High-performance lithium-ion batteries and sodium-ion batteries have been developed utilizing a hybrid anode material composed of zinc sulfide/sulfurized polyacrylonitrile.The in situ-generated zinc sulfide nanopartic...High-performance lithium-ion batteries and sodium-ion batteries have been developed utilizing a hybrid anode material composed of zinc sulfide/sulfurized polyacrylonitrile.The in situ-generated zinc sulfide nanoparticles serve as catalytic agents,significantly enhancing conductivity,shortening diffusion paths,and accelerating reaction kinetics.Simultaneously,the sulfurized polyacrylonitrile fibers form a three-dimensional matrix that not only provides a continuous network for rapid electron transfer but also prevents zinc sulfide nanoparticle aggregation and mitigates volume changes during charge-discharge cycles.Moreover,the heterointerface structure at the junction of zinc sulfide nanoparticles and the sulfurized polyacrylonitrile matrix increases the availability of active sites and facilitates both ion adsorption and electron transfer.As an anode material for lithium-ion batteries,the zinc sulfide/sulfurized polyacrylonitrile hybrid demonstrates a high reversible capacity of 1178 mAh g^(-1)after 100 cycles at a current density of 0.2 A g^(-1),maintaining a capacity of 788 mAh g^(-1)after 200 cycles at 1 A g^(-1).It also exhibits excellent sodium storage capabilities,retaining a capacity of 625 mAh g^(-1)after 150 cycles at 0.2 A g^(-1).Furthermore,ex-situ X-ray photoelectron spectroscopy,X-ray diffraction,7Li solid-state magic angle spinning nuclear magnetic resonance,and in situ Raman are employed to investigate the reaction mechanisms of the zinc sulfide/sulfurized polyacrylonitrile hybrid anode,providing valuable insights that pave the way for the advancement of hybrid anode materials in lithium-ion batteries and sodium-ion batteries.展开更多
Despite sulfurization offers the advantage of improving the photovoltaic performance in preparing Cu(In,Ga)Se2(CIGS)absorbers,deep level defects in the absorber and poor energy level alignment on the front surface are...Despite sulfurization offers the advantage of improving the photovoltaic performance in preparing Cu(In,Ga)Se2(CIGS)absorbers,deep level defects in the absorber and poor energy level alignment on the front surface are still main obstacles limiting the improvement of power co nversion efficiency(PCE)in sulfided CIGS solar cells.Herein,an in-situ Na doping strategy is proposed,in which the tailing effect of crystal growth is used to promote the sulfurization of CIGS absorbers.It is found that the grain growth is supported by Na incorporating due to the enrichment of NaSe_(x)near the upper surface.The high soluble Na during grain growth can not only suppress intrinsic In_(Cu) donor defects in the absorber,but also tailor S distribution in bulk and the band alignment at the heterojunction,which are both beneficial for the effective electron carriers.Meanwhile,the Na aggregation near the bottom of the absorber also contributes to the crystalline quality increasing and favorable ultra-thin MoSe_(2) formation at back contact,resulting in a reduced barrier height conducive to hole transport.PCE of the champion device is as high as 16.76%with a 28%increase.This research offers new insights into synthesizing CIGS solar cells and other chalcogenide solar cells with superior cell performance when using an intense sulfurization process.展开更多
Sulfurized polyacrylonitrile(SPAN)represents a unique class of cathode material for lithium sulfur(Li-S)batteries as it eradicates the polysulfides shuttling issue in carbonate-based electrolyte.However,due to the ess...Sulfurized polyacrylonitrile(SPAN)represents a unique class of cathode material for lithium sulfur(Li-S)batteries as it eradicates the polysulfides shuttling issue in carbonate-based electrolyte.However,due to the essential chemical S-linking and organic nature of SPAN,the active mass percentage and rate capability are two bottleneck issues preventing its ultimate deployment outside of laboratories.In the current work,aiming to endow both the charge conductivity and catalytic activity to SPAN for maximizing the redox kinetics of S conversion,a freestanding nanofibrous SPAN cathode embedding conductive CNTs and atomically dispersed Co centers is fabricated via multivariate electrospinning.While the CNTs enable dramatically enhancing the fiber conductivity and generating mesoscopic porosity for facilitating charge and mass transportation,the cross-linking of SPAN by Co-N_(4) S motifs creates extra charge conduction pathways and further serves as the catalytic active sites for expediting redox S conversion.As a result,an extraordinary Li-SPAN performance is achieved with a high specific capacity up to 1856 mAh g^(-1)@0.2 C,a superb rate capability up to 10 C,and an ultra-long battery life up to 1500 cycles@1 C.Consequently,our study here provides insights into the adoption of coordination chemistry to maximize the sulfur utilization by ensuring a more complete redox conversion from SPAN to Li2 S,and vice versa.展开更多
