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Carbon is one of the most important elements for both industrial applications and fundamental research, including life, physics, chemistry, materials, and even planetary science. Although theoretical predictions on the transition from diamond to the BC8 (Ia3[over ¯]) carbon were made more than thirty years ago, after tremendous experimental efforts, direct evidence for the existence of BC8 carbon is still lacking. In this study, a machine learning potential was developed for high-pressure carbon fitted from first-principles calculations, which exhibited great capabilities in modeling the melting and Hugoniot line. Using the molecular dynamics based on this machine learning potential, we designed a thermodynamic pathway that is achievable for the double shock compression experiment to obtain the elusive BC8 carbon. Diamond was compressed up to 584 GPa after the first shock at 20.5 km/s. Subsequently, in the second shock compression at 24.8 or 25.0 km/s, diamond was compressed to a supercooled liquid and then solidified to BC8 in around 1 ns. Furthermore, the critical nucleus size and nucleation rate of BC8 were calculated, which are crucial for nano-second x-ray diffraction measurements to observe BC8 carbon during shock compressions. The key to obtaining BC8 carbon lies in the formation of liquid at a sufficient supercooling. Our work provides a feasible pathway by which the long-sought BC8 phase of carbon can be reached in experiments.
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The municipal solid waste (MSW) with high water content can be pre-treated by the mechanical dewatering technology to significantly decrease the leachate generation in sequential landfill treatment or to improve the efficiency for solid waste incineration, which has attracted great concerns recently. However, the generated mechanical dewatering wastewater (MDW) containing high organics and nitrogenous content has been one of the big challenges for the sustainable treatment of MSW. In this study, a pilot-scale integrated system composed of physiochemical pretreatment, anaerobic sequencing batch reactor (ASBR), partial nitrification SBR (PN-SBR), denitrification SBR (DN-SBR), and UV/O3 advanced oxidation process, with a capacity of 1.0 m3/d to treat MDW containing over 34000 mg-chemical oxygen demand (COD)/L organics pollutant and 850 mg/L NH4+-N, was successfully developed. By explorations on the start-up of this integrated system and the process conditions optimization, after a long-term system operation, the findings demonstrated that this integrated system could reach the removal efficiency in the COD, NH4+-N and total nitrogen (TN) in the MDW of 99.7%, 98.2% and 96.9%, respectively. Partial nitrification and denitrification were successfully obtained for the TN removal with the nitrite accumulation rate of over 80%. The treatment condition parameters were optimized to be 800 mg/L polyaluminum chloride (PAC) and 2 mg/L polyacrylamide (PAM) under a pH of 9 for pretreatment, 36 h hydraulic retention time (HRT) for ASBR, 24 h for PN-SBR, and 2 h for UV/O3 unit. The organic sources in the MDW were also found to be feasible for the DN-SBR. Consequently, the resulting final effluent was stably in compliance with the discharge standard with high stability and reliability.
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Nitrificación , Contaminantes Químicos del Agua , Aguas Residuales , Desnitrificación , Reproducibilidad de los Resultados , Residuos Sólidos , Aguas del Alcantarillado/química , Reactores Biológicos , Contaminantes Químicos del Agua/química , Nitrógeno/química , Oxidación-ReducciónRESUMEN
Superconducting and superionic behaviors have physically intriguing dynamic properties of electrons and ions, respectively, both of which are conceptually important and have great potential for practical applications. Whether these two phenomena can appear in the same system is an interesting and important question. Here, using crystal structure predictions and first-principle calculations combined with machine learning, we identify several stable Li-Al compounds with electride behavior under high pressure, and we find that the electronic density of states of some of the compounds has characteristics of the two-dimensional electron gas. Among them, we estimate that Li_{6}Al at 150 GPa has a superconducting transition temperature of around 29 K and enters a superionic state at a high temperature and wide pressure range. The diffusion in Li_{6}Al is found to be affected by an electride and attributed to the atomic collective motion. Our results indicate that alkali metal alloys can be effective platforms to study the abundant physical properties and their manipulation with pressure and temperature.
