Article
Biochemistry & Molecular Biology
Eric C. Holmes, Yun-Chu Chen, Mary Beth Mudgett, Elizabeth S. Sattely
Summary: Systemic acquired resistance (SAR) in plants is modulated by the glycosylation of N-hydroxy-pipecolic acid (NHP) and salicylic acid by UGT76B1, enhancing defense responses to bacterial pathogens. The presence of UGT76B1 increases plant resistance to pathogens.
Article
Biochemistry & Molecular Biology
Jinping Yang, Victoria S. Banas, Ketan D. Patel, Gerry S. M. Rivera, Lisa S. Mydy, Andrew M. Gulick, Timothy A. Wencewicz
Summary: Siderophores are metabolites used by microbes to sequester environmental iron. Streptomyces strains produce desferrioxamine (DFO) siderophores, which consist of repeating units of hydroxamate-based desferrioxamine and succinate. In this study, we characterized four DesD orthologs from Streptomyces strains that produce unique DFO siderophores. We synthesized a structural mimic of N-1-hydroxy-N-1-succinyl-cadaverine and obtained crystal structures of DesD in different forms. Our findings suggest that acyl-AMS derivatives can be useful tools to study the mechanism and structure of this family of enzymes.
JOURNAL OF BIOLOGICAL CHEMISTRY
(2022)
Article
Biochemistry & Molecular Biology
Jinping Yang, Victoria S. S. Banas, Gerry S. M. Rivera, Timothy A. A. Wencewicz
Summary: Desferrioxamine siderophores are assembled by the nonribosomal-peptide-synthetase-independent siderophore (NIS) synthetase enzyme DesD via ATP-dependent iterative condensation of three N ( 1 )-hydroxy-N ( 1 )-succinyl-cadaverine (HSC) units. The directionality of desferrioxamine biosynthetic assembly, N-to-C versus C-to-N, is a longstanding knowledge gap that is limiting further progress in understanding the origins of natural products in this structural family. Here, through a chemoenzymatic approach, we establish the N-to-C condensation of HSC units as the mechanism for desferrioxamine biosynthesis.
ACS CHEMICAL BIOLOGY
(2023)
Article
Biochemistry & Molecular Biology
Natalie Krahn, Jingji Zhang, Sergey Melnikov, Jeffery M. Tharp, Alessandra Villa, Armaan Patel, Rebecca J. Howard, Haben Gabir, Trushar R. Patel, Jorg Stetefeld, Joseph Puglisi, Dieter Soll
Summary: Protein translation is achieved through tRNA aminoacylation and ribosomal elongation. This study explores the tRNA identity elements for a Delta pylSn tRNA(Pyl) and identifies five key elements necessary for MaPylRS activity.
NUCLEIC ACIDS RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Lisa Wagner, Theresa Ross, Tim Hollmann, Frank Hahn
Summary: This study demonstrates the immobilization of the PKS domain AmbDH3 as a CLEA, which improved its stability and activity in vitro, leading to high conversion and isolated yield in semi-preparative scale reactions. The results suggest that cross-linking can increase the applicability of this type of enzyme for chemoenzymatic synthesis.
Article
Chemistry, Organic
Ranuka T. Hewage, Rou-Jie Huang, Shu-Jung Lai, Ya-Chu Lien, Shao-Hsing Weng, Dehai Li, Yu-Ju Chen, Shih-Hsiung Wu, Rong-Jie Chein, Hsiao-Ching Lin
Summary: Meleagrin B is a terpene-alkaloid hybrid natural product with the conidiogenone and meleagrin scaffold. Derivatives of Meleagrin B show diverse biological activities, with compound 6 demonstrating stronger antibacterial effects against Staphylococcus aureus strains compared to compound 1.
