In this study,a cleaner method for separation and recovery of V/W/Na in waste selective catalytic reduction(SCR)catalyst alkaline leaching solution was proposed.The method involved membrane electrolysis followed by io...In this study,a cleaner method for separation and recovery of V/W/Na in waste selective catalytic reduction(SCR)catalyst alkaline leaching solution was proposed.The method involved membrane electrolysis followed by ion morphology pretreatme nt and solvent extraction.An acidic V(Ⅴ)/W(Ⅵ)solution was obtained using the me mbrane electrolysis method without adding any other chemical reagents.In addition,Na was recovered in the form of NaOH by product,avoiding the generation of Na containing wastewater.The electrolysis parameters were investigated,the lowest power consumption of 3063 kW·h·t^(-1)NaOH was obtained at a current density of 125 A·m^(-2)and an initial NaOH concentration of 2 mol·L^(-1).After electrolysis,oxalic acid was added to the acidic V/W containing solution,converting V(Ⅴ)negative ion to V(Ⅳ)positive ion.Since W(Ⅵ)ion state remained in negative form,the generation of heteropolyacid ions(W_(x)V_(y)O_(z)^(n-))was prevented.It was found that under the condition of oxalic acid addition/theoretical consumption 1.2 and reaction temperature 75℃,100%V(Ⅴ)was co nverted to V(Ⅳ4).Using 10%N263+10%noctanol+80%sulfonated kerosene as extractant,the highest W(Ⅵ)/V(Ⅳ)separation coefficient of 7559.76was obtained at pH=1.8,O:A ratio=1:1 and extraction time 15 min.With 2 mol·L^(-1)NaOH as stripping reagent,the W stripping efficiency reached 98.50%at O:A ratio=2:1 after 4-stages of stripping.The enrichment of V remained in the solution was realized using P204 as extractant and 20%(mass)H_(2)SO_(4)as stripping reagent.The parameters of extraction/stripping process were investigated,using 10%P204+10%TBP+80%sulfonated kerosene as extractant,the V extraction efficiency reached 97.50%at O:A ratio=1:2after 4 stages of extraction.Using 20%H_(2)SO_(4)as the stripping reagent,the V stripping efficiency was 98.30%at an O:A ratio of 4:1 after five stage s of stripping.After the entire process,a high-purity VOSO_(4)and Na_(2)WO_(4)product solutions were obtained with V/W recovery efficiency 95.84%/98.50%,separately.This study examined a more effective and cleaner method for separating V/W/Na in Na_(2)WO_(4)/NaVO_(3)solution,which may serve as a reference for the separation and recovery of V/W/Na in waste SCR catalysts.展开更多
The photoinduced ligand-to-metal charge transfer(LMCT)process has been extensively investigated,however,the recovery of photocatalysts has remained a persistent challenge in the field.In light of this issue,a novel ap...The photoinduced ligand-to-metal charge transfer(LMCT)process has been extensively investigated,however,the recovery of photocatalysts has remained a persistent challenge in the field.In light of this issue,a novel approach involving the development of iron-based ionic liquids as photocatalysts has been pursued for the first time,with the goal of simultaneously facilitating the LMCT process and addressing the issue of photocatalyst recovery.Remarkably,the iron-based ionic liquid 1-butyl-3-methylimidazolium tetrachloroferrate(C_(4)mim-Fe Cl_(4))demonstrates exceptional recyclability and stability for the photocatalytic hydroacylation of olefins.This study will pave the way for new approaches to photocatalytic organic synthesis using ionic liquids as recyclable photocatalysts.展开更多
Photocatalytic overall water splitting is a promising method for producing clean hydrogen energy,but faces challenges such as low light utilization efficiency and high charge carrier recombination rates.This study dem...Photocatalytic overall water splitting is a promising method for producing clean hydrogen energy,but faces challenges such as low light utilization efficiency and high charge carrier recombination rates.This study demonstrates that dielectric Mie resonance in TiO_(2)hollow nanoshells can enhance electric field intensity and increase light absorption through resonant energy transfer,compared to crushed TiO_(2)nanoparticles.The Mie resonance effect was confirmed through fluorescence spectra,photo-response current measurements,photocatalytic water splitting experiments,and Mie calculation.The incident electricfield amplitude was doubled in hollow nanoshells,allowing for increased light trapping.Additionally,the spatially separated Pt and RuO_(2)cocatalysts on the inner and outer surfaces facilitated the separation of photoinduced electrons and holes.Pt@TiO_(2)@RuO_(2)hollow nanoshells exhibited superior photocatalytic water splitting performance,with a stable H_(2)generation rate of 50.1μmol g^(−1)h^(−1)and O_(2)evolution rate of 25.1μmol g^(−1)h^(−1),outperforming other nanostructures such as TiO_(2),Pt@TiO_(2),and TiO_(2)@RuO_(2)hollow nanoshells.This study suggests that dielectric Mie resonance and spatially-separated cocatalysts offer a new approach to simultaneously enhance light absorption and charge carrier transfer in photocatalysis.展开更多
Cu catalysts can convert CO_(2) through an electrochemical reduction reaction into a variety of useful carbon-based products.However,this capability provides an obstacle to increasing the selectivity for a single prod...Cu catalysts can convert CO_(2) through an electrochemical reduction reaction into a variety of useful carbon-based products.However,this capability provides an obstacle to increasing the selectivity for a single product.Herein,we report a simple fabrication method for a Cu-Pd alloy catalyst for use in a membrane electrode assembly(MEA)-based CO_(2) electrolyzer for the electrochemical CO_(2) reduction reaction(ECRR)with high selectivity for CO production.When the composition of the Cu-Pd alloy catalyst was fabricated at 6:4,the selectivity for CO increased and the production of multi-carbon compounds and hydrogen is suppressed.Introducing a Cu-Pd alloy catalyst with 6:4 ratio as the cathode of the MEAbased CO_(2) electrolyzer showed a CO faradaic efficiency of 92.8%at 2.4 V_(cell).We assumed that these results contributed from the crystal planes on the surface of the Cu-Pd alloy.The phases of the Cu-Pd alloy catalyst were partially separated through annealing to fabricate a catalyst with high selectivity for CO at low voltage and C_(2)H_4 at high voltage.The results of CO-stripping testing confirmed that when Cu partially separates from the lattice of the Cu-Pd alloy,the desorption of~*CO is suppressed,suggesting that C-C coupling reaction is favored.展开更多
S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB...S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.展开更多