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Silica, water, and hydrogen are known to be the major components of celestial bodies, and have significant influence on the formation and evolution of giant planets, such as Uranus and Neptune. Thus, it is of fundamental importance to investigate their states and possible reactions under the planetary conditions. Here, using advanced crystal structure searches and first-principles calculations in the Si-O-H system, we find that a silica-water compound (SiO_{2})_{2}(H_{2}O) and a silica-hydrogen compound SiO_{2}H_{2} can exist under high pressures above 450 and 650 GPa, respectively. Further simulations reveal that, at high pressure and high temperature conditions corresponding to the interiors of Uranus and Neptune, these compounds exhibit superionic behavior, in which protons diffuse freely like liquid while the silicon and oxygen framework is fixed as solid. Therefore, these superionic silica-water and silica-hydrogen compounds could be regarded as important components of the deep mantle or core of giants, which also provides an alternative origin for their anomalous magnetic fields. These unexpected physical and chemical properties of the most common natural materials at high pressure offer key clues to understand some abstruse issues including demixing and erosion of the core in giant planets, and shed light on building reliable models for solar giants and exoplanets.
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Seawater desalination is one of the most applied approaches for freshwater replenishment. However, the process not only generates freshwater but also consumes it. It is important to evaluate the balance of the production and consumption of freshwater in desalination, which is also called as water footprint. It will reveal the feasibility of seawater desalination in terms of water production, but related study has not been reported. In this study, the water footprint of reverse osmosis desalination process has been investigated based on a real reverse osmosis desalination plant data. According to the calculation, the freshwater utilization of the reverse osmosis desalination plant was about 8.16 × 10-3 m3 with 1 m3 freshwater production. The study reveals that RO desalination is freshwater gain process as the utilized freshwater amount was less than the one produced. The sensitivity study showed that the energy source used in the process was the most significant parameter affecting on the water footprint. The freshwater required in the reverse osmosis desalination with energy supplied by thermal and solar was 8.01 × 10-3 m3 and 9.90 × 10-3 m3 in 1 m3 freshwater generation, respectively. It suggests that energy source selection is important in RO desalination system.
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Purificación del Agua , Filtración , Ósmosis , Agua de Mar , AguaRESUMEN
Silica (SiO_{2}), as a raw material of silicon, glass, ceramics, abrasive, and refractory substances, etc., is of significant importance in industrial applications and fundamental research such as electronics and planetary science. Here, using a crystal structure searching method and first-principles calculations, we predicted that a ground state crystalline phase of silica with R3[over ¯] symmetry is stable at around 645-890 GPa, which contains six-, eight-, and nine-coordinated silicon atoms and results in an average coordination number of eight. This mixed-coordination silica fills in the density, electronic band gap, and coordination number gaps between the previously known sixfold pyrite-type and ninefold Fe_{2}P-type phases, and may appear in the core or mantle of super-Earth exoplanets, or even the solar giant planets such as the Neptune. In addition, we also found that some silicon superoxides, Cmcm SiO_{3} and Ccce SiO_{6}, are stable in this pressure range and may appear in an oxygen-rich environment. Our finding enriches the high-pressure phase diagram of silicon oxides and improves understanding of the interior structure of giant planets in our solar system.
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Phosphate removal through in-situ Fe2+ oxidation induced homogenous phosphate precipitation has shown its advantages in municipal wastewater treatment. Its feasibility and suitability for phosphate removal in industrial wastewater with wide-range pH variation like electro-plating wastewater were investigated in bench scale experiments using synthetic wastewater and continuous experiment using real wastewater. Bench scale experiments showed that different Fe2+ oxidation approaches worked well for phosphate removal at varied pH conditions. Sole dosing Fe2+ salt with aeration achieved sound phosphate removal at alkaline condition (pHâ¯≥â¯8). At neutral pH (6â¯<â¯pHâ¯<â¯8), transition metallic ions catalytic oxidation is a suitable alternative. Cu2+ exhibited superior catalytic Fe2+ oxidization over Mn2+, Zn2+, and Ni2+. At acid pH (3.0 ï¼ pHâ¯≤â¯6.0), Fenton reaction oxidation (H2O2â¯=â¯5â¯mg/L) showed its efficiency. At their corresponding optimal pH conditions and with Fe2+/P ratio of 1.8, dosing sole Fe2+ salt, Cu2+ catalyzed Fe2+ oxidation, and Fe2+/H2O2 treatments can achieve the TP discharge limit of 0.5â¯mg/L. In a 30-day continuous experiment using real electro-plating wastewater (pH 4.9-5.5), in both direct Fe2+/H2O2 treatment and Cu2+ catalyzed Fe2+ oxidation treatment after wastewater pH being adjusted to 7 effluent TP met China's discharge requirement 0.5â¯mg/L.
