Atomistic Modeling of Lithium Materials from Deep Learning Potential with Ab Initio Accuracy

Lithium has been paid great attention in recent years thanks to its significant appli-cations for battery and lightweight alloy.Developing a potential model with high ac-curacy and efficiency is impor-tant for theoretical simulation of lithium materials.Here,we build a deep learning potential(DP)for elemental lithium based on a concurrent-learning scheme and DP representation of the density-functional theory(DFT)potential energy surface(PES),the DP model enables material simulations with close-to DFT accuracy but at much lower computational cost.The simulations show that basic parameters,equation of states,elasticity,defects and surface are consistent with the first principles results.More notably,the liquid radial distribution func-tion based on our DP model is found to match well with experiment data.Our results demon-strate that the developed DP model can be used for the simulation of lithium materials.

Active Micro-Nano-Collaborative Bioelectronic Device for Advanced Electrophysiological Recording

The development of precise and sensitive electrophysiological recording platforms holds the utmost importance for research in the fields of cardiology and neuroscience.In recent years,active micro/nano-bioelectronic devices have undergone significant advancements,thereby facilitating the study of electrophysiology.The distinctive configuration and exceptional functionality of these active micro-nano-collaborative bioelectronic devices offer the potential for the recording of high-fidelity action potential signals on a large scale.In this paper,we review three-dimensional active nano-transistors and planar active micro-transistors in terms of their applications in electroexcitable cells,focusing on the evaluation of the effects of active micro/nano-bioelectronic devices on electrophysiological signals.Looking forward to the possibilities,challenges,and wide prospects of active micro-nano-devices,we expect to advance their progress to satisfy the demands of theoretical investigations and medical implementations within the domains of cardiology and neuroscience research.

Green and Near-Infrared Dual-Mode Afterglow of Carbon Dots and Their Applications for Confidential Information Readout

Near-infrared(NIR),particularly NIR-containing dual-/multimode afterglow,is very attractive in many fields of application,but it is still a great challenge to achieve such property of materials. Herein,we report a facile method to prepare green and NIR dual-mode afterglow of carbon dots(CDs) through in situ embedding o-CDs(being prepared from o-phenylenediamine) into cyanuric acid(CA) matrix(named o-CDs@CA). Further studies reveal that the green and NIR afterglows of o-CDs@CA originate from thermal activated delayed fluorescence(TADF) and room temperature phosphorescence(RTP) of o-CDs,respectively. In addition,the formation of covalent bonds between o-CDs and CA,and the presence of multiple fixation and rigid e ects to the triplet states of o-CDs are confirmed to be critical for activating the observed dual-mode afterglow. Due to the shorter lifetime and insensitiveness to human vision of the NIR RTP of o-CDs@CA,it is completely covered by the green TADF during directly observing. The NIR RTP signal,however,can be readily captured if an optical filter(cut-o wavelength of 600 nm) being used. By utilizing these unique features,the applications of o-CDs@CA in anti-counterfeiting and information encryption have been demonstrated with great confidentiality. Finally,the as-developed method was confirmed to be applicable to many other kinds of CDs for achieving or enhancing their afterglow performances.

In Situ Synthesis of Fluorescent Mesoporous Silica–Carbon Dot Nanohybrids Featuring Folate Receptor-Overexpressing Cancer Cell Targeting and Drug Delivery

Multifunctional nanocarrier-based theranostics is supposed to overcome some key problems in cancer treatment.In this work,a novel method for the preparation of a fluorescent mesoporous silica–carbon dot nanohybrid was developed.Carbon dots(CDs),from folic acid as the raw material,were prepared in situ and anchored on the surface of amino-modified mesoporous silica nanoparticles(MSNs–NH2) via a microwave-assisted solvothermal reaction.The as-prepared nanohybrid(designated MSNs–CDs) not only exhibited strong and stable yellow emission but also preserved the unique features of MSNs(e.g.,mesoporous structure,large specific surface area,and good biocompatibility),demonstrating a potential capability for fluorescence imagingguided drug delivery.More interestingly,the MSNs–CDs nanohybrid was able to selectively target folate receptor-overexpressing cancer cells(e.g.,HeLa),indicating that folic acid still retained its function even after undergoing the solvothermal reaction.Benefited by these excellent properties,the fluorescent MSNs–CDs nanohybrid can be employed as a fluorescence-guided nanocarrier for the targeted deliveryof anticancer drugs(e.g.,doxorubicin),thereby enhancing chemotherapeutic efficacy and reducing side effects.Our studies may provide a facile strategy for the fabrication of multifunctional MSN-based theranostic platforms,which is beneficial in the diagnosis and therapy of cancers in future.

