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At least 19 records

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DOE OSTI2024

Reduction of CO to Methanol with Recyclable Organic Hydrides

We report the reaction steps for the selective conversion of a transition metal carbonyl complex to a hydroxymethyl complex that releases methanol upon irradiation with visible light have been successfully quantified in acetonitrile solution with dihydrobenzimidazole organic hydride reductants. Dihydrobenzimidazole reductants have been shown to be inactive toward H 2 generation in the presence of a wide range of proton sources and have been regenerated electrochemically or photochemically. Specifically, the reaction of cis-[Ru(bpy) 2 (CO) 2 ] 2+ (bpy = 2,2'-bipyridine) with one equivalent of a dihydrobenzimidazole quantitatively yields a formyl complex, cis-[Ru(bpy) 2 (CO)(CHO)] + , and the corresponding benzimidazolium on a seconds time scale. Kinetic experiments revealed a first-order dependence on the benzimidazole hydride concentration and an unusually large kinetic isotope effect, inconsistent with direct hydride transfer and more likely to occur by an electron transfer-proton-coupled electron transfer (EΤ-PCET) or related mechanism. Further reduction/protonation of cis-[Ru(bpy) 2 (CO)(CHO)] + with two equivalents of the organic hydride yields the hydroxymethyl complex cis-[Ru(bpy) 2 (CO)(CH 2 OH)] + . Visible light excitation of cis-[Ru(bpy) 2 (CO)(CH 2 OH)] + in the presence of excess organic hydride was shown to yield free methanol. Identification and quantification of methanol as the sole CO reduction product was confirmed by 1 H NMR spectroscopy and gas chromatography. The high selectivity and mild reaction conditions suggest a viable approach for methanol production from CO, and from CO 2 through cascade catalysis, with renewable organic hydrides that bear similarities to Nature's NADPH/NADP + .

14 SOLAR ENERGY↗

DOE OSTI2024

Unraveling iron oxides as abiotic catalysts of organic phosphorus recycling in soil and sediment matrices

In biogeochemical phosphorus cycling, iron oxide minerals are acknowledged as strong adsorbents of inorganic and organic phosphorus. Dephosphorylation of organic phosphorus is attributed only to biological processes, but iron oxides could also catalyze this reaction. Evidence of this abiotic catalysis has relied on monitoring products in solution, thereby ignoring iron oxides as both catalysts and adsorbents. Here we apply high-resolution mass spectrometry and X-ray absorption spectroscopy to characterize dissolved and particulate phosphorus species, respectively. In soil and sediment samples reacted with ribonucleotides, we uncover the abiotic production of particulate inorganic phosphate associated specifically with iron oxides. Reactions of various organic phosphorus compounds with the different minerals identified in the environmental samples reveal up to twenty-fold greater catalytic reactivities with iron oxides than with silicate and aluminosilicate minerals. Importantly, accounting for inorganic phosphate both in solution and mineral-bound, the dephosphorylation rates of iron oxides were within reported enzymatic rates in soils. Our findings thus imply a missing abiotic axiom for organic phosphorus mineralization in phosphorus cycling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Efficient Capture and Release of the Rare-Earth Element Neodymium in Aqueous Solution by Recyclable Covalent Organic Frameworks

Rare-earth elements (REEs) are present in a broad range of critical materials. The development of solid adsorbents for REE capture could enable the cost-effective recycling of REE-containing magnets and electronics. In this context, covalent organic frameworks (COFs) are promising candidates for REE adsorption due to their exceptionally high surface area. Despite having attractive physical properties, COFs are heavily underutilized for REE capture applications due to their limited lifecycle in aqueous acidic environments, as well as synthetic challenges associated with the incorporation of ligands suitable for REE capture. Here, in this work, we show how the Ugi multicomponent reaction can be leveraged to postsynthetically modify imine-based COFs for the introduction of a diglycolic acid (DGA) moiety, an efficient scaffold for REE capture. The adsorption capacity of the DGA-functionalized COF was found to be more than 40 times higher than that of the pristine imine COF precursor and more than four times higher than that of the next-best reported DGA-functionalized solid support. This rationally designed COF has appealing characteristics of high adsorption capacity, fast and efficient capture and release of the REE ions, and reliable recyclability, making it one of the most promising adsorbents for solid–liquid REE ion extractions reported to date.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Data sets for Unraveling Iron Oxides as Abiotic Catalysts of Organic Phosphorus Recycling in Soil and Sediment Matrices

