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1.
Angew Chem Int Ed Engl ; 63(17): e202401372, 2024 Apr 22.
Artículo en Inglés | MEDLINE | ID: mdl-38390783

RESUMEN

Herein, we present the first report on the synthesis of rare-earth complexes featuring a 9,10-diborataanthracene ligand. This 14-π-electron ligand is highly reductive and was previously used in small-molecule activation. Salt elimination reactions between dipotassium 9,10-diethyl-9,10-diborataanthracene [K2(DEDBA)] and [LnIII(η8-CotTIPS)(BH4)(thf)x] (CotTIPS=1,4-(iPr3Si)2C8H6) in a 1 : 1 ratio yielded heteroleptic sandwich complexes [K(η8-CotTIPS)LnIII(η6-DEDBA)] (Ln=Y, Dy, Er). These compounds form Lewis-base-free one-dimensional coordination polymers when crystallised from toluene. In contrast, reaction of [K2(DEDBA)] and [LnIII(η8-CotTIPS)(BH4)(thf)x] in a 1 : 2 ratio led to the formation of heteroleptic triple-decker complexes [(η8-CotTIPS)LnIII(µ-η6:η6-DEDBA)LnIII(η8-CotTIPS)] (Ln=Y, Dy, Er). Notably, these are not only the first lanthanide triple-decker compounds featuring a six-membered ring as a deck but also the first trivalent lanthanide triple-decker featuring a heterocycle in the coordination sphere. Magnetic investigations reveal that [K(η8-CotTIPS)LnIII(η6-DEDBA)] (Ln=Dy, Er) and [(η8-CotTIPS)ErIII(µ-η6:η6-DEDBA)ErIII(η8-CotTIPS)] exhibit Single-Molecule Magnet (SMM) behaviour. In the case of [(η8-CotTIPS)LnIII(µ-η6:η6-DEDBA)LnIII(η8-CotTIPS)] (Ln=Dy, Er), the introduction of a second near lanthanide ion results in strong antiferromagnetic interactions, allowing the enhancement of the magnetic characteristic of the system, compared to the quasi isolated counterpart. This research renews the overlooked coordination chemistry of the DBA ligand and expands it to encompass rare-earth elements.

2.
Food Chem ; 445: 138682, 2024 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-38350196

RESUMEN

Food matrices greatly impact TBBQ content during digestion, while lacking sufficient research and understanding. This study investigated the influence and mechanism of fried foods on the TBBQ-eliminated performance during in-vitro digestion. The results indicated that TBBQ content varied significantly among food matrices after in-vitro digestion, with the highest in peanuts (38.3%). The correlation analysis revealed that proteins remarkably facilitated TBBQ-eliminations while fats decreased the TBBQ-eliminated rate. The TBBQ-eliminated performance of proteins, protein digestive mixtures, and amino acids uncovered that sulfhydryl groups were crucial reactive groups to eliminate TBBQ, and TBBQ-eliminated rates under intestinal pH (8.0) were faster than gastric pH (1.5). Additionally, fats significantly reduced the protein-triggered TBBQ-eliminations, originating that the oil-water interface increased the interaction difficulty between lipophilic TBBQ and proteins. Thus, this work provided an in-depth understanding of food matrices (especially proteins and fats) in TBBQ eliminations to enlighten the promising TBBQ-risk-reduced strategies with high-protein and low-fat foods.


Asunto(s)
Alimentos , Intestinos , Digestión
3.
Chemosphere ; 346: 140606, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-37939928

RESUMEN

H2O2 is widely used in the treatment of refractory organic pollutants.However, due to its explosive and corrosive chemical characteristics, H2O2 will bring great safety risks and troubles in transportation.So we chose sodium percarbonate(SPC) to be used in catalytic wet peroxide oxidation enhanced by swirl flow(SF-CWPO) and we designed carbon nanotubes with Ni single atom sites(Ni-NCNTs/AC) to activate SPC to treat an m-cresol wastewater containing Si.Meanwhile, artificial intelligence which used Artificial neural network (ANN) was used to optimize the conditions.Under the conditions of pH = 9.27, reaction time of 8.91 min, m-cresol concentration is 59.09 mg L-1, SPC dosage is 2.80 g L-1 and Na2SiO3·9H2O dosage is 77.27 mg L-1, the degradation rate of total organic carbon(TOC) and m-cresol reaches 94.37% and 100%, respectively.Finally, the applicability of Ni-NCNTs/AC-SPC-SF-CWPO technology was evaluated in a wastewater system of a sewage treatment enterprise and Fourier transform ion cyclotron resonance mass spectrum(FT-ICR MS) analysis and chemical oxygen demand(COD) analysis showed the great ability of Ni-NCNTs/AC-SPC-SF-CWPO technology to treat wastewater.It is believed that this paper is of great significance to the design and construction of the in-depth research and industrial application of SF-CWPO.


Asunto(s)
Nanotubos de Carbono , Contaminantes Químicos del Agua , Peróxido de Hidrógeno , Aguas Residuales , Silicio , Inteligencia Artificial , Peróxidos , Oxidación-Reducción , Catálisis
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