Ion migration capability and interfacial chemistry of solid polymer electrolytes(SPEs)in all-solid-state sodium metal batteries(ASSMBs)are closely related to the Na^(+)coordination environment.Herein,an electrostatic ...Ion migration capability and interfacial chemistry of solid polymer electrolytes(SPEs)in all-solid-state sodium metal batteries(ASSMBs)are closely related to the Na^(+)coordination environment.Herein,an electrostatic engineering strategy is proposed to regulate the Na^(+)coordinated structure by employing a fluorinated metal–organic framework as an electron-rich model.Theoretical and experimental results revealed that the abundant electron-rich F sites can accelerate the disassociation of Na-salt through electrostatic attraction to release free Na^(+),while forcing anions into a Na^(+)coordination structure though electrostatic repulsion to weaken the Na^(+)coordination with polymer,thus promoting rapid Na^(+)transport.The optimized anion-rich weak solvation structure fosters a stable inorganic-dominated solid–electrolyte interphase,significantly enhancing the interfacial stability toward Na anode.Consequently,the Na/Na symmetric cell delivered stable Na plating/stripping over 2500 h at 0.1 mA cm^(−2).Impressively,the assembled ASSMBs demonstrated stable performance of over 2000 cycles even under high rate of 2 C with capacity retention nearly 100%,surpassing most reported ASSMBs using various solid-state electrolytes.This work provides a new avenue for regulating the Na^(+)coordination structure of SPEs by exploration of electrostatic effect engineering to achieve high-performance all-solid-state alkali metal batteries.展开更多
The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecul...The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecules and{[Co2(BINDI)(DMA)_(2)]·DMA}_(n)(Co-MOF,H4BINDI=N,N'-bis(5-isophthalic acid)naphthalenediimide,DMA=N,N-dimethylacetamide)was synthesized via a one-pot method,leveragingπ-πinteractions between pyrene and Co-MOF to modulate electrical conductivity.Results demonstrate that the Py@Co-MOF catalyst exhibited significantly enhanced OER performance compared to pure Co-MOF or pyrene-based electrodes,achieving an overpotential of 246 mV at a current density of 10 mA·cm^(-2) along with excellent stability.Density functional theory(DFT)calculations reveal that the formation of O*in the second step is the rate-determining step(RDS)during the OER process on Co-MOF,with an energy barrier of 0.85 eV due to the weak adsorption affinity of the OH*intermediate for Co sites.CCDC:2419276.展开更多
Protein aggregates,mitochondrial import stress and neurodegenerative disorders:A salient hallmark of several neurodegenerative diseases,including Parkinson’s disease,is the abundance of protein aggregates(Goiran et a...Protein aggregates,mitochondrial import stress and neurodegenerative disorders:A salient hallmark of several neurodegenerative diseases,including Parkinson’s disease,is the abundance of protein aggregates(Goiran et al.,2022).This molecular event is believed to lead to activation of stress pathways ultimately resulting in cellular dysfunction(Eldeeb et al.,2022).Accordingly,many lines of research investigations focused on dampening the formation of protein aggregates or augmenting the clearance of protein aggregates as a potential therapeutic strategy to counteract the progression of neurodegenerative diseases,albeit with little success(Costa-Mattioli and Walter,2020).Cell stress cues such as the accumulation of protein aggregates lead to the activation of stress response pathways that aid cells in responding to the damage.Despite the notion that the transient activation of these pathways helps cells cope with stressors,persistent activation can induce unwanted apoptosis of cells and reduce overall tissue strength as well as lead to an accumulation of aggregation-prone proteins(Hetz and Papa,2018).Mutations in proteins involved in stress signaling termination can cause conditions like ataxia and early-onset dementia(Conroy et al.,2014).Therefore,it is crucial for stress response signaling to be turned off once conditions have improved.Nevertheless,the mechanisms by which cells silence these signals are still elusive.展开更多
Traumatic spinal cord injury often leads to the disintegration of nerve cells and axons,resulting in a substantial accumulation of myelin debris that can persist for years.The abnormal buildup of myelin debris at site...Traumatic spinal cord injury often leads to the disintegration of nerve cells and axons,resulting in a substantial accumulation of myelin debris that can persist for years.The abnormal buildup of myelin debris at sites of injury greatly impedes nerve regeneration,making the clearance of debris within these microenvironments crucial for effective post-spinal cord injury repair.In this review,we comprehensively outline the mechanisms that promote the clearance of myelin debris and myelin metabolism and summarize their roles in spinal cord injury.First,we describe the composition and characteristics of myelin debris and explain its effects on the injury site.Next,we introduce the phagocytic cells involved in myelin debris clearance,including professional phagocytes(macrophages and microglia)and non-professional phagocytes(astrocytes and microvascular endothelial cells),as well as other cells that are also proposed to participate in phagocytosis.Finally,we focus on the pathways and associated targets that enhance myelin debris clearance by phagocytes and promote lipid metabolism following spinal cord injury.Our analysis indicates that myelin debris phagocytosis is not limited to monocyte-derived macrophages,but also involves microglia,astrocytes,and microvascular endothelial cells.By modulating the expression of genes related to phagocytosis and lipid metabolism,it is possible to modulate lipid metabolism disorders and influence inflammatory phenotypes,ultimately affecting the recovery of motor function following spinal cord injury.Additionally,therapies such as targeted mitochondrial transplantation in phagocytic cells,exosome therapy,and repeated trans-spinal magnetic stimulation can effectively enhance the removal of myelin debris,presenting promising potential for future applications.展开更多
