Electrochemical CO_(2) reduction reaction(CO_(2)RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demons...Electrochemical CO_(2) reduction reaction(CO_(2)RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demonstrated substantial potential for the advancement of electrocatalytic CO_(2) reduction to formate.However,due to the weak bonding of protons(H^(*)) of Bi,the available protonate of CO_(2) on Bi is insufficient,which limits the formation of OCHO^(*).Prediction by theoretical calculation,chlorine doping can effectively promote the dissociation of H_(2)O and thus achieve effective proton supply.We prepare chlorine-doped Bi(Cl-Bi) via an electrochemical conversion strategy for electroreduction of CO_(2) .An obvious improvement of faradaic efficiency(FE) of formate(96.7% at-0.95 V vs.RHE) can be achieved on Cl-Bi,higher than that of Bi(89.4%).Meanwhile,Cl-Bi has the highest formate production rate of 275 μmol h^(-1)cm^(-2)at-0.95 V vs.RHE,which is 1.2 times higher than that of Bi(224 μmol h^(-1)cm^(-2)).In situ characterizations and kinetic analysis reveal that chlorine doping promotes the activation of H_(2)O and supply sufficient protons to promote the protonation of CO_(2) to OCHO^(*),which is consistent with theoretical calculation.The study presents an effective strategy for rational design of highly efficient electrocatalysts to promote green chemical production.展开更多
This paper prepared a novel as-cast W-Zr-Ti metallic ESM using high-frequency vacuum induction melting technique.The above ESM performs a typical elastic-brittle material feature and strain rate strengthening behavior...This paper prepared a novel as-cast W-Zr-Ti metallic ESM using high-frequency vacuum induction melting technique.The above ESM performs a typical elastic-brittle material feature and strain rate strengthening behavior.The specimens exhibit violent chemical reaction during the fracture process under the impact loading,and the size distribution of their residual debris follows Rosin-Rammler model.The dynamic fracture toughness is obtained by the fitting of debris length scale,approximately 1.87 MPa·m~(1/2).Microstructure observation on residual debris indicates that the failure process is determined by primary crack propagation under quasi-static compression,while it is affected by multiple cracks propagation in both particle and matrix in the case of dynamic impact.Impact test demonstrates that the novel energetic fragment performs brilliant penetration and combustion effect behind the front target,leading to the effective ignition of fuel tank.For the brittleness of as-cast W-ZrTi ESM,further study conducted bond-based peridynamic(BB-PD)C++computational code to simulate its fracture behavior during penetration.The BB-PD method successfully captured the fracture process and debris cloud formation of the energetic fragment.This paper explores a novel as-cast metallic ESM,and provides an available numerical avenue to the simulation of brittle energetic fragment.展开更多
Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and l...Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and long-range electric vehicles.However,technical barriers such as dendrite growth and poor Li plating/stripping reversibility severely hinder the practical application of LMBs.However,lithium nitrate(LiNO_(3))is found to be able to stabilize the Li/electrolyte interface and has been used to address the above challenges.To date,considerable research efforts have been devoted toward understanding the roles of LiNO_(3) in regulating the surface properties of Li anodes and toward the development of many effective strategies.These research efforts are partially mentioned in some articles on LMBs and yet have not been reviewed systematically.To fill this gap,we discuss the recent advances in fundamental and technological research on LiNO_(3) and its derivatives for improving the performances of LMBs,particularly for Li-sulfur(S),Li-oxygen(O),and Li-Li-containing transition-metal oxide(LTMO)batteries,as well as LiNO_(3)-containing recipes for precursors in battery materials and interphase fabrication.This review pays attention to the effects of LiNO_(3) in lithium-based batteries,aiming to provide scientific guidance for the optimization of electrode/electrolyte interfaces and enrich the design of advanced LMBs.展开更多
The flexoelectric effect refers to the electromechanical coupling between electric polarization and mechanical strain gradient.It universally exists in a variety of materials in any space group,such as liquid crystals...The flexoelectric effect refers to the electromechanical coupling between electric polarization and mechanical strain gradient.It universally exists in a variety of materials in any space group,such as liquid crystals,dielectrics,biological materials,and semiconductors.Because of its unique size effect,nanoscale flexoelectricity has shown novel phenomena and promising applications in electronics,optronics,mechatronics,and photovoltaics.In this review,we provide a succinct report on the discovery and development of the flexoelectric effect,focusing on flexoelectric materials and related applications.Finally,we discuss recent flexoelectric research progress and still‐unsolved problems.展开更多
With the rapid development of artificial intelligence,magnetocaloric materials as well as other materials are being developed with increased efficiency and enhanced performance.However,most studies do not take phase t...With the rapid development of artificial intelligence,magnetocaloric materials as well as other materials are being developed with increased efficiency and enhanced performance.However,most studies do not take phase transitions into account,and as a result,the predictions are usually not accurate enough.In this context,we have established an explicable relationship between alloy compositions and phase transition by feature imputation.A facile machine learning is proposed to screen candidate NiMn-based Heusler alloys with desired magnetic entropy change and magnetic transition temperature with a high accuracy R^(2)≈0.98.As expected,the measured properties of prepared NiMn-based alloys,including phase transition type,magnetic entropy changes and transition temperature,are all in good agreement with the ML predictions.As well as being the first to demonstrate an explicable relationship between alloy compositions,phase transitions and magnetocaloric properties,our proposed ML model is highly predictive and interpretable,which can provide a strong theoretical foundation for identifying high-performance magnetocaloric materials in the future.展开更多
In the practice of healthcare,patient-reported outcomes(PROs)and PRO measures(PROMs)are used as an attempt to observe the changes in complex clinical situations.They guide us in making decisions based on the evidence ...In the practice of healthcare,patient-reported outcomes(PROs)and PRO measures(PROMs)are used as an attempt to observe the changes in complex clinical situations.They guide us in making decisions based on the evidence regarding patient care by recording the change in outcomes for a particular treatment to a given condition and finally to understand whether a patient will benefit from a particular treatment and to quantify the treatment effect.For any PROM to be usable in health care,we need it to be reliable,encapsulating the points of interest with the potential to detect any real change.Using structured outcome measures routinely in clinical practice helps the physician to understand the functional limitation of a patient that would otherwise not be clear in an office interview,and this allows the physician and patient to have a meaningful conver-sation as well as a customized plan for each patient.Having mentioned the rationale and the benefits of PROMs,understanding the quantification process is crucial before embarking on management decisions.A better interpretation of change needs to identify the treatment effect based on clinical relevance for a given condition.There are a multiple set of measurement indices to serve this effect and most of them are used interchangeably without clear demarcation on their differences.This article details the various quantification metrics used to evaluate the treatment effect using PROMs,their limitations and the scope of usage and implementation in clinical practice.展开更多
