Herein,3‑aminopropyltriethoxysilane(APTES)was used to modify F‑containing silica slag(SS)by simple grafting and served as a multifunctional barrier layer.The amino group(—NH2)in the amino‑modified SS(NH2‑SS)forms lig...Herein,3‑aminopropyltriethoxysilane(APTES)was used to modify F‑containing silica slag(SS)by simple grafting and served as a multifunctional barrier layer.The amino group(—NH2)in the amino‑modified SS(NH2‑SS)forms ligand bonds or hydrogen bonds with sulfur ions in lithium polysulfides(LiPSs),thus inhibiting the shuttle effect.Electrochemical analyses demonstrated that lithium‑sulfur(Li‑S)batteries employing the NH2‑SS interlayer exhibited discharge specific capacities of 1048 and 789 mAh·g^(-1) at 0.2C and 2C,respectively,and even at 4C,the initial discharge specific capacity remained at 590 mAh·g^(-1),outperforming the Li‑S battery with unmodified SS as the interlayer.展开更多
Sulfur is closely associated with various types of ore deposits,particularly orogenic gold(Au)systems,where sulfur-bearing melts and fluids play a critical role in transporting oreforming elements essential for ore fo...Sulfur is closely associated with various types of ore deposits,particularly orogenic gold(Au)systems,where sulfur-bearing melts and fluids play a critical role in transporting oreforming elements essential for ore formation.The widely accepted metamorphic devolatilization model suggests that compositionally fertile sedimentary rocks serve as potential gold sources.Therefore,understanding sulfur behavior during prograde metamorphism is essential for elucidating the mechanisms underlying metal activation and mobility.In this study,we conducted in-situ sulfur isotope(δ^(34)S)analyses using secondary ion mass spectrometry(SIMS)on samples from the Hongshankou area,a representative Barrovian-type metamorphic sequence characterized by intermediate pressure-temperature(P-T)conditions.This sequence comprises the biotite,garnet,staurolite,and kyanite zones.Our results show a systematic increase in δ^(34)S values(from 3.1‰ to 5.5‰)coupled with a progressive decrease in total sulfur content(from 320 ppm to 165 ppm)as metamorphic grade increases.The most pronounced sulfur mobilization occurs between the garnet and staurolite zones.In all analyzed samples,Au or Au-bearing minerals predominantly occur along the edges or within pyrite grains,highlighting the critical role of pyrite breakdown in controlling gold mobility.Thus,sulfur isotope fractionation provides robust constraints for quantitatively assessing sulfur mobility during metamorphism.These findings reinforce the concept that metasedimentary rocks and their metamorphic fluids represent fertile sources of Au and other metals enriched in orogenic gold deposits.展开更多
Sluggish kinetics coupled with parasitic shuttling reactions are pivotal challenges hindering the performance of lithium-sulfur(Li-S)batteries.Improving areal capacity and cyclability of Li-S batteries can be achieved...Sluggish kinetics coupled with parasitic shuttling reactions are pivotal challenges hindering the performance of lithium-sulfur(Li-S)batteries.Improving areal capacity and cyclability of Li-S batteries can be achieved by addressing these challenges.A composite sulfur host material is synthesized herein by in situ anchoring ultrafine cobalt-iron phosphide nanoparticles(5-7 nm)onto a hollow mesoporous carbon sphere(HMCS)framework.This strategy achieved exceptional spatial restriction and a high density of catalytically active sites through the encapsulation of sulfur within a hollow-structured framework.Specifically,HMCS expedites rapid Li_(2)S nucleation kinetics,while CoFeP facilitates robust Li_(2)S dissolution kinetics by mitigating decomposition barriers.This synergistic integration equips CoFeP@HMCS with robust bi-directional catalytic activity,significantly promoting interracial charge-transfer,facilitate sulfu r multistep catalytic conversion,and inhibiting shuttling.Consequently,the battery exhibits excellent rate performance(991 mA h g^(-1) at 5.0 C)and retains a high areal capacity of 6.06 mA h cm^(-2) after 200 cycles under a high areal sulfur loading of 8.2 mg cm^(-2) but a low electrolyte/sulfur ratio of 4.8μL mg^(-1).This work contributes to enhancing the practical specific capacity of lithium-sulfur batteries and deepens the understanding of catalysts enabling bidirectional electrocatalytic sulfur conversion.展开更多
To comprehensively explore the impact of binder content on the mechanical properties of the Polymer bonded explosive(PBX)substitute material(Polymer-bonded Analogue Explosive(PAE)—it is renowned for its outstanding h...To comprehensively explore the impact of binder content on the mechanical properties of the Polymer bonded explosive(PBX)substitute material(Polymer-bonded Analogue Explosive(PAE)—it is renowned for its outstanding high-temperature resistance,exceptional mechanical properties,excellent chemical stability,and superior electrical insulation),a series of experiments are meticulously carried out.The dynamic and static mechanical properties,along with the microstructure of PAE,are precisely measured through the Split Hopkinson Pressure Bar(SHPB)test,static compression tests,and Scanning Electron Microscopy(SEM).The dynamic performance test outcomes clearly indicate that both the binder content(2%,4%,6%)and temperature(25℃,45℃,70℃)exert a substantial influence on the dynamic mechanical properties of PAE.Specifically,as the binder content increases,the elasticmodulus increases,demonstrating higher stiffness,and the longer failure duration represents a prolonged fracture process rather than an improved deformation strain to failure.This means the strength-related stiffness rises with binder content,but the overall ductility does not increase.Notably,PAE with 2%the Ethylene-Vinyl Acetate Copolymer(EVA)—it bonds well with a variety ofmaterials,such asmetal,wood,and plastic—exhibits distinct plastic deformation behavior,while PAE samples with 4%and 6%EVA display evident brittle fracture characteristics.Additionally,the mechanical properties of PAE are highly sensitive to temperature variations.Among the tested temperatures,PAE showcases the most favorable performance at 45℃.The static performance test results reveal that an increment in binder content effectively helps to reduce the temperature sensitivity of temperature(-40℃,25℃,50℃,70℃)on PAE and enhance its static mechanical properties.The maximum compressive strength gradually diminishes as the temperature rises.However,it should be noted that an excessively high binder content will undermine the mechanical properties of PAE.With the increase in binder content,the compressive modulus demonstrates relatively stable changes under both lowtemperature and high-temperature conditions.The SEM analysis results demonstrate that,aside fromthe initial defects inherent in the material preparation process,the components of PAE are firmly combined.Throughout the tests,no new pores or microcracks emerge,which strongly indicates that the mechanical properties of PAE remain stable.展开更多
