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Tropical cyclones (TC) provide an important source of mixing for the upper ocean, bringing cold, nutrient-rich water to the surface and triggering phytoplankton blooms. TCs are changing in response to global warming, yet the impacts of those changes on the upper ocean are poorly known. Here we show a significant increasing trend in global TC-induced sea surface temperature (SST) cooling of 0.054oC per decade since 1982. The enhanced cooling has been driven primarily by an increase in the intensity of strong TCs (maximum wind speed > 33 m s-1) and associated strengthening of TC-induced mixing. Consistent with the enhanced mixing and SST cooling, we find a significant increase in TC-induced surface chlorophyll-a concentration of 3.7 x 10-3 mg m-3 per decade in oligotrophic areas. This enhancement of oceanic primary production by TCs is expected to partially offset its projected global decline under climate change.
Layered molybdenum disulfide has demonstrated great promise as a low-cost alternative to platinum-based catalysts for electrochemical hydrogen production from water. Research effort on this material has focused mainly on synthesizing highly nanostructured molybdenum disulfide that allows the exposure of a large fraction of active edge sites. Here we report a promising microwave-assisted strategy for the synthesis of narrow molybdenum disulfide nanosheets with edge-terminated structure and a significantly expanded interlayer spacing, which exhibit striking kinetic metrics with onset potential of -103 mV, Tafel slope of 49 mV per decade and exchange current density of 9.62 × 10-3 mA cm-2, performing among the best of current molybdenum disulfide catalysts. Besides benefits from the edge-terminated structure, the expanded interlayer distance with modified electronic structure is also responsible for the observed catalytic improvement, which suggests a potential way to design newly advanced molybdenum disulfide catalysts through modulating the interlayer distance.
Here, three-dimensional (3D) monodispersed sea urchin-like Ru-doped rutile TiO 2 hierarchical architectures composed of radially aligned, densely-packed TiO 2 nanorods have been successfully synthesized via an acid-hydrothermal method at low temperature without the assistance of any structure-directing agent and post annealing treatment. The addition of a minuscule concentration of ruthenium dopants remarkably catalyzes the formation of the 3D urchin structure and drives the enhanced photocatalytic H 2 production under visible light irradiation, not possible on undoped and bulk rutile TiO 2 . Increasing ruthenium doping dosage not only increases the surface area up to 166 m 2 g –1 but also induces enhanced photoresponse in the regime of visible and near infrared light. The doping introduces defect impurity levels, i.e. oxygen vacancy and under-coordinated Ti 3+ , significantly below the conduction band of TiO 2 , and ruthenium species act as electron donors/acceptors that accelerate the photogenerated hole and electron transfer and efficiently suppress the rapid charge recombination, therefore improving the visible-light-driven activity.
Alkylated mercury species (monomethylmercury, MeHg, and dimethylmercury, DMeHg) exhibit significant bioaccumulation, and pose significant risks to ecosystems and human health. Although decades of research have been devoted to understanding MeHg formation and degradation, little is known about the DMeHg formation in aquatic systems. Here, we combine complementary experimental and computational approaches to examine MeHg speciation and DMeHg formation in sulfidic aqueous solutions, with an emphasis on the formation and decomposition of the binuclear bis(methylmercuric(II)) sulfide complex (CH 3 Hg) 2 S. Experimental data indicate that the reaction 2CH 3 Hg + + HS- $→\atop{←}$ (CH 3 Hg) 2 S + H + has a log K = 26.0 ± 0.2. Thus, the binuclear (CH 3 Hg) 2 S complex is likely to be the dominant MeHg species under high MeHg concentrations typically used in experimental investigations of MeHg degradation by sulfate-reducing bacteria (SRB). Our finding of a significant abiotic removal mechanism for MeHg in sulfidic solutions through the formation of relatively insoluble (CH 3 Hg) 2 S suggests careful reexamination of reported “oxidative demethylation” of MeHg by SRB and perhaps other obligate anaerobes. We provide evidence for slow decomposition of (CH 3 Hg) 2 S to DMeHg and HgS, with a first-order rate constant k = 1.5 ± 0.4 × 10 -6 h -1 . Quantum chemical calculations suggest that the reaction proceeds by a novel mechanism involving rearrangement of the (CH 3 Hg) 2 S complex facilitated by strong Hg–Hg interactions that activate a methyl group for intramolecular transfer. Predictions of DMeHg formation rates under a variety of field and laboratory conditions indicate that this pathway for DMeHg formation will be significant in laboratory experiments utilizing high MeHg concentrations, favoring (CH 3 Hg) 2 S formation. Finally, in natural systems with relatively high MeHg/[H 2 S] T ratios (the oxic/anoxic interface, for example), DMeHg production may be observed, and warrants further investigation.
