Mangicol-type sesterterpenoids possess potent anti-inflammatory activity,characterized by a 5-5-6-5tetracyclic carbon skeleton formed by mangicdiene synthase Fg MS.Two proposed mechanisms for mangicdiene formation inv...Mangicol-type sesterterpenoids possess potent anti-inflammatory activity,characterized by a 5-5-6-5tetracyclic carbon skeleton formed by mangicdiene synthase Fg MS.Two proposed mechanisms for mangicdiene formation involve either C6-C10 cyclization(path a) or C2-C10 cyclization(path b) after the C10carbocation formation,but neither has been experimentally validated.Here,we have identified a second mangicdiene synthase Man D,which is derived from Fusarium sp.JNU-XJ070152-01 and shares high amino acid sequence identity with Fg MS.Through heterologous expression of man D in Aspergillus oryzae NSAR1,we observed production not only of mangicdiene(1) and variecoltetraene(2),previously identified by expression of Fg MS in Escherichia coli,but also two novel sesterterpene skeletons fusadiene(3)and fusatriene(4).The identification of fusadiene and fusatriene supports the occurrence of two key carbocation intermediates in path b,thus experimentally confirming that mangicdiene is built via path b for the first time,consistent with previous density functional theory(DFT) calculation results.展开更多
Optically pure chiral chemicals are important building blocks with widespread applications across mul-tiple scientific and industrial do-mains such as in pharmaceuticals,agrochemicals,and food,especially acting as pre...Optically pure chiral chemicals are important building blocks with widespread applications across mul-tiple scientific and industrial do-mains such as in pharmaceuticals,agrochemicals,and food,especially acting as precursors to synthesize biodegradable polymers.As an al-ternative to fossil resources,renew-able lignocellulosic biomass has been used to access chiral chemicals,due to the versatile inherent stere-ostructures and multiple functional groups,such as hydroxyl,carbonyl,and phenyl ether groups.Typically,as the two main units of(hemi)cel-lulose components in lignocellulosic biomass,D-xylose and D-glucose bear multiple chiral centers(e.g.,2R-3S-4R for D-xylose and 2R-3S-4R-5R for D-glucose).Lignin bearsβ-O-4 linkages,exhibiting(R,S/S,R)or(R,R/S,S)stereocenters at the side-chainαandβcarbon atoms.The valorization of biomass into optical-ly pure chiral chemicals is vital for developing a more sustainable future.This review discuss-es the production of typical chiral chemicals derived from biomass through chemocatalysis,including lactones(e.g.,R/S-valerolactone),carboxylic acids(e.g.,D/L-glyceric acid,D/L-lactic acid),polyols(e.g.,tetrose),furans,oligosaccharides,and others.Two strategies are generally employed.One approach involves first producing achiral platform chemicals from biomass,followed by the introduction of asymmetric catalysts to reconstruct stereocenters.The second relates to selectively preserving one or more inherent stereocenters in the natural biomass structure during complex cascade reactions in which biomass feedstock acts as a“chi-ral pool",thus eliminating the establishment of stereocenter.The feedstock,methods em-ployed,and enantioselectivity and applications of the target chiral chemicals are discussed.Despite these advances,the synthesis of optically pure chemicals from biomass is still in its in-fancy.The coming decade presents both extraordinary challenges and opportunities in biomass-derived chiral chemistry.Future research should be focused on:(1)integrating well-established asymmetric catalysis techniques and methods with biomass’s inherent chiral pools,presenting an unprecedented opportunity to expand the chemical space of sustainable chiral compounds;(2)mastering polyfunctional complexity of chiral chemicals through holis-tic utilization of biomass’multichiral centers;(3)unlocking lignin’s stereochemical treasury that represents the next frontier in biomass valorization.展开更多
The development of intrinsically conductive piezoresistive sensors with high strain tolerance has garnered significant interest.While elastomeric polymers exhibit excellent strain capabilities,their utility in sensing...The development of intrinsically conductive piezoresistive sensors with high strain tolerance has garnered significant interest.While elastomeric polymers exhibit excellent strain capabilities,their utility in sensing applications has been limited by inherent challenges such as high electrical resistivity,poor aging resistance,and interfacial incompatibility.To address these limitations,hydroxyl-terminated polybutadiene(HTPB)-based polyurethane was chemically modified with acetylferrocene-polyaniline conductive moieties to enhance charge transport properties.Remarkably,this covalent functionalization endowed the resulting ferrocene-polyaniline hybrid polyurethane(FPHP)with a conductivity of2.33 n A at 1 V bias while preserving piezoresistive functionality.The FPHP demonstrated exceptional mechanical-electrical performance,achieving 254% elongation at break with strain-dependent gauge factors of 7.28(0%-12.5% strain,R^(2)=0.9504)and 19.66(12.5%-35.0% strain,R^(2)=0.9929).Further characterization revealed a rapid 0.60 s response time and stability over 3500 strain-release cycles at compression strain,underscoring its durability under repetitive loading.The FPHP sensor was capable of monitoring various human movements and recognizing writing signals.These advances establish a materials design paradigm for fabricating flexible sensors that synergistically integrate high deformability,tunable sensitivity,and robust operational stability,positioning FPHP as a promising candidate for next-generation wearable electronics and soft robotics.展开更多
Conventional error cancellation approaches separate molecules into smaller fragments and sum the errors of all fragments to counteract the overall computational error of the parent molecules.However,these approaches m...Conventional error cancellation approaches separate molecules into smaller fragments and sum the errors of all fragments to counteract the overall computational error of the parent molecules.However,these approaches may be ineffective for systems with strong localized chemical effects,as fragmenting specific substructures into simpler chemical bonds can introduce additional errors instead of mitigating them.To address this issue,we propose the Substructure-Preserved Connection-Based Hierarchy(SCBH),a method that automatically identifies and freezes substructures with significant local chemical effects prior to molecular fragmentation.The SCBH is validated by the gas-phase enthalpy of formation calculation of CHNO molecules.Therein,based on the atomization scheme,the reference and test values are derived at the levels of Gaussian-4(G4)and M062X/6-31+G(2df,p),respectively.Compared to commonly used approaches,SCBH reduces the average computational error by half and requires only15%of the computational cost of G4 to achieve comparable accuracy.Since different types of local effect structures have differentiated influences on gas-phase enthalpy of formation,substituents with strong electronic effects should be retained preferentially.SCBH can be readily extended to diverse classes of organic compounds.Its workflow and source code allow flexible customization of molecular moieties,including azide,carboxyl,trinitromethyl,phenyl,and others.This strategy facilitates accurate,rapid,and automated computations and corrections,making it well-suited for high-throughput molecular screening and dataset construction for gas-phase enthalpy of formation.展开更多