The inclusion complex of fl-cyclodextrin(β-CD)and sulfurized isobutylene(T321)was prepared with a co-precipitation method.The tribological properties of the complex with different concentrations were investigated by ...The inclusion complex of fl-cyclodextrin(β-CD)and sulfurized isobutylene(T321)was prepared with a co-precipitation method.The tribological properties of the complex with different concentrations were investigated by a four-ball tester in the solution of polyethylene glycol-600(PEG-600).The experimental results suggest that the complex exhibits better anti-friction and anti-wear properties than fl-CD under different load conditions.The tribo-system shows the least friction coefficient when the concentration of the complex is 0.8%.During the friction process,the complex was decomposed into various molecular fragments and the T321 molecules were released onto the friction interface to provide effective lubrication.The XPS analytical results on the worn surfaces reveal that sulfide film formed by the released T321 plays a major role,and the iron alkoxide and carbon deposition films formed by theβ-CD fragments have better anti-friction effect on the sulfide film surface.The interactions of different films result in the formation of a mixed boundary lubrication film.展开更多
Sulfurized polyacrylonitrile(SPAN)as a promising cathode material for lithium sulfur(Li-S)batteries has drawn increasing attention for its improved electrochemical performance in carbonate-based electrolyte.However,th...Sulfurized polyacrylonitrile(SPAN)as a promising cathode material for lithium sulfur(Li-S)batteries has drawn increasing attention for its improved electrochemical performance in carbonate-based electrolyte.However,the relatively poor electronic and ionic conductivities of SPAN limit its high-rate and lowtemperature performances.In this work,a novel one-dimensional nanofiber SPAN(SFPAN)composite is developed as the cathode material for Li-S batteries.Benefitting from its one-dimensional nanostructure,the SFPAN composite cathode provides fast channels for the migration of ions and electronics,thus effectively improving its electrochemical performance at high rates and low temperature.As a result,the SFPAN maintains a high reversible specific capacity^1200 mAh g−1 after 400 cycles at 0.3 A g−1 and can deliver a high capacity of^850 mAh g−1 even at a high current density of 12.5 A g−1.What is more,the SFPAN can achieve a capacity of^800 mAh g−1 at 0℃and^1550 mAh g−1 at 60℃,thus providing a wider temperature range of applications.This work provides new perspectives on the cathode design for high-rate lithium-sulfur batteries.展开更多
The inclusion complex of β-cyclodextrin (β-CD) and sulfurized isobutylene (T321) was prepared with a co-precipitation method. The tribological properties of the complex with different concentrations were investigate...The inclusion complex of β-cyclodextrin (β-CD) and sulfurized isobutylene (T321) was prepared with a co-precipitation method. The tribological properties of the complex with different concentrations were investigated by a four-ball tester in the solution of polyethylene glycol-600 (PEG-600). The experimental results suggest that the complex exhibits better anti-friction and anti-wear properties than β-CD under different load conditions. The tribo-system shows the least friction coefficient when the concentration of the complex is 0.8%. During the friction process, the complex was decomposed into various molecular fragments and the T321 molecules were released onto the friction interface to provide effective lubrication. The XPS analytical results on the worn surfaces reveal that sulfide film formed by the released T321 plays a major role, and the iron alkoxide and carbon deposition films formed by the β-CD fragments have better anti-friction effect on the sulfide film surface. The interactions of different films result in the formation of a mixed boundary lubrication film.展开更多
Lithium–sulfur batteries have great potential for high energy applications due to their high capacities,low cost and eco-friendliness. However, the particularly rapid capacity decay owing to the dissolution and diffu...Lithium–sulfur batteries have great potential for high energy applications due to their high capacities,low cost and eco-friendliness. However, the particularly rapid capacity decay owing to the dissolution and diffusion of polysulfide intermediate into the electrolyte still hamper their practical applications.And the reported preparation procedures to sulfur based cathode materials are often complex, and hence are rather difficult to produce at large scale. Here, we report a simple mechano-chemical sulfurization methodology in vacuum environment applying ball-milling method combined both the chemical and physical interaction for the one-pot synthesis of edge-sulfurized grapheme nanoplatelets with 3D porous foam structure as cathode materials. The optimal sample of 70%S–Gn Ps-48 h(ball-milled 48 h) obtains 13.2 wt% sulfur that chemically bonded onto the edge of Gn Ps. And the assembled batteries exhibit high initial discharge capacities of 1089 mAh/g at 0.1 C and 950 mAh/g at 0.5 C, and retain a stable discharge capacity of 776 mAh/g after 250 cycles at 0.5 C with a high Coulombic efficiency of over 98%. The excellent performance is mainly attributed to the mechano-chemical interaction between sulfur and grapheme nanoplatelets. This definitely triggers the currently extensive research in lithium–sulfur battery area.展开更多
