Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 65
Filtrar
Mais filtros

Base de dados
País/Região como assunto
Tipo de documento
País de afiliação
Intervalo de ano de publicação
1.
Proc Natl Acad Sci U S A ; 119(31): e2202884119, 2022 08 02.
Artigo em Inglês | MEDLINE | ID: mdl-35878036

RESUMO

Traditional sulfide metallurgy produces harmful sulfur dioxide and is energy intensive. To this end, we develop an anode electrolysis approach in molten salt by which sulfide is electrochemically split into sulfur gas at a graphite inert anode while releasing metal ions that diffuse toward and are deposited at the cathode. The anodic splitting dictates the "sulfide-to-metal ion and sulfur gas" conversion that makes the reaction recur continuously. Using this approach, Cu2S is converted to sulfur gas and Cu in molten LiCl-KCl at 500 °C with a current efficiency of 99% and energy consumption of 0.420 kWh/kg-Cu (only considering the electricity for electrolysis). Besides Cu2S, the anode electrolysis can extract Cu from Cu matte that is an intermediate product from the traditional sulfide smelting process. More broadly, Fe, Ni, Pb, and Sb are extracted from FeS, CuFeS2, NiS, PbS, and Sb2S3, providing a general electrochemical method for sulfide metallurgy.


Assuntos
Eletrólise , Sulfetos , Eletrodos , Eletrólise/métodos , Grafite , Metais/síntese química , Sulfetos/química , Enxofre/química
2.
Small ; 20(30): e2311334, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38402440

RESUMO

Silicon nanotubes (SNTs) have been considered as promising anode materials for lithium-ion batteries (LIBs). However, the reported strategies for preparing SNTs generally have special requirements for either expensive templates or complex catalysts. It is necessary to explore a cost-effective and efficient approach for the preparation of high-performance SNTs. In this work, a biphasic transformation strategy involving "solid-state reduction" and "dissolution-deposition" in molten salts is developed to prepare SNTs using montmorillonite as a precursor. The rod-like intermediate of silicon-aluminum-calcium is initially reduced in solid state, which then triggers the continuous dissolution and deposition of calcium silicate in the inner space of the intermediate to form a hollow structure during the subsequent reduction process. The transition from solid to liquid is crucial for improving the kinetics of deoxygenation and induces the self-assembly of SNTs during electrolysis. When the obtained SNTs is used as anode materials for LIBs, they exhibit a high capacity of 2791 mAh g-1 at 0.2 A g-1, excellent rate capability of 1427 mA h g-1 at 2 A g-1, and stable cycling performance with a capacity of 2045 mAh g-1 after 200 cycles at 0.5 A g-1. This work provides a self-assembling, controllable, and cost-effective approach for fabricating SNTs.

3.
Environ Sci Technol ; 58(4): 2102-2111, 2024 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-38238255

RESUMO

Waste biomass is one of the promising feedstocks to supply syngas that can be used as fuels, chemicals, reductants, etc. However, the relationship between the component of biomass and the constituent of pyrolysis gas remains unclear. Here, we study the pyrolysis behaviors of various biomasses and reveal the relationship between the biomass components and gas compositions. Further, different pyrolysis gases are applied for the reduction of spent lithium cobalt oxide (LiCoO2) below 500 °C. The pyrolysis gas with a higher concentration of CO has a higher reductivity to convert LiCoO2 to CoO and Li2CO3 with a conversion rate close to 100% in 1 h at 500 °C. The biomass rich in cellulose and with a lower content of lignin tends to produce pyrolysis gas with a high concentration of CO, which comes from the deliberate breakdown of carboxyl, carbonyl, ether, and ester linkages. Moreover, LiCoO2 exerts catalytic functions over the deoxygenation and enhancement of oxygenates and single-ring aromatics. Overall, this paper offers a tailored approach to regulating biomass pyrolysis gases, enabling highly efficient battery recycling and syngas production.


