Conformational change-modulated spin transport at single-molecule level in carbon systems

Controlling the spin transport at the single-molecule level, especially without the use of ferromagnetic contacts, becomes a focus of research in spintronics. Inspired by the progress on atomic-level molecular synthesis, through first-principles calculations, we investigate the spin-dependent electronic transport of graphene nanoflakes with side-bonded functional groups, contacted by atomic carbon chain electrodes. It is found that, by rotating the functional group, the spin polarization of the transmission at the Fermi level could be switched between completely polarized and unpolarized states. Moreover, the transition between spin-up and spin-down polarized states can also be achieved, operating as a dual-spin filter. Further analysis shows that, it is the spin-dependent shift of density of states, caused by the rotation, that triggers the shift of transmission peaks, and then results in the variation of spin polarization. Such a feature is found to be robust to the length of the nanoflake and the electrode material, showing great application potential. Those findings may throw light on the development of spintronic devices.     

Machine-learning-driven on-demand design of phononic beams

The development of phononic crystals, especially their interaction with topological insulators, allows exploration of the anomalous properties of acoustic/elastic waves for various applications. However, rapidly and inversely exploring the geometry of specific targets remains a major challenge. In this work, we show how machine learning can address this challenge by studying phononic crystal beams using two different inverse design schemes. We first develop the theory of phononic beams using the transfer matrix method. Then, we use the reinforcement learning algorithm to effectively and inversely design the structural parameters to maximize the bandgap width. Furthermore, we employ the tandem-architecture neural network to solve the training-difficulty problem caused by inconsistent data and complete the task of inverse structure design with the targeted topological properties. The two inverse-design schemes have different adaptabilities, and both are characterized by high efficiency and stability. This work provides deep insights into the combination of machine learning, topological property,and phononic crystals and offers a reliable platform for rapidly and inversely designing complex material and structure properties.     

Trimetaphosphate-induced chiral selection between amino acid and nucleoside using 15N-31P coupling NMR

Life on Earth uses a common set of L-amino acids （L-aa） to construct proteins and D-nucleosides （D-Nu） to form nucleic acids,which serve as the carrier of genetic information.Herein,we reveal the intrinsic mechanism of chiral selection of L-aa and D-Nu from the perspective of chemical origin of life.This work employed¹⁵N-labeled L-aa and performed one-pot synthesis of nucleotide amidate of amino acid （N-aa-NMP） using equal amounts of L-¹⁵N-aa and D-¹⁴N-aa with D-...     

Defect-rich and ultrathin nitrogen-doped carbon nanosheets with enhanced peroxidase-like activity for the detection of urease activity and fluoride ion

Although carbon nanozymes have attracted great interest due to their good biocompatibility, low cost,and high stability, designing high-active carbon nanozymes still faces great challenges. Herein, ultrathin nitrogen-doped carbon nanosheets with rich defects(d-NC) were prepared through a high-temperature annealing process, using potassium chloride and ammonium chloride as templates. Owing to the large specific surface area, rich defects and the high exposure of active sites, the proposed d-NC na...     

Low-temperature Li-S batteries enabled by all amorphous con version process of organosulfur cathode

The high degree of crystallinity of discharging in termediates of Li-S batteries(Li₂S₂/Li₂S)causes a severe capacity attenuation at low temperatures.Herein,a sulfur-rich polymer is fabricated,which enables all the discharging in termediates to exist in an amorphous state without long-range order,promoti ng the substantial conversion of discharging intermediates and enhancing Li-S batteries'performance at low temperatures greatly.This cathode material exhibits excellent performance both at room and low temperatures.Even under an extremely low temperature(-40℃),the discharge capacity can remain 67% of that at room temperature.Besides,in-situ UV/Vis spectroscopy and density functional theory calculations reveal that this organosulfur cathode undergoes a new mechanism during discharge.Li₂S₆ and Li₂S₃ are the primary discharging intermediates that are quite different from conventional Li-S batteries.These results provide a new directi on for a broader range of applications of Li-S batteries.     

Visible-light-promoted radical alkylation/cyclization of allylic amide with N-hydroxyphthalimide ester: Synthesis of oxazolines

An efficient photocatalytic alkylation/cyclization of allylic amide with N-hydroxyphthalimide ester has been developed. The transformation is taken advantage of alkyl radicals to attack allylic amide with the assist of inexpensive rose bengal as photocatalyst to prepare a series of alkyl substituted oxazolines in moderate to excellent yields. High regioselectivity, operational safety, mild conditions and excellent substrate generality give this protocol broad application prospects.     