The wide application of electromagnetic technology has led to increasingly frequent information transmission and communication interconnection.When the intensity of the disordered radiation of electromagnetic waves is...The wide application of electromagnetic technology has led to increasingly frequent information transmission and communication interconnection.When the intensity of the disordered radiation of electromagnetic waves is too high,it will cause electromagnetic pollution and pose a huge threat to human health or the survival of other animals and plants.How to ingeniously design absorbing materials is the key to solving the problem.This paper proposes a new design concept.The Co-based zeolite imidazolite-structured material ZIF-67 was selected as the main body of the metal-organic frameworks(MOFs)template,and the dodecahedral structured ZIF-67 nanoparticles were prepared using the classic ion-ligand process.Subsequently,a dodecahedral NiCo-LDH nanoparticle precursor composed of NiCo bimetallic hydroxide nanosheets with hollow edges and interior was obtained based on the liquid-phase cationic etching process.On this basis,thioacetamide(TAA)was selected as the vulcanizing agent,and the ZIF-67-derived sulfide inheriting the micro-nano structure of the precursor was obtained through liquid-phase hydrothermal vulcanization.The vulcanization growth mechanism and electromagnetic wave absorption mechanism of the MOF_(S)-derived sulfide were deeply explored.展开更多
Potassium-ion batteries(PIBs)have garnered significant attention as a promising alternative to commercial lithium-ion batteries(LIBs)due to abundant and cost-efficient potassium reserves.However,the large size of pota...Potassium-ion batteries(PIBs)have garnered significant attention as a promising alternative to commercial lithium-ion batteries(LIBs)due to abundant and cost-efficient potassium reserves.However,the large size of potassium ions and the resulting sluggish reaction kinetics present major obstacles to the widespread use of PIBs.Herein,we present a simple method to ingeniously encapsulate SnS_(2)nanoparticles within sulfurized polyacrylonitrile(SPAN)fibers(SnS_(2)@SPAN)for serving as a high-performance PIB anode.The large interlayer spacing of SnS_(2)provides a fast transport channel for potassium ions during charge–discharge cycles,while the one-dimensional SPAN skeleton offers massive binding sites and shortens the diffusion path for potassium ions,facilitating faster reaction kinetics.Additionally,the excellent ductility of SPAN can effectively accommodate the large volume changes that occur in SnS_(2)upon potassium-ion insertion,thereby enhancing the cyclic stability of SnS_(2).Benefiting from the above advantages,the SnS_(2)@SPAN composites exhibit impressive cyclability over 500 cycles at 4 A g−1,with a capacity retention rate close to 100%.This study provides an effective approach for stabilizing high-capacity PIB anode materials with large volume variations.展开更多
Solid lithium-sulfur batteries(SLSBs)show potential for practical application due to their possibility for high energy density.However,SLSBs still face tough challenges such as the large interface impedance and lithiu...Solid lithium-sulfur batteries(SLSBs)show potential for practical application due to their possibility for high energy density.However,SLSBs still face tough challenges such as the large interface impedance and lithium dendrite formation.Herein,a highperformance SLSB is demonstrated by using a fiber network reinforced Li_(6.75)La_(3)Zr_(1.75)Ta_(0.25)O_(12)(LLZTO)based composite solid electrolyte(CSE)in combination with sulfurized polyacrylonitrile(SPAN)cathode.The CSE consisting of an electrospun polyimide(PI)film,LLZTO ionically conducting filler and polyacrylonitrile(PAN)matrix,which is named as PI-PAN/LLZTO CSE,possesses high room-temperature ionic conductivity(2.75×10^(-4)S/cm),high Li^(+)migration number(tLi+)of 0.67 and good interfacial wettability.SPAN is utilized due to its unique electrochemical properties:reasonable electronic conductivity and no polysulfides shuttle effect.The CSE enables a highly stable Li plating/stripping cycle for over 600 h and good rate performance.Moreover,the assembled SLSB exhibits good cycle performance of accomplishing 120 cycles at 0.2 C with the capacity retention of 474 mAh/g,good rate properties and excellent long-term cycling stability with a high capacity retention of 86.49%from 15^(th)to 1,000^(th)cycles at 1.0 C.This work rationalizes our design concept and may guide the future development of SLSBs.展开更多