Space exploration and manufacturing are of critical importance for scientific advancement,technological innovation,national security,and the acquisition of extraterrestrial resources.In view of this,chemical and biolo...Space exploration and manufacturing are of critical importance for scientific advancement,technological innovation,national security,and the acquisition of extraterrestrial resources.In view of this,chemical and biological nano-/micro-/meso-scale manufacturing provide complementary approaches to overcome key space exploration challenges by enabling the in-situ production of essential life-support materials,propellants,and other resources.This review examines the origin and historical evolution of space manufacturing and the latest advances across different environments—from orbital space stations and the lunar surface to Mars and asteroids.It is structured to present the current state of research,outline key manufacturing strategies and technologies,assess the technical and environmental challenges,and discuss emerging trends and future directions.Besides,the potential applications of emerging technologies such as synthetic biology and artificial intelligence in overcoming the limitations of microgravity,limited resources,and extreme conditions are discussed.Ultimately,this integrative review could serve to guide future development,from advancing space science and disruptive manufacturing to enabling interdisciplinary and application-level innovations.展开更多
Chemical warfare agents(CWAs)remain a persistent hazard in many parts of the world,necessitating a deeper exploration of their chemical and physical characteristics and reactions under diverse conditions.Diisopropyl m...Chemical warfare agents(CWAs)remain a persistent hazard in many parts of the world,necessitating a deeper exploration of their chemical and physical characteristics and reactions under diverse conditions.Diisopropyl methylphosphonate(DIMP),a commonly used CWA surrogate,is widely studied to enhance our understanding of CWA behavior.The prevailing thermal decomposition model for DIMP,developed approximately 25 years ago,is based on data collected in nitrogen atmospheres at temperatures ranging from 700 K to 800 K.Despite its limitations,this model continues to serve as a foundation for research across various thermal and reactive environments,including combustion studies.Our recent experiments have extended the scope of decomposition analysis by examining DIMP in both nitrogen and zero air across a lower temperature range of 175℃ to 250℃.Infrared spectroscopy results under nitrogen align well with the established model;however,we observed that catalytic effects,stemming from decomposition byproducts and interactions with stainless steel surfaces,alter the reaction kinetics.In zero air environments,we observed a novel infrared absorption band.Spectral fitting suggests this band may represent a combination of propanal and acetone,while GCMS analysis points to vinyl formate and acetone as possible constituents.Although the precise identity of these new products remains unresolved,our findings clearly indicate that the existing decomposition model cannot be reliably extended to lower temperatures or non-nitrogen environments without further revisions.展开更多
Groundwater is a key part of the terrestrial ecosystem,but it is vulnerable to pollution in the context of chemical industry development.Treating contaminated groundwater is challenging due to its stable water quality...Groundwater is a key part of the terrestrial ecosystem,but it is vulnerable to pollution in the context of chemical industry development.Treating contaminated groundwater is challenging due to its stable water quality,hidden contamination,and complex treatment requirements.Current research focuses on advanced treatment technologies,among which the advanced oxidation process(AOPs) of peroxomonosulfate(PMS) has great potential.Although there are many reviews of PMS-based AOP,most of them focus on surface water.This review aims to explore the activation reaction of PMS to groundwater by in-situ chemical oxidation(ISCO) technology,further study the reaction mechanism,compare the treatment effect of characteristic pollutants in the groundwater of the chemical industry park,propose new activation methods and catalyst selection,and provide guidance for future groundwater treatment research.展开更多
Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and l...Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and long-range electric vehicles.However,technical barriers such as dendrite growth and poor Li plating/stripping reversibility severely hinder the practical application of LMBs.However,lithium nitrate(LiNO_(3))is found to be able to stabilize the Li/electrolyte interface and has been used to address the above challenges.To date,considerable research efforts have been devoted toward understanding the roles of LiNO_(3) in regulating the surface properties of Li anodes and toward the development of many effective strategies.These research efforts are partially mentioned in some articles on LMBs and yet have not been reviewed systematically.To fill this gap,we discuss the recent advances in fundamental and technological research on LiNO_(3) and its derivatives for improving the performances of LMBs,particularly for Li-sulfur(S),Li-oxygen(O),and Li-Li-containing transition-metal oxide(LTMO)batteries,as well as LiNO_(3)-containing recipes for precursors in battery materials and interphase fabrication.This review pays attention to the effects of LiNO_(3) in lithium-based batteries,aiming to provide scientific guidance for the optimization of electrode/electrolyte interfaces and enrich the design of advanced LMBs.展开更多
Chemical exchange saturation transfer magnetic resonance imaging is an advanced imaging technique that enables the detection of compounds at low concentrations with high sensitivity and spatial resolution and has been...Chemical exchange saturation transfer magnetic resonance imaging is an advanced imaging technique that enables the detection of compounds at low concentrations with high sensitivity and spatial resolution and has been extensively studied for diagnosing malignancy and stroke.In recent years,the emerging exploration of chemical exchange saturation transfer magnetic resonance imaging for detecting pathological changes in neurodegenerative diseases has opened up new possibilities for early detection and repetitive scans without ionizing radiation.This review serves as an overview of chemical exchange saturation transfer magnetic resonance imaging with detailed information on contrast mechanisms and processing methods and summarizes recent developments in both clinical and preclinical studies of chemical exchange saturation transfer magnetic resonance imaging for Alzheimer’s disease,Parkinson’s disease,multiple sclerosis,and Huntington’s disease.A comprehensive literature search was conducted using databases such as PubMed and Google Scholar,focusing on peer-reviewed articles from the past 15 years relevant to clinical and preclinical applications.The findings suggest that chemical exchange saturation transfer magnetic resonance imaging has the potential to detect molecular changes and altered metabolism,which may aid in early diagnosis and assessment of the severity of neurodegenerative diseases.Although promising results have been observed in selected clinical and preclinical trials,further validations are needed to evaluate their clinical value.When combined with other imaging modalities and advanced analytical methods,chemical exchange saturation transfer magnetic resonance imaging shows potential as an in vivo biomarker,enhancing the understanding of neuropathological mechanisms in neurodegenerative diseases.展开更多
A new electrochemical strategy for trifluoromethylation/cyclization using TfNHNHBoc as a CF_(3)source was established.This approach was realized by the direct electrolysis of Tf NHNHBoc under external oxidantfree and ...A new electrochemical strategy for trifluoromethylation/cyclization using TfNHNHBoc as a CF_(3)source was established.This approach was realized by the direct electrolysis of Tf NHNHBoc under external oxidantfree and catalyst-free conditions,and afforded various trifluoromethylated oxindoles with good functional group compatibility and broad substrate scope.Preliminary mechanistic studies show that the reaction proceeds by a radical process.展开更多