Long-life energy storage batteries are integral to energy storage systems and electric vehicles,with lithium-ion batteries(LIBs)currently being the preferred option for extended usage-life energy storage.To further ex...Long-life energy storage batteries are integral to energy storage systems and electric vehicles,with lithium-ion batteries(LIBs)currently being the preferred option for extended usage-life energy storage.To further extend the life span of LIBs,it is essential to intensify investments in battery design,manufacturing processes,and the advancement of ancillary materials.The pursuit of long durability introduces new challenges for battery energy density.The advent of electrode material offers effective support in enhancing the battery’s long-duration performance.Often underestimated as part of the cathode composition,the binder plays a pivotal role in the longevity and electrochemical performance of the electrode.Maintaining the mechanical integrity of the electrode through judicious binder design is a fundamental requirement for achieving consistent long-life cycles and high energy density.This paper primarily concentrates on the commonly employed cathode systems in lithium-ion batteries,elucidates the significance of binders for both,discusses the application status,strengths,and weaknesses of novel binders,and ultimately puts forth corresponding optimization strategies.It underscores the critical function of binders in enhancing battery performance and advancing the sustainable development of lithium-ion batteries,aiming to offer fresh insights and perspectives for the design of high-performance LIBs.展开更多
Hard carbon(HC)in sodium-ion batteries is searched by numerous investigations,which can offer the excellent performance of reversible Na^(+)insertion and extraction.The covalent heteroatom doping in HC is recently wor...Hard carbon(HC)in sodium-ion batteries is searched by numerous investigations,which can offer the excellent performance of reversible Na^(+)insertion and extraction.The covalent heteroatom doping in HC is recently worth concentrating,which can dilate the interlayer spacing of graphite to adjust the electrochemical storage performance in carbon anodes.However,the reported doping strategies of the modified HC have only resulted in limited improvement,especially unobvious effects on tuning porous structure.In this study,tannin extract and K_(2)SO_(4) are respectively utilized as carbon source and sulfur source for the fabrication of HC,in which K_(2)SO_(4) can contribute to the heteroatom doping,and the pore forming as well.The tannin-derived sulfur-doped carbon anode shows the excellent cycle stability,achieving a high reversible capacity of 520.5 mAh/g at a current density of 100 mA/g.Even after 500 cycles at a current density of 3 A/g,a high specific capacity of 236.7 mAh/g and a capacity retention rate of 92.6%can be reserved.Compared with the initial carbon,the adsorption energy of Na^(+)is multifold times higher,whereas Na^(+)diffusion energy barriers manyfold decrease.Moreover,the full battery assembled with Na_(3)V_(2)(PO_(4))_(3)/tannin-based HC demonstrates a stable cycling performance.This work can manifest the potentiality of the tannin-based electrode as anode for a high-performance sodium-ion batteries(SIBs),which could especially offer an explanation of Na^(+)storage and solid-electrolyte interface(SEI)stability to the electrochemical performance.展开更多
Lithium-sulfur(Li-S)batteries require efficient catalysts to accelerate polysulfide conversion and mitigate the shuttle effect.However,the rational design of catalysts remains challenging due to the lack of a systemat...Lithium-sulfur(Li-S)batteries require efficient catalysts to accelerate polysulfide conversion and mitigate the shuttle effect.However,the rational design of catalysts remains challenging due to the lack of a systematic strategy that rationally optimizes electronic structures and mesoscale transport properties.In this work,we propose an autogenously transformed CoWO_(4)/WO_(2) heterojunction catalyst,integrating a strong polysulfide-adsorbing intercalation catalyst with a metallic-phase promoter for enhanced activity.CoWO_(4) effectively captures polysulfides,while the CoWO_(4)/WO_(2) interface facilitates their S-S bond activation on heterogenous catalytic sites.Benefiting from its directional intercalation channels,CoWO_(4) not only serves as a dynamic Li-ion reservoir but also provides continuous and direct pathways for rapid Li-ion transport.Such synergistic interactions across the heterojunction interfaces enhance the catalytic activity of the composite.As a result,the CoWO_(4)/WO_(2) heterostructure demonstrates significantly enhanced catalytic performance,delivering a high capacity of 1262 mAh g^(−1) at 0.1 C.Furthermore,its rate capability and high sulfur loading performance are markedly improved,surpassing the limitations of its single-component counterparts.This study provides new insights into the catalytic mechanisms governing Li-S chemistry and offers a promising strategy for the rational design of high-performance Li-S battery catalysts.展开更多
Ferroptosis has exhibited great potential in therapies and intracellular reducing agents of sulfur species(RSSs) in the thiol-dependent redox systems are crucial in ferroptosis.This makes the simultaneous detection of...Ferroptosis has exhibited great potential in therapies and intracellular reducing agents of sulfur species(RSSs) in the thiol-dependent redox systems are crucial in ferroptosis.This makes the simultaneous detection of multiple RSSs significant for evaluating ferroptosis therapy.However,the traditional techniques,including fluorescent(FL) imaging and electrospray ionization-based mass spectrometry(MS) detection,cannot achieve the discrimination of different RSSs.Herein,simultaneous MS detection of multiple RSSs,including cysteine(Cys),homocysteine(Hcy),glutathione(GSH) and hydrogen sulfide(H_(2)S),was obtained upon enhancing ionization efficiency by a fluorescent probe(NBD-O-1).Based on the interaction between NBD-O-1 and RSSs,the complex of RSSs with a fragment of NBD-O-1 can be generated,which can be easily ionized for MS detection in the negative mode.Therefore,the intracellular RSSs can be well detected upon the incubation of He La cells with the probe of NBD-O-1,exhibiting the total RSS levels by the FL imaging and further providing expression of each RSS by enhanced MS detection.Furthermore,the RSSs during ferroptosis in He La cells have been evaluated using the present strategy,demonstrating the potential for ferroptosis examinations.This work has made an unconventional application of a fluorescent probe to enhance the detection of multiple RSSs by MS,providing significant molecular information for addressing the ferroptosis mechanism.展开更多
The development of catalytic multicomponent reactions for constructing complex organic scaffolds from readily accessible commodity chemicals is a key pursuit in contemporary synthetic chemistry.Current methods for syn...The development of catalytic multicomponent reactions for constructing complex organic scaffolds from readily accessible commodity chemicals is a key pursuit in contemporary synthetic chemistry.Current methods for synthesizing thioesters primarily rely on the acylation of thiols,which produces substantial waste and requires malodorous,unstable sulfur sources.In this work,we introduce a photocatalyzed hydrogen transfer strategy that enables a three-component synthesis of thioesters using abundant primary alcohols,easily available alkenes and elemental sulfur under mild conditions.This protocol demonstrates broad applicability and high chemo-and regioselectivity for both primary alcohols and alkenes,highlighting the advantage and potential of photo-mediated hydrogen transfer in facilitating multicomponent reactions using primary alcohol and elemental sulfur feedstocks.展开更多
Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implem...Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implementation remains a significant challenge.Herein,we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs.Specifically,polypyrrole(PPy)is in situ vapor-phase polymerized on the surface of N-doped TiO_(2) nanorods supported on carbon cloth(N-TiO_(2)/CC),thereby forming a well-defined p–n heterojunction.This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field.Thus,the PPy@N-TiO_(2)/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur,enabling ultrafast sulfur redox dynamics,as convincingly validated by both theoretical simulations and experimental results.Consequently,the PPy@N-TiO_(2)/CC PALSB achieves a high discharge capacity of 1653 mAh g^(−1),reaching 98.7%of the theoretical value.Furthermore,5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g^(−1),achieving dual-mode energy harvesting capabilities.This work successfully integrates solar energy conversion and storage within a rechargeable battery system,providing a promising strategy for sustainable energy storage technologies.展开更多
The rapid increase in traffic loads and frequencies has rendered conventional asphalt pavement inadequate to maintain its durability under tropical climates.This challenge has necessitated the exploration of new sourc...The rapid increase in traffic loads and frequencies has rendered conventional asphalt pavement inadequate to maintain its durability under tropical climates.This challenge has necessitated the exploration of new sources of modified asphalt with enhanced stiffness and superior performance at high temperatures.Natural rubber(NR)is a renewable biopolymer that has received growing interest as a modifier for asphalt binders.Cup lump rubber(CLR),a type of NR,is used to enhance asphalt properties and improve the performance of road pavements.This study evaluates the influence of wax-based surfactants(WS)on CLR-modified asphalt binder(CMB).The assessment focuses on changes in chemical characteristics,rheological behaviour,activation energy,and morphology.Four concentrations of WS(0.1%,0.15%,0.2%,and 0.25%)were incorporated into CMB.Analysis of CMB chemical changes showed that viscosity increased due to higher sulfoxide,carbonyl,and aromatic bond indices.These chemical modifications contributed to improved resistance of the binder to heat-induced deterioration.In both unaged and aged CMB samples,the incorporation of WS reduced the sulfoxide index of the binder.Rheological analysis indicated that CMB improved rutting resistance and anti-ageing performance,while WS further enhanced fatigue resistance.Activation energy analysis suggested that the combination of CMB with 0.15%WS produced the most favourable enhancement.Micrograph results showed that WS improved binder homogeneity and interconnectivity.In conclusion,the findings indicated that incorporating 0.15%WS into CMB enhanced the performance and durability of the asphalt pavement.展开更多
Layered oxides present compelling potential as cathode materials for sodium-ion batteries(SIBs).However,challenges including interfacial instability and sluggish reaction kinetics critically limit their rate capabilit...Layered oxides present compelling potential as cathode materials for sodium-ion batteries(SIBs).However,challenges including interfacial instability and sluggish reaction kinetics critically limit their rate capability and cycling performance.Herein,we introduce the water-soluble sodium polyacrylate(NaPAA)binder as a promising approach to mitigating these issues in P2-type layered oxides.The NaPAA binder facilitates the formation of a uniform Na^(+) conductive interfacial film,which protects the cathode against electrolyte-induced corrosion and effectively inhibits the dissolution of transition metals in P2-Na_(0.85)Li_(0.12)Ni_(0.22)Mn_(0.66)O_(2)(NLNMO).Furthermore,we elucidate the mechanism by which the NaPAA binder dynamically regulates the coordination of free anions at the electrode-electrolyte interface.This regulation reduces solvent decomposition and promotes the formation of a stable,ionically conductive layer.Consequently,the P2-NLNMO@NaPAA integrated electrode exhibits enhanced electrochemical performance,achieving an 89.2%capacity retention after 200 cycles at 0.2 C and delivering an initial capacity of 102.9 mA h g^(-1) even at 0℃.This study advances the fundamental understanding of binder-mediated interface engineering and demonstrates a scalable and eco-friendly manufacturing pathway for high-performance SIBs.展开更多
In this work,ofloxacin(OFL),a kind of frequently detected antibiotic in groundwater,was selected to explore its impact(at ng/L-μg/L-level)on denitrification performance in an autotrophic denitrification system driven...In this work,ofloxacin(OFL),a kind of frequently detected antibiotic in groundwater,was selected to explore its impact(at ng/L-μg/L-level)on denitrification performance in an autotrophic denitrification system driven by pyrite/sulfur(FeS2/S0).Results showed that OFL restrained nitrate removal efficiency,and the inhibition degree was positively related to the concentration of OFL.After being exposed to increased OFL(200 ng/L-100μg/L)for 69 days,higher inhibition of electron transport activity(ETSA),enzyme activities of nitrate reductase(NAR),and nitrite reductase(NIR)were acquired.Meanwhile,the extracellular protein(PN)content of sludge samples was remarkably stimulated by OFL to resist the augmented toxicity.OFL contributed to increased microbial diversity and sulfur/sulfide oxidation functional genes in ng/L-level bioreactors,whereas led to a decline inμg/L level experiments.With OFL at concentrations of 200 ng/L and 100μg/L,the whole expression of 10 key denitrification functional genes was depressed,and the higher the OFL concentration,the lower the expression level.However,no significant proliferation of antibiotic resistance genes(ARGs)either in 200 ng/L-OFL or 100μg/L-OFL groups was observed.Two-factor correlation analysis results indicated that Thiobacillus,Anaerolineae,Anaerolineales,and Nitrospirae might be the main hosts of existing ARGs in this system.展开更多
The development of high-sulfur-loading Li-S batteries is a key prerequisite for their commercial applications.This requires to surmount the huge polarization,severe polysulfide shuttling and drastic volume change caus...The development of high-sulfur-loading Li-S batteries is a key prerequisite for their commercial applications.This requires to surmount the huge polarization,severe polysulfide shuttling and drastic volume change caused by electrode thickening.High-strength polar binders are ideal for constructing robust and long-life high-loading sulfur cathodes but show very weak interfacial interaction with non-polar sulfur materials.To address this issue,this work devises a highly integrated sulfur@polydopamine/highstrength binder composite cathodes,targeting long-lasting and high-sulfur-loading Li-S batteries.The super-adhesion polydopamine(PD)can form a uniform nano-coating over the graphene/sulfur(G-S)surface and provide strong affinity to the cross-linked polyacrylamide(c-PAM)binder,thus tightly integrating sulfur with the binder network and greatly boosting the overall mechanical strength/conductivity of the electrode.Moreover,the PD coating and c-PAM binder rich in polar groups can form two effective blockades against the effusion of soluble polysulfides.As such,the 4.5 mg cm−2 sulfur-loaded G-S@PD-c-PAM cathode achieves a capacity of 480 mAh g−1 after 300 cycles at 1 C,while maintaining a capacity of 396 mAh g−1 after 50 cycles at 0.2 C when the sulfur loading rises to 9.1 mg cm−2.This work provides a system-wide concept for constructing high-loading sulfur cathodes through integrated structural design.展开更多
