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The application of Pr-Nd-Dy alloy in the field of high-performance Nd-Fe-B permanent magnet materials has great potential. The composition of the PrF3-NdF3-DyF3-LiF (PND-LiF) electrolyte system used in the production of Pr-Nd-Dy alloys, the distribution of F, Li, RE and other elements in the electrolyte and their occurrence state were studied in this paper. The effect of temperature and lithium fluoride addition on electrolyte conductivity was revealed using the continuous conductivity cell constant (CVCC) method. The thermal analysis method was used to study the influence of lithium fluoride addition on the electrolyte's liquidus temperature and the optimal process conditions for the production of Pr-Nd-Dy alloy were determined. The results show that the overall distribution of praseodymium neodymium fluoride and lithium fluoride is uniform in the electrolyte and dysprosium fluoride is distributed between praseodymium-neodymium fluoride and lithium fluoride. Praseodymium-neodymium oxide is embedded in praseodymium neodymium fluoride in spotty pattern. The electrolyte's conductivity is increased as the temperature and lithium fluoride addition are going up, while the liquidus temperature is going down with increasing lithium fluoride addition. The best electrolysis process conditions for the PND-LiF system to produce praseodymium neodymium dysprosium alloy are as follows: temperature 1050 °C, 15.56 wt% PrF3-62.22 wt% NdF3-11.11 wt% DyF3-11.11 wt% LiF.

The evaluation index of camouflage patterns is important in the field of military application. It is the goal that researchers have always pursued to make the computable evaluation indicators more in line with the human visual mechanism. In order to make the evaluation method more computationally intelligent, a Multi-Feature Camouflage Fused Index (MF-CFI) is proposed based on the comparison of grayscale, color and texture features between the target and the background. In order to verify the effectiveness of the proposed index, eye movement experiments are conducted to compare the proposed index with existing indexes including Universal Image Quality Index (UIQI), Camouflage Similarity Index (CSI) and Structural Similarity (SSIM). Twenty-four different simulated targets are designed in a grassland background, 28 observers participate in the experiment and record the eye movement data during the observation process. The results show that the highest Pearson correlation coefficient is observed between MF-CFI and the eye movement data, both in the designed digital camouflage patterns and large-spot camouflage patterns. Since MF-CFI is more in line with the detection law of camouflage targets in human visual perception, the proposed index can be used for the comparison and parameter optimization of camouflage design algorithms.

Ni-rich layered oxide LiNixCoyMn1-x-yO2 (x ≥ 0.8) is the most promising cathodes for future high energy automotive lithium-ion batteries. However, its application is hindered by the undesirable cycle stability, mainly due to the irreversible structure change at high voltage. Herein, we demonstrate that F substitution with the appropriate amount (1 at%) is capable for improve the electrochemical performance of LiNi0.9Co0.05Mn0.05O2 cathode significantly. It is revealed that F substitution can reduce cation mixing, stabilize the crystal structure and improve Li transport kinetics. The resulted LiNi0.9Co0.05Mn0.05O1.99F0.01 cathode can deliver a high capacity of 194.4 mAh g−1 with capacity retention of 95.5% after 100 cycles at 2C and 165.2 mAh g−1 at 5C. In-situ synchrotron X-ray technique proves that F ions in the cathode materials can suppress the irreversible phase transition from H2 phase to H3 phase in high voltage region by preventing oxygen gliding in a-b planes, ensuring a long-term cycle stability.

The commercialization of solid oxide fuel cells (SOFCs) can be significantly promoted with the direct utilization of methane, which is the primary component in natural gas and the second most abundant anthropogenic greenhouse gas. However, carbon deposition on most commonly used Ni-based anode is the bottle-necking issue inhibiting long-term stability of direct methane SOFCs. To avoid such a problem, methane is typically reformed (internally or externally) in SOFCs. Considering the cost, system simplification, coking resistance, and material selection, the on-cell catalytic reforming layer (OCRL) is one of the most promising designs for direct methane SOFCs. Reforming catalytic materials are typically consisted of active component, substrate and catalytic promoter, all of which have a significant impact on the catalytic activity, sintering resistance and coking resistance of methane reforming catalysts. This review summarizes the influence of the various components, some common OCRL materials and their applications in direct methane SOFCs, reforming and coking resistance mechanism, as well as the remaining challenges. The effective utilization of OCRL plays a pivotal role in promoting the development of direct methane SOFCs and the commercialization of SOFCs.

Metal hydride is an encouraging way for H 2 storage owing to the large H 2 storage capacity and suitable physical properties. As a crucial equipment for reversible chemical reaction of metal hydride, we propose a new branch mini-channel reactor to promote heat transfer and reaction effectively in H 2 storage reactor, which can reduce more than 55% hydrogenation/dehydrogenation time compared with straight tube reactor. Meanwhile, the optimal performance of both reactors could be achieved at branch number of 3 and center distance of branch bifurcation point of 8.5 mm. The optimal and sensitivity analysis of 6 operation conditions reveal that both reactors performances are most sensitive to H 2 pressure and fluid temperature for hydrogenation and dehydrogenation, respectively. Moreover, quadratic response surface analysis indicates an extremely marked impact (99% believable probability) on the regression model, whose regression coefficient (R2) could achieve 0.9955.

Carbon dots (CDs), as a kind of carbon nanomaterials, have attracted widespread attention due to their unique structure and excellent optical properties, and they are low-cost, environmentally friendly and biocompatible. However, the development of near-infrared (NIR) emission CDs remains a challenge. In this study, we successfully prepared CDs with a maximum emission of 714 nm using citric acid as the carbon source, thiourea and ammonium fluoride as the dopant source, and N,N-dimethylformamide as the solvent. The quantum yield (QY) is as high as 22.64%. Interestingly, the prepared CDs self-oxidize in the presence of oxygen, resulting in a blue shift of their emission. Therefore, they can be used to prepare white light-emitting diodes (WLEDs) without adding other fluorescent substances. Notably, the work presented herein constitutes the first report of WLEDs preparation from single CDs.

Lanthanide-transition metal complexes continue to be of interest, not only because of their synthetic challenge but also of their promising magnetic properties. Computational work examining the chemical bonding between lanthanides and transition metals in PyCp2Ln-TMCp(CO)2 (DyPyCp22- = [2,6-(CH2C5H3)2C5H3N]2-) reveals strong Ln-TM dative bonds. Gas-phase optimized geometries are in good agreement with experimental structures at the density functional theory (DFT) level with large-core pseudopotentials. From La to Lu, there is a small increase in the bond dissociation energy, as well as a decrease in Ln-Fe bond lengths. Energy decomposition analyses attribute this trend to an increase in the electrostatic contribution from the decreasing bond length and a modest increase in the orbital contribution. The natural bond orbital analysis clearly indicates that 3d6 "lone pairs" in the [FeCp(CO)2]- fragment act as a Lewis bases donating nearly 0.5 electron to Ln virtual orbitals of mainly d character. The interfragment bonding was also quantified by the quantum theory of atoms in molecules, which indicates that the Ln-Fe bond is more covalent than the Ca-Fe bond in the hypothetical CpCa-FeCp(CO)2 but less covalent than the Zn-Fe bond in the hypothetical CpZn-FeCp(CO)2. Further comparisons suggest that to the [PyCp2Ln]+ cation the [FeCp(CO)2]- anion appears much like a halide. Overall, these Ln-TM dative bonds appear to have strong electrostatic contributions as well as significant orbital mixing and dispersion contributions.

