Effect of Holey Graphene Chemistry on Li – S/Se Battery Cathode Performance
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lithium-sulfur batteries, holey graphene, high mas↗
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Behavior of sulfur at high pressures and low temperatures
A new type of high-pressure apparatus for low-temperature experiments was built, which allows loading and measuring the load in situ at low temperature (1.5 K). It uses the diamond anvil in the flat-indentor configuration. It was used to investigate the high-conductivity state of sulfur at low temperatures. For pressures in the 50-GPa range, sulfur is still a semiconductor or at best a two phase semiconductor-metal system. As the temperature is lowered at 50 GPa, the resistance drops slightly, reaches a minimum around 230 deg K, and then increases dramatically.
Golopentia, D. A.↗
Heterogeneous Chemistry of HONO on Liquid Sulfuric Acid: A New Mechanism of Chlorine Activation on Stratospheric Sulfate Aerosols
Heterogeneous chemistry of nitrous acid (HONO) on liquid sulfuric acid (H2SO4) Was investigated at conditions that prevail in the stratosphere. The measured uptake coefficient (gamma) of HONO on H2SO4 increased with increasing acid content, ranging from 0.03 for 65 wt % to about 0.1 for 74 wt %. In the aqueous phase, HONO underwent irreversible reaction with H2SO4 to form nitrosylsulfuric acid (NO(+)HSO4(-). At temperatures below 230 K, NO(+)HSO4(-) was observed to be stable and accumulated in concentrated solutions (less than 70 wt % H2SO4) but was unstable and quickly regenerated HONO in dilute solutions (less than 70 wt %). HCl reacted with HONO dissolved in sulfuric acid, releasing gaseous nitrosyl chloride (ClNO). The reaction probability between HCl and HONO varied from 0.01 to 0.02 for 60-72 wt % H2SO4. In the stratosphere, ClNO photodissociates rapidly to yield atomic chlorine, which catalytically destroys ozone. Analysis of the laboratory data reveals that the reaction of HCl with HONO on sulfate aerosols can affect stratospheric ozone balance during elevated sulfuric acid loadings after volcanic eruptions or due to emissions from the projected high-speed civil transport (HSCT). The present results may have important implications on the assessment of environmental acceptability of HSCT.
Zhang, Renyi↗
NiF2 Cathodes For Rechargeable Na Batteries
Use of NiF2 cathodes in medium-to-high-temperature rechargeable sodium batteries increases energy and power densities by 25 to 30 percent without detracting from potential advantage of safety this type of sodium battery offers over sodium batteries having sulfur cathodes. High-energy-density sodium batteries with metal fluoride cathodes used in electric vehicles and for leveling loads on powerlines.
Bugga, Ratnakumar V.↗
Ultrahigh Mass Loading Batteries with Holey Graphene-Enabled Dry-Pressed Cathode Architectures
Holey graphene is a structural derivative of graphene with arrays of nanometer-sized, through-thickness holes across the lateral surface of the atomically thin nanosheet. It has been widely acknowledged that the presence of holes improves ion transport through the graphene planes, making holey graphene an ideal electrode material for electrochemical energy storage. We recently discovered another unique attribute of holey graphene in that it can be directly compressed from powder into electrode in a single step without the use of solvent or binder. In addition to neat holey graphene electrodes, composite electrodes with holey graphene as an ultralightweight scaffold host filled with various active materials can also be readily prepared in a similar solvent-free and binder-free fashion. The active materials can be metal-containing catalysts for lithium-oxygen batteries, lithium-ion battery electrode materials, or high energy density components such as sulfur. Compared to the conventional slurry-based process, the dry-press method is comparably much more suitable toward the facile and scalable preparation of ultrahigh mass loading electrodes with ultrahigh areal capacities.
