The remarkable power of chemistry over description and trans-formation of matters has been significantly enhanced through the development of dynamic chemistry and condensed matter chemistry[1].This progress has furthe...The remarkable power of chemistry over description and trans-formation of matters has been significantly enhanced through the development of dynamic chemistry and condensed matter chemistry[1].This progress has further elevated chemistry to a creative science and a thriving industry.The development of dynamic chemistry,span-ning from supramolecular chemistry to constitutional dynamic chem-istry,has witnessed significant advancements towards adaptive chemistry,which is characterized primarily by its self-adaption to external stimuli.This is particularly achieved in two-or three-dimensional dynamic frameworks.Meanwhile,the multi-phase evolution resulting from the emerging of solid-to-liquid transition plat-form is assuming an increasingly crucial role in condensed matter chemistry[2].展开更多
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 preparation,functionalization,and investigations in host-vip properties of high-level pillararene macrocycles have long been a big challenge because of the lack of efficient synthetic methods.Herein,a novel type...The preparation,functionalization,and investigations in host-vip properties of high-level pillararene macrocycles have long been a big challenge because of the lack of efficient synthetic methods.Herein,a novel type of pillararene derivative,namely desymmetrized pillar[8]arene(DP[8]A),has been successfully synthesized via a facile two-step strategy with high yield.Compared with its pillar[8]arene counterpart,DP[8]A is composed of four alkoxy-substituted benzene units and four bare benzene rings.Single crystal analysis has been performed in order to unveil the molecular conformation and packing mode of DP[8]A,which indicated that DP[8]A possesses a unique chair-like structure and much smaller steric hindrance.Density functional theory(DFT)calculations and electrostatic potential map suggested the inhomogeneous electronic distribution in the DP[8]A cavity.Water-soluble carboxylate-modified DP[8]A,that is,CDP[8]A,was also prepared to investigate the host-vip properties in aqueous solution with methyl viologen(MV),where the binding constant and morphologies of the formed host-vip complexes have been studied.In all,this new version of eight-membered pillararene derivative might potentially serve as a powerful macrocycle candidate for further applications in supramolecular chemistry.展开更多
Metal-carbon dioxide(CO_(2))batteries hold great promise for reducing greenhouse gas emissions and are regarded as one of the most promising energy storage techniques due to their efficiency advantages in CO_(2)recove...Metal-carbon dioxide(CO_(2))batteries hold great promise for reducing greenhouse gas emissions and are regarded as one of the most promising energy storage techniques due to their efficiency advantages in CO_(2)recovery and conversion.Moreover,rechargeable nonaqueous metal-CO_(2)batteries have attracted much attention due to their high theoretical energy density.However,the stability issues of the electrode-electrolyte interfaces of nonaqueous metal-CO_(2)(lithium(Li)/sodium(Na)/potassium(K)-CO_(2))batteries have been troubling its development,and a large number of related research in the field of electrolytes have conducted in recent years.This review retraces the short but rapid research history of nonaqueous metal-CO_(2)batteries with a detailed electrochemical mechanism analysis.Then it focuses on the basic characteristics and design principles of electrolytes,summarizes the latest achievements of various types of electrolytes in a timely manner and deeply analyzes the construction strategies of stable electrode-electrolyte interfaces for metal-CO_(2)batteries.Finally,the key issues related to electrolytes and interface engineering are fully discussed and several potential directions for future research are proposed.This review enriches a comprehensive understanding of electrolytes and interface engineering toward the practical applications of next-generation metal-CO_(2)batteries.展开更多
Graphite-silicon species(Gr-Si)hybrid anodes have merged as potential candidates for high-energy lithium-ion batteries(LIBs),yet long been plagued by rapid capacity fading due to their unstable mechano-electrochemistr...Graphite-silicon species(Gr-Si)hybrid anodes have merged as potential candidates for high-energy lithium-ion batteries(LIBs),yet long been plagued by rapid capacity fading due to their unstable mechano-electrochemistry.The dominant approach to enhance electrochemical stability of the Gr-Si hybrid anodes typically involves the optimization of the electrode material structures and the employment of low active Si species content in electrode(<10 wt%in most instances).However,the electrode structure design,a factor of equal importance in determining the electrochemical performance of Gr-Si hybrid anodes,has received scant attention.In this study,three Gr-Si hybrid anodes with the identical material composition but distinct electrode structures are designed to investigate the mechanoelectrochemistry of the electrodes.It is revealed that the substantial volume change of Si species particles in Gr-Si hybrid anodes led to the local lattice stress of Gr at their contact interface during the charge/discharge processes,thereby increasing thermodynamic and kinetic barrier of Li-ion migration.Furthermore,the huge disparity in volume change of Si species and Gr particles trigger the separate agglomeration of these two materials,resulting in a considerable electrode volume change and increased electrochemical resistance.An advanced Gr/Si hybrid anode with upper Gr and lower Si species layer structure design addresses the above challenges using photovoltaic waste silicon sources under high Si species content(17 wt%)and areal capacity(2.0 mA h cm^(-2))in Ah-level full pouch cells with a low negative/positive(N/P)ratio of 1.09.The cell shows stable cycling for 100 cycles at 0.3 C with an impressively low capacity decay rate of 0.0546%per cycle,outperforming most reported Gr-Si hybrid anodes.展开更多
Erigerontis Herba(EH),the dried whole plant of Erigeron breviscapus,is well-known for circulating blood,activating meridians to alleviate pain,expelling wind,and clearing away cold.It has been extensively utilized in ...Erigerontis Herba(EH),the dried whole plant of Erigeron breviscapus,is well-known for circulating blood,activating meridians to alleviate pain,expelling wind,and clearing away cold.It has been extensively utilized in southern China for the treatment of stroke hemiplegia,chest stuffiness and pains,rheumatic arthralgia,headache,and toothache.This review focuses on the botany,ethnopharmacology,phytochemistry,pharmacology and toxicity of EH and its related prescriptions to offer new insights for prospective research of EH.Relevant information about EH was retrieved from ancient records and books,PubMed,China National Knowledge Infrastructure,Chinese Pharmacopoeia,Web of Science,Doctoral and Master’s Theses,and various electronic databases.EH is a member of Compositae family and is mainly grown in southern China.Traditional Chinese medicine records that EH has the effects of circulating blood and removing blood stasis,expelling wind,and removing cold,as well as relieving rigidity of muscle and relieving pain.By now,nearly 200 ingredients have been characterized from EH,including flavonoids,caffeoyls,aromatic acids,coumarins,pentacyclic terpenoids,volatile oil and other compounds.EH extracts,EH related prescriptions(Dengzhan Xixin injection,Dengzhan Shengmai capsules,etc.)or compounds(scutellarin,scutellarein,etc.)possessed obvious therapeutic effects of ischemic stroke,cerebral hemorrhage,myocardial infarction,Alzheimer’s disease,diabetes and its complications,gastric cancer,bone,and joint degenerative diseases.Scutellarin,the major active compound of EH,has been used as a quality marker.And no obvious toxicity of EH has been reported.According to its traditional applications,ethnopharmacology,phytochemistry,pharmacology,and toxicity,EH was applied as a valuable herb for clinical application in food and medicine fields.While several compounds have been shown to possess diverse biological activities,the underlying mechanisms of their actions remain elusive.To fully exploit the medicinal potential of EH,further studies on understanding the effective material basis and mechanisms are warranted.展开更多
