Physisorption of nitrogen on 304 stainless steel at very low pressures
Physisorption isotherms for nitrogen on stainless steel at various temperatures and very low pressures
Troy, M.↗
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Physisorption of Ar, Kr, CH4, and N2 on 304 stainless steel at very low pressures.
Determination of physisorption isotherms of these gases on stainless steel by pressure change measurements in very low pressure cryogenic baths where a steel nipple was brought in contact with the test gas at 77 to 90 K in a sealed constant-volume system. The position of the nipple in the gas was changed in such a manner that gas adsorption on a 47.5 sq cm area of the steel surface could be measured. The Dubinin-Radushkevich (DR) equation (1947) was used for an empirical description of isotherms at different temperatures. The mean adsorption energies calculated from the DR plots were 1290, 1545, 1490 and 1903 cal/mol for Ar, Kr, CH4 and N2, respectively, being about 10% higher than the corresponding values on Pyrex.
Troy, M.↗
Experimental Investigation of a Physisorption-Based Hydrogen Storage System
This study discusses a practical system utilizing the principle of physisorption where hydrogen is weakly bound to the surface of a nanoporous silica aerogel blanket as an alternative to high-pressure and cryogenic hydrogen storage. Three different experiments are conducted to simulate various scenarios of such a storage method: change in pressure and change of scale. Transient responses of the charging and discharging cycles are of particular interest. It is observed that hydrogen uptake can be increased by up to 36-38 % at ambient conditions and 77 K when utilizing the aerogel blankets. Packing density, or the artificial increase of surface per volume, increases storage capacity as it is a mainly surface-driven phenomenon. High-pressure testing up to 50 bar showed benefits of the aerogel addition whereas the maximum uptake improvement was observed for 2 bar with a 105.3 % improvement over an empty vessel at identical conditions corresponding to 6.43 wt%. The scale-up of the system is highly sensitive to the design of the internal cooling design as aerogels are poor thermal conductors reducing the transient response of such systems. Furthermore, the high mass of metal-based pressure vessels further delays the thermal response. This makes the system suitable for day to week-long hydrogen storage but not for peak-shaving or load balancing.
Marcel Otto↗
Physisorption of argon on pyrex at low pressures.
Equilibrium pressures, numbers of argon atoms adsorbed per unit area and the DR parameters are given for argon adsorption on Pyrex for pressures ranging from 0.625 nanotorr to 12.7 microtorr at 77, 81.4, 87.8 and 90 K. Physical adsorption isotherms, Dubinin-Radushkevich plots, and isosteric heat curves are also given for argon on Pyrex.
Jen, J. S.-C.↗
Some interesting aspects of physisorption stay-time measurements obtained using molecular-beam techniques
Stay-time distributions have been obtained for Xe physisorbing on polycrystalline nickel as a function of the target temperature using a pulsed molecular-beam technique. Some interesting effects due to ion bombardment of the surface using He, Ar, and Xe ions are presented. Measured detector signal shapes are found to deviate from those predicted for first-order desorption with velocities corresponding to Maxwellian effusion at the surface temperature. Evidence is found for interaction between beam pulse adsorption and steady-state adsorption of beam species background atoms.
Wilmoth, R. G.↗
Sorption cooler technology development at JPL
Simple heating and cooling of chemisorption and physisorption compressors provide high pressure gas, which, when expanded through a Joule-Thomson (J- T) valve, can provide cooling from 0.3 to 200 K depending on the sorbent/gas combination. System life tests are under way on Pr(1-n)Ce(n)O(x)/O2 (PCO/O2) chemisorption compressors for 65-80 K cooling and on carbon/krypton (C/Kr) physisorption compressors for 120-140 K cooling. Investigations have been initiated to examine reliability physics issues related to critical compressor components such as sorbents, container materials and electrical heaters.
