Two-dimensional superconducting MoSi2N4(MoN)4n homologous compoundsOA

The number and stacking order of layers are two important degrees of freedom that can modulate the properties of 2D van der Waals(vdW) materials. However, the layers’ structures are essentially limited to the known layered 3D vdW materials. Recently, a new 2D vdW material, MoSi₂N₄, without known 3D counterparts, was synthesized by passivating the surface dangling bonds of non-layered 2D molybdenum nitride with elemental silicon, whose monolayer can be viewed as a monolayer ...     

Three Gorges Dam: friend or foe of riverine greenhouse gases?OA

Dams are often regarded as greenhouse gas(GHG) emitters. However, our study indicated that the world’s largest dam, the Three Gorges Dam(TGD), has caused significant drops in annual average emissions of CO₂, CH₄ and N₂O over 4300 km along the Yangtze River, accompanied by remarkable reductions in the annual export of CO₂(79%), CH₄(50%) and N₂O(9%) to the sea. Since the commencement of its operation in 2003, the TGD has altered the...     

Zeolite-encaged mononuclear copper centers catalyze CO2 selective hydrogenation to methanolOA

The selective hydrogenation of CO₂ to methanol by renewable hydrogen source represents an attractive route for CO₂ recycling and is carbon neutral.Stable catalysts with high activity and methanol selectivity are being vigorously pursued,and current debates on the active site and reaction pathway need to be clarified.Here,we report a design of faujasite-encaged mononuclear Cu centers,namely Cu@FAU,for this challenging reaction.Stable methanol space-time-yield(STY) of 12.8 mm...     

Linking deep CO2 outgassing to cratonic destructionOA

Outgassing of carbon dioxide from the Earth’s interior regulates the surface climate through deep time.Here we examine the role of cratonic destruction in mantle CO₂ outgassing via collating and presenting new data for Paleozoic kimberlites, Mesozoic basaltic rocks and their mantle xenoliths from the eastern North China Craton(NCC), which underwent extensive destruction in the early Cretaceous. High Ca/Al and low Ti/Eu and δ²⁶ Mg are widely observed in lamprophyres and mant...     

High-stability spherical lanthanide nanoclusters for magnetic resonance imagingOA

High-nuclear lanthanide clusters have shown great potential for the administration of high-dose mononuclear gadolinium chelates in magnetic resonance imaging(MRI). The development of high-nuclear lanthanide clusters with excellent solubility and high stability in water or solution has been challenging and is very important for expanding the performance of MRI. We used N-methylbenzimidazole-2-methanol(HL) and LnCl₃·6H₂O to synthesize two spherical lanthanide clusters, Ln     

N,N-dimethylformamide tailors solvent effect to boost Zn anode reversibility in aqueous electrolyteOA

Rechargeable aqueous Zn batteries are considered as promising energy-storage devices because of their high capacity,environmental friendliness and low cost.However,the hydrogen evolution reaction and growth of dendritic Zn in common aqueous electrolytes severely restrict the application of Zn batteries.Here,we develop a simple strategy to suppress side reactions and boost the reversibility of the Zn electrode.By introducing 30%(volume fractions) N,N-dimethylformamide(DMF) to the 2 M Zn(CF_3<...     

Pressure-induced superconductivity at 32 K in MoB2OA

Since the discovery of superconductivity in MgB₂(T_c～ 39 K),the search for superconductivity in related materials with similar structures or ingredients has never stopped.Although about 100 binary borides have been explored,only a few of them show superconductivity with relatively low T_c.In this work,we report the discovery of superconductivity up to 32 K,which is the highest T_c in transition-metal borides,in MoB₂under pressure.The T_c     

Unraveling the electrophilic oxygen-mediated mechanism for alcohol electrooxidation on NiOOA

Aqueous organic electrosynthesis such as nucleophile oxidation reaction(NOR) is an economical and green approach.However,its development has been hindered by the inadequate understanding of the synergy between the electrochemical and non-electrochemical steps.In this study,we unravel the NOR me chanism for the primary alcohol/vicinal diol electro oxidation on NiO.Thereinto,the ele ctrochemical step is the generation of Ni³⁺-(OH)_ads,and the spontaneous reaction between Ni     

Unraveling templated-regulated distribution of isolated SiO4 tetrahedra in silicoaluminophosphate zeolites with high-throughput computationsOA

Silicoaluminophosphate(SAPO) zeolites are well-known catalytic materials because of the mild acidity originating from the isolated SiO₄ tetrahedra in their frameworks. Regulating the distribution of isolated SiO₄ tetrahedra in SAPO zeolites is formidably challenging because SiO₄ tetrahedra tend to agglomerate to form Si islands and the isolated SiO₄ tetrahedra are difficult to determine using conventional characterization techniques. Here we synthesize...     