Article
Chemistry, Medicinal
Thanapon Charoenwongpaiboon, Methus Klaewkla, Pimchai Chaiyen, Chanakan Tongsook
Summary: 8-Demethyl-8-dimethylaminoriboflavin (RoF) is a natural riboflavin analogue with potent antibiotic properties. Catalyzed by N,N-8-Demethyl-8-aminoriboflavin dimethyltransferase (RosA), RoF is synthesized through a consecutive dimethylation reaction of 8-demethyl-8-aminoriboflavin (AF). Molecular dynamics simulations revealed mechanistic insights into RoF synthesis by RosA, suggesting the role of substrate positioning and ligand binding in the reaction.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2023)
Article
Biochemistry & Molecular Biology
Lennart Mohnike, Dmitrij Rekhter, Weijie Huang, Kirstin Feussner, Hainan Tian, Cornelia Herrfurth, Yuelin Zhang, Ivo Feussner
Summary: The study identified UGT76B1 as a key protein regulating plant immune response by modifying NHP structure to balance plant growth and defense. Accumulation of NHP in ugt76b1 mutant plants leads to enhanced disease resistance, highlighting the importance of NHP metabolism in plant immunity.
Article
Biochemistry & Molecular Biology
Anh Duc Tran, Kyoungwon Cho, Oksoo Han
Summary: OsPXG9 is a peroxygenase involved in the oxidative stress response in plants. It catalyzes the 12- or 15-epoxidation of fatty acids in rice cells, modulating the level of lipid peroxides to enhance defense against abiotic and biotic stressors.
BIOORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Elizabeth Parkinson, Hani G. Lakkis, Amir A. Alwali, Mary Elizabeth M. Metcalf, Ramya Modi, William W. Metcalf
Summary: The biosynthesis of dehydrofosmidomycin involves a unique transformation catalyzed by the enzyme DfmD, which rearranges, desaturates, and demethylates 2-(trimethylamino)ethylphosphonate. By characterizing the products of in vitro reactions, it is discovered that DfmD performs this transformation in two steps, yielding methyldehydrofosmidomycin.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Hayama Tsutsumi, Yoshitaka Moriwaki, Tohru Terada, Kentaro Shimizu, Kazuo Shin-ya, Yohei Katsuyama, Yasuo Ohnishi
Summary: In this study, we characterized the geranyl pyrophosphate C6-methyltransferase BezA and investigated the molecular basis of its catalytic mechanisms using multiple strategies. The results revealed the important role of E170 as a catalytic base in completing the methylation reaction. Additionally, we successfully altered the substrate specificity by introducing a W210A substitution, resulting in a novel farnesyl pyrophosphate C6-methyltransferase.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Biochemistry & Molecular Biology
Eike Schafer, Paula S. Seibold, Stefan Bartram, Felix Trottmann, Veit G. Haensch, Markus Gressler, Andrew R. Chadeayne, Christian Hertweck, Sarah E. O'Connor, Dirk Hoffmeister
Summary: This study identified several compounds present in various Psilocybe species, including cubebol, β-copaene, δ-cadinene, and germacrene D, through fluorescence staining and transgenic techniques. The results also revealed the presence of related enzymes encoded by CubA in multiple Psilocybe species.
Article
Chemistry, Physical
Hannes Frohnmeyer, Simon Rueben, Lothar Elling
Summary: Two processes for the gram-scale production of GDP-Fuc using multi-enzyme cascades were established in this study. The enzyme modules were optimized and scaled up to achieve high yields and production rates. Furthermore, a product purification protocol was developed to remove free phosphates from the product solution.
Article
Chemistry, Multidisciplinary
Yusuke Shikai, Seiji Kawai, Yohei Katsuyama, Yasuo Ohnishi
Summary: In this study, the biosynthetic pathway of azaserine, a natural product with anticancer activity, was investigated. The putative azaserine biosynthetic gene cluster was discovered using bioinformatics analysis, and azaserine was successfully produced by heterologous expression of the gene cluster. The study also identified key amino acid residues involved in the synthesis of azaserine.
