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Two novel cation-induced supramolecular polymers with 2-3D polymeric cuprous thiocyanate frameworks: Synthesis, characterization and photocatalytic activities for the degradation of organic dye contaminants

In order to systematically explore the photocatalytic activity of the inorganic-organic supramolecular polymers induced by 1,1?-(1,n-alkylidene)bis[4-methylpyridinium] (n = 1-2) cations, two novel cation-induced compounds, {(bmpm) [Cu2(SCN)4]}n (bmpm = 1,1?-methylenebis[4-methylpyridinium] (1) and {(bmpe) [Cu2(SCN)4]}n (bmpe = 1,1?-(1,2-ethanediyl)bis[4-methylpyridinium] (2) were obtained and characterized by X-ray crystallography. Compound 1 has a 3D framework with the cations trapped within host network cavities. Compound 2 possesses an infinite 2D supramolecular polypseudorotaxane structure linked by bridging thiocyanate groups. The third-order NLO, optical band gaps and photocatalytic activities of 1 and 2 were also evaluated. Remarkably, both 1 and 2 exhibited good photocatalytic abilities.

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Reference:
Copper catalysis in organic synthesis – NCBI,
Special Issue “Fundamentals and Applications of Copper-Based Catalysts”

 

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Structural characterisation of metal complexes containing 1-[(4-methylphenyl)sulfonamido]-2-[(2-pyridylmethylene)amino]benzene

The interaction of 2-pyridinecarboxaldehyde with N-tosyl-1,2-diaminobenzene leads to the isolation of two different products, {3-[ethoxy(2-pyridyl)methyl]-1-[(4-methylphenyl)sulfonyl]-2-(2-pyridyl)-2,3- dihydro-1H-benzo[d]imidazole}, L1, and {1-[(4-methylphenyl)sulfonyl]-2-(2-pyridyl)-2,3-dihydro-1H-benzo[d] imidazole}, L2, but not to the expected Schiff base 1-[(4-methylphenyl)sulfonamido]-2-[(2-pyridylmethylene)amino]benzene, HL3. Two kinds of complexes, containing the potentially tridentate and monoanionic [L3]- as a ligand, were obtained by different routes. ML3(p-Tos)(H2O)n complexes (p-TosH = p-toluenesulfonic acid; M = Co, Cu, Zn; n = 1-3) have been isolated by electrolysis of a solution phase composed of L1 and p-toluenesulfonic acid, using metal plates as the anode. Metal complexes of composition ML32(H2O)n (M = Mn, Co, Cu, Zn; n = 0-2) were obtained by template synthesis from M(acac)2, 2-pyridinecarboxaldehyde and N-tosyl-1,2-diaminobenzene. All these compounds have been characterised by elemental analyses, magnetic measurements, IR, mass spectrometry and, in the case of M = Zn, by 1H NMR spectroscopy. CuL3(p-Tos)(H2O), 1, ZnL3(p-Tos)(H2O), 2, CoL32, 3, CuL32, 4 and ZnL32 · 2CH3CN, 5, were also crystallographically characterised.

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Reference:
Copper catalysis in organic synthesis – NCBI,
Special Issue “Fundamentals and Applications of Copper-Based Catalysts”

 

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Triazapentadienes as acaricides

Certain heteroaryl triazapentadienes with acaricidal properties and their preparation are described.

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Reference:
Copper catalysis in organic synthesis – NCBI,
Special Issue “Fundamentals and Applications of Copper-Based Catalysts”

 

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Electronic Modulation of Electrocatalytically Active Center of Cu7S4 Nanodisks by Cobalt-Doping for Highly Efficient Oxygen Evolution Reaction

