One of the contaminants in coal is sulphur. The adverse impact of sulfur on coal, such as environmental pollution, degradation of steel quality, and reduction of coal’s thermal value, has led to the attention of sulf...One of the contaminants in coal is sulphur. The adverse impact of sulfur on coal, such as environmental pollution, degradation of steel quality, and reduction of coal’s thermal value, has led to the attention of sulfur separation methods in recent decades. Leaching (chemical dissolution) is one of the best methods for desulfurising coal, reducing sulfur in coal. In this study, hydrogen peroxide as an oxidising agent on sulfuric acid yield in reducing sulfur types of coal and chemical structure and the organic texture of high sulfur coal was investigated. The experiments were designed using a three-level response surface methodology with four duplicate points and 27 experiments. The independent variables studied were temperature, time, stirring speed and ratio of sulfuric acid to hydrogen peroxide. Dependent variables included reduction percentage of total, pyritic and organic sulfur. This study showed that 99.99% of total sulfur, 30.11% of pyritic sulfur and 69.08% of organic sulfur were reduced. These values were obtained at a temperature of 60°C, time 120 min, stirring speed 200 rpm and 3:1 ratio of sulfuric acid to hydrogen peroxide. Significant changes were observed by infrared spectroscopy (FTIR) of the coal structure before and after desulphurisation. On the other hand, the studies showed no specific changes in the bonds related to the organic coal matrix. The results showed that this method could be used as a secure process for removing inorganic and organic sulfur without destroying the organic coal matrix.展开更多
Coal-based graphene quantum dots(GQDs) were successfully produced via a one-step chemical synthesis from six different coal ranks, from which two superhigh organic sulfur(SHOS) coals were selected as natural S-doped c...Coal-based graphene quantum dots(GQDs) were successfully produced via a one-step chemical synthesis from six different coal ranks, from which two superhigh organic sulfur(SHOS) coals were selected as natural S-doped carbon sources for the preparation of S-doped GQDs. The effects of coal properties on coal-based GQDs were analyzed by means of high-resolution transmission electron microscopy(HRTEM), X-ray diffraction(XRD), Fourier transform infrared(FTIR) spectroscopy, X-ray photoelectron spectroscopy(XPS), ultraviolet-visible(UV-Vis) absorption spectroscopy, and fluorescence emission spectra. It was shown that all coal samples can be used to prepare GQDs, which emit bluegreen and blue fluorescence under ultraviolet light. Anthracite-based GQDs have a hexagonal crystal structure without defects, the largest size, and densely arranged carbon rings in their lamellae; the highrank bituminous coal-based GQDs are relatively reduced in size, with their hexagonal crystal structure being only faintly visible; the low-rank bituminous coal-based GQDs are the smallest, with sparse lattice fringes and visible internal defects. As the metamorphism of raw coals increases, the yield decreases and the fluorescence quantum yield(QY) initially increases and then decreases. Additionally, the surface of GQDs that were prepared using high-rank SHOS coal(high-rank bituminous coal) preserves rich sulfur content even after strong oxidation, which effectively adjusts the bandgap and improves the fluorescence QY. Thus, high-rank bituminous coal with SHOS content can be used as a natural S-doped carbon source to prepare S-doped GQDs, extending the clean utilization of low-grade coal.展开更多
Sulfatases which cleave sulfate esters in biological systems are key enzymes that deserve special attention due to their significant roles in organic sulfur (OS) mineralization and inorganic sulfur () release. In this...Sulfatases which cleave sulfate esters in biological systems are key enzymes that deserve special attention due to their significant roles in organic sulfur (OS) mineralization and inorganic sulfur () release. In this study, in-vitro experiments were conducted to evaluate S bonded substrate hydrolysis by a commercially available arylsulfatase (EC 3.1.6.1) from Aerobacter aerogenes. The enzyme-substrate interactions were assessed to determine: 1) rate of hydrolysis, 2) catalytic efficiency, 3) thermal stability, and 4) optimal pH of this enzyme. Arylsulfatase exhibited substrate hydrolysis with a high affinity for p-nitrophenyl sulfate (potassium 4-nitrophenyl sulfate (pNPS)). The optimum activity for the enzyme was observed to occur at a pH of 7.1. The optimal temperature was 37°C but ranged from 35°C - 45°C. The apparent Km and Kcat of the enzyme for pNPS hydrolysis at the optimal pH, and temperature were determined to be 1.03 mM and 75.73 μM/min, respectively. This work defines the catalytic and kinetic properties of arylsulfatase (EC 3.1.6.1) and confirms the optimal conditions for sulfatase activity testing. The resulting information is useful in elucidating the contributions that individual enzymes have for specific reactions rather than relying on traditional total enzyme activity measurements.展开更多
Cold diffusion methods are used to separate and quantify the three reduced inorganic sulfur species into acid volatile sulfide(AVS), pyrite–S and element sulfur(ES) in the sediments of the Yellow and East China Seas....Cold diffusion methods are used to separate and quantify the three reduced inorganic sulfur species into acid volatile sulfide(AVS), pyrite–S and element sulfur(ES) in the sediments of the Yellow and East China Seas. The results show that up to 25.02 μmol/g of AVS, 113.1 μmol/g of pyrite–S and 44.4 μmol/g of ES are observed in the sediments of the Yellow Sea and East China Sea. Pyrite–S is the predominant sulfide mineral in the sediments, while the concentration of AVS is quite low at most stations in the study area. The amounts and reactivity of organic matter are the primary limited factor for the sulfide formation, while an iron limitation and a sulfate limitation are not observed in the sediments of the Yellow Sea and East China Sea. The irregular profiles of the three reduced inorganic sulfur species also reflected the comprehensive influence of sediment composition and sedimentation rates.展开更多
Organic sulfur in high sulfur petroleum coke was treated as the S source for synthesis of ZnS photocatalyst. Experimental results showed that with ball milling and subsequent heating treatment, ZnS compound could be s...Organic sulfur in high sulfur petroleum coke was treated as the S source for synthesis of ZnS photocatalyst. Experimental results showed that with ball milling and subsequent heating treatment, ZnS compound could be successfully synthesized and showed considerable photocatalysis activity for decomposing industrial pollutants. The concentration of methyl orange or ethylene blue may be lowered to less than 5% after being decomposed by the synthesized-ZnS photocatalysis. Results of this study suggested a potential technique of turning high sulfur petroleum cokes from industrial wastes into useful products for environment improvement.展开更多
