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Interfacial water shuffling the intermediates of hydrogen oxidation and evolution reactions in aqueous media
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Composition-dependent hydrogen oxidation activity of Pt–Cu nanoparticles prepared using boron-rich nanosheets
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Electrocatalyst advances for hydrogen oxidation in phosphoric acid fuel cells
The important considerations that presently exist for achieving commercial acceptance of fuel cells are centered on cost (which translates to efficiency) and lifetime. This paper addresses the questions of electrocatalyst utilization within porous electrode structures and the preparation of low-cost noble metal electrocatalyst combinations with extreme dispersions of the metal. Now that electrocatalyst particles can be prepared with dimensions of 10 A, either singly or in alloy combinations, a very large percentage of the noble metal atoms in a crystallite are available for reaction. The cost savings for such electrocatalysts in the present commercially driven environment are considerable.
Hydrogen oxidation mechanism with applications to (1) the chaperon efficiency of carbon dioxide and (2) vitiated air testing
Ignition delay times for the hydrogen/oxygen/carbon dioxide/argon system were obtained behind reflected shock waves. A detailed kinetic mechanism modeled the experimental hydrogen/oxygen data, Skinner and Ringrose's high-pressure data, and Slack and Grillo's hydrogen/air data. A carbon dioxide chaperon efficiency of 7.0 +/- 0.2 was determined. The reaction pathway H2O yields H2O2 yields OH yields H was required to model the high-pressure data. It is suggested that some of the lowest temperature data points (1.0 and 0.5 atm) for Slack and Grillo's hydrogen/air experiments are in error. It was found that the technique of simplifying a detailed kinetic mechanism for a limited range of experimental data may render the model useless for other test conditions.
HO(x) Measurements in SONEX with the Airborne Tropospheric Hydrogen Oxides Sensor (ATHOS)
SONEX, which was delayed by aircraft inspection problems, began the second week of October and concluded in mid-November with 16 flights. These flights covered the Pacific Ocean off the western United States, transits across the United States, the western coast of Europe, and the North and Central Atlantic Ocean. Particular attention was paid to the North Atlantic Flight Corridor. ATHOS collected high-quality HO(x) data on 15 flights. Observations taken at 5 Hz were typically averaged into 20-second measurements. Each 20-second measurement has precision 1(sigma) of less than 0.01 pptv. OH measurements were generally made from the surface to flight altitudes. HO2 measurements, which require reagent NO flow, were made from flight altitudes to near the top of the planetary boundary layer. Measured OH and HO2 during SONEX was generally lower than the measured OH and HO2 during SUCCESS (April-May, 1996, central United States). Whereas during SUCCESS midday OH was 0.1-0.5 pptv and HO2 was 3-15 pptv, during SONEX midday OH was 0.02-0.2 pptv and HO2 was 0.5-8 pptv. Part of this difference results from the midday solar zenith angles, which were larger during SONEX than during SUCCESS due to both the season and the generally higher latitudes sampled during SONEX. However, some of the difference may be due to differences in HOx sources, since less air influenced by convection was sampled during SONEX. These possibilities await post-flight calibrations of ATHOS and analysis of observations of HO(x) and simultaneously measured meteorology and trace species.
HO(x) Measurements in PEM Tropics B with the Airborne Tropospheric Hydrogen Oxides Sensor (ATHOS)
The primary objective of PEM Tropics B was to study the processes responsible for the production and loss of tropospheric ozone over the tropical Pacific. This region of the globe contains very clean air as well as aged, polluted air that was advected from both the Asian and American continents. Understanding ozone requires understanding of HO(x) (HO(x) = OH + HO2) chemistry, since the reaction between H02 and NO leads to ozone production and the production of OH often requires ozone loss. In addition, OH is the atmosphere's primary oxidant. Since most atmospheric oxidation is thought to occur in the tropical lower troposphere, measurements during PEM Tropics B should provide an important test of the OH abundances and distributions. Thus, understanding and thoroughly testing HO(x) processes was an important objective of PEM Tropics B. Several issues need to be tested, One is HO, production rates and sources, since HO,, production directly affects ozone production and loss. Another is HO(x) behavior in and around clouds, since HO(x) is lost to cloud particles, but convection may bring HO(x) precursors from near the surface to the upper troposphere. A third is the rise and fall of HO(x) at sunrise and sunset, since these variations give strong indications of the important sources and sinks of HO(x). Making and interpreting high-quality OH and H02 measurements from the NASA DC-8 during PEM Tropics B is the objective of this research effort.
Density Functional Theory Modeling on the Positive Effect of H2O in Hydrogen Oxidation Reaction on Perovskite Oxide Anodes for Solid-Oxide Fuel Cells
Presented by LRST at the MS&T2020, 11/4
Minor constituents in the stratosphere and mesosphere
A review of the research in minor constituents in the stratosphere and mesosphere, carried out between 1975 and 1978, is presented. Much of the theoretical research was done with the aid of one-dimensional models. Different aspects of these models are discussed. Measurements of the chlorofluoromethanes, hydrochloric acid, nitric oxide, nitrous oxide, and hydrogen oxide were conducted. It is noted that the hydrogen oxides are now assuming a larger role in stratospheric photochemistry than have been postulated before. The effect of water vapor and the hydrogen oxides on the overall chemistry of the stratosphere was investigated theoretically, along with the possible relationship between solar activity and atmospheric ozone. The mesosphere study included ozone, water vapor, nitric oxide, and odd nitrogen investigations.
