120 research outputs found

    Investigation of Noncovalent Complexes Between β-Cyclodextrin and Polyamide Acids Containing N-Methylpyrrole and N-Methylimidazole by Electrospray Ionization Mass Spectrometry

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    Electrospray ionization (ESI) mass spectrometry was utilized to investigate noncovalent complexes between β-cyclodextrin (β-CD) and five novel polyamide acids containing N-methylpyrrole and N-methylimidazole. The 1:1 binding mode was specified by examining the binding stoichiometry from ESI mass spectra. It found that polyamide acids with β-CD have binding affinities in the order: ImImImβCOOH > ImPyImβCOOH > ImPyPyβCOOH > PyPyPyβCOOH > NO2PyPyPyβCOOH. The method gives, simultaneously, the binding constants between β-CD and polyamide acids based on a novel linear equation

    Self-assembled carbon nanoribbons with the heteroatom doping used as ultrafast charging cathodes in zinc-ion hybrid supercapacitors

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    Zinc-ion hybrid supercapacitors (ZHSs) are highly desirable for large-scale energy storage applications owing to the merits of high safety, low cost and ultra-long cycle life. The poor rate performance of cathodes, however, severely hinders their application. Herein, aqueous ZHSs with superior performance were fabricated by employing a series of ultrathin carbon nanobelts modified with B, N, O (CPTHB-Bx). The heteroatom doping can significantly modify the chemical behaviors of carbon frameworks, which could generate numerous active sites and accelerate the charge transport. The systematic investigation reveals that the B–N groups are active species for fast Zn-ion adsorption and desorption. As a result, the best-performed CPTHB-B2 exhibits an excellent electrochemical performance as cathodes in ZHSs, delivering a high specific capacitance of 415.3 F g−1 at 0.5 A g−1, a record high capacitance retention of 81% when increasing the current densities from 0.5 to 100 A g−1, an outstanding energy density of 131.9 W h kg−1 and an exceptionally high power density of 42.1 kW kg−1. Our work provides a new cathode design for ultrafast charging Zn-ion storage devices

    Multilayered Molybdate Microflowers Fabricated by One-Pot Reaction for Efficient Water Splitting

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    The development of high-performance, low-cost and rapid-production bifunctional electrocatalysts towards overall water splitting still poses huge challenges. Herein, the authors utilize a facile hydrothermal method to synthesize a novel structure of Co-doped ammonium lanthanum molybdate on Ni foams (Co-ALMO@NF) as self-supported electrocatalysts. Owing to large active surfaces, lattice defect and conductive channel for rapid charge transport, Co-ALMO@NF exhibits good electrocatalytic performances which requires only 349/341 mV to achieve a high current density of 600 mA cm-2 for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. Besides, a low cell voltage of 1.52 V is required to reach the current density of 10 mA cm-2 in alkaline medium along with an excellent long-term stability for two-electrode configurations. Density functional theory calculations are performed to reveal the reaction mechanism on Co-ALMO@NF, which shows that the Mo site is the most favorable ones for HER, while the introduction of Co is beneficial to reduce the adsorption intensity on the surface of Co-ALMO@NF, thus accelerating OER process. This work highlighted the importance of the structural design for self-supporting electrocatalysts

    Supplemental Information 4: Multicolor FACS analyses of cultured DC cells

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    This study investigated the mechanism of protein disulfide-isomerase A3 (PDIA3)-induced visceral hypersensitivity in irritable bowel syndrome (IBS). Rats were treated with saline (control), acetic acid and restraint stress (IBS model), empty vector (RNAi control) and PDIA3-RNAi vector (PDIA3-RNAi). Mesenteric lymph node DCs (MLNDCs) and splenic CD4+/CD8+ T cells were isolated for co-cultivation. Compared with control, MLNDCs co-cultured with CD4+ or CD8+ T cells showed an increased ability to promote T cell proliferation and produced more IL-4 or IL-9 secretion. Compared with the RNAi control, MLNDCs from the PDIA3 knockdown models were less effective in promoting the proliferation of CD4+/CD8+ T cells. It is concluded that PDIA3 plays an important role in the development of IBS through the DC-mediated activation of T cells, resulting in degranulation of MCs and visceral hypersensitivity

    How much Arctic fresh water participates in the subpolar overturning circulation?

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    Fresh Arctic waters flowing into the Atlantic are thought to have two primary fates. They may be mixed into the deep ocean as part of the overturning circulation, or flow alongside regions of deep water formation without impacting overturning. Climate models suggest that as increasing amounts of fresh water enter the Atlantic, the overturning circulation will be disrupted, yet we lack an understanding of how much fresh water is mixed into the overturning circulation’s deep limb in the present day. To constrain these fresh water pathways, we build steady-state volume, salt, and heat budgets east of Greenland that are initialized with observations and closed using inverse methods. Fresh water sources are split into oceanic Polar Waters from the Arctic and surface fresh water fluxes, which include net precipitation, runoff, and ice melt, to examine how they imprint the circulation differently. We find that 65 mSv of the total 110 mSv of surface fresh water fluxes that enter our domain participate in the overturning circulation, as do 0.6 Sv of the total 1.2 Sv of Polar Waters that flow through Fram Strait. Based on these results, we hypothesize that the overturning circulation is more sensitive to future changes in Arctic fresh water outflow and precipitation, while Greenland runoff and iceberg melt are more likely to stay along the coast of Greenland

