A hierarchical reduced graphene oxide-MnO_(2)@polypyrrole coaxial nanotube composite hydrogel was prepared via oxidative polymerization of pyrrole in the presence of MnO_(2)nanotubes,followed by the hydrothermal treat...A hierarchical reduced graphene oxide-MnO_(2)@polypyrrole coaxial nanotube composite hydrogel was prepared via oxidative polymerization of pyrrole in the presence of MnO_(2)nanotubes,followed by the hydrothermal treatment of graphene oxide and MnO_(2)@polypyrrole coaxial nanotubes.The stable composite hydrogel with a hierarchical network was composed of one-dimensional MnO_(2)@polypyrrole coaxial nanotube and two-dimensional graphene nanosheet and characterized by scanning electron microscope,Fourier transform infrared spectroscopy,X-ray diffraction,Brunauer-Emmett-Teller surface,and X-ray photoelectron spectroscopy measurements.The composite hydrogel can be used as an efficient adsorbent for Cr(Ⅵ)removal due to the synergistic interaction between graphene and MnO_(2)@polypyrrole and the hierarchical structure of the hydrogel.Moreover,the composite hydrogel is easily separated because of its stable monolith,and it is reusable(76.8%of removal ability remaining after five adsorption-desorption cycles).The simple fabrication and cost-effective separation process together with the excellent absorption performance endow the composite hydrogel with great potential for practical wastewater treatment.展开更多
The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly co...The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.展开更多
Although metal oxide compounds are considered as desirable anode materials for potassium-ion batteries(PIBs)due to their high theoretical capacity,the large volume variation remains a key issue in realizing metal oxid...Although metal oxide compounds are considered as desirable anode materials for potassium-ion batteries(PIBs)due to their high theoretical capacity,the large volume variation remains a key issue in realizing metal oxide anodes with long cycle life and excellent rate property.In this study,polypyrroleencapsulated Sb_(2)WO_(6)(denoted Sb_(2)WO_(6)@PPy)microflowers are synthesized by a one-step hydrothermal method followed by in-situ polymerization and coating by pyrrole.Leveraging the nanosheet-stacked Sb_(2)WO_(6)microflower structure,the improved electronic conductivity,and the architectural protection offered by the PPy coating,Sb_(2)WO_(6)@PPy exhibits boosted potassium storage properties,thereby demonstrating an outstanding rate property of 110.3 m A h g^(-1)at 5 A g^(-1)and delivering a long-period cycling stability with a reversible capacity of 197.2 m A h g^(-1)after 500 cycles at 1 A g^(-1).In addition,the conversion and alloying processes of Sb_(2)WO_(6)@PPy in PIBs with the generation of intermediates,K_(2)WO_(4)and K_(3)Sb,is determined by X-ray photoelectron spectroscopy,transmission electron microscopy,and exsitu X-ray diffraction during potassiation/depotassiation.Density functional theory calculations demonstrate that the robust coupling between PPy and Sb_(2)WO_(6)endues it with a much stronger total density of states and a built-in electric field,thereby increasing the electronic conductivity,and thus effectively reduces the K^(+)diffusion barrier.展开更多
In situ chemical oxidation polymerization of pyrrole on the surface of sulfur particles was carried out to synthesize a sulfur/polypyrrole (SIPPy) nanocomposite with core-shell structure. The composite was character...In situ chemical oxidation polymerization of pyrrole on the surface of sulfur particles was carried out to synthesize a sulfur/polypyrrole (SIPPy) nanocomposite with core-shell structure. The composite was characterized by elemental analysis, X-ray diffraction, scanning/transmission electron microscopy, and electrochemical measurements. XRD and FTIR results showed that sulfur well dispersed in the core-shell structure and PPy structure was successfully obtained via in situ oxidative polymerization of pyrrole on the surface of sulfur particles. TEM observation revealed that PPy was formed and fixed to the surface of sulfur nanoparticle after polymerization, developing a well-defined core-shell structure and the thickness of PPy coating layer was in the range of 20-30 nm. In the composite, PPy worked as a conducting matrix as well as a coating agent, which confined the active materials within the electrode. Consequently, the as prepared SIPPy composite cathode exhibited good cycling and rate performances for rechargeable lithium/sulfur batteries. The resulting cell containing SIPPy composite cathode yields a discharge capacity of 1039 mAh·g^-1 at the initial cycle and retains 59% of this value over 50 cycles at 0.1 C rate. At 1 C rate, the SIPPy composite showed good cycle stability, and the discharge capacity was 475 mAh·g^-1 after 50 cycles.展开更多
Polypyrrole(PPy)is wildly used as electrode material in supercapacitors due to its high conductivity,low cost,ease of handling,and ease of fabrication.However,limited capacitance and poor cycling stability hinder its ...Polypyrrole(PPy)is wildly used as electrode material in supercapacitors due to its high conductivity,low cost,ease of handling,and ease of fabrication.However,limited capacitance and poor cycling stability hinder its practical application.After developing carboxylated cellulose nanocrystals(CNC-COO^(-))as immobile dopants for PPy to improve its cycling stability,we investigated the effect of different commonly used salts(KCl,NaCl,KBr,and NaClO_(4))as dopants during electrode fabrication by electropolymerization.The film’s capacitance increased from 160.6 to 183.4 F g^(-1)after adding a combination of KCl and NaClO_(4) into the electrodeposition electrolyte.More importantly,the porous and interconnected PPy/CNC-COO^(-)-Cl-(Cl O_(4)^(-))_0.5 electrode film exhibited an excellent capacitance of 125.0 F g^(-1)(0.78 F cm^(-2))at a high current density of 2.0 Ag^(-1)(20 m A cm^(-2),allowing charging in less than 1 min),increasing almost 204%over PPy/CNC-COO-films.A symmetric PPy/CNC-COO^(-)-Cl-(ClO_(4)^(-))_0.5 supercapacitor retained its full capacitance after 5000 cycles,and displayed a high energy density of 5.2 Wh kg^(-1)at a power density of 25.4 W kg^(-1)(34.5μWh cm^(-2) at 1752.3μW cm^(-2)).These results reveal that the porous structure formed by doping with CNC-COO-and inorganic salts opens up more active reaction areas to store charges in PPy-based films as the stiff and ribbon-like CNC-COO-as permanent dopants improve the strength and stability of PPy-based films.Our demonstration provides a simple and practical way to deposit PPy based supercapacitors with high capacitance,fast charging,and excellent cycling stability.展开更多
