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DOE OSTI2025

Metabolic Redox Coupling Controls Methane Production in Permafrost‐Affected Peatlands Through Organic Matter Quality‐Dependent Energy Allocation

ABSTRACT Permafrost thaw represents one of Earth's largest climate feedback risks, potentially releasing vast carbon (C) stores as greenhouse gases (GHG). However, our ability to predict emissions remains limited by poor understanding of how changing organic matter (OM) composition affects microbial carbon processing. We test a metabolism‐centered redox framework, which views microbial processes as coupled oxidative‐reductive reactions, to mechanistically explain how organic matter metabolite quality controls greenhouse gas production in permafrost‐affected peatland ecosystems. Rather than relying solely on geochemical redox measurements, our approach examines how microbes balance electron flow through metabolic pathways. Using active layer peat (9–19 cm) from contrasting environments (bog and fen), we employed multi‐omics approaches, including metabolomics, metagenomics, and metatranscriptomics, to link OM chemistry to microbial function. Our results reveal distinct dissolved organic matter metabolite composition, with fen systems enriched in compounds with higher substrate quality (low molecular weight (MW) sugars with high H:C ratios and low aromaticity) and bog systems dominated by compounds with lower substrate quality (high MW phenols with lower H:C ratios and higher aromaticity). In fen samples, these sugar‐like compounds correlated with higher oxidative metabolism and methanogenesis, supported by increased glycolysis gene expression. Initially, electrons from increased oxidative metabolism were balanced through nitrate and sulfate reduction, but as these electron acceptors were depleted, methanogenesis increased to maintain redox balance. Fen samples showed rapid degradation of both high‐ and low‐substrate‐quality compounds, suggesting sufficient energy for efficient C cycling. Conversely, bog samples exhibited more polyphenolic compounds, lower glycolysis activity, and higher stress‐related gene expression, suggesting energy was diverted towards cell maintenance under acidic conditions rather than C processing. This approach suggests that predicting greenhouse gas emissions requires an understanding of how organic matter quality shapes microbial energy allocation strategies, providing a mechanistic framework for improving emission predictions from permafrost‐affected peatlands and similar ecosystems.

Biodiversity & Conservation↗

NASA NTRS1986

The energy balance of plasmoids in the solar atmosphere

The properties of an isolated magnetized plasmoid in a nonuniform magnetic field such as arises in stellar atmospheres are studied. The work of Pneuman and Cargill (1985) on the so-called melon-seed effect is extended to include an equation describing the energy balance, so giving a unified picture of the shape, motion, and energetics of the plasmoid. Three treatments of plasmoid energy balance are considered: (1) a polytropic law, (P = about N to the gamma); (2) one in which the plasmoid cools radiatively; and (3) one in which a heating function proportional to the local density balances the radiation. For a gamma = 4/3 polytrope the evolution is self-similar, so that the plasmoid maintains its shape as it moves out from the stellar surface. If gamma is less than 4/3, the final shape is a long thin cigar-shaped body, whereas if gamma is greater than or equal to 4/3, it ultimately becomes self-similar. In cases with radiation and also with heating, the ultimate shape of the plasmoid is determined by whether its gas or magnetic pressure dominate. The former is equivalent to the gamma-less-than-4/3 polytrope, and the latter to the gamma-greater-than-4/3 one. If radiation alone is present, the plasmoid cools rapidly and subsequently evolves self-similarly. If heating balances radiation initially, then the plasmoid heats up as it moves out, but, if the ratio of the transit of time of Alfven waves across it is much less than the radiative cooling time, it ultimately evolves as a gamma = 5/3 polytrope. In each case the plasmoid can be ejected to large distances (several radii) in a stellar atmosphere, for a reasonable choice of surface parameters.

