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1.
Angew Chem Int Ed Engl ; : e202409456, 2024 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-38976237

RESUMO

Extremely limited research exploring the photocatalytic potential of main group metals, such as aluminum, gallium, and tin, has been undertaken due to their weak light harvesting properties. This study reports the efficient transformation of sugars to 5-hydroxymethylfurfural (HMF) with high yield employing an original heterogenous photocatalyst comprising a gallium(III) complex immobilized on an alumina support. Under visible light irradiation, the reaction rate of HMF formation is ~143 times higher than the equivalent thermal reaction performed in the absence of light. The turnover number (TON) the heterogeneous gallium (III) photocatalyst was as high as 1500, which was two orders of magnitude higher than the TON of the homogeneous gallium (III) system. It is proposed that photoirradiation significantly enhances the Lewis acidity of the catalyst by forming a semi-coordination state between gallium(III) and N-donor ligands, enabling the increased interaction of reactant sugar molecules with gallium(III) active sites. Consistent with this, the photoresponsive coordination of the gallium(III) complex and the abstraction of the hydroxy group by the metal under irradiation with visible light is observed by NMR spectroscopy for the first time. These findings demonstrate that efficient photocatalysts derived from the main group elements can facilitate biomass conversion using visible light.

2.
Nat Commun ; 14(1): 4609, 2023 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-37528080

RESUMO

5-hydroxymethylfurfural (HMF) is a valuable and essential platform chemical for establishing a sustainable, eco-friendly fine-chemical and pharmaceutical industry based on biomass. The cost-effective production of HMF from abundant C6 sugars requires mild reaction temperatures and efficient catalysts from naturally abundant materials. Herein, we report how fulvic acid forms complexes with Al3+ ions that exhibit solar absorption and photocatalytic activity for glucose conversion to HMF in one-pot reaction, in good yield (~60%) and at moderate temperatures (80 °C). When using representative components of fulvic acid, catechol and pyrogallol as ligands, 70 and 67% HMF yields are achieved, respectively, at 70 °C. Al3+ ions are not recognised as effective photocatalysts; however, complexing them with fulvic acid components as light antennas can create new functionality. This mechanism offers prospects for new green photocatalytic systems to synthesise a range of substances that have not previously been considered.

3.
Microbiol Resour Announc ; 12(4): e0003223, 2023 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-36972233

RESUMO

Brucellosis is a class B infectious disease that is spreading rapidly in Inner Mongolia, China. Investigating the genetics of this disease might provide insights into the mechanism by which the bacteria adapt to their hosts. Here, we report the genome sequence of Brucella melitensis strain BM6144, which was isolated from a human patient.

4.
Angew Chem Int Ed Engl ; 61(24): e202203158, 2022 Jun 13.
Artigo em Inglês | MEDLINE | ID: mdl-35344246

RESUMO

Surface-plasmon-mediated phenylacetylide intermediate transfer from the Cu to the Pd surface affords a novel mechanism for transmetalation, enabling wavelength-tunable cross-coupling and homo-coupling reaction pathway control. C-C bond forming Sonogashira coupling and Glaser coupling reactions in O2 atmosphere are efficiently driven by visible light over heterogeneous Cu and Pd nanoparticles as a mixed catalyst without base or other additives. The reaction pathway can be controlled by switching the excitation wavelength. Shorter wavelengths (400-500 nm) give the Glaser homo-coupling diyne, whereas longer wavelength irradiation (500-940 nm) significantly increases the degree of cross-coupling Sonogashira coupling products. The ratio of the activated intermediates of alkyne to the iodobenzene is wavelength dependent and this regulates transmetalation. This wavelength-tunable reaction pathway is a novel way to optimize the product selectivity in important organic syntheses.

5.
J Hazard Mater ; 382: 121111, 2020 01 15.
Artigo em Inglês | MEDLINE | ID: mdl-31563089

RESUMO

Hydrotalcite materials are generally utilized for anionic pollutants due to its interlayered anion exchange ability. Their potentiality for cationic contaminants is rarely explored. In this study, disulfide (S2-) intercalated LDH material demonstrated capability to remove both heavy metal cations and oxyanions simultaneously from water. The S2- intercalation of LDH significantly improved its adsorption capability towards both heavy metal cations (Co2+ and Ni2+) and oxyanion (CrO42-). The adsorption amount of S-LDH towards Co2+ and Ni2+ reached 88.6mg/g and 76.2mg/g, which are 405% and 281% higher than that of pristine LDH. For CrO42- removal, the adsorption amount reached 34.7mg/g, 402% higher than that of pristine LDH. The cations capture mechanism mainly depends on the novel layer sheet cation substitution mechanism based on irreversible precipitation and the generation of metal sulfide precipitates. Meanwhile, the interlayered S2- can be easily replaced by CrO42- to realize the simultaneous removal of both heavy metal cations and oxyanions. In the fixed-bed column experiments, 448 bed volume (BV) (672 mL) of simulating electroplating wastewater can be efficiently treated by yielding only 1 BV(15 mL) of chemical sludge, which is practically acceptable. This work provided a highly practical adsorption technology based on the S2- modification hydrotalcite material for the purification of heavy metal ions contaminated wastewater.

6.
Chem Commun (Camb) ; 52(77): 11567-70, 2016 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-27606378

RESUMO

Nanoparticles (NPs) of Pd and Pt were used for the selective oxidation of aliphatic alcohols with molecular oxygen as an oxidant at near ambient temperatures under visible light irradiation. Distinct final products were obtained under identical reaction conditions, aliphatic esters formed over the Pd NPs while aldehydes formed over the Pt NPs. The reason for this different product selectivity is proven to be due to the much stronger interaction of Pd NPs with alcohol and aldehyde compared to Pt NPs. The photocatalytic activity is tuneable by light intensity or a moderate change in the reaction temperature.

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