Article
Chemistry, Multidisciplinary
Zhiyuan Cao, Chuyue Li, Yufei Shu, Meiyi Zhu, Bin Su, Haiyan Qin, Xiaogang Peng
Summary: Using CdSe/CdS/ZnS core/shell/shell quantum dots as a model system, time- and potential-resolved spectroelectrochemical measurements were successfully applied to study the mechanisms and kinetics of electrochemiluminescence (ECL) generation. The rate constant of electron injection into a negatively charged quantum dot increased with increasing potential, and the key intermediate for ECL generation was found to be structurally stable and possess slow deionization channels.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Review
Chemistry, Analytical
Yizhuo Fu, Xu Teng, Chao Lu
Summary: Benefiting from their long luminescent lifetime, large stokes shift, and high electrochemiluminescence efficiency, iridium-based materials have emerged as promising ECL emitters. This review focuses on the recent progress of iridium-based ECL systems in bioanalysis and summarizes the strategies for designing iridium-based materials for ECL biosensors.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Analytical
Ni Liao, Mei-Chen Pan, Li Wang, Fan Yang, Ruo Yuan, Ying Zhuo
Summary: A novel swing arm location-controllable DNA walker based on DNA tetrahedral nanostructures was developed for nucleic acid detection, demonstrating enhanced efficiency and potential in diagnostic analysis.
ANALYTICAL CHEMISTRY
(2021)
Article
Chemistry, Analytical
Mengxia Yan, Jianhui Xin, Libing Fan, Jing Ye, Ting Xiao, Jianshe Huang, Xiurong Yang
Summary: This study selected C545T as a new ECL illuminant and synthesized organic microrods of C545T for ECL detection in aqueous solution. Cyclic voltammetry and differential pulse voltammetry of C545T and C545T MRs showed multiple oxidation peaks, indicating that the multiple charge states of C545T could be produced by continuous electron- or hole-injection processes. The ECL system with C545T MRs/TEOA showed intense yellow emission with high selectivity and sensitivity for dopamine detection.
ANALYTICAL CHEMISTRY
(2021)
Article
Chemistry, Analytical
Shu-Shu Song, Jiale Zhan, Hao-Tian Zhu, Jing-Yi Bao, Ai-Jun Wang, Pei-Xin Yuan, Jiu-Ju Feng
Summary: This study investigates the use of palladium nanospheres-embedded metal-organic frameworks to enhance the electrochemiluminescence efficiency of organic emitters in aqueous solutions, leading to the development of a highly efficient electrochemiluminescence sensor.
Article
Chemistry, Multidisciplinary
Samuel D. L. Holman, Alfie G. Wills, Neal J. Fazakerley, Darren L. Poole, Diane M. Coe, Leonard A. Berlouis, Marc Reid
Summary: An electrochemical method for the synthesis of substituted isoxazoline cores is presented, which can efficiently convert both aryl and alkyl aldoximes. In-situ reaction monitoring and theoretical calculations support the mechanism and reaction pathway.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Physical
Mingyu Wan, Zhiyong Gu, Fanglin Che
Summary: By modifying Cu surface with SAM, the stability, activity, and selectivity of CO2 electroreduction to C-2 chemicals can be improved, mainly through decreasing surface energy, facilitating CO2 activation and C-C coupling, as well as inducing confinement effects and charge transfer.
Article
Chemistry, Analytical
Wenting Wu, Jing Li
Summary: Nanozymes, as emerging artificial enzymes, have attracted attention in the sensing field due to their superior catalytic properties and high stability. Nanozyme-based electrochemical sensing has experienced fast growth, providing high sensitivity, selectivity, ease of miniaturization, and versatile signal reporting modes. This article discusses representative works in the field, focusing on different signal reporting manners, such as traditional electrochemical assays, electrochemiluminescent, and photoelectrochemical sensing. Furthermore, the current challenges and future perspectives are also addressed.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2023)
Article
Biochemistry & Molecular Biology
Anton A. Ulantikov, Konstantin A. Brylev, Taisiya S. Sukhikh, Yuri Mironov, Viktoria K. Muravieva, Yakov M. Gayfulin
Summary: A series of new octahedral rhenium cluster complexes were synthesized and investigated, showing that the difference in the electronic structure of the ligands has a fundamental effect on the properties of the complexes. The complexes with bpp ligand exhibit higher photoluminescence performance.
