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
DBUH-Br_3 catalyzed selective conversion of sulfides to sulfoxides in the presence of H_2O_2 as oxidizing agent is described.The reaction was performed selectively at room temperature and relatively short reaction times.
Immobilizing chiral 1,1'-bi-2-naphthol (BINOL) in one step onto polymer backbone via stable carbon-carbon bond through Suzuki reaction was achieved. The application of this immobilized chiral BINOL to the catalytic...Immobilizing chiral 1,1'-bi-2-naphthol (BINOL) in one step onto polymer backbone via stable carbon-carbon bond through Suzuki reaction was achieved. The application of this immobilized chiral BINOL to the catalytic asymmetric oxidation of sulfide to sulfoxide exhibited good activity (up to 60% yield) and high enantioselectivity (up to 89% ee). The immobilized chiral catalyst was very stable and could be readily reused for over 5 times without significant loss of catalytic activity and enantioselectivity.展开更多
Zr(IV)-salen-MCM-41 was prepared by reaction of NH2-MCM-41 with salicylaldehyde to afford Schiff base ligands. Thereafter, ZrOCh.SH2O was reacted with the Schiff base ligands for complex formation. The structural pr...Zr(IV)-salen-MCM-41 was prepared by reaction of NH2-MCM-41 with salicylaldehyde to afford Schiff base ligands. Thereafter, ZrOCh.SH2O was reacted with the Schiff base ligands for complex formation. The structural properties of the synthesized materials were investigated by a number of analytical techniques including X-ray diffraction, N2 sorption-desorption, thermogravimetric analysis, Fourier transform infrared spectroscopy, inductively coupled plasma atomic emission spectroscpopy, and energy dispersive X-ray spectroscopy. Catalytic studies of the mesoporous materials functionalized with Zr(IV)-Schiff base complexes were investigated and extended to selective oxida- tion of sulfides to sulfoxides and the Knoevenagel condensation reactions of aldehydes with malo- nonitriles and ethyl cyanoacetate. Additionally, catalyst recycling of the Zr-salen-MCM-41 materials was also studied.展开更多
Constructing new environmentally friendly dielectric coupling models is an effective strategy for design-ing high-performance wave absorbers.However,biomass carbon materials with high potential energy and a lack of ma...Constructing new environmentally friendly dielectric coupling models is an effective strategy for design-ing high-performance wave absorbers.However,biomass carbon materials with high potential energy and a lack of magnetic response mechanism do not fulfill the requirements.In this work,the effects of different pyrolysis temperatures and the introduction of different metal sulfides on the microscopic morphology and dielectric-magnetic properties of the composites were investigated.Among them,K el-ement detected in the biomass effectively modulates the conduction loss.The minimum reflection loss(RL_(min))of-62.42 dB at 1.8 mm and the maximum effective absorption bandwidth(EAB_(max))of-62.42 dB at 1.9 mm were obtained due to the non-uniform interfacial-induced polarization of the metal-sulfide nanosheets and the scattering of the electromagnetic waves(EW)by the“island”microstructures.This study provides a powerful reference for the modification and application of biomass materials.展开更多
Compared with organic electrolytes,aqueous electrolytes exhibit significantly higher ionic conductivity and possess inherent safety features,showcasing unique advantages in supercapacitors.However,challenges remain fo...Compared with organic electrolytes,aqueous electrolytes exhibit significantly higher ionic conductivity and possess inherent safety features,showcasing unique advantages in supercapacitors.However,challenges remain for low-salt aqueous electrolytes operating at high voltage and low temperature.Herein,we report a low-salt(0.87 m,m means mol kg^(-1))'salt in dimethyl sulfoxide/water'hybrid electrolyte with non-flammability via hybridizing aqueous electrolyte with an organic co-solvent of dimethyl sulfoxide(hydrogen bond acceptor).As a result,the 0.87 m hybrid electrolyte exhibits enhanced electrochemical stability,a freezing temperature below-50℃,and an outstanding ionic conductivity of 0.52mS cm~(-1)at-50℃.Dimethyl sulfoxide can anchor water molecules through intermolecular hydrogen bond interaction,effectively reinforcing the stability of water in the hybrid electrolyte.Furthermore,the interaction between dimethyl sulfoxide and water molecules diminishes the involvement of water in the generation of ordered ice crystals,finally facilitating the low-temperature performance of the hybrid electrolyte.When paired with the 0.87 m'salt in dimethyl sulfoxide/water'hybrid electrolyte,the symmetric supercapacitor presents a 2.0 V high operating voltage at 25℃,and can operate stably at-50℃.Importantly,the suppressed electrochemical reaction of water at-50℃further leads to the symmetric supercapacitor operated at a higher voltage of 2.6 V.This modification strategy opens an effective avenue to develop low-salt electrolytes for high-voltage and low-temperature aqueous supercapacitors.展开更多
The flotation separation of Cu–Fe sulfide minerals at low alkalinity can be achieved using selective depressants.In the flotation system of Cu–Fe sulfide minerals,depressants usually preferentially interact with the...The flotation separation of Cu–Fe sulfide minerals at low alkalinity can be achieved using selective depressants.In the flotation system of Cu–Fe sulfide minerals,depressants usually preferentially interact with the pyrite surface to render the mineral surface hydrophilic and hinder the adsorption of the collector.This review summarizes the advances in depressants for the flotation separation of Cu–Fe sulfide minerals at low alkalinity.These advances include use of inorganic depressants (oxidants and sulfur–oxygen compounds),natural polysaccharides (starch,dextrin,konjac glucomannan,and galactomannan),modified polymers (carboxymethyl cellulose,polyacrylamide,lignosulfonate,and tricarboxylate sodium starch),organic acids (polyglutamic acid,sodium humate,tannic acid,pyrogallic acid,salicylic acid,and lactic acid),sodium dimethyl dithiocarbamate,and diethylenetriamine.The potential application of specific inorganic and organic depressants in the flotation separation of Cu–Fe sulfide minerals at low alkalinity is reviewed.The advances in the use of organic depressants with respect to the flotation separation of Cu–Fe sulfide minerals are comprehensively detailed.Additionally,the depression performances and mechanisms of different types of organic depressants on mineral surfaces are summarized.Finally,several perspectives on depressants vis-à-vis flotation separation of Cu–Fe sulfide minerals at low alkalinity are proposed.展开更多
