Earth, humans, and metals: investigating the role of iron and other metals in the atmospheric, oceanic, and energy systems

Includes bibliographical references.2022 Fall.Metals such as iron and copper have been an integral component of the Earth system since its beginnings and have formed the basis for modern human civilization growth since the Bronze and Iron Ages. Human activities include metals at various levels, from burning coal in power plants and mining ores lead to emissions of particulate and gaseous metallic products into the atmosphere. While suspended in the air, metal oxides such as hematite and magnetite absorb solar radiation, thus warming the atmosphere. After falling into the oceans, metals such as iron and magnesium act as important nutrients for oceanic biota, and thus affect the marine nutrient and carbon cycles. Human activities have increased many-fold since the beginning of the Industrial Era, and as the world moves from fossil fuel to renewable energy to reduce carbon emissions, the demand for metals is also projected to increase many folds. Yet, the past, present, and future impacts of anthropogenic activities on the atmospheric and marine metal cycles, particularly iron, remain poorly understood.In Chapter 2, I estimate the atmospheric radiative and oceanic biological impacts of anthropogenic iron emissions over the Industrial Era. I perform simulations using a mineralogy-based inventory and an Earth System Model and estimate the 1850-to-2010 global mean direct radiative forcing by anthropogenic iron to be +0.02 to +0.10 W/m2. I estimate that the enhanced phytoplankton primary production due to anthropogenic soluble iron deposition over the last 150 years caused carbon dioxide (CO2) sequestration of 0.2-13 ppmv. This sequestered CO2 also led to an 'avoided' CO2 forcing of -0.002 to -0.16 W/m2. While globally small, these impacts can be higher in specific regions; the anthropogenic iron oxide direct radiative forcing is +0.5 W/m2 over areas such as East Asia and India with more coal combustion and metal smelting. Anthropogenic soluble iron sustains >10% of marine net primary productivity in the high-latitude North Pacific Ocean, a region vulnerable to thermal stratification due to climate change. In Chapter 3, I focus on evaluating anthropogenic total iron emissions using observations and models. Performing the model-observation comparison only at sites where the modeled anthropogenic contribution is the highest, I find that the current emission inventory underestimates anthropogenic total iron emissions from North America and Europe by a factor of 3-5. Further isolating anthropogenic sectoral emissions over North America using Positive Matrix Factorization, I find that smelting and coal combustion emissions are overestimated by a factor of 3-10 in the current emission inventory, whereas heavy fuel oil emissions from ships and industrial boilers are underestimated by a factor of 2-5. By comparing modeled concentrations of iron oxides with observations from Japan, I find that the current smelting and coal combustion emissions from East Asia are only slightly overestimated in the inventory, by a factor of 1.2-1.5. Finally, in Chapter 4, I explore the regionality and magnitude of PM2.5 emissions from metal mining and smelting to meet projected global renewable energy demand. I estimate future PM2.5 (particulate matter smaller than 2.5 μm diameter) emissions from mining and smelting to meet the metal demand of renewable energy technologies in two climate pathways to be 0.3-0.6 Tg/yr in the 2020-2050 period, which is projected to contribute 10-30% of total anthropogenic primary PM2.5 combustion emissions in many countries. The concentration of mineral reserves in a few regions means the impacts are also regionally concentrated. Rapid decarbonization could lead to a faster reduction of overall anthropogenic PM2.5 emissions but also could create more unevenness in the distributions of emissions relative to where demand occurs

Impact of Changes to the Atmospheric Soluble Iron Deposition Flux on Ocean Biogeochemical Cycles in the Anthropocene