Article
Chemistry, Analytical
Shuangtian Dong, Dongyang Wang, Xuwen Gao, Li Fu, Jingna Jia, Yuqi Xu, Bin Zhang, Guizheng Zou
Summary: This study proposes a method to achieve chemiluminescence with different wavelengths and intensities by adjusting triggering agents, which shows promising potential for applications in immunoassays and other fields.
ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Kyoung-Rok Kim, Jiwoo Kim, Jinrok Oh, Joohoon Kim, Jong-In Hong
Summary: Donor-acceptor (D-A) type molecules with a skeleton consisting of a dimethylaminonaphthalene donor and an oxazaborine acceptor were designed as efficient electrochemiluminescence (ECL) luminophores with tunable intramolecular charge transfer (ICT). The experimental and computational results demonstrated that the ICT characteristics play a critical role in the electrochemistry and ECL of luminophores in the presence of tri-n-propylamine. Furthermore, the dual-peaked ECL-potential behaviors of the luminophores were rationalized using two competitive pathway ECL mechanisms, elucidated through the use of spooling ECL spectroscopy.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Tobias Hilche, Philip H. Reinsberg, Sven Klare, Theresa Liedtke, Luise Schaefer, Andreas Gansaeuer
Summary: The study successfully elucidated the impact of compounds such as thiourea, squaramide, and bissulfonamide on the EqCr equilibrium of Cp2TiCl2 through a combination of synthesis, electrochemical measurements, computational investigations, and DFT methods. Quantitative data and stoichiometry of adduct formation were provided for the first time, along with the determination of Gibbs energies, enthalpies, and complex structures. The results not only validated the use of the EqCr equilibrium in predicting sustainable catalysis, but also served as a design platform for the development of novel additives, particularly in enantioselective catalysis.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Jan Patrick Calupitan, Alexandre Poirot, Jinhui Wang, Beatrice Delavaux-Nicot, Mariusz Wolff, Maria Jaworska, Remi Metivier, Eric Benoist, Clemence Allain, Suzanne Fery-Forgues
Summary: The study presents the mechanoresponsive luminescence (MRL) activity of two Re-I complexes with solid-state luminescence enhancement (SLE). Quantum chemical calculations reveal the existence of two low-lying triplet excited states, affecting the emission properties with intraligand and metal-to-ligand charge-transfer character. The transition between these states is promoted by rotation around specific bonds, influencing the emitted wavelength of photoluminescence.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Analytical
Sara Knezevic, Emily Kerr, Bertrand Goudeau, Giovanni Valenti, Francesco Paolucci, Paul S. Francis, Frederic Kanoufi, Neso Sojic
Summary: Electrochemiluminescence (ECL) microscopy is a new technique used for imaging single entities and cells. In this study, a bimodal and bicolor approach was developed to record both positive ECL (PECL) and shadow label-free ECL (SECL) images of single cells. This dual approach enables the imaging of cell morphology and can contribute to multimodal ECL imaging and bioassays.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Paltan Laha, Ahmad Husain, Srikanta Patra
Summary: In this study, four mononuclear cyclometallated iridium complexes [1](PF6) - [4](PF6) were developed using alkyl chain appended benzimidazole-based cyclometallating ligands (L-1 and L-2). The complexes were characterized and their crystal structures revealed the distorted octahedral geometry around the iridium center. The complexes exhibited emissive properties with emission maxima dependent on the substituent present on the ligand framework. Tuning emission maxima by variation of substitution holds great importance in developing luminescent materials.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Chemistry, Multidisciplinary
Kimberly K. Hollister, Andrew Molino, Grace Breiner, Jacob E. Walley, Kelsie E. Wentz, Ashley M. Conley, Diane A. Dickie, David J. D. Wilson, Robert J. Gilliard
Summary: This article reports the synthesis, molecular structures, and optical properties of a new class of air-stable borenium ions stabilized by the strongly donating carbodicarbene ligand. These ions exhibit thermoluminescence in solution and increased quantum yields in the solid state, with the ability to emit white light at lower temperatures. The effect of anion size and ligand rotation on the optical properties is also investigated, complemented by theoretical analysis of the excited-state dynamics.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Emily Kerr, David J. Hayne, Lachlan C. Soulsby, Joseph C. Bawden, Steven J. Blom, Egan H. Doeven, Luke C. Henderson, Conor F. Hogan, Paul S. Francis
Summary: A novel 'redox mediator' pathway utilizing fac-[Ir(sppy)(3)](3-) has been discovered to significantly enhance the ECL reaction of [Ru(bpy)(3)](2+) and tri-n-propylamine. The green emission of [Ir(sppy)(3)](3-)* allows for internal standardization of the reaction, enabling superior sensitivity and precision for low-cost, portable ECL-based analytical devices when using a digital camera as the photodetector.
