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DOE OSTI2020

Fine-root dynamics vary with soil depth and precipitation in a lown-utrient tropical forest in the Central Amazonia

A common assumption in tropical ecology is that root systems respond rapidly to climatic cues but that most of that response is limited to the uppermost layer of the soil, with relatively limited changes in deeper layers. However, this assumption has not been tested directly, preventing models from accurately predicting the response of tropical forests to environmental change. We measured seasonal dynamics of fine roots in a Central Amazonia mature forest using minirhizotrons to 90 cm depth, which were calibrated with fine roots extracted from soil cores. Root productivity and mortality in superficial soil layers were positively correlated with precipitation, whereas root standing length was greater during the dry periods at the deeper layers. Contrary to historical assumptions, a large fraction of fine-root standing biomass (46%) and productivity (41%) were found in soil layers deeper than 30 cm. Furthermore, root turnover decreased linearly with soil depth. Our findings demonstrate a strong relationship between fine-root dynamics and precipitation regimes in Central Amazonia. Our results also emphasize the importance of deep roots for accurate estimates of primary productivity and the interaction between roots and carbon, water, and nutrients.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Coupled Biotic-Abiotic Processes Control Biogeochemical Cycling of Dissolved Organic Matter in the Columbia River Hyporheic Zone

A critical component of assessing the impacts of climate change on watershed ecosystems involves understanding the role that dissolved organic matter (DOM) plays in driving whole ecosystem metabolism. The hyporheic zone—a biogeochemical control point where ground water and river water mix—is characterized by high DOM turnover and microbial activity and is responsible for a large fraction of lotic respiration. Yet, the dynamic nature of this ecotone provides a challenging but important environment to parse out different DOM influences on watershed function and net carbon and nutrient fluxes. We used high-resolution Fourier-transform ion cyclotron resonance mass spectrometry to provide a detailed molecular characterization of DOM and its transformation pathways in the Columbia river watershed. Samples were collected from ground water (adjacent unconfined aquifer underlying the Hanford 300 Area), Columbia river water, and its hyporheic zone. The hyporheic zone was sampled at five locations to capture spatial heterogeneity within the hyporheic zone. Our results revealed that abiotic transformation pathways (e.g., carboxylation), potentially driven by abiotic factors such as sunlight, in both the ground water and river water are likely influencing DOM availability to the hyporheic zone, which could then be coupled with biotic processes for enhanced microbial activity. The ground water profile revealed high rates of N and S transformations via abiotic reactions. The river profile showed enhanced abiotic photodegradation of lignin-like molecules that subsequently entered the hyporheic zone as low molecular weight, more degraded compounds. While the compounds in river water were in part bio-unavailable, some were further shown to increase rates of microbial respiration. Together, river water and ground water enhance microbial activity within the hyporheic zone, regardless of river stage, as shown by elevated putative amino-acid transformations and the abundance of amino-sugar and protein-like compounds. This enhanced microbial activity is further dependent on the composition of ground water and river water inputs. Our results further suggest that abiotic controls on DOM should be incorporated into predictive modeling for understanding watershed dynamics, especially as climate variability and land use could affect light exposure and changes to ground water essential elements, both shown to impact the Columbia river hyporheic zone.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Energy efficiency in industrial drying: A hybrid ultrasonic system with a novel dynamic optimization framework

