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At least 19 records

BTRIC Technical Support for Appalachia: FY 2023 Summary Report on Net Negative Carbon Building Demonstration with AgPod

This study investigates the effects of various concentrations of carbon dioxide (CO 2 ) on the photosynthesis and biomass accumulation of crops growing in an Agricultural Pod (AgPod). The initial test crop was kale. It has been found that increasing the CO 2 concentration in the AgPod promotes higher photosynthetic rates in kale plants up to 1300 ppm (highest CO 2 concentration). An interesting finding was that net photosynthetic rates of kale leaves remain unsaturated until unusually high levels of photosynthetically active radiation (PAR, > 1200 µmolm-2s-1) and CO 2 concentration (> 1100 ppm) are reached. Such high levels of saturating PAR and CO 2 concentration values rarely occur under natural conditions, suggesting a promising potential for carbon capture via enriched greenhouse crop production. This task is one part of an overall plan to incorporate an AgPod to utilize carbon captured from the atmosphere to achieve net negative carbon emissions in a small neighborhood or community.

54 ENVIRONMENTAL SCIENCES↗

BTRIC Technical Support for Appalachia: FY 2024 Summary Report on Net Negative Carbon Building Demonstration with AgPod

This report investigates the effects of various concentrations of CO 2 on the photosynthesis and biomass accumulation of crops growing in an AgPod, using kale as the test crop. In the first year of the study, increasing the CO 2 concentration in the AgPod was found to promote higher photosynthetic rates in kale plants up to 1,300 ppm (the highest CO 2 concentration measured). An interesting finding was that net photosynthetic rates of kale leaves remain unsaturated until reaching unusually high levels of photosynthetically active radiation (PAR, > 1,200 µmol m -1 s -1 ) and CO 2 concentration (> 1,100 ppm). Such high levels of saturating PAR and CO 2 concentration values rarely occur under natural conditions, suggesting a promising potential for carbon capture via enriched controlled environment agriculture (ECEA). During the second year of the study, a second crop was planted to confirm the actual effects on growth with increased CO 2 concentrations. Our results suggest that growing kale plants in the AgPod system at higher CO 2 levels resulted in a successful and highly productive crop, up to three times the amount grown at 415 CO 2 . Further, the kale plants grown under higher CO 2 conditions (1000 ppm) are not CO 2 saturated and can potentially further improve yield at even higher CO 2 environments.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Strategies for connecting whole-building LCA to the low-carbon design process

Abstract Decarbonization is essential to meeting urgent climate goals. With the building sector in the United States accounting for 35% of total U.S. carbon emissions, reducing environmental impacts within the built environment is critical. Whole-building life cycle analysis (WBLCA) quantifies the impacts of a building throughout its life cycle. Despite being a powerful tool, WBLCA is not standard practice in the integrated design process. When WBLCA is used, it is typically either speculative and based on early design information or conducted only after design completion as an accounting measure, with virtually no opportunity to impact the actual design. This work proposes a workflow for fully incorporating WBLCA into the building design process in an iterative, recursive manner, where design decisions impact the WBLCA, which in turn informs future design decisions. We use the example of a negative-operational carbon modular building seeking negative upfront embodied carbon using bio-based materials for carbon sequestration as a case study for demonstrating the utility of the framework. Key contributions of this work include a framework of computational processes for conducting iterative WBLCA, using a combination of an existing building WBLCA tool (Tally) within the building information modeling superstructure (Revit) and a custom script (in R) for materials, life cycle stages, and workflows not available in the WBLCA tool. Additionally, we provide strategies for harmonizing the environmental impacts of novel materials or processes from various life cycle inventory sources with materials or processes in existing building WBLCA tool repositories. These strategies are useful for those involved in building design with an interest in reducing their environmental impact. For example, this framework would be useful for researchers who are conducting WBLCAs on projects that include new or unusual materials and for design teams who want to integrate WBLCA more fully into their design process in order to ensure the building materials are consciously chosen to advance climate goals, while still ensuring best performance by traditional measures.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Growing Insulation in Alaska

Buildings produce 40% of all carbon emissions in the U.S. This includes the energy needed to heat, cool, and power the nation's buildings and the energy used to manufacture, ship, and assemble the construction materials. In extreme climates and remote regions, buildings use even more energy, as building materials must be produced and shipped farther to the site, increasing the greenhouse gas emissions embodied in the buildings. The U.S. National Renewable Energy Laboratory (NREL) is developing technologies that reduce how much energy our buildings use and how much carbon goes into them in the first place. NREL researchers teamed up with the Biomaterials Laboratory at the University of Alaska, U.S. Forest Service Forest Products Lab, and the VTT Centre of Finland on a three-year project to "grow" insulation using trees in Alaska - improving the efficiency of buildings by providing envelope retrofit options using local resources.