The disconnection between teaching,learning,and evaluation is particularly pronounced in traditional high school chemistry teaching.To align with the demands of the new curriculum standards for talent development,it i...The disconnection between teaching,learning,and evaluation is particularly pronounced in traditional high school chemistry teaching.To align with the demands of the new curriculum standards for talent development,it is essential to implement reforms and innovations in teaching methods.This paper initially elucidates the integrated concept of teaching,learning,and evaluation,as well as its practical significance in the classroom.Subsequently,it explores the effective teaching design centered on the theme of iron and its compounds,actively investigating the implementation approach of the integration principle of teaching,learning,and evaluation in classroom.Furthermore,the paper emphasizes the pivotal role of the evaluation part in fostering the professional development of teachers and enhancing the core competencies of students,ultimately aiming to achieve high efficiency and quality in chemistry classroom teaching.展开更多
Directly occluding polymer nanoparticles into growing host crystals provides a versatile pathway for synthe sizing polymer-inorganic composite crystals,where vip nanoparticles are distributed within the crystal matr...Directly occluding polymer nanoparticles into growing host crystals provides a versatile pathway for synthe sizing polymer-inorganic composite crystals,where vip nanoparticles are distributed within the crystal matrix.However,systematically controlling the extent of nanoparticle occlusion within a host crystal remains a significant challenge.In this study,we employ a one-step,soap-free emulsion polymerization method to synthesize polyethyleneimine-functionalized poly(tert-butyl methacrylate)(PtBMA/PEI)nanoparticles.These cationic nanoparticles are subsequently modified using formaldehyde to systematically tune the content of surface amine group via the Eschweiler-Clarke reaction.This approach yields a series of model nanoparticles that allow us to investigate how surface chemistry influences the extent of nanoparticle occlusion within calcite crystals.Our findings reveal that the extent of nanoparticle occlusion within calcite crystals is proportional to the surface amine group content.This study offers a new design rule for creating composite crystals with tailored compositions through a nanoparticle occlusion strategy.展开更多
Natural enzymes are able to precisely bind substrates and catalyze activities because of their distinct framework structures.To mimic this ability,chemists are designing framework structures that resemble real enzymes...Natural enzymes are able to precisely bind substrates and catalyze activities because of their distinct framework structures.To mimic this ability,chemists are designing framework structures that resemble real enzymes.The use of metal-organic frameworks(MOFs)to mimic natural enzymes has advanced recently;this paper reviews these developments.This research specifically focuses on how the catalytically active center of natural enzymes can be exactly replicated by carefully controlling the composition and structure of MOFs.By identifying and attaching to substrates,MOFs can accelerate changes in a manner akin to that of real enzymes.The role of MOFs in simulating catalytic processes,enzyme activity,and potential uses in brain chemistry are also investigated in this work.It also discusses the most recent MOF applications in detecting and treating chemical abnormalities of the brain.The report finishes with a discussion of future research areas and potential applications,providing useful insights for researchers in the subject.展开更多
In chemical science,the vertical ionization potential(VIP)is a crucial metric for understanding the electronegativity,hardness and softness of chemical material systems as well as the electronic structure and stabilit...In chemical science,the vertical ionization potential(VIP)is a crucial metric for understanding the electronegativity,hardness and softness of chemical material systems as well as the electronic structure and stability of molecules.Ever since the last century,the model chemistry composite methods have witnessed tremendous developments in computing the thermodynamic properties as well as the barrier heights.However,their performance in realm of the vertical electron processes of molecular systems has been rarely explored.In this study,we for the first time benchmarked the model chemistry composite methods(e.g.,CBS-QB3,G4 and W1BD)in comparison with the commonly used Koopmans's theorem(KT),electron propagator theory(e.g.,OVGF,D2,P3 and P3+)and CCSD(T)methods in calculating the VIP for up to 613 molecular systems with available experimental measurements.The large-scale test calculations strongly showed that the CBS-QB3 model chemistry composite technique can be well recommended to calculate VIP from the perspectives of accuracy,economy and applicability.Notably,the VIP values of up to 7 molecules were identified to have the absolute errors of larger than 0.3 e V at all calculation levels,which have strong hints that their VIP experimental values should be re-investigated.展开更多
Electrolytes are crucial components in electrochemical energy storage devices,sparking considerable research interest.However,the significance of anions in the electrolytes is often underestimated.In fact,the anions h...Electrolytes are crucial components in electrochemical energy storage devices,sparking considerable research interest.However,the significance of anions in the electrolytes is often underestimated.In fact,the anions have significant impacts on the performance and stability of lithium batteries.Therefore,comprehensively understanding anion chemistry in electrolytes is of crucial importance.Herein,indepth comprehension of anion chemistry and its positive effects on the interface,solvation structure of Li-ions,as well as the electrochemical performance of the batteries have been emphasized and summarized.This review aims to present a full scope of anion chemistry and furnish systematic cognition for the rational design of advanced electrolytes for better lithium batteries with high energy density,lifespan,and safety.Furthermore,insightful analysis and perspectives based on the current research are proposed.We hope that this review sheds light on new perspectives on understanding anion chemistry in electrolytes.展开更多
