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1.
Environ Res ; 242: 117773, 2024 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-38029829

RESUMO

In this paper, a facile hydrothermal pretreatment and molten salt activation route was presented for preparing a self-doped porous biochar (HMBC) from a nitrogenous biomass precursor of water hyacinth. With an ultrahigh specific surface area (2240 m2 g-1), well-developed hierarchical porous structure, created internal structural defects and doped surface functionalities, HMBC exhibited an excellent adsorption performance and catalytic activity for phenol removal via peroxydisulfate (PDS) activation. Specifically, the porous structure promoted the adsorption of PDS on HMBC, forming a highly active HMBC/PDS* complex and thereby increasing the oxidation potential of the system. Meanwhile, the carbon defective structure, graphitic N and CO groups enhanced the electron transfer process, favoring the HMBC/PDS system to catalyze phenol oxidation via an electron transfer dominated pathway. Thus, the system degraded phenol effectively with an ultralow activation energy of 4.9 kJ mol-1 and a remarkable oxidant utilization efficiency of 8.2 mol mol-oxidant-1 h-1 g-1. More importantly, the system exhibited excellent resistance to water quality and good adaptability for decontaminating different organic pollutants with satisfactory mineralization efficiency. This study offers valuable insights into the rational designing of a low-cost biochar catalyst for efficient PDS activation towards organic wastewater remediation.


Assuntos
Carvão Vegetal , Eichhornia , Elétrons , Porosidade , Fenol , Oxidantes
2.
Nat Commun ; 14(1): 253, 2023 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-36650160

RESUMO

High-temperature molten-salt electrolyzers play a central role in metals, materials and chemicals production for their merit of favorable kinetics. However, a low-cost, long-lasting, and efficient high-temperature oxygen evolution reaction (HT-OER) electrode remains a big challenge. Here we report an iron-base electrode with an in situ formed lithium ferrite scale that provides enhanced stability and catalytic activity in both high-temperature molten carbonate and chloride salts. The finding is stemmed from a discovery of the ionic potential-stability relationship and a basicity modulation principle of oxide films in molten salt. Using the iron-base electrode, we build a kiloampere-scale molten carbonate electrolyzer to efficiently convert CO2 to carbon and oxygen. More broadly, the design principles lay the foundations for exploring cheap, Earth-abundant, and long-lasting HT-OER electrodes for electrochemical devices with molten carbonate and chloride electrolytes.

3.
Nanomaterials (Basel) ; 12(15)2022 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-35957017

RESUMO

Biochars are considered as promising materials in energy storage and environmental remediation because of their unique physicochemical properties and low cost. However, the fabrication of multifunctional biochar materials with a well-developed hierarchical porous structure as well as self-doped functionalities via a facile strategy remains a challenge. Herein, we demonstrate a heteroatom-doped porous biochar, prepared by a hydrothermal pretreatment followed by a molten salt activation route. With the creation of a high specific surface area (1501.9 m2/g), a hierarchical porous structure, and the incorporation of oxygen-/nitrogen-functional groups, the as-prepared biochar (BC-24) exhibits great potential for supercapacitor application and organic pollutant elimination. The assembled biochar electrode delivers a specific capacitance of 378 F/g at 0.2 A/g with a good rate capability of 198 F/g at 10 A/g, and excellent cycling stability with 94.5% capacitance retention after 10,000 recycles. Moreover, BC-24 also exhibits superior catalytic activity for phenol degradation through peroxydisulfate (PDS) activation. The phenol (0.2 mM) can be effectively absorbed and then completely degraded within only 25 min over a wide pH range with low catalyst and PDS dosages. More importantly, TOC analysis indicates 81.7% of the phenol is mineralized within 60 min, confirming the effectiveness of the BC-24/PDS system. Quenching experiments and EPR measurements reveal that SO4·- and ·OH as well as 1O2 are involved in the phenol degradation, while the non-radical pathway plays the dominant role. This study provides valuable insights into the preparation of cost-effective carbon materials for supercapacitor application and organic contaminant remediation.

4.
Nanomaterials (Basel) ; 12(14)2022 Jul 18.
Artigo em Inglês | MEDLINE | ID: mdl-35889679

RESUMO

Developing suitable photocatalysts for the oxygen evolution reaction (OER) is still a challenging issue for efficient water splitting due to the high requirements to create a significant impact on water splitting reaction kinetics. Herein, n-type Bi2WO6 with flower-like hierarchical structure and p-type Cu2O quantum dots (QDs) are coupled together to construct an efficient S-scheme heterojunction, which could enhance the migration efficiency of photogenerated charge carriers. The electrochemical properties are investigated to explore the transportation features and donor density of charge carriers in the S-scheme heterojunction system. Meanwhile, the as-prepared S-scheme heterojunction presents improved photocatalytic activity towards water oxidation in comparison with the sole Bi2WO6 and Cu2O QDs systems under simulated solar light irradiation. Moreover, the initial O2 evolution rate of the Cu2O QDs/Bi2WO6 heterojunction system is 2.3 and 9.7 fold that of sole Bi2WO6 and Cu2O QDs systems, respectively.

