Sulfamethoxazole(SMX)contamination in farmland disrupts soil micro-ecological functions,posing a risk to soil health and productivity.Sulfidated zero-valent iron(SZVI),a promising green material known for its good rea...Sulfamethoxazole(SMX)contamination in farmland disrupts soil micro-ecological functions,posing a risk to soil health and productivity.Sulfidated zero-valent iron(SZVI),a promising green material known for its good reactivity,had been used for soil remediation.However,existing studies often overlooked the effects of particle size and sulfur content on the long-term performance of SZVI and its impact on soil micro-ecological safety.This study employed polysulfide-modified nano,micro-nano,and micron-sized SZVI to investigate how particle size and sulfur content influenced the reactivity and durability,as well as the iron oxide forms and microbial community of soil during the SMX remediation.The results demonstrated that micro-nano sized SZVI(nm-SZVI)exhibited prolonged reactivity,achieving 83.12%-99.91%SMX removal over 30 days and maintaining higher levels of soil amorphous and reactive ferrous iron.Although sulfidation improved reactivity,excessive sulfur content reduced removal efficiency and accelerated the conversion to soil crystalline iron forms.Compared to nanoparticles,nm-SZVI fostered microbial diversity and balanced functional bacteria for electron transfer,organic matter utilization,and nutrient cycling.However,the elevated sulfur content in SZVI inhibited the stability of the microbial network.Finally,it was found that SMX underwent isoxazole reduction cleavage and oxidative removal pathways,reducing ecological toxicity.This study provided a new insight into the rational design of SZVI to achieve long-term pollutant removal and ensuring the health and stability of the microbial community by regulating particle size and sulfur content in soil remediation.展开更多
The MXenes,a new class of two-dimensional layered materials,have found extensive applications in water treatment for its excellent thermal stability,electrical conductivity,and excellent adsorption ability.Sulfidized ...The MXenes,a new class of two-dimensional layered materials,have found extensive applications in water treatment for its excellent thermal stability,electrical conductivity,and excellent adsorption ability.Sulfidized nano zero-valent iron(S-nZVI)is a good reducing agent,however,the practical application of S-nZVI is currently restricted due to the tendency of nano materials to agglomerate.Herein,MXenes use as a support and in situ loading S-nZVI on it to prepare a new material(S-nZVI/Ti_(3)C_(2)T_(x)),and applied it to U(VI)removal in water treatment.The microscopic characterization proves that S-nZVI on Ti_(3)C_(2)T_(x) has good dispersion and effectively alleviates agglomeration.Batch experiments shown that SnZVI/Ti_(3)C_(2)T_(x) has a very good effect on U(VI)removal,and themaximumadsorption capacity reaches 674.4mg/g under the aerobic condition at pH=6.0.The pseudo-second-order kinetic model and the Langmuir isotherm model were found to be more appropriate for describing the adsorption behavior.This indicates that the removal process is a single molecular layer chemisorption.Moreover,the S-nZVI/Ti_(3)C_(2)T_(x) maintained a removal efficiency of over 85%for U(VI)even after being reused five times,demonstrating its excellent reusability.It is worth noting that the material can remove 79.8%of 50 mg/L of U(VI)in simulated seawater,indicating that S-nZVI/Ti_(3)C_(2)T_(x) possessed an excellent uranium extraction performance from seawater.Experimental results and XPS analysis showed that U(VI)was removed by adsorption,reduction and co-precipitation.Moreover,S-nZVI/Ti_(3)C_(2)T_(x) was a lowtoxicitymaterial to Hyriopsis cumingii.Therefore,S-nZVI/Ti_(3)C_(2)T_(x) was expected to be a candidate as adsorbent with great potential in removal of uranium from wastewater and seawater.展开更多
Massive waste aluminum scraps produced from the spent aluminum products have high electron capacity and can be recycled as an attractive alternative to materials based on zerovalent iron(Fe^(0))for the removal of oxid...Massive waste aluminum scraps produced from the spent aluminum products have high electron capacity and can be recycled as an attractive alternative to materials based on zerovalent iron(Fe^(0))for the removal of oxidative contaminants from wastewater.This study thus proposed an approach to fabricate micron-sized sulfidated zero-valent iron-aluminum particles(S-Al^(0)@Fe^(0))with high reactivity,electron selectivity and capacity using recycled waste aluminum scraps.S-Al^(0)@Fe^(0)with a three-layer structure contained zero-valent aluminum(Al^(0))core,Fe^(0) middle layer and iron sulfide(FeS)shell.The rates of chromate(Cr(Ⅵ))removal by S-Al^(0)@Fe^(0)at pH 5.0-9.0 were 1.6-5.9 times greater than that by sulfidated zero-valent iron(S-Fe^(0)).The Cr(Ⅵ)removal capacity of S-Al^(0)@Fe^(0)was 8.2-,11.3-and 46.9-fold greater than those of S-Fe0,zero-valent iron-aluminum(Al^(0)-Fe^(0))and Fe^(0),respectively.The chemical cost of S-Al^(0)@Fe^(0) for the equivalent Cr(Ⅵ)removal was 78.5%lower than that of S-Fe^(0).Negligible release of soluble aluminum during the Cr(Ⅵ)removal was observed.The significant enhancement in the reactivity and capacity of S-Al^(0)@Fe^(0)was partially ascribed to the higher reactivity and electron density of the Al0core than Fe^(0).More importantly,S-Al^(0)@Fe^(0) served as an electric cell to harness the persistent and selective electron transfer from the Al^(0)-Fe^(0) core to Cr(Ⅵ)at the surface via coupling Fe^(0)-Fe^(2+)-Fe^(3+)redox cycles,resulting in a higher electron utilization efficiency.Therefore,S-Al^(0)@Fe^(0) fabricated using recycled waste aluminum scraps can be a cost-effective and environmentally-friendly alternative to S-Fe^(0) for the enhanced removal of oxidative contaminants in industrial wastewater.展开更多
After adding either organic or inorganic ligands,sulfidated nano-zero-valent iron(Sn ZVI)was used for aerobic degradation of phenol,and the effect of the ligand species on oxidation performance was investigated.We fou...After adding either organic or inorganic ligands,sulfidated nano-zero-valent iron(Sn ZVI)was used for aerobic degradation of phenol,and the effect of the ligand species on oxidation performance was investigated.We found that Sn ZVI hardly degraded phenol in the absence of ligand addition.Ligands initiated and promoted the degradation of pollutants by Sn ZVI.The data herein show that a characteristic inorganic ligand,tripolyphosphate(TPP),is more effective in enhancing oxidation than a characteristic organic ligand oxalate.In addition to the scavenging of reactive oxidants by the organic ligand,more ferrous ion(Fe(Ⅱ))dissolution from Sn ZVI in the TPP system is another cause for the superior enhancement by the inorganic ligand.In the oxalate system,as the sulfur content of Sn ZVI increased,the oxidation efficiency increased because Fe S shell promoted the transfer of electrons to produce more reactive oxygen species(ROS).In TPP system,the effect of sulfur content on oxidation performance is more complex.The Sn ZVI with low sulfur content showed poor oxidation performance compared with that of n ZVI.Further experiments proved that sulfidation might weaken the complexation of TPP with surface bound Fe,which would slow down the ionic Fe(II)dissolution rate.Therefore,sulfidation has the dual effects of enhancing electron transfer and inhibiting the complexation of inorganic ligands.In addition,the mechanisms of ROS generation in different ligand systems were investigated herein.Results showed that the critical ROS in both the oxalate and TPP systems are hydroxyl radicals,and that they are produced via one-electron activation of O_(2).展开更多