Sulfurized polyacrylonitrile(S@pPAN)composite provides a conductive pathway for sulfur active material at the molecular level and has already become one of the most promising cathode materials in lithium-sulfur batter...Sulfurized polyacrylonitrile(S@pPAN)composite provides a conductive pathway for sulfur active material at the molecular level and has already become one of the most promising cathode materials in lithium-sulfur batteries because of its outstanding electrochemical performances via novel solid-solid conversion mechanism.Although there are a great number of researches on the S@pPAN composite material,the accurate structure of S@pPAN and its redox reaction mechanism during the charge-discharge process still have not been determined.The previous research and inferences about the structure of S@pPAN and its electrochemical reaction mechanism were summarized in this review,providing a reference for the future study of lithiumsulfur batteries.展开更多
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
It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,...It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,and FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbents were prepared by coupling fly ash-based Si-Al carriers.The active components Fe-Ce-La oxides and Si-Al carriers were characterized by TPD,TG,XRF,BET and XPS,respectively.The effects of temperature,Si/Al ratio and FeCeLaO loading rate on the sulfur resistance were investigated.Results show that the SO_(2) promotes the arsenic removal of Fe_(2)O_(3),CeLaO and FeCeLaO.At 400℃,the arsenic removal efficiencies of the three oxides increase from 45.3%,72.5% and 81.3% without SO_(2) to 62.6%,80.5%and 91.0%,respectively.The SO_(2) inhibits the arsenic removal of La_(2)O_(2)CO_(3) and FeLaO,and the inhibition effect is pronounced at high temperatures.The sulfur poisoning resistance of Si-Al carriers increases with the increase of Si/Al ratio.When the Si/Al ratio is increased to 9.74,the arsenic removal efficiency in the SO_(2) environment is 13.9% higher than that in the absence of SO_(2).Introducing FeCeLaO active components is beneficial for enhancing the SO_(2) poisoning resistance of Si-Al carriers.The strong sulfur resistance of the FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbent results from multiple factors:protective effects of Ce on Fe,La and Al;sulfation-induced generation of Ce^(3+)and surface-adsorbed oxygen;and strong surface acidity of SiO_(2).展开更多
Sulfurized polyacrylonitrile(SPAN)has emerged as an excellent cathode material for lithium–sulfur batteries(LiSBs),and it addresses the shuttle effect through a solid‒solid reaction.However,the actual sulfur loadings...Sulfurized polyacrylonitrile(SPAN)has emerged as an excellent cathode material for lithium–sulfur batteries(LiSBs),and it addresses the shuttle effect through a solid‒solid reaction.However,the actual sulfur loadings in SPAN often remain below 40 wt%.Due to the susceptibility of polysulfides-to-nucleophilic reactions with electrolytes,achieving physical encapsulation of elemental sulfur is a challenging task.In this study,a free-standing cathode material with a high sulfur/selenium(S/Se)loading of 55 wt%was fabricated by introducing SeS_(x) into the unique lotus root-like pores of porous SeS_(x)PAN nanofiber membranes by electrospinning and a two-step heat treatment.Insoluble compounds were formed due to nucleophilic interactions between lithium polyselenosulfides(LiSeSx)and the electrolyte,which potently blocked the existing lotus root-like pores and facilitated the creation of a thin cathode–electrolyte interphase on the fiber surface.This dual functionality of LiSeS_(x) safeguarded the active material embedded within the porous structure.The SeS_(15)PAN cathode exhibited remarkable cycling stability with almost no degradation after 200 cycles at 0.2 C,along with a high discharge capacity of 580 mAh/g.This approach presents a solution for addressing the insufficient sulfur content in SPAN.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
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
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
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
Enantioselective intramolecular radical difunctionalization of alkenes involving sulfur dioxide through a three-component reaction of 4-arylpent-4-enoic acids,sodium hydrogen sulfite and thianthrenium salts under copp...Enantioselective intramolecular radical difunctionalization of alkenes involving sulfur dioxide through a three-component reaction of 4-arylpent-4-enoic acids,sodium hydrogen sulfite and thianthrenium salts under copper catalysis and photocatalysis is reported,allowing the construction of chiral 5-((sulfonyl)methyl)dihydrofuran-2(3H)-ones with β-quaternary stereocenters.During the transformation,sodium hydrogen sulfite is used as the sulfur dioxide surrogate.Excellent enantiocontrol(up to 99%ee)and wide functional group compatibility are observed in this asymmetric radical sulfonylation.展开更多
基金supported by“regional innovation mega project”program through the Korea Innovation Foundation funded by Ministry of Science and ICT(Project Number:2023-DD-UP-0026)the Energy Technology Evaluation and Planning(KETEP)and the Ministry of Trade,Industry&Energy(MOTIE)(No.RS-2024-00509401,RS-2023-00217581)“Regional Innovation Strategy(RIS)”through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(MOE)(2021RIS-001).
