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According to the Hofmeister series, thiocyanate is the strongest "salting in" anion. In fact, it has a strong denaturant activity against the native state of globular proteins. A molecular level rationalization of the Hofmeister series is still missing, and therefore the denaturant activity of thiocyanate also awaits a robust explanation. In the last years, different types of experimental studies have shown that thiocyanate is capable to directly interact with both polar and nonpolar groups of polypeptide chains. This finding has been scrutinized via a careful computational procedure based on density functional theory approaches. The results indicate that thiocyanate is able to make H-bonds via both the nitrogen and sulfur atom, and to make strong van der Waals interactions with almost all the groups of polypeptide chains, regardless of their polarity.
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Péptidos , Tiocianatos , Tiocianatos/química , Péptidos/química , Teoría Funcional de la Densidad , Enlace de HidrógenoRESUMEN
Developing inventive approaches to control crystallization and suppress trap defects in perovskite films is crucial for achieving efficient perovskite photovoltaics. Here, a synchronous regulation strategy is developed that involves the infusion of a zwitterionic ionic liquid additive, pyrrolidinium thiocyanate (PySCN), into the perovskite precursor to optimize the subsequent crystallization and defects. PySCN modification not only orchestrates the crystallization process but also deftly addresses trap defects in perovskite films. Within this, SCN- compensates for positively charged defects, while Py+ plays the role of passivating negatively charged defects. Based on the vacuum flash evaporation without anti-solvent, the air-processed perovskite solar cells (PSCs) with PySCN modification can achieve an extraordinary champion efficiency of 22.46% (0.1 cm2) and 21.15% (1.0 cm2) with exceptional stability surpassing 1200 h. Further, the self-powered photodetector goes above and beyond, showcasing an ultra-low dark current of 2.13 × 10-10 A·cm-2, a specific detection rate of 6.12 × 1013 Jones, and an expansive linear dynamic range reaching an astonishing 122.49 dB. PySCN modification not only signifies high efficiency but also ushers in a new era for crystallization regulation, promising a transformative impact on the optoelectronic performance of perovskite-based devices.
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Thiocyanate (SCN-), a non-volatile inorganic pollutant, is commonly found in various types of industrial wastewater, which is resistant to hydrolysis and has the potential to be toxic to organisms. Premagnetized iron-copper-carbon ternary micro-electrolytic filler (pre-Fe/Cu/C) was prepared to degrade SCN-. Pre-Fe/Cu/C exhibited the most significant enhancement effect on SCN- removal when magnetized for 5 min with an intensity of 100 mT, and the SCN- removal rate was the highest at an initial pH of 3.0 and an aeration rate of 1.6 L/min. The electrochemical corrosion and electron transfer in the pre-Fe/Cu/C system were confirmed through SEM, XPS, FTIR, XRD, and electrochemical tests. This resulted in the formation of more corrosion products and multiple cycles of Fe2+/Fe3+ and Cu0/Cu+/Cu2+. Additionally, density functional theory (DFT) calculations and electron paramagnetic resonance (EPR) were utilized to illustrate the oxygen adsorption properties of the materials and the participation of reactive oxygen species (1O2, ·O2-, and ·OH) in SCN- removal. The degradation products of SCN- were identified as SO42-, HCO3-, NH4+, and N2. This study introduced the use of permanent magnets for the first time to enhance Fe/Cu/C ternary micro-electrolytic fillers, offering a cost-effective, versatile, and stable approach that effectively effectively enhanced the degradation of SCN-.
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Cobre , Hierro , Tiocianatos , Contaminantes Químicos del Agua , Tiocianatos/química , Cobre/química , Hierro/química , Contaminantes Químicos del Agua/química , Contaminantes Químicos del Agua/análisis , Carbono/química , CorrosiónRESUMEN
This study presents a novel, cost-effective approach involving spectrophotometric and smartphone paper-based (SPB) methods and a distinctive salting-out air-assisted dispersive microextraction procedure to quantify thiocyanate in saliva samples. The method relies on the inhibitory effect of thiocyanate on quinoneimine dye formation during the Emerson reaction with sodium hypochlorite. Spectrophotometry quantifies the extracted dye by monitoring quinoneimine color intensity reduction at 525 nm. In the SPB method, extracted dye is applied to a paper strip, a smartphone captures the colored paper, and an application analyzes red, green, and blue components. All analyte determination and extraction variables were explored. Both methods exhibit good linearity (10-100 µg/L) with a coefficient of determination of 0.9991 and a limit of detection of 7.5 µg/L for the spectrophotometric method, and a coefficient of determination of 0.9988 and a limit of detection of 8.8 µg/L for the SPB method. The calculated values for the enrichment factor and extraction recovery of the developed extraction methodology were 46% and 93%, respectively. The methods detect thiocyanate in saliva samples, producing results comparable to a validated method.