Preparation and evaluation of advanced electrocatalysts for phosphoric acid fuel cells
Results are presented for hydrogen oxidation and hydrogen oxidation poisoned by carbon monoxide at levels between 0 and 30%. Due to the high activities that are now being observed for our platinum based electrocatalysts, the hydrogen concentrations were reduced to 10% levels in the gas supplies. Perturbation techniques were used to determine that a mechanism for the efficient operation of our porous gas diffusion electrodes is diffusion of the carbon monoxide out of the electrode structure through the electrolyte film on the electro-catalyst. A survey of the literature on platinum group materials (PGM) was carried out so that an identification of successful electrocatalysts could be made. Two PGM electrocatalysts were prepared and performance data for hydrogen oxidation in hot phosphoric acid in the presence of high carbon monoxide concentrations showed that they matched the best platinum on carbon electrocatalysts but with an electrocatalyst cost that was half of the platinum catalyst cost.
Enhanced Oxide Reduction by Hydrogen at Cuprous Oxide–Copper Interfaces near Ascending Step Edges
We report that understanding the dynamic processes involved in the interaction of hydrogen with oxides is of fundamental importance in catalysis. This paper probes the reduction of Cu 2 O-‘29’ surfaces by hydrogen at room temperature combining in situ ambient pressure scanning tunneling microscopy (STM), X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations. Reduction of the atomic layer thin Cu 2 O film is observed to be preferentially initiated2 at step edges and terrace defects, where perfect Cu 2 O(111) terraces are found to be stable towards hydrogenation under the same conditions. After a long induction period, regions of partially reduced Cu 2 O-‘29’ and metallic Cu co-exist before the surface is fully reduced to Cu(111). The reduction rate strongly depends on the nature of nearby Cu step edges. We propose a mechanism for the reduction of Cu 2 O-‘29’ by hydrogen where free copper atoms from ascending metallic step edges facilitate the formation of active ensembles for H 2 dissociation and transfer H to the edges of Cu2O regions
Cryopumping of hydrogen in vacuum chambers is aided by catalytic oxidation of hydrogen
Vacuum test facilities are required for high speed cryopumping of gaseous hydrogen at low pressures. One method involves the catalytic oxidation of hydrogen and condensation of the resulting water on a liquid nitrogen-cooled surface.
Hydrogen absorption in solid aluminum during high-temperature steam oxidation
Hydrogen is emitted by aluminum heated in a vacuum after high-temperature steam treatment. Wire samples are tested for this effect, showing dependence on surface area. Two different mechanisms of absorption are inferred, and reactions deduced.
Kinetics of the reaction of nitric oxide with hydrogen
The reaction of nitric oxide with hydrogen has been studied in the temperature range 2400-4500 K using a shock-tube technique. Mixtures of NO and H2 diluted in argon or krypton were heated by incident shock waves, and the infrared emission from the fundamental vibration-rotation band of NO at 5.3 microns was used to monitor the time-varying NO concentration. The decomposition of nitric oxide behind the shock was found to be modeled well by a fifteen-reaction system. A principal result of the study was the determination of the rate constant k1 for the reaction H + NO yields N + OH, which may be the rate-limiting step for NO removal in some combustion systems. Experimental values of k1 were obtained for each test through comparisons of measured and numerically predicted NO profiles. The data are fit closely by the expression k1 = 1.34 times 10 to the fourteenth power exp(-49 200/RT) cu cm/mole-sec. These data appear to be the first available for this rate constant.
Experimental Detonation Velocities and Induction Distances in Hydrogen- Nitrous Oxide Mixtures
Experimental detonation velocities and induction distances in hydrogen-nitrous oxide mixtures
Cu-induced robust Ni 2+ /Ni 3+ transition on amorphous Ni hydroxide-based electrocatalysts for advancing electrochemical ammonia oxidation and hydrogen evolution
The electrochemical ammonia oxidation reaction (AOR) is a promising anodic reaction for hydrogen production, offering a lower theoretical potential compared to oxygen evolution reaction. Despite this thermodynamic advantage, AOR suffers from sluggish multi-electron transfer reaction kinetics and the regeneration of catalytically active Ni 3+ species, which limits both activity and durability. In this study, amorphous NiCu bimetallic catalysts were prepared via facile precipitating metal nitrate deposition (PMND) method. The addition of Cu induces a robust Ni 2+ /Ni 3+ transition, stabilizing catalytically active Ni 3+ species and modulating the electronic structure of Ni. It alters the oxidation and desorption behavior of nitrogen-containing intermediates and facilitating their conversions to NO x species, resulting in fast active site regeneration. Furthermore, amorphous structure provides abundant dangling bonds, which enhances the intrinsic reactivity and accessibility of active sites rather than increasing the number of active sites. As a result, these effects accelerate the overall reaction kinetics. The optimized NiCu 5:1 catalyst achieved an ammonia removal efficiency of ∼100 % and a hydrogen production rate of 2.45 mmol/(h∙cm 2 ) at 1.6 V RHE .