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 global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous me...The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous metal oxide materials in the electrocatalytic reduction of CO_(2)(CO_(2)RR).The focus is on the development of robust and selective catalysts,particularly metal and metal-oxide-based materials.Porous metal oxides offer high surface area,enhancing the accessibility to active sites and improving reaction kinetics.The tunability of these materials allows for tailored catalytic behavior,targeting optimized reaction mechanisms for CO_(2)RR.The work also discusses the various synthesis strategies and identifies key structural and compositional features,addressing challenges like high overpotential,poor selectivity,and low stability.Based on these insights,we suggest avenues for future research on porous metal oxide materials for electrochemical CO_(2) reduction.展开更多
Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)...Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)FeO_(3-δ) perovskites as highly-active catalysts for LT-SOFCs.Sm doping can significantly enhance the electrocata lytic activity and chemical stability of cathode.At 600℃,Bi_(0.675)Sm_(0.025)Sr_(0.3)FeO_(3-δ)(BSSF25) cathode has been found to be the optimum composition with a polarization resistance of 0.098 Ω cm^2,which is only around 22.8% of Bi_(0.7)Sr_(0.3)FeO_(3-δ)(BSF).A full cell utilizing BSSF25 displays an exceptional output density of 790 mW cm^(-2),which can operate continuously over100 h without obvious degradation.The remarkable electrochemical performance observed can be attributed to the improved O_(2) transport kinetics,superior surface oxygen adsorption capacity,as well as O_(2)p band centers in close proximity to the Fermi level.Moreover,larger average bonding energy(ABE) and the presence of highly acidic Bi,Sm,and Fe ions restrict the adsorption of CO_(2) on the cathode surface,resulting in excellent CO_(2) resistivity.This work provides valuable guidance for systematic design of efficient and durable catalysts for LT-SOFCs.展开更多
For the application of carbon capture by membrane process,it is crucial to develop a highly permeable CO_(2)-selective membrane.In this work,we reported an ultra-thin polyether-block-amide(Pebax)mixedmatrix membranes(...For the application of carbon capture by membrane process,it is crucial to develop a highly permeable CO_(2)-selective membrane.In this work,we reported an ultra-thin polyether-block-amide(Pebax)mixedmatrix membranes(MMMs)incorporated by graphene oxide(GO),in which the interlayer channels were regulated to optimize the CO_(2)/N_(2) separation performance.Various membrane preparation conditions were systematically investigated on the influence of the membrane structure and separation performance,including the lateral size of GO nanosheets,GO loading,thermal reduction temperature,and time.The results demonstrated that the precisely regulated interlayer channel of GO nanosheets can rapidly provide CO_(2)-selective transport channels due to the synergetic effects of size sieving and preferential adsorption.The GO/Pebax ultra-thin MMMs exhibited CO_(2)/N_(2) selectivity of 72 and CO_(2) permeance of 400 GPU(1 GPU=106 cm^(3)(STP)·cm^(2)·s^(-1)·cmHg^(-1)),providing a promising candidate for CO_(2) capture.展开更多
In this study,the perovskite nanocomposite PrFe_(x)Co_(1-x)O_(3)(Pr(S))was successfully synthesized by the sol-gel method;PrFe_(x)Co_(1-x)O_(3)/Al-pillared montmorillonite(Pr(S)/Mt)catalysts were prepared by impregnat...In this study,the perovskite nanocomposite PrFe_(x)Co_(1-x)O_(3)(Pr(S))was successfully synthesized by the sol-gel method;PrFe_(x)Co_(1-x)O_(3)/Al-pillared montmorillonite(Pr(S)/Mt)catalysts were prepared by impregnation(D)method and solid-melting(G)method,respectively,with Pr(S)as the active component and Al-pillared montmorillonite as the carrier.The catalysts were applied to treat the 2-hydroxybenzoic acid(2-HA)-simulated wastewater by catalytic wet peroxide oxidation(CWPO)technique,and the chemical oxygen demand(COD)removal rate and the 2-HA degradation rate were used as indicators to evaluate the catalytic performance.The results of the experiment indicated that the solid-melting method was more conducive to preparing the catalyst when the Co/Fe molar ratio of 7:3 and the optimal structural properties of the catalysts were achieved.The influence of operating parameters,including reaction temperature,catalyst dosage,H_(2)O_(2)dosage,pH,and initial 2-HA concentration,were optimized for the degradation of 2-HA by CWPO.The results showed that 97.64%of 2-HA degradation and 75.23%of COD removal rate were achieved under more suitable experimental conditions.In addition,after the catalyst was used five times,the degradation rate of 2-HA could still reach 76.93%,which implied the high stability and reusability of the catalyst.The high catalytic activity of the catalyst was due to the doping of Co into PrFeO_(3),which could promote the generation of HO·,and the high stability could be attributed to the loading of Pr(S)onto Al-Mt,which reduced the leaching of reactive metals.The study of reaction mechanism and kinetics showed that the whole degradation process conformed to the pseudo-firstorder kinetic equation,and the Langmuir-Hinshelwood method was applied to demonstrate that catalysis was dominant in the degradation process.展开更多
Solid oxide electrolysis cells(SOECs),displaying high current density and energy efficiency,have been proven to be an effective technique to electrochemically reduce CO_(2)into CO.However,the insufficiency of cathode ...Solid oxide electrolysis cells(SOECs),displaying high current density and energy efficiency,have been proven to be an effective technique to electrochemically reduce CO_(2)into CO.However,the insufficiency of cathode activity and stability is a tricky problem to be addressed for SOECs.Hence,it is urgent to develop suitable cathode materials with excellent catalytic activity and stability for further practical application of SOECs.Herein,a reduced perovskite oxide,Pr_(0.35)Sr_(0.6)Fe_(0.7)Cu_(0.2)Mo_(0.1)O_(3-δ)(PSFCM0.35),is developed as SOECs cathode to electrolyze CO_(2).After reduction in 10%H_(2)/Ar,Cu and Fe nanoparticles are exsolved from the PSFCM0.35 lattice,resulting in a phase transformation from cubic perovskite to Ruddlesden-Popper(RP)perovskite with more oxygen vacancies.The exsolved metal nanoparticles are tightly attached to the perovskite substrate and afford more active sites to accelerate CO_(2)adsorption and dissociation on the cathode surface.The significantly strengthened CO_(2)adsorption capacity obtained after reduction is demonstrated by in situ Fourier transform-infrared(FT-IR)spectra.Symmetric cells with the reduced PSFCM0.35(R-PSFCM0.35)electrode exhibit a low polarization resistance of 0.43Ωcm^(2)at 850℃.Single electrolysis cells with the R-PSFCM0.35 cathode display an outstanding current density of 2947 mA cm^(-2)at 850℃and 1.6 V.In addition,the catalytic stability of the R-PSFCM0.35 cathode is also proved by operating at 800℃with an applied constant current density of 600 mA cm^(-2)for 100 h.展开更多
