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We have investigated a diamond crystal that consists of several misorientated subgrains. The main feature of the crystal is the dark areas in the cathodoluminescent core that has ‘estuary-like’ boundaries extending along the subgrain interfaces. The core has >3100 ppm of nitrogen, and the share of the B form is >95%; the absorbance of the centre N3VH at 3107 cm–1 reaches 75 cm–1. The N3 centre absorbance, as well as N3 luminescence, is absent in the core. In the outer part of the crystal, bright blue luminescence of the N3 centre is apparent, and the N3 absorbance reaches 5.3 cm–1. These observations could be explained by the conversion of N3 centres to N3VH after attaching a hydrogen atom. After the full conversion of the N3 centres, the diamond becomes darker under CL. We hypothesise the dark core has a specific shape due to the post-growth diffusion of the hydrogen.
Analysis and understanding of the role of hydrogen in metals is a significant challenge for the future of materials science, and this is a clear objective of recent work in the atom probe tomography (APT) community. Isotopic marking by deuteration has often been proposed as the preferred route to enable quantification of hydrogen by APT. Zircaloy-4 was charged electrochemically with hydrogen and deuterium under the same conditions to form large hydrides and deuterides. Our results from a Zr hydride and a Zr deuteride highlight the challenges associated with accurate quantification of hydrogen and deuterium, in particular associated with the overlap of peaks at a low mass-to-charge ratio and of hydrogen/deuterium containing molecular ions. We discuss possible ways to ensure that appropriate information is extracted from APT analysis of hydrogen in zirconium alloy systems that are important for nuclear power applications.
In this work, we demonstrate a new system for the examination of gas interactions with surfaces via atom probe tomography. This system provides capability of examining the surface and subsurface interactions of gases with a wide range of specimens, as well as a selection of input gas types. This system has been primarily developed to aid the investigation of hydrogen interactions with metallurgical samples, to better understand the phenomenon of hydrogen embrittlement. In its current form, it is able to operate at pressures from 10−6 to 1000 mbar (abs), can use a variety of gasses, and is equipped with heating and cryogenic quenching capabilities. We use this system to examine the interaction of hydrogen with Pd, as well as the interaction of water vapor and oxygen in Mg samples.
Consumption of marine protein in humans and animals can result in an apparent older radiocarbon (14C) age due to reservoir offsets. In order to correct for this, an estimate of the marine protein intake should be used to correct the 14C age for reservoir offsets, which is ordinarily done using δ13C or δ15N values. However, these two isotopic proxies can be influenced by a number of factors which can hamper estimation of the correct marine protein intake. A small dataset of 12 samples from the Limfjord, Denmark, ranging in age from Mesolithic to Viking Age, was used to test the use of δ2H values to quantify marine protein intake and determine the reservoir corrections. Each of the three stable isotopic values (δ2H, δ13C, δ15N) was used to estimate the percent marine protein intake, which produced three different calibrated 14C ages. The calculated percent marine protein intake differed between the use of the stable isotopic ratios with a maximum difference of 42.1% between the use of δ15N and δ13C, 23.8% between δ2H and δ13C, and 46.2% between δ2H and δ15N. In some cases the calculated percent marine protein intake changed the sample’s archaeological period, although there was generally still overlap in the archaeological periods for samples used in this study.
Kaolinite can be used for many applications, including the underground storage of gases. Density functional theory was employed to investigate the adsorption of hydrogen molecules on the kaolinite (001) surface. The coverage dependence of the adsorption sites and energetics was studied systematically for a wide range of coverage, Θ (from 1/16 to 1 monolayer). The three-fold hollow site is the most stable, followed by the bridge, top-z and top sites. The adsorption energy of H2 decreased with increasing coverage, thus indicating the lower stability of surface adsorption due to the repulsion of neighbouring H2 molecules. The coverage has obvious effects on hydrogen adsorption. Other properties of the H2/kaolinite (001) system, including the lattice relaxation and changes of electronic density of states, were also studied and are discussed in detail.
We review the formation of infrared solar spectral lines from highly excited levels in neutral atoms. The lines of Mg I and H I are the most interesting ones. We explain the NLTE processes by which they are affected and we study the sensitivity of the Mg I 12 μm lines to granulation and to flux tubes.
