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By E. V. Verhoej

The proposed EU directive on the restriction of the use of certain hazardous substances in electrical and electronic equipment promotes the substitution of lead in consumer electronics to reduce emissions from lead in the end of life phase. In this paper, the consequences of substituting lead in solders is assessed using the Eco-Indicator-99 method for the examples. The base metal production system is considered as an interconnected network modeled dynamically in Simulink 4 and Matlab 6 (Mathworks Inc 2000), where the recovery and production of metal components of the assessed product partially overlap. This approach requires global modeling of metal production processes and mass balances and resulting allocation choices. It also reveals the susceptibility of LCA scores to different choices in the modeling and data availability and uncertainty. Besides the comparison between lead-free and lead-containing solders, other side effects are revealed. Lead is carrier material for the recycling and production of many co-elements in the interconnected production and recovery system. Substitution may have adverse effects such as temporary shortages of other connected metals that are often not considered in normal LCA assessments, thus leading to erroneous results. The suggested approach provides directions for including these extemal effects and for further assessment of the environmental effects of substituting lead. This paper shows that in order to assess the environmental aspects of metallurgy, dynamic modeling of the total system is required based on the fundamental thermodynamics in each metallurgical reactor, the basis of this dynamic model. With this the true environmental impact of metallurgy can be explained. In the case of lead free solder, it is shown that the mining of substitutes has a very much larger impact.

Jan 1, 2003

By Cassandre Nowicki, Louis Gosselin, Carl Duchesne

"Quebec's primary aluminium production industry consumes roughly 39 TWh of electricity per year and is accountable for roughly 7 million tons of CO2 equivalent. By tapping only a small portion of waste heat and integrating it inside the production facility itself, we can significantly reduce GHG emissions and energy consumption. Although the amount of thermal waste can be adequately estimated by applying an energy balance to production processes, this provides very little information on the quality of waste heat and its potential for integration. A measure of exergy is required. Waste heat streams characterized by high exergy content may generally offer valuable incentives for recovery and integration. More generally, exergy values limit integration possibilities. An exergy analysis is provided for the aluminium electrolytic reduction process. This is meant to guide future heat recovery initiatives and energy efficiency measures.IntroductionCanada is one of the world leaders in primary aluminium production and 92% of its aluminium production capacities are located in the province of Quebec. In 2007, production capacity reached 2,786,000 tons in Quebec alone. Since it is estimated that 2.5 equivalent tons ofCO2 are released for each ton of aluminium produced in Canada, Quebec's aluminium production industry is accountable for roughly 7 million tons of CO2 yearly [1, 2]. Furthermore, with an average electricity consumption of 14 MWh per ton, primary aluminium accounts for 39 TWh of electricity per year in Quebec and this energy consumption represents 350 thousand tons ofCO2 equivalent [3, 4]. Natural gas consumption associated with primary aluminium production accounts for less than 1 TWh, but it represents an additional 350 thousand tons of CO2 equivalent [ 4].This work is meant to provide a tool to guide future efforts towards heat recovery and energy efficiency in the primary aluminium industry. Waste heat recovery and thermal integration can cut down both energy consumption costs and GHG emissions. In a primary aluminium production facility, waste heat represents roughly half of the energy input into the Hall-Heroult process. Tapping only a small portion of this energy could reduce natural gas and electricity consumption significantly. In order to evaluate how much of this energy is actually usable, we propose to apply an exergy analysis to individual transformation processes in an aluminium production facility, such that a potential to do work can be assigned to every waste heat flux. The approach will be described in the next section."

Jan 1, 2012

By J. M. Toguri

The viscosity of the molten FeO-Fe2O3-Si0z system in the composition range of interest to copper smelting has been investigated using a rotating cylinder technique. The silica content of the slag was varied from 20 to 35 wt percent while the oxygen pressure of the system was varied from 10-7 10-11 atm. The temperature range investigated was from 1200 to 1350°C. It was found that the viscosity of the slag generally decreased with increasing temperature and increasing oxygen pressure. As the silica content was increased, the viscosity was found to increase.