Rechargeable aqueous Zn-MoO_(x)batteries are promising energy storage devices with high theoretical specific capacity and low cost.However,MoO_(3)cathodes suffer drastic capacity decay during the initial discharging/c...Rechargeable aqueous Zn-MoO_(x)batteries are promising energy storage devices with high theoretical specific capacity and low cost.However,MoO_(3)cathodes suffer drastic capacity decay during the initial discharging/charging process in conventional electrolytes,resulting in a short cycle life and challenging the development of Zn-MoO_(x)batteries.Here we comprehensively investigate the dissolution mechanism of MoO_(3)cathodes and innovatively introduce a polymer to inhibit the irreversible processes.Our findings reveal that this capacity decay originates from the irreversible Zn^(2+)/H^(+)co-intercalation/extraction process in aqueous electrolytes.Even worse,during Zn^(2+)intercalation,the formed Zn_(x)MoO_(3-x)intermediate phase with lower valence states(Mo^(5+)/Mo^(4+))experiences severe dissolution in aqueous environments.To address these challenges,we developed a first instance of coating a polyaniline(PANI)shell around the MoO_(3)nanorod effectively inhibiting these irreversible processes and protecting structural integrity during long-term cycling.Detailed structural analysis and theoretical calculations indicate that=N-groups in PANI@MoO_(3-x)simultaneously weaken H+adsorption and enhance Zn^(2+)adsorption,which endowed the PANI@MoO_(3-x)cathode with reversible Zn^(2+)/H^(+)intercalation/extraction.Consequently,the obtained PANI@MoO_(3-x)cathode delivers an excellent discharge capacity of 316.86 mA h g^(-1)at 0.1 A g^(-1)and prolonged cycling stability of 75.49%capacity retention after 1000 cycles at 5 A g^(-1).This work addresses the critical issues associated with MoO_(3)cathodes and significantly advances the understanding of competitive multi-ion energy storage mechanisms in aqueous Zn-MoO_(3)batteries.展开更多
This study investigates the distribution and imbalances of research funding in the field of Environmental Chemistry,utilizing application and funding data fromthe National Natural Science Foundation of China(NSFC)over...This study investigates the distribution and imbalances of research funding in the field of Environmental Chemistry,utilizing application and funding data fromthe National Natural Science Foundation of China(NSFC)over the past decade.The findings reveal significant regional disparities,with Eastern regions receiving over 70%of the national funding,while the Northeast accounts for only 4%to 6.5%.Additionally,the analysis shows notable differences in funding allocation among various research institutions,with a substantial portion of funds concentrated in a few leading institutions,leading to inequities across different types and levels of organizations.The impact of applicant gender on funding disparities is relatively minor;although female applicants have a slightly lower funding rate,the concentration of funds is marginally higher among females.Furthermore,the study highlights that key projects and talent-oriented initiatives,due to their significant funding concentration,exacerbate the existing imbalances.Overall,this research provides valuable insights for optimizing funding policies and advocates for a more equitable distribution of resources in Environmental Chemistry research,addressing the identified disparities.展开更多
NASICON type solid electrolyte Li_(1+x)Al_(x)Ge_(2-x)(PO_(4))_(3)(LAGP)is one of the most potential candidates in view of their high ionic conductivity,high oxidation resistance and excellent air stability.However,ine...NASICON type solid electrolyte Li_(1+x)Al_(x)Ge_(2-x)(PO_(4))_(3)(LAGP)is one of the most potential candidates in view of their high ionic conductivity,high oxidation resistance and excellent air stability.However,inevitable interface issues often cause severe performance degradation,seriously affecting its commercial application.Herein,a lithiophilic carbon buffer layer is constructed on the LAGP surface adjacent to the Li electrode side by a facile pyrolysis reaction,then the LiC_(x) interlayer is generated in situ between the carbon buffer layer and lithium metal,which can guide uniform ion transport while improving interface contact.Thus,the LiC_(x)-LAGP showed excellent ionic conductivity,high flexibility and lithiophilic interphase.Specially,the Li|LiC_(x)-LAGP|Li battery has achieved a 1000 h stable cycles at 0.1 mA/cm^(2),remarkably,the Li|LiC_(x)-LAGP|LFP battery retains 85%of their initial capacity after 200 cycles under 1 C,even for the NCM811 cathode,the battery still has a good cycle performance.展开更多
A comprehensive examination of detrital sandstone modes from the Sylhet Trough reveals a diverse range of sub-lithic to sub-feldspathic quartz arenites.Soil samples were gathered from Dupi Gaon(Jaintiapur)in Banglades...A comprehensive examination of detrital sandstone modes from the Sylhet Trough reveals a diverse range of sub-lithic to sub-feldspathic quartz arenites.Soil samples were gathered from Dupi Gaon(Jaintiapur)in Bangladesh,followed by a thorough analysis using field examination,X-ray diffraction(XRD),X-ray fluorescence(XRF),petrography,and heavy mineral concentration analyses.Field observations revealed the soil sample varying from white to yellowish to variegated,with thicknesses ranging from 15 cm to about 4 m,and exhibiting moderate softness.XRF analysis revealed significant SiO_(2),Al_(2)O_(3),and Fe_(2)O_(3)levels in the samples,with zirconium(Zr)and copper(Cu)showing consistently high concentrations.XRD analysis identified quartz as predominant,along with muscovite,biotite,and accessory minerals like rutile and magnetite.Petrographic analysis highlighted quartz as dominant,with fractures suggesting tectonic influences,while heavy mineral separation techniques identified zircon,garnet,goethite,rutile,and magnetite.These findings provide insights into sediment provenance,depositional processes,and environ-mental conditions during the formation of the Dupi Tila Formation.The comprehensive geochemical data of the entire rock indicates that most of the sediments originated from felsic igneous sources,and also suggests a moderate to high level of weathering in the source region.Overall,the analyses suggested an in situ origin of the Dupi Tila Formation,with parent materials being predominantly detrital rather than authigenic,supported by the presence of detrital quartz and an assessment of the depositional environment,providing insights into the geological conditions of the era and potential modes of sediment transportation.展开更多
Surface with well-defined components and structures possesses unique electronic,magnetic,optical and chemical properties.As a result,surface chemistry research plays a crucial role in various fields such as catalysis,...Surface with well-defined components and structures possesses unique electronic,magnetic,optical and chemical properties.As a result,surface chemistry research plays a crucial role in various fields such as catalysis,energy,materials,quantum,and microelectronics.Surface science mainly investigates the correspondence between surface property and functionality.Scanning probe microscopy(SPM)techniques are important tools to characterize surface properties because of the capability of atomic-scale imaging,spectroscopy and manipulation at the single-atom level.In this review,we summarize recent advances in surface electronic,magnetic and optical properties characterized mainly by SPM-based methods.We focus on elucidating theπ-magnetism in graphene-based nanostructures,construction of spin qubits on surfaces,topology properties of surface organic structures,STM-based light emission,tip-enhanced Raman spectroscopy and integration of machine learning in SPM studies.展开更多