This study presents a thorough investigation into the use of single and twin-tailed cationic and anionic surfactant-modified chitosan(SMCS)hydrogel beads as effective adsorbents for the elimination of hazardous polycy...This study presents a thorough investigation into the use of single and twin-tailed cationic and anionic surfactant-modified chitosan(SMCS)hydrogel beads as effective adsorbents for the elimination of hazardous polycyclic aromatic hydrocarbons(PAHs)from aqueous solutions.The Chitosan(CS)hydrogel beads were modified with single/twin-tailed anionic surfactants,sodium dodecyl sulfate(SDS)and sodium bis(2-ethylhexyl)sulfosuccinate(AOT),and cationic surfactants,dodecyltrimethylammonium bromide(DTAB)and didodecyldimethylammonium bromide(DDAB),to enhance their adsorption capacity of PAHs.The CS and SMCS beads were evaluated for their structural,mechanical,and adsorption properties using a range of techniques,including infrared spectroscopy(IR),energy-dispersive X-ray spectroscopy(EDX),rheometry,and field emission scanning electron microscopy(FESEM).Adsorption experiments of naphthalene(Nap),acenaphthene(Ace),and phenanthrene(Phe)on SMCS beads demonstrate that they have significantly higher adsorption capacities than CS beads,due to increase in hydrophobic interactions.Adsorption capacity followed the trend,Phen>Ace>Nap for all the beads revealing that twin-tailed SMCS bead possess much higher adsorption capacities(Qmax)compared to single-tailed SMCS beads.For twin tailed surfactants,the maximum adsorption capacities for Nap,Ace and Phe varied as CS-AOT(CS-DDAB):430.0(323.8)611.60(538.18)633.39(536.99)mg/g respectively,outperforming other reported hydrogel beads.The study highlights the simplicity,eco-friendliness,and enhanced performance of surfactant modification for developing high-efficiency adsorbents,paving the way for cost-effective solutions in water re-mediation.展开更多
Although multicrystalline Si photovoltaics have been extensively studied and applied in the collection of solar energy,the same systems suffer significant efficiency losses in indoor settings,where ambient light condi...Although multicrystalline Si photovoltaics have been extensively studied and applied in the collection of solar energy,the same systems suffer significant efficiency losses in indoor settings,where ambient light conditions are considerably smaller in intensity and possess greater components of non-normal incidence.Yet,indoor light-driven,stand-alone devices can offer sustainable advances in next-generation technologies such as the Internet of Things.Here,we present a non-invasive solution to aid in photovoltaic indoor light collection—radially distributed waveguide-encoded lattice(RDWEL)slim films(thickness 1.5 mm).Embedded with a monotonical radial array of cylindrical waveguides(±20°),the RDWEL demonstrates seamless light collection(FoV(fields of view)=74.5°)and imparts enhancements in JSC(short circuit current density)of 44%and 14%for indoor and outdoor lighting conditions,respectively,when coupled to a photovoltaic device and compared to an unstructured but otherwise identical slim film coating.展开更多
Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previo...Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previous research,providing a long-term perspective on carbonyl compound variations and their environmental implica-tions.Atmospheric observations were conducted at Beijing(BJ)and Xianghe(XH)during the summer and winter months of 2018,2019,and 2023 to study the sources and impacts of carbonyl compounds in typical urban areas and peri‑urban areas.Notably,concentrations in the summer of 2023 increased compared to 2018 and 2019.The predominant carbonyl compounds—formaldehyde,acetaldehyde,and acetone—accounted for over 60%of the total.The mean values of OFP in BJ ranged from 18.55 to 58.61μg/m3,lower than those in XH(29.82 to 65.48μg/m3),with formaldehyde and acetaldehyde contributing over 80%of the total.SOAP exhibited a similar pattern,with values in XH(69.21 to 508.55μg/m3)significantly exceeding those in BJ(34.47 to 159.78μg/m3).The PMF model highlighted vehicle exhaust,secondary pollution,and biomass combustion as major sources of carbonyl compounds,emphasizing differences in source contributions between the two regions.This study’s com-parative analysis over different years and locations provides new insights into the dynamic changes in carbonyl compounds and their environmental importance.These results not only reinforce the importance of carbonyl compounds regulation but also offer a valuable reference for evaluating and refining emission control strategies during this period.展开更多
Fe reducing bacteria(FRB),through extracellular electron transfer(EET)pathway,can reduce Fe(III)nanoparticles,thereby affecting the migration,transformation,and degradation of pollutants.However,the interaction of Fe(...Fe reducing bacteria(FRB),through extracellular electron transfer(EET)pathway,can reduce Fe(III)nanoparticles,thereby affecting the migration,transformation,and degradation of pollutants.However,the interaction of Fe(III)nanoparticles with the most commonly identified FRB,Geobacter sulfurreducens PCA,remains poorly understood.Herein,we demonstrated that the synergistic role of outer membrane proteins and periplasmic proteins in the EET process for-Fe_(2)O_(3),Fe3O4,and𝛽α-FeOOH nanoparticles by construction of multiple gene knockout strain.oxpG(involved in the type II secretion system)and omcST(outer membrane c-type cytochrome)medi-ated pathways accounted for approximately 67%of the total reduction of𝛼α-Fe_(2)O_(3) nanoparticles.The residual reduction of𝛼α-Fe_(2)O_(3) nanoparticles in∆oxpG-omcST strain was likely caused by redox-active substances in cell supernatant.Conversely,the reduction of dissolved Fe(III)was almost unaffected in∆oxpG-omcST strain at the same concentration.However,at high dissolved Fe(III)concentration,the reduction significantly decreased due to the formation of Fe(III)nanoparticles,suggesting that this EET process is specific to Fe(III)nanoparticles.Overall,our study provided a more comprehensive understanding for the EET pathways between G.sulfurreducens PCA and different Fe(III)species,enriching our knowledge on the role of microorganisms in iron biogeochemical cycles and remediation strategies of pollutants.展开更多
Electron–hole(e–h)recombination is a fundamental process that governs energy dissipation and device efficiency in semiconductors.In two-dimensional(2D)materials,the formation of tightly bound excitons makes exciton-...Electron–hole(e–h)recombination is a fundamental process that governs energy dissipation and device efficiency in semiconductors.In two-dimensional(2D)materials,the formation of tightly bound excitons makes exciton-mediated e–h recombination the dominant decay pathway.In this work,nonradiative e–h recombination within excitons in monolayer MoS2 is investigated using first-principles simulations that combine nonadiabatic molecular dynamics with𝐺𝑊and real-time Bethe–Salpeter equation(BSE)propagation.A two-step process is identified:rapid intervalley redistribution induced by exchange interaction,followed by slower phonon-assisted recombination facilitated by exciton binding.By selectively removing the screened Coulomb and exchange terms from the BSE Hamiltonian,their respective contributions are disentangled—exchange interaction is found to increase the number of accessible recombination pathways,while binding reduces the excitation energy and enhances nonradiative decay.A reduction in recombination lifetime by over an order of magnitude is observed due to the excitonic many-body effects.These findings provide microscopic insights for understanding and tuning exciton lifetimes in 2D transition-metal dichalcogenides.展开更多