Cargill, P. J.↗

NASA NTRS1979

A temperature dependent fatigue failure criterion for graphite/epoxy laminates

A fatigue failure criterion applicable to composite materials is developed and applied to predict the fatigue behavior of graphite/epoxy laminates with particular emphasis on the influence of temperature. Tensile stress-strain curves and tension-tension fatigue curves for various unidirectional, angle-ply and symmetrically balanced laminates were developed at test temperatures of 25 C, 74 C and 114 C. In general for most laminates a reduction in both static strength and fatigue strength is observed with increasing temperature. This reduction appeared more severe in fatigue loading than in static tensile loading and most severe where the shear stress in the lamina is the dominant failure mode. Through an analytical formulation of shifting functions for the influences of temperature, all fatigue data are shown to be capable of being reduced to a single reference curve at some temperature. Additionally, examples are given which demonstrate the capability of the fatigue failure criterion to predict failure of complex symmetrically balanced laminates from relevant parameters obtained from the observed behavior of unidirectional and angle-ply laminates.

Rotem, A.↗

DOE OSTI2023

Mesospheric temperature and circulation response to the Hunga Tonga-Hunga-Ha'apai volcanic eruption

The Hunga Tonga Hunga-Ha'apai (HTHH) volcanic eruption on 15 January 2022 injected water vapor and SO 2 into the stratosphere. Several months after the eruption, significantly stronger westerlies, and a weaker Brewer-Dobson circulation developed in the stratosphere of the Southern Hemisphere and were accompanied by unprecedented temperature anomalies in the stratosphere and mesosphere. In August 2022, the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) satellite instrument observed record-breaking temperature anomalies in the stratosphere and mesosphere that alternate signs with altitude. Ensemble simulations carried out with the Whole Atmosphere Community Climate Model (WACCM6) indicate that the strengthening of the stratospheric westerlies explains the mesospheric temperature changes. The stronger westerlies cause stronger westward gravity wave drag in the mesosphere. Although the enhanced gravity wave drag is partly balanced by a weakening of planetary wave forcing, the net result is an acceleration of the mesospheric mean meridional circulation. The stronger mesospheric circulation, in turn, plays a dominant role in driving the changes in mesospheric temperatures. This study highlights the impact of large volcanic eruptions on middle atmospheric dynamics and provides insight into their long-term effects in the mesosphere. On the other hand, we could not discern a clear mechanism for the observed changes in stratospheric circulation. In fact, an examination of the WACCM ensemble reveals that not every member reproduces the large changes observed by SABER. We conclude that there is a stochastic component to the stratospheric response to the HTHH eruption.

58 GEOSCIENCES↗

DOE OSTI2025

Sizing and Location Selection of Medium‐Voltage Back‐to‐Back Converters for DER‐Dominated Distribution Systems

Medium‐voltage back‐to‐back (MVB2B) converters can connect two distribution systems and quantifiably transfer power between them. This function can enable the MVB2B converter to exchange distributed energy resource (DER)‐generated power between two systems and bring significant value to enhancing distribution system DER adoption. Our previous work analysed and demonstrated the value MVB2B converter can bring to DER integration. As continuous work, this paper presents a methodology that helps address the MVB2B converter sizing and location selection problem in distribution systems with high DER penetrations. The proposed methodology aims to address three critical problems for MVB2B converter implementation in the real world: (1) which distribution systems are better to be connected, (2) what converter size is appropriate for connecting the distribution systems, and (3) where the optimal connection points are in the systems for connecting the MVB2B converter. The proposed methodology has been demonstrated by case studies that include various scenarios involving distribution systems with different dominated load types and high photovoltaic penetrations. The results demonstrate that selecting the optimal converter size based on net revenue and time of return considerations leads to a balance between maximizing energy savings and minimizing financial payback periods. Furthermore, feeder pair selection based on load profile standard deviation effectively identifies systems that derive the greatest value from MVB2B integration. Finally, an optimized connection point selection approach using a voltage load sensitivity matrix ensures minimal system impact while facilitating efficient power exchange. These findings provide practical insights for the real‐world deployment of MVB2B converters to enhance DER hosting capacity and improve grid resilience.