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Microextracción en Fase Líquida , Fumadores , Humanos , Tiocianatos/análisis , Saliva/química , Teléfono Inteligente , Límite de DetecciónRESUMEN
In recent decades, there has been increasing interest in elucidating the role of sulfur-containing compounds in plant metabolism, particularly emphasizing their function as signaling molecules. Among these, thiocyanate (SCN-), a compound imbued with sulfur and nitrogen, has emerged as a significant environmental contaminant frequently detected in irrigation water. This compound is known for its potential to adversely impact plant growth and agricultural yield. Although adopting exogenous SCN- as a nitrogen source in plant cells has been the subject of thorough investigation, the fate of sulfur resulting from the assimilation of exogenous SCN- has not been fully explored. There is burgeoning curiosity in probing the fate of SCN- within plant systems, especially considering the possible generation of the gaseous signaling molecule, hydrogen sulfide (H2S) during the metabolism of SCN-. Notably, the endogenous synthesis of H2S occurs predominantly within chloroplasts, the cytosol, and mitochondria. In contrast, the production of H2S following the assimilation of exogenous SCN- is explicitly confined to chloroplasts and mitochondria. This phenomenon indicates complex interplay and communication among various subcellular organelles, influencing signal transduction and other vital physiological processes. This review, augmented by a small-scale experimental study, endeavors to provide insights into the functional characteristics of H2S signaling in plants subjected to SCN--stress. Furthermore, a comparative analysis of the occurrence and trajectory of endogenous H2S and H2S derived from SCN--assimilation within plant organisms was performed, providing a focused lens for a comprehensive examination of the multifaceted roles of H2S in rice plants. By delving into these dimensions, our objective is to enhance the understanding of the regulatory mechanisms employed by the gasotransmitter H2S in plant adaptations and responses to SCN--stress, yielding invaluable insights into strategies for plant resilience and adaptive capabilities.
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Sulfuro de Hidrógeno , Plantas , Transducción de Señal , Tiocianatos , Sulfuro de Hidrógeno/metabolismo , Tiocianatos/metabolismo , Plantas/metabolismo , Gasotransmisores/metabolismo , Cloroplastos/metabolismo , Inactivación MetabólicaRESUMEN
The new chalcogenylation of phosphines using nBu4Nâ§XCN (X = S, Se) is described. The reaction in 1,2-dichloroethane at 120 °C provided the corresponding phosphine sulfides in good to high yields. The protocol could be extended to the synthesis of phosphinic acid derivatives as well as sulfurization of poly(styrene-co-4-styryldiphenylphosphine).
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Calcógenos , Fosfinas , Compuestos de Amonio Cuaternario , Fosfinas/química , Compuestos de Amonio Cuaternario/química , Compuestos de Amonio Cuaternario/síntesis química , Calcógenos/química , Calcógenos/síntesis química , Estructura MolecularRESUMEN
CO2 reduction (CO2R) catalyzed by an efficient, stable, and earth-abundant electrocatalyst offers an attractive means to store energy derived from renewable sources. Here, we describe the synthesis of facet-defined Cu2SnS3 nanoplates and the ligand-controlled CO2R property. We show that thiocyanate-capped Cu2SnS3 nanoplates possess excellent selectivity toward formate over a wide range of potentials and current densities, attaining a maximum formate Faradaic efficiency of 92% and partial current densities as high as 181 mA cm-2 when tested using a flow cell with gas-diffusion electrode. In situ spectroscopic measurements and theoretical calculations reveal that the high formate selectivity originates from favorable adsorption of HCOO* intermediates on cationic Sn sites that are electronically modulated by thiocyanates bound to adjacent Cu sites. Our work illustrates that well-defined multimetallic sulfide nanocrystals with tailored surface chemistries could provide a new avenue for future CO2R electrocatalyst design.