Article
Chemistry, Multidisciplinary
Kimberly K. Hollister, Wenlong Yang, Ranajit Mondol, Kelsie E. Wentz, Andrew Molino, Aishvaryadeep Kaur, Diane A. Dickie, Gernot Frenking, Sudip Pan, David J. D. Wilson, Robert J. Gilliard
Summary: In this study, the first isolable, crystalline borepin radical and anion complexes were reported. These complexes were synthesized through the reduction of carbon-carbon double bonds in cyclic(alkyl)(amino) carbene-dibenzo[b,d]borepin precursors using potassium graphite. The resulting compounds have potential applications in the development of new materials and optoelectronics.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Biochemistry & Molecular Biology
Laena D'Alton, Serena Carrara, Gregory J. Barbante, David Hoxley, David J. Hayne, Paul S. Francis, Conor F. Hogan
Summary: This article describes a powerful, low-cost, and semi-portable electrochemiluminescence (ECL) biosensing device based on a Raspberry Pi single-board computer. The Pi serves as the controller and user interface, interfacing with an expansion board that controls the potential applied to a disposable screen-printed electrode and facilitates data acquisition from a photomultiplier tube (PMT). The Raspberry Pi-based setup demonstrates comparable analytical performance to a traditional ECL configuration and has the potential to replace conventional ECL setups at a fraction of the cost, without sacrificing sensitivity or versatility. This combination of a single-board computer and a sensitive light detector represents an important step towards mobile, point-of-care diagnostic platforms for ECL instruments.
BIOELECTROCHEMISTRY
(2022)
Article
Chemistry, Analytical
Marlin J. Pedrozo-Penafiel, Thais Lopes, Luis M. Gutierrez-Beleno, Jarol R. Miranda-Andrades, Marcelo E. H. Maia Da Costa, Dunieskys G. Larrude, Ricardo Q. Aucelio
Summary: A square-wave voltammetric method was developed for the determination of creatinine using glassy carbon electrode functionalized multi-walled carbon nanotubes and doped with copper. The linear responses at either pH 4.0 or 7.0 were evaluated allowing versatility in application. The electrode is simple to prepare and robust for routine analysis and it was used for the determination of creatinine in urine after simple thin-layer separation procedure to avoid interference from creatine.