In existing studies, most slope stability analyses concentrate on conditions with constant temperature, assuming the slope is intact, and employ the Mohr-Coulomb (M-C) failure criterion for saturated soil to character...In existing studies, most slope stability analyses concentrate on conditions with constant temperature, assuming the slope is intact, and employ the Mohr-Coulomb (M-C) failure criterion for saturated soil to characterize the strength of the backfill. However, the actual working temperature of slopes varies, and natural phenomena such as rainfall and groundwater infiltration commonly result in unsaturated soil conditions, with cracks typically present in cohesive slopes. This study introduces a novel approach for assessing the stability of unsaturated soil stepped slopes under varying temperatures, incorporating the effects of open and vertical cracks. Utilizing the kinematic approach and gravity increase method, we developed a three-dimensional (3D) rotational wedge failure mechanism to simulate slope collapse, enhancing the traditional two-dimensional analyses. We integrated temperature-dependent functions and nonlinear shear strength equations to evaluate the impact of temperature on four typical unsaturated soil types. A particle swarm optimization algorithm was employed to calculate the safety factor, ensuring our method’s accuracy by comparing it with existing studies. The results indicate that considering 3D effects yields a higher safety factor, while cracks reduce slope stability. Each unsaturated soil exhibits a distinctive temperature response curve, highlighting the importance of understanding soil types in the design phase.展开更多
As the main geomaterials for coral reefs oil or gas extraction and underground infrastructure construction,coral reef limestone demonstrates significantly distinct mechanical responses compared to terrigenous rocks.To...As the main geomaterials for coral reefs oil or gas extraction and underground infrastructure construction,coral reef limestone demonstrates significantly distinct mechanical responses compared to terrigenous rocks.To investigate the mechanical behaviour of coral reef limestone under the coupling impact of size and strain rate,the uniaxial compression tests were conducted on reef limestone samples with length-to-diameter(L/D)ratio ranging from 0.5 to 2.0 at strain rate ranging from 10^(−5)·s^(−1)to 10^(−2)·s^(−1).It is revealed that the uniaxial compressive strength(UCS)and residual compressive strength(RCS)of coral reef limestone exhibits a decreasing trend with L/D ratio increasing.The dynamic increase factor(DIF)of UCS is linearly correlated with the logarithm of strain rate,while increasing the L/D ratio further enhances the DIF.The elastic modulus increases with strain rate or L/D ratio increasing,whereas the Poisson’s ratio approximates to a constant value of 0.24.The failure strain increases with strain rate increasing or L/D ratio decreasing,while the increase in L/D ratio will inhibit the enhancing effect of the strain rate.The high porosity and low mineral strength are the primary factors contributing to a high RCS of 16.7%–64.9%of UCS,a lower brittleness index and multiple irregular fracture planes.The failure pattern of coral reef limestone transits from the shear-dominated to the splitting-dominated failure with strain rate increasing or L/D ratio decreasing,which is mainly governed by the constrained zones induced by end friction and the strain rate-dependent crack propagation.Moreover,a predictive formula incorporating coupling effect of size and strain rate for the UCS of reef limestone was established and verified to effectively capture the trend of UCS.展开更多
Excellent progress has been made in the last few decades in the cure rates of pediatric malignancies,with more than 80%of children with cancer who have access to contemporary treatment being cured.However,the therapie...Excellent progress has been made in the last few decades in the cure rates of pediatric malignancies,with more than 80%of children with cancer who have access to contemporary treatment being cured.However,the therapies responsible for this survival can also produce adverse physical and psychological long-term outcomes,referred to as late effects,which appear months to years after the completion of cancer treatment.Research has shown that 60%to 90%of childhood cancer survivors(CCSs)develop one or more chronic health conditions,and 20%to 80%of survivors experience severe or life-threatening complications during adulthood.Therefore,understanding the late side effects of such treatments is important to improve the health and quality of life of the growing population of CCSs.展开更多
Cancer multidrug resistance(MDR)impairs the therapeutic efficacy of various chemotherapeutics.Novel approaches,particularly the development of MDR reversal agents,are critically needed to address this challenge.This s...Cancer multidrug resistance(MDR)impairs the therapeutic efficacy of various chemotherapeutics.Novel approaches,particularly the development of MDR reversal agents,are critically needed to address this challenge.This study demonstrates that tenacissoside I(TI),a compound isolated from Marsdenia tenacissima(Roxb.)Wight et Arn,traditionally used in clinical practice as an ethnic medicine for cancer treatment,exhibits significant MDR reversal effects in ABCB1-mediated MDR cancer cells.TI reversed the resistance of SW620/AD300 and KBV200 cells to doxorubicin(DOX)and paclitaxel(PAC)by downregulating ABCB1 expression and reducing ABCB1 drug transport function.Mechanistically,protein arginine methyltransferase 1(PRMT1),whose expression correlates with poor prognosis and shows positive association with both ABCB1 and EGFR expressions in tumor tissues,was differentially expressed in TI-treated SW620/AD300 cells.SW620/AD300 and KBV200 cells exhibited elevated levels of EGFR asymmetric dimethylarginine(aDMA)and enhanced PRMT1-EGFR interaction compared to their parental cells.Moreover,TI-induced PRMT1 downregulation impaired PRMT1-mediated aDMA of EGFR,PRMT1-EGFR interaction,and EGFR downstream signaling in SW620/AD300 and KBV200 cells.These effects were significantly reversed by PRMT1 overexpression.Additionally,TI demonstrated resistance reversal to PAC in xenograft models without detectable toxicities.This study establishes TI's MDR reversal effect in ABCB1-mediated MDR human cancer cells through inhibition of PRMT1-mediated aDMA of EGFR,suggesting TI's potential as an MDR modulator for improving chemotherapy outcomes.展开更多
