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1.
ACS Omega ; 7(22): 18770-18779, 2022 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-35694459

RESUMO

Activated carbon (AC) made of single-substrate agricultural wastes is considered to be a suitable raw material for the production of low-cost adsorbents; however, the large-scale application of these materials is highly limited by their low efficiency, seasonal scarcity, poor stability, low surface area, and limited CO2 adsorption performance. In this study, composite activated carbon (CAC) was prepared via controlled carbonization followed by chemical activation of four wastes (i.e., peanut shell, coffee husk, corn cob, and banana peel) at an appropriate weight ratio. The Na2CO3-activated CAC showed a higher surface area and valuable textural properties for CO2 adsorption as compared with KOH- and NaOH-activated CAC. The CAC production parameters, including impregnation ratio, impregnation time, carbonization temperature, and time, were optimized in detail. The as-prepared CACs were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), Raman spectroscopy, N2 adsorption-desorption isotherm, and iodine number analysis. The CAC produced at optimal conditions exhibited the highest CO2 removal efficiency and adsorption capacity of 96.2% and 8.86 wt %, respectively, compared with the single-biomass-derived activated carbon. The enhanced CO2 adsorption performance is due to the large surface area, a considerable extent of mesopores, and suitable pore width. The adsorbent in this study reveals a promising strategy for mitigating the CO2 emission problems instead of more expensive and ineffective materials.

2.
Angew Chem Int Ed Engl ; 60(17): 9590-9597, 2021 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-33554402

RESUMO

Insufficient catalytic activity and stability and high cost are the barriers for Pt-based electrocatalysts in wide practical applications. Herein, a hierarchically porous PtNi nanoframe/N-doped graphene aerogel (PtNiNF-NGA) electrocatalyst with outstanding performance toward methanol oxidation reaction (MOR) in acid electrolyte has been developed via facile tert-butanol-assisted structure reconfiguration. The ensemble of high-alloying-degree-modulated electronic structure and correspondingly the optimum MOR reaction pathway, the structure superiorities of hierarchical porosity, thin edges, Pt-rich corners, and the anchoring effect of the NGA, endow the PtNiNF-NGA with both prominent electrocatalytic activity and stability. The mass and specific activity (1647 mA mgPt -1 , 3.8 mA cm-2 ) of the PtNiNF-NGA are 5.8 and 7.8 times higher than those of commercial Pt/C. It exhibits exceptional stability under a 5-hour chronoamperometry test and 2200-cycle cyclic voltammetry scanning.

3.
Angew Chem Int Ed Engl ; 59(33): 13891-13899, 2020 Aug 10.
Artigo em Inglês | MEDLINE | ID: mdl-32356333

RESUMO

Low-cost, non-noble-metal electrocatalysts are required for direct methanol fuel cells, but their development has been hindered by limited activity, high onset potential, low conductivity, and poor durability. A surface electronic structure tuning strategy is presented, which involves doping of a foreign oxophilic post-transition metal onto transition metal aerogels to achieve a non-noble-metal aerogel Ni97 Bi3 with unprecedented electrocatalytic activity and durability in methanol oxidation. Trace amounts of Bi are atomically dispersed on the surface of the Ni97 Bi3 aerogel, which leads to an optimum shift of the d-band center of Ni, large compressive strain of Bi, and greatly increased conductivity of the aerogel. The electrocatalyst is endowed with abundant active sites, efficient electron and mass transfer, resistance to CO poisoning, and outstanding performance in methanol oxidation. This work sheds light on the design of high-performance non-noble-metal electrocatalysts.

4.
BMC Chem ; 13(1): 44, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31384792

RESUMO

BACKGROUND: The existence of heavy metals and coliform bacteria contaminants in aquatic system of Akaki river basin, a sub city of Addis Ababa, Ethiopia has become a public concern as human population increases and land development continues. Hence, it is the right time to design treatment technologies that can handle multiple pollutants. RESULTS: In this study, we prepared a synthetic zeolites and copper doped zeolite composite adsorbents as cost effective and simple approach to simultaneously remove heavy metals and total coliforms from wastewater of Akaki river. The synthesized copper-zeolite X composite was obtained by ion exchange method of copper ions into zeolites frameworks. Iodine test, XRD, FTIR and autosorb IQ automated gas sorption analyzer were used to characterize the adsorbents. The mean concentrations of Cd, Cr, and Pb in untreated sample were 0.795, 0.654 and 0.7025 mg/L respectively. These concentrations decreased to Cd (0.005 mg/L), Cr (0.052 mg/L) and Pb (bellow detection limit, BDL) for sample treated with bare zeolite X while a further decrease in concentration of Cd (0.005 mg/L), Cr (BDL) and Pb (BDL) was observed for the sample treated with copper-zeolite composite. Zeolite X and copper-modified zeolite X showed complete elimination of total coliforms after 90 and 50 min contact time respectively. CONCLUSION: The results obtained in this study showed high antimicrobial disinfection and heavy metal removal efficiencies of the synthesized adsorbents. Furthermore, these sorbents are efficient in significantly reducing physical parameters such as electrical conductivity, turbidity, BOD and COD.