Na-alginate as a binder in an aqueous solvent has been applied in the preparation of sulfur cathodes for lithium-sulfur batteries.Their electrochemical performances have been investigated by a charge-discharge cycle t...Na-alginate as a binder in an aqueous solvent has been applied in the preparation of sulfur cathodes for lithium-sulfur batteries.Their electrochemical performances have been investigated by a charge-discharge cycle test and electrochemical impedance spectroscopy (EIS).The EIS tests indicated that the alginate sulfur cathode had lower resistance and better kinetic characteristics than those of the poly (vinylidene fluoride) (PVDF) sulfur cathode using PVDF as a binder in a N-methy-2-pyrrolidone (NMP) solvent.The charge-discharge tests showed that the discharge capacity and the capacity retention rate of Na-alginate sulfur cathode were 508 mAh·g-1and 65.4% at the 50th cycle with a current density of 335 mA·g-1.Compared with PVDF sulfur cathode,the alginate sulfur cathode showed a remarkably better cycle performance.These results show that the alginate binder has promising potential for lithium-sulfur battery applications.展开更多
Lithium sulfur(Li-S)batteries are the promising power sources,but their commercialization is significantly impeded by poor energy-storage functions at high sulfur loading.Here we report that such an issue can be effec...Lithium sulfur(Li-S)batteries are the promising power sources,but their commercialization is significantly impeded by poor energy-storage functions at high sulfur loading.Here we report that such an issue can be effectively addressed by using a mussel-inspired binder comprised of chitosan grafted with catecholic moiety for sulfur cathodes.The resulting sulfur cathodes possess a high loading up to 12.2 mg cm-2 but also exhibit one of the best electrochemical properties among their counterparts.The excellent performances are attributed to the strong adhesion of the binder to sulfur particles,conducting agent,current collector,and polysulfide.The versatile adhesion effectively increases the sulfur loading,depresses the shuttle effect,and alleviates mechanical pulverization during cycling processes.The present investigation offers a new insight into high performance sulfur cathodes through a bio-adhesion viewpoint.展开更多
Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large...Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large volume change and active material loss in lithium-ion batteries during prolonged cycles. Herein, a hydrophilic polymer poly(methyl vinyl ether-alt-maleic acid) (PMVEMA) was explored as a dual-functional aqueous binder for the preparation of high-performance silicon anode and sulfur cathode. Benefiting from the dual functions of PMVEMA, i.e., the excellent dispersion ability and strong binding forces, the as-prepared electrodes exhibit improved capacity, rate capability and long-term cycling performance. In particular, the as-prepared Si electrode delivers a high initial discharge capacity of 1346.5 mAh g^(−1) at a high rate of 8.4 A/g and maintains 834.5 mAh g^(−1) after 300 cycles at 4.2 A/g, while the as-prepared S cathode exhibits enhanced cycling performance with high remaining discharge capacities of 663.4 mAh g^(−1) after 100 cycles at 0.2 C and 487.07 mAh g^(−1) after 300 cycles at 1 C, respectively. These encouraging results suggest that PMVEMA could be a universal binder to facilitate the green manufacture of both anode and cathode for high-capacity energy storage systems.展开更多
Volume expansion and polysulfide shuttle effect are the main barriers for the commercialization of lithium-sulfur(Li-S) battery.In this work,we in-situ polymerized a cross-linked binder in sulfur cathode to solve the ...Volume expansion and polysulfide shuttle effect are the main barriers for the commercialization of lithium-sulfur(Li-S) battery.In this work,we in-situ polymerized a cross-linked binder in sulfur cathode to solve the aforementioned problems using a facile method under mild conditions.Polycarbonate diol(PCDL),triethanolamine(TEA) and hexamethylene diisocyanate(HDI) were chosen as precursors to prepare the cross-linked binder.The in-situ polymerized binder(PTH) builds a strong network in sulfur cathode,which could restrain the volume expansion of sulfu r.Moreover,by adopting functional groups of oxygen atoms and nitrogen atoms,the binder could effectively facilitate transportation of Li-ion and adsorb polysulfide chemically.The Li-S battery with bare sulfur and carbon/sulfur composite cathodes and cross-linked PTH binder displays much better electrochemical performance than that of the battery with PVDF.The PTH-bare S cathode with a mass loading of 5.97 mg/cm^2 could deliver a capacity of 733.3 mAh/g at 0.2 C,and remained 585.5 mAh/g after 100 cycles.This in-situ polymerized binder is proved to be quite effective on restraining the volume expansion and suppressing polysulfide shuttle effect,then improving the electrochemical performance of Li-S battery.展开更多
Lithium-sulfur(Li-S)batteries are promising next-generation high energy density batteries but their practical application is hindered by several key problems,such as the intermediate polysulfide shuttling and the elec...Lithium-sulfur(Li-S)batteries are promising next-generation high energy density batteries but their practical application is hindered by several key problems,such as the intermediate polysulfide shuttling and the electrode degradation caused by the sulfur volume changes.Binder acts as one of the most essential components to build the electrodes of Li-S batteries,playing vital roles in improving the performance and maintaining the integrity of the cathode structure during cycling,especially those with high sulfur loadings.To date,tremendous efforts have been devoted to improving the properties of binders,in terms of the viscosity,elasticity,stability,toughness and conductivity,by optimizing the composition and structure of polymer binders.Moreover,the binder modification endows them strong polysulfide trapping ability to suppress the shuttling and decreases the swelling to maintain the porous structure of cathode.In this review,we summarize the recent progress on the binders for Li-S batteries and discuss the various routes,including the binder combination use,functionalization,in-situ polymerization and ion cross-linking,etc.,to enhance their performance in stabilizing the cathode,building the high sulfur loading electrode and improving the cyclic stability.At last,the design principles and the problems in further applications are also highlighted.展开更多
文摘Herein,3‑aminopropyltriethoxysilane(APTES)was used to modify F‑containing silica slag(SS)by simple grafting and served as a multifunctional barrier layer.The amino group(—NH2)in the amino‑modified SS(NH2‑SS)forms ligand bonds or hydrogen bonds with sulfur ions in lithium polysulfides(LiPSs),thus inhibiting the shuttle effect.Electrochemical analyses demonstrated that lithium‑sulfur(Li‑S)batteries employing the NH2‑SS interlayer exhibited discharge specific capacities of 1048 and 789 mAh·g^(-1) at 0.2C and 2C,respectively,and even at 4C,the initial discharge specific capacity remained at 590 mAh·g^(-1),outperforming the Li‑S battery with unmodified SS as the interlayer.