During the hyperacute phase of intracerebral hemorrhage(ICH),the mass effect and blood components mechanically lead to brain damage and neurotoxicity.Our findings revealed that the mass effect and transferrin precipit...During the hyperacute phase of intracerebral hemorrhage(ICH),the mass effect and blood components mechanically lead to brain damage and neurotoxicity.Our findings revealed that the mass effect and transferrin precipitate neuronal oxidative stress and iron uptake,culminating in ferroptosis in neurons.M6A(N6-methyladenosine)modification,the most prevalent mRNA modification,plays a critical role in various cell death pathways.The Fto(fat mass and obesity-associated protein)demethylase has been implicated in numerous signaling pathways of neurological diseases by modulating m6A mRNA levels.Regulation of Fto protein levels in neurons effectively mitigated mass effect-induced neuronal ferroptosis.Applying nanopore direct RNA sequencing,we identified voltage-dependent anion channel 3(Vdac3)as a potential target associated with ferroptosis.Fto influenced neuronal ferroptosis by regulating the m6A methylation of Vdac3 mRNA.These findings elucidate the intricate interplay between Fto,Vdac3,m6A methylation,and ferroptosis in neurons during the hyperacute phase post-ICH and suggest novel therapeutic strategies for ICH.展开更多
Natural cemented calcareous sand and limestone are highly complex and not well understood in terms of the me-chanical behavior due to the difficulty of obtaining undisturbed samples from far sea.This paper proposes an...Natural cemented calcareous sand and limestone are highly complex and not well understood in terms of the me-chanical behavior due to the difficulty of obtaining undisturbed samples from far sea.This paper proposes an artificial method in a laboratory setting using microbial-induced carbonate precipitation(MICP)to simulate the natural process of cementation of limestone.The artificially cemented sand has a high degree of similarity with the natural weakly limestone in three aspects:(1)the mineral composition of the cemented material is also granular calcite and acicular aragonite;(2)the microstructure in interconnected open pore network can be gradually closed and contracted with cementation.The porosity reaches to approximately 9.2%;(3)both the stress-strain relationship and the unconfined strength closely resemble that of natural weakly limestone.Furthermore,both static and dynamic behaviors of artificial limestone were studied by quasi-static compression tests and Split Hopkinson Pressure Bar(SHPB)tests,finding that the unconfined strength of weakly artifical limestone exponentially increases with increasing strain rate.A rate-dependent bond strength was proposed and implemented in software to reveal the mechanism of strain rate effects.It is found that the loading velocity is too high to keep in sync with the initiation and propagation of cracks under impact loading.This delay-induced viscosity may restrict the movement of the surrounding balls,thus increasing resistance.展开更多
Evaluation of hydromechanical shear behavior of unsaturated soils is still a challenging issue. The time and cost needed for conducting precise experimental investigation on shear behavior of unsaturated soils have en...Evaluation of hydromechanical shear behavior of unsaturated soils is still a challenging issue. The time and cost needed for conducting precise experimental investigation on shear behavior of unsaturated soils have encouraged several investigators to develop analytical, empirical, or semi-empirical models for predicting the shear behavior of unsaturated soils. However, most of the previously proposed models are for specimens subjected to the isotropic state of stress, without considering the effect of initial shear stress. In this study, a hydromechanical constitutive model is proposed for unsaturated collapsible soils during shearing, with consideration of the effect of the initial shear stress. The model implements an effective stress-based disturbed state concept (DSC) to predict the stress-strain behavior of the soil. Accordingly, material/state variables were defined for both the start of the shearing stage and the critical state of the soil. A series of laboratory tests was performed using a fully automated unsaturated triaxial device to verify the proposed model. The experimental program included 23 suction-controlled unsaturated triaxial shear tests on reconstituted specimens of Gorgan clayey loess wetted to different levels of suctions under both isotropic and anisotropic stress states. The results show excellent agreement between the prediction by the proposed model and the experimental results.展开更多
The highly selective catalytic hydrogenation of halogenated nitroaromatics was achieved by employing Pd‑based catalysts that were co‑modified with organic and inorganic ligands.It was demonstrated that the catalysts c...The highly selective catalytic hydrogenation of halogenated nitroaromatics was achieved by employing Pd‑based catalysts that were co‑modified with organic and inorganic ligands.It was demonstrated that the catalysts contained Pd species in mixed valence states,with high valence Pd at the metal‑support interface and zero valence Pd at the metal surface.While the strong coordination of triphenylphosphine(PPh3)to Pd0 on the Pd surface prevents the adsorption of halogenated nitroaromatics and thus dehalogenation,the coordination of sodium metavanadate(NaVO3)to high‑valence Pd sites at the interface helps to activate H2 in a heterolytic pathway for the selective hydrogenation of nitro‑groups.The excellent catalytic performance of the interfacial active sites enables the selective hydrogenation of a wide range of halogenated nitroaromatics.展开更多
Thermally activated delayed fluorescence(TADF)molecules have outstanding potential for applications in organic light-emitting diodes(OLEDs).Due to the lack of systematic studies on the correlation between molecular st...Thermally activated delayed fluorescence(TADF)molecules have outstanding potential for applications in organic light-emitting diodes(OLEDs).Due to the lack of systematic studies on the correlation between molecular structure and luminescence properties,TADF molecules are far from meeting the needs of practical applications in terms of variety and number.In this paper,three twisted TADF molecules are studied and their photophysical properties are theoretically predicted based on the thermal vibrational correlation function method combined with multiscale calculations.The results show that all the molecules exhibit fast reverse intersystem crossing(RISC)rates(kRISC),predicting their TADF luminescence properties.In addition,the binding of DHPAzSi as the donor unit with different acceptors can change the dihedral angle between the ground and excited states,and the planarity of the acceptors is positively correlated with the reorganization energy,a property that has a strong influence on the non-radiative process.Furthermore,a decrease in the energy of the molecular charge transfer state and an increase in the kRISC were observed in the films.This study not only provides a reliable explanation for the observed experimental results,but also offers valuable insights that can guide the design of future TADF molecules.展开更多