Sulfidation of zero-valent iron(ZVI)has attracted broad attention in recent years for improving the sequestration of contaminants from water.However,sulfidated ZVI(S-ZVI)is mostly synthesized in the aqueous phase,whic...Sulfidation of zero-valent iron(ZVI)has attracted broad attention in recent years for improving the sequestration of contaminants from water.However,sulfidated ZVI(S-ZVI)is mostly synthesized in the aqueous phase,which usually causes the formation of a thick iron oxide layer on the ZVI surface and hinders the efficient electron transfer to the contaminants.In this study,an alcohothermal strategy was employed for S-ZVI synthesis by the one-step reaction of iron powder with elemental sulfur.It is found that ferrous sulfide(FeS)with high purity and fine crystallization was formed on the ZVI surface,which is extremely favorable for electron transfer.Cr(Ⅵ)removal experiments confirm that the rate constant of SZVI synthesized by the alcohothermal method was 267.1-and 5.4-fold higher than those of un-sulfidated ZVI and aqueous-phase synthesized S-ZVI,respectively.Systematic characterizations proved that Cr(Ⅵ)was reduced and co-precipitated on S-ZVI in the form of a Fe(Ⅲ)/Cr(Ⅲ)/Cr(Ⅵ)composite,suggesting its environmental benignancy.展开更多
It is difficult to recover chrysocolla from sulfidation flotation which is closely related to the mineral surface composition.In this study,the effects of fluoride roasting on the surface composition of chrysocolla we...It is difficult to recover chrysocolla from sulfidation flotation which is closely related to the mineral surface composition.In this study,the effects of fluoride roasting on the surface composition of chrysocolla were investigated,its impact on sulfidation flotation was explored,and the mechanisms involved in both fluoride roasting and sulfidation flotation were discussed.With CaF_(2)as the roasting reagent,Na_(2)S·9H_(2)O as the sulfidation reagent,and sodium butyl xanthate(NaBX)as the collector,the results of the flotation experiments showed that fluoride roasting improved the floatability of chrysocolla,and the recovery rate increased from 16.87%to 82.74%.X-ray diffraction analysis revealed that after fluoride roasting,approximately all the Cu on the chrysocolla surface was exposed in the form of CuO,which could provide a basis for subsequent sulfidation flotation.The microscopy and elemental analyses revealed that large quantities of"pagoda-like"grains were observed on the sulfidation surface of the fluoride-roasted chrysocolla,indicating high crystallinity particles of copper sulfide.This suggests that the effect of sulfide formation on the chrysocolla surface was more pronounced.X-ray photoelectron spectroscopy revealed that fluoride roasting increased the relative contents of sulfur and copper on the surface and that both the Cu~+and polysulfide fractions on the surface of the minerals increased.This enhances the effect of sulfidation,which is conducive to flotation recovery.Therefore,fluoride roasting improved the effect of copper species transformation and sulfidation on the surface of chysocolla,promoted the adsorption of collectors,and improved the recovery of chrysocolla from sulfidation flotation.展开更多
A series of leaching and electrochemical experiments were conducted to elucidate the critical role of hydrogen sulfide(H_(2)S)in copper-driven reduction of chalcopyrite.Results demonstrate that in the absence of H_(2)...A series of leaching and electrochemical experiments were conducted to elucidate the critical role of hydrogen sulfide(H_(2)S)in copper-driven reduction of chalcopyrite.Results demonstrate that in the absence of H_(2)S,metallic copper converts chalcopyrite into bornite(Cu_(5)FeS_(4)).However,the introduction of H_(2)S promotes the formation of chalcocite(Cu_(2)S)by altering the oxidation pathway of copper.Electrochemical analysis demonstrates that the presence of H₂S significantly reduces the corrosion potential of copper from 0.251 to−0.223 V(vs SHE),reaching the threshold necessary for the formation of Cu_(2)S.Nevertheless,excessive H_(2)S triggers sulfate reduction via the reaction of 8Cu+H_(2)SO_(4)+3H_(2)S=4Cu_(2)S+4H_(2)O(ΔG=−519.429 kJ/mol at 50℃),leading to inefficient copper utilization.展开更多
CM chondrites contain valuable insights into the formation and evolution of the solar nebula,as well as the secondary aqueous alteration processes that affected their parent bodies.Our study focuses on primary and sec...CM chondrites contain valuable insights into the formation and evolution of the solar nebula,as well as the secondary aqueous alteration processes that affected their parent bodies.Our study focuses on primary and secondary sulfides within the Aguas Zarcas(CM2)chondrite,investigating their formation mechanisms based on their morphology,textures,and compositions.Moreover,we infer the formation temperatures of the sulfides from 230 to 500℃ for primary and from 100 to 135℃ for secondary.We select representative grains and conduct Fe isotope measurements on them.The primary sulfides with δ^(56/54)Fe ranging from -2.44‰ to +0.69‰are associated with sulfidesilicate melt segregation,while secondary sulfides with δ^(56/54)Fe values between -1.83‰ and -0.14‰ are linked to aqueous alteration.Overall,the Ni content of the grains is positively correlated with δ^(56/54)Fe.It might be related to the changes in crystal structure and chemical bond lengths due to the increase in nickel content.Fe isotopes provide a new perspective on sulfide formation and the evolution of a carbonaceous chondrite parent body.展开更多
To address the poor mechanical performance and improve the tribological properties of self-lubricating polyphenylene sulfide/irradiation treated polytetrafluoroethylene(PPS/i-PTFE)blends,different aspect ratio carbon ...To address the poor mechanical performance and improve the tribological properties of self-lubricating polyphenylene sulfide/irradiation treated polytetrafluoroethylene(PPS/i-PTFE)blends,different aspect ratio carbon fibers(i.e.,PSCF:50,SCF:about 429)were introduced as reinforcement fillers.The results showed that the hybriding of PSCF and SCF at certain mass ratios exhibited simultaneous enhancement of mechanical and tribological performance for PPS/i-PTFE blend through the construction of synergistic lubrication and mechanical interlocking network.Specifically,the flexural strength and modulus of PPS/i-PTFE were increased by 125.6% and 389.3%,the friction coefficient and specific wear rate were decreased by 13.9% and 95%,respectively.It was worth noting that PPS composites possessed excellent integrated performance which were able to withstand sliding action under high PV(≥10 MPa·m/s)conditions,as assessed by a customized pin-on-disc tester.This work demonstrated that the formation of intact lubricating film combined with the enhanced thermal and mechanical properties were favorable for improving the tribological properties of PPS-based composites,which makes them suitable for advanced engineering applications.展开更多
Micro silicon(mSi)is a promising anode candidate for all-solid-state batteries due to its high specific capacity,low side reactions,and high tap density.However,silicon suffers from its poor electronic and ionic condu...Micro silicon(mSi)is a promising anode candidate for all-solid-state batteries due to its high specific capacity,low side reactions,and high tap density.However,silicon suffers from its poor electronic and ionic conductivity,which is particularly severe on a micro scale and in solid-state systems,leading to increased polarization and inferior electrochemical performance.Doping can broaden the transmission pathways and reduce the diffusion energy barrier for electrons and lithium ions.However,achieving effective,uniform doping in mSi is challenging due to its longer diffusion paths and higher energy barriers.Therefore,current doping research is primarily limited to nanosilicon.In this study,we successfully used a Joule-heating activated staged thermal treatment to achieve full-depth doping of germanium(Ge)in the mSi substrate.The Joule-heating process activated the mSi substrate,resulting in abundant vacancy defects that reduced the diffusion barrier of Ge into the silicon lattice and facilitated full-depth Ge doping.Surprisingly,the resulting Si-Ge anode exhibited significantly enhanced electrical conductivity(70 times).Meanwhile,the improved Li-ion conductivity in mSi and the reduced Young’s modulus enhance the electrode reaction kinetics and integrity after cycling.Ge-doped silicon anodes demonstrate excellent electrochemical performance when applied in sulfide solid-state half-cells and full-cells.This work provides substantial insights into the rational structural design of mSi alloyed anode materials,paving the way for the development of high-performance solid-state Li-ion batteries.展开更多
