Despite their attractive features of high energy density,low cost,and safety,polysulfide/iodide flow batteries(SIFBs)are hampered by the sluggish kinetics of the iodide redox couple,which restricts overall performance...Despite their attractive features of high energy density,low cost,and safety,polysulfide/iodide flow batteries(SIFBs)are hampered by the sluggish kinetics of the iodide redox couple,which restricts overall performance.Multicomponent sulfides are demonstrated as promising catalysts for accelerating I^(-)/I_(3)^(-) redox reactions.Concurrently,the enhanced configurational entropy arising from multinary compositions drives synergistic effects among constituent elements,establishing a viable pathway to optimize catalytic performance.Building on these foundations,this work introduces a targeted orbital hybridization-optimized electron density strategy to enhance the catalytic activity.Implementing this concept,we developed an in-situ solvothermal synthesis process for an entropy-enhanced AgCuZnSnS_(4) loaded graphite felt(ACZTS/GF)electrode.The engineered electrode demonstrates exceptional electrocatalytic performance with improved bulk conductivity and interfacial charge transfer kinetics within a SIFB.The cell achieves a high energy efficiency of 88.5%at 20 mA·cm^(−2) with 10%state-of-charge.Furthermore,the battery delivers a maximum power density of 119.8 mW·cm^(−2) and exhibits excellent long-term cycling stability.These significant results stem from orbital hybridization-driven electronic state optimization and entropy effect-induced synergistic catalysis.展开更多
High concentration of secondary hydrogen sulfide(sH_(2)S) in thermal recovery reservoirs of Liaohe Oilfield,NE China was concluded to originate from thermochemical sulfate reduction(TSR),and no biotic source of H_(2)S...High concentration of secondary hydrogen sulfide(sH_(2)S) in thermal recovery reservoirs of Liaohe Oilfield,NE China was concluded to originate from thermochemical sulfate reduction(TSR),and no biotic source of H_(2)S under abundant biomass has been reported in these presumed steam sterilized reservoirs ever before.In this study,we propose a new mechanism,biomass thermal decomposition for sulfur compounds(BTDS),to interpret the increasing of sH_(2)S.Sulfur of cells' dry weight took 0.20%-1.92% of the active strains isolated from the in-situ thermal recovery reservoirs of Liaohe Oilfield.When microbial organic sulfur compounds(MOSC) in biomass were exposed to injected steam,it resulted in the BTDS process.The isolated Bacillus subtilis D3(G+) and Pseudomonas aeruginosa XJ14(G-) were chosen to simulate this process.About 36% of sulfur in MOSC emitted as H_(2)S in steam chamber by BTDS.The δ^(34)S of H_(2)S from produced gas ranged from 8.7‰ to 17.0‰,close to the δ^(34)S of H_(2)S 11.2‰ from BTDS simulation experiment.It provides new insight into the contribution and sulfur cycle made by subterranean microorganisms on H_(2)S formation.展开更多
Due to the difference in chemical potential between sulfide solid electrolytes(SSEs)and high-energy nickel-rich layered oxide cathode materials LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811),the space charge layer(SCL)with l...Due to the difference in chemical potential between sulfide solid electrolytes(SSEs)and high-energy nickel-rich layered oxide cathode materials LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811),the space charge layer(SCL)with large impedance is formed at the interface,which severely compromises the electrochemical performance of all-solid-state lithium batteries(ASSLBs).Herein,a gradient sulfide Ti_(3)(PO_(4))_(4)coating for NCM811 was designed and prepared.Due to the highly favorable O-S exchange,a gradient sulfide coating with structural and chemical similarity to Li_(5.3)PS_(4.3)Cl_(1.7)SSE was formed by in situ sulfide Ti_(3)(PO_(4))_(4)on the surface of NCM811 using the sulfur-rich phosphorus sulfide molecule P_(4)S_(16).The increased sulfur content towards the outer surface of the coating reduces the chemical potential difference between the NCM811 cathode and SSEs,thereby reducing the formation of the SCL and ensuring stable and fast Li^(+)transport at the interface.The full cell with gradient sulfide Ti_(3)(PO_(4))_(4)-coated NCM811 cathode(PS-NCM811@TiP)exhibited excellent long-cycle stability,with a capacity retention rate of 95.2% after 100 cycles at 0.057 mA cm^(-2)and 25℃.This work provides a new perspective on the surface modification of cathodes for sulfide-based ASSLBs.展开更多
Lithium-sulfur(Li-S)batteries with high energy density suffer from the soluble lithium polysulfide species,Traditional metal sulfides containing a single metal element used as electrocatalysts for Li-S batteries commo...Lithium-sulfur(Li-S)batteries with high energy density suffer from the soluble lithium polysulfide species,Traditional metal sulfides containing a single metal element used as electrocatalysts for Li-S batteries commonly have limited catalytic abilities to improve battery performance.Herein,based on the Hume-Rothery rule and solvothermal method,the high-entropy sulfide NiCoCuTiVS_(x)derived from Co_(9)S_(8)was designed and synthesized,to realize the combination of small local strain and excellent catalytic performance.With all five metal elements(Ni,Co,Cu,Ti,and V)capable of chemical interactions with soluble polysulfides,NiCoCuTiVS_(x)exhibited strong chemical confinement of polysulfides and promoted fast kinetics for polysulfides conversion.Consequently,the S/NiCoCuTiVS_(x)cathode can maintain a high discharge capacity of 968.9 mA h g^(-1)after 200 cycles at 0.5 C and its capacity retention is 1.3 times higher than that of S/Co_(9)S_(8).The improved cycle stability can be attributed to the synergistic effect originating from the multiple metal elements,coupled with the reduced nucleation and activation barriers of Li_(2)S.The present work opens a path to explore novel electrocatalyst materials based on high entropy materials for the achievement of advanced Li-S batteries.展开更多