Loess is susceptible to loading effects such as significant changes in strength and volume variation caused by loading and wetting.In this study,considering the different connection states of pore water and gas in loe...Loess is susceptible to loading effects such as significant changes in strength and volume variation caused by loading and wetting.In this study,considering the different connection states of pore water and gas in loess fabric,the gas phase closure case is incorporated into a unified form of the generalized effective stress framework,introducing a damage parameter considering the effects of closed pore gas.The loading effects of unsaturated loess under wide variations in saturation are described in a unified way,and the model performance is verified by corresponding stress and hydraulic path tests.The results indicated that the collapse response involves the initial void ratio of loess,and the coupled outwards motion of the loading-collapse(LC)yield surface under loading enhances its structural strength.Suction-enhanced yield stress requires a greater"tensile stress"to counteract its structural stability.The nucleation of bubbles at high saturation causes a decrease in yield stress.The loading effect exhibits a smaller collapse behavior when the influence of closed gas is considered,whereas the suction path does not cross the LC in the stress space under hydraulic action for the same parameters,which amplifies the influence of closed gas on loess deformation.展开更多
Vanadium-based transition metal chalcogenides VmXn(X=S,Se,Te)with their distinctive quantum effects,tunable magnetism,spin-orbit coupling,and high carrier mobility are a valuable platform to explore the interplay betw...Vanadium-based transition metal chalcogenides VmXn(X=S,Se,Te)with their distinctive quantum effects,tunable magnetism,spin-orbit coupling,and high carrier mobility are a valuable platform to explore the interplay between magnetism and electronic correlations,especially with tunable structural phases and magnetic properties through stoichiometric variations,making them ideal candidates for advanced device applications.Here,we report the synthesis of high-quality V_(5+x)S_(8)single crystals with different concentrations of self-intercalated vanadium.V_(5+x)S_(8)crystals show an antiferromagnetic behavior and a spin-flop-like transition below TN of 30.6 K.The high-quality V_(5+x)S_(8)single crystals exhibit a large negative magnetoresistance of 12.3%at 2 K.Interestingly,V_(5+x)S_(8)crystals show an obvious low-temperature resistance upturn that gradually levels off with the increasing magnetic field,attributed to the Kondo effect arising from the interaction between conduction electrons and embedded vanadium magnetic impurities.With increasing V doping,the antiferromagnetic interactions intensify,weakening the coupling between the local moments and conduction electrons,which in turn lowers the Kondo temperature(TK).Furthermore,the anomalous Hall effect is observed in V5.73S8,with an anomalous Hall conductivity(AHC)of 50.46 W^(-1)·cm^(-1)and anomalous Hall angle of 0.73%at 2 K.Our findings offer valuable insights into the mechanisms of the Kondo effect and anomalous Hall effect in self-intercalated transition metal chalcogenides with complex magnetism and electronic correlation effects.展开更多
Urban green spaces and parks offer opportunities for retaining and increasing bird richness, diversity, and species abundance. However, urbanisation influences predator–prey interactions, leading to high predation ra...Urban green spaces and parks offer opportunities for retaining and increasing bird richness, diversity, and species abundance. However, urbanisation influences predator–prey interactions, leading to high predation rates in urban areas, in the UK notably through the presence of large populations of domestic cats and increased populations of synanthropic species, such as rats and squirrels. These high predation rates are assumed to be a significant cause of reproductive failure in birds. Some ecologists advocate for the use of buffer zones with reduced human influence to reduce potential hunting pressure in eco-sensitive areas. However, the buffer effect on predation rates of nesting birds in suburban areas is rarely investigated. In this study, we investigated how edge effects (how close nest sites are to housing) and nest height (i.e., ground vs. above-ground) affected nest predation rates in a suburban park using camera traps to monitor artificial nests containing quail eggs. Our hypothesis was that nests in the buffer area (<300 m inward from university boundary) and at low height would suffer higher predation rates than nests in the core area (>300 m from the university boundary) and at height, as the buffer zone effect, and ease of access to ground predators would result in higher predation rates. We found no significant effect of nest height in nest predation rates. However, contrary to our expectations, nests in the core zone suffered higher predation rates than those in the buffer zone, and corvids were responsible for almost half of the egg loss events. We speculate that this may be a consequence of higher levels of anthropogenic disturbance (e.g., pedestrians, dog walking, vehicles) adjacent to our buffer zone acting as a deterrent to avian nest predators. This work suggests that protecting urban sites from disturbance may not always act to support bird abundance.展开更多
The pressure and temperature increase resulting from the impact of different threats onto target materials is analyzed with a unified laboratory-scale setup.This allows deriving qualitative information on the occurrin...The pressure and temperature increase resulting from the impact of different threats onto target materials is analyzed with a unified laboratory-scale setup.This allows deriving qualitative information on the occurring phenomenology as well as quantitative statements about the relative effects sizes as a function of target material and threat.The considered target materials are steel,aluminum,and magnesium.As threats,kinetic energy penetrator,explosively formed projectile,and shaped charge jet are used.For the investigated combinations,the measured overpressures vary by a factor of up to 5 for a variation of the material,by a factor of up to 7 for a variation of the threat,and by a factor larger than 15for a simultaneous variation of both.The obtained results as well as the experimental approach are relevant for the basic understanding of impact effects and risks due to material reactivity.The paper combines two main aims.Firstly,to provide a summary of own prior work in a coherent journal article and,secondly,to review and discuss these earlier results with a new perspective.展开更多
基金financially supported by the Natural Science Foundation of Shandong Province (No.ZR2022QE076)the National Natural Science Foundation of China (No.52202092)the Science and Technology Support Plan for Youth Innovation of Colleges and Universities of Shandong Province of China (No.2023KJ104)。
文摘Electrochemical CO_(2) reduction reaction(CO_(2)RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demonstrated substantial potential for the advancement of electrocatalytic CO_(2) reduction to formate.However,due to the weak bonding of protons(H^(*)) of Bi,the available protonate of CO_(2) on Bi is insufficient,which limits the formation of OCHO^(*).Prediction by theoretical calculation,chlorine doping can effectively promote the dissociation of H_(2)O and thus achieve effective proton supply.We prepare chlorine-doped Bi(Cl-Bi) via an electrochemical conversion strategy for electroreduction of CO_(2) .An obvious improvement of faradaic efficiency(FE) of formate(96.7% at-0.95 V vs.RHE) can be achieved on Cl-Bi,higher than that of Bi(89.4%).Meanwhile,Cl-Bi has the highest formate production rate of 275 μmol h^(-1)cm^(-2)at-0.95 V vs.RHE,which is 1.2 times higher than that of Bi(224 μmol h^(-1)cm^(-2)).In situ characterizations and kinetic analysis reveal that chlorine doping promotes the activation of H_(2)O and supply sufficient protons to promote the protonation of CO_(2) to OCHO^(*),which is consistent with theoretical calculation.The study presents an effective strategy for rational design of highly efficient electrocatalysts to promote green chemical production.
