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1.
Chem Sci ; 15(5): 1611-1637, 2024 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-38303948

RESUMO

More than 8 billion tons of plastics have been generated since 1950. About 80% of these plastics have been dumped in landfills or went into natural environments, resulting in ever-worsening contamination. Among various strategies for waste plastics processing (e.g., incineration, mechanical recycling, thermochemical conversion and electrocatalytic/photocatalytic techniques), photocatalysis stands out as a cost-effective, environmentally benign and clean technique to upcycle plastic waste at ambient temperature and pressure using solar light. The mild reaction conditions for photocatalysis enable the highly selective conversion of plastic waste into targeted value-added chemicals/fuels. Here, we for the first time summarize the recent development of photocatalytic plastic upcycling based on the chemical composition of photocatalysts (e.g., metal oxides, metal sulfides, non-metals and composites). The pros and cons of various photocatalysts have been critically discussed and summarized. At last, the future challenges and opportunities in this area are presented in this review.

2.
Adv Mater ; 35(19): e2210164, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36828483

RESUMO

Solar hydrogen (H2 ) generation via photocatalytic water splitting is practically promising, environmentally benign, and sustainably carbon neutral. It is important therefore to understand how to controllably engineer photocatalysts at the atomic level. In this work, atomic-level engineering of defected ReSe2 nanosheets (NSs) is reported to significantly boost photocatalytic H2 evolution on various semiconductor photocatalysts including TiO2 , CdS, ZnIn2 S4 , and C3 N4 . Advanced characterizations, such as atomic-resolution aberration-corrected scanning transmission electron microscopy (AC-STEM), synchrotron-based X-ray absorption near edge structure (XANES), in situ X-ray photoelectron spectroscopy (XPS), transient-state surface photovoltage (SPV) spectroscopy, and transient-state photoluminescence (PL) spectroscopy, together with theoretical computations confirm that the strongly coupled ReSe2 /TiO2 interface and substantial atomic-level active sites of defected ReSe2 NSs result in the significantly raised activity of ReSe2 /TiO2 . This work not only for the first time realizes the atomic-level engineering of ReSe2 NSs as a versatile platform to significantly raise the activities on different photocatalysts, but, more importantly, underscores the immense importance of atomic-level synthesis and exploration on 2D materials for energy conversion and storage.

3.
Int J Biol Macromol ; 166: 1301-1311, 2021 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-33161085

RESUMO

A zeolitic imidazolate framework (ZIF-90) has been synthesized through solvothermal method. The structure was characterized by means of FT-IR spectroscopy, X-ray diffraction, thermogravimetric analysis (TGA), and scanning electron microscopy (SEM)/energy dispersive X-ray spectroscopy (EDS). The synthesized ZIF-90 was applied as a support for immobilization of porcine pancreatic lipase (PPL). The immobilized enzyme (PPL@ZIF-90) exhibited immobilization yield and efficiency of 66 ± 1.8% and 89 ± 1.4%, respectively. The pH and thermal stability of PPL was improved after immobilization and the initial activity was retained at about 57% after 20 days of storage at 4 °C for PPL@ZIF-90. Moreover, about 57% of the original activity was remained following 10 cycles of application. In Michaelis-Menten kinetic studies, Km value for PPL@ZIF-90 was lower, while, the Vmax was higher than free PPL. Moreover, optimized conditions to produce fruity banana flavour upon esterification of butyric acid were investigated. The optimum esterification yield was 73.79 ± 1.31% in the presence of 245 mg PPL@ZIF-90, alcohol/acid ratio of 2.78 and 39 h reaction time. PPL@ZIF-90 showed 39% relative esterification yield after six cycles of reuse. The results suggested that PPL@ZIF-90 can be used as a potential effective biocatalyst for synthesis of isoamyl butyrate.


Assuntos
Biocatálise , Enzimas Imobilizadas/química , Aromatizantes/síntese química , Lipase/química , Estruturas Metalorgânicas/química , Butiratos/química , Estabilidade Enzimática , Enzimas Imobilizadas/metabolismo , Esterificação , Imidazóis/química , Lipase/metabolismo , Musa/química
4.
J Hazard Mater ; 386: 121950, 2020 03 15.
Artigo em Inglês | MEDLINE | ID: mdl-31881496

RESUMO

Bisphenol A (BPA) is an environmental pollutant with adverse effects on different ecosystems. In this study, immobilized laccase enzymes onto inorganic supports were used to remove BPA. Laccase was successfully immobilized on sodium zeolite Y (NaY) and its modified desilicated (DSY) and dealuminated (DAY) forms. NaY-based supports were instrumentally characterized. The immobilized laccase on NaY (laccase@NaY), desilicated (laccase@DSY), and dealuminated (laccase@DAY) forms showed significant improvement on immobilization yield (IY%) and efficiency (IE%). Laccase@DSY and laccase@NaY showed IY% = 73.18 ±â€¯3.33 % and 46.23 ±â€¯1.81 % and IE% = 94.50 ±â€¯1.86 %, and 74.39 ±â€¯1.41 %, respectively, whereas IY% and IE% for laccase@DAY were achieved as 81.12 ±â€¯1.32 % and 98.56 ±â€¯2.93 %, respectively. The supports also increased the enzyme characteristics such as pH-temperature range, catalytic stability, and reusability. Km values were 0.73 ±â€¯0.05, 0.26 ±â€¯0.09, 0.31 ±â€¯0.5, and 1.01 ±â€¯0.03 mM for laccase@NaY, laccase@DAY, laccase@DSY, and the free enzyme, respectively. The enzyme demonstrated higher biodegradation ability of bisphenol A upon immobilization on the supports compared to that of the soluble enzyme. A bio-removal yield of 86.7 % was obtained considering three parameters including amount of laccase@DAY (8 U mg-1), concentration of BPA (0.5 mM), and treatment time (1 h) based on response surface methodology (RSM). Biodegradation metabolites (49 ±â€¯5.8 %) and unconverted BPA (14 ±â€¯5.2 %) were analyzed by gas chromatography-mass spectrometry.