Article
Plant Sciences
Zonghao Yue, Yanjuan Chen, Yifan Wang, Limin Zheng, Qiaoyang Zhang, Yongchuang Liu, Chunhong Hu, Can Chen, Keshi Ma, Zhongke Sun
Summary: This study investigated the effect of the endophytic strain Bacillus altitudinis WR10 on wheat salt tolerance and its potential mechanisms. The results showed that WR10 improved wheat salt tolerance at the seedling stage by upregulating certain gene expressions and regulating salt accumulation. These findings provide supporting evidence for the application of WR10 in salinized soil.
FRONTIERS IN PLANT SCIENCE
(2022)
Article
Biotechnology & Applied Microbiology
Daniel Zabala, Lijiang Song, Yousef Dashti, Gregory L. Challis, Jose Salas, Carmen Mendez
MICROBIAL CELL FACTORIES
(2020)
Article
Multidisciplinary Sciences
Alice M. Banks, Lijiang Song, Gregory L. Challis, Andy M. Bailey, Gary D. Foster
Article
Microbiology
Paul G. Becher, Vasiliki Verschut, Maureen J. Bibb, Matthew J. Bush, Bela P. Molnar, Elisabeth Barane, Mahmoud M. Al-Bassam, Govind Chandra, Lijiang Songs, Gregory L. Challis, Mark J. Buttner, Klas Flardh
NATURE MICROBIOLOGY
(2020)
Article
Chemistry, Multidisciplinary
Yousef Dashti, Ioanna T. Nakou, Alex J. Mullins, Gordon Webster, Xinyun Jian, Eshwar Mahenthiralingam, Gregory L. Challis
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2020)
Article
Chemistry, Multidisciplinary
Ioanna T. Nakou, Matthew Jenner, Yousef Dashti, Isolda Romero-Canelon, Joleen Masschelein, Eshwar Mahenthiralingam, Gregory L. Challis
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2020)
Article
Chemistry, Multidisciplinary
Savvas Louka, Sarah M. Barry, Derren J. Heyes, M. Qadri E. Mubarak, Hafiz Saqib Ali, Lona M. Alkhalaf, Andrew W. Munro, Nigel S. Scrutton, Gregory L. Challis, Sam P. de Visser
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Genetics & Heredity
Cerith Jones, Gordon Webster, Alex J. Mullins, Matthew Jenner, Matthew J. Bull, Yousef Dashti, Theodore Spilker, Julian Parkhill, Thomas R. Connor, John J. LiPuma, Gregory L. Challis, Eshwar Mahenthiralingam
Summary: Burkholderia gladioli is a diverse bacterium with significant ecological impacts on humans, animals, and plants, spanning diseases and beneficial interactions. Through exploring its genomic diversity and metabolic potential, it has shed light on its roles as a plant pathogen, food poisoning agent, and lung pathogen for CF patients. This research has identified potential therapeutic strategies to minimize poisoning risks associated with this bacterium.
MICROBIAL GENOMICS
(2021)
Review
Biotechnology & Applied Microbiology
Helen G. Smith, Matthew J. Beech, Jozef R. Lewandowski, Gregory L. Challis, Matthew Jenner
Summary: PKS and NRPS multienzymes produce valuable metabolites, with protein subunits requiring ordered self-assembly for correct organisation of catalytic domains. DDs at the N- and C-termini of each subunit interact in complementary pairs to facilitate substrate transfer and pathway fidelity. efforts to engineer biosynthetic pathways have focused on utilizing DDs.
JOURNAL OF INDUSTRIAL MICROBIOLOGY & BIOTECHNOLOGY
(2021)
Article
Multidisciplinary Sciences
Shanshan Zhou, Hussain Bhukya, Nicolas Malet, Peter J. Harrison, Dean Rea, Matthew J. Belousoff, Hariprasad Venugopal, Paulina K. Sydor, Kathryn M. Styles, Lijiang Song, Max J. Cryle, Lona M. Alkhalaf, Vilmos Fulop, Gregory L. Challis, Christophe Corre
Summary: Actinobacteria produce antibiotics and hormones with important applications in medicine and agriculture. Hormones control the production of metabolites by binding TFTRs, but the molecular basis for this process remains unclear. This study elucidates the structural basis for hormone recognition and the mechanism for DNA release upon hormone binding, providing insights into the role of individual amino acid residues and hormone functional groups in ligand recognition and DNA release.