Shared-probe system: An accurate,low-cost and general enzyme-assisted DNA probe system for detection of genetic mutation

Enzyme assisted DNA probes are powerful tools in molecular diagnostics for their simplicity, rapidity,and low detection limit. However, cost of probes, difficulty in optimization and disturbance of secondary structure hindered the wider application of enzyme assisted DNA probes. To solve the problems, we designed a new system named shared-probe system. By introducing two unlabeled single stranded DNA named Sh1 and Sh2 as the bridge between probe and the substrate, the same sequence of dually lab...     

Study on divertor plasma behavior through sweeping strike point in new lower divertor on EAST

A series of L-mode discharges have been conducted in the new ‘corner slot’ divertor on the Experimental Advanced Superconducting Tokamak (EAST) to study the divertor plasma behavior through sweeping strike point. The plasma control system controls the strike point sweeping from the horizontal target to the vertical target through poloidal field coils, with keeping the main plasma stability. The surface temperature of the divertor target cools down as the strike point moves away, indicating that sweeping strike point mitigates the heat load. To avoid the negative effect of probe tip damage, a method based on sweeping strike point is used to get the normalized profile and study the decay length of particle and heat flux on the divertor target λ_js, λ_q. In the discharges with high radio-frequency (RF) heating power, electron temperature T_e is lower and λ_js is larger when the strike point locates on the horizontal target compared to the vertical target, probably due to the corner effect. In the Ohmic discharges, λ_js, λ_q are much larger compared to the discharges with high RF heating power, which may be attributed to lower edge T_e.     

Insights into the efficient charge separation over Nb2O5/2D-C3N4 heterostructure for exceptional visible-light driven H2 evolution

Two-dimensional carbon nitride(2 D-C₃ N₄)nanosheets are promising materials in photocatalytic water splitting,but still suffer from easy agglomeration and fast photogene rated electron-hole pairs recombination.To tackle this issue,herein,a hierarchical Nb₂ O₅/2 D-C₃ N₄ heterostructure is precisely constructed and the built-in electric field between Nb₂O₅ and 2 D-C₃ N₄ can provide the driving force to separate/transfer the charge carriers efficiently.Moreover,the strongly Lewis acidic Nb₂O₅ can adsorb TEOA molecules on its surface at locally high concentrations to facilitate the oxidation reaction kinetics under irradiation,resulting in efficient photogene rated electrons-holes separation and exceptional photocatalytic hydrogen evolution.As expected,the champion Nb₂O₅/2 D-C₃N₄ heterostructure achieves an exceptional H2 evolution rate of 31.6 mmol g^-1 h^-1,which is 213.6 times and 4.3 times higher than that of pristine Nb₂O₅ and2 D-C₃N₄,respectively.Moreover,the champion heterostructure possesses a high apparent quantum efficiency(AQE)of 45.08%atλ=405 nm and superior cycling stability.Furthermore,a possible photocatalytic mechanism of the energy band alignment at the hetero-interface is proposed based on the systematical characterizations accompanied by density functional theory(DFT)calculations.This work paves the way for the precise construction of a high-quality heterostructured photocatalyst with efficient charge separation to boost hydrogen production.     

Interface engineering of porous Fe2P-WO2.92 catalyst with oxygen vacancies for highly active and stable large-current oxygen evolution and overall water splitting

Constructing a low cost,and high-efficiency oxygen evolution reaction(OER)electrocatalyst is of great significance for improving the performance of alkaline electrolyzer,which is still suffering from highenergy consumption.Herein,we created a porous iron phosphide and tungsten oxide self-supporting electrocatalyst with oxygen-containing vacancies on foam nickel(Fe₂P-WO_2.92/NF)through a facile insitu growth,etching and phosphating strategies.The sequence-controllable strategy will not only generate oxygen vacancies and improve the charge transfer between Fe₂P and WO_2.92 components,but also improve the catalyst porosity and expose more active sites.Electrochemical studies illustrate that the Fe₂P-WO_2.92/NF catalyst presents good OER activity with a low overpotential of 267 mV at 100 mA cm^-2,a small Tafel slope of 46.3 mV dec^-1,high electrical conductivity,and reliable stability at high current density(100 mA cm^-2 for over 60 h in 1.0 M KOH solution).Most significantly,the operating cell voltage of Fe₂P-WO_2.92/NF‖Pt/C is as low as 1.90 V at 400 mA cm^-2 in alkaline condition,which is one of the lowest reported in the literature.The electrocatalytic mechanism shows that the oxygen vacancies and the synergy between Fe₂P and WO_2.92 can adjust the electronic structure and provide more reaction sites,thereby synergistically increasing OER activity.This work provides a feasible strategy to fabricate high-efficiency and stable non-noble metal OER electrocatalysts on the engineering interface.