As silicon-based transistors face fundamental scaling limits,the search for breakthrough alternatives has led to innovations in 3D architectures,heterogeneous integration,and sub-3 nm semiconductor body thicknesses.Ho...As silicon-based transistors face fundamental scaling limits,the search for breakthrough alternatives has led to innovations in 3D architectures,heterogeneous integration,and sub-3 nm semiconductor body thicknesses.However,the true effectiveness of these advancements lies in the seamless integration of alternative semiconductors tailored for next-generation transistors.In this review,we highlight key advances that enhance both scalability and switching performance by leveraging emerging semiconductor materials.Among the most promising candidates are 2D van der Waals semiconductors,Mott insulators,and amorphous oxide semiconductors,which offer not only unique electrical properties but also low-power operation and high carrier mobility.Additionally,we explore the synergistic interactions between these novel semiconductors and advanced gate dielectrics,including high-K materials,ferroelectrics,and atomically thin hexagonal boron nitride layers.Beyond introducing these novel material configurations,we address critical challenges such as leakage current and long-term device reliability,which become increasingly crucial as transistors scale down to atomic dimensions.Through concrete examples showcasing the potential of these materials in transistors,we provide key insights into overcoming fundamental obstacles—such as device reliability,scaling down limitations,and extended applications in artificial intelligence—ultimately paving the way for the development of future transistor technologies.展开更多
The growing global energy demand and worsening climate change highlight the urgent need for clean,efficient and sustainable energy solutions.Among emerging technologies,atomically thin two-dimensional(2D)materials off...The growing global energy demand and worsening climate change highlight the urgent need for clean,efficient and sustainable energy solutions.Among emerging technologies,atomically thin two-dimensional(2D)materials offer unique advantages in photovoltaics due to their tunable optoelectronic properties,high surface area and efficient charge transport capabilities.This review explores recent progress in photovoltaics incorporating 2D materials,focusing on their application as hole and electron transport layers to optimize bandgap alignment,enhance carrier mobility and improve chemical stability.A comprehensive analysis is presented on perovskite solar cells utilizing 2D materials,with a particular focus on strategies to enhance crystallization,passivate defects and improve overall cell efficiency.Additionally,the application of 2D materials in organic solar cells is examined,particularly for reducing recombination losses and enhancing charge extraction through work function modification.Their impact on dye-sensitized solar cells,including catalytic activity and counter electrode performance,is also explored.Finally,the review outlines key challenges,material limitations and performance metrics,offering insight into the future development of nextgeneration photovoltaic devices encouraged by 2D materials.展开更多
Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and of...Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.展开更多
Aqueous zinc metal batteries(AZMBs)face significant challenges in achieving reversibility and cycling stability,primarily due to hydrogen evolution reactions(HER)and zinc dendrite growth.In this study,by employing car...Aqueous zinc metal batteries(AZMBs)face significant challenges in achieving reversibility and cycling stability,primarily due to hydrogen evolution reactions(HER)and zinc dendrite growth.In this study,by employing carefully designed cells that approximate the structural characteristics of practical batteries,we revisit this widely held view through in-operando X-ray radiography to examine zinc dendrite formation and HER under nearpractical operating conditions.While conventional understanding emphasizes the severity of these processes,our findings suggest that zinc dendrites and HER are noticeably less pronounced in dense,real-operation configurations compared to modified cells,possibly due to a more uniform electric field and the suppression of triple-phase boundaries.This study indicates that other components,such as degradation at the cathode current collector interface and configuration mismatches within the full cell,may also represent important barriers to the practical application of AZMBs,particularly during the early stages of electrodeposition.展开更多
Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances ar...Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances are far from practical needs due to the lack of efficient electrocatalysts.Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties.Herein,we realize boron(B)-insertion-induced phase regulation of rhodium(Rh)nanocrystals to obtain amorphous Rh_(4)B nanoparticles(NPs)and hexagonal close-packed(hcp)RhB NPs through a facile wet-chemical method.A high Faradaic efficiency(92.1±1.2%)and NH_(3) yield rate(629.5±11.0μmol h^(−1) cm^(−2))are achieved over hcp RhB NPs,far superior to those of most reported NORR nanocatalysts.In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center,enhanced NO adsorption/activation profile,and greatly reduced energy barrier of the rate-determining step.A demonstrative Zn-NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2,realizing simultaneous NO removal,NH3 synthesis,and electricity output.展开更多
Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains...Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains a confusing topic.Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures(SCSs)for Zn-ion storage with double-high capacitive activity and durability.Tetrachlorobenzoquinone(H-bond acceptor)and dimethylbenzidine(H-bond donator)can interact to form organic nanosheet modules,which are sequentially assembled,orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds(N-H···O).Featured with rich surface-active heterodiatomic motifs,more exposed nanoporous channels,and successive charge migration paths,SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers(3.3Ωs-0.5).Consequently,the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics,including high energy density(166 Wh kg-1),high-rate performance(172 m Ah g^(-1)at 20 A g^(-1)),and long-lasting cycling lifespan(95.5%capacity retention after 500,000 cycles).An opposite chargecarrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage,involving high-kinetics physical Zn^(2+)/CF_(3)SO_(3)-adsorption and chemical Zn^(2+)redox with carbonyl/pyridine groups.This work gives insights into H-bond-guided interfacial superassembly design of superstructural carbons toward advanced energy storage.展开更多
