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Highly electroactive N–Fe hydrothermal carbons and carbon nanotubes for the oxygen reduction reaction 被引量:5
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作者 R.G.Morais N.Rey-Raap +1 位作者 J.L.Figueiredo M.F.R.Pereira 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第11期260-270,共11页
Glucose-derived carbons were prepared by hydrothermal carbonization of glucose followed by carbonization or activation to obtain carbon materials with different microporosities. These microporous carbons and carbon na... Glucose-derived carbons were prepared by hydrothermal carbonization of glucose followed by carbonization or activation to obtain carbon materials with different microporosities. These microporous carbons and carbon nanotubes(CNTs) were functionalized with melamine and/or iron(Ⅱ) phthalocyanine(FePc)following three different methodologies:(i) Functionalization with melamine via thermal treatment,(ii)incorporation of the lowest amount of FePc reported in the literature via incipient wetness impregnation followed by thermal treatment and(iii) functionalization with melamine followed by Fe Pc incorporation.The chemical and textural characterization of the prepared materials and their electrochemical assessment allowed to understand the role of microporosity in the incorporation of FePc and its effect on the oxygen reduction reaction(ORR). It was observed that FePc was preferentially incorporated inside the porous structure, especially in samples with more developed microporosity. However, functionalization with melamine modified the textural properties and the surface chemistry, favoring the incorporation of FePc on the surface. Regarding the electrochemical performance, the presence of FePc greatly enhanced the electroactivity of the microporous catalysts. An onset potential of 0.88 V and a four-electron pathway were obtained for glucose-derived carbons, whereas the limiting current densities and kinetic current densities rose by 126% and 222%, respectively, in comparison to the base sample. Notwithstanding, the highest electrochemical activity was observed for the sample prepared with CNTs, due to the synergy between the active metal centers and their highly graphitic carbon structure. The electrochemical parameters of CNTFeP csurpass the commercial Pt/C. The half-wave potential is 40 mV higher, the limiting current density increases by 17%, and a negligible production of by-products(< 1%) was observed. 展开更多
关键词 Iron(Ⅱ)phthalocyanine Hydrothermal carbons Carbon nanotubes Oxygen reduction reaction ELECTROCATALYSIS
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Ethyl and butyl acetate oxidation over manganese oxides 被引量:2
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作者 Olívia Salomé G.P.Soares Raquel P.Rocha +2 位作者 Jose J.M.Orfao Manuel F.R.Pereira José L.Figueiredo 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第1期27-36,共10页
Mangenese oxides were synthesized using two new methods,a novel solvent‐free reaction and a reflux technique,that produced cryptomelane‐type products(K‐OMS‐2).Oxides were also synthesized using conventional method... Mangenese oxides were synthesized using two new methods,a novel solvent‐free reaction and a reflux technique,that produced cryptomelane‐type products(K‐OMS‐2).Oxides were also synthesized using conventional methods and all specimens were applied to the oxidation of ethyl acetate and butyl acetate,acting as models for the volatile organic compounds found in industrial emissions.The catalysts were also characterized using N2adsorption,X‐ray diffraction,scanning electron microscopy,temperature programmed reduction and X‐ray photoelectron spectroscopy.Each of the manganese oxides was found to be very active during the oxidation of both esters to CO2,and the synthesis methodology evidently had a significant impact on catalytic performance.The K‐OMS‐2nanorods synthesized by the solvent‐free method showed higher activity than K‐OMS‐2materials prepared by the reflux technique,and samples with cryptomelane were more active than those prepared by the conventional methods.The catalyst with the highest performance also exhibited good stability and allowed90%conversion of ethyl and butyl acetate to CO2at213and202°C,respectively.Significant differences in the catalyst performance were observed,clearly indicating that K‐OMS‐2nanorods prepared by the solvent‐free reaction were better catalysts for the selected VOC oxidations than the mixtures of manganese oxides traditionally obtained with conventional synthesis methods.The superior performance of the K‐OMS‐2catalysts might be related to the increased average oxidation state of the manganese in these structures.Significant correlations between the catalytic performance and the surface chemical properties were also identified,hig-hlighting the K‐OMS‐2properties associated with the enhanced catalytic performance of the materials.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved. 展开更多