The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular an...The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular and cellular mechanisms by which quinolinic acid contributes to Huntington's disease pathology remain unknown. In this study, we established in vitro and in vivo models of Huntington's disease by administering quinolinic acid to the PC12 neuronal cell line and the striatum of mice, respectively. We observed a decrease in the levels of hydrogen sulfide in both PC12 cells and mouse serum, which was accompanied by down-regulation of cystathionine β-synthase, an enzyme responsible for hydrogen sulfide production. However, treatment with NaHS(a hydrogen sulfide donor) increased hydrogen sulfide levels in the neurons and in mouse serum, as well as cystathionine β-synthase expression in the neurons and the mouse striatum, while also improving oxidative imbalance and mitochondrial dysfunction in PC12 cells and the mouse striatum. These beneficial effects correlated with upregulation of nuclear factor erythroid 2-related factor 2 expression. Finally, treatment with the nuclear factor erythroid 2-related factor 2inhibitor ML385 reversed the beneficial impact of exogenous hydrogen sulfide on quinolinic acid-induced oxidative stress. Taken together, our findings show that hydrogen sulfide reduces oxidative stress in Huntington's disease by activating nuclear factor erythroid 2-related factor 2,suggesting that hydrogen sulfide is a novel neuroprotective drug candidate for treating patients with Huntington's disease.展开更多
Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,how...Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,however,constrain their delicate constructions.Herein,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix.This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in M_(x)S_(y)/carbon composites(M-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial polarization.Such“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time.Consequently,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric response.Harnessing defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.展开更多
This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature&l...This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature<300℃.Sulfur vapor is a highly flammable gas,which then auto-ignites to produce a flame.This behavior suggests that an O_(2)-S gas-gas reaction mechanism may contribute to all-solid-state battery thermal runaway.To improve all-solid-state battery safety,current work focuses on eliminating the O_(2)source by changing the cathode active material.The conclusion of this study suggests that all-solidstate battery safety can also be realized by the development of solid-state electrolytes with less susceptibility to sulfur volatilization.展开更多
Transition metal sulfides are considered promising anode materials for sodium-ion batteries(SIBs)due to their high theoretical capacity and low synthesis cost.However,is-sues such as poor cyclic stability and rate per...Transition metal sulfides are considered promising anode materials for sodium-ion batteries(SIBs)due to their high theoretical capacity and low synthesis cost.However,is-sues such as poor cyclic stability and rate performance,arising from volume expansion and structural degradation,remain sig-nificant challenges.We report a novel FeS_(2)/CoS_(2) heterostruc-ture embedded in a 3D carbon aerogel matrix(FeS_(2)/CoS_(2)@C)synthesized by a cross-linking and vulcanization process.The resulting core-shell structure,with bimetallic FeS_(2)/CoS_(2) nano-particles encapsulated in a conductive carbon shell,effectively reduces the adverse effects of volume changes during sodiation/desodiation cycles.The 3D porous carbon network increases both ion and electron diffusion,while preventing agglomeration of the active material and maintaining interface integrity.The FeS_(2)/CoS_(2)@C composite has an outstanding electrochemical performance,including a high specific capacity of 725 mAh g^(-1)at 0.5 A g^(-1)and an exceptional rate capability of 572 mAh g^(-1)at 10 A g^(-1).It also has remarkable cycling stability with no signific-ant capacity decay over 1000 cycles at 5 A g^(-1).展开更多
CuS-C50,the cathode materials for magnesium ion batteries,was synthesized by adding the surfactant cetyltrimethyl ammonium bromide(CTAB)and adjusting the percentage of ethylene glycol to 50vol%in hydrothermal synthesi...CuS-C50,the cathode materials for magnesium ion batteries,was synthesized by adding the surfactant cetyltrimethyl ammonium bromide(CTAB)and adjusting the percentage of ethylene glycol to 50vol%in hydrothermal synthesis process.Results show that CuS-C50 has the complete nanoflower structure.In aluminum chloride-pentamethylcydopentodiene/tetrahydrofuran(APC/THF)electrolyte,the CuS-C50 exhibits a high specific capacity of 331.19 mAh/g when the current density is 50 mA/g and still keeps a specific capacity of 136.92 mAh/g over 50 cycles when the current density is 200 mA/g.Results of morphology characterizations indicate that the complete nanoflower structure can provide more active sites and reduce the barriers for Mg^(2+)movement,eventually improving the charge and discharge performance of the CuS cathode materials for magnesium ion batteries.展开更多
Using 2-dicyanomethylene-3-cyano-4,5,5-trimethyl-2,5-dihydrofuran(TCF)as a near-infrared fluorescent chromophore,we designed and synthesized a TCF-based fluorescent probe TCF-NS by introducing 2,4-dinitrophenyl ether ...Using 2-dicyanomethylene-3-cyano-4,5,5-trimethyl-2,5-dihydrofuran(TCF)as a near-infrared fluorescent chromophore,we designed and synthesized a TCF-based fluorescent probe TCF-NS by introducing 2,4-dinitrophenyl ether as the recognized site for H_(2)S.The probe TCF-NS displayed a rapid-response fluorescent against H_(2)S with high sensitivity and selection but had no significant fluorescence response to other biothiols.Furthermore,TCF-NS was applied to sense H_(2)S in living cells successfully with minimized cytotoxicity and a large Stokes shift.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
Sulfide precipitation is an effective method for treating acidic heavy metal wastewater.However,the process often generates tiny particles with poor settling performance.The factors and mechanisms influencing particle...Sulfide precipitation is an effective method for treating acidic heavy metal wastewater.However,the process often generates tiny particles with poor settling performance.The factors and mechanisms influencing particle size and settling performance remain unclear.In this study,the growth behavior of CuS particles generated by two sulfide precipitation methods,gas-liquid and liquid-liquid sulfidation,was investigated.The effects of acidity,sulfur-to-copper molar ratio,and temperature on particle size were analyzed.The results showed that increasing the temperature had an adverse effect on CuS particle growth.Additionally,we found that acidity and sulfur-to-copper molar ratio had a more significant impact on particle growth in the liquid-liquid sulfidation system than in the gas-liquid sulfidation system.Based on supersaturation calculations and XPS analysis,it is found that particle growth in gas-liquid sulfidation systems is mainly influenced by supersaturation,while particle growth in liquid-liquid sulfidation systems is mainly affected by surface charge.This study provides valuable insights into the factors that influence particle growth in sulfide precipitation and can inform the development of strategies to improve the effective precipitation of sulfide nanoparticles in acidic wastewater.展开更多