14 SOLAR ENERGY↗

NASA NTRS1988

Visual field influence on manual roll and pitch stabilization

Human control performance in nulling perceived tilt angles was investigated for combinations of pseudo-random vestibular disturbances and different waveforms of low frequency wide visual field motions. For both roll and pitch axes, subjects tilted the trainer in which they were seated in the direction of field rotation. This visual bias was much stronger for pitch backwards with upward field rotation. Frequency response analysis showed the dominance of visual cues at low frequencies (below 0.06 Hz) and the reliance on vestibular information in the high frequency range for both axes. Models suggest that operator balancing responses at high frequencies are mainly processed by the semicircular canals rather than the otolith organs. The results also suggest that the subject tends to rely less on the otolith organs for pitch perception than for roll.

Huang, J.-K.↗

NASA NTRS2003

Molybdenum Isotopic Composition of Iron Meteorites, Chondrites and Refractory Inclusions

Recent Mo isotopic studies of meteorites reported evidence for differences in isotopic compositions for whole rocks of some primitive and differentiated meteorites relative to terrestrial materials. Enrichments of r- and p-process isotopes of up to 3-4 units (e unit = parts in 10(exp 4) over s-process dominated isotopes are the most prominent features. Certain types of presolar grains show large enrichments in s-process isotopes, however, it was concluded on grounds of mass balance that incomplete digestion of such grains cannot explain the enrichments of r- and p-process isotopes in whole rocks of primitive chondrites. If the reported variability in r- and p-process isotope enrichments reflects the true isotopic characteristics of the whole rocks, the implications are quite profound. It would suggest the presence of large scale Mo isotopic heterogeneity within the solar accretion disk with likely collateral effects for other elements. However, such effects were not found for Ru isotopes, nor for Zr isotopes. Another recent Mo isotopic study by multi collector ICP-MS could not confirm the reported deviations in Allende, Murchison or iron meteorites. Here, we present new results for the Mo isotopic composition of iron meteorites, chondrites and CAIs obtained by negative thermal ionization mass spectrometry (NTIMS). We discuss analytical aspects and the homogeneity of Mo isotopic compositions in solar system materials.

Becker, H.↗

DOE OSTI2021

Photosynthetic adaptation to polar life: Energy balance, photoprotection and genetic redundancy

The persistent low temperature that characterize polar habitats combined with the requirement for light for all photoautotrophs creates a conundrum. The absorption of too much light at low temperature can cause an energy imbalance that decreases photosynthetic performance that has a negative impact on growth and can affect long-term survival. The goal of this review is to survey the mechanism(s) by which polar photoautotrophs maintain cellular energy balance, that is, photostasis to overcome the potential for cellular energy imbalance in their low temperature environments. Photopsychrophiles are photosynthetic organisms that are obligately adapted to low temperature (0⁰- 15 °C) but usually die at higher temperatures (≥20 °C). In contrast, photopsychrotolerant species can usually tolerate and survive a broad range of temperatures (5⁰- 40 °C). First, we summarize the basic concepts of excess excitation energy, energy balance, photoprotection and photostasis and their importance to survival in polar habitats. Second, we compare the photoprotective mechanisms that underlie photostasis and survival in aquatic cyanobacteria and green algae as well as terrestrial Antarctic and Arctic plants. We show that polar photopsychrophilic and photopsychrotolerant organisms attain energy balance at low temperature either through a regulated reduction in the efficiency of light absorption or through enhanced capacity to consume photosynthetic electrons by the induction of O 2 as an alternative electron acceptor. Finally, we compare the published genomes of three photopsychrophilic and one photopsychrotolerant alga with five mesophilic green algae including the model green alga, Chlamydomonas reinhardtii. We relate our genomic analyses to photoprotective mechanisms that contribute to the potential attainment of photostasis. Finally, we discuss how the observed genomic redundancy in photopsychrophilic genomes may confer energy balance, photoprotection and resilience to their harsh polar environment. Primary production in aquatic, Antarctic and Arctic environments is dependent on diverse algal and cyanobacterial communities. Although mosses and lichens dominate the Antarctic terrestrial landscape, only two extant angiosperms exist in the Antarctic. Furthermore, the identification of a single ‘molecular key’ to unravel adaptation of photopsychrophily and photopsychrotolerance remains elusive. Since these photoautotrophs represent excellent biomarkers to assess the impact of global warming on polar ecosystems, increased study of these polar photoautotrophs remains essential.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