Melamine sponge is a major concern for oil-water separation due to its lightweight,high porosity(>99%),cost-effectiveness,impressive mechanical properties,and chemical/thermal stability.However,its amphiphilic natu...Melamine sponge is a major concern for oil-water separation due to its lightweight,high porosity(>99%),cost-effectiveness,impressive mechanical properties,and chemical/thermal stability.However,its amphiphilic nature hinders selective oil absorption in water.Recent strategies to enhance hydrophobicity are reviewed,including synthetic methods and materials,with comprehensive explanations of the mechanisms driven by surface energy and roughness.Key performance indicators for MS in oil-water separation,including adsorption capacity,wettability,stability,emulsion separation,reversible wettability switching,flame retardancy,mechanical properties,and recyclability,are thoroughly discussed.In conclusion,this review provides insights into the future potential and direction of functional melamine sponges in oil-water separation.展开更多
Mineral fulvic acid(MFA)was used as an eco-friendly pyrite depressant to recover chalcopyrite by flotation with the use of the butyl xanthate as a collector.Flotation experiments showed that MFA produced a stronger in...Mineral fulvic acid(MFA)was used as an eco-friendly pyrite depressant to recover chalcopyrite by flotation with the use of the butyl xanthate as a collector.Flotation experiments showed that MFA produced a stronger inhibition effect on pyrite than on chalcopyrite.The separation of chalcopyrite from pyrite was realized by introducing 150 mg/L MFA at a pulp pH of approximately 8.0.The copper grade,copper recovery,and separation efficiency were 28.03%,84.79%,and 71.66%,respectively.Surface adsorption tests,zeta potential determinations,and localized electrochemical impedance spectroscopy tests showed that more MFA adsorbed on pyrite than on chalcopyrite,which weakened the subsequent interactions between pyrite and the collector.Atomic force microscope imaging further confirmed the adsorption of MFA on pyrite,and X-ray photoelectron spectroscopy results indicated that hydrophilic Fe-based species on the pyrite surfaces increased after exposure of pyrite to MFA,thereby decreasing the floatability of pyrite.展开更多
The pursuit of alternative fuel generation technologies has gained momentum due to the diminishing reserves of fossil fuels and global warming from increased CO_(2)emission.Among the proposed methods,the hydrogenation...The pursuit of alternative fuel generation technologies has gained momentum due to the diminishing reserves of fossil fuels and global warming from increased CO_(2)emission.Among the proposed methods,the hydrogenation of CO_(2)to produce marketable carbon-based products like methanol and ethanol is a practical approach that offers great potential to reduce CO_(2)emissions.Although significant volumes of methanol are currently produced from CO_(2),developing highly efficient and stable catalysts is crucial for further enhancing conversion and selectivity,thereby reducing process costs.An in-depth examination of the differences and similarities in the reaction pathways for methanol and ethanol production highlights the key factors that drive C-C coupling.Identifying these factors guides us toward developing more effective catalysts for ethanol synthesis.In this paper,we explore how different catalysts,through the production of various intermediates,can initiate the synthesis of methanol or ethanol.The catalytic mechanisms proposed by spectroscopic techniques and theoretical calculations,including operando X-ray methods,FTIR analysis,and DFT calculations,are summarized and presented.The following discussion explores the structural properties and composition of catalysts that influence C-C coupling and optimize the conversion rate of CO_(2)into ethanol.Lastly,the review examines recent catalysts employed for selective methanol and ethanol production,focusing on single-atom catalysts.展开更多
Comprehensive utilization of phosphogypsum(PG)has attracted much attention,especially for the recovery of rare earth elements(REEs)and gypsum due to the issues of stockpile,environmental pollution,and waste of associa...Comprehensive utilization of phosphogypsum(PG)has attracted much attention,especially for the recovery of rare earth elements(REEs)and gypsum due to the issues of stockpile,environmental pollution,and waste of associated resources.Traditional utilization methods suffered the issues of low REEs leaching efficiency,huge amount of CaSO_(4)saturated wastewater and high recovery cost.To solve these issues,this study investigated the occurrence of REEs in PG and the leaching of REEs.The results show that REEs in PG are in the forms of(1)REEs mineral inclusions,(2)REEs isomorphous substitution of Ca^(2+)in gypsum lattice,(3)dispersed soluble REEs salts.Acid leaching results demonstrate that(1)the dissolution of gypsum matrix is the control factor of REEs leaching;(2)H_(2)SO_(4)is a promising leachant considering the recycle of leachate;(3)the gypsum matrix suffers a recrystallization during the acid leaching and releases the soluble REEs from PG to aqueous solution.For the recovery of the undissolved REEs mineral inclusions,wet sieving concentrated 37.1 wt%of the REEs in a 10.7 wt%mass,increasing REEs content from 309 to 1071 ppm.Finally,a green process combining gravity separation and hydrometallurgy is proposed.This process owns the merits of wastewater free,considerable REEs recovery(about 10%increase compared with traditional processes),excellent gypsum purification(>95 wt%CaSO_(4)·2H_(2)O,with<0.06 wt%of soluble P_(2)O_(5) and<0.015 wt%of soluble F)and reagent saving(about 2/3less reagent consumption than non-cyclical leaching).展开更多
The efficient hydrogenolysis of esters to alkanes is the key protocol for producing advanced biofuels from renewable plant oils or fats.Due to the low reactivity of the carbonyl group in esters,a high reaction tempera...The efficient hydrogenolysis of esters to alkanes is the key protocol for producing advanced biofuels from renewable plant oils or fats.Due to the low reactivity of the carbonyl group in esters,a high reaction temperature(>250℃)is the prerequisite to ensure high conversion of esters.Here,we report a highly dispersed MoO_(x)-Ru/C bimetallic catalyst for the efficient hydrogenolysis of esters to alkanes under 150°C.The optimal catalyst exhibits>99%conversion of methyl stearate and 99%selectivity to diesel-range alkanes,reaching a high rate of up to 2.0 mmol gcat^(–1)h^(–1),5 times higher than that of Ru/C catalyst(MoO_(x)/C is inert).Integrated experimental and theoretical investigations attribute the high performance to the abundant MoO_(x)-Ru interfacial sites on the catalyst surface,which offers high activity for the C–O cleavage of esters.Furthermore,the dispersed MoO_(x)species significantly weaken the hydrocracking activity of the metallic Ru for C–C bonds,thus yielding alkane products without carbon loss.This study provides a facile and novel strategy for the design of high-performance heterogeneous catalysts for the hydrodeoxygenation of biomass-derived esters to alkane products.展开更多
