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
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
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
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
With the acceleration of industrialization,the pollution problem of sulfur dioxide(SO_(2))emitted from coal-fired power plants has become increasingly severe.Although wet flue gas desulfurization(FGD)technology can re...With the acceleration of industrialization,the pollution problem of sulfur dioxide(SO_(2))emitted from coal-fired power plants has become increasingly severe.Although wet flue gas desulfurization(FGD)technology can remove about 95%of SO_(2),its high energy consumption and the corrosion risk of downstream equipment caused by residual SO_(2)(500–3000 ppm)still need to be addressed[1].Previous porous materials(such as MOFs)achieve selective adsorption of SO_(2) through open metal sites,M–OH sites or functional organic groups,but the problem of CO_(2) co-adsorption limits their practical application[2].In recent years,hydrogen-bonded organic frameworks(HOFs)have emerged as a research hotspot due to their reversible hydrogen-bonding networks and flexible structures[3],but their stability under extreme conditions and efficient separation performance still need to be improved[4].展开更多
Lithium metal batteries(LMBs)have attracted great intention due to the high energy density[1].Among various battery technologies,lithium-sulfur(Li-S)batteries are also very unique but important due to its high energy ...Lithium metal batteries(LMBs)have attracted great intention due to the high energy density[1].Among various battery technologies,lithium-sulfur(Li-S)batteries are also very unique but important due to its high energy density,low cost and available sources[2].Although Li-s batteries exhibit high energy density,the cycling life is poor,especially for large-capacity pouch cells[3].The cycling performance of Li-s batteries is crucially determined by 16-electron complex sulfur reduction reaction(SRR)from S_(8)molecules to Li_(2)S,solid,which involves the multiple potential interwoven branches among lithium polysulfide intermediates(LiPS,e.g.,S_(8),Li_(2)S_(8),Li_(2)S_(6),Li_(2)S_(4)and Li_(2)S)[4].The obvious shuttle for soluble Lips across the cathode and anode leads to the battery capacity fading.Thus,it is necessary to decrease the accumulation of soluble Lips in the electrolyte through catalysts fastening the key conversion step from high-order polysulfides to insoluble Li_(2)S_(2)/Li_(2)S.Although some effort has been devoted to catalyze SRR,the complex mechanism remains unclear.To address this issue,Duan et al.tried to solve it based on nitrogen,sulfur,dualdoped holey graphene framework(N,S-HGF)electrocatalyst in Nature[5].展开更多
Sulfur was typically regarded as a poison to precious metal complex catalysts in hydroformylation of olefins.However,the combination of sulfur and phosphine may present an intriguing interaction with heterogeneous mon...Sulfur was typically regarded as a poison to precious metal complex catalysts in hydroformylation of olefins.However,the combination of sulfur and phosphine may present an intriguing interaction with heterogeneous mononuclear complex due to the difference of their electronegativities,and coordination capabilities.Herein,we report a novel sulfur-phosphine co-coordinated heterogeneous Rh mononuclear complex catalyst(Rh_(1)/POPs-PPh_(3)&S),which exhibits an unexpected 1.5–2.0 times catalytic activity for hydroformylation of olefins(C_(3)=,C_(5)=–C_(8)=),in comparison with the solely phosphine-coordinated Rh mononuclear complex catalyst(Rh_(1)/POPs-PPh_(3)).In contrast,sulfur coordination alone leads to severe sulfur poisoning with significantly inhibited catalytic performance.Experimental and theoretical analyses reveal that phosphine coordination promotes catalytic activity via its strong electron-donating ability,while sulfur occupies a coordination site and reduces the electronic density of Rh ions.The synergistical coordination of sulfur and phosphine optimizes the electronic density of active Rh ions and decreases the energy barrier of the rate-determining step of olefin insertion,thus enhancing the hydroformylation activity,regioselectivity and stability of Rh_(1)/POPs-PPh_(3)&S.展开更多
The practical application of lithium-sulfur(Li-S)batteries is still impeded by the severe shuttle effect of lithium polysulfides(LiPSs)and sluggish reaction kinetics of active sulfur.Designing catalytic carriers with ...The practical application of lithium-sulfur(Li-S)batteries is still impeded by the severe shuttle effect of lithium polysulfides(LiPSs)and sluggish reaction kinetics of active sulfur.Designing catalytic carriers with abundant active sites and strong chemisorption capability for LiPSs,is regarded as effective strategy to address these issues.Herein,Se-doping is introduced into the nitrogen-doped carbon coated CoP composite(Se-CoP@NC)to generate structural defects,which effectively enlarges the lattice spacing of CoP and reduces the conversion reaction energy