Article
Microbiology
Young-Saeng Kim, Haeri Baek, Hyun-Sik Yun, Jae-Hak Lee, Kyoung-In Lee, Han-Soon Kim, Ho-Sung Yoon
Summary: The research found that the microalga Limnothrix redekei KNUA012 from a South Korean lake has a high potential as a biofuel feedstock and can synthesize alkanes and fatty acids directly.
POLISH JOURNAL OF MICROBIOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Fabian B. H. Rehm, Tristan J. Tyler, Simon J. de Veer, David J. Craik, Thomas Durek
Summary: This study reports an engineered enzyme that accepts various nucleophile substrate mimetics, especially when a method to selectively inhibit the reactivity of byproducts is employed. In addition, C-terminal Leu-ethylenediamine motifs are identified as bona fide mimetics of native N-terminal sequences, enabling transpeptidase-catalyzed C-to-C ligations. This work significantly expands the synthetic scope of enzyme-catalyzed protein transpeptidation reactions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Fabian B. H. Rehm, Tristan J. Tyler, Kuok Yap, Thomas Durek, David J. Craik
Summary: The use of enzymes, specifically asparaginyl endopeptidases (AEPs), for site-specific modification of proteins/peptides has become a popular method in studying protein/peptide functions or generating therapeutic conjugates. A novel approach using metal-complexation-based strategy has been developed to shift the AEP-catalyzed transpeptidation equilibrium towards product formation, allowing efficient peptide/protein labeling and enhancing protein-protein ligation. This method shows promise in facilitating the formation of transpeptidation products that are typically challenging to attain.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Ferdinand H. Lutter, Matthieu Jouffroy
Summary: A simple and functional-group-tolerant decarbonylative alkynylation method was reported in this study, which converts complex (hetero)aryl carboxylic acids into alkynes and was successfully applied in the preparation of a triazole analog of a commercial drug. Mechanistic investigations using labeled carboxylic acid derivatives confirmed the decarbonylative nature of this transformation.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Applied
Zhaozhao Sun, Huawen Huang, Qiaolin Wang, Guo-Jun Deng
Summary: This report presents a visible-light-mediated hydroalkylation reaction of alkenes using aldehydes as alkyl sources via bromo radical-promoted photoredox decarbonylation. The protocol offers an alternative approach to C(sp(3))-C(sp(3)) bond formation, featuring mild and clean reaction conditions, obviation for transition-metal catalyst, and good functional group compatibility.
ADVANCED SYNTHESIS & CATALYSIS
(2022)
Article
Chemistry, Physical
Or Argaman, Zohar Ben-Barak Zelas, Ayelet Fishman, Giora Rytwo, Adi Radian
Summary: In this study, ALDH enzyme was successfully immobilized on montmorillonite by pre-stabilization with a polyelectrolyte, offering potential for efficient immobilization of large multimeric proteins and advancing the design of bio-catalysis and bioremediation technologies platforms.
APPLIED CLAY SCIENCE
(2021)
Article
Engineering, Environmental
Aophat Choonut, Poonsuk Prasertsan, Sappasith Klomklao, Kanokphorn Sangkharak
Summary: A new type of mcl-co-lcl PHA containing 39.25 mol% 3HHD was isolated and utilized as biofuel substrate, and 3HAME was successfully produced via enzyme-catalyzed transesterification. The properties of 3HAME met international standards and this study is the first to evaluate the feasibility of producing biofuel from a PHA containing 3HHD monomer.
JOURNAL OF POLYMERS AND THE ENVIRONMENT
(2022)
Article
Energy & Fuels
Norshakirah Ahmad Rashidi, Elnida Mustapha, Yeow Yean Theng, Noor Azira Abdul Razak, Najihah Abdul Bar, Khairul Basyar Baharudin, Darfizzi Derawi
Summary: Waste cooking oil is an attractive feedstock for producing advanced biofuels due to its low cost and abundant availability. This study focused on the synthesis and analysis of mesoporous bimetallic catalysts for the catalytic deoxygenation of waste cooking oil. The results showed that the catalyst with 10% Ni-Fe/SBA-15 had the highest liquid yield but low selectivity towards the diesel fraction, while the catalyst with 5% Ni-Co/SBA-15 had the highest selectivity towards the diesel fraction.