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Lead halide perovskite nanocrystals (LHP NCs) are regarded as promising emitters for next-generation ultrahigh-definition displays due to their high color purity and wide color gamut. Recently, the external quantum efficiency (EQE) of LHP NC based light-emitting diodes (PNC LEDs) has been rapidly improved to a level required by practical applications. However, the poor operational stability of the device, caused by halide ion migration at the grain boundary of LHP NC thin films, remains a great challenge. Herein, we report a resurfacing strategy via pseudohalogen ions to mitigate detrimental halide ion migration, aiming to stabilize PNC LEDs. We employ a thiocyanate solution processed post-treatment method to efficiently resurface CsPbBr3 NCs and demonstrate that the thiocyanate ions can effectively inhibit bromide ion migration in LHP NC thin films. Owing to thiocyanate resurfacing, we fabricated LEDs with a high EQE of 17.3%, a maximum brightness of 48000 cd m-2, and an excellent operation half-life time.
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Combining a strong second-order nonlinear optical (NLO) effect (>1×KH2PO4 (KDP)), a large band gap (>4.2â eV), and a moderate birefringence in ultraviolet (UV) NLO crystals remains a formidable challenge. Herein, Cd(SCN)2(C4H6N2)2, the first example of a thiocyanate capable of realizing a phase-matched UV NLO crystal material, is obtained by reducing the sulfur (S) content in the centrosymmetric (CS) structure of Cd(SCN)2(CH4N2S)2. Compared to the "shoulder-to-shoulder" one-dimensional (1D) chain of Cd(SCN)2(CH4N2S)2, Cd(SCN)2(C4H6N2)2 has a different sawtooth 1D chain structure. Cd(SCN)2(CH4N2S)2 has second harmonic generation (SHG) inertia with a band gap of 3.90â eV and a UV cutoff edge of 342â nm, however, it possesses a large birefringence (0.35@546â nm). In contrast, the symmetry center breaking of Cd(SCN)2(C4H6N2)2 leads to remarkably strong SHG intensity (10â times that of KDP). Furthermore, it has a wide band gap (4.74â eV), short UV cutoff edge (234â nm), and moderate birefringence capable of phase matching (0.17@546â nm). This research indicates that thiocyanates are a promising class of UV NLO crystal materials, and that modulation of the sulfur content of CS thiocyanates is an effective strategy for the development of UV NLO crystals with excellent overall performances.
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High-performance liquid chromatography (HPLC)-based analytical assays are used to effectively monitor purity and quantity of plasmid DNA (pDNA) throughout the purification process. However, the phenomenon of physical entrapment of open circular (OC) isoforms pDNA inside narrow channels of chromatographic support decreases its accuracy and precision and the effect increases with pDNA size. The purpose of the study was to develop a chromatographic method for accurate analytical separation between isoforms of <16 kbp pDNA using weak anion exchanging monolithic column with large (6 µm) convective channels. Purified samples of 4.7 and 15.4 kbp large pDNA with known isoform composition were prepared and their isoforms separated in ascending salt gradient. Both OC and supercoiled (SC) isoforms were baseline separated at a flow rate below 0.5 mL min-1 in a guanidinium chloride (GdnCl) gradient with a ≥95% OC pDNA elution recovery. However, these chromatographic conditions increased 2 times the peak width for linear (LIN) pDNA isoform compared to the results using monoliths with 1.4 µm channel size. If other chaotropic agents, such as urea or thiocyanate (SCN), were added to Gdn ions, the elution volume for LIN isoform decreased. Optimization of combined GdnCl/GdnSCN gradient for pDNA elution resulted in a simple and robust chromatographic method, where OC-LIN and LIN-SC pDNA (up to 15 kbp size) were separated with resolution above 1.0 and above 2.0, respectively. The accessibility and general acceptance of anion exchange chromatography for pDNA analytics give the newly developed method a great potential for in-process control monitoring of pDNA production processes.