carbon negative building↗

Life Cycle Assessment and Design of LignoBlock: A Lignin Bound Block on the Path Towards a Green Transition of the Construction Industry

Lignin-based biopolymer-bound soil composites (BSCs) are a new class of sustainable construction materials that utilize a bio-based biopolymer — lignin — as a binder. Prior use of lignin suggests that lignin is a promising candidate for the development of bio-based construction materials. Inspired by these applications, lignin-based BSCs were developed using lignoboost lignin, lignoforce lignin, alkali lignin, and hydrolysis lignin. Uni-axial compressive testing of lignin-based BSC shows that the compressive strength for these BSCs range from 1.6–8.1 MPa, which makes them appropriate for low compressive strength construction applications. We performed a life cycle assessment (LCA) of lignin-based BSC, with the functional unit being a CMU-sized block ( V =6423 cm -3 ). The major advantage of BSC lies in the elimination of ordinary portland cement, which is common to many construction materials, including many forms of concrete. Furthermore, the use of lignin in lignin-based BSC results in carbon sequestration (lignin ≈ 60 wt% carbon), potentially making construction materials made from lignin-based BSC carbon negative. Additionally, a design guide for estimating the life cycle carbon footprint of lignin-based BSC for a required compressive strength was developed. By utilizing the results from material tests and the LCA, designers are now able to use lignin effectively in construction applications, as they can now design lignin-based BSC for a target compressive strength with a full understanding of the life cycle carbon footprint implications.

Lignin↗

The Circular Home: Development and Demonstration of a Net Negative Carbon, Reusable Residence

This project started the development of an innovative modular building system intended for residential construction. The project was centered around single-family homes that were carbon-negative cradle-to-grave over a 100 year time frame, which is approximately double the current standard for operational life. The project sought to accomplish this objective by designing the modular home in a manner that ensures circularity, where the main house components can be used over several consecutive 50-year lifespans. To accomplish these objectives, this project utilized integrated design with the inclusion of life-cycle assessment to design the single-family house for architectural, structural, energy, mechanical, thermal, and moisture demands, while ensuring carbon negativity and annual net-zero energy use. The core technology of this project was the use of cross-laminated timber and biogenic materials, such as wood-fiber insulation, in the construction of the modular building units. The robustness and factory manufacturing ability of cross-laminated timber allow for factory construction of most of the home, which minimizes on-site time, saving money and reducing construction waste. During this project, initial milestones were met that delivered the architectural plans for the circular home and an initial structural testing matrix. Compared to current code-built homes, which average 13 kg CO2eq. / ft2 and are demolished at their end of life, the circular home has an estimated -30 kg CO2eq. / ft2 of embodied carbon emissions during its first build iteration. It is estimated that approximately 60%-70% of the total building mass could be reused and/or recycled during subsequent rebuilds. This project was concluded at approximately the 1/3 point and a separate project was established to conclude the remaining milestones. This project promises to benefit the public by delivering another option for single-family, and eventually multi-family, housing using a novel building construction system. The system of reusable modular construction facilitates not only lower emissions during the first building iteration, but also lower emissions during subsequent iterations that drastically reduce waste and help society meet its climate goals. Many other industries, such as clothing and technology sectors, are starting to focus on circularity and this project adds the residential building construction industry to that list.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Los Alamos Innovation Enables Carbon-Negative Infrastructure Through an AI Infrastructure Partnership

A material innovation first developed at Los Alamos National Laboratory (LANL) is now enabling a major step forward in carbon management. Licensed by Spiritus, the technology is being deployed in a $500 million partnership with Prometheus Hyperscale and Casper Carbon Capture to build one of the largest carbon-negative digital infrastructure projects in the world. Located in Casper, Wyoming, the initiative directly integrates permanent carbon removal with advanced computing systems, illustrating how Los Alamos research continues to advance national goals in energy, security, and innovation.

