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1.
Polarization-sensitive photodetection is central to optics applications and has been successfully demonstrated in photodetectors of two-dimensional (2D) materials, such as layered hybrid perovskites; however, achieving high polarization sensitivity in such a photodetector remains extremely challenging. Here, for the first time, we demonstrate a high-performance polarization-sensitive photodetector using single-crystalline 2D/3D perovskite heterostructure, namely, (4-AMP)(MA)2Pb3Br10/MAPbBr3 (MA = methylammonium; 4-AMP = 4-(aminomethyl)piperidinium), which exhibits ultrahigh polarization sensitivity up to 17.6 under self-driven mode. To our knowledge, such a high polarization selectivity has surpassed all of the reported perovskite-based devices, and is comparable to, or even better than, the traditional inorganic heterostructure-based photodetectors. Further studies reveal that the built-in electric field formed at the junction can spatially separate the photogenerated electrons and holes, reducing their recombination rate and thus enhancing the performance for polarization-sensitive photodetection. This work provides a new source of polarization-sensitive materials and insights into designing novel optoelectronic devices.  相似文献   

2.
Designing new cathodes with high capacity and moderate potential is the key to breaking the energy density ceiling imposed by current intercalation chemistry on rechargeable batteries. The carbonaceous materials provide high capacities but their low potentials limit their application to anodes. Here, we show that Fermi level tuning by p-type doping can be an effective way of dramatically raising electrode potential. We demonstrate that Li(Na)BCF2/Li(Na)B2C2F2 exhibit such change in Fermi level, enabling them to accommodate Li+(Na+) with capacities of 290–400 (250–320) mAh g−1 at potentials of 3.4–3.7 (2.7–2.9) V, delivering ultrahigh energy densities of 1000–1500 Wh kg−1. This work presents a new strategy in tuning electrode potential through electronic band structure engineering.  相似文献   

3.
The superconductivity of hydrides under high pressure has attracted a great deal of attention since the recent observation of the superconducting transition at 203 K in strongly compressed H2S. It has been realized that the stoichiometry of hydrides might change under high pressure, which is crucial in understanding the superconducting mechanism. In this study, PH3 was studied to understand its superconducting transition and stoichiometry under high pressure using Raman, IR and X-ray diffraction measurements, as well as theoretical calculations. PH3 is stable below 11.7 GPa and then it starts to dehydrogenate through two dimerization processes at room temperature and pressures up to 25 GPa. Two resulting phosphorus hydrides, P2H4 and P4H6, were verified experimentally and can be recovered to ambient pressure. Under further compression above 35 GPa, the P4H6 directly decomposed into elemental phosphorus. Low temperature can greatly hinder polymerization/decomposition under high pressure and retains P4H6 up to at least 205 GPa. The superconductivity transition temperature of P4H6 is predicted to be 67 K at 200 GPa, which agrees with the reported result, suggesting that it might be responsible for superconductivity at higher pressures. Our results clearly show that P2H4 and P4H6 are the only stable P–H compounds between PH3 and elemental phosphorus, which is helpful for shedding light on the superconducting mechanism.  相似文献   

4.
The present study was designed to understand the cigarette smoking-induced alterations in hormones and the resulting changes in platelet serotonin (5-hydroxytryptamine, 5-HT) and monoamine oxidase (MAO-B) activity in chronic smokers. Human male volunteers aged 35 ± 8 years, were divided into two groups, namely controls and smokers (12 ± 2 cigarettes per day for 7–10 years). Results showed that cigarette smoking significantly (p < 0.05) elevated plasma triiodothyronine (T3), cortisol and testosterone levels with significant (p < 0.05) reduction in plasma tryptophan and thyroxin (T4). Moreover, smokers showed reduced platelet 5-HT levels and MAO-B activity. In smokers, plasma cortisol was negatively correlated with tryptophan (r = −0.386), platelet MAO-B (r = −0.264), and 5-HT (r = −0.671), and positively correlated with testosterone (r = 0.428). However, testosterone was negatively correlated with platelet MAO-B (r = −0.315), and 5-HT (r = −.419) in smokers. Further, smokers plasma T3 levels were negatively correlated with platelet MAO-B (r = −0.398), and 5-HT (r = −0.541), whereas T4 levels were positively correlated with platelet MAO-B (r = 0.369), and 5-HT (r = 0.454). In conclusion, our study showed that altered testosterone and cortisol levels may aggravate behavior, mood disturbances and symptoms of depression by decreasing platelet 5-HT and MAO-B activity in smokers.  相似文献   