关键词 Volatile organic compound Ethyl acetate Butyl acetate Manganese oxide Catalytic oxidation
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Layered double hydroxide(LDH)-based materials:A mini-review on strategies to improve the performance for photocatalytic water splitting 被引量:11
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作者 Hanane Boumeriame Eliana S.Da Silva +3 位作者 Alexey S.Cherevan Tarik Chafik Joaquim L.Faria Dominik Eder 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第1期406-431,I0011,共27页
The high energy demand we currently face in society and the subsequent large consumption of fossil fuels cause its depletion and increase the pollution levels.The quest for the production of clean energy from renewabl... The high energy demand we currently face in society and the subsequent large consumption of fossil fuels cause its depletion and increase the pollution levels.The quest for the production of clean energy from renewable and sustainable sources remains open.The conversion of solar energy into hydrogen via the water-splitting process,assisted by pho tores pons ive semiconductor catalysts,is one of the most promising technologies.Significant progress has been made on water splitting in the past few years and a variety of photocatalysts active not only under ultra-violet(UV)light but especially with the visible part of the electromagnetic spectrum have been developed.Layered double hydroxides(LDH)-based materials have emerged as a promising class of nanomaterials for solar energy applications owing to their unique layered structure,compositional flexibility,tunable bandgaps,ease of synthesis and low manufacturing costs.This review covers the most recent research dedicated to LDH materials for photocatalytic water-splitting applications and encompasses a range of synthetic strategies and post-modifications used to enhance their performance.Moreover,we provide a thorough discussion of the experimental conditions crucial to obtaining improved photoactivity and highlight the impact of some specific parameters,namely,catalysts loading,cocatalysts,sacrificial agents,and irradiation sources.This review provides the necessary tools to select the election technique for adequately enhancing the photoactivity of LDH and modified LDH-based materials and concludes with a critical summary that outlines further research directions. 展开更多
关键词 Layered double hydroxides Water splitting PHOTOCATALYSIS Hydrogen generation Oxygen evolution NANOMATERIALS
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An advanced anaerobic biofilter with effluent recirculation for phenol removal and methane production in treatment of coal gasification wastewater 被引量:7
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作者 Yajie Li Salma Tabassum Zhenjia Zhang 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2016年第9期23-33,共11页
An advanced anaerobic biofilter(AF) was introduced for the treatment of coal gasification wastewater(CGW),and effluent recirculation was adopted to enhance phenol removal and methane production.The results indicat... An advanced anaerobic biofilter(AF) was introduced for the treatment of coal gasification wastewater(CGW),and effluent recirculation was adopted to enhance phenol removal and methane production.The results indicated that AF was reliable in treating diluted CGW,while its efficiency and stability were seriously reduced when directly treating raw CGW.However,its performance could be greatly enhanced by effluent recirculation.Under optimal effluent recirculation of 0.5 to the influent,concentrations of chemical oxygen demand(COD) and total phenol in the effluent could reach as low as 234.0 and 14.2 mg/L,respectively.Also,the rate of methane production reached 169.0 m L CH_4/L/day.Though CGW seemed to restrain the growth of anaerobic microorganisms,especially methanogens,the inhibition was temporary and reversible,and anaerobic bacteria presented strong tolerance.The activities of methanogens cultivated in CGW could quickly recover on feeding with glucose wastewater(GW).However,the adaptability of anaerobic bacteria to the CGW was very poor and the activity of methanogens could not be improved by long-term domestication.By analysis using the Haldane model,it was further confirmed that high effluent recirculation could result in high activity for hydrolytic bacteria and substrate affinity for toxic matters,but only suitable effluent recirculation could result in high methanogenic activity. 展开更多
关键词 Coal gasification wastewater Effluent recirculation Methane production Anaerobic biofilters
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Stable overall water splitting in an asymmetric acid/ alkaline electrolyzer comprising a bipolar membrane sandwiched by bifunctional cobalt-nickel phosphide nanowire electrodes 被引量:5