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Aguas Residuales , Contaminantes Químicos del Agua , China , Peróxido de Hidrógeno , Concentración de Iones de Hidrógeno , Hierro , Oxidación-Reducción , Fosfatos , Eliminación de Residuos LíquidosRESUMEN
Topological states of quantum matter have attracted great attention in condensed matter physics and materials science. The study of time-reversal-invariant topological states in quantum materials has made tremendous progress. However, the study of magnetic topological states falls much behind due to the complex magnetic structures. Here, we predict the tetradymite-type compound MnBi_{2}Te_{4} and its related materials host topologically nontrivial magnetic states. The magnetic ground state of MnBi_{2}Te_{4} is an antiferromagetic topological insulator state with a large topologically nontrivial energy gap (â¼0.2 eV). It presents the axion state, which has gapped bulk and surface states, and the quantized topological magnetoelectric effect. The ferromagnetic phase of MnBi_{2}Te_{4} might lead to a minimal ideal Weyl semimetal.
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van der Waals junctions of two-dimensional materials with an atomically sharp interface open up unprecedented opportunities to design and study functional heterostructures. Semiconducting transition metal dichalcogenides have shown tremendous potential for future applications due to their unique electronic properties and strong light-matter interaction. However, many important optoelectronic applications, such as broadband photodetection, are severely hindered by their limited spectral range and reduced light absorption. Here, we present a p-g-n heterostructure formed by sandwiching graphene with a gapless band structure and wide absorption spectrum in an atomically thin p-n junction to overcome these major limitations. We have successfully demonstrated a MoS2-graphene-WSe2 heterostructure for broadband photodetection in the visible to short-wavelength infrared range at room temperature that exhibits competitive device performance, including a specific detectivity of up to 10(11) Jones in the near-infrared region. Our results pave the way toward the implementation of atomically thin heterostructures for broadband and sensitive optoelectronic applications.
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Weyl semimetals are new states of matter which feature novel Fermi arcs and exotic transport phenomena. Based on first-principles calculations, we report that the chalcopyrites CuTlSe_{2}, AgTlTe_{2}, AuTlTe_{2}, and ZnPbAs_{2} are ideal Weyl semimetals, having largely separated Weyl points (â¼0.05 Å^{-1}) and uncovered Fermi arcs that are amenable to experimental detections. We also construct a minimal effective model to capture the low-energy physics of this class of Weyl semimetals. Our discovery is a major step toward a perfect playground of intriguing Weyl semimetals and potential applications for low-power and high-speed electronics.
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We report a new pressure-induced phase in TaAs with different Weyl fermions than the ambient structure with the aid of theoretical calculations, experimental transport and synchrotron structure investigations up to 53 GPa. We show that TaAs transforms from an ambient I4_{1}md phase (t-TaAs) to a high-pressure hexagonal P-6m2 (h-TaAs) phase at 14 GPa, along with changes of the electronic state from containing 24 Weyl nodes distributed at two energy levels to possessing 12 Weyl nodes at an isoenergy level, which substantially reduces the interference between the surface and bulk states. The new pressure-induced phase can be reserved upon releasing pressure to ambient condition, which allows one to study the exotic behavior of a single set of Weyl fermions, such as the interplay between surface states and other properties.
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We report an atomic-scale characterization of ZrTe_{5} by using scanning tunneling microscopy. We observe a bulk band gap of â¼80 meV with topological edge states at the step edge and, thus, demonstrate that ZrTe_{5} is a two-dimensional topological insulator. We also find that an applied magnetic field induces an energetic splitting of the topological edge states, which can be attributed to a strong link between the topological edge states and bulk topology. The relatively large band gap makes ZrTe_{5} a potential candidate for future fundamental studies and device applications.
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Electron-phonon interactions and electron-electron correlations represent two crucial facets of condensed matter physics. For instance, in a half-filled spin-1/2 anti-ferromagnetic chain, the lattice dimerization induced by electron-nucleus interaction can be intensified by onsite Coulomb repulsion, resulting in a spin-Peierls state. Through first-principles calculations and crystal structure prediction methods, we have identified that under mild pressures, potassium and ammonia can form stable compounds: R3¯m K(NH3)2, Pm3¯m K(NH3)2, and Cm K2(NH3)3. Our predictions suggest that the R3¯m K(NH3)2 exhibits electride characteristics, marked by the formation of interstitial anionic electrons (IAEs) in the interlayer space. These IAEs are arranged in quasi-two-dimensional triangular arrays. With increasing pressure, the electronic van-Hove singularity shifts toward the Fermi level, resulting in an augmented density of states and the onset of both Peierls and magnetic instabilities. Analyzing these instabilities, we determine that the ground state of the R3¯m K(NH3)2 is the dimerized P21/m phase with zigzag-type anti-ferromagnetic IAEs. This state can be described by the triangular-lattice antiferromagnetic Heisenberg model with modulated magnetic interactions. Furthermore, we unveil the coexistence and positive interplay between magnetic and Peierls instability, constituting a scenario of spin-Peierls instability unprecedented in realistic 2D materials, particularly involving IAEs. This work provides valuable insights into the coupling of IAEs with the adjacent lattice and their spin correlations in quantum materials.
