The demand for sustainable energy storage has accelerated the development of cellulose-based materials(CBMs)for flexible supercapacitors(FSCs).However,widespread commercialization of FSCs remains challenged by their l...The demand for sustainable energy storage has accelerated the development of cellulose-based materials(CBMs)for flexible supercapacitors(FSCs).However,widespread commercialization of FSCs remains challenged by their low gravimetric energy density(approximately 35 Wh kg^(-1)),far below lithium-ion batteries(exceeding 200 Wh kg^(-1)),and a limited operational temperature range(from-20℃ to 60℃),restricting their use in extreme environments.To date,no comprehensive review has elucidated the crucial role of the chemistry and structure-property relationships of CBMs in advancing FSC technology.This review fills this gap by examining the chemical attributes and versatility of cellulose and its derivatives,including their physicochemical characteris-tics,assembly methodologies,and functional modifications such as oxidation,esterification,etherification,grafting polymerization,nucleophilic substitution,and crosslinking reactions.We further provide an overview of the chemistry and structure-function correlations of various cellulose forms used in advanced electrodes,solid electrolytes,separators,binders,current collectors,and substrate/encapsulation materials,alongside relevant microelectrode processing technologies.Given that large-scale application of FSCs is still in its early stages,we offer insightful design principles for guiding future development of cellulose-based FSCs.By proposing a“chemistry-performance-sustainability”design framework,this review not only addresses existing limitations but also outlines a roadmap for next-generation eco-friendly FSCs.展开更多
Amid the global pursuit of innovative approaches to disease diagnosis and treatment,the interdisciplinary convergence of chemistry and biomedicine has emerged as a pivotal force driving advancements in the field.Cutti...Amid the global pursuit of innovative approaches to disease diagnosis and treatment,the interdisciplinary convergence of chemistry and biomedicine has emerged as a pivotal force driving advancements in the field.Cutting-edge technologies such as optical probes[1],nanotechnology[2],immunotherapy[3],and biosensors[4]are finding increasingly widespread application in disease diagnosis and treatment,sustaining intense interest from both academia and industry.Against this backdrop,the 5th Xihua Chemistry and Biomedicine Forum was successfully held at Xihua University(Chengdu)from July 12 to 15,2025,infusing new vitality into academic exchanges and innovative progress in this domain.展开更多
While oceanic and coastal acidification has gained increased attention,long-term pH trends and their drivers in large freshwater systems remain poorly understood.The Laurentian Great Lakes are the world’s largest fre...While oceanic and coastal acidification has gained increased attention,long-term pH trends and their drivers in large freshwater systems remain poorly understood.The Laurentian Great Lakes are the world’s largest freshwater system,and in many ways resemble marine ecosystems.However,unlike the open ocean and coastal waters where pH has declined due to rising atmospheric CO_(2),no significant pH trends have been observed in the Laurentian Great Lakes,despite significant ecosystem changes driven partly by the invasion of dreissenid mussels.This study examined 41 years of field observations from Lake Michigan to investigate the long-term carbonate chemistry dynamics.Observational results revealed substantial declines in both total alkalinity(TA)and dissolved inorganic carbon(DIC)over the four decades.Mussel shell calcification emerged as the primary mechanism behind these declines,accounting for 97%and 47%of the observed changes in TA and DIC,respectively,lowering water column pH by 0.24 units.Elevated carbon accumulation in soft mussel tissues,coupled with long-term changes in the air-water pCO_(2)gradient during summer,significantly contributed to long-term DIC variations,explaining 18%and 28%of the lake-wide DIC loss.These two mechanisms also resulted in an overall pH increase of 0.09 and 0.12 units,largely offsetting the calcification-driven pH decrease.These findings bridge a gap in acidification research for large freshwater systems and provide valuable insights for comprehensive lake-wide management strategies.展开更多