5.
Bioresour Technol ; 280: 213-221, 2019 May.
Artigo em Inglês | MEDLINE | ID: mdl-30771575

RESUMO

Metal-organic framework (MOF) assisted hydrothermal pretreatment and co-catalysis strategy based on UiO-66 MOF is developed for the first time. The Planetree exfoliating bark was pretreated with or without UiO-66 assisted hydrothermal method at a temperature ranging from 160 to 240 °C for 1-3 h residence. With the rise of pretreatment severity, the total reducing sugar (TRS) was increased till reached maximum, 180 mg g-1, in the presence of UiO-66. The fitting models validate the optimal hydrothermal condition was at 180 °C and 1 h, which was characterized with high TRS and very low yield of furfural and HMF. The TRS from enzymatic hydrolysis reaches maximum, 391 mg g-1, in the presence of MOF co-catalysis and the maximum ethanol yield achieved was 73%. Altered morphology, higher surface area and porosity are noticed after MOF assisted hydrothermal pretreatment. This study insights the MOFs' application in lignocellulose biomass processing.


Assuntos
Etanol/metabolismo , Magnoliopsida/metabolismo , Estruturas Metalorgânicas/farmacologia , Zircônio/farmacologia , Biomassa , Furaldeído/metabolismo , Hidrólise , Lignina/metabolismo , Casca de Planta/metabolismo
6.
Bioresour Technol ; 270: 377-382, 2018 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-30243245

RESUMO

Developing a new cellulase-MOF composite system with enhanced stability and reusability for cellulose hydrolysis was aimed. Physical adsorption strategy was employed to fabricate two cellulase composites, and the activity of composite was characterized by hydrolysis of carboxymethyl cellulose. The NH2 functionalized UiO-66-NH2 MOF exhibited higher protein loading than the precursor UiO-66, due to the extra anchor sites of NH2 groups. The immobilized cellulase showed enhanced thermostability, pH tolerance and lifetime. The maximum activity attained at 55 °C could be kept 85% when used at 80 °C, and the residual activities were 72% after ten cycles and 65% after 30 days storage. The abundant NH2 and COOH groups of MOF adsorb cellulase and enhance its stability, and the resulted heterogeneity offered the opportunity of recovering composite via mild centrifuge. The findings suggest the promising future of developing cellulase-MOF composite with ultrahigh activities and stabilities for practical application.


Assuntos
Celulase/metabolismo , Celulose/metabolismo , Estruturas Metalorgânicas/química , Zircônio/química , Adsorção , Celulose/química , Hidrólise
7.
Phys Chem Chem Phys ; 19(31): 20881-20890, 2017 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-28745359

RESUMO

Hematite (α-Fe2O3) is a suitable candidate for photoelectrochemical water splitting due to its well-suited band structure, stability, and availability. However, water splitting using a low external potential is the major challenge that limits the practical application of hematite. Here, we achieve a very low onset potential using a sequential surface treatment approach to overcome two fundamental limiting factors, sluggish hole transfer, and interfacial recombination, independently. First, a heavily doped Fe2-xSnxO3 surface passivation layer was created by Sn4+ surface treatment which can robustly inhibit interfacial recombination. Then, an NiOOH catalyst layer was deposited that greatly enhances the charge transfer process across the passivated electrode/electrolyte interface. By exploiting this approach, the optimized sequentially treated photoanode (Fe2O3/Fe2-xSnxO3/NiOOH) exhibits a low photocurrent onset potential of 0.49 V vs. RHE and a saturated photocurrent density of 2.4 mA cm-2 V at 1.5 V vs. RHE. Transient photocurrent and impedance spectroscopy measurements further reveal that the combined Fe2-xSnxO3/NiOOH layers reduce interfacial recombination and enhance charge transfer across the electrode/electrolyte interface. The results provide convincing evidence that it is possible to address the problems of surface trap recombination and sluggish catalysis independently by employing surface passivation layers first and catalysts later sequentially.

8.
Nanoscale Horiz ; 1(4): 243-267, 2016 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-32260645

RESUMO

Photoelectrochemical (PEC) water splitting is a promising technology for solar hydrogen production to build a sustainable, renewable and clean energy economy. Hematite (α-Fe2O3) based photoanodes offer promise for such applications, due to their high chemical stability, great abundance and low cost. Despite these promising properties, progress towards the manufacture of practical water splitting devices has been limited. This review is intended to highlight recent advancements and the limitations that still hamper the full utilization of hematite electrodes in PEC water splitting systems. We review recent progress in manipulating hematite for PEC water splitting through various approaches, focused on e.g. enhancing light absorption, water oxidation kinetics, and charge carrier collection efficiency. As the morphology affects various properties, progress in morphological characterization from thicker planar films to recent ultrathin nanophotonic morphologies is also examined. Special emphasis has been given to various ultrathin films and nanophotonic structures which have not been given much attention in previous review articles.

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