Tuning the nucleation and decomposition of Li2O_(2) by fluorine-doped carbon vesicles towards high performance Li-O_(2) batteries

Li-O_(2) batteries provide an attractive and potential strategy for energy conversion and storage with high specific energy densities.However,large over-potential in oxygen evolution reactions (OER) caused by the decomposition obstacles of Li_(2)O_(2) seriously impedes its electrochemical performances.Herein,a novel N,O,S and F co-doping vesicular carbon was prepared by self-template pyrolysis method and used in LiO_(2) battery to tune the nucleation and decomposition of Li_(2)O_(2).The introduction of F in the carbon matrix with suitable content can regulate the adsorption of intermediates,through which the morphology of Li_(2)O_(2) can be controlled to film,favorable to its decomposition in charge process.The cathode based on the optimized F doped carbon vesicle exhibits improved electrochemical performances including a low over-potential,large capacity and a long-term stability.Density functional theory (DFT) results show that F and C in C–F bond hasve a strong interaction to Li and O in Li_(2)O_(2),respectively,which can enhance the transfer of electrons from Li_(2)O_(2) to the carbon matrix to generate hole polaron and thus accelerate the delithiation and decomposition of Li_(2)O_(2).This work provides a new sight into understanding the mechanism of nucleation and decomposition of Li_(2)O_(2) for the development of high-performance Li-O_(2) batteries.

Regulating the nucleation of Li_(2)CO_(3) and C by anchoring Li-containing carbonaceous species towards high performance Li-CO_(2) batteries

Li-CO_(2) batteries provide an attractive and potential strategy for CO_(2) utilization as well as energy conversion and storage with high specific energy densities.However,the poor reversibility caused by the decomposition obstacles of Li_(2)CO_(3) and C products is still a challenge for Li-CO_(2) batteries,which seriously influences its electrochemical performances.Herein,a free-standing MnOOH arrays cathode has been prepared and employed in Li-CO_(2) battery,which realizes a great improvement of electrochemical performances by adjusting the discharge products distribution.Experiments coupled with theoretical calculations verifies that the formation of Li-containing carbonaceous species(LiCO_(2),LiCO and Li_(2) CO_(3))bonded with MnOOH through Li ion regulates the nucleation behavior of Li_(2)CO_(3) and C,making them grown on MnOOH uniformly.The fine Li_(2) CO_(3) grains(with a size about 5 nm)embedded into carbon matrix greatly enlarges the contact interface between them,facilitating the transmission of electrons through the discharge products and finally improves CO_(2) evolution activity.This ingenious design strategy of regulating discharge products distribution to improve electrochemical performances provides a promising way to develop advanced Li-CO_(2) batteries.

Anti-Inflammatory Glycosaminoglycan Oligosaccharides from Colwellia psychrerythraea 34H Capsule:Synthesis and Biological Evaluation

Capsular polysaccharides(CPS)of Colwellia psychrerythraea 34H consist of linear tetrasaccharides repeating units in a glycosaminoglycan-like fashion.Their biological function is likely involved in the cold adaptation of microbial organisms.The low availability of these glycosaminoglycan structures greatly limits the study of their functions and biological activities.Here,an efficient semisynthetic strategy for CPS tetrasaccharide derivatives is achieved by using disaccharide units degraded from hyaluronic acids.This new synthetic process is suitable for largescale preparation,and several rare tetrasaccharide derivatives containing GalA-GalNAc were readily obtained in high yields.Biological evaluation of their anti-inflammatory effects demonstrated that these CPS tetrasaccharides effectively attenuated the lipopolysaccharide-induced sepsis and acute lung injury by decreasing macrophage infiltration and secretion of microphage-related cytokines in mice.All these results suggest that this new type of CPS tetrasaccharide can be developed as an anti-inflammation agent.

以“聚集诱导发光(AIE)”理论为载体开展化学类课程思政建设的研究与实践

聚集诱导发光(AIE)作为一种由中国科学家首先提出并被世界所公认的前沿科学理论,为化学学科思政教育提供了一个极佳的载体。通过对AIE理论和其发现者——唐本忠院士科学研究事迹的学习,可以使学生在了解科学前沿进展的同时,增强民族自豪感、激发学习热情,为学生树立科研报国、永攀高峰的光辉典范。本文介绍了郑州大学化学学院以"聚集诱导发光(AIE)"理论为载体开展化学类课程思政建设的研究实践和相关思考。