The research,fabrication and development of piezoelectric nanofibrous materials offer effective solutions to the challenges related to energy consumption and non-renewable resources.However,enhancing their electrical ...The research,fabrication and development of piezoelectric nanofibrous materials offer effective solutions to the challenges related to energy consumption and non-renewable resources.However,enhancing their electrical output still remains a significant challenge.Here,a strategy of inducing constrained phase separation on single nanofibers via shear force was proposed.Employing electrospinning technology,a polyacrylonitrile/polyvinylidene difluoride(PAN/PVDF)nanofibrous membrane was fabricated in one step,which enabled simultaneous piezoelectric and triboelectric conversion within a single-layer membrane.Each nanofiber contained independent components of PAN and PVDF and exhibited a rough surface.The abundant frictional contact points formed between these heterogeneous components contributed to an enhanced endogenous triboelectric output,showcasing an excellent synergistic effect of piezoelectric and triboelectric response in the nanofibrous membrane.Additionally,the component mass ratio influenced the microstructure,piezoelectric conformation and piezoelectric performance of the PAN/PVDF nanofibrous membranes.Through comprehensive performance comparison,the optimal mass ratio of PAN to PVDF was determined to be 9∶1.The piezoelectric devices made of the optimal PAN/PVDF nanofibrous membranes with rough nanofiber surfaces generated an output voltage of 20 V,which was about 1.8 times that of the smooth one at the same component mass ratio.The strategy of constrained phase separation on the surface of individual nanofibers provides a new approach to enhance the output performance of single-layer piezoelectric nanofibrous materials.展开更多
To improve the catalytic performance of La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3)(LSCF)towards carbon soot,we utilized the impregnation method to incorporate Ag into the prepared LSCF catalyst.We conducted a series of cha...To improve the catalytic performance of La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3)(LSCF)towards carbon soot,we utilized the impregnation method to incorporate Ag into the prepared LSCF catalyst.We conducted a series of characterization tests and evaluated the soot catalytic activity of the composite catalyst by comparing it with the LaCoO_(3) group,LaFeO_(3) group,and catalyst-free group.The results indicate that the Ag-LSCF composite catalyst exhibits the highest soot catalytic activity,with the characteristic temperature values of 376.3,431.1,and 473.9℃at 10%,50%,and 90%carbon soot conversion,respectively.These values are 24.8,20.2,and 23.1℃lower than those of the LSCF group.This also shows that LSCF can improve the catalytic activity of soot after compounding with Ag,and reflects the necessity of using catalysts in soot combustion reaction.XPS characterization and BET test show that Ag-LSCF has more abundant surface-adsorbed oxygen species,larger specific surface area and pore volume than LSCF,which also proves that Ag-LSCF has higher soot catalytic activity.展开更多
Membrane technology holds significant potential for augmenting or partially substituting conventional separation techniques,such as heatdriven distillation,thereby reducing energy consumption.Organic solvent nanofiltr...Membrane technology holds significant potential for augmenting or partially substituting conventional separation techniques,such as heatdriven distillation,thereby reducing energy consumption.Organic solvent nanofiltration represents an advanced membrane separation technology capable of discerning molecules within a molecular weight range of approximately 100-1000 Da in organic solvents,offering low energy requirements and minimal carbon footprints.Molecular separation in non-polar solvent system,such as toluene,n-hexane,and n-heptane,has gained paramount importance due to their extensive use in the pharmaceutical,biochemical,and petrochemical industries.In this review,we presented recent advancements in membrane materials,membrane fabrication techniques and their promising applications for separation in nonpolar solvent system,encompassing hydrocarbon separation,bioactive molecule purification and organic solvent recovery.Furthermore,this review highlighted the challenges and opportunities associated with membrane scale-up strategies and the direct translation of this promising technology into industrial applications.展开更多
Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-perform...Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.展开更多
NH_(3)-SCR(SCR:Selective catalytic reduction)is an effective technology for the de-NO_(x)process from both mobile and stationary pollution sources,and the most commonly used catalysts are the vanadia-based catalysts.A...NH_(3)-SCR(SCR:Selective catalytic reduction)is an effective technology for the de-NO_(x)process from both mobile and stationary pollution sources,and the most commonly used catalysts are the vanadia-based catalysts.An innovative V_(2)O_(5)-CeO_(2)/TaTiO_(x)catalyst for NO_(x)removal was prepared in this study.The influences of Ce and Ta in the V_(2)O_(5)-CeO_(2)/TaTiO_(x)catalyst on the SCR performance and physicochemical properties were investigated.The V_(2)O_(5)-CeO_(2)/TaTiO_(x)catalyst not only exhibited excellent SCR activity in a wide temperature window,but also presented strong resistance to H_(2)Oand SO_(2)at 275◦C.A series of characterizationmethods was used to study the catalysts,including H2-temperature programmed reduction,X-ray photoelectron spectroscopy,NH_(3)-temperature programmed desorption,etc.It was discovered that a synergistic effect existed between Ce and Ta species.The introduction of Ce and Ta enlarged the specific surface area,increased the amount of acid sites and the ratio of Ce^(3+),(V^(3+)+V^(4+))and Oα,and strengthened the redox capability which were related to synergistic effect between Ce and Ta species,significantly improving the NH_(3)-SCR activity.展开更多
Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3...Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.展开更多
Separating oil/water mixtures via superhydrophobic stainless steel mesh(SSM)is a kind of efficient methods of treating oily wastewater,and the superhydrophobic SSM with a low cost,simple fabrication process and robust...Separating oil/water mixtures via superhydrophobic stainless steel mesh(SSM)is a kind of efficient methods of treating oily wastewater,and the superhydrophobic SSM with a low cost,simple fabrication process and robust usability remains a challenge.Herein,urushiol-based benzoxazine(U-D)with a strong substrate adhesion and low surface free energy was used to anchor SiO_(2) particles on the SSM surface to obtain a durable superhydrophobic SSM(PU-D/SiO_(2)/SSM)through a simple dip-coating process,meanwhile,epoxy resin was also introduced to further improve the adhesion between coating and SSM.PU-D/SiO_(2)/SSM could successfully separate various immiscible oil-water mixtures with a separation efficiency of over 96%and a flux up to 27100 L/m^(2) h only by gravity,respectively.Especially,the modified SSM could effectively remove water from water-in-oil emulsion with a separation efficiency of 99.7%.Moreover,PU-D/SiO_(2)/SSM had an outstanding reusability,whose water contact angle and separation efficiency only slightly decreased after 20 cycles of separating oil/water mixture.In addition,the modified SSM also displayed a satisfactory abrasion resistance,chemical stability and self-cleaning property.Thereby,the robust PU-D/SiO_(2)/SSM prepared by cheap raw materials and facile dip-coating method exhibits a high potential for separating oil/water mixtures.展开更多