Worldwide impacts of atmospheric vapor pressure deficit on the interannual variability of terrestrial carbon sinksOA

Interannual variability of the terrestrial ecosystem carbon sink is substantially regulated by various environmental variables and highly dominates the interannual variation of atmospheric carbon dioxide(CO₂) concentrations.Thus,it is necessary to determine dominating factors affecting the interannual variability of the carbon sink to improve our capability of predicting future terrestrial carbon sinks.Using global datasets derived from machine-learning methods and process-based ecosy...     

Two-dimensional ferromagnetic superlattices

Mechanically exfoliated two-dimensional ferromagnetic materials (2D FMs) possess long-range ferromagnetic order and topologically nontrivial skyrmions in few layers. However, because of the dimensionality effect, such few-layer systems usually exhibit much lower Curie temperature (T_C) compared to their bulk counterparts. It is therefore of great interest to explore effective approaches to enhance their T_C, particularly in wafer-scale for practical applications. Here, we report an interfacial proximity-induced high-T_C 2D FM Fe₃GeTe₂ (FGT) via A-type antiferromagnetic material CrSb (CS) which strongly couples to FGT. A superlattice structure of (FGT/CS)_n, where n stands for the period of FGT/CS heterostructure, has been successfully produced with sharp interfaces by molecular-beam epitaxy on 2-inch wafers. By performing elemental specific X-ray magnetic circular dichroism (XMCD) measurements, we have unequivocally discovered that T_C of 4-layer Fe₃GeTe₂ can be significantly enhanced from 140 K to 230 K because of the interfacial ferromagnetic coupling. Meanwhile, an inverse proximity effect occurs in the FGT/CS interface, driving the interfacial antiferromagnetic CrSb into a ferrimagnetic state as evidenced by double-switching behavior in hysteresis loops and the XMCD spectra. Density functional theory calculations show that the Fe-Te/Cr-Sb interface is strongly FM coupled and doping of the spin-polarized electrons by the interfacial Cr layer gives rise to the T_C enhancement of the Fe₃GeTe₂ films, in accordance with our XMCD measurements. Strikingly, by introducing rich Fe in a 4-layer FGT/CS superlattice, T_C can be further enhanced to near room temperature. Our results provide a feasible approach for enhancing the magnetic order of few-layer 2D FMs in wafer-scale and render opportunities for realizing realistic ultra-thin spintronic devices.     

Mineralogy of the deep lower mantle in the presence of H2O

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)O₂H_x (x ≤ 1) phase. The (Mg, Fe)O₂H_x 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 (Mg_0.6Fe_0.4)O or beyond 2300 km for (Mg_0.7Fe_0.3)O. The (Mg, Fe)O₂H_x 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.     

Large-scale multiferroic complex oxide epitaxy with magnetically switched polarization enabled by solution processing

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)/2Fe_yMg_(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 μ_B/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.     

Exposed facet-controlled N2 electroreduction on distinct Pt3Fe nanostructures of nanocubes,nanorods and nanowires

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⁻¹_cat (0.52 μg h⁻¹ cm⁻²_ECSA; 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.     

Evidence for oxygenation of Fe-Mg oxides at mid-mantle conditions and the rise of deep oxygen

As the reaction product of subducted water and the iron core, FeO₂ with more oxygen than hematite (Fe₂O₃) has been recently recognized as an important component in the D” layer just above the Earth''s core-mantle boundary. Here, we report a new oxygen-excess phase (Mg, Fe)₂O_3+δ (0 < δ < 1, denoted as ‘OE-phase’). It forms at pressures greater than 40 gigapascal when (Mg, Fe)-bearing hydrous materials are heated over 1500 kelvin. The OE-phase is fully recoverable to ambient conditions for ex situ investigation using transmission electron microscopy, which indicates that the OE-phase contains ferric iron (Fe³⁺) as in Fe₂O₃ but holds excess oxygen through interactions between oxygen atoms. The new OE-phase provides strong evidence that H₂O has extraordinary oxidation power at high pressure. Unlike the formation of pyrite-type FeO₂Hx which usually requires saturated water, the OE-phase can be formed with under-saturated water at mid-mantle conditions, and is expected to be more ubiquitous at depths greater than 1000 km in the Earth''s mantle. The emergence of oxygen-excess reservoirs out of primordial or subducted (Mg, Fe)-bearing hydrous materials may revise our view on the deep-mantle redox chemistry.     