Strongly acidic wastewater produced in nonferrous metal smelting industries often contains high concentrations of Ni(II), which is a valuable metal. In this study, the precipitation of Ni(II) from strongly acidic wastewater using sodium dimethyldithiocarbamate (DDTC) as the precipitant was evaluated. The effects of various factors on precipitation were investigated, and the precipitation mechanism was also identified. Finally, the nickel in the precipitates was recovered following a pyrometallurgical method. The results show that, under optimised conditions (DDTC:Ni(II) molar ratio = 4:1; temperature = 25 °C), the Ni(II) removal efficiency reached 99.3% after 10 min. In strongly acidic wastewater, the dithiocarbamate group of DDTC can react with Ni(II) to form DDTC Ni precipitates. Further recovery experiments revealed that high-purity NiO can be obtained by the calcination of DDTC Ni precipitates, with the nickel recovery efficiency reaching 98.2%. The gas released during the calcination process was composed of NO2, CS2, H2O, CO2, and SO2. These results provide a basis for an effective Ni(II) recovery method from strongly acidic wastewater.

Coking is a major issue with the traditional Ni-based anodes when directly oxidizing CH4 in solid oxide fuel cells (SOFCs). Dry reforming to convert CH4–CO2 into CO–H2 syngas before entering Ni-based anode may potentially be an effective and economical method to address the coking problem. Consequently, an on-cell reforming layer outside the Ni-based anode is expected to offer a unique solution for direct CH4–CO2 SOFCs without coking. In this study, Ni-GDC anode-supported cells with and without a Sr2Co0.4Fe1.2Mo0.4O6-δ (SCFM) layer outside the anode support have been fabricated and evaluated using either H2 or CH4–CO2 as fuel. Both types of cells show excellent electrochemical performance when H2 is used as fuel, and the SCFM layer has negligible impact on the cell performance. When CH4–CO2 is used as fuel, however, the electrochemical performance and durability of the cells with the SCFM layer are much better than those without the SCFM layer outside the Ni-GDC anode, indicating that the SCFM layer can efficiently perform dry reforming. This unique on-cell dry reforming design enables direct CH4–CO2 solid oxide fuel cells and offers a very promising route for energy storage and conversion.

The surface discharge of solid dielectric in liquid nitrogen has become one of the key problems in the development of high-temperature superconducting power devices. It is necessary to study the mechanism of surface discharge of the solid dielectric in liquid nitrogen. This article chose polytetrafluoroethylene and DW-3 epoxy resin as specimens, tested the surface discharge voltages of two kinds of specimens with different surface roughness under lightening impulse voltages in liquid nitrogen, and discussed the effect mechanism. The experimental results showed that the surface discharge voltage and discharge time of both materials in liquid nitrogen increased as the surface roughness increasing under lightning impulses. The surface roughness affects the surface discharge voltage of the solid dielectric in liquid nitrogen under lightning impulse, mainly in the charge left on the grinding surfaces of solid dielectrics, the heights of projections, and the creepage distance on the dielectric surfaces. The main discharge process is in the gasification path, and the effect of solid dielectric on surface discharge in liquid nitrogen is smaller. These reasons make the surface discharge in the liquid nitrogen less affected by the surface roughness. The results further explore the characteristics of surface discharge in liquid nitrogen and could provide methodological guidance to improve the surface discharge voltages in liquid nitrogen.

C/C–ZrC–SiC composites with different carbon sources (glucose, sucrose, and phenolic resin) were fabricated by precursor infiltration and pyrolysis. The effects of the structure of carbon matrix on the microstructure and ablation resistance were investigated. All three C/C–ZrC–SiC composites exhibited good ablation resistance under the plasma flame above 2300 °C, and the C/C–ZrC–SiC composites with phenolic resin has the highest thermal conductivity of 13.285 W/(m·K), as its compact pyrolyzed carbon had sealed defects and changed matrix structure. It also showed superior ablation resistance, and the mass and linear ablation rates are − 2.07 mg·s-1 and 1.02 μm·s-1, respectively. Besides, the SiC-coated C/C–ZrC–SiC composites displayed good ablation resistance under long-term plasma flame, among them the SiC-coated C/C–ZrC–SiC composites with phenolic resin has the best mass and linear ablation rates as 0.55 mg·s-1 and – 0.1 μm·s-1, respectively.

van der Waals (vdW) vertical p-n junctions based on two-dimensional (2D) materials have shown great potential in flexible, self-driven, high-efficiency electronic and optoelectronic applications. However, due to the complex nucleation dynamics, the controllable synthesis of vertical heterostructures remains a daunting challenge. Here, we report the controlled growth of vertical GaSe/MoS2 p-n heterojunctions via a liquid gallium (Ga)-assisted chemical vapor deposition method. The growth mechanism can be interpreted by theoretical calculations based on the Burton-Cabrera-Frank theory. By analyzing the diffusion barriers and the Ehrlich-Schwoebel barriers of adatoms, we found that the growth modes between vertical and lateral can be precisely switched by means of adjusting the amount of Ga. Based on the achieved high-quality vertical GaSe/MoS2 p-n heterojunctions, photosensing devices are further designed and systematically investigated. Upon light illumination, prominent photovoltaic effects with large open-circuit voltage (0.61 V) and broadband detection capability from 375 to 633 nm are observed, which can further be employed for self-powered photodetection with high responsivity (900 mA/W) and fast response speed (5 ms). The developed liquid-metal-assisted strategy provides an effective method for controllable synthesis of vdW heterostructures and will give impetus to their applications in high-performance optoelectronic device.