To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation betwe...To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation between the surface characteristics of four different alumina and the existing Mo species states was established.It was found that the Mo equilibrium adsorption capacity can be used as a specific descriptor to quantitatively evaluate the changes in surface characteristics of different alumina.A lower Mo equilibrium adsorption capacity for alumina means weaker metal-support interaction and the loaded Mo species are easier to transform into MoS2.However,the Mo-O-Al bonds still exist at the metal-support interface.The introduction of cationic surfactant hecadecyl trimethyl ammonium bromide(CTAB)can further improve Mo species dispersion through electrostatic attraction with Mo anions and interaction of its alkyl chain with the alumina surface;meanwhile,the introduction of ethylenediamine tetraacetic acid(EDTA)can complex with Ni ions to enhance the Ni-promoting effect on Mo.Therefore,the NiMo catalyst designed using alumina with lower Mo equilibrium adsorption capacity and the simultaneous addition of EDTA and CTAB exhibits the highest hydrodesulfurization activity for 4,6-dimethyl dibenzothiophene because of its proper metal-support interaction and more well-dispersed Ni-Mo-S active phases.展开更多
There have been several studies on sulfur depletion in dense cores like TMC-1(Taurus Molecular Cloud 1),employing updated reaction networks for sulfur species to explain the missing sulfur in the gas within dense clou...There have been several studies on sulfur depletion in dense cores like TMC-1(Taurus Molecular Cloud 1),employing updated reaction networks for sulfur species to explain the missing sulfur in the gas within dense clouds.Most of these studies used a C/O ratio of 0.7 or lower.We present NSRT(NanShan 26m Radio Telescope)observations of TMC-1 alongside results from time-dependent chemical simulations using an updated chemical network.Our findings highlight the impact of the C/O ratio on the gas-phase evolution of C2S and C3S.The simulation results show that the C/O ratio is an important parameter,playing a fundamental role in determining the gas-phase abundances of sulfur species in dense cores.展开更多
Porous organic molecular materials(POMMs)are an emergent class of molecular-based materials characterized by the formation of extended porous frameworks,mainly held by non-covalent interactions.POMMs represent a varie...Porous organic molecular materials(POMMs)are an emergent class of molecular-based materials characterized by the formation of extended porous frameworks,mainly held by non-covalent interactions.POMMs represent a variety of chemical families,such as hydrogen-bonded organic frameworks,porous organic salts,porous organic cages,C-H···πmicroporous crystals,supramolecular organic frameworks,π-organic frameworks,halogen-bonded organic framework,and intrinsically porous molecular materials.In some porous materials such as zeolites and metal organic frameworks,the integration of multiscale has been adopted to build materials with multifunctionality and optimized properties.Therefore,considering the significant role of hierarchy in porous materials and the growing importance of POMMs in the realm of synthetic porous materials,we consider it appropriate to dedicate for the first time a critical review covering both topics.Herein,we will provide a summary of literature examples showcasing hierarchical POMMs,with a focus on their main synthetic approaches,applications,and the advantages brought forth by introducing hierarchy.展开更多
Glucosinolates(GSLs) are a group of nitrogen-and sulfur-containing secondary metabolites, synthesized primarily in members of the Brassicaceae family, that play an important role in food flavor, plant antimicrobial ac...Glucosinolates(GSLs) are a group of nitrogen-and sulfur-containing secondary metabolites, synthesized primarily in members of the Brassicaceae family, that play an important role in food flavor, plant antimicrobial activity, resistance to insect attack, stress tolerance, and human anti-cancer effects. As a sulfur-containing compound, glutathione has a strong connection with GSLs biosynthesis as a sulfur donor or redox system, and exists in reduced(glutathione;GSH) and oxidized(glutathione disulfide;GSSG) forms. However, the mechanism of GSH regulating GSLs biosynthesis remainds unclear. Hence, the exogenous therapy to pakchoi under normal growth condition and sulfur deficiency condition were conducted in this work to explore the relevant mechanism. The results showed that exogenous application of buthionine sulfoximine, an inhibitor of GSH synthesis, decreased the transcript levels of GSLs synthesis-related genes and transcription factors, as well as sulfur assimilation-related genes under the normal growth condition. Application of exogenous GSH inhibited the expression of GSLs synthesis-and sulfur assimilation-related genes under the normal condition, while the GSLs biosynthesis and the sulfur assimilation pathway were activated by exogenous application of GSH when the content of GSH in vivo of plants decreased owing to sulfur deficiency. Moreover,exogenous application of GSSG increased the transcript levels of GSLs synthesis-and sulfur assimilation-related genes under the normal growth condition and under sulfur deficiency. The present work provides new insights into the molecular mechanisms of GSLs biosynthesis underlying glutathione regulation.展开更多
Understanding the adsorption interactions between carbon materials and sulfur compounds has far-reaching impacts,in addition to their well-known important role in energy storage and conversion,such as lithium-ion batt...Understanding the adsorption interactions between carbon materials and sulfur compounds has far-reaching impacts,in addition to their well-known important role in energy storage and conversion,such as lithium-ion batteries.In this paper,properties of intrinsic B or Si single-atom doped,and B-Si codoped graphene(GR)and graphdiyne(GDY)were investigated by using density functional theory-based calculations,in which the optimal doping configurations were explored for potential applications in adsorbing sulfur compounds.Results showed that both B or Si single-atom doping and B-Si codoping could substantially enhance the electron transport properties of GR and GDY,improving their surface activity.Notably,B and Si atoms displayed synergistic effects for the codoped configurations,where B-Si codoped GR/GDY exhibited much better performance in the adsorption of sulfurcontaining chemicals than single-atom doped systems.In addition,results demonstrated that,after B-Si codoping,the adsorption energy and charge transfer amounts of GDY with sulfur compounds were much larger than those of GR,indicating that B-Si codoped GDY might be a favorable material for more effectively interacting with sulfur reagents.展开更多