5.
J Hazard Mater ; 388: 122080, 2020 04 15.
Artigo em Inglês | MEDLINE | ID: mdl-31954299

RESUMO

Due to the long growth period of plants, phytoremediation is time costly. Improving the accumulation of cadmium (Cd) in shoots of plants will promote the efficiency of phytoremediation. In this study, two senescence-relative phytohormones, abscisic acid (ABA) and salicylic acid (SA), were applied to strengthening phytoremediation of Cd by tall fescue (Festuca arundinacea S.). Under hydroponic culture, phytohormones treatment increased the Cd content of shoots 11.4-fold over the control, reaching 316.3 mg/kg (dry weight). Phytohormones-induced senescence contributes to the transport of heavy metals, and HMA3 was found to play a key role in this process. Additionally, this strategy could strengthen the accumulation of Cu and Zn in tall fescue shoots. Moreover, in soil pot culture, the strategy increased shoot Cd contents 2.56-fold over the control in tall fescue, and 2.55-fold over the control in Indian mustard (Brassica juncea L.), indicating its comprehensive adaptability and potential use in the field. In summary, senescence-induced heavy metal transport is developed as a novel strategy to strengthen phytoremediation. The strategy could be applied at the end of phytoremediation with an additional short duration (7 days) with comprehensive adaptability, and markedly strengthen the phytoremediation in the field.


Assuntos
Ácido Abscísico/farmacologia , Cádmio/farmacologia , Festuca/metabolismo , Mostardeira/metabolismo , Reguladores de Crescimento de Plantas/farmacologia , Ácido Salicílico/farmacologia , Poluentes do Solo/farmacologia , Biodegradação Ambiental/efeitos dos fármacos , Transporte Biológico/efeitos dos fármacos , Senescência Celular , Raízes de Plantas/metabolismo , Brotos de Planta/metabolismo
6.
J Nanosci Nanotechnol ; 19(9): 5554-5561, 2019 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-30961709

RESUMO

In this study, a two-dimensional heterojunction consisting of bismuth trioxide nanoplates and layered reduced graphene oxide was synthesized using a facile In Situ growth route. A series of characterization tests indicated that the reduction of graphene oxide played a key role as an electron collector for enhancing photoinduced charge carrier separation efficiency. Thus, the as-prepared reduced graphene oxide/bismuth trioxide composite exhibited enhanced photocatalytic water oxidation, which was higher than that of pristine bismuth trioxide under simulated solar light irradiation. Furthermore, the photoelectrochemical properties of the prepared hybrid system were investigated to understand the transfer of photoinduced electrons and holes between layered reduced graphene oxide and bismuth trioxide nanoplates. Thus, this strategy provided an efficient approach for the fabrication of graphene composites containing hierarchical ternary oxides for photocatalysis.

7.
Bioresour Technol ; 267: 524-531, 2018 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-30048928

RESUMO

In this study, a novel nitrogen-doped biochar oxygen reduction reaction cathode-water hyacinth carbon, was prepared by ZnCl2 molten salt carbonization without additional nitrogen source, which displayed a high performance in electro-Fenton (E-Fenton) process. The BET result shows that water hyacinth carbon achieved a much larger specific surface area (829 m2·g-1) than non-melt salt carbonized one (323 m2·g-1) and graphite powder (28 m2·g-1). Furthermore, characterization by XPS and EIS shows that both pyridinic-N (43.24%) and graphitic-N (56.75%) existed in water hyacinth carbon and Warburg constant was only 0.051. Because of a high H2O2 producing yield 1.7 mmol·L-1 and corresponding current efficiency 81.2 ±â€¯2.5% in molten salt carbonized water hyacinth biochar, a high kinetic constant 0.318 min-1 in DMP degradation was achieved, which was 4 times higher than graphite powder (0.076 min-1). The TOC removal achieved 86.8% in 30 min and the corresponding energy consumption reached a low level 60.15 kW·h·kgTOC-1.


Assuntos
Carbono , Carvão Vegetal , Desnitrificação , Eichhornia , Carbono/isolamento & purificação , Eletrodos , Peróxido de Hidrogênio , Nitrogênio , Oxigênio
8.
J Hazard Mater ; 350: 88-97, 2018 05 15.
Artigo em Inglês | MEDLINE | ID: mdl-29454800

RESUMO

In this study, we designed a novel combined electro-Fenton system for the treatment of wastewater containing biological recalcitrant using electric-field-induced ceria (CeO2) as the synergistic catalysts. It was found that by applying this CeO2 electro-Fenton system, the current efficiency improved from 74.49% to 109.82% within 2.5 min; the removal efficiency for dimethyl phthalate (DMP) increased from 85.5% to 94.9% within 20 min; and the mineralization rate increased from 76.01% to 93.58% after 120 min. The effects of parameters such as the applied potential, electrolyte, and concentration of Fe2+ on the current efficiency were systematically studied. Investigations by LSV, zeta titration, X-ray photoelectron spectroscopy (XPS), X-Ray Diffraction (XRD)and electron spin resonance (ESR)revealed the reasons for achieving a current efficiency of over 100% in the CeO2 electro-Fenton system. A mechanism that involved Brønsted acid sites and the redox cycle of sulfate CeO2 was proposed.