Jan 1, 1976

By M. Kawakami

In relation to the designing of a new-type blast furnace, the reaction of carbonaceous materials with C02 is expected to occur at as low temperature as possible. In order to get a highly reactive carbonaceous material at low temperature, the reaction kinetics was investigated by measuring such quantities as the reaction rate from weight loss, the amount of CO adsorption and specific surface area by BET method. The reaction rates were large in the order of the Bintyo char, metallurgical coke, graphite and glassy carbon. If the rate was converted to the rate per unit area, however, those of the Bintyo char was smaller than that of graphite. Thus, it is suggested that the rate of the Bintyo char is influenced by the pore diffusion of C02. The rate had a positive relation with the amount of CO adsorption, showing that the rate determining step would be the desorption of CO from the active side on the surface. The rate independent of surface area was derived, combining al\ the obtained data.

Jan 1, 2003

By J. J. Moore

The application of plasma technology to process metallurgy is briefly discussed. Experiments involving in-flight reduction of minerals (taconite, chromite, in particular) with a solid-based carbon reductant are described. The resultant metallic and slag product analysis is discussed with respect to thermodynamic and kinetic considerations.

Jan 1, 1985

By Xiao Yang

Calcium oxide is one of the major fluxing agents used for steel refining. Because unreacted CaO remains in slag in most cases, discharged slag is difficult to be recycled smoothly. With the growth of environmental concerns, improving utilization efficiency of CaO is required to reduce the amount of discharged slag and energy consumption. The authors have reported a resource and energy-saving process by using multi-phase flux for dephosphorization. Reaction behavior of phosphorus in multi-phase CaO–FeOX–SiO2–P2O5 flux system was investigated. Formation mechanism of P2O5-rich phases was clarified at the interface between solid CaO or 2CaO, SiO2 and molten CaO–FeOx–SiO2–P2O5 slag. Phase relationship and thermodynamic properties of 2CaO, SiO2-3CaO, P2O5 solid solution were observed to confirm the condensation of P2O5 in solid phase. Based on these results, reduction of CaO consumption, discharged slag curtailment, and energy-saving effects in the novel refining process by using multi-phase flux were discussed.

By Christoph Sagadin

Corrosion mechanisms between high melting synthetic ferronickel slags and refractory were investigated. The used slags were prepared by mixing and melting of specific oxides. Substrates of the applied refractory material and specimens of FeNi slags were heated in a hot stage microscope up to 1650 °C. The experiments were performed under a defined gas atmosphere of 60% CO and 40% CO2. A further examination of the formed phases between slag and refractory occurred by scanning electron microscope. The investigations indicate that the slag penetrates between magnesia grains and partly dissolves magnesia. Spot analyses show that iron diffuses into the magnesia grains, which transform to magnesiawustite, meanwhile SiO2 forms different types of olivine like forsterite and monticellite. Thermodynamic calculations confirm the formation of these phases. The combination of practical lab scale experiments and thermodynamic calculations should finally contribute to an improvement of the refractory lifetime and performance.

By A. Kiziltas, D. J. Gardner, C. W. Mcllwraith, J. W. Bridge, M. L. Peterson

"Dynamic mechanical thermal analysis (DMTA) tests were conducted on high-oil content, paraffin-based wax used in wax-coated granular composites. These composites make up the surface of synthetic Thoroughbred horse racetracks used in North America. The modulus and damping response from the DMTA tests were correlated with the dynamic triaxial shear strength response of the bulk track material taken at two different operational temperatures and at four strain rates. The purpose of these tests is to understand the mechanisms of shear strengthening of the bulk track material as the wax is heated through the first crystalline solid to liquid nominal transition temperature. Previous work using differential scanning calorimetry confirmed that under common operational surface temperatures, the wax coatings undergo distinct thermal transitions. The resulting increase in triaxial shear strength values affects the consistency of the racetrack which, in turn, can potentially affect Thoroughbred racing performance and safety of the track surface.IntroductionSynthetic granular composite materials are being used in nine Thoroughbred horse racetracks in the United States as well as in other tracks around the world. In one case, their use was mandated by the state of California in 2007 due to testimony that these tracks were significantly safer than traditional dirt tracks [1]. Several synthetic tracks have shown substantial reductions in injuries since switching to synthetics; one California track showed a 75% reduction in catastrophic horse injuries during the first year as compared to the previous year racing on a dirt track [2]. The composition of the tracks in the U.S. generally consist of silica sand (>70%), polymer fibers (<5%), and rubber particles (0-15%) all coated with a paraffin-based, high oil content wax [3, 4]. In a recent study of several synthetic racetracks, to include the track location in this study, the oil content ranged from 34 to over 44% by mass [5]."