Drying processes are among the most energy-consuming operations in industrial and manufacturing settings, demanding strategic selection, design, and control for enhanced efficiency. Advancing drying technologies is critical for improving sustainability, lowering energy use, reducing carbon emissions, and minimizing waste. This study explores two innovative strategies aimed at transforming drying processes into sustainable, low-carbon systems by reducing energy consumption, minimizing waste, and maintaining a strong emphasis on preserving product quality. The first strategy showcases a sub-pilot scale hybrid ultrasonic-convective dryer for agrifood products. This technology, powered by electricity (process electrification), integrates non-thermal ultrasonic dehydration with convective heating and is presented as a sustainable and energy-efficient solution that enhances eco-friendly practices. The second strategy involves introducing and implementing a novel, multiobjective, mixed integer dynamic optimization technique to determine the optimal time-dependent process parameter values for the drying operation. This optimization technique yields operating conditions that are piecewise constant in time aiming to maximize the energy efficiency of the hybrid ultrasonic-convective dryer while ensuring strict adherence to product quality constraints. By adopting the hybrid ultrasonic-convective dryer, a notable 35% improvement in energy efficiency was achieved compared to conventional hot-air drying systems for drying apple slices. The proposed optimization framework further enhanced energy efficiency by nearly 14% over the most efficient process on the identical testbed, under static operating conditions. The reported enhancements have been experimentally validated. Regarding drying time (thereby improving production yield), the developed hybrid ultrasonic-convective dryer demonstrates as much as a 41% reduction in total processing time, which is further optimized by an additional 10% using our proposed optimization framework. The research outcomes have profound implications for the design and operation of drying systems, encompassing crucial aspects such as process electrification, cost-effectiveness, energy savings, time efficiency, product yield, product quality, and process automation.

Dynamic optimization↗

DOE OSTI2025

Effects of Particle Mixing and Gravitational Settling on Charge Transport in Carbon Flow-Electrode Cells

Flowable carbon slurries are actively studied and under development for charge transport in various electrochemical systems including flow capacitors, capacitive deionization cells, semi-solid flow batteries, and lithium extraction. However, much less is known about in operando slurry flow dynamics and their corresponding effect on charge transport. We performed an experimental study of mixing and settling dynamics of slurry electrodes within an electrochemical flow cell during continuous operations. The electrochemical cell consisted of two horizontal co-flowing channels, separated by a cation-exchange membrane (CEM). Here we used high-speed optical imaging of planes parallel to gravity and simultaneous electrochemical measurements. At low flow rates, dense yet dynamic particle beds formed on the bottom electrode in each channel, which unexpectedly yielded the highest currents. This approach enables the operation of the flow cell at low system-average particle concentrations while leveraging gravity-driven particle settling to locally enhance carbon concentrations precisely at the current collector sites. Conversely, high flow rates were characterized by thin particle beds and well-mixed particle flows. In the latter case, the electrodes in closest proximity (located on either side of the CEM) achieved a current higher than the other electrode pairs. The observations have implications for slurry control and electrode designs in electrochemical systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Effect of fluctuating redox conditions on trace metal release from wetland soils from South Carolina and stream sediments from Tennessee

Natural aquatic systems undergo fluctuating redox conditions due to microbial activity, varying water saturation levels, and nutrients dynamics. With fluctuating oxic and anoxic conditions, trace metals can be mobilized or sequestered in response to changes in iron and sulfur speciation and the concentrations and lability of organic carbon. We conducted a systematic laboratory-based microcosm study to examine the effect of redox fluctuations on trace metal mobility in samples collected from two different natural aquatic systems: riparian wetlands and a stream. We incubated water-saturated soils under three cycles of anoxic-oxic conditions (τanoxic:τoxic = 3) spanning 24 days and monitored the change in dissolved and bioavailable metal (copper (Cu), nickel (Ni), zinc (Zn), cobalt (Co), iron (Fe), and manganese (Mn)) concentrations. The dataset includes the results of the variation in metal concentrations due to redox fluctuations in wetland soils and stream sediments. Additionally, the variation in the bioavailable concentration of metals obtained using passive samplers based on diffuse gradient in thin-films technique is included in the dataset. We have also reported the change in the pH values and dissolved oxygen concentrations in the microcosms during the entire study of 24 days. The dataset also contains the dissolved organic carbon and sulfate concentrations, and the data on fractions of metals bound to reducible and oxidizable phases. For materials from both the wetlands and the stream, anoxic conditions favored Co and Zn release, which corresponded with the reductive dissolution of iron oxides. In contrast, dissolved Cu concentrations increased under oxic conditions for both sites and correlated positively with the release of sulfate. In wetland soils, dissolution of Fe (hydr)oxides increased Ni solubility; however, in stream sediments, Ni release occurred when sulfides or organic matter were oxidized. For stream sediments, each subsequent redox cycle increased the bioavailability of trace metals. Upon redox fluctuations in wetland soils, the bioavailability of Zn and Cu increased, whereas bioavailable Ni and Co decreased. This study illustrates that different trace metals display distinct bioavailability patterns during oxic-anoxic fluctuations in natural environments. The biogeochemical cycling of carbon and nitrogen in systems with redox fluctuations may be influenced by these patterns in trace metal availability in addition to the availability of electron donors and acceptors.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Enhancing CO 2 Transport Across a PEEK‐Ionene Membrane and Water‐Lean Solvent Interface

