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1.
J Phys Chem Lett ; 15(21): 5728-5737, 2024 May 30.
Artículo en Inglés | MEDLINE | ID: mdl-38771736

RESUMEN

Nitrogen-doped carbon dots (NCDs) featuring primary pyrrolic N and pyridinic N dominated configurations were prepared using hydrothermal (H-NCDs) and microwave (M-NCDs) methods, respectively. These H-NCDs and M-NCDs were subsequently applied to decorate CsPbBr3 nanocrystals (CPB NCs) individually, using a ligand-assisted reprecipitation process. Both CPB/M-NCDs and CPB/H-NCDs nanoheterostructures (NHSs) exhibited S-scheme charge transfer behavior, which enhanced their performance in photocatalytic CO2 reduction and selectivity of CO2-to-CH4 conversion, compared to pristine CPB NCs. The presence of pyrrolic N configuration at the heterojunction of CPB/H-NCDs facilitated efficient S-scheme charge transfer, leading to a remarkable 43-fold increase in photoactivity. In contrast, CPB/M-NCDs showed only a modest 3-fold enhancement in photoactivity, which was attributed to electron trapping by pyridinic N at the heterojunction. The study offers crucial insights into charge carrier dynamics within perovskite/carbon NHSs at the molecular level to advance the understanding of solar fuel generation.

2.
Chemosphere ; 341: 140118, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-37690552

RESUMEN

To maintain a comfortable and healthy indoor environment without large amounts of energy consumption is of great importance. The progress of multifunctional indoor coatings with formaldehyde photodegradation and humidity buffering capability is necessary. From the viewpoints of circular economy, the preparation of effective photocatalysts (denoted as sFCC/GCN-x and ESF/GCN-y) via the decoration of recycling industrial wastes (i.e., spent fluid catalytic cracking catalysts (sFCC) and enhancement silica fume (ESF)) onto graphitic carbon nitride (GCN) by using a simple route is reported. The obtained results show that the prepared sFCC/GCN-0.15 and ESF/GCN-0.15 photocatalysts have the rate constants of formaldehyde degradation of 0.0075 and 0.0082 min-1, respectively, which are superior to that of pristine GCN (0.0044 min-1) under visible-light irradiation. The enhanced transfer kinetics of photogenerated electrons and declined recombination of electron-hole pairs may account for the surpassing photocatalytic performance. Results obtained from electron paramagnetic resonance spectra and Mott-Schottky plots indicate that the formation of ï½¥O2- via the reaction of O2 with electrons generated on the conduction band is the major reaction pathway to photodegrade formaldehyde under visible light. To further assess the real applications of prepared photocatalysts, the sFCC/GCN-0.15 and ESF/GCN-0.15 are used to fabricate the multifunctional coatings (denoted as s- and E-coatings) with sFCC and ESF as the main compositions. Experimentally, the E-coatings could reach the formaldehyde degradation efficiency of ca. 84.5% after 3 h of visible light irradiation and excellent humidity buffering ability (293.8 g m-2) which is at least 10-folds higher than commercial coatings (28.9 g m-2). This notable progress of humidity buffering capacity on E-coatings can be attributed to their surface textural properties. Most importantly, this study exemplifies the valorization of inorganic silica wastes to produce sustainable and multifunctional coatings which may offer the practical and cost-effective applications in the indoor living space.


Asunto(s)
Formaldehído , Catálisis , Gases , Humedad , Fotólisis
3.
J Phys Chem Lett ; 14(1): 122-131, 2023 Jan 12.
Artículo en Inglés | MEDLINE | ID: mdl-36574643

RESUMEN

The photon energy-dependent selectivity of photocatalytic CO2-to-CO conversion by CsPbBr3 nanocrystals (NCs) and CsPbBr3/g-C3N4 nanoheterostructures (NHSs) was demonstrated for the first time. The surficial capping ligands of CsPbBr3 NCs would adsorb CO2, resulting in the carboxyl intermediate to process the CO2-to-CO conversion via carbene pathways. The type-II energy band structure at the heterojunction of CsPbBr3/g-C3N4 NHSs would separate the charge carriers, promoting the efficiency in photocatalytic CO2-to-CO conversion. The electron consumption rate of CO2-to-CO conversion for CsPbBr3/g-C3N4 NHSs was found to intensively depend on the rate constant of interfacial hole transfer from CsPbBr3 to g-C3N4. An in situ transient absorption spectroscopy investigation revealed that the half-life time of photoexcited electrons in optimized CsPbBr3/g-C3N4 NHS was extended two times more than that in the CsPbBr3 NCs, resulting in the higher probability of charge carriers to carry out the CO2-to-CO conversion. The current work presents important and novel insights of semiconductor NHSs for solar energy-driven CO2 conversion.