Cu-based electrocatalysts have seldom been studied for water oxidation because of their inferior activity and poor stability regardless of their low cost and environmentally benign nature. Therefore, exploring an efficient way to improve the activity of Cu-based electrocatalysts is very important for their practical application. Modifying electronic structure of the electrocatalytically active center of electrocatalysts by metal doping to favor the electron transfer between catalyst active sites and electrode is an important approach to optimize hydrogen and oxygen species adsorption energy, thus leading to the enhanced intrinsic electrocatalytic activity. Herein, Co-doped Cu7S4 nanodisks were synthesized and investigated as highly efficient electrocatalyst for oxygen evolution reaction (OER) due to the optimized electronic structure of the active center. Density-functional theory (DFT) calculations reveal that Co-engineered Cu7S4 could accelerate electron transfer between Co and Cu sites, thus decrease the energy barriers of intermediates and products during OER, which are crucial for enhanced catalytic properties. As expected, Co-engineered Cu7S4 nanodisks exhibit a low overpotential of 270 mV to achieve current density of 10 mA cm-2 as well as decreased Tafel slope and enhanced turnover frequencies as compared to bare Cu7S4. This discovery not only provides low-cost and efficient Cu-based electrocatalyst by Co doping, but also exhibits an in-depth insight into the mechanism of the enhanced OER properties.

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Reference:
Copper catalysis in organic synthesis – NCBI,
Special Issue “Fundamentals and Applications of Copper-Based Catalysts”

 

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Extending motifs in lithiocuprate chemistry: Unexpected structural diversity in thiocyanate complexes

The new area of lithio(thiocyanato)cuprates has been developed. Using inexpensive, stable and safe CuSCN for their preparation, these complexes revealed Lipshutz-type dimeric motifs with solvent-dependent point group identities; planar, boat-shaped and chair shaped conformers are seen in the solid state. In solution, both Lipshutz-type and Gilman structures are clearly seen. Since the advent in 2007 of directed ortho cupration, effort has gone into understanding the structure-reactivity effects of amide ligand variation in and alkali metal salt abstraction from Lipshutz-type cuprates such as (TMP)2Cu(CN)Li2(THF) 1 (TMP = 2,2,6,6-tetramethylpiperidide). The replacement of CN- with SCN- is investigated presently as a means of improving the safety of lithium cuprates. The synthesis and solid state structural characterization of reference cuprate (TMP)2Cu(CN)Li2(THP) 8 (THP = tetrahydropyran) precedes that of the thiocyanate series (TMP)2Cu(SCN)Li2(L) (L = OEt29, THF 10, THP 11). For each of 9-11, preformed TMPLi was combined with CuSCN (2 : 1) in the presence of sub-stoichiometric Lewis base (0.5 eq. wrt Li). The avoidance of Lewis basic solvents incurs formation of the unsolvated Gilman cuprate (TMP)2CuLi 12, whilst multidimensional NMR spectroscopy has evidenced the abstraction of LiSCN from 9-11 in hydrocarbon solution and the in situ formation of Gilman reagents. The synthetic utility of 10 is established in the selective deprotometalation of chloropyridine substrates, including effecting transition metal-free homocoupling in 51-69% yield.

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Reference:
Copper catalysis in organic synthesis – NCBI,
Special Issue “Fundamentals and Applications of Copper-Based Catalysts”

 

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Copper-Coupled Electron Transfer in Colloidal Plasmonic Copper-Sulfide Nanocrystals Probed by in Situ Spectroelectrochemistry

Copper-sulfide nanocrystals can accommodate considerable densities of delocalized valence-band holes, introducing localized surface plasmon resonances (LSPRs) attractive for infrared plasmonic applications. Chemical control over nanocrystal shape, composition, and charge-carrier densities further broadens their scope of potential properties and applications. Although a great deal of control over LSPRs in these materials has been demonstrated, structural complexities have inhibited detailed descriptions of the microscopic chemical processes that transform them from nearly intrinsic to degenerately doped semiconductors. A comprehensive understanding of these transformations will facilitate use of these materials in emerging technologies. Here, we apply spectroelectrochemical potentiometry as a quantitative in situ probe of copper-sulfide nanocrystal Fermi-level energies (EF) during redox reactions that switch their LSPR bands on and off. We demonstrate spectroscopically indistinguishable LSPR bands in low-chalcocite copper-sulfide nanocrystals with and without lattice cation vacancies and show that cation vacancies are much more effective than surface anions at stabilizing excess free carriers. The appearance of the LSPR band, the shift in EF, and the change in crystal structure upon nanocrystal oxidation are all fully reversible upon addition of outer-sphere reductants. These measurements further allow quantitative comparison of the coupled and stepwise oxidation/cation-vacancy-formation reactions associated with LSPRs in copper-sulfide nanocrystals, highlighting fundamental thermodynamic considerations relevant to technologies that rely on reversible or low-driving-force plasmon generation in semiconductor nanostructures.