barriers of LiPSs.Meanwhile,Se-doping sites bridges the interface of CoP and nitrogen-doped carbon,accelerating the charge transfer behavior and conversion reaction kinetics of LiPSs.Benefiting from the structural advantages,the assembled Li-S batteries with S/Se-CoP@NC as cathode exhibit high reversible capacity of 779.6 mAh/g at 0.5 C after 500 cycles,and high specific capacity of 805.9 mAh/g at 2 C.Even under extreme conditions(high sulfur-loading content of 6.9 mg/cm^(2);lean electrolyte dosage of 7μL/mg),the corresponding Li-S batteries also keep high reversible areal capacity of 4.5 mAh/cm^(2) after 100 cycles at 0.1 C.This work will inspire the design of metal compounds-based catalysts from atomic level to facilitate the practicability of Li-S batteries.展开更多
Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish ...Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.展开更多
The use of lithium-sulfur(Li-S)batteries is limited by sulfur redox reactions involving multi-phase transformations,especially at low-temperatures.To address this issue,we report a material(FCNS@NCFs)consisting of nit...The use of lithium-sulfur(Li-S)batteries is limited by sulfur redox reactions involving multi-phase transformations,especially at low-temperatures.To address this issue,we report a material(FCNS@NCFs)consisting of nitrogen-doped carbon fibers loaded with a ternary metal sulf-ide((Fe,Co,Ni)_(9)S_(8))for use as the sulfur host in Li-S batteries.This materi-al was prepared using transfer blot filter paper as the carbon precursor,thiourea as the source of nitrogen and sulfur,and FeCl_(3)·6H_(2)O,CoCl_(2)·6H_(2)O and NiCl_(2)·6H_(2)O as the metal ion sources.It was synthesized by an impreg-nation method followed by calcination.The nitrogen doping significantly in-creased the conductivity of the host,and the metal sulfides have excellent catalytic activities.Theoretical calculations,and adsorption and deposition experiments show that active sites on the surface of FCNS@NCFs selectively adsorb polysulfides,facilitate rapid adsorption and conversion,prevent cathode passivation and inhib-it the polysulfide shuttling.The FCNS@NCFs used as the sulfur host has excellent electrochemical properties.Its initial dis-charge capacity is 1639.0 mAh g^(−1) at 0.2 C and room temperature,and it remains a capacity of 1255.1 mAh g^(−1) after 100 cycles.At−20~C,it has an initial discharge capacity of 1578.5 mAh g^(−1) at 0.2 C,with a capacity of 867.5 mAh g^(−1) after 100 cycles.Its excellent performance at both ambient and low temperatures suggests a new way to produce high-performance low-temper-ature Li-S batteries.展开更多
In this work,a new process for achieving the recovery of elemental sulfur by utilizing a fluidized catalytic cracking(FCC) riser reactor for SOxtreatment(FCC-DeSOx) is proposed.The process leverages the high temperatu...In this work,a new process for achieving the recovery of elemental sulfur by utilizing a fluidized catalytic cracking(FCC) riser reactor for SOxtreatment(FCC-DeSOx) is proposed.The process leverages the high temperatures and hydrocarbon concentrations in the FCC riser reactor to convert SOxinto H_(2)S.Subsequently,H_(2)S,along with the cracked gas,is processed downstream to produce sulfur.Thermodynamic analysis of the key reduction reactions in the FCC-DeSOxprocess revealed that complete conversion of SOxto H_(2)S is feasible in the dry gas(hydrogen-rich) prelift zone,as well as the upper and lower zones of the riser,upon achieving thermodynamic equilibrium.Experimental studies were conducted to replicate the conditions of these reaction zones using a low concentration of hydrogen gas as the reducing agent.Through process optimization,investigation of the minimum reaction time,and kinetic studies,the potential of this method for the complete reduction of SOxwas further confirmed.展开更多
High-entropy oxides(HEOs)have sparked scientific interest recently as a potential material technology for lithium-sulfur(Li–S)batteries.This interest stems from their simultaneous roles as sulfur hosts and electrocat...High-entropy oxides(HEOs)have sparked scientific interest recently as a potential material technology for lithium-sulfur(Li–S)batteries.This interest stems from their simultaneous roles as sulfur hosts and electrocatalysts,which provide enhancements to the performance of sulfur cathode composites.Nonetheless,their incorporation into the active material blend results in compromised energy density,particularly when their gravimetric proportion is substantial(≥10 wt.%,in the sulfur-based cathode).展开更多