In biogeochemical phosphorus cycling, iron oxide minerals are acknowledged as strong adsorbents of inorganic and organic phosphorus species. The dephosphorylation of organic phosphorus is attributed only to biological processes, but iron oxides could also catalyze this hydrolytic cleavage. Limited evidence of this abiotic catalysis has relied on monitoring inorganic phosphate in solution, thereby ignoring iron oxides as both catalysts and adsorbents. Here we apply high-resolution mass spectrometry and X-ray absorption spectroscopy to characterize dissolved and particulate phosphorus species, respectively. In soil and sediment samples reacted with ribonucleotides, we uncover the abiotic production of particulate inorganic phosphate associated specifically with iron oxides. Experiments with various organic phosphorus compounds revealed up to 12-fold greater catalytic and adsorption reactivities with iron oxides than with the silicate and aluminosilicate minerals identified in the environmental samples. Remarkably, we obtained dephosphorylation rates by the iron oxides that are within reported enzymatic rates in soils. However, phosphorus cycle models do not yet include a quantitative account of the abiotic evolution of inorganic phosphate from organic phosphorus trapped on iron oxides in environmental matrices. Our findings imply a missing abiotic axiom for organic phosphorus mineralization in the phosphorus cycle.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Spatial and temporal characterization of municipal solid waste based on resource recovery pathways

This study presents a two-year, quarterly assessment of MSW across four source sectors (residential, schools, restaurants, and grocery stores) from sixteen sites across five U.S. states. MSW was manually sorted into 27 categories and aggregated into pathway fractions: high-moisture (HM) organics, low-moisture (LM) organics, recyclable (RC) materials, and residuals for disposal. Organics represented 89 % of the MSW stream. The largest fraction was HM organics consisting of food waste (31 %) and yard waste (3 %), with large coefficient of variations (CV), 79 and 278 %, respectively, reflecting high seasonal and site variability that varied significantly (p < 0.01) across sampling periods. The HM fraction showed properties favorable for anaerobic digestion, with moisture content ranging from 56 to 95 % and volatile solids ranges of 86-95 %. In contrast, the LM and RC fractions remained more stable (plastics CV = 41 %; paper CV = 53 %) with heating values up to 26.9 MJ/kg across sources, reflecting suitability for gasification. Microstructural analysis revealed less porosity in residential waste sampled at the landfill, which can influence preprocessing efficiency and microbial accessibility. Pathway informed allocations showed that 35 % of MSW is suitable for anaerobic digestion, 36 % for gasification, and 18 % for recycling, leaving 11 % requiring landfill disposal. These results provide quantitative evidence to determine feedstock allocation, waste-to-energy system design, and the development of data-driven sustainability and resource recovery strategies within a circular bioeconomy.

09 BIOMASS FUELS↗

DOE OSTI2022

Intraligand Charge Transfer Enables Visible‐Light‐Mediated Nickel‐Catalyzed Cross‐Coupling Reactions**

Abstract We demonstrate that several visible‐light‐mediated carbon−heteroatom cross‐coupling reactions can be carried out using a photoactive Ni II precatalyst that forms in situ from a nickel salt and a bipyridine ligand decorated with two carbazole groups (Ni(Czbpy)Cl 2 ). The activation of this precatalyst towards cross‐coupling reactions follows a hitherto undisclosed mechanism that is different from previously reported light‐responsive nickel complexes that undergo metal‐to‐ligand charge transfer. Theoretical and spectroscopic investigations revealed that irradiation of Ni(Czbpy)Cl 2 with visible light causes an initial intraligand charge transfer event that triggers productive catalysis. Ligand polymerization affords a porous, recyclable organic polymer for heterogeneous nickel catalysis of cross‐coupling reactions. The heterogeneous catalyst shows stable performance in a packed‐bed flow reactor during a week of continuous operation.

