Review
Biochemistry & Molecular Biology
Naoki Shibata, Tetsuo Toraya
Summary: Adenosylcobalamin (AdoCbl), or coenzyme B-12, is a naturally occurring organometallic compound that serves as a cofactor for enzymes that catalyze intramolecular group-transfer reactions and ribonucleotide reduction in a wide variety of organisms. Recent structural studies have revealed the importance of steric strain of the Co-C bond and conformational stabilization of the adenosyl radical in coenzyme B-12 catalysis. These findings provide insights into how enzymes activate and cleave the Co-C bond and utilize the reactivity of the adenosyl radical for catalysis.
Article
Microbiology
Kristopher J. Kennedy, Florian J. Widner, Olga M. Sokolovskaya, Lina Innocent, Rebecca R. Procknow, Kenny C. Mok, Michiko E. Taga
Summary: In bacteria, riboswitches are gene regulatory RNAs that directly bind and detect metabolites, controlling many essential metabolic processes. Cobalamin riboswitches are an exception as they can respond to multiple variants of cobalamin (vitamin B-12), known as corrinoids. This study found that cobalamin riboswitches vary in their specificity for corrinoids, with some being broadly responsive and others being more selective. Analyses and models suggest that cobalamin riboswitches indirectly differentiate among corrinoids by sensing differences in their structural conformation. These findings provide insights into how bacteria can sense and respond to the chemical diversity of essential metabolites.
Article
Chemistry, Inorganic & Nuclear
Laura D. Elmendorf, Thomas C. Brunold
Summary: Understanding the reactivities of cobalamins requires knowledge of their geometric and electronic structures. In this study, the ORCA_ASA computational tool was used with B3LYP and BP86 functionals to predict Abs bandshapes and rR spectra for vitamin B-12. The ORCA_ASA/B3LYP-computed Abs envelope and rR spectra were in good agreement with experimental data, while BP86 failed to reproduce them. This finding is important for understanding the different modeling of electronic properties by these density functionals.
INORGANIC CHEMISTRY
(2023)
Article
Green & Sustainable Science & Technology
Lei Li, Qilei Yang, Bin Wang, Dong Wang, Yue Peng, Junhua Li, John Crittenden
Summary: The study presents a simple and efficient strategy for preparing supported metal (oxide) nanoparticle catalysts with high loading and small nanoparticle size. The synthesized catalyst shows superior performance compared to traditional methods, attributed to the strong size-dependent effect and interaction between cobalt oxides and supports. This preparation strategy opens up a new pathway for highly loaded and dispersed supported heterogeneous catalysts.
JOURNAL OF CLEANER PRODUCTION
(2021)
Article
Engineering, Environmental
Tao Li, Bing Ding, Victor Malgras, Jongbeom Na, Zongyi Qin, Xiangjun Lu, Yoshio Bando, Hiroki Nara, Zeid A. Alothman, Jie Wang, Yusuke Yamauchi
Summary: In this study, hollow-structured mesoporous carbon (HOMC) nanoplates were successfully synthesized using a self-template method, with Fe-doped HOMC (Fe/HOMC) exhibiting higher electrocatalytic activity, efficiency, durability, and tolerance to methanol poisoning compared to traditional Pt/C benchmark. The Fe/HOMC also showed promising application in Zn-air batteries with high power densities and excellent cycling stability, demonstrating a new avenue for the design of ordered mesoporous materials with hollow structure.
CHEMICAL ENGINEERING JOURNAL
(2021)
Review
Biochemistry & Molecular Biology
Katarzyna Wozniak, Krzysztof Brzezinski
Summary: Most naturally occurring nucleotides and nucleosides are N-glycosyl derivatives of fi-Dribose, which play essential roles in genetic information storage, flow, and cellular catalysis. The unique chemical and structural features of these compounds make them versatile building blocks for life processes. Their universal function in encoding genetic information and cellular catalysis strongly suggests their essential role in the origins and evolution of life. This review summarizes the role of N-ribosides in biological systems, focusing on the origin of life and the reasons behind the preference for derivatives of beta-D-ribofuranose.
Article
Biochemistry & Molecular Biology
Megan J. Toda, Piotr Lodowski, Abdullah Al Mamun, Pawel M. Kozlowski
Summary: Hydridocobalamin (HCbl) is a member of the B-12 family of molecules with limited knowledge about its electronic and photolytic properties. Recent interest in HCbl has been driven by experiments proposing its role as an intermediary in the photoreaction of coenzyme B-12-dependent photoreceptor CarH. HCbl is a transient species with variable oxidation states and high instability.
