To explore the denitration mechanism of iron-vanadium/activated carbon(Fe-V/AC)catalysts in ammonia-selective catalytic reduction(NH_(3)-SCR),the physicochemical properties of Fe-V/AC catalysts were characterized.The ...To explore the denitration mechanism of iron-vanadium/activated carbon(Fe-V/AC)catalysts in ammonia-selective catalytic reduction(NH_(3)-SCR),the physicochemical properties of Fe-V/AC catalysts were characterized.The denitration activities of the Fe-V/AC catalysts in the range of 150-300℃ were evaluated.The increase in denitration temperature leads to the highest and fastest recovery rate of NO conversion in the 10Fe-15V/AC catalyst.However,more metal oxides were attached to the catalyst surface as the V loading increased,and the accumulation occurred.The surface-active components are FeO,Fe_(2)O_(3),Fe_(3)O_(4),VO_(2),and V_(2)O_(5).In addition,the increase in the V loading induced a series of modification effects.A large amount of Fe^(3+)was reduced to Fe^(2+),and a large amount of V^(4+)was oxidized to V^(5+).The surface oxygen species(O_(α))were transformed into lattice oxygen(O_(β)).The presence of a large amount of V species deteriorated the pore-structure parameters and destroyed the oxygen-containing functional groups.Increasing the V loading can effectively increase the Lewis acid sites,thereby promoting NH_(3) adsorption and NO reduction and increasing the stretching vibration of weakly adsorbed ammonia species on the catalyst.The NH_(3) adsorption process produces a notable increase in the concentration of monodentate nitrite(NH_(4)^(+)).The NH_(3)-SCR denitration mechanism of the Fe-V/AC catalyst includes reaction gas adsorption,catalytic denitration of metal active components,and gas desorption.展开更多
To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content ...To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content in coal)catalysts were prepared by the incipient wetness impregnation method,followed by acid washing to remove calcium-containing minerals.Comprehensive characterization and low-temperature denitrification tests revealed that calcite-induced structural modulation of coal-derived AC significantly enhances catalytic activity.Specifically,NO conversion increased from 88.3%of Mn-Ce/De-AC to 91.7%of Mn-Ce/De-AC-1CaCO_(3)(210℃).The improved SCR denitrification activity results from the enhancement of physicochemical properties including higher Mn^(4+)content and Ce^(4+)/Ce^(3+)ratio,an abundance of chemisorbed oxygen and acidic sites,which could strengthen the SCR reaction pathways(richer NH_(3)activated species and bidentate nitrate active species).Therefore,NO removal is enhanced.展开更多
As a potential adsorption material,it is still a challenge for activated carbon fiber(ACF)in efficient adsorption of ethanol due to its nonpolar surface,which is mainly emitted from the grain drying industry.This stud...As a potential adsorption material,it is still a challenge for activated carbon fiber(ACF)in efficient adsorption of ethanol due to its nonpolar surface,which is mainly emitted from the grain drying industry.This study prepared surface polarity-modified ACF using the heteroatom doping method.The modified ACF possessed a richer array of strongly polar oxygen/nitrogen-containing functional groups(primarily phenolic hydroxyl and lactone groups),a larger specific surface are1,and a more developed micropore structure.The adsorption capacities of ethanol for O-ACF and N-ACF were 4.110 mmol/g and 1.698 mmol/g,respectively,which were 11.3 times and 4.7 times those of unmodified ACF.This was a significant improvement over our previous work(0.363 mmol/g).The improvement of adsorption capacity for the N-ACF was mainly due to the higher specific surface are1,greater number of micropores(more adsorption sites)and abundant existence of defects,whereas,for O-ACF,the improvement mainly relied on the abundant presence of oxygen-containing functional groups on the surface.However,water had a negative effect on the adsorption of ethanol for the modified ACF due to competitive adsorption and the disappearance of capillary condensation.It was further revealed that the adsorption process of ethanol and water was quite different.It obeyed the linear driving force(LDF)model for ethanol adsorption,however,the intraparticle diffusion(IPD)model for water adsorption.展开更多
This study investigates the innovative reuse of sewage sludge with eco-friendly alkaline solutes to improve clayey soil without conventional cementitious binders.The unconfined compressive strength(UCS)was the main cr...This study investigates the innovative reuse of sewage sludge with eco-friendly alkaline solutes to improve clayey soil without conventional cementitious binders.The unconfined compressive strength(UCS)was the main criterion to assess the quality and effectiveness of the proposed solutions,as this test was performed to measure the strength of the stabilized clay by varying binders’dosages and curing times.Moreover,the direct shear test(DST)was used to investigate the Mohr-Coulomb parameters of the treated soil.Microstructure observations of the natural and treated soil were conducted using scanning electron microscope(SEM),energy-dispersive spectroscopy(EDS),and FTIR.Furthermore,toxicity characteristic leaching procedure(TCLP)tests were performed on the treated soil to investigate the leachability of metals.According to the results,using 2.5%of sewage sludge activated by NaOH and Na_(2)SiO_(3)increases the UCS values from 176 kPa to 1.46 MPa after 7 d and 56 d of curing,respectively.The results of the DST indicate that sewage sludge as a precursor increases cohesion and enhances frictional resistance,thereby improving the Mohr-Coulomb parameters of the stabilized soil.The SEM micrographs show that alkali-activated sewage sludge increases the integrity and reduces the cavity volumes in the stabilized soil.Moreover,TCLP tests revealed that the solubility of metals in the treated soil alkaliactivated by sewage sludge significantly decreased.This study suggests that using sewage sludge can replace cement and lime in ground improvement,improve the circular economy,and reduce the carbon footprint of construction projects.展开更多
In this study,supported Pd catalysts were prepared and used as heterogeneous catalysts for the activation of peroxymonosulfate(PMS)which successfully degrade bisphenol F(BPF).Among the supported catalysts(i.e.,Pd/SiO_...In this study,supported Pd catalysts were prepared and used as heterogeneous catalysts for the activation of peroxymonosulfate(PMS)which successfully degrade bisphenol F(BPF).Among the supported catalysts(i.e.,Pd/SiO_(2),Pd/CeO_(2),Pd/TiO_(2)and Pd/Al2O3),Pd/TiO_(2)exhibited the highest catalytic activity due to the high isoelectric point and high Pd0 content.Pd/TiO_(2)prepared by the deposition method leads to high Pd dispersion,which are the key factors for efficient BPF degradation.The influencing factors were investigated during the reaction process and two possible degradation pathways were proposed.Density functional theory(DFT)calculations demonstrate that stronger BPF adsorption and BPF degradation with lower reaction barrier occurs on smaller Pd particles.The catalytic activities are strongly dependent on the structural features of the catalysts.Both experiments and theoretical calculations prove that the reaction is actuated by electron transfer rather than radicals.展开更多