Objective:To investigate the relationship between ambient sulfur dioxide(SO2)exposure and semen quality parameters.Methods:A systematic literature search was conducted to identify relevant studies investigating the as...Objective:To investigate the relationship between ambient sulfur dioxide(SO2)exposure and semen quality parameters.Methods:A systematic literature search was conducted to identify relevant studies investigating the association between SO2 exposure and semen quality parameters.This search encompassed the timeframe from January 2000 to May 2023 and included electronic databases such as Web of Science,Google Scholar,PubMed,Cochrane,and Scopus.Pooled effect estimates with 95%confidence intervals(CI)were calculated using percent changes(PC).The meta-analysis included seven studies with 6711 participants and 15087 semen samples.Results:The results revealed a significant negative association between ambient SO2 exposure and certain semen quality parameters.In particular,SO2 exposure was associated with a significant decrease in progressive motility(PC=0.032;95%CI:-0.063 to-0.001;P=0.044)and sperm concentration(PC=-0.020;95%CI:-0.036 to-0.005;P=0.012).However,no statistically significant associations were observed for total sperm count(PC=-0.038;95%CI:-0.079 to 0.003;P=0.070),seminal fluid volume(PC=-0.009;95%CI:-0.048 to-0.030;P=0.662)and sperm motility(PC=-0.17;95%CI:-0.363 to 0.022;P=0.830).In addition,the results of the subgroup analysis revealed specific variables that were associated with the decrease in relevant sperm parameters.Conclusions:This systematic review and meta-analysis provides compelling evidence supporting a consistent negative association between exposure to ambient SO2 and semen quality parameters.展开更多
Organic solar cells(OSCs)have gained conspicuous progress during the past few decades due to the development of materials and upgrading of the device structure.The power conversion efficiency(PCE)of the single-junctio...Organic solar cells(OSCs)have gained conspicuous progress during the past few decades due to the development of materials and upgrading of the device structure.The power conversion efficiency(PCE)of the single-junction device had surpassed 19%.The cathode interface layer(CIL),by optimizing the connection between the active layer and the cathode electrode,has become a momentous part to strengthen the performances of the OSCs.Simultaneously,CIL is also indispensable to illustrating the working mechanism of OSCs and enhancing the stability of the OSCs.In this essay,hybrid CILs in OSCs have been summarized.Firstly,the advancement and operating mechanism of OSCs,and the effects and relevant design rules of CIL are briefly concluded;secondly,the significant influence of CIL on enhancing the stability and PCE of OSCs is presented;thirdly,the characteristics of organic hybrid CIL and organic-inorganic hybrid CIL are introduced.Finally,the conclusion and outlook of CIL are summarized.展开更多
The state-selective cross section data are useful for understanding and modeling the x-ray emission in celestial observations.In the present work,using the cold target recoil ion momentum spectroscopy,for the first ti...The state-selective cross section data are useful for understanding and modeling the x-ray emission in celestial observations.In the present work,using the cold target recoil ion momentum spectroscopy,for the first time we investigated the state-selective single electron capture processes for S^(q+)–He and H_(2)(q=11–15)collision systems at an impact energy of q×20 keV and obtained the relative state-selective cross sections.The results indicate that only a few principal quantum states of the projectile energy level are populated in a single electron capture process.In particular,the increase of the projectile charge state leads to the population of the states with higher principal quantum numbers.It is also shown that the experimental averaged n-shell populations are reproduced well by the over-barrier model.The database is openly available in Science Data Bank at 10.57760/sciencedb.j00113.00091.展开更多
The proper recycling of spent lithium-ion batteries(LIBs)can promote the recovery and utilization of valuable resources,while also negative environmental effects resulting from the presence of toxic and hazardous subs...The proper recycling of spent lithium-ion batteries(LIBs)can promote the recovery and utilization of valuable resources,while also negative environmental effects resulting from the presence of toxic and hazardous substances.In this study,a new environmentally friendly hydro-metallurgical process was proposed for leaching lithium(Li),nickel(Ni),cobalt(Co),and manganese(Mn)from spent LIBs using sulfuric acid with citric acid as a reductant.The effects of the concentration of sulfuric acid,the leaching temperature,the leaching time,the solid-liquid ratio,and the reducing agent dosage on the leaching behavior of the above elements were investigated.Key parameters were optimized using response surface methodology(RSM)to maximize the recovery of metals from spent LIBs.The maxim-um recovery efficiencies of Li,Ni,Co,and Mn can reach 99.08%,98.76%,98.33%,and 97.63%.under the optimized conditions(the sulfuric acid concentration was 1.16 mol/L,the citric acid dosage was 15wt%,the solid-liquid ratio was 40 g/L,and the temperature was 83℃ for 120 min),respectively.It was found that in the collaborative leaching process of sulfuric acid and citric acid,the citric acid initially provided strong reducing CO_(2)^(-),and the transition metal ions in the high state underwent a reduction reaction to produce transition metal ions in the low state.Additionally,citric acid can also act as a proton donor and chelate with lower-priced transition metal ions,thus speeding up the dissolution process.展开更多
Ploughing and fertilization practices in rice-wheat system have deteriorated the soil carbon (C) pools. Conservation agriculture (CA) based management approaches have proven to enhance C sequestration and reverse the ...Ploughing and fertilization practices in rice-wheat system have deteriorated the soil carbon (C) pools. Conservation agriculture (CA) based management approaches have proven to enhance C sequestration and reverse the loss of soil-organic-carbon (SOC), which further enhances soil fertility. Different fractions of SOC pools react to the alterations in management practices and indicate changes in SOC dynamics as compared to total C in the soil. Higher SOC levels in soil have been observed in case of reduced/no-till (NT) practices than conventional tillage (CT). However, between CT and zero tillage/NT, total SOC stocks diminished with an increase in soil depth, which demonstrated that the benefits of SOC are more pronounced in the topsoil under NT. Soil aggregation provides physical protection to C associated with different-sized particles, thus, the improvement in soil aggregation through CA is an effective way to mitigate soil C loss. Along with less soil disturbance, residual management, suitable crop rotation, rational application of manures and fertilizers, and integrated nutrient management have been found to be effective in not only improving soil C stock but also enhancing the soil health and productivity. Thus, CA can be considered as a potential method in the build-up of SOC of soil in rice-wheat system.展开更多