5.
Most metal–organic frameworks (MOFs) hardly maintain their physical and chemical properties after exposure to alkaline aqueous solutions, thus precluding their use as potential electrode materials for electrochemical energy storage devices. Here, we present the design and synthesis of a highly alkaline-stable metal oxide@MOF composite, Co3O4 nanocube@Co-MOF (Co3O4@Co-MOF), via a controllable and facile one-pot hydrothermal method under highly alkaline conditions. The obtained composite possesses exceptional alkaline stability, retaining its original structure in 3.0 M KOH for at least 15 days. Benefitting from the exceptional alkaline stability, unique structure, and larger surface area, the Co3O4@Co-MOF composite shows a specific capacitance as high as 1020 F g−1 at 0.5 A  g−1 and a high cycling stability with only 3.3% decay after 5000 cycles at 5 A g−1. The as-constructed solid-state flexible device exhibits a maximum energy density of 21.6 mWh cm−3.  相似文献   

6.
Understanding the correlation between exposed surfaces and performances of controlled nanocatalysts can aid effective strategies to enhance electrocatalysis, but this is as yet unexplored for the nitrogen reduction reaction (NRR). Here, we first report controlled synthesis of well-defined Pt3Fe nanocrystals with tunable morphologies (nanocube, nanorod and nanowire) as ideal model electrocatalysts for investigating the NRR on different exposed facets. The detailed electrocatalytic studies reveal that the Pt3Fe nanocrystals exhibit shape-dependent NRR electrocatalysis. The optimized Pt3Fe nanowires bounded with high-index facets exhibit excellent selectivity (no N2H4 is detected), high activity with NH3 yield of 18.3 μg h−1 mg−1cat (0.52 μg h−1 cm−2ECSA; ECSA: electrochemical active surface area) and Faraday efficiency of 7.3% at −0.05 V versus reversible hydrogen electrode, outperforming the {200} facet-enclosed Pt3Fe nanocubes and {111} facet-enclosed Pt3Fe nanorods. They also show good stability with negligible activity change after five cycles. Density functional theory calculations reveal that, with high-indexed facet engineering, the Fe-3d band is an efficient d-d coupling correlation center for boosting the Pt 5d-electronic exchange and transfer activities towards the NRR.  相似文献   

7.
Nitrogen oxides (NOx, the sum of nitric oxide (NO) and N dioxide (NO2)) emissions and deposition have increased markedly over the past several decades, resulting in many adverse outcomes in both terrestrial and oceanic environments. However, because the microbial NOx emissions have been substantially underestimated on the land and unconstrained in the ocean, the global microbial NOx emissions and their importance relative to the known fossil-fuel NOx emissions remain unclear. Here we complied data on stable N isotopes of nitrate in atmospheric particulates over the land and ocean to ground-truth estimates of NOx emissions worldwide. By considering the N isotope effect of NOx transformations to particulate nitrate combined with dominant NOx emissions in the land (coal combustion, oil combustion, biomass burning and microbial N cycle) and ocean (oil combustion, microbial N cycle), we demonstrated that microbial NOx emissions account for 24 ± 4%, 58 ± 3% and 31 ± 12% in the land, ocean and global environment, respectively. Corresponding amounts of microbial NOx emissions in the land (13.6 ± 4.7 Tg N yr−1), ocean (8.8 ± 1.5 Tg N yr−1) and globe (22.5 ± 4.7 Tg N yr−1) are about 0.5, 1.4 and 0.6 times on average those of fossil-fuel NOx emissions in these sectors. Our findings provide empirical constraints on model predictions, revealing significant contributions of the microbial N cycle to regional NOx emissions into the atmospheric system, which is critical information for mitigating strategies, budgeting N deposition and evaluating the effects of atmospheric NOx loading on the world.  相似文献   