holey graphene, cathode scaffold, lithium metal, h↗
Solvent-Free Preparation of High Energy, Binder-Free Electrodes Enabled by Dry Compressible Holey Graphene
Graphene is an atomically thick sheet consisting of a graphitic carbon network with excellent mechanical strength, electrical and thermal conductivity, and chemical stability. Holey graphene, a structural derivative of graphene, has an array of through-the-thickness holes across the lateral surface of the nanosheet. The presence of these holes has minimal detrimental effect on the graphene properties and leads to enhanced performance in applications such as electronics, sensors, and energy storage. For example, these holes allow more facile cross-plane ion and gas transport than intact graphene, making holey graphene an ideal electrode material for electrochemical energy storage. This presentation will focus on the ability of holey graphene to be compression molded into robust articles or architectures under solvent-free conditions without the need for potentially parasitic binders. The unique dry compressibility of holey graphene has enabled facile fabrication of high mass loading electrodes with both high density and high porosity, which have found use in supercapacitors and various high-energy battery systems such as lithium-oxygen, lithium-sulfur, and lithium-selenium batteries.
Yi Lin↗
Dry Pressed, High Areal Loading Electrode Architectures Enabled by Holey Graphene
For future electric aviation, advanced battery cell chemistry beyond lithium ion batteries are required to meet mission requirements. High energy density battery concepts such as lithium-sulfur (Li-S) and lithiumoxygen (Li-O2) chemistries are being intensively investigated to realize their extraordinary theoretical promise in terms of energy density. Most fabrication methods of cathodes for these novel battery chemistries followed a conventional approach. In this approach, the active material is mixed with a polymer binder and a conductive carbon in a high-boiling organic solvent to form a slurry, followed by casting onto a current collector and solvent evaporation. The process is usually lengthy and poses environmental hazards due to the use of organic solvents.
Lin Yi↗
Interrelationships Between Aerosol Characteristics and Light Scattering During Late-winter in a Eastern Mediterranean Arid Environment
An intensive field campaign involving measurement of various aerosol physical, chemical, and radiative properties was conducted at Sde Boker in the Negev Desert of Israel, from 18 February to 15 March 1997. Nephelometer measurements gave average background scattering coefficient values of about 25 M/m at 550 nm wavelength, but strong dust events caused the value of this parameter to rise up to about 800 M/m Backscattering fractions did not depend on aerosol loading, and generally fell in the range of 0.1 to 0.25, comparable to values reported for marine and Arctic environments. Chemical analysis of the aerosol revealed that, in the coarse size range (2 - 10 micrometer equivalent aerodynamic diameter (EAD)), calcium (Ca) was by far the most abundant element followed by silicon (Si), both of which are indicators for mineral dust. In the fine size fraction (< 2 micrometers EAD), sulfur (S) generally was the dominant element, except during high dust episodes when Ca and Si were again the most abundant. Furthermore, fine black carbon (BC) correlates with S, suggesting that they may have originated from the same sources or source regions. An indication of the short-term effect of aerosol loading on radiative forcing was provided by measurements of global and diffuse solar radiation, which showed that during high turbidity periods (strong dust events) almost all of the solar radiation reaching the area is scattered or absorbed.