To reduce the environmental pollution and meet the needs for wearable electronic devices, new requirements for electromagnetic interference(EMI) shielding materials include flexibility, biodegradability, and biocompat...To reduce the environmental pollution and meet the needs for wearable electronic devices, new requirements for electromagnetic interference(EMI) shielding materials include flexibility, biodegradability, and biocompatibility. Herein, we reported a polypyrrole-coated zein/epoxy(PPy/ZE) ultrafine fiber mat which was inherently biodegradable and skin-friendly. In addition, it could maintain its ultrafine fibrous structure after coating, which could provide the mat with mechanical compliance, high porosity, and a large specific area for high EMI shielding. With the assistance of the epoxide cross-linking, the breaking stresses of the PPy/ZE fiber mats could achieve 3.3 MPa and 1.4 MPa and the strains were 40.1% and 83.0% in dry and wet states, respectively, which met the needs of various wearable electronic devices. Along with the extension in the PPy treatment duration, more PPy was loaded on the fiber surfaces, which formed more integrated and conductive paths to generate increasing conductivities up to 401.76 S·m^(-1). Moreover, the EMI shielding performance was raised to 26.84 dB. The biobased mats provide a green and efficient choice for EMI shielding materials, which may be a promising strategy to address EMI problems in multiple fields.展开更多
A nano sulfur-based composite cathode material featured by uniform core@shell-structured sulfur@polypyrrole nanoparticles sandwiched in three-dimensional graphene sheets conductive network(S@PPy/GS) is fabricated vi...A nano sulfur-based composite cathode material featured by uniform core@shell-structured sulfur@polypyrrole nanoparticles sandwiched in three-dimensional graphene sheets conductive network(S@PPy/GS) is fabricated via a facile solution-based method. The S@PPy nanoparticles are synthesized by in situ chemical oxidative polymerization of pyrrole on the surface of sulfur particles,and then graphene sheets are covered outside the S@PPy nanoparticles,forming a three-dimensional conductive network. When evaluating the electrochemical performance of S@PPy/GS in a lithium–sulfur battery,it delivers large discharge capacity,excellent cycle stability,and good rate capability. The initial discharge capacity is up to 1040 m Ah/g at 0.1 C,the capacity can remain 537.8 m Ah/g at 0.2 C after 200 cycles,even at a higher rate of 1 C,the specific capacity still reaches 566.5 m Ah/g. The good electrochemical performance is attributed to the unique structure of S@PPy/GS,which can not only provide an excellent transport of lithium and electron ions within the electrodes,but also retard the shuttle effect of soluble lithium polysulfides effectively,thus plays a positive role in building better lithium-sulfur batteries.展开更多
We investigated the removal of the organic dye rhodamine B in wastewater with recyclable AgBr/polypyrrole(PPy)nano-photocatalysts.With PPy as an active base for electron transfer,and hexadecyltrimethylammonium bromide...We investigated the removal of the organic dye rhodamine B in wastewater with recyclable AgBr/polypyrrole(PPy)nano-photocatalysts.With PPy as an active base for electron transfer,and hexadecyltrimethylammonium bromide(CTAB)as both the soft-templating agent and the bromine source,a series of AgBr/PPy nano-photocatalysts containing various proportions of silver were prepared in a convenient one-step synthesis procedure.The synthesized catalysts were characterized by TG analysis to reveal that,in comparison with pure PPy,the interaction between PPy and AgBr led to increased thermal stability.Chemical combination of PPy and AgBr was observed through XRD and XPS analyses.For the morphology study,the AgBr particles were found to be well dispersed in the PPy nanowire network from SEM results.In the photodegradation experiments,up to 92%rhodamine B was degraded by the AgBr/PPy catalysts in the period of 1 hour under 254 nm UV light.The catalysts could maintain 60%catalytic efficiency after 3 cycles in the recyclability test.展开更多
Lithium–sulfur batteries are promising next-generation energy storage devices beyond conventional lithium ion batteries. However, it suffers from rapid capacity fading and poor cyclic stability. Here we report a faci...Lithium–sulfur batteries are promising next-generation energy storage devices beyond conventional lithium ion batteries. However, it suffers from rapid capacity fading and poor cyclic stability. Here we report a facile in situ sulfur deposition and chemical oxidative polymerization method for preparing acetylene black/sulfur@polypyrrole(AB/S@PPy) composite as a cathode material for lithium–sulfur batteries. It is demonstrated that PPy is covered uniformly onto the surface of the AB/S composite forming a core–shell structure. In the structure, AB in the matrix and PPy on the surface acts as a combined conductive framework to provide ions and electrons transport pathways, and to inhibit the dissolution or diffusion of polysulfide into the electrolyte. The as-designed AB/S@PPy composite exhibits excellent rate capability and cyclic stability. The initial discharge specific capacity is as high as 1179.4 m Ah/g, and remains at769.3 m Ah/g after 80 cycles at 0.2 C. Even at a high rate(0.5 C), a maximum discharge capacity of 811.1 m Ah/g is still achieved for the AB/S@PPy composite after activation, and the capacity retention is over62.5% after 200 cycles.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