Computer Science Research Needs for Parallel Discrete Event Simulation (PDES)

Historically, scientific computing efforts have demonstrated the clear need for, and effective use of, supercomputing with traditional time-stepped simulations. Nevertheless, there are several areas in the mission spaces of the U.S. Department of Energy and other agencies waiting to tap advanced computing research using a different, discrete event style of modeling, simulation, and analysis. These span a wide spectrum of applications including energy grid resilience, urban planning and policy, transportation science, building technologies, emergency response and planning, environmental impact analysis, computational epidemiology, Internet communications, cyber security, and cyber-physical systems, to name only a few. Even within traditional scientific applications, the role of discrete event modes of execution is increasing in the form of new event-based mathematical solvers such as quantized state integration methods and discrete-continuous hybrid system solvers. Co-design of advanced supercomputing hardware systems is another area that exploits discrete event simulation at its core for effective analyses. Complex systems, entity behaviors and interconnections play a significant role in all these applications, which are mapped to large-scale models with discrete event formulations. To make advancements in all the aforementioned scientific areas, many technical aspects need to be more thoroughly studied and deeply understood in parallel discrete event simulation (PDES). The unique dynamics inherent in a discrete event modeling approach, by their very nature, intersect and influence the entire stack of the computing system, including (a) the unique nature of the instruction sets exercised in PDES workloads without a predominance of high-precision floating point operations, (b) virtual time-constrained multi-threaded execution of many logical processes per processor, (c) extremely variable and difficult to predict network traffic characteristics, (d) interfaces and inter-dependencies with machine learning and artificial intelligence codes at higher software layers, and (e) highly challenging load balancing needs, especially in effectively accounting for accelerated/extremely heterogeneous computing in current and future high-performance computing systems. Efficient and accurate parallel execution of PDES workloads is also dominated by challenges in dealing with their asynchronous concurrency fundamentally present at the model level. Conservative synchronization, optimistic/speculative synchronization, and their hybrid schemes open new questions in fundamental computer science with respect to reversibility of computation and prediction (lookahead) of behaviors inherent within model codes. On the implementation front, there are relatively few scalable, general-purpose parallel discrete event simulators in the world, and even fewer have been studied on emerging hardware platforms. To enable scientific advances using PDES, the research needs in computer science must also be pursued and met in the intersection of the algorithmic and hardware-aware aspects of scalable PDES engines. This report is aimed at capturing a computer science-oriented view of this important area of research in PDES, presenting a sample of important applications with their inherent discrete event technology elements. Needs are outlined in core areas of parallel discrete event research as well as cross-cutting directions in computer science research that positively impact scientific advancements across several important application areas. A selection of priority research opportunities in advanced computing for PDES is identified to serve as reference for key research topics and their order of importance for scientific advancements.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2025

Characterizing Seasonal Variation of the Atmospheric Mixing Layer Height Using Machine Learning Approaches