Most carbon-based catalysts utilized in Fenton-like systems face challenges such as structural instability,susceptibility to deactivation,and a tendency to disperse during operation.Wood-derived catalysts have garnere...Most carbon-based catalysts utilized in Fenton-like systems face challenges such as structural instability,susceptibility to deactivation,and a tendency to disperse during operation.Wood-derived catalysts have garnered considerable attention due to their well-defined structures,extensive pipeline networks,superior mechanical strength,and adaptability for device customization.However,there remains a paucity of research that systematically summarizes Fenton-like systems based on wood-derived catalysts.In this review,we first summarize the structural designs of wood-derived catalysts based on nano-metal sites and single-atom sites,while also outlining their advantages and limitations applied in Fenton-like systems.Furthermore,we evaluate catalytic modules of wood-derived catalysts for scale-up and continuous Fenton-like systems.Additionally,wood-inspired catalytic materials utilizing commercial textures and their applications in Fenton-like processes are also discussed.This paper aims to comprehensively explore the fundamental mechanisms(e.g.,characteristics of catalytic sites,catalytic performance,and mechanisms)of wood-based catalysts in Fenton-like chemistry,as well as their equipment designs and application scenarios,as well as providing the insights into future developments.展开更多
Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution reaction.The surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has ...Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution reaction.The surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity enhancement.Here,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is reported.The substituting Fe content influences both current change tendency and surface reconstruction degree.LaNi_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)series.The reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based catalysts.Besides,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term stability.Furthermore,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction degree.The effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface reconstruction.This finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.展开更多
Low-temperature lithium sulfur(Li-S)batteries have attracted increasing attention,but lithium polysulfide(LiPSs)clu stering and tardy ionic mobility have been challenging issues,which could be exacerbated under high s...Low-temperature lithium sulfur(Li-S)batteries have attracted increasing attention,but lithium polysulfide(LiPSs)clu stering and tardy ionic mobility have been challenging issues,which could be exacerbated under high sulfur loading and lean electrolyte.The distinct behaviors of sulfur cathode in lowtemperature Li-S batteries call for special regulations of the sulfur host to improve the electrochemical performances.Here,a three-dimensional Ti_(3)C_(2)micro-cage(TCC)with an interfacial structure modulated by rich curvatures has been fabricated to propel the sulfur electrochemistry at subzero temperatures.Spectroscopic/microscopic analyses and theoretical calculations elucidate that the precipitation of ultrafine Ti-metal particles on the in-situ generated Ti_(3)C_(2)nanoribbons could trigger the self-scrolling of Ti_(3)C_(2)nanoribbons into TCC.Moreover,in-situ ultraviolet-visible spectra collected at low temperature and theoretical calculations verified that the TCC regulated by rich curvatures have effectively alleviated the Li+dissociation barrier,reduced the energy barrier for charge transfer at the electrode-electrolyte interface,and restrained the clustering and shuttling of LiPSs,thus accelerating the electrochemical conversion kinetics of sulfur species at low temperatures.The performances of the carbon-free TCC-S cathode at low temperatures have been also compared from the aspects of cathode configuration and measurement condition,to demonstrate the potential of TCC.This work can not only provide new methodology for regulating the interfacial structure of MXene to enrich the materials library for low-temperature Li-S batteries,but also expand understanding about the role of interfacial structure of sulfur host in Li-S batteries.展开更多
Aqueous batteries with metal anodes exhibit robust anodic capacities,but their energy densities are low because of the limited potential stabilities of aqueous electrolyte solutions.Current metal options,such as Zn an...Aqueous batteries with metal anodes exhibit robust anodic capacities,but their energy densities are low because of the limited potential stabilities of aqueous electrolyte solutions.Current metal options,such as Zn and Al,pose a dilemma:Zn lacks a sufficiently low redox potential,whereas Al tends to be strongly oxidized in aqueous environments.Our investigation introduces a novel rechargeable aqueous battery system based on Mn as the anode.We examine the effects of anions,electrolyte concentration,and diverse cathode chemistries.Notably,the ClO_(4)-based electrolyte solution exhibits improved deposition and dissolution efficiencies.Although stainless steel(SS 316 L)and Ni are stable current collectors for cathodes,they display limitations as anodes.However,using Ti as the anode resulted in increased Mn deposition and dissolution efficiencies.Moreover,we evaluate this system using various cathode materials,including Mn-intercalation-based inorganic(Ag0.33V2O5)and organic(perylenetetracarboxylic dianhydride)cathodes and an anionintercalation-chemistry(coronene)-based cathode.These configurations yield markedly higher output potentials compared to those of Zn metal batteries,highlighting the potential for an augmented energy density when using an Mn anode.This study outlines a systematic approach for use in optimizing metal anodes in Mn metal batteries,unlocking novel prospects for Mn-based batteries with diverse cathode chemistries.展开更多
基金the BAGUI talent program(No.2019AC26001)the National Natural Science Foundation of China(Nos.U23A2080,22371173,22171075).
文摘The remarkable power of chemistry over description and trans-formation of matters has been significantly enhanced through the development of dynamic chemistry and condensed matter chemistry[1].This progress has further elevated chemistry to a creative science and a thriving industry.The development of dynamic chemistry,span-ning from supramolecular chemistry to constitutional dynamic chem-istry,has witnessed significant advancements towards adaptive chemistry,which is characterized primarily by its self-adaption to external stimuli.This is particularly achieved in two-or three-dimensional dynamic frameworks.Meanwhile,the multi-phase evolution resulting from the emerging of solid-to-liquid transition plat-form is assuming an increasingly crucial role in condensed matter chemistry[2].
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.