Cavedon, Cristian↗

DOE OSTI2022

Intraligand Charge Transfer Enables Visible‐Light‐Mediated Nickel‐Catalyzed Cross‐Coupling Reactions**

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Pathways to a net-zero-carbon water sector through energy-extracting wastewater technologies

The energy-consuming and carbon-intensive wastewater treatment plants could become significant energy producers and recycled organic and metallic material generators, thereby contributing to broad sustainable development goals, the circular economy, and the water-energy-sanitation-food-carbon nexus. This review provides an overview of the waste(water)-based energy-extracting technologies, their engineering performance, techno-economic feasibility, and environmental benefits. Here, we propose four crucial strategies to achieve net-zero carbon along with energy sufficiency in the water sector, including (1) improvement in process energy efficiency; (2) maximizing on-site renewable capacities and biogas upgrading; (3) harvesting energy from treated effluent; (4) a new paradigm for decentralized water-energy supply units.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Switchable system for high-salinity brine desalination and fractional precipitation

A saline feed stream flows into a liquid-liquid extraction system; and a volatile organic solvent flows through a main compressor. The compressed volatile organic solvent then flows through a solvent regenerator, which can be a heat exchanger or a combination of a vaporization device and a condenser, to cool the volatile organic solvent. The cooled volatile organic solvent in liquid phase then flows into the liquid-liquid extraction system, where the saline feed stream contacts the volatile organic solvent to selectively extract water from the saline feed stream into the volatile organic solvent, producing a concentrated brine and an organic-rich mixture of water and the volatile organic solvent. The organic-rich mixture flows from the liquid-liquid extraction system into the solvent regenerator, where the organic-rich mixture is heated to produce an organic-rich vapor and desalinated water; and the organic-rich vapor is recycled as volatile organic solvent back into the liquid-liquid extraction system.

Wilson, Aaron D.↗

DOE OSTI2023

Biological carbon pump estimate based on multidecadal hydrographic data

The transfer of photosynthetically produced organic carbon from surface to mesopelagic waters draws carbon dioxide from the atmosphere. However, current observation-based estimates disagree on the strength of this biological carbon pump (BCP). Earth system models (ESMs) also exhibit a large spread of BCP estimates, indicating limited representations of the known carbon export pathways. Here we use several decades of hydrographic observations to produce a top-down estimate of the strength of the BCP with an inverse biogeochemical model that implicitly accounts for all known export pathways. Our estimate of total organic carbon (TOC) export at 73.4 m (model euphotic zone depth) is 15.00 ± 1.12 Pg C year –1 , with only two-thirds reaching 100 m depth owing to rapid remineralization of organic matter in the upper water column. Partitioned by sequestration time below the euphotic zone, τ, the globally integrated organic carbon production rate with τ > 3 months is 11.09 ± 1.02 Pg C year –1 , dropping to 8.25 ± 0.30 Pg C year –1 for τ > 1 year, with 81% contributed by the non-advective-diffusive vertical flux owing to sinking particles and vertically migrating zooplankton. Nevertheless, export of organic carbon by mixing and other fluid transport of dissolved matter and suspended particles remains regionally important for meeting the respiratory carbon demand. Here, the temperature dependence of the sequestration efficiency inferred from our inversion suggests that future global warming may intensify the recycling of organic matter in the upper ocean, potentially weakening the BCP.

58 GEOSCIENCES↗

DOE OSTI2024

Phosphorus recycling by mineral-catalyzed ribonucleotide cleavage on iron and manganese oxides

Abstract Phosphorus is an essential element influencing both food security via plant fertilization, and water pollution through excessive phosphorus use, yet the phosphorus cycle in ecosystems is poorly known. In particular, beyond adsorption, the role of iron and manganese oxides in catalyzing the abiotic dephosphorylation of biomolecules is debated. Here, we studied the reactions of ribonucleotides, containing different phosphate bonding, with goethite, hematite, and birnessite. We employed both high-resolution mass spectrometry of solution species and molecular modeling simulations of ribonucleotide-mineral complexes. Results disclose an up to fivefold preferential hydrolytic cleavage of a phosphoanhydride bond over a phosphoester bond, indicating that mineral-catalyzed reactions reflect the hierarchy reported for the activity of phosphatase enzymes. The fourfold higher catalytic reactivity of goethite and birnessite versus hematite is explained by mineral-specific binding rather than surface area differences. Corresponding simulated adsorbate conformations at the water–mineral interfaces are proposed. Overall, our findings provide new insights on the catalytic recycling of organic phosphorus species by mineral oxides.