Solid-state lithium(Li)batteries are hailed as the nextgeneration energy storage technology,garnering significant attention for their potential high energy density and safety.Particularly when using Li-rich manganese ...Solid-state lithium(Li)batteries are hailed as the nextgeneration energy storage technology,garnering significant attention for their potential high energy density and safety.Particularly when using Li-rich manganese layered oxide(LRMO)as cathodes(theoretical capacity exceeding250 mAh/g),energy densities over 600 Wh/kg can be theoretically achieved[1,2].展开更多
Weakly solvating electrolytes(WSEs)promote the formation of anion-driven solid electrolyte interphases(SEI),enabling stable lithium metal batteries.However,current strategies involving alkylated modification,steric hi...Weakly solvating electrolytes(WSEs)promote the formation of anion-driven solid electrolyte interphases(SEI),enabling stable lithium metal batteries.However,current strategies involving alkylated modification,steric hindrance incorporation,coordinated oxygen(O)regulation,and selective fluorination face poor-diversity interfacial chemistry,high cost,or environmental concerns.Here,we propose a heteroatom-substitution strategy to design a WSE composed of lithium bis(fluorosulfonyl)imide(LiFSI)and 1,4-oxathiane(OTA)as a single solvent.Substituting oxygen with sulfur in conventional 1,4-dioxane(1,4-DX)generates OTA with a modulated dipole and charge distribution,weakening Li^(+)-OTA coordination while promoting anion-involved solvation sheath.This unique solvation structure triggers the formation of an inorganic-rich SEI with sulfur-containing species,enabling high Li plating/stripping coulombic efficiency and stable Li‖Li symmetric cells cycling for 1000 h.Benefiting from the superior interfacial chemistry and wettability of the electrolyte to the LiFePO_(4) cathode,full cells exhibit exceptional cycling stability even at low negative-to-positive(N/P)ratios,A pouch cell coupled with3.58 mAh cm^(-2) LiFePO_(4) and 20μm Li(N/P~1.15)maintains 88.77%capacity after 150 cycles.This work shows a fluorine-free solvent design paradigm for advanced WSEs,providing novel insights toward stable LMBs.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
Dear Editors,This letter,reflecting on my research career,is dedi-cated to Professor Qingshi Zhu for his 80th Birthday.Part of this letter is based on my comment“A 20-year journey on the invention of vibrational phot...Dear Editors,This letter,reflecting on my research career,is dedi-cated to Professor Qingshi Zhu for his 80th Birthday.Part of this letter is based on my comment“A 20-year journey on the invention of vibrational photothermal microscopy”published in the May 2025 Nature Meth-ods Focus Issue on Bond-Selective Imaging[1].展开更多
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
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
About us:The College of Chemistry and Materials Engineering(CME)in Wenzhou University(Zhejiang Province,China)is looking for postdoctoral candidates(up to 25)specialized in Chemistry,Chemical Engineering and Materials...About us:The College of Chemistry and Materials Engineering(CME)in Wenzhou University(Zhejiang Province,China)is looking for postdoctoral candidates(up to 25)specialized in Chemistry,Chemical Engineering and Materials Science.The college has its Chemistry program ranking ESI Top 6%o worldwide,and Materials Science program ranking 589th in the world since2023.The college has led publications appearing in journals such as Nat.Catal.,Nat.Commun.,Sci.Adv.,J.Am.Chem.Soc.,Angew.Chem.展开更多
Facilitating anion redox chemistry is an effective strategy to increase the capacity of layered oxides for sodium-ion batteries.Nevertheless,there remains a paucity of literature pertaining to the oxygen redox chemist...Facilitating anion redox chemistry is an effective strategy to increase the capacity of layered oxides for sodium-ion batteries.Nevertheless,there remains a paucity of literature pertaining to the oxygen redox chemistry of O3-type layered oxide cathode materials.This work systematically investigates the effect of Fe doping on the anionic oxygen redox chemistry and electrochemical reactions in O3-NaNi_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1)O_(2).The results of the density functional theory(DFT)calculations indicate that the electrons of the O 2p occupy a higher energy level.In the ex-situ X-ray photoelectron spectrometer(XPS)of O 1s,the addition of Fe facilitates the lattice oxygen(O^(n-))to exhibit enhanced activity at 4.45 V.The in-situ X-ray diffraction(XRD)demonstrates that the doping of Fe effectively suppresses the Y phase transition at high voltages.Furthermore,the Galvanostatic Intermittent Titration Technique(GITT)data indicate that Fe doping significantly increases the Na~+migration rate at high voltages.Consequently,the substitution of Fe can elevate the cut-off voltage to 4.45 V,thereby facilitating electron migration from O^(2-).The redox of O^(2-)/O^(n-)(n<2)contributes to the overall capacity.O3-Na(Ni_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1))_(0.92)Fe_(0.08)O_(2)provides an initial discharge specific capacity of 180.55 mA h g^(-1)and71.6%capacity retention at 0.5 C(1 C=240 mA g^(-1)).This work not only demonstrates the beneficial impact of Fe substitution for promoting the redox activity and reversibility of O^(2-)in 03-type layered oxides,but also guarantees the structural integrity of the cathode materials at high voltages(>4.2 V).It offers a novel avenue for investigating the anionic redox reaction in O3-type layered oxides to design advanced cathode materials.展开更多