Abstract Efficient direct air capture (DAC) of CO 2 will require strategies to deal with the relatively low concentration in the atmosphere. One such strategy is to employ the combination of a CO 2 ‐selective membrane coupled with a CO 2 capture solvent acting as a draw solution. Here, the interactions between a leading water‐lean carbon‐capture solvent, a polyether ether ketone (PEEK)‐ionene membrane, CO 2 , and combinations were probed using advanced NMR techniques coupled with advanced simulations. We identify the speciation and dynamics of the solvent, membrane, and CO 2 , presenting spectroscopic evidence of CO 2 diffusion through benzylic regions within the PEEK‐ionene membrane, not spaces in the ionic lattice as expected. Our results demonstrate that water‐lean capture solvents provide a thermodynamic and kinetic funnel to draw CO 2 from the air through the membrane and into the bulk solvent, thus enhancing the performance of the membrane. The reaction between the carbon‐capture solvent and CO 2 produces carbamic acid, disrupting interactions between the imidazolium (Im + ) cations and the bistriflimide anions within the PEEK‐ionene membrane, thereby creating structural changes through which CO 2 can diffuse more readily. Consequently, this restructuring results in CO 2 diffusion at the interface that is faster than CO 2 diffusion in the bulk carbon‐capture solvent.

Walter, Eric D.↗

DOE OSTI2024

Disturbance–diversity relationships of microbial communities change based on growth substrate

Disturbance events can impact ecological community dynamics. Understanding how communities respond to disturbances and how those responses can vary is a challenge in microbial ecology. In this study, we grew a previously enriched specialized microbial community on either cellulose or glucose as a sole carbon source and subjected them to one of five different disturbance regimes of varying frequencies ranging from low to high. Using 16S rRNA gene amplicon sequencing, we show that the community structure is largely driven by substrate, but disturbance frequency affects community composition and successional dynamics. When grown on cellulose, bacteria in the genera Cellvibrio, Lacunisphaera, and Asticcacaulis are the most abundant microbes. However, Lacunisphaera is only abundant in the lower disturbance frequency treatments, while Asticcacaulis is more abundant in the highest disturbance frequency treatment. When grown on glucose, the most abundant microbes are two Pseudomonas sequence variants and a Cohnella sequence variant that is only abundant in the highest disturbance frequency treatment. Communities grown on cellulose exhibited a greater range of diversity (1.95–7.33 Hill 1 diversity) that peaks at the intermediate disturbance frequency treatment or one disturbance every 3 days. Communities grown on glucose, however, ranged from 1.63 to 5.19 Hill 1 diversity with peak diversity at the greatest disturbance frequency treatment. These results demonstrate that the dynamics of a microbial community can vary depending on substrate and the disturbance frequency and may potentially explain the variety of diversity–disturbance relationships observed in microbial systems.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

Defect formation and bending properties in graphite under He atom implantation investigated by molecular dynamics method

The formation and evolution of radiation defects and their effects on bending property of a single graphite under low energy helium atom implantation have been studied at atomic scale through molecular dynamics simulations. Various simple interstitial and vacancy defects are observed during the implantation process, which is a function of incident energy and cross section of helium-carbon interaction. Large defects are observed after continuous helium atom implantations. The effects of incident energy on the density, size and distribution of defects are analyzed in detail. Furthermore, the kinetic evolution process of radiation defects at different annealing temperatures have also been simulated, including the migration, aggregation, transformation, coalescence, and self-healing. Here, the large defect clusters, crossing several carbon layers, have been confirmed to be the primary reasons that affect the bending property of graphite. All these results provide a new understanding for further applications of graphite in nuclear reactors.