Advanced application of the superwettable surface with intelligent stimulus-responsive property invents a new way for designing controllable and effective oil-water separation material. Here, a smart superwettable fabric with tunable wettability has been fabricated via a low-cost and eco-friendly approach. With synergistic effect of the well-define micro/nano-hierarchical structure and pH-sensitive undecylenic acid, the as-prepared superwettable coating exhibits an excellent switchable surface wettability, which can reversibly transit between superhydrophobicity and superhydrophilicity in accordance with pH values of the contacting aqueous water. By virtue of the special wetting property, the obtained superwettable coating can be exploited to controllably and efficiently separate various oil-water mixtures, showing attractive separation efficiency (99 %) and favorable durability. Moreover, the complex oil/water/oil three-phase system also can be successfully separated with the superwettable coating as separation membrane, revealing an excellent in situ pH-responsiveness. Besides, it is worth noting that the superwettable coating is competent to selectively remove organic from oil, which has been seldom reported in previous works and providing a viable strategy for separating organic from oil. In light of the above advantages, it is believed that the functionalized smart coating with controllable tunable surface wettability will be a promising candidate for oily wastewater remediation under various harsh settings.

A type of grafted acrylate copolymer resins, containing 3‐oxo‐N‐allyl‐1,2‐benzisothiazole‐2(3H)‐carboxamide monomer and heterocyclic monomers, was synthesized through the copolymeri‐ zation of methyl methacrylate (MMA) and butyl acrylate (BA) with functional monomers. The structures of the monomers and copolymers were validated by infrared (IR) and 1H nuclear magnetic resonance (NMR) spectroscopies. The inhibitory activities of the copolymers on algae, bacteria, and barnacle larvae were measured, and the antifouling potencies against marine macrofouling organisms were investigated. The results showed that the grafted resin had significant inhibitory effects on the growth of three marine algae (Isochrysis galbana, Nannochloropsisoculata, and Chlorella pyrenoidosa), and three bacteria (Vibrio coralliilyticus, Staphylococcus aureus,and Vibrio parahaemolyticus). The target copolymers also showed excellent inhibition of the survival of barnacle larvae. Additionally, the release rate of the antifoulant and the results of the marine field tests indicated that the grafted copolymers had outstanding antifouling potency against the attachment of marine macrofouling organisms., Grafted acrylate copolymer resins containing 3‐oxo‐N‐allyl‐1,2‐benzisothiazole‐2(3H)‐carboxamide monomer and heterocyclic monomers, have been prepared via copolymerization of methyl methacrylate and butyl acrylate with functional monomers. The structures of the monomers and copolymers were validated by infrared and 1H nuclear magnetic resonance spectroscopies. The inhibitory activities of the copolymers on algae, bacteria, and barnacle larvae were measured, and the antifouling potencies against marine macrofouling organisms were investigated.

As China ramped-up coal power capacities rapidly while CO2 emissions need to decline, these capacities would turn into stranded assets. To deal with this risk, a promising option is to retrofit these capacities to co-fire with biomass and eventually upgrade to CCS operation (BECCS), but the feasibility is debated with respect to negative impacts on broader sustainability issues. Here we present a data-rich spatially explicit approach to estimate the marginal cost curve for decarbonizing the power sector in China with BECCS. We identify a potential of 222 GW of power capacities in 2836 counties generated by co-firing 0.9 Gt of biomass from the same county, with half being agricultural residues. Our spatially explicit method helps to reduce uncertainty in the economic costs and emissions of BECCS, identify the best opportunities for bioenergy and show the limitations by logistical challenges to achieve carbon neutrality in the power sector with large-scale BECCS in China., China has pledged to achieve carbon neutrality in 2060. Here the authors find a promising option to abate 1.0 Gt CO2-eq yr−1 of carbon emissions at a marginal cost of $69 (t CO2-eq)−1 by retrofitting 222 GW of coal power plants to co-fire with biomass and upgrading to CCS operation across 2836 counties in China.

As a potential physical blowing agent, sodium bicarbonate (SB) is environmentally friendly and low in cost, but its low decomposition temperature cannot meet the requirements of polyolefin foam materials. Herein, for enhancing the thermal properties of SB, a modified way was offered to fabricate various SB-based capsules via suspension polymerization. As the modified SB-based capsules, epoxy resin (EP) accompanied with several organic acids was successfully coated on the surface of SB, serving as heat-insulation layer of SB. Various physicochemical characterizations provided reliable evidences for the good coating effect, and the thermal performance of the modified SB was improved. Further, the composite SB capsules were applied for the foaming of polypropylene (PP), and the foaming behavior of the SB-based capsules in PP was significantly improved, with more uniform distribution, smaller cell diameter, and higher cell density. In all, this work fully proved that the coated shells enhanced the thermal properties of SB, and the modified SB capsules significantly improved the foaming quality of foamed PP.

A type of polyurethane elastomer with excellent self-healing ability has been fabricated through digital light processing 3D printing. First, a type of polyurethane acrylate containing disulfide bonds is synthesized and then compounded with reactive diluent and photoinitiators to get a photopolymer resin. Due to the good fluidity and high curing rate, the photopolymer resin can be applied in DLP 3D printing, and various 3D objects with complicated structures, high printing accuracy, and remarkable self-healing ability have been printed. The tensile strength and elongation at break of the polyurethane elastomer are 3.39 ± 0.09 MPa and 400.38 ± 14.26%, respectively, and the healing efficiency can get to 95% after healing at 80 °C for 12 h and can be healed for multiple times. With the ease of fabrication and excellent performance, the polyurethane elastomers from DLP 3D printing have great potential applications in flexible electronics, soft robotics, and sensors.

This study used remote sensing images from 1996 to 2016 as the main data source, and selected the average annual ecosystem type net change rate, ecosystem type transfer matrix, and comprehensive index of land development degree, to analyze the macro change of the ecosystem pattern in Xishuangbanna Dai Autonomous Prefecture in the past 20 years. Quantitative analysis was performed on amplitude, rate, type of transition, and degree of disturbance of human activities. The results reveal the spatial and temporal changes of the Xishuangbanna ecosystem and their regional differentiation. The results showed that (1) from 1996 to 2016, Xishuangbanna as a whole was dominated by forest ecosystems and rubber ecosystems, followed by tea, farmland, built-up area, and water ecosystems. (2) During 1996-2016, the ecosystem in Xishuangbanna accounted for more than 99% of the total area has not changed. From 1996 to 2003, the transfer of ecosystem types in Xishuangbanna was mainly between forest and rubber ecosystem. (3) The extent of land development and utilization in Xishuangbanna in the past 20 years is relatively low, slightly lower than the national average, and the overall level of land use is at a medium level of utilization, and over time, the degree of disturbance of human activities has shown an increasing trend.

A facile method for the quantitative preparation of silver dibenzo-fused corrole Ag-1 is described. In contrast to the saddle conformation resolved by single crystal X-ray analysis for Ag-1 , it adopts an unprecedented domed geometry, with up- and down-orientations, when adsorbed on Ag(111) surface. Sharp Kondo resonances near Fermi level, both at the corrole ligand and the silver center, were observed by cryogenic STM, with relatively high Kondo temperature (172 K), providing the first direct spectroscopic evidence for a non-innocent Ag II -corrole •2- species. Further investigation validates that benzene ring fusion and molecule-substrate interactions play pivotal roles in enhancing Ag (4d x2-y2 )-corrole (π) orbital interactions, thereby stabilizing the open-shell singlet Ag II -corrole •2- on Ag(111) surface. Moreover, this strategy used for constructing metal-free benzene-ring fused corrole ligand gives rise to inspiration of designing novel metal-corrole compound which could be applied to the research of multichannel molecular spintronics devices for data storage and logic gates.