54 ENVIRONMENTAL SCIENCES↗

Wabash Hydrogen Negative Emissions Technology Demonstration

The objectives of the Wabash Hydrogen Negative Emissions Technology Demonstration Project (Wabash Project) are to develop and design all aspects of the scope, cost, characteristics and investment case of a world class flexible gasification, net negative carbon, hydrogen co-products power plant. The outcome of this undertaking is a complete set of deliverables that has been produced by a preeminent team of engineers, constructors, operators, and developers, building upon previous technology, utilizing cutting edge technology, and thoroughly defining all aspects of this fully integrated 21st Century Powerplant. The Wabash Project encapsulates several cross-cutting initiatives within the US Department of Energy, such as 100% hydrogen powered combustion turbine, geological carbon sequestration, coal with biomass gasification and hydrogen energy storage. The flexible gasifier at the Wabash Valley Resources plant is a slurry-fed, entrained flow, high-temperature, oxygen-blown gasifier that has been proven commercially to operate successfully on various coals and petroleum coke (petcoke). The ability to be fuel flexible and feed various biomass (woody biomass and agriculture residue) and petroleum waste (plastics) was evaluated during BP 1 (BP1). This involved the preparation and testing of feedstocks into slurries to determine what fuels can be fed to the gasifier. By utilizing a flexible oxygen-blown gasifier, the ability to address operational issues common to lower temperature biomass gasification, such as the handling of tars, can be mitigated. The overall goal is to achieve a design capable of carbon-negative emissions while leveraging the substantial investments made and operating experience already gained at the Wabash site.

01 COAL, LIGNITE, AND PEAT↗

Biomethanation to Upgrade Biogas to Pipeline Grade Methane

NREL is working closely with DOE, Electrochaea GmbH, and Southern California Gas Company (SoCalGas) to reduce costs of a biomethanation process capable of megawatt-scale deployment that upgrades organic biogas waste streams to produce pipeline quality renewable natural gas (RNG). Biomethanation is a two-step process using a single-celled methanogenic archaea that converts low-carbon low-cost hydrogen (H2) and waste carbon dioxide (CO2) to produce renewable methane (CH4). The process upgrades the biogenic CO2 - while allowing the CH4 to pass through - from biogas sources like dairies, wastewater treatment plants, and landfills. The CH4 produced is a drop-in direct replacement fuel and producers can participate in the growing number of carbon markets; like California's Low Carbon Fuel Standard and the Federal Renewable Fuel Standard. NREL and Argonne National Laboratory have completed a life cycle analysis using the GREET model to show that the biomethanation process produces RNG that is carbon negative even when H2 production via low-temperature water electrolysis is driven by the existing carbon intensity of California's electricity grid. And of course, even further carbon negative (-233 kg CO2e/kWh) when the electricity is produced from low-carbon sources like wind and solar. Leveraging lessons learned from operating SoCalGas' 700L 18-bar bioreactor system, NREL is designing and building a flexible RD&D platform that will enable field trials at biogas and other CO2 sources. A custom 16' long trailer will house a 20L 18-bar bioreactor, 3 - 25 kW proton exchange membrane electrolyzer, and dosing, thermal, and controls systems to support operations with only power, biogas, and water feedstocks required by the field locations. The end-of-project goal is to demonstrate pipeline quality RNG production (> 95% CH4, < 4% H2, <1% CO2, < 0.2% O2 and < 4 parts per million H2 sulfide) using real biogas feedstocks - thereby recycling both greenhouse gases for injection into the natural gas network or to be used onsite.

biogas upgrading↗

The Role of Fuels in Transforming Energy End-Use in Buildings and Industrial Processes

This book examines what role fuels have in the transformation of end-use in buildings and industrial processes. Energy efficient technologies are necessary to lower the carbon footprint for a transition towards clean energy in a sustainable manner. Efficient utilization of primary energy resources including renewables to support the current and future energy needs while targeting grid resiliency, energy and environmental security, at an affordable cost is of significant value. Analysis of configurations consisting of heat pumps, fuel driven thermal providers and power systems is presented. Sensitivity of electrical grid's carbon intensity towards carbon footprint in comparison with fuel driven technologies is necessary to recognize the true value proposition of currently available energy solutions for different end consumers. Similarly, the role of low carbon, zero carbon, and carbon negative fuels such as power to gas, power to liquid, hydrogen, biogas, etc. in conjunction with polygeneration technologies are discussed. Transformation of the primary energy resources from conventional fossil fuels to renewable fuels or electricity will have a significant impact on the overall carbon footprint of various end use sectors, including buildings. Hence, this book also examines two different scenarios focused on sensitivity of the pace of decarbonization of electrical grid and fuel supply on operational energy related carbon emissions.

