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1.
Mikrochim Acta ; 191(9): 524, 2024 Aug 07.
Artículo en Inglés | MEDLINE | ID: mdl-39112828

RESUMEN

An electrochemical platform for signal amplification probing chloride ions (Cl-) is constructed by the composite integrating core-shell structured nitrogen-doped porous carbon@Ag-based metal-organic frameworks (NC@Ag-MOF) with polypyrrole (PPy). It is based on the signal of solid-state AgCl derived from Ag-MOF, since both NC and PPy have good electrical conductivity and promote the electron transport capacity of solid-state AgCl. NC@Ag-MOF was firstly synthesized with NC as the scaffold and then, PPy was anchored on NC@Ag-MOF by chemical polymerization. The composite NC@Ag-MOF-PPy was utilized to modify the electrode, which exhibited a higher peak current and lower peak potential during Ag oxidation compared with those of Ag-MOF and NC@Ag-MOF-modified electrodes. More importantly, in the coexistence of chloride (Cl-) ions in solution, the NC@Ag-MOF-PPy-modified electrode displayed a fairly stable and sharp peak of solid-state AgCl with the peak potentials gradually approaching zero, which might effectively overcome the background interference caused by electroactive substances. The oxidation peak currents of solid-state AgCl increased linearly with the concentration of  Cl- ions in a broad range of 0.15 µM-40 mM and 40-250 mM, with detection limits of 0.10 µM and 40 mM, respectively. The practical applicability for Cl- ions determination was demonstrated using human serum and urine samples. The results suggest that NC@Ag-MOF-PPy composite could be a promising candidate for the construction of the electrochemical sensor.

2.
J Colloid Interface Sci ; 660: 469-477, 2024 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-38246050

RESUMEN

Unsaturated furanic aldehydes are derived from lignocellulosic biomass resources and subsequently used to produce valuable chemicals. However, the highly efficient, selective hydrogenation of the biomass-derived unsaturated furan CO bond remains challenging. Here we report that graphene-like nitrogen doped porous carbon (GNPC) nanosheets are synthesized from carbon-rich, sustainable, and renewable biomass precursors (glucose, fructose and 5-hydroxymethylfurfural, HMF) with high surface areas, large pore volumes and narrow mesopores. GNPC derived from HMF is an excellent catalyst support for PtCo nanoparticles with ultrafine nanoparticles size and homogeneous distributions. This catalyst is highly efficient for hydrogenation of biomass-derived furan-based unsaturated aldehydes, with high yields, to the corresponding unsaturated alcohols under mild conditions. This design strategy should further allow the development of selective, simple, green heterogeneous catalysts for challenging chemical transformations.

3.
Sci Total Environ ; 914: 169856, 2024 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-38190916

RESUMEN

Waste polyethylene terephthalate (PET) with high carbon content (>60 wt%) has shown great potential in the field of synthesizing carbon materials for CO2 capture, attracting increasing attention. Herein, an innovative strategy was proposed to synthesize nitrogen-doped hierarchical porous carbon (PC) for CO2 capture using PET as precursor and sodium amide (NaNH2) as both nitrogen dopant and low-temperature activator. As-synthesized N-doped PC exhibited a significantly high micropore volume of 0.755 cm3/g and a rich content of N- and O-containing functional groups, offering ample active sites for CO2 molecules. Further, the adsorbents demonstrated excellent CO2 capture capacity, achieving 5.7 mmol/g (0 °C) and 3.3 mmol/g (25 °C) at 1 bar, respectively. This was primarily attributed to the synergistic effect of narrow micropores filling and electrostatic interactions. Moreover, as-synthesized PC exhibited rapid CO2 adsorption capability, and its dynamic adsorption process was effectively described using a pseudo-second-order kinetic model. After five consecutive cycles, PET-derived PC still maintained ~100 % of adsorption capacity. They also possessed good CO2/N2 selectivity and reasonable isosteric heat of adsorption. Therefore, as-synthesized nitrogen-doped PC is a promising CO2 adsorbent through low-temperature activation of carbonized PET with NaNH2. Such findings have substantial implications for waste plastic recycling and mitigating the greenhouse effect.