The development of efficient catalysts for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is of great significance for the practical application of water splitting in alkaline electrolytes.Transitio...The development of efficient catalysts for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is of great significance for the practical application of water splitting in alkaline electrolytes.Transition metal sulfide electrocatalysts have been widely recognized as efficient catalysts for water splitting in alkaline media.In this work,an original and efficient synthesis strategy is proposed for the fabrication of asymmetric anode(N-(Co-Cu)S_(x))and cathode(N-CoS/Cu_(2)S).Impressively,these electrodes exhibit superior performance,benefiting from the construction of three-dimensional(3D)structures and the electronic structure adjustment caused by N-doping with increased active sites,improved mass/charge transport and enhanced evolution and release of gas bubbles.Hence,N-(Co-Cu)S_(x)anode exhibits excellent OER performance with only 217 mV overpotential at 10 mA·cm^(-2),while N-CoS/Cu_(2)S cathode possesses excellent HER performance with only 67 mV overpotential at 10 mA·cm^(-2).N-(Co-Cu)S_(x)||N-CoS/Cu_(2)S electrolyzer presents a low cell voltage of 1.53 V at 10 mA·cm^(-2)toward overall water splitting,which is superior to most recently reported transition metal sulfide-based catalysts.展开更多
By introduction of hydrogen peroxide into the reaction system of ZrOCl_(2)·8H_(2)O and K14[As_(2)W_(19)O_(67)(H_(2)O)],a novel polyoxometalate K_(8)Na_(19.5)H_(0.5)[Zr_(2)(O_(2))_(2)(β-AsVW_(10)O_(38))]4·68...By introduction of hydrogen peroxide into the reaction system of ZrOCl_(2)·8H_(2)O and K14[As_(2)W_(19)O_(67)(H_(2)O)],a novel polyoxometalate K_(8)Na_(19.5)H_(0.5)[Zr_(2)(O_(2))_(2)(β-AsVW_(10)O_(38))]4·68H_(2)O(1)has been successfully obtained via one-pot method and systematically characterized by IR,XPS,solid UV spectra,PXRD pattern,and TGA analysis.The analysis of X-ray crystallography exhibits that compound 1 crystallizes in the triclinic space group P-1 and presents a novel square-shaped Zr-substituted tetrameric polyoxometalate.The catalytic oxidation of sulfides by 1 are carried out,which demonstrate that 1 exhibits a good performance for the catalytic oxidation of sulfides to sulfones with high conversion(100%)and high selectivity(100%).展开更多
The discovery of quantum dots(QDs)stands as one of the paramount technological breakthroughs of the 20th century.Their versatility spans from everyday applications to cutting-edge scientific research,encompassing area...The discovery of quantum dots(QDs)stands as one of the paramount technological breakthroughs of the 20th century.Their versatility spans from everyday applications to cutting-edge scientific research,encompassing areas such as displays,lighting,photocatalysis,bio-imaging,and photonics devices and so on.Among the myriad QDs technologies,industrially relevant CuInS_(2)(CIS)QDs have emerged as promising alternatives to traditional Cd-and Pb-based QDs.Their tunable optoelectronic properties,high absorption coefficient,compositional flexibility,remarkable stability as well as Restriction of Hazardous Substances-compliance,with recent trends revealing a renewed interest in this material for various visible and near-infrared technological applications.This review focuses on recent advancements in CIS QDs as multidisciplinary field from its genesis in the mid-1990 to date with an emphasis on key breakthroughs in their synthesis,surface chemistry,post-synthesis modifications,and various applications.First,the comparation of properties of CIS QDs with relevant knowledge from other classes of QDs and from Ⅰ-Ⅱ-Ⅲ semiconductors as well is summarized.Second,recent advances in the synthesis methods,structure-optoelectronic properties,their defects,and passivation strategies as well as CIS-based heterostructures are discussed.Third,the state-of-the-art applications of CIS QDs ranging from solar cells,luminescence solar concentrations,photocatalysis,light emitting diodes,bioimaging and some emerging applications are summarized.Finally,we discuss open challenges and future perspectives for further advancement in this field.展开更多
Industrial high-current-density oxygen evolution catalyst is the key to accelerating the practical application of hydrogen energy.Herein,Co_(9)S_(8)/CoS heterojunctions were rationally encapsulated in S,N-codoped carb...Industrial high-current-density oxygen evolution catalyst is the key to accelerating the practical application of hydrogen energy.Herein,Co_(9)S_(8)/CoS heterojunctions were rationally encapsulated in S,N-codoped carbon((Co_(9)S_(8)/CoS)@SNC)microleaf arrays,which are rooted on S-doped carbonized wood fibers(SCWF).Benefiting from the synergistic electronic interactions on heterointerfaces and the accelerated mass transfer by array structure,the obtained self-supporting(Co_(9)S_(8)/CoS)@SNC/SCWF electrode exhibits superior performance toward alkaline oxygen evolution reaction(OER)with an ultra-low overpotential of 274 mV at 1000 mA/cm^(2),a small Tafel slope of 48.84 mV/dec,and ultralong stability up to 100 h.Theoretical calculations show that interfacing Co_(9)S_(8)with CoS can upshift the d-band center of the Co atoms and strengthen the interactions with oxygen intermediates,thereby favoring OER performance.Furthermore,the(Co_(9)S_(8)/CoS)@SNC/SCWF electrode shows outstanding rechargeability and stable cycle life in aqueous Zn-air batteries with a peak power density of 201.3 mW/cm^(2),exceeding the commercial RuO_(2)and Pt/C hybrid catalysts.This work presents a promising strategy for the design of high-current-density OER electrocatalysts from sustainable wood fiber resources,thus promoting their practical applications in the field of electrochemical energy storage and conversion.展开更多