基金the Natural Science Foundation of Jilin Province(No.20230101052JC)he National Natural Science Foundation of China(Nos.52173200 and 52203138)the Jilin Province Science and Technology Development Plan Project(No.#YDZJ202201ZYTS523)for financial support。
文摘The preparation,functionalization,and investigations in host-vip properties of high-level pillararene macrocycles have long been a big challenge because of the lack of efficient synthetic methods.Herein,a novel type of pillararene derivative,namely desymmetrized pillar[8]arene(DP[8]A),has been successfully synthesized via a facile two-step strategy with high yield.Compared with its pillar[8]arene counterpart,DP[8]A is composed of four alkoxy-substituted benzene units and four bare benzene rings.Single crystal analysis has been performed in order to unveil the molecular conformation and packing mode of DP[8]A,which indicated that DP[8]A possesses a unique chair-like structure and much smaller steric hindrance.Density functional theory(DFT)calculations and electrostatic potential map suggested the inhomogeneous electronic distribution in the DP[8]A cavity.Water-soluble carboxylate-modified DP[8]A,that is,CDP[8]A,was also prepared to investigate the host-vip properties in aqueous solution with methyl viologen(MV),where the binding constant and morphologies of the formed host-vip complexes have been studied.In all,this new version of eight-membered pillararene derivative might potentially serve as a powerful macrocycle candidate for further applications in supramolecular chemistry.
基金supports from the Beijing Laboratory of New Energy Storage Technology, North China Electric Power Universitythe Program of the National Energy Storage Industry-Education Platformthe Interdisciplinary Innovation Program of North China Electric Power University (No. XM2212315)
文摘Metal-carbon dioxide(CO_(2))batteries hold great promise for reducing greenhouse gas emissions and are regarded as one of the most promising energy storage techniques due to their efficiency advantages in CO_(2)recovery and conversion.Moreover,rechargeable nonaqueous metal-CO_(2)batteries have attracted much attention due to their high theoretical energy density.However,the stability issues of the electrode-electrolyte interfaces of nonaqueous metal-CO_(2)(lithium(Li)/sodium(Na)/potassium(K)-CO_(2))batteries have been troubling its development,and a large number of related research in the field of electrolytes have conducted in recent years.This review retraces the short but rapid research history of nonaqueous metal-CO_(2)batteries with a detailed electrochemical mechanism analysis.Then it focuses on the basic characteristics and design principles of electrolytes,summarizes the latest achievements of various types of electrolytes in a timely manner and deeply analyzes the construction strategies of stable electrode-electrolyte interfaces for metal-CO_(2)batteries.Finally,the key issues related to electrolytes and interface engineering are fully discussed and several potential directions for future research are proposed.This review enriches a comprehensive understanding of electrolytes and interface engineering toward the practical applications of next-generation metal-CO_(2)batteries.
基金the financial support by the National Natural Science Foundation of China(52072137)the National Natural Science Foundation of China(22205068)the"CUG Scholar"Scientific Research Funds at China University of Geosciences(Wuhan)(2022118)。
文摘Graphite-silicon species(Gr-Si)hybrid anodes have merged as potential candidates for high-energy lithium-ion batteries(LIBs),yet long been plagued by rapid capacity fading due to their unstable mechano-electrochemistry.The dominant approach to enhance electrochemical stability of the Gr-Si hybrid anodes typically involves the optimization of the electrode material structures and the employment of low active Si species content in electrode(<10 wt%in most instances).However,the electrode structure design,a factor of equal importance in determining the electrochemical performance of Gr-Si hybrid anodes,has received scant attention.In this study,three Gr-Si hybrid anodes with the identical material composition but distinct electrode structures are designed to investigate the mechanoelectrochemistry of the electrodes.It is revealed that the substantial volume change of Si species particles in Gr-Si hybrid anodes led to the local lattice stress of Gr at their contact interface during the charge/discharge processes,thereby increasing thermodynamic and kinetic barrier of Li-ion migration.Furthermore,the huge disparity in volume change of Si species and Gr particles trigger the separate agglomeration of these two materials,resulting in a considerable electrode volume change and increased electrochemical resistance.An advanced Gr/Si hybrid anode with upper Gr and lower Si species layer structure design addresses the above challenges using photovoltaic waste silicon sources under high Si species content(17 wt%)and areal capacity(2.0 mA h cm^(-2))in Ah-level full pouch cells with a low negative/positive(N/P)ratio of 1.09.The cell shows stable cycling for 100 cycles at 0.3 C with an impressively low capacity decay rate of 0.0546%per cycle,outperforming most reported Gr-Si hybrid anodes.
基金funded by the State Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources(Guangxi Normal University)(CMEMR2022-B11)the Natural Science Research of Jiangsu Higher education Institution of China(22KJB360018)Jiangsu Province University Student Innovation and Entrepreneurial Training Program(202311117019Z).
文摘Erigerontis Herba(EH),the dried whole plant of Erigeron breviscapus,is well-known for circulating blood,activating meridians to alleviate pain,expelling wind,and clearing away cold.It has been extensively utilized in southern China for the treatment of stroke hemiplegia,chest stuffiness and pains,rheumatic arthralgia,headache,and toothache.This review focuses on the botany,ethnopharmacology,phytochemistry,pharmacology and toxicity of EH and its related prescriptions to offer new insights for prospective research of EH.Relevant information about EH was retrieved from ancient records and books,PubMed,China National Knowledge Infrastructure,Chinese Pharmacopoeia,Web of Science,Doctoral and Master’s Theses,and various electronic databases.EH is a member of Compositae family and is mainly grown in southern China.Traditional Chinese medicine records that EH has the effects of circulating blood and removing blood stasis,expelling wind,and removing cold,as well as relieving rigidity of muscle and relieving pain.By now,nearly 200 ingredients have been characterized from EH,including flavonoids,caffeoyls,aromatic acids,coumarins,pentacyclic terpenoids,volatile oil and other compounds.EH extracts,EH related prescriptions(Dengzhan Xixin injection,Dengzhan Shengmai capsules,etc.)or compounds(scutellarin,scutellarein,etc.)possessed obvious therapeutic effects of ischemic stroke,cerebral hemorrhage,myocardial infarction,Alzheimer’s disease,diabetes and its complications,gastric cancer,bone,and joint degenerative diseases.Scutellarin,the major active compound of EH,has been used as a quality marker.And no obvious toxicity of EH has been reported.According to its traditional applications,ethnopharmacology,phytochemistry,pharmacology,and toxicity,EH was applied as a valuable herb for clinical application in food and medicine fields.While several compounds have been shown to possess diverse biological activities,the underlying mechanisms of their actions remain elusive.To fully exploit the medicinal potential of EH,further studies on understanding the effective material basis and mechanisms are warranted.