4.
Front Chem ; 11: 1333475, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-38156020

RESUMEN

Capturing and separating carbon dioxide, particularly using porous carbon adsorption separation technology, has received considerable research attention due to its advantages such as low cost and ease of regeneration. In this study, we successfully developed a one-step carbonization activation method using freeze-thaw pre-mix treatment to prepare high-nitrogen-content microporous nitrogen-doped carbon materials. These materials hold promise for capturing and separating CO2 from complex gas mixtures, such as biogas. The nitrogen content of the prepared carbon adsorbents reaches as high as 13.08 wt%, and they exhibit excellent CO2 adsorption performance under standard conditions (1 bar, 273 K/298 K), achieving 6.97 mmol/g and 3.77 mmol/g, respectively. Furthermore, according to Ideal Adsorption Solution Theory (IAST) analysis, these materials demonstrate material selectivity for CO2/CH4 (10 v:90 v) and CO2/CH4 (50 v:50 v) of 33.3 and 21.8, respectively, at 1 bar and 298 K. This study provides a promising CO2 adsorption and separation adsorbent that can be used in the efficient purification process for carbon dioxide, potentially reducing greenhouse gas emissions in industrial and energy production, thus offering robust support for addressing climate change and achieving more environmentally friendly energy production and carbon capture goals.

5.
J Colloid Interface Sci ; 652(Pt B): 1734-1742, 2023 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-37672976

RESUMEN

Electrocatalytic reduction of CO2 (CO2RR) to value-added fuels and chemicals can potentially serve as a promising strategy to curb CO2 accumulation and carbon neutral cycle, but is still plagued by sluggish kinetics, poor selectivity and weak durability. Herein, we developed highly-dispersed nickel species on the nitrogen-doped carbon materials (Ni/NC) via the double solvent method (DSM), followed by the pyrolysis. The as-prepared Ni/NC possesses high CO2-to-CO selectivity of 93.2%∼98.6% at broad potential range (0.57 âˆ¼ 0.97 VRHE), decent jCO of 57.9 mAcm-2 at -1.07 VRHE, and significant robustness (retaining 96.3% of the initial faradaic efficiency for CO formation after 50 h electrolysis). As manifested by the rotating ring-disk electrode (RRDE) tests, the DSM-based Ni/NC possesses more significant pH-buffering capacity than Ni nanoparticles, thus promotes the CO2-to-CO. DFT calculations unveil that Ni/NC exhibits relatively lower d-band center, hence resulting in favorable desorption of CO from the catalyst surface that intrinsically boost the CO2-to-CO compared with the nanoparticle catalyst. These results suggest that the DSM-derived Ni/NC catalysts is a promising candidate towards large-scale application of CO2-to-CO.

6.
Anal Sci ; 39(10): 1727-1739, 2023 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-37344740

RESUMEN

Nanomaterials with intrinsic enzyme-like activity have gained substantial scientific attention as viable substitutes to natural biological enzymes owing to their cheap price and great stability. Numerous artificial enzyme mimics have been employed effectively in sectors such as sensing, environmental processing, and cancer treatment. In this study, novel nitrogen-doped porous carbon nanomaterials (CPs) were produced by modifying polypyrrole with magadiite using chemical oxidative polymerization and calcination methods. The obtained nitrogen-doped porous carbon nanomaterials exhibited improved peroxidase-like activity, which catalyzed the oxidation of 3,3,5,5-tetramethylbenzidine (TMB) in the presence of hydrogen peroxide (H2O2) to produce colorful compounds. Kinetic investigation revealed that the affinity for TMB of nitrogen-doped porous carbon peroxidase mimics was higher than that of genuine horseradish peroxidase (HRP). In addition, a sensitive assay with encouraging performance for the colorimetric detection of ascorbic acid (AA) was successfully fabricated employing nitrogen-doped porous carbon nanomaterials as peroxidase mimics. The results were satisfactory and demonstrated its potential application in antioxidant detection.