Hydrogen sulfide(H_(2)S)is a toxic,essential gas used in various biological and physical processes and has been the subject of many targeted studies on its role as a new gas transmitter.These studies have mainly focus...Hydrogen sulfide(H_(2)S)is a toxic,essential gas used in various biological and physical processes and has been the subject of many targeted studies on its role as a new gas transmitter.These studies have mainly focused on the production and pharmacological side effects caused by H_(2)S.Therefore,effective strategies to remove H_(2)S has become a key research topic.Furthermore,the development of novel nanoplatforms has provided new tools for the targeted removal of H_(2)S.This paper was performed to review the association between H_(2)S anddisease,relatedH_(2)S inhibitory drugs,aswell as H_(2)S responsive nanoplatforms(HRNs).This review first analyzed the role of H_(2)S in multiple tissues and conditions.Second,common drugs used to eliminate H_(2)S,as well as their potential for combination with anticancer agents,were summarized.Not only the existing studies on HRNs,but also the inhibition H_(2)S combined with different therapeutic methods were both sorted out in this review.Furthermore,this review provided in-depth analysis of the potential of HRNs about treatment or detection in detail.Finally,potential challenges of HRNs were proposed.This study demonstrates the excellent potential of HRNs for biomedical applications.展开更多
The production of toxic sulfides is a common environmental problem in mariculture.Therefore,the effective inhibition of sulfidogens is the key to prevent sulfides production.In this study,the possibility and mechanism...The production of toxic sulfides is a common environmental problem in mariculture.Therefore,the effective inhibition of sulfidogens is the key to prevent sulfides production.In this study,the possibility and mechanism of nitrate(NO_(3)^(−))inhibiting the activity of the sulfate-reducing microbiota(SRM)from mariculture sediments was investigated.The results showed that 1,3,and 5 mmol L^(−1)NO_(3)^(−)continuously inhibited sulfide production for 1-3 d.As NO_(3)^(−) dosage increased to 7 mmol L^(−1),the duration of inhibition increased to 6 days.Denitrifying product NO_(2)^(−)heavily inhibited the activity of dissimilar sulfate reductase gene(dsrB)by 3 orders,which was the main reason that the sulfate-reducing activity was inhibited.The SRM structure changed significantly with the dosage of NO_(3)^(−),while the abundance of sulfidogens Desulfovibrio species increased due to their capability of detoxifying nitrite through nitrite reductase.Hence,sulfidogens Desulfovibrio species are more adaptable to a high nitrate/nitrite environment,and the traditional control strategies by dosing nitrate/nitrite should be paid more attention to.The findings will serve as helpful guidelines for sulfate-reducing microbiota in the habitat of mariculture to reduce their generation of poisonous sulfide.展开更多
This paper is aimed to present a clean,inexpensive and sustainable method to synthesize high purity lithium sulfide(Li_(2)S)powder through hydrogen reduction of lithium sulfate(Li_(2)SO_(4)).A three-step reduction pro...This paper is aimed to present a clean,inexpensive and sustainable method to synthesize high purity lithium sulfide(Li_(2)S)powder through hydrogen reduction of lithium sulfate(Li_(2)SO_(4)).A three-step reduction process has been successfully developed to synthesize well-crystallized and single-phase Li_(2)S powder by investigating the melting,sintering and reduction behavior of the mixtures of Li_(2)SO_(4)-Li_(2)S.High purity alumina was found to be the most suitable crucible material for producing high purity Li_(2)S,because it was not attacked by the Li_(2)SO_(4)-Li_(2)S melt during heating,as compared with other materials,such as carbon,mullite,quartz,boron nitride and stainless steel.The use of synthesized LizS resulted in higher purity and substantially higher room temperature ionic conductivity(2.77 mS·cm^(-1))for the argyrodite sulfide electrolyte Li_(6)PS_(5)Cl than commercial Li_(2)S(1.12 mS·cm^(-1)).This novel method offers a great opportunity to produce battery grade Li_(2)S for sulfide solid electrolyte applications.展开更多
The solubility of H_(2)S was measured in solutions of N-butyl-N-methylmorpholine acetate([Bmmorp][Ac])containing 20%-40%(mass)water at experimental temperatures ranged from 298.15 to 328.15 K and pressures up to 320 k...The solubility of H_(2)S was measured in solutions of N-butyl-N-methylmorpholine acetate([Bmmorp][Ac])containing 20%-40%(mass)water at experimental temperatures ranged from 298.15 to 328.15 K and pressures up to 320 k Pa.The total solubility of H_(2)S increased with higher temperatures,lower pressures,and reduced water content.The reaction equilibrium thermodynamic model was used to correlate the solubility data.The results indicate that the chemical reaction equilibrium constant decrease with increasing water content and temperature,whereas Henry constant increase with increasing water content and temperature.Compared with other ionic liquids,H_(2)S exhibits a higher physical absorption enthalpy and a lower chemical absorption enthalpy in[Bmmorp][Ac]aqueous solution.This suggests that[Bmmorp][Ac]has a strong physical affinity for H_(2)S and low energy requirement for desorption.Quantum chemical methods were used to investigate the molecular mechanism of H_(2)S absorption in ionic liquids.The interaction energy analysis revealed that the binding of H_(2)S with the ionic liquid in a1:2 ratio is more stable.Detailed analyses by the methods of the interaction region indicator and the atoms in molecules were conducted to the interactions between H_(2)S and the ionic liquid.展开更多
