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1.
Nano Lett ; 2024 Jun 10.
Artículo en Inglés | MEDLINE | ID: mdl-38856118

RESUMEN

Copper-based catalysts have been attracting increasing attention for CO2 electroreduction into value-added multicarbon chemicals. However, most Cu-based catalysts are designed for ethylene production, while ethanol production with high Faradaic efficiency at high current density still remains a great challenge. Herein, Cu clusters supported on single-atom Cu dispersed nitrogen-doped carbon (Cux/Cu-N/C) show ethanol Faradaic efficiency of ∼40% and partial current density of ∼350 mA cm-2. Quasi in situ X-ray photoelectron spectroscopy and operando X-ray absorption spectroscopy results suggest the generation of surface asymmetrical sites of Cu+ and Cu0 as well as Cu clusters by electrochemical reduction and reconstruction during the CO2 electroreduction process. Density functional theory calculations indicate that the interaction between Cu clusters and the Cu-N/C support enhances *CO adsorption, facilitates the C-C coupling step, and favors the hydrogenation rather than dehydroxylation of the critical intermediate *CHCOH toward ethanol in the bifurcation.

2.
Carbohydr Polym ; 334: 122019, 2024 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-38553218

RESUMEN

Gleditsia fruits have been known as a valuable traditional Chinese herb for tens of centuries. Previous studies showed that the galactomannans are considered as one of the major bioactive components in Gleditsia fruits seeds (GSGs). Here, we systematically review the major studies of GSGs in recent years to promote their better understanding. The extraction methods of GSGs mainly include hot water extraction, microwave-assisted extraction, ultrasonic extraction, acid extraction, and alkali extraction. The analysis revealed that GGSs exhibited in the form of semi-flexible coils, and its molecular weight ranged from 0.018 × 103 to 2.778 × 103 KDa. GSGs are composed of various monosaccharide constituents such as mannose, galactose, glucose, and arabinose. In terms of pharmacological effects, GSGs exhibit excellent activity in antioxidation, hypoglycemic, hypolipidemic, anti-inflammation. Moreover, GSGs have excellent bioavailability, biocompatibility, and biodegradability, which make them used in food additives, food packaging, pharmaceutical field, industry and agriculture. Of cause, the shortcomings of the current research and the potential development and future research are also highlighted. We believe our work provides comprehensive knowledge and underpinnings for further research and development of GSGs.


Asunto(s)
Galactosa/análogos & derivados , Gleditsia , Gleditsia/química , Mananos/química , Semillas/química , Frutas , Polisacáridos
3.
Angew Chem Int Ed Engl ; 62(45): e202309893, 2023 Nov 06.
Artículo en Inglés | MEDLINE | ID: mdl-37747793

RESUMEN

Electrochemically converting CO2 to valuable chemicals holds great promise for closing the anthropogenic carbon cycle. Owing to complex reaction pathways and shared rate-determining steps, directing the selectivity of CO2 /CO electrolysis to a specific multicarbon product is very challenging. We report here a strategy for highly selective production of acetate from CO electrolysis by constructing metal-organic interfaces. We demonstrate that the Cu-organic interfaces constructed by in situ reconstruction of Cu complexes show very impressive acetate selectivity, with a high Faradaic efficiency of 84.2 % and a carbon selectivity of 92.1 % for acetate production, in an alkaline membrane electrode assembly electrolyzer. The maximum acetate partial current density and acetate yield reach as high as 605 mA cm-2 and 63.4 %, respectively. Thorough structural characterizations, control experiments, operando Raman spectroscopy measurements, and density functional theory calculation results indicate that the Cu-organic interface creates a favorable reaction microenvironment that enhances *CO adsorption, lowers the energy barrier for C-C coupling, and facilitates the formation of CH3 COOH over other multicarbon products, thus rationalizing the selective acetate production.

4.
Nat Nanotechnol ; 18(3): 299-306, 2023 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-36635334

RESUMEN

Tuning catalyst microenvironments by electrolytes and organic modifications is effective in improving CO2 electrolysis performance. An alternative way is to use mixed CO/CO2 feeds from incomplete industrial combustion of fossil fuels, but its effect on catalyst microenvironments has been poorly understood. Here we investigate CO/CO2 co-electrolysis over CuO nanosheets in an alkaline membrane electrode assembly electrolyser. With increasing CO pressure in the feed, the major product gradually switches from ethylene to acetate, attributed to the increased CO coverage and local pH. Under optimized conditions, the Faradaic efficiency and partial current density of multicarbon products reach 90.0% and 3.1 A cm-2, corresponding to a carbon selectivity of 100.0% and yield of 75.0%, outperforming thermocatalytic CO hydrogenation. The scale-up demonstration using an electrolyser stack achieves the highest ethylene formation rate of 457.5 ml min-1 at 150 A and acetate formation rate of 2.97 g min-1 at 250 A.

5.
Angew Chem Int Ed Engl ; 61(5): e202114238, 2022 Jan 26.
Artículo en Inglés | MEDLINE | ID: mdl-34859554

RESUMEN

The electrochemical CO2 reduction reaction (CO2 RR) over Cu-based catalysts shows great potential for converting CO2 into multicarbon (C2+ ) fuels and chemicals. Herein, we introduce an A2 M2 O7 structure into a Cu-based catalyst through a solid-state reaction synthesis method. The Cu2 P2 O7 catalyst is electrochemically reduced to metallic Cu with a significant structure evolution from grain aggregates to highly porous structure under CO2 RR conditions. The reconstructed Cu2 P2 O7 catalyst achieves a Faradaic efficiency of 73.6 % for C2+ products at an applied current density of 350 mA cm-2 , remarkably higher than the CuO counterparts. The reconstructed Cu2 P2 O7 catalyst has a high electrochemically active surface area, abundant defects, and low-coordinated sites. In situ Raman spectroscopy and density functional theory calculations reveal that CO adsorption with bridge and atop configurations is largely improved on Cu with defects and low-coordinated sites, which decreased the energy barrier of the C-C coupling reaction for C2+ products.

6.
Foods ; 10(11)2021 Nov 11.
Artículo en Inglés | MEDLINE | ID: mdl-34829055

RESUMEN

Ultrasound-assisted enzymatic treatment was used to treat Newhall navel orange peel and residue, and then the structural, physicochemical and functional properties of extracted soluble dietary fibers (SDF) and insoluble dietary fibers (IDF) were investigated. The structural properties were determined using scanning electron microscopy, X-ray diffraction, FT-IR and monosaccharide composition. Among these dietary fibers, residue-SDF showed a more complex structure, while peel-IDF exhibited a looser structure. Four samples showed representative infrared spectral features of polysaccharides, typical cellulose crystalline structure and diverse monosaccharide composition. Furthermore, residue-IDF exhibited higher oil-holding capacity (2.08 g/g), water-holding capacity (13.43 g/g) and nitrite ion adsorption capacity (NIAC) than other three samples, and residue-SDF showed the highest swelling capacity (23.33 mL/g), cation exchange capacity (0.89 mmol/g) and cholesterol adsorption capacity (CAC) among these dietary fibers. In summary, this study suggests that the residue-SDF and residue-IDF could be used as the ideal dietary fibers for application in the functional food industry.

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