Solvent extraction,a separation and purification technology,is crucial in critical metal metallurgy.Organic solvents commonly used in solvent extraction exhibit disadvantages,such as high volatility,high toxicity,and ...Solvent extraction,a separation and purification technology,is crucial in critical metal metallurgy.Organic solvents commonly used in solvent extraction exhibit disadvantages,such as high volatility,high toxicity,and flammability,causing a spectrum of hazards to human health and environmental safety.Neoteric solvents have been recognized as potential alternatives to these harmful organic solvents.In the past two decades,several neoteric solvents have been proposed,including ionic liquids(ILs)and deep eutectic solvents(DESs).DESs have gradually become the focus of green solvents owing to several advantages,namely,low toxicity,degradability,and low cost.In this critical review,their classification,formation mechanisms,preparation methods,characterization technologies,and special physicochemical properties based on the most recent advancements in research have been systematically described.Subsequently,the major separation and purification applications of DESs in critical metal metallurgy were comprehensively summarized.Finally,future opportunities and challenges of DESs were explored in the current research area.In conclusion,this review provides valuable insights for improving our overall understanding of DESs,and it holds important potential for expanding separation and purification applications in critical metal metallurgy.展开更多
We report a robust pillar-layered metal-organic framework,Zn‑tfbdc‑dabco(tfbdc:tetrafluoroterephthal-ate,dabco:1,4-diazabicyclo[2.2.2]octane),featuring the fluorinated pore environment,for the preferential binding of ...We report a robust pillar-layered metal-organic framework,Zn‑tfbdc‑dabco(tfbdc:tetrafluoroterephthal-ate,dabco:1,4-diazabicyclo[2.2.2]octane),featuring the fluorinated pore environment,for the preferential binding of propane over propylene and thus highly inverse selective separation of propane/propylene mixture.The inverse propane-selective performance of Zn‑tfbdc‑dabco for the propane/propylene separation was validated by single-component gas adsorption isotherms,isosteric enthalpy of adsorption calculations,ideal adsorbed solution theory calculations,along with the breakthrough experiment.The customized fluorinated networks served as a propane-trap to form more interactions with the exposed hydrogen atoms of propane,as unveiled by the simulation studies at the molecular level.With the advantage of inverse propane-selective adsorption behavior,high adsorption capacity,good cycling stability,and low isosteric enthalpy of adsorption,Zn‑tfbdc‑dabco can be a promising candidate adsorbent for the challenging propane/propylene separation to realize one-step purification of the target propylene substance.展开更多
Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal int...Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal into NiFe-based catalysts to construct asymmetrical M-NiFe units,the d-orbital and electronic structures can be adjusted,which is an important strategy to achieve sufficient oxygen evolution reaction(OER)performance in AEMWEs.Herein,the ternary NiFeM(M:La,Mo)catalysts featured with distinct M-NiFe units and varying d-orbitals are reported in this work.Experimental and theoretical calculation results reveal that the doping of La leads to optimized hybridization between d orbital in NiFeM and 2p in oxygen,resulting in enhanced adsorption strength of oxygen intermediates,and reduced rate-determining step energy barrier,which is responsible for the enhanced OER performance.More critically,the obtained NiFeLa catalyst only requires 1.58 V to reach 1 A cm^(−2) in an anion exchange membrane electrolyzer and demonstrates excellent long-term stability of up to 600 h.展开更多
基金the support the National Natural Science Foundation of China(5210440)S&T Program of Hebei(23311501D)Program of HBIS Group under HG2023222。
文摘In this study,a cleaner method for separation and recovery of V/W/Na in waste selective catalytic reduction(SCR)catalyst alkaline leaching solution was proposed.The method involved membrane electrolysis followed by ion morphology pretreatme nt and solvent extraction.An acidic V(Ⅴ)/W(Ⅵ)solution was obtained using the me mbrane electrolysis method without adding any other chemical reagents.In addition,Na was recovered in the form of NaOH by product,avoiding the generation of Na containing wastewater.The electrolysis parameters were investigated,the lowest power consumption of 3063 kW·h·t^(-1)NaOH was obtained at a current density of 125 A·m^(-2)and an initial NaOH concentration of 2 mol·L^(-1).After electrolysis,oxalic acid was added to the acidic V/W containing solution,converting V(Ⅴ)negative ion to V(Ⅳ)positive ion.Since W(Ⅵ)ion state remained in negative form,the generation of heteropolyacid ions(W_(x)V_(y)O_(z)^(n-))was prevented.It was found that under the condition of oxalic acid addition/theoretical consumption 1.2 and reaction temperature 75℃,100%V(Ⅴ)was co nverted to V(Ⅳ4).Using 10%N263+10%noctanol+80%sulfonated kerosene as extractant,the highest W(Ⅵ)/V(Ⅳ)separation coefficient of 7559.76was obtained at pH=1.8,O:A ratio=1:1 and extraction time 15 min.With 2 mol·L^(-1)NaOH as stripping reagent,the W stripping efficiency reached 98.50%at O:A ratio=2:1 after 4-stages of stripping.The enrichment of V remained in the solution was realized using P204 as extractant and 20%(mass)H_(2)SO_(4)as stripping reagent.The parameters of extraction/stripping process were investigated,using 10%P204+10%TBP+80%sulfonated kerosene as extractant,the V extraction efficiency reached 97.50%at O:A ratio=1:2after 4 stages of extraction.Using 20%H_(2)SO_(4)as the stripping reagent,the V stripping efficiency was 98.30%at an O:A ratio of 4:1 after five stage s of stripping.After the entire process,a high-purity VOSO_(4)and Na_(2)WO_(4)product solutions were obtained with V/W recovery efficiency 95.84%/98.50%,separately.This study examined a more effective and cleaner method for separating V/W/Na in Na_(2)WO_(4)/NaVO_(3)solution,which may serve as a reference for the separation and recovery of V/W/Na in waste SCR catalysts.