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Membranes for wastewater treatment should ideally exhibit sustainable high permeate production, enhanced pollutant removal, and intrinsic physical rejection. In this study, CoFe2O4/MoS2 serves as a non-homogeneous phase catalyst; it is combined with polyether sulfone membranes via liquid-induced phase separation to simultaneously sustain membrane permeability and enhance antibiotic pollutant degradation. The prepared catalytic membranes have higher pure water flux (329.34 L m-2 h-1) than pristine polyethersulfone membranes (219.03 L m-2 h-1), as well as higher mean pore size, porosity, and hydrophilicity. Under a moderate transmembrane pressure (0.05 MPa), tetracycline (TC) in synthetic and real wastewater was degraded by the optimal catalytic membrane by 72.7 % and 91.2 %, respectively. Owing to the generation of the reactive oxygen species (ROS) during the Fenton-like reaction process, the catalytic membrane could exclude the natural organics during the H2O2 backwash step and selectively promote fouling degradation in the membrane channel. The irreversible fouling ratio of the catalyzed membrane was significantly reduced, and the flux recovery rate increased by up to 91.6 %. A potential catalytic mechanism and TC degradation pathways were proposed. This study offers valuable insights for designing catalytic membranes with enhanced filtration performance.
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Antibacterianos , Disulfuros , Peróxido de Hidrógeno , Membranas Artificiales , Molibdeno , Permeabilidad , Contaminantes Químicos del Agua , Peróxido de Hidrógeno/química , Catálisis , Contaminantes Químicos del Agua/química , Antibacterianos/química , Disulfuros/química , Molibdeno/química , Sulfonas/química , Tetraciclina/química , Cobalto/química , Aguas Residuales/química , Purificación del Agua/métodos , Eliminación de Residuos Líquidos/métodos , Compuestos Férricos/química , Compuestos Ferrosos/química , PolímerosRESUMEN
Machine learning potential (MLP) has been a popular topic in recent years for its capability to replace expensive first-principles calculations in some large systems. Meanwhile, message passing networks have gained significant attention due to their remarkable accuracy, and a wave of message passing networks based on Cartesian coordinates has emerged. However, the information of the node in these models is usually limited to scalars, and vectors. In this work, we propose High-order Tensor message Passing interatomic Potential (HotPP), an E(n) equivariant message passing neural network that extends the node embedding and message to an arbitrary order tensor. By performing some basic equivariant operations, high order tensors can be coupled very simply and thus the model can make direct predictions of high-order tensors such as dipole moments and polarizabilities without any modifications. The tests in several datasets show that HotPP not only achieves high accuracy in predicting target properties, but also successfully performs tasks such as calculating phonon spectra, infrared spectra, and Raman spectra, demonstrating its potential as a tool for future research.
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Two-dimensional topological insulators hosting the quantum spin Hall effect have application potential in dissipationless electronics. To observe the quantum spin Hall effect at elevated temperatures, a wide band gap is indispensable to efficiently suppress bulk conduction. Yet, most candidate materials exhibit narrow or even negative band gaps. Here, via elegant control of van der Waals epitaxy, we have successfully grown monolayer ZrTe5 on a bilayer graphene/SiC substrate. The epitaxial ZrTe5 monolayer crystalizes in two allotrope isomers with different intralayer alignments of ZrTe3 prisms. Our scanning tunneling microscopy/spectroscopy characterization unveils an intrinsic full band gap as large as 254 meV and one-dimensional edge states localized along the periphery of the ZrTe5 monolayer. First-principles calculations further confirm that the large band gap originates from strong spin-orbit coupling, and the edge states are topologically nontrivial. These findings thus provide a highly desirable material platform for the exploration of the high-temperature quantum spin Hall effect.