Recent advances in high-pressure technologies and large-scale experimental and computational facilities have enabled scientists,at an unprecedented rate,to discover and predict novel states and materials under the ext...Recent advances in high-pressure technologies and large-scale experimental and computational facilities have enabled scientists,at an unprecedented rate,to discover and predict novel states and materials under the extreme pressure-temperature conditions found in deep,giant-planet interiors.Based on a well-documented body of work in this field of high-pressure research,we elucidate the fundamental principles that govern the chemistry of dense solids under extreme conditions.These include:(i)the pressure-induced evolution of chemical bonding and structure of molecular solids to extended covalent solids,ionic solids and,ultimately,metallic solids,as pressure increases to the terapascal regime;(ii)novel properties and complex transition mechanisms,arising from the subtle balance between electron hybridization(bonding)and electrostatic interaction(packing)in densely packed solids;and(iii)new dense framework solids with high energy densities,and with tunable properties and stabilities under ambient conditions.Examples are taken primarily fromlow-Z molecular systems that have scientific implications for giant-planet models,condensed materials physics,and solid-state core-electron chemistry.展开更多
Present review for the first time provides a complete botanical description and information on ethnomcdicinal uses of Clerodendron glandulosum.Coleb(CG:Fam.Verbenaceae).Recent studies conducted from our laborator) pro...Present review for the first time provides a complete botanical description and information on ethnomcdicinal uses of Clerodendron glandulosum.Coleb(CG:Fam.Verbenaceae).Recent studies conducted from our laborator) provide pharmacological evidence for its anti-hypertensive,antidiabetic and anti-obesity potentials.Further,its beneficial potential in preventing in vitro and in vivo non-alcoholic steatohepatitis and atherosclerosis and potent hcpatoprotective and free radical scavenging abilities along with its acute and sub- chronic toxicologiesl evaluations are also reported from our laboratory.In keeping with its traditional uses,CG extract was capable of ameliorating experimentally induced hypertension,diabetes and obesity.Its beneficial potential against NASH induced oxidative stress and atherosclerosis can be attributed to its potent free radical scavenging potential.Non—toxic nature of CG leaf extract further provides added merit to its reported pharmacological properties.The present review summarizes the pioneering scientific evidence for the pharmacological effects of CG against related metabolic disorders like hypertension,diabetes and obesity along with anti oxidant potential and beneficial elicits against non alcoholic steatohepatitis.展开更多
In nature,the properties of matter are ultimately governed by the electronic structures.Quantum chemistry(QC)at electronic level matches well with a few simple physical assumptions in solving simple problems.To date,m...In nature,the properties of matter are ultimately governed by the electronic structures.Quantum chemistry(QC)at electronic level matches well with a few simple physical assumptions in solving simple problems.To date,machine learning(ML)algorithm has been migrated to this field to simplify calculations and improve fidelity.This review introduces the basic information on universal electron structures of emerging energy materials and ML algorithms involved in the prediction of material properties.Then,the structure-property relationships based on ML algorithm and QC theory are reviewed.Especially,the summary of recently reported applications on classifying crystal structure,modeling electronic structure,optimizing experimental method,and predicting performance is provided.Last,an outlook on ML assisted QC calculation towards identifying emerging energy materials is also presented.展开更多
Two dinuclear organotin complexes C8H14（CO2SnCy3）2（1）（Cy = cyclohexyl group） and C8H14[CO2Sn（CH2CMe2Ph）3]2（2） were synthesized by the reactions of camphoric acid with tricyclohexyltin hydroxide and bis[tri（...Two dinuclear organotin complexes C8H14（CO2SnCy3）2（1）（Cy = cyclohexyl group） and C8H14[CO2Sn（CH2CMe2Ph）3]2（2） were synthesized by the reactions of camphoric acid with tricyclohexyltin hydroxide and bis[tri（2-methyl-2-phenyl）propyltin] oxide under solvothermal conditions, and these complexes were characterized by infrared spectra, elemental analyses, and H NMR spectra. The crystal of 1 belongs to the monoclinic system, space group P21/c with a = 1.83478（19）, b = 1.52707（18）, c = 1.9849（2） nm, β = 122.515（7）°, Z = 4, V = 4.6896（9） nm^3, Dc = 1.324 g/cm^3, μ（MoKα） = 1.103 mm^-1, F（000） = 1952, R = 0.0697 and wR = 0.2040. In addition, thermal stability and quantum chemical calculation of 1 were also studied.展开更多
The geometries of imidazole and its derivatives were respectively optimized by using ab initio method, and the molecular orbital energy levels and the charge densities were obtained for their optimum geometries. The f...The geometries of imidazole and its derivatives were respectively optimized by using ab initio method, and the molecular orbital energy levels and the charge densities were obtained for their optimum geometries. The frontier orbital energy levels, and the net charges of N (1) atom and the imidazole ring of those molecules were obtained with ab initio and SCC-DV-Xα methods. It was found that the inhibition properties of those compounds change with the highest occupied molecular orbital energy levels, and the net charges of N (1) atom. We took four iron atoms on the crystal plane (100) of α-iron as the surface which was used to study the adsorption towards the inhibitors. The adsorption models of the inhibitor to be adsorbed on the Fe-cluster surface were optimized with SCC-DV-Xα method. It turns out that the most favorable model is that the inhibitor molecule is adsorbed on the Fe-cluster surface in an inclined state. The calculation shows that the stabilization energies of the systems are well correlated with the inhibition efficiencies.展开更多
基金supported by the National Natural Science Foundation of China(No.52473213 and No.52203261)。
文摘Ion migration capability and interfacial chemistry of solid polymer electrolytes(SPEs)in all-solid-state sodium metal batteries(ASSMBs)are closely related to the Na^(+)coordination environment.Herein,an electrostatic engineering strategy is proposed to regulate the Na^(+)coordinated structure by employing a fluorinated metal–organic framework as an electron-rich model.Theoretical and experimental results revealed that the abundant electron-rich F sites can accelerate the disassociation of Na-salt through electrostatic attraction to release free Na^(+),while forcing anions into a Na^(+)coordination structure though electrostatic repulsion to weaken the Na^(+)coordination with polymer,thus promoting rapid Na^(+)transport.The optimized anion-rich weak solvation structure fosters a stable inorganic-dominated solid–electrolyte interphase,significantly enhancing the interfacial stability toward Na anode.Consequently,the Na/Na symmetric cell delivered stable Na plating/stripping over 2500 h at 0.1 mA cm^(−2).Impressively,the assembled ASSMBs demonstrated stable performance of over 2000 cycles even under high rate of 2 C with capacity retention nearly 100%,surpassing most reported ASSMBs using various solid-state electrolytes.This work provides a new avenue for regulating the Na^(+)coordination structure of SPEs by exploration of electrostatic effect engineering to achieve high-performance all-solid-state alkali metal batteries.