Pyrite is one of the common authigenic minerals in marine sediments.Previous studies have shown that the morphological and isotopic characteristics of pyrite are closely related to the geochemical environment where it...Pyrite is one of the common authigenic minerals in marine sediments.Previous studies have shown that the morphological and isotopic characteristics of pyrite are closely related to the geochemical environment where it is formed.To better understand the for-mation mechanism of authigenic pyrite,we analyzed the isotopic composition,morphology,and distribution of pyrite in the sediment at 500m below the seafloor from Xisha Trough,South China Sea.Mineral morphologies were observed by scanning electron micros-copy and Raman spectrography.X-Ray computed tomography was applied to measure the particle size of pyrite.The size of pyrite crystals in the matrix sediment mainly ranged between 25 and 65µm(av.ca.40µm),although crystals were larger(av.ca.50μm)in the veins.The pyrites had a fine-grained truncated octahedral shape with occasionally well-developed growth steps,which implies the low growth rate and weak anaerobic oxidation of methane-sulfate reduction when pyrite was formed.Theδ^(34)S values of pyrites ranged from+20.8‰Vienna-defined Canyon Diablo Troilite(V-CDT)to+33.2‰V-CDT and from+44.8‰V-CDT to+48.9‰,which suggest two growth stages.In the first stage,with the continuous low methane flux,the pyrite possibly formed in an environment with good access to seawater.In the second stage,the pyrites mainly developed in sediment fractures and appeared in veins,probably due to the limited availability of sulfate.The less exposure of pyrite to the environment in the second stage was probably caused by sediment accumulation or perturbation.In this study,an episodic pyritization process was identified,and the paleoenvironment was reconstructed for the sediment investigated.展开更多
Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore mic...Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.展开更多
This paper is intended to explore soil organic matter and carbon isotope fractionation at three locations of the Passaic River to determine if microbial degradation of organic contaminants in soil is correlated to the...This paper is intended to explore soil organic matter and carbon isotope fractionation at three locations of the Passaic River to determine if microbial degradation of organic contaminants in soil is correlated to the surrounding physical environment. Microbial degradation of organic contaminants is important for the detoxification of toxic substances thereby minimizing stagnation in the environment and accumulating in the food chain. Since organic contaminants are not easily dissolved in water, they will penetrate sediment and end up enriching the adjacent soil. The hypothesis that we are testing is microbial activity and carbon isotope fractionation will be greater in preserved soils than urban soils. The reason why this is expected to be the case is the expectation of higher microbial activity in preserved environments due to less exposure to pollutants, better soil structure, higher organic matter content, and more favorable conditions for microbial growth. This is contrasted with urban soils, which are impacted by pollutants and disturbances, potentially inhibiting microbial activity. We wish to collect soil samples adjacent to the Passaic River at a pristine location, Great Swamp Wildlife Refuge, a suburban location, Goffle Brook Park, Hawthorne NJ, and an urban location, Paterson NJ. These soil samples will be weighed for soil organic matter (SOM) and weighed for isotope ratio mass spectrometry (IRMS) to test organic carbon isotopes. High SOM and δ13C depletion activity indicate microbial growth based on the characteristics of the soil horizon rather than the location of the soil sample which results in degradation of organic compounds.展开更多
Lithium-sulfur(Li-S) batteries have attracted considerable attention as one of the most appealing energy storage systems.Strenuous efforts have been devoted to tackling the tremendous challenges,mainly pertaining to t...Lithium-sulfur(Li-S) batteries have attracted considerable attention as one of the most appealing energy storage systems.Strenuous efforts have been devoted to tackling the tremendous challenges,mainly pertaining to the severe shuttle effect,sluggish redox kinetics and lithium dendritic growth.Single-atomic mediators as promising candidates exhibit impressive performance in addressing these intractable issues.Related research often utilizes a trial-and-error approach,proposing solutions to fabricate single-atomic materials with diversified features.However,comprehensive review articles especially targeting demand-driven preparation are still in a nascent stage.Inspired by these considerations,this review summarizes the design of single-atomic mediators based on the application case-studies in LiS batteries and other metal-sulfur systems.Emerging preparation routes represented by chemical vapor deposition technology are introduced in a demand-oriented classification.Finally,future research directions are proposed to foster the advancement of single-atomic mediators in Li-S realm.展开更多
Applications of lithium-sulfur(Li-S)batteries are still limited by the sluggish conversion kinetics from polysulfide to Li_(2)S.Although various single-atom catalysts are available for improving the conversion kinetic...Applications of lithium-sulfur(Li-S)batteries are still limited by the sluggish conversion kinetics from polysulfide to Li_(2)S.Although various single-atom catalysts are available for improving the conversion kinetics,the sulfur redox kinetics for Li-S batteries is still not ultrafast.Herein,in this work,a catalyst with dual-single-atom Pt-Co embedded in N-doped carbon nanotubes(Pt&Co@NCNT)was proposed by the atomic layer deposition method to suppress the shuttle effect and synergistically improve the interconversion kinetics from polysulfides to Li_(2)S.The X-ray absorption near edge curves indicated the reversible conversion of Li_(2)Sx on the S/Pt&Co@NCNT electrode.Meanwhile,density functional theory demonstrated that the Pt&Co@NCNT promoted the free energy of the phase transition of sulfur species and reduced the oxidative decomposition energy of Li_(2)S.As a result,the batteries assembled with S/Pt&Co@NCNT electrodes exhibited a high capacity retention of 80%at 100 cycles at a current density of 1.3 mA cm^(−2)(S loading:2.5 mg cm^(−2)).More importantly,an excellent rate performance was achieved with a high capacity of 822.1 mAh g^(−1) at a high current density of 12.7 mA cm^(−2).This work opens a new direction to boost the sulfur redox kinetics for ultrafast Li-S batteries.展开更多
文摘One of the contaminants in coal is sulphur. The adverse impact of sulfur on coal, such as environmental pollution, degradation of steel quality, and reduction of coal’s thermal value, has led to the attention of sulfur separation methods in recent decades. Leaching (chemical dissolution) is one of the best methods for desulfurising coal, reducing sulfur in coal. In this study, hydrogen peroxide as an oxidising agent on sulfuric acid yield in reducing sulfur types of coal and chemical structure and the organic texture of high sulfur coal was investigated. The experiments were designed using a three-level response surface methodology with four duplicate points and 27 experiments. The independent variables studied were temperature, time, stirring speed and ratio of sulfuric acid to hydrogen peroxide. Dependent variables included reduction percentage of total, pyritic and organic sulfur. This study showed that 99.99% of total sulfur, 30.11% of pyritic sulfur and 69.08% of organic sulfur were reduced. These values were obtained at a temperature of 60°C, time 120 min, stirring speed 200 rpm and 3:1 ratio of sulfuric acid to hydrogen peroxide. Significant changes were observed by infrared spectroscopy (FTIR) of the coal structure before and after desulphurisation. On the other hand, the studies showed no specific changes in the bonds related to the organic coal matrix. The results showed that this method could be used as a secure process for removing inorganic and organic sulfur without destroying the organic coal matrix.
