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Fluoropolymer‐Stabilized Chromophore–Catalyst Assemblies in Aqueous Buffer Solutions for Water‐Oxidation Catalysis
Abstract Here, the application of the fluorinated polymer [Dupont AF, a copolymer of 4,5‐difluoro‐2,2‐bis(trifluoromethyl)‐1,3‐dioxole and tetrafluoroethylene] is described in stabilizing phosphonate‐derivatized molecular assemblies on oxide electrodes. In the procedure, the polymer was dip‐coated onto the surfaces of oxide electrodes with pre‐bound, phosphonate‐derivatized chromophores and assemblies, including assemblies for water oxidation. The results of the experiments showed a high degree of stabilization by the added polymer and a demonstration of its use in stabilizing surface‐bound assemblies for water‐oxidation catalysis.
Covalent Attachment of the Water‐insoluble Ni(P Cy 2 N Phe 2 ) 2 Electrocatalyst to Electrodes Showing Reversible Catalysis in Aqueous Solution
Abstract Hydrogenases are a diverse group of metalloenzymes which catalyze the reversible conversion between molecular hydrogen and protons at high rates. The catalytic activity of these enzymes does not require overpotential because their active site has been evolutionarily optimized to operate fast and efficiently. These enzymes have inspired the development of molecular catalysts, which have dramatically improved in efficiency in recent years, to the point that some synthetic catalysts even outperform hydrogenases under certain conditions. In this work, we use a reversible noble‐metal‐free homogeneous catalyst, the [Ni(P Cy 2 N Phe 2 ) 2 ] 2+ complex, and we covalently immobilize it on a functionalized highly oriented pyrolytic graphite “edge” (HOPG e ) electrode surface. This catalyst is not water soluble, but once it is surface‐confined on the electrode, it maintains its catalytic properties in aqueous solutions, showing reversibility for H 2 oxidation/reduction. Immobilization of the [Ni(P Cy 2 N Phe 2 ) 2 ] 2+ complex onto a multi‐walled carbon nanotubes coated electrode leads to even higher catalytic current densities and enhanced stability.
Carbon Fiber Reinforced Epoxy Vitrimer: Robust Mechanical Performance and Facile Hydrothermal Decomposition in Pure Water
Conventional carbon fiber reinforced thermosetting polymers (CFRPs) are neither recyclable nor repairable due to their crosslinked network. The rapid growing CFRP market raises a serious concern of the waste management. In this work, a viable method to develop a readily recyclable CFRP based on epoxy vitrimer is introduced. First, a self-catalytic epoxy prepolymer with built-in hydroxy and tertiary amine groups is designed, which upon reaction with an anhydride formed a catalyst-free epoxy vitrimer. The epoxy prepolymer is synthesized from a diamine and an excess of bisphenol A epoxy resin. The hydroxyls and tertiary amines of the epoxy prepolymer efficiently catalyze both curing and the dynamic transesterification of the crosslinked polymer without the need of a catalyst. Then, the epoxy vitrimer is used as the matrix resin to prepare CFRP. The resulting CFRP exhibited a tensile strength as high as 356 MPa. More interestingly, the matrix of the CFRP is efficiently degraded in pure water at above 160 °C. This is because the built-in tertiary amines catalyze the hydrolysis of the ester bonds of the crosslinked network. The simple method developed in this work provides a framework for the development of recyclable CFRP.
New prospects for PV powered water desalination plants: case studies in Saudi Arabia: New prospects for PV powered water desalination plants
Increased water demand and increased drought episodes in the Middle East and other regions necessitate an expansion in desalination projects and create a great market opportunity for photovoltaics (PV). PV-powered desalination has previously been regarded as not being a cost-competitive solution when compared with conventionally powered desalination; however, the decline in PV costs over the last few years has changed this outlook. Here, this article presents up-to-date performance and cost analysis of reverse osmosis (RO) desalination powered with PV connected to the Saudi Arabian grid. Reference cases include relatively small (i.e., producing 6550 m 3 water per day) and large (i.e., 190 000 m 3 /day) desalination plants using seawater at a salinity of 40 000 ppm. We used data from a King Abdullah University for Science and Technology presentation and Hybrid Optimization Model for Electric Renewables 2.81 Energy Modeling Software (HOMER Energy LLC) in tandem with Desalination Economic Evaluation Program 4.0 (International Atomic Energy Agency) desalination software to analyze the techno-economic feasibility of these plants. The first phase of our work entailed a comparison between dual-axis high concentration PV (CPV) equipped with triple junction III/V solar cells and CdTe PV-powered RO systems. The estimated levelized cost of electricity from CPV is 0.16/kWh dollars, whereas that from CdTe PV is $0.10/kWh dollars and 0.09/kWh dollars for fixed-tilt and one-axis tracking systems, respectively. These costs are higher than the price of diesel-based grid electricity in the region because diesel fuel is heavily subsidized in Saudi Arabia.
