electrochemistry

High sulfur content polymeric materials, known for their intriguing properties such as high refractive indices and high electrochemical capacities, have garnered significant interest in recent years for their applications in optics, antifouling surfaces, triboelectrics, and electrochemistry. Despite the high interest, most high sulfur-content polymers reported to date are either bulk materials or thin films, and there is a general lack of research into sulfur-rich polymer colloids. Water-dispersed, sulfur-rich particles are anticipated to broaden the range of applications for sulfur-containing materials...

Radicals can feature theoretically 100% light utilization owing to their nonelectron spin-forbidden transition and represent the most advanced luminescent materials at present. 2,2,6,6-Tetramethyl-1-piperidinyloxy (TEMPO) acts as a typically stable radical with very broad applications. However, their luminescent properties have not been discovered to date. In the present work, we observed the bright electrochemiluminescence (ECL) emission of TEMPO with a higher efficiency (72.3%) via the electrochemistry and coreactant strategies for the first time...

Three hybrid electrochemical protocols, which involve the energy transfer, direct photolysis and N-hydroxyphthalimide catalyst, respectively, are presented for the selenylation/cyclization of the fragile substrates of 3-aza-1,5-dienes with diorganyl diselenides to afford 3-selenomethyl-4-pyrrolin-2-ones. The two electrophotocatalytic reactions and the indirect electrolysis one are both regioselective and external-oxidant- and transition-metal-free, and are associated with a broad substrate scope and high Se-economy, and all three methods are amenable to gram-scale syntheses, late-stage functionalizations, sunlight-induced experiments and all-solar-driven syntheses...

There is a rising need to create high-performing, affordable electrocatalysts in the new field of oxygen electrochemistry. Here, a cost-effective, activity-modulated electrocatalyst with the capacity to trigger both the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) in an alkaline environment is presented. The catalyst (Al, Co/N-rGCNT) is made up of aluminium, nitrogen-dual-doped reduced graphene oxide sheets co-existing with cobalt-encapsulated carbon nanotube units. Based on X-ray Absorption Spectroscopy (XAS) studies, it is established that the superior reaction kinetics in Al, Co/N-rGCNT over their bulk counterparts can be attributed to their electronic regulation...

Rare-earth metalloligand supported low-valent cobalt complexes were synthesized by utilizing a small-sized heptadentate phosphinomethylamine L s N H3 and a large-sized arene-anchored hexadentate phosphinomethylamine L l Ar H3 ligand precursors. The RE(III)-Co(-I)-N2 (RE = Sc, Lu, Y, Gd, La) complexes containing rare-earth metals including the smallest Sc and largest La were characterized by multinuclear NMR spectroscopy, X-ray diffraction analysis, electrochemistry, and computational studies. The Co(-I)→RE(III) dative interactions were all polarized with major contributions from the 3d z 2 orbital of the cobalt center, which was slightly affected by the identity of rare-earth metalloligands...

Alkylamines form the backbone of countless nitrogen-containing small molecules possessing desirable biological properties. Despite advances in amine synthesis through transition metal catalysis and photoredox chemistry, multicomponent reactions that leverage inexpensive materials to transform abundant chemical feedstocks into three-dimensional α-substituted alkylamines bearing complex substitution patterns remain scarce. Here, we report the design of a catalyst-free electroreductive manifold that merges amines, carbonyl compounds and carbon-based radical acceptors under ambient conditions without rigorous exclusion of air and moisture...

Electrochemical liquid electron microscopy has revolutionized our understanding of nanomaterial dynamics by allowing for direct observation of their electrochemical production. This technique, primarily applied to inorganic materials, is now being used to explore the self-assembly dynamics of active molecular materials. Our study examines these dynamics across various scales, from the nanoscale behavior of individual fibers to the micrometer-scale hierarchical evolution of fiber clusters. To isolate the influences of the electron beam and electrical potential on material behavior, we conducted thorough beam-sample interaction analyses...

Alternating current (AC) and pulsed electrolysis are gaining traction in electro(organic) synthesis due to their advantageous characteristics. We employed AC electrolysis in electrochemically mediated Atom Transfer Radical Polymerization (eATRP) to facilitate the regeneration of the activator CuI complex on Cu0 electrodes. Additionally, Cu0 served as a slow supplemental activator and reducing agent (SARA ATRP), enabling the activation of alkyl halides and the regeneration of the CuI activator through a comproportionation reaction...

Carcinoembryonic antigen (CEA) is a critical biomarker for identifying colon cancer. This work presents an electrochemical impedance spectroscopy (EIS) based aptasensor for detecting CEA, utilizing a single-stranded DNA (ssDNA) aptamer previously selected and characterized by our research group. The surface of an interdigitated gold electrode (IDE) was successfully functionalized with an 18-HEG-modified aptamer sequence. The developed aptasensor demonstrated high specificity and sensitivity with detection limits of 2...

Voltammetry is a powerful electroanalytical tool that makes fast, real-time measurements of neurotransmitters and other molecules. Electroanalytical methods like cyclic, pulse, and stripping voltammetry are useful for qualitative and quantitative examination. Neurochemical sensing has been enhanced using carbon-based electrodes and waveform modification methods that improve sensitivity and stability of electrode performance. Voltammetry has revolutionized neurochemical monitoring by providing real-time information on neurotransmitter dynamics for neurochemical studies...