文摘This paper prepared a novel as-cast W-Zr-Ti metallic ESM using high-frequency vacuum induction melting technique.The above ESM performs a typical elastic-brittle material feature and strain rate strengthening behavior.The specimens exhibit violent chemical reaction during the fracture process under the impact loading,and the size distribution of their residual debris follows Rosin-Rammler model.The dynamic fracture toughness is obtained by the fitting of debris length scale,approximately 1.87 MPa·m~(1/2).Microstructure observation on residual debris indicates that the failure process is determined by primary crack propagation under quasi-static compression,while it is affected by multiple cracks propagation in both particle and matrix in the case of dynamic impact.Impact test demonstrates that the novel energetic fragment performs brilliant penetration and combustion effect behind the front target,leading to the effective ignition of fuel tank.For the brittleness of as-cast W-ZrTi ESM,further study conducted bond-based peridynamic(BB-PD)C++computational code to simulate its fracture behavior during penetration.The BB-PD method successfully captured the fracture process and debris cloud formation of the energetic fragment.This paper explores a novel as-cast metallic ESM,and provides an available numerical avenue to the simulation of brittle energetic fragment.
基金supported by the Yunnan Fundamental Research Projects(Grant Nos.202401AU070163 and 202501AT070298)the Yunnan Engineering Research Center Innovation Ability Construction and Enhancement Projects(Grant No.2023-XMDJ-00617107)+5 种基金the University Service Key Industry Project of Yunnan Province(Grant No.FWCY-ZD2024005)the Expert Workstation Support Project of Yunnan Province(Grant No.202405AF140069)the Scientific Research Foundation of Kunming University of Science and Technology(Grant No.20220122)the Analysis and Test Foundation of Kunming University of Science and Technology(Grant No.2023T20220122)the Natural Science Foundation of Inner Mongolia Autonomous Region of China(Grant No.2025QN02057)the Ordos City Strategic Pioneering Science and Technology Special Program for New Energy(Grant No.DC2400003365).
文摘Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and long-range electric vehicles.However,technical barriers such as dendrite growth and poor Li plating/stripping reversibility severely hinder the practical application of LMBs.However,lithium nitrate(LiNO_(3))is found to be able to stabilize the Li/electrolyte interface and has been used to address the above challenges.To date,considerable research efforts have been devoted toward understanding the roles of LiNO_(3) in regulating the surface properties of Li anodes and toward the development of many effective strategies.These research efforts are partially mentioned in some articles on LMBs and yet have not been reviewed systematically.To fill this gap,we discuss the recent advances in fundamental and technological research on LiNO_(3) and its derivatives for improving the performances of LMBs,particularly for Li-sulfur(S),Li-oxygen(O),and Li-Li-containing transition-metal oxide(LTMO)batteries,as well as LiNO_(3)-containing recipes for precursors in battery materials and interphase fabrication.This review pays attention to the effects of LiNO_(3) in lithium-based batteries,aiming to provide scientific guidance for the optimization of electrode/electrolyte interfaces and enrich the design of advanced LMBs.
基金support of the National Natural Science Foundation of China(Grant Nos.52192611,51872031,61904013,and 62405157)China Postdoctoral Science Foundation(Nos.2023M741890 and GZC20231215)the Fundamental Research Funds for the Central Universities.
文摘The flexoelectric effect refers to the electromechanical coupling between electric polarization and mechanical strain gradient.It universally exists in a variety of materials in any space group,such as liquid crystals,dielectrics,biological materials,and semiconductors.Because of its unique size effect,nanoscale flexoelectricity has shown novel phenomena and promising applications in electronics,optronics,mechatronics,and photovoltaics.In this review,we provide a succinct report on the discovery and development of the flexoelectric effect,focusing on flexoelectric materials and related applications.Finally,we discuss recent flexoelectric research progress and still‐unsolved problems.
基金supported by the National Key R&D Program of China(No.2022YFE0109500)the National Natural Science Foundation of China(Nos.52071255,52301250,52171190 and 12304027)+2 种基金the Key R&D Project of Shaanxi Province(No.2022GXLH-01-07)the Fundamental Research Funds for the Central Universities(China)the World-Class Universities(Disciplines)and the Characteristic Development Guidance Funds for the Central Universities.