Iron can be a growth‐limiting nutrient for phytoplankton, modifying rates of net primary production, nitrogen fixation, and carbon export ‐ highlighting the importance of new iron inputs from the atmosphere. The bioavailable iron fraction depends on the emission source and the dissolution during transport. The impacts of anthropogenic combustion and land use change on emissions from industrial, domestic, shipping, desert, and wildfire sources suggest that Northern Hemisphere soluble iron deposition has likely been enhanced between 2% and 68% over the Industrial Era. If policy and climate follow the intermediate Representative Concentration Pathway 4.5 trajectory, then results suggest that Southern Ocean (>30°S) soluble iron deposition would be enhanced between 63% and 95% by 2100. Marine net primary productivity and carbon export within the open ocean are most sensitive to changes in soluble iron deposition in the Southern Hemisphere; this is predominantly driven by fire rather than dust iron sources. Changes in iron deposition cause large perturbations to the marine nitrogen cycle, up to 70% increase in denitrification and 15% increase in nitrogen fixation, but only modestly impacts the carbon cycle and atmospheric CO2 concentrations (1–3 ppm). Regionally, primary productivity increases due to increased iron deposition are often compensated by offsetting decreases downstream corresponding to equivalent changes in the rate of phytoplankton macronutrient uptake, particularly in the equatorial Pacific. These effects are weaker in the Southern Ocean, suggesting that changes in iron deposition in this region dominates the global carbon cycle and climate response

Modelling of the effect of ELMs on fuel retention at the bulk W divertor of JET

Effect of ELMs on fuel retention at the bulk W target of JET ITER-Like Wall was studied with multi-scale calculations. Plasma input parameters were taken from ELMy H-mode plasma experiment. The energetic intra-ELM fuel particles get implanted and create near-surface defects up to depths of few tens of nm, which act as the main fuel trapping sites during ELMs. Clustering of implantation-induced vacancies were found to take place. The incoming flux of inter-ELM plasma particles increases the different filling levels of trapped fuel in defects. The temperature increase of the W target during the pulse increases the fuel detrapping rate. The inter-ELM fuel particle flux refills the partially emptied trapping sites and fills new sites. This leads to a competing effect on the retention and release rates of the implanted particles. At high temperatures the main retention appeared in larger vacancy clusters due to increased clustering rate

On the mechanisms governing gas penetration into a tokamak plasma during a massive gas injection

A new 1D radial fluid code, IMAGINE, is used to simulate the penetration of gas into a tokamak plasma during a massive gas injection (MGI). The main result is that the gas is in general strongly braked as it reaches the plasma, due to mechanisms related to charge exchange and (to a smaller extent) recombination. As a result, only a fraction of the gas penetrates into the plasma. Also, a shock wave is created in the gas which propagates away from the plasma, braking and compressing the incoming gas. Simulation results are quantitatively consistent, at least in terms of orders of magnitude, with experimental data for a D 2 MGI into a JET Ohmic plasma. Simulations of MGI into the background plasma surrounding a runaway electron beam show that if the background electron density is too high, the gas may not penetrate, suggesting a possible explanation for the recent results of Reux et al in JET (2015 Nucl. Fusion 55 093013)

Modelling of tungsten erosion and deposition in the divertor of JET-ILW in comparison to experimental findings

The erosion, transport and deposition of tungsten in the outer divertor of JET-ILW has been studied for an HMode discharge with low frequency ELMs. For this specific case with an inter-ELM electron temperature at the strike point of about 20 eV, tungsten sputtering between ELMs is almost exclusively due to beryllium impurity and self-sputtering. However, during ELMs tungsten sputtering due to deuterium becomes important and even dominates. The amount of simulated local deposition of tungsten relative to the amount of sputtered tungsten in between ELMs is very high and reaches values of 99% for an electron density of 5E13 cm$^{-3}$ at the strike point and electron temperatures between 10 and 30 eV. Smaller deposition values are simulated with reduced electron density. The direction of the B-field significantly influences the local deposition and leads to a reduction if the E×B drift directs towards the scrape-off-layer. Also, the thermal force can reduce the tungsten deposition, however, an ion temperature gradient of about 0.1 eV/mm or larger is needed for a significant effect. The tungsten deposition simulated during ELMs reaches values of about 98% assuming ELM parameters according to free-streaming model. The measured WI emission profiles in between and within ELMs have been reproduced by the simulation. The contribution to the overall net tungsten erosion during ELMs is about 5 times larger than the one in between ELMs for the studied case. However, this is due to the rather low electron temperature in between ELMs, which leads to deuterium impact energies below the sputtering threshold for tungsten