Although transition metal-catalyzed methylene C(sp^(3))—H functionalization is a great challenge, it has made noticeable progress in recent years. This review specifically describes Pd-catalyzed intermolecular functi...Although transition metal-catalyzed methylene C(sp^(3))—H functionalization is a great challenge, it has made noticeable progress in recent years. This review specifically describes Pd-catalyzed intermolecular functionalization of unactivated methylene C(sp^(3))—H bonds. A variety of reactions, including arylation, alkylation, alkenylation/alkynylation, acetoxylation, amination, halogenation, borylation, and silylation reactions, have been discussed. Due to the inert properties, methylene C(sp^(3))—H functionalization reaction usually relies on the use of directing group strategies, which can not only control regioselectivity but also address low reactivity issue. Various directing groups, including strongly coordinating bidentate auxiliaries and weakly coordinating innate functional groups, have proven to be effective for enabling methylene C(sp^(3))—H functionalization.展开更多
Iron-Vanadium(FeV)catalyst showed a unique catalytic activity for the selective oxidation of methanol to formaldehyde;however,due to its complex compositions,the identification of catalytic active sites still remains ...Iron-Vanadium(FeV)catalyst showed a unique catalytic activity for the selective oxidation of methanol to formaldehyde;however,due to its complex compositions,the identification of catalytic active sites still remains challenging,inhibiting the rational design of excellent FeV-based catalysts.Here,in this work,a series of FeV catalysts with various compositions,including FeVO_(4),isolated VO_(x),low-polymerized V_(n)O_(x),and crystalline V_(2)O_(5) were prepared by controlling the preparation conditions,and were applied to methanol oxidation to formaldehyde reaction.A FeV_(1.1) catalyst,which consisted of FeVO_(4) and low-polymerized V_(n)O_(x) species showed an excellent catalytic performance with a methanol conversion of 92.3%and a formaldehyde selectivity of 90.6%,which was comparable to that of conventional iron-molybdate catalyst.The results of CH_(3)OH-IR,O_(2) pulse and control experiments revealed a crucial synergistic effect between FeVO_(4) and low-polymerized V_(n)O_(x).It enhanced the oxygen supply capacity and suitable binding and adsorption strengths for formaldehyde intermediates,contributing to the high catalytic activity and formaldehyde selectivity.This study not only advances the understanding of FeV structure but also offers valuable guidelines for selective methanol oxidation to formaldehyde.展开更多
The use of carbon from waste biomass has the potential to eliminate the drawbacks of Li-S batteries and improve their overall performance.Chrome-tanned-leather-shavings(CTLS)are a readily available waste product that ...The use of carbon from waste biomass has the potential to eliminate the drawbacks of Li-S batteries and improve their overall performance.Chrome-tanned-leather-shavings(CTLS)are a readily available waste product that can be transformed into porous carbon.We prepared an ac-tivated carbon by microwave pyrolysis combined with KOH activator using the CTLS as starting materials.The carbon had a specific surface area of 556 m^(2)g^(-1) and a honeycomb-like structure.Two kinds of N-doped activated carbons were then synthesized by thermal decomposition of the activated carbon,either combined with urea,or impregnated with eth-anolamine.Both N-doped activated carbons have an in-creased number of nitrogen and amine surface groups.However,only the urea treatment was effective in improv-ing the initial capacity of the cell(1363 mAh g^(-1)),which is probably linked to the sorption of long-chain polysulfides.This investigation confirms that it is possible to use the thermal de-composition of urea to obtain carbon materials from CTLS for use as the sulfur-host cathode in Li-S batteries and improve their performance.A radial basis function neural network was fitted to provide statistical support for the experimental results,which confirmed the importance of the nitrogen content of the carbons in determining the discharge capacity of the cells.展开更多
Lithium-ion capacitors(LICs)combine the high power dens-ity of electrical double-layer capacitors with the high energy density of lithium-ion batteries.However,they face practical limitations due to the narrow operati...Lithium-ion capacitors(LICs)combine the high power dens-ity of electrical double-layer capacitors with the high energy density of lithium-ion batteries.However,they face practical limitations due to the narrow operating voltage window of their activated carbon(AC)cathodes.We report a scalable thermal treatment strategy to develop high-voltage-tolerant AC cathodes.Through controlled thermal treatment of commer-cial activated carbon(Raw-AC)under a H_(2)/Ar atmosphere at 400-800℃,the targeted reduction of degradation-prone functional groups can be achieved while preserving the critical pore structure and increasing graph-itic microcrystalline ordering.The AC treated at 400℃(HAC-400)had a significant increase in specific capacity(96.0 vs.75.1 mAh/g at 0.05 A/g)and better rate capability(61.1 vs.36.1 mAh/g at 5 A/g)in half-cell LICs,along with an 83.5%capacity retention over 7400 cycles within an extended voltage range of 2.0-4.2 V in full-cell LICs.Scalability was demonstrated by a 120 g batch production,enabling fabrication of pouch-type LICs with commercial hard carbon anodes that delivered a higher energy density of 28.3 Wh/kg at 1 C,and a peak power density of 12.1 kW/kg compared to devices using raw AC.This simple,industry-compatible approach may be used for producing ad-vanced cathode materials for practical high-performance LICs.展开更多
Sewage sludge(SS)and SS impregnated with activating agents(ZnCl_(2) and KOH)were pyrolyzed in a fixed-bed reactor to produce gaseous fuel and activated char.The effects of heating rate,pyrolysis temperature and activa...Sewage sludge(SS)and SS impregnated with activating agents(ZnCl_(2) and KOH)were pyrolyzed in a fixed-bed reactor to produce gaseous fuel and activated char.The effects of heating rate,pyrolysis temperature and activator type on gas yields,pore structure and adsorption properties of activated char were systematically studied.The results demonstrated that increasing the pyrolysis temperature from 450℃ to 850℃ propo rtionally enhanced H_(2) and CO yields from the rapid pyrolysis of SS,while CH_(4) yield showed minimal variation between 650℃ and 850℃.ZnCl_(2) notably increased the CO yield,reaching71.9 ml·g^(-1)at 850℃,but caused a marked reduction in CH_(4) yield under the tested conditions.Similarly,KOH promoted CO yield at 750℃ and 850℃,with minimal impact on CH_(4) production.Both activators facilitated higher H_(2) yields in the range of 450-550℃,while the maximum H_(2) yield(109.8 ml·g^(-1))was observed at 850℃ in the absence of activator.The activated char derived from ZnCl_(2)-assisted pyrolysis exhibited well-developed micro-and mesopore structures,with specific surface areas ranging from 188.2 to 54.1 m^(2)·g^(-1)across pyrolysis temperatures of 450-850℃.When evaluated as adsorbents for methylene blue removal,activated char with greater specific surface area and total pore volume exhibited superior adsorption capacity.The adsorption process was well-described by the pseudo-second-order kinetic model.展开更多