Sorption-enhanced synthetic natural gas (SNG) production from syngas: A novel process combining CO methanation, water-gas shift, and CO2 capture
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Investigation of the structural environment of Ta in a silicate glass and water system under high P–T conditions
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Nanostructure of metallic particles in light water reactor used nuclear fuel
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Investigation of water assisted phase transformation process from AlPO4-5 to AlPO4-tridymite
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Multi-decade high-resolution regional hindcasts for wave energy resource characterization in U.S. coastal waters
Long-term, high-resolution, regional wave hindcast datasets were generated using unstructured-grid Simulating WAves Nearshore (SWAN) models for the U.S. coastal waters to support nearshore wave energy development in the U.S. including those bordering U.S. territorial islands. The model domains resolved the entire U.S. exclusive economic zones, with a spatial resolution of approximately 200 m nearshore. The regional SWAN models were driven by the global WAVEWATCH III® model outputs and run for a 42-year period from 1979 to 2020. Extensive model validations were performed using buoy observations and altimeter data. Regional resource characterization was performed based on hindcast data points at 2 km from shore and along the 100 m isobath. Aggregations of wave resource parameters were produced, and spatial and seasonal variations were analyzed for all the regions. Wave resource metrics recommended by international standards, including a 3-hour time series of six resource parameters, hourly frequency- and directionally resolved wave spectra at selected “virtual buoy” locations, and average-annual values of omni-directional wave power, significant wave height, and energy period are publicly disseminated through an Amazon Web Service and a Marine Energy Atlas web application tool to facilitate wave energy research and a wide range of coastal ocean applications.
Characterization of iron oxide nanoparticle films at the air–water interface in Arctic tundra waters
Here, massive amounts of organic carbon have accumulated in Arctic permafrost and soils due to anoxic and low temperature conditions that limit aerobic microbial respiration. Alternative electron acceptors are thus required for microbes to degrade organic carbon in these soils. Iron or iron oxides have been recognized to play an important role in carbon cycle processes in Arctic soils, although the exact form and role as an electron acceptor or donor remain poorly understood. Here, Arctic biofilms collected during the summers of 2016 and 2017 from tundra surface waters on the Seward Peninsula of western Alaska were characterized with a suite of microscopic and spectroscopic methods. We hypothesized that these films contain redox-active minerals bound to biological polymers. The major components of the films were found to be iron oxide nanoparticle aggregates associated with extracellular polymeric substances. The observed mineral phases varied between films collected in different years with magnetite (Fe 2+ Fe 2 3+ O 4 ) nanoparticles (<5 nm) predominantly identified in the 2016 films, while for films collected in 2017 ferrihydrite-like amorphous iron oxyhydroxides were found. While the exact formation mechanism of these Artic iron oxide films remains to be explored, the presence of magnetite and other iron oxide/oxyhydroxide nanoparticles at the air–water interface may represent a previously unknown source of electron acceptors for continual anaerobic microbial respiration of organic carbon within poorly drained Arctic tundra.
Examinations of Oxidation and Sulfidation of Grain Boundaries in Alloy 600 Exposed to Simulated Pressurized Water Reactor Primary Water
High-resolution characterizations of intergranular attack in alloy 600 (Ni-17Cr-9Fe) exposed to 325 °C simulated pressurized water reactor (PWR) primary water have been conducted using a combination of scanning electron microscopy, NanoSIMS, analytical transmission electron microscopy and atom probe tomography. The intergranular attack exhibited a two-stage microstructure that consisted of continuous corrosion/oxidation to a depth of ~200 nm from the surface followed by discrete Cr-rich sulfides to a further depth of ~500 nm. The continuous oxidation region contained primarily nanocrystalline MO-structure oxide particles and ended at Ni-rich, Cr-depleted grain boundaries with spaced CrS precipitates. Three-dimensional characterization of the sulfidized region using site-specific atom probe tomography revealed extraordinary grain boundary composition changes, including total depletion of Cr across a several nm wide dealloyed zone as a result of grain boundary migration.
