Project description:The dataset presented in this article is related to the uncertainty quantification of fuel variability effect on high hydrogen content syngas combustion physicochemical properties. The 1D flame data included in this dataset are collected using PREMIX module available in Chemkin-Pro. Inputs to and outputs collected from the PREMIX module are generated and post-processed using UQTk-3.0.4, an open-access uncertainty quantification (UQ) toolkit developed at Sandia National Laboratories. The 1D flame data here refers to the calculation of flame speed, flame temperature, NO emission, etc. using three detailed chemical mechanisms: the GRI-Mech 3.0, the San Diego, and the NUI Galway Mechanism. The main analysis performed using UQTk-3.0.4 focuses on obtaining main and joint sensitivity effects (Sobol Indices) of uniformly distributed fuel uncertainty on 1D premixed physicochemical property. Other parameters such as the resulted probability density function or fluctuation of these properties are also explored. This new and original dataset is suitable for further analyzing fuel variability effect on other significant flame controlling parameters such as Karlovitz number, flame thickness, etc. in the discipline of turbulent combustion simulation.
Project description:Carbon capture and utilization has gained attention to potentially curb CO2 emissions while generating valuable chemicals. These technologies will coexist with fossil analogs, creating synergies to leverage circular economy principles. In this context, flue gas valorization from power plants can assist in the transition. Here, we assessed the absolute sustainability of a simulated integrated facility producing ammonia and synthetic natural gas from flue gas from a combined-cycle natural gas power plant based in Germany, using hydrogen from three water electrolysis technologies (proton exchange membrane, alkaline, and solid oxide cells), nitrogen, and CO2. For the first time, we applied the planetary boundaries (PBs) framework to a circular integrated system, evaluating its performance relative to the safe operating space. The PB-LCA assessment showed that the alternative technologies could significantly reduce, among others, the impact on climate change and biosphere integrity when compared to their fossil counterparts, which could be deemed unsustainable in climate change. Nevertheless, these alternative technologies could also lead to burden shifting and are not yet economically viable. Overall, the investigated process could smoothen the transition toward low-carbon technologies, but its potential collateral damages should be carefully considered. Furthermore, the application of the PBs provides an appealing framework to quantify the absolute sustainability level of integrated circular systems.
Project description:Nutrient and energy recovery is becoming more important for a sustainable future. Recently, we developed a hydrogen gas recycling electrochemical system (HRES) which combines a cation exchange membrane (CEM) and a gas-permeable hydrophobic membrane for ammonia recovery. This allowed for energy-efficient ammonia recovery, since hydrogen gas produced at the cathode was oxidized at the anode. Here, we successfully up-scaled and optimized this HRES for ammonia recovery. The electrode surface area was increased to 0.04 m2 to treat up to 11.5 L/day (∼46 gN/day) of synthetic urine. The system was operated stably for 108 days at current densities of 20, 50, and 100 A/m2. Compared to our previous prototype, this new cell design reduced the anode overpotential and ionic losses, while the use of an additional membrane reduced the ion transport losses. Overall, this reduced the required energy input from 56.3 kJ/gN (15.6 kW h/kgN) at 50 A/m2 (prototype) to 23.4 kJ/gN (6.5 kW h/kgN) at 100 A/m2 (this work). At 100 A/m2, an average recovery of 58% and a TAN (total ammonia nitrogen) removal rate of 598 gN/(m2 day) were obtained across the CEM. The TAN recovery was limited by TAN transport from the feed to concentrate compartment.