The properties of direct reduced iron(DRI)smelting slag are important in the DRI melting process for molten iron production to ensure the slag-iron separation and quality of molten iron.The influence of binary basicit...The properties of direct reduced iron(DRI)smelting slag are important in the DRI melting process for molten iron production to ensure the slag-iron separation and quality of molten iron.The influence of binary basicity on the viscosity and sulfide capacity of CaO-SiO_(2)-MgO-Al_(2)O_(3)-FeO slag was investigated by the high-temperature experiments,structural analysis and thermodynamic calculation.The viscosity of the slag decreased rapidly with an increase in basicity from 0.4 to 0.8,and this trend became slow as the basicity further increased to 1.2.For the acidic slag with basicity of 0.4 and 0.6,the viscosity at 1500℃ was higher than 0.6 Pa s,which was harmful for the fluidity of slag melt.The slags with basicity of 0.8,1.0 and 1.2 at 1500℃ showed the low viscosity of less than 0.6 Pa s.For the basic slag with basicity of 1.0 and 1.2,the rapid precipitation of melilite led to the abrupt increase behavior of the viscosity,and the acidic slag showed the gentle temperature-viscosity curves.The Raman analysis revealed that the conversion from Q^(3) to Q^(2),Q^(1) and Q^(0) mainly occurred with the basicity increasing from 0.4 to 0.8,and the conversion from Q^(2) to Q^(1) and Q^(0) was dominant with further increase in basicity to 1.2,decreasing the degree of polymerization.The sulfide capacity was improved with the increasing basicity due to the increase in O^(2-)ions,and CaS could be formed dominantly for S^(2-)stabilization in present slag.The sulfur partition ratio was derived from sulfide capacity,and the values of sulfur partition ratio at basicity of 0.4 and 0.6 were much smaller than those at basicity of 0.8,1.0 and 1.2,indicating a weak desulfurization ability of the slag with a low basicity.展开更多
Traditional pyrometallurgical and hydrometallurgical methods to extract bismuth from sulfide ores face problems such as high cost,low-concentration SO_(2)generation,and long process time.In this study,the cyclone tech...Traditional pyrometallurgical and hydrometallurgical methods to extract bismuth from sulfide ores face problems such as high cost,low-concentration SO_(2)generation,and long process time.In this study,the cyclone technology and slurry electrolysis method were combined.The bismuth sulfide ore was dissolved directly at the anode,while the high purity bismuth was deposited efficiently at the cathode under the advantages of the two methods.The short process and high-efficiency extraction of bismuth sulfide ore were realized,and the pollution of low-concentration SO_(2)was avoided.Then,the effects of several crucial experimental conditions(current density,reaction time,temperature,pH,liquid-solid ratio,and circulation flow rate)on the leaching efficiency and recovery efficiency of bismuth were investigated.The leaching and electrowinning mechanisms during the recovery process were also analyzed according to the research results of this paper to better understand the cyclone slurry electrolysis process.The experimental results showed that 95.19%bismuth was leached into the acid solution in the anode area under optimal conditions,and the recovery efficiency and purity of bismuth on the cathode reached 91.13%and 99.26%,respectively,which were better than those by the traditional hydrometallurgy recovery process.展开更多
Lithium sulfide(Li_(2)S)is widely regarded as the next-generation cathode material for rechargeable batteries due to its satisfactory theoretical capacity and excellent compatibility with lithium-free anodes.However,t...Lithium sulfide(Li_(2)S)is widely regarded as the next-generation cathode material for rechargeable batteries due to its satisfactory theoretical capacity and excellent compatibility with lithium-free anodes.However,the large-scale applications of Li_(2)S cathodes are limited by the shuttle effect of soluble intermediate lithium polysulfides(LiPSs)and the sluggish redox kinetics of the interconversion between Li_(2)S and sulfur(S).Herein,we report novel nitrogen-doped carbon nanoflakes in-situ embedded with WN-Ni_(2)P heterostructures(WN-Ni_(2)P@NCN)as a multifunctional host to promote the cycling performance and reaction kinetics of Li_(2)S.After loading Li_(2)S,the WNNi_(2)P@NCN/Li_(2)S exhibits stable reversible capacity of 597mAh g^(-1)at 0.5 A g^(-1)over 150 cycles,and superior cycling stability over 800 cycles.The high reversible capacities,excellent cycling properties and superior reaction kinetics of WN-Ni_(2)P@NCN/Li_(2)S are attributed to the strong LiPSs fixation,remarkable catalytic activation and high electronic/ionic conductivity of the WN-Ni_(2)P@NCN framework,confirmed by the experiment and the density function theory calculation results.This work offers a new strategy for designing heterostructure nanoflakes with metal nitride and metal phosphide to facilitate the applications of advanced lithium-sulfur batteries.展开更多
The development of high-performance and stable electrocatalysts for oxygen evolution reaction(OER)is essential to improve the overall efficiency of water splitting.Here,S-vacancies and iron-doped nickel sulfide nanosh...The development of high-performance and stable electrocatalysts for oxygen evolution reaction(OER)is essential to improve the overall efficiency of water splitting.Here,S-vacancies and iron-doped nickel sulfide nanosheets(Vs-Ni_(2)Fe_(1)S_(2)/NF)were successfully prepared on the surface of nickel foam via solvothermal reaction of nickel-iron layered double hydroxide with sublimed sulfur added with sodium borohydride.Under the synergistic regulation of iron-doped and S-vacancies,Vs-Ni_(2)Fe_(1)S_(2)/NF shows excellent electrocatalytic performance and long-term durability.To reach current densities of 10 and500 mA cm^(-2),Vs-Ni_(2)Fe_(1)S_(2)/NF requires only 185(±5)and 248(±5)mV overpotential,respectively,and can maintain long stability for 350 h at 500 mA cm^(-2).The change of the mechanical pathway from adsorbate evolution mechanism to lattice oxygen oxidation mechanism is due to the increased acidity of the Ni site in Vs-Ni_(2)Fe_(1)S_(2)/NF,which facilitates the decouped proton and electron transfer process.Density functional calculation results show that the introduction of Fe atoms and S vacancies in Ni3S_(2)can enhance the conductivity of the intermediates by regulating the electronic structure of the intermediates,optimize the adsorption or desorption energy,and thus significantly improve the OER activity.For Vs-Ni_(2)Fe_(1)S_(2)/NF(+,-)cell,a voltage of 1.56 V is required to achieve 10 mA cm^(-2).In addition,Vs-Ni_(2)Fe_(1)S_(2)/NF catalyst also showed low overpotential(270 mV at 100 mA cm^(-2))and high alkaline tolerance(100 h at 100 mA cm^(-2))at 30 wt%KOH of 70℃.This shows that it has potential industrial application.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22171180,22461142137,and 22478242)the Shanghai Municipal Science and Technology Major Project,China.