Article
Chemistry, Inorganic & Nuclear
Manjur O. Akram, John R. Tidwell, Jason L. Dutton, David J. D. Wilson, Andrew Molino, Caleb D. Martin
Summary: Borole-doped polycyclic aromatic hydrocarbons (PAHs) have been synthesized and studied in this work. Intermolecular nitrene and oxygen atom insertion reactions were used to access 1,2-azaborine- and 1,2-oxaborine-containing analogues. Iodosobenzene was established as a versatile reagent for oxygen atom insertion reactions into various borole species to access 1,2-oxaborine systems.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Kelsie E. Wentz, Andrew Molino, Lucas A. Freeman, Diane A. Dickie, David J. D. Wilson, Robert J. Gilliard
Summary: The impact of the spatial arrangement of the alkali metal on the electronic properties of 9-carbene-9-borafluorene monoanions has been evaluated, leading to the isolation of a series of [K][9-CAAC-9-borafluorene] complexes. These complexes show potential for controlling the nucleophilic and electron transfer properties of the monoanions, with the formation of new air-stable spirocycles that display fluorescence properties under UV light.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Aishvaryadeep Kaur, David J. D. Wilson
Summary: A theoretical investigation has been conducted to assess the bonding and electronic structure of ligand-stabilized MX diatomics (M = group 13, X = group 15 element) with N-heterocyclic carbene (NHC) ligands. The study suggests that binding of two ligands in the form L-MX-L is generally more favorable than binding of a single ligand. The bonding between carbene and boron/nitrogen is described as an electron-sharing double bond with both sigma and pi bonding interactions, while bonding with carbon is best described as a donor-acceptor sigma single bond.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2022)
Article
Multidisciplinary Sciences
Srividhya Swaminathan, Katie E. Lineburg, Archana Panikkar, Jyothy Raju, Lawton D. Murdolo, Christopher Szeto, Pauline Crooks, Laetitia Le Texier, Sweera Rehan, Michael J. Dewar-Oldis, Peter J. Barnard, George R. Ambalathingal, Michelle A. Neller, Kirsty R. Short, Stephanie Gras, Rajiv Khanna, Corey Smith
Summary: The T cell response to SARS-CoV-2 can be affected by mutations in emerging variants, reducing the effectiveness of T cell immunity. While antibody-mediated immunity may be reduced against the Omicron variant, T cell recognition is less affected. However, the complexity of human leukocyte antigen genetics suggests that T cell immunity may not be universally maintained.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Kelsie E. Wentz, Andrew Molino, Lucas A. Freeman, Diane A. Dickie, David J. D. Wilson, Robert J. J. Gilliard Jr
Summary: In this study, dianionic 10-membered bora-crown ethers were synthesized for the first time, and their reaction mechanism and electronic structure were elucidated through experiments and theoretical calculations.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Electrochemistry
Georgina Armendariz-Vidales, Pria Ramkissoon, Peter J. Barnard, Conor F. Hogan
Summary: This study investigated a multicolour ECL system composed of BODIPY and DOTA. Energy transfer could be initiated by optical excitation when a lanthanide ion was bound to the DOTA ligand. In the absence of lanthanide ions, the conjugate exhibited a dual wavelength ECL behavior at 549 and 730 nm in both annihilation and co-reactant pathways, which could be modulated by controlling the potential. Using the 3D ECL technique, the potential and concentration dependence of the ECL emission were characterized, revealing various mechanisms giving rise to ECL emissions in the visible and near-infrared.
ELECTROCHIMICA ACTA
(2023)
Article
Chemistry, Multidisciplinary
Samir Kumar Sarkar, Kimberly K. Hollister, Andrew Molino, Akachukwu D. Obi, Chun-Lin Deng, Bi Youan E. Tra, Brennan M. Stewart, Diane A. Dickie, David J. D. Wilson, Robert J. Gilliard
Summary: In this study, we report the ligand-mediated control of boraphenanthrene electronic states, leading to the first structurally characterized examples of neutral bis(9-boraphenanthrene) and its corresponding biradical. These compounds exhibit dual emission in solution and possess a high degree of biradical character.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
David J. D. Wilson
Summary: The structure and NMR shielding of a set of N-F containing cations have been accurately determined through extensive ab initio calculations. The study reveals the possibility of even shorter N-F bonds and predicts extreme 19F and 15N chemical shifts in these cations.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Organic
Tania, Andrew Molino, Lachlan Sharp-Bucknall, David J. D. Wilson, Jason L. Dutton
Summary: PhIBr2, a substance with low stability, has been recently shown to be formed in situ by reacting PIFA with TMSBr, and has demonstrated efficacy in aryl brominations.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2022)
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)