Article
Chemistry, Multidisciplinary
Beatrice Battistella, Thomas Lohmiller, Beatrice Cula, Peter Hildebrandt, Uwe Kuhlmann, Holger Dau, Stefan Mebs, Kallol Ray
Summary: In class Ib ribonucleotide reductases (RNRs), a dimanganese(II) cluster activates superoxide (O-2(center dot-)) to form a high valent Mn-III-O-2-Mn-IV species responsible for the oxidation of tyrosine. A thiolate-bound dimanganese complex [Mn-2(II)(BPMT)(OAc)(2)](ClO)(4) was synthesized as a biomimetic model for RNRs and proved to be a capable oxidant in aldehyde deformylation and phenol oxidation reactions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Shari L. Meichsner, Yury Kutin, Muge Kasanmascheff
Summary: The study examined the essential radical Y-122 (center dot) in whole cells and found that its structure and distribution are consistent under in vivo and in vitro conditions. Experimental results also indicated a distinct in vivo Y-122 (center dot) per beta 2 distribution, highlighting the key role of Y-center dot concentrations in regulating RNR activity. Furthermore, the successful generation of an unnatural amino acid radical, F3Y122 center dot, in whole cells provides valuable insights into RNR catalysis under physiological conditions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Panagiota Stathi, Evgenia Fotou, Vassilios Moussis, Vassilios Tsikaris, Maria Louloudi, Yiannis Deligiannakis
Summary: This study investigates the formation, lifetime, and redox properties of tyrosyl radicals in hybrid biomimetic materials (HBMs) that consist of tyrosine-containing oligopeptides grafted on SiO2 nanoparticles. The results show that the lifetime of the tyrosyl radical can be enhanced by adjusting factors such as a proximal histidine, the length of the oligopeptide, and the interface with the SiO2 nanomatrix. The E-1/2 of tyrosine radicals is lowered when grafted on SiO2, and the positioning of a histidine at a H-bonding distance from the tyrosine further favors tyrosine radical stabilization.
Article
Cell Biology
Liyuan Wu, Le Yin, Linxiang Ma, Jiarui Yang, Feiya Yang, Baofa Sun, Xing Nianzeng
Summary: High expression of RRM2 is associated with tumor prognosis and immunotherapy. The study reveals that high levels of RRM2 are associated with worse patient survival and immunotherapy effects through pan-cancer analysis and risk score analysis.
Article
Chemistry, Multidisciplinary
Shiny Joseph Srinivasan, Sarah E. Cleary, Miguel A. Ramirez, Holly A. Reeve, Caroline E. Paul, Kylie A. Vincent
Summary: A new activity of the [NiFe] uptake hydrogenase 1 in Escherichia coli (Hyd1) was discovered, allowing direct reduction of the biological flavin cofactors FMN and FAD. The robust nature of Hyd1 was utilized for flavin reduction across a range of temperatures and reaction times, demonstrating potential for regenerating FMNH2 or FADH(2) and supporting asymmetric alkene reductions. High turnover frequencies and total turnover numbers were achieved during flavin recycling, showing the efficiency of this system.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Cell Biology
Yang Gao, Bin Chen, Ruru Wang, An Xu, Lijun Wu, Huayi Lu, Guoping Zhao
Summary: Targeting RRM1 promotes ferroptosis and affects the sensitivity of cancer cells to radiation and chemotherapy. RRM1 disrupts the activity and expression of antioxidant enzyme GPX4, leading to increased accumulation of reactive oxygen species and lipid peroxidation. Furthermore, targeting RRM1 also increases radiation-induced DNA damage and apoptotic signaling, causing crosstalk between ferroptosis and apoptosis.
CELL DEATH DISCOVERY
(2022)
Article
Cell Biology
Junlei Han, Jianping Hu, Fang Sun, Hongzhi Bian, Bingxiang Tang, Xiang Fang
Summary: miR-20a suppresses NSCLC growth by inhibiting the RRM2-mediated PI3K/Akt signaling pathway, serving as a potential tumor suppressor and molecular target for NSCLC treatment.
