Article
Chemistry, Physical
Wei Peng, Xiaoyang Qu, Sason Shaik, Binju Wang
Summary: This study deciphers the catalytic cycle of pMMO in the presence of the physiological reductant duroquinol (DQH(2)), revealing that O-2 activation is initiated by the Cu-C(ii)-DQH(-) species. The research also uncovers the important roles of the phenol co-substrate for O-2 activation.
Review
Chemistry, Multidisciplinary
Sangyong Shin, Robert Haaring, Jungseob So, Yunji Choi, Hyunjoo Lee
Summary: Single-atom catalysts (SACs), single-atom alloys (SAAs), and ensemble catalysts are heterogeneous atomic catalysts with intentionally controlled surface metal atomic structures. These catalysts have received significant attention for their ability to fully utilize precious metals and induce unique surface reactions. However, durability and stability are crucial factors that need to be considered for practical applications. The properties of the support material and the susceptibility to impurities can significantly affect the performance of these catalysts. High durability heterogeneous atomic catalysts have great potential for sustainable chemical production.
ACCOUNTS OF CHEMICAL RESEARCH
(2022)
Article
Multidisciplinary Sciences
Ioannis Kipouros, Agnieszka Stanczak, Jake W. Ginsbach, Prokopis C. Andrikopoulos, Lubomir Rulsek, Edward I. Solomon
Summary: Melanins are important biopolymer pigments that provide photoprotection, and their biosynthesis involves the catalytic role of tyrosinase (Ty). This study combines spectroscopic, kinetic, and computational methods to investigate the mechanism of the rate-limiting step in melanin biosynthesis. The results provide insights into the O-2 activation and reactivity by the active sites of coupled binuclear copper, with implications in biocatalysis.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Inorganic & Nuclear
Jianhui Xie, Bing Li, Huijing Liu, Yijun Li, Jian-Bo He, Yanzhen Zheng, Kai-Chung Lau, Tai-Chu Lau
Summary: The study investigated the kinetics and mechanisms of ferrate oxidation on 4-alkylbenzenesulfonates using UV/Vis spectrophotometry. The results indicated that [Fe(O)(3)(OH)](-) is two orders of magnitude more reactive than [FeO4](2-) and is the predominant oxidant in neutral and slightly alkaline solutions. Additionally, a hydrogen atom transfer (HAT) mechanism was proposed for the reactions between [Fe(O)(3)(OH)](-) and 4-alkylbenzenesulfonates.
DALTON TRANSACTIONS
(2021)
Article
Chemistry, Physical
Zhenzhuo Lan, Jacob Toney, Shaama Mallikarjun Sharada
Summary: This study computationally investigates the mechanism and active site identification of methane hydroxylation by monocopper complexes. The results suggest that the oxyl species is the likely active site, and spin crossing may provide a lower energy pathway for hydroxylation.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Review
Biotechnology & Applied Microbiology
Noemi Poma, Andrea Bonini, Federico Vivaldi, Denise Biagini, Mariagrazia Di Luca, Daria Bottai, Fabio Di Francesco, Arianna Tavanti
Summary: Climate change due to increased greenhouse gas emissions has had a significant impact on the sustainability of life on Earth. Methane, a greenhouse gas, is increasing in concentration and its measurement is important for the environment and safety. The use of methane-oxidizing bacteria in biosensing systems shows promise for methane quantification and monitoring.
APPLIED MICROBIOLOGY AND BIOTECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Florian Leisinger, Dzmitry A. Miarzlou, Florian P. Seebeck
Summary: Molecular oxygen is a sustainable oxidation reagent with strong oxidizing properties and stability, ultimately forming water as the reaction product. The activation of O-2 can occur through various pathways, with enzymes typically forming metal-oxygen coordination complexes to facilitate the process. The formylglycine generating enzyme (FGE) demonstrates a unique strategy for activating O-2, involving binding of O-2 near, but not coordinated to, its catalytic copper atom.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Review
Chemistry, Multidisciplinary
Rahul Banerjee, John D. Lipscomb
Summary: Rigorous substrate selectivity in enzyme catalysis is attributed to the favorable process of substrate binding to the enzyme active site based on complementary physiochemical characteristics. However, this selectivity becomes more difficult to rationalize for diminutive molecules with too narrow a range of physical characteristics.
ACCOUNTS OF CHEMICAL RESEARCH
(2021)
Article
Ecology
Olivia E. Mosley, Emilie Gios, Murray Close, Louise Weaver, Chris Daughney, Kim M. Handley
Summary: The nitrogen cycle plays a crucial role in aquatic ecosystems, including the subsurface. However, the diversity of nitrogen transformations in these environments is not well understood. This study investigated how nitrogen cycling microorganisms respond to different groundwater chemistries. The results showed that regardless of site-specific conditions, nitrogen cycling mechanisms were prevalent and highly redundant in groundwater communities. The study also revealed the presence of oxic-anoxic interfaces and potential synergistic interactions between microorganisms at these interfaces. The findings provide insights into cooperative relationships in groundwater communities and the complexity of metabolic mechanisms leading to nitrogen loss.
