Easy tuning of nanotexture and N doping of carbonaceous particles produced by spark discharge

A better understanding of the effects of carbonaceous particulates in air pollution on human health and on the transmission of viruses requires studies with artificially produced aerosols that mimic the real ones. To produce such aerosols, methods to precisely tailor the morphology as well as the physical and chemical properties of carbon-based nanomaterials are crucial. Here we describe a facile and flexible approach to produce carbon-based nanoparticles with tailored N content by spark discharge utilizing graphite rods. Carbon-based nanoparticles with different nanotexture and N doping could be obtained by simply changing dilution gas (nitrogen, argon) and dilution gas purity (99 and 99.999%). The effect of the discharge frequency (50, 300 Hz) was also explored. The carbon-based nanoparticles were characterized by Fourier transform infrared and X-ray photoelectron spectroscopy, thermogravimetric analysis, and transmission electron microscopy. We find that the nanotexture is strictly linked to the chemical reactivity and to the surface chemistry. The use of N2 as dilution gas allowed for the incorporation of significant amounts of nitrogen (5–7 wt.%) in the carbonaceous particle network mainly as pyrrolic N, graphitic N and N-oxide functional groups

Oscillatory Behavior in Methane Combustion: Influence of the Operating Parameters

The influence of the main process parameters on the oscillatory behavior of methane oxidation was analyzed in conditions relevant for low-temperature combustion processes. The investigation was performed by means of direct comparisons between experimental measurements realized in two jet-stirred flow reactors used at atmospheric pressure. With the operating conditions of the two systems coupled, wide ranges of the inlet temperature (790-1225 K), equivalence ratio (0.5 < Φ < 1.5), methane mole fraction (XCH4 from 0.01 to 0.05), bath gases (i.e., He, N2, CO2, or H2O) and different overall mixture dilution levels were exploited in relation to the identification of oscillatory regimes. Although the reference systems mainly differ in thermal conditions (i.e., heat exchange to the surroundings), temperature measurements suggested that the oscillatory phenomena occurred when the system working temperature accessed a well-identifiable temperature range. Experimental results were simulated by means of a detailed kinetic scheme and commercial codes developed for complex chemistry processes. Simulations were also extended considering systems with different heat losses to the surroundings, thus passing from adiabatic to isothermal systems. Results highlighted the kinetic nature of the dynamic behavior. Because predictions were consistent with experimental tests, further numerical analyses were realized to identify the kinetics responsible for the establishment of oscillatory phenomena. Temperature oscillations were predicted for a significant reactor working temperature range, where oxidation and recombination kinetic routes, involving carbon C1-2 species as well as reactions of the H2/O2 sub-scheme, become competitive, thus boosting limit cycle behaviors. Oscillatory phenomena cease when the system working temperatures exceed characteristic threshold values with the promotion of faster oxidation routes that diminish the inhibiting effects of recombination reactions

Review on ammonia as a potential fuel: from synthesis to economics

Ammonia, a molecule that is gaining more interest as a fueling vector, has been considered as a candidate to power transport, produce energy, and support heating applications for decades. However, the particular characteristics of the molecule always made it a chemical with low, if any, benefit once compared to conventional fossil fuels. Still, the current need to decarbonize our economy makes the search of new methods crucial to use chemicals, such as ammonia, that can be produced and employed without incurring in the emission of carbon oxides. Therefore, current efforts in this field are leading scientists, industries, and governments to seriously invest efforts in the development of holistic solutions capable of making ammonia a viable fuel for the transition toward a clean future. On that basis, this review has approached the subject gathering inputs from scientists actively working on the topic. The review starts from the importance of ammonia as an energy vector, moving through all of the steps in the production, distribution, utilization, safety, legal considerations, and economic aspects of the use of such a molecule to support the future energy mix. Fundamentals of combustion and practical cases for the recovery of energy of ammonia are also addressed, thus providing a complete view of what potentially could become a vector of crucial importance to the mitigation of carbon emissions. Different from other works, this review seeks to provide a holistic perspective of ammonia as a chemical that presents benefits and constraints for storing energy from sustainable sources. State-of-the-art knowledge provided by academics actively engaged with the topic at various fronts also enables a clear vision of the progress in each of the branches of ammonia as an energy carrier. Further, the fundamental boundaries of the use of the molecule are expanded to real technical issues for all potential technologies capable of using it for energy purposes, legal barriers that will be faced to achieve its deployment, safety and environmental considerations that impose a critical aspect for acceptance and wellbeing, and economic implications for the use of ammonia across all aspects approached for the production and implementation of this chemical as a fueling source. Herein, this work sets the principles, research, practicalities, and future views of a transition toward a future where ammonia will be a major energy player