4.
Chemosphere ; 307(Pt 3): 135984, 2022 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-35964722

RESUMEN

Cu2O nanoparticles are decorated with biochars derived from spent coffee grounds (denoted as Cu2O/SCG) and applied as visible-light-active photocatalysts in the sulfamethoxazole (SMX) degradation. The physicochemical properties of Cu2O/SCG are identified by various spectral analysis, electrochemical and photochemical techniques. As a result, the Cu2O/SCG exhibits the higher removal efficiency of SMX than the pristine Cu2O under visible light irradiation. We can observe that Cu2O could be incorporated onto the SCG biochars with rich oxygen vacancies/adsorbed hydroxyl groups. In addition, the Cu2O/SCG has the lower charge transfer resistance, faster interfacial electron transfer kinetics, decreased recombination of charge carriers and superior absorbance of visible light. The construction of band diagrams for Cu2O/SCG and pristine Cu2O via UV-vis spectra and Mott-Schottky plots suggest that the band energy shifts and higher carrier density of Cu2O/SCG may be responsible for the photocatalytic activity enhancements. From the radical scavenger experiments and electron paramagnetic resonance spectra, the aforementioned energy shifts could decrease the energy requirement of transferring photoinduced electrons to the potential for the formation of active superoxide radicals (·O2-) via one and two-electron reduction routes in the photocatalytic reaction. A proposed degradation pathway shows that ·O2- and h+ are two main active species which can efficiently degrade SMX into reaction intermediates by oxidation, hydroxylation, and ring opening. This research demonstrates the alternative replacement of conventional carbon materials for the preparation of biochar-assisted Cu2O photocatalysts which are applied in the environmental decontamination by using solar energy.


Asunto(s)
Sulfametoxazol , Superóxidos , Carbono , Carbón Orgánico , Café , Luz , Oxígeno , Fotólisis , Sulfametoxazol/química
5.
J Colloid Interface Sci ; 592: 416-429, 2021 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-33691223

RESUMEN

Aerobic oxidation of 5-Hydroxymethylfurfural (HMF) to 2,5-Diformylfuran (DFF) using O2 gas represents a sustainable approach for valorization of lignocellulosic compounds. As manganese dioxide (MnO2) is validated as a useful oxidation catalyst and many crystalline forms of MnO2 exist, it is critical to explore how the crystalline structures of MnO2 influence their physical/chemical properties, which, in turn, determine catalytic activities of MnO2 crystals for HMF oxidation to DFF. In particular, six MnO2 crystals, α-MnO2, ß-MnO2, γ-MnO2, δ-MnO2, ε-MnO2, and λ-MnO2 are prepared and investigated for their catalytic activities for HMF oxidation to DFF. With different morphologies and crystalline structures, these MnO2 crystals possess very distinct surficial chemistry, redox capabilities, and textural properties, making these MnO2 exhibit different catalytic activities towards HMF conversion. Especially, ß-MnO2 can produce much higher DFF per surface area than other MnO2 crystals. ß-MnO2 could achieve the highest CHMF = 99% and YDFF = 97%, which are much higher than the reported values in literature, possibly because the surficial reactivity of ß-MnO2 appears to be highest in comparison to other MnO2 crystals. Especially, ß-MnO2 could exhibit YDFF > 90% over 5 cycles of reusability test, and maintain its crystalline structure, revealing its advantageous feature for aerobic oxidation of HMF to DFF. Through this study, the relationship between morphology, surface chemistry, and catalytic activity of MnO2 with different crystal forms is elucidated for providing scientific insights into design, application and development of MnO2-based materials for aerobic oxidation of bio-derived molecules to value-added products.

6.
Zhong Yao Cai ; 31(3): 410-2, 2008 Mar.
Artículo en Chino | MEDLINE | ID: mdl-18619250

RESUMEN

OBJECTIVE: To study the effects of HuDan Granules on lipid metabolism and antioxidant activity of mice with hyperlipidemia. METHODS: Seventy-eight mice were divided into six groups randomly: the normal control group, hyperlipemia group, HuDan Granules high, middle, low dose group and the Simvastatin group. Besides the normal control group, all the mice in the other groups were fed with lipid emulsion for 4 weeks. The Chinese medicine groups were treated with HuDan Granules at the dose of 12,6,3 g/kg, the normal control group and hyperlipemia group were treated with normal sodium, the Simvastatin group were treated with Simvastatin. After 4 weeks, the TC, TG, HDL-C, LDL-C, SOD, GSH-Px and LPO in serum were measured. RESULTS: HuDan Granules groups could significantly decrease the serum TC, TG, HDL-C in the experimental hyperlipidemia mice, and markedly increase the level of serum HDL-C. Mean level of serum LPO in the experimental groups treated by HuDan Granules at different dosages were much lower than that in hyperlipidemia group (P<0.05), but higher than the Simvastatin group (P<0.05). And the SOD and GSH-Px activities of serum in the group of HuDan Granules were much higher than those in hyperlipidemia group and the Simvastatin group (P<0.05). CONCLUSION: HuDan Granules can regulate lipid metabolism, enhance the antioxidation and reduce the lipid peroxidation in mice with hyperlipidemia.


Asunto(s)
Antioxidantes/farmacología , Medicamentos Herbarios Chinos/farmacología , Hiperlipidemias/tratamiento farmacológico , Metabolismo de los Lípidos/efectos de los fármacos , Animales , Antioxidantes/uso terapéutico , HDL-Colesterol/sangre , LDL-Colesterol/sangre , Quimioterapia Combinada , Medicamentos Herbarios Chinos/uso terapéutico , Femenino , Hiperlipidemias/sangre , Hiperlipidemias/metabolismo , Hipolipemiantes/farmacología , Hipolipemiantes/uso terapéutico , Peroxidación de Lípido/efectos de los fármacos , Masculino , Ratones , Fitoterapia , Distribución Aleatoria , Simvastatina/farmacología , Simvastatina/uso terapéutico , Superóxido Dismutasa/sangre , Triglicéridos/sangre
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