Dysregulation of miRNA expression occurs in many cancers, making miRNAs useful in cancer diagnosis and therapeutic guidance. In a clinical context using methods such as polymerase chain reaction (PCR), the limited amount of miRNAs in circulation often limits their quantification. Here, we present a PCR-free and sensitive singlet oxygen (1 O2 )-based strategy for the detection and quantification of miRNAs in untreated human plasma from patients diagnosed with prostate cancer. A target miRNA is specifically captured by functionalised magnetic beads and a detection oligonucleotide probe in a sandwich-like format...

Pyridoxal hydrochloride, a vitamin B6 vitamer, was synthetically converted to a series of diverse redox-active benzoyl pyridinium salts. Cyclic voltammetry studies demonstrated redox reversibility under basic conditions, and two of the most promising salts were subjected to laboratory-scale redox flow battery tests involving galvanostatic cycling at 10 mM in 0.1 M NaOH. In these tests, the battery was charged completely, corresponding to the transfer of two electrons to the electrolyte, but no discharge was observed...

H+ co-intercalation chemistry of the cathode is perceived to have damaging consequences on the low-rate and long-term cycling of aqueous zinc batteries, which is a critical hindrance to their promise for stationary storage applications. Herein, the thermodynamically competitive H+ storage chemistry of an attractive high-voltage cathode LiMn2 O4 is revealed by employing operando and ex-situ analytical techniques together with density functional theory-based calculations. The H+ electrochemistry leads to the previously unforeseen voltage decay with cycling, impacting the available energy density, particularly at lower currents...

Ca2+ , in combination with SP or EP, induces cell cytotoxicity much faster compared to BLM. The application of BLM in combination with, SP or EP, reaches the level of cell death, induced by similar combination with Ca2+ , only after 72 h. The methods of SP and EP were calibrated according to the level of differential cytotoxicity, determined after 6 days (using cell clonogenic assay). The combination of Ca2+ SP induces cell death faster than Ca2+ EP - after Ca2+ SP it increases to a maximum level after 15 min and remains constant for up to 6 days, while the cytotoxic efficiency after Ca2+ EP increases to the level of Ca2+ SP only after 72 h...

The main challenges (sluggish electron transfer, low energy density) hinder the future application of enzymatic biofuel cells (EBFCs), which urgent to take effective measures to solve these issues. In this work, a composite of Au nanoparticles decorated graphdiyne (AuNPs@GDY) is fabricated and employed as the carrier of enzyme (G6PDH), and a mechanism based on π-π interaction of electron transfer is proposed to understand bioelectrocatalysis processes. The results show that the AuNPs@GDY composite exhibits the highest current density among the three materials (GDY, AuNPs, and AuNPs@GDY), which is 3...

Sulphide oxidising bacteria (SOB) have the potential to be used for bioelectrochemical removal, i.e. oxidation, of sulphide from waste streams. In anaerobic conditions, SOB are able to spatially separate sulphide removal and terminal electron transfer to an electrode and act as a sulphide shuttle. However, it is not fully understood how SOB anaerobically remove sulphide and store charge equivalents, and where in this process sulphur is formed. Therefore, the redox behaviour of sulphide shuttling SOB was investigated at haloalkaline conditions using a glassy carbon rotating disc electrode (RDE) and cyclic voltammetry...

We present herein the synthesis, characterization and complexation of ferrocenyl-substituted MIIs (mesoionic imines) and their metal complexes. In the free MIIs, strong hydrogen bonding interactions are observed between the imine-N and the C-H bonds of the ferrocenyl substituents both in the solid state and in solution. The influence of this hydrogen bonding is so strong that complexation of the MIIs with [IrCp*Cl2]2 yields unique six-membered iridacycles via C-H-activation of the corresponding C-H-site at the Fc-substituent and not the Ph-substituent...

Metabolomics provides powerful tools that can inform about heterogeneity in disease and response to treatments. In this study, we employed an electrochemistry-based targeted metabolomics platform to assess the metabolic effects of three randomly-assigned treatments: escitalopram, duloxetine, and Cognitive Behavior Therapy (CBT) in 163 treatment-naïve outpatients with major depressive disorder. Serum samples from baseline and 12 weeks post-treatment were analyzed using targeted liquid chromatography-electrochemistry for metabolites related to tryptophan, tyrosine metabolism and related pathways...

Recent advances in paper-based microsupercapacitors (p-MSCs) have attracted significant attention due to their potential as substrates for flexible electronics. This review summarizes progress in the field of p-MSCs, discussing their challenges and prospects. It covers various aspects, including the fundamental characteristics of paper, the modification of paper with functional materials, and different methods for device fabrication. The review critically analyzes recent advancements, materials, and fabrication techniques for p-MSCs, exploring their potential applications and benefits, such as flexibility, cost-effectiveness, and sustainability...

Impact electrochemistry allows for the investigation of the properties of single entities, ranging from nanoparticles (NPs) to soft bio-particles. It has introduced a novel dimension in the field of biological analysis, enhancing researchers' ability to comprehend biological heterogeneity and offering a new avenue for developing novel diagnostic devices for quantifying biological analytes. This review aims to summarize the recent advancements in impact electrochemistry-based biosensing over the past two to three years and provide insights into the future directions of this field...