文摘High-performance lithium-ion batteries and sodium-ion batteries have been developed utilizing a hybrid anode material composed of zinc sulfide/sulfurized polyacrylonitrile.The in situ-generated zinc sulfide nanoparticles serve as catalytic agents,significantly enhancing conductivity,shortening diffusion paths,and accelerating reaction kinetics.Simultaneously,the sulfurized polyacrylonitrile fibers form a three-dimensional matrix that not only provides a continuous network for rapid electron transfer but also prevents zinc sulfide nanoparticle aggregation and mitigates volume changes during charge-discharge cycles.Moreover,the heterointerface structure at the junction of zinc sulfide nanoparticles and the sulfurized polyacrylonitrile matrix increases the availability of active sites and facilitates both ion adsorption and electron transfer.As an anode material for lithium-ion batteries,the zinc sulfide/sulfurized polyacrylonitrile hybrid demonstrates a high reversible capacity of 1178 mAh g^(-1)after 100 cycles at a current density of 0.2 A g^(-1),maintaining a capacity of 788 mAh g^(-1)after 200 cycles at 1 A g^(-1).It also exhibits excellent sodium storage capabilities,retaining a capacity of 625 mAh g^(-1)after 150 cycles at 0.2 A g^(-1).Furthermore,ex-situ X-ray photoelectron spectroscopy,X-ray diffraction,7Li solid-state magic angle spinning nuclear magnetic resonance,and in situ Raman are employed to investigate the reaction mechanisms of the zinc sulfide/sulfurized polyacrylonitrile hybrid anode,providing valuable insights that pave the way for the advancement of hybrid anode materials in lithium-ion batteries and sodium-ion batteries.
基金supported by the National Natural Science Foundation of China(62204074)the Hebei Natural Science Foundation(F2022201061,F2023201025)+2 种基金the Open bidding for selecting the best candidates of Baoding(2023chuang206)the High-level Talent Research Startup Project of Hebei University(521100221085)the Post-graduate's Innovation Fund Project of Hebei University(HBU2024BS030).
文摘Despite sulfurization offers the advantage of improving the photovoltaic performance in preparing Cu(In,Ga)Se2(CIGS)absorbers,deep level defects in the absorber and poor energy level alignment on the front surface are still main obstacles limiting the improvement of power co nversion efficiency(PCE)in sulfided CIGS solar cells.Herein,an in-situ Na doping strategy is proposed,in which the tailing effect of crystal growth is used to promote the sulfurization of CIGS absorbers.It is found that the grain growth is supported by Na incorporating due to the enrichment of NaSe_(x)near the upper surface.The high soluble Na during grain growth can not only suppress intrinsic In_(Cu) donor defects in the absorber,but also tailor S distribution in bulk and the band alignment at the heterojunction,which are both beneficial for the effective electron carriers.Meanwhile,the Na aggregation near the bottom of the absorber also contributes to the crystalline quality increasing and favorable ultra-thin MoSe_(2) formation at back contact,resulting in a reduced barrier height conducive to hole transport.PCE of the champion device is as high as 16.76%with a 28%increase.This research offers new insights into synthesizing CIGS solar cells and other chalcogenide solar cells with superior cell performance when using an intense sulfurization process.
基金supported by the National Natural Science Foundation of China(No.21805201)the NSFC-NRF China-Korea International Joint Research Project(No.51911540473)+1 种基金the Postdoctoral Research Foundation of China(No.2018T110544 and No.2017 M611899)the support by Suzhou Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies。
文摘Sulfurized polyacrylonitrile(SPAN)represents a unique class of cathode material for lithium sulfur(Li-S)batteries as it eradicates the polysulfides shuttling issue in carbonate-based electrolyte.However,due to the essential chemical S-linking and organic nature of SPAN,the active mass percentage and rate capability are two bottleneck issues preventing its ultimate deployment outside of laboratories.In the current work,aiming to endow both the charge conductivity and catalytic activity to SPAN for maximizing the redox kinetics of S conversion,a freestanding nanofibrous SPAN cathode embedding conductive CNTs and atomically dispersed Co centers is fabricated via multivariate electrospinning.While the CNTs enable dramatically enhancing the fiber conductivity and generating mesoscopic porosity for facilitating charge and mass transportation,the cross-linking of SPAN by Co-N_(4) S motifs creates extra charge conduction pathways and further serves as the catalytic active sites for expediting redox S conversion.As a result,an extraordinary Li-SPAN performance is achieved with a high specific capacity up to 1856 mAh g^(-1)@0.2 C,a superb rate capability up to 10 C,and an ultra-long battery life up to 1500 cycles@1 C.Consequently,our study here provides insights into the adoption of coordination chemistry to maximize the sulfur utilization by ensuring a more complete redox conversion from SPAN to Li2 S,and vice versa.