文摘The disconnection between teaching,learning,and evaluation is particularly pronounced in traditional high school chemistry teaching.To align with the demands of the new curriculum standards for talent development,it is essential to implement reforms and innovations in teaching methods.This paper initially elucidates the integrated concept of teaching,learning,and evaluation,as well as its practical significance in the classroom.Subsequently,it explores the effective teaching design centered on the theme of iron and its compounds,actively investigating the implementation approach of the integration principle of teaching,learning,and evaluation in classroom.Furthermore,the paper emphasizes the pivotal role of the evaluation part in fostering the professional development of teachers and enhancing the core competencies of students,ultimately aiming to achieve high efficiency and quality in chemistry classroom teaching.
基金financial supports from the National Natural Science Foundation of China(Nos.22475084 and 22101100)Guangdong Basic and Applied Basic Research Foundation(Nos.2024A1515012114 and 2025A1515012931)College Students’Innovation and Entrepreneurship Training Program.
文摘Directly occluding polymer nanoparticles into growing host crystals provides a versatile pathway for synthe sizing polymer-inorganic composite crystals,where vip nanoparticles are distributed within the crystal matrix.However,systematically controlling the extent of nanoparticle occlusion within a host crystal remains a significant challenge.In this study,we employ a one-step,soap-free emulsion polymerization method to synthesize polyethyleneimine-functionalized poly(tert-butyl methacrylate)(PtBMA/PEI)nanoparticles.These cationic nanoparticles are subsequently modified using formaldehyde to systematically tune the content of surface amine group via the Eschweiler-Clarke reaction.This approach yields a series of model nanoparticles that allow us to investigate how surface chemistry influences the extent of nanoparticle occlusion within calcite crystals.Our findings reveal that the extent of nanoparticle occlusion within calcite crystals is proportional to the surface amine group content.This study offers a new design rule for creating composite crystals with tailored compositions through a nanoparticle occlusion strategy.
基金financially supported by the National Natural Science Foundation,China(Nos.22074095&22374103(Y.Lin))Beijing Natural Science Foundation(No.2222005(Y.Lin))。
文摘Natural enzymes are able to precisely bind substrates and catalyze activities because of their distinct framework structures.To mimic this ability,chemists are designing framework structures that resemble real enzymes.The use of metal-organic frameworks(MOFs)to mimic natural enzymes has advanced recently;this paper reviews these developments.This research specifically focuses on how the catalytically active center of natural enzymes can be exactly replicated by carefully controlling the composition and structure of MOFs.By identifying and attaching to substrates,MOFs can accelerate changes in a manner akin to that of real enzymes.The role of MOFs in simulating catalytic processes,enzyme activity,and potential uses in brain chemistry are also investigated in this work.It also discusses the most recent MOF applications in detecting and treating chemical abnormalities of the brain.The report finishes with a discussion of future research areas and potential applications,providing useful insights for researchers in the subject.
基金funded by the National Natural Science Foundation of China(Nos.22073069,21773082)Science Research Project of Hebei Education Department(No.QN2024255)。
文摘In chemical science,the vertical ionization potential(VIP)is a crucial metric for understanding the electronegativity,hardness and softness of chemical material systems as well as the electronic structure and stability of molecules.Ever since the last century,the model chemistry composite methods have witnessed tremendous developments in computing the thermodynamic properties as well as the barrier heights.However,their performance in realm of the vertical electron processes of molecular systems has been rarely explored.In this study,we for the first time benchmarked the model chemistry composite methods(e.g.,CBS-QB3,G4 and W1BD)in comparison with the commonly used Koopmans's theorem(KT),electron propagator theory(e.g.,OVGF,D2,P3 and P3+)and CCSD(T)methods in calculating the VIP for up to 613 molecular systems with available experimental measurements.The large-scale test calculations strongly showed that the CBS-QB3 model chemistry composite technique can be well recommended to calculate VIP from the perspectives of accuracy,economy and applicability.Notably,the VIP values of up to 7 molecules were identified to have the absolute errors of larger than 0.3 e V at all calculation levels,which have strong hints that their VIP experimental values should be re-investigated.
基金supported by National Key Research and Development Program of China(2022YFB2402200)the China Postdoctoral Science Foundation(grant nos.2023T160591)the Joint Fund of the Technical R&D Program of Henan Province(grant nos.232301420044).
文摘Electrolytes are crucial components in electrochemical energy storage devices,sparking considerable research interest.However,the significance of anions in the electrolytes is often underestimated.In fact,the anions have significant impacts on the performance and stability of lithium batteries.Therefore,comprehensively understanding anion chemistry in electrolytes is of crucial importance.Herein,indepth comprehension of anion chemistry and its positive effects on the interface,solvation structure of Li-ions,as well as the electrochemical performance of the batteries have been emphasized and summarized.This review aims to present a full scope of anion chemistry and furnish systematic cognition for the rational design of advanced electrolytes for better lithium batteries with high energy density,lifespan,and safety.Furthermore,insightful analysis and perspectives based on the current research are proposed.We hope that this review sheds light on new perspectives on understanding anion chemistry in electrolytes.