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY B-BIOLOGY
(2021)
Article
Chemistry, Inorganic & Nuclear
Xiaobo Chen, Yefei Zhuang
Summary: In this study, a unique bimetallic phosphide, NiCoP, with a hollow microcube structure, was synthesized and demonstrated as an excellent electrode material for supercapacitors, showing high capacity, superior cycling performance, and high specific energy.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Inorganic & Nuclear
Mads Sondrup Moller, Jacob Kongsted, Christine J. McKenzie
Summary: This study discusses the coupling of selective C-H activation with O-2 activation in organic synthesis, highlighting the connection between O-2 activation and C-H activation by classic Co(salen) complexes and the mechanism of forming various complexes. DFT calculations demonstrate the participation of different intermediates in hydrogen atom transfer reactions, with the reaction conditions and solvent substrates properties determining the reaction pathways.
DALTON TRANSACTIONS
(2021)
Article
Materials Science, Ceramics
Liwen He, Chen Lin, Yican Zhao, Wenhai Gao, Hailian Zhang, Bizhou Lin, Dongya Sun
Summary: A novel 3D network morphology Co3O4@C composite was successfully fabricated, showing excellent capacitance and durability. An asymmetric supercapacitor consisting of DF-2 and active carbon also exhibited high energy density and stability. These outstanding performances are attributed to the unique structure and properties of the carbon skeleton.
CERAMICS INTERNATIONAL
(2022)
Article
Engineering, Environmental
Long Zheng, Yiqiang Wu, Xingong Li, Yingfeng Zuo
Summary: By constructing a molecular topological structure in the composite system, the deep cross fusion of heterogeneous interfaces has been achieved in traditional inorganic composites, endowing them with unique properties such as lightweight ultrastrong, thermal insulation, shock absorption, and fire resistance.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Yan Cheng, Juhui Gong, Bo Cao, Xuan Xu, Peng Jing, Baocang Liu, Rui Gao, Jun Zhang
Summary: An innovative strategy was developed in this paper to construct a well-aligned nitrogen-doped carbon nanotube array electrode integrated with multiple electrocatalytically active components for the hydrogen evolution reaction. Through various characterizations and density functional theory calculations, it was found that synergistic coupling interactions exist among NCNTs, CoSAs, Co, and MC, contributing to the enhanced HER performance.
Article
Chemistry, Multidisciplinary
Jia Zhang, Songyi Li, Huayi Fang
Summary: The reactive HO/(Salophen(t-Bu))Co(ii) radical pair is generated through homolysis of the terminal Co(iii)-OH bond in transient (Salophen(t-Bu))(L)Co(iii)(OH) complexes, as confirmed by UV-Vis and EPR measurements. This elementary process enables C-H bond activations in acetone, 2-butanone, acetonitrile, and benzene under ambient conditions. The products obtained from the reactions of the first three substrates are alkylcobalt(iii) complexes.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Shuai Cao, Yong Li, Yijian Tang, Yangyang Sun, Wenting Li, Xiaotian Guo, Feiyu Yang, Guangxun Zhang, Huijie Zhou, Zheng Liu, Qing Li, Mohsen Shakouri, Huan Pang
Summary: In this study, various metal ions with different valence states were successfully confined in quasi-microcube shaped cobalt benzimidazole frameworks using a space-confined synthesis strategy. The derived carbon materials from high-temperature pyrolysis showed electric double-layer and pseudocapacitance properties due to the presence of metal ions with different valence states. The materials containing Ti ions exhibited enhanced insertion/extraction of Na+ and had a high desalination capacity in capacitive deionization applications.
ADVANCED MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Zhenyu Xie, Ting Zhang, Zhongkui Zhao
Summary: Efficiently increasing the dispersity of metal nanoparticles on supported catalysts is crucial for enhancing catalytic performance. In this work, a carbon interlayer sacrificial strategy was developed to prepare supported Ni NP catalysts with high dispersity, leading to superior catalytic properties for chemoselective hydrogenation reactions.