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作者 Junyuan Xu Isilda Amorim +6 位作者 Yue Li Junjie Li Zhipeng Yu Bingsen Zhang Ana Araujo Nan Zhang Lifeng Liu 《Carbon Energy》 CAS 2020年第4期646-655,共10页
Water splitting has been proposed to be a promising approach to producing clean hydrogen fuel.The two half-reactions of water splitting,that is,the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),ta... Water splitting has been proposed to be a promising approach to producing clean hydrogen fuel.The two half-reactions of water splitting,that is,the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),take place kinetically fast in solutions with completely different pH values.Enabling HER and OER to simultaneously occur under kinetically favorable conditions while using exclusively low-cost,earth-abundant electrocatalysts is highly desirable but remains a challenge.Herein,we demonstrate that using a bipolar membrane(BPM)we can accomplish HER in a strongly acidic solution and OER in a strongly basic solution,with bifunctional self-supported cobaltnickel phosphide nanowire electrodes to catalyze both reactions.Such asymmetric acid/alkaline water electrolysis can be achieved at 1.567 V to deliver a current density of 10 mA/cm2 with ca.100%Faradaic efficiency.Moreover,using an“irregular”BPM with unintentional crossover the voltage needed to afford 10 mA/cm2 can be reduced to 0.847 V,due to the assistance of electrochemical neutralization between acid and alkaline.Furthermore,we show that BPM-based asymmetric water electrolysis can be accomplished in a circulated single-cell electrolyzer delivering 10 mA/cm2 at 1.550 V and splitting water very stably for at least 25 hours,and that water electrolysis is enabled by a solar panel operating at 0.908 V(@13 mA/cm2),using an“irregular”BPM.BPMbased asymmetric water electrolysis is a promising alternative to conventional proton and anion exchange membrane water electrolysis. 展开更多
关键词 bipolar membrane cobalt nickel phosphide hydrogen production noble metalfree water splitting
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O_(3) based advanced oxidation for ibuprofen degradation
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作者 Vitória M.Almeida Carla A.Orge +1 位作者 M.Fernando R.Pereira O.SaloméG.P.Soares 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2022年第2期277-284,共8页
The degradation of the anti-inflammatory ibuprofen(IBP)was evaluated by several advanced oxidation processes.IBP was treated by single ozonation and oxidation with hydrogen peroxide(H_(2)O_(2)),as well as a combinatio... The degradation of the anti-inflammatory ibuprofen(IBP)was evaluated by several advanced oxidation processes.IBP was treated by single ozonation and oxidation with hydrogen peroxide(H_(2)O_(2)),as well as a combination of these treatments.In order to improve the efficiency,the presence of catalysts such as original carbon nanotubes,labelled as CNT,and iron oxide supported on carbon nanotubes,named as Fe/CNT sample,was considered.The evolution of IBP degradation,mineralization and toxicity of the solutions was assessed.The formation of intermediates was also monitored.In the non-catalytic processes,IBP was faster removed by single ozonation,whereas no significant total organic carbon(TOC)removal was achieved.Oxidation with H_(2)O_(2) did not present satisfactory results.When ozone and H_(2)O_(2) were combined,a higher mineralization was attained(70%after 180 min of reaction).On the other hand,in the catalytic processes,this combined process allowed the fastest IBP degradation.In terms of mineralization degree,the presence of Fe/CNT increases the removal rate in the first hour of reaction,achieving a TOC removal of 85%.Four compounds were detected as by-products.All treated solutions presented lower toxicity than the initial solution,suggesting that the released intermediates during applied processes are less toxic. 展开更多
关键词 Advanced oxidation processes CATALYSTS Emerging pollutants IBUPROFEN
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Easy preparation of multifunctional ternary PdNiP/C catalysts toward enhanced small organic molecule electro-oxidation and hydrogen evolution reactions
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作者 Zhipeng Yu Junyuan Xu +2 位作者 Isilda Amorim Yue Li Lifeng Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第7期256-263,共8页