基金supported by the National Natural Science Foundation of China(Nos.42225301 and 42330304)。
文摘Sulfur is closely associated with various types of ore deposits,particularly orogenic gold(Au)systems,where sulfur-bearing melts and fluids play a critical role in transporting oreforming elements essential for ore formation.The widely accepted metamorphic devolatilization model suggests that compositionally fertile sedimentary rocks serve as potential gold sources.Therefore,understanding sulfur behavior during prograde metamorphism is essential for elucidating the mechanisms underlying metal activation and mobility.In this study,we conducted in-situ sulfur isotope(δ^(34)S)analyses using secondary ion mass spectrometry(SIMS)on samples from the Hongshankou area,a representative Barrovian-type metamorphic sequence characterized by intermediate pressure-temperature(P-T)conditions.This sequence comprises the biotite,garnet,staurolite,and kyanite zones.Our results show a systematic increase in δ^(34)S values(from 3.1‰ to 5.5‰)coupled with a progressive decrease in total sulfur content(from 320 ppm to 165 ppm)as metamorphic grade increases.The most pronounced sulfur mobilization occurs between the garnet and staurolite zones.In all analyzed samples,Au or Au-bearing minerals predominantly occur along the edges or within pyrite grains,highlighting the critical role of pyrite breakdown in controlling gold mobility.Thus,sulfur isotope fractionation provides robust constraints for quantitatively assessing sulfur mobility during metamorphism.These findings reinforce the concept that metasedimentary rocks and their metamorphic fluids represent fertile sources of Au and other metals enriched in orogenic gold deposits.
基金financially supported by the Nation Key R&D Program China(2018YFA0703200)the Key Research and Development Program of Hubei Province(2022BAA026)+1 种基金the National Natural Science Foundation of China(51772110)the Open Research Fund(2024JYBKF01)of Key Laboratory of Material Chemistry for Energy Conversion and Storage(HUST),Ministry of Education。
文摘Sluggish kinetics coupled with parasitic shuttling reactions are pivotal challenges hindering the performance of lithium-sulfur(Li-S)batteries.Improving areal capacity and cyclability of Li-S batteries can be achieved by addressing these challenges.A composite sulfur host material is synthesized herein by in situ anchoring ultrafine cobalt-iron phosphide nanoparticles(5-7 nm)onto a hollow mesoporous carbon sphere(HMCS)framework.This strategy achieved exceptional spatial restriction and a high density of catalytically active sites through the encapsulation of sulfur within a hollow-structured framework.Specifically,HMCS expedites rapid Li_(2)S nucleation kinetics,while CoFeP facilitates robust Li_(2)S dissolution kinetics by mitigating decomposition barriers.This synergistic integration equips CoFeP@HMCS with robust bi-directional catalytic activity,significantly promoting interracial charge-transfer,facilitate sulfu r multistep catalytic conversion,and inhibiting shuttling.Consequently,the battery exhibits excellent rate performance(991 mA h g^(-1) at 5.0 C)and retains a high areal capacity of 6.06 mA h cm^(-2) after 200 cycles under a high areal sulfur loading of 8.2 mg cm^(-2) but a low electrolyte/sulfur ratio of 4.8μL mg^(-1).This work contributes to enhancing the practical specific capacity of lithium-sulfur batteries and deepens the understanding of catalysts enabling bidirectional electrocatalytic sulfur conversion.
文摘To comprehensively explore the impact of binder content on the mechanical properties of the Polymer bonded explosive(PBX)substitute material(Polymer-bonded Analogue Explosive(PAE)—it is renowned for its outstanding high-temperature resistance,exceptional mechanical properties,excellent chemical stability,and superior electrical insulation),a series of experiments are meticulously carried out.The dynamic and static mechanical properties,along with the microstructure of PAE,are precisely measured through the Split Hopkinson Pressure Bar(SHPB)test,static compression tests,and Scanning Electron Microscopy(SEM).The dynamic performance test outcomes clearly indicate that both the binder content(2%,4%,6%)and temperature(25℃,45℃,70℃)exert a substantial influence on the dynamic mechanical properties of PAE.Specifically,as the binder content increases,the elasticmodulus increases,demonstrating higher stiffness,and the longer failure duration represents a prolonged fracture process rather than an improved deformation strain to failure.This means the strength-related stiffness rises with binder content,but the overall ductility does not increase.Notably,PAE with 2%the Ethylene-Vinyl Acetate Copolymer(EVA)—it bonds well with a variety ofmaterials,such asmetal,wood,and plastic—exhibits distinct plastic deformation behavior,while PAE samples with 4%and 6%EVA display evident brittle fracture characteristics.Additionally,the mechanical properties of PAE are highly sensitive to temperature variations.Among the tested temperatures,PAE showcases the most favorable performance at 45℃.The static performance test results reveal that an increment in binder content effectively helps to reduce the temperature sensitivity of temperature(-40℃,25℃,50℃,70℃)on PAE and enhance its static mechanical properties.The maximum compressive strength gradually diminishes as the temperature rises.However,it should be noted that an excessively high binder content will undermine the mechanical properties of PAE.With the increase in binder content,the compressive modulus demonstrates relatively stable changes under both lowtemperature and high-temperature conditions.The SEM analysis results demonstrate that,aside fromthe initial defects inherent in the material preparation process,the components of PAE are firmly combined.Throughout the tests,no new pores or microcracks emerge,which strongly indicates that the mechanical properties of PAE remain stable.
基金We would like to show gratitude to the Yunnan Province Basic Research Major Project(202501BC070006(Y.Wang))Key Industry Science and Technology Projects for University Services in Yunnan Province(FWCY ZNT2024002(Y.Wang))+3 种基金National Natural Science Foundation of China(22279070(L.Wang))and(U21A20170(X.He))the Ministry of Science and Technology of China(2019YFA0705703(L.Wang))Beijing Natural Science Foundation(L242005(X.He))Key Industry Science and Technology Projects for University Services in Yunnan Province(FWCY BSPY2024011(T.Lai)).
文摘Long-life energy storage batteries are integral to energy storage systems and electric vehicles,with lithium-ion batteries(LIBs)currently being the preferred option for extended usage-life energy storage.To further extend the life span of LIBs,it is essential to intensify investments in battery design,manufacturing processes,and the advancement of ancillary materials.The pursuit of long durability introduces new challenges for battery energy density.The advent of electrode material offers effective support in enhancing the battery’s long-duration performance.Often underestimated as part of the cathode composition,the binder plays a pivotal role in the longevity and electrochemical performance of the electrode.Maintaining the mechanical integrity of the electrode through judicious binder design is a fundamental requirement for achieving consistent long-life cycles and high energy density.This paper primarily concentrates on the commonly employed cathode systems in lithium-ion batteries,elucidates the significance of binders for both,discusses the application status,strengths,and weaknesses of novel binders,and ultimately puts forth corresponding optimization strategies.It underscores the critical function of binders in enhancing battery performance and advancing the sustainable development of lithium-ion batteries,aiming to offer fresh insights and perspectives for the design of high-performance LIBs.