Cheekatamarla, Praveen↗

Electrochemically Enhanced Carbonate Precipitation into Building Materials: A Scalable Carbon Sequestration Strategy

Decarbonization goals across hard-to-abate industries have prompted an urgent need for advanced carbon capture and storage technologies. Sequestering CO2 into carbonate minerals is a scalable method of carbon management with the ability to produce value-added carbon negative materials from waste streams for the construction industry. Waste streams rich in Ca and Mg such as nickel mine tailings, iron/steel slag, and reverse osmosis brines can store 7.6 Mt CO2/year as minerals. Additionally, CO2 mineralization in acid-neutralization processes currently present in industrial waste treatment can eliminate associated CO2 emissions of lime processing by improving process circularity. The carbonate minerals formed from these waste sources are valuable as components of carbon-negative concrete, which have the potential to sequester 1.8 billion Mt of CO2/year. Electrochemical means of CO2 mineralization improves the kinetics of the thermodynamically favorable mineralization process, lessening or eliminating the high energy requirements of traditional methods. Here, we investigate benchtop scale electrochemical CO2 mineralization of alkaline mining waste, highlighting the effects of key constituents in mining waste on the mineralization process.

carbon capture↗

Isotopic compositions of carbonates and organic carbon from upper Proterozoic successions in Namibia: stratigraphic variation and the effects of diagenesis and metamorphism

The carbon isotope geochemistry of carbonates and organic carbon in the late Proterozoic Damara Supergroup of Namibia, including the Nama, Witvlei, and Gariep groups on the Kalahari Craton and the Mulden and Otavi groups on the Congo Craton, has been investigated as an extension of previous studies of secular variations in the isotopic composition of late Proterozoic seawater. Subsamples of microspar and dolomicrospar were determined, through petrographic and cathodoluminescence examination, to represent the "least-altered" portions of the rock. Carbon-isotopic abundances in these phases are nearly equal to those in total carbonate, suggesting that 13C abundances of late Proterozoic fine-grained carbonates have not been significantly altered by meteoric diagenesis, although 18O abundances often differ significantly. Reduced and variable carbon-isotopic differences between carbonates and organic carbon in these sediments indicate that isotopic compositions of organic carbon have been altered significantly by thermal and deformational processes, likely associated with the Pan-African Orogeny. Distinctive stratigraphic patterns of secular variation, similar to those noted in other, widely separated late Proterozoic basins, are found in carbon-isotopic compositions of carbonates from the Nama and Otavi groups. For example, in Nama Group carbonates delta 13C values rise dramatically from -4 to +5% within a short stratigraphic interval. This excursion suggests correlation with similar excursions noted in Ediacaran-aged successions of Siberia, India, and China. Enrichment of 13C (delta 13C> +5%) in Otavi Group carbonates reflects those in Upper Riphean successions of the Akademikerbreen Group, Svalbard, its correlatives in East Greenland, and the Shaler Group, northwest Canada. The widespread distribution of successions with comparable isotopic signatures supports hypotheses that variations in delta 13C reflect global changes in the isotopic composition of late Proterozoic seawater. Within the Damara basin, carbon-isotopic compositions of carbonates provide a potentially useful tool for the correlation of units between the Kalahari and Congo cratons. Carbonates depleted in 13C were deposited during and immediately following three separate glacial episodes in Namibia. The correspondence between ice ages and negative delta 13C excursions may reflect the effects of lowered sea levels; enhanced circulation of deep, cold, O2-rich seawater; and/or the upwelling of 13C-depleted deep water. Iron-formation is additionally associated with one of the glacial horizons, the Chuos tillite. Carbon-13 enriched isotopic abundances in immediately pre-glacial carbonates suggest that oceanographic conditions favored high rates of organic burial. It is likely that marine waters were stratified, with deep waters anoxic. A prolonged period of ocean stratification would permit the build-up of ferrous iron, probably from hydrothermal sources. At the onset of glaciation, upwelling would have brought 13C-depleted and iron-rich deep water onto shallow shelves where contact with cold, oxygenated surface waters led to the precipitation of ferric iron.