As machine learning becomes more integrated into atmospheric science, XGBoost has gained popularity for its ability to assess the relative contributions of influencing factors in the atmospheric boundary layer height. To examine how these factors vary across seasons, a seasonal analysis is necessary. However, dividing data by season reduces the sample size, which can affect result reliability and complicate factor comparisons. To address these challenges, this study replaces default parameters with grid search optimization and incorporates cross-validation to mitigate dataset limitations. Using XGBoost with four years of data from the atmospheric radiation measurement (ARM) (Southern Great Plains (SGP) C1 site, cross-validation stabilizes correlation coefficient fluctuations from 0.3 to within 0.1. With optimized parameters, the R value can reach 0.81. Analysis of the C1 site reveals that the relative importance of different factors changes across seasons. Lower tropospheric stability (LTS, ~0.53) is the dominant factor at C1 throughout the year. However, during DJF, latent heat flux (LHF, 0.44) surpasses LTS (0.22). In SON, LTS (0.58) becomes more influential than LHF (0.18). Further comparisons among the four long-term SGP sites (C1, E32, E37, and E39) show seasonal variations in relative importance. Notably, during JJA, the differences in the relative importance of the three factors across all sites are lower than in other seasons. This suggests that boundary layer development in the summer is not dominated by a single factor, reflecting a more intricate process likely influenced by seasonal conditions such as enhanced convective activity, higher temperatures, and humidity, which collectively contribute to a balanced distribution of parameter impacts. Furthermore, the relative importance of LTS gradually increases from morning to noon, indicating that LTS becomes more significant as the boundary layer approaches its maximum height. Consequently, the LTS in the early morning in autumn exhibits greater relative importance compared to other seasons. This reflects a faster development of the mixing layer height (MLH) in autumn, suggesting that it is easier to retrieve the MLH from the previous day during this period. The findings enhance understanding of boundary layer evolution and contribute to improved boundary layer parameterization.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1986

Diagnostic analysis of two-dimensional monthly average ozone balance with Chapman chemistry

Chapman chemistry has been used in a two-dimensional model to simulate ozone balance phenomenology. The similarity between regions of ozone production and loss calculated using Chapman chemistry and those computed using LIMS and SAMS data with a photochemical equilibrium model indicate that such simplified chemistry is useful in studying gross features in stratospheric ozone balance. Net ozone production or loss rates are brought about by departures from the photochemical equilibrium (PCE) condition. If transport drives ozone above its PCE condition, then photochemical loss dominates production. If transport drives ozone below its PCE condition, then photochemical production dominates loss. Gross features of ozone loss/production (L/P) inferred for the real atmosphere from data are also simulated using only eddy diffusion. This indicates that one must be careful in assigning a transport scheme for a two-dimensional model that mimics only behavior of the observed ozone L/P.

Stolarski, Richard S.↗

NASA NTRS2000

The Generation of Smooth High Speed Solar Wind From Plume-Interplume Mixing

Ulysses has shown that fast solar wind is extremely smooth, with a variance of less than 5%, in contrast to slow wind with a variance of approximately 30%. Now UVCS has produced the surprising result that the flow speed within coronal holes, the source of fast wind, is not at all smooth. Specifically, Giordano et al. (ApJ, v531, L79-L82, 2000) report that at 1.7 R(sub SUN) the interplume flow speed is typically more than twice the plume flow speed. Other less direct evidence supports this same result, with speeds from less than 300 to over 1000 km/s reported at approximately 5 R(sub SUN). This presents the paradox of how strongly differing plume and interplume flow speeds can exist near the Sun and be absent far from the Sun. The only answer is that plume and interplume material or momentum must be strongly mixed and that the mixing must occur mainly inside 0.3 AU to be consistent with Helios observations of smooth fast wind. Pressure balance structures (PBSs) and He abundance anomalies (Reisenfeld, et al., GRL, v26(13), 1805-1808, 1999) have been identified as interplanetary remnants of plumes, implying momentum mixing is the dominant coronal process. One possible source for plume/interplume momentum mixing is MHD Kelvin-Helmholtz (KH) shear instabilities occurring on the velocity shear interfaces. The velocity shear is a source of free energy and KH fluctuations could, through nonlinear cascade, provide the forcing required for the plasma oscillations (Cranmer, ApJ, v532, 1197-1208, 2000) reported to exist in coronal holes. The physical properties in coronal holes are now sufficiently well known that we can show plume/interplume shear interfaces become unstable to the KH instability at 5 - 10 R(sub SUN). The KH dispersion relation can be used to analyze marginal stability, the most unstable wavelengths, and linear growth rates. Numerical simulations can be used to verify results from the linear analysis and study the nonlinear development of KH modes. Here we will describe the marginal stability criterion for the KH instability, how and where this condition is met in the corona, and the possible character of the resultant fluctuations.