9.
Sci Rep ; 7(1): 14387, 2017 10 30.
Artigo em Inglês | MEDLINE | ID: mdl-29085018

RESUMO

Tall fescue (Festuca arundinacea Schreb) is a turf grass species which is widely used for rhizoremediation of organic contaminants and shows notable prospects in heavy metal phytoremediation. In this study, different concentrations of cadmium ion (Cd2+) were applied to study toxic effects of Cd2+ and responses of tall fescue by soilless culture. Tall fescue showed comparable high tolerance to Cd2+ as Indian mustard (Brassica juncea L.). Additionally, the treatment with high concentration of Cd2+ leaded to decreased chlorophyll contents, production of reactive oxygen species (ROS) and lipid peroxidation, as well as damage of cell membrane, necrosis and apoptosis in tall fescue roots, and toxicity of Cd2+ on physiologic properties of tall fescue has been well discussed. Moreover, in photosystem II electron donor side, electron transport from oxygen evolution complex (OEC) to Yz residue of D1 protein was inhibited under high Cd2+ treatments, which may be due to the Cd2+ induced ROS production and the replacement of Ca2+ in the core of OEC. In electron acceptor side, electron transport efficiency from quinone B to photosystem I acceptors increased under high Cd2+ treatments, which may be an important response for plants against Cd2+ toxicity and its mechanism needs our further study.


Assuntos
Cádmio/toxicidade , Festuca/efeitos dos fármacos , Fotossíntese/efeitos dos fármacos , Biodegradação Ambiental , Intoxicação por Cádmio/fisiopatologia , Clorofila/metabolismo , Elétrons , Festuca/metabolismo , Metais Pesados/metabolismo , Complexo de Proteína do Fotossistema I/efeitos dos fármacos , Complexo de Proteína do Fotossistema II/metabolismo , Folhas de Planta/metabolismo , Raízes de Plantas/metabolismo , Plantas/efeitos dos fármacos , Poaceae/metabolismo , Espécies Reativas de Oxigênio/metabolismo
10.
Front Plant Sci ; 8: 1373, 2017.
Artigo em Inglês | MEDLINE | ID: mdl-28848577

RESUMO

L-Ascorbate (Asc) plays important roles in plant development, hormone signaling, the cell cycle and cellular redox system, etc. The higher content of Asc in plant chloroplasts indicates its important role in the photosystem. The objective of this study was to study the roles of Asc in tall fescue leaves against heat stress. After a heat stress treatment, we observed a lower value of the maximum quantum yield for primary photochemistry (φPo), which reflects the inhibited activity of the photochemical phase of photosystem II (PSII). Moreover, we observed a higher value of efficiency of electron transfer from QB to photosystem I acceptors (δR0), which reflects elevated activity of the thermal phase of the photosystem of the tall fescue. The addition of Asc facilitate the behavior of the photochemical phase of the PSII by lowering the ROS content as well as that of the alternative electron donor to provide electron to the tyrosine residue of the D1 protein. Additionally, exogenous Asc reduces the activity of the thermal phase of the photosystem, which could contribute to the limitation of energy input into the photosystem in tall fescue against heat stress. Synthesis of the Asc increased under heat stress treatment. However, under heat stress this regulation does not occur at the transcription level and requires further study.

11.
Environ Sci Technol ; 48(14): 8101-8, 2014 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-24983414

RESUMO

Conversion of waste biomass to value-added carbon is an environmentally benign utilization of waste biomass to reduce greenhouse gas emissions and air pollution caused by open burning. In this study, various waste biomasses are converted to capacitive carbon by a single-step molten salt carbonization (MSC) process. The as-prepared carbon materials are amorphous with oxygen-containing functional groups on the surface. For the same type of waste biomass, the carbon materials obtained in Na2CO3-K2CO3 melt have the highest Brunauer-Emmett-Teller (BET) surface area and specific capacitance. The carbon yield decreases with increasing reaction temperature, while the surface area increases with increasing carbonization temperature. A working temperature above 700 °C is required for producing capacitive carbon. The good dissolving ability of alkaline carbonate molten decreases the yield of carbon from waste biomasses, but helps to produce high surface area carbon. The specific capacitance data confirm that Na2CO3-K2CO3 melt is the best for producing capacitive carbon. The specific capacitance of carbon derived from peanut shell is as high as 160 F g(-1) and 40 µF cm(-2), and retains 95% after 10,000 cycles at a rate of 1 A g(-1). MSC offers a simple and environmentally sound way for transforming waste biomass to highly capacitive carbon as well as an effective carbon sequestration method.


Assuntos
Biomassa , Carbono/análise , Carbonatos/química , Capacitância Elétrica , Potássio/química , Sais/química , Resíduos/análise , Poluição do Ar/análise , Arachis/química , Varredura Diferencial de Calorimetria , Técnicas Eletroquímicas , Espectrometria por Raios X , Temperatura , Termogravimetria , Difração de Raios X
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