Jones, J. A.↗
Heat cascading regenerative sorption heat pump
A simple heat cascading regenerative sorption heat pump process with rejected or waste heat from a higher temperature chemisorption circuit (HTCC) powering a lower temperature physisorption circuit (LTPC) which provides a 30% total improvement over simple regenerative physisorption compression heat pumps when ammonia is both the chemisorbate and physisorbate, and a total improvement of 50% or more for LTPC having two pressure stages. The HTCC contains ammonia and a chemisorbent therefor contained in a plurality of canisters, a condenser-evaporator-radiator system, and a heater, operatively connected together. The LTPC contains ammonia and a physisorbent therefor contained in a plurality of compressors, a condenser-evaporator-radiator system, operatively connected together. A closed heat transfer circuit (CHTC) is provided which contains a flowing heat transfer liquid (FHTL) in thermal communication with each canister and each compressor for cascading heat from the HTCC to the LTPC. Heat is regenerated within the LTPC by transferring heat from one compressor to another. In one embodiment the regeneration is performed by another CHTC containing another FHTL in thermal communication with each compressor. In another embodiment the HTCC powers a lower temperature ammonia water absorption circuit (LTAWAC) which contains a generator-absorber system containing the absorbent, and a condenser-evaporator-radiator system, operatively connected together. The absorbent is water or an absorbent aqueous solution. A CHTC is provided which contains a FHTL in thermal communication with the generator for cascading heat from the HTCC to the LTAWAC. Heat is regenerated within the LTAWAC by transferring heat from the generator to the absorber. The chemical composition of the chemisorbent is different than the chemical composition of the physisorbent, and the absorbent. The chemical composition of the FHTL is different than the chemisorbent, the physisorbent, the absorbent, and ammonia.
Jones, Jack A.↗
Evaluating the Adsorptive Capabilites of Chemsorb 1000 and Chemsorb 1425
The removal of trace contaminants from spacecraft cabin air is necessary for crew health and comfort during long duration space exploration missions. The air revitalization technologies used in these future exploration missions will evolve from current ISS ISS State-of-Art (SOA) and is being designed and tested by the Advanced Exploration Systems (AES) Program's Atmosphere Resource Recovery and Environmental Monitoring (ARREM) project. The ARREM project is working to mature optimum atmosphere revitalization and environmental monitoring system architectures to enable exploration beyond Lower Earth Orbit (LEO). The Air Revitalization Lab at KSC is one of six NASA field centers participating in the ARREM that specializes in adsorbent and catalyst characterization with simulated spacecraft gas streams using combinations of pressure, O2 partial pressure, CO2 partial pressure, and humidity that are representative of a range of anticipated cabin atmospheric conditions and loads. On board ISS, the Trace Contaminant Control Subassembly (TCCS) provides active control of trace contaminants from the cabin atmosphere utilizing physical adsorption, thermal catalytic oxidation, and chemical adsorption processes. High molecular weight contaminants and ammonia (NH3) are removed a granular activated carbon treated with approx. 10% by weight phosphoric acid (H3PO4) (B-S Type 3032 4×6 mesh), which is expendable and is periodically refurbished. The Type 3032 granular activated carbon bed is no longer commercially available and therefore it is important to characterize the efficiency and capacity of commercially available NH3 sorbents. This paper describes the characterization of two Molecular Products LTD activated carbons: Chemsorb 1000 and Chemsorb 1425. Untreated activated carbons (e.g. Chemsorb 1000) remove contaminants by physisorption, which concentrates the contaminant within the pores of the carbon while letting air to pass through the sorbent4. Low molecular weight or polar gases (e.g. HCl, SO2, formaldehyde, and NH3) are not removed by physisorption and typically require chemisorption for removal. Treated activated carbons (e.g. Chemsorb 1425) are impregnated with a a chemical agent (e.g. phosphoric acid) that reacts with those gases, converting them to solids or salts within the carbon and removes them from the air stream. This process occurs via neutralization or catalysis reactions and adsorption capacity is exhaustedwhen the available impregnated chemicals are consumed. Moisture affects removal performance since adsorption sites within the pores are filled with water. The performance of impregnated carbons may be enhanced by moisture content because the mechanisms of contaminant removal are chemical reactions that occur in reagents contained within the pores. The adsorptive capacity data (mol/kg) of Chemsorb 1000 and 1425 for gas mixtures (ethanol, acetone, toluene, acetaldehyde, dichloromethane, and xylene) was measured with 40% relative humidity at 23 deg C air temperature. The adsorptive capacity data (mol/kg) of Chemsorb 1425 was measured using NH3 gas streams.