Development of a high-performance bifunctional catalyst is essential for the actual implementation of zinc-air batteries in practical applications.Herein,a bifunctional cathode of Co_(3)S_(4)/FeS heterogeneous nanopar...Development of a high-performance bifunctional catalyst is essential for the actual implementation of zinc-air batteries in practical applications.Herein,a bifunctional cathode of Co_(3)S_(4)/FeS heterogeneous nanoparticles embedded in Co/Fe single-atom-loaded nitrogen-doped carbon nanosheets is designed.Cobalt-iron sulfides and single atomic sites with Co-N_(4)/Fe-N_(4)configurations are confirmed to coexist on the carbon matrix by EXAFS spectroscopy.3D self-supported super-hydrophobic multiphase composite cathode provides abundant active sites and facilitates gas–liquid-solid three-phase interface reactions,resulting in excellent electrocatalytic activity and batteries performance,i.e.,an OER overpotential(η_(10))of 260 mV,a half-wave potential(E_(1/2))of 0.872 V for ORR,aΔE of 0.618 V,and a discharge power density of 170 mW cm^(−2),a specific capacity of 816.3 mAh g^(−1).DFT analysis shows multiphase coupling of sulfide heterojunction through single-atomic metal doped carbon nanosheets reduces offset on center of electronic density of states before and after oxygen adsorption,and spin density of adsorbed oxygen with same spin orientation,leading to weakened charge/spin interactions between adsorbed oxygen and substrate,and a lowered oxygen adsorption energy to accelerate OER/ORR.展开更多
Silicon(Si)is a competitive anode material owing to its high theoretical capacity and low electrochemical potential.Recently,the prospect of Si anodes in solid-state batteries(SSBs)has been proposed due to less solid ...Silicon(Si)is a competitive anode material owing to its high theoretical capacity and low electrochemical potential.Recently,the prospect of Si anodes in solid-state batteries(SSBs)has been proposed due to less solid electrolyte interphase(SEI)formation and particle pulverization.However,major challenges arise for Si anodes in SSBs at elevated temperatures.In this work,the failure mechanisms of Si-Li_(6)PS_(5)Cl(LPSC)composite anodes above 80℃are thoroughly investigated from the perspectives of interface stability and(electro)chemo-mechanical effect.The chemistry and growth kinetics of Lix Si|LPSC interphase are demonstrated by combining electrochemical,chemical and computational characterizations.Si and/or Si–P compound formed at Lix Si|LPSC interface prove to be detrimental to interface stability at high temperatures.On the other hand,excessive volume expansion and local stress caused by Si lithiation at high temperatures damage the mechanical structure of Si-LPSC composite anodes.This work elucidates the behavior and failure mechanisms of Si-based anodes in SSBs at high temperatures and provides insights into upgrading Si-based anodes for application in SSBs.展开更多
Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au...Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au nanoparticles(NPs)(denoted as HP-Au@CoxSy@ZIF-67)hybrid is synthesized by low-temperature sulfuration treatment.The well-defined macroporous-mesoporous-microporous structure is obtained based on the combination of polystyrene spheres,as-formed CoxSy nanosheets,and ZIF-67 frameworks.This novel three-dimensional hierarchical structure significantly enlarges the three-phase interfaces,accelerating the mass transfer and exposing the active centers for oxygen evolution reaction.The electronic structure of Co is modulated by Au through charge transfer,and a series of experiments,together with theoretical analysis,is performed to ascertain the electronic modulation of Co by Au.Meanwhile,HP-Au@CoxSy@ZIF-67 catalysts with different amounts of Au were synthesized,wherein Au and NaBH4 reductant result in an interesting“competition effect”to regulate the relative ratio of Co^(2+)/Co^(3+),and moderate Au assists the electrochemical performance to reach the highest value.Consequently,the optimized HP-Au@CoxSy@ZIF-67 exhibits a low overpotential of 340 mV at 10 mA cm^(-2)and a Tafel slope of 42 mV dec-1 for OER in 0.1 M aqueous KOH,enabling efficient water splitting and Zn-air battery performance.The work here highlights the pivotal roles of both microstructural and electronic modulation in enhancing electrocatalytic activity and presents a feasible strategy for designing and optimizing advanced electrocatalysts.展开更多
Electrocatalytic hydrogen evolution and sulfion(S^(2-))recycling are promising strategies for boosting H_(2)production and removing environmental pollutants.Here,a nano-Ni-functionalized molybdenum disulfide(MoS_(2))n...Electrocatalytic hydrogen evolution and sulfion(S^(2-))recycling are promising strategies for boosting H_(2)production and removing environmental pollutants.Here,a nano-Ni-functionalized molybdenum disulfide(MoS_(2))nanosheet was assembled on steel mesh(Ni-MoS_(2)/SM)for use in sulfide oxidation reaction-assisted,energy-saving H_(2)production.Experimental and theoretical calculation results revealed that anchoring nano-Ni on high-surface-area slack MoS_(2)nanosheets not only optimized catalyst adsorption of polysulfides but also played an important role in promoting hydrogen evolution reaction kinetics by absorbing OH_(ad),thereby greatly enhancing the catalytic performance toward sulfide oxidation reaction and hydrogen evolution reaction.Meanwhile,the Ni/MoS^(2-)based hydrogen evolution reaction+sulfide oxidation reaction system achieved nearly 100%hydrogen production efficiency and only consumed 61%less power per kWh than the oxygen evolution reaction+hydrogen evolution reaction system,which suggested our proposed Ni-MoS_(2)and novel hydrogen production system are promising for sustainable energy production.展开更多
Sulfide-based inorganic solid electrolytes are promising materials for high-performance safe solid-state batteries.The high ion conductivity,mechanical characteristics,and good processability of sulfide-based inorgani...Sulfide-based inorganic solid electrolytes are promising materials for high-performance safe solid-state batteries.The high ion conductivity,mechanical characteristics,and good processability of sulfide-based inorganic solid electrolytes are desirable properties for realizing high-performance safe solid-state batteries by replacing conventional liquid electrolytes.However,the low chemical and electrochemical stability of sulfide-based inorganic solid electrolytes hinder the commercialization of sulfide-based safe solid-state batteries.Particularly,the instability of sulfide-based inorganic solid electrolytes is intensified in the cathode,comprising various materials.In this study,carbonate-based ionic conductive polymers are introduced to the cathode to protect cathode materials and suppress the reactivity of sulfide electrolytes.Several instruments,including electrochemical spectroscopy,X-ray photoelectron spectroscopy,and scanning electron microscopy,confirm the chemical and electrochemical stability of the polymer electrolytes in contact with sulfide-based inorganic solid electrolytes.Sulfide-based solid-state cells show stable electrochemical performance over 100 cycles when the ionic conductive polymers were applied to the cathode.展开更多