Project description:Hydrogen is a clean energy source, and blending it with natural gas in existing pipeline networks is a key transition solution for transportation cost reduction. However, during the transportation process, a non-uniform distribution of hydrogen concentration occurs in the pipeline due to gravity. Therefore, it is necessary to study the hydrogen concentration distribution law of hydrogen-blended natural gas in pipelines. The undulation and ball valve pipelines, which are common in transport pipelines, were constructed in this study. The effects of the undulation angle, height, pipeline diameter, ball valve opening, and temperature on the distribution of the hydrogen concentration were investigated using computational fluid dynamic (CFD) methods. The results indicated that the hydrogen concentration gradient changed gently with the larger diameter of the undulating pipeline, minimizing hydrogen accumulation. Higher undulation angle and smaller height differences reduces the hydrogen accumulation risk. Increasing vertical height difference of the pipeline from 5 m to 15 m increased the hydrogen volume fraction gradient by1.3 times. In the ball valve pipeline, the velocity fluctuation decreased as the ball valve opening increased. However, the hydrogen accumulation phenomenon was obvious. The opening increased from 25% to 100% and the hydrogen volume fraction gradient increased more than two times. Selecting delivery conditions with low hydrogen blending ratios, high temperatures, low pressures, and high flow rates reduces the occurrence of hydrogen buildup in the pipeline.
Project description:Driven by dual-carbon targets, marine engines are accelerating their transition towards low-carbon and zero-carbon. Ammonium-hydrogen fusion fuel is considered to be one of the most promising fuels for ship decarbonization. Using non-thermal plasma (NTP) catalytic ammonia on-line hydrogen production technology to achieve hydrogen supply is one of the most important means to guarantee the safety and effectiveness of hydrogen energy in the storage and transportation process. However, the efficiency of ammonia catalytic hydrogen production can be influenced to some extent by the presence of several factors, and the reaction mechanism is complex under the conditions of ship engine temperature emissions. This makes it difficult to realize the precise control of plasma catalytic hydrogen production from ammonia technology under temperature emission conditions, thus restricting an improvement in the ammonia conversion rate. In this study, a kinetic model of hydrogen production from ammonia catalyzed by NTP was established. The influencing factors (reaction temperature, pressure, N2/NH3 ratio in the feed gas) and mechanism path of hydrogen production from ammonia decomposition were explored. The results show that the increase in reaction temperature will lead to an increase in the ammonia conversion rate, while the ammonia conversion rate will decrease with the increase in reaction pressure and N2/NH3 ratio. When the reaction temperature is 300 K, the pressure is 1 bar, the feed gas is 98%N2/2%NH3, and the ammonia conversion rate is 16.7%. The reason why the addition of N2 is conducive to the hydrogen production from NH3 decomposition is that the reaction N2(A3) + NH3 => N2 + NH2 + H, triggered by the electron excited-state N2(A3), is the main reaction for NH3 decomposition.
Project description:The hydrogen evolution reaction (HER) is often considered parasitic to numerous cathodic electro-transformations of high technological interest, including but not limited to metal plating (e.g., for semiconductor processing), the CO2 reduction reaction (CO2RR), the dinitrogen → ammonia conversion (N2RR), and the nitrate reduction reaction (NO3-RR). Herein, we introduce a porous Cu foam material electrodeposited onto a mesh support through the dynamic hydrogen bubble template method as an efficient catalyst for electrochemical nitrate → ammonia conversion. To take advantage of the intrinsically high surface area of this spongy foam material, effective mass transport of the nitrate reactants from the bulk electrolyte solution into its three-dimensional porous structure is critical. At high reaction rates, NO3-RR becomes, however, readily mass transport limited because of the slow nitrate diffusion into the three-dimensional porous catalyst. Herein, we demonstrate that the gas-evolving HER can mitigate the depletion of reactants inside the 3D foam catalyst through opening an additional convective nitrate mass transport pathway provided the NO3-RR becomes already mass transport limited prior to the HER onset. This pathway is achieved through the formation and release of hydrogen bubbles facilitating electrolyte replenishment inside the foam during water/nitrate co-electrolysis. This HER-mediated transport effect "boosts" the effective limiting current of nitrate reduction, as evidenced by potentiostatic electrolyses combined with an operando video inspection of the Cu-foam@mesh catalysts under operating NO3-RR conditions. Depending on the solution pH and the nitrate concentration, NO3-RR partial current densities beyond 1 A cm-2 were achieved.