Despite significant progress has been achieved regarding the shuttle-effect of lithium polysulfides,the suppressed specific capacity and retarded redox kinetics under high sulfur loading still threat the actual energy...Despite significant progress has been achieved regarding the shuttle-effect of lithium polysulfides,the suppressed specific capacity and retarded redox kinetics under high sulfur loading still threat the actual energy density and power density of lithium-sulfur batteries.In this study,a graham condenser-inspired carbon@WS_(2)host with coil-in-tube structure was designed and synthesized using anodic aluminum oxide(AAO)membrane with vertically aligned nanopores as template.The vertical array of carbon nanotubes with internal carbon coils not only leads to efficient charge transfer across through the thickness of the cathode,but also provides significant confinement to polysulfide diffusion towards both the lateral and longitudinal directions.Few-layer WS_(2)in the carbon coils perform a synergistic role in suppressing the shuttle-effect as well as boosting the cathodic kinetics.As a result,high specific capacity(1180 m Ah/g at 0.1 C)and long-cycling stability at 0.5 C for 500 cycles has been achieved at 3 mgS/cm^(2).Impressive areal capacity of 7.4 m Ah/cm^(2)has been demonstrated when the sulfur loading reaches 8.4 mg/cm^(2).The unique coil-in-tube structure developed in this work provides a new solution for high sulfur loading cathode towards practical lithium-sulfur batteries.展开更多
Many catalysts have shown excellent activity for the sulfur reduction reaction(SRR),but sluggish electrochemistry kinetics have hindered the development of lithium-sulfur batteries.It has been found that the activity ...Many catalysts have shown excellent activity for the sulfur reduction reaction(SRR),but sluggish electrochemistry kinetics have hindered the development of lithium-sulfur batteries.It has been found that the activity of catalysts for the sulfur evolution reaction(SER)plays a crucial role in determining the overall reaction kinetics.To address this issue,the rational design of catalysts is crucial.Here,we proposed a popular rule to accelerate SER by using chip-like high-entropy perovskite oxide La_(0.7)Sr_(0.3)(Fe_(0.2)Co_(0.2)Ni_(0.2)Zn_(0.2)Mn_(0.2))O_(3-δ)(LMO-HEO)as advanced electrocatalysts.The strong interaction between the adjacent metal atoms in different metals of LMO-HEO electrocatalysts could lead to a"cocktail effect",which not only greatly improved the catalytic capacity toward sulfur species,but also accelerated the oxidation reaction kinetics of Li_2S.As a result,the S/La_(0.7)Sr_(0.3)(Fe_(0.2)Co_(0.2)Ni_(0.2)Zn_(0.2))Mn_(0.2)O_(3-δ)cathodes delivered excellent cyclic stability with a capacity decay of only 0.025%after 1200 cycles at 2 C.This work has provided a rational design idea for new multifunctional electrocatalysts with high catalytic capacity.展开更多
Lithium-sulfur(Li–S) battery has become one of the most promising next-generation electrical storage systems because of its exceptional energy density of 2600 Wh kg^(-1). However, their commercialization is hindered ...Lithium-sulfur(Li–S) battery has become one of the most promising next-generation electrical storage systems because of its exceptional energy density of 2600 Wh kg^(-1). However, their commercialization is hindered by several key obstacles, notably the polysulfide shuttle effect,poor electrical conductance of sulfur, and considerable volumetric change during cycling. This review addresses current advancements in microstructural innovations aimed at improving Li–S battery performance, focusing on modifying cathode materials. The strategies discussed primarily revolve around enhancing the conductivity of sulfur and effectively confining polysulfides to reduce the dissolving of lithium polysulfides in organic electrolytes. Key findings highlight the effectiveness of porous carbon structures and metal compounds in stabilizing polysulfides and enhancing electrochemical performances. Additionally, the roles of advanced synthesis techniques that facilitate the creation of hybrid cathodes with superior mechanical properties and cycling stability are summarized. By addressing the inherent limitations of traditional Li–S battery designs, these innovations pave the way for more efficient and reliable energy storage systems, positioning Li–S technology as a viable alternative to conventional lithium-ion batteries in future applications.展开更多
Lithium-sulfur(Li-S)batteries hold great promise for next-generation energy storage,yet suffer from sluggish redox kinetics and polysulfide shuttling.Herein,a novel Ni_(3)S_(2)/Ni_(2)B heterostructure is developed to ...Lithium-sulfur(Li-S)batteries hold great promise for next-generation energy storage,yet suffer from sluggish redox kinetics and polysulfide shuttling.Herein,a novel Ni_(3)S_(2)/Ni_(2)B heterostructure is developed to improve sulfur electrochemistry by synergistically enhancing polysulfide fixation and catalytic conversions.Fabricated through mild sequential boronation and sulfurization,this hybrid nanocatalyst integrates the strong polysulfide adsorbability and high conductivity of Ni_(2)B with the high catalytic activity of Ni_(3)S_(2).More importantly,the as-constructed heterointerface inspires new,highly catalytic sites that smooth consecutive sulfur conversions with lower energy barriers,while the built-in electric fields promote directional charge transfer,collectively contributing to fast-kinetic and highly efficient sulfur redox reactions.As a result,Li-S cells incorporating the Ni_(3)S_(2)/Ni_(2)B nanocatalyst exhibit excellent cyclability,with minimal capacity decay of 0.017%per cycle over 900 cycles at 1 C and a superb rate capability of up to 5 C.Even under demanding conditions,such as a high sulfur loading of 5.0 mg cm^(-2)and a low electrolyte-to-sulfur(E/S)ratio of 4.8 mL g^(-1),high capacity and cyclability are maintained,highlighting the great potential of this unique heterointerface engineering in advancing high-performance and practically viable Li-S batteries.展开更多