Xiarihamu deposit is the only super-large Ni-Co deposit found in East Kunlun orogenic belt(EKOB)until present.Shitoukengde(STKD)intrusion is considered to have the potential to become a large Ni-Co deposit in East Kun...Xiarihamu deposit is the only super-large Ni-Co deposit found in East Kunlun orogenic belt(EKOB)until present.Shitoukengde(STKD)intrusion is considered to have the potential to become a large Ni-Co deposit in East Kunlun.In order to discuss the metallogenic potential,this study present petrographical,geochemical data,and zircon U-Pb dating for the STKD intrusion.The STKD intrusion is hosted within mafic-ultramafic rocks which contain peridotite,pyroxenite and gabbro,and mainly intruded into the marble of the Paleoproterozoic Jinshuikou Group.Harzburgite and orthopyroxenite are the main country rocks for the Cu-Ni sulfide mineralization.Combine with the positiveε_(Hf)(t)values(+1.1 to+8.6)of zircons,the enrichment of LILEs,depletion of HFSEs,and lower Ce/Pb ratios of whole rocks indicate that the parental magma was originated from the depleted asthenospheric mantle and experienced 5%–15%crustal contamination.Troctolite formed during the Early Devonian and it has weighted mean^(206)Pb/^(238)U age of 412 Ma.Regional background information has indicated that the post-collisional extension setting has already existed during the Early Devonian,leading to the formation of STKD intrusion and Cu-Ni sulfide mineralization.STKD intrusion may have the potential to be one economic Cu-Ni sulfide deposit but seems unlikely to be a super-large one.展开更多
Although the internal electric field(IEF)of photocatalysts is acknowledged as a potent driving force for photocharge separation,modulating the IEF intensity to achieve enhanced photocatalytic performances remains a ch...Although the internal electric field(IEF)of photocatalysts is acknowledged as a potent driving force for photocharge separation,modulating the IEF intensity to achieve enhanced photocatalytic performances remains a challenge.Herein,cuprous sulfide nanosheets with different Cu vacancy concentration were employed to study IEF modulation and corresponding direct charge transfer.Among the samples,Cu_(1.8)S nanosheets possessed intensified IEF intensity compared with those of Cu_(2)S and Cu_(1.95)S nanosheets,suggesting that an enhanced IEF intensity could be achieved by introducing more Cu vacancies.This intensified IEF of Cu_(1.8)S nanosheets induced numerous photogenerated electrons to migrate to its surface,and the dissociative electrons were then captured by Cu vacancies,resulting in efficient charge separation spatially.In addition,the Cu vacancies on Cu_(1.8)S nanosheets accumulated electrons as active sites to lower the energy barrier of rate-determining step of CO_(2)photoreduction,leading to the selective conversion of CO_(2)to CO.Herein,the manipulation of IEF intensity through Cu vacancy concentration regulation of cuprous sulfide photocatalysts for efficient charge separation has been discussed,providing a scientific strategy to rationally improve photocata lytic performances for solar energy conversion.展开更多
FeS_(2)cathode is promising for all-solid-state lithium batteries due to its ultra-high capacity,low cost,and environmental friendliness.However,the poor performances,induced by limited electrode-electrolyte interface...FeS_(2)cathode is promising for all-solid-state lithium batteries due to its ultra-high capacity,low cost,and environmental friendliness.However,the poor performances,induced by limited electrode-electrolyte interface,severe volume expansion,and polysulfide shuttle,hinder the application of FeS_(2)in all-solid-state lithium batteries.Herein,an integrated 3D FeS_(2)electrode with full infiltration of Li6PS5Cl sulfide electrolytes is designed to address these challenges.Such a 3D integrated design not only achieves intimate and maximized interfacial contact between electrode and sulfide electrolytes,but also effectively buffers the inner volume change of FeS_(2)and completely eliminates the polysulfide shuttle through direct solid-solid conversion of Li2S/S.Besides,the vertical 3D arrays guarantee direct electron transport channels and horizontally shortened ion diffusion paths,endowing the integrated electrode with a remarkably reduced interfacial impedance and enhanced reaction kinetics.Benefiting from these synergies,the integrated all-solid-state lithium battery exhibits the largest reversible capacity(667 mAh g^(-1)),best rate performance,and highest capacity retention of 82%over 500 cycles at 0.1 C compared to both a liquid battery and non-integrated all-solid-state lithium battery.The cycling performance is among the best reported for FeS_(2)-based all-solid-state lithium batteries.This work presents an innovative synergistic strategy for designing long-cycling high-energy all-solid-state lithium batteries,which can be readily applied to other battery systems,such as lithium-sulfur batteries.展开更多
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DBUH-Br_3 catalyzed selective conversion of sulfides to sulfoxides in the presence of H_2O_2 as oxidizing agent is described.The reaction was performed selectively at room temperature and relatively short reaction times.
文摘Immobilizing chiral 1,1'-bi-2-naphthol (BINOL) in one step onto polymer backbone via stable carbon-carbon bond through Suzuki reaction was achieved. The application of this immobilized chiral BINOL to the catalytic asymmetric oxidation of sulfide to sulfoxide exhibited good activity (up to 60% yield) and high enantioselectivity (up to 89% ee). The immobilized chiral catalyst was very stable and could be readily reused for over 5 times without significant loss of catalytic activity and enantioselectivity.