Jan 1, 2011

By G. Johnston, J. Greenly, R. G. Buchheit, D. C. McIntyre, R. Muenchausen, D. J. Rej, R W. Stinnett

"Rapid thermal treatment of materials using high energy, high flux, pulsed ion beams can produce modified surface layers with unique microstrutures and properties. High energy ions loose their energy during the slowing down process in the workpiece and thus deposit their energy continuously over a depth of a few microns. The deposition of energy can lead to melting and in some causes ablation of the heated layer. Because the pulse duration of the ion beams is typically only 50-200 ns, steep thermal gradients generated during heating facilitate rapid cooling (107K/sec-108K/sec) of the treated layer by thermal diffusion into the underlying material. Rapid heating and cooling of materials can generate surface layers with non-equilibrium amorphous or nano-crystalline microstructures that exhibit increased hardness, wear resistance, and corrosion resistance. Pulsed ion beam treatment can also lead to surface smoothening or can be used to mix thin « 1 11m thick) coatings into underlying substrates. Pulsed ion beams can be generated using existing ""flashover"" ion source technology which is capable of producing single shot, mixed C, H, and O ion beams with beam cross sections of approximately 100 cm2 and energy fluxes up to 100 J/ cm2. Recent advances in repetitive high energy pulsed power technology and development of magnetically confined anode plasma ion sources have facilitated the development of ion beam systems that generate single species beams that pulse continuously at 120 shots/second. These capabilities will allow rapid treatment of large surface area workpieces at low cost.IntroductionThe rapid solidification of liquid materials can create unique materials and material microstructures that often have properties that can lead to enhanced performance. Rapid solidification processing of the surfaces of materials using continuous and pulsed laser beams (laser glazing) has been explored for over 20 years (1-5). Advances in high energy, pulsed electron and ion beam technologies over the past decade have provided rapid thermal treatment techniques that may be less expensive to impliment than laser surface treatment for many surface modification applications (6). High energy pulsed ion beams have recently been used to harden aluminum(7), copper(8) and tool steel surfaces (6,9), increase corrosion resistance of Al alloys (6), mix coatings into underlying substrates (10), and create amorphous films (11,12)."

Jan 1, 1994

By Francis Vanbellen

Umicore Precious Metals Refining operates an integrated precious metals smelting and refining plant in Hoboken, Belgium. Once a smelter and refiner of complex concentrates, the plant today?s feed consists exclusively of industrial and consumer recycled products, making it the world?s largest recycling facility for precious metals. Unlike the fairy tale of the Frog Prince, it took much more than a princess? kiss to successfully realize this makeover. A completely renewed plant has been built over the past decade.

Jan 1, 2006

By Akira Yazawa

The continuous converting has attractive advantages, but further experimental studies on the slag are required, when the process is considered thermodynamically. The summarized experimental results, obtained with iron silicate slag and with ferrite slag and results relating to actual operation are described and discussed in this paper. At first, equilibrium relations at controlled oxygen potentials among three melts of silica-saturated iron silicate slag, white metal and copper are investigated. The results obtained for slag agreed with the thermo-dynamical predictions. Namely, to suppress a magnetite separation, the system should be at high temperature; in the case of the S02 gas of 10 kPa, for example, magnetite did not separate from the slag at 1300°C, but at 1250 and 1200°C the slag was saturated with magnetite even at lower SO2 pressure. Copper losses caused by dissolution of its oxide increased with increasing 5O2 pressure, and were slightly lower than those reported in previous papers without the matte phase. When the continuous converting slag does not contain any appreciable amount of silica - in contrast to the conventional smelting slag ferrite slag would form, but there was no published fundamental work on-ferrite slags. Hence, the melting behavior and activities of the system CaO-Cu2O-Fe2O3 have been investigated. The liquidus diagram in nitrogen atmosphere was, constructed using both thermal analysis and quenching method. The low liquidus temperature region without magnetite separation was found in the part of low content of Cu2O in the section Cu2O-CaO-Fe2O3 and Cu2O?Fe2O3¬CaO?Fe2O3. The activity of Cu2O in the system was also measured. Slags, composed-of CaO, Cu2O and Fe2O3, in platinum crucibles were equilibrated at 1250°C and controlled oxygen pressures. After quenching, the-composition of slag and platinum crucible were determined qualitatively. On the thermo-dynamic analysis of the results, iso-activity lines were drawn, and it was shown that the slag in the converting furnace of the Mitsubishi process exists in an adequate region of the composition triangle.

