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A comprehensive assessment of process design, cost efficiency, critical mineral recovery, and CO 2 storage in mine tailings.
As global temperatures rise, large amounts of carbon sequestered in permafrost are becoming available for microbial degradation. However, accurate prediction of carbon gas emissions produced from thawing permafrost is limited by our understanding of the resident microbial communities and their associated carbon metabolism. Here, metagenomic sequencing of 214 samples from intact, thawing and thawed sites collected over three years enabled the recovery of 1,529 metagenome-assembled genomes (MAGs), including many from phyla with poor genomic representation. These genomes were shown to broadly reflect the diversity of this complex ecosystem with genus-level representatives recovered for >60% of the community, constituting a two orders of magnitude increase in the number of genomes available for understanding carbon processing in this environment. Metabolic reconstruction, supported by metatranscriptomic and metaproteomic data, revealed key populations involved in organic matter degradation, including bacteria encoding a pathway for xylose degradation only previously identified in fungi. Combined analysis of the microbial communities and geochemical data highlighted lineages correlated with the production of greenhouse gases and suggest novel syntrophic relationships. Our findings link changing biogeochemistry to specific microbial lineages involved in each stage of carbon processing, providing key information for predicting the impact of climate change on these systems.
The low hydration and carbonation of reactive MgO cement (RMC) under ambient conditions causes prolonged setting and low compressive strengths (~4 MPa). This study proposed a unique technique which led to the enhancement of the hydration and carbonation processes via the synergistic combination of microbial carbonation process (MCP) with a hydration agent (HA) that enabled the self‑carbonation of RMC-based mixes without using of any special curing environments. Through hydrolysing urea (CO(NH{sub 2}){sub 2}) using ureolytic bacteria, CO{sub 3}{sup 2−} ions were produced to facilitate the carbonation of dissolved Mg{sup 2+} ions to form hydrated magnesium hydroxy carbonates (HMHCs). The self‑carbonation of RMC enabled by the MCP resulted in formation of brucite with a poor crystallinity and its rapid conversion into HMHCs, which improved the setting time and compressive strength of RMC-based samples. The simultaneous use of MCP with 2 M urea and HA revealed HMHCs with improved morphologies, resulting in the highest compressive strength (~15 MPa).
Geostationary Carbon Process Mapper (GCPM) is an earth science mission to measure key atmospheric trace gases related to climate change and human activity.Understanding of sources and sinks of CO2 is currently limited by frequency of observations and uncertainty in vertical transport. GCPM improves this situation by making simultaneous high resolution measurements of CO2, CH4, CF, and CO in near-IR, many times per day. GCPM is able to investigate processes with time scales of minutes to hours. CO2, CH4, CF, Co selected because their combination provides information needed to disentangle natural and anthropogenic sources/sinks. Quasi-continuous monitoring effectively eliminates atmospheric transport uncertainties from source/sink inversion modeling. will have one instrument (GeoFTS), hosted on a commercial communications satellite, planned for two years operation. GCPM will affordably advance the understanding of observed cycle variability improving future climate projections.
Terrestrial carbon processes are affected by soil moisture, soil temperature, nitrogen availability and solar radiation, among other factors. Most of the current ecosystem biogeochemistry models represent one point in space, and have limited characterization of hydrologic processes. Therefore these models can neither resolve the topographically driven spatial variability of water, energy, and nutrient, nor their effects on carbon processes. A spatially-distributed land surface hydrologic biogeochemistry model, Flux-PIHM-BGC, is developed by coupling the Biome-BGC model with a physically-based land surface hydrologic model, Flux-PIHM. In the coupled system, each Flux-PIHM model grid couples a 1-D Biome-BGC model. In addition, a topographic solar radiation module and an advection-driven nitrogen transport module are added to represent the impact of topography on nutrient transport and solar energy distribution. Because Flux-PIHM is able to simulate lateral groundwater flow and represent the land surface heterogeneities caused by topography, Flux-PIHM-BGC is capable of simulating the complex interaction among water, energy, nutrient, and carbon in time and space. The Flux-PIHM-BGC model is tested at the Susquehanna/Shale Hills Critical Zone Observatory. Model results show that distributions of carbon and nitrogen stocks and fluxes are strongly affected by topography and landscape position, and tree growth is nitrogen limited. The predicted aboveground and soil carbon distributions generally agree with the macro patterns observed. Although the model underestimates the spatial variation, the predicted watershed average values are close to the observations. Lastly, the coupled Flux-PIHM-BGC model provides an important tool to study spatial variations in terrestrial carbon and nitrogen processes and their interactions with environmental factors, and to predict the spatial structure of the responses of ecosystems to climate change.
