Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because ...Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because it has a high specific surfacearea for sulfur loading.We have developed a pressurizedphysical activation(PPA)method that producedan activated carbon(PPAC)with a high specific surfacearea comparable to that of CAC.The pore structure of PPAC could be changed and its use as a cathode material for Li–Sbatteries was investigated.Battery tests at different capacity rates(C-rates)showed that it had a much improved high-rate performancewith a discharge capacity of 900 mAh/(g of sulfur)at 1 C,in contrast to only 600 mAh/(g of sulfur)for CAC.Porestructure analyses showed that PPAC prepared at a high activation temperature(1000℃)had unusual channel-like mesoporesbetween the microdomains that are the basic structural units of artificial carbon materials.These are connected to microporesdeveloped in each microdomain,and deliver ions from the surroundings to the internal pores and vice versa.The well-developedmicropores and mesopores of PPAC respectively ensured the high adsorption of lithium polysulfides and a high rate ofion diffusion.Compared to CAC,PPAC is a high-performance,low-cost cathode material that is promising for use in futureLi–S batteries.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
A series of blue and blue‑green Ir(Ⅲ)complexes has been investigated theoretically to explore their electronic structures,photophysical properties,efficiency roll‑off effect,and thermal activation delayed fluorescenc...A series of blue and blue‑green Ir(Ⅲ)complexes has been investigated theoretically to explore their electronic structures,photophysical properties,efficiency roll‑off effect,and thermal activation delayed fluorescence(TADF)properties.All calculations were performed using density functional theory(DFT)and time‑dependent density functional theory(TDDFT).Calculations for electronic structures,frontier molecular orbital characteristics(which determine the efficiency roll‑off effect of the complexes),and photophysical properties were conducted using the Gaussian 09 software package.The calculation of spin‑orbit coupling matrix elements<T|HSOC|S>,which determine the TADF properties of the complexes,was performed using the ORCA software package.The calculation results show that the auxiliary ligand tetraphenylimidodiphosphinate(tpip),a strong electron‑withdrawing group,can mitigate the efficiency roll‑off effect of the complex.Furthermore,TADF is observed in one of the designed complexes,(F_(3)Phppy)_(2)Ir(tpip),where F_(3)Phppy=2‑[4‑(2,4,6‑trifluorophenyl)phenyl]pyridine.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
The ACF adsorbent with high Cu loading was treated with dielectric barrier discharge plasma to mitigate the negative effects of high Cu loading and enhance PH_(3)and H_(2)S adsorption and oxidation.Bruno-Emmett-Taylor...The ACF adsorbent with high Cu loading was treated with dielectric barrier discharge plasma to mitigate the negative effects of high Cu loading and enhance PH_(3)and H_(2)S adsorption and oxidation.Bruno-Emmett-Taylor(BET)result showed that the specific surface area of the adsorbent after air plasma modification was almost three times that before modification.X-ray photoelectron spectroscopy(XPS)findings revealed that the amino group was added to the adsorbent's surface,increasing lattice oxygen and chemisorbed oxygen.The adsorbent's large specific surface area,excellent surface active oxygen,and abundance of basic groups facilitate PH_(3)and H_(2)S adsorption and oxidation.The scanning electron microscopy showed that air plasma modification exposed more active components and uniformly dispersed them on the surface of adsorbent,thereby improving the adsorption performance.Activity evaluation results showed that the adsorbent has the best ability to capture PH_(3)and H_(2)S after being modified by air plasma at 4 kV voltage for 10 min.The adsorbent's breakthrough ability at high space velocity(WHSV:60,000 h^(−1))is 190 mg P/g and 146 mg S/g,respectively,which is 74%and 60%greater than that before modification.This is a great improvement over previous studies.In addition,the possible mechanism of adsorbent deactivation was proposed.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