文摘With the rapid development of artificial intelligence,magnetocaloric materials as well as other materials are being developed with increased efficiency and enhanced performance.However,most studies do not take phase transitions into account,and as a result,the predictions are usually not accurate enough.In this context,we have established an explicable relationship between alloy compositions and phase transition by feature imputation.A facile machine learning is proposed to screen candidate NiMn-based Heusler alloys with desired magnetic entropy change and magnetic transition temperature with a high accuracy R^(2)≈0.98.As expected,the measured properties of prepared NiMn-based alloys,including phase transition type,magnetic entropy changes and transition temperature,are all in good agreement with the ML predictions.As well as being the first to demonstrate an explicable relationship between alloy compositions,phase transitions and magnetocaloric properties,our proposed ML model is highly predictive and interpretable,which can provide a strong theoretical foundation for identifying high-performance magnetocaloric materials in the future.
文摘In the practice of healthcare,patient-reported outcomes(PROs)and PRO measures(PROMs)are used as an attempt to observe the changes in complex clinical situations.They guide us in making decisions based on the evidence regarding patient care by recording the change in outcomes for a particular treatment to a given condition and finally to understand whether a patient will benefit from a particular treatment and to quantify the treatment effect.For any PROM to be usable in health care,we need it to be reliable,encapsulating the points of interest with the potential to detect any real change.Using structured outcome measures routinely in clinical practice helps the physician to understand the functional limitation of a patient that would otherwise not be clear in an office interview,and this allows the physician and patient to have a meaningful conver-sation as well as a customized plan for each patient.Having mentioned the rationale and the benefits of PROMs,understanding the quantification process is crucial before embarking on management decisions.A better interpretation of change needs to identify the treatment effect based on clinical relevance for a given condition.There are a multiple set of measurement indices to serve this effect and most of them are used interchangeably without clear demarcation on their differences.This article details the various quantification metrics used to evaluate the treatment effect using PROMs,their limitations and the scope of usage and implementation in clinical practice.
基金Project(51378510) supported by the National Natural Science Foundation of China。
文摘In existing studies, most slope stability analyses concentrate on conditions with constant temperature, assuming the slope is intact, and employ the Mohr-Coulomb (M-C) failure criterion for saturated soil to characterize the strength of the backfill. However, the actual working temperature of slopes varies, and natural phenomena such as rainfall and groundwater infiltration commonly result in unsaturated soil conditions, with cracks typically present in cohesive slopes. This study introduces a novel approach for assessing the stability of unsaturated soil stepped slopes under varying temperatures, incorporating the effects of open and vertical cracks. Utilizing the kinematic approach and gravity increase method, we developed a three-dimensional (3D) rotational wedge failure mechanism to simulate slope collapse, enhancing the traditional two-dimensional analyses. We integrated temperature-dependent functions and nonlinear shear strength equations to evaluate the impact of temperature on four typical unsaturated soil types. A particle swarm optimization algorithm was employed to calculate the safety factor, ensuring our method’s accuracy by comparing it with existing studies. The results indicate that considering 3D effects yields a higher safety factor, while cracks reduce slope stability. Each unsaturated soil exhibits a distinctive temperature response curve, highlighting the importance of understanding soil types in the design phase.
基金supported by the National Natural Science Foundation of China(Nos.52222110,52401354,and 52301353).
文摘As the main geomaterials for coral reefs oil or gas extraction and underground infrastructure construction,coral reef limestone demonstrates significantly distinct mechanical responses compared to terrigenous rocks.To investigate the mechanical behaviour of coral reef limestone under the coupling impact of size and strain rate,the uniaxial compression tests were conducted on reef limestone samples with length-to-diameter(L/D)ratio ranging from 0.5 to 2.0 at strain rate ranging from 10^(−5)·s^(−1)to 10^(−2)·s^(−1).It is revealed that the uniaxial compressive strength(UCS)and residual compressive strength(RCS)of coral reef limestone exhibits a decreasing trend with L/D ratio increasing.The dynamic increase factor(DIF)of UCS is linearly correlated with the logarithm of strain rate,while increasing the L/D ratio further enhances the DIF.The elastic modulus increases with strain rate or L/D ratio increasing,whereas the Poisson’s ratio approximates to a constant value of 0.24.The failure strain increases with strain rate increasing or L/D ratio decreasing,while the increase in L/D ratio will inhibit the enhancing effect of the strain rate.The high porosity and low mineral strength are the primary factors contributing to a high RCS of 16.7%–64.9%of UCS,a lower brittleness index and multiple irregular fracture planes.The failure pattern of coral reef limestone transits from the shear-dominated to the splitting-dominated failure with strain rate increasing or L/D ratio decreasing,which is mainly governed by the constrained zones induced by end friction and the strain rate-dependent crack propagation.Moreover,a predictive formula incorporating coupling effect of size and strain rate for the UCS of reef limestone was established and verified to effectively capture the trend of UCS.
文摘Excellent progress has been made in the last few decades in the cure rates of pediatric malignancies,with more than 80%of children with cancer who have access to contemporary treatment being cured.However,the therapies responsible for this survival can also produce adverse physical and psychological long-term outcomes,referred to as late effects,which appear months to years after the completion of cancer treatment.Research has shown that 60%to 90%of childhood cancer survivors(CCSs)develop one or more chronic health conditions,and 20%to 80%of survivors experience severe or life-threatening complications during adulthood.Therefore,understanding the late side effects of such treatments is important to improve the health and quality of life of the growing population of CCSs.