基金Funded by the National Natural Science Foundation of China(No.51075366)
文摘The inclusion complex of fl-cyclodextrin(β-CD)and sulfurized isobutylene(T321)was prepared with a co-precipitation method.The tribological properties of the complex with different concentrations were investigated by a four-ball tester in the solution of polyethylene glycol-600(PEG-600).The experimental results suggest that the complex exhibits better anti-friction and anti-wear properties than fl-CD under different load conditions.The tribo-system shows the least friction coefficient when the concentration of the complex is 0.8%.During the friction process,the complex was decomposed into various molecular fragments and the T321 molecules were released onto the friction interface to provide effective lubrication.The XPS analytical results on the worn surfaces reveal that sulfide film formed by the released T321 plays a major role,and the iron alkoxide and carbon deposition films formed by theβ-CD fragments have better anti-friction effect on the sulfide film surface.The interactions of different films result in the formation of a mixed boundary lubrication film.
基金supported by the National Natural Science Foundation of China(Grant nos.21773077,51632001,and 51532005)the Ministry of Science and Technology“973”program(Grant No.2015CB258400)the National Key R&D Program of China(2018YFB0905400)。
文摘Sulfurized polyacrylonitrile(SPAN)as a promising cathode material for lithium sulfur(Li-S)batteries has drawn increasing attention for its improved electrochemical performance in carbonate-based electrolyte.However,the relatively poor electronic and ionic conductivities of SPAN limit its high-rate and lowtemperature performances.In this work,a novel one-dimensional nanofiber SPAN(SFPAN)composite is developed as the cathode material for Li-S batteries.Benefitting from its one-dimensional nanostructure,the SFPAN composite cathode provides fast channels for the migration of ions and electronics,thus effectively improving its electrochemical performance at high rates and low temperature.As a result,the SFPAN maintains a high reversible specific capacity^1200 mAh g−1 after 400 cycles at 0.3 A g−1 and can deliver a high capacity of^850 mAh g−1 even at a high current density of 12.5 A g−1.What is more,the SFPAN can achieve a capacity of^800 mAh g−1 at 0℃and^1550 mAh g−1 at 60℃,thus providing a wider temperature range of applications.This work provides new perspectives on the cathode design for high-rate lithium-sulfur batteries.
基金Funded by the National Natural Science Foundation of China(No.51075366)
文摘The inclusion complex of β-cyclodextrin (β-CD) and sulfurized isobutylene (T321) was prepared with a co-precipitation method. The tribological properties of the complex with different concentrations were investigated by a four-ball tester in the solution of polyethylene glycol-600 (PEG-600). The experimental results suggest that the complex exhibits better anti-friction and anti-wear properties than β-CD under different load conditions. The tribo-system shows the least friction coefficient when the concentration of the complex is 0.8%. During the friction process, the complex was decomposed into various molecular fragments and the T321 molecules were released onto the friction interface to provide effective lubrication. The XPS analytical results on the worn surfaces reveal that sulfide film formed by the released T321 plays a major role, and the iron alkoxide and carbon deposition films formed by the β-CD fragments have better anti-friction effect on the sulfide film surface. The interactions of different films result in the formation of a mixed boundary lubrication film.
基金the Link Project of the National Natural Science Foundation of China and Guangdong Province(Grant no.U1301244)the National Natural Science Foundation of China(Grant nos.51573215,21506260)+2 种基金Guangdong Province Science&Technology Foundation(2011B050300008)Guangdong Natural Science Foundation(Grant nos.2014A030313159,2016A030313354)Guangzhou Scientific and Technological Planning Project(2014J4500002,201607010042)for financial support of this work
文摘Lithium–sulfur batteries have great potential for high energy applications due to their high capacities,low cost and eco-friendliness. However, the particularly rapid capacity decay owing to the dissolution and diffusion of polysulfide intermediate into the electrolyte still hamper their practical applications.And the reported preparation procedures to sulfur based cathode materials are often complex, and hence are rather difficult to produce at large scale. Here, we report a simple mechano-chemical sulfurization methodology in vacuum environment applying ball-milling method combined both the chemical and physical interaction for the one-pot synthesis of edge-sulfurized grapheme nanoplatelets with 3D porous foam structure as cathode materials. The optimal sample of 70%S–Gn Ps-48 h(ball-milled 48 h) obtains 13.2 wt% sulfur that chemically bonded onto the edge of Gn Ps. And the assembled batteries exhibit high initial discharge capacities of 1089 mAh/g at 0.1 C and 950 mAh/g at 0.5 C, and retain a stable discharge capacity of 776 mAh/g after 250 cycles at 0.5 C with a high Coulombic efficiency of over 98%. The excellent performance is mainly attributed to the mechano-chemical interaction between sulfur and grapheme nanoplatelets. This definitely triggers the currently extensive research in lithium–sulfur battery area.