基金supported by National Natural Science Foundation of China(22209064,52071171,and 52202248)the Fundamental Research Funds for Public Universities in Liaoning(LJKLJ202434)+6 种基金the Australian Research Council(ARC)through Future Fellowship(FT210100298)Discovery Project(DP220100603)Linkage Project(LP210200504,LP220100088,LP230200897)Industrial Transformation Research Hub(IH240100009)schemesthe Australian Government through the Cooperative Research Centres Projects(CRCPXIII000077)the Australian Renewable Energy Agency(ARENA)as part of ARENA’s Transformative Research Accelerating Commercialisation Program(TM021)European Commission’s Australia-Spain Network for Innovation and Research Excellence(AuSpire)。
文摘Rechargeable aqueous Zn-MoO_(x)batteries are promising energy storage devices with high theoretical specific capacity and low cost.However,MoO_(3)cathodes suffer drastic capacity decay during the initial discharging/charging process in conventional electrolytes,resulting in a short cycle life and challenging the development of Zn-MoO_(x)batteries.Here we comprehensively investigate the dissolution mechanism of MoO_(3)cathodes and innovatively introduce a polymer to inhibit the irreversible processes.Our findings reveal that this capacity decay originates from the irreversible Zn^(2+)/H^(+)co-intercalation/extraction process in aqueous electrolytes.Even worse,during Zn^(2+)intercalation,the formed Zn_(x)MoO_(3-x)intermediate phase with lower valence states(Mo^(5+)/Mo^(4+))experiences severe dissolution in aqueous environments.To address these challenges,we developed a first instance of coating a polyaniline(PANI)shell around the MoO_(3)nanorod effectively inhibiting these irreversible processes and protecting structural integrity during long-term cycling.Detailed structural analysis and theoretical calculations indicate that=N-groups in PANI@MoO_(3-x)simultaneously weaken H+adsorption and enhance Zn^(2+)adsorption,which endowed the PANI@MoO_(3-x)cathode with reversible Zn^(2+)/H^(+)intercalation/extraction.Consequently,the obtained PANI@MoO_(3-x)cathode delivers an excellent discharge capacity of 316.86 mA h g^(-1)at 0.1 A g^(-1)and prolonged cycling stability of 75.49%capacity retention after 1000 cycles at 5 A g^(-1).This work addresses the critical issues associated with MoO_(3)cathodes and significantly advances the understanding of competitive multi-ion energy storage mechanisms in aqueous Zn-MoO_(3)batteries.
基金supported by the Major Project of Philosophy and Social Science Research of Jiangsu(No.2019SJZDA073).
文摘This study investigates the distribution and imbalances of research funding in the field of Environmental Chemistry,utilizing application and funding data fromthe National Natural Science Foundation of China(NSFC)over the past decade.The findings reveal significant regional disparities,with Eastern regions receiving over 70%of the national funding,while the Northeast accounts for only 4%to 6.5%.Additionally,the analysis shows notable differences in funding allocation among various research institutions,with a substantial portion of funds concentrated in a few leading institutions,leading to inequities across different types and levels of organizations.The impact of applicant gender on funding disparities is relatively minor;although female applicants have a slightly lower funding rate,the concentration of funds is marginally higher among females.Furthermore,the study highlights that key projects and talent-oriented initiatives,due to their significant funding concentration,exacerbate the existing imbalances.Overall,this research provides valuable insights for optimizing funding policies and advocates for a more equitable distribution of resources in Environmental Chemistry research,addressing the identified disparities.
基金financially supported by the National Natural Science Foundation of China(Nos.52372188,51902090)Henan Key Research Project Plan for Higher Education Institutions(Nos.24A150019,23A150038)+4 种基金Key Scientific Research Project of Education Department of Henan Province(No.22A150042)the National students’platform for innovation and entrepreneurship training program(No.201910476010)CAS Henan Industrial Technology Innovation&Incubation Center(No.2024121)2023 Introduction of studying abroad talent program,the China Postdoctoral Science Foundation(No.2019 M652546)the Henan Province Postdoctoral Start-Up Foundation(No.1901017).
文摘NASICON type solid electrolyte Li_(1+x)Al_(x)Ge_(2-x)(PO_(4))_(3)(LAGP)is one of the most potential candidates in view of their high ionic conductivity,high oxidation resistance and excellent air stability.However,inevitable interface issues often cause severe performance degradation,seriously affecting its commercial application.Herein,a lithiophilic carbon buffer layer is constructed on the LAGP surface adjacent to the Li electrode side by a facile pyrolysis reaction,then the LiC_(x) interlayer is generated in situ between the carbon buffer layer and lithium metal,which can guide uniform ion transport while improving interface contact.Thus,the LiC_(x)-LAGP showed excellent ionic conductivity,high flexibility and lithiophilic interphase.Specially,the Li|LiC_(x)-LAGP|Li battery has achieved a 1000 h stable cycles at 0.1 mA/cm^(2),remarkably,the Li|LiC_(x)-LAGP|LFP battery retains 85%of their initial capacity after 200 cycles under 1 C,even for the NCM811 cathode,the battery still has a good cycle performance.
文摘A comprehensive examination of detrital sandstone modes from the Sylhet Trough reveals a diverse range of sub-lithic to sub-feldspathic quartz arenites.Soil samples were gathered from Dupi Gaon(Jaintiapur)in Bangladesh,followed by a thorough analysis using field examination,X-ray diffraction(XRD),X-ray fluorescence(XRF),petrography,and heavy mineral concentration analyses.Field observations revealed the soil sample varying from white to yellowish to variegated,with thicknesses ranging from 15 cm to about 4 m,and exhibiting moderate softness.XRF analysis revealed significant SiO_(2),Al_(2)O_(3),and Fe_(2)O_(3)levels in the samples,with zirconium(Zr)and copper(Cu)showing consistently high concentrations.XRD analysis identified quartz as predominant,along with muscovite,biotite,and accessory minerals like rutile and magnetite.Petrographic analysis highlighted quartz as dominant,with fractures suggesting tectonic influences,while heavy mineral separation techniques identified zircon,garnet,goethite,rutile,and magnetite.These findings provide insights into sediment provenance,depositional processes,and environ-mental conditions during the formation of the Dupi Tila Formation.The comprehensive geochemical data of the entire rock indicates that most of the sediments originated from felsic igneous sources,and also suggests a moderate to high level of weathering in the source region.Overall,the analyses suggested an in situ origin of the Dupi Tila Formation,with parent materials being predominantly detrital rather than authigenic,supported by the presence of detrital quartz and an assessment of the depositional environment,providing insights into the geological conditions of the era and potential modes of sediment transportation.
文摘Surface with well-defined components and structures possesses unique electronic,magnetic,optical and chemical properties.As a result,surface chemistry research plays a crucial role in various fields such as catalysis,energy,materials,quantum,and microelectronics.Surface science mainly investigates the correspondence between surface property and functionality.Scanning probe microscopy(SPM)techniques are important tools to characterize surface properties because of the capability of atomic-scale imaging,spectroscopy and manipulation at the single-atom level.In this review,we summarize recent advances in surface electronic,magnetic and optical properties characterized mainly by SPM-based methods.We focus on elucidating theπ-magnetism in graphene-based nanostructures,construction of spin qubits on surfaces,topology properties of surface organic structures,STM-based light emission,tip-enhanced Raman spectroscopy and integration of machine learning in SPM studies.