Surface superconductivity in the type II Weyl semimetal TaIrTe4

The search for unconventional superconductivity in Weyl semimetal materials is currently an exciting pursuit, since such superconducting phases could potentially be topologically non-trivial and host exotic Majorana modes. The layered material TaIrTe₄ is a newly predicted time-reversal invariant type II Weyl semimetal with the minimum number of Weyl points. Here, we report the discovery of surface superconductivity in Weyl semimetal TaIrTe₄. Our scanning tunneling microscopy/spectroscopy (STM/STS) visualizes Fermi arc surface states of TaIrTe₄ that are consistent with the previous angle-resolved photoemission spectroscopy results. By a systematic study based on STS at ultralow temperature, we observe uniform superconducting gaps on the sample surface. The superconductivity is further confirmed by electrical transport measurements at ultralow temperature, with an onset transition temperature (T_c) up to 1.54 K being observed. The normalized upper critical field h*(T/T_c) behavior and the stability of the superconductivity against the ferromagnet indicate that the discovered superconductivity is unconventional with the p-wave pairing. The systematic STS, and thickness- and angular-dependent transport measurements reveal that the detected superconductivity is quasi-1D and occurs in the surface states. The discovery of the surface superconductivity in TaIrTe₄ provides a new novel platform to explore topological superconductivity and Majorana modes.     

Correlating the electronic structures of metallic/semiconducting MoTe2 interface to its atomic structures

Contact interface properties are important in determining the performances of devices that are based on atomically thin two-dimensional (2D) materials, especially for those with short channels. Understanding the contact interface is therefore important to design better devices. Herein, we use scanning transmission electron microscopy, electron energy loss spectroscopy, and first-principles calculations to reveal the electronic structures within the metallic (1T^′)-semiconducting (2H) MoTe₂ coplanar phase boundary across a wide spectral range and correlate its properties to atomic structures. We find that the 2H-MoTe₂ excitonic peaks cross the phase boundary into the 1T^′ phase within a range of approximately 150 nm. The 1T^′-MoTe₂ crystal field can penetrate the boundary and extend into the 2H phase by approximately two unit-cells. The plasmonic oscillations exhibit strong angle dependence, that is a red-shift of π+σ (approximately 0.3–1.2 eV) occurs within 4 nm at 1T^′/2H-MoTe₂ boundaries with large tilt angles, but there is no shift at zero-tilted boundaries. These atomic-scale measurements reveal the structure–property relationships of the 1T^′/2H-MoTe₂ boundary, providing useful information for phase boundary engineering and device development based on 2D materials.     

Kinetic regulation of MXene with water-in-LiCl electrolyte for high-voltage micro-supercapacitors

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 Ti₃C₂T_x 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.     

Room-temperature multiferroicity and diversified magnetoelectric couplings in 2D materials

Multiferroics are rare in nature due to the mutual exclusive origins of magnetism and ferroelectricity. The simultaneous coexistence of robust magnetism/ferroelectricity and strong magnetoelectric coupling in single multiferroics is hitherto unreported, which may also be attributed to their potential conflictions. In this paper, we show the first-principles evidence of such desired coexistence in ultrathin-layer CuCrS₂ and CuCrSe₂. The vertical ferroelectricity is neither induced by an empty d shell nor spin-driven, giving rise to an alternative possibility of resolving those intrinsic exclusions and contradictions. Compared with their bulk phases, the ferromagnetism in the thin-layer structures (two–six layers) can be greatly stabilized due to the enhanced carrier density and orbital shifting by vertical polarization, and the Curie temperatures of both ferromagnetism and ferroelectricity can be above room temperature. Moreover, a considerable net magnetization can be reversed upon ferroelectric switching, where the change in spin-resolved band structure also renders efficient ‘magnetic reading + electrical writing’. The thickness-different layers may even exhibit diversified types of magnetoelectric coupling, which both enriches the physics of multiferroics and facilitates their practical applications.     

Influence of Altered Hormonal Status on Platelet 5-HT and MAO-B Activity in Cigarette Smokers

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.