Assuntos
Fontes de Energia Elétrica , Pirólise , Biomassa , Lignina/química , Reciclagem , Gases
4.
Angew Chem Int Ed Engl ; 63(26): e202404025, 2024 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-38659286

RESUMO

Reactive metals hydrolysis offers significant advantages for hydrogen storage and production. However, the regeneration of common reactive metals (e.g., Mg, Al, etc.) is energy-intensive and produces unwanted byproducts such as CO2 and Cl2. Herein, we employ Zn as a reactive mediator that can be easily regenerated by electrolysis of ZnO in an alkaline solution with a Faradaic efficiency of >99.9 %. H2 is produced in the same electrolyte by constructing a Zn-H2O hydrolysis battery consisting of a Zn anode and a Raney-Ni cathode to unlock the Zn-H2O reaction. The entire two-step water splitting reaction with a net energy efficiency of 70.4 % at 80 °C and 50 mA cm-2. Additionally, the Zn-H2O system can be charged using renewable energy to produce H2 on demand and runs for 600 cycles only sacrificing 3.76 % energy efficiency. DFT calculations reveal that the desorption of H* on Raney-Ni (-0.30 eV) is closer to zero compared with that on Zn (-0.87 eV), indicating a faster desorption of H* at low overpotential. Further, a 24 Ah electrolyzer is demonstrated to produce H2 with a net energy efficiency of 65.5 %, which holds promise for its real application.

5.
Small ; : e2308549, 2023 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-38054764

RESUMO

Boosting the hydrogen evolution reaction (HER) activity of α-MoB2 at large current densities and in pH-universal medium is significant for efficient hydrogen production. In this work, Co2 B/MoB2 heterostructured nanoclusters are prepared by molten-salt electrolysis (MSE) and then used as a HER catalyst. The composition, structure, and morphology of Co2 B/MoB2 can be modulated by altering the stoichiometries of raw materials and synthesis temperatures. Impressively, the obtained Co2 B/MoB2 at optimized conditions exhibits a low overpotential of 297 and 304 mV at 500 mA cm-2 in 0.5 m H2 SO4 and 1 m KOH, respectively. Moreover, the Co2 B/MoB2 catalyst possesses a long-term catalytic stability of over 190 h in both acidic and alkaline medium. The excellent HER performance is due to the modified electronic structure at the Co2 B/MoB2 heterointerface where electrons are accumulated at the Mo sites to strengthen the H adsorption. Density functional theory (DFT) calculations reveal that the formation of the Co2 B/MoB2 heterointerface decreases the H adsorption and H2 O dissociation free energies, contributing to the boosted HER intrinsic catalytic activity of Co2 B/MoB2 . Overall, this work provides an experimental and theoretical paradigm for the design of efficient pH-universal boride heterostructure electrocatalysts.

6.
Environ Sci Technol ; 57(19): 7599-7611, 2023 05 16.
Artigo em Inglês | MEDLINE | ID: mdl-37140343

RESUMO

Spent lithium-ion batteries (LIBs) and benzene-containing polymers (BCPs) are two major pollutants that cause serious environmental burdens. Herein, spent LIBs and BCPs are copyrolyzed in a sealed reactor to generate Li2CO3, metals, and/or metal oxides without emitting toxic benzene-based gases. The use of a closed reactor allows the sufficient reduction reaction between the BCP-derived polycyclic aromatic hydrocarbon (PAH) gases and lithium transition metal oxides, achieving the Li recovery efficiencies of 98.3, 99.9, and 97.5% for LiCoO2, LiMn2O4, and LiNi0.6Co0.2Mn0.2O2, respectively. More importantly, the thermal decomposition of PAHs (e.g., phenol and benzene) is further catalyzed by the in situ generated Co, Ni, and MnO2 particles, which forms metal/carbon composites and thus prevent the emissions of toxic gases. Overall, the copyrolysis in a closed system paves a green way to synergistically recycle spent LIBs and handle waste BCPs.


Assuntos
Benzeno , Lítio , Plásticos , Compostos de Manganês , Óxidos , Metais , Fontes de Energia Elétrica , Reciclagem , Polímeros
7.
Nano Lett ; 22(1): 97-104, 2022 01 12.
Artigo em Inglês | MEDLINE | ID: mdl-34958590

RESUMO

The reported mechanical strength of carbon nanocoils (CNCs) obtained from traditional preparation of catalytic acetylene pyrolysis is far below its theoretical value. Herein, we report a molten salt electrolysis method that employs CO32- as feedstock to grow CNCs without using metal catalyst. We meticulously mediate the alkalinity of molten carbonate to tune the electrochemical reduction of CO32- on graphite electrode to selectively grow CNCs in Li2CO3-Na2CO3-K2CO3-0.001 wt %Li2O. Graphite substrate, current density, and alkalinity of molten salt dictate the growth of CNCs. In addition, the electrolytic CNCs shows a spring constant of 1.92-39.41 N/m and a shear modulus of 21-547 GPa, which are 10-200 times that of CNCs obtained from catalyst-assisted gas-to-solid conversions. Overall, this paper opens up an electrochemical way to prepare CNCs through liquid-to-solid conversion without using catalysts and acetylene, providing new perspectives on green synthesis of 1D carbon nanomaterials with high mechanical strength.