Asunto(s)
Nanoestructuras , Peroxidasa , Peroxidasa/química , Antioxidantes , Polímeros , Ácido Ascórbico , Carbono/química , Nitrógeno , Glucosa , Colorimetría/métodos , Peróxido de Hidrógeno/química , Porosidad , Pirroles , Peroxidasas , Nanoestructuras/química , Colorantes
7.
Int J Mol Sci ; 24(10)2023 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-37240130

RESUMEN

Benefiting from the additional active sites for sodium-ion (Na+) adsorption and porous architecture for electrolyte accessibility, nitrogen-doped porous carbon has been considered the alternative anode material for Na+-storage applications. In this study, nitrogen-doped and zinc-confined microporous carbon (N,Z-MPC) powders are successfully prepared by thermally pyrolyzing the polyhedral ZIF-8 nanoparticles under an argon atmosphere. Following the electrochemical measurements, the N,Z-MPC not only delivers good reversible capacity (423 mAh/g at 0.02 A/g) and comparable rate capability (104 mAh/g at 1.0 A/g) but also achieves a remarkable cyclability (capacity retention: 96.6% after 3000 cycles at 1.0 A/g). Those can be attributed to its intrinsic characteristics: (a) 67% of the disordered structure, (b) 0.38 nm of interplanar distance, (c) a great proportion of sp2-type carbon, (d) abundant microporosity, (e) 16.1% of nitrogen doping, and (f) existence of sodiophilic Zn species, synergistically enhancing the electrochemical performances. Accordingly, the findings observed here support the N,Z-MPC to be a potential anode material enabling exceptional Na+-storage abilities.


Asunto(s)
Carbono , Zinc , Iones , Nitrógeno , Sodio
8.
J Colloid Interface Sci ; 645: 297-305, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37150003

RESUMEN

Supercapacitors are attracting extensive attention in energy storage fields thanks to their high safety, cost-effectiveness, and environmental friendliness. The carbon materials, especially for the porous carbon materials derived from renewable biomass materials, are important electrode materials with cost-effective feature for supercapacitors. However, the inferior ionic conductivity of biomass materials inhibits their electrochemical performance in energy storage devices. Herein, an immiscible liquid-mediated method is provided to improve the ionic conductivity of silk-derived nitrogen-doped porous carbon (NPC) electrodes. Natural Bombyx mori (silkworm) silk is used as a carbon source for the preparation of electrode of supercapacitor. Further introducing immiscible organic liquid into the NPCs promotes the ion transport in the inner pores of the electrodes. With the assistance of organic liquid, the supercapacitor presents a specific capacitance of 565.3 F g-1 at a current density of 1 A g-1. The supercapacitor shows the maximum specific energy and power density of 26.2 Wh kg-1 and 263.9 W kg-1, and holds a capacitance retention of approximately 93.3% after 10 000 cycles. This work provides a facile method for the rational design of carbon material derived from biomass material to fabricate electrode with high ionic conductivity, and the strategy will be extendable to other biomass materials for a wide range of applications.

9.
J Chromatogr A ; 1695: 463929, 2023 Apr 26.
Artículo en Inglés | MEDLINE | ID: mdl-37003076

RESUMEN

Benzotriazole ultraviolet stabilizers (BUVSs) that are added to pharmaceutical and personal care products (PPCPs) have raised global concerns because of their high toxicity. An efficient method to monitor its pollution level is urgently imperative. Here, a nitrogen-doped metal-organic framework (MOF) derived porous carbon (UiO-66-NH2/DC) was prepared and integrated into polyvinylidene fluoride mixed matrix membrane (PVDF MMM) as an adsorbent for the first time. The hydrophobic UiO-66-NH2/DC with a pore size of 162 Å exhibited outstanding extraction performance for BUVSs, which solves the problem of difficult enrichment of large-size and hydrophobic targets. Notably, the density functional theory simulation was employed to reveal the structure of the derived carbon material and explored the recognition and enrichment mechanism (synergy of π-π conjugation, hydrogen bond, coordination, hydrophobic interaction and mesoporous channel) of BUVSs by UiO-66-NH2/DC-PVDF MMM. And then, an influential method based on dispersive membrane extraction (DME) coupled with ultrahigh-performance liquid chromatography-tandem mass spectrometry (UHPLC-MS/MS) was developed for the simultaneous analysis of four BUVSs in environmental water samples. The validated method benefited from the high sensitivity (the limits of detection within 0.25-1.40 ng/L), accuracy (recoveries of 71.9-102.8% for wastewater) and rapidity (50 min to enrich 9 samples). This study expands the application prospects of porous carbon derived from MOF for sample pretreatment of pollutants in water.