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Reference:
Copper catalysis in organic synthesis – NCBI,
Special Issue “Fundamentals and Applications of Copper-Based Catalysts”

 

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3-Aryluracils having an ether (thio) carbomyloxy or sulphomyloxy substituent on the aromatic moiety

The invention is concerned with 3-aryluracils of the formula STR1 wherein R1, R2, R3, R4, R5 and R6 are as described herein, as well as salts thereof and their manufacture, weed control compositions which contain such compounds as the active substance and the use of the active substances or compositions for weed control. The invention is also concerned with herbicidally-active starting materials and weed control compositions containing these.

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Reference:
Copper catalysis in organic synthesis – NCBI,
Special Issue “Fundamentals and Applications of Copper-Based Catalysts”

 

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High- k Gate Dielectrics for Emerging Flexible and Stretchable Electronics

Recent advances in flexible and stretchable electronics (FSE), a technology diverging from the conventional rigid silicon technology, have stimulated fundamental scientific and technological research efforts. FSE aims at enabling disruptive applications such as flexible displays, wearable sensors, printed RFID tags on packaging, electronics on skin/organs, and Internet-of-things as well as possibly reducing the cost of electronic device fabrication. Thus, the key materials components of electronics, the semiconductor, the dielectric, and the conductor as well as the passive (substrate, planarization, passivation, and encapsulation layers) must exhibit electrical performance and mechanical properties compatible with FSE components and products. In this review, we summarize and analyze recent advances in materials concepts as well as in thin-film fabrication techniques for high-k (or high-capacitance) gate dielectrics when integrated with FSE-compatible semiconductors such as organics, metal oxides, quantum dot arrays, carbon nanotubes, graphene, and other 2D semiconductors. Since thin-film transistors (TFTs) are the key enablers of FSE devices, we discuss TFT structures and operation mechanisms after a discussion on the needs and general requirements of gate dielectrics. Also, the advantages of high-k dielectrics over low-k ones in TFT applications were elaborated. Next, after presenting the design and properties of high-k polymers and inorganic, electrolyte, and hybrid dielectric families, we focus on the most important fabrication methodologies for their deposition as TFT gate dielectric thin films. Furthermore, we provide a detailed summary of recent progress in performance of FSE TFTs based on these high-k dielectrics, focusing primarily on emerging semiconductor types. Finally, we conclude with an outlook and challenges section.

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Reference:
Copper catalysis in organic synthesis – NCBI,
Special Issue “Fundamentals and Applications of Copper-Based Catalysts”

 

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Synthesis, Crystal Structure and Chemical Reactivity of Dichloro(thiosemicarbazide)copper(II)

The structure of dichloro(thiosemicarbazide)copper(II), , has been determined by X-ray crystallography.Contrary to earlier proposals the compound is found to be monomeric.Electron spin resonance studies of the compound both as a polycrystalline solid and in dimethylformamide solution are also in accordance with a monomeric structure.The reactivity of towards some Lewis bases such as imidazole, 2,2′-bipyridyl etc. has also been studied.

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Reference:
Copper catalysis in organic synthesis – NCBI,
Special Issue “Fundamentals and Applications of Copper-Based Catalysts”

 

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Perfluoroalkylsulfonamidoaryl compounds

Phenyl-substituted perfluoroalkanesulfonanilides in which the phenyl rings are linked by sulfur, sulfinyl or sulfonyl and salts thereof in which the rings and the perfluoroalkylsulfonamido nitrogen are optionally substituted. The compounds are active herbicides and some are anti-inflammatory agents and analgesic agents.

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Reference:
Copper catalysis in organic synthesis – NCBI,
Special Issue “Fundamentals and Applications of Copper-Based Catalysts”