We recently reported biomass-derived tetrahydrofuran-2,5-dicarboxylic acid (THFDCA) as a potential renewable feedstock for adipic acid (AA) production by combining HI and molecular H 2 in organic acid solvents.
Ultra-rapid biohydrogen production from water splitting energized by a natural energy storage compound starch with an artificial enzymatic biosystem.
The relationship between noble metal phase particles and fission gas bubble production in used nuclear fuel is described. The majority of Te atoms within noble metal phase undergo radioactive decay to form stable Xe within a few hours after particle formation. This results in the production of clusters of Xe atoms contained within the solid metal matrix exhibiting an equivalent gas bubble pressure approaching 1 GPa. These high pressure bubbles are stabilized by the UO2 within the bulk of the fuel. However, when these bubbles form near the fuel / cladding interface, in combination with local and temporal damage caused by fission recoil, they are capable of overcoming the fracture strength of the UO2 and rupturing catastrophically. The force of the resulting bubble rupture is sufficient to eject noble metal phase particles several microns into the cladding. This proposed mechanism explains the observance of noble metal phase in cladding and is consistent with a host of morphological features found near the fuel / cladding interface.
Stepwise process of cellulose being hydrolyzed into oligomers in MSH followed by product separation.
The hydrogenase maturase HydG produces multiple equivalents of free CO and CN - during catalysis. This production correlates with the activation of hydrogenase, supporting a model in which free CO and CN - are relevant to maturation.
Building a stronger bioeconomy requires production capabilities that are largely generated through microbial genetic engineering. Plant feedstocks can additionally be genetically engineered to generate desirable feedstock traits and provide precursors for direct microbial conversion into desired products. The oleaginous yeast Rhodosporidium toruloides is a promising organism for this type of conversion as it can grow on a wide range of deconstructed biomass and consume a variety of carbon sources. Here, we leveraged R. toruloides native p-coumaric acid consumption pathway to accumulate protocatechuate (PCA) from 4-hydroxybenzoate (4HBA) released from a sorghum feedstock line genetically engineered to overproduce 4HBA. We did so by generating and evaluating an R. toruloides strain that accumulates PCA, RSΔ12623. We then show that at two scales a cholinium lysinate pretreatment with enzymatic saccharification successfully extracts 95% of the 4HBA from the engineered sorghum biomass while producing deconstructed lignin that can be more efficiently depolymerized in a subsequent thermochemical reaction. We also demonstrate that strain RSΔ12623 can convert more than 95% of 4HBA to PCA while consuming >95% of the glucose and >80% of the xylose present in sorghum hydrolysates. Finally, to evaluate the scalability of such fermentations, we conducted the conversion of 4HBA to PCA in a 2 L bioreactor under controlled conditions. Importantly, this work demonstrates the potential of purposefully producing aromatic precursors in planta that can be liberated during biomass deconstruction for direct microbial conversion to desirable bioproducts.
Measurements of hadronic resonances produced in photoproduction reactions at Jefferson Lab are shown and discussed. Emphasis is placed on the production of the excited hyperon states Sigma(1385), Lambda(1405), and Lambda(1520). Some future prospects for the upcoming Jefferson Lab 12 GeV era are given, where the CLAS12 and GlueX detectors will see unprecedented amounts of data using electromagnetic probes and further our knowledge of hadronic resonances.
The performance of new iron-based laser-driven x-ray sources has been tested at the OMEGA laser facility for production of x rays in the 6.5-8.5 keV range. Two types of targets were experimentally investigated: low-density iron oxide aerogels (density 6-16 mg/cm{sup 3}) and stainless steel foil-lined cavity targets (steel thickness 1-5 {mu}m). The targets were irradiated by 40 beams of the OMEGA laser (500 J/beam, 1 ns pulse, wavelength 351 nm). All targets showed good coupling with the laser, with <5% of the incident laser light backscattered by the resulting plasma in all cases (typically <2.5%). The aerogel targets produced T{sub e}=2 to 3 keV, n{sub e}=0.12-0.2 critical density plasmas yielding a 40%-60% laser-to-x-ray total conversion efficiency (CE) (1.2%-3% in the Fe K-shell range). The foil cavity targets produced T{sub e}{approx} 2 keV, n{sub e}{approx} 0.15 critical density plasmas yielding a 60%-75% conversion efficiency (1.6%-2.2% in the Fe K-shell range). Time-resolved images illustrate that the volumetric heating of low-density aerogels allow them to emit a higher K-shell x-ray yield even though they contain fewer Fe atoms. However, their challenging fabrication process leads to a larger shot-to-shot variation than cavity targets.
