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At least 703 records · Page 39

Interaction of Soil pH and Mineralogy Controls Soil Organic Matter Persistence through Changes in the Composition and Amount of Microbial Necromass

Microbial necromass–mineral associations are key to long-term soil organic matter (SOM) persistence. However, how soil pH and mineralogy interact to regulate SOM stability remains poorly understood. Here, we used artificial soils to test how three clay minerals (bentonite, kaolinite, and goethite), adjusted to four pH levels (5–8), affect microbial activity (respiration), microbial physiology (carbon use efficiency, CUE), microbial-derived residue material (necromass), and the formation and stability of mineral-associated organic matter (MAOM). Artificial soils were inoculated with a rhizosphere-derived microbial community cultured under the same pH conditions and on two representative simulated exudate types (organic acids and carbohydrates) and incubated for 6 weeks. In two complementary experiments, we added necromass from known microbial taxa to the same minerals across pH levels to isolate the role of necromass chemistry and loading. We found that soil pH shaped MAOM chemistry by altering microbial activity and necromass composition. In interaction with mineral type, pH also controlled MAOM thermal stability. Higher necromass loading weakened mineral-organic bonding, reducing MAOM stability, consistent with zonal mineral–organic interaction models. Our results demonstrate that microbial activity, rather than carbon use efficiency, better predicts MAOM formation and that pH-dependent necromass composition and loading govern MAOM persistence. These findings advance mechanistic understanding of SOM stabilization and have implications for predicting soil carbon dynamics under shifting environmental conditions.

carbon use efficiency↗

Pushing and Pulling: A Dual pH Trigger Controlled by Varying the Alkyl Tail Length in Heme Coordinating Peptide Amphiphiles

Some organisms in nature that undergo anaerobic respiration utilize 1D nanoscale arrays of densely packed cytochromes containing the molecule heme. The assemblies can be mimicked with 1D nanoscale fibrils composed of peptide amphiphiles designed to coordinate heme in dense arrays. To create such materials and assemblies it is critical to understand the assembly process and what controls the various aspects of hierarchical assembly. MD simulations suggest that shorter alkyl chains on the peptide lead to more dynamic structures than the peptides with longer chains that yield kinetically trapped states. The hydration parameters manifest themselves experimentally through the observation of a dual pH trigger which controls the peptide assembly rate, the heme binding affinity, and heme organization kinetics. Great strides in understanding the relative complexity of the self-assembly process in relation to incorporating a functional moiety like heme opens up many possibilities in developing abiotic assemblies for bioelectronic devices and assemblies

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Perspective on Integrative Simulations of Bioenergetic Domains

Bioenergetic processes in cells, such as photosynthesis or respiration, integrate many time and length scales, which makes the simulation of energy conversion with a mere single level of theory impossible. Just like the myriad of experimental techniques required to examine each level of organization, an array of overlapping computational techniques is necessary to model energy conversion. Here, in this work, a perspective is presented on recent efforts for modeling bioenergetic phenomena with a focus on molecular dynamics simulations and its variants as a primary method. An overview of the various classical, quantum mechanical, enhanced sampling, coarse-grained, Brownian dynamics, and Monte Carlo methods is presented. Example applications discussed include multiscale simulations of membrane-wide electron transport, rate kinetics of ATP turnover from electrochemical gradients, and finally, integrative modeling of the chromatophore, a photosynthetic pseudo-organelle.

59 BASIC BIOLOGICAL SCIENCES↗

Metagenome-Guided Proteomic Quantification of Reductive Dehalogenases in the Dehalococcoides mccartyi -Containing Consortium SDC-9