Atmospheric chemistry research and atmospheric measurement techniques have mutually promoted each other and developed rapidly in China in recent years.Cavity-based absorption spectroscopy,which uses a high-finesse cav...Atmospheric chemistry research and atmospheric measurement techniques have mutually promoted each other and developed rapidly in China in recent years.Cavity-based absorption spectroscopy,which uses a high-finesse cavity to achieve very long absorption path-length,thereby achieving ultra-high detection sensitivity,plays an extremely important role in atmospheric chemistry research.Based on the Beer–Lambert law,this technology has the unique advantages of being non-destructive,chemical-free,and highly selective.It does not require any sample preparation and can quantitatively analyze atmospheric trace gases in real time and in situ.In this paper,we review the following:(1)key technological advances in different cavity-based absorption spectroscopy techniques,including cavity ring-down spectroscopy,cavityenhanced absorption spectroscopy,cavity attenuated phase shift spectroscopy,and their extensions;and(2)applications of these techniques in the detection of atmospheric reactive species,such as total peroxy radical,formaldehyde,and reactive nitrogen(e.g.,NOx,HONO,peroxy nitrates,and alkyl nitrates).The review systematically introduces cavity-based absorption spectroscopy techniques and their applications in atmospheric chemistry,which will help promote further communication and cooperation in the fields of laser spectroscopy and atmospheric chemistry.展开更多
Changes to the microstructure of a hard carbon(HC)and its solid electrolyte interface(SEI)can be effective in improving the electrode kinetics.However,achieving fast charging using a simple and inexpensive strategy wi...Changes to the microstructure of a hard carbon(HC)and its solid electrolyte interface(SEI)can be effective in improving the electrode kinetics.However,achieving fast charging using a simple and inexpensive strategy without sacrificing its initial Coulombic efficiency remains a challenge in sodium ion batteries.A simple liquid-phase coating approach has been used to generate a pitch-derived soft carbon layer on the HC surface,and its effect on the porosity of HC and SEI chemistry has been studied.A variety of structural characterizations show a soft carbon coating can increase the defect and ultra-micropore contents.The increase in ultra-micropore comes from both the soft carbon coatings and the larger pores within the HC that are partially filled by pitch,which provides more Na+storage sites.In-situ FTIR/EIS and ex-situ XPS showed that the soft carbon coating induced the formation of thinner SEI that is richer in NaF from the electrolyte,which stabilized the interface and promoted the charge transfer process.As a result,the anode produced fastcharging(329.8 mAh g^(−1)at 30 mA g^(−1)and 198.6 mAh g^(−1)at 300 mA g^(−1))and had a better cycling performance(a high capacity retention of 81.4%after 100 cycles at 150 mA g^(−1)).This work reveals the critical role of coating layer in changing the pore structure,SEI chemistry and diffusion kinetics of hard carbon,which enables rational design of sodium-ion battery anode with enhanced fast charging capability.展开更多
About us:The College of Chemistry and Materials Engineering(CME)in Wenzhou University(Zhejiang Province,China)is looking for postdoctoral candidates(up to 25)specialized in Chemistry,Chemical Engineering and Materials...About us:The College of Chemistry and Materials Engineering(CME)in Wenzhou University(Zhejiang Province,China)is looking for postdoctoral candidates(up to 25)specialized in Chemistry,Chemical Engineering and Materials Science.The collegehas its Chemistry program ranking ESI Top 6‰ worldwide,and Materials Scienceprogram ranking 589th in the world since 2023.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
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