The small organic molecule electro-oxidation(OMEO) and the hydrogen evolution(HER) are two important half-reactions in direct liquid fuel cells(DLFCs) and water electrolyzers,respectively,whose performance is largely ... The small organic molecule electro-oxidation(OMEO) and the hydrogen evolution(HER) are two important half-reactions in direct liquid fuel cells(DLFCs) and water electrolyzers,respectively,whose performance is largely hindered by the low activity and poor stability of electrocatalysts.Herein,we demonstrate that a simple phosphorization treatment of commercially available palladium-nickel(PdNi) catalysts results in multifunctional ternary palladium nickel phosphide(PdNiP) catalysts,which exhibit substantially enhanced electrocatalytic activity and stability for HER and OMEO of a number of molecules including formic acid,methanol,ethanol,and ethylene glycol,in acidic and/or alkaline media.The improved performance results from the modification of electronic structure of palladium and nickel by the introduced phosphorus and the enhanced corrosion resistance of PdNiP.The simple phosphorization approach reported here allows for mass production of highly-active OMEO and HER electrocatalysts,holding substantial promise for their large-scale application in direct liquid fuel cells and water electrolyzers. 展开更多
关键词 PdNiP Multifunctional catalyst Phosphorization Small molecule electro-oxidation Hydrogen evolution
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Oxypropylation of Brazilian Pine-Fruit Shell Evaluated by Principal Component Analysis
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作者 Stephany Cde Rezende João APinto +2 位作者 Isabel PFernandes Fernanda VLeimann Maria-Filomena Barreiro 《Journal of Renewable Materials》 SCIE 2018年第7期715-723,共9页
Pine-fruit shell (PFS) is a lignocellulosic residue derived from the fruit of Araucaria angustifolia, a coniferoustree native of South America, part of a whole vegetation of the Atlantic Forest, found in the South and... Pine-fruit shell (PFS) is a lignocellulosic residue derived from the fruit of Araucaria angustifolia, a coniferoustree native of South America, part of a whole vegetation of the Atlantic Forest, found in the South and Southwestof Brazil. In this work PFS will be characterized and used in the production of PFS-based polyols throughoxypropylation. Three series were chosen (PFS/propylene oxide (PO) (w/v, g/mL) of 30/70, 20/80 and 10/90)with four catalyst levels (5%, 10%, 15% and 20%, (w/w, PFS based)). Oxypropylation occurred at moderateconditions of temperature, pressure and time giving rise to liquid polyols with a homopolymer content (PPO)ranging from 4-65%, a hydroxyl number (IOH) between 257-605 mg KOH/g and viscosities (V) varying from0.76 Pa.s to 373.90 Pa.s (20°C) for the series 20/80 and 10/90, while for the series 30/70, the viscosity reachedvalues higher than 500 Pa.s, 20°C. The unreacted PFS (UR) varied between 3.6% and 77.4% (PFS-basis). Afterthe PFS-based polyols production and characterization, a principal component analysis (PCA) was performed inorder to evaluate the established interactions between the used formulation variables and the obtained polyolproperties. The PCA analysis allowed to clarify the interactions between PFS and PO contents and the finalbiopolyol properties (PPO, IOH, V and UR). This approach showed to be a simple method to rationally analyzethe influence of the input formulation variables on the final polyol properties. 展开更多
关键词 Principal components analysis Brazilian pine-fruit shell (PFS) oxypropylation POLYOLS
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Disclosing the potential of Cupressus leylandii A.B.Jacks&Dallim,Eucalyptus globulus Labill.,Aloysia citrodora Paláu,and Melissa officinalis L.hydrosols as eco-friendly antimicrobial agents
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作者 Heloísa H.S.Almeida Pedro J.L.Crugeira +2 位作者 Joana S.Amaral Alírio E.Rodrigues Maria-Filomena Barreiro 《Natural Products and Bioprospecting》 CSCD 2024年第1期1-12,共12页
Antimicrobial resistance is a major global health concern,threatening the effective prevention and treatment of infections caused by microorganisms.These factors boosted the study of safe and green alternatives,with h... Antimicrobial resistance is a major global health concern,threatening the effective prevention and treatment of infections caused by microorganisms.These factors boosted the study of safe and green alternatives,with hydrosols,the by-products of essential oils extraction,emerging as promising natural antimicrobial agents.In this context,four hydrosols obtained from Cupressus leylandii A.B.Jacks&Dallim,Eucalyptus globulus Labill.,Aloysia citrodora Paláu and Melissa officinalis L.were studied.Their chemical composition comprises neral,geranial,1,8-cineole,terpinen-4-ol,and oplopanonyl acetate,compounds with recognised antimicrobial activity.Concerning antimicrobial activity,significant differences were found using different hydrosol concentrations(10-20%v/v)in comparison to a control(without hydrosol),showing the potential of the tested hydrosols to inhibit the microbial growth of Escherichia coli,Staphylococcus aureus,and Candida albicans.A.citrodora hydrosol was the most effective one,inhibiting 90%of E.coli growth and 80%of C.albicans growth,for both hydrosol concentrations(p<0.0001).With hydrosol concentration increase,it was possible to observe an improved antimicrobial activity with significant reductions(p<0.0001).The findings of this work indicate the viability of reusing and valuing the hydrosols,encouraging the development of green applications for different fields(e.g.,food,agriculture,pharmaceuticals,and cosmetics). 展开更多