Human activity transforms a land surface into a complex surface where artificial and natural landforms coexist and continuous and emergent landforms merge. In this background, the problems of conventional digital elevation models (DEMs), such as morphological distortion, complicated updates, and lack of information, are increasingly prominent. This study proposes a new idea of DEM construction based on the concept of geographic ontology. First, landforms with common features are abstracted into a certain type of topographic entity based on their morphologies and semantics. For each type of topographic entity, a DEM was constructed independently based on the available elevation information and other information about the semantics and spatial relationships. Second, individual DEMs were merged into a complete DEM following certain rules. A 1 km2 area located in the suburb of Nanjing, Jiangsu Province, China, was selected as the experimental area. The effectiveness of the model construction method proposed in this study was verified. The results show that the DEM constructed according to the idea of this study has a significantly better performance than the conventional DEMs. The constructed DEM in this study can well represent ground objects, such as slopes, farmland, and ditches. In particular, the constructed DEM ensures the morphological accuracy of the ground objects.

It is nowadays essential to avoid electromagnetic interferes (EMI) not only in electronic equipment but also in human health with the rapid development of electronic technology. Damage or invalid in complex and harsh environments is still one of the major challenges facing the field of EMI shielding materials, but superhydrophobic surface have recently shown potential to enhance mechanical stability and chemical durability for this material. As one of the vital research directions of superwetting field, superamphiphobic surface have been often used to solve problems of other fields to improve their surface properties. Therefore, combining the superamphiphobic surface to overcome the problems of electromagnetic shielding materials is the main work of this paper. Here, a superamphiphobic surface was introduced through constructing micro-nano structure with low surface energy, which was mainly contributed from 1H,1H,2H,2H-perfluorodecyltriethoxysilane, micro-ordered array polypyrrole, multi-walled carbon nanotubes and silica. Finally, the as-prepared materials after 5000 times of kneading-releasing cycles, 60 min of ultrasonic, 50 times of abrasion by using sandpaper, 24 h of ultraviolet irradiation, and 10 h of immersion in acid, alkali and different organic solvents, still has superamphiphobic performance which means it can be used extreme environment to endow a widely applications for EMI shielding materials.

Levoglucosan has been widely used to quantitatively assess biomass burning's contribution to ambient aerosols, but previous such assessments have not accounted for levoglucosan's degradation in the atmosphere. We develop the first global simulation of atmospheric levoglucosan, explicitly accounting for its chemical degradation, to evaluate the impacts on levoglucosan's use in quantitative aerosol source apportionment. Levoglucosan is emitted into the atmosphere from the burning of plant matter in open fires (1.7 Tg yr-1) and as biofuels (2.1 Tg yr-1). Sinks of atmospheric levoglucosan include aqueous-phase oxidation (2.9 Tg yr-1), heterogeneous oxidation (0.16 Tg yr-1), gas-phase oxidation (1.4 × 10-4 Tg yr-1), and dry and wet deposition (0.27 and 0.43 Tg yr -1). The global atmospheric burden of levoglucosan is 19 Gg with a lifetime of 1.8 days. Observations show a sharp decline in levoglucosan's concentrations and its relative abundance to organic carbon aerosol (OC) and particulate K+ from near-source to remote sites. We show that such features can only be reproduced when levoglucosan's chemical degradation is included in the model. Using model results, we develop statistical parametrizations to account for the atmospheric degradation in levoglucosan measurements, improving their use for quantitative aerosol source apportionment.

Multidimensional fabrication of metal-organic frameworks (MOFs) into multilevel channel integrated devices are in high demanded for Li-S separators. Such separators have advantages in pore-engineering that might fulfill requirements such as intercepting the diffusing polysulfides and improving the Li+ /electrolyte transfer in Li-S batteries. However, most reported works focus on the roles of MOFs as ionic sieves for polysulfides while offering limited investigation on the tuning of Li+ transfer across the separators. A photoinduced heat-assisted processing strategy is proposed to fabricate MOFs into multidimensional devices (e.g., hollow/Janus fibers, double-or triple-layer membranes). For the first time, a triple-layer separator with stepped-channels has been designed and demonstrated as a powerful separator with outstanding specific capacity (1365.0 mAh g-1 ) and cycling performance (0.03 % fading per cycle from 100th to 700th cycle), which is superior to single/double-layer and commercial separators. The findings may expedite the development of MOF-based membranes and extend the scope of MOFs in energy-storage technologies.

Background Over recent decades, many efficacious insecticides have been applied for control of Bemisia tabaci, one of the most notorious insect pests worldwide. Field-evolved insecticide resistance in B. tabaci has developed globally, but remains poorly understood in China. Results In this study, a total of 30 field samples of the whitefly Bemisia tabaci from eight provinces of China were collected in 2015 to 2018. Twenty-four of the populations were identified as Mediterranean, 'Q' type (MED), three were Middle East-Asia Minor 1, 'B' type (MEAM1), and three were mixtures of MED/ MEAM1. After identifying whether they belong to MED or MEAM1, the selected individuals were used in bioassays assessing insecticide resistance to abamectin, thiamethoxam, spirotetramat, cyantraniliprole, and pyriproxyfen. Our results showed that all populations in the eight regions had little or no resistance to abamectin; abamectin resistance was highest in the Hunan (Changsha) and Hubei (Wuhan) regions and was lowest in the island region of Hainan (Sanya). The resistance of B. tabaci to spirotetramat, cyantraniliprole, and pyriproxyfen increased each year. The resistance to thiamethoxam remained low because of the high LC50 value for the laboratory strain. Conclusion These findings suggest that a rotation system using efficacious B. tabaci insecticides with differing mode of actions ought to be implemented for sustainable control to reduce the potential of resistance development. This study provides important data to support the integrated pest management and insecticide resistance management of B. tabaci in China. © 2021 Society of Chemical Industry.

Alkanes are an important part of petroleum, the stability of alkanes under extreme conditions is of great significance to explore the origin of petroleum and the carbon cycle in the deep Earth. Here, we performed Raman and infrared (IR) spectroscopy studies of n-hexane and cyclohexane under high pressure up to ~42 ​GPa ​at room temperature (RT) and high temperature (HT). n-Hexane and cyclohexane undergo several phase transitions at RT around 1.8, 8.5, 18 ​GPa and 1.1, 2.1, 4.6, 13, 30 ​GPa, respectively, without any chemical reaction. By using resistive heating combined with diamond anvil cell at pressure up to 20 ​GPa and temperature up to 1000 ​K, both n-hexane and cyclohexane decompose to hydrogenated graphitic carbon and n-hexane exhibits higher stability than cyclohexane. Our results indicate that hydrocarbons tend to dehydrogenate in the upper mantle, and the extension of carbon chains may lead to the formation of some unsaturated compounds and eventually transfer into graphitic products.