Jan 1, 1976

By Alicia E. Ares, Carlos E. Schvezov

In the present work it was observed the nucleation and growth of grains in the equiaxed zone of metal matrix composites (MMCs) samples directionally solidified wit the presence of columnarto- equiaxed transition (CET) in the samples. In order to do so, first, it was defined the difference between the real temperature at a given instant, which it is used in the analysis, its variation and furthermore, the variation in the solid fraction with time between the beginning and the end of solidification. It was determined a growth law assuming a lineal variation of equiaxed grain radius as a function of time, and also, it was expressed a law of grain density as a function of time, considering the presence of SiC and Al2O3 particles in the matrix. Finally, the results obtained were validated with measured values of grain density at each position of the thermocouples in the equiaxed zone of the solidified samples.

Jan 1, 2015

By Kouji Mimura, Tamas Kekesi, Yongfu Zhu, Masahito Uchikoshi, Minoru Isshiki

"The formation and anion exchange sorption of chloro complex ions can offer a great potential to be utilized for the separation and purification of metals in aqueous solutions. Available stability data were primarily used to estimate the predominance of chloro complex species, indicating the feasibility of such separations. Anion-exchange sorption functions, describing the equilibrium distribution of a number of important elements have been determined by the batch equilibrating method in the practical HC1 concentration range. Various oxidation states were stabilized by the addition of appropriate agents. Tendencies in oxidation, complex formation and anion exchange sorption were confirmed by spectrophotometric investigations. Based on the fundamental results, anion exchange processes have been developed for the purification of iron, cobalt, copper and zinc. The efficiency of separation was assessed and the procedure optimized by the analysis of experimental elution curves. Results have demonstrated that by properly controlling the oxidation states and HC1 concentrations, practically all the impurities can be eliminated. Computer programs have been developed to estimate complex formation and redox equilibria, to screen and correct analytical data, to determine distribution coefficients and to evaluate efficiencies of separation.IntroductionBase transition metals have long been used as the staple materials in various fields of industry. In general, there has been an increasing tendency in purity requirements but recent advances have created a rapidly increasing demand for ultra-high purity metals. To give a few examples, ultra high purity copper can be used as bonding wire and interconnection in integrated circuits, or as material for superconductor stabilizing, high-field magnets, beside its use in cryogenics and ultra high vacuum technology [1]. Iron holds promises as a constituent element in the ß-FeSi2 material to be applied in new opto-electronic devices [2] and it is currently used, together with chromium and manganese, in the production of special magneto-optical materials for digital recording. The use of ultra high purity manganese and chromium in semiconductor technology is evolving. Although not considered a transition metal, zinc is also treated here because of the major significance in compound ZnSe semiconductors [3], and the possibility to purify it by the anion exchange method."

Jan 1, 2000

By M. Okido, H. Yamamoto, T. Sakamoto, R. Ichino, K. Kuroda

"Hydrogen absorption alloy films have been produced by molten salt electrolysis. Lanthanum-Nickel alloy film can be formed on a nickel substrate in KCl-NaCl-LaCb molten salts by electrolysis diffusion process. LaNi5 alloy was formed by mutual diffusion between La ·and Ni after La deposition on Ni substrate. Though several kinds of La-Ni compound existed in deposits, the alloy compounds on Ni substrate changed by electrolysis condition. According to the open-circuit potential measurement in molten salts after La electrodeposition, the formed compounds had a relation to the potential. In the case of the substrate electroplated a cobalt thin film on nickel, LaNi4_5Co0.5 was formed by the electrolysis in the molten salts with lanthanum ions. This ternary alloy film showed better hydrogen absorption behavior in cyclic charge/discharge test in alkaline solution.IntroductionHydrogen storage alloys have attracted attention as the active materials for batteries with the charge/discharge property at ambient temperature. The alloy of nickel and misch metal, mainly consisting of La and Ce, has been commercially 'used as a metal hydride with rechargeable property. In recent years, researches have been developed many kind of new alloys with better hydrogen absorption properties. The hydrogen absorbing alloy ingots are commonly produced by melting method of both metals in furnace, otherwise, prepared by mechanical grinding and metallurgical sintering technique with metal powders. The film is also made by vapor-phase techniques such as sputtering method, ion plating method, etc. ·We have proposed a new method to produce hydrogen absorbing alloy films by molten salts electrolysis technique [1-3]. The hydrogen absorbing film, LaNi5, Mg2Ni and CaNi5, were obtained in this process through controlling the electrolytic condition. The active metals, La, Mg and Ca, are electrodeposited on Ni substrate, diffuse into the substrate and form various kinds of intermetallic compounds. This technique provides a direct process using metal chlorides as resources to produce functional films without using active metals such as La, Ca and Mg."