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ADN , Plásmidos , Cromatografía Líquida de Alta Presión/métodos , Aniones , Isoformas de ProteínasRESUMEN
Copper thiocyanate (CuSCN) has been widely used in photodetectors (PDs). However, the reported CuSCN-based PDs are suffered from narrow operating wavelength range and relatively low photodetection performance. Here, we fabricate an CuSCN/Si heterojunction PD by a simple low-temperature solution spin-coating method achieving excellent performance. Our designed CuSCN/Si PD exhibits a broadband response range covering ultraviolet-visible-infrared, a high detectivity of 2.26 × 1012Jones coming from an ultralow dark current of 23 pA, and a decent responsivity of 11 mA W-1, a high linear dynamic range of 122 dB, and short response time of 25/150µ(rise and decay time). Moreover, we demonstrate multi-color imaging across the wide wavelength range, indicating the CuSCN/Si PD has a promising potential in the imaging field. This work may pave the way for fabricating low-cost, nontoxicity, and high-performance CuSCN-based PD and broadening its applications.
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Studies about the impacts of maternal exposure to perchlorate, thiocyanate, and nitrate on offspring neurodevelopment are scarce. Based on a birth cohort in China, 1,028 mothers provided urine samples at three trimesters for determination of the three target analytes, and their offspring neurodevelopment was evaluated at 2 years old. Associations of maternal exposure to the three chemicals with offspring neurodevelopment were estimated using three statistical methods. Trimester-specific analyses using generalized estimating equation models showed that double increment of thiocyanate and nitrate during the first trimester was associated with 1.56 (95% CI: -2.82, -0.30) and 1.22 (-2.40, -0.03) point decreases in the offspring mental development index (MDI), respectively. Weighted quantile sum (WQS) regression analyses showed that the mixture exposure at the first and second trimesters was negatively associated with the offspring MDI (ß = -2.39, 95% CI: -3.85, -0.93; ß = -1.75, 95% CI: -3.04, -0.47, respectively) and thiocyanate contributed the most to the association (65.0 and 91.6%, respectively). Bayesian kernel machine regression analyses suggested an inverted U-shape relationship of maternal urinary thiocyanate with the offspring MDI. These findings suggested that prenatal exposure to the three chemicals (at current levels), especially thiocyanate and nitrate, may impair neurodevelopment. Early pregnancy seems to be the sensitive window.
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Nitratos , Percloratos , Niño , Embarazo , Femenino , Humanos , Preescolar , Nitratos/orina , Estudios de Cohortes , Percloratos/orina , Tiocianatos/orina , Teorema de Bayes , Exposición MaternaRESUMEN
Cyanide (in the form of cyanide anion (CN-) or hydrogen cyanide (HCN), inclusively represented as CN) can be a rapidly acting and deadly poison, but it is also a common chemical component of a variety of natural and anthropogenic substances. The main mechanism of acute CN toxicity is based on blocking terminal electron transfer by inhibiting cytochrome c oxidase, resulting in cellular hypoxia, cytotoxic anoxia, and potential death. Due to the well-established link between blood CN concentrations and the manifestation of symptoms, the determination of blood concentration of CN, along with the major metabolite, thiocyanate (SCN-), is critical. Because currently there is no method of analysis available for the simultaneous detection of CN and SCN- from blood, a sensitive method for the simultaneous analysis of CN and SCN- from human ante- and postmortem blood via liquid chromatography-tandem MS analysis was developed. For this method, sample preparation for CN involved active microdiffusion with subsequent chemical modification using naphthalene-2,3-dicarboxaldehyde (NDA) and taurine (i.e., the capture solution). Preparation for SCN- was accomplished via protein precipitation and monobromobimane (MBB) modification. The method produced good sensitivity for CN with antemortem limit of detection (LODs) of 219 nM and 605 nM for CN and SCN-, respectively, and postmortem LODs of 352 nM and 509 nM. The dynamic ranges of the method were 5-500 µM and 10-500 µM in ante- and postmortem blood, respectively. In addition, the method produced good accuracy (100 ± 15%) and precision (≤ 15.2% relative standard deviation). The method was able to detect elevated levels of CN and SCN- in both antemortem (N = 5) and postmortem (N = 4) blood samples from CN-exposed swine compared to nonexposed swine.