The robustness of electrostatic sensitive devices is important in state-of-the-art silicon technology. However, the electrical breakdown-induced microstructure evolution remains unclear. In this work, we performed the physical failure analysis of breakdown in an enhanced modified lateral silicon-controlled rectifier-based electrostatic discharge (ESD) device. Direct visualization of the conductive metal filaments in the doped silicon substrate has been achieved by high-resolution transmission electron microscopy. The locations of these metal filaments induced by breakdown are found near the cathode. The evolution of these microstructural changes and chemical properties provides guide to the failure analysis of ESD devices.

Doppler ultrasound technology is widespread in clinical applications and is principally used for blood flow measurements in the heart, arteries, and veins. A commonly extracted parameter is the maximum velocity envelope. However, current methods of extracting it cannot produce stable envelopes in high noise conditions. This can limit clinical and research applications using the technology. In this article, a new method of automatic envelope estimation is presented. The method can handle challenging signals with high levels of noise and variable envelope shapes. Envelopes are extracted from a Doppler spectrogram image generated directly from the Doppler audio signal, making it less device-dependent than existing image-processing methods. The method’s performance is assessed using simulated pulsatile flow, a flow phantom, and in vivo ascending aortic flow measurements and is compared with three state-of-the-art methods. The proposed method is the most accurate in noisy conditions, achieving, on average, for phantom data with signal-to-noise ratios (SNRs) below 10 dB, bias and standard deviation of 0.7% and 3.3% lower than the next-best performing method. In addition, a new method for beat segmentation is proposed. When combined, the two proposed methods exhibited the best performance using in vivo data, producing the least number of incorrectly segmented beats and 8.2% more correctly segmented beats than the next best performing method. The ability of the proposed methods to reliably extract timing indices for cardiac cycles across a range of signal quality is of particular significance for research and monitoring applications.

Digital terrain analysis (DTA) is one of the most important contents in the research of geographical information science (GIS). However, on the basis of the digital elevation model (DEM), many problems exist in the current research of DTA in geomorphological studies. For instance, the current DTA research appears to be focused more on morphology, phenomenon, and modern surface rather than mechanism, process, and underlying terrain. The current DTA research needs to be urgently transformed from the study of landform morphology to one focusing on landform process and mechanism. On this basis, this study summarizes the current research status of geomorphology-oriented DTA and systematically reviews and analyzes the research about the knowledge of geomorphological ontology, terrain modeling, terrain derivative calculation, and terrain analytical methods. With the help of DEM data, DTA research has the advantage of carrying out geomorphological studies from the perspective of surface morphology. However, the study of DTA has inherent defects in terms of data expression and analytic patterns. Thus, breakthroughs in basic theories and key technologies are necessary. Moreover, scholars need to realize that DTA research must be transformed from phenomenon to mechanism, from morphology to process, and from terrain to landform. At present, the research development of earth science has reached the critical stage in which the DTA research should focus more on geomorphological ontology. Consequently, this study proposes several prospects of geomorphology-oriented DTA from the aspects of value-added DEM data model, terrain derivatives and their spatial relations, and macro-terrain analysis. The study of DTA based on DEM is at a critical period along with the issue on whether the current GIS technology can truly support the development of geography. The research idea of geomorphology-oriented DTA is expected to be an important exploration and practice in the field of GIS.

The Beijing area experienced daily ozone increases after the Belt and Road Forum in May 2017, with the maximum hourly O3 peak exceeding 400 μg/m3. The high O3 event was analyzed by using observed data and model simulations. Results indicated that the local photochemistry was the major driver boosting O3 formation for northern suburban sites and regional transport in the late afternoon made another peak in O3 diurnal variation for urban sites. A prominent VOC-limited sensitivity regime was dominant in the Beijing area, even over suburban areas far away from the Beijing urban center. The rapid increase in VOCs emissions from both biogenic and anthropogenic sources under high air temperatures provided the needed VOCs for O3 formation, resulting in a dramatic O3 increase after the summit. It was also found that PM2.5 experienced steady daily increases after the summit, leading to a gradual decrease in the UV radiation measured at the ground; however, O3 showed a dramatically increasing trend, in contrast to the expectation that the high-level PM2.5 would restrain the O3 formation by the theoretical deduction in the O3 and aerosol interaction. The results suggest that the abrupt change in emissions during the study period overwhelmed the effects of the O3 and aerosol interaction. Such temporary changes in emissions should be considered in mitigation strategies of O3 control.

Paper, as a foldable, pollution-free, and low-cost material, has become a suitable support substrate for producing flexible thermoelectric (TE) generators to realize waste heat recycling and the application of human-powered electronic devices. We propose a facile fabrication method to modify cellulose paper with inorganic TE powders via vacuum filtration, making a modified paper that possesses good thermoelectric properties. By connecting the modified paper to copper foils, flexible paper-based TE generators (PTGs) are fabricated. The obtained PTG with three units of P–N modules can generate an output voltage of ∼41.2 mV at a temperature difference of 50 K. Based on this modified paper, a thermal sensor that responds to heat sources, such as fingers, is proposed with a rapid response time of 0.25 s. This work offers a promising strategy for the simple fabrication of PTGs, paving the way for achieving the commercial application of self-powered wearable electronics.

A novel precursor of SiC prepared by mixing boron phenolic resin and hydrolytic solution of tetraethyl orthosilicate was employed to fabricate the ablation-resistant C/C–SiC composites. The pyrolysis behaviors of precursor and the ablation properties of prepared composites were discussed. Results show that during the pyrolyzation process of the precursor, the carbon phase was evenly surrounded by the silica phase, benefitting the occurrence of the carbothermal reaction. The precursor was totally transformed into SiC with the carbon left (7.77–8.11 wt%) after heating at 1600 °C. Due to the unique surrounded structure between the carbon and silica phases, part of the residual carbon was encircled by the generated SiC ceramics. During ablation, the carbon nucleus played a positive role in enhancing ablation resistance of composites by hindering the flow of molten silica. Compared with the composites employed polycarbosilane as precursor, this prepared C/C–SiC composites exhibited a decent anti-ablation performance.