During the carbonization process of raw polymer precursors, graphitic structures can evolve. The presence of these graphitic structures affects mechanical properties of the carbonized carbon fibers. To gain a better understanding of the chemistry behind the evolution of these structures, we performed atomistic-scale simulations using the ReaxFF reactive force field. Three different polymers were considered as a precursor: idealized ladder PAN (polyacrylonitrile), a proposed oxidized PAN, and poly(p-phenylene- 2,6-benzobisoxazole). We determined the underlying molecular details of polymer conversion into a carbon fiber structure. Because these are C/H/O/ N-based polymers, we first developed an improved force field for C/H/O/N chemistry based on the density functional theory data with a particular focus on N2 formation kinetics and its interactions with polymer-associated radicals formed during the carbonization process. Then, using this improved force field, we performed atomistic-scale simulations of the initial stage of the carbonization process for the considered polymers. On the basis of our simulation data, the molecular pathways for the formation of low-molecular-weight gas species and all-carbon ring formation were determined. We also examined the possible alignment of the developed all-carbon 6-membered ring clusters, which is crucial for the further graphitic structure evolution.
ABSTRACT Rapidly thawing permafrost harbors ∼30 to 50% of global soil carbon, and the fate of this carbon remains unknown. Microorganisms will play a central role in its fate, and their viruses could modulate that impact via induced mortality and metabolic controls. Because of the challenges of recovering viruses from soils, little is known about soil viruses or their role(s) in microbial biogeochemical cycling. Here, we describe 53 viral populations (viral operational taxonomic units [vOTUs]) recovered from seven quantitatively derived (i.e., not multiple-displacement-amplified) viral-particle metagenomes (viromes) along a permafrost thaw gradient at the Stordalen Mire field site in northern Sweden. Only 15% of these vOTUs had genetic similarity to publicly available viruses in the RefSeq database, and ∼30% of the genes could be annotated, supporting the concept of soils as reservoirs of substantial undescribed viral genetic diversity. The vOTUs exhibited distinct ecology, with different distributions along the thaw gradient habitats, and a shift from soil-virus-like assemblages in the dry palsas to aquatic-virus-like assemblages in the inundated fen. Seventeen vOTUs were linked to microbial hosts ( in silico ), implicating viruses in infecting abundant microbial lineages from Acidobacteria , Verrucomicrobia , and Deltaproteobacteria , including those encoding key biogeochemical functions such as organic matter degradation. Thirty auxiliary metabolic genes (AMGs) were identified and suggested virus-mediated modulation of central carbon metabolism, soil organic matter degradation, polysaccharide binding, and regulation of sporulation. Together, these findings suggest that these soil viruses have distinct ecology, impact host-mediated biogeochemistry, and likely impact ecosystem function in the rapidly changing Arctic. IMPORTANCE This work is part of a 10-year project to examine thawing permafrost peatlands and is the first virome-particle-based approach to characterize viruses in these systems. This method yielded >2-fold-more viral populations (vOTUs) per gigabase of metagenome than vOTUs derived from bulk-soil metagenomes from the same site (J. B. Emerson, S. Roux, J. R. Brum, B. Bolduc, et al., Nat Microbiol 3:870–880, 2018, https://doi.org/10.1038/s41564-018-0190-y). We compared the ecology of the recovered vOTUs along a permafrost thaw gradient and found (i) habitat specificity, (ii) a shift in viral community identity from soil-like to aquatic-like viruses, (iii) infection of dominant microbial hosts, and (iv) carriage of host metabolic genes. These vOTUs can impact ecosystem carbon processing via top-down (inferred from lysing dominant microbial hosts) and bottom-up (inferred from carriage of auxiliary metabolic genes) controls. This work serves as a foundation which future studies can build upon to increase our understanding of the soil virosphere and how viruses affect soil ecosystem services.
This study investigates how operating conditions (temperature and residence time) and benzoyl chloride impact hydrochar production from almond shells through hydrothermal carbonization. Carbon content rises while volatile matter decreases with increasing temperature, yielding a hydrochar with an estimated heating value of 28 MJ/kg. Elevated temperatures lower the O/C and H/C atomic ratios of hydrochars. Even at the lowest temperature under scrutiny, catalytic experiments using benzoyl chloride enhance carbonization and fuel ratio across all temperatures. Hydrochars produced through catalytic runs demonstrate elevated fuel ratios relative to those generated through noncatalytic runs, despite operating under the same conditions. These insights reveal the capacity of benzoyl chloride as a catalyst to improve hydrochar properties, suggesting its utility for advancing both the efficiency and effectiveness of hydrothermal carbonization processes.