基金supported by the National Natural Science Foundation of China(Nos.82274211 and 82474190)the Natural Science Foundation of Tianjin(Nos.24JCZDJC00120 and 24PTLYHZ00280)Liaoning Provincial Department of Education Basic Research Projects for Higher Education Institutions(No.LJ212510163021)。
文摘Cancer multidrug resistance(MDR)impairs the therapeutic efficacy of various chemotherapeutics.Novel approaches,particularly the development of MDR reversal agents,are critically needed to address this challenge.This study demonstrates that tenacissoside I(TI),a compound isolated from Marsdenia tenacissima(Roxb.)Wight et Arn,traditionally used in clinical practice as an ethnic medicine for cancer treatment,exhibits significant MDR reversal effects in ABCB1-mediated MDR cancer cells.TI reversed the resistance of SW620/AD300 and KBV200 cells to doxorubicin(DOX)and paclitaxel(PAC)by downregulating ABCB1 expression and reducing ABCB1 drug transport function.Mechanistically,protein arginine methyltransferase 1(PRMT1),whose expression correlates with poor prognosis and shows positive association with both ABCB1 and EGFR expressions in tumor tissues,was differentially expressed in TI-treated SW620/AD300 cells.SW620/AD300 and KBV200 cells exhibited elevated levels of EGFR asymmetric dimethylarginine(aDMA)and enhanced PRMT1-EGFR interaction compared to their parental cells.Moreover,TI-induced PRMT1 downregulation impaired PRMT1-mediated aDMA of EGFR,PRMT1-EGFR interaction,and EGFR downstream signaling in SW620/AD300 and KBV200 cells.These effects were significantly reversed by PRMT1 overexpression.Additionally,TI demonstrated resistance reversal to PAC in xenograft models without detectable toxicities.This study establishes TI's MDR reversal effect in ABCB1-mediated MDR human cancer cells through inhibition of PRMT1-mediated aDMA of EGFR,suggesting TI's potential as an MDR modulator for improving chemotherapy outcomes.
基金supported by the National Key R&D Program of China(2022YFE0131000)the National Natural Science Foundation of China(82220108012,82271306,and 82071307)+1 种基金The Science and Education for Health Foundation of Suzhou for Youth(KJXW2023001)the Boxi Youth Natural Science Foundation(BXQN2023028).
文摘During the hyperacute phase of intracerebral hemorrhage(ICH),the mass effect and blood components mechanically lead to brain damage and neurotoxicity.Our findings revealed that the mass effect and transferrin precipitate neuronal oxidative stress and iron uptake,culminating in ferroptosis in neurons.M6A(N6-methyladenosine)modification,the most prevalent mRNA modification,plays a critical role in various cell death pathways.The Fto(fat mass and obesity-associated protein)demethylase has been implicated in numerous signaling pathways of neurological diseases by modulating m6A mRNA levels.Regulation of Fto protein levels in neurons effectively mitigated mass effect-induced neuronal ferroptosis.Applying nanopore direct RNA sequencing,we identified voltage-dependent anion channel 3(Vdac3)as a potential target associated with ferroptosis.Fto influenced neuronal ferroptosis by regulating the m6A methylation of Vdac3 mRNA.These findings elucidate the intricate interplay between Fto,Vdac3,m6A methylation,and ferroptosis in neurons during the hyperacute phase post-ICH and suggest novel therapeutic strategies for ICH.
基金The authors would like to acknowledge the support of the National Natural Science Foundation of China(No.52279097,No.51779264)Blue and Green Project of Jiangsu Province.
文摘Natural cemented calcareous sand and limestone are highly complex and not well understood in terms of the me-chanical behavior due to the difficulty of obtaining undisturbed samples from far sea.This paper proposes an artificial method in a laboratory setting using microbial-induced carbonate precipitation(MICP)to simulate the natural process of cementation of limestone.The artificially cemented sand has a high degree of similarity with the natural weakly limestone in three aspects:(1)the mineral composition of the cemented material is also granular calcite and acicular aragonite;(2)the microstructure in interconnected open pore network can be gradually closed and contracted with cementation.The porosity reaches to approximately 9.2%;(3)both the stress-strain relationship and the unconfined strength closely resemble that of natural weakly limestone.Furthermore,both static and dynamic behaviors of artificial limestone were studied by quasi-static compression tests and Split Hopkinson Pressure Bar(SHPB)tests,finding that the unconfined strength of weakly artifical limestone exponentially increases with increasing strain rate.A rate-dependent bond strength was proposed and implemented in software to reveal the mechanism of strain rate effects.It is found that the loading velocity is too high to keep in sync with the initiation and propagation of cracks under impact loading.This delay-induced viscosity may restrict the movement of the surrounding balls,thus increasing resistance.
文摘Evaluation of hydromechanical shear behavior of unsaturated soils is still a challenging issue. The time and cost needed for conducting precise experimental investigation on shear behavior of unsaturated soils have encouraged several investigators to develop analytical, empirical, or semi-empirical models for predicting the shear behavior of unsaturated soils. However, most of the previously proposed models are for specimens subjected to the isotropic state of stress, without considering the effect of initial shear stress. In this study, a hydromechanical constitutive model is proposed for unsaturated collapsible soils during shearing, with consideration of the effect of the initial shear stress. The model implements an effective stress-based disturbed state concept (DSC) to predict the stress-strain behavior of the soil. Accordingly, material/state variables were defined for both the start of the shearing stage and the critical state of the soil. A series of laboratory tests was performed using a fully automated unsaturated triaxial device to verify the proposed model. The experimental program included 23 suction-controlled unsaturated triaxial shear tests on reconstituted specimens of Gorgan clayey loess wetted to different levels of suctions under both isotropic and anisotropic stress states. The results show excellent agreement between the prediction by the proposed model and the experimental results.
文摘The highly selective catalytic hydrogenation of halogenated nitroaromatics was achieved by employing Pd‑based catalysts that were co‑modified with organic and inorganic ligands.It was demonstrated that the catalysts contained Pd species in mixed valence states,with high valence Pd at the metal‑support interface and zero valence Pd at the metal surface.While the strong coordination of triphenylphosphine(PPh3)to Pd0 on the Pd surface prevents the adsorption of halogenated nitroaromatics and thus dehalogenation,the coordination of sodium metavanadate(NaVO3)to high‑valence Pd sites at the interface helps to activate H2 in a heterolytic pathway for the selective hydrogenation of nitro‑groups.The excellent catalytic performance of the interfacial active sites enables the selective hydrogenation of a wide range of halogenated nitroaromatics.