Control of N-nitrosodimethylamine(NDMA)in drinking water could be achieved by removing its precursors as one practical way.Herein,superfine powdered activated carbons with a diameter of about 1μm(SPACs)were successfu...Control of N-nitrosodimethylamine(NDMA)in drinking water could be achieved by removing its precursors as one practical way.Herein,superfine powdered activated carbons with a diameter of about 1μm(SPACs)were successfully prepared by grinding powdered activated carbon(PAC,D50=24.3μm)and applied to remove model NDMA precursors,i.e.ranitidine(RAN)and nizatidine(NIZ).Results fromgrain diameter experiments demonstrated that the absorption velocity increased dramatically with decreasing particle size,and the maximum increase in k2 was 26.8-folds for RAN and 33.4-folds for NIZ.Moreover,kinetic experiments explained that rapid absorption could be attributed to the acceleration of intraparticle diffusion due to the shortening of the diffusion path.Furthermore,performance comparison experiments suggested that the removal of RAN and NIZ(C_(0)=0.5 mg/L)could reach 61.3%and 60%,respectively,within 5 min,when the dosage of SAPC-1.1(D_(50)=1.1μm)was merely 5 mg/L,while PAC-24.3 could only eliminate 17.5%and 18.6%.The adsorption isotherm was well defined by Langmuir isotherm model,indicating that the adsorption of RAN/NIZ was a monolayer coverage process.The adsorption of RAN or NIZ by SAPC-1.1 and PAC-24.3 was strongly pH dependent,and high adsorption capacity could be observed under the condition of pH>pk_(a)+1.The coexistence of humic acid(HA)had no significant effect on the adsorption performance because RAN/NIZ may be coupled with HA and removed simultaneously.The coexistence of anions had little effect on the adsorption also.This study is expected to provide an alternative strategy for drinking water safety triggered by NDMA.展开更多
High electrochemical performance supercapacitors require activated carbon with high specific surface area,suitable pore size distribution and surface properties,and high electrical conductivity as electrode materials,...High electrochemical performance supercapacitors require activated carbon with high specific surface area,suitable pore size distribution and surface properties,and high electrical conductivity as electrode materials,whereas there exists a trade-off relationship between specific surface area and electrical conductivity,which is not well met by a single type of carbon source.To solve this problem,the coal and sargassum are adopted to obtain the coupling product via co-thermal dissolution,followed by carbonization and KOH activation.The effects of mixing mass ratio and activation temperature on the prepared activated carbon(AC)are investigated using single factor experimental method.The experimental results show that AC_(1/3-800)has abundant micropore and mesopore content,good pore structure connectivity,high electrical conductivity and good wettability,and superior electrochemical properties compared with other activated carbons prepared in this experiment.Its total specific surface area is up to 2098.5 m^(2)·g^(-1),the pore volume is up to 1.33 cm^(3)·g^(-1),the content of mespores with diameter of 6-8 nm is significantly increased,and the pore size distribution is wide and uniform.When the current density increases from 0.1 to 10 A·g^(-1),the gravimetric capacitance decreases from 219 to 186 F·g^(-1)with a capacitance retention of 84.9%,the equivalent series resistance is very small,and the rate performance and reversibility of charging and discharging have also been excellent.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
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
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
In this work,we investigate how activated carbon(AC)derived from olive pomace biomass can be used as an anode material in lithium-ion batteries.The biomass-derived activated carbon has the potential to be highly effic...In this work,we investigate how activated carbon(AC)derived from olive pomace biomass can be used as an anode material in lithium-ion batteries.The biomass-derived activated carbon has the potential to be highly efficient,deliver high performance,sustainable,and cost-effective in LIBs-related production.The activated carbon is prepared by using H3PO4 as a chemical activation agent,and then calcining the obtained product at 500℃ for different controlled atmospheres under(i)air(AC-Atm),(ii)vacuum(AC-Vac),and(iii)argon(ACArg).The different samples were systematically analyzed using scanning electron microscopy(SEM),Highresolution transmission electron microscopy(HRTEM),energy dispersive spectroscopy(EDS),X-ray fluores-cence(XRF),X-ray diffraction(XRD),FT-IR and Raman spectroscopy,and thermogravimetric analysis(TGA)to assess their properties.The electrochemical properties of the carbonaceous materials were studied by galvano-static cycling,cyclic voltammetry(CV),and electrochemical impedance spectroscopy(EIS).The results showed high specific capacity and stable cycling performance,with capacities of 288,184,and 56 mAh g^(-1) at the current density of 25 mA g^(-1) after 70 cycles for AC-Arg,AC-Vac,and AC-Atm respectively.Furthermore,the CE efficiency was nearly 100%from the first cycles.This study opens up interesting prospects and offers promising oppor-tunities for more efficient recovery of unused olive pomace waste,by integrating it into energy storage appli-cations,particularly sustainable lithium-ion batteries.展开更多