Jan 1, 2000

By Baoxiang Zhang, Jing Zhang

"As extruded Mg-9Zn-0.6Zr-2Er magnesium alloys were hot-rolled at 400°C, followed by solution treatment at 400 °c for 1. 5h and artificial aging at 200°C for 10h. Microstructures and tensile mechanical properties of the alloys after hot rolling, solution and aging treatment were examined respectively. Optical micrographs of the as-rolled and as-solution alloys showed fine grain structures, due to the formation of Er-and Zn-bearing compounds at grain boundaries which obviously improved the thermal stability of the alloy. Yield strength as high as about 335 MPa was obtained for the as-rolled alloy, showing that the mechanical properties of the alloy was greatly benefit from the grain refinement and dynamic precipitation of fine MgZn2 during hot rolling. Due to solution heat treatment, vast majority of the Mg-Zn phases dissolved into the matrix, and precipitated out again as fine dispersoid during the subsequent aging, resulting in an enhanced aging-hardening effect.IntroductionWith high specific strength and low density, magnesium alloy has stimulated significant interest for the applications in microelectronics, aerospace and automobile industries. Due to its HCP structure, magnesium alloys exhibit relatively poor strength and ductility. Great efforts have been made to improve the properties of magnesium alloys.Thermo-mechanical processing which combined with subsequent heat treatment can strengthen magnesium alloys due to the strain-hardening mechanism, homogeneous distribution of second particles and grain refinement [1, 2]. However, commercial wrought magnesium alloys have high tendency of grain growth at high temperature due to lack of effective solutions to stabilize the microstructure [3, 4, and 6]. But Magnesium-RE alloys containing high rare earth were reported to have remarkable thermal-stability, Rare earth (RE), such as Y, Nd, Yb, Gd, Ce, were known to form second-phase particles that have higher thermal stability combining with Zn and matrix in Mg[12-17]."

Jan 1, 2012

By Jan G. H. du Preez, C. Viviers, B. J. A. M. van Brecht, H. E. Rohwer, Nicole M. Sumter

"At the basis of metal ion separation lies some particularly metal ion specific chemical property which lends itself towards exploitation. This could be in the form of an anionic complex or a neutral chelate complex. In the former a cationic centre with a particularly high affinity for the complex will have to be designed. In the latter case a stereospecific chelate ligand containing the correct symmetry and type of donor atoms will have to be designed. In both above cases the ""active centre"" can be entered in a from that it can function in different media of hydrophobicity, eg a precipitant, a resin or a solvent extractant. Recent results obtained in this laboratory will be used to illustrate how the above variables can be exploited to develop improved processes for the separation of base metal and platinum group metals.IntroductionThe separation of metal ions in hydrometallurgy can be performed broadly speaking with two major aims. Firstly the separation/removal of a certain group of metal ions, either as a means of preconcentration or as a removal from effluent as part of a purification process and, secondly the removal of a specific metal ion from an industrial stream in order to produce a specific metal in a pure form. This latter operation is by far the most difficult of the two and is becoming more so in the light of the fact that the world is moving in the direction of lower grade ores and increasing pollution. Such a process can be divided into three essential parts, firstly the molecular one in which an active centre is required to obtain specificity, secondly a matrix within which this active centre must function, i.e. as part of a resin or solvent extractant and thirdly the design of the total system to optimize the realization of the operation."

Jan 1, 1996

By Fathi Habashi

Solid gas reactions of metallurgical importance can be classified into three groups: Physical processes, e.g., drying and sublimation Chemical processes which may be an addition or a thermal decomposition reaction Electrochemical processes which may be addition, oxidation-reduction, or displacement reactions. Examples are given and the role of the boundary layer is emphasized.