文摘The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecules and{[Co2(BINDI)(DMA)_(2)]·DMA}_(n)(Co-MOF,H4BINDI=N,N'-bis(5-isophthalic acid)naphthalenediimide,DMA=N,N-dimethylacetamide)was synthesized via a one-pot method,leveragingπ-πinteractions between pyrene and Co-MOF to modulate electrical conductivity.Results demonstrate that the Py@Co-MOF catalyst exhibited significantly enhanced OER performance compared to pure Co-MOF or pyrene-based electrodes,achieving an overpotential of 246 mV at a current density of 10 mA·cm^(-2) along with excellent stability.Density functional theory(DFT)calculations reveal that the formation of O*in the second step is the rate-determining step(RDS)during the OER process on Co-MOF,with an energy barrier of 0.85 eV due to the weak adsorption affinity of the OH*intermediate for Co sites.CCDC:2419276.
文摘Protein aggregates,mitochondrial import stress and neurodegenerative disorders:A salient hallmark of several neurodegenerative diseases,including Parkinson’s disease,is the abundance of protein aggregates(Goiran et al.,2022).This molecular event is believed to lead to activation of stress pathways ultimately resulting in cellular dysfunction(Eldeeb et al.,2022).Accordingly,many lines of research investigations focused on dampening the formation of protein aggregates or augmenting the clearance of protein aggregates as a potential therapeutic strategy to counteract the progression of neurodegenerative diseases,albeit with little success(Costa-Mattioli and Walter,2020).Cell stress cues such as the accumulation of protein aggregates lead to the activation of stress response pathways that aid cells in responding to the damage.Despite the notion that the transient activation of these pathways helps cells cope with stressors,persistent activation can induce unwanted apoptosis of cells and reduce overall tissue strength as well as lead to an accumulation of aggregation-prone proteins(Hetz and Papa,2018).Mutations in proteins involved in stress signaling termination can cause conditions like ataxia and early-onset dementia(Conroy et al.,2014).Therefore,it is crucial for stress response signaling to be turned off once conditions have improved.Nevertheless,the mechanisms by which cells silence these signals are still elusive.
基金supported by the National Natural Science Foundation of China,Nos.82271411(to RG),51803072(to WL)the International Cooperative Project of Talent Cultivation“Xinghai Project”at the China-Japan Union Hospital of Jilin University,No.XHLH202404(to WL)+1 种基金the Science and Technology Development Plan of Jilin Province,No.YDZJ202201ZYTS038(to WL)Jilin Provincial Finance Program,No.2022SCZ10(to WL)。
文摘Traumatic spinal cord injury often leads to the disintegration of nerve cells and axons,resulting in a substantial accumulation of myelin debris that can persist for years.The abnormal buildup of myelin debris at sites of injury greatly impedes nerve regeneration,making the clearance of debris within these microenvironments crucial for effective post-spinal cord injury repair.In this review,we comprehensively outline the mechanisms that promote the clearance of myelin debris and myelin metabolism and summarize their roles in spinal cord injury.First,we describe the composition and characteristics of myelin debris and explain its effects on the injury site.Next,we introduce the phagocytic cells involved in myelin debris clearance,including professional phagocytes(macrophages and microglia)and non-professional phagocytes(astrocytes and microvascular endothelial cells),as well as other cells that are also proposed to participate in phagocytosis.Finally,we focus on the pathways and associated targets that enhance myelin debris clearance by phagocytes and promote lipid metabolism following spinal cord injury.Our analysis indicates that myelin debris phagocytosis is not limited to monocyte-derived macrophages,but also involves microglia,astrocytes,and microvascular endothelial cells.By modulating the expression of genes related to phagocytosis and lipid metabolism,it is possible to modulate lipid metabolism disorders and influence inflammatory phenotypes,ultimately affecting the recovery of motor function following spinal cord injury.Additionally,therapies such as targeted mitochondrial transplantation in phagocytic cells,exosome therapy,and repeated trans-spinal magnetic stimulation can effectively enhance the removal of myelin debris,presenting promising potential for future applications.
基金the Department of Science and Technology(DST),Govt.of India for providing funds under the FIST program and PURSE grant vide No.SR/PURSE/2020/31 to the department of Chemistry,University of Kashmir.
文摘This study presents a thorough investigation into the use of single and twin-tailed cationic and anionic surfactant-modified chitosan(SMCS)hydrogel beads as effective adsorbents for the elimination of hazardous polycyclic aromatic hydrocarbons(PAHs)from aqueous solutions.The Chitosan(CS)hydrogel beads were modified with single/twin-tailed anionic surfactants,sodium dodecyl sulfate(SDS)and sodium bis(2-ethylhexyl)sulfosuccinate(AOT),and cationic surfactants,dodecyltrimethylammonium bromide(DTAB)and didodecyldimethylammonium bromide(DDAB),to enhance their adsorption capacity of PAHs.The CS and SMCS beads were evaluated for their structural,mechanical,and adsorption properties using a range of techniques,including infrared spectroscopy(IR),energy-dispersive X-ray spectroscopy(EDX),rheometry,and field emission scanning electron microscopy(FESEM).Adsorption experiments of naphthalene(Nap),acenaphthene(Ace),and phenanthrene(Phe)on SMCS beads demonstrate that they have significantly higher adsorption capacities than CS beads,due to increase in hydrophobic interactions.Adsorption capacity followed the trend,Phen>Ace>Nap for all the beads revealing that twin-tailed SMCS bead possess much higher adsorption capacities(Qmax)compared to single-tailed SMCS beads.For twin tailed surfactants,the maximum adsorption capacities for Nap,Ace and Phe varied as CS-AOT(CS-DDAB):430.0(323.8)611.60(538.18)633.39(536.99)mg/g respectively,outperforming other reported hydrogel beads.The study highlights the simplicity,eco-friendliness,and enhanced performance of surfactant modification for developing high-efficiency adsorbents,paving the way for cost-effective solutions in water re-mediation.