58 GEOSCIENCES↗

DOE OSTI2023

A critical review of existing and emerging technologies and systems to optimize solid waste management for feedstocks and energy conversion

Solid waste generation and its accumulation is increasing at an alarming pace due to population growth and urbanization posing severe risks to health, safety, and natural ecosystems. Herein this review strategically addresses the challenges and solutions to increasing the sustainability footprint of solid waste management (SWM) systems by revealing multipronged approaches that reduce solid waste and handling costs while generating revenue and reducing greenhouse gas and related emissions. For example, the United States sends ~150 million tons of waste to landfills, which is composed of over 75% organic and recyclable materials having a potential to be diverted to alternative scenarios. The emergence of an automated upstream and downstream sorting process for solid waste to increase material diversion from landfills is a promising approach for creating sustainable SWM. The utilization of artificial-intelligence-enabled smart and automated systems at the home and industrial scales, comprehensive public re-education including awareness of the adverse effects of landfilled waste on the ecosystem, and more eco-friendly product development are required to significantly reduce landfills and their negative footprint.

09 BIOMASS FUELS↗

DOE OSTI2023

Climate-driven tradeoffs between landscape connectivity and the maintenance of the coastal carbon sink

Abstract Ecosystem connectivity tends to increase the resilience and function of ecosystems responding to stressors. Coastal ecosystems sequester disproportionately large amounts of carbon, but rapid exchange of water, nutrients, and sediment makes them vulnerable to sea level rise and coastal erosion. Individual components of the coastal landscape (i.e., marsh, forest, bay) have contrasting responses to sea level rise, making it difficult to forecast the response of the integrated coastal carbon sink. Here we couple a spatially-explicit geomorphic model with a point-based carbon accumulation model, and show that landscape connectivity, in-situ carbon accumulation rates, and the size of the landscape-scale coastal carbon stock all peak at intermediate sea level rise rates despite divergent responses of individual components. Progressive loss of forest biomass under increasing sea level rise leads to a shift from a system dominated by forest biomass carbon towards one dominated by marsh soil carbon that is maintained by substantial recycling of organic carbon between marshes and bays. These results suggest that climate change strengthens connectivity between adjacent coastal ecosystems, but with tradeoffs that include a shift towards more labile carbon, smaller marsh and forest extents, and the accumulation of carbon in portions of the landscape more vulnerable to sea level rise and erosion.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Fungi and viruses as important players in microbial mats

ABSTRACT Microbial mats are compacted, surface-associated microbial ecosystems reminiscent of the first living communities on early Earth. While often considered predominantly prokaryotic, recent findings show that both fungi and viruses are ubiquitous in microbial mats, albeit their functional roles remain unknown. Fungal research has mostly focused on terrestrial and freshwater ecosystems where fungi are known as important recyclers of organic matter, whereas viruses are exceptionally abundant and important in aquatic ecosystems. Here, viruses have shown to affect organic matter cycling and the diversity of microbial communities by facilitating horizontal gene transfer and cell lysis. We hypothesise fungi and viruses to have similar roles in microbial mats. Based on the analysis of previous research in terrestrial and aquatic ecosystems, we outline novel hypotheses proposing strong impacts of fungi and viruses on element cycling, food web structure and function in microbial mats, and outline experimental approaches for studies needed to understand these interactions.