基金supported by National Natural Science Foundation of China(Nos.52170086,22308194,U22A20423)Natural Science Foundation of Shandong Province(No.ZR2021ME013)+4 种基金Shandong Provincial Excellent Youth(No.ZR2022YQ47)the doctor research start Foundation of Shaanxi University of Technology(No.SLGRCQD004)Science and Technology Innovation Team Project of Shaanxi Province(No.2025RS-CXTD-040)the General Special Scientific Research Program of the Shaanxi Provincial Department of Education(No.24JK0366)supported by funding from Shandong Provincial Key Laboratory of Monocrystalline Silicon Semiconductor Materials and Technology。
文摘Most carbon-based catalysts utilized in Fenton-like systems face challenges such as structural instability,susceptibility to deactivation,and a tendency to disperse during operation.Wood-derived catalysts have garnered considerable attention due to their well-defined structures,extensive pipeline networks,superior mechanical strength,and adaptability for device customization.However,there remains a paucity of research that systematically summarizes Fenton-like systems based on wood-derived catalysts.In this review,we first summarize the structural designs of wood-derived catalysts based on nano-metal sites and single-atom sites,while also outlining their advantages and limitations applied in Fenton-like systems.Furthermore,we evaluate catalytic modules of wood-derived catalysts for scale-up and continuous Fenton-like systems.Additionally,wood-inspired catalytic materials utilizing commercial textures and their applications in Fenton-like processes are also discussed.This paper aims to comprehensively explore the fundamental mechanisms(e.g.,characteristics of catalytic sites,catalytic performance,and mechanisms)of wood-based catalysts in Fenton-like chemistry,as well as their equipment designs and application scenarios,as well as providing the insights into future developments.
基金funded by the National Key R&D Program of China(2021YFA1501101)the National Natural Science Foundation of China(No.22471103,22425105,22201111,21931001,22221001,and 22271124)+5 种基金Young Elite Scientists Sponsorship Program by CAST(2023QNRC001)the Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province(2019ZX-04)the 111 Project(B20027)as well as the National Natural Science Foundation of Gansu Province(22JR5RA470)the Fundamental Research Funds for the Central Universities(lzujbky-2023-eyt03)supported by the Agency for Science,Technology and Research(A*STAR)MTC Individual Research Grants(IRG)M22K2c0078.
文摘Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution reaction.The surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity enhancement.Here,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is reported.The substituting Fe content influences both current change tendency and surface reconstruction degree.LaNi_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)series.The reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based catalysts.Besides,density functional theory calculations reveal that Fe substitution can lower the O 2p level,which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term stability.Furthermore,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction degree.The effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface reconstruction.This finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.
基金support from the National Natural Science Foundation of China for financial support(22175054)the Distinguished Project for Scientific Research in Universities of Anhui Province(2024AH020011)+2 种基金the Key Project for Cultivation of Outstanding Young Scholars in Universities of Anhui Province(YQZD2024015)the Key Project of Provincial Natural Science Research Foundation of Anhui Universities,China(No.2022AH050406)the Anhui Province Research Funding for Outstanding Young Talents in Colleges and Universities,China(No.gxyq2022021)。
文摘Low-temperature lithium sulfur(Li-S)batteries have attracted increasing attention,but lithium polysulfide(LiPSs)clu stering and tardy ionic mobility have been challenging issues,which could be exacerbated under high sulfur loading and lean electrolyte.The distinct behaviors of sulfur cathode in lowtemperature Li-S batteries call for special regulations of the sulfur host to improve the electrochemical performances.Here,a three-dimensional Ti_(3)C_(2)micro-cage(TCC)with an interfacial structure modulated by rich curvatures has been fabricated to propel the sulfur electrochemistry at subzero temperatures.Spectroscopic/microscopic analyses and theoretical calculations elucidate that the precipitation of ultrafine Ti-metal particles on the in-situ generated Ti_(3)C_(2)nanoribbons could trigger the self-scrolling of Ti_(3)C_(2)nanoribbons into TCC.Moreover,in-situ ultraviolet-visible spectra collected at low temperature and theoretical calculations verified that the TCC regulated by rich curvatures have effectively alleviated the Li+dissociation barrier,reduced the energy barrier for charge transfer at the electrode-electrolyte interface,and restrained the clustering and shuttling of LiPSs,thus accelerating the electrochemical conversion kinetics of sulfur species at low temperatures.The performances of the carbon-free TCC-S cathode at low temperatures have been also compared from the aspects of cathode configuration and measurement condition,to demonstrate the potential of TCC.This work can not only provide new methodology for regulating the interfacial structure of MXene to enrich the materials library for low-temperature Li-S batteries,but also expand understanding about the role of interfacial structure of sulfur host in Li-S batteries.
基金supported by the Global Joint Research Program funded by the Pukyong National University(202411790001)。
文摘Aqueous batteries with metal anodes exhibit robust anodic capacities,but their energy densities are low because of the limited potential stabilities of aqueous electrolyte solutions.Current metal options,such as Zn and Al,pose a dilemma:Zn lacks a sufficiently low redox potential,whereas Al tends to be strongly oxidized in aqueous environments.Our investigation introduces a novel rechargeable aqueous battery system based on Mn as the anode.We examine the effects of anions,electrolyte concentration,and diverse cathode chemistries.Notably,the ClO_(4)-based electrolyte solution exhibits improved deposition and dissolution efficiencies.Although stainless steel(SS 316 L)and Ni are stable current collectors for cathodes,they display limitations as anodes.However,using Ti as the anode resulted in increased Mn deposition and dissolution efficiencies.Moreover,we evaluate this system using various cathode materials,including Mn-intercalation-based inorganic(Ag0.33V2O5)and organic(perylenetetracarboxylic dianhydride)cathodes and an anionintercalation-chemistry(coronene)-based cathode.These configurations yield markedly higher output potentials compared to those of Zn metal batteries,highlighting the potential for an augmented energy density when using an Mn anode.This study outlines a systematic approach for use in optimizing metal anodes in Mn metal batteries,unlocking novel prospects for Mn-based batteries with diverse cathode chemistries.