基金supported by the European Research Council(ERC)under the European Union's Horizon 2020 Research and Innovation Programme(Grant Agreement No.818762)the Engineering and Physical Sciences Research Council(Grant No.EP/V048953/1)and the Isaac Newton Trust(grant 22.39(m))。
文摘Although multicrystalline Si photovoltaics have been extensively studied and applied in the collection of solar energy,the same systems suffer significant efficiency losses in indoor settings,where ambient light conditions are considerably smaller in intensity and possess greater components of non-normal incidence.Yet,indoor light-driven,stand-alone devices can offer sustainable advances in next-generation technologies such as the Internet of Things.Here,we present a non-invasive solution to aid in photovoltaic indoor light collection—radially distributed waveguide-encoded lattice(RDWEL)slim films(thickness 1.5 mm).Embedded with a monotonical radial array of cylindrical waveguides(±20°),the RDWEL demonstrates seamless light collection(FoV(fields of view)=74.5°)and imparts enhancements in JSC(short circuit current density)of 44%and 14%for indoor and outdoor lighting conditions,respectively,when coupled to a photovoltaic device and compared to an unstructured but otherwise identical slim film coating.
基金supported by the National Natural Science Foundation of China(Nos.41905108 and 42130704).
文摘Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previous research,providing a long-term perspective on carbonyl compound variations and their environmental implica-tions.Atmospheric observations were conducted at Beijing(BJ)and Xianghe(XH)during the summer and winter months of 2018,2019,and 2023 to study the sources and impacts of carbonyl compounds in typical urban areas and peri‑urban areas.Notably,concentrations in the summer of 2023 increased compared to 2018 and 2019.The predominant carbonyl compounds—formaldehyde,acetaldehyde,and acetone—accounted for over 60%of the total.The mean values of OFP in BJ ranged from 18.55 to 58.61μg/m3,lower than those in XH(29.82 to 65.48μg/m3),with formaldehyde and acetaldehyde contributing over 80%of the total.SOAP exhibited a similar pattern,with values in XH(69.21 to 508.55μg/m3)significantly exceeding those in BJ(34.47 to 159.78μg/m3).The PMF model highlighted vehicle exhaust,secondary pollution,and biomass combustion as major sources of carbonyl compounds,emphasizing differences in source contributions between the two regions.This study’s com-parative analysis over different years and locations provides new insights into the dynamic changes in carbonyl compounds and their environmental importance.These results not only reinforce the importance of carbonyl compounds regulation but also offer a valuable reference for evaluating and refining emission control strategies during this period.
基金supported by the National Key Research and Development Project(No.2020YFA0907500)the National Natural Science Foundation of China(No.22476206)+1 种基金the supports from the National Young Top-Notch Talents(No.W03070030)Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.Y202011).
文摘Fe reducing bacteria(FRB),through extracellular electron transfer(EET)pathway,can reduce Fe(III)nanoparticles,thereby affecting the migration,transformation,and degradation of pollutants.However,the interaction of Fe(III)nanoparticles with the most commonly identified FRB,Geobacter sulfurreducens PCA,remains poorly understood.Herein,we demonstrated that the synergistic role of outer membrane proteins and periplasmic proteins in the EET process for-Fe_(2)O_(3),Fe3O4,and𝛽α-FeOOH nanoparticles by construction of multiple gene knockout strain.oxpG(involved in the type II secretion system)and omcST(outer membrane c-type cytochrome)medi-ated pathways accounted for approximately 67%of the total reduction of𝛼α-Fe_(2)O_(3) nanoparticles.The residual reduction of𝛼α-Fe_(2)O_(3) nanoparticles in∆oxpG-omcST strain was likely caused by redox-active substances in cell supernatant.Conversely,the reduction of dissolved Fe(III)was almost unaffected in∆oxpG-omcST strain at the same concentration.However,at high dissolved Fe(III)concentration,the reduction significantly decreased due to the formation of Fe(III)nanoparticles,suggesting that this EET process is specific to Fe(III)nanoparticles.Overall,our study provided a more comprehensive understanding for the EET pathways between G.sulfurreducens PCA and different Fe(III)species,enriching our knowledge on the role of microorganisms in iron biogeochemical cycles and remediation strategies of pollutants.
基金supported by the National Key Research and Development Program of China (Grant Nos.2024YFA1409800 for J.Z.and2024YFA1408603 for Q.Z.)the National Natural Science Foundation of China (Grant Nos.12125408,12334004for J.Z.,and 12174363 for Q.Z.)+1 种基金the Innovation Program for Quantum Science and Technology (Grant No.2021ZD0303306 for J.Z.)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB0450101 for J.Z.)。
文摘Electron–hole(e–h)recombination is a fundamental process that governs energy dissipation and device efficiency in semiconductors.In two-dimensional(2D)materials,the formation of tightly bound excitons makes exciton-mediated e–h recombination the dominant decay pathway.In this work,nonradiative e–h recombination within excitons in monolayer MoS2 is investigated using first-principles simulations that combine nonadiabatic molecular dynamics with𝐺𝑊and real-time Bethe–Salpeter equation(BSE)propagation.A two-step process is identified:rapid intervalley redistribution induced by exchange interaction,followed by slower phonon-assisted recombination facilitated by exciton binding.By selectively removing the screened Coulomb and exchange terms from the BSE Hamiltonian,their respective contributions are disentangled—exchange interaction is found to increase the number of accessible recombination pathways,while binding reduces the excitation energy and enhances nonradiative decay.A reduction in recombination lifetime by over an order of magnitude is observed due to the excitonic many-body effects.These findings provide microscopic insights for understanding and tuning exciton lifetimes in 2D transition-metal dichalcogenides.
基金supported by the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(MSIT),South Korea(RS-2024-00421181)financially supported in part by National R&D Program(2021M3H4A3A02086430)through NRF(National Research Foundation of Korea)funded by Ministry of Science and ICT+2 种基金the National Research Council of Science&Technology(NST)grant by the Korea government(MSIT)(No.GTL25021-210)The Inter-University Semiconductor Research Center,Institute of Engineering Research,and Soft Foundry Institute at Seoul National University provided research facilities for this workhe grant by the National Research Foundation of Korea(NSF)supported by the Korea government(MIST)(RS-2025-16903034)。
文摘As silicon-based transistors face fundamental scaling limits,the search for breakthrough alternatives has led to innovations in 3D architectures,heterogeneous integration,and sub-3 nm semiconductor body thicknesses.However,the true effectiveness of these advancements lies in the seamless integration of alternative semiconductors tailored for next-generation transistors.In this review,we highlight key advances that enhance both scalability and switching performance by leveraging emerging semiconductor materials.Among the most promising candidates are 2D van der Waals semiconductors,Mott insulators,and amorphous oxide semiconductors,which offer not only unique electrical properties but also low-power operation and high carrier mobility.Additionally,we explore the synergistic interactions between these novel semiconductors and advanced gate dielectrics,including high-K materials,ferroelectrics,and atomically thin hexagonal boron nitride layers.Beyond introducing these novel material configurations,we address critical challenges such as leakage current and long-term device reliability,which become increasingly crucial as transistors scale down to atomic dimensions.Through concrete examples showcasing the potential of these materials in transistors,we provide key insights into overcoming fundamental obstacles—such as device reliability,scaling down limitations,and extended applications in artificial intelligence—ultimately paving the way for the development of future transistor technologies.