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
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
The removal of organic sulfur through catalytic hydrolysis is a significant area of research in the field of desulfurization.This review provides an overview of recent advancements in catalytic hydrolysis technology o...The removal of organic sulfur through catalytic hydrolysis is a significant area of research in the field of desulfurization.This review provides an overview of recent advancements in catalytic hydrolysis technology of organic sulfur,including the activity,stability,and atmosphere effects of hydrolysis catalysts.The emphasis is on strategies for enhancing hydrolysis activity and anti-oxygen poisoning property of catalysts.Surface modification,metal doping and nitrogen doping have been found to improve the activity of catalysts.Alkaline components modification is the most commonly used method,the formation of oxygen vacancies through metal doping and creation of nitrogen basic sites through nitrogen doping also contribute to the hydrolysis of organic sulfur.The strategies for anti-oxygen poisoning are discussed in a systematic manner.The structural regulation of catalysts is beneficial for the desorption and diffusion of hydrogen sulfide(H_(2)S),thereby effectively inhibiting its oxidation.Nitrogen doping and the addition of electronic promoters such as transition metals can protect active sites and decrease the number of active oxygen species.These methods have been proven to enhance the anti-poisoning performance of catalysts.Additionally,this article summarizes how different atmospheres affect the activity of hydrolysis catalysts.The objective of this review is to pave the way for the development of efficient,stable and widely used catalysts for organic sulfur hydrolysis.展开更多
Transition metal sulfides have high theoretical capacities and are considered as potential anode materials for sodium-ion batteries.However,due to low inherent conductivity and significant volume expansion,the electro...Transition metal sulfides have high theoretical capacities and are considered as potential anode materials for sodium-ion batteries.However,due to low inherent conductivity and significant volume expansion,the electrochemical performance is greatly limited.In this study,a nickel/manganese sulfide material(Ni_(0.96)S_(x)/MnS_(y)-NC)with adjustable sulfur vacancies and heterogeneous hollow spheres was prepared using a simple method.The introduction of a concentration-adjustable sulfur vacancy enables the generation of a heterogeneous interface between bimetallic sulfide and sulfur vacancies.This interface collectively creates an internal electric field,improving the mobility of electrons and ions,increasing the number of electrochemically active sites,and further optimizing the performance of Na~+storage.The direction of electron flow is confirmed by Density functional theory(DFT)calculations.The hollow nano-spherical material provides a buffer for expansion,facilitating rapid transfer kinetics.Our innovative discovery involves the interaction between the ether-based electrolyte and copper foil,leading to the formation of Cu_9S_5,which grafts the active material and copper current collector,reinforcing mechanical supporting.This results in a new heterostructure of Cu_9S_5 with Ni_(0.96)S_(x)/MnS_(y),contributing to the stabilization of structural integrity for long-cycle performance.Therefore,Ni_(0.96)S_(x)/MnS_(y)-NC exhibits excellent electrochemical properties following our modification route.Regarding stability performance,Ni0_(.96)S_(x)/MnS_(y)-NC demonstrates an average decay rate of 0.00944%after 10,000 cycles at an extremely high current density of 10000 mA g^(-1),A full cell with a high capacity of 304.2 mA h g^(-1)was also successfully assembled by using Na_(3)V_(2)(PO_(4))_(3)/C as the cathode.This study explores a novel strategy for interface/vacancy co-modification in the fabrication of high-performance sodium-ion batteries electrode.展开更多
Expediting redox kinetics of sulfur species on conductive scaffolds with limited charge accessible surface is considered as an imperative approach to realize energy-dense and power-intensive lithium-sulfur(Li-S)batter...Expediting redox kinetics of sulfur species on conductive scaffolds with limited charge accessible surface is considered as an imperative approach to realize energy-dense and power-intensive lithium-sulfur(Li-S)batteries.In this work,the concept of concurrent hetero-/homo-geneous electrocatalysts is proposed to simultaneously mediate liquid-solid conversion of lithium polysulfides(LiPSs)and solid lithium disulfide/sulfide(Li_(2)S_(2)/Li_(2)S)propagation,the latter of which suffers from sluggish reduction kinetics due to buried conductive scaffold surface by extensive deposition of Li_(2)S_(2)/Li_(2)S.The selected model material to verify this concept is a two-in-one catalyst:carbon nanotube(CNT)scaffold supported iron-cobalt(Fe-Co)alloy nanoparticles and partially carbonized selenium(C-Se)component.The Fe-Co alloy serves as a heterogeneous electrocatalyst to seed Li_(2)S_(2)/Li_(2)S through sulphifilic active sites,while the C-Se sustainably releases soluble lithium polyselenides and functions as a homogeneous electrocatalyst to propagate Li_(2)S_(2)/Li_(2)S via solution pathways.Such bi-phasic mediation of the sulfur species benefits reduction kinetics of LiPS conversion,especially for the massive Li_(2)S_(2)/Li_(2)S growth scenario by affording an additional solution directed route in case of conductive surface being largely buried.This strategy endows the Li-S batteries with improved cycling stability(836 mA h g^(-1)after 180 cycles),rate capability(547 mA h g^(-1)at 4 C)and high sulfur loading superiority(2.96 mA h cm^(-2)at 2.4 mg cm^(-2)).This work hopes to enlighten the employment of bi-phasic electrocatalysts to dictate liquid-solid transformation of intermediates for conversion chemistry batteries.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
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