基金Financial support to this work by the Ilam University
文摘Zr(IV)-salen-MCM-41 was prepared by reaction of NH2-MCM-41 with salicylaldehyde to afford Schiff base ligands. Thereafter, ZrOCh.SH2O was reacted with the Schiff base ligands for complex formation. The structural properties of the synthesized materials were investigated by a number of analytical techniques including X-ray diffraction, N2 sorption-desorption, thermogravimetric analysis, Fourier transform infrared spectroscopy, inductively coupled plasma atomic emission spectroscpopy, and energy dispersive X-ray spectroscopy. Catalytic studies of the mesoporous materials functionalized with Zr(IV)-Schiff base complexes were investigated and extended to selective oxida- tion of sulfides to sulfoxides and the Knoevenagel condensation reactions of aldehydes with malo- nonitriles and ethyl cyanoacetate. Additionally, catalyst recycling of the Zr-salen-MCM-41 materials was also studied.
基金supported by the National Natural Science Foundation of China(Nos.52377026 and 52301192)Natural Science Foundation of Shandong Province(Nos.ZR2019YQ24 and ZR2020QF084)+1 种基金Taishan Scholars and Young Experts Program of Shandong Province(No.tsqn202103057)the Qingchuang Talents Induction Program of Shandong Higher Education Institution(Research and Innovation Team of Structural-Functional Polymer Composites)and Special Financial of Shandong Province(Structural Design of High-efficiency Electromagnetic Wave-absorbing Composite Materials and Construction of Shandong Provincial Talent Teams).
文摘Constructing new environmentally friendly dielectric coupling models is an effective strategy for design-ing high-performance wave absorbers.However,biomass carbon materials with high potential energy and a lack of magnetic response mechanism do not fulfill the requirements.In this work,the effects of different pyrolysis temperatures and the introduction of different metal sulfides on the microscopic morphology and dielectric-magnetic properties of the composites were investigated.Among them,K el-ement detected in the biomass effectively modulates the conduction loss.The minimum reflection loss(RL_(min))of-62.42 dB at 1.8 mm and the maximum effective absorption bandwidth(EAB_(max))of-62.42 dB at 1.9 mm were obtained due to the non-uniform interfacial-induced polarization of the metal-sulfide nanosheets and the scattering of the electromagnetic waves(EW)by the“island”microstructures.This study provides a powerful reference for the modification and application of biomass materials.
基金partly supported by the National Key R&D Program of China(2022YFB4101602)the National Natural Science Foundation of China(22078052)the Fundamental Research Funds for the Central Universities(DUT22ZD207)。
文摘Compared with organic electrolytes,aqueous electrolytes exhibit significantly higher ionic conductivity and possess inherent safety features,showcasing unique advantages in supercapacitors.However,challenges remain for low-salt aqueous electrolytes operating at high voltage and low temperature.Herein,we report a low-salt(0.87 m,m means mol kg^(-1))'salt in dimethyl sulfoxide/water'hybrid electrolyte with non-flammability via hybridizing aqueous electrolyte with an organic co-solvent of dimethyl sulfoxide(hydrogen bond acceptor).As a result,the 0.87 m hybrid electrolyte exhibits enhanced electrochemical stability,a freezing temperature below-50℃,and an outstanding ionic conductivity of 0.52mS cm~(-1)at-50℃.Dimethyl sulfoxide can anchor water molecules through intermolecular hydrogen bond interaction,effectively reinforcing the stability of water in the hybrid electrolyte.Furthermore,the interaction between dimethyl sulfoxide and water molecules diminishes the involvement of water in the generation of ordered ice crystals,finally facilitating the low-temperature performance of the hybrid electrolyte.When paired with the 0.87 m'salt in dimethyl sulfoxide/water'hybrid electrolyte,the symmetric supercapacitor presents a 2.0 V high operating voltage at 25℃,and can operate stably at-50℃.Importantly,the suppressed electrochemical reaction of water at-50℃further leads to the symmetric supercapacitor operated at a higher voltage of 2.6 V.This modification strategy opens an effective avenue to develop low-salt electrolytes for high-voltage and low-temperature aqueous supercapacitors.
基金financially supported by the Yunnan Major Scientific and Technological Projects,China (No.202202AG050015)the National Natural Science Foundation of China (No.51464029)。
文摘The flotation separation of Cu–Fe sulfide minerals at low alkalinity can be achieved using selective depressants.In the flotation system of Cu–Fe sulfide minerals,depressants usually preferentially interact with the pyrite surface to render the mineral surface hydrophilic and hinder the adsorption of the collector.This review summarizes the advances in depressants for the flotation separation of Cu–Fe sulfide minerals at low alkalinity.These advances include use of inorganic depressants (oxidants and sulfur–oxygen compounds),natural polysaccharides (starch,dextrin,konjac glucomannan,and galactomannan),modified polymers (carboxymethyl cellulose,polyacrylamide,lignosulfonate,and tricarboxylate sodium starch),organic acids (polyglutamic acid,sodium humate,tannic acid,pyrogallic acid,salicylic acid,and lactic acid),sodium dimethyl dithiocarbamate,and diethylenetriamine.The potential application of specific inorganic and organic depressants in the flotation separation of Cu–Fe sulfide minerals at low alkalinity is reviewed.The advances in the use of organic depressants with respect to the flotation separation of Cu–Fe sulfide minerals are comprehensively detailed.Additionally,the depression performances and mechanisms of different types of organic depressants on mineral surfaces are summarized.Finally,several perspectives on depressants vis-à-vis flotation separation of Cu–Fe sulfide minerals at low alkalinity are proposed.
基金supported by National Key Research and Development Program of China(contract No.2019YFA0904800)National Nature Science Foundation of China(32030065,31722033,92049304 to Y.Z.)+5 种基金Shanghai Sailing Program(contract No.21YF1410300)Science and Technology Commission of Shanghai Municipality(contract No.10DZ2220500)The Shanghai Committee of Science and Technology(grant No.11DZ2260600)Shanghai Frontiers Science Center of Optogenetic Techniques for CellMetabolism(Y.Z.)Research Unit of New Techniques for Live-cell Metabolic Imaging(Chinese Academy of Medical Sciences,2019-I2M-5-013 to Y.Z.)the State Key Laboratory of Bioreactor Engineering,the Fundamental Research Funds for the Central Universities.