Combining farmers' decision rules and landscape stochastic regularities for landscape modelling

International audienceLandscape spatial organization (LSO) strongly impacts many environmental issues. Modelling agricultural landscapes and describing meaningful landscape patterns are thus regarded as key-issues for designing sustainable landscapes. Agricultural landscapes are mostly designed by farmers. Their decisions dealing with crop choices and crop allocation to land can be generic and result in landscape regularities, which determine LSO. This paper comes within the emerging discipline called "landscape agronomy", aiming at studying the organization of farming practices at the landscape scale. We here aim at articulating the farm and the landscape scales for landscape modelling. To do so, we develop an original approach consisting in the combination of two methods used separately so far: the identification of explicit farmer decision rules through on-farm surveys methods and the identification of landscape stochastic regularities through data-mining. We applied this approach to the Niort plain landscape in France. Results show that generic farmer decision rules dealing with sunflower or maize area and location within landscapes are consistent with spatiotemporal regularities identified at the landscape scale. It results in a segmentation of the landscape, based on both its spatial and temporal organization and partly explained by generic farmer decision rules. This consistency between results points out that the two modelling methods aid one another for land-use modelling at landscape scale and for understanding the driving forces of its spatial organization. Despite some remaining challenges, our study in landscape agronomy accounts for both spatial and temporal dimensions of crop allocation: it allows the drawing of new spatial patterns coherent with land-use dynamics at the landscape scale, which improves the links to the scale of ecological processes and therefore contributes to landscape ecology.L'organisation du paysage influe sur les problèmes environnementaux. Modéliser les paysages pour les décrire à l'aide de formes significatives est une étage clé. Les paysages agricoles sont principalement construits par les agriculteurs dont les décision d'assolement peuvent être génériques et déterminer des régularités dans l'organisation du paysage. Cet article contribue à l'agronomie des paysage qui est une discipline émergente. Nous cherchons à articuler les échelles du paysage et de l'exploitation agricole en développant deux méthodes : l'une consiste à identifier les décisions des agriculteurs par le bais d'enquêtes, l'autre consiste à retrouver des régularités stochastiques dans le paysage par le bais de fouille de données. Nous avons appliqué cette approche au paysage de la plaine de Niort en France. Les résultats montrent que les décisions des agriculteurs en matière de tournesol et maïs sont génériques et ont des effets sur le paysages que des méthodes de fouille de données révèlent et quantifient

HDDI in Mild combustion

Mild combustion is an emerging technology in several fields of practical applications, from material treatment to energy conversion as well as to pollutant abatement [1]. In a survey of potential keys for the mitigation of environmental problem, it represents a flexible and clean process that is the result of a trade-off in the optimization of fuel conversion with respect to efficiency (in term of energy saving and pollutant abatement) while not requiring drastic changes in the configuration of traditional plants. In this chapter the attention will be focused on non-premixed combustion processes, thus on configurations where the fuel and the oxidant flows are fed separately, then mix and react. A combination of both heating and dilution of oxidant and/or fuel yields a not premixed combustion process which is named Hot Diluted Diffusion Ignition (HDDI) [2, 4] when • heating contributes significantly to the creation of an oxidative structure in the sense that no combustion process occurs without it; • dilution is so intense that the maximum temperature attainable inside this structure is so low that, in turn, it affects significantly its placement in the mixture fraction domain, the structure itself and the physical and chemical kinetics when compared to a diffusion flame process