The self-made MnFeO_(x) catalysts doped with cerium and samarium were prepared by impregnation method for low-temperature selective catalytic reduction(SCR)by NH3.In this work,the surface properties of the series of M...The self-made MnFeO_(x) catalysts doped with cerium and samarium were prepared by impregnation method for low-temperature selective catalytic reduction(SCR)by NH3.In this work,the surface properties of the series of MnFe-based catalysts were studied.The results indicate Sm-modified catalyst have superior low-temperature SCR activity;NO_(x) conversion maintained at nearby to 100%at 90℃ to 240℃.In addition,The N_(2) selectivity of Sm doping remains above 80%in the range of 60℃ to 150℃.In SO_(2) poisoning test,the NO_(x) conversion can be remained>90%after 10 h of reaction.The XPS,NH_(3)-TPD and H_(2)-TPR results show the catalyst with Sm doping enhances the acid sites and oxidation catalytic sites of mixed oxides serves for improving oxygen vacancies and transfer electrons.In situ diffuse reflaxions infrared Fourier transformations spectroscopy(DRIFTS)results show that NO_(x) is more easily adsorbed on the surface after Sm doping,which provided favorable conditions for the NH_(3)-SCR reaction to proceed.The reaction at the catalyst surface will follow the L-H reaction mechanism by transient reaction test.展开更多
Refinery sour water primarily originates from the tops of towers in various units and coker condensate,and cannot be discharged directly to a wastewater treatment plant due to high levels of chemical oxygen demand(COD...Refinery sour water primarily originates from the tops of towers in various units and coker condensate,and cannot be discharged directly to a wastewater treatment plant due to high levels of chemical oxygen demand(COD)and organic sulfur contents.Even after the recovery of H_(2)S from the sour water by the stripping process,the effluent still contains a high concentration of dissolved organic sulfur(DOS),which can have a huge bad influence.While chemical composition of dissolved organic matter(DOM)in refinery wastewater has been extensively studied,the investigation of recalcitrant DOS from sour waters remains unclear.In the present study,chemical composition of sour water DOMs(especially DOS)was investigated using fluorescence spectroscopy(excitation-emission matrix,EEM)and mass spectrometry,including gas chromatography-mass spectrometry(GC-MS)and high-resolution Orbitrap MS.The GC-MS and EEM results showed that volatile and low-aromaticity compounds were effectively removed during the stripping process,while compounds with high hydrophilicity and humification degree were found to be more recalcitrant.The Orbitrap MS results showed that weak-polar oxygenated sulfur compounds were easier to be removed than oxygenated compounds.However,the effluent still contained significant amounts of sulfur-containing compounds with multiple sulfur atoms,particularly in the form of highly unsaturated and aromatic compounds.The Orbitrap MS/MS results of CHOS-containing compounds from the effluent indicate that the sulfur atoms may exist as sulfonates,disulfide bonds,thioethers.Understanding the composition and structure of sour water DOS is crucial for the development of effective treatment processes that can target polysulfide compounds and minimize their impact on the environment.展开更多
Soybean is a crucial crop utilized for both food and oil production,with balanced crop nutrition being a key determinant of soybean yield throughout its growth cycle.Sulfur,an essential nutrient for crop growth,substa...Soybean is a crucial crop utilized for both food and oil production,with balanced crop nutrition being a key determinant of soybean yield throughout its growth cycle.Sulfur,an essential nutrient for crop growth,substantially impacts soybean yield.In this study,two soybean cultivars,Laidou 2 and Hefeng 55,were used to study the changes in nitrogen,phosphorus,potassium,and sulfur contents in soybean plants at different growth stages.Additionally,the effects of dry matter accumulation under five different sulfur levels were examined.The results showed that the sulfur levels had varying effects on the nitrogen,phosphorus,potassium,and sulfur contents and accumulation in different parts of the soybean plants.There were marked differences in the accumulation and distribution of dry matter in different parts of the soybean plant.Soybean dry matter weight shows the best overall performance under the S80 treatment.With increasing sulfur nutrition,the nitrogen,phosphorus,potassium,and sulfur contents in various plant parts exhibited an unimodal trend,reaching maximum values when the sulfur content was 80 mg/L.This study elucidates the dynamic changes in nutrient elements in soybeans under different sulfur levels and is important in guiding the rational application of sulfur fertilizers in agricultural production.展开更多
基金Funded by the Open/Innovation Fund of Hubei Three Gorges Laboratory(No.SK212002)。
文摘A hierarchical reduced graphene oxide-MnO_(2)@polypyrrole coaxial nanotube composite hydrogel was prepared via oxidative polymerization of pyrrole in the presence of MnO_(2)nanotubes,followed by the hydrothermal treatment of graphene oxide and MnO_(2)@polypyrrole coaxial nanotubes.The stable composite hydrogel with a hierarchical network was composed of one-dimensional MnO_(2)@polypyrrole coaxial nanotube and two-dimensional graphene nanosheet and characterized by scanning electron microscope,Fourier transform infrared spectroscopy,X-ray diffraction,Brunauer-Emmett-Teller surface,and X-ray photoelectron spectroscopy measurements.The composite hydrogel can be used as an efficient adsorbent for Cr(Ⅵ)removal due to the synergistic interaction between graphene and MnO_(2)@polypyrrole and the hierarchical structure of the hydrogel.Moreover,the composite hydrogel is easily separated because of its stable monolith,and it is reusable(76.8%of removal ability remaining after five adsorption-desorption cycles).The simple fabrication and cost-effective separation process together with the excellent absorption performance endow the composite hydrogel with great potential for practical wastewater treatment.