The unique characteristics of nanofibers in rational electrode design enable effec-tive utilization and maximizing material properties for achieving highly efficient and sustainable CO_(2) reduction reactions( CO_(2)R...The unique characteristics of nanofibers in rational electrode design enable effec-tive utilization and maximizing material properties for achieving highly efficient and sustainable CO_(2) reduction reactions( CO_(2)RRs)in solid oxide elec-trolysis cells(SOECs).However,practical appli-cation of nanofiber-based electrodes faces chal-lenges in establishing sufficient interfacial contact and adhesion with the dense electrolyte.To tackle this challenge,a novel hybrid nanofiber electrode,La_(0.6)Sr_(0.4)Co_(0.15)Fe_(0.8)Pd_(0.05)O_(3-δ)(H-LSCFP),is developed by strategically incorporating low aspect ratio crushed LSCFP nanofibers into the excess porous interspace of a high aspect ratio LSCFP nanofiber framework synthesized via electrospinning technique.After consecutive treatment in 100% H_(2) and CO_(2) at 700°C,LSCFP nanofibers form a perovskite phase with in situ exsolved Co metal nanocatalysts and a high concentration of oxygen species on the surface,enhancing CO_(2) adsorption.The SOEC with the H-LSCFP electrode yielded an outstanding current density of 2.2 A cm^(-2) in CO_(2) at 800°C and 1.5 V,setting a new benchmark among reported nanofiber-based electrodes.Digital twinning of the H-LSCFP reveals improved contact adhesion and increased reaction sites for CO_(2)RR.The present work demonstrates a highly catalytically active and robust nanofiber-based fuel electrode with a hybrid structure,paving the way for further advancements and nanofiber applications in CO_(2)-SOECs.展开更多
P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phas...P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phases remains a necessity.Herein,we design a P2/O3-type Na_(0.76)Ni_(0.31)Zn_(0.07)Mn_(0.50)Ti_(0.12)0_(2)(NNZMT)with high chemical/electrochemical stability by enhancing the coupling between the two phases.For the first time,a unique Na*extraction is observed from a Na-rich O3 phase by a Na-poor P2 phase and systematically investigated.This process is facilitated by Zn^(2+)/Ti^(4+)dual doping and calcination condition regulation,allowing a higher Na*content in the P2 phase with larger Na^(+)transport channels and enhancing Na transport kinetics.Because of reduced Na^(+)in the O3 phase,which increases the difficulty of H^(+)/Na^(+) exchange,the hydrostability of the O3 phase in NNZMT is considerably improved.Furthermore,Zn^(2+)/Ti^(4+)presence in NNZMT synergistically regulates oxygen redox chemistry,which effectively suppresses O_(2)/CO_(2) gas release and electrolyte decomposition,and completely inhibits phase transitions above 4.0 V.As a result,NNZMT achieves a high discharge capacity of 144.8 mA h g^(-1) with a median voltage of 3.42 V at 20 mA g^(-1) and exhibits excellent cycling performance with a capacity retention of 77.3% for 1000 cycles at 2000 mA g^(-1).This study provides an effective strategy and new insights into the design of high-performance layered-oxide cathode materials with enhanced structure/interface stability forSIBs.展开更多
Removing hydrogen sulfide(H_(2)S)via the selective oxidation has been considered an effective way to further purify the indusial sulfurcontaining due to it can completely transform residual H_(2)S into elemental sulfu...Removing hydrogen sulfide(H_(2)S)via the selective oxidation has been considered an effective way to further purify the indusial sulfurcontaining due to it can completely transform residual H_(2)S into elemental sulfur.While N-doped porous carbon was applied to H_(2)S selective oxidation,a sustainable methodology for the synthesis of efficient and stable N-doped carbon catalysts remains a difficulty,limiting its future development in large-scale applications.Herein,we present porous,honeycomb-like N-doped carbon catalysts with large specific surface areas,high pyridinic N content,and numerous structural defects for H_(2)S selective oxidation prepared using reusable NaCl as the template.The asprepared NC-10-800 catalyst exhibits excellent catalytic performance(sulfur formation rate of 784 g_(sulfur) kg_(cat.)^(-1) h^(-1)),outstanding stability(>100 h),and excellent anti-water vapor,anti-CO_(2) and anti-oxidation properties,suggesting significant potential for practical industrial application.The characterization results and kinetic study demonstrate that the large surface areas and structural defects created by the molten salt at high temperature enhance the exposure of pyridinic N sites and thus accelerate the catalytic activity.Importantly,the water-soluble NaCl template could be easily washed from the carbon nanomaterials,and thus the downstream salt-containing wastewater could be subsequently reused for the dissolution of carbon precursors.This environment-friendly,low-cost,reusable salt-template strategy has significant implications for the development of N-doped carbon catalysts for practical applications.展开更多
Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox activities.H...Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox activities.However,continuous voltage decay during cycling remains the primary obstacle for practical applications,which has yet to be fundamentally addressed.It is widely acknowledged that voltage decay originates from the irreversible migration of transition metal ions,which usually further exacerbates structural evolution and aggravates the irreversible oxygen redox reactions.Recently,constructing O2-type structure has been considered one of the most promising approaches for inhibiting voltage decay.In this review,the relationship between voltage decay and structural evolution is systematically elucidated.Strategies to suppress voltage decay are systematically summarized.Additionally,the design of O2-type structure and the corresponding mechanism of suppressing voltage decay are comprehensively discussed.Unfortunately,the reported O2-type LRLO cathodes still exhibit partially disordered structure with extended cycles.Herein,the factors that may cause the irreversible transition metal migrations in O2-type LRLO materials are also explored,while the perspectives and challenges for designing high-performance O2-type LRLO cathodes without voltage decay are proposed.展开更多
The metal oxide/nitrogen-doped carbon(NC)compounds zirconium oxide/NC(ZrO_(2)/NC)and cerium oxide/NC(CeO_(2)/NC)were synthesized via the pyrolysis of polyaniline on the metal oxide surface.The characterization of the ...The metal oxide/nitrogen-doped carbon(NC)compounds zirconium oxide/NC(ZrO_(2)/NC)and cerium oxide/NC(CeO_(2)/NC)were synthesized via the pyrolysis of polyaniline on the metal oxide surface.The characterization of the ZrO_(2)/NC and CeO_(2)/NC catalysts showed more active CO_(2) reduction reaction activity than that of NC catalyst without metal oxide.Gas chromatography analysis revealed that CO and H_(2)were the primary products,and no liquid-phase products were detected via proton nuclear magnetic resonance spectroscopy or high-performance liquid chromatography.The maximum Faraday effi ciency of ZrO_(2)/NC reached 90%at−0.73 V(vs.RHE),with the current density of CO at 5.5 mA/cm^(2);this Faraday effi ciency value was higher than that of NC(41%),with the current density of CO at 3.1 mA/cm^(2).The interaction between the metal oxide and carbon allowed the effi cient formation of defect sites,especially imine-type nitrogen,strengthening the adsorption of the key reaction intermediate CO_(2)^(•−) and thus promoting the CO_(2) reduction reaction.展开更多