基金financial support from the National Natural Science Foundation of China(Nos.22071222,22171249)the Natural Science Foundation of Henan Province(Nos.232300421363,242300420526)+2 种基金Key Research Projects of Universities in Henan Province(No.23A180010)Science&Technology Innovation Talents in Universities of Henan Province(No.23HASTIT003)Science and Technology Research and Development Plan Joint Fund of Henan Province(No.242301420006)。
文摘The photoinduced ligand-to-metal charge transfer(LMCT)process has been extensively investigated,however,the recovery of photocatalysts has remained a persistent challenge in the field.In light of this issue,a novel approach involving the development of iron-based ionic liquids as photocatalysts has been pursued for the first time,with the goal of simultaneously facilitating the LMCT process and addressing the issue of photocatalyst recovery.Remarkably,the iron-based ionic liquid 1-butyl-3-methylimidazolium tetrachloroferrate(C_(4)mim-Fe Cl_(4))demonstrates exceptional recyclability and stability for the photocatalytic hydroacylation of olefins.This study will pave the way for new approaches to photocatalytic organic synthesis using ionic liquids as recyclable photocatalysts.
基金supported by the National Natural Science Foundation of China(Nos.51702023,62274017)Natural Science Foundation of Jiangsu Province(No.BK20231224)China Postdoctoral Science Foundation(No.2022M711138).
文摘Photocatalytic overall water splitting is a promising method for producing clean hydrogen energy,but faces challenges such as low light utilization efficiency and high charge carrier recombination rates.This study demonstrates that dielectric Mie resonance in TiO_(2)hollow nanoshells can enhance electric field intensity and increase light absorption through resonant energy transfer,compared to crushed TiO_(2)nanoparticles.The Mie resonance effect was confirmed through fluorescence spectra,photo-response current measurements,photocatalytic water splitting experiments,and Mie calculation.The incident electricfield amplitude was doubled in hollow nanoshells,allowing for increased light trapping.Additionally,the spatially separated Pt and RuO_(2)cocatalysts on the inner and outer surfaces facilitated the separation of photoinduced electrons and holes.Pt@TiO_(2)@RuO_(2)hollow nanoshells exhibited superior photocatalytic water splitting performance,with a stable H_(2)generation rate of 50.1μmol g^(−1)h^(−1)and O_(2)evolution rate of 25.1μmol g^(−1)h^(−1),outperforming other nanostructures such as TiO_(2),Pt@TiO_(2),and TiO_(2)@RuO_(2)hollow nanoshells.This study suggests that dielectric Mie resonance and spatially-separated cocatalysts offer a new approach to simultaneously enhance light absorption and charge carrier transfer in photocatalysis.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government MSIT(2021R1A2C2093358,2021R1A4A3027878,2022M3I3A1081901)financial support from the Lotte Chemical Company。
文摘Cu catalysts can convert CO_(2) through an electrochemical reduction reaction into a variety of useful carbon-based products.However,this capability provides an obstacle to increasing the selectivity for a single product.Herein,we report a simple fabrication method for a Cu-Pd alloy catalyst for use in a membrane electrode assembly(MEA)-based CO_(2) electrolyzer for the electrochemical CO_(2) reduction reaction(ECRR)with high selectivity for CO production.When the composition of the Cu-Pd alloy catalyst was fabricated at 6:4,the selectivity for CO increased and the production of multi-carbon compounds and hydrogen is suppressed.Introducing a Cu-Pd alloy catalyst with 6:4 ratio as the cathode of the MEAbased CO_(2) electrolyzer showed a CO faradaic efficiency of 92.8%at 2.4 V_(cell).We assumed that these results contributed from the crystal planes on the surface of the Cu-Pd alloy.The phases of the Cu-Pd alloy catalyst were partially separated through annealing to fabricate a catalyst with high selectivity for CO at low voltage and C_(2)H_4 at high voltage.The results of CO-stripping testing confirmed that when Cu partially separates from the lattice of the Cu-Pd alloy,the desorption of~*CO is suppressed,suggesting that C-C coupling reaction is favored.
基金financially supported by the National Natural Science Foundation of China(Nos.51602018 and 51902018)the Natural Science Foundation of Beijing Municipality(No.2154052)+3 种基金the China Postdoctoral Science Foundation(No.2014M560044)the Fundamental Research Funds for the Central Universities(No.FRF-MP-20-22)USTB Research Center for International People-to-people Exchange in Science,Technology and Civilization(No.2022KFYB007)Education and Teaching Reform Foundation at University of Science and Technology Beijing(Nos.2023JGC027,KC2022QYW06,and KC2022TS09)。
文摘S and Co co-doped carbon catalysts were prepared via pyrolysis of MOF-71 and thiourea mixtures at 800℃at a mass ratio of MOF-71 to thiourea of 1:0.1 to effectively activate peroxymonosulfate(PMS)for methylene blue(MB)degradation.The effects of two different mixing routes were identified on the MB degradation performance.Particularly,the catalyst obtained by the alcohol solvent evaporation(MOF-AEP)mixing route could degrade 95.60%MB(50 mg/L)within 4 min(degradation rate:K=0.78 min^(-1)),which was faster than that derived from the direct grinding method(MOF-DGP,80.97%,K=0.39 min^(-1)).X-ray photoelectron spectroscopy revealed that the Co-S content of MOF-AEP(43.39at%)was less than that of MOF-DGP(54.73at%),and the proportion of C-S-C in MOF-AEP(13.56at%)was higher than that of MOF-DGP(10.67at%).Density functional theory calculations revealed that the adsorption energy of Co for PMS was -2.94 eV when sulfur was doped as C-S-C on the carbon skeleton,which was higher than that when sulfur was doped next to cobalt in the form of Co-S bond(-2.86 eV).Thus,the C-S-C sites might provide more contributions to activate PMS compared with Co-S.Furthermore,the degradation parameters,including pH and MOF-AEP dosage,were investigated.Finally,radical quenching experiments and electron paramagnetic resonance(EPR)measurements revealed that ^(1)O_(2)might be the primary catalytic species,whereas·O~(2-)might be the secondary one in degrading MB.
