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  1. A survey of 23 commercially available cation exchange membranes was performed for the downselection of membranes for use in a polysulfide-permanganate redox flow battery (pS-Mn RFB). The survey measured the flux of permanganate ions across a 0.1 mol L−1concentration gradient as well as the membrane resistance in a 0.5 mol L−1sodium chloride solution. The membranes exhibited the characteristic flux/resistance trade-off observed in most classes of membranes. To connect the individual membrane testing to how the membranes will perform in a device, cell performance data in a pS-Mn RFB was collected for three membranes from the survey. The coulombic, voltaic, and energy efficiency at low cycle counts aligned with the predictions from the membrane flux and resistance survey results. The study also identified three membranes—Fumapem F-930-RFS, Fumapem FS-715-RFS, and Aquivion E98-09S—that outperformed most other membranes regarding their position on the flux-resistance trade-off curve, indicating them to be good candidates for further testing.

     
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  2. Free, publicly-accessible full text available November 28, 2024
  3. Monoligated and bis-ligated CCC-NHC pincer Fe complexes with n-butyl substituents have been synthesized by the Zr metalation/transmetalation route. Both the direct metalation/transmetalation and transmetalation from the isolated (BuCiCiCBu)ZrNMe2Cl2, 3, yielded the octahedrally coordinated Fe(III) bis-ligated complex [(BuCiCiCBu)2Fe]Cl, 2a. Transmetalation from in situ and isolated (BuCiCiCBu)ZrCl3, 5, in the presence of excess TMSCl and 1 equiv of the Fe source yielded the monoligated (BuCiCiCBu)FeCl2, 4. Conditions that convert [(BuCiCiCBu)2Fe]+, 2, to (BuCiCiCBu)FeCl2, 4, complex have been found. Characterization included 1H NMR, UV−visible, femtosecond transient absorption spectroscopies, TDDFT computations, and mass spectroscopy along with X-ray crystallographic structure determinations. 
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    Free, publicly-accessible full text available February 12, 2025
  4. The loss of plant productivity with declining diversity is well established, exceeding other global change drivers including drought. These patterns are most clearly established for aboveground productivity, it remains poorly understood whether productivity increases associated with diversity are replicated belowground. To address this gap, we established a plant diversity-manipulation experiment in 2018. It is a full factorial manipulation of plant species richness and community composition, and precipitation. Three and five years post-establishment, two bulk soil cores (20cm depth) were collected and composited from each plot and were processed for roots to determine belowground biomass as root standing crop. We observed a strong positive relationship between richness and aboveground production and belowground biomass, generating positive combined above and belowground with diversity. Root standing crop increased 1.4-fold from years three to five. Grass communities produced more root biomass (monoculture mean 463.9 ± 410.3g m−2), and the magnitude of the relationship between richness and root standing crop was greatest within those communities. Legume communities produced the fewest roots (monoculture mean 212.2 ± 155.1g m−2), and belowground standing crop was not affected by diversity. Root standing crops in year three were 1.8 times higher under low precipitation conditions, while in year five we observed comparable root standing crops between precipitation treatments. Plant family was a strong mediator of increased belowground biomass observed with diversity, with single family grass and aster families generating 1.7 times greater root standing crops in six compared to single species communities, relationships between diversity and aboveground production were consistently observed in both single-family and multiple family communities. Diverse communities with species from multiple families generated only 1.3 times the root standing crop compared to monoculture average root biomass. We surprisingly observe diverse single family communities can generate increases in root standing crops that exceed those generated by diverse multiple family communities, highlighting the importance of plant richness within plant family for a given community. These patterns have potential implications for understanding the interactions of multiple global change drivers as changes in both precipitation and plant community composition do alter whether plant production aboveground is translated belowground biomass.

     
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    Free, publicly-accessible full text available November 27, 2024
  5. Free, publicly-accessible full text available December 1, 2024
  6. Abstract

    We report on the successful completion of a project to upgrade the positional accuracy of every response to the 1990, 2000, and 2010 U.S. decennial censuses. The resulting data set, called Optimized Spatial Census Information Linked Across Time (OSCILAT), resides within the restricted-access data warehouse of the Federal Statistical Research Data Center (FSRDC) system where it is available for use with approval from the U.S. Census Bureau. OSCILAT greatly improves the accuracy and completeness of spatial information for older censuses conducted prior to major quality improvements undertaken by the Bureau. Our work enables more precise spatial and longitudinal analysis of census data and supports exact tabulations of census responses for arbitrary spatial units, including tabulating responses from 1990, 2000, and 2010 within 2020 block boundaries for precise measures of change over time for small geographic areas.