Achieving regioselectivity in radical cyclization reactions is of central importance,yet extremely challenging.Although Baldwin’s rules provided guidance on the addition of radical species with alkenes/alkynes,the or...Achieving regioselectivity in radical cyclization reactions is of central importance,yet extremely challenging.Although Baldwin’s rules provided guidance on the addition of radical species with alkenes/alkynes,the ortho-/ipso-selectivity of the cyclic reaction between radical species(especially alkyl and alkenyl radical)and aryl groups is still ambiguous.Herein,we develop an electrochemically enabled regioselective ortho-(4+2)/ipso-(3+2)cyclization of alkyl/alkenyl radicals with aryl groups,which provides a series of tetrahydronaphthalene and spirocarbocycle derivatives,exhibiting a broad substrate scope and functional group tolerance.Alkyl/alkenyl radicals are generated by Cp2Fe-mediated electrochemical oxidative radical addition of benzylic malonates with alkenes and alkynes.The method avoids the use of chemical oxidant/base/noble metal,the pre-functionalization of substrates,and the over-oxidation of compounds.Theoretical studies reveal that the dominant factor promoting the alkene-preferred ortho-addition is the favorable interaction energy;the alkyne-preferred ipso-addition regioselectivity is controlled by the distortion energy.Notably,this strategy is regarded as an important supplement to Baldwin’s rules for radical cyclization.展开更多
Parkinson’s disease is a common neurodegenerative disease with movement disorders associated with the intracytoplasmic deposition of aggregate proteins such asα-synuclein in neurons.As one of the major intracellular...Parkinson’s disease is a common neurodegenerative disease with movement disorders associated with the intracytoplasmic deposition of aggregate proteins such asα-synuclein in neurons.As one of the major intracellular degradation pathways,the autophagy-lysosome pathway plays an important role in eliminating these proteins.Accumulating evidence has shown that upregulation of the autophagy-lysosome pathway may contribute to the clearance ofα-synuclein aggregates and protect against degeneration of dopaminergic neurons in Parkinson’s disease.Moreover,multiple genes associated with the pathogenesis of Parkinson’s disease are intimately linked to alterations in the autophagy-lysosome pathway.Thus,this pathway appears to be a promising therapeutic target for treatment of Parkinson’s disease.In this review,we briefly introduce the machinery of autophagy.Then,we provide a description of the effects of Parkinson’s disease–related genes on the autophagy-lysosome pathway.Finally,we highlight the potential chemical and genetic therapeutic strategies targeting the autophagy–lysosome pathway and their applications in Parkinson’s disease.展开更多
Angelica sinensis(A.sinensis),as a kind of Chinese medicine,has the effects of tonifying blood,promoting blood circulation,regulating menstrual flow,relieving pain,moistening bowel and so on.By consulting Sciencedirec...Angelica sinensis(A.sinensis),as a kind of Chinese medicine,has the effects of tonifying blood,promoting blood circulation,regulating menstrual flow,relieving pain,moistening bowel and so on.By consulting Sciencedirect database and Web of Science database,163 related articles were found,of which 36 were related to chemical composition and pharmacological activities of A.sinensis.In this paper,the chemical structures and different derivatives were systematically summarized by reviewing relevant literatures,and the pharmacological effects were also summarized.展开更多
As a diuretic and dampness-eliminating medicinal agent in traditional Chinese medicine(TCM),Zexie(Alismatis Rhizoma)is commonly used for symptoms such as dysuria,edema and abdominal distension,diarrhea with oliguria,a...As a diuretic and dampness-eliminating medicinal agent in traditional Chinese medicine(TCM),Zexie(Alismatis Rhizoma)is commonly used for symptoms such as dysuria,edema and abdominal distension,diarrhea with oliguria,and dizziness due to phlegm–fluid retention.Systematic phytochemical studies have revealed that the active components of Zexie(Alismatis Rhizoma)are primarily triterpenoids,along with sesquiterpenes,polysaccharides,sterols,alkaloids,phenolic acids,and lignans.These components form the material basis for its pharmacological activities.Recent breakthroughs in pharmacological research have expanded beyond its traditionally recognized diuretic and anti-inflammatory effects:Its antiurolithiasis effect has been clearly linked to inhibiting the crystallization of stone components and promoting stone expulsion;its renal protective effect can ameliorate kidney injury by reducing oxidative stress and suppressing inflammatory responses in renal tissues;its lipid-lowering mechanism involves regulating lipid metabolism pathways and reducing lipid deposition;in terms of anticancer activity,it exhibits proliferation inhibition and apoptosis induction in various tumor cells such as liver,lung,and colon cancers;additionally,it shows significant antibacterial activity against pathogens,including Escherichia coli and Staphylococcus aureus.展开更多
This study examines the evolving use of synthetic chemicals in intensive agriculture over the past decade.It highlights the negative impacts of chemical inputs on soil health and ecosystem integrity and recommends kno...This study examines the evolving use of synthetic chemicals in intensive agriculture over the past decade.It highlights the negative impacts of chemical inputs on soil health and ecosystem integrity and recommends knowledge-sharing platforms,soil protection laws,and collaborative efforts between regulatory agencies and agricultural experts.The study emphasizes the need for a balanced approach that includes natural methods alongside synthetic chemicals,particularly herbicides.Ten years ago,farmers primarily used urea,DAP,and potassium for nutrients.However,increased awareness,market forces,and government subsidies have led to a significant rise in herbicide use as a cost-effective weed management strategy.Over the past decade,synthetic fertilizer use for cotton cultivation has increased by 80%,leading to deteriorating soil quality.Paddy cultivation has decreased by 23%,while cotton cultivation has increased by 20.4%due to higher economic incentives.Currently,89.1%of farmers use herbicides,compared to 97.2%who did not a decade ago.Insecticide use has also surged,with 97.8%of farmers applying 1.5 liters or more per acre.The excessive use of chemicals threatens soil fertility and disrupts the ecosystem’s balance.This article explores the reasons behind the adoption of chemical-intensive farming practices and offers insights into farmers’decision-making processes.The careful use of synthetic chemicals is essential to safeguard soil health and maintain ecological balance.展开更多
Recently,diffusion models have emerged as a promising paradigm for molecular design and optimization.However,most diffusion-based molecular generative models focus on modeling 2D graphs or 3D geom-etries,with limited ...Recently,diffusion models have emerged as a promising paradigm for molecular design and optimization.However,most diffusion-based molecular generative models focus on modeling 2D graphs or 3D geom-etries,with limited research on molecular sequence diffusion models.The International Union of Pure and Applied Chemistry(IUPAC)names are more akin to chemical natural language than the simplified molecular input line entry system(SMILES)for organic compounds.In this work,we apply an IUPAC-guided conditional diffusion model to facilitate molecular editing from chemical natural language to chemical language(SMILES)and explore whether the pre-trained generative performance of diffusion models can be transferred to chemical natural language.We propose DiffIUPAC,a controllable molecular editing diffusion model that converts IUPAC names to SMILES strings.Evaluation results demonstrate that our model out-performs existing methods and successfully captures the semantic rules of both chemical languages.Chemical space and scaffold analysis show that the model can generate similar compounds with diverse scaffolds within the specified constraints.Additionally,to illustrate the model’s applicability in drug design,we conducted case studies in functional group editing,analogue design and linker design.展开更多