The electrochemical carbon dioxide reduction reaction(CO_(2)RR),which can produce value-added chemical feedstocks,is a proton-coupled-electron process with sluggish kinetics.Thus,highly efficient,cheap catalysts are u...The electrochemical carbon dioxide reduction reaction(CO_(2)RR),which can produce value-added chemical feedstocks,is a proton-coupled-electron process with sluggish kinetics.Thus,highly efficient,cheap catalysts are urgently required.Transition metal oxides such as CoO_(x),FeO_(x),and NiO_(x)are low-cost,low toxicity,and abundant materials for a wide range of electrochemical reactions,but are almost inert for CO_(2)RR.Here,we report for the first time that nitrogen doped carbon nanotubes(N-CNT)have a surprising activation effect on the activity and selectivity of transition metal-oxide(MO_(x)where M=Fe,Ni,and Co)nanoclusters for CO_(2)RR.MO_(x)supported on N-CNT,MO_(x)/N-CNT,achieves a CO yield of 2.6–2.8 mmol cm−2 min−1 at an overpotential of−0.55 V,which is two orders of magnitude higher than MO_(x)supported on acid treated CNTs(MO_(x)/O-CNT)and four times higher than pristine N-CNT.The faraday efficiency for electrochemical CO_(2)-to-CO conversion is as high as 90.3%at overpotential of 0.44 V.Both in-situ XAS measurements and DFT calculations disclose that MO_(x)nanoclusters can be hydrated in CO_(2)saturated KHCO_(3),and the N defects of N-CNT effectively stabilize these metal hydroxyl species under carbon dioxide reduction reaction conditions,which can split the water molecules and provide local protons to inhibit the poisoning of active sites under carbon dioxide reduction reaction conditions.展开更多
V-Pd/γ-Al2O3-TiO2 catalysts with different vanadium contents were prepared by a combined sol-gel and impregnation method. X-ray diffraction (XRD), N2 adsorption-desorption (BET), X-ray photoelectron spectroscopy ...V-Pd/γ-Al2O3-TiO2 catalysts with different vanadium contents were prepared by a combined sol-gel and impregnation method. X-ray diffraction (XRD), N2 adsorption-desorption (BET), X-ray photoelectron spectroscopy (XPS) and catalytic removal of ethanol, acetaldehyde and nitrogen oxides at low temperature (〈300 ?C) were used to assess the properties of the catalysts. The results showed that the sample with 1wt% vanadium exhibited an excellent catalytic performance for simultaneous removal of ethanol, acetaldehyde and nitrogen oxides. The conversions of ethanol, acetaldehyde and nitrogen oxides at 250 ?C were 100%, 74.4% and 98.7%, respectively. V-Pd/γ-Al2O3-TiO2 catalyst with 1 wt% vanadium showed the largest surface area and higher dispersion of vanadium oxide on the catalyst surface, and possessed a larger mole fraction of V4+ species and unique PdO species on the surface, which can be attributed to the strong synergistic effect among palladium, vanadium and the carriers. The higher activity of V-Pd/γ-Al2O3-TiO2 catalyst is related to the V4+ and Pd2+ species on the surface, which might be favorable for the formation of active sites.展开更多
Unique MoS_(2)‐SnS_(2)heterogeneous nanoplates have successfully in‐situ grown on poly(3‐(1‐vinylimidazolium‐3‐yl)propane‐1‐sulfonate)functionalized polypyrrole/graphene oxide(PVIPS/PPy/GO).PVIPS can attract h...Unique MoS_(2)‐SnS_(2)heterogeneous nanoplates have successfully in‐situ grown on poly(3‐(1‐vinylimidazolium‐3‐yl)propane‐1‐sulfonate)functionalized polypyrrole/graphene oxide(PVIPS/PPy/GO).PVIPS can attract heptamolybdate ion(Mo7O246−)and Sn^(4+)as the precursors by the ion‐exchange,resulting in the simultaneous growth of 1T’‐MoS2 and the berndtite‐2T‐type hexagonal SnS_(2)by the interfacial induced effect of PVIPS.The obtained MoS_(2)‐SnS_(2)/PVIPS/PPy/GO can serve as electrocatalysts,exhibiting good NRR performance by the synergistic effect.The semi‐conducting SnS_(2)would limit the surface electron accessibility for suppressing HER process of 1T’‐MoS_(2),while metallic 1T’‐MoS_(2)might efficiently improve the NRR electroactivity of SnS_(2)by the creation of Mo‐Sn‐Sn trimer catalytic sites.Otherwise,the irreversible crystal phase transition has taken place during the NRR process.Partial 1T’‐MoS_(2)and SnS_(2)have electrochemically reacted with N_(2),and irreversibly converted into Mo^(2)N and SnxNz due to the formation of Mo−N and Sn−N bonding,meanwhile,partial SnS_(2) has been irreversibly evolved into SnS due to the reduction by the power source in the electrochemical system.It would put forward a new design idea for optimizing the preparation method and electrocatalytic activity of transition metal dichalcogenides.展开更多
In order to improve the total-dose radiation har dness of the buried oxides(BOX) in the structure of separation-by-implanted-oxygen(SIMOX) silicon-on-insulator(SOI),nitrogen ions are implanted into the buried oxides w...In order to improve the total-dose radiation har dness of the buried oxides(BOX) in the structure of separation-by-implanted-oxygen(SIMOX) silicon-on-insulator(SOI),nitrogen ions are implanted into the buried oxides with two different doses,2×10 15 and 3×10 15 cm -2 ,respectively.The experimental results show that the radiation hardness of the buried oxides is very sensitive to the doses of nitrogen implantation for a lower dose of irradiation with a Co-60 source.Despite the small difference between the doses of nitrogen implantation,the nitrogen-implanted 2×10 15 cm -2 BOX has a much higher hardness than the control sample (i.e.the buried oxide without receiving nitrogen implantation) for a total-dose irradiation of 5×104rad(Si),whereas the nitrogen-implanted 3×10 15 cm -2 BOX has a lower hardness than uhe control sample.However,this sensitivity of radiation hardness to the doses of nitrogen implantation reduces with the increasing total-dose of irradiation (from 5×104 to 5×105rad (Si)).The radiation hardness of BOX is characterized by MOS high-frequency (HF) capacitance-voltage (C-V) technique after the top silicon layers are removed.In addition,the abnormal HF C-V curve of the metal-silicon-BOX-silicon(MSOS) structure is observed and explained.展开更多
Ida2--H2O system(iminodiacetate aqueous solution) was used to leach a low grade zinc oxide ore for Zn extraction.The effects of leaching time,liquid-solid ratio(L/S),total concentration of Ida2-([Ida2-]T),leachi...Ida2--H2O system(iminodiacetate aqueous solution) was used to leach a low grade zinc oxide ore for Zn extraction.The effects of leaching time,liquid-solid ratio(L/S),total concentration of Ida2-([Ida2-]T),leaching temperature and pH on Zn leaching recovery and the dissolution of impurities such as Ca,Mg,Cu,Ni,Fe,Pb and Cd were investigated.Results show that Ca,Mg and Fe in ores were hardly dissolved in alkalescent iminodiacetate aqueous solution,while valuable metals such as Cu,Ni,Pb and Cd were partly dissolved into leaching liquor with Zn.The recovery of Zn reaches 76.6% when the ores were leached for 4 h at 70 ℃ by 0.9 mol/L iminodiacetate aqueous solution with pH of 8 and L/S of 5:1.展开更多