Sulfide solid electrolytes are considered promising candidates for all-solid-state lithium batteries(ASSLBs)because of their high ionic conductivity and favorable mechanical properties.However,the uncontrolled growth ...Sulfide solid electrolytes are considered promising candidates for all-solid-state lithium batteries(ASSLBs)because of their high ionic conductivity and favorable mechanical properties.However,the uncontrolled growth of lithium dendrites at the lithium metal-electrolytes interface remains a major obstacle to their practical application.In this work,we introduced a scalable three-dimensional(3D)Li-B skeleton structure designed to suppress dendrite formation.The alloy anode demonstrates a lower Young's modulus,which helps alleviate the accumulation of localized stresses at the interface.Additionally,the 3D alloy anode provided a uniform potential distribution,which promoted homogeneous lithium deposition.Benefiting from these structural advantages,symmetric cells with the Li-B alloy achieved a high critical current density of 2.8 mA cm^(-2).Notably,Li-B‖LPSCI‖LVO-NCM ASSLBs exhibited long-term cycling stability,retaining 97.8%of their capacity after 1500 cycles at 2 C.Furthermore,ASSLBs incorporating the Li-B alloy showed cycling stability comparable with Li-In-based cells,while delivering a higher energy density.Overall,this work presents a practical strategy that may accelerate the commercialization of sulfide-based ASSLBs.展开更多
High-nickel cathode,LiNi0.8Co0.1Mn0.1O_(2)(NCM811),and sulfide-solid electrolyte are a promising combination for all-solid-state lithium batteries(ASSLBs).However,this combination faces the issue of interfacial instab...High-nickel cathode,LiNi0.8Co0.1Mn0.1O_(2)(NCM811),and sulfide-solid electrolyte are a promising combination for all-solid-state lithium batteries(ASSLBs).However,this combination faces the issue of interfacial instability between the cathode and electrolyte.Given the surface alkalinity of NCM811,we propose a strategy to construct a solid-polymer-electrolyte(SPE)interphase on NCM811 surface by leveraging the surface alkaline residues to nucleophilically initiate the in-situ ring-opening polymerization of cyclic organic molecules.As a proof-of-concept,this study demonstrates that the ring-opening copolymerization of 1,3-dioxolane and maleic anhydride produces a homogeneous,compact,and conformal SPE layer on NCM811 surface to prevent the cathode from contact and reaction with Li6PS5Cl solid-state electrolyte.Consequently,the SPE-modified-NCM811 in ASSLBs exhibits high capacities of 193.5 mA h g^(-1) at 0.2 C,160.9 mA h g^(-1) at 2.0 C and 112.3 mA h g^(-1) at 10 C,and particularly,excellent long-term cycling stabilities over 11000 cycles with a 71.95%capacity retention at 10 C at 25℃,as well as a remained capacity of 117.9 mA h g^(-1) after 8000 cycles at 30 C at 60℃,showing a great application prospect.This study provides a new route for creating electrochemically and structurally stable solid-solid interfaces for ASSLBs.展开更多
Microwave roasting self-leaching is an innovative method for recovering gold from high-sulfur refractory gold concentrates,without using deadly toxic cyanide reagents.However,the mechanism of gold self-leaching,which ...Microwave roasting self-leaching is an innovative method for recovering gold from high-sulfur refractory gold concentrates,without using deadly toxic cyanide reagents.However,the mechanism of gold self-leaching,which relies on lixiviants prepared using volatilized sulfur obtained from roasting,has not been fully elucidated.This study employs the response surface methodology to optimize processing parameters,resulting in an increased gold extraction rate of 96.18%.Analytical factorization and the Tafel curve indicate that CuSO_(4) and NH_(3)·H_(2)O significantly influence the self-leaching process.Furthermore,X-ray photoelectron spectroscopy(XPS)analysis reveals that S^(2−),S_(2)^(2−),polysulfides(S_(n)^(2−)),and thiosulfate(S_(2)O_(3)^(2−))are involved in the gold leaching reaction,with S^(2−),S_(2)^(2−),and S_(n)^(2−) serving as primary ligands for gold complexation.The role of S_(2)O_(3)^(2−) in the early stages of the gold-leaching reaction is also noteworthy.The copper–ammonia complex catalyzes the self-leaching gold reaction;however,an improper addition ratio can lead to copper-sulfur compound precipitates,reducing the extraction rate.展开更多
In this study,the influences of sulfidation on zero-valent iron(ZVI)performance toward As(Ⅴ)immobilization in soil were systemically investigated.It was found that,compared to unamended ZVI,sulfidated ZVI(S-ZVI)is mo...In this study,the influences of sulfidation on zero-valent iron(ZVI)performance toward As(Ⅴ)immobilization in soil were systemically investigated.It was found that,compared to unamended ZVI,sulfidated ZVI(S-ZVI)is more favorable to immobilize As(Ⅴ)in soil and promote the conversion of water soluble As to less mobile Fe-Mn bound As.Specifically,under the optimal S/Fe molar ratio of 0.05,almost all of the leached As could be sequestrated by>0.5 wt.%S-ZVI within 3 h.Although the presence of HA could decrease the desorption of As from soil,HA inhibited the reactivity of S-ZVI to a greater extent.Column experiments further proved the feasibility of applying S-ZVI on soil As(Ⅴ)immobilization.More importantly,to achieve a good As retention performance,S-ZVI should be fully mixed with soil or located on the downstream side of As migration.The test simulating the flooding conditions in rice culture revealed there was also a good long-term stability of soil As(Ⅴ)after S-ZVI remediation,where only 0.7%of As was desorbed after 30 days of incubation.Magnetic separation was employed to separate the immobilized As(Ⅴ)from soil after S-ZVI amendment,where the separation efficiency was found to be dependent of the iron dosage,liquid to soil ratio,and reaction time.Toxicity characteristic leaching procedure(TCLP)tests revealed that the leachability of As from soil was significantly reduced after the S-ZVI amendment and magnetic separation treatment.All these findings provided some insights into the remediation of As(Ⅴ)-polluted soil by ZVI.展开更多
Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,how...Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,however,constrain their delicate constructions.Herein,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix.This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in M_(x)S_(y)/carbon composites(M-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial polarization.Such“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time.Consequently,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric response.Harnessing defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.展开更多
The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular an...The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular and cellular mechanisms by which quinolinic acid contributes to Huntington's disease pathology remain unknown. In this study, we established in vitro and in vivo models of Huntington's disease by administering quinolinic acid to the PC12 neuronal cell line and the striatum of mice, respectively. We observed a decrease in the levels of hydrogen sulfide in both PC12 cells and mouse serum, which was accompanied by down-regulation of cystathionine β-synthase, an enzyme responsible for hydrogen sulfide production. However, treatment with NaHS(a hydrogen sulfide donor) increased hydrogen sulfide levels in the neurons and in mouse serum, as well as cystathionine β-synthase expression in the neurons and the mouse striatum, while also improving oxidative imbalance and mitochondrial dysfunction in PC12 cells and the mouse striatum. These beneficial effects correlated with upregulation of nuclear factor erythroid 2-related factor 2 expression. Finally, treatment with the nuclear factor erythroid 2-related factor 2inhibitor ML385 reversed the beneficial impact of exogenous hydrogen sulfide on quinolinic acid-induced oxidative stress. Taken together, our findings show that hydrogen sulfide reduces oxidative stress in Huntington's disease by activating nuclear factor erythroid 2-related factor 2,suggesting that hydrogen sulfide is a novel neuroprotective drug candidate for treating patients with Huntington's disease.展开更多