    Local and downstream relationships between Labrador Sea Water volume and North Atlantic meridional overturning circulation variability

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    While it has generally been understood that the production of Labrador Sea Water (LSW) impacts the Atlantic meridional overturning circulation (MOC), this relationship has not been explored extensively nor validated against observations. To explore this relationship, a suite of global ocean and ocean–sea-ice models forced by the same interannually-varying atmospheric dataset, varying in resolution from non-eddy-permitting to eddy-permitting (1°–1/4°), is analyzed to investigate the local and downstream relationships between LSW formation and the MOC on interannual to decadal time scales. While all models display a strong relationship between changes in the LSW volume and the MOC in the Labrador Sea, this relationship degrades considerably downstream of the Labrador Sea. In particular, there is no consistent pattern among the models in the North Atlantic subtropical basin over interannual to decadal time scales. Furthermore, the strong response of the MOC in the Labrador Sea to LSW volume changes in that basin may be biased by the overproduction of LSW in many models compared to observations. This analysis shows that changes in LSW volume in the Labrador Sea cannot be clearly and consistently linked to a coherent MOC response across latitudes over interannual to decadal time scales in ocean hindcast simulations of the last half-century. Similarly, no coherent relationships are identified between the MOC and the Labrador Sea mixed layer depth or the density of newly formed LSW across latitudes or across models over interannual to decadal time scales

    Insights on Flexible Zinc‐Ion Batteries from Lab Research to Commercialization

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    Owing to the development of aqueous rechargeable zinc-ion batteries (ZIBs), flexible ZIBs are deemed as potential candidates to power wearable electronics. ZIBs with solid-state polymer electrolytes can not only maintain additional load-bearing properties, but exhibit enhanced electrochemical properties by preventing dendrite formation and inhibiting cathode dissolution. Substantial efforts have been applied to polymer electrolytes by developing solid polymer electrolytes, hydrogel polymer electrolytes, and hybrid polymer electrolytes; however, the research of polymer electrolytes for ZIBs is still immature. Herein, the recent progress in polymer electrolytes is summarized by category for flexible ZIBs, especially hydrogel electrolytes, including their synthesis and characterization. Aiming to provide an insight from lab research to commercialization, the relevant challenges, device configurations, and life cycle analysis are consolidated. As flexible batteries, the majority of polymer electrolytes exploited so far only emphasizes the electrochemical performance but the mechanical behavior and interactions with the electrode materials have hardly been considered. Hence, strategies of combining softness and strength and the integration with electrodes are discussed for flexible ZIBs. A ranking index, combining both electrochemical and mechanical properties, is introduced. Future research directions are also covered to guide research toward the commercialization of flexible ZIBs

    Distinct sources of interannual subtropical and subpolar Atlantic overturning variability

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    The Atlantic meridional overturning circulation (AMOC) is pivotal for regional and global climate due to its key role in the uptake and redistribution of heat and carbon. Establishing the causes of historical variability in AMOC strength on different timescales can tell us how the circulation may respond to natural and anthropogenic changes at the ocean surface. However, understanding observed AMOC variability is challenging because the circulation is influenced by multiple factors that co-vary and whose overlapping impacts persist for years. Here we reconstruct and unambiguously attribute intermonthly and interannual AMOC variability at two observational arrays to the recent history of surface wind stress, temperature and salinity. We use a state-of-the-art technique that computes space- and time-varying sensitivity patterns of the AMOC strength with respect to multiple surface properties from a numerical ocean circulation model constrained by observations. While, on interannual timescales, AMOC variability at 26° N is overwhelmingly dominated by a linear response to local wind stress, overturning variability at subpolar latitudes is generated by the combined effects of wind stress and surface buoyancy anomalies. Our analysis provides a quantitative attribution of subpolar AMOC variability to temperature, salinity and wind anomalies at the ocean surface

    Overturning in the Subpolar North Atlantic Program: A New International Ocean Observing System

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    For decades oceanographers have understood the Atlantic meridional overturning circulation (AMOC) to be primarily driven by changes in the production of deep-water formation in the subpolar and subarctic North Atlantic. Indeed, current Intergovernmental Panel on Climate Change (IPCC) projections of an AMOC slowdown in the twenty-first century based on climate models are attributed to the inhibition of deep convection in the North Atlantic. However, observational evidence for this linkage has been elusive: there has been no clear demonstration of AMOC variability in response to changes in deep-water formation. The motivation for understanding this linkage is compelling, since the overturning circulation has been shown to sequester heat and anthropogenic carbon in the deep ocean. Furthermore, AMOC variability is expected to impact this sequestration as well as have consequences for regional and global climates through its effect on the poleward transport of warm water. Motivated by the need for a mechanistic understanding of the AMOC, an international community has assembled an observing system, Overturning in the Subpolar North Atlantic Program (OSNAP), to provide a continuous record of the transbasin fluxes of heat, mass, and freshwater, and to link that record to convective activity and water mass transformation at high latitudes. OSNAP, in conjunction with the Rapid Climate Change–Meridional Overturning Circulation and Heatflux Array (RAPID–MOCHA) at 26°N and other observational elements, will provide a comprehensive measure of the three-dimensional AMOC and an understanding of what drives its variability. The OSNAP observing system was fully deployed in the summer of 2014, and the first OSNAP data products are expected in the fall of 2017
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