Chlorine dioxide (ClO2), an alternative disinfectant to chlorine, has been widely applied in water and wastewater disinfection. This paper aims at presenting an overview of the inactivation kinetics and mechanisms of ClO2 with viruses. The inactivation efficiencies vary greatly among different virus species. The inactivation rates for different serotypes within a family of viruses can differ by over 284%. Generally, to achieve a 4-log removal, the exposure doses, also being referred to as Ct values (mutiplying the concentration of ClO2 and contact time) vary in the range of 0.06–10 mg L−1 min. Inactivation kinetics of viruses show two phases: an initial rapid inactivation phase followed by a tailing phase. Inactivation rates of viruses increase as pH or temperature increases, but show different trends with increasing concentrations of dissolved organic matter (DOM). Both damages in viral proteins and in the 5′ noncoding region within the genome contribute to virus inactivation upon ClO2 disinfection. Supplementary Information The online version contains supplementary material available at 10.1007/s00128-021-03137-3.

Rhodamine B (RhB) is considered as a potential source of water pollution because it is harmful to the environment and humans, and thus, it should be removed from the water system. Hydrogels derived...

Summary γ-butyrolactone (γ-BL), serving as the monomer of biocompatible and recyclable poly(γ-butyrolactone) plastic, faces a giant challenge in ring-opening polymerization (ROP) due to its low strain energy. The ROP of γ-BL is generally achieved under harsh conditions (e.g., high-pressure or gas-protected atmosphere) and is mostly based on homogeneous systems. Here, we synthesize a series of lanthanum metal-organic framework-based porous nanospheres and successfully apply them as heterogeneous catalysts in efficient ROP of γ-BL under mild conditions. Specifically, NNU-mIM-3 presents a yield of 24.6% with low polydispersity distribution centered at 3.6 kDa and the obtained PγBL can be completely and quantitatively recycled into monomers by simple heat treatment. Besides, the ROP catalysis systems have been intensively explored with various imine-based additives, proven to exhibit largely improved performance with PγBL yield of ~50% and Mw of ~8 kDa. This work paves a new way to explore novel heterogeneous catalysts in producing biocompatible and degradable plastics.

Selective laser melting technology was proposed to form the multi-element mixed rare earth magnesium alloys of Mg–3.4Y–3.6Sm–2.6Zn–0.8Zr (wt-%). The formation process, relative density, evaporation...

The microstructure evolution and the pitting corrosion resistance of a supermartensitic stainless steel after deep cryogenic treatment process were clarified through X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy (TEM) and electrochemical methods. The results showed that the microstructure of supermartensitic stainless steel mainly consisted of reversed austenite, tempered martensite, and M23C6 carbides after tempering. The deep cryogenic treatment promoted the refinement of the martensite laths and the precipitation of the carbides in comparison with the traditional process. TEM analysis indicated that the segregation of Si atoms at the boundary was found at the interface between carbide and martensite. The pitting corrosion potential of the specimens subjected to deep cryogenic treatment decreased with the elevated tempering temperature, and the lowest pitting corrosion potential was found at the tempering temperature of 650 °C. The sensitivity of the pitting corrosion potential was attributed to the precipitation of M23C6 carbides and Si atoms segregation. Si atoms segregation engendered the formation of Cr-depleted zone near M23C6 and impeded the recovery of Cr-depleted zone.

Corallorhiza sinensis, a new species of mycoheterotrophic orchid from western Sichuan, China, is described and illustrated based on molecular and morphological evidence. It is morphologically similar to Corallorhiza trifida, but can be distinguished by bigger flowers, both sepals and petals with 3 veins, and longer lateral lobes of lip. To distinguish the new Corallorhiza species and explore its phylogenetic position within subtribe Calypsoinae, this study employed sequences of the nuclear ribosomal DNA (nrDNA) and whole plastome assembled from the genome skimming approach. The plastome is 148,124 bp in length, including a pair of inverted repeats (IRs) of 26,165 bp, a large single-copy region (LSC) of 82,207 bp, and a small single-copy region (SSC) of 13,587 bp. Further, phylogenetic analyses were performed using nrDNA sequence and 79 coding sequences (CDSs) from 26 complete plastomes of subtribe Calypsoinae. The phylogenetic tree based on nrDNA sequence suggested that Corallorhiza is a monophyletic group, and strongly support C. sinensis as sister to the rest species of Corallorhiza. The plastid tree showed that 10 Corallorhiza species grouped into two clades and C. sinensis is most closely related to the North American C. striata and C. bentleyi instead of Oreorchis foliosa and O.angustata in the same clade. The plastid tree and nrDNA tree indicate Oreorchis is a paraphyletic. Although the topological conflicts are displayed between plastome and nrDNA phylogenies of C. sinensis, it is still the most closely related to Corallorhiza. Comparative analysis showed that C. sinensis populations are characteristic of the intermediate morphological traits between Corallorhiza and Oreorchis. The finding of this new species from China shed new light on the phylogeny of Oreorchis and Corallorhiza., Highlights • In this study, Corallorhiza sinensis G.W. Hu & Q.F. Wang, a new species of orchids from western Sichuan, China is described and illustrated. • Complete plastid genome of C. sinensis was sequenced, assembled, and analyzed in comparison with congeneric species. Results showed that some photosynthesis-related genes either lost or pseudogenized. • The result of the plastome structure comparison showed that one small inversion in C. sinensis. • Both the plastid and nrDNA tree indicate Oreorchis is a paraphyletic. The finding of this new species from China shed new light on the phylogenetic relationship of Oreorchis and Corallorhiza.

The construction of hierarchical titanosilicate beta zeolites with desirably interconnected meso-/microporosity, controllable morphology and enhanced activity of catalytic oxidation is a pervasive challenge in the zeolite community. We report here in the synthesis of the hierarchical titanosilicate beta zeolite with a three-dimensionally ordered mesoporous-imprinted structure (3DOm-i Ti-beta) through the postsynthetic treatment of the parent 3DOm-i Al-beta by successive dealumination and titanation. The highly interconnected intracrystalline meso-/microporosity derived from the well-retained 3DOm-i structure led to both enhanced diffusion property and better accessibility of active sites to the bulky substrates, which was confirmed by the improved catalytic performances in the epoxidation of cyclic olefins (cyclohexene and cyclooctene) compared with the conventional solely microporous Ti-beta and TS-1. Moreover, the demonstrated that 3DOm-i Ti-beta catalyst exhibited not only a superior stability but also a facile recyclability by simple calcination in the epoxidation reaction.

Quaternary compound BiAgSeS shows an excellent thermoelectric performance with ultralow thermal conductivity. However, competition between the trigonal and cubic phases, which is strongly dependent on experimental processing, results in ambiguous transport behavior. The highly stable n-type polycrystalline BiAgSe2−xSx (x = 1.2) sample was successfully synthesized, guided by phase boundary engineering. Whilst maintaining promising thermoelectric properties, significant enhancement of the thermodynamical stability was obtained due to the strengthened chemical bonding caused by the substitution of Se with high-electronegativity S. Cubic BiAgSe0.8S1.2 can be well preserved after thermoelectric measurements. Our work demonstrates that phase boundary engineering is an applicable route to stabilize some compounds with moderate thermodynamical stability.