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Thiocyanate in irrigation water can adversely affect plant growth and development. A previously constructed microflora with effective thiocyanate-degrading ability was used to investigate the potential of bacterial degradation for thiocyanate bioremediation. The root and aboveground part dry weight of plants inoculated with the degrading microflora increased by 66.67% and 88.45%, respectively, compared to those plants without the microflora. The supplementation of thiocyanate-degrading microflora (TDM) significantly alleviated the interference of thiocyanate in mineral nutrition metabolism. Moreover, the supplementation of TDM significantly reduced the activities of antioxidant enzymes, lipid peroxidation, and DNA damage and it protected plants from excessive thiocyanate, while the crucial antioxidant enzyme (peroxidase) decreased by 22.59%. Compared with the control without TDM supplementation, the soil sucrase content increased by 29.58%. The abundances of Methylophilus, Acinetobacter, unclassified Saccharimonadales, and Rhodanobacter changed from 19.92%, 6.63%, 0.79%, and 3.90%-13.19%, 0.27%, 3.06%, and 5.14%, respectively, with TDM supplementation. Caprolactam, 5,6-dimethyldecane, and pentadecanoic acid seem to have an effect on the structure of the microbial community in the rhizosphere soil. The above results indicated TDM supplementation can significantly reduce the toxic effects of thiocyanate on the tomato-soil microenvironment.
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Plantones , Solanum lycopersicum , Plantones/microbiología , Rizosfera , Antioxidantes/farmacología , Tiocianatos/farmacología , Plantas , Suelo/química , Microbiología del Suelo , Raíces de Plantas/microbiologíaRESUMEN
Thiocyanate may have played as important a role as cyanide in the synthesis of several molecules. However, its concentration in the seas of the prebiotic Earth could have been very low. Thiocyanate was dissolved in two different seawaters: a) a composition that comes close to the seawater of the prebiotic Earth (seawater-B, Ca2+ and Cl-) and b) a seawater (seawater-A, Mg2+ and SO42-) that could be related to the seas of Mars and other moons in the solar system. In addition, forsterite-91 was a very common mineral on the prebiotic Earth and Mars. Two important results are reported in this work: 1) thiocyanate adsorbed onto forsterite-91 and 2) the amount of thiocyanate adsorbed, adsorption thermodynamic, and adsorption kinetic depend on the composition of the artificial seawater. For all experiments, the adsorption was thermodynamically favorable (ΔG < 0). The adsorption data fitted well in the Freundlich and Langmuir-Freundlich models. When dissolving thiocyanate in seawater 4.0-A-Gy and seawater 4.0-B-Gy, the adsorption of thiocyanate onto forsterite-91 was ruled by enthalpy and entropy, respectively. As shown by n values, the thiocyanate/foraterite-91 system is heterogeneous. For all kinetic data, the pseudo-first-order model presented the best fit. The constant rate for thiocyanate dissolved in seawater 4.0-A-Gy was twice that compared to thiocyanate dissolved in seawater 4.0-B-Gy or ultrapure-water. The interaction between thiocyanate and Fe2+ of forsterite-91 was with the nitrogen atom of thiocyanate. In the presence of thiocyanate, sulfate interacts with forsterite-91 as an inner-sphere surface complex, and without thiocyanate as an outer-sphere surface complex.
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Sales (Química) , Tiocianatos , Adsorción , Prebióticos , Minerales , Agua de Mar , CinéticaRESUMEN
Biocatalytic copper centers are generally involved in the activation and reduction of dioxygen, with only few exceptions known. Here we report the discovery and characterization of a previously undescribed copper center that forms the active site of a copper-containing enzyme thiocyanate dehydrogenase (suggested EC 1.8.2.7) that was purified from the haloalkaliphilic sulfur-oxidizing bacterium of the genus Thioalkalivibrio ubiquitous in saline alkaline soda lakes. The copper cluster is formed by three copper ions located at the corners of a near-isosceles triangle and facilitates a direct thiocyanate conversion into cyanate, elemental sulfur, and two reducing equivalents without involvement of molecular oxygen. A molecular mechanism of catalysis is suggested based on high-resolution three-dimensional structures, electron paramagnetic resonance (EPR) spectroscopy, quantum mechanics/molecular mechanics (QM/MM) simulations, kinetic studies, and the results of site-directed mutagenesis.