基金supported by National Natural Science Foundation of China(Nos.32271791,32171709 and 22475053)Hunan Provincial Natural Science Foundation of China(No.2024JJ7643)Natural Science Foundation of Shanghai(No.22ZR1404100).
文摘Hard carbon(HC)in sodium-ion batteries is searched by numerous investigations,which can offer the excellent performance of reversible Na^(+)insertion and extraction.The covalent heteroatom doping in HC is recently worth concentrating,which can dilate the interlayer spacing of graphite to adjust the electrochemical storage performance in carbon anodes.However,the reported doping strategies of the modified HC have only resulted in limited improvement,especially unobvious effects on tuning porous structure.In this study,tannin extract and K_(2)SO_(4) are respectively utilized as carbon source and sulfur source for the fabrication of HC,in which K_(2)SO_(4) can contribute to the heteroatom doping,and the pore forming as well.The tannin-derived sulfur-doped carbon anode shows the excellent cycle stability,achieving a high reversible capacity of 520.5 mAh/g at a current density of 100 mA/g.Even after 500 cycles at a current density of 3 A/g,a high specific capacity of 236.7 mAh/g and a capacity retention rate of 92.6%can be reserved.Compared with the initial carbon,the adsorption energy of Na^(+)is multifold times higher,whereas Na^(+)diffusion energy barriers manyfold decrease.Moreover,the full battery assembled with Na_(3)V_(2)(PO_(4))_(3)/tannin-based HC demonstrates a stable cycling performance.This work can manifest the potentiality of the tannin-based electrode as anode for a high-performance sodium-ion batteries(SIBs),which could especially offer an explanation of Na^(+)storage and solid-electrolyte interface(SEI)stability to the electrochemical performance.
基金support of the National Natural Science Foundation of China(22075131 and 22078265)the Shaanxi Fundamental Science Research Project for Mathematics and Physics under Grants(No.22JSZ005)the State-Key Laboratory of Multiphase Complex Systems(No.MPCS-2021-A).
文摘Lithium-sulfur(Li-S)batteries require efficient catalysts to accelerate polysulfide conversion and mitigate the shuttle effect.However,the rational design of catalysts remains challenging due to the lack of a systematic strategy that rationally optimizes electronic structures and mesoscale transport properties.In this work,we propose an autogenously transformed CoWO_(4)/WO_(2) heterojunction catalyst,integrating a strong polysulfide-adsorbing intercalation catalyst with a metallic-phase promoter for enhanced activity.CoWO_(4) effectively captures polysulfides,while the CoWO_(4)/WO_(2) interface facilitates their S-S bond activation on heterogenous catalytic sites.Benefiting from its directional intercalation channels,CoWO_(4) not only serves as a dynamic Li-ion reservoir but also provides continuous and direct pathways for rapid Li-ion transport.Such synergistic interactions across the heterojunction interfaces enhance the catalytic activity of the composite.As a result,the CoWO_(4)/WO_(2) heterostructure demonstrates significantly enhanced catalytic performance,delivering a high capacity of 1262 mAh g^(−1) at 0.1 C.Furthermore,its rate capability and high sulfur loading performance are markedly improved,surpassing the limitations of its single-component counterparts.This study provides new insights into the catalytic mechanisms governing Li-S chemistry and offers a promising strategy for the rational design of high-performance Li-S battery catalysts.
基金supported by the National Key Research and Development Program of China (No.2024YFA1509600)National Natural Science Foundation of China (Nos.22474010 and 22274012)the Fundamental Research Funds for the Central Universities (No.2233300007)。
文摘Ferroptosis has exhibited great potential in therapies and intracellular reducing agents of sulfur species(RSSs) in the thiol-dependent redox systems are crucial in ferroptosis.This makes the simultaneous detection of multiple RSSs significant for evaluating ferroptosis therapy.However,the traditional techniques,including fluorescent(FL) imaging and electrospray ionization-based mass spectrometry(MS) detection,cannot achieve the discrimination of different RSSs.Herein,simultaneous MS detection of multiple RSSs,including cysteine(Cys),homocysteine(Hcy),glutathione(GSH) and hydrogen sulfide(H_(2)S),was obtained upon enhancing ionization efficiency by a fluorescent probe(NBD-O-1).Based on the interaction between NBD-O-1 and RSSs,the complex of RSSs with a fragment of NBD-O-1 can be generated,which can be easily ionized for MS detection in the negative mode.Therefore,the intracellular RSSs can be well detected upon the incubation of He La cells with the probe of NBD-O-1,exhibiting the total RSS levels by the FL imaging and further providing expression of each RSS by enhanced MS detection.Furthermore,the RSSs during ferroptosis in He La cells have been evaluated using the present strategy,demonstrating the potential for ferroptosis examinations.This work has made an unconventional application of a fluorescent probe to enhance the detection of multiple RSSs by MS,providing significant molecular information for addressing the ferroptosis mechanism.
基金National Natural Science Foundation of China (Nos.22071185 and 22271224)the Fundamental Research Funds for the Central Universities (No.2042019kf0008)Wuhan University startup funding for financial support。
文摘The development of catalytic multicomponent reactions for constructing complex organic scaffolds from readily accessible commodity chemicals is a key pursuit in contemporary synthetic chemistry.Current methods for synthesizing thioesters primarily rely on the acylation of thiols,which produces substantial waste and requires malodorous,unstable sulfur sources.In this work,we introduce a photocatalyzed hydrogen transfer strategy that enables a three-component synthesis of thioesters using abundant primary alcohols,easily available alkenes and elemental sulfur under mild conditions.This protocol demonstrates broad applicability and high chemo-and regioselectivity for both primary alcohols and alkenes,highlighting the advantage and potential of photo-mediated hydrogen transfer in facilitating multicomponent reactions using primary alcohol and elemental sulfur feedstocks.
基金the financial support from the National Natural Science Foundation of China (22109127)the Chinese Postdoctoral Science Foundation (2021M702666)+2 种基金the Research Fund of the State Key Laboratory of Solidification Processing (NPU),China (Grant No.2023-TS-02)The financial support from the Youth Project of"Shaanxi High-level Talents Introduction Plan"the Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) are also sincerely appreciated
文摘Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implementation remains a significant challenge.Herein,we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs.Specifically,polypyrrole(PPy)is in situ vapor-phase polymerized on the surface of N-doped TiO_(2) nanorods supported on carbon cloth(N-TiO_(2)/CC),thereby forming a well-defined p–n heterojunction.This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field.Thus,the PPy@N-TiO_(2)/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur,enabling ultrafast sulfur redox dynamics,as convincingly validated by both theoretical simulations and experimental results.Consequently,the PPy@N-TiO_(2)/CC PALSB achieves a high discharge capacity of 1653 mAh g^(−1),reaching 98.7%of the theoretical value.Furthermore,5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g^(−1),achieving dual-mode energy harvesting capabilities.This work successfully integrates solar energy conversion and storage within a rechargeable battery system,providing a promising strategy for sustainable energy storage technologies.