Sulfuric acid slag,a common byproduct with high iron content,poses challenges due to its high levels of harmful impurities and is often discarded as solid waste,leading to significant environmental and water pollution...Sulfuric acid slag,a common byproduct with high iron content,poses challenges due to its high levels of harmful impurities and is often discarded as solid waste,leading to significant environmental and water pollution.To address this issue and improve resource utilization,the preparation process of oxidized pellets from sulfuric acid slag was studied,exploring suitable pelletizing systems and thermal parameters.Additionally,the removal of harmful elements and the consolidation mechanism were established during the oxidation roasting process.The findings revealed that sulfuric acid slag along with specific processing conditions,such as using two high-pressure grinding rolls and adding 1.25 wt.%bentonite,resulted in the production of qualified green pellets with desirable physical properties.Through a thermal treatment process involving preheating and roasting,the desulfurization rate of the pellets reached 95.55%and the removal efficiency of arsenic achieved 27.11%.Hematite recrystallizes,shrinks,and forms a reticulated structure with Fe2O3 recrystallization as the backbone,resulting in higher consolidation strength.展开更多
Lithium-sulfur batteries are considered to be a new generation of high energy density batteries due to their non-toxicity,low cost and high theoretical specific capacity.However,the development of practical lithium-su...Lithium-sulfur batteries are considered to be a new generation of high energy density batteries due to their non-toxicity,low cost and high theoretical specific capacity.However,the development of practical lithium-sulfur batteries is seriously impeded by the sluggish multi-electron redox reaction of sulfur species and obstinate shuttle effect of polysulfides.In this study,a porous lanthanum oxychloride(LaOCl)nanofiber is designed as adsorbent and electrocatalyst of polysulfides to regulate the redox kinetics and suppress shuttling of sulfur species.Benefiting from the porous architecture and luxuriant active site of LaOCl nanofibers,the meliorative polarization effect and sulfur expansion can be accomplished.The LaOCl/S electrode exhibits an initial discharge specific capacity of 1112.3 mAh/g at 0.1 C and maintains a superior cycling performance with a slight decay of 0.02%per cycle over 1000 cycles at 1.0 C.Furthermore,even under a high sulfur loading of 4.6mg/cm^(2),the S cathode with LaOCl nanofibers still retains a high reversible areal capacity of 4.2 mAh/cm^(2)at 0.2 C and a stable cycling performance.Such a porous host expands the application of rare earth based catalysts in lithium-sulfur batteries and provides an alternative approach to facilitate the polysulfides conversion kinetics.展开更多
Metal-sulfur electrochemistry represents a promising energy storage technology due to the natural abundance and unparalleled theoretical specific capacity of 1675 mAh g^(-1)of sulfur based on two-electron redox reacti...Metal-sulfur electrochemistry represents a promising energy storage technology due to the natural abundance and unparalleled theoretical specific capacity of 1675 mAh g^(-1)of sulfur based on two-electron redox reaction(S^(0)■S^(2-)).Commercially viable metal-sulfur batteries(MSBs)are hindered by sluggish sulfur conversion kinetics,which reduce the utilization efficiency of sulfur and lead to polysulfide shuttling.Single-atom catalysts(SACs)exhibit specific catalytic activity,a high atomic utilization ratio,and flexible selectivity,and are considered exceptional electrocatalysts for addressing the intractable challenges encountered by the MSBs.This review summarizes the recent progress in SACs for boosting the sulfur electrochemistry in MSBs,focusing on sulfur host materials,modified separators and functional interlayers,and analyzes the in-depth mechanisms of SACs.Moreover,the correlation between the coordination environments and the intrinsic activity of SACs is discussed.Finally,the main challenges and potential research directions of SACs for high-energy-density and long-life MSBs are outlined.This study provides significant guidance for constructing novel SACs that can accelerate the sulfur conversion kinetics in MSBs.展开更多
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 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 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the support of the National Natural Science Foundation of China(Nos.22205207 and 22378369).