The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and catalytic activity tests. Acco...The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and catalytic activity tests. According to the results, a CeO2-TiO2solid solution is formed when the mole ratio of cerium to titanium n(Ce):n(Ti) is 5:5 or greater, and the most suitable n(Ce):n(Ti) isdetermined as 7:3, over which the conversion rate of SO2 and the yield of sulfur at 500℃ reach 93% and 99%, respectively.According to the activity testing curve, Ce0.7Ti0.3O2 (n(Ce):n(Ti)=7:3) without any pretreatment can be gradually activated by reagentgas after about 10 min, and reaches a steady activation status 60 min later. The XPS results of Ce0.7Ti0.3O2 after different time ofSO2+CO reaction show that CeO2 is the active component that offers the redox couple Ce4+/Ce3+ and the labile oxygen vacancies, andTiO2 only functions as a catalyst structure stabilizer during the catalytic reaction process. After 48 h of catalytic reaction at 500℃,Ce0.7Ti0.3O2 still maintains a stable structure without being vulcanized, demonstrating its good anti-sulfur poisoning performance.展开更多
The selective recovery of lead from the zinc oxide dust using an alkaline Na2EDTA solution was investigated. The effects of temperature, leaching time, Na2EDTA concentration and initial NaOH concentration on the leach...The selective recovery of lead from the zinc oxide dust using an alkaline Na2EDTA solution was investigated. The effects of temperature, leaching time, Na2EDTA concentration and initial NaOH concentration on the leaching rates of lead and zinc were studied. The following optimized leaching conditions were obtained: liquid-to-solid ratio 5:1 mL/g, stirring speed 650 r/min, Na2EDTA concentration 0.12 mol/L, initial NaOH concentration 0.5 mol/L, leaching temperature 70 ℃, leaching time 120 min. Under the optimized conditions, the average leaching rates of lead, zinc, fluoride and chloride are 89.92%, 0.94%, 62.84% and 90.02%, respectively. The filtrate was used to electrowin lead powders. The average current efficiency of electrowinning is about 93% and lead content is higher than 98% under the conditions of temperature of 60 ℃, current density of 200 A/m2, H3PO4 concentration of 1.5 g/L, and lead ion concentration of above 5 g/L. The consumption of Na2EDTA and the direct current are about respectively 0.218 kg and 0.958 kW·h for per kilogram of lead powder.展开更多
Hierarchical microspheres of a graphene oxide(GO) coupled to N‐doped(BiO)2CO3 composite(N‐BOC‐GO) was synthesized by a simple hydrothermal approach. The N‐BOC‐GO composite gave enhancement in photocatalytic...Hierarchical microspheres of a graphene oxide(GO) coupled to N‐doped(BiO)2CO3 composite(N‐BOC‐GO) was synthesized by a simple hydrothermal approach. The N‐BOC‐GO composite gave enhancement in photocatalytic activity compared to the pure BOC and N‐BOC samples. With 1.0wt% GO, 62% NO removal was obtained with N‐BOC‐GO. The factors enhancing the photocatalytic performance were the high electron‐withdrawing ability and high conductivity of GO and improved visible light‐harvesting ability of N‐BOC‐GO with a 3D hierarchical architecture due to the surface scattering and reflecting(SSR) effect. An effective charge transfer from N‐BOC to GO was demonstrated by the much weakened photoluminescene intensity of the N‐BOC‐GO composite. This work highlights the potential application of GO‐based photocatalysts in air purification.展开更多
Electrochemical oxidation of aniline in aqueous solution was investigated over a novel Ti/TiOxHy/Sb-SnO2 electrode prepared by the electrodeposition method.Scanning electron microscopy,X-ray diffraction,and electroche...Electrochemical oxidation of aniline in aqueous solution was investigated over a novel Ti/TiOxHy/Sb-SnO2 electrode prepared by the electrodeposition method.Scanning electron microscopy,X-ray diffraction,and electrochemical measurements were used to characterize its morphology,crystal structure,and electrochemical properties.Removal of aniline by the Ti/TiOxHy/Sb-SnO2electrode was investigated by ultraviolet-Visible spectroscopy and chemical oxygen demand(COD)analysis under different conditions,including current densities,initial concentrations of aniline,pH values,concentrations of chloride ions,and types of reactor.It was found that a higher current density,a lower initial concentration of aniline,an acidic solution,the presence of chloride ions(0.2wt%NaCl),and a three-dimensional(3D) reactor promoted the removal efficiency of aniline.Electrochemical degradation of aniline followed pseudo-first-order kinetics.The aniline(200 mL of 100mg·L-(-1)) and COD removal efficiencies reached 100%and 73.5%,respectively,at a current density of 20 mA·cm-(-2),pH of 7.0,and supporting electrolyte of 0.5 wt%Na2SO4 after 2 h electrolysis in a 3D reactor.These results show that aniline can be significantly removed on the Ti/TiOxHy/Sb-SnO2electrode,which provides an efficient way for elimination of aniline from aqueous solution.展开更多
基金supported by the National Natural Science Foundation of China,Nos.82271327 (to ZW),82072535 (to ZW),81873768 (to ZW),and 82001253 (to TL)。
文摘The pathophysiology of Huntington's disease involves high levels of the neurotoxin quinolinic acid. Quinolinic acid accumulation results in oxidative stress, which leads to neurotoxicity. However, the molecular and cellular mechanisms by which quinolinic acid contributes to Huntington's disease pathology remain unknown. In this study, we established in vitro and in vivo models of Huntington's disease by administering quinolinic acid to the PC12 neuronal cell line and the striatum of mice, respectively. We observed a decrease in the levels of hydrogen sulfide in both PC12 cells and mouse serum, which was accompanied by down-regulation of cystathionine β-synthase, an enzyme responsible for hydrogen sulfide production. However, treatment with NaHS(a hydrogen sulfide donor) increased hydrogen sulfide levels in the neurons and in mouse serum, as well as cystathionine β-synthase expression in the neurons and the mouse striatum, while also improving oxidative imbalance and mitochondrial dysfunction in PC12 cells and the mouse striatum. These beneficial effects correlated with upregulation of nuclear factor erythroid 2-related factor 2 expression. Finally, treatment with the nuclear factor erythroid 2-related factor 2inhibitor ML385 reversed the beneficial impact of exogenous hydrogen sulfide on quinolinic acid-induced oxidative stress. Taken together, our findings show that hydrogen sulfide reduces oxidative stress in Huntington's disease by activating nuclear factor erythroid 2-related factor 2,suggesting that hydrogen sulfide is a novel neuroprotective drug candidate for treating patients with Huntington's disease.