基金supported by the IITP(Institute of Information & Communications Technology Planning & Evaluation)-ITRC(Information Technology Research Center) grant funded by the Korea government(Ministry of Science and ICT) (IITP-2025-RS-2024-00437191, and RS-2025-02303505)partly supported by the Korea Basic Science Institute (National Research Facilities and Equipment Center) grant funded by the Ministry of Education. (No. 2022R1A6C101A774)the Deanship of Research and Graduate Studies at King Khalid University, Saudi Arabia, through Large Research Project under grant number RGP-2/527/46
文摘The growing global energy demand and worsening climate change highlight the urgent need for clean,efficient and sustainable energy solutions.Among emerging technologies,atomically thin two-dimensional(2D)materials offer unique advantages in photovoltaics due to their tunable optoelectronic properties,high surface area and efficient charge transport capabilities.This review explores recent progress in photovoltaics incorporating 2D materials,focusing on their application as hole and electron transport layers to optimize bandgap alignment,enhance carrier mobility and improve chemical stability.A comprehensive analysis is presented on perovskite solar cells utilizing 2D materials,with a particular focus on strategies to enhance crystallization,passivate defects and improve overall cell efficiency.Additionally,the application of 2D materials in organic solar cells is examined,particularly for reducing recombination losses and enhancing charge extraction through work function modification.Their impact on dye-sensitized solar cells,including catalytic activity and counter electrode performance,is also explored.Finally,the review outlines key challenges,material limitations and performance metrics,offering insight into the future development of nextgeneration photovoltaic devices encouraged by 2D materials.
基金supported by Basic Science Research Program(Priority Research Institute)through the NRF of Korea funded by the Ministry of Education(2021R1A6A1A10039823)by the Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Ministry of Education(2020R1A6C101B194)。
文摘Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.
基金the fundamental Research Funds for the central Universities(x2wjD2240360)for the funding supportMeanwhile,Engineering and Physical Sciences Research Council(EPSRC,EP/V027433/3)+2 种基金UK Research and Innovation(UKRI)under the UK government’s Horizon Europe funding(101077226,EP/Y008707/1)Faraday Institution(EP/S003053/1)Degradation project(FIRG001),Royal Society(IEC\NSFC\233361),QUB Agility Fund and Wright Technology and Research Centre(W-Tech,R5240MEE)Funding from UK aid from the UK Government through the Faraday Institution and the Transforming Energy Access Programme(Grant number FIRG050-Device engineering of Zn-based hybrid micro-flow batteries and by-product H2 collection for Emerging Economies)。
文摘Aqueous zinc metal batteries(AZMBs)face significant challenges in achieving reversibility and cycling stability,primarily due to hydrogen evolution reactions(HER)and zinc dendrite growth.In this study,by employing carefully designed cells that approximate the structural characteristics of practical batteries,we revisit this widely held view through in-operando X-ray radiography to examine zinc dendrite formation and HER under nearpractical operating conditions.While conventional understanding emphasizes the severity of these processes,our findings suggest that zinc dendrites and HER are noticeably less pronounced in dense,real-operation configurations compared to modified cells,possibly due to a more uniform electric field and the suppression of triple-phase boundaries.This study indicates that other components,such as degradation at the cathode current collector interface and configuration mismatches within the full cell,may also represent important barriers to the practical application of AZMBs,particularly during the early stages of electrodeposition.
基金funding support from General Research Fund[Project No.14300525]from the Research Grants Council(RGC)of Hong Kong SAR,Chinafunding support from Natural Science Foundation of China(NSFC)Young Scientists Fund(Project No.22305203)+2 种基金NSFC Projects Nos.22309123,22422303,22303011,22033002,92261112 and U21A20328support from the Hong Kong Branch of National Precious Metals Material Engineering Research Center(NPMM)at City University of Hong Kongsupport from Young Collaborative Research Grant[Project No.C1003-23Y]support from RGC of Hong Kong SAR,China.
文摘Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances are far from practical needs due to the lack of efficient electrocatalysts.Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties.Herein,we realize boron(B)-insertion-induced phase regulation of rhodium(Rh)nanocrystals to obtain amorphous Rh_(4)B nanoparticles(NPs)and hexagonal close-packed(hcp)RhB NPs through a facile wet-chemical method.A high Faradaic efficiency(92.1±1.2%)and NH_(3) yield rate(629.5±11.0μmol h^(−1) cm^(−2))are achieved over hcp RhB NPs,far superior to those of most reported NORR nanocatalysts.In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center,enhanced NO adsorption/activation profile,and greatly reduced energy barrier of the rate-determining step.A demonstrative Zn-NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2,realizing simultaneous NO removal,NH3 synthesis,and electricity output.
基金financially supported by the National Natural Science Foundation of China(Nos.22272118,22172111,and 22309134)the Science and Technology Commission of Shanghai Municipality,China(Nos.22ZR1464100,20ZR1460300,and 19DZ2271500)+2 种基金the China Postdoctoral Science Foundation(2022M712402),the Shanghai Rising-Star Program(23YF1449200)the Zhejiang Provincial Science and Technology Project(2022C01182)the Fundamental Research Funds for the Central Universities(2023-3-YB-07)。
文摘Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains a confusing topic.Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures(SCSs)for Zn-ion storage with double-high capacitive activity and durability.Tetrachlorobenzoquinone(H-bond acceptor)and dimethylbenzidine(H-bond donator)can interact to form organic nanosheet modules,which are sequentially assembled,orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds(N-H···O).Featured with rich surface-active heterodiatomic motifs,more exposed nanoporous channels,and successive charge migration paths,SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers(3.3Ωs-0.5).Consequently,the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics,including high energy density(166 Wh kg-1),high-rate performance(172 m Ah g^(-1)at 20 A g^(-1)),and long-lasting cycling lifespan(95.5%capacity retention after 500,000 cycles).An opposite chargecarrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage,involving high-kinetics physical Zn^(2+)/CF_(3)SO_(3)-adsorption and chemical Zn^(2+)redox with carbonyl/pyridine groups.This work gives insights into H-bond-guided interfacial superassembly design of superstructural carbons toward advanced energy storage.