Article
Biochemistry & Molecular Biology
Kevin Blanco-Esperguez, Inaki Tunon, Johannes Kastner, Fernando Mendizabal, Sebastian Miranda-Rojas
Summary: In this study, the impact of mutations in the catalytic site of MLL3 on its enzymatic activity and product specificity was investigated using QMMM calculations. Results showed that mutations of Y44 and Y128 led to enzyme inactivation, while mutation of Y128 to alanine reactivated the enzyme and even enhanced its ability to methylate lysine 4. Furthermore, the mechanism of inactivation was elucidated, revealing the importance of Y130 as a water occlusion structure.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Biochemistry & Molecular Biology
Lidia A. S. Cavaca, Rafael F. A. Gomes, Carlos A. M. Afonso
Summary: This study describes a method for the formation of thioaminals in water promoted by copper(II) triflate. Thioaminals, the N,S-analogues of O,O-acetals, are often overlooked due to the lack of efficient and sustainable preparation procedures for this functional group.
Article
Chemistry, Physical
Ziqiao Zhou, Hongchao Liu, Zhiyang Chen, Wenliang Zhu, Zhongmin Liu
Summary: Decarbonylation of carboxylic acids using heterogeneous zeolite catalyst can efficiently produce methyl acetate from acetic acid, ethylene from propionic acid, and propylene from butanoic acid, with selectivities around 70%-90%. This approach provides new insights into alkene production from biomass.
Article
Chemistry, Multidisciplinary
Palraj Kalimuthu, Dominik Hege, Agnieszka Winiarska, Yvonne Gemmecker, Maciej Szaleniec, Johann Heider, Paul V. Bernhardt
Summary: In contrast to molybdenum enzymes, tungsten enzymes have lower redox potentials and can perform reversible redox transformations. However, the electrochemical properties of tungsten enzymes have received less attention. In this study, the tungsten enzyme aldehyde oxidoreductase (AOR) from Aromatoleum aromaticum was immobilized on a glassy carbon electrode. The system showed electrocatalytic oxidation of aromatic and aliphatic aldehydes in the presence of electron transfer mediators. The different mediators had different electron transfer rates and methylene blue acted as a two-electron acceptor. This work demonstrates a highly energy efficient catalytic process for aldehyde oxidation at low applied electrochemical potential.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Wen-Qian Zhang, Hong-Cheng Shen
Summary: All-carbon quaternary stereocenters are important components of natural products and bioactive compounds, and a nickel and chiral amine cooperative catalysis has been disclosed to enable highly enantioselective allylic alkylation reactions. This method allows for the synthesis of diverse compounds with excellent enantioselectivity, and has been demonstrated in the synthesis of key chiral building blocks for bioactive compounds such as (+)-eptazocine and (-)-aphanorphine.
Article
Chemistry, Multidisciplinary
Changcheng Wei, Jinzhe Li, Zhongmin Liu
Summary: This study reported a method for the selective transformation of GVL to 1,3-butadiene using zeolite catalysts under ambient pressure and continuous flow conditions. The factors influencing the conversion rate were investigated, and the reaction pathway was revealed. This work provided a promising route for the sustainable and selective production of 1,3-butadiene from renewable materials.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Microbiology
Mahmudul Hasan, Sabrina Schulze, Leona Berndt, Gottfried J. Palm, Daniel Braga, Ingrid Richter, Daniel Last, Michael Lammers, Gerald Lackner
Summary: This study reveals the amino acid residues governing the substrate specificity of CofC in the formation of 3PG-F-420 through analysis of its crystal structure. Site-directed mutagenesis experiments further validate the role of these residues in substrate selectivity. Additionally, an unstable reaction product of CofC is discovered, and its binding mode is revealed. The role of CofD enzyme in controlling the specificity of the combined CofC/D reaction is also demonstrated. These findings provide novel insights into the biosynthesis and evolution of 3PG-F-420 and have implications for future research and biotechnological production of coenzyme F-420 derivatives.