基金supported by the National Natural Science Foundation of China(No.52172295)Basic Research Program of Jiangsu(No.BK20232013)+2 种基金Opening Project of Science and Technology on Reliability Physics and Application Technology of Electronic Component Laboratory(No.ZHD202305)Postgraduate Research&Practice Innovation Program of Jiangsu Province(Nos.KYCX24_0571 and KYCX25_0602)Interdisciplinary Innovation Fund for Doctoral Students of Nanjing University of Aeronautics and Astronautics(No.KXKCXJJ202408)。
文摘The wide application of electromagnetic technology has led to increasingly frequent information transmission and communication interconnection.When the intensity of the disordered radiation of electromagnetic waves is too high,it will cause electromagnetic pollution and pose a huge threat to human health or the survival of other animals and plants.How to ingeniously design absorbing materials is the key to solving the problem.This paper proposes a new design concept.The Co-based zeolite imidazolite-structured material ZIF-67 was selected as the main body of the metal-organic frameworks(MOFs)template,and the dodecahedral structured ZIF-67 nanoparticles were prepared using the classic ion-ligand process.Subsequently,a dodecahedral NiCo-LDH nanoparticle precursor composed of NiCo bimetallic hydroxide nanosheets with hollow edges and interior was obtained based on the liquid-phase cationic etching process.On this basis,thioacetamide(TAA)was selected as the vulcanizing agent,and the ZIF-67-derived sulfide inheriting the micro-nano structure of the precursor was obtained through liquid-phase hydrothermal vulcanization.The vulcanization growth mechanism and electromagnetic wave absorption mechanism of the MOF_(S)-derived sulfide were deeply explored.
基金National Natural Science Foundation of China,Grant/Award Numbers:22109023,22179022,22209027Industry‐University‐Research Joint Innovation Project of Fujian Province,Grant/Award Number:2021H6006+3 种基金Youth Innovation Fund of Fujian Province,Grant/Award Numbers:2022J05046,2021J05043FuXia Quan National Independent Innovation Demonstration Zone Collaborative Innovation Platform Project of Fuzhou Science and Technology Bureau,Grant/Award Number:2022‐P‐027Award Program for Fujian Minjiang Scholar ProfessorshipTalent Fund Program of Fujian Normal University。
文摘Potassium-ion batteries(PIBs)have garnered significant attention as a promising alternative to commercial lithium-ion batteries(LIBs)due to abundant and cost-efficient potassium reserves.However,the large size of potassium ions and the resulting sluggish reaction kinetics present major obstacles to the widespread use of PIBs.Herein,we present a simple method to ingeniously encapsulate SnS_(2)nanoparticles within sulfurized polyacrylonitrile(SPAN)fibers(SnS_(2)@SPAN)for serving as a high-performance PIB anode.The large interlayer spacing of SnS_(2)provides a fast transport channel for potassium ions during charge–discharge cycles,while the one-dimensional SPAN skeleton offers massive binding sites and shortens the diffusion path for potassium ions,facilitating faster reaction kinetics.Additionally,the excellent ductility of SPAN can effectively accommodate the large volume changes that occur in SnS_(2)upon potassium-ion insertion,thereby enhancing the cyclic stability of SnS_(2).Benefiting from the above advantages,the SnS_(2)@SPAN composites exhibit impressive cyclability over 500 cycles at 4 A g−1,with a capacity retention rate close to 100%.This study provides an effective approach for stabilizing high-capacity PIB anode materials with large volume variations.
基金The authors are indebted to the National Key Research and Development Program of China(No.2019YFE0122500)the National Natural Science Foundation of China(Nos.21878185 and 51772188)the Natural Science Foundation of Shanghai(No.21ZR1434800).
文摘Solid lithium-sulfur batteries(SLSBs)show potential for practical application due to their possibility for high energy density.However,SLSBs still face tough challenges such as the large interface impedance and lithium dendrite formation.Herein,a highperformance SLSB is demonstrated by using a fiber network reinforced Li_(6.75)La_(3)Zr_(1.75)Ta_(0.25)O_(12)(LLZTO)based composite solid electrolyte(CSE)in combination with sulfurized polyacrylonitrile(SPAN)cathode.The CSE consisting of an electrospun polyimide(PI)film,LLZTO ionically conducting filler and polyacrylonitrile(PAN)matrix,which is named as PI-PAN/LLZTO CSE,possesses high room-temperature ionic conductivity(2.75×10^(-4)S/cm),high Li^(+)migration number(tLi+)of 0.67 and good interfacial wettability.SPAN is utilized due to its unique electrochemical properties:reasonable electronic conductivity and no polysulfides shuttle effect.The CSE enables a highly stable Li plating/stripping cycle for over 600 h and good rate performance.Moreover,the assembled SLSB exhibits good cycle performance of accomplishing 120 cycles at 0.2 C with the capacity retention of 474 mAh/g,good rate properties and excellent long-term cycling stability with a high capacity retention of 86.49%from 15^(th)to 1,000^(th)cycles at 1.0 C.This work rationalizes our design concept and may guide the future development of SLSBs.