地方高校一流化学专业建设的系统设计与实践

郑州大学化学专业具有悠久的办学历史和优良的办学传统,面对新高考模式对化学专业选材的冲击和拔尖学生培养的新挑战,郑州大学化学学院在人才培养模式方面进行了一系列探索和实践,找到了一条适合地方高校一流专业建设与发展的道路。

Carbazole and tetrahydro-carboline derivatives as dopamine D_(3) receptor antagonists with the multiple antipsychotic-like properties

Dopamine D_(3) receptor(D_(3)R)is implicated in multiple psychotic symptoms.Increasing the D_(3)R selectivity over dopamine D_2 receptor(D_2R)would facilitate the antipsychotic treatments.Herein,novel carbazole and tetrahydro-carboline derivatives were reported as D_(3)R selective ligands.Through a structure-based virtual screen,ZLG-25(D_(3)R K_i=685 nmol/L;D_2R K_i>10,000 nmol/L)was identified as a novel D_(3)R selective bitopic ligand with a carbazole scaffold.Scaffolds hopping led to the discovery of novel D_(3)R-selective analogs with tetrahydro-β-carboline or tetrahydro-γ-carboline core.Further functional studies showed that most derivatives acted as h D_(3)R-selective antagonists.Several lead compounds could dose-dependently inhibit the MK-801-induced hyperactivity.Additional investigation revealed that 23j and 36b could decrease the apomorphine-induced climbing without cataleptic reaction.Furthermore,36b demonstrated unusual antidepressant-like activity in the forced swimming tests and the tail suspension tests,and alleviated the MK-801-induced disruption of novel object recognition in mice.Additionally,preliminary studies confirmed the favorable PK/PD profiles,no weight gain and limited serum prolactin levels in mice.These results revealed that 36b provided potential opportunities to new antipsychotic drugs with the multiple antipsychotic-like properties.

Investigating evolutionary perspective of carcinogenesis with single-cell transcriptome analysis

We developed phase-switch microfluidic devices for molecular profiling of a large number of single cells.Whole genome microarrays and RNA-sequencing are commonly used to determine the expression levels of genes in cell lysates(a physical mix of millions of cells)for inferring gene functions.However,cellular heterogeneity becomes an inherent noise in the measurement of gene expression.The unique molecular characteristics of individual cells,as well as the temporal and quantitative information of gene expression in cells,are lost when averaged among all cells in cell lysates.Our single-cell technology overcomes this limitation and enables us to obtain a large number of single-cell transcriptomes from a population of cells.A collection of single-cell molecular profiles allows us to study carcinogenesis from an evolutionary perspective by treating cancer as a diverse population of cells with abnormal molecular characteristics.Because a cancer cell population contains cells at various stages of development toward drug resistance,clustering similar single-cell molecular profiles could reveal how drug-resistant subclones evolve during cancer treatment.Here,we discuss how single-cell transcriptome analysis technology could enable the study of carcinogenesis from an evolutionary perspective and the development of drugresistance in leukemia.The single-cell transcriptome analysis reported here could have a direct and significant impact on current cancer treatments and future personalized cancer therapies.

Generation of color-controllable room-temperature phosphorescence via luminescent center engineering and in-situ immobilization

Materials with controllable luminescence colors are highly desirable for numerous promising applications, however, the preparation of such materials, particularly with color-controllable room-temperature phosphorescence(RTP), remains a formidable challenge. In this work, we reported on a facile strategy to prepare color-controllable RTP materials via the pyrolysis of a mixture containing 1-(2-hydroxyethyl)-urea(H-urea) and boric acid(BA). By controlling the pyrolysis temperatures, the as-prepared materials exhibited ultralong RTP with emission colors ranging from cyan, green, to yellow. Further studies revealed that multiple luminescent centers formed from H-urea, which were in-situ embedded in the B2O3matrix(produced from BA) during the pyrolysis process. The contents of the different luminescent centers could be regulated by the pyrolysis temperatures, resulting in color-tunable RTP. Significantly, the luminescent center engineering and in-situ immobilization strategy not only provided a facile method for conveniently preparing color-controllable RTP materials, but also endowed the materials prepared at relatively lower temperatures with color-changeable RTP features under thermal stimulus. Considering their unique properties, the potential applications of the as-obtained materials for advanced anti-counterfeiting and information encryption were preliminarily demonstrated.