Project description:Hydrogen is an efficient source of clean and environmentally friendly energy. However, because it is explosive at concentrations higher than 4%, safety issues are a great concern. As its applications are extended, the need for the production of reliable monitoring systems is urgent. In this work, mixed copper-titanium oxide ((CuTi)Ox) thin films with various copper concentrations (0-100 at.%), deposited by magnetron sputtering and annealed at 473 K, were investigated as a prospective hydrogen gas sensing material. Scanning electron microscopy was applied to determine the morphology of the thin films. Their structure and chemical composition were investigated by X-ray diffraction and X-ray photoelectron spectroscopy, respectively. The prepared films were nanocrystalline mixtures of metallic copper, cuprous oxide, and titanium anatase in the bulk, whereas at the surface only cupric oxide was found. In comparison to the literature, the (CuTi)Ox thin films already showed a sensor response to hydrogen at a relatively low operating temperature of 473 K without using any extra catalyst. The best sensor response and sensitivity to hydrogen gas were found in the mixed copper-titanium oxides containing similar atomic concentrations of both metals, i.e., 41/59 and 56/44 of Cu/Ti. Most probably, this effect is related to their similar morphology and to the simultaneous presence of Cu and Cu2O crystals in these mixed oxide films. In particular, the studies of surface oxidation state revealed that it was the same for all annealed films and consisted only of CuO. However, in view of their crystalline structure, they consisted of Cu and Cu2O nanocrystals in the thin film volume.
Project description:Underground nuclear weapon testing produces radionuclide gases which may seep to the surface. Barometric pumping of gas through explosion-fractured rock is investigated using a new sequentially-coupled hydrodynamic rock damage/gas transport model. Fracture networks are produced for two rock types (granite and tuff) and three depths of burial. The fracture networks are integrated into a flow and transport numerical model driven by surface pressure signals of differing amplitude and variability. There are major differences between predictions using a realistic fracture network and prior results that used a simplified geometry. Matrix porosity and maximum fracture aperture have the greatest impact on gas breakthrough time and window of opportunity for detection, with different effects between granite and tuff simulations highlighting the importance of accurately simulating the fracture network. In particular, maximum fracture aperture has an opposite effect on tuff and granite, due to different damage patterns and their effect on the barometric pumping process. From stochastic simulations using randomly generated hydrogeologic parameters, normalized detection curves are presented to show differences in optimal sampling time for granite and tuff simulations. Seasonal and location-based effects on breakthrough, which occur due to differences in barometric forcing, are stronger where the barometric signal is highly variable.
Project description:Soot from jet fuel combustion in aircraft engines contributes to global warming through the formation of contrail cirrus clouds that make up to 56% of the total radiative forcing from aviation. Here, the elimination of such emissions is explored through N2 injection (containing 0-25 vol % O2) at the exhaust of enclosed spray combustion of jet fuel that nicely emulates aircraft soot emissions. It is shown that injecting N2 containing 5 vol % of O2 enhances the formation of polyaromatic hydrocarbons (PAHs) that adsorb on the surface of soot. This increases soot number density and volume fraction by 25 and 80%, respectively. However, further increasing the O2 concentration to 20 or 25 vol % enhances oxidation and nearly eliminates soot emissions from jet fuel spray combustion, reducing the soot number density and volume fraction by 87.3 or 95.4 and 98.3 or 99.6%, respectively. So, a judicious injection of air just after the aircraft engine exhaust can drastically reduce soot emissions and halve the radiative forcing due to aviation, as shown by soot mobility, X-ray diffraction, Raman spectroscopy, nitrogen adsorption, microscopy, and thermogravimetric analysis (for the organic to total carbon ratio) measurements.