The use of visible-light responsive photocatalysts for removing heavy metal ions in wastewater has received great attention.However,the development of photocatalysts with high activity and recyclability remains a huge...The use of visible-light responsive photocatalysts for removing heavy metal ions in wastewater has received great attention.However,the development of photocatalysts with high activity and recyclability remains a huge challenge.Herein,a recyclable carbon fiber cloth-supported porous CdS nanorod photocatalyst was fabricated by a two-step hydrothermal treatment using AgVO_(3) nanowires as templates.The results indicated that under visible-light illumination,the carbon cloth-supported porous CdS nanorods showed improved photocatalytic activity for the reduction of Cr(Ⅵ),with an apparent rate constant exceeding that of carbon cloth-supported CdS nanospheres by a factor of 1.65 times.Moreover,the carbon cloth-supported porous CdS nanorods can be easily separated and be reused.This brings a new perspective for developing photocatalysts with high efficiency and recyclability for wastewater treatment.展开更多
Reasonable manipulation of component and microstructure is considered as a potential route to realize high-performance microwave absorber.In this paper,micro-sized hexapod-like CuS/Cu_(9)S_(5) composites were synthesi...Reasonable manipulation of component and microstructure is considered as a potential route to realize high-performance microwave absorber.In this paper,micro-sized hexapod-like CuS/Cu_(9)S_(5) composites were synthesized via a facile approach involving the solvothermal method and subsequent sulfuration treatment.The resultant CuS/Cu_(9)S_(5) exhibited superb microwave absorbing capacity with a minimum reflection loss(RLmin)of-59.38 dB at 2.7 mm.The maximum effective absorption bandwidth(EABmax)was 7.44 GHz(10.56-18 GHz)when the thickness was reduced to 2.3 mm.The outstanding microwave absorbing ability of CuS/Cu_(9)S_(5) composites is mainly related to its unique hexapod shape and the formation of heterogeneous interfaces.The unique hexapod shape significantly promotes the multi-reflection of the incident electromagnetic wave(EMW)increasing the attenuation path of EMWs in the material.Hetero-geneous interfaces between CuS/Cu_(9)S_(5) enable powerful interface polarization,contributing to the atten-uation of EMWs propagating in the medium.In addition,the EMW absorption performance of CuS/Cu_(9)S_(5) composites is also inseparable from the conduction loss.This study provides a strong reference for the research of EMW absorbent materials based on transition metal sulfides.展开更多
This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature&l...This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature<300℃.Sulfur vapor is a highly flammable gas,which then auto-ignites to produce a flame.This behavior suggests that an O_(2)-S gas-gas reaction mechanism may contribute to all-solid-state battery thermal runaway.To improve all-solid-state battery safety,current work focuses on eliminating the O_(2)source by changing the cathode active material.The conclusion of this study suggests that all-solidstate battery safety can also be realized by the development of solid-state electrolytes with less susceptibility to sulfur volatilization.展开更多
Mg-based hydrogen storage materials have attracted much attention due to their high hydrogen content,abundant resources,and environmental friendliness.However,the high dehydrogenation temperature,slow kinetics and poo...Mg-based hydrogen storage materials have attracted much attention due to their high hydrogen content,abundant resources,and environmental friendliness.However,the high dehydrogenation temperature,slow kinetics and poor cycling stability are limiting its practical application.This work demonstrates the improved dehydrogenation kinetics and cycling stability of MgH_(2) modified by a hybrid of metallic Ni and layered MoS_(2)(denoted as“Ni-MoS_(2)”)introduced by ball milling,with Ni as the catalyst for MgH_(2) and MoS_(2) as the support for both Ni and MgH_(2).The onset dehydrogenation temperature of MgH_(2) is reduced to 198℃,and the rehydrogenation begins at a low temperature of 50℃.The MgH_(2)+10 wt%Ni-MoS_(2) composite has a fast dehydrogenation kinetics and can release 6.1 wt% hydrogen in 10 min at a constant temperature of 300℃,with the dehydrogenation activation energy significantly reduced from 151 to 85 kJ mol^(-1).During the cycling,the reversible capacity of the composite first exhibits a gradual increase for the initial 22 cycles and then maintains at 6.1 wt% from the 23th cycle to the 50th cycle.The Ni/MoS_(2) addition does not change the overall thermodynamic properties of MgH_(2) but can weaken the Mg-H bonds in the local regions as evident by theoretical calculation.Microstructure studies reveal that the metallic Ni will react with MgH_(2) to form Mg_(2)NiH_(0.3),which can act as a hydrogen pump,while the layered MoS_(2) serves as a support for the well dispersion of MgH_(2) and Ni.It is believed that the synergy of Mg_(2)NiH_(0.3) and layered MoS_(2) contributes to the significantly enhanced hydrogen storage of MgH_(2).This work provides a promising and simple strategy for enhancing the Mg-based hydrogen storage materials by combination of transition metals and layered materials introduced via simple ball milling.展开更多
基金supported by the National Natural Science Foundation of China(No.22478226)Shandong Provincial Natural Science Foundation(Nos.ZR2023JQ022 and ZR2024QE165)+1 种基金the Postdoctoral Fellowship Program of CPSF(No.GZC20240917)Taishan Scholars Project of Shandong Province(No.tstp20230604)。
文摘Sulfamethoxazole(SMX)contamination in farmland disrupts soil micro-ecological functions,posing a risk to soil health and productivity.Sulfidated zero-valent iron(SZVI),a promising green material known for its good reactivity,had been used for soil remediation.However,existing studies often overlooked the effects of particle size and sulfur content on the long-term performance of SZVI and its impact on soil micro-ecological safety.This study employed polysulfide-modified nano,micro-nano,and micron-sized SZVI to investigate how particle size and sulfur content influenced the reactivity and durability,as well as the iron oxide forms and microbial community of soil during the SMX remediation.The results demonstrated that micro-nano sized SZVI(nm-SZVI)exhibited prolonged reactivity,achieving 83.12%-99.91%SMX removal over 30 days and maintaining higher levels of soil amorphous and reactive ferrous iron.Although sulfidation improved reactivity,excessive sulfur content reduced removal efficiency and accelerated the conversion to soil crystalline iron forms.Compared to nanoparticles,nm-SZVI fostered microbial diversity and balanced functional bacteria for electron transfer,organic matter utilization,and nutrient cycling.However,the elevated sulfur content in SZVI inhibited the stability of the microbial network.Finally,it was found that SMX underwent isoxazole reduction cleavage and oxidative removal pathways,reducing ecological toxicity.This study provided a new insight into the rational design of SZVI to achieve long-term pollutant removal and ensuring the health and stability of the microbial community by regulating particle size and sulfur content in soil remediation.