Researches of New Anti-metastasis Drugs-GLB Compounds Structured on AO.P1 Water Channel

果糖并螺杂环化合物（GLB和GLM），经体外和整体动物实验证实有显著的抑制肿瘤生长和抑制血管生成活性，其中GLB的作用更强些，我们拟在本课题中继续研究以GLB为代表的果糖并螺杂环类化合物，研究该类化合物影响肿瘤转移及血管生成的药效学，并研究其初步的药物代谢动力学特性和初步的毒性等。

Built-in electric field induced S-scheme g-C_(3)N_(4)homojunction for efficient photocatalytic hydrogen evolution:Interfacial engineering and morphology control

S-scheme possesses superior redox capabilities compared with the II-scheme,providing an effective method to solve the innate defects of g-C_(3)N_(4)(CN).In this study,S-doped g-C_(3)N_(4)/g-C_(3)N_(4)(SCN-tm/CN)S-scheme homojunction was constructed by rationally integrating morphology control with interfacial engineering to enhance the photocatalytic hydrogen evolution performance.In-situ Kelvin probe force microscopy(KPFM)confirms the transport of photo-generated electrons from CN to SCN.Density functional theory(DFT)calculations reveal that the generation of a built-in electric field between SCN and CN enables the carrier separation to be more efficient and effective.Femtosecond transient absorption spectrum(fs-TAS)indicates prolonged lifetimes of SCN-tm/CN_(3)(τ1:9.7,τ2:110,andτ3:1343.5 ps)in comparison to those of CN(τ1:4.86,τ2:55.2,andτ3:927 ps),signifying that the construction of homojunction promotes the separation and transport of electron hole pairs,thus favoring the photocatalytic process.Under visible light irradiation,the optimized SCN-tm/CN_(3)exhibits excellent photocatalytic activity with the hydrogen evolution rate of 5407.3μmol·g^(−1)·h^(−1),which is 20.4 times higher than that of CN(265.7μmol·g^(−1)·h^(−1)).Moreover,the homojunction also displays an apparent quantum efficiency of 26.8%at 435 nm as well as ultra-long and ultra-stable cycle ability.This work offers a new strategy to construct highly efficient photocatalysts based on the metal-free conjugated polymeric CN for realizing solar energy conversion.

N-Glycosylated type Ⅱ collagen peptides as therapeutic saccharide vaccines for rheumatoid arthritis

The interaction among type Ⅱ collagen(CⅡ),human DR4 major histocompatibility complex type Ⅱ molecule(MHC Ⅱ)and T-cell receptor(TCR)is associated with the development of rheumatoid arthritis(RA).The activation of T cells can be reduced through exposure to modified CⅡ(263-272)glycopeptide fragment via competitive inhibition with self-antigen.In this work,30 peptides based on the sequence of CⅡ(263-272)were prepared and evaluated for their binding to DR4 protein by surface plasmon resonance(SPR)assay.The effect on the secretion of pro-inflammatory factors by the spleen cells in collagen induced rheumatoid arthritis(CIA)mouse was also investigated.Two N-glycosylated CⅡ peptides were identified to have strong binding to the human recombinant DR4 protein and weak proinflammatory effect.These glycopeptides could be developed as therapeutic saccharide vaccines for the treatment of rheumatoid arthritis(RA).

Revealing of the ultrafast third-order nonlinear optical response and enabled photonic application in two-dimensional tin sulfide

Black phosphorus(BP), a typical mono-elemental and two-dimensional(2D) material, has gathered significant attention owing to its distinct optoelectronic properties and promising applications, despite its main obstacle of long-term stability. Consequently, BP-analog materials with long-term chemical stability show additional potential. In this contribution, tin sulfide(SnS), a novel two-elemental and 2D structural BP-analog monochalcogenide, has been demonstrated to show enhanced stability under ambient conditions. The broadband nonlinear optical properties and carrier dynamics have been systematically investigated via Z-scan and transient absorption approaches. The excellent nonlinear absorption coefficient of 50.5 × 10^-3 cm∕GW, 1 order of magnitude larger than that of BP, endows the promising application of SnS in ultrafast laser generation. Two different decay times of τ1~873 fs and τ2~96.9 ps allow the alteration between pure Q switching and continuous-wave(CW) mode locking in an identical laser resonator. Both mode-locked and Q-switched operations have been experimentally demonstrated using an SnS saturable absorber at the telecommunication window. Femtosecond laser pulses with tunable wavelength and high stability are easily obtained, suggesting the promising potential of SnS as an efficient optical modulator for ultrafast photonics. This primary investigation may be considered an important step towards stable and high-performance BP-analog material-based photonic devices.