Asunto(s)
Estructuras Metalorgánicas , Agua , Agua/química , Estructuras Metalorgánicas/química , Polímeros , Espectrometría de Masas en Tándem/métodos , Carbono , Porosidad , Extracción en Fase Sólida/métodos , Cromatografía Líquida de Alta Presión/métodos
10.
J Chromatogr A ; 1685: 463600, 2022 Dec 06.
Artículo en Inglés | MEDLINE | ID: mdl-36334561

RESUMEN

In this work, magnetic nitrogen-doped porous carbon (Fe3O4@N-PC) was prepared via incomplete combustion coupled with solvothermal synthesis for extraction of four benzoylureas (BUs) insecticides. Among them, nitrogen-doped porous carbon was produced through incomplete combustion of filter paper loaded with mixture formed by Zn(NO3)2·6H2O and polyethyleneimine solution, and magnetic nanoparticles were further introduced by solvothermal method. Compared with magnetic porous carbon (Fe3O4@PC), the surface hydrophilicity of Fe3O4@N-PC was improved by virtue of the doping of nitrogen atoms, and the dispersion of Fe3O4 was more uniform, which greatly exposed the adsorption site. The characterization of Fe3O4@N-PC were carried out by TEM, XRD, elemental analysis, XPS, BET and magnetic hysteresis curve. Besides, Fe3O4@N-PC was successfully used as magnetic solid-phase extraction (MSPE) adsorbent, which showed excellent enrichment factors and extraction recoveries toward polar BUs insecticides due to the polar surface and introduction of Lewis-basic nitrogen. The optimum amount of Fe3O4@N-PC adsorbent, extraction time, pH value, desorption solvent, desorption time and PEI concentration for BUs insecticides extraction were determined to be 3 mg, 10 min, 8, acetone/acetic acid (19:1, V/V), 6 min and 60 g L-1, respectively. Under this experimental condition, the enrichment factors ranged from 182 to 192 with good intra- and inter-day relative standard deviations (RSDs). The calibration lines were linear over the concentration in the range of 1-800 µg L-1, the limit of detection (LOD) and limit of quantification (LOQ) were 0.3 µg L-1 as well as 1 µg L-1, respectively. The recoveries for spiked sample ranged from 90.7 to 107.3% in spiked Yellow River water with the RSDs less than 7.0%. The results showed that the established MSPE strategy based on Fe3O4@N-PC could be used for the detection of trace BUs in complex samples.


Asunto(s)
Insecticidas , Insecticidas/análisis , Carbono/química , Agua/química , Porosidad , Nitrógeno , Extracción en Fase Sólida/métodos , Límite de Detección , Fenómenos Magnéticos , Cromatografía Líquida de Alta Presión
11.
Micromachines (Basel) ; 13(9)2022 Sep 14.
Artículo en Inglés | MEDLINE | ID: mdl-36144141

RESUMEN

The preparation of N-doped porous carbon (NC-800) is presented via facile mango stone carbonization at 800 °C. The NC-800 material exhibits good cycle stability (the capacity retention is 97.8% after 5000 cycles) and high specific capacitance of 280 F/g at 1 A/g. Furthermore, the assembled symmetric device of NC-800//NCs-800 exhibits about 31.1 Wh/kg of energy density at 800 W/kg in a voltage range of 0-1.6 V. The results of the study suggest that NC-800 may be a promising energy storage material for practical application.