Air-processed carbon-based perovskite solar cells (C-PSCs) offer scalable and cost-effective photovoltaic manufacturing but face efficiency loss compared to metal-contact perovskite solar cells. Surface passivation of three-dimensional (3D) perovskites with two-dimensional (2D) perovskite layers has emerged as a promising strategy to enhance device performance. However, the mechanisms by which 2D perovskites more effectively improve C-PSC efficiency and stability remain underexplored. This study investigates the efficacy of 2D/3D heterostructures using n-hexylammonium bromide (C6Br), phenethylammonium iodide (PEAI), and n-octylammonium iodide (OAI) as surface passivators for C-PSCs. C-PSCs treated with C 6 Br achieved a champion power conversion efficiency (PCE) of 21.0%. This enhancement is attributed to superior defect passivation, improved charge extraction, and suppressed non-radiative recombination. Transient ion-drift characterization demonstrates that C 6 Br and OAI reduce ionic conductivity by 2–3 orders of magnitude, correlating with enhanced operational stability under continuous illumination. Our findings highlight the role of short-chain bromide cations (C 6 Br) in optimizing halide-mediated defect healing and interfacial band alignment, positioning 2D-passivated C-PSCs as viable competitors to conventional metal-contact perovskite solar cells.
This study quantifies black carbon (BC) processes in three global climate models and one chemistry transport model, with focus on the seasonality of BC transport, emissions, wet and dry deposition in the Arctic. In the models, transport of BC to the Arctic from lower latitudes is the major BC source for this region while Arctic emissions are very small. All models simulated a similar annual cycle of BC transport from lower latitudes to the Arctic, with maximum transport occurring in July. Substantial differences were found in simulated BC burdens and vertical distributions, with CanAM (NorESM) producing the strongest (weakest) seasonal cycle. CanAM also has the shortest annual mean residence time for BC in the Arctic followed by SMHI-MATCH, CESM and NorESM. The relative contribution of wet and dry deposition rates in removing BC varies seasonally and is one of the major factors causing seasonal variations in BC burdens in the Arctic. Overall, considerable differences in wet deposition efficiencies in the models exist and are a leading cause of differences in simulated BC burdens. Results from model sensitivity experiments indicate that scavenging of BC in convective clouds acts to substantially increase the overall efficiency of BC wet deposition in the Arctic, which leads to low BC burdens and a more pronounced seasonal cycle compared to simulations without convective BC scavenging. In contrast, the simulated seasonality of BC concentrations in the upper troposphere is only weakly influenced by wet deposition in stratiform (layer) clouds whereas lower tropospheric concentrations are highly sensitive.
Carbon capture remains an integral technology to mitigate pollution from one of the most prevalent greenhouse gases. CO 2 desorption/absorbent regeneration for both solid- and liquid-based systems is widely recognized as an energy-intensive and costly process operation. Consequently, tremendous work was devoted towards developing new absorbents and regeneration processes to promote their economic feasibility for extensive implementation. In this review, we broadly and deeply review more than 10,000 papers and extract the hidden trends of carbon capture and absorbents regeneration in the past few decades, using a novel data-mining analysis technique. We comprehensively analyzed an array of recent absorbent regeneration methods utilized in post-combustion, pre-combustion, carbon capture from industrial point sources, and direct air carbon capture, with an emphasis on sorbent and solvent-based techniques. In conclusion, advanced regeneration methods in these techniques were illustrated and discussed, followed by recommendations for further research efforts.
In 2018, nuclear energy generated 55% of United States’ and one third of the world’s carbon free electricity, making nuclear energy a key tool in efforts to mitigate climate change before 2050. However, the current nuclear technology, light water reactors (LWRs), is limited to 300°C, so it cannot be used to decarbonize industrial process heat which accounts for 12% of US greenhouse gas emissions. High temperature gas reactors (HTGRs) can meet the high temperature demand with carbon free nuclear heat. The estimated cost of HTGRs, such as the Next Generation Nuclear Plant (NGNP), are even higher than state-of-the-art LWRs. In this paper, we expanded our nuclear cost estimating tool to include HTGRs and find that the NGNP overnight capital costs were 32% higher than an advanced LWR per unit capacity. The higher cost will naturally result in larger risk to cost overrun as recently experienced by larger LWRs in western nations. With a design-to-build mindset to minimize cost and construction risk, we introduce the horizontal, compact HTGR (HC-HTGR). The reactor core and steam generator are mounted horizontally on rails and in-line with one another, decreasing the size of the reactor building relative to the power capacity four times when compared to traditional HTGRs. The HC-HTGR reduced overnight civil structure costs by 42%, indirect costs by 38%, and total capital costs by 20% from NGNP. We discussed the required engineering of new systems for the HC-HTGR including vessel supports, the reactor cavity cooling system, and steam generator design. Finally, we estimated the fuel and operations costs of the HC-HTGR, and a survey of low-carbon industrial process heat technology showed the HC-HTGR can deliver a highly competitive levelized cost of heat in the range of $6.13–12.48/GJ.