基金supported by the National Natural Science Foundation of China (grant No. 41172146)National Key Basic Research Program of China (grant No. 2014CB238905)
文摘Coal-based graphene quantum dots(GQDs) were successfully produced via a one-step chemical synthesis from six different coal ranks, from which two superhigh organic sulfur(SHOS) coals were selected as natural S-doped carbon sources for the preparation of S-doped GQDs. The effects of coal properties on coal-based GQDs were analyzed by means of high-resolution transmission electron microscopy(HRTEM), X-ray diffraction(XRD), Fourier transform infrared(FTIR) spectroscopy, X-ray photoelectron spectroscopy(XPS), ultraviolet-visible(UV-Vis) absorption spectroscopy, and fluorescence emission spectra. It was shown that all coal samples can be used to prepare GQDs, which emit bluegreen and blue fluorescence under ultraviolet light. Anthracite-based GQDs have a hexagonal crystal structure without defects, the largest size, and densely arranged carbon rings in their lamellae; the highrank bituminous coal-based GQDs are relatively reduced in size, with their hexagonal crystal structure being only faintly visible; the low-rank bituminous coal-based GQDs are the smallest, with sparse lattice fringes and visible internal defects. As the metamorphism of raw coals increases, the yield decreases and the fluorescence quantum yield(QY) initially increases and then decreases. Additionally, the surface of GQDs that were prepared using high-rank SHOS coal(high-rank bituminous coal) preserves rich sulfur content even after strong oxidation, which effectively adjusts the bandgap and improves the fluorescence QY. Thus, high-rank bituminous coal with SHOS content can be used as a natural S-doped carbon source to prepare S-doped GQDs, extending the clean utilization of low-grade coal.
文摘Sulfatases which cleave sulfate esters in biological systems are key enzymes that deserve special attention due to their significant roles in organic sulfur (OS) mineralization and inorganic sulfur () release. In this study, in-vitro experiments were conducted to evaluate S bonded substrate hydrolysis by a commercially available arylsulfatase (EC 3.1.6.1) from Aerobacter aerogenes. The enzyme-substrate interactions were assessed to determine: 1) rate of hydrolysis, 2) catalytic efficiency, 3) thermal stability, and 4) optimal pH of this enzyme. Arylsulfatase exhibited substrate hydrolysis with a high affinity for p-nitrophenyl sulfate (potassium 4-nitrophenyl sulfate (pNPS)). The optimum activity for the enzyme was observed to occur at a pH of 7.1. The optimal temperature was 37°C but ranged from 35°C - 45°C. The apparent Km and Kcat of the enzyme for pNPS hydrolysis at the optimal pH, and temperature were determined to be 1.03 mM and 75.73 μM/min, respectively. This work defines the catalytic and kinetic properties of arylsulfatase (EC 3.1.6.1) and confirms the optimal conditions for sulfatase activity testing. The resulting information is useful in elucidating the contributions that individual enzymes have for specific reactions rather than relying on traditional total enzyme activity measurements.
基金The National Basic Research Program(973 Program)of China under contract Nos 2010CB428901 and 2011CB409802the National Natural Science Foundation of China under contract Nos 40925017 and 41221004
文摘Cold diffusion methods are used to separate and quantify the three reduced inorganic sulfur species into acid volatile sulfide(AVS), pyrite–S and element sulfur(ES) in the sediments of the Yellow and East China Seas. The results show that up to 25.02 μmol/g of AVS, 113.1 μmol/g of pyrite–S and 44.4 μmol/g of ES are observed in the sediments of the Yellow Sea and East China Sea. Pyrite–S is the predominant sulfide mineral in the sediments, while the concentration of AVS is quite low at most stations in the study area. The amounts and reactivity of organic matter are the primary limited factor for the sulfide formation, while an iron limitation and a sulfate limitation are not observed in the sediments of the Yellow Sea and East China Sea. The irregular profiles of the three reduced inorganic sulfur species also reflected the comprehensive influence of sediment composition and sedimentation rates.
基金financially supported by Beijing Natural Science Foundation (3053018) the Key Project of Chinese Ministry of Education (No.105108)
文摘Organic sulfur in high sulfur petroleum coke was treated as the S source for synthesis of ZnS photocatalyst. Experimental results showed that with ball milling and subsequent heating treatment, ZnS compound could be successfully synthesized and showed considerable photocatalysis activity for decomposing industrial pollutants. The concentration of methyl orange or ethylene blue may be lowered to less than 5% after being decomposed by the synthesized-ZnS photocatalysis. Results of this study suggested a potential technique of turning high sulfur petroleum cokes from industrial wastes into useful products for environment improvement.
基金funding of the National Key Research and Development Plan(Grant 2017YFB0306600)the Project of SINOPEC(NO.117006).
文摘To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation between the surface characteristics of four different alumina and the existing Mo species states was established.It was found that the Mo equilibrium adsorption capacity can be used as a specific descriptor to quantitatively evaluate the changes in surface characteristics of different alumina.A lower Mo equilibrium adsorption capacity for alumina means weaker metal-support interaction and the loaded Mo species are easier to transform into MoS2.However,the Mo-O-Al bonds still exist at the metal-support interface.The introduction of cationic surfactant hecadecyl trimethyl ammonium bromide(CTAB)can further improve Mo species dispersion through electrostatic attraction with Mo anions and interaction of its alkyl chain with the alumina surface;meanwhile,the introduction of ethylenediamine tetraacetic acid(EDTA)can complex with Ni ions to enhance the Ni-promoting effect on Mo.Therefore,the NiMo catalyst designed using alumina with lower Mo equilibrium adsorption capacity and the simultaneous addition of EDTA and CTAB exhibits the highest hydrodesulfurization activity for 4,6-dimethyl dibenzothiophene because of its proper metal-support interaction and more well-dispersed Ni-Mo-S active phases.