Ichoku, C.↗
Heterogeneous Reactions of ClONO2, HCl, and HOCl on Liquid Sulfuric Acid Surfaces
The heterogeneous reactions of ClONO2 + H2O yields HNO3 + HOCl (1), ClONO2 + HCl yields C12 + HNO3 (2), and HOCl + HCl yields Cl2 + H2O (3) on liquid sulfuric acid surfaces have been studied using a fast flow reactor coupled to a quadrupole mass spectrometer. The main objectives of the study are to investigate: (a) the temperature dependence of these reactions at a fixed H2O partial pressure typical of the lower stratosphere (that is, by changing temperature at a constant water partial pressure, the H2SO4 content of the surfaces is also changed), (b) the relative importance or competition between reactions 1 and 2, and (c) the effect of HNO3 on the reaction probabilities due to the formation of a H2SO4/HNO3/H2O ternary system. The measurements show that all the reactions depend markedly on temperature at a fixed H2O partial pressure: they proceed efficiently at temperatures near 200 K and much slower at temperatures near 220 K. The reaction probability (gamma(sub 1)) for ClONO2 hydrolysis approaches 0.01 at temperatures below 200 K, whereas the values for gamma(sub 2) and gamma(sub 3) are on the order of a few tenths at 200 K. Although detailed mechanisms for these reactions are still unknown, the present data indicate that the competition between ClONO2 hydrolysis and ClONO2 reaction with HCl may depend on temperature (or H2SO4 Wt %): in the presence of gaseous HCl at stratospheric concentrations, reaction 2 is dominant at lower temperatures (less than 200 K), but reaction 1 becomes important at temperatures above 210 K. Furthermore, reaction probability measurements performed on the H2SO4/HNO3/ H2O ternary solutions do not exhibit noticeable deviation from those performed on the H2SO4/H2O binary system, suggesting little effect of HNO3 in sulfate aerosols on the ClONO2 and HOCl reactions with HCl. The results reveal that significant reductions in the chlorine-containing reservoir species (such as ClONO2 and HCl) can take place on stratospheric sulfate aerosols at high latitudes in winter and early spring, even at temperatures too warm for Polar Stratospheric Clouds (PSCs) to form or in regions where nucleation of PSCs is sparse. This is particularly true under elevated sulfuric acid loading, such as that after the eruption of Mt. Pinatubo. Comparisons between our results and those presently available have also been made.
Zhang, Renyi↗
Data set for background investigation of atmospheric constituents for Cape Henry site: August 5-22, 1974
The laboratory was located within the Fort Story Military Reservation at Cape Henry between 5 August and 21 August 1974. Total sulfur, total hydrocarbons, NO, NO2, Nox, and O3 were monitored and reported as hourly averages. Visibility was measured using an integrating nephelometer and reported as hourly averages. Twenty-four hour averaged mass loading was determined using two high volume air samplers located on different levels (25' and 50') at the site. Temperature, wind speed, relative humidity, barometric pressure and solar radiation intensity were measured at the site or supplemented by readings taken by the U. S. Coast Guard at the Cape Henry Light House.
Source record↗
Effects on stratospheric ozone from high-speed civil transport: Sensitivity to stratospheric aerosol loading
The potential impact of high-speed civil transport (HSCT) aircraft emissions on stratospheric ozone and the sensitivity of these results to changes in aerosol loading are examined with a two-dimensional model. With aerosols fixed at background levels, calculated ozone changes due to HSCT aircraft emissions range from negligible up to 4-6% depletions in column zone at northern high latitudes. The magnitude of the ozone change depends mainly on the NO(x) increase due to aircraft emissions, which depends on fleet size, cruise altitude, and engine design. The partitioning of the odd nitrogen species in the lower stratosphere among NO, NO2, N2O5, is strongly dependent on the concentration of sulfuric acid aerosol particles, and thus the sensitivity of O3 to NO(x) emissions changes when the stratospheric aerosol loading changes. Aerosol concentrations 4 times greater than background levels have not been unusual in the last 2 decades. Our model results show that a factor of 4 increase in aerosol loading would significantly reduce the calculated ozone depletion due to HSCT emissions. Because of the neutral variabiltiy of stratospheric aerosols, the possible impact of HSCT emissions on ozone must be viewed as a range of possible results.