Direct enantioselective allylic C—H functionalization has emerged as a powerful strategy for the asymmetric syn-thesis of highly valuable chiral products.Herein,a Rh(III)-catalyzed enantioselective allylic C—H alkyl...Direct enantioselective allylic C—H functionalization has emerged as a powerful strategy for the asymmetric syn-thesis of highly valuable chiral products.Herein,a Rh(III)-catalyzed enantioselective allylic C—H alkylation of unactivated alkenes withα-diazo carbonyl compounds is described,enabling direct access to chiral products with high efficiency(up to 77%yield,92%ee,and>10∶1 B/L(branched/linear)selectivity).This atom-and step-economical protocol directly converts simple,unactivated substrates into valuable enantioenriched products under mild conditions,providing an efficient catalytic system for asymmetric allylic C—H functionalization.展开更多
Chromium is one of the heavy metal pollutants. Heavy metal chromium-contaminated water will seriously endanger human health after use. There are many ways to remove chromium-containing sewage, and the adsorption metho...Chromium is one of the heavy metal pollutants. Heavy metal chromium-contaminated water will seriously endanger human health after use. There are many ways to remove chromium-containing sewage, and the adsorption method is the most effective and convenient method. The adsorption amount of traditional activated carbon is limited, so it needs to be modified to improve the adsorption rate. This experiment determined a reasonable modification method, and the calcination method was selected for the modification. This paper mainly compares the surface morphological characteristics of activated carbon before and after modification. The modified X-ray diffraction peak is increased and the infrared ray absorption peak increased, and the results show that the surface of the modified activated carbon is more rough than that of the modified activated carbon, the functional groups are increased, and the sulfur and nitrogen are doped on the activated carbon. Therefore, the modified activated carbon has a high removal rate and the best performance under acidic conditions.展开更多
Modified activated carbons(AS)were fabricated through the oxidation effect of ammonium persulfate and applied to the dynamic adsorption of different acrylate gas.The pore structures,surface chemical properties and sur...Modified activated carbons(AS)were fabricated through the oxidation effect of ammonium persulfate and applied to the dynamic adsorption of different acrylate gas.The pore structures,surface chemical properties and surface morphology of AS were respectively characterized by N2 adsorption,Boehm titration,X-ray Photoelectron Spectroscopy(XPS)and scanning electron microscopy(SEM)techniques.After modification,the specific surface area increased from 954 to 1154 m^(2)·g^(-1).The contents of oxygen-containing functional groups on the AS surface increase obviously and have a great effect on the adsorption behavior of acrylate gases.According to the results of dynamic adsorption,the adsorption capacities of acrylates are as the following order:methyl acrylate(461.9 mg·g^(-1))>methyl methacrylate(436.9 mg·g^(-1))>butyl acrylate(381.8 mg·g^(-1)),which is attributed to the size adaptability of AS pores and acrylates.The adsorption behavior of AS for acrylate gases conforms to the Bangham model and the Temkin model.展开更多
Anaerobic ammonia oxidation(Anammox)is an economical and sustainablewastewater nitrogen removal technology,and its application in the mainstream process is the inevitable trend of the development of Anammox.However,ho...Anaerobic ammonia oxidation(Anammox)is an economical and sustainablewastewater nitrogen removal technology,and its application in the mainstream process is the inevitable trend of the development of Anammox.However,how to effectively enriching Anammox bacteria from the activated sludge remains challenging and restricts its extensive applications.In this study,the rapid and efficient enrichment of Anammox bacteriawas achieved by raising the reflux ratio and nitrogen loading rate(NLR)using conventional activated sludge as the inoculant.In the screening phase(days 1–90),the reflux ratio was increased to discharge partial floc sludge,resulting in the relative abundance of Candidatus Brocadiaceae increased from0.04%to 22.54%,which effectively reduced thematrix and spatial competition between other microorganisms and Anammox bacteria.On day 90,the stoichiometric ratio of the Anammox process closely approached the theoretical value of 1:1.32:0.26,indicating that the Anammox reaction was the primary nitrogen removal process in the system.In the enrichment phase(days 91–238),the NLR increased from 0.43 to 1.20 kgN/(m^(3)·d)and removal efficiency was 71.89%,resulting in the relative abundance of Candidatus Brocadiaceae increased to 61.27%on day 180.The reactor operated steadily from days 444 to 498,maintaining the nitrogen removal rate(NRR)of 3.00 kgN/(m^(3)·d)and achieving successful sludge granulation with the particle size of 392.4μm.In short,this study provided a simple and efficient approach for enriching Anammox bacteria from the activated sludge,supporting to start an Anammox process efficiently.展开更多
In this study,a string of Cr-Mnco-modified activated coke catalysts(XCryMn1-y/AC)were prepared to investigate toluene and Hg^(0) removal performance.Multifarious characterizations including XRD,TEM,SEM,in situ DRIFTS,...In this study,a string of Cr-Mnco-modified activated coke catalysts(XCryMn1-y/AC)were prepared to investigate toluene and Hg^(0) removal performance.Multifarious characterizations including XRD,TEM,SEM,in situ DRIFTS,BET,XPS and H_(2)-TPR showed that 4%Cr0.5Mn0.5/AC had excellent physicochemical properties and exhibited the best toluene and Hg^(0) removal efficiency at 200℃.By varying the experimental gas components and conditions,it was found that too large weight hourly space velocity would reduce the removal efficiency of toluene and Hg^(0).Although O_(2) promoted the abatement of toluene and Hg^(0),the inhibitory role of H_(2)O and SO_(2) offset the promoting effect of O_(2) to some extent.Toluene significantly inhibited Hg^(0) removal,resulting from that toluene was present at concentrations orders of magnitude greater than mercury’s or the catalyst was more prone to adsorb toluene,while Hg^(0) almost exerted non-existent influence on toluene elimination.The mechanistic analysis showed that the forms of toluene and Hg^(0) removal included both adsorption and oxidation,where the high-valent metal cations and oxygen vacancy clusters promoted the redox cycle of Cr^(3+)+Mn^(3+)/Mn^(4+)+Cr^(6+)+Mn^(2+),which facilitated the conversion and replenishment of reactive oxygen species in the oxidation process,and even the CrMn_(1.5)O_(4) spinel structure could provide a larger catalytic interface,thus enhancing the adsorption/oxidation of toluene and Hg^(0).Therefore,its excellent physicochemical properties make it a costeffective potential industrial catalyst with outstanding synergistic toluene and Hg^(0) removal performance and preeminent resistance to H_(2)O and SO_(2).展开更多