Coastal wetlands are global hotspots of carbon storage. Marshes, mangroves, and seagrass meadows account for about half of the total marine soil carbon budget and bury carbon at rates roughly equivalent to terrestrial forests despite occupying just 2.5% of Earth’s land area. Coastal wetlands have recently been recognized as important for storing carbon, but the future sink strength and carbon stock stability of these systems is uncertain because global change drivers such as temperature and elevated CO 2 disturb the complex ecology that drives high rates of soil carbon sequestration. The dynamics of coastal wetland carbon pools are not presently represented in earth system models. Our goals are to understand the influence of warming and elevated CO 2 on C cycling and to forecast the stability of tidal wetland soil carbon pools at the terrestrial-aquatic interface. We designed and implemented a novel field manipulation of elevated CO 2 and temperature and operated it from 2016 to 2020. We learned that plant communities and microbial communities respond differently to rising temperature, and that the net effects of these responses means that a modest amount of warming will increase tidal marsh carbon sequestration, while warming above that level will diminish the potential for additional carbon sequestration. In mathematical terms the system showed non-linear responses which are important for building forecast models.
Plants strongly influence soil properties through rhizodeposition, in which exudates diffuse from roots, additional secretions are actively released, and root cells are sloughed into the soil. This contribution by plants of carbon compounds belowground is at the core of soil health, water holding capacity, and the soil carbon storage that pulls carbon dioxide out of the atmosphere. Once in soil, organic matter can bind with minerals such as iron hydroxides, where it can be protected from microbial attack for millenia, preserving very large terrestrial soil carbon pools. However, those same compounds contributed by roots to soil may also destabilize the long-term protective associations of SOM with minerals, making that soil organic matter (SOM) more vulnerable to microbial attack and decomposition. Plant roots thus influence both the buildup and breakdown of soil carbon pools. DOE’s E3SM Land Model (ELM) includes a representation of soil carbon storage on minerals, but the potential vulnerability of SOM–mineral associations to effects of rhizodeposition is not yet represented in ELM. To begin testing for this effect of rhizodeposition on soil carbon storage and decomposition, we worked to develop a novel approach during this TES Exploratory project DE-SC0019142 – we harnessed the power of plant viral infection. We examined whether plant virus infection can serve as a tool to intensify rhizodeposition at the root surface, and therefore possibly intensify mobilization of SOM from minerals making it visible to our analytical techniques. Viral infection is widespread in terrestrial ecosystems; 25-70% of plants have virus infection, yet the influence of such infection on root traits and terrestrial soil carbon dynamics remains largely unexplored. We used two plant hosts: the annual Avena sativa (oats) and the genetically tractable, model grass Brachypodium distachyon. These grasses were infected with the broad host range virus Barley Yellow Dwarf Virus (BYDV) via aphids (Rhopalosiphum padi). BYDV infects at least 150 grass species in agricultural and natural ecosystems, and in previous experiments, oats infected with BYDV had roots that were very sticky to the touch, strongly suggesting that infection altered rhizodeposition. We developed this new experimental approach mostly in a one virus (Barley Yellow Dwarf Virus)–one plant (Avena sativa) system. (Several effects of infection in a Brachypodium-BYDV system were similar in nature to effects on Avena sativa, but were more variable.) In the BYDV-Avena system, we developed protocols for consistently infecting target plants (and avoiding infection of control plants) using aphid caging on leaves. We measured that infected plants exhibited reduced photosynthesis, plant (including root) biomass, and root:shoot ratio, as well as simplified root system architecture. We established procedures for sampling the organic compounds carried specifically in phloem (vascular tissue) of leaves and roots, using aphid stylectomy. We used FTICR-MS, Orbitrap GC-MS, and LC-MS/MS to analyze organic compounds in phloem, liquid around roots of plants grown hydroponically, and pore water around roots in soil, and found differences in the compounds in solution bathing roots when infected and uninfected plants were grown hydroponically. Finally, we synthesized isotopically-labeled mineral–organic matter (MAOM) associations in the lab and developed assays using them in solution and in soil. Assays quantified