At groundwater sites contaminated with chlorinated ethenes, fermentable substrates are often added to promote reductive dehalogenation by indigenous or augmented microorganisms. Contemporary bioremediation performance monitoring relies on nucleic acid biomarkers of key organohalide-respiring bacteria, such as Dehalococcoides mccartyi (Dhc). In this work, metagenome sequencing of the commercial, Dhc-containing consortium, SDC-9, identified 12 reductive dehalogenase (RDase) genes, including pceA (two copies), vcrA, and tceA, and allowed for specific detection and quantification of RDase peptides using liquid chromatography coupled with tandem mass spectrometry (LC-MS/MS). Shotgun (i.e., untargeted) proteomics applied to the SDC-9 consortium grown with tetrachloroethene (PCE) and lactate identified 143 RDase peptides, and 36 distinct peptides that covered greater than 99% of the protein-coding sequences of the PceA, TceA, and VcrA RDases. Quantification of RDase peptides using multiple reaction monitoring (MRM) assays with 13 C-/ 15 N-labeled peptides determined 1.8 × 10 3 TceA and 1.2 × 10 2 VcrA RDase molecules per Dhc cell. Ultimately, the MRM mass spectrometry approach allowed for sensitive detection and accurate quantification of relevant Dhc RDases and has potential utility in bioremediation monitoring regimes.

59 BASIC BIOLOGICAL SCIENCES↗

Polymer, Additives, and Processing Effects on N95 Filter Performance

The current severe acute respiratory syndrome coronavirus 2 (SARS-COV-2) pandemic has highlighted the need for personal protective equipment, specifically filtering facepiece respirators like N95 masks. While it is common knowledge that polypropylene (PP) is the industry standard material for filtration media, trial and error is often required to identify suitable commercial precursors for filtration media production. This work aims to identify differences between several commercial grades of PP and demonstrate the development of N95 filtration media with the intent that the industry partners can pivot and help address N95 shortages. Three commercial grades of high melt flow index PP were melt blown at Oak Ridge National Laboratory and broadly characterized by several methods including differential scanning calorimetry (DSC), X-ray diffraction (XRD), and neutron scattering. Despite the apparent similarities (high melt flow and isotacticity) between PP feedstocks, the application of corona charging and charge enhancing additives improve each material to widely varying degrees. From the analysis performed here, the most differentiating factor appears to be related to crystallization of the polymer and the resulting electret formation. Materials with higher crystallization onset temperatures, slower crystallization rates, and larger number of crystallites form a stronger electret and are more effective at filtration.

36 MATERIALS SCIENCE↗

Mediated Electrochemical Probing: A Systems-Level Tool for Redox Biology

Biology uses well-known redox mechanisms for energy harvesting (e.g., respiration), biosynthesis, and immune defense (e.g., oxidative burst), and now we know biology uses redox for systems-level communication. Currently, we have limited abilities to “eavesdrop” on this redox modality, which can be contrasted with our abilities to observe and actuate biology through its more familiar ionic electrical modality. In this Perspective, we argue that the coupling of electrochemistry with diffusible mediators (electron shuttles) provides a unique opportunity to access the redox communication modality through its electrical features. Here, we highlight previous studies showing that mediated electrochemical probing (MEP) can “communicate” with biology to acquire information and even to actuate specific biological responses (i.e., targeted gene expression). We suggest that MEP may reveal an extent of redox-based communication that has remained underappreciated in nature and that MEP could provide new technological approaches for redox biology, bioelectronics, clinical care, and environmental sciences.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Decontamination of SARS-CoV-2 and Other RNA Viruses from N95 Level Meltblown Polypropylene Fabric Using Heat under Different Humidities

In March of 2020, the World Health Organization declared a pandemic of coronavirus disease 2019 (COVID-19), caused by the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). The pandemic led to a shortage of N95-grade filtering facepiece respirators (FFRs), especially surgical-grade N95 FFRs for protection of healthcare professionals against airborne transmission of SARS-CoV-2. We and others have previously reported promising decontamination methods that may be applied to the recycling and reuse of FFRs. In this study we tested disinfection of three viruses, including SARS-CoV-2, dried on a piece of meltblown fabric, the principal component responsible for filtering of fine particles in N95-level FFRs, under a range of temperatures (60–95 °C) at ambient or 100% relative humidity (RH) in conjunction with filtration efficiency testing. We found that heat treatments of 75 °C for 30 min or 85 °C for 20 min at 100% RH resulted in efficient decontamination from the fabric of SARS-CoV-2, human coronavirus NL63 (HCoV-NL63), and another enveloped RNA virus, chikungunya virus vaccine strain 181/25 (CHIKV-181/25), without lowering the meltblown fabric’s filtration efficiency.