Herein,the association between the dynamic adsorption capacity of toluene and several important characteristic values on activated carbon(AC)samples was investigated by multidimensional linear regression.Among the cha...Herein,the association between the dynamic adsorption capacity of toluene and several important characteristic values on activated carbon(AC)samples was investigated by multidimensional linear regression.Among the characteristic values,the carbon tetrachloride(CTC)adsorption value has demonstrated relatively stronger correlation with the toluene adsorption capacity on AC sampleswith diverse sources and forms,particularly in exposure to high-concentration toluene.Notably,the relevance of the toluene adsorption capacity to the CTC value could also be extended to a series of other porous adsorbents,which proved the wide applicability of CTC value in characterizing the adsorption behaviors.Based on these results,a mathematical and visual model was then established to predict the toluene adsorption saturation under different conditions(inlet concentration,adsorption time,initial CTC value,etc.)on diverse AC samples,of which the accuracy has later been verified by experimental data.As such,a fast and accurate estimation of the adsorption behaviors over AC samples,and possibly other porous adsorbents,was realized.展开更多
Designing xerogels at the molecular level to overcome volume shrinkage is a promising strategy for carbon xerogels with desirable structure and performance.Here,we design a xerogel with non-shrinkage by introducing Zn...Designing xerogels at the molecular level to overcome volume shrinkage is a promising strategy for carbon xerogels with desirable structure and performance.Here,we design a xerogel with non-shrinkage by introducing ZnCl_(2) into resorcinol-melamine-formaldehyde polymerization.The gel network consisting of micrometer pores and large particles(0.26-1.35μm)is constructed by the coordination of Zn^(2+) with oxygen/nitrogen-containing groups,which is attributed to the structural support of the rigid triazine skeleton with large steric hindrance.Therefore,the reinforced gel network possesses enough strength to withstand capillary forces during atmospheric drying,and special drying and solvent exchange are avoided.The xerogels show non-shrinkage and a short preparation time of 24 h.The resulted activated carbon xerogels with interconnected hierarchically micro-meso-macropores exhibit an optimal specific surface area of 1520 m^(2)/g(through xerogels pyrolysis and the pore-forming of ZnCl_(2)),high adsorption(methylene blue,I-,Cu^(2+),etc.),and repeated adsorption ability.This work provides novel thought for porous nanomaterials with non-shrinkage and desirable structures in adsorption and energy storage.展开更多
Obtaining large specific surface areas(SSA)for carbon xerogels poses a significant challenge due to the inevitable volume shrinkage of xerogel.Here,the Zn^(2+) coordination-catalyzed in-situ polymerization approach wa...Obtaining large specific surface areas(SSA)for carbon xerogels poses a significant challenge due to the inevitable volume shrinkage of xerogel.Here,the Zn^(2+) coordination-catalyzed in-situ polymerization approach was proposed to fabricate xerogels with a low shrinkage of 13.03% and a short preparation period of 24 h.In resorcinolformaldehyde(RF)polymerization,ZnCl_(2) could accelerate the reaction kinetics through the coordination of the Zn^(2+) and hydroxyl groups.The gel network with adjustable RF particles(46.5 nm-1.89μm)and narrow neck structures was constructed by changing ZnCl_(2) and ethanol contents,which could resist volume shrinkage during atmospheric drying without solvent exchange.The activated carbon xerogels(ACXs)with hierarchical structure were designed by one-step carbonization/activation due to the pore-forming of ZnCl_(2).The obtained ACXs showed a large SSA of 1689 m^(2)/g,multi-dyes adsorption capacity(methylene blue,Congo red,methyl orange,and Sudan Ⅲ were 625.90,359.46,320.69,and 453.92 mg/g,respectively),and reusability of 100%.The maximum monolayer MB adsorption capacity was 630.28 mg/g.This work presents an efficient strategy to design porous nanomaterials with low shrinkage and large SSA,which illustrates promising applications in separation,adsorption,and photoelectric catalysis.展开更多
Common activations of sulfite(S(Ⅳ))-based advanced oxidation processes(AOPs)utilized metal ions and oxides as catalysts,which are constrained by challenges in catalyst recovery,inadequate stability,and susceptibility...Common activations of sulfite(S(Ⅳ))-based advanced oxidation processes(AOPs)utilized metal ions and oxides as catalysts,which are constrained by challenges in catalyst recovery,inadequate stability,and susceptibility to secondary pollution in application.Calcium sulfite(CaSO_(3)),one of the byproducts of flue gas desulfurization,is of interest in AOPs because of its ability to slowly release S(Ⅳ),low toxicity,and costeffectiveness.Therefore,a heterogenous activator,molybdenum carbide(Mo_(2)C)was selected to stimulate Ca SO3for typical antibiotic elimination.Benefiting from the dissociation form of HSO_(3^(-))from CaSO_(3)and improved electron transfer of Mo_(2)C at pH 6,the simulated target metronidazole(MTZ)can be removed by 85.65%with rate constant of 0.02424 min^(-1)under near-neutral circumstance.The combining determinations of quenching test,electron spin resonance spectrum,and reactive species probe demonstrated singlet oxygen(^(1)O_(2))and sulfate radicals played leading role for MTZ decontamination.Characterization and theoretical calculation suggested the alteration of Mo valence state drove the activation of S(Ⅳ),and revealed that dissolved oxygen promoted the adsorption of HSO_(3^(-))on the surface of Mo_(2)C,then facilitating production of^(1)O_(2).The favorable stability and applicability for Mo_(2)C/CaSO_(3)process indicated an applied prospect in actual pharmaceutical wastewater.展开更多
The scintillating photonic glass has the great potential for medicine imaging,nuclear physics,highenergy physics,and national defense.However,the development of the candidate with the high density remains a significan...The scintillating photonic glass has the great potential for medicine imaging,nuclear physics,highenergy physics,and national defense.However,the development of the candidate with the high density remains a significant challenge.Herein,the superdense scintillating glasses derived from the Ce^(3+)-activated Lu_(2)O_(3)-SiO_(2)binary system were successfully fabricated by the strategy of contactless aerodynamic levitation heating under the N_(2)atmosphere.These glasses are colorless,optical homogeneous,and exhibit superdense density from 6.59 to 7.15 g/cm^(3),representing the highest density among the fast decay glass systems.The materials present excellent radiation-blocking ability,suitable emission wavelength,and fast response,indicating the promise for fast-eve nt X-ray detection.The micro radiation probe was fabricated by connecting the scintillating glass and the optical fiber.The practical application in remote radiation detection is demonstrated and it exhibits excellent linear response and high signalto-noise ratio.The results confirm that the fabricated superdense scintillating glass is promising for application in the field of high-energy radiation detection.展开更多
基金financially supported by National Natural Science Foundation of China(No.52264043).