Atomic implantation↗

DOE OSTI2022

Tropical extreme droughts drive long-term increase in atmospheric CO 2 growth rate variability

The terrestrial carbon sink slows the accumulation of carbon dioxide (CO 2 ) in the atmosphere by absorbing roughly 30% of anthropogenic CO 2 emissions, but varies greatly from year to year. The resulting variations in the atmospheric CO 2 growth rate (CGR) have been related to tropical temperature and water availability. The apparent sensitivity of CGR to tropical temperature ( ${{{{{{\rm{\gamma }}}}}}}_{{{{{{\rm{CGR}}}}}}}^{{{{{{\rm{T}}}}}}}$ ) has changed markedly over the past six decades, however, the drivers of the observation to date remains unidentified. Here, we use atmospheric observations, multiple global vegetation models and machine learning products to analyze the cause of the sensitivity change. We found that a threefold increase in ${{{{{{\rm{\gamma }}}}}}}_{{{{{{\rm{CGR}}}}}}}^{{{{{{\rm{T}}}}}}}$ emerged due to the long-term changes in the magnitude of CGR variability (i.e., indicated by one standard deviation of CGR; STD CGR ), which increased 34.7% from 1960-1979 to 1985-2004 and subsequently decreased 14.4% in 1997-2016. We found a close relationship (r 2 = 0.75, p < 0.01) between STD CGR and the tropical vegetated area (23°S – 23°N) affected by extreme droughts, which influenced 6-9% of the tropical vegetated surface. A 1% increase in the tropical area affected by extreme droughts led to about 0.14 Pg C yr -1 increase in STD CGR . The historical changes in STD CGR were dominated by extreme drought-affected areas in tropical Africa and Asia, and semi-arid ecosystems. The outsized influence of extreme droughts over a small fraction of vegetated surface amplified the interannual variability in CGR and explained the observed long-term dynamics of ${{{{{{\rm{\gamma }}}}}}}_{{{{{{\rm{CGR}}}}}}}^{{{{{{\rm{T}}}}}}}$ .

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Intrinsic and Extrinsic Factors Influencing the Dynamics of VO 2 Mott Oscillators

Oscillatory devices have gained significant interest recently as key components of computing systems based on biomimetic neuronal spiking. An understanding of the time scales underlying the spiking is essential for engineering fast, controllable, low energy devices. However, we find that the intrinsic dynamics of these devices are difficult to properly characterize, as they can be heavily influenced by the external circuitry used to measure them. Here we demonstrate these challenges using a VO 2 Mott oscillator with a sub-100 nm effective size, achieved using a nanogap cut in a metallic carbon nanotube electrode. Given the nanoscale thermal volume of this device, it would be expected to exhibit rapid oscillations. However, due to external parasitics present within commonly used current sources, we see orders of magnitude slower dynamics. Here, we outline methods for determining when measurements are dominated by extrinsic factors and discuss the operating conditions under which intrinsic oscillation frequencies may be observed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

BESS-STAIR: a framework to estimate daily, 30m, and all-weather crop evapotranspiration using multi-source satellite data for the US Corn Belt