Weisenstein, Debra K.↗
Intumescent Coatings as Fire Retardants
The development of fire-retardant coatings to protect surfaces which may be exposed to fire or extreme heat is a subject of intense interest to many industries. A fire-retardant paint has been developed which represents a new chemical approach for preparing intumescent coatings, and potentially, is very important to fire-prevention authorities. The requirements for a superior coating include ease of application, suitability to a wide variety of surfaces and finishes, and stability over an extended period of time within a broad range of ambient temperature and humidity conditions. These innovative coatings, when activated by the heat of a fire, react to form a thick, low-density, polymeric coating or char layer. Water vapor and sulphur dioxide are released during the intumescent reaction. Two fire-protection mechanisms thus become available: (1) the char layer retards the flow of heat, due to the extremely low thermal conductivity; and (2) water vapor and sulfur dioxide are released, providing fire quenching properties. Still another mechanism functions in cases where the char, by virtue of its high oxidation resistance and low thermal conductivity, reaches a sufficiently high temperature to re-radiate much of the incident heat load. The coatings consist of dispersions of selective salts of a nitro-amino-arornatic compound. Specifically, para-nitroaniline bisulfate and the ammonium salt of para-nitroaniline-ortho sulphuric acid (2-amino-5-nitrobenzenesulphuric acid) are used. Suitable vehicles are cellulose nitrate of lacquer grade, a nitrite-phenolic modified rubber, or epoxy-polysulfide copolymer. Three separate formulations have been developed. A solvent is usually employed, such as methylethyl ketone, butyl acetate, or toluene, which renders the coatings suitably thin and which evaporates after the coatings are applied. Generally, the intumescent material is treated as insoluble in the vehicle, and is ground and dispersed in the vehicle and solvent like an ordinary coating pigment. The char found on intumescence is better in terms of yield and physical properties than chars obtained from many previously known intumescent materials. Prior to intumescence, the coating has a density of 85 pounds per cubic foot. After intumescence, the density is approximately 0.3 pounds per cubic loot. The linear expansion of the coatings ranges from 70 to 200 times the applied coating thickness.
Parker, J. A.↗
Friction and wear of iron in sulfuric acid
Elemental iron sliding on aluminum oxide in aerated sulfuric acid concentrations ranging from very dilute (0.000007 N; i.e., 4 ppm) to very concentrated (96 percent acid) was studied. Load and reciprocating sliding speeds were kept constant. With the most dilute acid of 0.7 to 0.0002 N, a complex corrosion product formed that was friable and often increased friction and wear. At concentrations of 0.001 N, metal losses were essentially by wear alone. Because no buildup of corrosion products occurred, this acid concentration became the standard from which to separate metal loss from direct corrosion and mechanical wear losses. When the acid concentration was increased to 5 percent, the high corrosion rate of iron in sulfuric acid strongly dominated the total wear loss. This strong corrosion increased to 30 percent acid, and decreased somewhat at 50 percent in accordance with expectations. However, the low corrosion of iron expected at acid concentrations of 65 to 96 percent was not observed in the wear area. It is apparent that the normal passivating film was being worn away and a galvanic cell established which rapidly attached to the wear area.
Rengstorff, G. W. P.↗
Interaction of sulfuric acid corrosion and mechanical wear of iron
Friction and wear experiments were conducted with elemental iron sliding on aluminum oxide in aerated sulfuric acid at concentrations ranging from very dilute (0.00007 N; i.e., 4 ppm) to very concentrated (96 percent acid). Load and reciprocating sliding speed were kept constant. With the most dilute acid concentration of 0.00007 to 0.0002 N, a complex corrosion product formed that was friable and often increased friction and wear. At slightly higher concentrations of 0.001 N, metal losses were essentially by wear alone. Because no buildup of corrosion products occurred, this acid concentration became the standard from which to separate metal loss from direct corrosion and mechanical wear losses. When the acid concentration was increased to 5 percent (1 N), the well-established high corrosion rate of iron in sulfuric acid strongly dominated the total wear loss. This strong corrosion increased to 30 percent acid and decreased somewhat to 50 percent acid in accordance with expectations. However, the low corrosion of iron expected at acid concentrations of 65 to 96 percent was not observed in the wear area. It was apparent that the normal passivating film was being worn away and a galvanic cell established that rapidly attacked the wear area. Under the conditions where direct corrosion losses were highest, the coefficient of friction was the lowest.