adsorptive capacities↗
Laboratory simulation of meteoritic noble gases. I - Sorption of xenon on carbon: Trapping experiments
The sorption of Xe-127 at 5 x 10 to the -7th atm onto carbon black, pyrolyzed polyvinylidene chloride, and pyrolyzed acridine at 100-1000 C for 5 min-240 h is measured experimentally by gamma spectrometry. The results are presented in tables and graphs and characterized in detail. The tightly bound Xe remaining in the samples after 4000 min pumping at temperatures above 100 C is found to comprise two components: a low-temperature component attributed to physisorption within an atomic-scale labyrinth of micropores, and a high-temperature component due to volume diffusion. The implications for the trapping of noble gases near grain surfaces of amorphous carbon in meteorites are considered.
Wacker, J. F.↗
Use of Hydration Inhibitors to Improve Bond Durability of Aluminum Adhesive Joints
An investigation is conducted of the mechanisms by which nitrilotris methylene phosphonic acid (NTMP) and related compounds are adsorbed onto oxidized aluminum surfaces to inhibit hydration and increase the durability of adhesive bonds formed with inhibitor-treated panels. P - O - Al bonds are identified as the basis of adsorption, and it is found that water initially adsorbed onto the etched aluminum surfaces is displaced by the NTMP. The hydration of the NTMP-treated surfaces occurs in three stages, namely the reverisble physisorption of water, the slow dissolution of NTMP followed by rapid hydration of the freshly exposed Al2O3 to AlOOH and further hydration of the surface to Al(OH)3. Five properties of an ideal inhibitor are identified.
Davis, G. D.↗
Reaction of N2O5 with H2O on carbonaceous surfaces
The heterogeneous reaction of N2O5 with commercially available ground charcoal in the absence of H2O revealed a physisorption process (gamma = 0.003), together with a redox reaction generating mostly NO. Slow HNO3 formation was the result of the interaction of N2O5 with H2O that was still adsorbed after prolonged pumping at 0.0001 torr. In the presence of H2O, the same processes with gamma = 0.005 are observed. The redox reaction dominates in the early stages of the reaction, whereas the hydrolysis gains importance later at the expense of the redox reaction. The rate law for HNO3 generation was found to be d(HNO3)/dt = k(bi)(H2O)(N2O5) with k(bi), the effective bimolecular rate constants, for 10 mg of carbon being (1.6 + or - 0.3) x 10 to the -13th cu cm/s.
Brouwer, L.↗
Sorption cryogenic refrigeration - Status and future
The operation principles of sorption cryogenic refrigeration are discussed. Sorption refrigerators have virtually no wear-related moving parts, have negligible vibration, and offer extremely long life (at least ten years), making it possible to obtain efficient, long life and low vibration cooling to as low as 7 K for cryogenic sensors. The physisorption and chemisorption systems recommended for various cooling ranges down to 7 K are described in detail. For long-life cooling at 4-5 K temperatures, a hybrid chemisorption-mechanical refrigeration system is recommended.