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
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
Cresyl diphenyl phosphate(CDP),an emerging aryl organophosphate ester(OPE),exhibits potential toxic effects and is frequently found in diverse environmental media,thereby raising concerns about environmental pollution...Cresyl diphenyl phosphate(CDP),an emerging aryl organophosphate ester(OPE),exhibits potential toxic effects and is frequently found in diverse environmental media,thereby raising concerns about environmental pollution.Biodegradation demonstrates substantial potential for CDP removal from the environment.This study investigated the biodegradation mechanisms of CDP using anaerobic activated sludge(AnAS).The biodegradation of 1-mg/L CDP followed a first-order kinetic model with a degradation kinetic constant of 0.943 d^(-1),and the addition of different electron acceptors affected the degradation rate.High-resolution mass spectrometry identified seven transformation products(TPs)of CDP.The pathways of CDP degradation in anaerobic conditions were proposed,with carboxylation products being the most dominant intermediate products.The structure of the anaerobic microbial community at different degradation time points in CDP-amended microcosms was examined.The linear discriminant analysis(LDA)of effect size(LEfSe)potentially underscored the pivotal role of Methyloversatilis in CDP biodegradation.Zebrafish embryotoxicity experiments revealed both lethal and morphogenetic impacts of CDP on zebrafish embryos.The survival rate,hatching rate,and body length indicators of zebrafish embryos underscored the detoxification of CDP and its resultant intermediates by AnAS.This study offers new insights into the fate and biodegradation mechanisms of CDP in wastewater treatment plants.展开更多
As a key step in waste activated sludge(WAS)treatment and disposal,WAS dewatering can minimize the amount of WAS and decrease the costs of transportation,storage management,treatment,and disposal.Advanced oxidation pr...As a key step in waste activated sludge(WAS)treatment and disposal,WAS dewatering can minimize the amount of WAS and decrease the costs of transportation,storage management,treatment,and disposal.Advanced oxidation processes(AOPs)have been widely explored in WAS dewatering due to the excellent oxidizing properties and efficient decomposition capacity since the 21^(st)century.This review outlined the mechanisms of AOPs to improve WAS dewatering and pointed out the shortcomings of the existing mechanisms.Then,the applications of AOPs-based WAS dewatering processes for enhanced WAS dewatering were reviewed,and the intrinsic limitations of AOPs-based WAS dewatering processes in engineering applications were proposed.In addition,an overall review of AOPs-based WAS dewatering researches was also conducted through bibliometric analysis,and future research hotspots in the field of AOPs-based WAS dewatering were proposed.Finally,the positive effects of the AOPs-based WAS dewatering processes on pollutant removal and resource recovery were investigated,and an integrated plan for the harmless disposal of WAS was constructed to achieve a positive reform of the traditional WAS management plan.This review provided theoretical basis and technical reference for the development of efficient,economical,and environmental AOPs for enhanced WAS dewatering to facilitate the application of AOPs in actual WAS dewatering engineering.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
This study addresses the challenges posed by dispersive soil in various engineering fields,including hydraulic and agricultural engineering,by exploring the effects of physical adsorption on soil modification.The prim...This study addresses the challenges posed by dispersive soil in various engineering fields,including hydraulic and agricultural engineering,by exploring the effects of physical adsorption on soil modification.The primary objective is to identify an environmentally friendly stabilizer that can alleviate cracking and erosion resulting from soil dispersivity.Activated carbon(AC),known for its porous nature,was examined for its potential to enhance soil strength and erosion resistance.The charge neutralization process was evaluated by monitoring pH and conductivity,in addition to a comprehensive analysis of microscopic and mineral properties.The results show that high sodium levels or low clay contents result in the dispersive nature of soil in water.However,the incorporation of AC can transform such soil into a non-dispersive state.Moreover,both soil strength and erosion resistance exhibited enhancements with increasing AC content and curing duration.The incorporation of AC resulted in a maximum 5.6-fold increase in unconfined compressive strength and a 1.8-fold increase in tensile strength for dispersive soil.Notably,a significant correlation was observed during the curing phase among soil dispersivity,mechanical properties,and pH values.Microscopic analyses revealed that the porous structure of AC facilitated a filling effect and enhanced adsorption capacity,which contributed to improved soil characteristics and reduced dispersivity.The release of hydrogen ions and the formation of aggregates promote water stability.Validation tests conducted on dispersive soil from northern Shaanxi demonstrated the efficacy of physical adsorption using AC as a viable method for modifying dispersive soil in the water conservancy hub.展开更多