Article
Biochemistry & Molecular Biology
Rakesh Saroay, Gheorghe-Doru Roiban, Lona M. Alkhalaf, Gregory L. Challis
Summary: The variant R59C of TxtE has a broader substrate scope, allowing it to nitrate a range of tryptamine analogues. This presents a new direction for developing TxtE into a useful aromatic nitration biocatalyst.
Article
Multidisciplinary Sciences
Thierry Izore, Y. T. Candace Ho, Joe A. Kaczmarski, Athina Gavriilidou, Ka Ho Chow, David L. Steer, Robert J. A. Goode, Ralf B. Schittenhelm, Julien Tailhades, Manuela Tosin, Gregory L. Challis, Elizabeth H. Krenske, Nadine Ziemert, Colin J. Jackson, Max J. Cryle
Summary: Non-ribosomal peptide synthetases (NRPSs) are essential for assembling complex natural products, with condensation domains playing a central role in chain assembly. Structural snapshots of a condensation domain bound to an aminoacyl-PCP substrate reveal a mechanism for controlling substrate access and tuning selectivity, without requiring a distinct pocket for side chain selection during peptide assembly.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Organic
Jieyan Lim, Venkaiah Chintalapudi, Haraldur G. Gudmundsson, Minh Tran, Alice Bernasconi, Araceli Blanco, Lijiang Song, Gregory L. Challis, Edward A. Anderson
Summary: Stambomycins are bioactive macrolides isolated from Streptomyces ambofaciens, with their stereochemistry predicted by sequence analysis of the polyketide synthase. The synthesis of the C1-C27 fragment of stambomycin D matched well with the natural product's spectroscopic data, confirming the effectiveness of predictive sequence analysis in stereochemical assignment of complex polyketide natural products.
Article
Microbiology
Alex J. Mullins, Jinlian Zhao, Gordon Webster, Hak Joong Kim, Yoana D. Petrova, Christina E. Ramming, Matthew Jenner, James A. H. Murray, Thomas R. Connor, Christian Hertweck, Gregory L. Challis, Eshwar Mahenthiralingam
Summary: The study revealed the widespread distribution of natural products with alkyne and polyyne moieties in bacteria, with their biosynthetic gene clusters showing evolutionary connections. Through genomic and phylogenetic analyses, the diversity and biosynthetic logic of polyyne were explored, providing insights into discovering new natural products and enhancing the understanding of polyyne synthesis.
Article
Chemistry, Organic
Yongchen Wang, Venkaiah Chintalapudi, Haraldur G. Gudmundsson, Gregory L. Challis, Edward A. Anderson
Summary: The stereochemical assignment of macrolide antibiotics stambomycins A-D was based on sequence analysis of the associated polyketide synthase, except for two stereocentres at C28 and C50. The synthesis of two C50 diastereomers of the C33-C51 region of the stambomycins confirms the PKS-based configurational assignment and establishes a strategy for accessing the extended stambomycin framework.
ORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Biochemistry & Molecular Biology
Christian Hobson, Matthew Jenner, Xinyun Jian, Daniel Griffiths, Douglas M. Roberts, Matias Rey-Carrizo, Gregory L. Challis
Summary: This study reports the discovery of a new variant of a dehydratase domain that eliminates two molecules of water in sequential steps during polyketide chain assembly, leading to the introduction of a conjugated E,Z-diene. These findings expand the catalytic versatility of modular PKSs and highlight the role of a conserved histidine residue in the reaction.
NATURE CHEMICAL BIOLOGY
(2022)
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)