We compare infrared hydrogen lines observed with ATMOS with computations for two models of the solar atmosphere, one without and one with a chromosphere. The weaker H I lines are formed in the photosphere. Proper evaluation of Stark broadening is required to reproduce their profiles; the heavy ion contribution is most important. The cores of the stronger lines are sensitive to the structure of the chromosphere, but detailed NLTE modeling is needed for diagnostic applications.
The adsorption of C2H4 and H2 gases by bentonite from the Ünye region, Turkey both as raw (B) and as K+-, Li+-, Ag+- and Mg2+ -exchanged forms, was investigated using automated volumetric equipment and pressures up to 100 kPa at 273 K and 77 K, respectively. X-ray powder diffraction (XRD) and specific surface area measurement (BET) methods were employed to characterize the bentonite samples. The C2H4 and H2 gas adsorption capacities of the original and modified forms were in the ranges 1.817–0.201 mmol g−1 and 0.522–0.388 mmol g−1, respectively. The influence of salt modifications on the gas adsorption properties of bentonite is discussed.
In this work, we report on the atom probe tomography analysis of two metallic hydrides formed by pressurized charging using an ex situ hydrogen charging cell, in the pressure range of 200–500 kPa (2–5 bar). Specifically we report on the deuterium charging of Pd/Rh and V systems. Using this ex situ system, we demonstrate the successful loading and subsequent atom probe analysis of deuterium within a Pd/Rh alloy, and demonstrate that deuterium is likely present within the oxide–metal interface of a native oxide formed on vanadium. Through these experiments, we demonstrate the feasibility of ex situ hydrogen analysis for hydrides via atom probe tomography, and thus a practical route to three-dimensional imaging of hydrogen in hydrides at the atomic scale.
Data based on end-member formulae of 4872 minerals (4975 entries) were subjected to numerical treatment and plotting. Most conspicuous among the findings is the hydration trend that spans the whole mineralogical system– something that may be related to the geological history of
mineral formation on Earth. Interesting negative relationships were confirmed for pairs O and F, O and Cl, and Al and Si, while the O vs. S graph documents the dual nature of the behaviour of sulfur. Determinations of Al and Si have the potential of alarming the analyst that his phase
might contain hydrogen. The dataset available also permitted the plotting of histograms that illustrate the preferred concentration distribution of individual elements throughout the mineral kingdom.
Oatmeal porridge has been consumed for centuries and has several health benefits. We aimed to investigate the effect of oatmeal porridge on gut microflora functions. A total of ten healthy subjects ingested 60 g oatmeal porridge daily for 1 week. The following microflora-associated characteristics were assessed before and after the intervention: intestinal gas production following lactulose ingestion, faecal excretion of SCFA and faecal levels of urease and β-galactosidase. In addition, rectal levels of PGE2 were measured. Microbial fermentation as evaluated by intestinal gas production and excretion of SCFA did not change significantly following the dietary intervention. However, faecal levels of β-galactosidase and urease decreased after eating oatmeal porridge (P=0·049 and 0·031, respectively). Host inflammatory state, as measured by rectal levels of PGE2, also decreased, but the change was not significant (P=0·168). The results suggest that oatmeal porridge has an effect on gut microbial functions and may possess potential prebiotic properties that deserve to be investigated further.
High elevation plant and animal communities are considered extremely sensitive to environmental change. We investigated an exceptional fossil record of yellow-bellied marmot (Marmota flaviventris) specimens that was recovered from Cement Creek Cave (elev. 2860 m) and ranged in age from radiocarbon background circa 49.8 cal ka BP to ~ 1 cal ka BP. We coupled isotopic and radiocarbon measurements (δ18O, δD, δ15N, δ13C, and 14C) of bone collagen from individually-AMS dated specimens of marmots to assess ecological responses by this species to environmental change over time in a high elevation basin in the Rocky Mountains of southwestern Colorado, USA. We find little change in all four isotope ratios over time, demonstrating considerable environmental stability during periods when the marmots were present. The stable ecology and the apparent persistence of the small mammal community in the cave fauna throughout the late Quaternary are in marked contrast to the changes that occurred in the large mammal community, including local extirpation and extinction, at the end of the Pleistocene.