基金supported by the National Natural Science Foundation of China(Nos.52372093 and 52102145)the Key R&D Program of Shaanxi Province(Nos.2023GXLH-045 and 2022SF-168)+4 种基金the Xi’an Programs for Science and Technology Plan(Nos.2020KJRC0090 and 21XJZZ0045)the Opening Project of Shanxi Key Laboratory of Advanced Manufacturing Technology(No.XJZZ202001)the Xi’an Municipal Bureau of Science and Technology(No.21XJZZ0054)the Open Foundation of Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry,Ministry of Education,Shaanxi University of Science and Technology(No.KFKT2021-01)the Shaanxi Collaborative Innovation Center of Industrial Auxiliary Chemistry and Technology,Shaanxi University of Science and Technology(No.KFKT2021-01).
文摘Melamine sponge is a major concern for oil-water separation due to its lightweight,high porosity(>99%),cost-effectiveness,impressive mechanical properties,and chemical/thermal stability.However,its amphiphilic nature hinders selective oil absorption in water.Recent strategies to enhance hydrophobicity are reviewed,including synthetic methods and materials,with comprehensive explanations of the mechanisms driven by surface energy and roughness.Key performance indicators for MS in oil-water separation,including adsorption capacity,wettability,stability,emulsion separation,reversible wettability switching,flame retardancy,mechanical properties,and recyclability,are thoroughly discussed.In conclusion,this review provides insights into the future potential and direction of functional melamine sponges in oil-water separation.
基金supported by Fundamental Research Projects of Yunnan Province,China(Nos.202101BE070001-009,202301AU070189).
文摘Mineral fulvic acid(MFA)was used as an eco-friendly pyrite depressant to recover chalcopyrite by flotation with the use of the butyl xanthate as a collector.Flotation experiments showed that MFA produced a stronger inhibition effect on pyrite than on chalcopyrite.The separation of chalcopyrite from pyrite was realized by introducing 150 mg/L MFA at a pulp pH of approximately 8.0.The copper grade,copper recovery,and separation efficiency were 28.03%,84.79%,and 71.66%,respectively.Surface adsorption tests,zeta potential determinations,and localized electrochemical impedance spectroscopy tests showed that more MFA adsorbed on pyrite than on chalcopyrite,which weakened the subsequent interactions between pyrite and the collector.Atomic force microscope imaging further confirmed the adsorption of MFA on pyrite,and X-ray photoelectron spectroscopy results indicated that hydrophilic Fe-based species on the pyrite surfaces increased after exposure of pyrite to MFA,thereby decreasing the floatability of pyrite.
基金the Canadian NRCan OERD Energy Innovation Programthe Natural Sciences and Engineering Research Council of Canada,and the Carbon Solution Program for their financial support.
文摘The pursuit of alternative fuel generation technologies has gained momentum due to the diminishing reserves of fossil fuels and global warming from increased CO_(2)emission.Among the proposed methods,the hydrogenation of CO_(2)to produce marketable carbon-based products like methanol and ethanol is a practical approach that offers great potential to reduce CO_(2)emissions.Although significant volumes of methanol are currently produced from CO_(2),developing highly efficient and stable catalysts is crucial for further enhancing conversion and selectivity,thereby reducing process costs.An in-depth examination of the differences and similarities in the reaction pathways for methanol and ethanol production highlights the key factors that drive C-C coupling.Identifying these factors guides us toward developing more effective catalysts for ethanol synthesis.In this paper,we explore how different catalysts,through the production of various intermediates,can initiate the synthesis of methanol or ethanol.The catalytic mechanisms proposed by spectroscopic techniques and theoretical calculations,including operando X-ray methods,FTIR analysis,and DFT calculations,are summarized and presented.The following discussion explores the structural properties and composition of catalysts that influence C-C coupling and optimize the conversion rate of CO_(2)into ethanol.Lastly,the review examines recent catalysts employed for selective methanol and ethanol production,focusing on single-atom catalysts.
基金Project supported by the National Natural Science Foundation of China(52104354)the National Natural Science Foundation of China(51674036)+1 种基金Joint Fund for Nuclear Technology Innovation Sponsored by the National Natural Science Foundation of Chinathe China National Nuclear Corporation(U2067201)。
文摘Comprehensive utilization of phosphogypsum(PG)has attracted much attention,especially for the recovery of rare earth elements(REEs)and gypsum due to the issues of stockpile,environmental pollution,and waste of associated resources.Traditional utilization methods suffered the issues of low REEs leaching efficiency,huge amount of CaSO_(4)saturated wastewater and high recovery cost.To solve these issues,this study investigated the occurrence of REEs in PG and the leaching of REEs.The results show that REEs in PG are in the forms of(1)REEs mineral inclusions,(2)REEs isomorphous substitution of Ca^(2+)in gypsum lattice,(3)dispersed soluble REEs salts.Acid leaching results demonstrate that(1)the dissolution of gypsum matrix is the control factor of REEs leaching;(2)H_(2)SO_(4)is a promising leachant considering the recycle of leachate;(3)the gypsum matrix suffers a recrystallization during the acid leaching and releases the soluble REEs from PG to aqueous solution.For the recovery of the undissolved REEs mineral inclusions,wet sieving concentrated 37.1 wt%of the REEs in a 10.7 wt%mass,increasing REEs content from 309 to 1071 ppm.Finally,a green process combining gravity separation and hydrometallurgy is proposed.This process owns the merits of wastewater free,considerable REEs recovery(about 10%increase compared with traditional processes),excellent gypsum purification(>95 wt%CaSO_(4)·2H_(2)O,with<0.06 wt%of soluble P_(2)O_(5) and<0.015 wt%of soluble F)and reagent saving(about 2/3less reagent consumption than non-cyclical leaching).
