Article
Chemistry, Multidisciplinary
Pinar Tunay Tasli, Tugba Soganci, Sevgi Ozdemir Kart, Hasan Huseyin Kart, Metin Ak
Summary: The study investigates the relationship between the structure and electronic properties of conjugated polymers through quantum mechanical calculations, providing a connection between the calculated electronic properties of monomers and the observed optical and electrical properties of their conjugated polymers. By synthesizing compounds with varying numbers of electroactive groups and optimizing their molecular structures using Density Functional Theory, the electronic properties of the monomeric structures and reactive regions on the molecule surfaces have been determined. Analysis of Total Density of State, Partial Density of State, and Mulliken charge has been performed to compare the ab-initio calculations of monomers with the optical and electrical properties of their conductive polymers.
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
(2021)
Article
Chemistry, Inorganic & Nuclear
Marc Schnierle, Mario Winkler, Vasileios Filippou, Joris van Slageren, Mark R. Ringenberg
Summary: The electrochemistry and spectroelectrochemistry of three [ReCl(CO)(3)(N N)] complexes were investigated with N N=3-(pyrid-2-yl)-1,2,4,5-tetrazine [1], 3-(pyrid-2-yl)-4-ferrocenyl-4,5-dihydropyridazine [1H(2)Fc], and 3-(pyrid-2-yl)-4-ferrocenyl-pyridazine [1Fc]. The conjugation of the ligands was found to affect the reduction potentials and intramolecular charge transfers observed in the UV-vis-NIR spectrum, with support from DFT calculations.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2022)
Review
Pharmacology & Pharmacy
Anh Thu Nguyen, Hee-Kwon Kim
Summary: Hypoxia, a common feature of solid tumors, can induce many cancer characteristics and is associated with metastases and resistance to therapy. Non-invasive imaging methods using hypoxia-targeting radiopharmaceuticals have been used for tumor hypoxia detection and therapy. Nitroimidazoles, which can selectively bind to intracellular macromolecules under hypoxic conditions, have been the focus of PET and SPECT radiotracer development for imaging and treatment of hypoxic tumors. This review summarizes the development of novel PET and SPECT radiotracers containing nitroimidazoles, including their physicochemical properties, cellular uptake values, biodistribution, and imaging results.
Review
Biochemistry & Molecular Biology
Anh Thu Nguyen, Hee-Kwon Kim
Summary: Positron emission tomography (PET) is a noninvasive molecular imaging method widely used in the detection and treatment of various diseases. Hypoxia, a common phenomenon in solid tumors, can be detected using radiopharmaceuticals containing nitroimidazole. Gallium-68, a positron-emitting radioisotope, has been developed as a convenient radiotracer for PET imaging of hypoxic tumors. This review provides a comprehensive overview of the development of Ga-68-labeled radiopharmaceuticals with nitroimidazole moieties for the diagnosis of hypoxia.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Review
Biochemistry & Molecular Biology
Sweety Mittal, Madhava B. Mallia
Summary: Although evidence supporting dose escalation based on molecular level images of hypoxic tumor sub-volumes is increasing, the concept still requires validation. Molecular imaging of tumor hypoxia using radiopharmaceuticals is crucial for planning Image Guided Radiation Therapy (IGRT) to target radioresistant hypoxic tumor cells. The available literature on radiopharmaceuticals for imaging hypoxia is biased towards nitroimidazole, given their ability to undergo oxygen dependent reduction in hypoxic cells. A review on nitroimidazole radiopharmaceuticals would greatly benefit researchers in understanding the current achievements and exploring new approaches for better hypoxia imaging agents.
BIOORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Yong-Sok Lee, Zhongyu Mou, Ana Christina L. Opina, Olga Vasalatiy
Summary: The study investigated the geometries, energetics, and electrostatic potentials of Lu complexes with various DOTA-based chelates to understand the origin of isomer stability. It was found that electrostatic and steric repulsions play key roles in destabilizing certain isomers, and potential energy barriers for inter-conversion via arm rotation were also calculated. The possibility of designing better chelates for Ln(3+) ions for molecular medicine was discussed.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Tomasz Koczorowski, Jacek Kujawski, Weronika Porolnik, Jaroslaw Piskorz
Summary: Four boron-dipyrromethene derivatives (BODIPYs) with iodine substitution were studied for their electrochemical properties. The iodine substitution resulted in an increase in the number of redox pairs and a decrease in the energy band gap, indicating potential application as semiconductors. Electrolysis confirmed the formation of anion radicals of BODIPYs. DFT studies supported the decrease in the HOMO-LUMO energy band gap caused by halide atom insertion.