Isotopic labeling experiments have revealed correlations between hydrogen reactions, Ga desorption, and ammonia decomposition in GaN CVD. Low energy electron diffraction (LEED) and temperature programmed desorption (TPD) were used to demonstrate that hydrogen atoms are available on the surface for reaction after exposing GaN(0001) to deuterium at elevated temperatures. Hydrogen reactions also lowered the temperature for Ga desorption significantly. Ammonia did not decompose on the surface before hydrogen exposure. However, after hydrogen reactions altered the surface, N15H3 did undergo both reversible and irreversible decomposition. This also resulted in the desorption of N2 of mixed isotopes below the onset of GaN sublimation. This suggests that the driving force of the high nitrogen-nitrogen bond strength (226 kcal/mol) can lead to the removal of nitrogen from the substrate when the surface is nitrogen rich. Overall, these findings indicate that hydrogen can influence GaN CVD significantly, being a common factor in the reactivity of the surface, the desorption of Ga, and the decomposition of ammonia.
The aims of the present study were to quantify hydrogen (H2) and methane (CH4) emissions from beef cattle under different dietary conditions and to assess how cattle genotype and rumen microbial community affected these emissions. A total of thirty-six Aberdeen Angus-sired (AAx) and thirty-six Limousin-sired (LIMx) steers were fed two diets with forage:concentrate ratios (DM basis) of either 8:92 (concentrate) or 52:48 (mixed). Each diet was fed to eighteen animals of each genotype. Methane (CH4) and H2 emissions were measured individually in indirect respiration chambers. H2 emissions (mmol/min) varied greatly throughout the day, being highest after feed consumption, and averaged about 0·10 mol H2/mol CH4. Higher H2 emissions (mol/kg DM intake) were recorded in steers fed the mixed diet. Higher CH4 emissions (mol/d and mol/kg DM intake) were recorded in steers fed the mixed diet (P< 0·001); the AAx steers produced more CH4 on a daily basis (mol/d, P< 0·05) but not on a DM intake basis (mol/kg DM intake). Archaea (P= 0·002) and protozoa (P< 0·001) were found to be more abundant and total bacteria (P< 0·001) less abundant (P< 0·001) on feeding the mixed diet. The relative abundance of Clostridium cluster IV was found to be greater (P< 0·001) and that of cluster XIVa (P= 0·025) lower on feeding the mixed diet. The relative abundance of Bacteroides plus Prevotella was greater (P= 0·018) and that of Clostridium cluster IV lower (P= 0·031) in the LIMx steers. There were no significant relationships between H2 emissions and microbial abundance. In conclusion, the rate of H2 production immediately after feeding may lead to transient overloading of methanogenic archaea capacity to use H2, resulting in peaks in H2 emissions from beef cattle.
In this work, direct potential measurements during cold rolling of zinc and X20Cr13
stainless steel were carried out in the rolling slit to follow the tribologic and galvanic
mechanisms of hydrogen formation and absorption on the surface of the working rolls made
of DHQ1 grade steel. An Ag/AgCl in 3.5 M KCl reference microelectrode was used to record
the open circuit potential of the electrochemical system roller-product immersed into
commercially relevant electrolyte (rolling emulsion) with a pH value of 4.5 and an
electric conductivity 46 mS cm-1. The potential shift into either negative or positive
direction of the rolls-product system gives information on the processes taking place at
the surface in the course of the friction. A detailed discussion of the in-situ
potentiometry experiments reveals a stationary situation established between the
destruction and repassivation of the surface structures during continuous cold rolling
accompanied with intensive hydrogen evolution. Galvanic coupling of the working rolls with
the product significantly intensifies the hydrogen embrittlement related problems of the
rolls. Atomic hydrogen is adsorbed on the surface and exhibits a pressure supported
absorption into the rolls during their whole lifetime.
The effects of the anti-methanogenic compound, bromochloromethane (BCM), on rumen microbial fermentation and ecology were examined in vivo. Japanese goats were fed a diet of 50 % Timothy grass and 50 % concentrate and then sequentially adapted to low, mid and high doses of BCM. The goats were placed into the respiration chambers for analysis of rumen microbial function and methane and H2 production. The levels of methane production were reduced by 5, 71 and 91 %, and H2 production was estimated at 545, 2941 and 3496 mmol/head per d, in response to low, mid and high doses of BCM, respectively, with no effect on maintenance feed intake and digestibility. Real-time PCR quantification of microbial groups showed a significant decrease relative to controls in abundance of methanogens and rumen fungi, whereas there were increases in Prevotella spp. and Fibrobacter succinogenes, a decrease in Ruminococcus albus and R. flavefaciens was unchanged. The numbers of protozoa were also unaffected. Denaturing gradient gel electrophoresis and quantitative PCR analysis revealed that several Prevotella spp. were the bacteria that increased most in response to BCM treatment. It is concluded that the methane-inhibited rumen adapts to high hydrogen levels by shifting fermentation to propionate via Prevotella spp., but the majority of metabolic hydrogen is expelled as H2 gas.