Assuntos
Carbono , Grafite , Carbonatos , Catálise , Eletrodos
8.
Langmuir ; 37(35): 10594-10601, 2021 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-34436905

RESUMO

The wettability of molten carbonate on carbon determines the electrochemical performances of high-temperature direct carbon fuel cells (DCFCs). However, a universal method to measure the high-temperature wettability of molten carbonate is absent and the wetting kinetics is not well understood. Herein, we develop a dispensed drop (DD) method to measure the wetting kinetics of molten carbonate (Li2CO3-Na2CO3-K2CO3, 43.5:31.5:25.0, molar ratio) on the carbon substrate at 450-750 °C under controlled atmospheres (100%Ar, 100%CO2, and 1%O2-99%N2). The measured contact angles under different conditions reveal that increasing the O2- concentration in the gas-liquid-solid (GLS) interface decreases the contact angle. In addition, elevating the temperature, introducing O2 in the gas atmosphere, or pretreating the carbon substrate can enhance the wetting kinetics of molten carbonates. The molten carbonate completely wets the carbon substrate in 150 min in Ar gas atmosphere and in 30 min in 1%O2-99%N2 gas atmosphere at 600 °C. Further, it takes only 30 min to completely wet the pretreated carbon substrate in Ar atmosphere at 600 °C. Overall, this paper offers the DD method to study the wettability of molten carbonate on the carbon substrate, which is helpful to understand the underlying wetting mechanism and engineer the electrode design for DCFCs.

9.
Environ Res ; 195: 110883, 2021 04.
Artigo em Inglês | MEDLINE | ID: mdl-33607091

RESUMO

Understanding of the correlation between physico-chemical property of adsorbent and the adsorption performance of contaminant is very significant for developing high-efficient materials to remove antibiotic contamination from water. In this work, a novel kind of carbon adsorbent (EC) derived from CO2 and activated ECs with modified structure via a facile chemical method using H2 and KOH were prepared. The synthetic carbon materials (EC, EC-H2, and EC-KOH) were then applied to remove tetracycline (TC). The kinetics of adsorption for these three carbon materials all well fitted the pseudo-second-order kinetic model. The experimental data of adsorption isotherm had good compatibility with Langmuir and Freundlich models (R2 > 0.90), but the Temkin model was the most applicable for all adsorbents (R2 > 0.98). A super-high adsorption capacity of EC-KOH obtained from Langmuir fitting was 933.56 mg g-1, which was much higher than that of EC-H2 (538.91 mg g-1) and EC (423.30 mg g-1), possibly due to its larger specific surface area (SBET), pore volume, and specific surface chemical structure. Moreover, it was found that surface functional groups and large aperture of adsorbents had a positive effect on adsorption rate. More adsorption sites and surface functional groups of adsorbents were beneficial to enhance the adsorption affinity. These results are of great benefit to the directional control of carbon structure to increase the adsorption performance in rate, capacity, and affinity of antibiotics.


Assuntos
Dióxido de Carbono , Poluentes Químicos da Água , Adsorção , Antibacterianos , Carbono , Cinética , Tetraciclina , Água
10.
Langmuir ; 36(12): 3141-3148, 2020 Mar 31.
Artigo em Inglês | MEDLINE | ID: mdl-32146816

RESUMO

Eco-friendly and economical adsorbents are desirable for removing organic pollutants from the environment. Herein, a kind of green carbon material, electrolytic carbon (EC) prepared by the electrochemical conversion of greenhouse gas (CO2) in molten carbonate, is verified as an effective adsorbent for aniline and other small aromatic organic molecules. The EC consists of nanoparticles and nanoflakes, featuring the specific surface area of ∼641 m2/g with an enriched micropore structure. It exhibits a large adsorption capacity (Qmax > 114.1 mg/g) for aniline, especially in water with a lower contamination level. The adsorption conforms to the pseudo-second-order equation kinetically and the Freundlich model thermodynamically in the temperature range of 303-323 K. Moreover, it is found that the adsorption performance of the material can be further improved through reducing surface oxygen functional groups by a simple thermotreatment. Its adsorption capacity for aniline is enhanced by 1.7 times, demonstrating that the π-π dispersive interaction plays a primary role for the efficient adsorption. This adsorption mechanism is further confirmed by the excellent adsorption performance of the carbon materials for other analogue aromatic compounds (phenol, nitrobenzene). The super performance of the CO2-derived carbon adsorbents will be helpful for capturing CO2 as well as for removing organic pollutants.