Assuntos
Compostos Benzidrílicos/análise , Disruptores Endócrinos/análise , Poluentes Ambientais/análise , Enzimas Imobilizadas/metabolismo , Lacase/metabolismo , Fenóis/análise , Zeolitas/química , Compostos Benzidrílicos/metabolismo , Biocatálise , Biodegradação Ambiental , Disruptores Endócrinos/metabolismo , Poluentes Ambientais/metabolismo , Estabilidade Enzimática , Concentração de Íons de Hidrogênio , Cinética , Fenóis/metabolismo , Trametes/enzimologia
5.
Front Chem ; 6: 573, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-30534550

RESUMO

The last 20 years have seen an unprecedented breakthrough in the biodiesel industry worldwide leads to abundance of glycerol. Therefore, the economic utilization of glycerol to various value-added chemicals is vital for the sustainability of the biodiesel industry. One of the promising processes is acetalization of glycerol to acetals and ketals for applications as fuel additives. These products could be obtained by acid-catalyzed reaction of glycerol with aldehydes and ketones. Application of different supported heterogeneous catalysts such as zeolites, heteropoly acids, metal-based and acid-exchange resins have been evaluated comprehensively in this field. In this review, the glycerol acetalization has been reported, focusing on innovative and potential technologies for sustainable production of solketal. In addition, the impacts of various parameters such as application of different reactants, reaction temperature, water removal, utilization of crude-glycerol on catalytic activity in both batch and continuous processes are discussed. The outcomes of this research will therefore significantly improve the technology required in tomorrow's bio-refineries. This review provides spectacular opportunities for us to use such renewables and will consequently benefit the industry, environment and economy.

6.
Waste Manag ; 73: 256-264, 2018 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-29150259

RESUMO

As the world's second largest palm oil producer and exporter, Malaysia could capitalize on its oil palm biomass waste for power generation. The emission factors from this renewable energy source are far lower than that of fossil fuels. This study applies an integrated carbon accounting and mitigation (INCAM) model to calculate the amount of CO2 emissions from two biomass thermal power plants. The CO2 emissions released from biomass plants utilizing empty fruit bunch (EFB) and palm oil mill effluent (POME), as alternative fuels for powering steam and gas turbines, were determined using the INCAM model. Each section emitting CO2 in the power plant, known as the carbon accounting center (CAC), was measured for its carbon profile (CP) and carbon index (CI). The carbon performance indicator (CPI) included electricity, fuel and water consumption, solid waste and waste-water generation. The carbon emission index (CEI) and carbon emission profile (CEP), based on the total monthly carbon production, were determined across the CPI. Various innovative strategies resulted in a 20%-90% reduction of CO2 emissions. The implementation of reduction strategies significantly reduced the CO2 emission levels. Based on the model, utilization of EFB and POME in the facilities could significantly reduce the CO2 emissions and increase the potential for waste to energy initiatives.


Assuntos
Dióxido de Carbono/análise , Centrais Elétricas , Biomassa , Carbono , Malásia
7.
Bioresour Technol ; 136: 565-73, 2013 May.
Artigo em Inglês | MEDLINE | ID: mdl-23567732

RESUMO

The synthesis of fatty acid ethyl esters (FAEEs) by a two-step in situ (reactive) esterification/transesterification from Jatropha curcas L. (JCL) seeds using microwave system has been investigated. Free fatty acid was reduced from 14% to less than 1% in the first step using H2SO4 as acid catalyst after 35 min of microwave irradiation heating. The organic phase in the first step was subjected to a second reaction by adding 5 N KOH in ethanol as the basic catalyst. Response surface methodology (RSM) based on central composite design (CCD) was utilized to design the experiments and analyze the influence of process variables (particles seed size, time of irradiation, agitation speed and catalyst loading) on conversion of triglycerides (TGs) in the second step. The highest triglycerides conversion to fatty acid ethyl esters (FAEEs) was 97.29% at the optimum conditions:<0.5mm seed size, 12.21 min irradiation time, 8.15 ml KOH catalyst loading and 331.52 rpm agitation speed in the 110 W microwave power system.


Assuntos
Biocombustíveis , Biotecnologia/métodos , Jatropha/metabolismo , Micro-Ondas , Sementes/metabolismo , Análise de Variância , Catálise , Ésteres/metabolismo , Ácidos Graxos/metabolismo , Probabilidade , Análise de Regressão , Fatores de Tempo
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