Carreira, Cátia↗

DOE OSTI2025

CACTUS: CO 2 Aerogel Capture Towards Utilization and Sequestration

The CACTUS project aimed to develop a novel solid sorbent and sorption module prototype for direct air capture (DAC) of carbon dioxide, by a moisture-swing adsorption (MSA) mechanism. Because MSA uses changes in humidity, not temperature to switch the sorbent from capturing CO 2 to releasing concentrated CO 2 it is > 4X more energy-efficient than the thermal swing process. The goal was to develop a sorbent with a CO 2 capture capacity of 1 mmol CO 2 /g sorbent (or 0.75 mmol CO 2 /g structured sorbent), at a projected scaled cost of < $\$$15/kg sorbent and demonstration of a path to < $\$$100/ton CO 2 . At the end of the project, we achieved 0.8 mmol CO 2 /g sorbent powders, 0.37 mmol CO 2 /g structured sorbent (50% of target), at a projected cost of $\$$29/kg sorbent and an estimated cost of $\$$160/ton CO 2 . The key innovation was SRI’s patented polymer aerogel synthesis platform, which was adapted to produce a nanoporous aerogel with a high density of CO 2 -adsorbing quaternary ammonium groups. This research discovered a new ammonium polymer sorbent and identified a chemical path for its fabrication. The new process solved the monomer immiscibility challenge encountered with the initial method (ammonium is hydrophilic and the crosslinker is hydrophobic). The team fabricated structured sorbent sheets consisting of a non-woven porous substrate impregnated with ammonium polymer and demonstrated its operation in custom made breakthrough test setup MSA DAC built at SRI, and which operates similarly to the envisioned large-scale CO 2 capture plant, to provide data for techno-economic analysis (TEA). TEA sensitivity analysis indicated that ∼$\$$100/ton CO 2 can be achieved if the target capacity of 0.75 mmol CO 2 /g structured sorbent is met. Also identified routes to decrease sorbent manufacturing cost to ∼$\$$19/kg by reducing amounts and recycling the organic solvents. More work is needed on transitioning process manufacturing from powders (which showed a capacity of up to 0.8 mmol/g sorbent) to structured sheets which showed a capacity of 0.37 mmol CO 2 /g structured sorbent (or 0.44 mmol/g sorbent if one excludes the inert porous substrate). This is likely due to different micro/nano-structure of the sorbent and material processing constraints at the laboratory scale. Sorbent cycling studies (> 100 cycles) are needed to investigate its performance stability over time.

99 GENERAL AND MISCELLANEOUS↗

DOE OSTI2026

Green Era Anaerobic Digester

Green Era Educational NFP constructed and commissioned the Green Era Renewable Energy & Urban Farming Campus in Chicago’s Auburn Gresham neighborhood. The project transformed a long-vacant brownfield site into a commercial-scale anaerobic digestion facility that converts food waste into renewable natural gas and nutrient-rich material for agricultural use. The facility can process up to 80,000 wet tons of food waste annually and supports approximately 15 permanent jobs while advancing food waste diversion, renewable energy production, nutrient recovery and community revitalization.

03 NATURAL GAS↗

DOE OSTI2020

Outdoor Home Gardener Preferences for Environmental Attributes in Gardening Supplies and Use of Ecofriendly Gardening Practices

Home gardeners’ concerns for the environment are expressed both in the ecofriendly gardening practices they use and in environmental attributes they prefer in the gardening products they purchase. This study uses data from a 2018 survey of 601 Tennessee outdoor home gardeners and a multiple indicators multiple causes (MIMIC) model to illustrate how outdoor home gardener demographics, expenditures, information use, and attitudes influence use of ecofriendly gardening practices and preferences for environmental attributes in home gardening supplies. Practices considered include planting pollinator plants, using rainwater collectors, composting, recycling gardening supplies packaging, using organic gardening methods, and use of soil testing. Gardening supply product attributes include decreased need for fertilizer, pesticides, and water; native plant species; organically produced products; and recyclable packaging. The most widely used practice is recycling gardening supplies packaging, and the least used is soil testing. Gardeners with a greater propensity to use the six gardening practices include male, college graduates, who spend relatively more of their income on gardening supplies, and consider themselves as being knowledgeable about environmental issues. The gardening supply product attribute most widely considered as important is decreased need for pesticides, and least widely considered as important are native species and organically produced. Gardeners more likely to prefer the six gardening supply product attributes include older gardeners, who seek other gardeners for information, and who perceived themselves as being knowledgeable about the environment. This same group likes to grow their own food and feels responsibility for protecting the environment for future generations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Phosphorus Recycling from Ribonucleotide Structures by Iron Oxide Minerals

In this research, we combined experimental and molecular modeling to obtain a fundamental understanding required to evaluate and predict the role of three natural iron oxides minerals (ferrihydrite, goethite, and hematite) in recycling phosphorus from organic matter, particularly ribonucleotides.

58 GEOSCIENCES↗