11.
Environ Sci Technol ; 54(2): 1242-1249, 2020 01 21.
Artigo em Inglês | MEDLINE | ID: mdl-31838856

RESUMO

Dissolved silicate, as a ubiquitous inorganic component in natural waters, is reported to depress the reactivity of zero-valent iron (ZVI) for reductive reactions under anoxic conditions, but it is unclear if the same inhibitory effect occurs for a ZVI/O2 system. In this study, the role of dissolved silicate for the reactivity of micron-sized ZVI (mZVI) was revisited under aerobic conditions, and different observations were found. Silicate had a volcano-type enhancing effect on the performance of the ZVI/O2 system for sulfamethazine (SMT) degradation. The results showed that, under a circum-neutral or alkaline pH condition (pH 6.0-9.0), the presence of dissolved silicate could significantly enhance the degradation of SMT because silicate coordinated with ferrous ions and further led to the generation of reactive oxygen species (ROS). This study suggests that silicate can act as both a ligand and corrosion inhibitor in a ZVI/O2 system: the coordination of silicate and ferrous iron accelerated the oxidative degradation of organic pollutants in an oxic aqueous solution, while the corrosion inhibitory effect of surface-bound silicate at higher concentrations may decrease the reactivity of the ZVI/O2 system, thereby offsetting the enhancing effect from the silicate-coordinated ferrous iron. This study not only redefines the role of naturally occurring silicate for a ZVI reaction system but also gives clues to develop high-efficiency ZVI/O2 technologies for water remediation.


Assuntos
Ferro , Poluentes Químicos da Água , Estresse Oxidativo , Silicatos , Sulfametazina
12.
J Environ Sci (China) ; 84: 13-20, 2019 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-31284904

RESUMO

Herein, with the exploitation of iron and nickel electrodes, the 2,4-dichlorophenol (2,4-DCP) dechlorinating processes at the anode and cathode, respectively, were separately studied via various electrochemical techniques (e.g., Tafel polarization, linear polarization, electrochemical impedance spectroscopy). With this in mind, Ni/Fe nanoparticles were prepared by chemical solution deposition, and utilized to test the dechlorination activities of 2,4-DCP over a bimetallic system. For the iron anode, the results showed that higher 2,4-DCP concentration and solution acidity aggravated the corrosion within the electrode. The charge transfer resistance (Rct) values of the iron electrode were 703, 473, 444, and 437 Ω∙cm2 for the initial 2,4-DCP concentrations of 0, 20, 50, and 80 mg/L, respectively. When the bulk pH of the 2,4-DCP solution varied from 3.0, 5.0 to 7.0, the corresponding Rct values were 315, 376, and 444 Ω∙cm2, respectively. For the nickel cathode, the reduction current densities on the electrode at -0.75 V (vs. saturated calomel electrode) were 80, 106, and 111 µA/cm2, for initial 2,4-DCP concentrations of 40, 80, and 125 mg/L. The dechlorination experiments demonstrated that when the initial pH of the solution was 7.0, 5.0, and 3.0, the dechlorination percentage of 2,4-DCP by Ni/Fe nanoparticles was 62%, 69%, and 74%, respectively, which was in line with the electrochemical experiments. 10 wt.% Ni loading into Ni/Fe bimetal was affordable and gave a good dechlorination efficiency of 2,4-DCP, and fortunately the Ni/Fe nanoparticles remained comparatively stable in the dechlorination processes at pH 3.0.