文摘To explore the denitration mechanism of iron-vanadium/activated carbon(Fe-V/AC)catalysts in ammonia-selective catalytic reduction(NH_(3)-SCR),the physicochemical properties of Fe-V/AC catalysts were characterized.The denitration activities of the Fe-V/AC catalysts in the range of 150-300℃ were evaluated.The increase in denitration temperature leads to the highest and fastest recovery rate of NO conversion in the 10Fe-15V/AC catalyst.However,more metal oxides were attached to the catalyst surface as the V loading increased,and the accumulation occurred.The surface-active components are FeO,Fe_(2)O_(3),Fe_(3)O_(4),VO_(2),and V_(2)O_(5).In addition,the increase in the V loading induced a series of modification effects.A large amount of Fe^(3+)was reduced to Fe^(2+),and a large amount of V^(4+)was oxidized to V^(5+).The surface oxygen species(O_(α))were transformed into lattice oxygen(O_(β)).The presence of a large amount of V species deteriorated the pore-structure parameters and destroyed the oxygen-containing functional groups.Increasing the V loading can effectively increase the Lewis acid sites,thereby promoting NH_(3) adsorption and NO reduction and increasing the stretching vibration of weakly adsorbed ammonia species on the catalyst.The NH_(3) adsorption process produces a notable increase in the concentration of monodentate nitrite(NH_(4)^(+)).The NH_(3)-SCR denitration mechanism of the Fe-V/AC catalyst includes reaction gas adsorption,catalytic denitration of metal active components,and gas desorption.
基金Supported by the Science and Technology Cooperation and Exchange special project of Cooperation of Shanxi Province(202404041101014)the Fundamental Research Program of Shanxi Province(202403021212333)+3 种基金the Joint Funds of the National Natural Science Foundation of China(U24A20555)the Lvliang Key R&D of University-Local Cooperation(2023XDHZ10)the Initiation Fund for Doctoral Research of Taiyuan University of Science and Technology(20242026)the Outstanding Doctor Funding Award of Shanxi Province(20242080).
文摘To elucidate the effect of calcite-regulated activated carbon(AC)structure on low-temperature denitrification performance of SCR catalysts,this work prepared a series of Mn-Ce/De-AC-xCaCO_(3)(x is the calcite content in coal)catalysts were prepared by the incipient wetness impregnation method,followed by acid washing to remove calcium-containing minerals.Comprehensive characterization and low-temperature denitrification tests revealed that calcite-induced structural modulation of coal-derived AC significantly enhances catalytic activity.Specifically,NO conversion increased from 88.3%of Mn-Ce/De-AC to 91.7%of Mn-Ce/De-AC-1CaCO_(3)(210℃).The improved SCR denitrification activity results from the enhancement of physicochemical properties including higher Mn^(4+)content and Ce^(4+)/Ce^(3+)ratio,an abundance of chemisorbed oxygen and acidic sites,which could strengthen the SCR reaction pathways(richer NH_(3)activated species and bidentate nitrate active species).Therefore,NO removal is enhanced.
基金supported by the National Key R&D Program of China(Nos.2022YFB4101500 and 2022YFE0209500)the National Natural Science Foundation of China(Nos.22276191 and 21976177)the Qinghai Province Air Pollution Assessment and Fine Management Support Project,and the University of Chinese Academy of Science.
文摘As a potential adsorption material,it is still a challenge for activated carbon fiber(ACF)in efficient adsorption of ethanol due to its nonpolar surface,which is mainly emitted from the grain drying industry.This study prepared surface polarity-modified ACF using the heteroatom doping method.The modified ACF possessed a richer array of strongly polar oxygen/nitrogen-containing functional groups(primarily phenolic hydroxyl and lactone groups),a larger specific surface are1,and a more developed micropore structure.The adsorption capacities of ethanol for O-ACF and N-ACF were 4.110 mmol/g and 1.698 mmol/g,respectively,which were 11.3 times and 4.7 times those of unmodified ACF.This was a significant improvement over our previous work(0.363 mmol/g).The improvement of adsorption capacity for the N-ACF was mainly due to the higher specific surface are1,greater number of micropores(more adsorption sites)and abundant existence of defects,whereas,for O-ACF,the improvement mainly relied on the abundant presence of oxygen-containing functional groups on the surface.However,water had a negative effect on the adsorption of ethanol for the modified ACF due to competitive adsorption and the disappearance of capillary condensation.It was further revealed that the adsorption process of ethanol and water was quite different.It obeyed the linear driving force(LDF)model for ethanol adsorption,however,the intraparticle diffusion(IPD)model for water adsorption.
文摘This study investigates the innovative reuse of sewage sludge with eco-friendly alkaline solutes to improve clayey soil without conventional cementitious binders.The unconfined compressive strength(UCS)was the main criterion to assess the quality and effectiveness of the proposed solutions,as this test was performed to measure the strength of the stabilized clay by varying binders’dosages and curing times.Moreover,the direct shear test(DST)was used to investigate the Mohr-Coulomb parameters of the treated soil.Microstructure observations of the natural and treated soil were conducted using scanning electron microscope(SEM),energy-dispersive spectroscopy(EDS),and FTIR.Furthermore,toxicity characteristic leaching procedure(TCLP)tests were performed on the treated soil to investigate the leachability of metals.According to the results,using 2.5%of sewage sludge activated by NaOH and Na_(2)SiO_(3)increases the UCS values from 176 kPa to 1.46 MPa after 7 d and 56 d of curing,respectively.The results of the DST indicate that sewage sludge as a precursor increases cohesion and enhances frictional resistance,thereby improving the Mohr-Coulomb parameters of the stabilized soil.The SEM micrographs show that alkali-activated sewage sludge increases the integrity and reduces the cavity volumes in the stabilized soil.Moreover,TCLP tests revealed that the solubility of metals in the treated soil alkaliactivated by sewage sludge significantly decreased.This study suggests that using sewage sludge can replace cement and lime in ground improvement,improve the circular economy,and reduce the carbon footprint of construction projects.
基金supported by the National Natural Science Foundation of China(NSFC)(No.21978137).
文摘In this study,supported Pd catalysts were prepared and used as heterogeneous catalysts for the activation of peroxymonosulfate(PMS)which successfully degrade bisphenol F(BPF).Among the supported catalysts(i.e.,Pd/SiO_(2),Pd/CeO_(2),Pd/TiO_(2)and Pd/Al2O3),Pd/TiO_(2)exhibited the highest catalytic activity due to the high isoelectric point and high Pd0 content.Pd/TiO_(2)prepared by the deposition method leads to high Pd dispersion,which are the key factors for efficient BPF degradation.The influencing factors were investigated during the reaction process and two possible degradation pathways were proposed.Density functional theory(DFT)calculations demonstrate that stronger BPF adsorption and BPF degradation with lower reaction barrier occurs on smaller Pd particles.The catalytic activities are strongly dependent on the structural features of the catalysts.Both experiments and theoretical calculations prove that the reaction is actuated by electron transfer rather than radicals.