基金supported by the Natural Science Foundation of Xinjiang Uygur Autonomous Region (Grant No. 2022D01B221)he Xinjiang Tianchi Talent Program (2023)+4 种基金the NSRT operators for their assistance during the observationspartly supported by the OperationMaintenance and Upgrading Fund for Astronomical Telescopes and Facility Instrumentsbudgeted from the Ministry of Finance of China and administrated by the Chinese Academy of Sciencesthe Urumqi Nanshan Astronomy and Deep Space Exploration Observation and Research Station of Xinjiang (Grant No. XJYWZ2303)
文摘There have been several studies on sulfur depletion in dense cores like TMC-1(Taurus Molecular Cloud 1),employing updated reaction networks for sulfur species to explain the missing sulfur in the gas within dense clouds.Most of these studies used a C/O ratio of 0.7 or lower.We present NSRT(NanShan 26m Radio Telescope)observations of TMC-1 alongside results from time-dependent chemical simulations using an updated chemical network.Our findings highlight the impact of the C/O ratio on the gas-phase evolution of C2S and C3S.The simulation results show that the C/O ratio is an important parameter,playing a fundamental role in determining the gas-phase abundances of sulfur species in dense cores.
基金the MICINN (Spain)(Projects PID2019-104778GB-I00, PID2020-115100GB-I00Excellence Unit “Maria de Maeztu” CEX2019-000919-M)+5 种基金the Royal Society of Chemistryfunded by Generalitat Valenciana(PROMETEU/2021/054 and SEJI/2020/034)the “Ramón y Cajal” program (RYC2019-027940-I)the Royal Society (RGSR1221390)Royal Society of Chemistry (R21-5119312833) for the funding.
文摘Porous organic molecular materials(POMMs)are an emergent class of molecular-based materials characterized by the formation of extended porous frameworks,mainly held by non-covalent interactions.POMMs represent a variety of chemical families,such as hydrogen-bonded organic frameworks,porous organic salts,porous organic cages,C-H···πmicroporous crystals,supramolecular organic frameworks,π-organic frameworks,halogen-bonded organic framework,and intrinsically porous molecular materials.In some porous materials such as zeolites and metal organic frameworks,the integration of multiscale has been adopted to build materials with multifunctionality and optimized properties.Therefore,considering the significant role of hierarchy in porous materials and the growing importance of POMMs in the realm of synthetic porous materials,we consider it appropriate to dedicate for the first time a critical review covering both topics.Herein,we will provide a summary of literature examples showcasing hierarchical POMMs,with a focus on their main synthetic approaches,applications,and the advantages brought forth by introducing hierarchy.
基金funded by the National Natural Science Foundation of China (Grant Nos.31972394 and 31501748)。
文摘Glucosinolates(GSLs) are a group of nitrogen-and sulfur-containing secondary metabolites, synthesized primarily in members of the Brassicaceae family, that play an important role in food flavor, plant antimicrobial activity, resistance to insect attack, stress tolerance, and human anti-cancer effects. As a sulfur-containing compound, glutathione has a strong connection with GSLs biosynthesis as a sulfur donor or redox system, and exists in reduced(glutathione;GSH) and oxidized(glutathione disulfide;GSSG) forms. However, the mechanism of GSH regulating GSLs biosynthesis remainds unclear. Hence, the exogenous therapy to pakchoi under normal growth condition and sulfur deficiency condition were conducted in this work to explore the relevant mechanism. The results showed that exogenous application of buthionine sulfoximine, an inhibitor of GSH synthesis, decreased the transcript levels of GSLs synthesis-related genes and transcription factors, as well as sulfur assimilation-related genes under the normal growth condition. Application of exogenous GSH inhibited the expression of GSLs synthesis-and sulfur assimilation-related genes under the normal condition, while the GSLs biosynthesis and the sulfur assimilation pathway were activated by exogenous application of GSH when the content of GSH in vivo of plants decreased owing to sulfur deficiency. Moreover,exogenous application of GSSG increased the transcript levels of GSLs synthesis-and sulfur assimilation-related genes under the normal growth condition and under sulfur deficiency. The present work provides new insights into the molecular mechanisms of GSLs biosynthesis underlying glutathione regulation.
基金the support of the National Natural Science Foundation of China(Grant No.51472074).
文摘Understanding the adsorption interactions between carbon materials and sulfur compounds has far-reaching impacts,in addition to their well-known important role in energy storage and conversion,such as lithium-ion batteries.In this paper,properties of intrinsic B or Si single-atom doped,and B-Si codoped graphene(GR)and graphdiyne(GDY)were investigated by using density functional theory-based calculations,in which the optimal doping configurations were explored for potential applications in adsorbing sulfur compounds.Results showed that both B or Si single-atom doping and B-Si codoping could substantially enhance the electron transport properties of GR and GDY,improving their surface activity.Notably,B and Si atoms displayed synergistic effects for the codoped configurations,where B-Si codoped GR/GDY exhibited much better performance in the adsorption of sulfurcontaining chemicals than single-atom doped systems.In addition,results demonstrated that,after B-Si codoping,the adsorption energy and charge transfer amounts of GDY with sulfur compounds were much larger than those of GR,indicating that B-Si codoped GDY might be a favorable material for more effectively interacting with sulfur reagents.