Suess, Steve↗

NASA NTRS2006

Precipitation Measurements from Space: Why Do We Need Them?

Water is fundamental to the life on Earth and its phase transition between the gaseous, liquid, and solid states dominates the behavior of the weather/climate/ecological system. Precipitation, which converts atmospheric water vapor into rain and snow, is central to the global water cycle. It regulates the global energy balance through interactions with clouds and water vapor (the primary greenhouse gas), and also shapes global winds and dynamic transport through latent heat release. Surface precipitation affects soil moisture, ocean salinity, and land hydrology, thus linking fast atmospheric processes to the slower components of the climate system. Precipitation is also the primary source of freshwater in the world, which is facing an emerging freshwater crisis in many regions. Accurate and timely knowledge of global precipitation is essential for understanding the behavior of the global water cycle, improving freshwater management, and advancing predictive capabilities of high-impact weather events such as hurricanes, floods, droughts, and landslides. With limited rainfall networks on land and the impracticality of making extensive rainfall measurements over oceans, a comprehensive description of the space and time variability of global precipitation can only be achieved from the vantage point of space. This presentation will examine current capabilities in space-borne rainfall measurements, highlight scientific and practical benefits derived from these observations to date, and provide an overview of the multi-national Global Precipitation Measurement (GPM) Mission scheduled to be launched in the early next decade.

Hou, Arthur Y.↗

NASA NTRS2007

Precipitation Measurements from Space: The Global Precipitation Measurement Mission

Hou, Arthur Y.↗

NASA NTRS2012

Spacecraft Avionics Software Development Then and Now: Different but the Same

NASA has always been in the business of balancing new technologies and techniques to achieve human space travel objectives. NASA s historic Software Production Facility (SPF) was developed to serve complex avionics software solutions during an era dominated by mainframes, tape drives, and lower level programming languages. These systems have proven themselves resilient enough to serve the Shuttle Orbiter Avionics life cycle for decades. The SPF and its predecessor the Software Development Lab (SDL) at NASA s Johnson Space Center (JSC) hosted flight software (FSW) engineering, development, simulation, and test. It was active from the beginning of Shuttle Orbiter development in 1972 through the end of the shuttle program in the summer of 2011 almost 40 years. NASA s Kedalion engineering analysis lab is on the forefront of validating and using many contemporary avionics HW/SW development and integration techniques, which represent new paradigms to NASA s heritage culture in avionics software engineering. Kedalion has validated many of the Orion project s HW/SW engineering techniques borrowed from the adjacent commercial aircraft avionics environment, inserting new techniques and skills into the Multi-Purpose Crew Vehicle (MPCV) Orion program. Using contemporary agile techniques, COTS products, early rapid prototyping, in-house expertise and tools, and customer collaboration, NASA has adopted a cost effective paradigm that is currently serving Orion effectively. This paper will explore and contrast differences in technology employed over the years of NASA s space program, due largely to technological advances in hardware and software systems, while acknowledging that the basic software engineering and integration paradigms share many similarities.

Mangieri, Mark L.↗

DOE OSTI2021

Pore-Scale Dynamics of Liquid CO2–Water Displacement in 2D Axisymmetric Porous Micromodels Under Strong Drainage and Weak Imbibition Conditions: High-Speed μPIV Measurements