Abstract. With increasing crop water demands and drought threats, mapping andmonitoring of cropland evapotranspiration (ET) at high spatial and temporalresolutions become increasingly critical for water management andsustainability. However, estimating ET from satellites for precise waterresource management is still challenging due to the limitations in bothexisting ET models and satellite input data. Specifically, the process of ETis complex and difficult to model, and existing satellite remote-sensing datacould not fulfill high resolutions in both space and time. To address theabove two issues, this study presents a new high spatiotemporal resolution ETmapping framework, i.e., BESS-STAIR, which integrates a satellite-drivenwater–carbon–energy coupled biophysical model, BESS (Breathing Earth SystemSimulator), with a generic and fully automated fusion algorithm, STAIR(SaTallite dAta IntegRation). In this framework, STAIR provides daily 30'mmultispectral surface reflectance by fusing Landsat and MODIS satellite datato derive a fine-resolution leaf area index and visible/near-infrared albedo,all of which, along with coarse-resolution meteorological and CO 2 data, are used to drive BESS to estimate gap-free 30 m resolution daily ET.We applied BESS-STAIR from 2000 through 2017 in six areas across the US CornBelt and validated BESS-STAIR ET estimations using flux-tower measurementsover 12 sites (85 site years). Results showed that BESS-STAIR daily ETachieved an overall R2=0.75, with root mean square error RMSE=0.93 mm d -1 and relative error RE =27.9 % when benchmarkedwith the flux measurements. In addition, BESS-STAIR ET estimations capturedthe spatial patterns, seasonal cycles, and interannual dynamics well indifferent sub-regions. The high performance of the BESS-STAIR frameworkprimarily resulted from (1) the implementation of coupled constraints onwater, carbon, and energy in BESS, (2) high-quality daily 30 m data from theSTAIR fusion algorithm, and (3) BESS's applicability under all-skyconditions. BESS-STAIR is calibration-free and has great potentials to be areliable tool for water resource management and precision agricultureapplications for the US Corn Belt and even worldwide given the globalcoverage of its input data.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Interactions with microbial consortia have variable effects in organic carbon and production of exometabolites among genotypes of Populus trichocarpa

Abstract Poplar is a short‐rotation woody crop frequently studied for its significance as a sustainable bioenergy source. The successful establishment of a poplar plantation partially depends on its rhizosphere—a dynamic zone governed by complex interactions between plant roots and a plethora of commensal, mutualistic, symbiotic, or pathogenic microbes that shape plant fitness. In an exploratory endeavor, we investigated the effects of a consortium consisting of ectomycorrhizal fungi and a beneficial Pseudomonas sp. strain GM41 on plant growth (including height, stem girth, leaf, and root growth) and as well as growth rate over time, across four Populus trichocarpa genotypes. Additionally, we compared the level of total organic carbon and plant exometabolite profiles across different poplar genotypes in the presence of the microbial consortium. These data revealed no significant difference in plant growth parameters between the treatments and the control across four different poplar genotypes at 7 weeks post‐inoculation. However, total organic carbon and exometabolite profiles were significantly different between the genotypes and the treatments. These findings suggest that this microbial consortium has the potential to trigger early signaling responses in poplar, influencing its metabolism in ways crucial for later developmental processes and stress tolerance.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

Influence of isoelectronic mass modulation on phonon decay and transport in layered pnictogen-carbon systems

This study systematically investigates the structural, electronic, and thermal transport properties of layered pnictogen–carbon (Pn 2 C 2 ; Pn = P, As, Sb, Bi) monolayers, revealing a profound influence of isoelectronic mass modulation on phonon dynamics and thermal conductivity. Through first-principles calculations and lattice dynamics analysis, we demonstrate that increasing the atomic mass of pnictogens leads to elongated Pn-C bonds, weakened interatomic interactions, and enhanced phonon-phonon scattering, resulting in a dramatic reduction in lattice thermal conductivity (κ). Specifically, κ decreases exponentially from 65.6 W/m-K in P 2 C 2 to an ultralow 0.37 W/m-K in Bi 2 C 2 , driven by suppressed acoustic-optical phonon gaps Δ$^{Γ}_{A-0}$, increased anharmonicity, and reduced phonon lifetimes and group velocities. The transition from semiconducting to metallic behavior in heavier pnictogen-based systems further enhances phonon-electron scattering, contributing to thermal conductivity suppression. Structural analysis highlights the strengthening of out-of-plane C—C bonds and the contraction of C—Pn—C bond angles, which disrupt in-plane phonon transport. Further, these findings establish a design framework for engineering ultralow-κ materials through chemical substitution and structural tuning, offering significant potential for thermoelectric and thermal management applications. This work provides fundamental insights into phonon decay mechanisms and thermal transport in 2D materials, paving the way for advanced phononic and energy-efficient devices.