Editorial Material
Biochemistry & Molecular Biology
Soumi Ghosh, E. Neil G. Marsh
Summary: A study has revealed that a high salt diet may make mice more susceptible to carrying viruses, attributed to a decrease in the levels of the antiviral protein viperin caused by salt. These findings provide further insights into the regulation of proteins involved in the cellular antiviral response.
Article
Chemistry, Physical
Tobias M. Hedison, Andreea I. Iorgu, Donato Calabrese, Derren J. Heyes, Muralidharan Shanmugam, Nigel S. Scrutton
Summary: This study investigates the structural, dynamical, and functional relationship of copper nitrite reductases (CuNiRs) through combining crystallographic techniques and solution-state approaches. The findings shed light on the catalytic mechanisms of these enzymes and suggest the involvement of protein dynamics. The importance of integrating high-resolution crystallographic techniques and low-resolution solution-state approaches in studying metalloenzymes is emphasized.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Multidisciplinary Sciences
Samuel L. Rose, Seiki Baba, Hideo Okumura, Svetlana Antonyuk, Daisuke Sasaki, Tobias M. Hedison, Muralidharan Shanmugam, Derren J. Heyes, Nigel S. Scrutton, Takashi Kumasaka, Takehiko Tosha, Robert R. Eady, Masaki Yamamoto, S. Samar Hasnain
Summary: Redox reactions play a crucial role in substrate binding and utilization in enzyme catalysis. A recent study found that a CuNiR with lower catalytic activity had its catalytic site occupied by water molecules. The study showed that there was less inter-Cu electron transfer in the presence of nitrite, which may explain the lower activity.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Multidisciplinary Sciences
Matthew Russell, Andrew Currin, William Rowe, Guo-Qiang Chen, Perdita Barran, Nigel S. Scrutton
Summary: Despite its environmental benefits, biomanufacturing is not financially competitive compared to the carbon emitting chemical industry. The use of novel organisms, such as halophilic bacteria, can help reduce costs by thriving in environments unsuitable for other organisms. However, the lack of annotation for these organisms requires rapid characterization and data sharing to facilitate their adoption in biomanufacturing.
Article
Biochemistry & Molecular Biology
Andrew M. Stewart, Muralidharan Shanmugam, Roger J. Kutta, Nigel S. Scrutton, Janet E. Lovett, Sam Hay
Summary: This study investigates the conformational changes of calmodulin (CaM) using PELDOR measurements. The results support a three-state conformational model of CaM, including an open apo-state, an extended Ca2+-replete state, and a compact target protein-bound state. Molecular dynamics simulations suggest that the presence of molecular crowding agents affects the stability of different conformational states.
Article
Chemistry, Physical
Joshua N. Whitehead, Nicole G. H. Leferink, Gajendar Komati Reddy, Colin W. Levy, Sam Hay, Eriko Takano, Nigel S. Scrutton
Summary: This study presents the crystal structure of ScCubS and investigates its catalytic mechanism. The findings reveal that specific residues can control the reaction chemistry and product formation, enabling the reengineering of ScCubS. This highlights the importance of mechanistic understanding of cation stabilization in TSs for guiding catalytic outcomes.
Article
Biochemistry & Molecular Biology
April K. Kaneshiro, Prathamesh M. Datar, E. Neil G. Marsh
Summary: This study presents a detailed kinetic analysis of the reaction between FDC catalyst and styrene and phenylacrylic acid, proposing a two-stroke kinetic model in which negative cooperativity plays a crucial role in catalysis. The study also notes the need for further experiments to confirm or refute the proposed mechanism.
Article
Chemistry, Physical
Hanan L. L. Messiha, Nigel S. S. Scrutton, David Leys
Summary: Biosynthetic routes for cost-efficient, eco-friendly, and sustainable production of compounds like styrene are urgently needed. The traditional biosynthesis of styrene from L-phenylalanine via trans-cinnamate is limited by styrene toxicity. This study demonstrates that using an E. coli consortium, whole-cell cascade biotransformation can efficiently convert L-phenylalanine to styrene, avoiding the issue of styrene toxicity and the need for enzyme purification.