We investigated whether the feeding of high H2-generating dietary fibre and resistant starch (RS) could suppress hepatic ischaemia–reperfusion (IR) injury, which results from oxidative stress, in rats fed a pectin (Pec) or high-amylose maize starch (HAS) diet. Male Sprague–Dawley rats were fed a control (C) diet, with or without Pec (0–5 % Pec) or HAS (0–30 % HAS) supplementation for 7 d. Portal H2 concentration showed a significant dose-dependent increase with the amount of Pec or HAS supplementation. Plasma alanine and aspartate aminotransferase activities remarkably increased in the C rats (5 % cellulose) due to IR treatment, while it decreased significantly or showed tendencies to decrease in 5 % Pec and 20 % HAS diet-fed rats. The hepatic oxidised glutathione (GSSG):total glutathione ratio increased significantly in IR rats maintained on the C diet compared with sham-operated rats. On the other hand, reduced glutathione (GSH):total glutathione and GSH:GSSG ratios decreased significantly. The GSSG:total glutathione ratio that increased due to IR treatment decreased significantly on HAS and Pec intake, while GSH:total glutathione and GSH:GSSG ratios increased significantly. Hepatic sinusoids of IR rats fed the C diet were occluded, but those of IR rats fed the Pec diet were similar to those in the sham-operated rats. In conclusion, we found that Pec or HAS, which enhance H2 generation in the large intestine, alleviated hepatic IR injury. The present study demonstrates another physiological significance of dietary fibre and RS.
A Ni/MgO-La2O3-Al2O3 catalyst with Ni as active component, Al2O3 as support, MgO and La2O3 as additives was prepared and its catalytic activity was evaluated in the process of hydrogen production from catalytic steam reforming of bio-oil. In the catalytic evaluation, some typical components present in bio-oil such as acetic acid, butanol, furfural, cyclopentanone and m-cresol were mixed following a certain proportion as model compounds. Reaction parameters like temperature, steam to carbon molar ratio and liquid hourly space velocity were studied with hydrogen yield as index. The optimal reaction conditions were obtained as follows: temperature 750-850 °C, steam to carbon molar ratio 5-9, liquid hourly space velocity 1.5-2.5 h-1. The maximum hydrogen yield was 88.14%. The carbon deposits were formed on the catalyst surface but its content decreased as reaction temperature increased in the bio-oil steam reforming process.
The structure of prehnite Ca2Al(AlSi3O10)(OH)2, including H positions, has been determined by a combination of single-crystal X-ray diffraction and neutron powder diffraction on four natural samples. The symmetry of the average structure with Al/Si disordered at the T2 siteis Pncm. However, for four of the crystals studied, numerous violations of the n- and c-glide reflection conditions indicate lower symmetry corresponding to space groups P2cm and P2/n and Al-Si ordered structures, possibly as domains of different symmetries and ordering within a single crystal. Time-of-flight neutron powder diffraction was carried out on a sample from Mali at 293 K and 2 K. The structure was refined in space group Pncm by Rietveld analysis. Although it was not possible to locate the missing H using the 293 K neutron data, these data were used to refine the H position located approximately by single-crystal XRD and to refine Uiso. For the 2 K neutron powder diffraction data, H was located directly by difference-Fourier synthesis and its refined position found to be in close agreement with that obtained by the combined XRD/neutron 293 K dataset.
X-ray powder diffraction data for ErH2−xDx formed by hydrogen (i.e., protium)–deuterium loading of Er metal are reported. Lattice parameters for the varying hydrogen–deuterium compositions followed Vergard’s law behavior. The cubic lattice parameter at room temperature for ErH2−xDx obeys a linear relationship according to the formula a=5.1287−1.1120×10−4⋅x, where a is the lattice parameter of the fluorite-type structure and x is the mole percent of deuterium. Microstrain measurements suggest a possible ordering of hydrogen and deuterium in the composition ErH1D1.