2D materials↗

DOE OSTI2025

CFD modeling of non-catalytic, partial-oxidation engine reformer for flare mitigation

Flaring associated natural gas is commonly employed in the oil and gas industry to reduce methane (CH 4 ) emissions but generates carbon dioxide (CO 2 ) and harmful pollutants, significantly contributing to air pollution and posing risks to public health. To mitigate this impact, M2X Energy Inc. has developed a small-scale, modular gas-to-methanol system. This system features an engine reformer that performs fuel-rich partial oxidation of wellhead gas to produce syngas—a mixture of carbon monoxide (CO) and hydrogen (H 2 )—followed by a downstream reactor for methanol synthesis. This study focused on computational fluid dynamics (CFD) modeling of the engine reformer to simulate partial oxidation chemistry, predict the rich-burn operating limit, and assess syngas quality, ultimately aiding in design and operational optimization. The CFD model, developed within a Reynolds-Averaged Navier-Stokes (RANS) turbulence framework, incorporated sub-models for turbulent combustion, a chemical mechanism with polycyclic aromatic hydrocarbon (PAH) pathways, and soot emissions to accurately capture the fuel-rich, turbulent jet ignition and combustion processes. Model validation against experimental data showed good agreement across pre- and main-chamber pressures, apparent heat release rates, and exhaust gas concentrations of key species (H 2 , CO, CO 2 , CH 4 ) for varying intake equivalence ratios. Here, the model identified a rich-burn operating limit near a fuel-air equivalence ratio of 2.35, consistent with experimental observations. Furthermore, syngas quality analysis revealed that extending the rich-burn limit through engine reformer optimization could enhance syngas production, contributing to higher methanol synthesis efficiency.

Computational Fluid Dynamics↗

DOE OSTI2022

Pathways of clean energy heating electrification programs for reducing carbon emissions in Northwest China

We report clean energy heating electrification programs provide a promising way to reduce carbon emissions from fossil fuel combustion and consumption. This work studies the cost competitiveness of clean energy heating technologies under three dynamic mechanisms: investment costs, subsidy policies, and operating costs with real data. It provides key insights into the cost competitiveness of the different heating technologies deployed in different areas, as well as their sensitivity to the three dynamic mechanisms. The results show that currently, the distinct heating programs are more cost-efficient in the urban area with existing heating networks. The average payback period of all district clean energy heating programs in the urban area is 14.9 years, while that of the individual clean heating programs is 24.7 years. The individual heating programs are becoming increasingly cost-competitive with the incentive mechanisms, especially the electricity pricing mechanisms. Moreover, individual heating technologies present remarkable advantages on flexibility and sustainability in the long run. According to the technology diffusion model proposed in this paper, the individual clean heating programs will occupy more than 50% of the market share in 2050 under the comprehensive effect of CAPEX, government subsidies, and OPEX. The real-world results and analysis render references to shape the pathway of clean energy heating electrification in Northwest China and other regions with a similar situation.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2024