文摘Despite their attractive features of high energy density,low cost,and safety,polysulfide/iodide flow batteries(SIFBs)are hampered by the sluggish kinetics of the iodide redox couple,which restricts overall performance.Multicomponent sulfides are demonstrated as promising catalysts for accelerating I^(-)/I_(3)^(-) redox reactions.Concurrently,the enhanced configurational entropy arising from multinary compositions drives synergistic effects among constituent elements,establishing a viable pathway to optimize catalytic performance.Building on these foundations,this work introduces a targeted orbital hybridization-optimized electron density strategy to enhance the catalytic activity.Implementing this concept,we developed an in-situ solvothermal synthesis process for an entropy-enhanced AgCuZnSnS_(4) loaded graphite felt(ACZTS/GF)electrode.The engineered electrode demonstrates exceptional electrocatalytic performance with improved bulk conductivity and interfacial charge transfer kinetics within a SIFB.The cell achieves a high energy efficiency of 88.5%at 20 mA·cm^(−2) with 10%state-of-charge.Furthermore,the battery delivers a maximum power density of 119.8 mW·cm^(−2) and exhibits excellent long-term cycling stability.These significant results stem from orbital hybridization-driven electronic state optimization and entropy effect-induced synergistic catalysis.
文摘High concentration of secondary hydrogen sulfide(sH_(2)S) in thermal recovery reservoirs of Liaohe Oilfield,NE China was concluded to originate from thermochemical sulfate reduction(TSR),and no biotic source of H_(2)S under abundant biomass has been reported in these presumed steam sterilized reservoirs ever before.In this study,we propose a new mechanism,biomass thermal decomposition for sulfur compounds(BTDS),to interpret the increasing of sH_(2)S.Sulfur of cells' dry weight took 0.20%-1.92% of the active strains isolated from the in-situ thermal recovery reservoirs of Liaohe Oilfield.When microbial organic sulfur compounds(MOSC) in biomass were exposed to injected steam,it resulted in the BTDS process.The isolated Bacillus subtilis D3(G+) and Pseudomonas aeruginosa XJ14(G-) were chosen to simulate this process.About 36% of sulfur in MOSC emitted as H_(2)S in steam chamber by BTDS.The δ^(34)S of H_(2)S from produced gas ranged from 8.7‰ to 17.0‰,close to the δ^(34)S of H_(2)S 11.2‰ from BTDS simulation experiment.It provides new insight into the contribution and sulfur cycle made by subterranean microorganisms on H_(2)S formation.
基金supported by the National Natural Science Foundation of China(No.52272258)the Beijing Nova Program(No.20220484214)。
文摘Due to the difference in chemical potential between sulfide solid electrolytes(SSEs)and high-energy nickel-rich layered oxide cathode materials LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811),the space charge layer(SCL)with large impedance is formed at the interface,which severely compromises the electrochemical performance of all-solid-state lithium batteries(ASSLBs).Herein,a gradient sulfide Ti_(3)(PO_(4))_(4)coating for NCM811 was designed and prepared.Due to the highly favorable O-S exchange,a gradient sulfide coating with structural and chemical similarity to Li_(5.3)PS_(4.3)Cl_(1.7)SSE was formed by in situ sulfide Ti_(3)(PO_(4))_(4)on the surface of NCM811 using the sulfur-rich phosphorus sulfide molecule P_(4)S_(16).The increased sulfur content towards the outer surface of the coating reduces the chemical potential difference between the NCM811 cathode and SSEs,thereby reducing the formation of the SCL and ensuring stable and fast Li^(+)transport at the interface.The full cell with gradient sulfide Ti_(3)(PO_(4))_(4)-coated NCM811 cathode(PS-NCM811@TiP)exhibited excellent long-cycle stability,with a capacity retention rate of 95.2% after 100 cycles at 0.057 mA cm^(-2)and 25℃.This work provides a new perspective on the surface modification of cathodes for sulfide-based ASSLBs.
基金financially supported by the National Natural Science Foundation of China(U22A20113,52261135543)。
文摘Lithium-sulfur(Li-S)batteries with high energy density suffer from the soluble lithium polysulfide species,Traditional metal sulfides containing a single metal element used as electrocatalysts for Li-S batteries commonly have limited catalytic abilities to improve battery performance.Herein,based on the Hume-Rothery rule and solvothermal method,the high-entropy sulfide NiCoCuTiVS_(x)derived from Co_(9)S_(8)was designed and synthesized,to realize the combination of small local strain and excellent catalytic performance.With all five metal elements(Ni,Co,Cu,Ti,and V)capable of chemical interactions with soluble polysulfides,NiCoCuTiVS_(x)exhibited strong chemical confinement of polysulfides and promoted fast kinetics for polysulfides conversion.Consequently,the S/NiCoCuTiVS_(x)cathode can maintain a high discharge capacity of 968.9 mA h g^(-1)after 200 cycles at 0.5 C and its capacity retention is 1.3 times higher than that of S/Co_(9)S_(8).The improved cycle stability can be attributed to the synergistic effect originating from the multiple metal elements,coupled with the reduced nucleation and activation barriers of Li_(2)S.The present work opens a path to explore novel electrocatalyst materials based on high entropy materials for the achievement of advanced Li-S batteries.
基金supported by the National Natural Science Foundation of China,Nos.82271327 (to ZW),82072535 (to ZW),81873768 (to ZW),and 82001253 (to TL)。
文摘The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular and cellular mechanisms by which quinolinic acid contributes to Huntington's disease pathology remain unknown. In this study, we established in vitro and in vivo models of Huntington's disease by administering quinolinic acid to the PC12 neuronal cell line and the striatum of mice, respectively. We observed a decrease in the levels of hydrogen sulfide in both PC12 cells and mouse serum, which was accompanied by down-regulation of cystathionine β-synthase, an enzyme responsible for hydrogen sulfide production. However, treatment with NaHS(a hydrogen sulfide donor) increased hydrogen sulfide levels in the neurons and in mouse serum, as well as cystathionine β-synthase expression in the neurons and the mouse striatum, while also improving oxidative imbalance and mitochondrial dysfunction in PC12 cells and the mouse striatum. These beneficial effects correlated with upregulation of nuclear factor erythroid 2-related factor 2 expression. Finally, treatment with the nuclear factor erythroid 2-related factor 2inhibitor ML385 reversed the beneficial impact of exogenous hydrogen sulfide on quinolinic acid-induced oxidative stress. Taken together, our findings show that hydrogen sulfide reduces oxidative stress in Huntington's disease by activating nuclear factor erythroid 2-related factor 2,suggesting that hydrogen sulfide is a novel neuroprotective drug candidate for treating patients with Huntington's disease.