文摘Hydrogen sulfide(H_(2)S)is a toxic,essential gas used in various biological and physical processes and has been the subject of many targeted studies on its role as a new gas transmitter.These studies have mainly focused on the production and pharmacological side effects caused by H_(2)S.Therefore,effective strategies to remove H_(2)S has become a key research topic.Furthermore,the development of novel nanoplatforms has provided new tools for the targeted removal of H_(2)S.This paper was performed to review the association between H_(2)S anddisease,relatedH_(2)S inhibitory drugs,aswell as H_(2)S responsive nanoplatforms(HRNs).This review first analyzed the role of H_(2)S in multiple tissues and conditions.Second,common drugs used to eliminate H_(2)S,as well as their potential for combination with anticancer agents,were summarized.Not only the existing studies on HRNs,but also the inhibition H_(2)S combined with different therapeutic methods were both sorted out in this review.Furthermore,this review provided in-depth analysis of the potential of HRNs about treatment or detection in detail.Finally,potential challenges of HRNs were proposed.This study demonstrates the excellent potential of HRNs for biomedical applications.
基金supported by the National Natural Science Foundation of China(No.41977315)the Fundamental Research Funds for the Central Universities of China(No.201964004).
文摘The production of toxic sulfides is a common environmental problem in mariculture.Therefore,the effective inhibition of sulfidogens is the key to prevent sulfides production.In this study,the possibility and mechanism of nitrate(NO_(3)^(−))inhibiting the activity of the sulfate-reducing microbiota(SRM)from mariculture sediments was investigated.The results showed that 1,3,and 5 mmol L^(−1)NO_(3)^(−)continuously inhibited sulfide production for 1-3 d.As NO_(3)^(−) dosage increased to 7 mmol L^(−1),the duration of inhibition increased to 6 days.Denitrifying product NO_(2)^(−)heavily inhibited the activity of dissimilar sulfate reductase gene(dsrB)by 3 orders,which was the main reason that the sulfate-reducing activity was inhibited.The SRM structure changed significantly with the dosage of NO_(3)^(−),while the abundance of sulfidogens Desulfovibrio species increased due to their capability of detoxifying nitrite through nitrite reductase.Hence,sulfidogens Desulfovibrio species are more adaptable to a high nitrate/nitrite environment,and the traditional control strategies by dosing nitrate/nitrite should be paid more attention to.The findings will serve as helpful guidelines for sulfate-reducing microbiota in the habitat of mariculture to reduce their generation of poisonous sulfide.
基金Fiscal Year 2023-2024 High-Level and Growth Research and Development Subsidy for supporting the research and development activities for small and medium-size enterprise(SMEs),which is administered by Chiba Industry Advancement Center(Grant No.2066 and 2027)。
文摘This paper is aimed to present a clean,inexpensive and sustainable method to synthesize high purity lithium sulfide(Li_(2)S)powder through hydrogen reduction of lithium sulfate(Li_(2)SO_(4)).A three-step reduction process has been successfully developed to synthesize well-crystallized and single-phase Li_(2)S powder by investigating the melting,sintering and reduction behavior of the mixtures of Li_(2)SO_(4)-Li_(2)S.High purity alumina was found to be the most suitable crucible material for producing high purity Li_(2)S,because it was not attacked by the Li_(2)SO_(4)-Li_(2)S melt during heating,as compared with other materials,such as carbon,mullite,quartz,boron nitride and stainless steel.The use of synthesized LizS resulted in higher purity and substantially higher room temperature ionic conductivity(2.77 mS·cm^(-1))for the argyrodite sulfide electrolyte Li_(6)PS_(5)Cl than commercial Li_(2)S(1.12 mS·cm^(-1)).This novel method offers a great opportunity to produce battery grade Li_(2)S for sulfide solid electrolyte applications.
基金Financial support from the National Natural Science Foundation of China(21775081)Shandong Province Natural Science Foundation(ZR2020MB145)。
文摘The solubility of H_(2)S was measured in solutions of N-butyl-N-methylmorpholine acetate([Bmmorp][Ac])containing 20%-40%(mass)water at experimental temperatures ranged from 298.15 to 328.15 K and pressures up to 320 k Pa.The total solubility of H_(2)S increased with higher temperatures,lower pressures,and reduced water content.The reaction equilibrium thermodynamic model was used to correlate the solubility data.The results indicate that the chemical reaction equilibrium constant decrease with increasing water content and temperature,whereas Henry constant increase with increasing water content and temperature.Compared with other ionic liquids,H_(2)S exhibits a higher physical absorption enthalpy and a lower chemical absorption enthalpy in[Bmmorp][Ac]aqueous solution.This suggests that[Bmmorp][Ac]has a strong physical affinity for H_(2)S and low energy requirement for desorption.Quantum chemical methods were used to investigate the molecular mechanism of H_(2)S absorption in ionic liquids.The interaction energy analysis revealed that the binding of H_(2)S with the ionic liquid in a1:2 ratio is more stable.Detailed analyses by the methods of the interaction region indicator and the atoms in molecules were conducted to the interactions between H_(2)S and the ionic liquid.
基金supported by National Natural Science Foundation of China(Nos.51772213,12004283,12274324)Science and Technology Commission of Shanghai Municipality(No 21JC405700)Shanghai Key Laboratory of Special Artificial Microstructure Materials and Technology.
文摘Development of a high-performance bifunctional catalyst is essential for the actual implementation of zinc-air batteries in practical applications.Herein,a bifunctional cathode of Co_(3)S_(4)/FeS heterogeneous nanoparticles embedded in Co/Fe single-atom-loaded nitrogen-doped carbon nanosheets is designed.Cobalt-iron sulfides and single atomic sites with Co-N_(4)/Fe-N_(4)configurations are confirmed to coexist on the carbon matrix by EXAFS spectroscopy.3D self-supported super-hydrophobic multiphase composite cathode provides abundant active sites and facilitates gas–liquid-solid three-phase interface reactions,resulting in excellent electrocatalytic activity and batteries performance,i.e.,an OER overpotential(η_(10))of 260 mV,a half-wave potential(E_(1/2))of 0.872 V for ORR,aΔE of 0.618 V,and a discharge power density of 170 mW cm^(−2),a specific capacity of 816.3 mAh g^(−1).DFT analysis shows multiphase coupling of sulfide heterojunction through single-atomic metal doped carbon nanosheets reduces offset on center of electronic density of states before and after oxygen adsorption,and spin density of adsorbed oxygen with same spin orientation,leading to weakened charge/spin interactions between adsorbed oxygen and substrate,and a lowered oxygen adsorption energy to accelerate OER/ORR.