基金the financial support provided under the Fundamental Research Grant Scheme(FRGS),Project Code:FRGS/1/2021/TK01/USM/02/1,which made this research possible,The kind assistance and collaboration of all material suppliers were also gratefully acknowledged.Additional appreciation is extended to the Public Works Department Malaysia for the scholarship provided through the Hadiah Latihan Persekutuan programme for professional and managerial officers pursuing doctoral studies(JPA-1-840622086040)The APC was funded by Prof.Hui Yao from Beijing University of Technology.
文摘The rapid increase in traffic loads and frequencies has rendered conventional asphalt pavement inadequate to maintain its durability under tropical climates.This challenge has necessitated the exploration of new sources of modified asphalt with enhanced stiffness and superior performance at high temperatures.Natural rubber(NR)is a renewable biopolymer that has received growing interest as a modifier for asphalt binders.Cup lump rubber(CLR),a type of NR,is used to enhance asphalt properties and improve the performance of road pavements.This study evaluates the influence of wax-based surfactants(WS)on CLR-modified asphalt binder(CMB).The assessment focuses on changes in chemical characteristics,rheological behaviour,activation energy,and morphology.Four concentrations of WS(0.1%,0.15%,0.2%,and 0.25%)were incorporated into CMB.Analysis of CMB chemical changes showed that viscosity increased due to higher sulfoxide,carbonyl,and aromatic bond indices.These chemical modifications contributed to improved resistance of the binder to heat-induced deterioration.In both unaged and aged CMB samples,the incorporation of WS reduced the sulfoxide index of the binder.Rheological analysis indicated that CMB improved rutting resistance and anti-ageing performance,while WS further enhanced fatigue resistance.Activation energy analysis suggested that the combination of CMB with 0.15%WS produced the most favourable enhancement.Micrograph results showed that WS improved binder homogeneity and interconnectivity.In conclusion,the findings indicated that incorporating 0.15%WS into CMB enhanced the performance and durability of the asphalt pavement.
基金supported by the National Natural Science Foundation of China(52374311)National Key R&D Program of China(2023YFE0203000)+3 种基金the National Natural Science Foundation of Shaanxi(2023KXJ-262,2025SYS-SYSZD-035)the Fund of the State Key Laboratory of Solidification Processing in NPU(2025-TS-10)the Fundamental Research Funds for the Central Universities(D5000250277)the Youth Innovation Team of Shaanxi Universities。
文摘Layered oxides present compelling potential as cathode materials for sodium-ion batteries(SIBs).However,challenges including interfacial instability and sluggish reaction kinetics critically limit their rate capability and cycling performance.Herein,we introduce the water-soluble sodium polyacrylate(NaPAA)binder as a promising approach to mitigating these issues in P2-type layered oxides.The NaPAA binder facilitates the formation of a uniform Na^(+) conductive interfacial film,which protects the cathode against electrolyte-induced corrosion and effectively inhibits the dissolution of transition metals in P2-Na_(0.85)Li_(0.12)Ni_(0.22)Mn_(0.66)O_(2)(NLNMO).Furthermore,we elucidate the mechanism by which the NaPAA binder dynamically regulates the coordination of free anions at the electrode-electrolyte interface.This regulation reduces solvent decomposition and promotes the formation of a stable,ionically conductive layer.Consequently,the P2-NLNMO@NaPAA integrated electrode exhibits enhanced electrochemical performance,achieving an 89.2%capacity retention after 200 cycles at 0.2 C and delivering an initial capacity of 102.9 mA h g^(-1) even at 0℃.This study advances the fundamental understanding of binder-mediated interface engineering and demonstrates a scalable and eco-friendly manufacturing pathway for high-performance SIBs.
基金supported by the National Natural Science Foundation of China(No.42377083)the Natural Science Foundation of Sichuan Province,China(No.2025 ZNSFSC0433).
文摘In this work,ofloxacin(OFL),a kind of frequently detected antibiotic in groundwater,was selected to explore its impact(at ng/L-μg/L-level)on denitrification performance in an autotrophic denitrification system driven by pyrite/sulfur(FeS2/S0).Results showed that OFL restrained nitrate removal efficiency,and the inhibition degree was positively related to the concentration of OFL.After being exposed to increased OFL(200 ng/L-100μg/L)for 69 days,higher inhibition of electron transport activity(ETSA),enzyme activities of nitrate reductase(NAR),and nitrite reductase(NIR)were acquired.Meanwhile,the extracellular protein(PN)content of sludge samples was remarkably stimulated by OFL to resist the augmented toxicity.OFL contributed to increased microbial diversity and sulfur/sulfide oxidation functional genes in ng/L-level bioreactors,whereas led to a decline inμg/L level experiments.With OFL at concentrations of 200 ng/L and 100μg/L,the whole expression of 10 key denitrification functional genes was depressed,and the higher the OFL concentration,the lower the expression level.However,no significant proliferation of antibiotic resistance genes(ARGs)either in 200 ng/L-OFL or 100μg/L-OFL groups was observed.Two-factor correlation analysis results indicated that Thiobacillus,Anaerolineae,Anaerolineales,and Nitrospirae might be the main hosts of existing ARGs in this system.
基金supported by the National Natural Science Foundation of China(21875155,51675275,21703185 and 21473119)Q.B.Z.acknowledges the Leading Project Foundation of Science Department of Fujian Province(2018H0034)Shenzhen Science and Technology Planning Project(JCYJ20170818153427106).
文摘The development of high-sulfur-loading Li-S batteries is a key prerequisite for their commercial applications.This requires to surmount the huge polarization,severe polysulfide shuttling and drastic volume change caused by electrode thickening.High-strength polar binders are ideal for constructing robust and long-life high-loading sulfur cathodes but show very weak interfacial interaction with non-polar sulfur materials.To address this issue,this work devises a highly integrated sulfur@polydopamine/highstrength binder composite cathodes,targeting long-lasting and high-sulfur-loading Li-S batteries.The super-adhesion polydopamine(PD)can form a uniform nano-coating over the graphene/sulfur(G-S)surface and provide strong affinity to the cross-linked polyacrylamide(c-PAM)binder,thus tightly integrating sulfur with the binder network and greatly boosting the overall mechanical strength/conductivity of the electrode.Moreover,the PD coating and c-PAM binder rich in polar groups can form two effective blockades against the effusion of soluble polysulfides.As such,the 4.5 mg cm−2 sulfur-loaded G-S@PD-c-PAM cathode achieves a capacity of 480 mAh g−1 after 300 cycles at 1 C,while maintaining a capacity of 396 mAh g−1 after 50 cycles at 0.2 C when the sulfur loading rises to 9.1 mg cm−2.This work provides a system-wide concept for constructing high-loading sulfur cathodes through integrated structural design.
