Review
Chemistry, Organic
Saumitra Sengupta, Srihari Pabbaraja, Goverdhan Mehta
Summary: Recursive Anionic Cyclization (RAC) is a mechanistically distinct domino strategy that continues to grow. By using nitroalkanes as a source of recursive carbanions, it has created a unique operating space for generating molecular complexity and diversity. The recursive nitronate cyclization, based on a domino [5 C+1 C] cyclization strategy, allows rapid access to densely functionalized carbo- and heterocycles with multiple chiral centers and regio-, stereo- and enantioselectivity. Extension to aromatic domains, particularly through benzannulation reactions, has further expanded the operating space. The functional versatility of nitro group has also been leveraged for post-domino modifications, leading to total synthesis of various natural products.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Engineering, Environmental
Zhiping Ye, Guanjie Wang, Jean-marc Giraudon, Anton Nikiforov, Jun Chen, Liang Zhao, Xiuwen Zhang, Jiade Wang
Summary: The study found that the different crystal phases have a significant impact on the Cu-Mn catalytic ozonation of toluene, with the amorphous phase Cu0.2MnOx showing better catalytic performance.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Biochemistry & Molecular Biology
Ravikumar Reddi, Kimberly Matulef, Erika Riederer, Pierre Moenne-Loccoz, Francis Valiyaveetil
Summary: Regulation of ion conduction through the pore of a K+ channel involves coordinated action of the activation gate and inactivation gate, with the W67F mutant of the KcsA channel showing reduced inactivation and enhanced activation rate. Structural studies provide insights into the allosteric pathway and highlight the importance of ion occupancy at the S2 site for channel inactivation.
JOURNAL OF MOLECULAR BIOLOGY
(2021)
Article
Chemistry, Physical
Jianghao Zhou, Jing Guo, Alexander Moiseevich Mebel, Govinda Ghimire, Feng Liang, Shuai Chang, Jin He
Summary: Investigated the dehydration reaction of primary amides in visible-light driven self-assembled gold nanoparticle-aromatic primary amide-gold nanoelectrode junctions. Used time-resolved surface enhanced Raman spectroscopy (SERS) to study the reaction dynamics and intermediates, revealing the role of gold surface adatoms and picocavities in stabilizing and amplifying the intermediates.
Review
Chemistry, Physical
Young Hyun Hong, Yong-Min Lee, Wonwoo Nam, Shunichi Fukuzumi
Summary: This review provides an overview of the functional model reactions of photosystem II (PSII) and photosystem I (PSI) for photocatalytic water oxidation and reduction, respectively. The roles of high-valent metal-oxo, -hydroperoxo,-peroxo, and-superoxo complexes as reaction intermediates in photocatalytic water oxidation are discussed, as well as the catalytic mechanisms of water oxidation. The roles of metal hydride complexes in hydrogen evolution and NAD+ reduction to NADH are also explored. The aim is to construct molecular artificial photosynthetic systems that can split water into H2 and O2 in a 2:1 ratio, thus achieving artificial photosynthesis at the molecular level.
Review
Chemistry, Physical
Young Hyun Hong, Yong-Min Lee, Wonwoo Nam, Shunichi Fukuzumi
Summary: Water oxidation in photosystem II (PSII) is catalyzed by Mn4Ca clusters in the oxygen-evolving complex (OEC), involving a manganese(V)oxo species as an active reaction intermediate. Photogenerated charge separation in the PSII photosynthetic reaction center is used to reduce plastoquinone to plastoquinol. In photosystem I (PSI), plastoquinol reduces NADP+ to NADPH via photogenerated charge separation, which serves as a reductant for CO2 reduction in the Calvin cycle. Extensive research has been conducted to mimic PSII and PSI for photocatalytic water oxidation and reduction, with a focus on high-valent metal-oxo, -hydroperoxo, -peroxo, and -superoxo intermediates and metal hydride complexes.