Difluoromethyl compounds are widely found in natural products,bioactive molecule and pharmaceuticals.A visible-light induced difluoromethylation/cyclization of 2-aryl indoles is described to construct indolo[2,1-a]iso...Difluoromethyl compounds are widely found in natural products,bioactive molecule and pharmaceuticals.A visible-light induced difluoromethylation/cyclization of 2-aryl indoles is described to construct indolo[2,1-a]isoquinolin-6(5H)-one derivatives using the inexpensive and easy-to-handle HCF_(2)SO_(2)Na as an HCF2 sources.Diverse difluoromethylated indolo[2,1-a]isoquinolines were readily obtained in moderate to good yields.Mechanistic studies demonstrate that the reaction may involve a radical process.展开更多
Solid-state electrolytes(SSEs),as the core component within the next generation of key energy storage technologies-solid-state lithium batteries(SSLBs)-are significantly leading the development of future energy storag...Solid-state electrolytes(SSEs),as the core component within the next generation of key energy storage technologies-solid-state lithium batteries(SSLBs)-are significantly leading the development of future energy storage systems.Among the numerous types of SSEs,inorganic oxide garnet-structured superionic conductors Li7La3Zr2O12(LLZO)crystallized with the cubic Iaˉ3d space group have received considerable attention owing to their highly advantageous intrinsic properties encompassing reasonable lithium-ion conductivity,wide electrochemical voltage window,high shear modulus,and excellent chemical stability with electrodes.However,no SSEs possess all the properties necessary for SSLBs,thus both the ionic conductivity at room temperature and stability in ambient air regarding cubic garnet-based electrolytes are still subject to further improvement.Hence,this review comprehensively covers the nine key structural factors affecting the ion conductivity of garnet-based electrolytes comprising Li concentration,Li vacancy concentration,Li carrier concentration and mobility,Li occupancy at available sites,lattice constant,triangle bottleneck size,oxygen vacancy defects,and Li-O bonding interactions.Furthermore,the general illustration of structures and fundamental features being crucial to chemical stability is examined,including Li concentration,Li-site occupation behavior,and Li-O bonding interactions.Insights into the composition-structure-property relations among cubic garnet-based oxide ionic conductors from the perspective of their crystal structures,revealing the potential compatibility conflicts between ionic transportation and chemical stability resulting from Li-O bonding interactions.We believe that this review will lay the foundation for future reasonable structural design of oxide-based or even other types of superionic conductors,thus assisting in promoting the rapid development of alternative green and sustainable technologies.展开更多
Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capac...Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capacity fading.Herein,the dual-strategy of Cr,B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature.Density functional theory(DFT)calculations prove that stable B-O and Cr-O bonds through the local gradient doping can significantly reduce the high-energy O 2p states of interfacial lattice O,which is also effective for the near-surface lattice O,thus greatly stabilizing the LLO surface,Besides,differential electrochemical mass spectrometry(DEMS)indicates that the Cr_(x)B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions,including allowing speedy Li^(+)migration,The voltage and capacity fading of the modified cathode(LLO-C_(r)B)are adequately suppressed,which are benefited from the uniformly dense cathode electrolyte interface(CEI)composed of balanced organic/inorganic composition.Therefore,the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g^(-1)(with a retention rate of 95.1%).This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.展开更多
The development of chemical technologies,which involves a multistage process covering laboratory research,scale‐up to industrial deployment,and necessitates interdisciplinary collaboration,is often accompanied by sub...The development of chemical technologies,which involves a multistage process covering laboratory research,scale‐up to industrial deployment,and necessitates interdisciplinary collaboration,is often accompanied by substantial time and economic costs.To address these challenges,in this work,we report ChemELLM,a domain‐specific large language model(LLM)with 70 billion parameters for chemical engineering.ChemELLM demonstrates state‐of‐the‐art performance across critical tasks ranging from foundational understanding to professional problem‐solving.It outperforms mainstream LLMs(e.g.,O1‐Preview,GPT‐4o,and DeepSeek‐R1)on ChemEBench,the first multidimensional benchmark for chemical engineering,which encompasses 15 dimensions across 101 distinct essential tasks.To support robust model development,we curated ChemEData,a purpose‐built dataset containing 19 billion tokens for pre‐training and 1 billion tokens for fine‐tuning.This work establishes a new paradigm for artificial intelligence‐driven innovation,bridging the gap between laboratory‐scale innovation and industrial‐scale implementation,thus accelerating technological advancement in chemical engineering.ChemELLM is publicly available at https://chemindustry.iflytek.com/chat.展开更多
基金financially supported by grants from the National Key Research and Development Program of China (No.2024YFE0102000)the National Natural Science Foundation of China (Nos.81925037,82321004,U22A20371,U24A20782,32170060,22177037,22207039,22307045)+6 种基金the Guangdong Major Project of Basic and Applied Basic Research (No.2023B0303000026)the Guangdong Natural Science Funds for Distinguished Young Scholars (No.2022B1515020028,China)the Guangdong International Science and Technology Cooperation Base (No.2021A0505020015,China)the Guangdong Basic and Applied Basic Research Foundation (Nos.2023B1515040016,2023A1515110388)the Innovative and Research Teams Project of Guangdong Higher Education Institution (No.2021KCXTD001,China)the Guangzhou Science and Technology Project (Nos.202206010020,2024A04J6241,2023A04J0080,China)the Fundamental Research Funds for the Central Universities (Nos.21623105,21624210)。
文摘Mangicol-type sesterterpenoids possess potent anti-inflammatory activity,characterized by a 5-5-6-5tetracyclic carbon skeleton formed by mangicdiene synthase Fg MS.Two proposed mechanisms for mangicdiene formation involve either C6-C10 cyclization(path a) or C2-C10 cyclization(path b) after the C10carbocation formation,but neither has been experimentally validated.Here,we have identified a second mangicdiene synthase Man D,which is derived from Fusarium sp.JNU-XJ070152-01 and shares high amino acid sequence identity with Fg MS.Through heterologous expression of man D in Aspergillus oryzae NSAR1,we observed production not only of mangicdiene(1) and variecoltetraene(2),previously identified by expression of Fg MS in Escherichia coli,but also two novel sesterterpene skeletons fusadiene(3)and fusatriene(4).The identification of fusadiene and fusatriene supports the occurrence of two key carbocation intermediates in path b,thus experimentally confirming that mangicdiene is built via path b for the first time,consistent with previous density functional theory(DFT) calculation results.