文摘Although transition metal-catalyzed methylene C(sp^(3))—H functionalization is a great challenge, it has made noticeable progress in recent years. This review specifically describes Pd-catalyzed intermolecular functionalization of unactivated methylene C(sp^(3))—H bonds. A variety of reactions, including arylation, alkylation, alkenylation/alkynylation, acetoxylation, amination, halogenation, borylation, and silylation reactions, have been discussed. Due to the inert properties, methylene C(sp^(3))—H functionalization reaction usually relies on the use of directing group strategies, which can not only control regioselectivity but also address low reactivity issue. Various directing groups, including strongly coordinating bidentate auxiliaries and weakly coordinating innate functional groups, have proven to be effective for enabling methylene C(sp^(3))—H functionalization.
文摘Iron-Vanadium(FeV)catalyst showed a unique catalytic activity for the selective oxidation of methanol to formaldehyde;however,due to its complex compositions,the identification of catalytic active sites still remains challenging,inhibiting the rational design of excellent FeV-based catalysts.Here,in this work,a series of FeV catalysts with various compositions,including FeVO_(4),isolated VO_(x),low-polymerized V_(n)O_(x),and crystalline V_(2)O_(5) were prepared by controlling the preparation conditions,and were applied to methanol oxidation to formaldehyde reaction.A FeV_(1.1) catalyst,which consisted of FeVO_(4) and low-polymerized V_(n)O_(x) species showed an excellent catalytic performance with a methanol conversion of 92.3%and a formaldehyde selectivity of 90.6%,which was comparable to that of conventional iron-molybdate catalyst.The results of CH_(3)OH-IR,O_(2) pulse and control experiments revealed a crucial synergistic effect between FeVO_(4) and low-polymerized V_(n)O_(x).It enhanced the oxygen supply capacity and suitable binding and adsorption strengths for formaldehyde intermediates,contributing to the high catalytic activity and formaldehyde selectivity.This study not only advances the understanding of FeV structure but also offers valuable guidelines for selective methanol oxidation to formaldehyde.
文摘The use of carbon from waste biomass has the potential to eliminate the drawbacks of Li-S batteries and improve their overall performance.Chrome-tanned-leather-shavings(CTLS)are a readily available waste product that can be transformed into porous carbon.We prepared an ac-tivated carbon by microwave pyrolysis combined with KOH activator using the CTLS as starting materials.The carbon had a specific surface area of 556 m^(2)g^(-1) and a honeycomb-like structure.Two kinds of N-doped activated carbons were then synthesized by thermal decomposition of the activated carbon,either combined with urea,or impregnated with eth-anolamine.Both N-doped activated carbons have an in-creased number of nitrogen and amine surface groups.However,only the urea treatment was effective in improv-ing the initial capacity of the cell(1363 mAh g^(-1)),which is probably linked to the sorption of long-chain polysulfides.This investigation confirms that it is possible to use the thermal de-composition of urea to obtain carbon materials from CTLS for use as the sulfur-host cathode in Li-S batteries and improve their performance.A radial basis function neural network was fitted to provide statistical support for the experimental results,which confirmed the importance of the nitrogen content of the carbons in determining the discharge capacity of the cells.
文摘Lithium-ion capacitors(LICs)combine the high power dens-ity of electrical double-layer capacitors with the high energy density of lithium-ion batteries.However,they face practical limitations due to the narrow operating voltage window of their activated carbon(AC)cathodes.We report a scalable thermal treatment strategy to develop high-voltage-tolerant AC cathodes.Through controlled thermal treatment of commer-cial activated carbon(Raw-AC)under a H_(2)/Ar atmosphere at 400-800℃,the targeted reduction of degradation-prone functional groups can be achieved while preserving the critical pore structure and increasing graph-itic microcrystalline ordering.The AC treated at 400℃(HAC-400)had a significant increase in specific capacity(96.0 vs.75.1 mAh/g at 0.05 A/g)and better rate capability(61.1 vs.36.1 mAh/g at 5 A/g)in half-cell LICs,along with an 83.5%capacity retention over 7400 cycles within an extended voltage range of 2.0-4.2 V in full-cell LICs.Scalability was demonstrated by a 120 g batch production,enabling fabrication of pouch-type LICs with commercial hard carbon anodes that delivered a higher energy density of 28.3 Wh/kg at 1 C,and a peak power density of 12.1 kW/kg compared to devices using raw AC.This simple,industry-compatible approach may be used for producing ad-vanced cathode materials for practical high-performance LICs.
基金financially supported by the National Natural Science Foundation of China(U21A2062)National innovative training program for college students of China(202410792014)。
文摘Sewage sludge(SS)and SS impregnated with activating agents(ZnCl_(2) and KOH)were pyrolyzed in a fixed-bed reactor to produce gaseous fuel and activated char.The effects of heating rate,pyrolysis temperature and activator type on gas yields,pore structure and adsorption properties of activated char were systematically studied.The results demonstrated that increasing the pyrolysis temperature from 450℃ to 850℃ propo rtionally enhanced H_(2) and CO yields from the rapid pyrolysis of SS,while CH_(4) yield showed minimal variation between 650℃ and 850℃.ZnCl_(2) notably increased the CO yield,reaching71.9 ml·g^(-1)at 850℃,but caused a marked reduction in CH_(4) yield under the tested conditions.Similarly,KOH promoted CO yield at 750℃ and 850℃,with minimal impact on CH_(4) production.Both activators facilitated higher H_(2) yields in the range of 450-550℃,while the maximum H_(2) yield(109.8 ml·g^(-1))was observed at 850℃ in the absence of activator.The activated char derived from ZnCl_(2)-assisted pyrolysis exhibited well-developed micro-and mesopore structures,with specific surface areas ranging from 188.2 to 54.1 m^(2)·g^(-1)across pyrolysis temperatures of 450-850℃.When evaluated as adsorbents for methylene blue removal,activated char with greater specific surface area and total pore volume exhibited superior adsorption capacity.The adsorption process was well-described by the pseudo-second-order kinetic model.
文摘Direct enantioselective allylic C—H functionalization has emerged as a powerful strategy for the asymmetric syn-thesis of highly valuable chiral products.Herein,a Rh(III)-catalyzed enantioselective allylic C—H alkylation of unactivated alkenes withα-diazo carbonyl compounds is described,enabling direct access to chiral products with high efficiency(up to 77%yield,92%ee,and>10∶1 B/L(branched/linear)selectivity).This atom-and step-economical protocol directly converts simple,unactivated substrates into valuable enantioenriched products under mild conditions,providing an efficient catalytic system for asymmetric allylic C—H functionalization.