JOURNAL OF MOLECULAR STRUCTURE
(2023)
Article
Multidisciplinary Sciences
Yuzhu Zhou, Quan Zhou, Hengjie Liu, Wenjie Xu, Zhouxin Wang, Sicong Qiao, Honghe Ding, Dongliang Chen, Junfa Zhu, Zeming Qi, Xiaojun Wu, Qun He, Li Song
Summary: Developing efficient electrocatalysts for selective CO2 conversion is important. In this study, the authors demonstrate that a Ni single-atom catalyst coordinated with pyrrolic nitrogen and pyridinic nitrogen efficiently converts CO2 to CO. The catalyst shows high CO partial current density and turnover frequency, as well as excellent Faradaic efficiency of CO. The study also provides insights into the origin of the catalyst's catalytic activity.
NATURE COMMUNICATIONS
(2023)
Article
Materials Science, Multidisciplinary
Worasak Sukkabot
Summary: This study analyzes the effects of substituted VIB transition metals on In2O3 semiconductor properties, finding that W doping is the most stable structure and all transition metals transform semiconducting behavior to metallic behavior. The d orbitals of transition metals play a dominant role in the conduction bands, and VIB transition-metal dopants cause a red shift in the absorption spectra.
PHILOSOPHICAL MAGAZINE
(2021)
Review
Chemistry, Physical
Tommaso Salzillo, Andrea Marchetti, Jana Vejpravova, Pablo Fanjul Bolado, Claudio Fontanesi
Summary: This work summarizes the state-of-the-art results achieved by synergistically combining the outcomes obtained from electrochemical, spectroscopic, and theoretical methods. Several selected case studies are presented, where this synergistic approach allows for a comprehensive understanding of complex experimental systems. Finally, the importance of integrating experimental and theoretical approaches in solid-state electrochemistry, an area at the forefront of novel concepts in solid-state electronics, is highlighted.
CURRENT OPINION IN ELECTROCHEMISTRY
(2022)
Article
Nuclear Science & Technology
Masashi Kaneko, Yuji Sasaki, Masahiko Matsumiya, Masahiko Nakase, Kenji Takeshita
Summary: Density-functional theory calculations were used to model the molecular structure and complex formation reactions of metal ion complexes with DTPA and DTPABA chelates, revealing that Am3+ forms more stable complexes with both chelates than Eu3+. The higher selectivity of Am3+ over Eu3+ is attributed to the larger bond overlap between the Am3+ 5 f-orbital and N 2s, 2p-orbital, leading to differences in complex formation stabilities. This study may help in understanding the origin of metal ion selectivity and in exploring novel ligands.
JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY
(2021)
Article
Chemistry, Analytical
Yuan Fang, Ren Hu, Song-Yuan Ding, Zhong-Qun Tian
Summary: In-situ electrochemical infrared (EC-IR) and Raman (EC-Raman) spectroscopies are powerful tools for characterizing electrochemical interfacial structures. However, the interpretation of the observed EC-IR and Raman spectra can be challenging due to the complex nature of electrochemical interfaces. By combining vibrational spectra simulations with electrochemical interface models, a computational method has been developed to quantitatively simulate these spectra and can be expanded to study more complicated materials and interface structures.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Yumin Yang, Shuang Feng, Jianan Su, Yutong Gong, Junjie Wang
Summary: The effects of modification strategies on the activation of nitrogen molecules and the electrocatalytic nitrogen reduction reaction (eNRR) were systematically studied. It was found that Mo(II)-Fe2(DOAnBDC) and Mo(II)-Fe2F2(BBTA) are potential high-performance eNRR electrocatalysts, with their activity related to the arrangement of molybdenum's d orbitals and charge transfer.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Physical
Ya-Wei Zhou, Ya-Feng Chen, Kun Jiang, Zhen Liu, Zi-Jie Mao, Wei-Yi Zhang, Wen-Feng Lin, Wen-Bin Cai
Summary: The study employs Pt-SnO2 nanoflakes as a catalyst, where the electronic structure manipulation favors the selective enhancement of the non-CO pathway for electrochemical methanol oxidation reaction.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Multidisciplinary
Marcos A. S. Francisco, Felipe Fantuzzi, Thiago M. Cardozo, Pierre M. Esteves, Bernd Engels, Ricardo R. Oliveira
Summary: This study discusses the design principles and computational investigation of new organometallic platforms containing stable manganese-manganese bonds. The analysis focuses on the metal-carbene interaction and auxiliary coordination to generate short metal-metal bonds, closed-shell singlet multiplicities, and positive singlet-triplet energy gaps. The research identifies two classes of viable synthetic targets with thoroughly investigated electrostructural properties.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Editorial Material
Chemistry, Inorganic & Nuclear
Jennifer C. Green
Summary: The evolution of the Covalent Bond Classification as a pedagogical tool for classifying an element's chemistry is described in this passage.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Medicinal
Amaury Guillou, Eda Nisli, Simon Klingler, Anthony Linden, Jason P. Holland
Summary: Fluorescent protein conjugates are important tools in scientific research, and the synthesis of photoactivatable fluorophores provides a potential approach for protein labeling and imaging.