Article
Biochemistry & Molecular Biology
Aoife Taylor, Derren J. Heyes, Nigel S. Scrutton
Summary: Photoenzymes utilize light energy to facilitate enzyme catalysis, which is important for the design of man-made photocatalysts. They can be classified into two families based on the nature of the light-sensing chromophores used. Light absorption leads to excited state electron transfer, initiating photocatalysis.
CURRENT OPINION IN STRUCTURAL BIOLOGY
(2022)
Article
Chemistry, Physical
Rhys D. Barker, Yuqi Yu, Leonardo De Maria, Linus O. Johannissen, Nigel S. Scrutton
Summary: In order to rationally engineer flavin-dependent halogenases (FDHs), it is important to understand the reaction mechanism and substrate interactions in the active site. This study presents the most likely mechanism for halogenation based on molecular dynamics simulations and density functional theory cluster models of FDH PrnA.
Article
Biotechnology & Applied Microbiology
Helen Park, Helen S. Toogood, Guo-Qiang Chen, Nigel S. Scrutton
Summary: The engineered strain Halomonas bluephagenesis TD1.0 was able to produce propane, bioplastic PHB, and biochemicals mandelate and hydroxymandelate in a single fermentation process. Multi-product separation was achieved, showcasing the versatility of biotechnology. This achievement further establishes H. bluephagenesis as a valuable platform for industrial biotechnology.
MICROBIAL BIOTECHNOLOGY
(2023)
Editorial Material
Biochemistry & Molecular Biology
Nigel S. S. Scrutton
Summary: The study of enzymes has a long history and continues to advance rapidly. Modern enzymology focuses on understanding the complex relationships between enzyme structures, catalytic mechanisms, and biological function. Topics of interest include the regulation of enzymes at the gene and post-translational levels, as well as how catalytic activity is influenced by interactions with small molecules, macromolecules, and the enzyme environment. Insights from enzymology research have practical applications in diagnostics, pharmaceuticals, and industrial processes. The FEBS Journal seeks to highlight the latest research and provide informative reviews to showcase the breadth and importance of contemporary molecular enzymology research.
Article
Chemistry, Physical
Magnus Speirs, Samantha J. O. Hardman, Andreea I. Iorgu, Linus O. Johannissen, Derren J. Heyes, Nigel S. Scrutton, Igor Sazanovich, Sam Hay
Summary: Recent reports have shown the use of ene-reductase flavoenzymes for non-natural photochemical reactions. These studies have focused on reduced flavoenzymes, but oxidized flavins have better light harvesting properties. In a binary complex of the oxidized ene-reductase with nonreactive nicotinamide coenzyme analogs, visible photoexcitation of flavin mononucleotide leads to electron transfer, but longer-lived excited states may be achieved through enzyme engineering and substrate choice.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Multidisciplinary Sciences
Harshwardhan Poddar, Ronald Rios-Santacruz, Derren J. J. Heyes, Muralidharan Shanmugam, Adam Brookfield, Linus O. O. Johannissen, Colin W. W. Levy, Laura N. N. Jeffreys, Shaowei Zhang, Michiyo Sakuma, Jacques-Philippe Colletier, Sam Hay, Giorgio Schiro, Martin Weik, Nigel S. S. Scrutton, David Leys
Summary: This study provides insights into the mechanism of CarH, a photoreceptor involved in transcriptional regulation. The authors show that the response of CarH to light integrates both B-12 photochemistry and redox changes to drive large-scale conformational changes.
NATURE COMMUNICATIONS
(2023)
Review
Chemistry, Physical
Joshua N. Whitehead, Nicole G. H. Leferink, Linus O. Johannissen, Sam Hay, Nigel S. Scrutton
Summary: This article reviews the important discoveries and advances in terpene synthase/cyclase (TS) biocatalysis, summarizes the recent literature, and explores the future prospects of TS rational design. The article highlights the catalytic motifs in TSs that control product outcome and examines the recent strategies for TS engineering, including machine learning and data-driven approaches. The ultimate goal is to achieve rational and predictive engineering of TSs for designer terpene synthases.