Assuntos
Cloro/isolamento & purificação , Clorofenóis/química , Poluentes Químicos da Água/química , Eletrodos , Concentração de Íons de Hidrogênio , Ferro/química , Nanopartículas/química , Níquel/química
13.
Environ Sci Technol ; 51(14): 8077-8084, 2017 Jul 18.
Artigo em Inglês | MEDLINE | ID: mdl-28609093

RESUMO

Sodium disilicate (SD), an inorganic and environmentally friendly ligand, is introduced into the conventional iron electrolysis system to achieve an oxidizing Fenton process to degrade organic pollutants. Electrolytic ferrous ions, which are complexed by the disilicate ions, can chemically reduce dioxygen molecules via consecutive reduction steps, producing H2O2 for the Fenton-oxidation of organics. At the near-neutral pH (from 6 to 8), the disilicate-Fe(II) complexes possess strong reducing capabilities; therefore, a near-neutral pH rather than an acid condition is preferable for the disilicate-assisted iron electrolysis (DAIE) process. Following the DAIE process, the different complexing capacities of disilicate for ferrous/ferric ions and calcium ions can be used to break the disilicate-iron complexes. The addition of CaO or CaCl2 can precipitate ferrous/ferric ions, disilicates and possibly heavy metals in the wastewater. Compared to previously reported organic and phosphorus ligands, SD is a low-cost inorganic agent that does not lead to secondary pollution, and would not compete with the target organic pollutants for •OH; therefore, it would greatly expand the application fields of the O2 activation process. The combination of DAIE and CaO treatments is envisioned to be a versatile and affordable method for treating wastewater with complicated pollutants (e.g., mixtures of biorefractory organics and heavy metals).


Assuntos
Peróxido de Hidrogênio , Metais Pesados/química , Águas Residuárias , Eletrólise , Ferro , Oxirredução
14.
Faraday Discuss ; 190: 147-59, 2016 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-27193579

RESUMO

Carbon powders are building blocks for electrochemical energy storage/conversion devices. Green, cost-affordable and facile preparation of carbon with applicable electrochemical properties is therefore essential for effective utilization of fluctuating renewable energy. Herein, the preparation of carbon nanoflakes via impregnation of waste biomass i.e. boiled coffee beans in molten Na2CO3-K2CO3 (with equal mass) at 800 °C and molten CaCl2 at 850 °C is reported. The microstructure and surface chemistry of the obtained carbons are specified. The correlations between synthetic conditions and microstructure/surface chemistry of the obtained carbons are rationalized. The derived carbon nanosheets are tested and compared as active materials for supercapacitors in a configuration of symmetric full cells in 1 M MeEt3NBF4 in acetonitrile and electrocatalysts towards the oxygen reduction reaction (ORR) in O2-saturated 0.1 M aqueous KOH. Despite the lower surface area, the carbon nanosheets derived in molten Na2CO3-K2CO3 exhibit enhanced capacitive properties and electrocatalytic ORR activity. The present study highlights the importance of thermal media on the microstructure, surface chemistry and electrochemistry of carbon from biomass.


Assuntos
Biomassa , Carbono/química , Oxigênio/química , Eliminação de Resíduos/métodos , Carbonatos/química , Catálise , Café/química , Eletroquímica , Química Verde , Oxirredução , Potássio/química , Propriedades de Superfície , Difração de Raios X
15.
Faraday Discuss ; 190: 241-58, 2016 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-27193751

RESUMO

Electrochemical transformation of CO2 into functional materials or fuels (i.e., carbon, CO) in high temperature molten salts has been demonstrated as a promising way of carbon capture, utilisation and storage (CCUS) in recent years. In a view of continuous operation, the electrolysis process should match very well with the CO2 absorption kinetics. At the same time, in consideration of the energy efficiency, a molten salt electrochemical cell running at lower temperature is more beneficial to a process powered by the fluctuating renewable electricity from solar/wind farms. Ternary carbonates (Li : Na : K = 43.5 : 31.5 : 25.0) and binary chlorides (Li : K = 58.5 : 41.5), two typical kinds of eutectic melt with low melting points and a wide electrochemical potential window, could be the ideal supporting electrolyte for the molten salt CO2 capture and electro-transformation (MSCC-ET) process. In this work, the CO2 absorption behaviour in Li2O/CaO containing carbonates and chlorides were investigated on a home-made gas absorption testing system. The electrode processes as well as the morphology and properties of carbon obtained in different salts are compared to each other. It was found that the composition of molten salts significantly affects the absorption of CO2, electrode processes and performance of the product. Furthermore, the relationship between the absorption and electro-transformation kinetics are discussed based on the findings.