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Crystal structure predictions based on first-principles calculations have gained great success in materials science and solid state physics. However, the remaining challenges still limit their applications in systems with a large number of atoms, especially the complexity of conformational space and the cost of local optimizations for big systems. Here, we introduce a crystal structure prediction method, MAGUS, based on the evolutionary algorithm, which addresses the above challenges with machine learning and graph theory. Techniques used in the program are summarized in detail and benchmark tests are provided. With intensive tests, we demonstrate that on-the-fly machine-learning potentials can be used to significantly reduce the number of expensive first-principles calculations, and the crystal decomposition based on graph theory can efficiently decrease the required configurations in order to find the target structures. We also summarized the representative applications of this method on several research topics, including unexpected compounds in the interior of planets and their exotic states at high pressure and high temperature (superionic, plastic, partially diffusive state, etc.); new functional materials (superhard, high-energy-density, superconducting, photoelectric materials), etc. These successful applications demonstrated that MAGUS code can help to accelerate the discovery of interesting materials and phenomena, as well as the significant value of crystal structure predictions in general.
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Magnesium Oxide (MgO) and water (H2O) are abundant in the interior of planets. Their properties, and in particular their interaction, significantly affect the planet interior structure and thermal evolution. Here, using crystal structure predictions and ab initio molecular dynamics simulations, we find that MgO and H2O can react again at ultrahigh pressure, although Mg(OH)2 decomposes at low pressure. The reemergent MgO-H2O compounds are: Mg2O3H2 above 400 GPa, MgO3H4 above 600 GPa, and MgO4H6 in the pressure range of 270-600 GPa. Importantly, MgO4H6 contains 57.3 wt % of water, which is a much higher water content than any reported hydrous mineral. Our results suggest that a substantial amount of water can be stored in MgO rock in the deep interiors of Earth to Neptune mass planets. Based on molecular dynamics simulations we show that these three compounds exhibit superionic behavior at the pressure-temperature conditions as in the interiors of Uranus and Neptune. Moreover, the water-rich compound MgO4H6 could be stable inside the early Earth and therefore may serve as a possible early Earth water reservoir. Our findings, in the poorly explored megabar pressure regime, provide constraints for interior and evolution models of wet planets in our solar system and beyond.
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An integrated process of electrochemical pre-treatment with carrier-based membrane bioreactor (MBR) was constructed for fresh leachate from waste transfer stations with high organic and NH4+-N content. Results showed that within a hydraulic retention time 40 h, the removal efficiencies of chemical oxygen demand (COD), NH4+-N, suspended solids (SS) and total phosphorus (TP) were over 98.5%, 91.2%, 98.3% and 98.4%, respectively, with the organic removal rate of 18.7 kg/m3. The effluent met the Grade A Standard of China (GB/T31962-2015). Pre-treatment contributed about 70 % of the degraded refractory organics and almost all the SS, with the transformation of the humic-like acid to readily biodegradable organics. Biotreatment further removed over 50% of nitrogen pollutants through simultaneous nitrification and denitrification (SND) and consumed about 30% of organics. Meanwhile, the addition of carriers in the oxic MBR enhanced the attached biomass and denitrification enzyme activity, alleviating membrane fouling.
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Reactores Biológicos , Nitrificación , Nitrógeno/química , Fósforo , Análisis de la Demanda Biológica de OxígenoRESUMEN
Metal cations are present in domestic and industrial wastewater and have adverse effects on human and aqueous life. The present study describes the development of the molecular probe 9-anthracen-9-ylmethylene)hydrazineylidene)methyl)-2,3,6,7-tetrahydro-1H,5H-pyrido[3,2,1-ij]quinolin-8-ol (AMHMPQ) to detect Cr3+, Cu2+, Fe3+, and Gd3+ ions by using UV-visible, fluorescence, colorimetric and excitation-emission matrix (EEM) spectroscopy techniques. The interaction of Cr3+, Cu2+, Fe3+, and Gd3+ can be observed by the absorption maxima shift, turn-off, colour changes, and EEM shifts. In addition, fluorescence limits of detection 17.66 × 10-6 M, 6.44 × 10-9 M, 28.87 × 10-8 M, and 12.49 × 10-6 M in wide linear ranges, low limits of quantifications, high values of Stern-Volmer constant, Job's plot and Benesi-Hildebrand plot justify the 1:1 association affinity with association constants of 1.46 × 104 M-1, 1.86 × 107 M-1, 2.69 × 105 M-1, 2.13 × 104 M-1 for AMHMPQ-metal ions (Cr3+, Cu2+, Fe3+, and Gd3+ ions), respectively. Paper- and mask-based kits are developed to explore the utility of the designed chemosensor. Additionally, AMHMPQ acts as a reusable sensor for two, seven, two, and zero cycles for Cr3+, Cu2+, Fe3+, and Gd3+ ions, respectively, when checked with EDTA.