基金supported by the National Natural Science Foundation of China(No.42277063)the Postdoctoral Research Foundation of China(No.2021M702886)+1 种基金the Leading Innovative Talents cultivation Project of Changzhou City(No.CQ20230096)the Research Initiation Project of Changzhou University.
文摘The MXenes,a new class of two-dimensional layered materials,have found extensive applications in water treatment for its excellent thermal stability,electrical conductivity,and excellent adsorption ability.Sulfidized nano zero-valent iron(S-nZVI)is a good reducing agent,however,the practical application of S-nZVI is currently restricted due to the tendency of nano materials to agglomerate.Herein,MXenes use as a support and in situ loading S-nZVI on it to prepare a new material(S-nZVI/Ti_(3)C_(2)T_(x)),and applied it to U(VI)removal in water treatment.The microscopic characterization proves that S-nZVI on Ti_(3)C_(2)T_(x) has good dispersion and effectively alleviates agglomeration.Batch experiments shown that SnZVI/Ti_(3)C_(2)T_(x) has a very good effect on U(VI)removal,and themaximumadsorption capacity reaches 674.4mg/g under the aerobic condition at pH=6.0.The pseudo-second-order kinetic model and the Langmuir isotherm model were found to be more appropriate for describing the adsorption behavior.This indicates that the removal process is a single molecular layer chemisorption.Moreover,the S-nZVI/Ti_(3)C_(2)T_(x) maintained a removal efficiency of over 85%for U(VI)even after being reused five times,demonstrating its excellent reusability.It is worth noting that the material can remove 79.8%of 50 mg/L of U(VI)in simulated seawater,indicating that S-nZVI/Ti_(3)C_(2)T_(x) possessed an excellent uranium extraction performance from seawater.Experimental results and XPS analysis showed that U(VI)was removed by adsorption,reduction and co-precipitation.Moreover,S-nZVI/Ti_(3)C_(2)T_(x) was a lowtoxicitymaterial to Hyriopsis cumingii.Therefore,S-nZVI/Ti_(3)C_(2)T_(x) was expected to be a candidate as adsorbent with great potential in removal of uranium from wastewater and seawater.
基金supported by the National Natural Science Foundation of China(No.42177358)the Natural Science Foundation of Guangdong Province(No.2023A1515011232)。
文摘Massive waste aluminum scraps produced from the spent aluminum products have high electron capacity and can be recycled as an attractive alternative to materials based on zerovalent iron(Fe^(0))for the removal of oxidative contaminants from wastewater.This study thus proposed an approach to fabricate micron-sized sulfidated zero-valent iron-aluminum particles(S-Al^(0)@Fe^(0))with high reactivity,electron selectivity and capacity using recycled waste aluminum scraps.S-Al^(0)@Fe^(0)with a three-layer structure contained zero-valent aluminum(Al^(0))core,Fe^(0) middle layer and iron sulfide(FeS)shell.The rates of chromate(Cr(Ⅵ))removal by S-Al^(0)@Fe^(0)at pH 5.0-9.0 were 1.6-5.9 times greater than that by sulfidated zero-valent iron(S-Fe^(0)).The Cr(Ⅵ)removal capacity of S-Al^(0)@Fe^(0)was 8.2-,11.3-and 46.9-fold greater than those of S-Fe0,zero-valent iron-aluminum(Al^(0)-Fe^(0))and Fe^(0),respectively.The chemical cost of S-Al^(0)@Fe^(0) for the equivalent Cr(Ⅵ)removal was 78.5%lower than that of S-Fe^(0).Negligible release of soluble aluminum during the Cr(Ⅵ)removal was observed.The significant enhancement in the reactivity and capacity of S-Al^(0)@Fe^(0)was partially ascribed to the higher reactivity and electron density of the Al0core than Fe^(0).More importantly,S-Al^(0)@Fe^(0) served as an electric cell to harness the persistent and selective electron transfer from the Al^(0)-Fe^(0) core to Cr(Ⅵ)at the surface via coupling Fe^(0)-Fe^(2+)-Fe^(3+)redox cycles,resulting in a higher electron utilization efficiency.Therefore,S-Al^(0)@Fe^(0) fabricated using recycled waste aluminum scraps can be a cost-effective and environmentally-friendly alternative to S-Fe^(0) for the enhanced removal of oxidative contaminants in industrial wastewater.
基金the National Key R&D Program of China(No.2018YFC1802500)the Key Project of National Natural Science Foundation of China(No.41530636)“the Fundamental Research Funds for the Central Universities”。
文摘After adding either organic or inorganic ligands,sulfidated nano-zero-valent iron(Sn ZVI)was used for aerobic degradation of phenol,and the effect of the ligand species on oxidation performance was investigated.We found that Sn ZVI hardly degraded phenol in the absence of ligand addition.Ligands initiated and promoted the degradation of pollutants by Sn ZVI.The data herein show that a characteristic inorganic ligand,tripolyphosphate(TPP),is more effective in enhancing oxidation than a characteristic organic ligand oxalate.In addition to the scavenging of reactive oxidants by the organic ligand,more ferrous ion(Fe(Ⅱ))dissolution from Sn ZVI in the TPP system is another cause for the superior enhancement by the inorganic ligand.In the oxalate system,as the sulfur content of Sn ZVI increased,the oxidation efficiency increased because Fe S shell promoted the transfer of electrons to produce more reactive oxygen species(ROS).In TPP system,the effect of sulfur content on oxidation performance is more complex.The Sn ZVI with low sulfur content showed poor oxidation performance compared with that of n ZVI.Further experiments proved that sulfidation might weaken the complexation of TPP with surface bound Fe,which would slow down the ionic Fe(II)dissolution rate.Therefore,sulfidation has the dual effects of enhancing electron transfer and inhibiting the complexation of inorganic ligands.In addition,the mechanisms of ROS generation in different ligand systems were investigated herein.Results showed that the critical ROS in both the oxalate and TPP systems are hydroxyl radicals,and that they are produced via one-electron activation of O_(2).