60 APPLIED LIFE SCIENCES↗

Transcriptional Regulatory Networks Involved in C3–C4 Alcohol Stress Response and Tolerance in Yeast

Alcohol toxicity significantly impacts the titer and productivity of industrially produced biofuels. To overcome this limitation, we must find and use strategies to improve stress tolerance in production strains. Previously, we developed a multiplex navigation of a global regulatory network (MINR) library that targeted 25 regulatory genes that are predicted to modify global regulation in yeast under different stress conditions. Herein, we expanded this concept to target the active sites of 47 transcriptional regulators using a saturation mutagenesis library. The 47 targeted regulators interact with more than half of all yeast genes. We then screened and selected for C3–C4 alcohol tolerance. We identified specific mutants that have resistance to isopropanol and isobutanol. Notably, the WAR1_K110N variant improved tolerance to both isopropanol and isobutanol. In addition, we investigated the mechanisms for improvement of isopropanol and isobutanol stress tolerance and found that genes related to glycolysis play a role in tolerance to isobutanol, while changes in ATP synthesis and mitochondrial respiration play a role in tolerance to both isobutanol and isopropanol. Overall, this work sheds light on basic mechanisms for isopropanol and isobutanol toxicity and demonstrates a promising strategy to improve tolerance to C3–C4 alcohols by perturbing the transcriptional regulatory network.

09 BIOMASS FUELS↗

Single-Molecule Detection of the Encounter and Productive Electron Transfer Complexes of a Photosynthetic Reaction Center

Small, diffusible redox proteins play an essential role in electron transfer (ET) in respiration and photosynthesis, sustaining life on Earth by shuttling electrons between membrane-bound complexes via finely tuned and reversible interactions. Ensemble kinetic studies show transient ET complexes form in two distinct stages: an “encounter” complex largely mediated by electrostatic interactions, which subsequently, through subtle reorganization of the binding interface, forms a “productive” ET complex stabilized by additional hydrophobic interactions around the redox-active cofactors. Here, using single-molecule force spectroscopy (SMFS) we dissected the transient ET complexes formed between the photosynthetic reaction center-light harvesting complex 1 (RC-LH1) of Rhodobacter sphaeroides and its native electron donor cytochrome c 2 (cyt c 2 ). Importantly, SMFS resolves the distribution of interaction forces into low (~150 pN) and high (~330 pN) components, with the former more susceptible to salt concentration and to alteration of key charged residues on the RC. Thus, the low force component is suggested to reflect the contribution of electrostatic interactions in forming the initial encounter complex, whereas the high force component reflects the additional stabilization provided by hydrophobic interactions to the productive ET complex. Employing molecular dynamics simulations, we resolve five intermediate states that comprise the encounter, productive ET and leaving complexes, predicting a weak interaction between cyt c 2 and the LH1 ring near the RC-L subunit that could lie along the exit path for oxidized cyt c 2 . The multimodal nature of the interactions of ET complexes captured here may have wider implications for ET in all domains of life.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Seasonal Controls of CO 2 and CH 4 Dynamics in a Temporarily Flooded Subtropical Wetland

Subtropical and tropical wetlands play a prominent role in the global carbon (C) cycle; yet factors that influence their C fluxes remain uncertain. We collected measurements from a temporarily flooded subtropical wetland over 3 years to investigate environmental drivers impacting CO 2 and CH 4 fluxes. The wetland was a sink of CO 2 (-469 to -380 g C-CO 2 · m -2 · year -1 ) and a source of CH 4 (25.1 to 32.1 g C-CH 4 · m -2 · year -1 ) to the atmosphere. Dry season CH 4 emissions represented 41 to 49% of the annual budget, reflecting the importance of continuous CH 4 flux measurements. Gross primary productivity (GPP) increased with temperature and radiation, and the influence of VPD on GPP varied with soil inundation. Higher water tables decreased Reco and increased GPP, and a higher GPP in turn lead to enhanced R eco likely through enhancements of GPP on autotrophic respiration. This suggests that the impact of the water table on R eco depends on the cancelling effects of hydrology and GPP. Emissions of CH 4 increased with soil temperature, water table, and GPP until soils were inundated at which point temperature and GPP became the main drivers. Water table and temperature influenced GPP and CH 4 fluxes, and increases in GPP directly enhanced CH 4 emissions. In addition to impacting C fluxes directly through water table depth, hydrology also determined the hierarchy of the dominance of factors controlling C fluxes and their response. The positive climate forcing of subtropical wetlands may be dictated by plant-mediated and climate interactions, with hydrological factors playing a major role in determining the greenhouse gas sink or source strength of subtropical wetlands.