16.
Environ Sci Technol ; 50(19): 10588-10595, 2016 10 04.
Artigo em Inglês | MEDLINE | ID: mdl-27602783

RESUMO

Efficient and high-flux capture of CO2 is the prerequisite of its utilization. Static absorption of CO2 with solid Li2O and molten salts (Li2O-free and Li2O-containing Li-Na-K carbonates) was investigated using a reactor with in situ pressure monitoring. The absorption capacity of dissolved Li2O was 0.835 molCO2/molLi2O at 723 K, larger than that of solid Li2O. For the solid Li2O absorbents, formation of solid Li2CO3 on the surface can retard the further reactions between Li2O and CO2, whereas the dissociation/dissolution effect of molten carbonate on Li2O improved the mass-specific absorption capacity of liquid Li2O. In Li2O-containing Li-Na-K molten carbonate, CO2 was mostly absorbed by alkaline oxide ions (O2-). The chemical interactions between CO2 and CO32- contributed to CO2 uptake via formation of multiple carbonate ions. The mass transfer of these absorbing ions was found as the dominating factor governing the rate of static absorption. Higher temperatures reduced the thermodynamic tendency of CO2 absorption, but a lower viscosity at elevated temperature was conducive to absorption kinetics. Compared with the commonly used CaO absorbent, Li2O was much more dissolvable in molten carbonate. The Li2O-containing molten carbonate is potentially a promising medium for industrial carbon capture and electrochemical transformation process.


Assuntos
Dióxido de Carbono/química , Lítio/química , Carbonatos/química , Sais/química , Termodinâmica
17.
Phys Chem Chem Phys ; 18(48): 32653-32657, 2016 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-27886323

RESUMO

A spontaneous redox reaction of reduced graphene oxide (rGO) in molten Li2CO3-Na2CO3-K2CO3 with a small amount of Li2SO4 at 550 °C was applied to synthesize sulfur and sulfur-cobalt doped rGOs (S-rGO/S-Co-rGO). The obtained S-rGOs and S-Co-rGOs show enhanced catalytic activity for the oxygen reduction reaction (ORR) in alkaline aqueous solutions. The onset reduction potential and the half-wave potential of S-Co-rGO are 60 and 40 mV more positive than those of the original rGO, respectively. The reduction current density of S-Co-rGO increases by nearly five times. This study provides a green and continuous molten salt doping approach for the fabrication of heteroatom-doped graphene with excellent catalytic activity for the ORR.

18.
Angew Chem Int Ed Engl ; 55(26): 7427-31, 2016 06 20.
Artigo em Inglês | MEDLINE | ID: mdl-27159140

RESUMO

Crystalline silicon(Si)/germanium(Ge) alloy nanotubes and hollow particles are synthesized for the first time through a one-pot electrolytic process. The morphology of these alloy structures can be easily tailored from nanotubes to hollow particles by varying the overpotential during the electro-reduction reaction. The continuous solid diffusion governed by the nanoscale Kirkendall effect results in the formation of inner void in the alloy particles. Benefitting from the compositional and structural advantages, these SiGe alloy nanotubes exhibit much enhanced lithium-storage performance compared with the individual solid Si and Ge nanowires as the anode material for lithium-ion batteries.

19.
Chem Soc Rev ; 43(10): 3215-28, 2014 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-24535552

RESUMO

Solid electrode processes fall in the central focus of electrochemistry due to their broad-based applications in electrochemical energy storage/conversion devices, sensors and electrochemical preparation. The electrolytic production of metals, alloys, semiconductors and oxides via the electrochemical reduction of solid compounds (especially solid oxides) in high temperature molten salts has been well demonstrated to be an effective and environmentally friendly process for refractory metal extraction, functional materials preparation as well as spent fuel reprocessing. The (electro)chemical reduction of solid compounds under cathodic polarizations generally accompanies a variety of changes at the cathode/melt electrochemical interface which result in diverse electrolytic products with different compositions, morphologies and microstructures. This report summarizes various (electro)chemical reactions taking place at the compound cathode/melt interface during the electrochemical reduction of solid compounds in molten salts, which mainly include: (1) the direct electro-deoxidation of solid oxides; (2) the deposition of the active metal together with the electrochemical reduction of solid oxides; (3) the electro-inclusion of cations from molten salts; (4) the dissolution-electrodeposition process, and (5) the electron hopping process and carbon deposition with the utilization of carbon-based anodes. The implications of the forenamed cathodic reactions on the energy efficiency, chemical compositions and microstructures of the electrolytic products are also discussed. We hope that a comprehensive understanding of the cathodic processes during the electrochemical reduction of solid compounds in molten salts could form a basis for developing a clean, energy efficient and affordable production process for advanced/engineering materials.

20.
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
SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA