yuka Adachi Katayama, Ayumi Tanimura, Masao Inoue, Ryoma Kamikawa, Takashi Yoshida, Yoshihiko Sako
Summary: Microbial CO oxidation contributes to global carbon cycling and serves as a remover of toxic CO. Some microbial CO oxidizers have sister relationships with non-CO oxidizers. We discovered a versatile CO oxidizer, Parageobacillus sp. G301, capable of anaerobic and aerobic CO oxidation using both types of CODH. Comparative genomic analysis suggests that CO oxidation genes are not essential in the genus Parageobacillus.
APPLIED AND ENVIRONMENTAL MICROBIOLOGY
(2023)
Article
Chemistry, Physical
T. Bhowmick, S. Nag, S. B. Majumder
Summary: A highly sensitive and selective carbon monoxide sensor has been developed using a LaFe0.8Co0.2O3 perovskite thin-film sensing element. Proper utilization of perovskite surface's catalytic properties and microstructural control in a thin film sensor enabled selective CO sensing. High selectivity to CO was achieved due to low metal-oxygen binding energy, favorable electronic configuration of transition metal cations, and perovskite surface composition.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Chemistry, Multidisciplinary
Csaba Arvai, Laszlo T. Mika
Summary: This review summarizes the recent applications of alternative solvents in improving the efficiency, safety, and environmental friendliness of carbonylation reactions. The use of water, biomass-based alcohols, ionic liquids, and other alternative solvents can enhance the reaction protocols.
CHINESE JOURNAL OF CHEMISTRY
(2023)
Article
Biochemistry & Molecular Biology
Elisabeth Darrouzet, Clara Rinaldi, Barbara Zambelli, Stefano Ciurli, Christine Cavazza
Summary: Nickel insertion into nickel-dependent CODH is a key step in enzyme activation, with CooJ playing a significant role in this process by binding Ni(II) ions through HAS motif. CooJ homologues exhibit distinct motifs for Ni(II) binding, suggesting potential significance in CODH maturation and nickel homeostasis.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2021)
Article
Chemistry, Physical
Man Ho Han, Dongjin Kim, Sangkuk Kim, Seung-Ho Yu, Da Hye Won, Byoung Koun Min, Keun Hwa Chae, Woong Hee Lee, Hyung-Suk Oh
Summary: This study demonstrates that nickel sulfide nanoparticles can mimic the electronic structure of nickel single atom catalysts and enhance catalytic activity in CO2 reduction reaction. However, the stability of nickel sulfide is low and needs further improvement.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Xinzhou Chen, Gang Chen, Zhong Lian
Summary: Carbonyl compounds are widely used in drug discovery and as intermediates in carbon-carbon and carbon-heteroatom bond formation. Transition-metal-catalyzed carbonylation via CO insertion is a highly efficient strategy, but often requires expensive and toxic noble-metal catalysts. The exploration of nickel-catalyzed carbonylation reactions has grown due to the abundance and low cost of nickel. However, this area is relatively underdeveloped compared to palladium-catalyzed carbonylation due to the strong binding of CO to nickel. Recent research has focused on using CO surrogates or specific catalysts to overcome this issue.
CHINESE JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Umberto Contaldo, Mathieu Curtil, Julien Perard, Christine Cavazza, Alan Le Goff
Summary: An AcPyTACN compound was synthesized for immobilizing recombinant CODH on carbon-nanotube electrodes, resulting in high current density and stability for electroenzymatic CO2 reduction.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Jian Luo, Bo Hu, Wenda Wu, Maowei Hu, T. Leo Liu
Summary: This study reports a redox neutral electrochemical C(sp(2))-C(sp(3)) cross-coupling reaction conducted under ambient conditions using nonprecious metal catalysts. The reaction demonstrated good yields and a broad scope, with potential applications in pharmaceuticals and natural amino acid modification. The method, which proceeds through an unconventional radical transmetalation mechanism, is highly productive and expected to have widespread applications in organic synthesis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Jimin Park, Joy S. Zeng, Atharva Sahasrabudhe, Kyoungsuk Jin, Yoel Fink, Karthish Manthiram, Polina Anikeeva
Summary: Researchers have developed an electrochemical approach to on-demand release CO by reducing dissolved CO2, modulating signaling pathways mediated by CO receptor. By exploring the effects of CO release kinetics on neuronal signaling, and integrating components into microscale fibers, they localized CO synthesis and activated signaling cascades in targeted cells. This approach may facilitate studies of physiological processes affected by this gaseous molecular messenger.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Review
Chemistry, Multidisciplinary
Song Jin, Zhimeng Hao, Kai Zhang, Zhenhua Yan, Jun Chen
Summary: The electrochemical carbon dioxide reduction reaction is an important pathway for converting renewable electricity into fuels and feedstocks, with the conversion of CO2 into CO being a promising reaction. Advancements in catalyst and electrolyte design, along with understanding the catalytic mechanism, are crucial for promoting the technology towards industrial implementation. However, there are still challenges and future directions for the industrial application of this technology.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Review
Chemistry, Multidisciplinary
Ying Shu, Weibin Liang, Jun Huang
Summary: Enzymatic reactions have emerged as a promising alternative to traditional chemical catalysis for CO2 conversion. However, the use of enzymes is limited due to their fragility, instability, and lack of recyclability. Metal-organic frameworks (MOFs) have recently gained attention as immobilization scaffolds for enzymes. This review discusses the various forms of heterogeneity in enzyme/MOF systems and explores their benefits, synthesis strategies, and recent research progress. The integration of enzymatic systems and MOFs for CO2 conversion is also examined, alongside the challenges and potential future directions of biocatalytic CO2 conversion using MOF-based biocatalysts.
Review
Chemistry, Multidisciplinary
Chen Zhu, Huifeng Yue, Jiaqi Jia, Magnus Rueping
Summary: The formation of C-heteroatom bonds through recent advances in homo- and heterogeneous Ni-catalyzed reactions under mild conditions is attractive due to sustainability and practicability. The generation of Ni-III and excited Ni-II intermediates enables mild cross-couplings, leading to the development of various catalytic systems involving photoredox and nickel dual catalysis, photoexcited nickel catalysis, electro and nickel dual catalysis, and heterogeneous photoredox and nickel dual catalysis using different materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Microbiology
Marisa R. Myers, G. M. King
Summary: This article explores the relationship between CO and perchlorate reduction, and found that Ni-COX can use CO to reduce perchlorate and support growth.
Article
Biochemistry & Molecular Biology
Angela S. Fleischhacker, Amanda L. Gunawan, Brent A. Kochert, Liu Liu, Thomas E. Wales, Maelyn C. Borowy, John R. Engen, Stephen W. Ragsdale
JOURNAL OF BIOLOGICAL CHEMISTRY
(2020)
Article
Chemistry, Multidisciplinary
Christopher D. James, Seth Wiley, Stephen W. Ragsdale, Brian M. Hoffman
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Chemistry, Physical
Steven E. Cohen, Mehmet Can, Elizabeth C. Wittenborn, Rachel A. Hendrickson, Stephen W. Ragsdale, Catherine L. Drennan
Article
Biology
Connor J. Cooper, Kaiyuan Zheng, Katherine W. Rush, Alexander Johs, Brian C. Sanders, Georgios A. Pavlopoulos, Nikos C. Kyrpides, Mircea Podar, Sergey Ovchinnikov, Stephen W. Ragsdale, Jerry M. Parks
COMMUNICATIONS BIOLOGY
(2020)
Article
Biochemistry & Molecular Biology
Liu Liu, Arti B. Dumbrepatil, Angela S. Fleischhacker, E. Neil G. Marsh, Stephen W. Ragsdale
JOURNAL OF BIOLOGICAL CHEMISTRY
(2020)
Article
Biochemistry & Molecular Biology
Steven E. Cohen, Edward J. Brignole, Elizabeth C. Wittenborn, Mehmet Can, Samuel Thompson, Stephen W. Ragsdale, Catherine L. Drennan
Summary: Electron microscopy was used to capture multiple snapshots of ACS, revealing previously uncharacterized domain motion and forming extended and hyperextended structural states, where the A-cluster is accessible for methylation by CFeSP.
Article
Multidisciplinary Sciences
Anindita Sarkar, Eric L. Carter, Jill B. Harland, Amy L. Speelman, Nicolai Lehnert, Stephen W. Ragsdale
Summary: Rev-Erb beta is a nuclear receptor that plays a key role in regulating circadian rhythm, metabolism, and inflammation. Heme binding to the protein affects its function as a repressor and its ability to bind other proteins. Interestingly, Rev-Erb beta exists in the Fe3+ form within the cell, contradicting its role as a gas sensor. This study demonstrates how the Fe3+ state is congruent with heme binding and cellular gas sensing, suggesting a potential mechanism for CO/NO-mediated regulation of circadian rhythm through redox changes in Rev-Erb beta.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Multidisciplinary
Anjali Patwardhan, Ritimukta Sarangi, Bojana Ginovska, Simone Raugei, Stephen W. Ragsdale
Summary: Methyl-coenzyme M reductase (MCR) plays a crucial role in catalyzing both the synthesis and anaerobic oxidation of methane. Studies have shown that the active Ni(I) state of MCR binds to substrates methyl-SCoM and CoMSSCoB through their sulfonate groups to form a hexacoordinate complex, rather than directly interacting with sulfur. This suggests that both forward and reverse MCR reactions proceed through long-range electron transfer from the Ni(I)-sulfonate complexes.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Review
Biochemistry & Molecular Biology
Angela S. Fleischhacker, Anindita Sarkar, Liu Liu, Stephen W. Ragsdale
Summary: This review explores the essential roles of heme in biological processes, focusing on how it binds to HRMs and regulates protein structure, function, and degradation through changes in redox state. Two HRM-containing proteins, human heme oxygenase-2 and the transcriptional regulator Rev-erb beta, are discussed in relation to cellular heme composition and CO sensing. The importance of understanding heme distribution, CO, and heme binding affinities in various biological processes is emphasized.
CRITICAL REVIEWS IN BIOCHEMISTRY AND MOLECULAR BIOLOGY
(2022)
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
Biochemistry & Molecular Biology
Stephen W. Ragsdale
Summary: The article highlights the integral involvement of the gut microbiome in producing beneficial metabolites and preventing the formation of disease-promoting compounds.
JOURNAL OF BIOLOGICAL CHEMISTRY
(2022)
Article
Biochemistry & Molecular Biology
David A. Hanna, Courtney M. Moore, Liu Liu, Xiaojing Yuan, Iramofu M. Dominic, Angela S. Fleischhacker, Iqbal Hamza, Stephen W. Ragsdale, Amit R. Reddi
Summary: Humans express two isoforms of heme oxygenase, HO-1 and HO-2, with distinct roles in regulating heme homeostasis. HO-2 acts as a buffering factor to control heme bioavailability, while both HO-1 and HO-2 provide protection from heme toxicity via enzymatic degradation when heme is in excess.
JOURNAL OF BIOLOGICAL CHEMISTRY
(2022)
Article
Biochemistry & Molecular Biology
Christopher J. Ohmer, Medhanjali Dasgupta, Anjali Patwardhan, Isabel Bogacz, Corey Kaminsky, Margaret D. Doyle, Percival Yang-Ting Chen, Stephen M. Keable, Hiroki Makita, Philipp S. Simon, Ramzi Massad, Thomas Fransson, Ruchira Chatterjee, Asmit Bhowmick, Daniel W. Paley, Nigel W. Moriarty, Aaron S. Brewster, Leland B. Gee, Roberto Alonso-Mori, Frank Moss, Franklin D. Fuller, Alexander Batyuk, Nicholas K. Sauter, Uwe Bergmann, Catherine L. Drennan, Vittal K. Yachandra, Junko Yano, Jan F. Kern, Stephen W. Ragsdale
Summary: Methyl-Coenzyme M Reductase (MCR) is a crucial enzyme in methanogenesis that has significant implications for global energy balances. However, the structure and reaction mechanism of this enzyme are still poorly understood.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2022)
Article
Chemistry, Physical
David W. White, Daniel Esckilsen, Seung Kyu Lee, Stephen W. Ragsdale, R. Brian Dyer
Summary: This study reports a light-driven photocatalytic system for efficient reduction of carbon dioxide to carbon monoxide using CODH II and CdSe/CdS nanocrystals. High quantum yields and turnover frequencies were achieved by incorporating a low-potential redox mediator. This provides new insights into the mechanism of the enzyme.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Biochemistry & Molecular Biology
Yue Dai, Angela S. Fleischhacker, Liu Liu, Sara Fayad, Amanda L. Gunawan, Dennis J. Stuehr, Stephen W. Ragsdale
Summary: GAPDH is involved in heme delivery to HO2, maintaining cellular heme homeostasis.
BIOLOGICAL CHEMISTRY
(2022)