基金supported by the National Natural Sci-ence Foundation of China(Nos.22478263,22308230)Natural Science Foundation of Sichuan(No.2024NSF-SC1134)+2 种基金China Postdoctoral Science Foundation(No.2024T170612)111 center(B17030)the Fun-damental Research Funds for the Central Universities.
文摘Optically pure chiral chemicals are important building blocks with widespread applications across mul-tiple scientific and industrial do-mains such as in pharmaceuticals,agrochemicals,and food,especially acting as precursors to synthesize biodegradable polymers.As an al-ternative to fossil resources,renew-able lignocellulosic biomass has been used to access chiral chemicals,due to the versatile inherent stere-ostructures and multiple functional groups,such as hydroxyl,carbonyl,and phenyl ether groups.Typically,as the two main units of(hemi)cel-lulose components in lignocellulosic biomass,D-xylose and D-glucose bear multiple chiral centers(e.g.,2R-3S-4R for D-xylose and 2R-3S-4R-5R for D-glucose).Lignin bearsβ-O-4 linkages,exhibiting(R,S/S,R)or(R,R/S,S)stereocenters at the side-chainαandβcarbon atoms.The valorization of biomass into optical-ly pure chiral chemicals is vital for developing a more sustainable future.This review discuss-es the production of typical chiral chemicals derived from biomass through chemocatalysis,including lactones(e.g.,R/S-valerolactone),carboxylic acids(e.g.,D/L-glyceric acid,D/L-lactic acid),polyols(e.g.,tetrose),furans,oligosaccharides,and others.Two strategies are generally employed.One approach involves first producing achiral platform chemicals from biomass,followed by the introduction of asymmetric catalysts to reconstruct stereocenters.The second relates to selectively preserving one or more inherent stereocenters in the natural biomass structure during complex cascade reactions in which biomass feedstock acts as a“chi-ral pool",thus eliminating the establishment of stereocenter.The feedstock,methods em-ployed,and enantioselectivity and applications of the target chiral chemicals are discussed.Despite these advances,the synthesis of optically pure chemicals from biomass is still in its in-fancy.The coming decade presents both extraordinary challenges and opportunities in biomass-derived chiral chemistry.Future research should be focused on:(1)integrating well-established asymmetric catalysis techniques and methods with biomass’s inherent chiral pools,presenting an unprecedented opportunity to expand the chemical space of sustainable chiral compounds;(2)mastering polyfunctional complexity of chiral chemicals through holis-tic utilization of biomass’multichiral centers;(3)unlocking lignin’s stereochemical treasury that represents the next frontier in biomass valorization.
文摘The development of intrinsically conductive piezoresistive sensors with high strain tolerance has garnered significant interest.While elastomeric polymers exhibit excellent strain capabilities,their utility in sensing applications has been limited by inherent challenges such as high electrical resistivity,poor aging resistance,and interfacial incompatibility.To address these limitations,hydroxyl-terminated polybutadiene(HTPB)-based polyurethane was chemically modified with acetylferrocene-polyaniline conductive moieties to enhance charge transport properties.Remarkably,this covalent functionalization endowed the resulting ferrocene-polyaniline hybrid polyurethane(FPHP)with a conductivity of2.33 n A at 1 V bias while preserving piezoresistive functionality.The FPHP demonstrated exceptional mechanical-electrical performance,achieving 254% elongation at break with strain-dependent gauge factors of 7.28(0%-12.5% strain,R^(2)=0.9504)and 19.66(12.5%-35.0% strain,R^(2)=0.9929).Further characterization revealed a rapid 0.60 s response time and stability over 3500 strain-release cycles at compression strain,underscoring its durability under repetitive loading.The FPHP sensor was capable of monitoring various human movements and recognizing writing signals.These advances establish a materials design paradigm for fabricating flexible sensors that synergistically integrate high deformability,tunable sensitivity,and robust operational stability,positioning FPHP as a promising candidate for next-generation wearable electronics and soft robotics.
基金the support of the National Natural Science Foundation of China(22575230)。
文摘Conventional error cancellation approaches separate molecules into smaller fragments and sum the errors of all fragments to counteract the overall computational error of the parent molecules.However,these approaches may be ineffective for systems with strong localized chemical effects,as fragmenting specific substructures into simpler chemical bonds can introduce additional errors instead of mitigating them.To address this issue,we propose the Substructure-Preserved Connection-Based Hierarchy(SCBH),a method that automatically identifies and freezes substructures with significant local chemical effects prior to molecular fragmentation.The SCBH is validated by the gas-phase enthalpy of formation calculation of CHNO molecules.Therein,based on the atomization scheme,the reference and test values are derived at the levels of Gaussian-4(G4)and M062X/6-31+G(2df,p),respectively.Compared to commonly used approaches,SCBH reduces the average computational error by half and requires only15%of the computational cost of G4 to achieve comparable accuracy.Since different types of local effect structures have differentiated influences on gas-phase enthalpy of formation,substituents with strong electronic effects should be retained preferentially.SCBH can be readily extended to diverse classes of organic compounds.Its workflow and source code allow flexible customization of molecular moieties,including azide,carboxyl,trinitromethyl,phenyl,and others.This strategy facilitates accurate,rapid,and automated computations and corrections,making it well-suited for high-throughput molecular screening and dataset construction for gas-phase enthalpy of formation.