Synergistic therapy using multiple modalities is a highly promising therapeutic strategy.Near-infrared-Ⅱ(NIR-Ⅱ)fluorescence imaging,with its deep penetration and high fidelity,has frequently been employed in the lit...Synergistic therapy using multiple modalities is a highly promising therapeutic strategy.Near-infrared-Ⅱ(NIR-Ⅱ)fluorescence imaging,with its deep penetration and high fidelity,has frequently been employed in the literature to guide and assist treatment.Herein,we report the development of a NIR-Ⅱfluorescence imaging guided multi-therapy platform PDI-DS NPs,which integrates a novel activatable phototheranostic agent PDI-DBU,a H_(2)S donor DPS and an amphiphilic polymer DSPE-m PEG2000.In order to maximize redshift of absorption and emission of PDI derivatives,we introduced an electron donating group DBU on PDI to obtain PDI-DBU.PDI-DBU exhibits a distinct absorption band at 700-900 nm and demonstrates excellent NIR-Ⅱfluorescence emission/imaging properties and good photothermal effects under 808 nm laser irradiation.More importantly,under 808 nm laser irradiation,PDI-DBU could be oxidized,and the photodynamic effect of the material could be subsequently activated under 530 nm laser irradiation,achieving the combination of photothermal and activatable photodynamic dual modality treatment.The H_(2)S donor DPS,when triggered by the abundant glutathione(GSH)within the tumor microenvironment(TME),is capable of generating H_(2)S.On one hand,H_(2)S can inhibit tumor growth by disrupting mitochondrial function,on the other hand,it can also repress the expression of heat shock protein 90(HSP90),thereby reversing tumor cell resistance mechanism against photothermal therapy.The utilization of PDI-DS NPs combined with DPS for efficient tumor ablation has been successfully demonstrated both in vitro and in vivo.This synergistic therapeutic platform thus offers a promising strategy in the field of NIR-Ⅱfluorescence imaging guided tumor therapy.展开更多
文摘Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because it has a high specific surfacearea for sulfur loading.We have developed a pressurizedphysical activation(PPA)method that producedan activated carbon(PPAC)with a high specific surfacearea comparable to that of CAC.The pore structure of PPAC could be changed and its use as a cathode material for Li–Sbatteries was investigated.Battery tests at different capacity rates(C-rates)showed that it had a much improved high-rate performancewith a discharge capacity of 900 mAh/(g of sulfur)at 1 C,in contrast to only 600 mAh/(g of sulfur)for CAC.Porestructure analyses showed that PPAC prepared at a high activation temperature(1000℃)had unusual channel-like mesoporesbetween the microdomains that are the basic structural units of artificial carbon materials.These are connected to microporesdeveloped in each microdomain,and deliver ions from the surroundings to the internal pores and vice versa.The well-developedmicropores and mesopores of PPAC respectively ensured the high adsorption of lithium polysulfides and a high rate ofion diffusion.Compared to CAC,PPAC is a high-performance,low-cost cathode material that is promising for use in futureLi–S batteries.
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.
文摘A series of blue and blue‑green Ir(Ⅲ)complexes has been investigated theoretically to explore their electronic structures,photophysical properties,efficiency roll‑off effect,and thermal activation delayed fluorescence(TADF)properties.All calculations were performed using density functional theory(DFT)and time‑dependent density functional theory(TDDFT).Calculations for electronic structures,frontier molecular orbital characteristics(which determine the efficiency roll‑off effect of the complexes),and photophysical properties were conducted using the Gaussian 09 software package.The calculation of spin‑orbit coupling matrix elements<T|HSOC|S>,which determine the TADF properties of the complexes,was performed using the ORCA software package.The calculation results show that the auxiliary ligand tetraphenylimidodiphosphinate(tpip),a strong electron‑withdrawing group,can mitigate the efficiency roll‑off effect of the complex.Furthermore,TADF is observed in one of the designed complexes,(F_(3)Phppy)_(2)Ir(tpip),where F_(3)Phppy=2‑[4‑(2,4,6‑trifluorophenyl)phenyl]pyridine.