Interstitial Lithium Doping in BiVO4 Thin Film Photoanode for Enhanced Solar Water Splitting Activity
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First-Principles Modeling of Sodium Ion and Water Intercalation into Titanium Disulfide Interlayers for Water Desalination
Recent experiments revealed the possibility of using titanium disulfide (TiS 2 ) as the cathode material in capacitive deionization (CDI) devices for water desalination. Although it performed stably up to 70 cycles with a salt removal capacity of 14 mg/g (corresponding to a sodium ion removal capacity of 35.8 mg/g) at high molar concentration (600 mM NaCl), the maximum capacity of TiS 2 as a CDI electrode was much lower (~70 mAh/g) than as a supercapacitor (239 mAh/g). Understanding why the ion capacities of these two configurations of the same material differ will entail elucidating detailed charge/discharge mechanisms at the atomic scale. Here, we present density functional theory simulations of sodium intercalation into TiS 2 interlayers in order to gain such understanding. We systematically investigated TiS 2 stacking patterns and ion intercalation sites, energetics of the intercalated compounds, and phase transformation during sodium intercalation. The calculated structural evolution and capacitance–voltage curve agree quite well with previous measurements. We conclude that the different maximum capacities of TiS 2 measured in aqueous and dry environments originate from weaker interlayer interactions with respect to shear strain after ~33% intercalation of Na + –H 2 O pairs, which is detrimental to the mechanical stability of TiS 2 . In conclusion, this study sheds light on the underlying mechanisms of ion intercalation into layered materials and contributes to understanding requirements for future design and optimization of CDI electrode materials for water desalination.
Gas Production from Hot Water Circulation through Hydraulic Fractures in Methane Hydrate-Bearing Sediments: THC-Coupled Simulation of Production Mechanisms
Methane hydrates, widely found in permafrost and deep marine sediments, have great potential as a future energy 6 source. Conventional production schemes perform poorly for challenging hydrate reservoirs with low permeability. We propose an 7 efficient production scheme by combining hydraulic fracturing from horizontal wells and hot water circulation through fractures. A 8 fully coupled thermo-hydro-chemical (THC) model is developed to simulate the key physical processes during gas production from 9 a hydrate reservoir representative of typical geological settings in Shenhu, South China Sea. We found that the gas production 10 process has two distinct stages divided by thermal breakthrough: a relatively short prebreakthrough stage and a postbreakthrough 11 stage yielding stable gas production. Heat advection along and near the hydraulic fracture dominates the prebreakthrough stage, 12 whereas conduction-driven thermal recovery in the volume around fractures dominates the postbreakthrough stage. We identified 13 that the steady-state injection temperature has a strong effect on the performance of the proposed scheme while the fluid mass 14 circulation rate has a moderate impact beyond a threshold. The proposed scheme proves to be efficient and robust over a range of 15 reservoir conditions with respect to initial hydrate saturation and intrinsic permeability, including their spatial heterogeneities, 16 thereby offering a promising solution for challenging reservoir conditions.
Uranium redistribution due to water table fluctuations in sandy wetland mesocosms
In order to better understand the fate and stability of immobilized uranium (U) in wetland sediments, and how intermittent dry periods affect U stability, we dosed saturated wetland mesocosms planted with Scirpus acutus with low levels of uranyl acetate for 4 months before imposing a short drying and rewetting period. Concentrations of U in mesocosm effluent increased after drying and rewetting, but the cumulative amount of U released following the dry period constituted less than 1% of the total U immobilized in the soil during the 4 months prior. This low level of remobilization suggests, and XAS analyses confirm, that microbial reduction was not the primary means of U immobilization, as the U immobilized in mesocosms was primarily U(VI) rather than U(IV). Drying followed by re-wetting caused a redistribution of U downward in the soil profile and on to root surfaces. While the U on roots before drying was primarily associated with minerals, the U that relocated to the roots during drying and rewetting was bound diffusely to root surfaces. Results show that short periods of drought conditions in a wetland, which expose reduced sediments to air, may impact U distribution, but these conditions may not cause large releases of soil-bound U from planted wetlands to surface waters.