8.
Complex oxides with tunable structures have many fascinating properties, though high-quality complex oxide epitaxy with precisely controlled composition is still out of reach. Here we have successfully developed solution-based single-crystalline epitaxy for multiferroic (1-x)BiTi(1-y)/2FeyMg(1-y)/2O3–(x)CaTiO3 (BTFM–CTO) solid solution in large area, confirming its ferroelectricity at the atomic scale with strong spontaneous polarization. Careful compositional tuning leads to a bulk magnetization of 0.07 ± 0.035 μB/Fe at room temperature, enabling magnetically induced polarization switching exhibiting a large magnetoelectric coefficient of 2.7–3.0 × 10−7 s/m. This work demonstrates the great potential of solution processing in large-scale complex oxide epitaxy and establishes novel room-temperature magnetoelectric coupling in epitaxial BTFM–CTO film, making it possible to explore a much wider space of composition, phase, and structure that can be easily scaled up for industrial applications.  相似文献   

9.
MXenes are one of the key materials for micro-supercapacitors (MSCs), integrating miniaturized energy-storage components with microelectronics. However, the energy densities of MSCs are greatly hampered by MXenes’ narrow working potential window (typically ≤0.6 V) in aqueous electrolytes. Here, we report the fabrication of high-voltage MXene-MSCs through the efficient regulation of reaction kinetics in 2D Ti3C2Tx MXene microelectrodes using a water-in-LiCl (WIL, 20 m LiCl) salt gel electrolyte. Importantly, the intrinsic energy-storage mechanism of MXene microelectrodes in WIL, which is totally different from traditional electrolytes (1 m LiCl), was revealed through insitu and exsitu characterizations. We validated that the suppression of MXene oxidation at high anodic potential occurred due to the high content of WIL regulating anion intercalation in MXene electrodes, which effectively broadened the voltage window of MXene-MSCs. Remarkably, the symmetric planar MXene-MSCs presented a record operating voltage of 1.6 V, resulting in an exceptionally high volumetric energy density of 31.7 mWh cm−3. With the ultra-high ionic conductivity (69.5 mS cm−1) and ultralow freezing point (−57°C) of the WIL gel electrolyte, our MSCs could be operated in a wide temperature range of −40 to 60°C, and worked for a long duration even at −40°C, demonstrative of its practicality in extreme environments.  相似文献   

10.
Two-dimensional(2D) ferromagnetic materials have been discovered with tunable magnetism and orbital-driven nodal-line features. Controlling the 2D magnetism in exfoliated nanoflakes via electric/magnetic fields enables a boosted Curie temperature(TC) or phase transitions. One of the challenges, however, is the realization of high TC2D magnets that are tunable, robust and suitable for large scale fabrication. Here, we report molecular-beam epitaxy growth of wafer-scale Fe  相似文献   

11.
Molybdenum dinitrogen complexes supported by monodentate arylsilylamido ligand, [Ar(Me3Si)N]3MoN2Mg(THF)2[N(SiMe3)Ar] (5) and [Ar(Me3Si)N]3MoN2SiMe3 (6) (Ar = 3,5-Me2C6H3) were synthesized and structurally characterized, and proved to be effective catalysts for the disproportionation of cyclohexadienes and isomerization of terminal alkenes. The 1H NMR spectrum suggested that the bridging nitrogen ligand remains intact during the catalytic reaction, indicating possible catalytic ability of the Mo-N=N motif.  相似文献   