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 Yunnan Major Scientific and Technological Projects(No.202202AG050005)Yunnan Fundamental Research Projects(No.202101BE070001-001).
文摘The ACF adsorbent with high Cu loading was treated with dielectric barrier discharge plasma to mitigate the negative effects of high Cu loading and enhance PH_(3)and H_(2)S adsorption and oxidation.Bruno-Emmett-Taylor(BET)result showed that the specific surface area of the adsorbent after air plasma modification was almost three times that before modification.X-ray photoelectron spectroscopy(XPS)findings revealed that the amino group was added to the adsorbent's surface,increasing lattice oxygen and chemisorbed oxygen.The adsorbent's large specific surface area,excellent surface active oxygen,and abundance of basic groups facilitate PH_(3)and H_(2)S adsorption and oxidation.The scanning electron microscopy showed that air plasma modification exposed more active components and uniformly dispersed them on the surface of adsorbent,thereby improving the adsorption performance.Activity evaluation results showed that the adsorbent has the best ability to capture PH_(3)and H_(2)S after being modified by air plasma at 4 kV voltage for 10 min.The adsorbent's breakthrough ability at high space velocity(WHSV:60,000 h^(−1))is 190 mg P/g and 146 mg S/g,respectively,which is 74%and 60%greater than that before modification.This is a great improvement over previous studies.In addition,the possible mechanism of adsorbent deactivation was proposed.
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.
基金supported by the Key Technology Research and Development Program of Shandong(No.2020CXGC011406)the National Natural Science Foundation of China(No.22076091)the State Key Joint Laboratory of Environment Simulation and Pollution Control,China(No.21L01ESPC).
文摘Control of N-nitrosodimethylamine(NDMA)in drinking water could be achieved by removing its precursors as one practical way.Herein,superfine powdered activated carbons with a diameter of about 1μm(SPACs)were successfully prepared by grinding powdered activated carbon(PAC,D50=24.3μm)and applied to remove model NDMA precursors,i.e.ranitidine(RAN)and nizatidine(NIZ).Results fromgrain diameter experiments demonstrated that the absorption velocity increased dramatically with decreasing particle size,and the maximum increase in k2 was 26.8-folds for RAN and 33.4-folds for NIZ.Moreover,kinetic experiments explained that rapid absorption could be attributed to the acceleration of intraparticle diffusion due to the shortening of the diffusion path.Furthermore,performance comparison experiments suggested that the removal of RAN and NIZ(C_(0)=0.5 mg/L)could reach 61.3%and 60%,respectively,within 5 min,when the dosage of SAPC-1.1(D_(50)=1.1μm)was merely 5 mg/L,while PAC-24.3 could only eliminate 17.5%and 18.6%.The adsorption isotherm was well defined by Langmuir isotherm model,indicating that the adsorption of RAN/NIZ was a monolayer coverage process.The adsorption of RAN or NIZ by SAPC-1.1 and PAC-24.3 was strongly pH dependent,and high adsorption capacity could be observed under the condition of pH>pk_(a)+1.The coexistence of humic acid(HA)had no significant effect on the adsorption performance because RAN/NIZ may be coupled with HA and removed simultaneously.The coexistence of anions had little effect on the adsorption also.This study is expected to provide an alternative strategy for drinking water safety triggered by NDMA.
基金supported by the Science and Technology Support Plan for Youth Innovation of Colleges and Universities of Shandong Province of China(2023KJ122)State Grid Shandong Electric Power Company Science and Technology Project(520618240009)Doctoral Research Fund of Shandong Jianzhu University(XNBS1838).
文摘High electrochemical performance supercapacitors require activated carbon with high specific surface area,suitable pore size distribution and surface properties,and high electrical conductivity as electrode materials,whereas there exists a trade-off relationship between specific surface area and electrical conductivity,which is not well met by a single type of carbon source.To solve this problem,the coal and sargassum are adopted to obtain the coupling product via co-thermal dissolution,followed by carbonization and KOH activation.The effects of mixing mass ratio and activation temperature on the prepared activated carbon(AC)are investigated using single factor experimental method.The experimental results show that AC_(1/3-800)has abundant micropore and mesopore content,good pore structure connectivity,high electrical conductivity and good wettability,and superior electrochemical properties compared with other activated carbons prepared in this experiment.Its total specific surface area is up to 2098.5 m^(2)·g^(-1),the pore volume is up to 1.33 cm^(3)·g^(-1),the content of mespores with diameter of 6-8 nm is significantly increased,and the pore size distribution is wide and uniform.When the current density increases from 0.1 to 10 A·g^(-1),the gravimetric capacitance decreases from 219 to 186 F·g^(-1)with a capacitance retention of 84.9%,the equivalent series resistance is very small,and the rate performance and reversibility of charging and discharging have also been excellent.