基金funded by the National Natural Science Foundation of China,China (Nos.52272303 and 52073212)the General Program of Municipal Natural Science Foundation of Tianjin,China (Nos.17JCYBJC22700 and 17JCYBJC17000)the State Scholarship Fund of China Scholarship Council,China (Nos.201709345012 and 201706255009)。
文摘The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous metal oxide materials in the electrocatalytic reduction of CO_(2)(CO_(2)RR).The focus is on the development of robust and selective catalysts,particularly metal and metal-oxide-based materials.Porous metal oxides offer high surface area,enhancing the accessibility to active sites and improving reaction kinetics.The tunability of these materials allows for tailored catalytic behavior,targeting optimized reaction mechanisms for CO_(2)RR.The work also discusses the various synthesis strategies and identifies key structural and compositional features,addressing challenges like high overpotential,poor selectivity,and low stability.Based on these insights,we suggest avenues for future research on porous metal oxide materials for electrochemical CO_(2) reduction.
基金supported by the National Natural Science Foundation of China(22279025,21773048)the Natural Science Foundation of Heilongjiang Province(LH2021A013)+1 种基金the Sichuan Science and Technology Program(2021YFSY0022)the Fundamental Research Funds for the Central Universities(2023FRFK06005,HIT.NSRIF202204)。
文摘Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)FeO_(3-δ) perovskites as highly-active catalysts for LT-SOFCs.Sm doping can significantly enhance the electrocata lytic activity and chemical stability of cathode.At 600℃,Bi_(0.675)Sm_(0.025)Sr_(0.3)FeO_(3-δ)(BSSF25) cathode has been found to be the optimum composition with a polarization resistance of 0.098 Ω cm^2,which is only around 22.8% of Bi_(0.7)Sr_(0.3)FeO_(3-δ)(BSF).A full cell utilizing BSSF25 displays an exceptional output density of 790 mW cm^(-2),which can operate continuously over100 h without obvious degradation.The remarkable electrochemical performance observed can be attributed to the improved O_(2) transport kinetics,superior surface oxygen adsorption capacity,as well as O_(2)p band centers in close proximity to the Fermi level.Moreover,larger average bonding energy(ABE) and the presence of highly acidic Bi,Sm,and Fe ions restrict the adsorption of CO_(2) on the cathode surface,resulting in excellent CO_(2) resistivity.This work provides valuable guidance for systematic design of efficient and durable catalysts for LT-SOFCs.
基金financially supported by The Natural Science Foundation of the Jiangsu Higher Education Institutions of China(22KJB530007,22KJA530001)National Natural Science Foundation of China(22208151)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20220002)the State Key Laboratory of MaterialsOriented Chemical Engineering(SKL-MCE-22B07).
文摘For the application of carbon capture by membrane process,it is crucial to develop a highly permeable CO_(2)-selective membrane.In this work,we reported an ultra-thin polyether-block-amide(Pebax)mixedmatrix membranes(MMMs)incorporated by graphene oxide(GO),in which the interlayer channels were regulated to optimize the CO_(2)/N_(2) separation performance.Various membrane preparation conditions were systematically investigated on the influence of the membrane structure and separation performance,including the lateral size of GO nanosheets,GO loading,thermal reduction temperature,and time.The results demonstrated that the precisely regulated interlayer channel of GO nanosheets can rapidly provide CO_(2)-selective transport channels due to the synergetic effects of size sieving and preferential adsorption.The GO/Pebax ultra-thin MMMs exhibited CO_(2)/N_(2) selectivity of 72 and CO_(2) permeance of 400 GPU(1 GPU=106 cm^(3)(STP)·cm^(2)·s^(-1)·cmHg^(-1)),providing a promising candidate for CO_(2) capture.
基金supported by the Key Research and Development Program of Shaanxi,China(2018GY-067).
文摘In this study,the perovskite nanocomposite PrFe_(x)Co_(1-x)O_(3)(Pr(S))was successfully synthesized by the sol-gel method;PrFe_(x)Co_(1-x)O_(3)/Al-pillared montmorillonite(Pr(S)/Mt)catalysts were prepared by impregnation(D)method and solid-melting(G)method,respectively,with Pr(S)as the active component and Al-pillared montmorillonite as the carrier.The catalysts were applied to treat the 2-hydroxybenzoic acid(2-HA)-simulated wastewater by catalytic wet peroxide oxidation(CWPO)technique,and the chemical oxygen demand(COD)removal rate and the 2-HA degradation rate were used as indicators to evaluate the catalytic performance.The results of the experiment indicated that the solid-melting method was more conducive to preparing the catalyst when the Co/Fe molar ratio of 7:3 and the optimal structural properties of the catalysts were achieved.The influence of operating parameters,including reaction temperature,catalyst dosage,H_(2)O_(2)dosage,pH,and initial 2-HA concentration,were optimized for the degradation of 2-HA by CWPO.The results showed that 97.64%of 2-HA degradation and 75.23%of COD removal rate were achieved under more suitable experimental conditions.In addition,after the catalyst was used five times,the degradation rate of 2-HA could still reach 76.93%,which implied the high stability and reusability of the catalyst.The high catalytic activity of the catalyst was due to the doping of Co into PrFeO_(3),which could promote the generation of HO·,and the high stability could be attributed to the loading of Pr(S)onto Al-Mt,which reduced the leaching of reactive metals.The study of reaction mechanism and kinetics showed that the whole degradation process conformed to the pseudo-firstorder kinetic equation,and the Langmuir-Hinshelwood method was applied to demonstrate that catalysis was dominant in the degradation process.