12.
Mikrochim Acta ; 189(9): 359, 2022 09.
Artículo en Inglés | MEDLINE | ID: mdl-36040532

RESUMEN

A sandwich-type electrochemical immunosensor was designed for the ultrasensitive detection of prostate-specific antigen (PSA), using Au nanoparticles (Au NPs) modified nitrogen-doped porous carbon (NPC) as sensor platform and trimetallic PdAgCu mesoporous nanospheres (PdAgCu MNSs) as enzyme-mimicking labels. NPC was prepared by a facile one-step pyrolysis strategy of biomimetic phylloid zeolite imidazole framework (ZIF-L) nanosheets. Through this strategy, the graphitization of the microcrystalline structure enhanced the electrical conductivity, while its enlarged specific surface area and abundant pore volume can enrich H2O2 to improve the catalytic efficiency. Moreover, Au NPs were used to modify NPC without cross-linking agents to further optimize electron transport while capturing primary antibodies, improving stability and sensitivity of the immunosensor. PdAgCu MNSs with uniform size, cylindrical open mesoporous channels, and continuous crystal frame structure were self-assembling synthesized by electrostatic adsorption and ascorbic acid (AA) co-reduction with amphiphilic dioctadecyldimethylammonium chloride (DODAC) as surfactant-cum-micelle, whose unique structure maximizes the use of polyatoms to expose catalytic sites, exhibiting good biocompatibility and electrocatalytic ability. Under the optimal conditions, the immunosensor showed superior sensitivity, a wide dynamic detection range (10 fg mL-1 ~ 100 ng mL-1) and a low limit of detection (LOD, 3.29 fg mL-1). This work provides a convenient strategy for the clinical detection of PSA.


Asunto(s)
Técnicas Biosensibles , Nanopartículas del Metal , Nanoporos , Anticuerpos Inmovilizados/química , Carbono/química , Técnicas Electroquímicas , Oro/química , Humanos , Peróxido de Hidrógeno/química , Inmunoensayo , Límite de Detección , Masculino , Nanopartículas del Metal/química , Nitrógeno , Porosidad , Antígeno Prostático Específico
13.
Sci Total Environ ; 805: 150353, 2022 Jan 20.
Artículo en Inglés | MEDLINE | ID: mdl-34818788

RESUMEN

Recovering high value-added resources from waste activated sludge (WAS) is a potential way for the sustainable wastewater treatment. In this study, hydrothermal treatment at 180 °C was used to simultaneously improve sludge dewaterability and recover sludge organic matters (SOMs). The recovered SOMs were subsequently employed as precursors to prepare nitrogen-doped porous carbon nanosheets via a facile stepwise synthesis method. The as-prepared optimal carbon (AP-SOM800) was characterized with an ultrahigh specific surface area (3473 m2/g), appropriate porosity (1.77 cm3/g), and abundant heteroatoms (1.47% N and 7.44% O). AP-SOM800 exhibited a high specific capacitance (409 F/g at 0.25 A/g), low resistance (0.52 Ω), and superior cyclic stability (only 9.09% loss after 10,000 cycles) in 6 M KOH aqueous electrolyte. Furthermore, AP-SOM800 demonstrated an extraordinary adsorption capacity (1528 mg/g for methyl orange (MO) and 1265 mg/g for tetracycline (TC)) that can be maintained (˃ 1200 mg/g) over a wide range of pH conditions. Specifically, 80.97% of MO and 66.67% of TC were rapidly absorbed through AP-SOM800 within 10 min, and 90.27% of MO and 81.24% of TC were eventually removed from wastewater after 60 min. The adsorption processes fit closely with the pseudo-second-order kinetic (R2 > 0.999) and Langmuir models (R2 > 0.914), revealing that the adsorption processes were dominated by a monolayer chemical adsorption reaction. This study suggests that high value-added materials can be obtained from the WAS through improving and extending the traditional sludge treatment processes, which will enrich the technical options available for future sustainable sludge treatment and disposal.


Asunto(s)
Aguas del Alcantarillado , Purificación del Agua , Adsorción , Carbono , Nitrógeno , Aguas Residuales
14.
Small ; 18(6): e2105310, 2022 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-34854537

RESUMEN

The enhancement of the structural stability of conversion-based metal sulfides at high current densities remains a major challenge in realizing the practical application of sodium-ion batteries (SIBs). The instability of metal sulfides is caused by the large volume variation and sluggish reaction kinetics upon sodiation/desodiation. To overcome this, herein, a heterostructured nanocube anode composed of CuS/FeS2 embedded in nitrogen-doped carbon (CuS/FeS2 @NC) is synthesized. Size- and shape-controlled porous carbon nanocubes containing metallic nanoparticles are synthesized by the two-step pyrolysis of a bimetallic Prussian blue analog (PBA) precursor. The simple sulfurization-induced formation of highly conductive CuS along with FeS2 facilitates sodium-ion diffusion and enhances the redox reversibility upon cycling. The mesoporous carbon structure provides excellent electrolyte impregnation, efficient charge transport pathways, and good volume expansion buffering. The CuS/FeS2 @NC nanocube anode exhibits excellent sodium storage characteristics including high desodiation capacity (608 mAh g-1 at 0.2 A g-1 ), remarkable long-term cycle life (99.1% capacity retention after 300 cycles at 5 A g-1 ), and good rate capability up to 5 A g-1 . The simple, facile synthetic route combined with the rational design of bimetallic PBA nanostructures can be widely utilized in the development of conversion-based metal sulfides and other high-capacity anode materials for high-performance SIBs.