基金supported by the National Key Research and Development(R&D)Program of China(No.2021YFB2400300)the National Natural Science Foundation of China(No.22179083)+1 种基金Program of Shanghai Academic Research Leader(No.20XD1401900)Key-Area Research and Development Program of Guangdong Province(No.2019B090908001).
文摘Sulfurized polyacrylonitrile(S@pPAN)composite provides a conductive pathway for sulfur active material at the molecular level and has already become one of the most promising cathode materials in lithium-sulfur batteries because of its outstanding electrochemical performances via novel solid-solid conversion mechanism.Although there are a great number of researches on the S@pPAN composite material,the accurate structure of S@pPAN and its redox reaction mechanism during the charge-discharge process still have not been determined.The previous research and inferences about the structure of S@pPAN and its electrochemical reaction mechanism were summarized in this review,providing a reference for the future study of lithiumsulfur batteries.
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.
文摘It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,and FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbents were prepared by coupling fly ash-based Si-Al carriers.The active components Fe-Ce-La oxides and Si-Al carriers were characterized by TPD,TG,XRF,BET and XPS,respectively.The effects of temperature,Si/Al ratio and FeCeLaO loading rate on the sulfur resistance were investigated.Results show that the SO_(2) promotes the arsenic removal of Fe_(2)O_(3),CeLaO and FeCeLaO.At 400℃,the arsenic removal efficiencies of the three oxides increase from 45.3%,72.5% and 81.3% without SO_(2) to 62.6%,80.5%and 91.0%,respectively.The SO_(2) inhibits the arsenic removal of La_(2)O_(2)CO_(3) and FeLaO,and the inhibition effect is pronounced at high temperatures.The sulfur poisoning resistance of Si-Al carriers increases with the increase of Si/Al ratio.When the Si/Al ratio is increased to 9.74,the arsenic removal efficiency in the SO_(2) environment is 13.9% higher than that in the absence of SO_(2).Introducing FeCeLaO active components is beneficial for enhancing the SO_(2) poisoning resistance of Si-Al carriers.The strong sulfur resistance of the FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbent results from multiple factors:protective effects of Ce on Fe,La and Al;sulfation-induced generation of Ce^(3+)and surface-adsorbed oxygen;and strong surface acidity of SiO_(2).
基金supported by the New Materials Research Key Program of Tianjin(Grant No.18ZXJMTG00110).
文摘Sulfurized polyacrylonitrile(SPAN)has emerged as an excellent cathode material for lithium–sulfur batteries(LiSBs),and it addresses the shuttle effect through a solid‒solid reaction.However,the actual sulfur loadings in SPAN often remain below 40 wt%.Due to the susceptibility of polysulfides-to-nucleophilic reactions with electrolytes,achieving physical encapsulation of elemental sulfur is a challenging task.In this study,a free-standing cathode material with a high sulfur/selenium(S/Se)loading of 55 wt%was fabricated by introducing SeS_(x) into the unique lotus root-like pores of porous SeS_(x)PAN nanofiber membranes by electrospinning and a two-step heat treatment.Insoluble compounds were formed due to nucleophilic interactions between lithium polyselenosulfides(LiSeSx)and the electrolyte,which potently blocked the existing lotus root-like pores and facilitated the creation of a thin cathode–electrolyte interphase on the fiber surface.This dual functionality of LiSeS_(x) safeguarded the active material embedded within the porous structure.The SeS_(15)PAN cathode exhibited remarkable cycling stability with almost no degradation after 200 cycles at 0.2 C,along with a high discharge capacity of 580 mAh/g.This approach presents a solution for addressing the insufficient sulfur content in SPAN.
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supported by the National Natural Science Foundation of China(22171206)the Natural Science Foundation of Zhejiang Province(LZ23B020001)the Zhejiang Provincial Ten Thousand Talent Program(2023R5244)。
文摘Enantioselective intramolecular radical difunctionalization of alkenes involving sulfur dioxide through a three-component reaction of 4-arylpent-4-enoic acids,sodium hydrogen sulfite and thianthrenium salts under copper catalysis and photocatalysis is reported,allowing the construction of chiral 5-((sulfonyl)methyl)dihydrofuran-2(3H)-ones with β-quaternary stereocenters.During the transformation,sodium hydrogen sulfite is used as the sulfur dioxide surrogate.Excellent enantiocontrol(up to 99%ee)and wide functional group compatibility are observed in this asymmetric radical sulfonylation.