NASA Program Exobiology↗

Retrofittable Thermal Switches for Dynamic Building Envelopes Integrated with Thermal Energy Storage: Preprint

Buildings in the United States consume about 40 quadrillion BTU of primary energy annually, which accounts for the nation's 40% of total energy use, 75% of all electricity use, and 35% of the net carbon emissions. Deploying thermal energy storage in the form of phase change material (PCM) in building envelopes is an effective method to reduce space heating/cooling loads, provide load shedding, and shift demand to periods of lower energy cost. However, the full potential of PCM-integrated envelopes can only be realized if the PCM undergoes complete phase change using free ambient heating/cooling, and the stored energy is effectively transferred between the exterior and the interior environments. Conventional thermal insulation (with a fixed thermal resistance) limits PCM utilization, particularly with the increasing emphasis on higher R-value in building envelopes, which negatively affects the energy-saving potential of a PCM-integrated envelope. In contrast, dynamic building envelopes integrated with PCMs provide the option of varying the thermal resistance based on the indoor and outdoor conditions, thereby enhancing utilization of free ambient cooling and heating to charge/discharge the PCM thermal storage, reducing the buildings' heating and cooling load, and shifting the peak energy demand. In this study, we demonstrate innovative retrofittable thermal switches in the form of the insertable plugs inside an insulation to provide variable thermal resistance depending on the operating temperature and direction of temperature gradient, thus allowing preferential directional heat flow. Notably, they are passive in nature, requiring no external power, and work solely based on the ambient temperature.

buildings↗

Electrochemical Hydrogen Peroxide Generator

Two-electron reduction of oxygen to produce hydrogen peroxide is a much researched topic. Most of the work has been done in the production of hydrogen peroxide in basic media, in order to address the needs of the pulp and paper industry. However, peroxides under alkaline conditions show poor stabilities and are not useful in disinfection applications. There is a need to design electrocatalysts that are stable and provide good current and energy efficiencies to produce hydrogen peroxide under acidic conditions. The innovation focuses on the in situ generation of hydrogen peroxide using an electrochemical cell having a gas diffusion electrode as the cathode (electrode connected to the negative pole of the power supply) and a platinized titanium anode. The cathode and anode compartments are separated by a readily available cation-exchange membrane (Nafion 117). The anode compartment is fed with deionized water. Generation of oxygen is the anode reaction. Protons from the anode compartment are transferred across the cation-exchange membrane to the cathode compartment by electrostatic attraction towards the negatively charged electrode. The cathode compartment is fed with oxygen. Here, hydrogen peroxide is generated by the reduction of oxygen. Water may also be generated in the cathode. A small amount of water is also transported across the membrane along with hydrated protons transported across the membrane. Generally, each proton is hydrated with 3-5 molecules. The process is unique because hydrogen peroxide is formed as a high-purity aqueous solution. Since there are no hazardous chemicals or liquids used in the process, the disinfection product can be applied directly to water, before entering a water filtration unit to disinfect the incoming water and to prevent the build up of heterotrophic bacteria, for example, in carbon based filters. The competitive advantages of this process are: 1. No consumable chemicals are needed in the process. The only raw materials needed are water and oxygen or air. 2. The product is pure and can therefore be used in disinfection applications directly or after proper dilution with water. 3. Oxygen generated in the anode compartment is used in the electrochemical reduction process; in addition, external oxygen is used to establish a high flow rate in the cathode compartment to remove the desired product efficiently. Exiting oxygen can be recycled after separation of liquid hydrogen peroxide product, if so desired. 4. The process can be designed for peroxide generation under microgravity conditions. 5. High concentrations of the order of 6-7 wt% can be generated by this method. This method at the time of this reporting is superior to what other researchers have reported. 6. The cell design allows for stacking of cells to increase the hydrogen peroxide production. 7. The catalyst mix containing a diquaternary ammonium compound enabled not only higher concentration of hydrogen peroxide but also higher current efficiency, improved energy efficiency, and catalyst stability. 8. The activity of the catalyst is maintained even after repeated periods of system shutdown. 9. The catalyst system can be extended for fuel-cell cathodes with suitable modifications.

Tennakoon, Charles L. K.↗

Synergism of Saturn, Enceladus and Titan and Formation of HCNO Exobiological Molecules