文摘The efficient hydrogenolysis of esters to alkanes is the key protocol for producing advanced biofuels from renewable plant oils or fats.Due to the low reactivity of the carbonyl group in esters,a high reaction temperature(>250℃)is the prerequisite to ensure high conversion of esters.Here,we report a highly dispersed MoO_(x)-Ru/C bimetallic catalyst for the efficient hydrogenolysis of esters to alkanes under 150°C.The optimal catalyst exhibits>99%conversion of methyl stearate and 99%selectivity to diesel-range alkanes,reaching a high rate of up to 2.0 mmol gcat^(–1)h^(–1),5 times higher than that of Ru/C catalyst(MoO_(x)/C is inert).Integrated experimental and theoretical investigations attribute the high performance to the abundant MoO_(x)-Ru interfacial sites on the catalyst surface,which offers high activity for the C–O cleavage of esters.Furthermore,the dispersed MoO_(x)species significantly weaken the hydrocracking activity of the metallic Ru for C–C bonds,thus yielding alkane products without carbon loss.This study provides a facile and novel strategy for the design of high-performance heterogeneous catalysts for the hydrodeoxygenation of biomass-derived esters to alkane products.
基金National Natural Science Foundation of China(No.52373281)National Energy-Saving and Low-Carbon Materials Production and Application Demonstration Platform Program,China(No.TC220H06N)。
文摘The research,fabrication and development of piezoelectric nanofibrous materials offer effective solutions to the challenges related to energy consumption and non-renewable resources.However,enhancing their electrical output still remains a significant challenge.Here,a strategy of inducing constrained phase separation on single nanofibers via shear force was proposed.Employing electrospinning technology,a polyacrylonitrile/polyvinylidene difluoride(PAN/PVDF)nanofibrous membrane was fabricated in one step,which enabled simultaneous piezoelectric and triboelectric conversion within a single-layer membrane.Each nanofiber contained independent components of PAN and PVDF and exhibited a rough surface.The abundant frictional contact points formed between these heterogeneous components contributed to an enhanced endogenous triboelectric output,showcasing an excellent synergistic effect of piezoelectric and triboelectric response in the nanofibrous membrane.Additionally,the component mass ratio influenced the microstructure,piezoelectric conformation and piezoelectric performance of the PAN/PVDF nanofibrous membranes.Through comprehensive performance comparison,the optimal mass ratio of PAN to PVDF was determined to be 9∶1.The piezoelectric devices made of the optimal PAN/PVDF nanofibrous membranes with rough nanofiber surfaces generated an output voltage of 20 V,which was about 1.8 times that of the smooth one at the same component mass ratio.The strategy of constrained phase separation on the surface of individual nanofibers provides a new approach to enhance the output performance of single-layer piezoelectric nanofibrous materials.
文摘To improve the catalytic performance of La_(0.6)Sr_(0.4)Co_(0.2)Fe_(0.8)O_(3)(LSCF)towards carbon soot,we utilized the impregnation method to incorporate Ag into the prepared LSCF catalyst.We conducted a series of characterization tests and evaluated the soot catalytic activity of the composite catalyst by comparing it with the LaCoO_(3) group,LaFeO_(3) group,and catalyst-free group.The results indicate that the Ag-LSCF composite catalyst exhibits the highest soot catalytic activity,with the characteristic temperature values of 376.3,431.1,and 473.9℃at 10%,50%,and 90%carbon soot conversion,respectively.These values are 24.8,20.2,and 23.1℃lower than those of the LSCF group.This also shows that LSCF can improve the catalytic activity of soot after compounding with Ag,and reflects the necessity of using catalysts in soot combustion reaction.XPS characterization and BET test show that Ag-LSCF has more abundant surface-adsorbed oxygen species,larger specific surface area and pore volume than LSCF,which also proves that Ag-LSCF has higher soot catalytic activity.
基金supported by the National Natural Science Foundation of China(Grant No.2230081973)Shanghai Pilot Program for Basic Research(22TQ1400100-4).
文摘Membrane technology holds significant potential for augmenting or partially substituting conventional separation techniques,such as heatdriven distillation,thereby reducing energy consumption.Organic solvent nanofiltration represents an advanced membrane separation technology capable of discerning molecules within a molecular weight range of approximately 100-1000 Da in organic solvents,offering low energy requirements and minimal carbon footprints.Molecular separation in non-polar solvent system,such as toluene,n-hexane,and n-heptane,has gained paramount importance due to their extensive use in the pharmaceutical,biochemical,and petrochemical industries.In this review,we presented recent advancements in membrane materials,membrane fabrication techniques and their promising applications for separation in nonpolar solvent system,encompassing hydrocarbon separation,bioactive molecule purification and organic solvent recovery.Furthermore,this review highlighted the challenges and opportunities associated with membrane scale-up strategies and the direct translation of this promising technology into industrial applications.
基金supported by the National Natural Science Foundation of China(No.21571062)the Program for Professor of Special Appointment(Eastern Scholar)at the Shanghai Institutions of Higher Learning to JGL,and the Fundamental Research Funds for the Central Universities(No.222201717003)。
文摘Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.
基金supported by the National Natural Science Foundation of China(Nos.22276182 and 22188102)the Natural Science Foundation of Fujian Province,China(No.2023J06048)the Youth Innovation Promotion Association of Chinese Academy of Sciences(No.2021303).