基金financially supported by the National Natural Science Foundation of China(Grants nos.62201411,62371378,22205168,52302150 and 62304171)the China Postdoctoral Science Foundation(2022M722500)+1 种基金the Fundamental Research Funds for the Central Universities(Grants nos.ZYTS2308 and 20103237929)Startup Foundation of Xidian University(10251220001).
文摘Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,however,constrain their delicate constructions.Herein,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix.This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in M_(x)S_(y)/carbon composites(M-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial polarization.Such“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time.Consequently,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric response.Harnessing defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.
文摘This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature<300℃.Sulfur vapor is a highly flammable gas,which then auto-ignites to produce a flame.This behavior suggests that an O_(2)-S gas-gas reaction mechanism may contribute to all-solid-state battery thermal runaway.To improve all-solid-state battery safety,current work focuses on eliminating the O_(2)source by changing the cathode active material.The conclusion of this study suggests that all-solidstate battery safety can also be realized by the development of solid-state electrolytes with less susceptibility to sulfur volatilization.
文摘Transition metal sulfides are considered promising anode materials for sodium-ion batteries(SIBs)due to their high theoretical capacity and low synthesis cost.However,is-sues such as poor cyclic stability and rate performance,arising from volume expansion and structural degradation,remain sig-nificant challenges.We report a novel FeS_(2)/CoS_(2) heterostruc-ture embedded in a 3D carbon aerogel matrix(FeS_(2)/CoS_(2)@C)synthesized by a cross-linking and vulcanization process.The resulting core-shell structure,with bimetallic FeS_(2)/CoS_(2) nano-particles encapsulated in a conductive carbon shell,effectively reduces the adverse effects of volume changes during sodiation/desodiation cycles.The 3D porous carbon network increases both ion and electron diffusion,while preventing agglomeration of the active material and maintaining interface integrity.The FeS_(2)/CoS_(2)@C composite has an outstanding electrochemical performance,including a high specific capacity of 725 mAh g^(-1)at 0.5 A g^(-1)and an exceptional rate capability of 572 mAh g^(-1)at 10 A g^(-1).It also has remarkable cycling stability with no signific-ant capacity decay over 1000 cycles at 5 A g^(-1).
基金National Natural Science Foundation of China(52171101)Fundamental Research Funds for the Central Universities(2024IAIS-QN009)National Key R&D Program of China(2021YFB3701100)。
文摘CuS-C50,the cathode materials for magnesium ion batteries,was synthesized by adding the surfactant cetyltrimethyl ammonium bromide(CTAB)and adjusting the percentage of ethylene glycol to 50vol%in hydrothermal synthesis process.Results show that CuS-C50 has the complete nanoflower structure.In aluminum chloride-pentamethylcydopentodiene/tetrahydrofuran(APC/THF)electrolyte,the CuS-C50 exhibits a high specific capacity of 331.19 mAh/g when the current density is 50 mA/g and still keeps a specific capacity of 136.92 mAh/g over 50 cycles when the current density is 200 mA/g.Results of morphology characterizations indicate that the complete nanoflower structure can provide more active sites and reduce the barriers for Mg^(2+)movement,eventually improving the charge and discharge performance of the CuS cathode materials for magnesium ion batteries.
基金financially supported by the Natural Science Foundation of Jiangsu Province(Grant No.BK20241181)the State Key Laboratory of AnalyticalChemistry for Life Science,School of Chemistry and Chemical Engineering,Nanjing University(Grant No.SKLACLS2419)。
文摘Using 2-dicyanomethylene-3-cyano-4,5,5-trimethyl-2,5-dihydrofuran(TCF)as a near-infrared fluorescent chromophore,we designed and synthesized a TCF-based fluorescent probe TCF-NS by introducing 2,4-dinitrophenyl ether as the recognized site for H_(2)S.The probe TCF-NS displayed a rapid-response fluorescent against H_(2)S with high sensitivity and selection but had no significant fluorescence response to other biothiols.Furthermore,TCF-NS was applied to sense H_(2)S in living cells successfully with minimized cytotoxicity and a large Stokes shift.
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 the Foundation for Innovative Research Groups of the National Natural Science Foundation of China(No.52121004)the National Natural Science Foundation of China(No.52274414).
文摘Sulfide precipitation is an effective method for treating acidic heavy metal wastewater.However,the process often generates tiny particles with poor settling performance.The factors and mechanisms influencing particle size and settling performance remain unclear.In this study,the growth behavior of CuS particles generated by two sulfide precipitation methods,gas-liquid and liquid-liquid sulfidation,was investigated.The effects of acidity,sulfur-to-copper molar ratio,and temperature on particle size were analyzed.The results showed that increasing the temperature had an adverse effect on CuS particle growth.Additionally,we found that acidity and sulfur-to-copper molar ratio had a more significant impact on particle growth in the liquid-liquid sulfidation system than in the gas-liquid sulfidation system.Based on supersaturation calculations and XPS analysis,it is found that particle growth in gas-liquid sulfidation systems is mainly influenced by supersaturation,while particle growth in liquid-liquid sulfidation systems is mainly affected by surface charge.This study provides valuable insights into the factors that influence particle growth in sulfide precipitation and can inform the development of strategies to improve the effective precipitation of sulfide nanoparticles in acidic wastewater.
基金supported by the Science and Technology Project of Southwest Petroleum University(No.2021JBGS03)the Local Science and Technology Development Fund Projects Guided by the Central Government of China(No.2021ZYD0060)+2 种基金the National Natural Science Foundation of China(Nos.22209143 and 52371241)Guangdong High-level Innovation Institute Project(Nos.2021B0909050001 and 2021CX02L365)Guangdong Basic and Applied Basic Research Foundation(No.2023B1515120095).