Jones, Jack A.↗
Diffusion on Cu surfaces
Understanding surface diffusion is essential in understanding surface phenomena, such as crystal growth, thin film growth, corrosion, physisorption, and chemisorption. Because of its importance, various experimental and theoretical efforts have been directed to understand this phenomena. The Field Ion Microscope (FIM) has been the major experimental tool for studying surface diffusion. FIM have been employed by various research groups to study surface diffusion of adatoms. Because of limitations of the FIM, such studies are only limited to a few surfaces: nickel, platinum, aluminum, iridium, tungsten, and rhodium. From the theoretical standpoint, various atomistic simulations are performed to study surface diffusion. In most of these calculations the Embedded Atom Method (EAM) along with the molecular static (MS) simulation are utilized. The EAM is a semi-empirical approach for modeling the interatomic interactions. The MS simulation is a technique for minimizing the total energy of a system of particles with respect to the positions of its particles. One of the objectives of this work is to develop the EAM functions for Cu and use them in conjunction with the molecular static (MS) simulation to study diffusion of a Cu atom on a perfect as well as stepped Cu(100) surfaces. This will provide a test of the validity of the EAM functions on Cu(100) surface and near the stepped environments. In particular, we construct a terrace-ledge-kink (TLK) model and calculate the migration energies of an atom on a terrace, near a ledge site, near a kink site, and going over a descending step. We have also calculated formation energies of an atom on the bare surface, a vacancy in the surface, a stepped surface, and a stepped-kink surface. Our results are compared with the available experimental and theoretical results.
Karimi, Majid↗
Chemisorption and Diffusion of H on a Graphene Sheet and Single-Wall Carbon Nanotubes
Recent experiments on hydrogen storage in single wall nanotubes and nanotube bundles have reported large fractional weight of stored molecular hydrogen which are not in agreement with theoretical estimates based of simulation of hydrogen storage by physisorption mechanisms. Hydrogen storage in catalytically doped nanotube bundles indicate that atomic H might undergo chemisorption changing the basic nature of the storage mechanism under investigation by many groups. Using a generalized tight-binding molecular dynamics (GTBMD) method for reactive C-H dynamics, we investigate chemisorption and diffusion of atomic H on graphene sheet and C nanotubes. Effective potential energy surfaces (EPS) for chemisorption and diffusion are calculated for graphene sheet and nanotubes of different curvatures. Analysis of the activation barriers and quantum rate constants, computed via wave-packet dynamics method, will be discussed in this presentation.
Srivastava, Deepak↗
Transport Modeling for Metallic Electrode: Semiconducting Nanotube Systems
Recently, current-voltage (I-V) characteristics have been reported by Collins et al. for a system with a scanning tunneling microscope (STM) tip and a carbon nanotube. The STM tip was driven forward into a film of many entangled nanotubes on a substrate, and then was retracted, so that one of nanotubes bridged the STM and the film. I-V characteristics had two different patterns for different heights. One showed large dI/ dV with V greater than 0, small dI/dV with V less than 0, and I = 0 near V = 0 (type-I), while the other showed rectification, i.e., I does not equal 0 only with V less than 0 (type-II), with the tip grounded. We propose a physical mechanism to explain the observed I-V patterns. We consider that the observed characteristics strongly reflected the nature of the tip (metal) - nanotube (semiconductor) contact. The other end of the nanotube was entangled well in the film, and simply provided a good Ohmic contact. We will argue that there are two different contact modes: vacuum gap and touching modes, depending on the presence or absence of a tiny vacuum gap d approx. 0.1 - 0.2 nm at the junction. These modes may be related to physisorption and chemisorption, respectively. Once admitting their existence, it is naturally shown that I-V characteristics are type-I in the vacuum gap mode, and type-II in the touching mode. We argue that the nanotube had to be an n-type semiconductor judging from the I-V characteristics, contrary to often observed p-type in the transistor applications, where p-type is probably due to the oxidation in air or the trapped charges in the silicon dioxide. Additional information is contained in the original extended abstract.