MOLECULAR AND CELLULAR BIOCHEMISTRY
(2021)
Article
Chemistry, Physical
Muhammad Shafiq Bin Mohd Yusof, Yong Liang Lim, Zhi-Heng Loh
Summary: The study investigates the ultrafast structural reorganization dynamics following the photodetachment of the tyrosinate dianion in aqueous solution using femtosecond optical pump-probe spectroscopy. Vibrational wave packet motion along seven vibrational modes coupled to the photodetachment process is observed, offering insight into the elementary dynamics of ionized biomolecules. This approach may be extended to study the ionization-induced structural rearrangement of other aromatic amino acids and larger biomolecules.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Cell Biology
Qian Liu, Lijuan Guo, Hongyan Qi, Meng Lou, Rui Wang, Boning Hai, Kailun Xu, Lijun Zhu, Yongfeng Ding, Chen Li, Lingdan Xie, Jing Shen, Xueping Xiang, Jimin Shao
Summary: The study revealed a significant correlation between the expression of MYBL2 and RRM2 in colorectal cancer (CRC), with MYBL2 playing a crucial role in CRC cell proliferation, DNA synthesis, and cell cycle progression in an RRM2-dependent manner. MYBL2 was found to directly bind to the promoter of RRM2 gene and promote its transcription during S-phase in collaboration with TAF15 and MuvB components. Combined suppression of MYBL2 and WEE1 was shown to synergistically inhibit CRC growth with low systemic toxicity in vivo, suggesting a potential novel approach for CRC treatment targeting both transcription and degradation machinery of RRM2.
CELL DEATH & DISEASE
(2021)
Article
Chemistry, Multidisciplinary
Magan M. Powell, Guodong Rao, R. David Britt, Jonathan Rittle
Summary: The 2-aminoisobutyric acid hydroxylase from Rhodococcus wratislaviensis requires manganese to functionize a strong, aliphatic C-H bond. Structural and spectroscopic studies reveal a redox-active, heterobimetallic manganese-iron active site at the locus of O-2 activation and substrate coordination. This expands the known reactivity of biological manganese-iron cofactors and suggests the involvement of manganese in oxidative biochemical tasks.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Review
Medicine, Research & Experimental
Yaqiong Zhan, Lushun Jiang, Xuehang Jin, Shuaibing Ying, Zhe Wu, Li Wang, Wei Yu, Jiepeng Tong, Li Zhang, Yan Lou, Yunqing Qiu
Summary: RRM2, the small subunit of ribonucleotide reductase, is commonly overexpressed in chemo-resistant cancer cells, mediating resistance to many chemotherapeutic drugs. Inhibition of RRM2 could enhance the anticancer activity of chemotherapy.
BIOMEDICINE & PHARMACOTHERAPY
(2021)
Article
Multidisciplinary Sciences
Ami Maruyama, Yuzo Sato, Joji Nakayama, Junko Murai, Takamasa Ishikawa, Tomoyoshi Soga, Hideki Makinoshima
Summary: This study demonstrates that RRM1 is essential for the growth of small-cell lung carcinoma cells, with its deletion inducing DNA damage response and reducing the number of cells in S phase cell cycle arrest. Additionally, RRM1 deletion causes overall changes in the metabolic profile of SCLC cells, revealing a potential link between tumor growth and the regulation of deoxyribonucleotide metabolism in SCLC.
SCIENTIFIC REPORTS
(2021)
Article
Oncology
Zhongqiang Qin, Bo Xie, Jingyu Qian, Xiang Ma, Lan Zhang, Jianzhu Wei, Zhaoying Wang, Longfei Fan, Ziyi Zhu, Zhen Qian, Hongxiang Yin, Fangquan Zhu, Yulin Tan
Summary: The study evaluated the importance of ribonucleotide reductase regulatory subunit M2 (RRM2) in hepatocellular carcinoma (HCC) using the Cancer Genome Atlas (TCGA) database. The results showed that RRM2 overexpression was associated with worse prognosis and immune infiltrates in HCC, suggesting that RRM2 may serve as a significant molecular biomarker for HCC diagnosis and prognosis.
FRONTIERS IN ONCOLOGY
(2023)
Article
Chemistry, Inorganic & Nuclear
Glendin Swart, Eleanor Fourie, Jannie C. Swarts
Summary: In this study, a series of phthalocyanine compounds with different functional groups were synthesized, and their spectroscopic and electrochemical properties were investigated.
INORGANIC CHEMISTRY
(2022)
Article
Multidisciplinary Sciences
Bangjie Chen, Tao Jin, Ziyue Fu, Haiwen Li, Junfa Yang, Yucheng Liu, Yanxun Han, Xinyi Wang, Zhengwei Wu, Tao Xu
Summary: Non-thermal plasma (NTP) enhances the anticancer effects of melatonin (MEL) in hepatocellular carcinoma (HCC) cells by promoting apoptosis, delaying cell cycle progression, and inhibiting cell invasion and migration. This mechanism is associated with the regulation of intracellular reactive oxygen species levels and ribonucleotide reductase regulatory subunit M2 expression. The findings highlight the pharmacological role of MEL and the adjuvant value of NTP in the combination therapy for HCC, with important implications for the development of new approaches for treatment.