基金financially supported by the National Natural Science Foundation of China(No.51933007,No.52373047,No.52302106)the Sichuan Youth Science and Technology Innovation Research Team Project(No.2022JDTD0012)+2 种基金the Program for Featured Directions of Engineering Multidisciplines of Sichuan University(No.2020SCUNG203)the Natural Science Foundation of Sichuan Province(No.2023NSFSC0418)the Program for State Key Laboratory of Polymer Materials Engineering(No.sklpme2022-3-10)。
文摘The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.
基金supported by the National Natural Science Foundation of China(22075147 and 22179063)。
文摘Although metal oxide compounds are considered as desirable anode materials for potassium-ion batteries(PIBs)due to their high theoretical capacity,the large volume variation remains a key issue in realizing metal oxide anodes with long cycle life and excellent rate property.In this study,polypyrroleencapsulated Sb_(2)WO_(6)(denoted Sb_(2)WO_(6)@PPy)microflowers are synthesized by a one-step hydrothermal method followed by in-situ polymerization and coating by pyrrole.Leveraging the nanosheet-stacked Sb_(2)WO_(6)microflower structure,the improved electronic conductivity,and the architectural protection offered by the PPy coating,Sb_(2)WO_(6)@PPy exhibits boosted potassium storage properties,thereby demonstrating an outstanding rate property of 110.3 m A h g^(-1)at 5 A g^(-1)and delivering a long-period cycling stability with a reversible capacity of 197.2 m A h g^(-1)after 500 cycles at 1 A g^(-1).In addition,the conversion and alloying processes of Sb_(2)WO_(6)@PPy in PIBs with the generation of intermediates,K_(2)WO_(4)and K_(3)Sb,is determined by X-ray photoelectron spectroscopy,transmission electron microscopy,and exsitu X-ray diffraction during potassiation/depotassiation.Density functional theory calculations demonstrate that the robust coupling between PPy and Sb_(2)WO_(6)endues it with a much stronger total density of states and a built-in electric field,thereby increasing the electronic conductivity,and thus effectively reduces the K^(+)diffusion barrier.
基金supported by the Natural Science Foundation of Shaanxi Province,China(2013JM2009)
文摘In situ chemical oxidation polymerization of pyrrole on the surface of sulfur particles was carried out to synthesize a sulfur/polypyrrole (SIPPy) nanocomposite with core-shell structure. The composite was characterized by elemental analysis, X-ray diffraction, scanning/transmission electron microscopy, and electrochemical measurements. XRD and FTIR results showed that sulfur well dispersed in the core-shell structure and PPy structure was successfully obtained via in situ oxidative polymerization of pyrrole on the surface of sulfur particles. TEM observation revealed that PPy was formed and fixed to the surface of sulfur nanoparticle after polymerization, developing a well-defined core-shell structure and the thickness of PPy coating layer was in the range of 20-30 nm. In the composite, PPy worked as a conducting matrix as well as a coating agent, which confined the active materials within the electrode. Consequently, the as prepared SIPPy composite cathode exhibited good cycling and rate performances for rechargeable lithium/sulfur batteries. The resulting cell containing SIPPy composite cathode yields a discharge capacity of 1039 mAh·g^-1 at the initial cycle and retains 59% of this value over 50 cycles at 0.1 C rate. At 1 C rate, the SIPPy composite showed good cycle stability, and the discharge capacity was 475 mAh·g^-1 after 50 cycles.