文摘With the acceleration of industrialization,the pollution problem of sulfur dioxide(SO_(2))emitted from coal-fired power plants has become increasingly severe.Although wet flue gas desulfurization(FGD)technology can remove about 95%of SO_(2),its high energy consumption and the corrosion risk of downstream equipment caused by residual SO_(2)(500–3000 ppm)still need to be addressed[1].Previous porous materials(such as MOFs)achieve selective adsorption of SO_(2) through open metal sites,M–OH sites or functional organic groups,but the problem of CO_(2) co-adsorption limits their practical application[2].In recent years,hydrogen-bonded organic frameworks(HOFs)have emerged as a research hotspot due to their reversible hydrogen-bonding networks and flexible structures[3],but their stability under extreme conditions and efficient separation performance still need to be improved[4].
文摘Lithium metal batteries(LMBs)have attracted great intention due to the high energy density[1].Among various battery technologies,lithium-sulfur(Li-S)batteries are also very unique but important due to its high energy density,low cost and available sources[2].Although Li-s batteries exhibit high energy density,the cycling life is poor,especially for large-capacity pouch cells[3].The cycling performance of Li-s batteries is crucially determined by 16-electron complex sulfur reduction reaction(SRR)from S_(8)molecules to Li_(2)S,solid,which involves the multiple potential interwoven branches among lithium polysulfide intermediates(LiPS,e.g.,S_(8),Li_(2)S_(8),Li_(2)S_(6),Li_(2)S_(4)and Li_(2)S)[4].The obvious shuttle for soluble Lips across the cathode and anode leads to the battery capacity fading.Thus,it is necessary to decrease the accumulation of soluble Lips in the electrolyte through catalysts fastening the key conversion step from high-order polysulfides to insoluble Li_(2)S_(2)/Li_(2)S.Although some effort has been devoted to catalyze SRR,the complex mechanism remains unclear.To address this issue,Duan et al.tried to solve it based on nitrogen,sulfur,dualdoped holey graphene framework(N,S-HGF)electrocatalyst in Nature[5].
文摘Sulfur was typically regarded as a poison to precious metal complex catalysts in hydroformylation of olefins.However,the combination of sulfur and phosphine may present an intriguing interaction with heterogeneous mononuclear complex due to the difference of their electronegativities,and coordination capabilities.Herein,we report a novel sulfur-phosphine co-coordinated heterogeneous Rh mononuclear complex catalyst(Rh_(1)/POPs-PPh_(3)&S),which exhibits an unexpected 1.5–2.0 times catalytic activity for hydroformylation of olefins(C_(3)=,C_(5)=–C_(8)=),in comparison with the solely phosphine-coordinated Rh mononuclear complex catalyst(Rh_(1)/POPs-PPh_(3)).In contrast,sulfur coordination alone leads to severe sulfur poisoning with significantly inhibited catalytic performance.Experimental and theoretical analyses reveal that phosphine coordination promotes catalytic activity via its strong electron-donating ability,while sulfur occupies a coordination site and reduces the electronic density of Rh ions.The synergistical coordination of sulfur and phosphine optimizes the electronic density of active Rh ions and decreases the energy barrier of the rate-determining step of olefin insertion,thus enhancing the hydroformylation activity,regioselectivity and stability of Rh_(1)/POPs-PPh_(3)&S.
基金the financial support from the National Natural Science Foundation of China(No.52101250)the S&T program of Hebei(Nos.215A4401D and 225A4404D)+5 种基金the Collaborative Innovation Center of Marine Science and Technology of Hainan University(No.XTCX2022HYC14)the Fundamental Research Funds for the Hebei University(No.2021YWF11)the Science Research Project of Hebei Education Department(No.QN2024087)the Xingtai City Natural Science Foundation(No.2023ZZ027)the Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),College of Chemistry,Nankai Universitypartially supported by the Pico Election Microscopy Center of Hainan University。
文摘The practical application of lithium-sulfur(Li-S)batteries is still impeded by the severe shuttle effect of lithium polysulfides(LiPSs)and sluggish reaction kinetics of active sulfur.Designing catalytic carriers with abundant active sites and strong chemisorption capability for LiPSs,is regarded as effective strategy to address these issues.Herein,Se-doping is introduced into the nitrogen-doped carbon coated CoP composite(Se-CoP@NC)to generate structural defects,which effectively enlarges the lattice spacing of CoP and reduces the conversion reaction energy barriers of LiPSs.Meanwhile,Se-doping sites bridges the interface of CoP and nitrogen-doped carbon,accelerating the charge transfer behavior and conversion reaction kinetics of LiPSs.Benefiting from the structural advantages,the assembled Li-S batteries with S/Se-CoP@NC as cathode exhibit high reversible capacity of 779.6 mAh/g at 0.5 C after 500 cycles,and high specific capacity of 805.9 mAh/g at 2 C.Even under extreme conditions(high sulfur-loading content of 6.9 mg/cm^(2);lean electrolyte dosage of 7μL/mg),the corresponding Li-S batteries also keep high reversible areal capacity of 4.5 mAh/cm^(2) after 100 cycles at 0.1 C.This work will inspire the design of metal compounds-based catalysts from atomic level to facilitate the practicability of Li-S batteries.