关键词 Hydrosols Essential oil by-products Chemical composition Antimicrobial activity Natural preservatives Waste valorisation
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Unveiling the potential of olive oil production residues as adsorbent materials for water treatment:A literature review
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作者 Iris Correia Maria Eduarda Fernandes Dorinda Marques-da-Silva 《Journal of Bioresources and Bioproducts》 2025年第4期460-475,共16页
Olive oil is a nutritionally and economically valuable product whose global production has steadily increased,alongside the generation of large volumes of solid and liquid waste.Olive oil mill wastewater and solid res... Olive oil is a nutritionally and economically valuable product whose global production has steadily increased,alongside the generation of large volumes of solid and liquid waste.Olive oil mill wastewater and solid residues such as olive pomace and olive stones have become ma-jor environmental concerns due to their high pollutant load.At the same time,these byproducts offer an opportunity:their valorization as low-cost,sustainable adsorbents for water treatment.Addressing this dual environmental challenge,this review provides a comprehensive and sys-tematized synthesis of the current state of research on the use of olive oil production residues for water decontamination via adsorption.Specifically,the study maps the types of byproducts used,their target pollutants,removal efficiencies,and adsorption capacities.Unlike previous re-views,this work emphasizes studies that apply raw or minimally processed residues,as well as experiments conducted with real wastewater or under environmentally relevant conditions.The data are presented in a structured and comparative format,highlighting promising results and underexplored combinations.By identifying trends,gaps,and practical applications,this review contributes to advancing the development of circular economy-based,eco-friendly solutions for water pollution control and provides a valuable resource for future research and implementation. 展开更多
关键词 Olive oil production residues Olive pomace Olive stones Adsorbent materials Water treatment Circular economy
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Metal alginates for polyphenol delivery systems: Studies on crosslinking ions and easy-to-use patches for release of protective flavonoids in skin 被引量:2
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作者 João Silva Pavlo Vanat +2 位作者 Dorinda Marques-da-Silva Joaquim Rui Rodrigues Ricardo Lagoa 《Bioactive Materials》 SCIE 2020年第3期447-457,共11页
Incorporation of bioactive natural compounds like polyphenols is an attractive approach for enhanced functionalities of biomaterials.In particular flavonoids have important pharmacological activities,and controlled re... Incorporation of bioactive natural compounds like polyphenols is an attractive approach for enhanced functionalities of biomaterials.In particular flavonoids have important pharmacological activities,and controlled release systems may be instrumental to realize the full potential of these phytochemicals.Alginate presents interesting attributes for dermal and other biomaterial applications,and studies were carried here to support the development of polyphenol-loaded alginate systems.Studies of capillary viscosity indicated that ionic medium is an effective strategy to modulate the polyelectrolyte effect and viscosity properties of alginates.On gelation,considerable differences were observed between alginate gels produced with Ca^2+,Ba^2+,Cu^2+,Fe^2+,Fe^3+and Zn^2+as crosslinkers,especially concerning shrinkage and morphological regularity.Stability assays with different polyphenols in the presence of alginate-gelling cations pointed to the choice of calcium,barium and zinc as safer crosslinkers.Alginate-based films loaded with epicatechin were prepared and the kinetics of release of the flavonoid investigated.The results with calcium,barium and zinc alginate matrices indicated that the release dynamics is dependent on film thicknesses,but also on the crosslinking metal used.On these grounds,an alginate-based system of convenient use was devised,so that flavonoids can be easily loaded at simple point-of-care conditions before dermal application.This epicatechin-loaded patch was tested on an ex-vivo skin model and demonstrated capacity to deliver therapeutically relevant concentrations on skin surface.Moreover,the flavonoid released was not modified and retained full antioxidant bioactivity.The alginate-based system proposed offers a multifunctional approach for flavonoid controllable delivery and protection of skin injured or under risk. 展开更多
关键词 Topical drug delivery Intrinsic viscosity BIOPOLYMER Epigallocatechin-gallate Antioxidant dressing
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