In pursuit of low cost and long life for lithium-ion batteries in electric vehicles,the most promising strategy is to replace the commercial LiCoO_(2)with a high-energy-density Ni-rich cathode.However,the irreversible...In pursuit of low cost and long life for lithium-ion batteries in electric vehicles,the most promising strategy is to replace the commercial LiCoO_(2)with a high-energy-density Ni-rich cathode.However,the irreversible redox couples induce rapid capacity decay,poor long-term cycling life,vast gas evolution,and unstable structure transformations of the Ni-rich cathode,limiting its practical applications.Element doping has been considered as the most promising strategy for addressing these issues.However,the relationships between element doping functions and redox chemistry still remain confused.To clarify this connection,this review places the dynamic evolution of redox couples(Li^(*),Ni^(2+)/Ni^(3+)/Ni^(4+)-e^(-),O^(2-)/O^(n-)/O_(2)-e^(-))as the tree trunk.The material structure,degradation mechanisms,and addressing element doping strategies are considered as the tree branches.This comprehensive summary aims to provide an overview of the current understanding and progress of Ni-rich cathode materials.In the last section,promising strategies based on element doping functions are provided to encourage the practical application of Ni-rich cathodes.These strategies also offer a new approach for the development of other intercalated electrode materials in Na and K-based battery systems.展开更多
Sometimes chemistry doesn’t just make new molecules-it overturns old assumptions.For 140 years,drugmakers have accepted that transforming aromatic amines-a very important reaction for building drug molecules-means li...Sometimes chemistry doesn’t just make new molecules-it overturns old assumptions.For 140 years,drugmakers have accepted that transforming aromatic amines-a very important reaction for building drug molecules-means living with explosive risks.The danger was considered unavoidable,the tradeoff permanent-until a team in Hangzhou proved otherwise.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
基金support from the National Key R&D Program of China(Grant No.2023YFB4005204)the National Natural Science Foundation of China(Grant No.22125903,U24A20553,22579025,52502038)+2 种基金Fundamental Research Funds for the Central Universities(No.2572023CT06)Key Joint Project of the Natural Science Foundation of Heilongjiang Province,China(No.ZL2024E007)the Innovation Foundation for Doctoral Program of Forestry Engineering of Northeast Forestry University(No.LYGC202220).
文摘The demand for sustainable energy storage has accelerated the development of cellulose-based materials(CBMs)for flexible supercapacitors(FSCs).However,widespread commercialization of FSCs remains challenged by their low gravimetric energy density(approximately 35 Wh kg^(-1)),far below lithium-ion batteries(exceeding 200 Wh kg^(-1)),and a limited operational temperature range(from-20℃ to 60℃),restricting their use in extreme environments.To date,no comprehensive review has elucidated the crucial role of the chemistry and structure-property relationships of CBMs in advancing FSC technology.This review fills this gap by examining the chemical attributes and versatility of cellulose and its derivatives,including their physicochemical characteris-tics,assembly methodologies,and functional modifications such as oxidation,esterification,etherification,grafting polymerization,nucleophilic substitution,and crosslinking reactions.We further provide an overview of the chemistry and structure-function correlations of various cellulose forms used in advanced electrodes,solid electrolytes,separators,binders,current collectors,and substrate/encapsulation materials,alongside relevant microelectrode processing technologies.Given that large-scale application of FSCs is still in its early stages,we offer insightful design principles for guiding future development of cellulose-based FSCs.By proposing a“chemistry-performance-sustainability”design framework,this review not only addresses existing limitations but also outlines a roadmap for next-generation eco-friendly FSCs.
文摘Amid the global pursuit of innovative approaches to disease diagnosis and treatment,the interdisciplinary convergence of chemistry and biomedicine has emerged as a pivotal force driving advancements in the field.Cutting-edge technologies such as optical probes[1],nanotechnology[2],immunotherapy[3],and biosensors[4]are finding increasingly widespread application in disease diagnosis and treatment,sustaining intense interest from both academia and industry.Against this backdrop,the 5th Xihua Chemistry and Biomedicine Forum was successfully held at Xihua University(Chengdu)from July 12 to 15,2025,infusing new vitality into academic exchanges and innovative progress in this domain.