基金supported by the Strategic Emerging Industries Program of Shenzhen,China(JCYJ20120618164543322)the National Natural Science Foundation of China(20803095)
文摘Na-alginate as a binder in an aqueous solvent has been applied in the preparation of sulfur cathodes for lithium-sulfur batteries.Their electrochemical performances have been investigated by a charge-discharge cycle test and electrochemical impedance spectroscopy (EIS).The EIS tests indicated that the alginate sulfur cathode had lower resistance and better kinetic characteristics than those of the poly (vinylidene fluoride) (PVDF) sulfur cathode using PVDF as a binder in a N-methy-2-pyrrolidone (NMP) solvent.The charge-discharge tests showed that the discharge capacity and the capacity retention rate of Na-alginate sulfur cathode were 508 mAh·g-1and 65.4% at the 50th cycle with a current density of 335 mA·g-1.Compared with PVDF sulfur cathode,the alginate sulfur cathode showed a remarkably better cycle performance.These results show that the alginate binder has promising potential for lithium-sulfur battery applications.
基金supported by the National Natural Science Foundation of China(51473041)the Foundation for Innovative Research Groups of the National Natural Science Foundation of China(51521003)+2 种基金China Postdoctoral Science Foundation(no.2017M621262)Fundamental Research Funds for the Central Universities(No.HIT.NSRIF.201831)Postdoctoral Foundation of Hei long Jiang Province(LBH-Z17065)。
文摘Lithium sulfur(Li-S)batteries are the promising power sources,but their commercialization is significantly impeded by poor energy-storage functions at high sulfur loading.Here we report that such an issue can be effectively addressed by using a mussel-inspired binder comprised of chitosan grafted with catecholic moiety for sulfur cathodes.The resulting sulfur cathodes possess a high loading up to 12.2 mg cm-2 but also exhibit one of the best electrochemical properties among their counterparts.The excellent performances are attributed to the strong adhesion of the binder to sulfur particles,conducting agent,current collector,and polysulfide.The versatile adhesion effectively increases the sulfur loading,depresses the shuttle effect,and alleviates mechanical pulverization during cycling processes.The present investigation offers a new insight into high performance sulfur cathodes through a bio-adhesion viewpoint.
基金This work was financially supported by the Australian Research Council(ARC)Discovery Projects(DP210103266 and DPI 701048343)the Griffith University Ph.D.Scholarships.
文摘Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large volume change and active material loss in lithium-ion batteries during prolonged cycles. Herein, a hydrophilic polymer poly(methyl vinyl ether-alt-maleic acid) (PMVEMA) was explored as a dual-functional aqueous binder for the preparation of high-performance silicon anode and sulfur cathode. Benefiting from the dual functions of PMVEMA, i.e., the excellent dispersion ability and strong binding forces, the as-prepared electrodes exhibit improved capacity, rate capability and long-term cycling performance. In particular, the as-prepared Si electrode delivers a high initial discharge capacity of 1346.5 mAh g^(−1) at a high rate of 8.4 A/g and maintains 834.5 mAh g^(−1) after 300 cycles at 4.2 A/g, while the as-prepared S cathode exhibits enhanced cycling performance with high remaining discharge capacities of 663.4 mAh g^(−1) after 100 cycles at 0.2 C and 487.07 mAh g^(−1) after 300 cycles at 1 C, respectively. These encouraging results suggest that PMVEMA could be a universal binder to facilitate the green manufacture of both anode and cathode for high-capacity energy storage systems.
基金supported by the National Natural Science Foundation of China(No.51672156)Guangdong special support program(No.2015TQ01 N401)+2 种基金Guangdong Province Technical Plan Project(Nos.2017B010119001 and 20178090907005)Shenzhen Technical Plan Project(Nos.JCYJ20170412170706047,JCYJ20170307153806471 and GJHS20170314165324888)Shenzhen Graphene Manufacturing Innovation Center(No.201901161513)。
文摘Volume expansion and polysulfide shuttle effect are the main barriers for the commercialization of lithium-sulfur(Li-S) battery.In this work,we in-situ polymerized a cross-linked binder in sulfur cathode to solve the aforementioned problems using a facile method under mild conditions.Polycarbonate diol(PCDL),triethanolamine(TEA) and hexamethylene diisocyanate(HDI) were chosen as precursors to prepare the cross-linked binder.The in-situ polymerized binder(PTH) builds a strong network in sulfur cathode,which could restrain the volume expansion of sulfu r.Moreover,by adopting functional groups of oxygen atoms and nitrogen atoms,the binder could effectively facilitate transportation of Li-ion and adsorb polysulfide chemically.The Li-S battery with bare sulfur and carbon/sulfur composite cathodes and cross-linked PTH binder displays much better electrochemical performance than that of the battery with PVDF.The PTH-bare S cathode with a mass loading of 5.97 mg/cm^2 could deliver a capacity of 733.3 mAh/g at 0.2 C,and remained 585.5 mAh/g after 100 cycles.This in-situ polymerized binder is proved to be quite effective on restraining the volume expansion and suppressing polysulfide shuttle effect,then improving the electrochemical performance of Li-S battery.
基金supported by the National Natural Science Foundation of China(Nos.51772164 and U1601206)the Guangdong Natural Science Funds for Distinguished Young Scholars(2017B030306006)+2 种基金the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01N111)the Guangdong Special Support Program(2017TQ04C664)the Shenzhen Basic Research Project(Grant Nos.JCYJ20170412171359175)
文摘Lithium-sulfur(Li-S)batteries are promising next-generation high energy density batteries but their practical application is hindered by several key problems,such as the intermediate polysulfide shuttling and the electrode degradation caused by the sulfur volume changes.Binder acts as one of the most essential components to build the electrodes of Li-S batteries,playing vital roles in improving the performance and maintaining the integrity of the cathode structure during cycling,especially those with high sulfur loadings.To date,tremendous efforts have been devoted to improving the properties of binders,in terms of the viscosity,elasticity,stability,toughness and conductivity,by optimizing the composition and structure of polymer binders.Moreover,the binder modification endows them strong polysulfide trapping ability to suppress the shuttling and decreases the swelling to maintain the porous structure of cathode.In this review,we summarize the recent progress on the binders for Li-S batteries and discuss the various routes,including the binder combination use,functionalization,in-situ polymerization and ion cross-linking,etc.,to enhance their performance in stabilizing the cathode,building the high sulfur loading electrode and improving the cyclic stability.At last,the design principles and the problems in further applications are also highlighted.