基金supported by the Research Foundation Flanders(grant 3E181170)supported by the China Scholarship Council(CSC,201806220066)。
文摘Polypyrrole(PPy)is wildly used as electrode material in supercapacitors due to its high conductivity,low cost,ease of handling,and ease of fabrication.However,limited capacitance and poor cycling stability hinder its practical application.After developing carboxylated cellulose nanocrystals(CNC-COO^(-))as immobile dopants for PPy to improve its cycling stability,we investigated the effect of different commonly used salts(KCl,NaCl,KBr,and NaClO_(4))as dopants during electrode fabrication by electropolymerization.The film’s capacitance increased from 160.6 to 183.4 F g^(-1)after adding a combination of KCl and NaClO_(4) into the electrodeposition electrolyte.More importantly,the porous and interconnected PPy/CNC-COO^(-)-Cl-(Cl O_(4)^(-))_0.5 electrode film exhibited an excellent capacitance of 125.0 F g^(-1)(0.78 F cm^(-2))at a high current density of 2.0 Ag^(-1)(20 m A cm^(-2),allowing charging in less than 1 min),increasing almost 204%over PPy/CNC-COO-films.A symmetric PPy/CNC-COO^(-)-Cl-(ClO_(4)^(-))_0.5 supercapacitor retained its full capacitance after 5000 cycles,and displayed a high energy density of 5.2 Wh kg^(-1)at a power density of 25.4 W kg^(-1)(34.5μWh cm^(-2) at 1752.3μW cm^(-2)).These results reveal that the porous structure formed by doping with CNC-COO-and inorganic salts opens up more active reaction areas to store charges in PPy-based films as the stiff and ribbon-like CNC-COO-as permanent dopants improve the strength and stability of PPy-based films.Our demonstration provides a simple and practical way to deposit PPy based supercapacitors with high capacitance,fast charging,and excellent cycling stability.
基金Fundamental Research Funds for the Central Universities,China(No. 2232022D-13)Fundamental Research Funds of Shanghai Collaborative Innovation Center of High Performance Fibers and Composites (Province-M inistry Joint),China(No. X12812101/015)。
文摘To reduce the environmental pollution and meet the needs for wearable electronic devices, new requirements for electromagnetic interference(EMI) shielding materials include flexibility, biodegradability, and biocompatibility. Herein, we reported a polypyrrole-coated zein/epoxy(PPy/ZE) ultrafine fiber mat which was inherently biodegradable and skin-friendly. In addition, it could maintain its ultrafine fibrous structure after coating, which could provide the mat with mechanical compliance, high porosity, and a large specific area for high EMI shielding. With the assistance of the epoxide cross-linking, the breaking stresses of the PPy/ZE fiber mats could achieve 3.3 MPa and 1.4 MPa and the strains were 40.1% and 83.0% in dry and wet states, respectively, which met the needs of various wearable electronic devices. Along with the extension in the PPy treatment duration, more PPy was loaded on the fiber surfaces, which formed more integrated and conductive paths to generate increasing conductivities up to 401.76 S·m^(-1). Moreover, the EMI shielding performance was raised to 26.84 dB. The biobased mats provide a green and efficient choice for EMI shielding materials, which may be a promising strategy to address EMI problems in multiple fields.
文摘A nano sulfur-based composite cathode material featured by uniform core@shell-structured sulfur@polypyrrole nanoparticles sandwiched in three-dimensional graphene sheets conductive network(S@PPy/GS) is fabricated via a facile solution-based method. The S@PPy nanoparticles are synthesized by in situ chemical oxidative polymerization of pyrrole on the surface of sulfur particles,and then graphene sheets are covered outside the S@PPy nanoparticles,forming a three-dimensional conductive network. When evaluating the electrochemical performance of S@PPy/GS in a lithium–sulfur battery,it delivers large discharge capacity,excellent cycle stability,and good rate capability. The initial discharge capacity is up to 1040 m Ah/g at 0.1 C,the capacity can remain 537.8 m Ah/g at 0.2 C after 200 cycles,even at a higher rate of 1 C,the specific capacity still reaches 566.5 m Ah/g. The good electrochemical performance is attributed to the unique structure of S@PPy/GS,which can not only provide an excellent transport of lithium and electron ions within the electrodes,but also retard the shuttle effect of soluble lithium polysulfides effectively,thus plays a positive role in building better lithium-sulfur batteries.
基金Funded by Guizhou Provincial Natural Science Foundation(No.[2020]1Y030)Young Science and Technology Talents of Education Department of Guizhou Province(No.KY[2016]136)+1 种基金Doctoral Start-up Fund by Guizhou Normal University in 2014,The Guizhou Province Science and Technology Planning Project(No.[2016]1100)National Natural Science Foundation of China(No.21764004)。
文摘We investigated the removal of the organic dye rhodamine B in wastewater with recyclable AgBr/polypyrrole(PPy)nano-photocatalysts.With PPy as an active base for electron transfer,and hexadecyltrimethylammonium bromide(CTAB)as both the soft-templating agent and the bromine source,a series of AgBr/PPy nano-photocatalysts containing various proportions of silver were prepared in a convenient one-step synthesis procedure.The synthesized catalysts were characterized by TG analysis to reveal that,in comparison with pure PPy,the interaction between PPy and AgBr led to increased thermal stability.Chemical combination of PPy and AgBr was observed through XRD and XPS analyses.For the morphology study,the AgBr particles were found to be well dispersed in the PPy nanowire network from SEM results.In the photodegradation experiments,up to 92%rhodamine B was degraded by the AgBr/PPy catalysts in the period of 1 hour under 254 nm UV light.The catalysts could maintain 60%catalytic efficiency after 3 cycles in the recyclability test.