文摘Chromium is one of the heavy metal pollutants. Heavy metal chromium-contaminated water will seriously endanger human health after use. There are many ways to remove chromium-containing sewage, and the adsorption method is the most effective and convenient method. The adsorption amount of traditional activated carbon is limited, so it needs to be modified to improve the adsorption rate. This experiment determined a reasonable modification method, and the calcination method was selected for the modification. This paper mainly compares the surface morphological characteristics of activated carbon before and after modification. The modified X-ray diffraction peak is increased and the infrared ray absorption peak increased, and the results show that the surface of the modified activated carbon is more rough than that of the modified activated carbon, the functional groups are increased, and the sulfur and nitrogen are doped on the activated carbon. Therefore, the modified activated carbon has a high removal rate and the best performance under acidic conditions.
基金Funded by the National Natural Science Foundation of China(No.51873167)the Self-determined and Innovative Research Funds of WUT(No.2024-CL-B1-02)。
文摘Modified activated carbons(AS)were fabricated through the oxidation effect of ammonium persulfate and applied to the dynamic adsorption of different acrylate gas.The pore structures,surface chemical properties and surface morphology of AS were respectively characterized by N2 adsorption,Boehm titration,X-ray Photoelectron Spectroscopy(XPS)and scanning electron microscopy(SEM)techniques.After modification,the specific surface area increased from 954 to 1154 m^(2)·g^(-1).The contents of oxygen-containing functional groups on the AS surface increase obviously and have a great effect on the adsorption behavior of acrylate gases.According to the results of dynamic adsorption,the adsorption capacities of acrylates are as the following order:methyl acrylate(461.9 mg·g^(-1))>methyl methacrylate(436.9 mg·g^(-1))>butyl acrylate(381.8 mg·g^(-1)),which is attributed to the size adaptability of AS pores and acrylates.The adsorption behavior of AS for acrylate gases conforms to the Bangham model and the Temkin model.
基金supported by the National Natural Science Foundation of China(No.52070149)Shaanxi Innovative Research Team for Key Science and Technology(No.2023-CXTD-36)+1 种基金Shaanxi Province Key Program for International S&T Cooperation Projects(No.2024GH-ZDXM-04)the Bureau of Science and Technology of Xi’an City of China(No.23SFSF0011).
文摘Anaerobic ammonia oxidation(Anammox)is an economical and sustainablewastewater nitrogen removal technology,and its application in the mainstream process is the inevitable trend of the development of Anammox.However,how to effectively enriching Anammox bacteria from the activated sludge remains challenging and restricts its extensive applications.In this study,the rapid and efficient enrichment of Anammox bacteriawas achieved by raising the reflux ratio and nitrogen loading rate(NLR)using conventional activated sludge as the inoculant.In the screening phase(days 1–90),the reflux ratio was increased to discharge partial floc sludge,resulting in the relative abundance of Candidatus Brocadiaceae increased from0.04%to 22.54%,which effectively reduced thematrix and spatial competition between other microorganisms and Anammox bacteria.On day 90,the stoichiometric ratio of the Anammox process closely approached the theoretical value of 1:1.32:0.26,indicating that the Anammox reaction was the primary nitrogen removal process in the system.In the enrichment phase(days 91–238),the NLR increased from 0.43 to 1.20 kgN/(m^(3)·d)and removal efficiency was 71.89%,resulting in the relative abundance of Candidatus Brocadiaceae increased to 61.27%on day 180.The reactor operated steadily from days 444 to 498,maintaining the nitrogen removal rate(NRR)of 3.00 kgN/(m^(3)·d)and achieving successful sludge granulation with the particle size of 392.4μm.In short,this study provided a simple and efficient approach for enriching Anammox bacteria from the activated sludge,supporting to start an Anammox process efficiently.
基金supported by the Scientific Research Project of Hunan Provincial Department of Education (No.22B0458)the National Natural Science Foundation of China (No.52270102).
文摘In this study,a string of Cr-Mnco-modified activated coke catalysts(XCryMn1-y/AC)were prepared to investigate toluene and Hg^(0) removal performance.Multifarious characterizations including XRD,TEM,SEM,in situ DRIFTS,BET,XPS and H_(2)-TPR showed that 4%Cr0.5Mn0.5/AC had excellent physicochemical properties and exhibited the best toluene and Hg^(0) removal efficiency at 200℃.By varying the experimental gas components and conditions,it was found that too large weight hourly space velocity would reduce the removal efficiency of toluene and Hg^(0).Although O_(2) promoted the abatement of toluene and Hg^(0),the inhibitory role of H_(2)O and SO_(2) offset the promoting effect of O_(2) to some extent.Toluene significantly inhibited Hg^(0) removal,resulting from that toluene was present at concentrations orders of magnitude greater than mercury’s or the catalyst was more prone to adsorb toluene,while Hg^(0) almost exerted non-existent influence on toluene elimination.The mechanistic analysis showed that the forms of toluene and Hg^(0) removal included both adsorption and oxidation,where the high-valent metal cations and oxygen vacancy clusters promoted the redox cycle of Cr^(3+)+Mn^(3+)/Mn^(4+)+Cr^(6+)+Mn^(2+),which facilitated the conversion and replenishment of reactive oxygen species in the oxidation process,and even the CrMn_(1.5)O_(4) spinel structure could provide a larger catalytic interface,thus enhancing the adsorption/oxidation of toluene and Hg^(0).Therefore,its excellent physicochemical properties make it a costeffective potential industrial catalyst with outstanding synergistic toluene and Hg^(0) removal performance and preeminent resistance to H_(2)O and SO_(2).
基金supported by the Key Research and Development Projects in Zhejiang Province(Nos.2023C03127,2024C03114,2024C03108)the Natural Science Foundation of China(Nos.22208300,22078294)+2 种基金the Natural Science Foundation of Zhejiang Province(No.LQ23B060007)the Fundamental Research Funds for the Provincial Universities of Zhejiang(No.RF-A2023004)Zhejiang Provincial Postdoctoral Science Foundation(No.ZJ2023145).
文摘Herein,the association between the dynamic adsorption capacity of toluene and several important characteristic values on activated carbon(AC)samples was investigated by multidimensional linear regression.Among the characteristic values,the carbon tetrachloride(CTC)adsorption value has demonstrated relatively stronger correlation with the toluene adsorption capacity on AC sampleswith diverse sources and forms,particularly in exposure to high-concentration toluene.Notably,the relevance of the toluene adsorption capacity to the CTC value could also be extended to a series of other porous adsorbents,which proved the wide applicability of CTC value in characterizing the adsorption behaviors.Based on these results,a mathematical and visual model was then established to predict the toluene adsorption saturation under different conditions(inlet concentration,adsorption time,initial CTC value,etc.)on diverse AC samples,of which the accuracy has later been verified by experimental data.As such,a fast and accurate estimation of the adsorption behaviors over AC samples,and possibly other porous adsorbents,was realized.