JOURNAL OF MEDICINAL CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Monica de Simone, Marcello Coreno, Roberta Totani, Nicolas E. Capra, Louis Messerle, Jennifer C. Green, Alfred P. Sattelberger
Summary: The valence electronic structures of two dinuclear alkyl compounds containing sigma(2)pi(4) triple bonds between group 6 metals have been investigated using a combination of molecular orbital theory and variable photon energy photoelectron spectroscopy. The orbital energy pattern confirms a D-3d M2C6 skeleton, with higher orbital energies for W compared to Mo. Spin-orbit splitting in the pi ionization of W-2(CH2CMe3)(6) has been resolved and modeled successfully, showing variations in Mo-Mo pi and sigma levels as a function of the ligand set.
Article
Multidisciplinary Sciences
Simon Klingler, Jason P. Holland
Summary: This study introduces a fully automated synthesis box for the production of Zr-89-radiolabeled antibodies. The automated method eliminates the need for manual synthesis and improves the yield and purity of the radiolabeled antibodies. This will benefit the Nuclear Medicine and research institutions in accessing state-of-the-art Zr-89-radiolabeled antibodies.
SCIENTIFIC REPORTS
(2022)
Article
Chemistry, Physical
Rachel Roberts, Robin Orr, Ian Mein, Alex Paddon, Jonathan Cheesewright, Ruth Edge
Summary: Pathogenic bacteria, even at low levels in natural water systems, can be a threat to human health if conditions are favorable for growth and aerosol creation. This study demonstrates that γ radiation can effectively eliminate Legionella pneumophila and Pseudomonas aeruginosa. The approximate D-10 values for these bacteria are 166.3 Gy and 70.9 Gy, respectively.
RADIATION PHYSICS AND CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Faustine d'Orchymont, Jason P. Holland
Summary: We synthesized and characterized bimodal mechanically interlocked rotaxane-based imaging agents using the cucurbit[6]uril CB[6]-mediated alkyne-azide 'click' reaction. Two synthetic routes involving four- or six-component reactions were developed to access asymmetric rotaxanes. A peptide-based rotaxane targeted toward the clinical prostate cancer biomarker, prostate-specific membrane antigen (PSMA), was synthesized with Ga-68-radiometal ion complex for positron emission tomography and fluorescein as an optically active imaging agent. The results showed the feasibility of using an asymmetric rotaxane platform to produce dual-modality imaging agents specifically targeting prostate cancer cells.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Ina Hierlmeier, Amaury Guillou, Daniel F. Earley, Anthony Linden, Jason P. Holland, Mark D. Bartholomae
Summary: In this study, we synthesized and investigated the coordination chemistry of novel copper(II) and zinc(II) complexes using two heterocyclic triazacyclononane(tacn)-based chelators (HNODThia and NODThia-AcNHEt). The modified chelator HNODThia was used to develop a PSMA-based bioconjugate (NODThia-PSMA) and a photoactivatable azamacrocyclic analogue (NODThia-PEG ( 3 ) -ArN ( 3 )) for copper-64 radiopharmaceuticals. The metal-binding chelates showed rapid radiolabeling, stability in human plasma, and successful photoconjugation to albumin and antibodies. These findings have significant implications for the development of stable Cu-64-based radiopharmaceuticals and the future application of Cu-67 in targeted radioimmunotherapy.
INORGANIC CHEMISTRY
(2023)
Article
Agriculture, Dairy & Animal Science
Lavinia E. Chiti, Brian Park, Faustine d'Orchymont, Jason P. Holland, Mirja C. Nolff
Summary: The use of near-infrared fluorophores has promising applications in surgical oncology. The performance of dedicated camera systems is affected by the lighting condition of the operating theatre. LED and halogen lights have a detrimental effect on the diagnostic performances of the camera systems. Surgeons should evaluate the spectral contribution of the lights when implementing fluorescence-guided surgery (FGS) into the clinical routine.