12.
Development of novel catalysts for nitrogen reduction at ambient pressures and temperatures with ultrahigh ammonia (NH3) yield and selectivity is challenging. In this work, an atomic catalyst with separated Pd atoms on graphdiyne (Pd-GDY) was synthesized, which shows fascinating electrocatalytic properties for nitrogen reduction. The catalyst has the highest average NH3 yield of 4.45 ± 0.30 mgNH3 mgPd−1 h−1, almost tens of orders larger than for previously reported catalysts, and 100% reaction selectivity in neutral media. Pd-GDY exhibits almost no decreases in NH3 yield and Faradaic efficiency. Density functional theory calculations show that the reaction pathway prefers to perform at the (Pd, C1, C2) active area because of the strongly coupled (Pd, C1, C2), which elevates the selectivity via enhanced electron transfer. By adjusting the p–d coupling accurately, reduction of self-activated nitrogen is promoted by anchoring atom selection, and side effects are minimized.  相似文献   

13.
Energy consumption dominates annual CO2 emissions in China. It is essential to significantly reduce CO2 emissions from energy consumption to reach national carbon neutrality by 2060, while the role of terrestrial carbon sequestration in offsetting energy-related CO2 emissions cannot be underestimated. Natural climate solutions (NCS), including improvements in terrestrial carbon sequestration, represent readily deployable options to offset anthropogenic greenhouse gas emissions. However, the extent to which China''s terrestrial carbon sequestration in the future, especially when target-oriented managements (TOMs) are implemented, can help to mitigate energy-related CO2 emissions is far from certain. By synthesizing available findings and using several parameter-sparse empirical models that have been calibrated and/or fitted against contemporary measurements, we assessed China''s terrestrial carbon sequestration over 2010–2060 and its contribution to offsetting national energy-related CO2 emissions. We show that terrestrial C sequestration in China will increase from 0.375 ± 0.056 (mean ± standard deviation) Pg C yr−1 in the 2010s to 0.458 ± 0.100 Pg C yr−1 under RCP2.6 and 0.493 ± 0.108 Pg C yr−1 under the RCP4.5 scenario in the 2050s, when TOMs are implemented. The majority of carbon sequestration comes from forest, accounting for 67.8–71.4% of the total amount. China''s terrestrial ecosystems can offset 12.2–15.0% and 13.4–17.8% of energy-related peak CO2 emissions in 2030 and 2060, respectively. The implementation of TOMs contributes 11.9% of the overall terrestrial carbon sequestration in the 2020s and 23.7% in the 2050s. The most likely strategy to maximize future NCS effectiveness is a full implementation of all applicable cost-effective NCS pathways in China. Our findings highlight the role of terrestrial carbon sequestration in offsetting energy-related CO2 emissions and put forward future needs in the context of carbon neutrality.  相似文献   

14.
In early 2020, unprecedented lockdowns and travel bans were implemented in Chinese mainland to fight COVID-19, which led to a large reduction in anthropogenic emissions. This provided a unique opportunity to isolate the effects from emission and meteorology on tropospheric nitrogen dioxide (NO2). Comparing the atmospheric NO2 in 2020 with that in 2017, we found the changes of emission have led to a 49.3 ± 23.5% reduction, which was ∼12% more than satellite-observed reduction of 37.8 ± 16.3%. The discrepancy was mainly a result of changes of meteorology, which have contributed to an 8.1 ± 14.2% increase of NO2. We also revealed that the emission-induced reduction of NO2 has significantly negative correlations to human mobility, particularly that inside the city. The intra-city migration index derived from Baidu Location-Based-Service can explain 40.4% ± 17.7% variance of the emission-induced reduction of NO2 in 29 megacities, each of which has a population of over 8 million in Chinese mainland.  相似文献   