基金Supported by the National Natural Science Foundation of China(No.43277051)the Key Laboratory of Integrated Regulation and Resources Development of Shallow Lakes of Ministry of Education(No.B230203006).
文摘While oceanic and coastal acidification has gained increased attention,long-term pH trends and their drivers in large freshwater systems remain poorly understood.The Laurentian Great Lakes are the world’s largest freshwater system,and in many ways resemble marine ecosystems.However,unlike the open ocean and coastal waters where pH has declined due to rising atmospheric CO_(2),no significant pH trends have been observed in the Laurentian Great Lakes,despite significant ecosystem changes driven partly by the invasion of dreissenid mussels.This study examined 41 years of field observations from Lake Michigan to investigate the long-term carbonate chemistry dynamics.Observational results revealed substantial declines in both total alkalinity(TA)and dissolved inorganic carbon(DIC)over the four decades.Mussel shell calcification emerged as the primary mechanism behind these declines,accounting for 97%and 47%of the observed changes in TA and DIC,respectively,lowering water column pH by 0.24 units.Elevated carbon accumulation in soft mussel tissues,coupled with long-term changes in the air-water pCO_(2)gradient during summer,significantly contributed to long-term DIC variations,explaining 18%and 28%of the lake-wide DIC loss.These two mechanisms also resulted in an overall pH increase of 0.09 and 0.12 units,largely offsetting the calcification-driven pH decrease.These findings bridge a gap in acidification research for large freshwater systems and provide valuable insights for comprehensive lake-wide management strategies.
基金supported by the National Natural Science Foundation of China(No.22479021).
文摘Solid-state lithium(Li)batteries are hailed as the nextgeneration energy storage technology,garnering significant attention for their potential high energy density and safety.Particularly when using Li-rich manganese layered oxide(LRMO)as cathodes(theoretical capacity exceeding250 mAh/g),energy densities over 600 Wh/kg can be theoretically achieved[1,2].
基金the financial support from the National Natural Science Foundation of China,China(Grant Nos.52502258 and 52162030)the Yunnan Fundamental Research Projects,China(Grant Nos.202501AT070298,202401AU070163 and 202401AT070368)+5 种基金the Yunnan Engineering Research Center Innovation Ability Construction and Enhancement Projects,China(Grant No.2023-XMDJ-00617107)the Expert Workstation Support Project of Yunnan Province,China(Grant Nos.202405AF140069 and 202505AF350019)the University Service Key Industry Project of Yunnan Province,China(Grant No.FWCY-ZD2024005)the Shenzhen Science and Technology Program,China(Grant No.KJZD20230923114107014)the Scientific Research Foundation of Kunming University of Science and Technology,China(20220122)the Analysis and Test Foundation of Kunming University of Science and Technology,China(Grant No.2023T20220122)。
文摘Weakly solvating electrolytes(WSEs)promote the formation of anion-driven solid electrolyte interphases(SEI),enabling stable lithium metal batteries.However,current strategies involving alkylated modification,steric hindrance incorporation,coordinated oxygen(O)regulation,and selective fluorination face poor-diversity interfacial chemistry,high cost,or environmental concerns.Here,we propose a heteroatom-substitution strategy to design a WSE composed of lithium bis(fluorosulfonyl)imide(LiFSI)and 1,4-oxathiane(OTA)as a single solvent.Substituting oxygen with sulfur in conventional 1,4-dioxane(1,4-DX)generates OTA with a modulated dipole and charge distribution,weakening Li^(+)-OTA coordination while promoting anion-involved solvation sheath.This unique solvation structure triggers the formation of an inorganic-rich SEI with sulfur-containing species,enabling high Li plating/stripping coulombic efficiency and stable Li‖Li symmetric cells cycling for 1000 h.Benefiting from the superior interfacial chemistry and wettability of the electrolyte to the LiFePO_(4) cathode,full cells exhibit exceptional cycling stability even at low negative-to-positive(N/P)ratios,A pouch cell coupled with3.58 mAh cm^(-2) LiFePO_(4) and 20μm Li(N/P~1.15)maintains 88.77%capacity after 150 cycles.This work shows a fluorine-free solvent design paradigm for advanced WSEs,providing novel insights toward stable LMBs.