文摘Objective:To investigate the relationship between ambient sulfur dioxide(SO2)exposure and semen quality parameters.Methods:A systematic literature search was conducted to identify relevant studies investigating the association between SO2 exposure and semen quality parameters.This search encompassed the timeframe from January 2000 to May 2023 and included electronic databases such as Web of Science,Google Scholar,PubMed,Cochrane,and Scopus.Pooled effect estimates with 95%confidence intervals(CI)were calculated using percent changes(PC).The meta-analysis included seven studies with 6711 participants and 15087 semen samples.Results:The results revealed a significant negative association between ambient SO2 exposure and certain semen quality parameters.In particular,SO2 exposure was associated with a significant decrease in progressive motility(PC=0.032;95%CI:-0.063 to-0.001;P=0.044)and sperm concentration(PC=-0.020;95%CI:-0.036 to-0.005;P=0.012).However,no statistically significant associations were observed for total sperm count(PC=-0.038;95%CI:-0.079 to 0.003;P=0.070),seminal fluid volume(PC=-0.009;95%CI:-0.048 to-0.030;P=0.662)and sperm motility(PC=-0.17;95%CI:-0.363 to 0.022;P=0.830).In addition,the results of the subgroup analysis revealed specific variables that were associated with the decrease in relevant sperm parameters.Conclusions:This systematic review and meta-analysis provides compelling evidence supporting a consistent negative association between exposure to ambient SO2 and semen quality parameters.
基金supported by the National Natural Science Foundation of China(52263017,21965023,52173170,51973087,and22065025)the Science Fund for Distinguished Young Scholars of Jiangxi Province(20212ACB214009)+2 种基金the Natural Science Foundation of Jiangxi Province(20212ACB203010,20224BAB214007 and20212BAB204052)the Training Project of High-level and Highskilled Leading Talents of Jiangxi Province(2023)the Thousand Talents Plan of Jiangxi Province(jxsq2019201004 and jxsq2020101068)。
文摘Organic solar cells(OSCs)have gained conspicuous progress during the past few decades due to the development of materials and upgrading of the device structure.The power conversion efficiency(PCE)of the single-junction device had surpassed 19%.The cathode interface layer(CIL),by optimizing the connection between the active layer and the cathode electrode,has become a momentous part to strengthen the performances of the OSCs.Simultaneously,CIL is also indispensable to illustrating the working mechanism of OSCs and enhancing the stability of the OSCs.In this essay,hybrid CILs in OSCs have been summarized.Firstly,the advancement and operating mechanism of OSCs,and the effects and relevant design rules of CIL are briefly concluded;secondly,the significant influence of CIL on enhancing the stability and PCE of OSCs is presented;thirdly,the characteristics of organic hybrid CIL and organic-inorganic hybrid CIL are introduced.Finally,the conclusion and outlook of CIL are summarized.
基金Project supported by the National Key Research and Development Program of China(Grant No.2017YFA0402400)the National Natural Science Foundation of China(Grant Nos.11974358 and 11934004)+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB34020000)the Heavy Ion Research Facility in Lanzhou(HIRFL).
文摘The state-selective cross section data are useful for understanding and modeling the x-ray emission in celestial observations.In the present work,using the cold target recoil ion momentum spectroscopy,for the first time we investigated the state-selective single electron capture processes for S^(q+)–He and H_(2)(q=11–15)collision systems at an impact energy of q×20 keV and obtained the relative state-selective cross sections.The results indicate that only a few principal quantum states of the projectile energy level are populated in a single electron capture process.In particular,the increase of the projectile charge state leads to the population of the states with higher principal quantum numbers.It is also shown that the experimental averaged n-shell populations are reproduced well by the over-barrier model.The database is openly available in Science Data Bank at 10.57760/sciencedb.j00113.00091.
基金supported by Key R&D Program of Zhejiang Province,China (No.2022C03061)the National Natural Science Foundation of China (No.52074204)the Fundamental Research Funds for the Central Universities (No.2023-vb-032).
文摘The proper recycling of spent lithium-ion batteries(LIBs)can promote the recovery and utilization of valuable resources,while also negative environmental effects resulting from the presence of toxic and hazardous substances.In this study,a new environmentally friendly hydro-metallurgical process was proposed for leaching lithium(Li),nickel(Ni),cobalt(Co),and manganese(Mn)from spent LIBs using sulfuric acid with citric acid as a reductant.The effects of the concentration of sulfuric acid,the leaching temperature,the leaching time,the solid-liquid ratio,and the reducing agent dosage on the leaching behavior of the above elements were investigated.Key parameters were optimized using response surface methodology(RSM)to maximize the recovery of metals from spent LIBs.The maxim-um recovery efficiencies of Li,Ni,Co,and Mn can reach 99.08%,98.76%,98.33%,and 97.63%.under the optimized conditions(the sulfuric acid concentration was 1.16 mol/L,the citric acid dosage was 15wt%,the solid-liquid ratio was 40 g/L,and the temperature was 83℃ for 120 min),respectively.It was found that in the collaborative leaching process of sulfuric acid and citric acid,the citric acid initially provided strong reducing CO_(2)^(-),and the transition metal ions in the high state underwent a reduction reaction to produce transition metal ions in the low state.Additionally,citric acid can also act as a proton donor and chelate with lower-priced transition metal ions,thus speeding up the dissolution process.
文摘Ploughing and fertilization practices in rice-wheat system have deteriorated the soil carbon (C) pools. Conservation agriculture (CA) based management approaches have proven to enhance C sequestration and reverse the loss of soil-organic-carbon (SOC), which further enhances soil fertility. Different fractions of SOC pools react to the alterations in management practices and indicate changes in SOC dynamics as compared to total C in the soil. Higher SOC levels in soil have been observed in case of reduced/no-till (NT) practices than conventional tillage (CT). However, between CT and zero tillage/NT, total SOC stocks diminished with an increase in soil depth, which demonstrated that the benefits of SOC are more pronounced in the topsoil under NT. Soil aggregation provides physical protection to C associated with different-sized particles, thus, the improvement in soil aggregation through CA is an effective way to mitigate soil C loss. Along with less soil disturbance, residual management, suitable crop rotation, rational application of manures and fertilizers, and integrated nutrient management have been found to be effective in not only improving soil C stock but also enhancing the soil health and productivity. Thus, CA can be considered as a potential method in the build-up of SOC of soil in rice-wheat system.
基金supported by the Guangdong Major Project of Basic and Applied Basic Research(No.2020B0301030003).