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)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.
文摘In this work,we investigate how activated carbon(AC)derived from olive pomace biomass can be used as an anode material in lithium-ion batteries.The biomass-derived activated carbon has the potential to be highly efficient,deliver high performance,sustainable,and cost-effective in LIBs-related production.The activated carbon is prepared by using H3PO4 as a chemical activation agent,and then calcining the obtained product at 500℃ for different controlled atmospheres under(i)air(AC-Atm),(ii)vacuum(AC-Vac),and(iii)argon(ACArg).The different samples were systematically analyzed using scanning electron microscopy(SEM),Highresolution transmission electron microscopy(HRTEM),energy dispersive spectroscopy(EDS),X-ray fluores-cence(XRF),X-ray diffraction(XRD),FT-IR and Raman spectroscopy,and thermogravimetric analysis(TGA)to assess their properties.The electrochemical properties of the carbonaceous materials were studied by galvano-static cycling,cyclic voltammetry(CV),and electrochemical impedance spectroscopy(EIS).The results showed high specific capacity and stable cycling performance,with capacities of 288,184,and 56 mAh g^(-1) at the current density of 25 mA g^(-1) after 70 cycles for AC-Arg,AC-Vac,and AC-Atm respectively.Furthermore,the CE efficiency was nearly 100%from the first cycles.This study opens up interesting prospects and offers promising oppor-tunities for more efficient recovery of unused olive pomace waste,by integrating it into energy storage appli-cations,particularly sustainable lithium-ion batteries.
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(Grants No.52270155 and 92047201).
文摘Cresyl diphenyl phosphate(CDP),an emerging aryl organophosphate ester(OPE),exhibits potential toxic effects and is frequently found in diverse environmental media,thereby raising concerns about environmental pollution.Biodegradation demonstrates substantial potential for CDP removal from the environment.This study investigated the biodegradation mechanisms of CDP using anaerobic activated sludge(AnAS).The biodegradation of 1-mg/L CDP followed a first-order kinetic model with a degradation kinetic constant of 0.943 d^(-1),and the addition of different electron acceptors affected the degradation rate.High-resolution mass spectrometry identified seven transformation products(TPs)of CDP.The pathways of CDP degradation in anaerobic conditions were proposed,with carboxylation products being the most dominant intermediate products.The structure of the anaerobic microbial community at different degradation time points in CDP-amended microcosms was examined.The linear discriminant analysis(LDA)of effect size(LEfSe)potentially underscored the pivotal role of Methyloversatilis in CDP biodegradation.Zebrafish embryotoxicity experiments revealed both lethal and morphogenetic impacts of CDP on zebrafish embryos.The survival rate,hatching rate,and body length indicators of zebrafish embryos underscored the detoxification of CDP and its resultant intermediates by AnAS.This study offers new insights into the fate and biodegradation mechanisms of CDP in wastewater treatment plants.
基金funded under the auspices of the National Key Research and Development Program of China(No.2023YFC3207404-01)the Postdoctoral Fellowship Program of CPSF(No.GZC20233450)the Heilongjiang Province Postdoctoral Science Foundation(No.LBHZ23154)。
文摘As a key step in waste activated sludge(WAS)treatment and disposal,WAS dewatering can minimize the amount of WAS and decrease the costs of transportation,storage management,treatment,and disposal.Advanced oxidation processes(AOPs)have been widely explored in WAS dewatering due to the excellent oxidizing properties and efficient decomposition capacity since the 21^(st)century.This review outlined the mechanisms of AOPs to improve WAS dewatering and pointed out the shortcomings of the existing mechanisms.Then,the applications of AOPs-based WAS dewatering processes for enhanced WAS dewatering were reviewed,and the intrinsic limitations of AOPs-based WAS dewatering processes in engineering applications were proposed.In addition,an overall review of AOPs-based WAS dewatering researches was also conducted through bibliometric analysis,and future research hotspots in the field of AOPs-based WAS dewatering were proposed.Finally,the positive effects of the AOPs-based WAS dewatering processes on pollutant removal and resource recovery were investigated,and an integrated plan for the harmless disposal of WAS was constructed to achieve a positive reform of the traditional WAS management plan.This review provided theoretical basis and technical reference for the development of efficient,economical,and environmental AOPs for enhanced WAS dewatering to facilitate the application of AOPs in actual WAS dewatering engineering.