ACS APPLIED NANO MATERIALS
(2021)
Article
Biochemistry & Molecular Biology
Greg J. Dodge, Danialle Ronnow, Richard E. Taylor, Janet L. Smith
ACS CHEMICAL BIOLOGY
(2018)
Review
Biochemistry & Molecular Biology
Greg J. Dodge, Finn P. Maloney, Janet L. Smith
NATURAL PRODUCT REPORTS
(2018)
Article
Multidisciplinary Sciences
Greg J. Dodge, Ashay Patel, Kara L. Jaremko, J. Andrew McCammon, Janet L. Smith, Michael D. Burkart
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2019)
Article
Clinical Neurology
Jesse J. Corry, Bridget Ho, Emily Marino, Aditi Gupta, Jaya Ravichandran, Michael A. Sperl, Megan E. Tipps
CLINICAL NEUROLOGY AND NEUROSURGERY
(2019)
Article
Multidisciplinary Sciences
Markus Ruetz, Gregory C. Campanello, Meredith Purchal, Hongying Shen, Liam McDevitt, Harsha Gouda, Shoko Wakabayashi, Junhao Zhu, Eric J. Rubin, Kurt Warncke, Vamsi K. Mootha, Markos Koutmos, Ruma Banerjee
Review
Chemistry, Multidisciplinary
Ruma Banerjee, Harsha Gouda, Shubhadra Pillay
Summary: Metals, particularly cobalamins like Vitamin B-12, play a crucial role in the functioning of enzymes in the human body. Genetic studies on cobalamin metabolism disorders have identified key genetic loci and pathways. Understanding the intricate chemistry and coordination involved in B-12 trafficking can provide insights into potential therapeutic interventions for related disorders.
ACCOUNTS OF CHEMICAL RESEARCH
(2021)
Article
Biochemistry & Molecular Biology
Sebastian Carballal, Victor Vitvitsky, Roshan Kumar, David A. Hanna, Marouane Libiad, Aditi Gupta, Jace W. Jones, Ruma Banerjee
Summary: This study demonstrates that H2S increases lipid synthesis in cells by affecting mitochondrial NAD(P)H pools and enabling reductive carboxylation of alpha-ketoglutarate. H2S also leads to time-dependent changes in various lipid classes, upregulating triglycerides while downregulating phosphatidylcholine.
JOURNAL OF BIOLOGICAL CHEMISTRY
(2021)
Article
Biochemistry & Molecular Biology
Harsha Gouda, Romila Mascarenhas, Shubhadra Pillay, Markus Ruetz, Markos Koutmos, Ruma Banerjee
Summary: Human ATP:cob(I)alamin adenosyltransferase (ATR) is responsible for catalyzing adenosyl transfer to cob(I)alamin, generating AdoCbl or coenzyme B-12. Mutations in ATR can lead to metabolic disorders. Characterization of patient mutations R190C/H and E193K in ATR revealed weakened affinities for substrates and products, with E193K potentially responding better to cobalamin therapy due to spared catalytic activity.
JOURNAL OF BIOLOGICAL CHEMISTRY
(2021)
Article
Multidisciplinary Sciences
Harsha Gouda, Romila Mascarenhas, Markus Ruetz, Madeline Yaw, Ruma Banerjee
Summary: This study identifies an unconventional strategy for controlling metal redox state by using bivalent molecular mimicry with ADP to protect against cob(II)alamin overoxidation. ADP induces a conformational change that seals off solvent access, exerting control over the metal oxidation state. This research reveals the importance of metabolites in preserving and recycling a rare, essential metal cofactor.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Biochemistry & Molecular Biology
Alyssa J. J. Anderson, Greg J. J. Dodge, Karen N. N. Allen, Barbara Imperiali
Summary: In this study, the C-terminus of a prototypic monoPGT was structurally characterized for the first time, revealing that 19 C-terminal residues play a significant structural role in a subset of monoPGTs. This new structural information enabled the identification of co-conserved sequence fingerprints that predict NDP-sugar substrate specificity for this subset of monoPGTs. A Hidden Markov model was generated to assign the substrate of previously unannotated monoPGTs accurately.
Article
Multidisciplinary Sciences
Romila Mascarenhas, Markus Ruetz, Harsha Gouda, Natalie Heitman, Madeline Yaw, Ruma Banerjee
Summary: G-proteins and their cofactors MMAA and MMAB orchestrate cofactor translocation and repair in B-12-dependent human MMUT, and their crystal structure reveals a dramatic conformational change and the basis of GTPase activation. Disease-causing mutations at the MMAA-MMUT interfaces are explained by the structure.
NATURE COMMUNICATIONS
(2023)
Article
Clinical Neurology
Ganesh Asaithambi, Amy L. Castle, Michael A. Sperl, Ayashree Ravichandran, Aditi Gupta, Bridget M. Ho, Sandra K. Hanson