In order to find a new type of antifouling coating with higher biological activity and more environmental protection, heterocyclic compounds and benzisothiazolinone were introduced into acrylic resin to prepare a new type of antifouling resin. In this study, a series of grafted acrylic resins simultaneously containing benzoisothiazolinone and heterocyclic monomers were prepared by the copolymerization of an allyl monomer with methyl methacrylate (MMA) and butyl acrylate (BA). Inhibitory activities of the copolymers against marine fouling organisms were also investigated. Results revealed that the copolymers exhibit a clear synergistic inhibitory effect on the growth of three seaweeds: Chlorella, Isochrysis galbana and Chaetoceros curvisetus, respectively, and three bacteria, Staphylococcus aureus, Vibrio coralliilyticus and Vibrio parahaemolyticus, respectively. In addition, the copolymers exhibited excellent inhibition against barnacle larvae. Marine field tests indicated that the resins exhibit outstanding antifouling potency against marine fouling organisms. Moreover, the introduction of the heterocyclic group led to the significantly enhanced antifouling activities of the resins; the addition of the heterocyclic unit in copolymers led to better inhibition than that observed in the case of the resin copolymerized with only the benzoisothiazolinone active monomer.

Monocular depth estimation is a basic task in machine vision. In recent years, the performance of monocular depth estimation has been greatly improved. However, most depth estimation networks are based on a very deep network to extract features that lead to a large amount of information lost. The loss of object information is particularly serious in the encoding and decoding process. This information loss leads to the estimated depth maps lacking object structure detail and have non-clear edges. Especially in a complex indoor environment, which is our research focus in this paper, the consequences of this loss of information are particularly serious. To solve this problem, we propose a Dense feature fusion network that uses a feature pyramid to aggregate various scale features. Furthermore, to improve the fusion effectiveness of decoded object contour information and depth information, we propose an adaptive depth fusion module, which allows the fusion network to fuse various scale depth maps adaptively to increase object information in the predicted depth map. Unlike other work predicting depth maps relying on U-NET architecture, our depth map predicted by fusing multi-scale depth maps. These depth maps have their own characteristics. By fusing them, we can estimate depth maps that not only include accurate depth information but also have rich object contour and structure detail. Experiments indicate that the proposed model can predict depth maps with more object information than other prework, and our model also shows competitive accuracy. Furthermore, compared with other contemporary techniques, our method gets state-of-the-art in edge accuracy on the NYU Depth V2 dataset.

A series of novel bis-acenaphthoquinone diimides featuring a highly electron-deficient bis-acenaphthoquinone core are facilely synthesized via Knoevenagel condensation reaction. The diimides show high electron deficiency and good coplanar conformation, together with one of them having a maximum electron mobility up to 0.038 cm2 V-1 s-1.

In this paper we consider 2D nonlocal diffusion models with a finite nonlocal horizon parameterδcharacterizing the range of nonlocal interactions, and consider the treatment of Neumann-like boundary conditions that have proven challenging for discretizations of nonlocal models. We propose a new generalization of classical local Neumann conditions by converting the local flux to a correction term in the nonlocal model, which provides an estimate for the nonlocal interactions of each point with points outside the domain. While existing 2D nonlocal flux boundary conditions have been shown to exhibit at most first order convergence to the local counter part asδ → 0, the proposed Neumann-type boundary formulation recovers the local case asO(δ2) in theL∞(Ω) norm, which is optimal considering theO(δ2) convergence of the nonlocal equation to its local limit away from the boundary. We analyze the application of this new boundary treatment to the nonlocal diffusion problem, and present conditions under which the solution of the nonlocal boundary value problem converges to the solution of the corresponding local Neumann problem as the horizon is reduced. To demonstrate the applicability of this nonlocal flux boundary condition to more complicated scenarios, we extend the approach to less regular domains, numerically verifying that we preserve second-order convergence for non-convex domains with corners. Based on the new formulation for nonlocal boundary condition, we develop an asymptotically compatible meshfree discretization, obtaining a solution to the nonlocal diffusion equation with mixed boundary conditions that converges withO(δ2) convergence.

Carrier-free nanomedicines without structural modification are attractive for the development of natural small molecules (NSMs) and biomedical applications. Moreover, the combination of NSMs is expected to obtain nanomedicines with high efficacy and low side effects due to their inherent pharmacological activities and health benefits. However, poor water solubility and low bioavailability of NSMs limit their wider biomedical and clinical applications. In this study, we revealed the co-assembly properties of pentacyclic triterpenoids and constructed a series of carrier-free nanodrugs, which are co-assembled nanoparticles (NPs) formed by the combination of two NSMs via a supramolecular assembly strategy. Experimental work and simulation studies were combined to reveal the co-assembly mechanism of non-covalent interactions between NSMs. Not only do co-assembled NPs have rapid cellular uptake ability and passive targeting tumor ability based on the EPR effect, but also their constituent units could arrest the cell cycle at different stages of tumor cells and induce apoptosis, showing synergistic anti-tumor effects (CI < 0.7). Compared with self-assembled NPs and positive control, co-assembled NPs show the strongest therapeutic effect in vivo. Importantly, the co-assembled NPs highlight the unique advantages of NSMs in terms of biosafety and health benefits, and systemic toxicity and histological examination confirm that co-assembled NPs have reliable biosafety, and no side effects and nano toxicity risks were observed.

The immense reduction in aerosol levels during the COVID-19 pandemic provides an opportunity to reveal how atmospheric chemistry is regulating our climate, among which the effect of aerosols on climate is a phenomenon of great interest but still in hot debate. The Intergovernmental Panel on Climate Change (IPCC) has continually identified the effect of aerosols on climate to have the largest uncertainty among the factors contributing to global climate change. Several studies indicate an inverse relationship between aerosol presence in the atmosphere and the diurnal surface air temperature range (DTR). Herein, we test this relationship by analyzing the DTR values from in situ weather station records for periods before and during the COVID-19 epidemic in China where aerosol levels have substantially reduced, compared with the climatological mean levels for a 19 year period. Our analyses find that DTRs from February to June during the COVID-19 pandemic are greater than 3 standard deviations above the climatological mean DTR. This anomaly has never occurred before in the 21st century and is at least in part associated with the observed reduction in aerosols.