基金Project supported by the Major Program of the National Natural Science Foundation of China (Grant No.22393904)the National Key Research and Development Program of China (Grant No.2022YFB2502200)+1 种基金Beijing Municipal Science&Technology Commission (Grant No.Z221100006722015)the New Energy Vehicle Power Battery Life Cycle Testing and Verification Public Service Platform Project (Grant No.2022-235-224)。
文摘Silicon(Si)is a competitive anode material owing to its high theoretical capacity and low electrochemical potential.Recently,the prospect of Si anodes in solid-state batteries(SSBs)has been proposed due to less solid electrolyte interphase(SEI)formation and particle pulverization.However,major challenges arise for Si anodes in SSBs at elevated temperatures.In this work,the failure mechanisms of Si-Li_(6)PS_(5)Cl(LPSC)composite anodes above 80℃are thoroughly investigated from the perspectives of interface stability and(electro)chemo-mechanical effect.The chemistry and growth kinetics of Lix Si|LPSC interphase are demonstrated by combining electrochemical,chemical and computational characterizations.Si and/or Si–P compound formed at Lix Si|LPSC interface prove to be detrimental to interface stability at high temperatures.On the other hand,excessive volume expansion and local stress caused by Si lithiation at high temperatures damage the mechanical structure of Si-LPSC composite anodes.This work elucidates the behavior and failure mechanisms of Si-based anodes in SSBs at high temperatures and provides insights into upgrading Si-based anodes for application in SSBs.
基金National Natural Science Foundation of China,Grant/Award Numbers:52102260,52171211,51972220,61903235,U22A20145Shandong Provincial Natural Science Foundation,Grant/Award Numbers:ZR2020QB069,ZR2022ME051+4 种基金National Key Research and Development Program of China,Grant/Award Number:2022YFB4002004Scientific and Technological Innovation Ability Improvement Project of Minor Enterprises in Shandong Province,Grant/Award Number:2022TSGC1021Announce the List and Take Charge Project in Jinan,Grant/Award Number:202214012Major innovation project for integrating science,education and industry of Qilu University of Technology (Shandong Academy of Sciences),Grant/Award Numbers:2022JBZ01-07,2022PY044China Postdoctoral Science Foundation,Grant/Award Number:2022M711545。
文摘Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au nanoparticles(NPs)(denoted as HP-Au@CoxSy@ZIF-67)hybrid is synthesized by low-temperature sulfuration treatment.The well-defined macroporous-mesoporous-microporous structure is obtained based on the combination of polystyrene spheres,as-formed CoxSy nanosheets,and ZIF-67 frameworks.This novel three-dimensional hierarchical structure significantly enlarges the three-phase interfaces,accelerating the mass transfer and exposing the active centers for oxygen evolution reaction.The electronic structure of Co is modulated by Au through charge transfer,and a series of experiments,together with theoretical analysis,is performed to ascertain the electronic modulation of Co by Au.Meanwhile,HP-Au@CoxSy@ZIF-67 catalysts with different amounts of Au were synthesized,wherein Au and NaBH4 reductant result in an interesting“competition effect”to regulate the relative ratio of Co^(2+)/Co^(3+),and moderate Au assists the electrochemical performance to reach the highest value.Consequently,the optimized HP-Au@CoxSy@ZIF-67 exhibits a low overpotential of 340 mV at 10 mA cm^(-2)and a Tafel slope of 42 mV dec-1 for OER in 0.1 M aqueous KOH,enabling efficient water splitting and Zn-air battery performance.The work here highlights the pivotal roles of both microstructural and electronic modulation in enhancing electrocatalytic activity and presents a feasible strategy for designing and optimizing advanced electrocatalysts.
基金financially supported by the National Natural Science Foundation of China(22272131,2221154071221972111)+4 种基金the Natural Science Foundation of Chongqing(CSTB2022NSCQ-MSX1411)the Venture&Innovation Support Program for Chongqing Overseas Returnees(cx2019073)Chongqing Doctoral Research and Innovation Project(CYB21106)Chongqing Engineering Research Center for Micro-Nano Biomedical Materials and DevicesChongqing Key Laboratory for Advanced Materials and Technologies
文摘Electrocatalytic hydrogen evolution and sulfion(S^(2-))recycling are promising strategies for boosting H_(2)production and removing environmental pollutants.Here,a nano-Ni-functionalized molybdenum disulfide(MoS_(2))nanosheet was assembled on steel mesh(Ni-MoS_(2)/SM)for use in sulfide oxidation reaction-assisted,energy-saving H_(2)production.Experimental and theoretical calculation results revealed that anchoring nano-Ni on high-surface-area slack MoS_(2)nanosheets not only optimized catalyst adsorption of polysulfides but also played an important role in promoting hydrogen evolution reaction kinetics by absorbing OH_(ad),thereby greatly enhancing the catalytic performance toward sulfide oxidation reaction and hydrogen evolution reaction.Meanwhile,the Ni/MoS^(2-)based hydrogen evolution reaction+sulfide oxidation reaction system achieved nearly 100%hydrogen production efficiency and only consumed 61%less power per kWh than the oxygen evolution reaction+hydrogen evolution reaction system,which suggested our proposed Ni-MoS_(2)and novel hydrogen production system are promising for sustainable energy production.