Quantum state-to-state dynamics of a prototypical four-atom reaction, namely, Cl + H{sub 2}O → HCl + OH, is investigated for the first time in full dimensionality using a transition-state wave packet method. The state-to-state reactivity and its dependence on the reactant internal excitations are analyzed and found to share many similarities both energetically and dynamically with the H + H{sub 2}O → H{sub 2} + OH reaction. The strong enhancement of reactivity by the H{sub 2}O stretching vibrational excitations in both reactions is attributed to the favorable energy flow into the reaction coordinate near the transition state. On the other hand, the insensitivity of the product state distributions with regard to reactant internal excitation stems apparently from the transition-state control of product energy disposal.
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Microalgae have potential to help meet energy and food demands without exacerbating environmental problems. There is interest in the unicellular green alga Chromochloris zofingiensis, because it produces lipids for biofuels and a highly valuable carotenoid nutraceutical, astaxanthin. Here, to advance understanding of its biology and facilitate commercial development, we present a C. zofingiensis chromosome-level nuclear genome, organelle genomes, and transcriptome from diverse growth conditions. The assembly, derived from a combination of short- and long-read sequencing in conjunction with optical mapping, revealed a compact genome of ~58 Mbp distributed over 19 chromosomes containing 15,274 predicted protein-coding genes. The genome has uniform gene density over chromosomes, low repetitive sequence content (~6%), and a high fraction of protein-coding sequence (~39%) with relatively long coding exons and few coding introns. Functional annotation of gene models identified orthologous families for the majority (~73%) of genes. Synteny analysis uncovered localized but scrambled blocks of genes in putative orthologous relationships with other green algae. Two genes encoding beta-ketolase (BKT), the key enzyme synthesizing astaxanthin, were found in the genome, and both were up-regulated by high light. Isolation and molecular analysis of astaxanthin-deficient mutants showed that BKT1 is required for the production of astaxanthin. Moreover, the transcriptome under high light exposure revealed candidate genes that could be involved in critical yet missing steps of astaxanthin biosynthesis, including ABC transporters, cytochrome P450 enzymes, and an acyltransferase. Finally, the high-quality genome and transcriptome provide insight into the green algal lineage and carotenoid production.
Pseudomonas aeruginosa is an opportunistic human pathogen that secretes the exopolysaccharide alginate during infection of the respiratory tract of individuals afflicted with cystic fibrosis and chronic obstructive pulmonary disease. Among the proteins required for alginate production, Alg44 has been identified as an inner membrane protein whose bis-(3',5')-cyclic dimeric guanosine monophosphate (c-di-GMP) binding activity post-translationally regulates alginate secretion. In this study, we report the 1.8 Å crystal structure of the cytoplasmic region of Alg44 in complex with dimeric self-intercalated c-di-GMP and characterize its dinucleotide-binding site using mutational analysis. The structure shows that the c-di-GMP binding region of Alg44 adopts a PilZ domain fold with a dimerization mode not previously observed for this family of proteins. Moreover, calorimetric binding analysis of residues in the c-di-GMP binding site demonstrate that mutation of Arg-17 and Arg-95 alters the binding stoichiometry between c-di-GMP and Alg44 from 2:1 to 1:1. Introduction of these mutant alleles on the P. aeruginosa chromosome show that the residues required for binding of dimeric c-di-GMP in vitro are also required for efficient alginate production in vivo. Our results suggest that the dimeric form of c-di-GMP represents the biologically active signaling molecule needed for the secretion of an important virulence factor produced by P. aeruginosa.
An alternative target design with potential improvements, including a major increase in 238 Pu production rate and annual capacity; fewer targets to be fabricated, irradiated, and processed; and a significant replacement of a large volume of caustic-nitrate, aluminum-bearing radioactive liquid waste with a smaller volume of solid metal waste, has been conceived and evaluated using reactor physics and thermal-hydraulic analyses. The alternative target design uses pressed pellets of 237 NpO 2 , sintered to 92% to 93% of theoretical density, and stacked inside a Zircaloy-4 cladding tube. Additionally, four test targets were fabricated, irradiated, and examined. No melting or other potential problems were indicated. Projections from measured constituents indicated annual production could be increased by a factor of ~2, and the number of targets required to be fabricated, irradiated, and processed could be reduced by a factor of ~5.