基金supported by National Natural Science Foundation of China(22278241)a grant from the Institute Guo Qiang,Tsinghua University(2021GQG1016).
文摘Space exploration and manufacturing are of critical importance for scientific advancement,technological innovation,national security,and the acquisition of extraterrestrial resources.In view of this,chemical and biological nano-/micro-/meso-scale manufacturing provide complementary approaches to overcome key space exploration challenges by enabling the in-situ production of essential life-support materials,propellants,and other resources.This review examines the origin and historical evolution of space manufacturing and the latest advances across different environments—from orbital space stations and the lunar surface to Mars and asteroids.It is structured to present the current state of research,outline key manufacturing strategies and technologies,assess the technical and environmental challenges,and discuss emerging trends and future directions.Besides,the potential applications of emerging technologies such as synthetic biology and artificial intelligence in overcoming the limitations of microgravity,limited resources,and extreme conditions are discussed.Ultimately,this integrative review could serve to guide future development,from advancing space science and disruptive manufacturing to enabling interdisciplinary and application-level innovations.
基金sponsored by the Department of Defense,Defense Threat Reduction Agency under the Materials Science in Extreme Environments University Research Alliance,HDTRA1-20-2-0001。
文摘Chemical warfare agents(CWAs)remain a persistent hazard in many parts of the world,necessitating a deeper exploration of their chemical and physical characteristics and reactions under diverse conditions.Diisopropyl methylphosphonate(DIMP),a commonly used CWA surrogate,is widely studied to enhance our understanding of CWA behavior.The prevailing thermal decomposition model for DIMP,developed approximately 25 years ago,is based on data collected in nitrogen atmospheres at temperatures ranging from 700 K to 800 K.Despite its limitations,this model continues to serve as a foundation for research across various thermal and reactive environments,including combustion studies.Our recent experiments have extended the scope of decomposition analysis by examining DIMP in both nitrogen and zero air across a lower temperature range of 175℃ to 250℃.Infrared spectroscopy results under nitrogen align well with the established model;however,we observed that catalytic effects,stemming from decomposition byproducts and interactions with stainless steel surfaces,alter the reaction kinetics.In zero air environments,we observed a novel infrared absorption band.Spectral fitting suggests this band may represent a combination of propanal and acetone,while GCMS analysis points to vinyl formate and acetone as possible constituents.Although the precise identity of these new products remains unresolved,our findings clearly indicate that the existing decomposition model cannot be reliably extended to lower temperatures or non-nitrogen environments without further revisions.
基金supported by the National Key Research and Development Program of China (No.2023YFC3708005)the National Natural Science Foundation of China (Nos.21872102,22172080)the Fundamental Research Funds for the Central Universities (Nankai University,No.63241208)。
文摘Groundwater is a key part of the terrestrial ecosystem,but it is vulnerable to pollution in the context of chemical industry development.Treating contaminated groundwater is challenging due to its stable water quality,hidden contamination,and complex treatment requirements.Current research focuses on advanced treatment technologies,among which the advanced oxidation process(AOPs) of peroxomonosulfate(PMS) has great potential.Although there are many reviews of PMS-based AOP,most of them focus on surface water.This review aims to explore the activation reaction of PMS to groundwater by in-situ chemical oxidation(ISCO) technology,further study the reaction mechanism,compare the treatment effect of characteristic pollutants in the groundwater of the chemical industry park,propose new activation methods and catalyst selection,and provide guidance for future groundwater treatment research.
基金supported by the Yunnan Fundamental Research Projects(Grant Nos.202401AU070163 and 202501AT070298)the Yunnan Engineering Research Center Innovation Ability Construction and Enhancement Projects(Grant No.2023-XMDJ-00617107)+5 种基金the University Service Key Industry Project of Yunnan Province(Grant No.FWCY-ZD2024005)the Expert Workstation Support Project of Yunnan Province(Grant No.202405AF140069)the Scientific Research Foundation of Kunming University of Science and Technology(Grant No.20220122)the Analysis and Test Foundation of Kunming University of Science and Technology(Grant No.2023T20220122)the Natural Science Foundation of Inner Mongolia Autonomous Region of China(Grant No.2025QN02057)the Ordos City Strategic Pioneering Science and Technology Special Program for New Energy(Grant No.DC2400003365).
文摘Lithium metal batteries(LMBs)have been regarded as one of the most promising alternatives in the post-lithium battery era due to their high energy density,which meets the needs of light-weight electronic devices and long-range electric vehicles.However,technical barriers such as dendrite growth and poor Li plating/stripping reversibility severely hinder the practical application of LMBs.However,lithium nitrate(LiNO_(3))is found to be able to stabilize the Li/electrolyte interface and has been used to address the above challenges.To date,considerable research efforts have been devoted toward understanding the roles of LiNO_(3) in regulating the surface properties of Li anodes and toward the development of many effective strategies.These research efforts are partially mentioned in some articles on LMBs and yet have not been reviewed systematically.To fill this gap,we discuss the recent advances in fundamental and technological research on LiNO_(3) and its derivatives for improving the performances of LMBs,particularly for Li-sulfur(S),Li-oxygen(O),and Li-Li-containing transition-metal oxide(LTMO)batteries,as well as LiNO_(3)-containing recipes for precursors in battery materials and interphase fabrication.This review pays attention to the effects of LiNO_(3) in lithium-based batteries,aiming to provide scientific guidance for the optimization of electrode/electrolyte interfaces and enrich the design of advanced LMBs.
基金supported by The University of Hong Kong,China(109000487,109001694,204610401,and 204610519)National Natural Science Foundation of China(82402225)(to JH).