基金the National Key Research and Development Program of China(No.2019YFC1806203)for financial support。
文摘Sulfidation of zero-valent iron(ZVI)has attracted broad attention in recent years for improving the sequestration of contaminants from water.However,sulfidated ZVI(S-ZVI)is mostly synthesized in the aqueous phase,which usually causes the formation of a thick iron oxide layer on the ZVI surface and hinders the efficient electron transfer to the contaminants.In this study,an alcohothermal strategy was employed for S-ZVI synthesis by the one-step reaction of iron powder with elemental sulfur.It is found that ferrous sulfide(FeS)with high purity and fine crystallization was formed on the ZVI surface,which is extremely favorable for electron transfer.Cr(Ⅵ)removal experiments confirm that the rate constant of SZVI synthesized by the alcohothermal method was 267.1-and 5.4-fold higher than those of un-sulfidated ZVI and aqueous-phase synthesized S-ZVI,respectively.Systematic characterizations proved that Cr(Ⅵ)was reduced and co-precipitated on S-ZVI in the form of a Fe(Ⅲ)/Cr(Ⅲ)/Cr(Ⅵ)composite,suggesting its environmental benignancy.
基金financially supported by the National Natural Science Foundation of China(No.52374259)the Open Fund of the State Key Laboratory of Mineral Processing Science and Technology,China(No.BGRIMM-KJSKL-2023-11)the Major Science and Technology Projects in Yunnan Province,China(No.202302 AF080004)。
文摘It is difficult to recover chrysocolla from sulfidation flotation which is closely related to the mineral surface composition.In this study,the effects of fluoride roasting on the surface composition of chrysocolla were investigated,its impact on sulfidation flotation was explored,and the mechanisms involved in both fluoride roasting and sulfidation flotation were discussed.With CaF_(2)as the roasting reagent,Na_(2)S·9H_(2)O as the sulfidation reagent,and sodium butyl xanthate(NaBX)as the collector,the results of the flotation experiments showed that fluoride roasting improved the floatability of chrysocolla,and the recovery rate increased from 16.87%to 82.74%.X-ray diffraction analysis revealed that after fluoride roasting,approximately all the Cu on the chrysocolla surface was exposed in the form of CuO,which could provide a basis for subsequent sulfidation flotation.The microscopy and elemental analyses revealed that large quantities of"pagoda-like"grains were observed on the sulfidation surface of the fluoride-roasted chrysocolla,indicating high crystallinity particles of copper sulfide.This suggests that the effect of sulfide formation on the chrysocolla surface was more pronounced.X-ray photoelectron spectroscopy revealed that fluoride roasting increased the relative contents of sulfur and copper on the surface and that both the Cu~+and polysulfide fractions on the surface of the minerals increased.This enhances the effect of sulfidation,which is conducive to flotation recovery.Therefore,fluoride roasting improved the effect of copper species transformation and sulfidation on the surface of chysocolla,promoted the adsorption of collectors,and improved the recovery of chrysocolla from sulfidation flotation.
基金financially supported by the National Key Research and Development Program of China (No. 2022YFC2105300)。
文摘A series of leaching and electrochemical experiments were conducted to elucidate the critical role of hydrogen sulfide(H_(2)S)in copper-driven reduction of chalcopyrite.Results demonstrate that in the absence of H_(2)S,metallic copper converts chalcopyrite into bornite(Cu_(5)FeS_(4)).However,the introduction of H_(2)S promotes the formation of chalcocite(Cu_(2)S)by altering the oxidation pathway of copper.Electrochemical analysis demonstrates that the presence of H₂S significantly reduces the corrosion potential of copper from 0.251 to−0.223 V(vs SHE),reaching the threshold necessary for the formation of Cu_(2)S.Nevertheless,excessive H_(2)S triggers sulfate reduction via the reaction of 8Cu+H_(2)SO_(4)+3H_(2)S=4Cu_(2)S+4H_(2)O(ΔG=−519.429 kJ/mol at 50℃),leading to inefficient copper utilization.
基金supported by the National Science Foundation of China(Nos.42225202 and 41827802)。
文摘CM chondrites contain valuable insights into the formation and evolution of the solar nebula,as well as the secondary aqueous alteration processes that affected their parent bodies.Our study focuses on primary and secondary sulfides within the Aguas Zarcas(CM2)chondrite,investigating their formation mechanisms based on their morphology,textures,and compositions.Moreover,we infer the formation temperatures of the sulfides from 230 to 500℃ for primary and from 100 to 135℃ for secondary.We select representative grains and conduct Fe isotope measurements on them.The primary sulfides with δ^(56/54)Fe ranging from -2.44‰ to +0.69‰are associated with sulfidesilicate melt segregation,while secondary sulfides with δ^(56/54)Fe values between -1.83‰ and -0.14‰ are linked to aqueous alteration.Overall,the Ni content of the grains is positively correlated with δ^(56/54)Fe.It might be related to the changes in crystal structure and chemical bond lengths due to the increase in nickel content.Fe isotopes provide a new perspective on sulfide formation and the evolution of a carbonaceous chondrite parent body.
基金financially supported by the National Natural Science Foundation of China(No.52103040)China Postdoctoral Science Foundation(No.2020M673217)the Fundamental Research Funds for the Central Universities(No.2023SCU12022)。
文摘To address the poor mechanical performance and improve the tribological properties of self-lubricating polyphenylene sulfide/irradiation treated polytetrafluoroethylene(PPS/i-PTFE)blends,different aspect ratio carbon fibers(i.e.,PSCF:50,SCF:about 429)were introduced as reinforcement fillers.The results showed that the hybriding of PSCF and SCF at certain mass ratios exhibited simultaneous enhancement of mechanical and tribological performance for PPS/i-PTFE blend through the construction of synergistic lubrication and mechanical interlocking network.Specifically,the flexural strength and modulus of PPS/i-PTFE were increased by 125.6% and 389.3%,the friction coefficient and specific wear rate were decreased by 13.9% and 95%,respectively.It was worth noting that PPS composites possessed excellent integrated performance which were able to withstand sliding action under high PV(≥10 MPa·m/s)conditions,as assessed by a customized pin-on-disc tester.This work demonstrated that the formation of intact lubricating film combined with the enhanced thermal and mechanical properties were favorable for improving the tribological properties of PPS-based composites,which makes them suitable for advanced engineering applications.
基金financially supported by the National Key Research and Development Program(2022YFE0127400)the National Natural Science Foundation of China(52172040,52202041,and U23B2077)+1 种基金Taishan Scholar Project of Shandong Province(tsqn202211086,ts202208832,tsqnz20221118)the Fundamental Research Funds for the Central Universities(23CX06055A).