Article
Biochemistry & Molecular Biology
Melanie Gut, Birgit Dreier, Sven Furler, Jens Sobek, Andreas Pluckthun, Jason P. Holland
Summary: Late-stage prostate cancer often becomes resistant to standard chemotherapy and transforms into a hormone-resistant, drug-resistant, and incurable disease. Developing non-invasive tools to detect biochemical changes that indicate drug efficacy and identify drug resistance could have significant implications in managing individual patients' treatment plans. In this study, new Designed Ankyrin Repeat Proteins (DARPins) with high affinity for prostate-specific antigen (PSA) were selected using ribosome display and in vitro screening tools. These PSAbinding DARPins showed nanomolar affinity for PSA and could be radiolabeled for potential use in imaging-based monitoring of androgen receptor (AR)-targeted therapies.
RSC CHEMICAL BIOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Faustine D'Orchymont, Jason P. Holland
Summary: In this study, a unique rotaxane-antibody conjugate was developed for PET imaging and quantification of specific tumor receptors. The experimental results showed that the rotaxane-radiotracer has improved pharmacokinetic properties and reduced radiation exposure to critical organs.
Article
Chemistry, Inorganic & Nuclear
Joel C. Mather, Jessica A. Wyllie, Alex Hamilton, Tatiana P. Soares da Costa, Peter J. Barnard
Summary: A series of gold(I) and silver(I) complexes were synthesized and their antibacterial activities were tested. The gold(I) complexes showed good activity against Gram-positive bacteria, with the complexes of the 1,2,4-triazolylidene ligands being more active. The silver(I) complexes exhibited good antibacterial activity against Acinetobacter baumannii. High levels of antibacterial activity were observed against multi-drug resistant bacterial strains for both the gold(I) and silver(I) complexes. Resistance to these metal-containing complexes was less likely to develop compared to the widely used broad-spectrum antibiotic. Furthermore, the stability of these complexes was investigated, revealing possible decomposition reactions for silver complexes in aqueous solution.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Inorganic & Nuclear
Amaury Guillou, Ali Ouadi, Jason P. Holland
Summary: In this study, the synthesis of bifunctional heptadentate metal ion binding chelates derived from DFO linked to a tripeptide unit was reported. The chelates were functionalised with a photoactivatable aryl azide unit for light-triggered labelling of proteins. The results showed that the chelates had good radiolabelling efficiency with zirconium-89 and exhibited high stability in the presence of different competitors. PET imaging and biodistribution studies further confirmed the pharmacokinetic profile and tumor binding of the chelates in nude mice bearing human gastric cancer xenografts.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Multidisciplinary
Daniel F. Earley, Amaury Guillou, Simon Klingler, Rachael Fay, Melanie Gut, Faustine d'Orchymont, Shamisa Behmaneshfar, Linus Reichert, Jason P. Holland
Summary: This study reports on the light-triggered synthesis of human serum albumin using a series of photoactivatable DFO derivatives. The findings demonstrate that photochemistry is a viable option for making diverse, functionalized protein conjugates.
Article
Chemistry, Inorganic & Nuclear
Nuchareenat Wiratpruk, Guneet K. Bindra, Alex Hamilton, Mark D. Hulett, Peter J. Barnard
Summary: A family of rhenium(i) tricarbonyl complexes with pyridyl-imidazolylidene or bis-imidazolylidene ligands in combination with a series of N-acetyl amino acids ligands and an acetate have been synthesized and characterized. These complexes show potential as anticancer agents, with the ability to exchange the bound carboxylate ligand with water to form cytotoxic cationic complexes. Cytotoxicity studies reveal that the complexes with the bis-imidazolylidene ligand exhibit higher toxicity compared to those with the pyridyl-imidazolylidene ligand.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Inorganic & Nuclear
Daniel F. Earley, Jose Esteban Flores, Amaury Guillou, Jason P. Holland
Summary: In recent years, copper-64 and copper-67 have been considered as a useful theranostic pair in nuclear medicine. This study successfully demonstrates the viability of photochemically induced conjugation methods for the development of copper-based radiotracers for potential applications in diagnostic PET imaging and targeted radionuclide therapy.
DALTON TRANSACTIONS
(2022)