Article
Chemistry, Multidisciplinary
Yao-Hui Wang, Xiao-Ting Wang, Huajie Ze, Xia-Guang Zhang, Petar M. Radjenovic, Yue-Jiao Zhang, Jin-Chao Dong, Zhong-Qun Tian, Jian-Feng Li
Summary: This study investigated the hydrogen oxidation reaction (HOR) mechanisms in alkaline conditions on PtNi alloy and Pt surfaces using in situ electrochemical surface-enhanced Raman spectroscopy (SERS) and DFT. The results showed that Ni doping promoted hydroxy adsorption on the platinum-alloy surface, enhancing the HOR activity. Designing bifunctional catalysts to tune OH adsorption could be an efficient method for improving HOR activity in anion-exchange-membrane fuel cells.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Biochemistry & Molecular Biology
Melissa Carrillo, Suraj Pandey, Juan Sanchez, Moraima Noda, Ishwor Poudyal, Luis Aldama, Tek Narsingh Malla, Elin Claesson, Weixiao Yuan Wahlgren, Denisse Feliz, Vukica Srajer, Michal Maj, Leticia Castillon, So Iwata, Eriko Nango, Rie Tanaka, Tomoyuki Tanaka, Luo Fangjia, Kensuke Tono, Shigeki Owada, Sebastian Westenhoff, Emina A. Stojkovic, Marius Schmidt
Summary: This study presents short-lived crystal structures of the photosensory core modules of bacteriophytochrome, capturing the structural changes after light illumination, revealing the mechanism of signal transduction. The results demonstrate with atomic precision how the signal progresses from the chromophore to the entire protein.
Article
Chemistry, Multidisciplinary
Gabriele Hierlmeier, Paolo Tosatti, Kurt Puentener, Paul J. J. Chirik
Summary: This study reports a new molybdenum ligand for catalyzing the hydrogenation of benzene, which is formed by the coordination of phosphino(imino)pyridine and cyclooctadiene. The experimental results indicate that the ligand can selectively generate cyclohexane catalyst in the presence of benzene, and the formation of the insertion product is a key step.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Heather O. LeClerc, Rasha Atwi, Sydney F. Niles, Amy M. McKenna, Michael T. Timko, Richard H. West, Andrew R. Teixeira
Summary: Hydrothermal liquefaction (HTL) is a promising strategy for converting organic waste into energy-dense biocrude. This study investigates the distribution and reaction pathways of nitrogen in different hydrothermal products generated from food waste. The results suggest that the Maillard reaction is the dominant pathway for converting reactive nitrogen intermediates into observed products.
Article
Multidisciplinary Sciences
Fangzhu Han, Yiqi Hu, Mengchen Wu, Zhaoxiang He, Hongtao Tian, Long Zhou
Summary: "Tetrahymena thermophila possesses tubular mitochondria with highly divergent electron transport chain composed of four transmembrane protein complexes (I-IV). We report the cryo-EM structures of megacomplexes IV2+(I+III2+II)(2) and (IV2+I+III2+II)(2), revealing their half ring-shaped architecture and their role in maintaining mitochondrial cristae curvature and cytochrome c binding sites proximity. This expands our understanding of eukaryotic electron transport chain organization and its relationship with mitochondrial morphology."
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Hashem Amini, Nancy Weisbach, Sebastien Gauthier, Helene Kuhn, Nattamai Bhuvanesh, Frank Hampel, Joseph H. Reibenspies, John A. Gladysz
Summary: The conversion of silylated hexatriynyl complex into various length polyynes through cross coupling with diynes was studied, yielding a series of C-C bonded products. Crystallographic characterization was used to analyze the structural and spectroscopic properties, revealing different structures and phases in the products.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Multidisciplinary Sciences
Long Zhou, Maria Maldonado, Abhilash Padavannil, Fei Guo, James A. Letts
Summary: This study reveals the functional and structural diversity of eukaryotic respiration through investigating the respiratory chain of the ciliate Tetrahymena thermophila. It expands our understanding of core metabolism by identifying divergence in key components of eukaryotic respiration.
Article
Chemistry, Multidisciplinary
Marcelo Augusto Pereira Januario, Demetrius P. de Souza, Julio Zukerman-Schpector, Arlene G. Correa
Summary: Highly functionalized indole derivatives were synthesized via Rh(III)-catalyzed C-2 alkylation with nitroolefins. A total of 23 examples were prepared under optimized conditions with yields ranging from 39% to 80%. Furthermore, the nitro compounds were reduced and subjected to the Ugi four-component reaction, resulting in a series of new indole-peptidomimetics with moderate to good overall yields.
Article
Chemistry, Multidisciplinary
Tian Huang, Bo Li, Huan Wang, Steve Granick
Summary: This paper focuses on studying the absolute diffusion coefficient during the CuAAC reaction, observing time-dependent diffusion enhancements for some intermediate molecular species and decreases for those whose size increases due to complex formation. The findings suggest that the conventional Stokes-Einstein equation fails to fully explain diffusivity during chemical reactions, highlighting aspects of the physics of chemical reactions that are not completely understood. The systematic data presented in the study can be used to evaluate hypotheses in the field.