文摘NH_(3)-SCR(SCR:Selective catalytic reduction)is an effective technology for the de-NO_(x)process from both mobile and stationary pollution sources,and the most commonly used catalysts are the vanadia-based catalysts.An innovative V_(2)O_(5)-CeO_(2)/TaTiO_(x)catalyst for NO_(x)removal was prepared in this study.The influences of Ce and Ta in the V_(2)O_(5)-CeO_(2)/TaTiO_(x)catalyst on the SCR performance and physicochemical properties were investigated.The V_(2)O_(5)-CeO_(2)/TaTiO_(x)catalyst not only exhibited excellent SCR activity in a wide temperature window,but also presented strong resistance to H_(2)Oand SO_(2)at 275◦C.A series of characterizationmethods was used to study the catalysts,including H2-temperature programmed reduction,X-ray photoelectron spectroscopy,NH_(3)-temperature programmed desorption,etc.It was discovered that a synergistic effect existed between Ce and Ta species.The introduction of Ce and Ta enlarged the specific surface area,increased the amount of acid sites and the ratio of Ce^(3+),(V^(3+)+V^(4+))and Oα,and strengthened the redox capability which were related to synergistic effect between Ce and Ta species,significantly improving the NH_(3)-SCR activity.
基金Research Institute for Smart Energy(CDB2)the grant from the Research Institute for Advanced Manufacturing(CD8Z)+4 种基金the grant from the Carbon Neutrality Funding Scheme(WZ2R)at The Hong Kong Polytechnic Universitysupport from the Hong Kong Polytechnic University(CD9B,CDBZ and WZ4Q)the National Natural Science Foundation of China(22205187)Shenzhen Municipal Science and Technology Innovation Commission(JCYJ20230807140402006)Start-up Foundation for Introducing Talent of NUIST and Natural Science Foundation of Jiangsu Province of China(BK20230426).
文摘Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.
基金Funded by the National Natural Science Foundation of China(No.22165019)。
文摘Separating oil/water mixtures via superhydrophobic stainless steel mesh(SSM)is a kind of efficient methods of treating oily wastewater,and the superhydrophobic SSM with a low cost,simple fabrication process and robust usability remains a challenge.Herein,urushiol-based benzoxazine(U-D)with a strong substrate adhesion and low surface free energy was used to anchor SiO_(2) particles on the SSM surface to obtain a durable superhydrophobic SSM(PU-D/SiO_(2)/SSM)through a simple dip-coating process,meanwhile,epoxy resin was also introduced to further improve the adhesion between coating and SSM.PU-D/SiO_(2)/SSM could successfully separate various immiscible oil-water mixtures with a separation efficiency of over 96%and a flux up to 27100 L/m^(2) h only by gravity,respectively.Especially,the modified SSM could effectively remove water from water-in-oil emulsion with a separation efficiency of 99.7%.Moreover,PU-D/SiO_(2)/SSM had an outstanding reusability,whose water contact angle and separation efficiency only slightly decreased after 20 cycles of separating oil/water mixture.In addition,the modified SSM also displayed a satisfactory abrasion resistance,chemical stability and self-cleaning property.Thereby,the robust PU-D/SiO_(2)/SSM prepared by cheap raw materials and facile dip-coating method exhibits a high potential for separating oil/water mixtures.
基金financially supported by the Original Exploration Project of the National Natural Science Foundation of China(No.52150079)the National Natural Science Foundation of China(Nos.U22A20130,U2004215,and 51974280)+1 种基金the Natural Science Foundation of Henan Province of China(No.232300421196)the Project of Zhongyuan Critical Metals Laboratory of China(Nos.GJJSGFYQ202304,GJJSGFJQ202306,GJJSGFYQ202323,GJJSGFYQ202308,and GJJSGFYQ202307)。
文摘Solvent extraction,a separation and purification technology,is crucial in critical metal metallurgy.Organic solvents commonly used in solvent extraction exhibit disadvantages,such as high volatility,high toxicity,and flammability,causing a spectrum of hazards to human health and environmental safety.Neoteric solvents have been recognized as potential alternatives to these harmful organic solvents.In the past two decades,several neoteric solvents have been proposed,including ionic liquids(ILs)and deep eutectic solvents(DESs).DESs have gradually become the focus of green solvents owing to several advantages,namely,low toxicity,degradability,and low cost.In this critical review,their classification,formation mechanisms,preparation methods,characterization technologies,and special physicochemical properties based on the most recent advancements in research have been systematically described.Subsequently,the major separation and purification applications of DESs in critical metal metallurgy were comprehensively summarized.Finally,future opportunities and challenges of DESs were explored in the current research area.In conclusion,this review provides valuable insights for improving our overall understanding of DESs,and it holds important potential for expanding separation and purification applications in critical metal metallurgy.
文摘We report a robust pillar-layered metal-organic framework,Zn‑tfbdc‑dabco(tfbdc:tetrafluoroterephthal-ate,dabco:1,4-diazabicyclo[2.2.2]octane),featuring the fluorinated pore environment,for the preferential binding of propane over propylene and thus highly inverse selective separation of propane/propylene mixture.The inverse propane-selective performance of Zn‑tfbdc‑dabco for the propane/propylene separation was validated by single-component gas adsorption isotherms,isosteric enthalpy of adsorption calculations,ideal adsorbed solution theory calculations,along with the breakthrough experiment.The customized fluorinated networks served as a propane-trap to form more interactions with the exposed hydrogen atoms of propane,as unveiled by the simulation studies at the molecular level.With the advantage of inverse propane-selective adsorption behavior,high adsorption capacity,good cycling stability,and low isosteric enthalpy of adsorption,Zn‑tfbdc‑dabco can be a promising candidate adsorbent for the challenging propane/propylene separation to realize one-step purification of the target propylene substance.
基金financially supported by the National Natural Science Foundation of China(22309137,22279095)Open subject project State Key Laboratory of New Textile Materials and Advanced Processing Technologies(FZ2023001).
文摘Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal into NiFe-based catalysts to construct asymmetrical M-NiFe units,the d-orbital and electronic structures can be adjusted,which is an important strategy to achieve sufficient oxygen evolution reaction(OER)performance in AEMWEs.Herein,the ternary NiFeM(M:La,Mo)catalysts featured with distinct M-NiFe units and varying d-orbitals are reported in this work.Experimental and theoretical calculation results reveal that the doping of La leads to optimized hybridization between d orbital in NiFeM and 2p in oxygen,resulting in enhanced adsorption strength of oxygen intermediates,and reduced rate-determining step energy barrier,which is responsible for the enhanced OER performance.More critically,the obtained NiFeLa catalyst only requires 1.58 V to reach 1 A cm^(−2) in an anion exchange membrane electrolyzer and demonstrates excellent long-term stability of up to 600 h.