基金supported by the National Natural Science Foundation of China(No.22278203,No.22279057)the support of the Inner Mongolia major science and technology project(2021ZD0042),Development of integrated technology for CO_(2)emission reduction in electric power metallurgy industry
文摘Solid oxide electrolysis cells(SOECs),displaying high current density and energy efficiency,have been proven to be an effective technique to electrochemically reduce CO_(2)into CO.However,the insufficiency of cathode activity and stability is a tricky problem to be addressed for SOECs.Hence,it is urgent to develop suitable cathode materials with excellent catalytic activity and stability for further practical application of SOECs.Herein,a reduced perovskite oxide,Pr_(0.35)Sr_(0.6)Fe_(0.7)Cu_(0.2)Mo_(0.1)O_(3-δ)(PSFCM0.35),is developed as SOECs cathode to electrolyze CO_(2).After reduction in 10%H_(2)/Ar,Cu and Fe nanoparticles are exsolved from the PSFCM0.35 lattice,resulting in a phase transformation from cubic perovskite to Ruddlesden-Popper(RP)perovskite with more oxygen vacancies.The exsolved metal nanoparticles are tightly attached to the perovskite substrate and afford more active sites to accelerate CO_(2)adsorption and dissociation on the cathode surface.The significantly strengthened CO_(2)adsorption capacity obtained after reduction is demonstrated by in situ Fourier transform-infrared(FT-IR)spectra.Symmetric cells with the reduced PSFCM0.35(R-PSFCM0.35)electrode exhibit a low polarization resistance of 0.43Ωcm^(2)at 850℃.Single electrolysis cells with the R-PSFCM0.35 cathode display an outstanding current density of 2947 mA cm^(-2)at 850℃and 1.6 V.In addition,the catalytic stability of the R-PSFCM0.35 cathode is also proved by operating at 800℃with an applied constant current density of 600 mA cm^(-2)for 100 h.
基金This work was supported by the National Research Foundation of Korea(NRF)grant funded by the Korean Government(MSIT)(2019M3E6A1103944,2020R1A2C2010690).
文摘The unique characteristics of nanofibers in rational electrode design enable effec-tive utilization and maximizing material properties for achieving highly efficient and sustainable CO_(2) reduction reactions( CO_(2)RRs)in solid oxide elec-trolysis cells(SOECs).However,practical appli-cation of nanofiber-based electrodes faces chal-lenges in establishing sufficient interfacial contact and adhesion with the dense electrolyte.To tackle this challenge,a novel hybrid nanofiber electrode,La_(0.6)Sr_(0.4)Co_(0.15)Fe_(0.8)Pd_(0.05)O_(3-δ)(H-LSCFP),is developed by strategically incorporating low aspect ratio crushed LSCFP nanofibers into the excess porous interspace of a high aspect ratio LSCFP nanofiber framework synthesized via electrospinning technique.After consecutive treatment in 100% H_(2) and CO_(2) at 700°C,LSCFP nanofibers form a perovskite phase with in situ exsolved Co metal nanocatalysts and a high concentration of oxygen species on the surface,enhancing CO_(2) adsorption.The SOEC with the H-LSCFP electrode yielded an outstanding current density of 2.2 A cm^(-2) in CO_(2) at 800°C and 1.5 V,setting a new benchmark among reported nanofiber-based electrodes.Digital twinning of the H-LSCFP reveals improved contact adhesion and increased reaction sites for CO_(2)RR.The present work demonstrates a highly catalytically active and robust nanofiber-based fuel electrode with a hybrid structure,paving the way for further advancements and nanofiber applications in CO_(2)-SOECs.
基金supported by the National Natural Science Foundation of China (22169002)the Chongzuo Key Research and Development Program of China (20220603)the Counterpart Aid Project for Discipline Construction from Guangxi University(2023M02)
文摘P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phases remains a necessity.Herein,we design a P2/O3-type Na_(0.76)Ni_(0.31)Zn_(0.07)Mn_(0.50)Ti_(0.12)0_(2)(NNZMT)with high chemical/electrochemical stability by enhancing the coupling between the two phases.For the first time,a unique Na*extraction is observed from a Na-rich O3 phase by a Na-poor P2 phase and systematically investigated.This process is facilitated by Zn^(2+)/Ti^(4+)dual doping and calcination condition regulation,allowing a higher Na*content in the P2 phase with larger Na^(+)transport channels and enhancing Na transport kinetics.Because of reduced Na^(+)in the O3 phase,which increases the difficulty of H^(+)/Na^(+) exchange,the hydrostability of the O3 phase in NNZMT is considerably improved.Furthermore,Zn^(2+)/Ti^(4+)presence in NNZMT synergistically regulates oxygen redox chemistry,which effectively suppresses O_(2)/CO_(2) gas release and electrolyte decomposition,and completely inhibits phase transitions above 4.0 V.As a result,NNZMT achieves a high discharge capacity of 144.8 mA h g^(-1) with a median voltage of 3.42 V at 20 mA g^(-1) and exhibits excellent cycling performance with a capacity retention of 77.3% for 1000 cycles at 2000 mA g^(-1).This study provides an effective strategy and new insights into the design of high-performance layered-oxide cathode materials with enhanced structure/interface stability forSIBs.
基金financially supported by the National Key R&D Program of China(No.2022YFC3701900)National Natural Science Foundation of China(Nos.21606243)+1 种基金LiaoNing Revitalization Talents Program(XLYC1907053)Dalian National Laboratory for Clean Energy(DNL202021).
文摘Removing hydrogen sulfide(H_(2)S)via the selective oxidation has been considered an effective way to further purify the indusial sulfurcontaining due to it can completely transform residual H_(2)S into elemental sulfur.While N-doped porous carbon was applied to H_(2)S selective oxidation,a sustainable methodology for the synthesis of efficient and stable N-doped carbon catalysts remains a difficulty,limiting its future development in large-scale applications.Herein,we present porous,honeycomb-like N-doped carbon catalysts with large specific surface areas,high pyridinic N content,and numerous structural defects for H_(2)S selective oxidation prepared using reusable NaCl as the template.The asprepared NC-10-800 catalyst exhibits excellent catalytic performance(sulfur formation rate of 784 g_(sulfur) kg_(cat.)^(-1) h^(-1)),outstanding stability(>100 h),and excellent anti-water vapor,anti-CO_(2) and anti-oxidation properties,suggesting significant potential for practical industrial application.The characterization results and kinetic study demonstrate that the large surface areas and structural defects created by the molten salt at high temperature enhance the exposure of pyridinic N sites and thus accelerate the catalytic activity.Importantly,the water-soluble NaCl template could be easily washed from the carbon nanomaterials,and thus the downstream salt-containing wastewater could be subsequently reused for the dissolution of carbon precursors.This environment-friendly,low-cost,reusable salt-template strategy has significant implications for the development of N-doped carbon catalysts for practical applications.
基金funded by the National Natural Science Foundation of China(Grant Nos.22279092 and 5202780089).
