Search for: All records

Arctic hydrology is experiencing rapid changes including earlier snow melt, permafrost degradation, increasing active layer depth, and reduced river ice, all of which are expected to lead to changes in stream flow regimes. Recently, long-term (>60 years) climate reanalysis and river discharge observation data have become available. We utilized these data to assess long-term changes in discharge and their hydroclimatic drivers. River discharge during the cold season (October–April) increased by 10% per decade. The most widespread discharge increase occurred in April (15% per decade), the month of ice break-up for the majority of basins. In October, when river ice formation generally begins, average monthly discharge increased by 7% per decade. Long-term air temperature increases in October and April increased the number of days above freezing (+1.1 d per decade) resulting in increased snow ablation (20% per decade) and decreased snow water equivalent (−12% per decade). Compared to the historical period (1960–1989), mean April and October air temperature in the recent period (1990–2019) have greater correlation with monthly discharge from 0.33 to 0.68 and 0.0–0.48, respectively. This indicates that the recent increases in air temperature are directly related to these discharge changes. Ubiquitous increases in cold and shoulder-season discharge demonstrate the scale at which hydrologic and biogeochemical fluxes are being altered in the Arctic.

 

Due to the emergence of wide-spread infectious diseases, there is a heightened need for antimicrobial and/or antifouling coatings that can be used to prevent infection and transmission in a variety of applications, ranging from healthcare devices to public facilities. While antimicrobial coatings kill pathogenic bacteria upon contact with the surface, the antimicrobial function alone often lacks long-term effectiveness due to the accumulation of dead cells and their debris on the surface, thus reducing the performance of the coating over time. Therefore, it is desirable to develop coatings with the dual functions of antimicrobial efficacy and fouling resistance, in which antifouling coatings provide the added benefit of preventing the adhesion of dead cells and debris. Leveraging the outstanding antifouling properties of zwitterionic coatings, we synthesized copolymers with this antimicrobial-antifouling dual function by immobilizing lysozyme, a common antimicrobial enzyme, to the surface of a pyridinium-based zwitterionic copolymer. Specifically, poly(4-vinylpyridine- co -pentaflurophenyl methacrylate- co -divinyl benzene) [P(4VP-PFPMA-DVB)] thin films were synthesized by an all-dry vapor deposition technique, initiated Chemical Vapor Deposition, and derivatized using 1,3-propane sultone to obtain sulfobetaine moieties. Lysozyme, known to hydrolyze polysaccharides in the cell wall of Gram-positive bacteria, was immobilized by forming amide bonds with the copolymer coating via nucleophilic substitution of the pentafluorophenyl group. The antifouling and antibacterial performance of the novel lysozyme-zwitterionic coating was tested against Gram-positive Bacillus subtilis and Gram-negative Pseudomonas aeruginosa . A reduction in surface adhesion of 87% was achieved for P. aeruginosa , and of 75% for B. subtilis , when compared to a common poly(vinyl chloride) surface. The lysozyme-zwitterionic coating also deactivated 67% of surface-attached Gram-positive bacteria, B. subtilis . This novel dual-function material can produce anti -infection surfaces for medical devices and surgical tools, personal care products, and surfaces in public facilities. 

To reduce the severe health risk and the huge economic impact associated with the fomite transmission of SARS-CoV-2, an imidazolium-based zwitterionic polymer was designed, synthesized, and demonstrated to achieve contact deactivation of a human coronavirus under dry ambient conditions that resemble fomite transmission. The zwitterionic polymer further demonstrated excellent antifouling properties, reducing the adhesion of coronavirus and the formation of bacteria biofilms under wetted conditions. The polymer was synthesized using a substrate-independent and solvent-free process, leveraging an all-dry technique named initiated chemical vapor deposition (iCVD). The broad applicability of this approach was demonstrated by applying the polymer to a range of substrates that are curved and/or with high-aspect-ratio nano/microporous structures, which remained intact after the coating process. The zwitterionic polymer and the synthesis approach reported here present an effective solution to mitigate viral transmission without the need for manual disinfection, reducing the health and economic impact of the ongoing pandemic. 

The Arctic hydrological system is an interconnected system that is experiencing rapid change. It is comprised of permafrost, snow, glacier, frozen soils, and inland river systems. In this study, we aim to lower the barrier of using complex land models in regional applications by developing a generalizable optimization methodology and workflow for the Community Terrestrial Systems Model (CTSM), to move them toward a more Actionable Science paradigm. Further end‐user engagement is required to make science such as this “fully actionable.” We applied CTSM across Alaska and the Yukon River Basin at 4‐km spatial resolution. We highlighted several potentially useful high‐resolution CTSM configuration changes. Additionally, we performed a multi‐objective optimization using snow and river flow metrics within an adaptive surrogate‐based model optimization scheme. Four representative river basins across our study domain were selected for optimization based on observed streamflow and snow water equivalent observations at 10 SNOTEL sites. Fourteen sensitive parameters were identified for optimization with half of them not directly related to hydrology or snow processes. Across fifteen out‐of‐sample river basins, 13 had improved flow simulations after optimization and the mean Kling‐Gupta Efficiency of daily flow increased from 0.43 to 0.63 in a 30‐year evaluation. In addition, we adapted the Shapley Decomposition to disentangle each parameter's contribution to streamflow performance changes, with the seven non‐hydrological parameters providing a non‐negligible contribution to performance gains. The snow simulation had limited improvement, likely because snow simulation is influenced more by meteorological forcing than model parameter choices.