文摘The development of efficient catalysts for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is of great significance for the practical application of water splitting in alkaline electrolytes.Transition metal sulfide electrocatalysts have been widely recognized as efficient catalysts for water splitting in alkaline media.In this work,an original and efficient synthesis strategy is proposed for the fabrication of asymmetric anode(N-(Co-Cu)S_(x))and cathode(N-CoS/Cu_(2)S).Impressively,these electrodes exhibit superior performance,benefiting from the construction of three-dimensional(3D)structures and the electronic structure adjustment caused by N-doping with increased active sites,improved mass/charge transport and enhanced evolution and release of gas bubbles.Hence,N-(Co-Cu)S_(x)anode exhibits excellent OER performance with only 217 mV overpotential at 10 mA·cm^(-2),while N-CoS/Cu_(2)S cathode possesses excellent HER performance with only 67 mV overpotential at 10 mA·cm^(-2).N-(Co-Cu)S_(x)||N-CoS/Cu_(2)S electrolyzer presents a low cell voltage of 1.53 V at 10 mA·cm^(-2)toward overall water splitting,which is superior to most recently reported transition metal sulfide-based catalysts.
基金financially supported by the National Natural Science Foundation of China(No.22071043).
文摘By introduction of hydrogen peroxide into the reaction system of ZrOCl_(2)·8H_(2)O and K14[As_(2)W_(19)O_(67)(H_(2)O)],a novel polyoxometalate K_(8)Na_(19.5)H_(0.5)[Zr_(2)(O_(2))_(2)(β-AsVW_(10)O_(38))]4·68H_(2)O(1)has been successfully obtained via one-pot method and systematically characterized by IR,XPS,solid UV spectra,PXRD pattern,and TGA analysis.The analysis of X-ray crystallography exhibits that compound 1 crystallizes in the triclinic space group P-1 and presents a novel square-shaped Zr-substituted tetrameric polyoxometalate.The catalytic oxidation of sulfides by 1 are carried out,which demonstrate that 1 exhibits a good performance for the catalytic oxidation of sulfides to sulfones with high conversion(100%)and high selectivity(100%).
基金X.H.acknowledges the financial support by Australian Research Council(ARC)Future Fellowship(FT190100756)M.P.S.gratefully acknowledges the support by the ARC under Discovery Early Career Researcher Award(DECRA)(DE210101565)and Discovery Project(DP230101676).
文摘The discovery of quantum dots(QDs)stands as one of the paramount technological breakthroughs of the 20th century.Their versatility spans from everyday applications to cutting-edge scientific research,encompassing areas such as displays,lighting,photocatalysis,bio-imaging,and photonics devices and so on.Among the myriad QDs technologies,industrially relevant CuInS_(2)(CIS)QDs have emerged as promising alternatives to traditional Cd-and Pb-based QDs.Their tunable optoelectronic properties,high absorption coefficient,compositional flexibility,remarkable stability as well as Restriction of Hazardous Substances-compliance,with recent trends revealing a renewed interest in this material for various visible and near-infrared technological applications.This review focuses on recent advancements in CIS QDs as multidisciplinary field from its genesis in the mid-1990 to date with an emphasis on key breakthroughs in their synthesis,surface chemistry,post-synthesis modifications,and various applications.First,the comparation of properties of CIS QDs with relevant knowledge from other classes of QDs and from Ⅰ-Ⅱ-Ⅲ semiconductors as well is summarized.Second,recent advances in the synthesis methods,structure-optoelectronic properties,their defects,and passivation strategies as well as CIS-based heterostructures are discussed.Third,the state-of-the-art applications of CIS QDs ranging from solar cells,luminescence solar concentrations,photocatalysis,light emitting diodes,bioimaging and some emerging applications are summarized.Finally,we discuss open challenges and future perspectives for further advancement in this field.
基金supported by National Key Research and Development Program of China(No.2023YFD2200503)the Young Elite Scientists Sponsorship Program from National Forestry and Grassland Administration of China(No.2019132614)+1 种基金the Science and Technology Innovation Program of Hunan Province(Nos.2021RC3103 and 2022RC3054)the Scientific Research Project of Hunan Provincial Education Department(Nos.23B0276 and 21B0225).
文摘Industrial high-current-density oxygen evolution catalyst is the key to accelerating the practical application of hydrogen energy.Herein,Co_(9)S_(8)/CoS heterojunctions were rationally encapsulated in S,N-codoped carbon((Co_(9)S_(8)/CoS)@SNC)microleaf arrays,which are rooted on S-doped carbonized wood fibers(SCWF).Benefiting from the synergistic electronic interactions on heterointerfaces and the accelerated mass transfer by array structure,the obtained self-supporting(Co_(9)S_(8)/CoS)@SNC/SCWF electrode exhibits superior performance toward alkaline oxygen evolution reaction(OER)with an ultra-low overpotential of 274 mV at 1000 mA/cm^(2),a small Tafel slope of 48.84 mV/dec,and ultralong stability up to 100 h.Theoretical calculations show that interfacing Co_(9)S_(8)with CoS can upshift the d-band center of the Co atoms and strengthen the interactions with oxygen intermediates,thereby favoring OER performance.Furthermore,the(Co_(9)S_(8)/CoS)@SNC/SCWF electrode shows outstanding rechargeability and stable cycle life in aqueous Zn-air batteries with a peak power density of 201.3 mW/cm^(2),exceeding the commercial RuO_(2)and Pt/C hybrid catalysts.This work presents a promising strategy for the design of high-current-density OER electrocatalysts from sustainable wood fiber resources,thus promoting their practical applications in the field of electrochemical energy storage and conversion.
基金the financial support from China Postdoctoral Science Foundation(2024M750177)National Natural Science Foundation of China(52474345)and Science and Technology Major Project of WuHan(2023020302020572).