15.
Nano Lett ; 21(22): 9691-9698, 2021 Nov 24.
Artículo en Inglés | MEDLINE | ID: mdl-34748344

RESUMEN

Lithium-sulfur (Li-S) batteries suffer from multiple complex and often interwoven issues, such as the low electronic conductivity of sulfur and Li2S/Li2S2, shuttle effect, and sluggish electrochemical kinetics of lithium polysulfides (LiPSs). Guided by theoretical calculations, a multifunctional catalyst of isolated single-atom nickel in an optimal Ni-N5 active moiety incorporated in hollow nitrogen-doped porous carbon (Ni-N5/HNPC) is constructed and acts as an ideal host for a sulfur cathode. The host improved electrical conductivity, enhanced physical-chemical dual restricting capability toward LiPSs, and, more importantly, boosted the redox reaction kinetics by the Ni-N5 active moiety. Therefore, the Ni-N5/HNPC/S cathode exhibits superior rate performance, long-term cycling stability, and good areal capacity at high sulfur loading. This work highlights the important role of the coordination number of active centers in single-atom catalysts and provides a strategy to design a hollow nanoarchitecture with single-atom active sites for high-performance Li-S batteries.

16.
Mikrochim Acta ; 188(10): 338, 2021 Sep 12.
Artículo en Inglés | MEDLINE | ID: mdl-34510324

RESUMEN

An electrochemical sensor based on an antimony/nitrogen-doped porous carbon (Sb/NPC) composite has been developed for the quantitative detection of albumin from hepatocellular carcinoma (HCC) patients. Sb/NPC is hydrothermally synthesized from Sn/NPC precursors. The synthesized precursor (Sn/NPC) and the product (Sb/NPC) are characterized by XRD, FTIR, TGA, UV/Vis, SEM, and AFM. Cyclic voltammetry, chronoamperometry, and electrochemical impedance studies are used to investigate the electrochemical performance of Sb/NPC-GCE. Sb/NPC-GCE detects albumin at physiological pH of 7.4 in the potential range 0.92 V and 0.09 V for oxidation and reduction, respectively. LOD and recovery of Sb/NPC-GCE for the determination of albumin are 0.13 ng.mL-1 and 66.6 ± 0.97-100 ± 2.73%, respectively. Chronoamperometry of the modified working electrode demonstrates its stability for 14 h, indicating its reusability and reproducibility. Sb/NPC-GCE is a selective sensor for albumin detection in the presence of interfering species. The electrode has been applied for albumin detection in human serum samples of HCC patients. A negative correlation of albumin with alpha-fetoprotein levels in HCC patients is observed by statistical analysis.


Asunto(s)
Antimonio/química , Carbono/química , Carcinoma Hepatocelular/sangre , Neoplasias Hepáticas/sangre , Nitrógeno/química , Albúmina Sérica/análisis , Estaño/química , Técnicas Electroquímicas , Humanos , Albúmina Sérica/química
17.
Sci Total Environ ; 759: 143575, 2021 Mar 10.
Artículo en Inglés | MEDLINE | ID: mdl-33223181

RESUMEN

Carbon-based materials have been applied as cost-effective electrocatalysts to reduce carbon dioxide (CO2) into valuable chemicals. Here, an environment-friendly method is proposed to obtain nitrogen-doped porous carbons (NPCs) from digested sludge, which is an abundant waste product from sewage treatment plants. The materials were used as a metal-free electrocatalyst for electrochemical reduction of CO2 to formate. The synthesized material (NPC-600) had a mesoporous and microporous structure with a specific surface area of 246.21 m2 g-1 and pore volume of 0.494 cm3 g-1. Active sites based on nitrogen atoms accounted for 2.98 atom% of the content and included pyrrolic-, pyridinic-, and graphitic-N, which is useful for CO2 adsorption and electron transfer in electrochemical reduction. The Faradaic efficiency for formate production from CO2 in the presence of NPC-600 was 68% at the potential of -1.5 V vs. SCE. Tafel analysis indicated that the pathway of CO2 conversion involved the reduction of CO2 to CO2*- intermediate, which was then converted to HCOO*- and finally formate.