基金supported by the National Key Research and Development Program of China(No.2023YFB3711501)the Shanghai Industrial Collaborative Innovation Leading Group Office(No.XTCX-KJ-2023-53)+3 种基金the Fundamental Research Funds for the Central Universities(No.23D110609)the Open Research Fund of Songshan Lake Materials Laboratory(No.2022SLABFN09)the Foundation of State Key Laboratory of Biobased Material and Green Paper-making,Qilu University of Technology,Shandong Academy of Sciences(No.GZKF202231)the Fundamental Research Funds for the Central Universities and Graduate Student Innovation Fund of Donghua University(No.CUSF-DH-d-2022012).
文摘Designing xerogels at the molecular level to overcome volume shrinkage is a promising strategy for carbon xerogels with desirable structure and performance.Here,we design a xerogel with non-shrinkage by introducing ZnCl_(2) into resorcinol-melamine-formaldehyde polymerization.The gel network consisting of micrometer pores and large particles(0.26-1.35μm)is constructed by the coordination of Zn^(2+) with oxygen/nitrogen-containing groups,which is attributed to the structural support of the rigid triazine skeleton with large steric hindrance.Therefore,the reinforced gel network possesses enough strength to withstand capillary forces during atmospheric drying,and special drying and solvent exchange are avoided.The xerogels show non-shrinkage and a short preparation time of 24 h.The resulted activated carbon xerogels with interconnected hierarchically micro-meso-macropores exhibit an optimal specific surface area of 1520 m^(2)/g(through xerogels pyrolysis and the pore-forming of ZnCl_(2)),high adsorption(methylene blue,I-,Cu^(2+),etc.),and repeated adsorption ability.This work provides novel thought for porous nanomaterials with non-shrinkage and desirable structures in adsorption and energy storage.
基金supported by the National Key Research and Development Program of China(No.2023YFB3711501)Shanghai Industrial Collaborative Innovation Leading Group Office(No.XTCX-KJ-2023-53)+3 种基金the Fundamental Research Funds for the Central Universities(No.23D110609)the Open Research Fund of Songshan Lake Materials Laboratory(No.2022SLABFN09)the Foundation of State Key Laboratory of Biobased Material and Green Papermaking,Qilu University of Technology,Shandong Academy of Sciences(No.GZKF202231)the Fundamental Research Funds for the Central Universities and Graduate Student Innovation Fund of Donghua University(No.CUSF-DH-D-2022012).
文摘Obtaining large specific surface areas(SSA)for carbon xerogels poses a significant challenge due to the inevitable volume shrinkage of xerogel.Here,the Zn^(2+) coordination-catalyzed in-situ polymerization approach was proposed to fabricate xerogels with a low shrinkage of 13.03% and a short preparation period of 24 h.In resorcinolformaldehyde(RF)polymerization,ZnCl_(2) could accelerate the reaction kinetics through the coordination of the Zn^(2+) and hydroxyl groups.The gel network with adjustable RF particles(46.5 nm-1.89μm)and narrow neck structures was constructed by changing ZnCl_(2) and ethanol contents,which could resist volume shrinkage during atmospheric drying without solvent exchange.The activated carbon xerogels(ACXs)with hierarchical structure were designed by one-step carbonization/activation due to the pore-forming of ZnCl_(2).The obtained ACXs showed a large SSA of 1689 m^(2)/g,multi-dyes adsorption capacity(methylene blue,Congo red,methyl orange,and Sudan Ⅲ were 625.90,359.46,320.69,and 453.92 mg/g,respectively),and reusability of 100%.The maximum monolayer MB adsorption capacity was 630.28 mg/g.This work presents an efficient strategy to design porous nanomaterials with low shrinkage and large SSA,which illustrates promising applications in separation,adsorption,and photoelectric catalysis.
基金the support received from the National Natural Science Foundation of China(No.51908485)the Central Guidance on Local Science and Technology Development Fund of Hebei Province(Nos.246Z3603G and 226Z3603G)。
文摘Common activations of sulfite(S(Ⅳ))-based advanced oxidation processes(AOPs)utilized metal ions and oxides as catalysts,which are constrained by challenges in catalyst recovery,inadequate stability,and susceptibility to secondary pollution in application.Calcium sulfite(CaSO_(3)),one of the byproducts of flue gas desulfurization,is of interest in AOPs because of its ability to slowly release S(Ⅳ),low toxicity,and costeffectiveness.Therefore,a heterogenous activator,molybdenum carbide(Mo_(2)C)was selected to stimulate Ca SO3for typical antibiotic elimination.Benefiting from the dissociation form of HSO_(3^(-))from CaSO_(3)and improved electron transfer of Mo_(2)C at pH 6,the simulated target metronidazole(MTZ)can be removed by 85.65%with rate constant of 0.02424 min^(-1)under near-neutral circumstance.The combining determinations of quenching test,electron spin resonance spectrum,and reactive species probe demonstrated singlet oxygen(^(1)O_(2))and sulfate radicals played leading role for MTZ decontamination.Characterization and theoretical calculation suggested the alteration of Mo valence state drove the activation of S(Ⅳ),and revealed that dissolved oxygen promoted the adsorption of HSO_(3^(-))on the surface of Mo_(2)C,then facilitating production of^(1)O_(2).The favorable stability and applicability for Mo_(2)C/CaSO_(3)process indicated an applied prospect in actual pharmaceutical wastewater.
基金supported by the National Science Fund for Distinguished Young Scholars(62125502)the National Natural Science Foundation of China(52302002,62305115)Guangdong Basic and Applied Basic Research Foundation(2024A1515011827)。
文摘The scintillating photonic glass has the great potential for medicine imaging,nuclear physics,highenergy physics,and national defense.However,the development of the candidate with the high density remains a significant challenge.Herein,the superdense scintillating glasses derived from the Ce^(3+)-activated Lu_(2)O_(3)-SiO_(2)binary system were successfully fabricated by the strategy of contactless aerodynamic levitation heating under the N_(2)atmosphere.These glasses are colorless,optical homogeneous,and exhibit superdense density from 6.59 to 7.15 g/cm^(3),representing the highest density among the fast decay glass systems.The materials present excellent radiation-blocking ability,suitable emission wavelength,and fast response,indicating the promise for fast-eve nt X-ray detection.The micro radiation probe was fabricated by connecting the scintillating glass and the optical fiber.The practical application in remote radiation detection is demonstrated and it exhibits excellent linear response and high signalto-noise ratio.The results confirm that the fabricated superdense scintillating glass is promising for application in the field of high-energy radiation detection.