文摘Chemical exchange saturation transfer magnetic resonance imaging is an advanced imaging technique that enables the detection of compounds at low concentrations with high sensitivity and spatial resolution and has been extensively studied for diagnosing malignancy and stroke.In recent years,the emerging exploration of chemical exchange saturation transfer magnetic resonance imaging for detecting pathological changes in neurodegenerative diseases has opened up new possibilities for early detection and repetitive scans without ionizing radiation.This review serves as an overview of chemical exchange saturation transfer magnetic resonance imaging with detailed information on contrast mechanisms and processing methods and summarizes recent developments in both clinical and preclinical studies of chemical exchange saturation transfer magnetic resonance imaging for Alzheimer’s disease,Parkinson’s disease,multiple sclerosis,and Huntington’s disease.A comprehensive literature search was conducted using databases such as PubMed and Google Scholar,focusing on peer-reviewed articles from the past 15 years relevant to clinical and preclinical applications.The findings suggest that chemical exchange saturation transfer magnetic resonance imaging has the potential to detect molecular changes and altered metabolism,which may aid in early diagnosis and assessment of the severity of neurodegenerative diseases.Although promising results have been observed in selected clinical and preclinical trials,further validations are needed to evaluate their clinical value.When combined with other imaging modalities and advanced analytical methods,chemical exchange saturation transfer magnetic resonance imaging shows potential as an in vivo biomarker,enhancing the understanding of neuropathological mechanisms in neurodegenerative diseases.
基金supported by the Natural Science Foundation of Shanghai(No.20ZR1471600)the Science and Technology Commission of Shanghai Municipality(No.19DZ2271100)the Open Research Fund Program of CAS Key Laboratory of Energy Regulation Materials(No.ORFP2020–06)。
文摘A new electrochemical strategy for trifluoromethylation/cyclization using TfNHNHBoc as a CF_(3)source was established.This approach was realized by the direct electrolysis of Tf NHNHBoc under external oxidantfree and catalyst-free conditions,and afforded various trifluoromethylated oxindoles with good functional group compatibility and broad substrate scope.Preliminary mechanistic studies show that the reaction proceeds by a radical process.
文摘Achieving regioselectivity in radical cyclization reactions is of central importance,yet extremely challenging.Although Baldwin’s rules provided guidance on the addition of radical species with alkenes/alkynes,the ortho-/ipso-selectivity of the cyclic reaction between radical species(especially alkyl and alkenyl radical)and aryl groups is still ambiguous.Herein,we develop an electrochemically enabled regioselective ortho-(4+2)/ipso-(3+2)cyclization of alkyl/alkenyl radicals with aryl groups,which provides a series of tetrahydronaphthalene and spirocarbocycle derivatives,exhibiting a broad substrate scope and functional group tolerance.Alkyl/alkenyl radicals are generated by Cp2Fe-mediated electrochemical oxidative radical addition of benzylic malonates with alkenes and alkynes.The method avoids the use of chemical oxidant/base/noble metal,the pre-functionalization of substrates,and the over-oxidation of compounds.Theoretical studies reveal that the dominant factor promoting the alkene-preferred ortho-addition is the favorable interaction energy;the alkyne-preferred ipso-addition regioselectivity is controlled by the distortion energy.Notably,this strategy is regarded as an important supplement to Baldwin’s rules for radical cyclization.
基金supported by the National Natural Science Foundation of China,No.82101340(to FJ).
文摘Parkinson’s disease is a common neurodegenerative disease with movement disorders associated with the intracytoplasmic deposition of aggregate proteins such asα-synuclein in neurons.As one of the major intracellular degradation pathways,the autophagy-lysosome pathway plays an important role in eliminating these proteins.Accumulating evidence has shown that upregulation of the autophagy-lysosome pathway may contribute to the clearance ofα-synuclein aggregates and protect against degeneration of dopaminergic neurons in Parkinson’s disease.Moreover,multiple genes associated with the pathogenesis of Parkinson’s disease are intimately linked to alterations in the autophagy-lysosome pathway.Thus,this pathway appears to be a promising therapeutic target for treatment of Parkinson’s disease.In this review,we briefly introduce the machinery of autophagy.Then,we provide a description of the effects of Parkinson’s disease–related genes on the autophagy-lysosome pathway.Finally,we highlight the potential chemical and genetic therapeutic strategies targeting the autophagy–lysosome pathway and their applications in Parkinson’s disease.
基金financially supported by National Nature Science Foundation of China(81973284)Scientific Research Foundation of the Education Department of Liaoning Province(LJKZ0944).
文摘Angelica sinensis(A.sinensis),as a kind of Chinese medicine,has the effects of tonifying blood,promoting blood circulation,regulating menstrual flow,relieving pain,moistening bowel and so on.By consulting Sciencedirect database and Web of Science database,163 related articles were found,of which 36 were related to chemical composition and pharmacological activities of A.sinensis.In this paper,the chemical structures and different derivatives were systematically summarized by reviewing relevant literatures,and the pharmacological effects were also summarized.
文摘As a diuretic and dampness-eliminating medicinal agent in traditional Chinese medicine(TCM),Zexie(Alismatis Rhizoma)is commonly used for symptoms such as dysuria,edema and abdominal distension,diarrhea with oliguria,and dizziness due to phlegm–fluid retention.Systematic phytochemical studies have revealed that the active components of Zexie(Alismatis Rhizoma)are primarily triterpenoids,along with sesquiterpenes,polysaccharides,sterols,alkaloids,phenolic acids,and lignans.These components form the material basis for its pharmacological activities.Recent breakthroughs in pharmacological research have expanded beyond its traditionally recognized diuretic and anti-inflammatory effects:Its antiurolithiasis effect has been clearly linked to inhibiting the crystallization of stone components and promoting stone expulsion;its renal protective effect can ameliorate kidney injury by reducing oxidative stress and suppressing inflammatory responses in renal tissues;its lipid-lowering mechanism involves regulating lipid metabolism pathways and reducing lipid deposition;in terms of anticancer activity,it exhibits proliferation inhibition and apoptosis induction in various tumor cells such as liver,lung,and colon cancers;additionally,it shows significant antibacterial activity against pathogens,including Escherichia coli and Staphylococcus aureus.
文摘This study examines the evolving use of synthetic chemicals in intensive agriculture over the past decade.It highlights the negative impacts of chemical inputs on soil health and ecosystem integrity and recommends knowledge-sharing platforms,soil protection laws,and collaborative efforts between regulatory agencies and agricultural experts.The study emphasizes the need for a balanced approach that includes natural methods alongside synthetic chemicals,particularly herbicides.Ten years ago,farmers primarily used urea,DAP,and potassium for nutrients.However,increased awareness,market forces,and government subsidies have led to a significant rise in herbicide use as a cost-effective weed management strategy.Over the past decade,synthetic fertilizer use for cotton cultivation has increased by 80%,leading to deteriorating soil quality.Paddy cultivation has decreased by 23%,while cotton cultivation has increased by 20.4%due to higher economic incentives.Currently,89.1%of farmers use herbicides,compared to 97.2%who did not a decade ago.Insecticide use has also surged,with 97.8%of farmers applying 1.5 liters or more per acre.The excessive use of chemicals threatens soil fertility and disrupts the ecosystem’s balance.This article explores the reasons behind the adoption of chemical-intensive farming practices and offers insights into farmers’decision-making processes.The careful use of synthetic chemicals is essential to safeguard soil health and maintain ecological balance.