文摘Pyrite is one of the common authigenic minerals in marine sediments.Previous studies have shown that the morphological and isotopic characteristics of pyrite are closely related to the geochemical environment where it is formed.To better understand the for-mation mechanism of authigenic pyrite,we analyzed the isotopic composition,morphology,and distribution of pyrite in the sediment at 500m below the seafloor from Xisha Trough,South China Sea.Mineral morphologies were observed by scanning electron micros-copy and Raman spectrography.X-Ray computed tomography was applied to measure the particle size of pyrite.The size of pyrite crystals in the matrix sediment mainly ranged between 25 and 65µm(av.ca.40µm),although crystals were larger(av.ca.50μm)in the veins.The pyrites had a fine-grained truncated octahedral shape with occasionally well-developed growth steps,which implies the low growth rate and weak anaerobic oxidation of methane-sulfate reduction when pyrite was formed.Theδ^(34)S values of pyrites ranged from+20.8‰Vienna-defined Canyon Diablo Troilite(V-CDT)to+33.2‰V-CDT and from+44.8‰V-CDT to+48.9‰,which suggest two growth stages.In the first stage,with the continuous low methane flux,the pyrite possibly formed in an environment with good access to seawater.In the second stage,the pyrites mainly developed in sediment fractures and appeared in veins,probably due to the limited availability of sulfate.The less exposure of pyrite to the environment in the second stage was probably caused by sediment accumulation or perturbation.In this study,an episodic pyritization process was identified,and the paleoenvironment was reconstructed for the sediment investigated.
基金This research was supported by Natural Science Foundation of Jiangsu Province(BK20220405)National Natural Science Foundation of China(21834004,22276100,22304086)+5 种基金Key Laboratory for Organic Electronics&Information Displays,NJUPT(GZR2022010010,GZR2023010045)Nanjing Science and Technology Innovation Project for Chinese Scholars Studying Abroad(NJKCZYZZ2022-01)Research Fund for Jiangsu Distinguished Professor(RK030STP22001)Natural Science Research Start-up Foundation of Recruiting Talents of NJUPT(NY221006,NY223051)Natural Science Foundation of the Jiangsu Higher Education Institutions of China(23KJB150025)State Key Laboratory of Analytical Chemistry for Life Science,Nanjing University(SKLACLS2311).
文摘Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.
文摘This paper is intended to explore soil organic matter and carbon isotope fractionation at three locations of the Passaic River to determine if microbial degradation of organic contaminants in soil is correlated to the surrounding physical environment. Microbial degradation of organic contaminants is important for the detoxification of toxic substances thereby minimizing stagnation in the environment and accumulating in the food chain. Since organic contaminants are not easily dissolved in water, they will penetrate sediment and end up enriching the adjacent soil. The hypothesis that we are testing is microbial activity and carbon isotope fractionation will be greater in preserved soils than urban soils. The reason why this is expected to be the case is the expectation of higher microbial activity in preserved environments due to less exposure to pollutants, better soil structure, higher organic matter content, and more favorable conditions for microbial growth. This is contrasted with urban soils, which are impacted by pollutants and disturbances, potentially inhibiting microbial activity. We wish to collect soil samples adjacent to the Passaic River at a pristine location, Great Swamp Wildlife Refuge, a suburban location, Goffle Brook Park, Hawthorne NJ, and an urban location, Paterson NJ. These soil samples will be weighed for soil organic matter (SOM) and weighed for isotope ratio mass spectrometry (IRMS) to test organic carbon isotopes. High SOM and δ13C depletion activity indicate microbial growth based on the characteristics of the soil horizon rather than the location of the soil sample which results in degradation of organic compounds.
基金supported by the National Natural Science Foundation of China(22179089)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX23_3245)support from Suzhou Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies,Suzhou,China。
文摘Lithium-sulfur(Li-S) batteries have attracted considerable attention as one of the most appealing energy storage systems.Strenuous efforts have been devoted to tackling the tremendous challenges,mainly pertaining to the severe shuttle effect,sluggish redox kinetics and lithium dendritic growth.Single-atomic mediators as promising candidates exhibit impressive performance in addressing these intractable issues.Related research often utilizes a trial-and-error approach,proposing solutions to fabricate single-atomic materials with diversified features.However,comprehensive review articles especially targeting demand-driven preparation are still in a nascent stage.Inspired by these considerations,this review summarizes the design of single-atomic mediators based on the application case-studies in LiS batteries and other metal-sulfur systems.Emerging preparation routes represented by chemical vapor deposition technology are introduced in a demand-oriented classification.Finally,future research directions are proposed to foster the advancement of single-atomic mediators in Li-S realm.
基金supported by the National Natural Science Foundation of China(22208039)the Basic Scientific Research Project of the Educational Department of Liaoning Province(LJKMZ20220878)+1 种基金and the Dalian Science and Technology Talent Innovation Support Plan(2022RQ036)supported by the Natural Science and Engineering Research Council of Canada(NSERC),the Canada Research Chair Program(CRC),the Canada Foundation for Innovation(CFI),and Western University。
文摘Applications of lithium-sulfur(Li-S)batteries are still limited by the sluggish conversion kinetics from polysulfide to Li_(2)S.Although various single-atom catalysts are available for improving the conversion kinetics,the sulfur redox kinetics for Li-S batteries is still not ultrafast.Herein,in this work,a catalyst with dual-single-atom Pt-Co embedded in N-doped carbon nanotubes(Pt&Co@NCNT)was proposed by the atomic layer deposition method to suppress the shuttle effect and synergistically improve the interconversion kinetics from polysulfides to Li_(2)S.The X-ray absorption near edge curves indicated the reversible conversion of Li_(2)Sx on the S/Pt&Co@NCNT electrode.Meanwhile,density functional theory demonstrated that the Pt&Co@NCNT promoted the free energy of the phase transition of sulfur species and reduced the oxidative decomposition energy of Li_(2)S.As a result,the batteries assembled with S/Pt&Co@NCNT electrodes exhibited a high capacity retention of 80%at 100 cycles at a current density of 1.3 mA cm^(−2)(S loading:2.5 mg cm^(−2)).More importantly,an excellent rate performance was achieved with a high capacity of 822.1 mAh g^(−1) at a high current density of 12.7 mA cm^(−2).This work opens a new direction to boost the sulfur redox kinetics for ultrafast Li-S batteries.