18.
J Colloid Interface Sci ; 587: 290-301, 2021 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-33360902

RESUMEN

Clean energy conversion/storage techniques have become increasingly significant because of the increasing energy consumption. Regarding practical applications like zinc-air batteries and supercapacitors, electrode materials are essential and often require both porous networks and active species to enhance their electrochemical performance. Nitrogen-doped porous carbon (NPC) is a kind of promising material, which provides efficient active sites and large surface areas for energy conversion/storage applications. However, rational modulation of properties for maximizing NPC performance is still a challenge. Herein, a promising NPC material derived from natural biomass is successfully synthesized by following a stepwise preparation method. Physisorption and X-ray photoelectron spectroscopy (XPS) analyses demonstrate both pore structures and nitrogen species of the NPC have been delicately tuned. The optimized sample NPC-800-m exhibits excellent performance in both oxygen reduction reaction (ORR) and three-electrode supercapacitor measurement. Moreover, the homemade zinc-air battery and symmetric supercapacitor assembled with NPC-800-m also display outstanding energy and power density as well as durable stability. Density functional theory (DFT) calculations further confirm the synergistic effects among graphitic, pyridinic and pyrrolic nitrogen. The existence of multispecies of nitrogen combined with the optimized pore structure is the key to the high electrochemical performance for NPC-800-m. This work not only provides feasible and green synthetic methodology but also offers original insights into the effective pores and the synergistic effects of different nitrogen species in the NPC materials.

19.
Nanomaterials (Basel) ; 10(9)2020 Sep 07.
Artículo en Inglés | MEDLINE | ID: mdl-32906605

RESUMEN

Biomass-derived porous carbon materials have drawn considerable attention due to their natural abundance and low cost. In this work, nitrogen-doped porous carbons with high nitrogen content and large surface areas were designed and prepared from cottonseed hull and cattail. The two plant-based biomass compositions are similar, but the structures are very different, generating distinctly different property and performance of the prepared carbon materials. NRPC-112 has good electrochemical properties, while CN800 has good adsorption properties. By comparing the microstructure differences between the two starting materials, it was found that the structure of the raw materials would significantly affect the properties and performance of the materials. The work provided an important theoretical basis and reference for the selection of bio-resources for preparing carbon material. It is also important for choosing the appropriate synthesis method, process optimization, and application scenarios.

20.
Front Chem ; 8: 226, 2020.
Artículo en Inglés | MEDLINE | ID: mdl-32351930

RESUMEN

Juncus is a perennial herb aquatic plant found worldwide, with high reproductive ability in warm regions. It has three-dimensional hierarchical porous triangular networks structures composited of tubular fibers. Here, juncus derived nitrogen-doped porous carbon (NDPC) was prepared by mixing juncus and ZnCl2 through one-step pyrolysis and activation which is a low-cost, simple, and environmentally friendly method. The NDPC had hierarchical porous structures and a high specific surface area and was applied for supercapacitor and oxygen reduction reaction (ORR). The resulted NDPC-3-800 was prepared by mixing juncus with ZnCl2 at a mass ratio of 1:3 and then carbonized at 800°C, it was used as electrode material of a supercapacitor. The supercapacitor exhibited excellent specific capacitance of 290.5 F g-1 and 175.0 F g-1 in alkaline electrolyte at the current densities of 0.5 A g-1 and 50 A g-1, respectively. The supercapacitor showed good cycle stability, and the capacitance was maintained at 94.5% after 10,000 cycles. The NDPC-5-800 was prepared by mixing juncus with ZnCl2 at a mass ratio of 1:5 and then carbonized at 800°C. It exhibited outstanding ORR catalytic activity and stability attributing to their high specific surface area and abundant actives sites. The juncus can derive various materials for application in different fields.

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