Article
Physics, Atomic, Molecular & Chemical
Martyna Judd, Greg Jolley, Dieter Suter, Nicholas Cox, Anton Savitsky
Summary: This mechanism provides a robust and efficient way to tune the microwave coupling of a cylindrical EPR cavity, allowing it to adapt to different frequency ranges. By combining the dielectric plate and movable waveguide short, the coupling adjustment of the cavity is achieved in different modes.
APPLIED MAGNETIC RESONANCE
(2022)
Article
Materials Science, Multidisciplinary
Varshini J. Kumar, Jian-Zhong Wu, Martyna Judd, Elodie Rousset, Marcus Korb, Stephen A. Moggach, Nicholas Cox, Paul J. Low
Summary: A series of 6-oxo-verdazyl radicals functionalised at the 1- and 5-positions with tolyl, thioanisole and iodophenyl groups were synthesised using conventional methods. Sonogashira cross-coupling reactions were used for further synthetic elaboration of the verdazyl core structure. The radicals were characterised using various techniques, showing chemically and electrochemically reversible oxidation and reduction properties.
JOURNAL OF MATERIALS CHEMISTRY C
(2022)
Article
Biochemical Research Methods
Takahiro Imanishi, Koji Nishikawa, Midori Taketa, Katsuhiro Higuchi, Hulin Tai, Shun Hirota, Hironobu Hojo, Toru Kawakami, Kiriko Hataguchi, Kayoko Matsumoto, Hideaki Ogata, Yoshiki Higuchi
Summary: This study investigated the binding state of CO with the hydrogenase in Citrobacter sp. S-77 using activity assays, spectroscopic techniques, and X-ray crystallography. The results showed a positive correlation between CO tolerance and oxygen tolerance in [NiFe]-hydrogenases.
ACTA CRYSTALLOGRAPHICA SECTION F-STRUCTURAL BIOLOGY COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Saman Naghibi, Sara Sangtarash, Varshini J. Kumar, Jian-Zhong Wu, Martyna M. Judd, Xiaohang Qiao, Elena Gorenskaia, Simon J. Higgins, Nicholas Cox, Richard J. Nichols, Hatef Sadeghi, Paul J. Low, Andrea Vezzoli
Summary: Integrating radical species into non-cryogenic nanodevices is crucial for molecular electronics. This study successfully fabricates single-molecule devices incorporating a persistent radical and demonstrates the retention of open-shell character at room temperature. Electrochemical gating enables reduction to a closed-shell state, and bias-dependent alignment of open-shell resonances leads to electronically driven rectification.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Multidisciplinary
Sven T. Stripp, Benjamin R. Duffus, Vincent Fourmond, Christophe Leger, Silke Leimkueshler, Shun Hirota, Yilin Hu, Andrew Jasniewski, Hideaki Ogata, Markus W. Ribbe
Summary: Gases like H-2, N-2, CO2, and CO are important feedstock for green energy conversion and as sources of nitrogen and carbon. However, their industrial transformation and production require significant energy input, whereas nature efficiently converts them at ambient conditions using gas-processing metalloenzymes (GPMs). In this review, the importance of the cofactor/protein interface in GPMs is emphasized, and the effects of second and outer coordination sphere on catalytic activity are discussed.
Article
Cultural Studies
Nicholas Cox, Lisa Taylor
Summary: "Divided Britain" is a documentary that explores the tensions in post-Brexit Britain through the perspective of artist-ethnographer Grayson Perry. The documentary provides a space for people from different camps to debate the limitations of the "post-political" formation through discussions of emotional and symbolic differences.
EUROPEAN JOURNAL OF CULTURAL STUDIES
(2023)
Article
Chemistry, Multidisciplinary
Christopher A. Rosengarten, K. Yuvaraj, Li Feng Lim, Nicholas Cox, Cameron Jones
Summary: The study shows that aryl ketones can react with beta diketiminato dimagnesium(I) compounds to form stable magnesium ketyl complexes, which can undergo selective C-C coupling reactions.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Xuying Li, Haoxin Mai, Nicholas Cox, Junlin Lu, Xiaoming Wen, Dehong Chen, Rachel A. Caruso
Summary: The photocatalytic performance of all-inorganic halide perovskites as photocatalysts for selective aromatic C(sp3)-H bond activation can be enhanced by introducing Sb dopant and forming heterointerface and staggered band structure. The developed Sb-substituted Cs2AgBiBr6/g-C3N4 composite exhibits significantly improved visible light photocatalytic toluene oxidation rate with high selectivity. The development of all-inorganic lead-free halide perovskite-based heterostructures for visible light photocatalytic organic transformations is expected to have wide-reaching application.