Saturn as a system has two very exotic moons Titan and Enceladus. Titan with energy input from Saturn's magnetosphere, solar UV irradiation, and cosmic rays can make HCN based molecules as discussed in earlier paper by [1]. Space radiation effects at both moons, and as coupled by the Saturn magnetosphere could cause an unexpected series of events leading to the evolution of biological models at Titan composed of HCNO with oxygen as the new ingredient. The "Old Faithful" model by [2] suggests that Enceladus, highly irradiated by Saturn magnetospheric electrons, has episodic ejections of water vapor driven by radiolytic oxidation gas products into Saturn's magnetosphere. At Titan Cassini discovered 1) that keV oxygen ions, evidently from Enceladus, are bombarding Titan's upper atmosphere [3] and 2) the discovery of heavy positive and negative ions within Titan's upper atmosphere [4]. Initial models of heavy ion formation in Titan's upper atmosphere invoked polymerization of aromatics such as Benzenes and their radicals to make PAHs [5], while a more recent model by [6] has raised the possibility of carbon chains forming from the polymerization of acetylene and its radicals to eventually make fullerenes. Laboratory measurements indicate that fullerenes, which are hollow carbon shells, can trap the keV oxygen and with the clustering of fullerenes and possible mixture with PAHs, some with nitrogen molecules, can make the larger aerosols with oxygen within them. Then with further ionizing irradiation from cosmic rays deep in the atmosphere "tholin" molecules are produced with all the molecular components present from which organic molecules can form. Among the molecular components are amino acids, the fundamental building blocks of life as we know it. This process maybe a common chemical pathway, both at the system level and at the molecular level, to form prebiotic and perhaps even biotic molecules. Such processes can be occurring throughout our universe, such as molecular clouds in the ISM.

Sittler, Edward C., Jr.↗

Strangelove Ocean and Deposition of Unusual Shallow-Water Carbonates After the End-Permian Mass Extinction

The severe mass extinction of marine and terrestrial organisms at the end of the Permian Period (approx. 251 Ma) was accompanied by a rapid negative excursion of approx. 3 to 4 per mil in the carbon-isotope ratio of the global surface oceans and atmosphere that persisted for some 500,000 into the Early Triassic. Simulations with an ocean-atmosphere/carbon-cycle model suggest that the isotope excursion can be explained by collapse of ocean primary productivity (a Strangelove Ocean) and changes in the delivery and cycling of carbon in the ocean and on land. Model results also suggest that perturbations of the global carbon cycle resulting from the extinctions led to short-term fluctuations in atmospheric pCO2 and ocean carbonate deposition, and to a long-term (>1 Ma) decrease in sedimentary burial of organic carbon in the Triassic. Deposition of calcium carbonate is a major sink of river-derived ocean alkalinity and for CO2 from the ocean/atmosphere system. The end of the Permian was marked by extinction of most calcium carbonate secreting organisms. Therefore, the reduction of carbonate accumulation made the oceans vulnerable to a build-up of alkalinity and related fluctuations in atmospheric CO2. Our model results suggest that an increase in ocean carbonate-ion concentration should cause increased carbonate accumulation rates in shallow-water settings. After the end-Permian extinctions, early Triassic shallow-water sediments show an abundance of abiogenic and microbial carbonates that removed CaCO3 from the ocean and may have prevented a full 'ocean-alkalinity crisis' from developing.

Rampino, Michael R.↗

An ionic mechanism of carbon formation in flames

The formation of incipient carbon in flames can be described by a series of elementary reactions in which the precursor of soot is the ion C3H3+, and the major building block is acetylene, polyacetylenes, or other hydrocarbon fragments which are present in large concentrations. The precursor ion is produced by nonequilibrium chemi-ionization reactions, e.g., CH asterisk plus C2H2 yields C3H3+ plus e or CH asterisk plus O yields CHO+ plus e. The CHO+ rapidly becomes C3H3+ through a series of ion-molecule reactions. The chemi-ion then adds acetylene in a series of very rapid ion-molecule reactions producing larger and larger ions. Ions isomerize very rapidly to produce aromatic structures overcoming one of the major problems with neutral species mechanisms: how to form the first carbon ring. As the ions grow, their recombination rate coefficients with electrons increase so that the larger ions are removed by dissociative recombination. These neutral species now continue to grow by the addition of more acetylene producing even larger neutral species. With increasing size, the rate coefficient of electron attachment also increases causing the reaction to become important, depending upon the temperature. Appreciable concentrations of negative ions shift the ion removal process to dissociative ion-ion recombination, which is orders of magnitude slower than ion-electron recombination. As the neutral species continue to grow by the addition of acetylene, they gradually take on the aspect of particles, i.e., the bulk properties of the substance CxHy dominate over the chemical properties. This change is gradual and there is no distinct size at which a large molecule becomes a particle. Evidence will be presented supporting the above mechanism. All of the ions proposed in the mechanism have been observed by mass spectrometric analysis, their concentrations measured, and their rates of reaction in the flame environment determined to be adequate to account for the observed rate of formation of carbon.

Calcote, H. F.↗