基金Institute of Technology Research Fund Program for Young Scholars21C Innovation Laboratory Contemporary Amperex Technology Co.,Limited,Ninde, 352100, China (21C–OP-202314)。
文摘Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.
基金partially supported by National Natural Science Foundation of China(52172250)Institute of Process Engineering(IPE)Project for Frontier Basic Research(QYJC-2023-06)。
文摘The use of lithium-sulfur(Li-S)batteries is limited by sulfur redox reactions involving multi-phase transformations,especially at low-temperatures.To address this issue,we report a material(FCNS@NCFs)consisting of nitrogen-doped carbon fibers loaded with a ternary metal sulf-ide((Fe,Co,Ni)_(9)S_(8))for use as the sulfur host in Li-S batteries.This materi-al was prepared using transfer blot filter paper as the carbon precursor,thiourea as the source of nitrogen and sulfur,and FeCl_(3)·6H_(2)O,CoCl_(2)·6H_(2)O and NiCl_(2)·6H_(2)O as the metal ion sources.It was synthesized by an impreg-nation method followed by calcination.The nitrogen doping significantly in-creased the conductivity of the host,and the metal sulfides have excellent catalytic activities.Theoretical calculations,and adsorption and deposition experiments show that active sites on the surface of FCNS@NCFs selectively adsorb polysulfides,facilitate rapid adsorption and conversion,prevent cathode passivation and inhib-it the polysulfide shuttling.The FCNS@NCFs used as the sulfur host has excellent electrochemical properties.Its initial dis-charge capacity is 1639.0 mAh g^(−1) at 0.2 C and room temperature,and it remains a capacity of 1255.1 mAh g^(−1) after 100 cycles.At−20~C,it has an initial discharge capacity of 1578.5 mAh g^(−1) at 0.2 C,with a capacity of 867.5 mAh g^(−1) after 100 cycles.Its excellent performance at both ambient and low temperatures suggests a new way to produce high-performance low-temper-ature Li-S batteries.
基金supported by General Program of National Natural Science Foundation of China (22178385)。
文摘In this work,a new process for achieving the recovery of elemental sulfur by utilizing a fluidized catalytic cracking(FCC) riser reactor for SOxtreatment(FCC-DeSOx) is proposed.The process leverages the high temperatures and hydrocarbon concentrations in the FCC riser reactor to convert SOxinto H_(2)S.Subsequently,H_(2)S,along with the cracked gas,is processed downstream to produce sulfur.Thermodynamic analysis of the key reduction reactions in the FCC-DeSOxprocess revealed that complete conversion of SOxto H_(2)S is feasible in the dry gas(hydrogen-rich) prelift zone,as well as the upper and lower zones of the riser,upon achieving thermodynamic equilibrium.Experimental studies were conducted to replicate the conditions of these reaction zones using a low concentration of hydrogen gas as the reducing agent.Through process optimization,investigation of the minimum reaction time,and kinetic studies,the potential of this method for the complete reduction of SOxwas further confirmed.
基金financially supported by the National Natural Science Foundation of China(52372289 and 52102368)Guangdong Special Fund for Key Areas(20237DZX3042)+2 种基金State Key Laboratory of New Ceramic Materials Tsinghua University(No.KF202415)Shenzhen Stable Support Projectsupported by the Centre for Advances in Reliability and Safety(CAiRS)admitted under AIR@Inno HK Research Cluster and HK Poly U Postdoc Matching Fund Scheme(1-W28H)。
文摘High-entropy oxides(HEOs)have sparked scientific interest recently as a potential material technology for lithium-sulfur(Li–S)batteries.This interest stems from their simultaneous roles as sulfur hosts and electrocatalysts,which provide enhancements to the performance of sulfur cathode composites.Nonetheless,their incorporation into the active material blend results in compromised energy density,particularly when their gravimetric proportion is substantial(≥10 wt.%,in the sulfur-based cathode).