the extent and rate of mineralization of labeled MAOM that was mobilized by functionally distinct rhizodeposits and then attacked by microbes. Two mechanisms for MAOM mobilization emerged, with distinct dynamics. During “direct” mobilization, rhizodeposits such as the strong ligand oxalic acid could drive rapid dissolution of minerals, mobilizing MAOM. During “indirect” mobilization, rhizodeposits such as the simple sugar glucose did not attack minerals directly but instead intensified microbial activity, which led to mobilization via changes in e.g. pH, Eh, and microbial metabolite production (Li et al. 2021). Mechanistic understanding derived from these data and our ongoing experiments using these techniques will inform future development of ELM. Plant roots not only contribute newly fixed organic compounds to soils, but also root activities can drive mineralization of the carbon and nutrients mobilized off minerals via “indirect” or “direct” mechanisms. Using viral infection as a new tool, ongoing combined experimentation and modeling will explore the strength and larger-scale significance of the cascade of processes from rhizodeposition to MAOM mobilization for soil carbon storage and nutrient cycling in terrestrial ecosystems. And if viral infection leads quite generally to “sticky roots”, our perception of the potential importance of prevalent virus infection in terrestrial landscapes will be transformed.
The Faraday method has been used to measure the diamagnetic susceptibilities of small bundles of aligned carbon fibers of different types at room temperature. It was found that the tensor trace susceptibility of the fibers varies systematically over the range 0.8-20 (in units of -10 to the -6th emu/g) as a function of precursor type and processing history. The susceptibility increases, in general, with increasing nominal treatment temperature and hot stretching, and with increasing tensile elastic modulus. The anisotropy ratio of fibers increases approximately linearly with tensile elastic modulus for all fibers from about 1 for a modulus of about 70 GN/sq m to about 22 for a modulus of 700 GN/sq m in air, and is quantitatively consistent with the layer-plane orientation textures determined by X-ray diffraction when appropriate values of the crystallite principal susceptibilities are used.
A comprehensive, merged data set of trace gases (NO, NO 2 , CO 2 , CH 4 and O 3 ) along with has been tabulated and subjected to meticulous quality assurance and quality control (QA/QC). The merged data set is being submitted to the ARM website dedicated to the Green Ocean Experiment: https://www.arm.gov/research/campaigns/amf2014goamazon Analysis using the final data set is in progress to determine the magnitudes of the fluxes for CH 4 , H 2 O, CO 2 , O 3 , NO x , sensible and latent heat, momentum, and their seasonal variations. Here are summary statements, from the discussion above: Total NO fluxes were calculated following Keller et al., 1986. A vertical gradient is established in the mixing ratio of NO because it is emitted at the soil surface and mixed upward in the atmosphere (see above). Once in the atmosphere, the NO reacts rapidly with O 3 to produce NO 2 (NO + O 3 → NO 2 + O 2 ). Therefore, if the vertical profiles of the mixing ratios of NO and O 3 are known, the surface flux of NO may be determined. If any other reaction removes NO (e.g., deposition on leaves), FNO should estimate the lower limit to the NO flux from the soil in this forest. Our preliminary results show fluxes of NO averaged 133 x 10 9 molecules cm -2 s -1 , a factor of 4 higher than fluxes previously observed in white sand soils in the Amazon, and a factor of 3 to 14 higher than fluxes observed for yellow clay soils (Bakwin et al., 1990 and references therein). The soil in the km 67 site is predominately oxisol with pockets of sandy ultisols, both having low reduced nutrient contents, mostly due to efficient microorganism decomposition and acid leaching by rain water. Oxisols contain both oxidized and reduced forms of nitrogen, of which concentrations vary independently of leaching (Jordan et al., 1982), with most part of the cycling processes occurring in the top layers. Methane fluxes showed no statistical difference between 2015 wet and dry seasons, and the forest at this site appear to be a methane sink throughout the year. The vertical profiles suggest that if a methane source exists in this forest, it might be in the canopy. Next steps include modeling and analysis using the Master Chemical Mechanism (Jenkin et al., 1997; Saunders et al., 2003 (A/B); http://mcm.leeds.ac.uk/MCM/) and the Ecosystem Demography-2 (ED-2) model. A final manuscript with the results from this work is in preparation and expected to be submitted for publication within the next several months. Publications to date are listed below.
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