文摘Micro silicon(mSi)is a promising anode candidate for all-solid-state batteries due to its high specific capacity,low side reactions,and high tap density.However,silicon suffers from its poor electronic and ionic conductivity,which is particularly severe on a micro scale and in solid-state systems,leading to increased polarization and inferior electrochemical performance.Doping can broaden the transmission pathways and reduce the diffusion energy barrier for electrons and lithium ions.However,achieving effective,uniform doping in mSi is challenging due to its longer diffusion paths and higher energy barriers.Therefore,current doping research is primarily limited to nanosilicon.In this study,we successfully used a Joule-heating activated staged thermal treatment to achieve full-depth doping of germanium(Ge)in the mSi substrate.The Joule-heating process activated the mSi substrate,resulting in abundant vacancy defects that reduced the diffusion barrier of Ge into the silicon lattice and facilitated full-depth Ge doping.Surprisingly,the resulting Si-Ge anode exhibited significantly enhanced electrical conductivity(70 times).Meanwhile,the improved Li-ion conductivity in mSi and the reduced Young’s modulus enhance the electrode reaction kinetics and integrity after cycling.Ge-doped silicon anodes demonstrate excellent electrochemical performance when applied in sulfide solid-state half-cells and full-cells.This work provides substantial insights into the rational structural design of mSi alloyed anode materials,paving the way for the development of high-performance solid-state Li-ion batteries.
基金supported by the National Natural Science Foundation of China(Grant Nos.52002094)the Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2025A1515011995)+3 种基金the Shenzhen Science and Technology Innovation Program(GXWD20221030205923001)the Shandong Provincial Natural Science Foundation of China(Grant Nos.ZR2024QE525)the Shenzhen Key Laboratory of New Materials Technology(Grant Nos.SYSPG20241211173609003)the State Key Laboratory of Precision Welding&Joining of Materials and Structures(Grant Nos.2024-Z-17,2024-T-08)。
文摘Sulfide solid electrolytes are considered promising candidates for all-solid-state lithium batteries(ASSLBs)because of their high ionic conductivity and favorable mechanical properties.However,the uncontrolled growth of lithium dendrites at the lithium metal-electrolytes interface remains a major obstacle to their practical application.In this work,we introduced a scalable three-dimensional(3D)Li-B skeleton structure designed to suppress dendrite formation.The alloy anode demonstrates a lower Young's modulus,which helps alleviate the accumulation of localized stresses at the interface.Additionally,the 3D alloy anode provided a uniform potential distribution,which promoted homogeneous lithium deposition.Benefiting from these structural advantages,symmetric cells with the Li-B alloy achieved a high critical current density of 2.8 mA cm^(-2).Notably,Li-B‖LPSCI‖LVO-NCM ASSLBs exhibited long-term cycling stability,retaining 97.8%of their capacity after 1500 cycles at 2 C.Furthermore,ASSLBs incorporating the Li-B alloy showed cycling stability comparable with Li-In-based cells,while delivering a higher energy density.Overall,this work presents a practical strategy that may accelerate the commercialization of sulfide-based ASSLBs.
基金supported by the National Key R&D Program of China(2021YFB3800300).
文摘High-nickel cathode,LiNi0.8Co0.1Mn0.1O_(2)(NCM811),and sulfide-solid electrolyte are a promising combination for all-solid-state lithium batteries(ASSLBs).However,this combination faces the issue of interfacial instability between the cathode and electrolyte.Given the surface alkalinity of NCM811,we propose a strategy to construct a solid-polymer-electrolyte(SPE)interphase on NCM811 surface by leveraging the surface alkaline residues to nucleophilically initiate the in-situ ring-opening polymerization of cyclic organic molecules.As a proof-of-concept,this study demonstrates that the ring-opening copolymerization of 1,3-dioxolane and maleic anhydride produces a homogeneous,compact,and conformal SPE layer on NCM811 surface to prevent the cathode from contact and reaction with Li6PS5Cl solid-state electrolyte.Consequently,the SPE-modified-NCM811 in ASSLBs exhibits high capacities of 193.5 mA h g^(-1) at 0.2 C,160.9 mA h g^(-1) at 2.0 C and 112.3 mA h g^(-1) at 10 C,and particularly,excellent long-term cycling stabilities over 11000 cycles with a 71.95%capacity retention at 10 C at 25℃,as well as a remained capacity of 117.9 mA h g^(-1) after 8000 cycles at 30 C at 60℃,showing a great application prospect.This study provides a new route for creating electrochemically and structurally stable solid-solid interfaces for ASSLBs.
基金supported by the National Natural Science Foundation of China(No.51974016).
文摘Microwave roasting self-leaching is an innovative method for recovering gold from high-sulfur refractory gold concentrates,without using deadly toxic cyanide reagents.However,the mechanism of gold self-leaching,which relies on lixiviants prepared using volatilized sulfur obtained from roasting,has not been fully elucidated.This study employs the response surface methodology to optimize processing parameters,resulting in an increased gold extraction rate of 96.18%.Analytical factorization and the Tafel curve indicate that CuSO_(4) and NH_(3)·H_(2)O significantly influence the self-leaching process.Furthermore,X-ray photoelectron spectroscopy(XPS)analysis reveals that S^(2−),S_(2)^(2−),polysulfides(S_(n)^(2−)),and thiosulfate(S_(2)O_(3)^(2−))are involved in the gold leaching reaction,with S^(2−),S_(2)^(2−),and S_(n)^(2−) serving as primary ligands for gold complexation.The role of S_(2)O_(3)^(2−) in the early stages of the gold-leaching reaction is also noteworthy.The copper–ammonia complex catalyzes the self-leaching gold reaction;however,an improper addition ratio can lead to copper-sulfur compound precipitates,reducing the extraction rate.
基金the National Key Research and Development Program of China(No.2019YFC1805202)the National Natural Science Foundation of China(Nos.21876129 and 51608431).
文摘In this study,the influences of sulfidation on zero-valent iron(ZVI)performance toward As(Ⅴ)immobilization in soil were systemically investigated.It was found that,compared to unamended ZVI,sulfidated ZVI(S-ZVI)is more favorable to immobilize As(Ⅴ)in soil and promote the conversion of water soluble As to less mobile Fe-Mn bound As.Specifically,under the optimal S/Fe molar ratio of 0.05,almost all of the leached As could be sequestrated by>0.5 wt.%S-ZVI within 3 h.Although the presence of HA could decrease the desorption of As from soil,HA inhibited the reactivity of S-ZVI to a greater extent.Column experiments further proved the feasibility of applying S-ZVI on soil As(Ⅴ)immobilization.More importantly,to achieve a good As retention performance,S-ZVI should be fully mixed with soil or located on the downstream side of As migration.The test simulating the flooding conditions in rice culture revealed there was also a good long-term stability of soil As(Ⅴ)after S-ZVI remediation,where only 0.7%of As was desorbed after 30 days of incubation.Magnetic separation was employed to separate the immobilized As(Ⅴ)from soil after S-ZVI amendment,where the separation efficiency was found to be dependent of the iron dosage,liquid to soil ratio,and reaction time.Toxicity characteristic leaching procedure(TCLP)tests revealed that the leachability of As from soil was significantly reduced after the S-ZVI amendment and magnetic separation treatment.All these findings provided some insights into the remediation of As(Ⅴ)-polluted soil by ZVI.