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Dear Editors,This letter,reflecting on my research career,is dedi-cated to Professor Qingshi Zhu for his 80th Birthday.Part of this letter is based on my comment“A 20-year journey on the invention of vibrational photothermal microscopy”published in the May 2025 Nature Meth-ods Focus Issue on Bond-Selective Imaging[1].
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.
文摘About us:The College of Chemistry and Materials Engineering(CME)in Wenzhou University(Zhejiang Province,China)is looking for postdoctoral candidates(up to 25)specialized in Chemistry,Chemical Engineering and Materials Science.The college has its Chemistry program ranking ESI Top 6%o worldwide,and Materials Science program ranking 589th in the world since2023.The college has led publications appearing in journals such as Nat.Catal.,Nat.Commun.,Sci.Adv.,J.Am.Chem.Soc.,Angew.Chem.
基金financial support from the Natural Science Foundation of Shandong Province of China(ZR2023ME051,ZR2019MEM020)。
文摘Facilitating anion redox chemistry is an effective strategy to increase the capacity of layered oxides for sodium-ion batteries.Nevertheless,there remains a paucity of literature pertaining to the oxygen redox chemistry of O3-type layered oxide cathode materials.This work systematically investigates the effect of Fe doping on the anionic oxygen redox chemistry and electrochemical reactions in O3-NaNi_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1)O_(2).The results of the density functional theory(DFT)calculations indicate that the electrons of the O 2p occupy a higher energy level.In the ex-situ X-ray photoelectron spectrometer(XPS)of O 1s,the addition of Fe facilitates the lattice oxygen(O^(n-))to exhibit enhanced activity at 4.45 V.The in-situ X-ray diffraction(XRD)demonstrates that the doping of Fe effectively suppresses the Y phase transition at high voltages.Furthermore,the Galvanostatic Intermittent Titration Technique(GITT)data indicate that Fe doping significantly increases the Na~+migration rate at high voltages.Consequently,the substitution of Fe can elevate the cut-off voltage to 4.45 V,thereby facilitating electron migration from O^(2-).The redox of O^(2-)/O^(n-)(n<2)contributes to the overall capacity.O3-Na(Ni_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1))_(0.92)Fe_(0.08)O_(2)provides an initial discharge specific capacity of 180.55 mA h g^(-1)and71.6%capacity retention at 0.5 C(1 C=240 mA g^(-1)).This work not only demonstrates the beneficial impact of Fe substitution for promoting the redox activity and reversibility of O^(2-)in 03-type layered oxides,but also guarantees the structural integrity of the cathode materials at high voltages(>4.2 V).It offers a novel avenue for investigating the anionic redox reaction in O3-type layered oxides to design advanced cathode materials.
基金supported by the National Natural Science Foundation of China(Grant Nos.U21A2028,42022051,62275250,42030609,41627810,91644107,and 91544228).
文摘Atmospheric chemistry research and atmospheric measurement techniques have mutually promoted each other and developed rapidly in China in recent years.Cavity-based absorption spectroscopy,which uses a high-finesse cavity to achieve very long absorption path-length,thereby achieving ultra-high detection sensitivity,plays an extremely important role in atmospheric chemistry research.Based on the Beer–Lambert law,this technology has the unique advantages of being non-destructive,chemical-free,and highly selective.It does not require any sample preparation and can quantitatively analyze atmospheric trace gases in real time and in situ.In this paper,we review the following:(1)key technological advances in different cavity-based absorption spectroscopy techniques,including cavity ring-down spectroscopy,cavityenhanced absorption spectroscopy,cavity attenuated phase shift spectroscopy,and their extensions;and(2)applications of these techniques in the detection of atmospheric reactive species,such as total peroxy radical,formaldehyde,and reactive nitrogen(e.g.,NOx,HONO,peroxy nitrates,and alkyl nitrates).The review systematically introduces cavity-based absorption spectroscopy techniques and their applications in atmospheric chemistry,which will help promote further communication and cooperation in the fields of laser spectroscopy and atmospheric chemistry.