基金the National Natural Science Foundation of China(Nos.22075027,52003030)Starting Grant from Beijing Institute of Technology and financial support from the State Key Laboratory of Explosion Science and Safety Protection(Nos.YBKT2106,YBKT23-05)Beijing Institute of Technology Research Fund Program for Young Scholars。
文摘Despite significant progress has been achieved regarding the shuttle-effect of lithium polysulfides,the suppressed specific capacity and retarded redox kinetics under high sulfur loading still threat the actual energy density and power density of lithium-sulfur batteries.In this study,a graham condenser-inspired carbon@WS_(2)host with coil-in-tube structure was designed and synthesized using anodic aluminum oxide(AAO)membrane with vertically aligned nanopores as template.The vertical array of carbon nanotubes with internal carbon coils not only leads to efficient charge transfer across through the thickness of the cathode,but also provides significant confinement to polysulfide diffusion towards both the lateral and longitudinal directions.Few-layer WS_(2)in the carbon coils perform a synergistic role in suppressing the shuttle-effect as well as boosting the cathodic kinetics.As a result,high specific capacity(1180 m Ah/g at 0.1 C)and long-cycling stability at 0.5 C for 500 cycles has been achieved at 3 mgS/cm^(2).Impressive areal capacity of 7.4 m Ah/cm^(2)has been demonstrated when the sulfur loading reaches 8.4 mg/cm^(2).The unique coil-in-tube structure developed in this work provides a new solution for high sulfur loading cathode towards practical lithium-sulfur batteries.
基金partially supported by grants from the National Natural Science Foundation of China(No.52072099)Team program of the Natural Science Foundation of Heilongjiang Province,China(No.TD2021E005)Joint Guidance Project of the Natural Science Foundation of Heilongjiang Province,China(No.LH2022E093)。
文摘Many catalysts have shown excellent activity for the sulfur reduction reaction(SRR),but sluggish electrochemistry kinetics have hindered the development of lithium-sulfur batteries.It has been found that the activity of catalysts for the sulfur evolution reaction(SER)plays a crucial role in determining the overall reaction kinetics.To address this issue,the rational design of catalysts is crucial.Here,we proposed a popular rule to accelerate SER by using chip-like high-entropy perovskite oxide La_(0.7)Sr_(0.3)(Fe_(0.2)Co_(0.2)Ni_(0.2)Zn_(0.2)Mn_(0.2))O_(3-δ)(LMO-HEO)as advanced electrocatalysts.The strong interaction between the adjacent metal atoms in different metals of LMO-HEO electrocatalysts could lead to a"cocktail effect",which not only greatly improved the catalytic capacity toward sulfur species,but also accelerated the oxidation reaction kinetics of Li_2S.As a result,the S/La_(0.7)Sr_(0.3)(Fe_(0.2)Co_(0.2)Ni_(0.2)Zn_(0.2))Mn_(0.2)O_(3-δ)cathodes delivered excellent cyclic stability with a capacity decay of only 0.025%after 1200 cycles at 2 C.This work has provided a rational design idea for new multifunctional electrocatalysts with high catalytic capacity.
基金Songshan Lake Materials Laboratory(2022SLABFN26)National Natural Science Foundation of China(21773024).
文摘Lithium-sulfur(Li–S) battery has become one of the most promising next-generation electrical storage systems because of its exceptional energy density of 2600 Wh kg^(-1). However, their commercialization is hindered by several key obstacles, notably the polysulfide shuttle effect,poor electrical conductance of sulfur, and considerable volumetric change during cycling. This review addresses current advancements in microstructural innovations aimed at improving Li–S battery performance, focusing on modifying cathode materials. The strategies discussed primarily revolve around enhancing the conductivity of sulfur and effectively confining polysulfides to reduce the dissolving of lithium polysulfides in organic electrolytes. Key findings highlight the effectiveness of porous carbon structures and metal compounds in stabilizing polysulfides and enhancing electrochemical performances. Additionally, the roles of advanced synthesis techniques that facilitate the creation of hybrid cathodes with superior mechanical properties and cycling stability are summarized. By addressing the inherent limitations of traditional Li–S battery designs, these innovations pave the way for more efficient and reliable energy storage systems, positioning Li–S technology as a viable alternative to conventional lithium-ion batteries in future applications.
基金supported by the National Natural Science Foundation of China(22379069,22109072)the Fundamental Research Funds for the Central Universities(30922010304)。
文摘Lithium-sulfur(Li-S)batteries hold great promise for next-generation energy storage,yet suffer from sluggish redox kinetics and polysulfide shuttling.Herein,a novel Ni_(3)S_(2)/Ni_(2)B heterostructure is developed to improve sulfur electrochemistry by synergistically enhancing polysulfide fixation and catalytic conversions.Fabricated through mild sequential boronation and sulfurization,this hybrid nanocatalyst integrates the strong polysulfide adsorbability and high conductivity of Ni_(2)B with the high catalytic activity of Ni_(3)S_(2).More importantly,the as-constructed heterointerface inspires new,highly catalytic sites that smooth consecutive sulfur conversions with lower energy barriers,while the built-in electric fields promote directional charge transfer,collectively contributing to fast-kinetic and highly efficient sulfur redox reactions.As a result,Li-S cells incorporating the Ni_(3)S_(2)/Ni_(2)B nanocatalyst exhibit excellent cyclability,with minimal capacity decay of 0.017%per cycle over 900 cycles at 1 C and a superb rate capability of up to 5 C.Even under demanding conditions,such as a high sulfur loading of 5.0 mg cm^(-2)and a low electrolyte-to-sulfur(E/S)ratio of 4.8 mL g^(-1),high capacity and cyclability are maintained,highlighting the great potential of this unique heterointerface engineering in advancing high-performance and practically viable Li-S batteries.