基金financially supported by the National Natural Science Foundation of China(Grants nos.62201411,62371378,22205168,52302150 and 62304171)the China Postdoctoral Science Foundation(2022M722500)+1 种基金the Fundamental Research Funds for the Central Universities(Grants nos.ZYTS2308 and 20103237929)Startup Foundation of Xidian University(10251220001).
文摘Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,however,constrain their delicate constructions.Herein,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix.This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in M_(x)S_(y)/carbon composites(M-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial polarization.Such“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time.Consequently,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric response.Harnessing defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.
基金supported by the National Natural Science Foundation of China,Nos.82271327 (to ZW),82072535 (to ZW),81873768 (to ZW),and 82001253 (to TL)。
文摘The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular and cellular mechanisms by which quinolinic acid contributes to Huntington's disease pathology remain unknown. In this study, we established in vitro and in vivo models of Huntington's disease by administering quinolinic acid to the PC12 neuronal cell line and the striatum of mice, respectively. We observed a decrease in the levels of hydrogen sulfide in both PC12 cells and mouse serum, which was accompanied by down-regulation of cystathionine β-synthase, an enzyme responsible for hydrogen sulfide production. However, treatment with NaHS(a hydrogen sulfide donor) increased hydrogen sulfide levels in the neurons and in mouse serum, as well as cystathionine β-synthase expression in the neurons and the mouse striatum, while also improving oxidative imbalance and mitochondrial dysfunction in PC12 cells and the mouse striatum. These beneficial effects correlated with upregulation of nuclear factor erythroid 2-related factor 2 expression. Finally, treatment with the nuclear factor erythroid 2-related factor 2inhibitor ML385 reversed the beneficial impact of exogenous hydrogen sulfide on quinolinic acid-induced oxidative stress. Taken together, our findings show that hydrogen sulfide reduces oxidative stress in Huntington's disease by activating nuclear factor erythroid 2-related factor 2,suggesting that hydrogen sulfide is a novel neuroprotective drug candidate for treating patients with Huntington's disease.
文摘The use of visible-light responsive photocatalysts for removing heavy metal ions in wastewater has received great attention.However,the development of photocatalysts with high activity and recyclability remains a huge challenge.Herein,a recyclable carbon fiber cloth-supported porous CdS nanorod photocatalyst was fabricated by a two-step hydrothermal treatment using AgVO_(3) nanowires as templates.The results indicated that under visible-light illumination,the carbon cloth-supported porous CdS nanorods showed improved photocatalytic activity for the reduction of Cr(Ⅵ),with an apparent rate constant exceeding that of carbon cloth-supported CdS nanospheres by a factor of 1.65 times.Moreover,the carbon cloth-supported porous CdS nanorods can be easily separated and be reused.This brings a new perspective for developing photocatalysts with high efficiency and recyclability for wastewater treatment.
基金supported by the National Natural Science Foundation of China(Nos.52377026 and 52301192)the Taishan Scholars and Young Experts Program of Shandong Province(No.tsqn202103057)+3 种基金the Postdoctoral Fellow-ship Program of CPSF under Grant Number(No.GZB20240327)the Shandong Postdoctoral Science Foundation(No.SDCX-ZG-202400275)the Qingdao Postdoctoral Application Research Project(No.QDBSH20240102023)the Qingchuang Talents Induction Program of Shandong Higher Education Institution(Research and Innovation Team of Structural-Functional Polymer Composites).
文摘Reasonable manipulation of component and microstructure is considered as a potential route to realize high-performance microwave absorber.In this paper,micro-sized hexapod-like CuS/Cu_(9)S_(5) composites were synthesized via a facile approach involving the solvothermal method and subsequent sulfuration treatment.The resultant CuS/Cu_(9)S_(5) exhibited superb microwave absorbing capacity with a minimum reflection loss(RLmin)of-59.38 dB at 2.7 mm.The maximum effective absorption bandwidth(EABmax)was 7.44 GHz(10.56-18 GHz)when the thickness was reduced to 2.3 mm.The outstanding microwave absorbing ability of CuS/Cu_(9)S_(5) composites is mainly related to its unique hexapod shape and the formation of heterogeneous interfaces.The unique hexapod shape significantly promotes the multi-reflection of the incident electromagnetic wave(EMW)increasing the attenuation path of EMWs in the material.Hetero-geneous interfaces between CuS/Cu_(9)S_(5) enable powerful interface polarization,contributing to the atten-uation of EMWs propagating in the medium.In addition,the EMW absorption performance of CuS/Cu_(9)S_(5) composites is also inseparable from the conduction loss.This study provides a strong reference for the research of EMW absorbent materials based on transition metal sulfides.
文摘This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature<300℃.Sulfur vapor is a highly flammable gas,which then auto-ignites to produce a flame.This behavior suggests that an O_(2)-S gas-gas reaction mechanism may contribute to all-solid-state battery thermal runaway.To improve all-solid-state battery safety,current work focuses on eliminating the O_(2)source by changing the cathode active material.The conclusion of this study suggests that all-solidstate battery safety can also be realized by the development of solid-state electrolytes with less susceptibility to sulfur volatilization.
基金supported by the Science and Technology Department of Guangxi Zhuang Autonomous[grant numbers 2025GXNSFFA069003]the National Natural Science Foundation of China[grant numbers 22379030]+1 种基金Bagui Young Scholars Program of Guangxi Zhuang Autonomous Regionthe high-performance computing platform of Guangxi University.
文摘Mg-based hydrogen storage materials have attracted much attention due to their high hydrogen content,abundant resources,and environmental friendliness.However,the high dehydrogenation temperature,slow kinetics and poor cycling stability are limiting its practical application.This work demonstrates the improved dehydrogenation kinetics and cycling stability of MgH_(2) modified by a hybrid of metallic Ni and layered MoS_(2)(denoted as“Ni-MoS_(2)”)introduced by ball milling,with Ni as the catalyst for MgH_(2) and MoS_(2) as the support for both Ni and MgH_(2).The onset dehydrogenation temperature of MgH_(2) is reduced to 198℃,and the rehydrogenation begins at a low temperature of 50℃.The MgH_(2)+10 wt%Ni-MoS_(2) composite has a fast dehydrogenation kinetics and can release 6.1 wt% hydrogen in 10 min at a constant temperature of 300℃,with the dehydrogenation activation energy significantly reduced from 151 to 85 kJ mol^(-1).During the cycling,the reversible capacity of the composite first exhibits a gradual increase for the initial 22 cycles and then maintains at 6.1 wt% from the 23th cycle to the 50th cycle.The Ni/MoS_(2) addition does not change the overall thermodynamic properties of MgH_(2) but can weaken the Mg-H bonds in the local regions as evident by theoretical calculation.Microstructure studies reveal that the metallic Ni will react with MgH_(2) to form Mg_(2)NiH_(0.3),which can act as a hydrogen pump,while the layered MoS_(2) serves as a support for the well dispersion of MgH_(2) and Ni.It is believed that the synergy of Mg_(2)NiH_(0.3) and layered MoS_(2) contributes to the significantly enhanced hydrogen storage of MgH_(2).This work provides a promising and simple strategy for enhancing the Mg-based hydrogen storage materials by combination of transition metals and layered materials introduced via simple ball milling.