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Proteínas Bacterianas/química , Dominio Catalítico , Cobre/química , Ectothiorhodospiraceae/enzimología , Oxidorreductasas/química , Bacterias Reductoras del Azufre/enzimología , Biocatálisis , Espectroscopía de Resonancia por Spin del Electrón , Concentración de Iones de Hidrógeno , Oxidación-Reducción , Oxígeno/química , Azufre/químicaRESUMEN
Cancer still represents one of the biggest challenges in current medical practice. Among different types of cancer, oral cancer has a huge impact on patients due to its great visibility, which is more likely to create social stigma and increased anxiety. New early diagnose methods are still needed to improve treatment efficiency and patients' life quality. Raman/SERS (Surface Enhanced Raman Spectroscopy) spectroscopy has a unique and powerful potential for detecting specific molecules that can become priceless biomarkers in different pathologies, such as oral cancer. In this study, a batch of saliva samples obtained from a group of 17 patients with oro-maxillofacial pathologies compared with saliva samples from 18 healthy donors using the aforementioned methods were evaluated. At the same time, opiorphin, potassium thiocyanate and uric acid were evaluated as potential specific biomarkers for oro-maxillofacial pathologies using multivariate analysis. A careful examination of SERS spectra collected on saliva samples showed that the spectra are dominated by the vibrational bands of opiorphin, potassium thiocyanate and uric acid. Given the fact that all these small molecules are found in very small amounts, we filtrated all the samples to get rid of large molecules and to improve our analysis. By using solid plasmonic substrates, we were able to gain information about molecular concentration and geometry of interaction. On the other hand, the multivariate analysis of the salivary spectra contributed to developing a new detection method for oral cancer.
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Neoplasias de la Boca , Ácido Úrico , Humanos , Neoplasias de la Boca/diagnóstico , Tiocianatos , Biomarcadores , Espectrometría Raman/métodosRESUMEN
The first three compounds based on a {copper-thiocyanate-dabco} combination, namely, (Hdabco)[Cu2(NCS)3] (1), (H2dabco)[Cu(NCS)3] (2), and [Cu(Hdabco)2(NCS)4]â2dmso (3), where dabco = 1,4-diazabicyclo[2.2.2]octane were synthesized and characterized by single-crystal XRD, elemental analysis, Raman, and partial IR spectroscopy. In copper(I) derivatives, the influence of the charge of the organic cation on the dimensionality of the crystal structure is observed. Thus, in the case of 1, monoprotonated Hdabco+ cations provide the template for the formation of a polymeric anionic 3D framework {[Cu2(NCS)3]-}n, while in the case of 2, diprotonated H2dabco2+ cations together with discrete [Cu(SCN)3]2- anions generate a simple ionic 0D structure with an island-like crystal lattice. The anionic {[Cu2(SCN)3]-}n framework has infinite square channels of 10 × 10 Å size running along the 001 crystallographic direction. In 3, both the Hdabco+ and thiocyanato units behave as terminal monodentate ligands attached to copper(II) centers via N-donor atoms, forming neutral molecular complexes with an elongated (4+2) octahedral environment. The crystallization molecules of dmso are hydrogen bonded to the protonated parts of the coordinated dabco molecules. A series of by-products Cu(SCN)2(dmso)2 (4), (Hdabco)SCN (5), (H2dabco)(SCN)2 (6), and (H2dabco)(SCN)2âH2O (7) were identified and characterized.
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Organothiocyanates and selenocyanates are valuable compounds, both in terms of functional group interconversion and due to their biological activities. In this contribution, we report the synthesis of a series of these important substances in a mixture of water and dimethyl carbonate (20/1 proportion) using potassium thio- or selenocyanates salts and organic bromides. The key to the effectiveness of the reaction is a chalcogen bond interaction between a selenonium salt catalyst and the organic substrate.
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A series of cyclometalated complexes of ruthenium (II) with four different substituents in the aryl fragment of benzimidazole was synthesized in order to study the effect of substituent donation on the electronic structure of the substances. The resulting complexes were studied using X-ray diffraction, NMR spectroscopy, MALDI mass spectrometry, electron absorption spectroscopy, luminescence spectroscopy, and cyclic voltammetry as well as DFT/TDDFT was also used to interpret the results. All the complexes have intense absorption in the range of up to 700 nm, the triplet nature of the excited state was confirmed by measurement of luminescence decay. With an increase in substituent donation, a red shift of the absorption and emission bands occurs, and the lifetime of the excited state and the redox potential of the complex decrease. The combination of these properties shows that the complexes are excellent dyes and can be used as photosensitizers.