基金National Key Research and Development Program of China(2022YFE0206300)National Natural Science Foundation of China(U21A2081,22075074,22209047)+2 种基金Guangdong Basic and Applied Basic Research Foundation(2024A1515011620)Hunan Provincial Natural Science Foundation of China(2024JJ5068)Foundation of Yuelushan Center for Industrial Innovation(2023YCII0119)。
文摘Changes to the microstructure of a hard carbon(HC)and its solid electrolyte interface(SEI)can be effective in improving the electrode kinetics.However,achieving fast charging using a simple and inexpensive strategy without sacrificing its initial Coulombic efficiency remains a challenge in sodium ion batteries.A simple liquid-phase coating approach has been used to generate a pitch-derived soft carbon layer on the HC surface,and its effect on the porosity of HC and SEI chemistry has been studied.A variety of structural characterizations show a soft carbon coating can increase the defect and ultra-micropore contents.The increase in ultra-micropore comes from both the soft carbon coatings and the larger pores within the HC that are partially filled by pitch,which provides more Na+storage sites.In-situ FTIR/EIS and ex-situ XPS showed that the soft carbon coating induced the formation of thinner SEI that is richer in NaF from the electrolyte,which stabilized the interface and promoted the charge transfer process.As a result,the anode produced fastcharging(329.8 mAh g^(−1)at 30 mA g^(−1)and 198.6 mAh g^(−1)at 300 mA g^(−1))and had a better cycling performance(a high capacity retention of 81.4%after 100 cycles at 150 mA g^(−1)).This work reveals the critical role of coating layer in changing the pore structure,SEI chemistry and diffusion kinetics of hard carbon,which enables rational design of sodium-ion battery anode with enhanced fast charging capability.
文摘About us:The College of Chemistry and Materials Engineering(CME)in Wenzhou University(Zhejiang Province,China)is looking for postdoctoral candidates(up to 25)specialized in Chemistry,Chemical Engineering and Materials Science.The collegehas its Chemistry program ranking ESI Top 6‰ worldwide,and Materials Scienceprogram ranking 589th in the world since 2023.
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supported by the National Natural Science Foundation of China(22209055)the China Postdoctoral Science Foundation(2022M721330)+2 种基金the Foshan Postdoctoral Science Foundation(X221081MS210)the Innovation Team of Universities of Guangdong Province(2022KCXTD030)the“Targeted Technology Innovation Initiative”Project at the Foshan National Institute of Innovation(JBGS2024002)。
文摘In pursuit of low cost and long life for lithium-ion batteries in electric vehicles,the most promising strategy is to replace the commercial LiCoO_(2)with a high-energy-density Ni-rich cathode.However,the irreversible redox couples induce rapid capacity decay,poor long-term cycling life,vast gas evolution,and unstable structure transformations of the Ni-rich cathode,limiting its practical applications.Element doping has been considered as the most promising strategy for addressing these issues.However,the relationships between element doping functions and redox chemistry still remain confused.To clarify this connection,this review places the dynamic evolution of redox couples(Li^(*),Ni^(2+)/Ni^(3+)/Ni^(4+)-e^(-),O^(2-)/O^(n-)/O_(2)-e^(-))as the tree trunk.The material structure,degradation mechanisms,and addressing element doping strategies are considered as the tree branches.This comprehensive summary aims to provide an overview of the current understanding and progress of Ni-rich cathode materials.In the last section,promising strategies based on element doping functions are provided to encourage the practical application of Ni-rich cathodes.These strategies also offer a new approach for the development of other intercalated electrode materials in Na and K-based battery systems.
文摘Sometimes chemistry doesn’t just make new molecules-it overturns old assumptions.For 140 years,drugmakers have accepted that transforming aromatic amines-a very important reaction for building drug molecules-means living with explosive risks.The danger was considered unavoidable,the tradeoff permanent-until a team in Hangzhou proved otherwise.
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.