54 ENVIRONMENTAL SCIENCES↗

A Multiyear Gridded Data Ensemble of Surface Biogenic Carbon Fluxes for North America: Evaluation and Analysis of Results

Accurate and fine-scale estimates of biogenic carbon fluxes are critical for measuring and monitoring the biosphere's responses and feedback to the climate system. Currently available data products from flux towers and model-intercomparison projects struggle to adequately represent spatiotemporal dynamics of surface biogenic carbon fluxes, and to quantify their uncertainties, which also are crucial to atmospheric inversion systems. To address these gaps, we introduce a new perturbed-parameter model ensemble with the CASA model to estimate surface biogenic carbon fluxes at monthly and 3-hourly scales for North America at ~500-m and 5-km resolutions. We first use the Extended Fourier Amplitude Sensitivity Testing to choose the three most sensitive parameters to be perturbed, maximum light use efficiency (E max ), optimal temperature of photosynthesis (T opt ), and temperature response of respiration (Q 10 ). The initial range for each parameter is broadly sampled for the L1 ensemble, but then we pruned E max with site-level primary productivity to derive an L2 ensemble with narrower uncertainty ranges. Ensembles are strongly correlated with site-level results at both monthly and 3-hourly scales, and the spread across L1/L2 ensemble members encompasses the range of AmeriFlux observations. Monthly variability in the L2 ensemble mean is 85% of the observed variability. The L2 ensemble outperforms diverse data products with the highest Taylor skill scores at diurnal to annual scales. Finally, the ensemble's seasonality agrees well with other models for most biome types and in high and middle latitudes, but inconsistencies are found in subtropical and tropical ecoregions and for annual totals over North America.

54 ENVIRONMENTAL SCIENCES↗

Partitioning Net Ecosystem Exchange (NEE) of CO 2 Using Solar-Induced Chlorophyll Fluorescence (SIF)

Accurate partitioning of net ecosystem exchange (NEE) of CO 2 to gross primary production (GPP) and ecosystem respiration (R eco ) is crucial for understanding carbon cycle dynamics under changing climate. However, it remains as a long-standing problem in global ecology due to lack of independent constraining information for the two offsetting component fluxes. solar-induced chlorophyll fluorescence (SIF), a mechanistic proxy for photosynthesis, holds great promise to improve NEE partitioning by constraining GPP. We developed a parsimonious SIF-based approach for NEE partitioning and examined its performance using synthetic simulations and field measurements. This approach outperforms conventional approaches in reproducing simulated GPP and R eco , especially under high vapor pressure deficit. For field measurements, it results in lower daytime GPP and R eco than conventional approaches. Furthermore, this study made the first attempt to demonstrate SIF's potential for improving NEE partitioning accuracy and sets the stage for future efforts to examine its robustness and scalability under real-world environmental conditions.

54 ENVIRONMENTAL SCIENCES↗

High Vapor Pressure Deficit Decreases the Productivity and Water Use Efficiency of Rain‐Induced Pulses in Semiarid Ecosystems

Abstract Intermittent rain events drive dynamic pulses of carbon and water exchange in many arid and semiarid ecosystems. Although soil moisture is known to control these pulses, the effect of atmospheric dryness on pulses is not well documented. Here we hypothesized that vapor pressure deficit ( VPD ) modulates net ecosystem production ( NEP ) and ecosystem‐scale water use efficiency ( WUE ) during pulse events due to its effects on canopy stomatal conductance and evapotranspiration. We quantified relationships between VPD and carbon and water exchange during growing season rain events and tested their generality across four semiarid flux sites with varied vegetation in the southwest United States. Across grassland, shrubland, and savanna sites, we found that high VPD during pulses suppressed ecosystem photosynthesis and surface conductance to a greater degree than respiration or evapotranspiration, particularly when soil moisture was high. Thus, periods of high VPD were associated with a 13–64% reduction in NEP and an 11–25% decrease in WUE , relative to moderate VPD conditions. Sites dominated by shrubs with the C3 photosynthetic pathway were more sensitive to VPD than sites dominated by C4 grasses. We found that a 1 kPa increase in VPD reduced the average NEP of pulse events by 13–56%, which illustrates the potential for projected increases in atmospheric demand to reduce the net productivity of semiarid ecosystems.