Yamada, Toshishige↗
Interstellar Grain Surface Chemistry
Chemistry on grain surfaces plays an Important role in the formation of interstellar Ices, It can also influence the composition of the gas phase through outgassing near luminous, newly formed stars. This paper reviews the chemical processes taking place on Interstellar grain surfaces with the emphasis on those transforming CO into other hydrocarbons. At low, molecular cloud temperatures (approximately equal to 10K), physisorption processes dominate interstellar grain surface chemistry and GO is largely hydrogenated through reactions with atomic H and oxidized through reactions with atomic O. The former will lead to the formation of H2CO and CH3OH ices, while the latter results in CO2 ice. The observational evidence for these ices in molecular clouds will be discussed. Very close to protostars, the gas and grain temperatures are much higher (approximately equal to 500K) and chemisorption processes, including catalytic surface reactions, becomes important. This will be illustrated based upon our studies of the Fischer-Tropsch Synthesis of CH4 from CO on metallic surfaces. Likely, this process has played an important role in the early solar nebula. Observational consequences will be pointed out.
Tielens, Alexander G. G. M.↗
Development of Metal-impregnated Single Walled Carbon Nanotubes for Toxic Gas Contaminant Control in Advanced Life Support Systems
The success of physico-chemical waste processing and resource recovery technologies for life support application depends partly on the ability of gas clean-up systems to efficiently remove trace contaminants generated during the process with minimal use of expendables. Carbon nanotubes promise superior performance over conventional approaches to gas clean-up due to their ability to direct the selective uptake of gaseous species based on their controlled pore size, high surface area, ordered chemical structure that allows functionalization and their effectiveness also as catalyst support materials for toxic gas conversion. We present results and findings from a preliminary study on the effectiveness of metal impregnated single walled nanotubes as catalyst/catalyst support materials for toxic gas contaminate control. The study included the purification of single walled nanotubes, the catalyst impregnation of the purified nanotubes, the experimental characterization of the surface properties of purified single walled nanotubes and the characterization of physisorption and chemisorption of uptake molecules.
Pisharody, Suresh A.↗
Electronic Transport through Self Assembled Thiol Molecules: Effect of Monolayer Order, Dynamics and Temperature
We present the charge transport and tunneling conductance of self assembled organic thiol molecules and discuss the influence of order and dynamics in the monolayer on the transport behavior and the effect of temperature. Conjugated thiol molecular wires and organometals such as terpyridine metal complexes provide a new platform for molecular electronic devices and we study their self assembly on Au(111) substrates by the scanning tunneling microscope. Determining the organization of the molecule and the ability to control the nature of its interface with the substrate is important for reliable performance of the molecular electronic devices. By concurrent scanning tunneling microscopy and spectroscopy studies on SAMs formed from oligo (phenelyne ethynelyne) monolayers with and without molecular order, we show that packing and order determine the response of a self assembled monolayer (SAM) to competing interactions. Molecular resolution STM imaging in vacuum shows that the OPES adopt an imcommensurate SAM structure on Au(111) with a rectangular unit cell. Tunneling spectroscopic measurements were performed on the SAM as a function of junction resistance. STS results show that the I-Vs are non linear and asymmetric due to the inherent asymmetry in the molecular structure, with larger currents at negative sample biases. The asymmetry increases with increasing junction resistance due to the asymmetry in the coupling to the leads. This is brought out clearly in the differential conductance, which also shows a gap at the Fermi level. We also studied the effect of order and dynamics in the monolayer on the charge transport and found that competing forces between the electric field, intermolecular interactions, tip-molecule physisorption and substrate-molecule chemisorption impact the transport measurements and its reliability and that the presence of molecular order is very important for reproducible transport measurements. Thus while developing new electronic platforms based on molecules, it is important to have a good control of the molecule-substrate interface, for the devices to perform reliably. While such a control would minimize fluctuations and dynamics in the ensemble, the real challenge is to develop device architectures that are tolerant to fluctuations, since they cannot be totally eliminated in these low dimensional soft systems. Results of temperature dependent STS measurements will also be discussed.
Dholakia, Geetha↗