基金the financial support from the National Natural Science Foundation of China (No. 51674221)
文摘Lithium–sulfur batteries are promising next-generation energy storage devices beyond conventional lithium ion batteries. However, it suffers from rapid capacity fading and poor cyclic stability. Here we report a facile in situ sulfur deposition and chemical oxidative polymerization method for preparing acetylene black/sulfur@polypyrrole(AB/S@PPy) composite as a cathode material for lithium–sulfur batteries. It is demonstrated that PPy is covered uniformly onto the surface of the AB/S composite forming a core–shell structure. In the structure, AB in the matrix and PPy on the surface acts as a combined conductive framework to provide ions and electrons transport pathways, and to inhibit the dissolution or diffusion of polysulfide into the electrolyte. The as-designed AB/S@PPy composite exhibits excellent rate capability and cyclic stability. The initial discharge specific capacity is as high as 1179.4 m Ah/g, and remains at769.3 m Ah/g after 80 cycles at 0.2 C. Even at a high rate(0.5 C), a maximum discharge capacity of 811.1 m Ah/g is still achieved for the AB/S@PPy composite after activation, and the capacity retention is over62.5% after 200 cycles.
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(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.
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supported by Fundamental Research Program of Shanxi Province,China(202203021212245)the Science and Technology Achievement Transformation Guidance Special Program of Shanxi Province,China(202104021301052)the Patent Transformation Program of Shanxi Province,China(202306013).
文摘The removal of organic sulfur through catalytic hydrolysis is a significant area of research in the field of desulfurization.This review provides an overview of recent advancements in catalytic hydrolysis technology of organic sulfur,including the activity,stability,and atmosphere effects of hydrolysis catalysts.The emphasis is on strategies for enhancing hydrolysis activity and anti-oxygen poisoning property of catalysts.Surface modification,metal doping and nitrogen doping have been found to improve the activity of catalysts.Alkaline components modification is the most commonly used method,the formation of oxygen vacancies through metal doping and creation of nitrogen basic sites through nitrogen doping also contribute to the hydrolysis of organic sulfur.The strategies for anti-oxygen poisoning are discussed in a systematic manner.The structural regulation of catalysts is beneficial for the desorption and diffusion of hydrogen sulfide(H_(2)S),thereby effectively inhibiting its oxidation.Nitrogen doping and the addition of electronic promoters such as transition metals can protect active sites and decrease the number of active oxygen species.These methods have been proven to enhance the anti-poisoning performance of catalysts.Additionally,this article summarizes how different atmospheres affect the activity of hydrolysis catalysts.The objective of this review is to pave the way for the development of efficient,stable and widely used catalysts for organic sulfur hydrolysis.
基金financially supported by the National Nature Science Foundation of Jiangsu Province(BK20221259)。
文摘Transition metal sulfides have high theoretical capacities and are considered as potential anode materials for sodium-ion batteries.However,due to low inherent conductivity and significant volume expansion,the electrochemical performance is greatly limited.In this study,a nickel/manganese sulfide material(Ni_(0.96)S_(x)/MnS_(y)-NC)with adjustable sulfur vacancies and heterogeneous hollow spheres was prepared using a simple method.The introduction of a concentration-adjustable sulfur vacancy enables the generation of a heterogeneous interface between bimetallic sulfide and sulfur vacancies.This interface collectively creates an internal electric field,improving the mobility of electrons and ions,increasing the number of electrochemically active sites,and further optimizing the performance of Na~+storage.The direction of electron flow is confirmed by Density functional theory(DFT)calculations.The hollow nano-spherical material provides a buffer for expansion,facilitating rapid transfer kinetics.Our innovative discovery involves the interaction between the ether-based electrolyte and copper foil,leading to the formation of Cu_9S_5,which grafts the active material and copper current collector,reinforcing mechanical supporting.This results in a new heterostructure of Cu_9S_5 with Ni_(0.96)S_(x)/MnS_(y),contributing to the stabilization of structural integrity for long-cycle performance.Therefore,Ni_(0.96)S_(x)/MnS_(y)-NC exhibits excellent electrochemical properties following our modification route.Regarding stability performance,Ni0_(.96)S_(x)/MnS_(y)-NC demonstrates an average decay rate of 0.00944%after 10,000 cycles at an extremely high current density of 10000 mA g^(-1),A full cell with a high capacity of 304.2 mA h g^(-1)was also successfully assembled by using Na_(3)V_(2)(PO_(4))_(3)/C as the cathode.This study explores a novel strategy for interface/vacancy co-modification in the fabrication of high-performance sodium-ion batteries electrode.