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financially supported by the National Postdoctoral Program for Innovative Talents(Grant No.BX20200287)the National Natural Science Foundation of China(Grant Nos.52079116 and 52378322).
文摘This study addresses the challenges posed by dispersive soil in various engineering fields,including hydraulic and agricultural engineering,by exploring the effects of physical adsorption on soil modification.The primary objective is to identify an environmentally friendly stabilizer that can alleviate cracking and erosion resulting from soil dispersivity.Activated carbon(AC),known for its porous nature,was examined for its potential to enhance soil strength and erosion resistance.The charge neutralization process was evaluated by monitoring pH and conductivity,in addition to a comprehensive analysis of microscopic and mineral properties.The results show that high sodium levels or low clay contents result in the dispersive nature of soil in water.However,the incorporation of AC can transform such soil into a non-dispersive state.Moreover,both soil strength and erosion resistance exhibited enhancements with increasing AC content and curing duration.The incorporation of AC resulted in a maximum 5.6-fold increase in unconfined compressive strength and a 1.8-fold increase in tensile strength for dispersive soil.Notably,a significant correlation was observed during the curing phase among soil dispersivity,mechanical properties,and pH values.Microscopic analyses revealed that the porous structure of AC facilitated a filling effect and enhanced adsorption capacity,which contributed to improved soil characteristics and reduced dispersivity.The release of hydrogen ions and the formation of aggregates promote water stability.Validation tests conducted on dispersive soil from northern Shaanxi demonstrated the efficacy of physical adsorption using AC as a viable method for modifying dispersive soil in the water conservancy hub.
基金supported by the National Natural Science Foundation of China(No.22274148)the Science and Technology Development Foundation of Jilin Province(Nos.20220204098YY,20230402045GH,20230402018GH,YDZJ202201ZYTS359,YDZJ202201ZYTS351,20240404070ZP,SKL202302030)the Jilin Province Development and Reform Commission’s Innovation Capacity Building Program(No.2023C041-8)。
文摘Synergistic therapy using multiple modalities is a highly promising therapeutic strategy.Near-infrared-Ⅱ(NIR-Ⅱ)fluorescence imaging,with its deep penetration and high fidelity,has frequently been employed in the literature to guide and assist treatment.Herein,we report the development of a NIR-Ⅱfluorescence imaging guided multi-therapy platform PDI-DS NPs,which integrates a novel activatable phototheranostic agent PDI-DBU,a H_(2)S donor DPS and an amphiphilic polymer DSPE-m PEG2000.In order to maximize redshift of absorption and emission of PDI derivatives,we introduced an electron donating group DBU on PDI to obtain PDI-DBU.PDI-DBU exhibits a distinct absorption band at 700-900 nm and demonstrates excellent NIR-Ⅱfluorescence emission/imaging properties and good photothermal effects under 808 nm laser irradiation.More importantly,under 808 nm laser irradiation,PDI-DBU could be oxidized,and the photodynamic effect of the material could be subsequently activated under 530 nm laser irradiation,achieving the combination of photothermal and activatable photodynamic dual modality treatment.The H_(2)S donor DPS,when triggered by the abundant glutathione(GSH)within the tumor microenvironment(TME),is capable of generating H_(2)S.On one hand,H_(2)S can inhibit tumor growth by disrupting mitochondrial function,on the other hand,it can also repress the expression of heat shock protein 90(HSP90),thereby reversing tumor cell resistance mechanism against photothermal therapy.The utilization of PDI-DS NPs combined with DPS for efficient tumor ablation has been successfully demonstrated both in vitro and in vivo.This synergistic therapeutic platform thus offers a promising strategy in the field of NIR-Ⅱfluorescence imaging guided tumor therapy.