CHEMISTRY OF MATERIALS
(2023)
Article
Cardiac & Cardiovascular Systems
Samer Noaman, David M. Kaye, Shane Nanayakkara, Anthony M. Dart, Andy S. C. Yong, Martin Ng, Donna Vizi, Stephen J. Duffy, Nicholas Cox, William Chan
Summary: This study aimed to evaluate microcirculatory resistance (MR) and myocardial metabolic adaptations in patients with suspected coronary microvascular dysfunction (CMD) at rest and in response to increased cardiac workload. Microcirculatory assessment and transcardiac blood sampling were conducted during graded exercise with adenosine-mediated hyperaemia in patients with objective ischaemia and/or myocardial injury and non-obstructive coronary artery disease. The results showed that patients with suspected CMD exhibited distinct microcirculatory resistive and myocardial metabolic profiles at rest and in response to exercise.
Article
Nanoscience & Nanotechnology
Shuwen Cheng, Zhehao Sun, Kang Hui Lim, Tianxi Zhang, Emmerson Hondo, Tao Du, Liying Liu, Martyna Judd, Nicholas Cox, Zongyou Yin, Gang Kevin Li, Sibudjing Kawi
Summary: In this study, uniform BiOCl hierarchical nanoflowers with tunable thickness and abundant oxygen vacancies (OVs) were synthesized. The OV-rich BiOCl nanoflower showed a significant increase in photocatalytic conversion of CO2 to CO compared to BiOCl nanosheets. Analysis and calculations revealed the anisotropy in CO2 reduction activity across different crystal facets, and the morphology affected the conduction band and band gap, resulting in a more negative CB edge for BiOCl compared to CO2 reduction potential.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Nipa Chongdar, Patricia Rodriguez-Macia, Edward J. Reijerse, Wolfgang Lubitz, Hideaki Ogata, James A. Birrell
Summary: This study investigates the influence of the protein environment on the catalytic, spectroscopic, and redox properties of [FeFe] hydrogenases. Mutations at the non-conserved serine 267 site resulted in a significant decrease in activity and a lower redox potential for the [4Fe-4S] subcluster. These findings highlight the important role of the secondary coordination sphere in tuning the catalytic properties of [FeFe] hydrogenases.
Article
Chemistry, Multidisciplinary
Takeshi Hiromoto, Koji Nishikawa, Seiya Inoue, Hideaki Ogata, Yuta Hori, Katsuhiro Kusaka, Yu Hirano, Kazuo Kurihara, Yasuteru Shigeta, Taro Tamada, Yoshiki Higuchi
Summary: This study reports that [NiFe]-hydrogenase from Desulfovibrio vulgaris Miyazaki F can recover its catalytic activity by reacting with H2 under anaerobic conditions after being inactivated in the presence of O2. Neutron structure analysis revealed that a part of the Ni ion dissociates from the active site Ni-Fe complex and forms a new square-planar Ni complex, accompanied by rearrangement of the coordinated thiolate ligands. The analysis also found that the Cys17(S) thiolate forms an unusual hydrogen bond with the main-chain amide N atom of Gly19(S), providing insights into the redox reaction of the Fe-S cluster.
Article
Chemistry, Inorganic & Nuclear
Liam M. M. Pascoe, Li Feng Lim, Fabian Kallmeier, Nicholas Cox, Penelope J. J. Brothers, Jamie Hicks
Summary: The redox reaction between a bulky BODIPY and a magnesium(i) reducing agent results in the formal one-electron reduction of the BODIPY, producing a dipyrromethene-centred radical compound that forms dimers via C-C bond formation. On the other hand, reduction with magnesium anthracene leads to the formal two-electron reduction of the BODIPY, leading to the formation of the corresponding anion.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Michael A. Stevens, Li Feng Lim, Le Nhan Pham, Nicholas Cox, Michelle L. Coote, Annie L. Colebatch
Summary: The reaction between the ligand 2,7-bis(6-methyl-2-pyridyl)-1,8-naphthyridine (MeL) and the MnI and MnII precursors resulted in the formation of monometallic and bimetallic manganese complexes. The EPR results showed the magnetic properties of one of the complexes.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Physical
Martyna Judd, Elwy H. Abdelkader, Mian Qi, Jeffrey R. Harmer, Thomas Huber, Adelheid Godt, Anton Savitsky, Gottfried Otting, Nicholas Cox
Summary: This study demonstrates the use of gadolinium ions as paramagnetic tags for measuring longer distances in proteins. Gadolinium ions have greater electronic spin and faster electronic spin-lattice relaxation compared to nitroxide radicals, enhancing the sensitivity of the measurements. The use of trifluoromethyl groups further enhances signal intensity.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