文摘Li-rich layered oxide(LRLO)cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density,which combines cationic and anionic redox activities.However,continuous voltage decay during cycling remains the primary obstacle for practical applications,which has yet to be fundamentally addressed.It is widely acknowledged that voltage decay originates from the irreversible migration of transition metal ions,which usually further exacerbates structural evolution and aggravates the irreversible oxygen redox reactions.Recently,constructing O2-type structure has been considered one of the most promising approaches for inhibiting voltage decay.In this review,the relationship between voltage decay and structural evolution is systematically elucidated.Strategies to suppress voltage decay are systematically summarized.Additionally,the design of O2-type structure and the corresponding mechanism of suppressing voltage decay are comprehensively discussed.Unfortunately,the reported O2-type LRLO cathodes still exhibit partially disordered structure with extended cycles.Herein,the factors that may cause the irreversible transition metal migrations in O2-type LRLO materials are also explored,while the perspectives and challenges for designing high-performance O2-type LRLO cathodes without voltage decay are proposed.
基金The work was supported by the National Key R&D Program of China(No.2016YFB0600901)Changyi Hydrogen Industrial Technology Fund.
文摘The metal oxide/nitrogen-doped carbon(NC)compounds zirconium oxide/NC(ZrO_(2)/NC)and cerium oxide/NC(CeO_(2)/NC)were synthesized via the pyrolysis of polyaniline on the metal oxide surface.The characterization of the ZrO_(2)/NC and CeO_(2)/NC catalysts showed more active CO_(2) reduction reaction activity than that of NC catalyst without metal oxide.Gas chromatography analysis revealed that CO and H_(2)were the primary products,and no liquid-phase products were detected via proton nuclear magnetic resonance spectroscopy or high-performance liquid chromatography.The maximum Faraday effi ciency of ZrO_(2)/NC reached 90%at−0.73 V(vs.RHE),with the current density of CO at 5.5 mA/cm^(2);this Faraday effi ciency value was higher than that of NC(41%),with the current density of CO at 3.1 mA/cm^(2).The interaction between the metal oxide and carbon allowed the effi cient formation of defect sites,especially imine-type nitrogen,strengthening the adsorption of the key reaction intermediate CO_(2)^(•−) and thus promoting the CO_(2) reduction reaction.
基金Y.C.and J.C.are contributed equally to the paper.Project supported by the National Natural Science Foundation of China (U19A2017)the Fundamental Research Funds for the Central South University and the Australian Research Council (DP180100731 and DP180100568)。
文摘The electrochemical carbon dioxide reduction reaction(CO_(2)RR),which can produce value-added chemical feedstocks,is a proton-coupled-electron process with sluggish kinetics.Thus,highly efficient,cheap catalysts are urgently required.Transition metal oxides such as CoO_(x),FeO_(x),and NiO_(x)are low-cost,low toxicity,and abundant materials for a wide range of electrochemical reactions,but are almost inert for CO_(2)RR.Here,we report for the first time that nitrogen doped carbon nanotubes(N-CNT)have a surprising activation effect on the activity and selectivity of transition metal-oxide(MO_(x)where M=Fe,Ni,and Co)nanoclusters for CO_(2)RR.MO_(x)supported on N-CNT,MO_(x)/N-CNT,achieves a CO yield of 2.6–2.8 mmol cm−2 min−1 at an overpotential of−0.55 V,which is two orders of magnitude higher than MO_(x)supported on acid treated CNTs(MO_(x)/O-CNT)and four times higher than pristine N-CNT.The faraday efficiency for electrochemical CO_(2)-to-CO conversion is as high as 90.3%at overpotential of 0.44 V.Both in-situ XAS measurements and DFT calculations disclose that MO_(x)nanoclusters can be hydrated in CO_(2)saturated KHCO_(3),and the N defects of N-CNT effectively stabilize these metal hydroxyl species under carbon dioxide reduction reaction conditions,which can split the water molecules and provide local protons to inhibit the poisoning of active sites under carbon dioxide reduction reaction conditions.
基金supported by the National Natural Science Foundation of China (No. 21073131)the Shanxi Natural Science Foundation(No. 2009011011-3)
文摘V-Pd/γ-Al2O3-TiO2 catalysts with different vanadium contents were prepared by a combined sol-gel and impregnation method. X-ray diffraction (XRD), N2 adsorption-desorption (BET), X-ray photoelectron spectroscopy (XPS) and catalytic removal of ethanol, acetaldehyde and nitrogen oxides at low temperature (〈300 ?C) were used to assess the properties of the catalysts. The results showed that the sample with 1wt% vanadium exhibited an excellent catalytic performance for simultaneous removal of ethanol, acetaldehyde and nitrogen oxides. The conversions of ethanol, acetaldehyde and nitrogen oxides at 250 ?C were 100%, 74.4% and 98.7%, respectively. V-Pd/γ-Al2O3-TiO2 catalyst with 1 wt% vanadium showed the largest surface area and higher dispersion of vanadium oxide on the catalyst surface, and possessed a larger mole fraction of V4+ species and unique PdO species on the surface, which can be attributed to the strong synergistic effect among palladium, vanadium and the carriers. The higher activity of V-Pd/γ-Al2O3-TiO2 catalyst is related to the V4+ and Pd2+ species on the surface, which might be favorable for the formation of active sites.
文摘Unique MoS_(2)‐SnS_(2)heterogeneous nanoplates have successfully in‐situ grown on poly(3‐(1‐vinylimidazolium‐3‐yl)propane‐1‐sulfonate)functionalized polypyrrole/graphene oxide(PVIPS/PPy/GO).PVIPS can attract heptamolybdate ion(Mo7O246−)and Sn^(4+)as the precursors by the ion‐exchange,resulting in the simultaneous growth of 1T’‐MoS2 and the berndtite‐2T‐type hexagonal SnS_(2)by the interfacial induced effect of PVIPS.The obtained MoS_(2)‐SnS_(2)/PVIPS/PPy/GO can serve as electrocatalysts,exhibiting good NRR performance by the synergistic effect.The semi‐conducting SnS_(2)would limit the surface electron accessibility for suppressing HER process of 1T’‐MoS_(2),while metallic 1T’‐MoS_(2)might efficiently improve the NRR electroactivity of SnS_(2)by the creation of Mo‐Sn‐Sn trimer catalytic sites.Otherwise,the irreversible crystal phase transition has taken place during the NRR process.Partial 1T’‐MoS_(2)and SnS_(2)have electrochemically reacted with N_(2),and irreversibly converted into Mo^(2)N and SnxNz due to the formation of Mo−N and Sn−N bonding,meanwhile,partial SnS_(2) has been irreversibly evolved into SnS due to the reduction by the power source in the electrochemical system.It would put forward a new design idea for optimizing the preparation method and electrocatalytic activity of transition metal dichalcogenides.