15.
Hydrothermal fluid is essential for transporting metals in the crust and mantle. To explore the potential of Cu isotopes as a tracer of hydrothermal-fluid activity, Cu-isotope fractionation factors between Cl-bearing aqueous fluids and silicate magmas (andesite, dacite, rhyolite dacite, rhyolite and haplogranite) were experimentally calibrated. Fluids containing 1.75–14 wt.% Cl were mixed together with rock powders in Au95Cu5 alloy capsules, which were equilibrated in cold-seal pressure vessels for 5–13 days at 800–850°C and 2 kbar. The elemental and Cu-isotopic compositions of the recovered aqueous fluid and solid phases were analyzed by (LA-) ICP–MS and multi-collector inductively coupled plasma mass spectrometry, respectively. Our experimental results show that the fluid phases are consistently enriched in heavy Cu isotope (65Cu) relative to the coexisting silicates. The Cu-isotope fractionation factor (Δ65CuFLUID-MELT) ranges from 0.08 ± 0.01‰ to 0.69 ± 0.02‰. The experimental results show that the Cu-isotopic fractionation factors between aqueous fluids and silicates strongly depend on the Cu speciation in the fluids (e.g. CuCl(H2O), CuCl2 and CuCl32−) and silicate melts (CuO1/2), suggesting that the exsolved fluids may have higher δ65Cu than the residual magmas. Our results suggest the elevated δ65Cu values in Cu-enriched rocks could be produced by addition of aqueous fluids exsolved from magmas. Together with previous studies on Cu isotopes in the brine and vapor phases of porphyry deposits, our results are helpful for better understanding Cu-mineralization processes.  相似文献   

16.
Atmospheric methane (CH4) concentrations have shown a puzzling resumption in growth since 2007 following a period of stabilization from 2000 to 2006. Multiple hypotheses have been proposed to explain the temporal variations in CH4 growth, and attribute the rise of atmospheric CH4 either to increases in emissions from fossil fuel activities, agriculture and natural wetlands, or to a decrease in the atmospheric chemical sink. Here, we use a comprehensive ensemble of CH4 source estimates and isotopic δ13C-CH4 source signature data to show that the resumption of CH4 growth is most likely due to increased anthropogenic emissions. Our emission scenarios that have the fewest biases with respect to isotopic composition suggest that the agriculture, landfill and waste sectors were responsible for 53 ± 13% of the renewed growth over the period 2007–2017 compared to 2000–2006; industrial fossil fuel sources explained an additional 34 ± 24%, and wetland sources contributed the least at 13 ± 9%. The hypothesis that a large increase in emissions from natural wetlands drove the decrease in atmospheric δ13C-CH4 values cannot be reconciled with current process-based wetland CH4 models. This finding suggests the need for increased wetland measurements to better understand the contemporary and future role of wetlands in the rise of atmospheric methane and climate feedback. Our findings highlight the predominant role of anthropogenic activities in driving the growth of atmospheric CH4 concentrations.  相似文献   

17.
Retrieving historical fine particulate matter (PM2.5) data is key for evaluating the long-term impacts of PM2.5 on the environment, human health and climate change. Satellite-based aerosol optical depth has been used to estimate PM2.5, but estimations have largely been undermined by massive missing values, low sampling frequency and weak predictive capability. Here, using a novel feature engineering approach to incorporate spatial effects from meteorological data, we developed a robust LightGBM model that predicts PM2.5 at an unprecedented predictive capacity on hourly (R= 0.75), daily (R= 0.84), monthly (R= 0.88) and annual (R= 0.87) timescales. By taking advantage of spatial features, our model can also construct hourly gridded networks of PM2.5. This capability would be further enhanced if meteorological observations from regional stations were incorporated. Our results show that this model has great potential in reconstructing historical PM2.5 datasets and real-time gridded networks at high spatial-temporal resolutions. The resulting datasets can be assimilated into models to produce long-term re-analysis that incorporates interactions between aerosols and physical processes.  相似文献   