Resolving pore-scale transient flow dynamics is crucial to understanding the physics underlying multiphase flow in porous media and informing large-scale predictive models. Surface properties of the porous matrix play an important role in controlling such physics, yet interfacial mechanisms remain poorly understood, in part due to a lack of direct observations. This study reports on an experimental investigation of the pore-scale flow dynamics of liquid CO 2 and water in two-dimensional (2D) circular porous micromodels with different surface characteristics employing high-speed microscopic particle image velocimetry (μPIV). The design of the micromodel minimized side boundary effects due to the limited size of the domain. The high-speed μPIV technique resolved the spatial and temporal dynamics of multiphase flow of CO 2 and water under reservoir-relevant conditions, for both drainage and imbibition scenarios. When CO 2 displaced water in a hydrophilic micromodel (i.e., drainage), unstable capillary fingering occurred and the pore flow was dominated by successive pore-scale burst events (i.e., Haines jumps). When the same experiment was repeated in a nearly neutral wetting micromodel (i.e., weak imbibition), flow instability and fluctuations were virtually eliminated, leading to a more compact displacement pattern. Energy balance analysis indicates that the conversion efficiency between surface energy and external work is less than 30%, and that kinetic energy is a disproportionately smaller contributor to the energy budget. This is true even during a Haines jump event, which induces velocities typically two orders of magnitude higher than the bulk velocity. These novel measurements further enabled direct observations of the meniscus displacement, revealing a significant alteration of the pore filling mechanisms during drainage and imbibition. While the former typically featured burst events, which often occur only at one of the several throats connecting a pore, the latter is typically dominated by a cooperative filling mechanism involving simultaneous invasion of a pore from multiple throats. This cooperative filling mechanism leads to merging of two interfaces and releases surface energy, causing instantaneous high-speed events that are similar, yet fundamentally different from, burst events. Finally, pore-scale velocity fields were statistically analyzed to provide a quantitative measure of the role of capillary effects in these pore flows.

Li, Yaofa↗

DOE OSTI2026

Multisite Proton–Coupled Electron Transfer at a Keggin-Type Polyoxotungstate

Proton−coupled electron transfer (PCET) governs many redox transformations, but is thermodynamically constrained when proton and electron transfer occur at a single site. Here, we introduce a new multisite PCET (MSPCET) platform, based on the Keggin-type polyoxotungstate, [VW 12 O 40 ] 3− (VW 12 ). Pairing VW 12 with either Brønsted bases or acids yields reagent pairs with tunable effective bond dissociation free energies (BDFE eff ) over 15 kcal mol −1 , enabling both oxidative and reductive H atom transfer reactions. Kinetic studies on the oxidative pathway by using 2,4,6- t Bu 3 PhOH as a model hydrogen atom (H atom) donor reveal a product-like, entropy-dominated concerted proton−electron transfer (CPET) pathway from a preorganized hydrogen-bonded complex. By contrast, reductive H atom transfer reactions exhibit larger ΔH ‡ values, measurable kinetic isotope effects, and balanced Brønsted slope, consistent with synchronous CPET-type mechanism. Extension to N−H, O−H, and C−H substrates demonstrates the versatility of the VW 12 MS-PCET platform for tunable (de)hydrogenation.

Charge transfer↗

DOE OSTI2022

Earlier snowmelt may lead to late season declines in plant productivity and carbon sequestration in Arctic tundra ecosystems

Arctic warming is affecting snow cover and soil hydrology, with consequences for carbon sequestration in tundra ecosystems. The scarcity of observations in the Arctic has limited our understanding of the impact of covarying environmental drivers on the carbon balance of tundra ecosystems. In this study, we address some of these uncertainties through a novel record of 119 site-years of summer data from eddy covariance towers representing dominant tundra vegetation types located on continuous permafrost in the Arctic. Here we found that earlier snowmelt was associated with more tundra net CO 2 sequestration and higher gross primary productivity (GPP) only in June and July, but with lower net carbon sequestration and lower GPP in August. Although higher evapotranspiration (ET) can result in soil drying with the progression of the summer, we did not find significantly lower soil moisture with earlier snowmelt, nor evidence that water stress affected GPP in the late growing season. Our results suggest that the expected increased CO 2 sequestration arising from Arctic warming and the associated increase in growing season length may not materialize if tundra ecosystems are not able to continue sequestering CO 2 later in the season.

54 ENVIRONMENTAL SCIENCES↗