文摘Thermally activated delayed fluorescence(TADF)molecules have outstanding potential for applications in organic light-emitting diodes(OLEDs).Due to the lack of systematic studies on the correlation between molecular structure and luminescence properties,TADF molecules are far from meeting the needs of practical applications in terms of variety and number.In this paper,three twisted TADF molecules are studied and their photophysical properties are theoretically predicted based on the thermal vibrational correlation function method combined with multiscale calculations.The results show that all the molecules exhibit fast reverse intersystem crossing(RISC)rates(kRISC),predicting their TADF luminescence properties.In addition,the binding of DHPAzSi as the donor unit with different acceptors can change the dihedral angle between the ground and excited states,and the planarity of the acceptors is positively correlated with the reorganization energy,a property that has a strong influence on the non-radiative process.Furthermore,a decrease in the energy of the molecular charge transfer state and an increase in the kRISC were observed in the films.This study not only provides a reliable explanation for the observed experimental results,but also offers valuable insights that can guide the design of future TADF molecules.
基金funded by the National Natural Science Foundation of China (Grant Nos.42230712,42472357)the China Postdoctoral Science Foundation (Grant No.2023MD734211).
文摘Loess is susceptible to loading effects such as significant changes in strength and volume variation caused by loading and wetting.In this study,considering the different connection states of pore water and gas in loess fabric,the gas phase closure case is incorporated into a unified form of the generalized effective stress framework,introducing a damage parameter considering the effects of closed pore gas.The loading effects of unsaturated loess under wide variations in saturation are described in a unified way,and the model performance is verified by corresponding stress and hydraulic path tests.The results indicated that the collapse response involves the initial void ratio of loess,and the coupled outwards motion of the loading-collapse(LC)yield surface under loading enhances its structural strength.Suction-enhanced yield stress requires a greater"tensile stress"to counteract its structural stability.The nucleation of bubbles at high saturation causes a decrease in yield stress.The loading effect exhibits a smaller collapse behavior when the influence of closed gas is considered,whereas the suction path does not cross the LC in the stress space under hydraulic action for the same parameters,which amplifies the influence of closed gas on loess deformation.
基金supported by the National Key R&D Program of China(Grant No.2022YFA1204100)the National Natural Science Foundation of China(Grant Nos.62488201 and 1240041502)+2 种基金the CAS Project for Young Scientists in Basic Research(Grant No.YSBR-003)the Chinese Academy of Sciences(Grant No.XDB33030100)the Innovation Program of Quantum Science and Technology(Grant No.2021ZD0302700).
文摘Vanadium-based transition metal chalcogenides VmXn(X=S,Se,Te)with their distinctive quantum effects,tunable magnetism,spin-orbit coupling,and high carrier mobility are a valuable platform to explore the interplay between magnetism and electronic correlations,especially with tunable structural phases and magnetic properties through stoichiometric variations,making them ideal candidates for advanced device applications.Here,we report the synthesis of high-quality V_(5+x)S_(8)single crystals with different concentrations of self-intercalated vanadium.V_(5+x)S_(8)crystals show an antiferromagnetic behavior and a spin-flop-like transition below TN of 30.6 K.The high-quality V_(5+x)S_(8)single crystals exhibit a large negative magnetoresistance of 12.3%at 2 K.Interestingly,V_(5+x)S_(8)crystals show an obvious low-temperature resistance upturn that gradually levels off with the increasing magnetic field,attributed to the Kondo effect arising from the interaction between conduction electrons and embedded vanadium magnetic impurities.With increasing V doping,the antiferromagnetic interactions intensify,weakening the coupling between the local moments and conduction electrons,which in turn lowers the Kondo temperature(TK).Furthermore,the anomalous Hall effect is observed in V5.73S8,with an anomalous Hall conductivity(AHC)of 50.46 W^(-1)·cm^(-1)and anomalous Hall angle of 0.73%at 2 K.Our findings offer valuable insights into the mechanisms of the Kondo effect and anomalous Hall effect in self-intercalated transition metal chalcogenides with complex magnetism and electronic correlation effects.
文摘Urban green spaces and parks offer opportunities for retaining and increasing bird richness, diversity, and species abundance. However, urbanisation influences predator–prey interactions, leading to high predation rates in urban areas, in the UK notably through the presence of large populations of domestic cats and increased populations of synanthropic species, such as rats and squirrels. These high predation rates are assumed to be a significant cause of reproductive failure in birds. Some ecologists advocate for the use of buffer zones with reduced human influence to reduce potential hunting pressure in eco-sensitive areas. However, the buffer effect on predation rates of nesting birds in suburban areas is rarely investigated. In this study, we investigated how edge effects (how close nest sites are to housing) and nest height (i.e., ground vs. above-ground) affected nest predation rates in a suburban park using camera traps to monitor artificial nests containing quail eggs. Our hypothesis was that nests in the buffer area (<300 m inward from university boundary) and at low height would suffer higher predation rates than nests in the core area (>300 m from the university boundary) and at height, as the buffer zone effect, and ease of access to ground predators would result in higher predation rates. We found no significant effect of nest height in nest predation rates. However, contrary to our expectations, nests in the core zone suffered higher predation rates than those in the buffer zone, and corvids were responsible for almost half of the egg loss events. We speculate that this may be a consequence of higher levels of anthropogenic disturbance (e.g., pedestrians, dog walking, vehicles) adjacent to our buffer zone acting as a deterrent to avian nest predators. This work suggests that protecting urban sites from disturbance may not always act to support bird abundance.
文摘The pressure and temperature increase resulting from the impact of different threats onto target materials is analyzed with a unified laboratory-scale setup.This allows deriving qualitative information on the occurring phenomenology as well as quantitative statements about the relative effects sizes as a function of target material and threat.The considered target materials are steel,aluminum,and magnesium.As threats,kinetic energy penetrator,explosively formed projectile,and shaped charge jet are used.For the investigated combinations,the measured overpressures vary by a factor of up to 5 for a variation of the material,by a factor of up to 7 for a variation of the threat,and by a factor larger than 15for a simultaneous variation of both.The obtained results as well as the experimental approach are relevant for the basic understanding of impact effects and risks due to material reactivity.The paper combines two main aims.Firstly,to provide a summary of own prior work in a coherent journal article and,secondly,to review and discuss these earlier results with a new perspective.