文摘The properties of direct reduced iron(DRI)smelting slag are important in the DRI melting process for molten iron production to ensure the slag-iron separation and quality of molten iron.The influence of binary basicity on the viscosity and sulfide capacity of CaO-SiO_(2)-MgO-Al_(2)O_(3)-FeO slag was investigated by the high-temperature experiments,structural analysis and thermodynamic calculation.The viscosity of the slag decreased rapidly with an increase in basicity from 0.4 to 0.8,and this trend became slow as the basicity further increased to 1.2.For the acidic slag with basicity of 0.4 and 0.6,the viscosity at 1500℃ was higher than 0.6 Pa s,which was harmful for the fluidity of slag melt.The slags with basicity of 0.8,1.0 and 1.2 at 1500℃ showed the low viscosity of less than 0.6 Pa s.For the basic slag with basicity of 1.0 and 1.2,the rapid precipitation of melilite led to the abrupt increase behavior of the viscosity,and the acidic slag showed the gentle temperature-viscosity curves.The Raman analysis revealed that the conversion from Q^(3) to Q^(2),Q^(1) and Q^(0) mainly occurred with the basicity increasing from 0.4 to 0.8,and the conversion from Q^(2) to Q^(1) and Q^(0) was dominant with further increase in basicity to 1.2,decreasing the degree of polymerization.The sulfide capacity was improved with the increasing basicity due to the increase in O^(2-)ions,and CaS could be formed dominantly for S^(2-)stabilization in present slag.The sulfur partition ratio was derived from sulfide capacity,and the values of sulfur partition ratio at basicity of 0.4 and 0.6 were much smaller than those at basicity of 0.8,1.0 and 1.2,indicating a weak desulfurization ability of the slag with a low basicity.
基金Projects(52104355,52074363,52374364)supported by the National Natural Science Foundation of ChinaProject(2023YFC2907904)supported by the National Key R&D Program of China。
文摘Traditional pyrometallurgical and hydrometallurgical methods to extract bismuth from sulfide ores face problems such as high cost,low-concentration SO_(2)generation,and long process time.In this study,the cyclone technology and slurry electrolysis method were combined.The bismuth sulfide ore was dissolved directly at the anode,while the high purity bismuth was deposited efficiently at the cathode under the advantages of the two methods.The short process and high-efficiency extraction of bismuth sulfide ore were realized,and the pollution of low-concentration SO_(2)was avoided.Then,the effects of several crucial experimental conditions(current density,reaction time,temperature,pH,liquid-solid ratio,and circulation flow rate)on the leaching efficiency and recovery efficiency of bismuth were investigated.The leaching and electrowinning mechanisms during the recovery process were also analyzed according to the research results of this paper to better understand the cyclone slurry electrolysis process.The experimental results showed that 95.19%bismuth was leached into the acid solution in the anode area under optimal conditions,and the recovery efficiency and purity of bismuth on the cathode reached 91.13%and 99.26%,respectively,which were better than those by the traditional hydrometallurgy recovery process.
基金financially supported by the National Key R&D Program of China(No.2022YFB2502000)the National Natural Science Foundation of China(Nos.51902079,52072342,52377216 and 52102324)+3 种基金Anhui Provincial Natural Science Foundation(Nos.2008085QE271 and 2208085ME108)Excellent Research and Innovation Team of Anhui Universities(No.2022AH010096)Natural Science Research Project for Anhui Universities(No.2024AH051519)Hefei Institutes of Physical Science,Chinese Academy of Sciences Director's Fund(Nos.BJPY2023B04,YZJJ-GGZX-2022-01 and YZJJ202102)
文摘Lithium sulfide(Li_(2)S)is widely regarded as the next-generation cathode material for rechargeable batteries due to its satisfactory theoretical capacity and excellent compatibility with lithium-free anodes.However,the large-scale applications of Li_(2)S cathodes are limited by the shuttle effect of soluble intermediate lithium polysulfides(LiPSs)and the sluggish redox kinetics of the interconversion between Li_(2)S and sulfur(S).Herein,we report novel nitrogen-doped carbon nanoflakes in-situ embedded with WN-Ni_(2)P heterostructures(WN-Ni_(2)P@NCN)as a multifunctional host to promote the cycling performance and reaction kinetics of Li_(2)S.After loading Li_(2)S,the WNNi_(2)P@NCN/Li_(2)S exhibits stable reversible capacity of 597mAh g^(-1)at 0.5 A g^(-1)over 150 cycles,and superior cycling stability over 800 cycles.The high reversible capacities,excellent cycling properties and superior reaction kinetics of WN-Ni_(2)P@NCN/Li_(2)S are attributed to the strong LiPSs fixation,remarkable catalytic activation and high electronic/ionic conductivity of the WN-Ni_(2)P@NCN framework,confirmed by the experiment and the density function theory calculation results.This work offers a new strategy for designing heterostructure nanoflakes with metal nitride and metal phosphide to facilitate the applications of advanced lithium-sulfur batteries.
基金supported by the National Natural Science Foundation of China(22308206 and 22278255)the Graduate Innovation Fund of Shaanxi University of Science and Technology,China。
文摘The development of high-performance and stable electrocatalysts for oxygen evolution reaction(OER)is essential to improve the overall efficiency of water splitting.Here,S-vacancies and iron-doped nickel sulfide nanosheets(Vs-Ni_(2)Fe_(1)S_(2)/NF)were successfully prepared on the surface of nickel foam via solvothermal reaction of nickel-iron layered double hydroxide with sublimed sulfur added with sodium borohydride.Under the synergistic regulation of iron-doped and S-vacancies,Vs-Ni_(2)Fe_(1)S_(2)/NF shows excellent electrocatalytic performance and long-term durability.To reach current densities of 10 and500 mA cm^(-2),Vs-Ni_(2)Fe_(1)S_(2)/NF requires only 185(±5)and 248(±5)mV overpotential,respectively,and can maintain long stability for 350 h at 500 mA cm^(-2).The change of the mechanical pathway from adsorbate evolution mechanism to lattice oxygen oxidation mechanism is due to the increased acidity of the Ni site in Vs-Ni_(2)Fe_(1)S_(2)/NF,which facilitates the decouped proton and electron transfer process.Density functional calculation results show that the introduction of Fe atoms and S vacancies in Ni3S_(2)can enhance the conductivity of the intermediates by regulating the electronic structure of the intermediates,optimize the adsorption or desorption energy,and thus significantly improve the OER activity.For Vs-Ni_(2)Fe_(1)S_(2)/NF(+,-)cell,a voltage of 1.56 V is required to achieve 10 mA cm^(-2).In addition,Vs-Ni_(2)Fe_(1)S_(2)/NF catalyst also showed low overpotential(270 mV at 100 mA cm^(-2))and high alkaline tolerance(100 h at 100 mA cm^(-2))at 30 wt%KOH of 70℃.This shows that it has potential industrial application.