基金supported by the Enhancement of Performance and Production Technology of Lithium-based Next-generation Rechargeable Battery(project number 20012371)from the Ministry of Trade,Industry and Energy(MOTIE)of Koreasupported by project number KS2322-20(A Study on the Convergence Materials for Off-Grid Energy Conversion/Storage Integrated Devices)of the Korea Research Institute of Chemical Technology(KRICT).
文摘Sulfide-based inorganic solid electrolytes are promising materials for high-performance safe solid-state batteries.The high ion conductivity,mechanical characteristics,and good processability of sulfide-based inorganic solid electrolytes are desirable properties for realizing high-performance safe solid-state batteries by replacing conventional liquid electrolytes.However,the low chemical and electrochemical stability of sulfide-based inorganic solid electrolytes hinder the commercialization of sulfide-based safe solid-state batteries.Particularly,the instability of sulfide-based inorganic solid electrolytes is intensified in the cathode,comprising various materials.In this study,carbonate-based ionic conductive polymers are introduced to the cathode to protect cathode materials and suppress the reactivity of sulfide electrolytes.Several instruments,including electrochemical spectroscopy,X-ray photoelectron spectroscopy,and scanning electron microscopy,confirm the chemical and electrochemical stability of the polymer electrolytes in contact with sulfide-based inorganic solid electrolytes.Sulfide-based solid-state cells show stable electrochemical performance over 100 cycles when the ionic conductive polymers were applied to the cathode.
基金financially supported by the National Natural Science Foundation of China(41272052)the projects(1212011120158 and 12120114080101)of the China Geological Survey。
文摘Xiarihamu deposit is the only super-large Ni-Co deposit found in East Kunlun orogenic belt(EKOB)until present.Shitoukengde(STKD)intrusion is considered to have the potential to become a large Ni-Co deposit in East Kunlun.In order to discuss the metallogenic potential,this study present petrographical,geochemical data,and zircon U-Pb dating for the STKD intrusion.The STKD intrusion is hosted within mafic-ultramafic rocks which contain peridotite,pyroxenite and gabbro,and mainly intruded into the marble of the Paleoproterozoic Jinshuikou Group.Harzburgite and orthopyroxenite are the main country rocks for the Cu-Ni sulfide mineralization.Combine with the positiveε_(Hf)(t)values(+1.1 to+8.6)of zircons,the enrichment of LILEs,depletion of HFSEs,and lower Ce/Pb ratios of whole rocks indicate that the parental magma was originated from the depleted asthenospheric mantle and experienced 5%–15%crustal contamination.Troctolite formed during the Early Devonian and it has weighted mean^(206)Pb/^(238)U age of 412 Ma.Regional background information has indicated that the post-collisional extension setting has already existed during the Early Devonian,leading to the formation of STKD intrusion and Cu-Ni sulfide mineralization.STKD intrusion may have the potential to be one economic Cu-Ni sulfide deposit but seems unlikely to be a super-large one.
基金supported by the National Natural Science Foundation of China(52200123)the Open Project of Key Laboratory of Green Chemical Engineering Process of Ministry of Education(GCP2022007)the Scientific Research and Innovation Team Program of Sichuan University of Science and Engineering(SUSE652A014)。
文摘Although the internal electric field(IEF)of photocatalysts is acknowledged as a potent driving force for photocharge separation,modulating the IEF intensity to achieve enhanced photocatalytic performances remains a challenge.Herein,cuprous sulfide nanosheets with different Cu vacancy concentration were employed to study IEF modulation and corresponding direct charge transfer.Among the samples,Cu_(1.8)S nanosheets possessed intensified IEF intensity compared with those of Cu_(2)S and Cu_(1.95)S nanosheets,suggesting that an enhanced IEF intensity could be achieved by introducing more Cu vacancies.This intensified IEF of Cu_(1.8)S nanosheets induced numerous photogenerated electrons to migrate to its surface,and the dissociative electrons were then captured by Cu vacancies,resulting in efficient charge separation spatially.In addition,the Cu vacancies on Cu_(1.8)S nanosheets accumulated electrons as active sites to lower the energy barrier of rate-determining step of CO_(2)photoreduction,leading to the selective conversion of CO_(2)to CO.Herein,the manipulation of IEF intensity through Cu vacancy concentration regulation of cuprous sulfide photocatalysts for efficient charge separation has been discussed,providing a scientific strategy to rationally improve photocata lytic performances for solar energy conversion.
基金supported by the National Natural Science Foundation of China(Grant nos.52272201,52072136,52172229,52302303,and 51972257)Yanchang Petroleum-WHUT Joint Program(yc-whlg-2022ky-05)+1 种基金the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology,2022-KF-20)Fundamental Research Funds for the Central Universities(2023IVA106)for financial support
文摘FeS_(2)cathode is promising for all-solid-state lithium batteries due to its ultra-high capacity,low cost,and environmental friendliness.However,the poor performances,induced by limited electrode-electrolyte interface,severe volume expansion,and polysulfide shuttle,hinder the application of FeS_(2)in all-solid-state lithium batteries.Herein,an integrated 3D FeS_(2)electrode with full infiltration of Li6PS5Cl sulfide electrolytes is designed to address these challenges.Such a 3D integrated design not only achieves intimate and maximized interfacial contact between electrode and sulfide electrolytes,but also effectively buffers the inner volume change of FeS_(2)and completely eliminates the polysulfide shuttle through direct solid-solid conversion of Li2S/S.Besides,the vertical 3D arrays guarantee direct electron transport channels and horizontally shortened ion diffusion paths,endowing the integrated electrode with a remarkably reduced interfacial impedance and enhanced reaction kinetics.Benefiting from these synergies,the integrated all-solid-state lithium battery exhibits the largest reversible capacity(667 mAh g^(-1)),best rate performance,and highest capacity retention of 82%over 500 cycles at 0.1 C compared to both a liquid battery and non-integrated all-solid-state lithium battery.The cycling performance is among the best reported for FeS_(2)-based all-solid-state lithium batteries.This work presents an innovative synergistic strategy for designing long-cycling high-energy all-solid-state lithium batteries,which can be readily applied to other battery systems,such as lithium-sulfur batteries.