 

As the Arctic and its rivers continue to warm, a better understanding of the possible future impacts on people would benefit from close partnership with Indigenous communities and scientists from diverse fields of study. We present efforts by the Arctic Rivers Project to conduct community‐engaged research to increase collective understanding of the historical and potential future impacts of climate change on rivers, fish, and Indigenous communities. Working in central to northern Alaska and the Yukon Territory in Canada, the project seeks to engage with Indigenous communities in ethical and equitable ways to produces science that is useful, useable, and used that may serve as an example for future research efforts. Toward this goal, we formed an Indigenous Advisory Council and together developed project‐specific knowledge co‐production protocols. This paper provides a novel model of design and implementation to co‐produce knowledge with communities across a large study domain.

 

Conformal coating of nanopores with functional polymer nanolayers is the key to many emerging technologies such as miniature sensors and membranes for advanced molecular separations. While the polymer coatings are often used to introduce functional moieties, their controlled growth under nanoconfinement could serve as a new approach to manipulate the size and shape of coated nanopores, hence, enabling novel functions like molecular separation. However, precise control of coating thickness in the longitudinal direction of a nanopore is limited by the lack of a characterization method to profile coating thickness within the nanoconfined space. Here, we report an experimental approach that combines ion milling (IM) and high-resolution field emission scanning electron microscopy (FESEM) for acquiring an accurate depth profile of ultrathin (∼20 nm or less) coatings synthesized inside nanopores via initiated chemical vapor deposition (iCVD). The enhanced capability of this approach stems from the excellent x–y resolution achieved by FESEM (i.e., 4.9 nm/pixel), robust depth ( z) control enabled by IM (step size as small as 100 nm with R² = 0.992), and the statistical power afforded by high-throughput sampling (i.e., ∼2000 individual pores). With that capability, we were able to determine with unparalleled accuracy and precision the depth profile of coating thickness and iCVD kinetics along 110-nm-diameter nanopores. That allowed us to uncover an unexpected coating depth profile featuring a maximum rate of polymerization at ∼250 nm underneath the top surface, i.e., down the pores, which we termed “necking.” The necking phenomenon deviates considerably from the conventionally assumed monotonous decrease in thickness along the longitudinal direction into a nanopore, as predicted by the diffusion-limited kinetics model of free radical polymerization. An initiator-centric collision model was then developed, which suggests that under the experimental conditions, the confinement imposed by the nanopores may lead to local amplification of the effective free radical concentration at z ≤ 100 nm and attenuation at z ≥ 500 nm, thus contributing to the observed necking phenomenon. The ion-milling-enabled depth profiling of ultrathin coatings inside nanopores, along with the initiator-mediated coating thickness control in the z-direction, may serve to enhance the performance of size-exclusion filtration membranes and even provide more flexible control of nanopore shape in the z dimension.

 

Seasonal thermal stratification in reservoirs changes the thermal regime of regulated river systems as well as stream temperature responses to climate change. Cold releases from the reservoir hypolimnion can depress downstream river temperature during warm seasons. Recent large‐scale climate change studies on stream temperature have largely ignored reservoir thermal stratification. In this study, we used established models to develop a framework which considers water demand and reservoir regulation with thermal stratification and applied this model framework to the southeastern United States. About half of all 271 reservoirs in our study area retain strong thermal stratification by the 2080s (2070–2099) under RCP8.5 even as median residence times decrease to 60 days from 69 days in the historic period (1979–2010). Reservoir impacts on downstream temperatures become slightly weaker in the future because of higher air temperature and stronger solar radiation. We defined a “cooling potential” to quantify the thermal energy that a water body can absorb before exceeding a water temperature threshold. In the future, higher river temperatures will reduce the cooling potential for all river segments, but more so for river segments minimally impacted by thermal stratification. Reservoir impacts on cooling potential remain strong for river segments downstream of reservoirs with strong thermal stratification. We conducted a sensitivity analysis to evaluate the robustness of our findings to errors in the hydrological simulations. Although river segments subject to reservoir regulation are more sensitive to errors in hydrology than those without regulation impacts, our overall findings do not materially change due to these errors.