基金supported by the Yonsei University graduate school Department of Integrative Biotechnology.
文摘Recently,diffusion models have emerged as a promising paradigm for molecular design and optimization.However,most diffusion-based molecular generative models focus on modeling 2D graphs or 3D geom-etries,with limited research on molecular sequence diffusion models.The International Union of Pure and Applied Chemistry(IUPAC)names are more akin to chemical natural language than the simplified molecular input line entry system(SMILES)for organic compounds.In this work,we apply an IUPAC-guided conditional diffusion model to facilitate molecular editing from chemical natural language to chemical language(SMILES)and explore whether the pre-trained generative performance of diffusion models can be transferred to chemical natural language.We propose DiffIUPAC,a controllable molecular editing diffusion model that converts IUPAC names to SMILES strings.Evaluation results demonstrate that our model out-performs existing methods and successfully captures the semantic rules of both chemical languages.Chemical space and scaffold analysis show that the model can generate similar compounds with diverse scaffolds within the specified constraints.Additionally,to illustrate the model’s applicability in drug design,we conducted case studies in functional group editing,analogue design and linker design.
文摘Difluoromethyl compounds are widely found in natural products,bioactive molecule and pharmaceuticals.A visible-light induced difluoromethylation/cyclization of 2-aryl indoles is described to construct indolo[2,1-a]isoquinolin-6(5H)-one derivatives using the inexpensive and easy-to-handle HCF_(2)SO_(2)Na as an HCF2 sources.Diverse difluoromethylated indolo[2,1-a]isoquinolines were readily obtained in moderate to good yields.Mechanistic studies demonstrate that the reaction may involve a radical process.
基金supported by the National Natural Science Foundation of China(Nos.22171102 and 22090044)the National Key R&D Program of China(Nos.2021YFF0500502 and 2023YFA1506304)+2 种基金the Jilin Province Science and Technology Development Plan(No.20230101024JC)the"Medicine+X"crossinnovation team of Bethune Medical Department of Jilin University"Leading the Charge with Open Competition"construction project(No.2022JBGS04)the Jilin University Graduate Training Office(Nos.2021JGZ08 and 2022YJSJIP20).
文摘Solid-state electrolytes(SSEs),as the core component within the next generation of key energy storage technologies-solid-state lithium batteries(SSLBs)-are significantly leading the development of future energy storage systems.Among the numerous types of SSEs,inorganic oxide garnet-structured superionic conductors Li7La3Zr2O12(LLZO)crystallized with the cubic Iaˉ3d space group have received considerable attention owing to their highly advantageous intrinsic properties encompassing reasonable lithium-ion conductivity,wide electrochemical voltage window,high shear modulus,and excellent chemical stability with electrodes.However,no SSEs possess all the properties necessary for SSLBs,thus both the ionic conductivity at room temperature and stability in ambient air regarding cubic garnet-based electrolytes are still subject to further improvement.Hence,this review comprehensively covers the nine key structural factors affecting the ion conductivity of garnet-based electrolytes comprising Li concentration,Li vacancy concentration,Li carrier concentration and mobility,Li occupancy at available sites,lattice constant,triangle bottleneck size,oxygen vacancy defects,and Li-O bonding interactions.Furthermore,the general illustration of structures and fundamental features being crucial to chemical stability is examined,including Li concentration,Li-site occupation behavior,and Li-O bonding interactions.Insights into the composition-structure-property relations among cubic garnet-based oxide ionic conductors from the perspective of their crystal structures,revealing the potential compatibility conflicts between ionic transportation and chemical stability resulting from Li-O bonding interactions.We believe that this review will lay the foundation for future reasonable structural design of oxide-based or even other types of superionic conductors,thus assisting in promoting the rapid development of alternative green and sustainable technologies.
基金financially supported by the National Natural Science Foundation of China(No.12304077)the Natural Science Foundation of Science and Technology Department of Sichuan Province(No.23NSFSC6224)+3 种基金Sichuan Science and Technology Program(No.2024NSFSC0989)the Key Laboratory of Computational Physics of Sichuan Province(No.YBUJSWL-YB-2022-03)the Material Corrosion and Protection Key Laboratory of Sichuan Province(No.2023CL14 and No.2023CL01)the National Innovation Practice Project(No.202411079005S).
文摘Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capacity fading.Herein,the dual-strategy of Cr,B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature.Density functional theory(DFT)calculations prove that stable B-O and Cr-O bonds through the local gradient doping can significantly reduce the high-energy O 2p states of interfacial lattice O,which is also effective for the near-surface lattice O,thus greatly stabilizing the LLO surface,Besides,differential electrochemical mass spectrometry(DEMS)indicates that the Cr_(x)B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions,including allowing speedy Li^(+)migration,The voltage and capacity fading of the modified cathode(LLO-C_(r)B)are adequately suppressed,which are benefited from the uniformly dense cathode electrolyte interface(CEI)composed of balanced organic/inorganic composition.Therefore,the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g^(-1)(with a retention rate of 95.1%).This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.
文摘The development of chemical technologies,which involves a multistage process covering laboratory research,scale‐up to industrial deployment,and necessitates interdisciplinary collaboration,is often accompanied by substantial time and economic costs.To address these challenges,in this work,we report ChemELLM,a domain‐specific large language model(LLM)with 70 billion parameters for chemical engineering.ChemELLM demonstrates state‐of‐the‐art performance across critical tasks ranging from foundational understanding to professional problem‐solving.It outperforms mainstream LLMs(e.g.,O1‐Preview,GPT‐4o,and DeepSeek‐R1)on ChemEBench,the first multidimensional benchmark for chemical engineering,which encompasses 15 dimensions across 101 distinct essential tasks.To support robust model development,we curated ChemEData,a purpose‐built dataset containing 19 billion tokens for pre‐training and 1 billion tokens for fine‐tuning.This work establishes a new paradigm for artificial intelligence‐driven innovation,bridging the gap between laboratory‐scale innovation and industrial‐scale implementation,thus accelerating technological advancement in chemical engineering.ChemELLM is publicly available at https://chemindustry.iflytek.com/chat.