基金The present study has been performed in support of the NSF(Grant No.DMR 1701360),DOE-NNSA(Grant No.DENA0003342),ARO(Grant No.W911NF-17-1-0468),DARPA(Grant No.W31P4Q-12-1-0009),and ADD in Korea.
文摘Recent advances in high-pressure technologies and large-scale experimental and computational facilities have enabled scientists,at an unprecedented rate,to discover and predict novel states and materials under the extreme pressure-temperature conditions found in deep,giant-planet interiors.Based on a well-documented body of work in this field of high-pressure research,we elucidate the fundamental principles that govern the chemistry of dense solids under extreme conditions.These include:(i)the pressure-induced evolution of chemical bonding and structure of molecular solids to extended covalent solids,ionic solids and,ultimately,metallic solids,as pressure increases to the terapascal regime;(ii)novel properties and complex transition mechanisms,arising from the subtle balance between electron hybridization(bonding)and electrostatic interaction(packing)in densely packed solids;and(iii)new dense framework solids with high energy densities,and with tunable properties and stabilities under ambient conditions.Examples are taken primarily fromlow-Z molecular systems that have scientific implications for giant-planet models,condensed materials physics,and solid-state core-electron chemistry.
基金Council of Scientific and Industrial Research(CSIR),New Delhi, INDIA for providing financial asistant in the form of CSIR-Senior Research Fellowship(Award No.09/114/(0179)/2011/ EMR-1)
文摘Present review for the first time provides a complete botanical description and information on ethnomcdicinal uses of Clerodendron glandulosum.Coleb(CG:Fam.Verbenaceae).Recent studies conducted from our laborator) provide pharmacological evidence for its anti-hypertensive,antidiabetic and anti-obesity potentials.Further,its beneficial potential in preventing in vitro and in vivo non-alcoholic steatohepatitis and atherosclerosis and potent hcpatoprotective and free radical scavenging abilities along with its acute and sub- chronic toxicologiesl evaluations are also reported from our laboratory.In keeping with its traditional uses,CG extract was capable of ameliorating experimentally induced hypertension,diabetes and obesity.Its beneficial potential against NASH induced oxidative stress and atherosclerosis can be attributed to its potent free radical scavenging potential.Non—toxic nature of CG leaf extract further provides added merit to its reported pharmacological properties.The present review summarizes the pioneering scientific evidence for the pharmacological effects of CG against related metabolic disorders like hypertension,diabetes and obesity along with anti oxidant potential and beneficial elicits against non alcoholic steatohepatitis.
基金supported by the National Natural Science Foundation of China(grant number 51872157)Shenzhen Technical Plan Project(grant number KQJSCX20160226191136 and JCYJ20170412170911187)Research Grants Council of the Hong Kong Special Administrative Region,China[grant number PF17-10186]。
文摘In nature,the properties of matter are ultimately governed by the electronic structures.Quantum chemistry(QC)at electronic level matches well with a few simple physical assumptions in solving simple problems.To date,machine learning(ML)algorithm has been migrated to this field to simplify calculations and improve fidelity.This review introduces the basic information on universal electron structures of emerging energy materials and ML algorithms involved in the prediction of material properties.Then,the structure-property relationships based on ML algorithm and QC theory are reviewed.Especially,the summary of recently reported applications on classifying crystal structure,modeling electronic structure,optimizing experimental method,and predicting performance is provided.Last,an outlook on ML assisted QC calculation towards identifying emerging energy materials is also presented.
基金Supported by Natural Science Foundation of Hunan Province(No.13JJ3112)Scientific & Technological Projects of Hunan Province(No.2013TZ2025,2014NK3086)+3 种基金Open Foundation of Innovation Platform of Hunan Provincial University(No.13K105,14K014)Scientific & Technological Projects of Hengyang City(No.2012KJ30)Cultivation projects Based on Collaborative Innovation Center of Hengyang Normal University(No.12XT02)the Youth Backbone Teacher Training Program of Hengyang Normal University(2012)
文摘Two dinuclear organotin complexes C8H14（CO2SnCy3）2（1）（Cy = cyclohexyl group） and C8H14[CO2Sn（CH2CMe2Ph）3]2（2） were synthesized by the reactions of camphoric acid with tricyclohexyltin hydroxide and bis[tri（2-methyl-2-phenyl）propyltin] oxide under solvothermal conditions, and these complexes were characterized by infrared spectra, elemental analyses, and H NMR spectra. The crystal of 1 belongs to the monoclinic system, space group P21/c with a = 1.83478（19）, b = 1.52707（18）, c = 1.9849（2） nm, β = 122.515（7）°, Z = 4, V = 4.6896（9） nm^3, Dc = 1.324 g/cm^3, μ（MoKα） = 1.103 mm^-1, F（000） = 1952, R = 0.0697 and wR = 0.2040. In addition, thermal stability and quantum chemical calculation of 1 were also studied.
基金Supported by the National Natural Science Foundation of China(No. 29703003).
文摘The geometries of imidazole and its derivatives were respectively optimized by using ab initio method, and the molecular orbital energy levels and the charge densities were obtained for their optimum geometries. The frontier orbital energy levels, and the net charges of N (1) atom and the imidazole ring of those molecules were obtained with ab initio and SCC-DV-Xα methods. It was found that the inhibition properties of those compounds change with the highest occupied molecular orbital energy levels, and the net charges of N (1) atom. We took four iron atoms on the crystal plane (100) of α-iron as the surface which was used to study the adsorption towards the inhibitors. The adsorption models of the inhibitor to be adsorbed on the Fe-cluster surface were optimized with SCC-DV-Xα method. It turns out that the most favorable model is that the inhibitor molecule is adsorbed on the Fe-cluster surface in an inclined state. The calculation shows that the stabilization energies of the systems are well correlated with the inhibition efficiencies.