Rengstorff, G. W. P.↗
Interaction of sulfuric acid corrosion and mechanical wear of iron
Friction and wear experiment were conducted with elemental iron sliding on aluminum oxide in aerated sulfuric acid at concentrations ranging from very dilute (0.00007 N; i.e., 4 ppm) to very concentrated (96 percent acid). Load and reciprocating sliding speed were kept constant. With the most dilute acid concentration of 0.00007 to 0.0002 N, a complex corrosion product formed that was friable and often increased friction and wear. At slightly higher concentrations of 0.001 N, metal losses were essentially by wear alone. Because no buildup of corrosion products occurred, this acid concentration became the standard from which to separate metal loss from direct corrosion and mechanical wear losses. When the acid concentration was increased to 5 percent (1 N), the well-established high corrosion rate of iron in sulfuric acid strongly dominated the total wear loss. This strong corrosion increased to 30 percent acid and decreased somewhat to 50 percent acid in accordance with expectations. However, the low corrosion of iron expected at acid concentrations of 65 to 96 percent was not observed in the wear area. It was apparent that the normal passivating film was being worn away and a galvanic cell established that rapidly attacked the wear area. Under the conditions where direct corrosion losses were highest, the coefficient of friction was the lowest.
Rengstorff, G. W. P.↗
Conceptual design study of potential early commercial MHD powerplant. Report of task 2 results
The conceptual design of one of the potential early commercial MHD power plants was studied. The plant employs oxygen enrichment of the combustion air and preheating of this oxygen enriched air to an intermediate temperature of 1200 F attainable with a tubular type recuperative heat exchanger. Conceptual designs of plant componets and equipment with performance, operational characteristics, and costs are reported. Plant economics and overall performance including full and part load operation are reviewed. The projected performance and estimated cost of this early MHD plant are compared to conventional power plants, although it does not offer the same high efficiency and low costs as the mature MHD power plant. Environmental aspects and the methods incorporated in plant design for emission control of sulfur and nitrogen are reviewed.
Hals, F. A.↗
Friction and wear of nickel in sulfuric acid
Experiments were conducted with elemental nickel sliding on aluminum oxide in aerated sulfuric acid in concentrations ranging from very dilute (10 -4 N, i.e., 5 ppm) to very concentrated (96 percent) acid. Load and reciprocating sliding speeds were kept constant. With the most dilute concentration (10 -4 N) no observable corrosion occurred in or outside the wear area. This was used as the base condition to determine the high contribution of corrosion to total wear loss at acid concentrations between 0.5 percent (0.1 N) and 75 percent. Corrosion reached a maximum rate of 100 millimeters per year at 30 percent acid. At the same time, general corrosion outside the wear area was very low, in agreement with published information. It is clear that friction and wear greatly accelerated corrosion in the wear area. At dilute concentrations of 0.001 and 0.01 N, corrosion in the wear area was low, and general corrosion outside was also low, but local outside regions in the direction of the wear motion experienced some enhanced corrosion, apparently due to fluid motion of the acid.
Rengstorff, G. W. P.↗
Comparison of Modeled Backscatter using Measured Aerosol Microphysics with Focused CW Lidar Data over Pacific
During NASA's GLObal Backscatter Experiment (GLOBE) II flight mission over the Pacific Ocean in May-June 1990, extensive aerosol backscatter data sets from two continuous wave, focused CO2 Doppler lidars and an aerosol microphysics data set from a laser optical particle counter (LOPC) were obtained. Changes in aerosol loading in various air masses with associated changes in chemical composition, from sulfuric acid and sulfates to dustlike crustal material, significantly affected aerosol backscatter, causing variation of about 3 to 4 orders of magnitude. Some of the significant backscatter features encountered in different air masses were the low backscatter in subtropical air with even lower values in the tropics near the Intertropical Convergence Zone (ITCZ), highly variable backscatter in the ITCZ, mid-tropospheric aerosol backscatter background mode, and high backscatter in an Asian dust plume off the Japanese coast. Differences in aerosol composition and backscatter for northern and southern hemisphere also were observed. Using the LOPC measurements of physical and chemical aerosol properties, we determined the complex refractive index from three different aerosol mixture models to calculate backscatter. These values provided a well-defined envelope of modeled backscatter for various atmospheric conditions, giving good agreement with the lidar data over a horizontal sampling of approximately 18000 km in the mid-troposphere.
Srivastava, Vandana↗