基金supported by the National Natural Science Foundation of China(22379121)Shenzhen Foundation Research Program(JCYJ20220530112812028)+1 种基金Fundamental Research Funds for the Central Universities(G2022KY0606)Zhejiang Province Key Laboratory of Flexible Electronics Open Fund(2023FE005)。
文摘Expediting redox kinetics of sulfur species on conductive scaffolds with limited charge accessible surface is considered as an imperative approach to realize energy-dense and power-intensive lithium-sulfur(Li-S)batteries.In this work,the concept of concurrent hetero-/homo-geneous electrocatalysts is proposed to simultaneously mediate liquid-solid conversion of lithium polysulfides(LiPSs)and solid lithium disulfide/sulfide(Li_(2)S_(2)/Li_(2)S)propagation,the latter of which suffers from sluggish reduction kinetics due to buried conductive scaffold surface by extensive deposition of Li_(2)S_(2)/Li_(2)S.The selected model material to verify this concept is a two-in-one catalyst:carbon nanotube(CNT)scaffold supported iron-cobalt(Fe-Co)alloy nanoparticles and partially carbonized selenium(C-Se)component.The Fe-Co alloy serves as a heterogeneous electrocatalyst to seed Li_(2)S_(2)/Li_(2)S through sulphifilic active sites,while the C-Se sustainably releases soluble lithium polyselenides and functions as a homogeneous electrocatalyst to propagate Li_(2)S_(2)/Li_(2)S via solution pathways.Such bi-phasic mediation of the sulfur species benefits reduction kinetics of LiPS conversion,especially for the massive Li_(2)S_(2)/Li_(2)S growth scenario by affording an additional solution directed route in case of conductive surface being largely buried.This strategy endows the Li-S batteries with improved cycling stability(836 mA h g^(-1)after 180 cycles),rate capability(547 mA h g^(-1)at 4 C)and high sulfur loading superiority(2.96 mA h cm^(-2)at 2.4 mg cm^(-2)).This work hopes to enlighten the employment of bi-phasic electrocatalysts to dictate liquid-solid transformation of intermediates for conversion chemistry batteries.
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.
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supported by the Fundamental Research Funds for the Central Universities(222201817001)Shanghai Sailing Program(21YF140800).
文摘The self-made MnFeO_(x) catalysts doped with cerium and samarium were prepared by impregnation method for low-temperature selective catalytic reduction(SCR)by NH3.In this work,the surface properties of the series of MnFe-based catalysts were studied.The results indicate Sm-modified catalyst have superior low-temperature SCR activity;NO_(x) conversion maintained at nearby to 100%at 90℃ to 240℃.In addition,The N_(2) selectivity of Sm doping remains above 80%in the range of 60℃ to 150℃.In SO_(2) poisoning test,the NO_(x) conversion can be remained>90%after 10 h of reaction.The XPS,NH_(3)-TPD and H_(2)-TPR results show the catalyst with Sm doping enhances the acid sites and oxidation catalytic sites of mixed oxides serves for improving oxygen vacancies and transfer electrons.In situ diffuse reflaxions infrared Fourier transformations spectroscopy(DRIFTS)results show that NO_(x) is more easily adsorbed on the surface after Sm doping,which provided favorable conditions for the NH_(3)-SCR reaction to proceed.The reaction at the catalyst surface will follow the L-H reaction mechanism by transient reaction test.
基金supported by the National Natural Science Foundation of China(42003059)State Key Laboratory of Coal Mining and Clean Utilization(2021-CMCU-KF009)the Science Foundation of China University of Petroleum,Beijing(No.2462023YJRC003)。
文摘Refinery sour water primarily originates from the tops of towers in various units and coker condensate,and cannot be discharged directly to a wastewater treatment plant due to high levels of chemical oxygen demand(COD)and organic sulfur contents.Even after the recovery of H_(2)S from the sour water by the stripping process,the effluent still contains a high concentration of dissolved organic sulfur(DOS),which can have a huge bad influence.While chemical composition of dissolved organic matter(DOM)in refinery wastewater has been extensively studied,the investigation of recalcitrant DOS from sour waters remains unclear.In the present study,chemical composition of sour water DOMs(especially DOS)was investigated using fluorescence spectroscopy(excitation-emission matrix,EEM)and mass spectrometry,including gas chromatography-mass spectrometry(GC-MS)and high-resolution Orbitrap MS.The GC-MS and EEM results showed that volatile and low-aromaticity compounds were effectively removed during the stripping process,while compounds with high hydrophilicity and humification degree were found to be more recalcitrant.The Orbitrap MS results showed that weak-polar oxygenated sulfur compounds were easier to be removed than oxygenated compounds.However,the effluent still contained significant amounts of sulfur-containing compounds with multiple sulfur atoms,particularly in the form of highly unsaturated and aromatic compounds.The Orbitrap MS/MS results of CHOS-containing compounds from the effluent indicate that the sulfur atoms may exist as sulfonates,disulfide bonds,thioethers.Understanding the composition and structure of sour water DOS is crucial for the development of effective treatment processes that can target polysulfide compounds and minimize their impact on the environment.
基金supported by the Natural Science Foundation of the Heilongjiang Province of China(Grant No.LH2021C023).
文摘Soybean is a crucial crop utilized for both food and oil production,with balanced crop nutrition being a key determinant of soybean yield throughout its growth cycle.Sulfur,an essential nutrient for crop growth,substantially impacts soybean yield.In this study,two soybean cultivars,Laidou 2 and Hefeng 55,were used to study the changes in nitrogen,phosphorus,potassium,and sulfur contents in soybean plants at different growth stages.Additionally,the effects of dry matter accumulation under five different sulfur levels were examined.The results showed that the sulfur levels had varying effects on the nitrogen,phosphorus,potassium,and sulfur contents and accumulation in different parts of the soybean plants.There were marked differences in the accumulation and distribution of dry matter in different parts of the soybean plant.Soybean dry matter weight shows the best overall performance under the S80 treatment.With increasing sulfur nutrition,the nitrogen,phosphorus,potassium,and sulfur contents in various plant parts exhibited an unimodal trend,reaching maximum values when the sulfur content was 80 mg/L.This study elucidates the dynamic changes in nutrient elements in soybeans under different sulfur levels and is important in guiding the rational application of sulfur fertilizers in agricultural production.