文摘In order to improve the total-dose radiation har dness of the buried oxides(BOX) in the structure of separation-by-implanted-oxygen(SIMOX) silicon-on-insulator(SOI),nitrogen ions are implanted into the buried oxides with two different doses,2×10 15 and 3×10 15 cm -2 ,respectively.The experimental results show that the radiation hardness of the buried oxides is very sensitive to the doses of nitrogen implantation for a lower dose of irradiation with a Co-60 source.Despite the small difference between the doses of nitrogen implantation,the nitrogen-implanted 2×10 15 cm -2 BOX has a much higher hardness than the control sample (i.e.the buried oxide without receiving nitrogen implantation) for a total-dose irradiation of 5×104rad(Si),whereas the nitrogen-implanted 3×10 15 cm -2 BOX has a lower hardness than uhe control sample.However,this sensitivity of radiation hardness to the doses of nitrogen implantation reduces with the increasing total-dose of irradiation (from 5×104 to 5×105rad (Si)).The radiation hardness of BOX is characterized by MOS high-frequency (HF) capacitance-voltage (C-V) technique after the top silicon layers are removed.In addition,the abnormal HF C-V curve of the metal-silicon-BOX-silicon(MSOS) structure is observed and explained.
基金Project (2007CB613604) supported by the National Basic Research Program of China
文摘Ida2--H2O system(iminodiacetate aqueous solution) was used to leach a low grade zinc oxide ore for Zn extraction.The effects of leaching time,liquid-solid ratio(L/S),total concentration of Ida2-([Ida2-]T),leaching temperature and pH on Zn leaching recovery and the dissolution of impurities such as Ca,Mg,Cu,Ni,Fe,Pb and Cd were investigated.Results show that Ca,Mg and Fe in ores were hardly dissolved in alkalescent iminodiacetate aqueous solution,while valuable metals such as Cu,Ni,Pb and Cd were partly dissolved into leaching liquor with Zn.The recovery of Zn reaches 76.6% when the ores were leached for 4 h at 70 ℃ by 0.9 mol/L iminodiacetate aqueous solution with pH of 8 and L/S of 5:1.
文摘The structure and catalytic desulfurization characteristics of CeO2-TiO2 mixed oxides were investigated by means ofX-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and catalytic activity tests. According to the results, a CeO2-TiO2solid solution is formed when the mole ratio of cerium to titanium n(Ce):n(Ti) is 5:5 or greater, and the most suitable n(Ce):n(Ti) isdetermined as 7:3, over which the conversion rate of SO2 and the yield of sulfur at 500℃ reach 93% and 99%, respectively.According to the activity testing curve, Ce0.7Ti0.3O2 (n(Ce):n(Ti)=7:3) without any pretreatment can be gradually activated by reagentgas after about 10 min, and reaches a steady activation status 60 min later. The XPS results of Ce0.7Ti0.3O2 after different time ofSO2+CO reaction show that CeO2 is the active component that offers the redox couple Ce4+/Ce3+ and the labile oxygen vacancies, andTiO2 only functions as a catalyst structure stabilizer during the catalytic reaction process. After 48 h of catalytic reaction at 500℃,Ce0.7Ti0.3O2 still maintains a stable structure without being vulcanized, demonstrating its good anti-sulfur poisoning performance.
基金Project (50974138) supported by the National Natural Science Foundation of ChinaProject (2010ssxt158) supported by Graduate Student Innovation Foundation of Central South University,China
文摘The selective recovery of lead from the zinc oxide dust using an alkaline Na2EDTA solution was investigated. The effects of temperature, leaching time, Na2EDTA concentration and initial NaOH concentration on the leaching rates of lead and zinc were studied. The following optimized leaching conditions were obtained: liquid-to-solid ratio 5:1 mL/g, stirring speed 650 r/min, Na2EDTA concentration 0.12 mol/L, initial NaOH concentration 0.5 mol/L, leaching temperature 70 ℃, leaching time 120 min. Under the optimized conditions, the average leaching rates of lead, zinc, fluoride and chloride are 89.92%, 0.94%, 62.84% and 90.02%, respectively. The filtrate was used to electrowin lead powders. The average current efficiency of electrowinning is about 93% and lead content is higher than 98% under the conditions of temperature of 60 ℃, current density of 200 A/m2, H3PO4 concentration of 1.5 g/L, and lead ion concentration of above 5 g/L. The consumption of Na2EDTA and the direct current are about respectively 0.218 kg and 0.958 kW·h for per kilogram of lead powder.
基金supported by the National Natural Science Foundation of China(21277097)the Key Projects in the National Science&Technology Pillar Program during the 12th Five-Year Plan Period(2012BAJ21B01)~~
文摘Hierarchical microspheres of a graphene oxide(GO) coupled to N‐doped(BiO)2CO3 composite(N‐BOC‐GO) was synthesized by a simple hydrothermal approach. The N‐BOC‐GO composite gave enhancement in photocatalytic activity compared to the pure BOC and N‐BOC samples. With 1.0wt% GO, 62% NO removal was obtained with N‐BOC‐GO. The factors enhancing the photocatalytic performance were the high electron‐withdrawing ability and high conductivity of GO and improved visible light‐harvesting ability of N‐BOC‐GO with a 3D hierarchical architecture due to the surface scattering and reflecting(SSR) effect. An effective charge transfer from N‐BOC to GO was demonstrated by the much weakened photoluminescene intensity of the N‐BOC‐GO composite. This work highlights the potential application of GO‐based photocatalysts in air purification.
基金supported by the National Natural Science Foundation of China(21507104)the Fundamental Research Funds for the Central Universities of China
文摘Electrochemical oxidation of aniline in aqueous solution was investigated over a novel Ti/TiOxHy/Sb-SnO2 electrode prepared by the electrodeposition method.Scanning electron microscopy,X-ray diffraction,and electrochemical measurements were used to characterize its morphology,crystal structure,and electrochemical properties.Removal of aniline by the Ti/TiOxHy/Sb-SnO2electrode was investigated by ultraviolet-Visible spectroscopy and chemical oxygen demand(COD)analysis under different conditions,including current densities,initial concentrations of aniline,pH values,concentrations of chloride ions,and types of reactor.It was found that a higher current density,a lower initial concentration of aniline,an acidic solution,the presence of chloride ions(0.2wt%NaCl),and a three-dimensional(3D) reactor promoted the removal efficiency of aniline.Electrochemical degradation of aniline followed pseudo-first-order kinetics.The aniline(200 mL of 100mg·L-(-1)) and COD removal efficiencies reached 100%and 73.5%,respectively,at a current density of 20 mA·cm-(-2),pH of 7.0,and supporting electrolyte of 0.5 wt%Na2SO4 after 2 h electrolysis in a 3D reactor.These results show that aniline can be significantly removed on the Ti/TiOxHy/Sb-SnO2electrode,which provides an efficient way for elimination of aniline from aqueous solution.