Roby, Matthew C.↗

Tundra Underlain By Thawing Permafrost Persistently Emits Carbon to the Atmosphere Over 15 Years of Measurements

Warming of the Arctic can stimulate microbial decomposition and release of permafrost soil carbon (C) as greenhouse gases, and thus has the potential to influence climate change. At the same time, plant growth can be stimulated and offset C release. This study presents a 15-year time series comprising chamber and eddy covariance measurements of net ecosystem C exchange in a tundra ecosystem in Alaska where permafrost has been degrading due to regional warming. The site was a carbon dioxide source to the atmosphere with a cumulative total loss of 781.6 g C m -2 over the study period. Both gross primary productivity (GPP) and ecosystem respiration (R eco ) were already likely higher than historical levels such that increases in R eco losses overwhelmed GPP gains in most years. This shift to a net C source to the atmosphere likely started in the early 1990s when permafrost was observed to warm and thaw at the site. Shifts in the plant community occur more slowly and are likely to constrain future GPP increases as compared to more rapid shifts in the microbial community that contribute to increased Reco. Observed rates suggest that cumulative net soil C loss of 4.18–10.00 kg C m -2 —8%–20% of the current active layer soil C pool—could occur from 2020 to the end of the century. This amount of permafrost C loss to the atmosphere represents a significant accelerating feedback to climate change if it were to occur at a similar magnitude across the permafrost region.

54 ENVIRONMENTAL SCIENCES↗

Modeling Profiles of Micrometeorological Variables in a Tropical Premontane Rainforest Using Multi-Layered CLM (CLM-ML)

This study updates the multi-layered Community Land Model (CLM-ml) for hillslopes and compares predictions from against observations collected in tropical montane rainforest, Costa Rica. Modifications are made in order to capture a wider array of vertical leaf area distributions, predict CO 2 profiles, account for soil respiration, and adjust wind forcings for difficult topographic settings. Test results indicate that the modified multi-layer CLM model can successfully replicate the shape of various micrometeorological profiles (humidity, CO 2 , temperature, and wind speed) under the canopy. In the single-layer models (CLM4.5 and CLM5), excessive day-to-night differences in leaf temperature and leaf wetness were originally noted, but CLM-ml significantly improved these issues, decreasing the amplitudes of diurnal cycles by 67% and 47%. Sub-canopy considerations, such as canopy shapes and turbulent transfer parameters, also played a significant role in model performance. More importantly, unlike single layer models, the results that CLM-ml produces can be compared to variables measured within the canopy to provide far more detailed diagnostic information. Further observations and model developments, aimed at reflecting surface heterogeneity, will be necessary to adequately capture the complexity and the features of the tropical montane rainforest.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dynamics of Fungal and Bacterial Biomass Carbon in Natural Ecosystems: Site-level Applications of the CLM-Microbe Model