Carrier-free pure drug self-assembled nanosystems have been proposed as a promising strategy for synergetic anticancer therapy. Herein, we purposefully designed and synthesized disulfide-modified glutathione (GSH)-responsive natural pentacyclic triterpene betulinic acid (BA) with better biodegradability and biocompatibility to construct carrier-free photosensitive prodrugs BA-S-S/Ce6 NPs for synergistically enhanced and biosafe photochemotherapy. The molecular dynamics simulation elucidates the possible coassembly mechanism that the coplanar arrangement of BA-S-S dimeric may be primarily responsible for the formation of a long lamella-like or spherical morphology. The density functional theory calculations demonstrate that the reduced energy gap (ΔEST) of Ce6 facilitates the improved singlet oxygen generation of BA-S-S/Ce6 nanoparticles (NPs). The assembled prodrugs exhibited remarkable GSH-responsive property and multiple favorable therapeutic features, leading to enhanced synergistic antitumor efficacy without noticeable toxicity. Additionally, evaluation of the antitumor efficacy of another tetracyclic triterpene stigmasterol (ST)-mediated ST-S-S/Ce6 NPs further confirmed the effectiveness of this rational design. This work provides a promising insight for exploring the pure drug self-assembly behavior and construction of GSH-responsive carrier-free triterpenoid prodrugs toward improved multiple combination antitumor therapies.

Kenaf (Hibiscus cannabinus L.) is an important bast fiber crop, and a source of fiber to many industries. This crop is diploid (2n = 2x = 36) in nature, and belongs to Malvaceae family. Kenaf breed...

Within the framework of the International Arctic Systems for Observing the Atmosphere (IASOA), we report a modelling-based study on surface ozone across the Arctic. We use surface ozone from six sites – Summit (Greenland), Pallas (Finland), Barrow (USA), Alert (Canada), Tiksi (Russia), and Villum Research Station (VRS) at Station Nord (North Greenland, Danish realm) – and ozone-sonde data from three Canadian sites: Resolute, Eureka, and Alert. Two global chemistry models – a global chemistry transport model (parallelised-Tropospheric Offline Model of Chemistry and Transport, p-TOMCAT) and a global chemistry climate model (United Kingdom Chemistry and Aerosol, UKCA) – are used for model data comparisons. Remotely sensed data of BrO from the GOME-2 satellite instrument and ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) at Eureka, Canada, are used for model validation. The observed climatology data show that spring surface ozone at coastal sites is heavily depleted, making ozone seasonality at Arctic coastal sites distinctly different from that at inland sites. Model simulations show that surface ozone can be greatly reduced by bromine chemistry. In April, bromine chemistry can cause a net ozone loss (monthly mean) of 10–20 ppbv, with almost half attributable to open-ocean-sourced bromine and the rest to sea-ice-sourced bromine. However, the open-ocean-sourced bromine, via sea spray bromide depletion, cannot by itself produce ozone depletion events (ODEs; defined as ozone volume mixing ratios, VMRs, < 10 ppbv). In contrast, sea-ice-sourced bromine, via sea salt aerosol (SSA) production from blowing snow, can produce ODEs even without bromine from sea spray, highlighting the importance of sea ice surface in polar boundary layer chemistry. Modelled total inorganic bromine (BrY) over the Arctic sea ice is sensitive to model configuration; e.g. under the same bromine loading, BrY in the Arctic spring boundary layer in the p-TOMCAT control run (i.e. with all bromine emissions) can be 2 times that in the UKCA control run. Despite the model differences, both model control runs can successfully reproduce large bromine explosion events (BEEs) and ODEs in polar spring. Model-integrated tropospheric-column BrO generally matches GOME-2 tropospheric columns within ∼ 50 % in UKCA and a factor of 2 in p-TOMCAT. The success of the models in reproducing both ODEs and BEEs in the Arctic indicates that the relevant parameterizations implemented in the models work reasonably well, which supports the proposed mechanism of SSA production and bromide release on sea ice. Given that sea ice is a large source of SSA and halogens, changes in sea ice type and extent in a warming climate will influence Arctic boundary layer chemistry, including the oxidation of atmospheric elemental mercury. Note that this work dose not necessary rule out other possibilities that may act as a source of reactive bromine from the sea ice zone.

Chlorine radicals, including Cl• and Cl2•-, can be produced in sunlight waters (rivers, oceans, and lakes) or water treatment processes (e.g., electrochemical and advanced oxidation processes). Dissolved organic matter (DOM) is a major reactant with, or a scavenger of, Cl• and Cl2•- in water, but limited quantitative information exists regarding the influence of DOM structure on its reactivity with Cl• and Cl2•-. This study aimed at quantifying the reaction rates and the formation of chlorinated organic byproducts produced from Cl• and Cl2•- reactions with DOM. Laser flash photolysis experiments were conducted to quantify the second-order reaction rate constants of 19 DOM isolates with Cl• (kDOM-Cl•) and Cl2•- (kDOM-Cl2•-), and compare those with the hydroxyl radical rate constants (kDOM-•OH). The values for kDOM-Cl• ((3.71 ± 0.34) × 108 to (1.52 ± 1.56) × 109 MC-1 s-1) were orders of magnitude greater than the kDOM-Cl2•- values ((4.60 ± 0.90) × 106 to (3.57 ± 0.53) × 107 MC-1 s-1). kDOM-Cl• negatively correlated with the weight-averaged molecular weight (MW) due to the diffusion-controlled reactions. DOM with high aromaticity and total antioxidant capacity tended to react faster with Cl2•-. During the same experiments, we also monitored the formation of chlorinated byproducts through the evolution of total organic chlorine (TOCl) as a function of chlorine radical oxidant exposure (CT value). Maximum TOCl occurred at a CT of 4-8 × 10-12 M·s for Cl• and 1.1-2.2 × 10-10 M·s for Cl2•-. These results signify the importance of DOM in scavenging chlorine radicals and the potential risks of producing chlorinated byproducts of unknown toxicity.

We report a novel authigenic nanoscale magnetite source in marine methane seep sediments. The magnetite occurs in large concentrations in multiple horizons in a 230 m sediment core with gas hydrate–bearing intervals. In contrast to typical biogenic magnetite produced by magnetotactic bacteria and dissimilatory iron-reducing bacteria, most particles have sizes of 200–800 nm and many are aligned in distinctive structures that resemble microbial precipitates. The magnetite is interpreted to be a byproduct of microbial iron reduction within methanic sediments with rapidly changing redox conditions. Iron sulfides that accumulated at a shallow sulfate-methane transition zone were oxidized after methane seepage intensity decreased. The alteration process produced secondary iron (oxyhydr)oxides that then became a reactive iron source for magnetite authigenesis when methane seepage increased again. This interpretation is consistent with 13C depletion in coexisting carbonate nodules. The authigenic magnetite will record younger paleomagnetic signals than surrounding sediments, which is important for paleomagnetic interpretations in seep systems. The microbial and possibly abiotic processes that caused these magnetic minerals to form at moderate burial depths remain to be determined.