Article
Engineering, Environmental
Hyesung Lee, Choah Kwon, Changjoon Keum, Hee-Eun Kim, Hyunjoo Lee, Byungchan Han, Sang-Yup Lee
Summary: Inspired by the active site of particulate methane monooxygenase (pMMO), a copper-doped zeolitic imidazolate framework-7 (Cu/ZIF-7) was synthesized and showed catalytic activity in converting methane to various products without overoxidation.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Jingjing Dai, Hongbo Zhang
Summary: This study systematically investigates the C-H bond activation mechanism on Pt/MgO catalyst with O-2, O-H2O, and CO2. It is found that dry reforming of CH4 (DRM) exhibits weaker activity compared to reforming or partial oxidation of CH4. Pressure dependence shows that CO has negligible effect, suggesting the involvement of CO2 in CH4 activation as a whole molecule. The reaction between adsorbed CH4 and CO2 to form formate and methyl species is kinetically relevant. Experimental results confirm that both CO2 and CH4 derivatives are the most abundant surface intermediates.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Anna Zanina, Vita A. Kondratenko, Henrik Lund, Jianshu Li, Juan Chen, Yuming Li, Guiyuan Jiang, Evgenii Kondratenko
Summary: This study shows that MnOx-Na2WO4/SiO2 is not the necessary catalyst to achieve high selectivity in the oxidative coupling of methane. Experimental results reveal that M2WO4/SiO2 materials perform similarly to MnOx-Na2WO4/SiO2 in terms of selectivity and conversion. An alternative concept is proposed, suggesting that the activity and product selectivity of M2WO4/SiO2 are determined by the interaction between lattice oxygen of M2WO4 and adsorbed oxygen species from the gas phase.
Article
Microbiology
Hidehiro Ito, Kosei Yoshimori, Masahito Ishikawa, Katsutoshi Hori, Toshiaki Kamachi
Summary: In this study, a methanol production system was established using methanotroph mutants to control the expression of methanol dehydrogenase (MDH), allowing for methanol accumulation. By modulating the metal ion composition, the conditions for cell growth inhibition and methanol accumulation were repeatedly alternated, showcasing the potential for efficient conversion of methane to methanol.
FRONTIERS IN MICROBIOLOGY
(2021)
Article
Chemistry, Multidisciplinary
Julia Kratky, Daniel Eggerichs, Thomas Heine, Sarah Hofmann, Philipp Sowa, Renato H. Weisse, Dirk Tischler, Norbert Straeter
Summary: This study presents the crystal structure of VpIndA1, an indole monooxygenase from bacterium Variovorax paradoxus EPS, and reveals the structural basis of substrate binding and stereoselectivity through substrate complex structures and force-field calculations. By redesigning the substrate cavity based on the structural information, variants with new substrate selectivity and greatly enhanced stereoselectivity were successfully generated. This research opens up new possibilities for structure-based design of these powerful biocatalysts.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Jinping Tang, Li Song, Han Xie, Jinyu Zhu, Wei Li, Guangyang Xu, Linjun Cai, Xiao Xia Han
Summary: The study demonstrates the potential of SERRS for monitoring the interaction between mitochondria and endoplasmic reticula in apoptosis. SERRS allows for label-free, in situ, and real-time monitoring of ROS formation and cytochrome c release, providing a novel strategy for cancer treatment.
Article
Multidisciplinary Sciences
Rahul Banerjee, Yegor Proshlyakov, John D. Lipscomb, Denis A. Proshlyakov
Article
Chemistry, Multidisciplinary
Rebeca G. Castillo, Rahul Banerjee, Caleb J. Allpress, Gregory T. Rohde, Eckhard Bill, Lawrence Que, John D. Lipscomb, Serena DeBeer
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2017)
Article
Chemistry, Multidisciplinary
Williamson N. Oloo, Rahul Banerjee, John D. Lipscomb, Lawrence Que
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2017)
Article
Biochemistry & Molecular Biology
Rahul Banerjee, Katlyn K. Meier, Eckard Muenck, John D. Lipscomb
Article
Chemistry, Multidisciplinary
George E. Cutsail, Rahul Banerjee, Ang Zhou, Lawrence Que, John D. Lipscomb, Serena DeBeer
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2018)
Article
Biochemistry & Molecular Biology
Jason C. Jones, Rahul Banerjee, Ke Shi, Hideki Aihara, John D. Lipscomb
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)
Review
Chemistry, Multidisciplinary
Rahul Banerjee, John D. Lipscomb
Summary: Rigorous substrate selectivity in enzyme catalysis is attributed to the favorable process of substrate binding to the enzyme active site based on complementary physiochemical characteristics. However, this selectivity becomes more difficult to rationalize for diminutive molecules with too narrow a range of physical characteristics.
ACCOUNTS OF CHEMICAL RESEARCH
(2021)
Article
Biochemistry & Molecular Biology
Jason C. Jones, Rahul Banerjee, Ke Shi, Manny M. Semonis, Hideki Aihara, William C. K. Pomerantz, John D. Lipscomb
Summary: This study investigates the interactions between MMOR and MMOB with sMMOH by specific modifications and F-19 NMR technology. The findings suggest a new regulatory model for the methane conversion cycle, where MMOR and MMOB competitively bind to sMMOH with similar affinity, allowing the transient formation of reactive complexes to advance the reaction cycle.
Article
Chemistry, Multidisciplinary
Ariel Benjamin Jacobs, Rahul Banerjee, Dory Ellen Deweese, Augustin Braun, Jeffrey Thomas Babicz, Leland Bruce Gee, Kyle David Sutherlin, Lars Hendrik Bottger, Yoshitaka Yoda, Makina Saito, Shinji Kitao, Yasuhiro Kobayashi, Makoto Seto, Kenji Tamasaku, John D. Lipscomb, Kiyoung Park, Edward Solomon
Summary: Methanotrophic bacteria use soluble methane monooxygenase to convert methane to methanol, with controversy surrounding the geometric and electronic structure of the intermediate Q. Studies using nuclear resonance vibrational spectroscopy reveal decay of Q during experiments, with closed core models reproducing the acquired data.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Biotechnology & Applied Microbiology
Paul B. Hatzinger, Rahul Banerjee, Rachael Rezes, Sheryl H. Streger, Kevin McClay, Charles E. Schaefer