Enabling robust and hour-level organic long persistent luminescence from carbon dots by covalent fixation

The first carbon dot(CD)-based organic long persistent luminescence(OLPL)system exhibiting more than 1 h of duration was developed.In contrast to the established OLPL systems,herein,the reported CDs-based system(named m-CDs@CA)can be facilely and effectively fabricated using a household microwave oven,and more impressively,its LPL can be observed under ambient conditions and even in aqueous media.XRD and TEM characterizations,afterglow decay,time-resolved spectroscopy,and ESR analysis were performed,showing the successful composition of CDs and.CA,the formation of exciplexes and long-lived charged-separated states.Further studies suggest that the production of covalent bonds between CA and CDs plays pivotal roles in activating LPL and preventing its quenching from oxygen and water.To the best of our knowledge,this is a very rare example of an OLPL system that exhibits hourlevel afterglow under ambient conditions.Finally,applications of m-CDs@C.A in glow-in-the-dark paints for emergency signs and multicolored luminous pearls were preliminarily demonstrated.This work may provide new insights for the development of rare earth-free and robust OLPL materials.

Long-wavelength(red to near-infrared) emissive carbon dots: Key factors for synthesis, fluorescence mechanism, and applications in biosensing and cancer theranostics

Carbon dots(CDs), as a new member of carbon nanostructures, have been widely applied in extensive fields due to their exceptional physicochemical properties. While, the emissions of most reported CDs are located in the blue to green range under the excitation of ultraviolet or blue light, which severely limits their practical applications, especially in photovoltaic and biological fields. Studies that focused on synthesizing CDs with long-wavelength(red to near-infrared) emission/excitation features(simply named L-w CDs) and exploring their potential applications have been frequently reported in recent years. In this review, we analyzed the key influence factors for the synthesis of CDs with long wavelength and multicolor(containing long wavelength) emissive properties, discussed possible fluorescence mechanism,and summarized their applications in sensing and cancer theranostics. Finally, the existing challenges and potential opportunities of L-w CDs are presented.

Determination of inulin-type fructo-oligosaccharides in inulin by HPLC-ELSD

To develop an HPLC-ELSD method for the determination of nine inulin-type fructo-oligosaccharides in inulin,the HPLC-ELSD system consisted of Waters XBridge■ Amide column(4.6 mm×250 mm,5μm)with a gradient elution mobile phase consisting of acetonitrile and water at a flow rate of 1.2 mL/min at 30°C.The detector was an Agilent Technologies 380-ELSD.The drift tube temperature for the ELSD was set at 55°C with a nitrogen flow rate of 1.8 L/min.The injection volume was 15μL.The results showed that the detection range for the nine inulin-type fructo-oligosaccharides was 3.81–30.60μg R^(2)=0.99969 for kestose,3.73–29.97μg R^(2)=0.99981 for nystose,3.82–30.69μg R^(2)=0.99993 for fructosylnystose,3.80–30.48μg R^(2)=0.99995 for GF5,3.73–29.96μg R^(2)=0.99993 for GF6,3.78–30.30μg R^(2)=0.99983 for GF7,3.82–30μg R^(2)=0.99989 for GF8,3.71–29.80μg R^(2)=0.99974 for GF9,3.61–29.00μg R^(2)=0.99970 for GF10,respectively.The recovery of the nine oligosaccharides ranged between 96.48%–100.84%(n=6).The method was simple,accurate,and reproducible that it could be used as an analytical method for evaluating the quality of inulin effectively.

Tumor-specific and photothermal-augmented chemodynamic therapy by ferrocene-carbon dot-crosslinked nanoparticles

Extensive research have been devoted to the exploration of multifunctional theranostic agents for cancer,but the poor tumor specificity and unsatisfactory treatment efficacy are some of the critical obstacles for their clinical translations.Herein,ferrocene-carbon dot-crosslinked nanoparticles(Fc-CD NPs)were designed and fabricated for achieving highly specific and photothermal-augmented chemodynamic therapy(CDT).The Fc-CD NPs were found not only to inherit the immanent fluorescence,photoacoustic,and photothermal properties of carbon dots(CDs),but also be endowed with CDT that could occur selectively in tumor microenvironment(TME)due to the presence of Fc for triggering Fenton reaction.Moreover,the enlarged particle size of Fc-CD NPs facilitated their effective accumulation at tumor sites,thus realizing great improvement for antitumor treatment outcomes.Once docking at tumor and being exposed to 660 nm laser irradiation,significantly amplified CDT effect of Fc-CD NPs was observed due to heataccelerating generation of reactive oxygen species(ROS).More interestingly,since the produced ROS could in turn alleviate the thermal-resistance of photothermal therapy(PTT),the therapeutic efficiency of integrated PTT and CDT was synergized to the maximum extent.This study on the one hand provides a facile approach to fabricate CDs-based multifunctional theranostic nanoplatform with enhanced tumor accumulation and specificity,on the other hand emphasizes the merits of synergizing mutually beneficial therapeutic modalities for more efficient cancer therapy.