Structure–Composition Relationships for Mg–Ni and Mg–Fe Olivine

Olivine is a dynamic and important mineral in the crust and mantle with relevance to processes important to climate change technology, such as geologic carbon storage and critical mineral recovery. In this work, we critically evaluated and compiled a new database of olivine diffraction data, lattice parameters, and composition to enable rapid Ni-Mg-Fe olivine composition determination. A compilation of olivine X-ray diffraction data and chemical compositions from both the literature and the International Centre for Diffraction Data (ICDD) powder database was assembled to plot both the forsterite-fayalite and forsterite-liebenbergite solid solution lines. Here we present an expanded dataset to delineate equations and relationships used for quantifying the correlations between olivine lattice parameters and chemical compositions in Mg 2 SiO 4 -Fe 2 SiO 4 (forsterite-fayalite) and Mg 2 SiO 4 -Ni 2 SiO 4 (forsterite-liebenbergite) olivine solid solution series.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Dynamic Bubbling Balanced Proactive CO 2 Capture and Reduction on a Triple-Phase Interface Nanoporous Electrocatalyst

The formation and preservation of the active phase of the catalysts at the triple-phase interface during CO 2 capture and reduction is essential for improving the conversion efficiency of CO 2 electroreduction toward value-added chemicals and fuels under operational conditions. Designing such ideal catalysts that can mitigate parasitic hydrogen generation and prevent active phase degradation during the CO 2 reduction reaction (CO 2 RR), however, remains a significant challenge. Herein, we developed an interfacial engineering strategy to build a new SnO x catalyst by invoking multiscale approaches. This catalyst features a hierarchically nanoporous structure coated with an organic F-monolayer that modifies the triple-phase interface in aqueous electrolytes, substantially reducing competing hydrogen generation (less than 5%) and enhancing CO 2 RR selectivity (~90%). This rationally designed triple-phase interface overcomes the issue of limited CO 2 solubility in aqueous electrolytes via proactive CO 2 capture and reduction. Concurrently, we utilized pulsed square-wave potentials to dynamically recover the active phase for the CO 2 RR to regulate the production of C1 products such as formate and carbon monoxide (CO). This protocol ensures profoundly enhanced CO 2 RR selectivity (~90%) compared with constant potential (~70%) applied at -0.8 V (V vs RHE). We further achieved a mechanistic understanding of the CO 2 capture and reduction processes under pulsed square-wave potentials via in situ Raman spectroscopy, thereby observing the potential-dependent intensity of Raman vibrational modes of the active phase and CO 2 RR intermediates. Finally, this work will inspire material design strategies by leveraging triple-phase interface engineering for emerging electrochemical processes, as technology moves toward electrification and decarbonization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Molecular Tuning of Ether Cosolvent Chemistry for High-Voltage Sodium-Ion Batteries

Ethers as electrolyte cosolvents in sodium-ion batteries (SIBs) provide favorable Na + solvation and interfacial properties, but their low oxidative stability limits their use in high-voltage SIBs. Herein, we address this limitation via molecular tuning of ether cosolvents for high-voltage (4.2 V) hard carbon || NaNi 0.33 Fe 0.33 Mn 0.33 O 2 full cells. Tetrahydropyran (THP) is functionalized with a nitrile group to form tetrahydropyran-4-carbonitrile (THPCN). To delineate the effect of nitrile functionalization and benchmark ether against a conventional carbonate, THP, THPCN, and diethyl carbonate (DEC) are evaluated as cosolvents with ethylene carbonate. Nitrile functionalization lowers the HOMO energy of the ether, extends the electrolyte stability window, and alters Na⁺ solvation. Spectroscopic techniques and molecular dynamics simulations reveal that THPCN exhibits predominantly aggregate-dominated solvation (95.1 %) with weakened Na + -solvent interactions, producing the most anion-rich environment relative to DEC and THP cosolvents. THPCN-modified solvation promotes the formation of highly conductive, fluorine-enriched interphases that suppress parasitic reactions. Pouch full cells with THPCN sustained ~ 600 cycles at 4.2 V, outperforming THP and DEC. Operando gas analysis reveals that THPCN reduces CO 2 generation by 45% and H 2 generation by 30% relative to THP. Furthermore, the findings demonstrate nitrile functionalization as a molecular design strategy to stabilize ethers and enable high-voltage SIBs.

25 ENERGY STORAGE↗