基金financially supported by the Fundamental Research Funds for the Central Universities of Central South University(2023ZZTS0506).
文摘Sulfuric acid slag,a common byproduct with high iron content,poses challenges due to its high levels of harmful impurities and is often discarded as solid waste,leading to significant environmental and water pollution.To address this issue and improve resource utilization,the preparation process of oxidized pellets from sulfuric acid slag was studied,exploring suitable pelletizing systems and thermal parameters.Additionally,the removal of harmful elements and the consolidation mechanism were established during the oxidation roasting process.The findings revealed that sulfuric acid slag along with specific processing conditions,such as using two high-pressure grinding rolls and adding 1.25 wt.%bentonite,resulted in the production of qualified green pellets with desirable physical properties.Through a thermal treatment process involving preheating and roasting,the desulfurization rate of the pellets reached 95.55%and the removal efficiency of arsenic achieved 27.11%.Hematite recrystallizes,shrinks,and forms a reticulated structure with Fe2O3 recrystallization as the backbone,resulting in higher consolidation strength.
基金supported by the Scientific Research Program Funded by Education Department of Shaanxi Provincial Government(No.22JK0411)the Natural Science Basic Research Program of Shaanxi Province(No.2023-JC-QN-0165)the National Natural Science Foundation of China(No.21603109).
文摘Lithium-sulfur batteries are considered to be a new generation of high energy density batteries due to their non-toxicity,low cost and high theoretical specific capacity.However,the development of practical lithium-sulfur batteries is seriously impeded by the sluggish multi-electron redox reaction of sulfur species and obstinate shuttle effect of polysulfides.In this study,a porous lanthanum oxychloride(LaOCl)nanofiber is designed as adsorbent and electrocatalyst of polysulfides to regulate the redox kinetics and suppress shuttling of sulfur species.Benefiting from the porous architecture and luxuriant active site of LaOCl nanofibers,the meliorative polarization effect and sulfur expansion can be accomplished.The LaOCl/S electrode exhibits an initial discharge specific capacity of 1112.3 mAh/g at 0.1 C and maintains a superior cycling performance with a slight decay of 0.02%per cycle over 1000 cycles at 1.0 C.Furthermore,even under a high sulfur loading of 4.6mg/cm^(2),the S cathode with LaOCl nanofibers still retains a high reversible areal capacity of 4.2 mAh/cm^(2)at 0.2 C and a stable cycling performance.Such a porous host expands the application of rare earth based catalysts in lithium-sulfur batteries and provides an alternative approach to facilitate the polysulfides conversion kinetics.
基金financial support from the National Natural Science Foundation of China(No.22379001 and 22309003)the Natural Science Research Project of Anhui Province Education department(No.2022AH030046)the Top Young Talents of Anhui University of Technology,the Young Scholars of the Introduction and Education of Talents in Anhui Province,and the Scientific Research Foundation of Anhui University of Technology for Talent Introduction。
文摘Metal-sulfur electrochemistry represents a promising energy storage technology due to the natural abundance and unparalleled theoretical specific capacity of 1675 mAh g^(-1)of sulfur based on two-electron redox reaction(S^(0)■S^(2-)).Commercially viable metal-sulfur batteries(MSBs)are hindered by sluggish sulfur conversion kinetics,which reduce the utilization efficiency of sulfur and lead to polysulfide shuttling.Single-atom catalysts(SACs)exhibit specific catalytic activity,a high atomic utilization ratio,and flexible selectivity,and are considered exceptional electrocatalysts for addressing the intractable challenges encountered by the MSBs.This review summarizes the recent progress in SACs for boosting the sulfur electrochemistry in MSBs,focusing on sulfur host materials,modified separators and functional interlayers,and analyzes the in-depth mechanisms of SACs.Moreover,the correlation between the coordination environments and the intrinsic activity of SACs is discussed.Finally,the main challenges and potential research directions of SACs for high-energy-density and long-life MSBs are outlined.This study provides significant guidance for constructing novel SACs that can accelerate the sulfur conversion kinetics in MSBs.