Explicitly representing microbial processes has been recognized as a key improvement to Earth system models for the realistic projections of soil carbon (C) and climate dynamics. The CLM-Microbe model builds upon the CLM4.5 and explicitly represents two major soil microbial groups, fungi and bacteria. Based on the compiled time-series data of fungal (FBC) and bacterial (BBC) biomass C from nine biomes, we parameterized and validated the CLM-Microbe model, and further conducted sensitivity analysis and uncertainty analysis for simulating C cycling. The model performance was evaluated with mean absolute error (MAE), root mean square error (RMSE), and coefficient of determination (R2) for relative change in FBC and BBC. The CLM-Microbe model is able to reasonably capture the seasonal dynamics of FBC and BBC across biomes, particularly for tropical/subtropical forest, temperate broadleaf forest, and grassland, with MAE < 0.49 for FBC and <0.36 for BBC and RMSE <0.52 FBC and <0.39 for BBC, while R2 values are relatively smaller in some biomes (e.g., shrub) due to small sample sizes. We found good consistencies between simulated and observed FBC (R 2 =0.70, P<0.001) and BBC (R 2 =0.26, P<0.05) on average across biomes, but the model is not able to fully capture the large variation in observed FBC and BBC. Sensitivity analysis shows the most critical parameters are turnover rate, carbon-to-nitrogen ratio of fungi and bacteria, and microbial assimilation efficiency. This study confirms that the explicit representation of soil microbial mechanisms enhances model performance in simulating C variables such as heterotrophic respiration and soil organic C density. The further application of the CLM-Microbe model would deepen our understanding of microbial contributions to the global C cycle.

54 ENVIRONMENTAL SCIENCES↗

Improving CLM5.0 Biomass and Carbon Exchange Across the Western United States Using a Data Assimilation System

The Western United States is dominated by natural lands that play a critical role for carbon balance, water quality, and timber reserves. This region is also particularly vulnerable to forest mortality from drought, insect attack, and wildfires, thus requiring constant monitoring to assess ecosystem health. Carbon monitoring techniques are challenged by the complex mountainous terrain, thus there is an opportunity for data assimilation systems that combine land surface models and satellite-derived observations to provide improved carbon monitoring. Here, we use the Data Assimilation Research Testbed to adjust the Community Land Model (CLM5.0) with remotely sensed observations of leaf area and above-ground biomass. The adjusted simulation significantly reduced the above-ground biomass and leaf area, leading to a reduction in both photosynthesis and respiration fluxes. The reduction in the carbon fluxes mostly offset, thus both the adjusted and free simulation projected a weak carbon sink to the land. This result differed from a separate observation-constrained model (FLUXCOM) that projected strong carbon uptake to the land. Simulation diagnostics suggested water limitation had an important influence upon the magnitude and spatial pattern of carbon uptake through photosynthesis. We recommend that additional observations important for water cycling (e.g., snow water equivalent, land surface temperature) be included to improve the veracity of the spatial pattern in carbon uptake. Furthermore, the assimilation system should be enhanced to maximize the number of the simulated state variables that are adjusted, especially those related to the recommended observed quantities including water cycling and soil carbon.

54 ENVIRONMENTAL SCIENCES↗

Influence of Tundra Polygon Type and Climate Variability on CO 2 and CH 4 Fluxes Near Utqiagvik, Alaska

Arctic tundra has the potential to generate significant climate feedbacks, but spatial complexity makes it difficult to quantify the impacts of climate on ecosystem-atmosphere fluxes, particularly in polygonal tundra comprising wetter and drier polygon types on the scale of tens of meters. We measured CO 2 , CH 4 , and energy fluxes using eddy covariance for 7 yr (April to November, 2013–2019) in polygonal tundra near Utqiagvik, Alaska. This period saw the earliest snowmelt, latest snow accumulation, and hottest summer on record. To estimate fluxes by polygon type, we combined a polygon classification with a flux-footprint model. Methane fluxes were highest in the summer months but were also large during freeze-up and increased with the warming trend in August–November temperatures. While CO 2 respiration had a consistent, exponential relationship with temperature, net ecosystem exchange was more variable among years. CO 2 and CH 4 exchange (June–September) ranged between -0.83 (Standard error [SE] = 0.03) and -1.32 (SE = 0.04) μmol m -2 s-1 and 13.92 (SE = 0.26)—23.42 (SE = 0.45) nmol m -2 s -1 , respectively, and varied interannually (p ≤ 0.05). The maximum-influence method effectively attributed fluxes to polygon types. Areas dominated by low-centered polygons had higher CO 2 fluxes except in 2016–2017. Methane fluxes were highest in low-centered polygons 2013–2015 and in flat-centered polygons in subsequent years, possibly due to increasing temperature and precipitation. Sensible and latent heat fluxes also varied significantly among polygon types. Accurate characterization of Arctic fluxes and their climate dependencies requires spatial disaggregation and long term observations.

54 ENVIRONMENTAL SCIENCES↗