     
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  7. Abstract Shape-morphable electrode arrays can form 3D surfaces to conform to complex neural anatomy and provide consistent positioning needed for next-generation neural interfaces. Retinal prostheses need a curved interface to match the spherical eye and a coverage of several cm to restore peripheral vision. We fabricated a full-field array that can (1) cover a visual field of 57° based on electrode position and of 113° based on the substrate size; (2) fold to form a compact shape for implantation; (3) self-deploy into a curvature fitting the eye after implantation. The full-field array consists of multiple polymer layers, specifically, a sandwich structure of elastomer/polyimide-based-electrode/elastomer, coated on one side with hydrogel. Electrodeposition of high-surface-area platinum/iridium alloy significantly improved the electrical properties of the electrodes. Hydrogel over-coating reduced electrode performance, but the electrodes retained better properties than those without platinum/iridium. The full-field array was rolled into a compact shape and, once implanted into ex vivo pig eyes, restored to a 3D curved surface. The full-field retinal array provides significant coverage of the retina while allowing surgical implantation through an incision 33% of the final device diameter. The shape-changing material platform can be used with other neural interfaces that require conformability to complex neuroanatomy. 
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    Free, publicly-accessible full text available December 1, 2024
  8. Abstract

    Productivity benefits from diversity can arise when compatible pathogen hosts are buffered by unrelated neighbors, diluting pathogen impacts. However, the generality of pathogen dilution has been controversial and rarely tested within biodiversity manipulations. Here, we test whether soil pathogen dilution generates diversity- productivity relationships using a field biodiversity-manipulation experiment, greenhouse assays, and feedback modeling. We find that the accumulation of specialist pathogens in monocultures decreases host plant yields and that pathogen dilution predicts plant productivity gains derived from diversity. Pathogen specialization predicts the strength of the negative feedback between plant species in greenhouse assays. These feedbacks significantly predict the overyielding measured in the field the following year. This relationship strengthens when accounting for the expected dilution of pathogens in mixtures. Using a feedback model, we corroborate that pathogen dilution drives overyielding. Combined empirical and theoretical evidence indicate that specialist pathogen dilution generates overyielding and suggests that the risk of losing productivity benefits from diversity may be highest where environmental change decouples plant-microbe interactions.

     
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    Free, publicly-accessible full text available December 1, 2024
  9. Atmospheric chemistry models generally assume organic aerosol (OA) to be photochemically inert. Recent mechanisms for the oxidation of biogenic isoprene, a major source of secondary organic aerosol (iSOA), produce excessive OA in the absence of subsequent OA reactivity. At the same time, models underestimate atmospheric concentrations of formic and acetic acids for which OA degradation could provide a source. Here we show that the aqueous photooxidation of an isoprene-derived organosulfate (2-methyltriolsulfate or MTS), an important iSOA component, produces formic and acetic acids in high yields and at timescales competitive with deposition. Experimental data are well fit by a kinetic model in which three sequential oxidation reactions of the isoprene organosulfate produce two molar equivalents of formic acid and one of acetic acid. We incorporate this chemistry and that of 2-methyltetrol, another ubiquitous iSOA component, into the GEOS-Chem global atmospheric chemistry model. Simulations show that photooxidation and subsequent revolatilization of this iSOA may account for up to half of total iSOA loss globally, producing 4 Tg a−1 each of formic and acetic acids. This reduces model biases in gas-phase formic acid and total organic aerosol over the Southeast United States in summer by ∼30% and 60% respectively. While our study shows the importance of adding iSOA photochemical sinks into atmospheric models, uncertainties remain that warrant further study. In particular, improved understanding of reaction dependencies on particle characteristics and concentrations of particle-phase OH and other oxidants are needed to better simulate the effects of this chemistry on the atmospheric budgets of organic acids and iSOA. 
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    Free, publicly-accessible full text available November 9, 2024
  10. Abstract Private lands are important for conservation worldwide, but knowledge about their effectiveness is still insufficient. To help fill this important knowledge gap, we analyzed the impacts of a national policy for conservation on private lands in Brazil, a global biodiversity hotspot with high potential for nature-based climate solutions. Through the evaluation of over 4 million private rural properties from the Rural Environmental Cadastre, we found that the last policy review in 2012 mainly affected the Amazon Forest. The amnesty granted to 80% of landowners of small properties prevented the restoration of 14.6 million hectares of agricultural land with a carbon sequestration potential of 2.4 gigatonnes. We found that private lands exist within the limits of public conservation areas and that between 2003 and 2020 deforestation rates in these private lands were higher than those across all conservation areas. The Rural Environmental Cadastre can be an effective tool for managing forests within private lands, with potential to integrate governance approaches to control deforestation and mitigate climate change. 
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    Free, publicly-accessible full text available December 1, 2024