18.
Prostate carcinoma is the most frequently diagnosed malignancy and the second leading cause of death as a result of cancer in men in the US and other parts of the world. There are conflicting reports on the serum levels of testosterone and 17β-estradiol (E2) in benign prostatic hyperplasia (BPH) and prostate cancer. This study was designed to evaluate the serum concentrations of these hormones in patients with these disorders. Serum levels of prostate specific antigen (PSA), total testosterone and estradiol were determined in 228 subjects comprising of 116 subjects with BPH, 62 subjects with prostate cancer (CaP) and 50 age-matched apparently healthy controls, using ELISA methods. PSA levels were significantly elevated (p < 0.05) in BPH subjects than controls, while there was no significant difference (p > 0.05) in testosterone and estradiol levels of these subjects. PSA and estradiol levels were significantly higher (p < 0.05) in CaP subjects than in controls, while there was no observed significant difference (p > 0.05) in testosterone levels. CaP subjects had significantly raised PSA, testosterone, and estradiol levels than BPH subjects. The mean molar ratio of testosterone: E2 was lowest among CaP patients (134:1) and highest among controls (166:1). Significant positive correlation between PSA and 17β-estradiol was observed in prostate disorders (BPH and CaP patients: r = 0.347; p = 0.000). Significant negative correlations between testosterone and PSA were also observed among BPH patients (r = −0.221, p = 0.049) and control subjects (r = −0.490, p = 0.000). No significant correlation existed between testosterone and PSA in CaP patients (r = 0.051, p = 0.693). Correlations between age and estradiol in both BPH and CaP were not significant (p > 0.05). This study has shown that, there was a significant increase in serum estradiol in CaP subjects, while the testosterone levels in both BPH and CaP subjects were not different from those of controls.  相似文献   

19.
Grapes are the richest source of antioxidants due to the presence of potent bioactive phytochemicals. In this study, the phytochemical contents, scavenging activities and protective role against H2O2-induced oxidative stress in liver tissue ex vivo of four grape (Vitis vinifera) cultivars extracts, namely Flame seedless (black), Kishmish chorni (black with reddish brown), Red globe (red) and Thompson seedless mutant (green), were evaluated. The total phenolics and flavonoids content in pulp or skin fractions of different grape cultivars were in the range of 47.6–310 mg gallic acid equivalent/g fresh weight (fw), and 46.6–733.3 µg catechin equivalent/g fw respectively. The scavenging activities in skin of different grape varieties against 2,2-diphenyl-1-picrylhydrazyl (44–58 %), hydrogen peroxide (15.3–18.6 %), and hydroxyl radicals (50–85 %), were higher than pulp of the corresponding cultivars. These scavenging activities of grape extracts were found to be significantly (p < 0.01) correlated with the levels of total phenols, flavonoids and ascorbic acid. Liver tissues from goat treated with H2O2 (500 μM) showed significantly decreased GSH content by 42.9 % and activities of catalase by 50 % and glutathione reductase by 66.6 %; while increased thiobarbituric acid reactive substances and nitric oxide level by 2.53- and 0.86-fold, respectively, and activity of glutathione S-transferase by 0.96-fold. Grape skin extracts showed the stronger protective activity against H2O2-induced oxidative stress in liver tissue ex vivo, than its pulp of any cultivar; and the Flame seedless (black) cultivar showed the highest potential. In conclusion, our study suggested that the higher antioxidant potential, phytochemical contents and significant scavenging capacities in pulp and skin of grape extracts showed the protective action of grape extracts against H2O2-induced oxidative stress in liver tissue ex vivo.  相似文献   

20.
Understanding the mineralogy of the Earth''s interior is a prerequisite for unravelling the evolution and dynamics of our planet. Here, we conducted high pressure-temperature experiments mimicking the conditions of the deep lower mantle (DLM, 1800–2890 km in depth) and observed surprising mineralogical transformations in the presence of water. Ferropericlase, (Mg, Fe)O, which is the most abundant oxide mineral in Earth, reacts with H2O to form a previously unknown (Mg, Fe)O2Hx (x ≤ 1) phase. The (Mg, Fe)O2Hx has a pyrite structure and it coexists with the dominant silicate phases, bridgmanite and post-perovskite. Depending on Mg content and geotherm temperatures, the transformation may occur at 1800 km for (Mg0.6Fe0.4)O or beyond 2300 km for (Mg0.7Fe0.3)O. The (Mg, Fe)O2Hx is an oxygen excess phase that stores an excessive amount of oxygen beyond the charge balance of maximum cation valences (Mg2+, Fe3+ and H+). This important phase has a number of far-reaching implications including extreme redox inhomogeneity, deep-oxygen reservoirs in the DLM and an internal source for modulating oxygen in the atmosphere.  相似文献   

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