Editorial Material
Biology
Allen M. Orville
Article
Biochemical Research Methods
Jonathan M. Grimes, David R. Hall, Alun W. Ashton, Gwyndaf Evans, Robin L. Owen, Armin Wagner, Katherine E. McAuley, Frank von Delft, Allen M. Orville, Thomas Sorensen, Martin A. Walsh, Helen M. Ginn, David I. Stuart
ACTA CRYSTALLOGRAPHICA SECTION D-STRUCTURAL BIOLOGY
(2018)
Article
Instruments & Instrumentation
Bradley Davy, Danny Axford, John H. Beale, Agata Butryn, Peter Docker, Ali Ebrahim, Gabriel Leen, Allen M. Orville, Robin L. Owen, Pierre Aller
JOURNAL OF SYNCHROTRON RADIATION
(2019)
Article
Biochemistry & Molecular Biology
Agata Butryn, Hadeeqa Raza, Heather Rada, Isabel Moraes, Raymond J. Owens, Allen M. Orville
Article
Multidisciplinary Sciences
E. Sethe Burgie, Jonathan A. Clinger, Mitchell D. Miller, Aaron S. Brewster, Pierre Aller, Agata Butryn, Franklin D. Fuller, Sheraz Gul, Iris D. Young, Cindy C. Pham, In-Sik Kim, Asmit Bhowmick, Lee J. O'Riordan, Kyle D. Sutherlin, Joshua V. Heinemann, Alexander Batyuk, Roberto Alonso-Mori, Mark S. Hunter, Jason E. Koglin, Junko Yano, Vittal K. Yachandra, Nicholas K. Sauter, Aina E. Cohen, Jan Kern, Allen M. Orville, George N. Phillips, Richard D. Vierstra
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2020)
Article
Multidisciplinary Sciences
Mohamed Ibrahim, Thomas Fransson, Ruchira Chatterjee, Mun Hon Cheah, Rana Hussein, Louise Lassalle, Kyle D. Sutherlin, Iris D. Young, Franklin D. Fuller, Sheraz Gul, In-Sik Kim, Philipp S. Simon, Casper de Lichtenberg, Petko Chernev, Isabel Bogacz, Cindy C. Pham, Allen M. Orville, Nicholas Saichek, Trent Northen, Alexander Batyuk, Sergio Carbajo, Roberto Alonso-Mori, Kensuke Tono, Shigeki Owada, Asmit Bhowmick, Robert Bolotovsky, Derek Mendez, Nigel W. Moriarty, James M. Holton, Holger Dobbek, Aaron S. Brewster, Paul D. Adams, Nicholas K. Sauter, Uwe Bergmann, Athina Zouni, Johannes Messinger, Jan Kern, Vittal K. Yachandra, Junko Yano
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2020)
Article
Chemistry, Multidisciplinary
Vivek Srinivas, Rahul Banerjee, Hugo Lebrette, Jason C. Jones, Oskar Aurelius, In-Sik Kim, Cindy C. Pham, Sheraz Gul, Kyle D. Sutherlin, Asmit Bhowmick, Juliane John, Esra Bozkurt, Thomas Fransson, Pierre Aller, Agata Butryn, Isabel Bogacz, Philipp Simon, Stephen Keable, Alexander Britz, Kensuke Tono, Kyung Sook Kim, Sang-Youn Park, Sang Jae Lee, Jaehyun Park, Roberto Alonso-Mori, Franklin D. Fuller, Alexander Batyuk, Aaron S. Brewster, Uwe Bergmann, Nicholas K. Sauter, Allen M. Orville, Vittal K. Yachandra, Junko Yano, John D. Lipscomb, Jan Kern, Martin Hogbom
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Biochemical Research Methods
Joshua M. Lawrence, Julien Orlans, Gwyndaf Evans, Allen M. Orville, James Foadi, Pierre Aller
ACTA CRYSTALLOGRAPHICA SECTION D-STRUCTURAL BIOLOGY
(2020)
Article
Chemistry, Multidisciplinary
Patrick Rabe, John H. Beale, Agata Butryn, Pierre Aller, Anna Dirr, Pauline A. Lang, Danny N. Axford, Stephen B. Carr, Thomas M. Leissing, Michael A. McDonough, Bradley Davy, Ali Ebrahim, Julien Orlans, Selina L. S. Storm, Allen M. Orville, Christopher J. Schofield, Robin L. Owen
Article
Biochemistry & Molecular Biology
Allen M. Orville
CURRENT OPINION IN STRUCTURAL BIOLOGY
(2020)
Article
Chemistry, Medicinal
Anka Lucic, Philip Hinchliffe, Tika R. Malla, Catherine L. Tooke, Jurgen Brem, Karina Calvopina, Christopher T. Lohans, Patrick Rabe, Michael A. McDonough, Timothy Armistead, Allen M. Orville, James Spencer, Christopher J. Schofield
Summary: Penems have shown potential as antibacterials and beta-lactamase inhibitors, but their clinical use is limited compared to carbapenems. Faropenem, with a C-2 tetrahydrofuran ring, is resistant to some beta-lactamases. Studies on reactions of faropenem with beta-lactamases demonstrate different outcomes, suggesting further research is needed for optimizing the interactions between penems and beta-lactamases.
EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
(2021)
Article
Biochemistry & Molecular Biology
Julien Orlans, Carole Vincent-Monegat, Isabelle Rahioui, Catherine Sivignon, Agata Butryn, Laurent Soulere, Anna Zaidman-Remy, Allen M. Orville, Abdelaziz Heddi, Pierre Aller, Pedro Da Silva
Summary: The study analyzed the activity of different isoforms of Drosophila PGRP-LB towards various PGN substrates and elucidated the mechanism of amidase activity through site directed mutagenesis and X-ray structure determination. The findings suggest a dynamic role of residue Y78 in the amidase mechanism by nucleophilic attack through a water molecule to the carbonyl group of the amide function destabilized by Zn2+.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2021)
Article
Multidisciplinary Sciences
Agata Butryn, Philipp S. Simon, Pierre Aller, Philip Hinchliffe, Ramzi N. Massad, Gabriel Leen, Catherine L. Tooke, Isabel Bogacz, In-Sik Kim, Asmit Bhowmick, Aaron S. Brewster, Nicholas E. Devenish, Jurgen Brem, Jos J. A. G. Kamps, Pauline A. Lang, Patrick Rabe, Danny Axford, John H. Beale, Bradley Davy, Ali Ebrahim, Julien Orlans, Selina L. S. Storm, Tiankun Zhou, Shigeki Owada, Rie Tanaka, Kensuke Tono, Gwyndaf Evans, Robin L. Owen, Frances A. Houle, Nicholas K. Sauter, Christopher J. Schofield, James Spencer, Vittal K. Yachandra, Junko Yano, Jan F. Kern, Allen M. Orville
Summary: Serial femtosecond crystallography has provided new opportunities for studying protein dynamics with high resolution. However, the challenge lies in studying enzyme-catalyzed reactions. A drop-on-drop sample delivery system has been proposed in this study, showing potential for widespread application in studying enzyme reactions in crystallography.
NATURE COMMUNICATIONS
(2021)
Article
Multidisciplinary Sciences
Patrick Rabe, Jos J. A. G. Kamps, Kyle D. Sutherlin, James D. S. Linyard, Pierre Aller, Cindy C. Pham, Hiroki Makita, Ian Clifton, Michael A. McDonough, Thomas M. Leissing, Denis Shutin, Pauline A. Lang, Agata Butryn, Jurgen Brem, Sheraz Gul, Franklin D. Fuller, In-Sik Kim, Mun Hon Cheah, Thomas Fransson, Asmit Bhowmick, Iris D. Young, Lee O'Riordan, Aaron S. Brewster, Ilaria Pettinati, Margaret Doyle, Yasumasa Joti, Shigeki Owada, Kensuke Tono, Alexander Batyuk, Mark S. Hunter, Roberto Alonso-Mori, Uwe Bergmann, Robin L. Owen, Nicholas K. Sauter, Timothy D. W. Claridge, Carol V. Robinson, Vittal K. Yachandra, Junko Yano, Jan F. Kern, Allen M. Orville, Christopher J. Schofield
Summary: IPNS catalyzes the reaction between ACV and dioxygen to produce IPN, revealing the importance of protein dynamics in regulating intermediate conformations. This study also has implications for catalysis by multiple IPNS-related oxygenases.
Article
Chemistry, Medicinal
Lennart Brewitz, Jos J. A. G. Kamps, Petra Lukacik, Claire Strain-Damerell, Yilin Zhao, Anthony Tumber, Tika R. Malla, Allen M. Orville, Martin A. Walsh, Christopher J. Schofield
Summary: This study reports a mass spectrometry-based assay for monitoring the catalysis of SARS-CoV-2 papain-like protease (PLpro). The results show that the potencies of some reported PLpro inhibitors differ substantially from those obtained using fluorescence-based assays. Some M-pro inhibitors also show inhibitory effects on PLpro. The MS-based assay provides a useful tool for validating inhibitor potencies, especially for those operating by non-covalent mechanisms.