Jan 1, 1996

By S. Mattlgod

Self-assembled monolayers on mesoporous supports (SAMMS) have been developed for the removal of heavy metals and some transition metals. The thiol functional groups were assembled on the internal and external surfaces of mesoporous silica with a uniform pore size of about 55 A. The mesoporous supports provide high surface area (>900 m2/g) needed for high metal loading in chemical separation. Self-assembled monolayers of organic molecules bond to the ceramic substrate with prescribed densities, and with terminal functional groups for excellent molecular selectivity. The unique characteristics include: (1) High metal absorption capacity, up to 3.2 mmol/g of SAMMS. (2) Fast Hg-binding kinetics (reducing mercury concentration from 0.5 ppm to 0.5 ppb in less than 5 minutes). (3) High selectivity in the presence of a range of cations, anions, and organic species. (4) Applicability in both aqueous and non-aqueous solvents. (5) Flexibility in surface chemistry. The materials can be designed to adsorb heavy metals, transitional metals, and radionuclides. (6) Chemical stability, and potential for regeneration or waste storage. This paper discusses the results on mercury adsorption.

Jan 1, 1999

By C. Beckennann, C. Y. Wang

"Computer simulations of structural and compositional development in equiaxed dendritic alloy solidification are performed using a recently developed multi phase model. The model not only accounts for the transport phenomena occurring on the macroscopic (system) scale, but includes also the grain nucleation and growth mechanisms taking place at various microscopic length scales. In this paper, a numerical technique consisting of a fully implicit control-volume based finite difference method and a multiple time step scheme is developed for accurate and efficient simulations of both micro- and macro-phenomena. Sample numerical results are presented to reveal the effects of liquid now and crystal sedimentation on segregation and the final grain size distribution. In particular, the importance of the interplay between the dendrite microstructure and multiphase now patterns is shown.IntroductionIn recent years, modeling of equiaxed dendritic solidification without convection has experienced considerable progress (1,2]. Nucleation and growth kinetic laws have been coupled with transient heat conduction calculations to determine the solidification microstructure. However, modeling of equiaxed dendritic solidification with melt convection and solid movement has not been attempted so far, largely because of the complications associated with the transport of free equiaxed crystals in the melt. The gravity-induced transport of free crystals is fundamental to the development and extent of the equiaxed zone and also greatly affects the columnar to equiaxed transition. Another possible effect of crystal sedimentation or floatation is to cause severe macrosegregation as well as structural inhomogeneities. The only study available in the literature that accounts for both liquid convection and solid transport is by Ni and Beckermann (3], but deals with globulitic structures (as opposed to dendritic)"

Jan 1, 1994

By Dinesh P. Amalnerkar, Nagegownivari Munirathnam, Tirthalli Prakash, Katia Vutova, Vania Vassileva, Veliko Donchev

"A time-dependent model for electron beam melting and refining (EBMR) of different metals and alloys is developed. The model is 3D axi-symmetrical and an adapted numerical scheme of Pismen-Rekftord type is applied. The developed computer program computes the thermal fields in the metal ingots during EBMR process as well as the dynamics of the thermal streams and the geometry of the molten metal pools. Calculated results for different regimes of EBMR of titanium are obtained and discussed in the paper. Experiments are performed and impurities' concentration data are presented. Simulation results are compared with experimental data and are used for optimization of the EBMR process in the case of Ti.IntroductionElectron beam melting and refining (EBMR) has an important role in the special electrometallurgy[ 1-6] and it is approved for obtaining of pure titanium [7]. EBMR of metals and alloys is being recognized as a competitive and even the single method for obtaining new materials for all areas of human activity.The principal scheme of the EBMR drip process is shown in Fig.1. A thin layer of molten metal is formed on the front part of the feeding rod during the e-beam processing and generated droplets fall into the molten pool in the crucible where the ingot is formed. The refining is mainly realized at the boundary liquid metal - vacuum. There are three zones in EBMR (Fig.1) - on the front part of the feeding rod (zone I in Fig.1 ), on the surface of the generated droplets (zone II in Fig.1) and the surface of the molten pool in the water-cooled copper crucible (zone III in Fig.1)."

Jan 1, 2013