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
The recycling of waste activated carbon is of great significance in environmental protection.Porous mullite ceramics were prepared by impregnating the mullite precursor with activated carbon,adding a pore-forming agen...The recycling of waste activated carbon is of great significance in environmental protection.Porous mullite ceramics were prepared by impregnating the mullite precursor with activated carbon,adding a pore-forming agent,and adopting aluminum sulfate octahydrate,ammonia and silica micropowder as raw materials,waste activated carbon after heat treatment as the pore-forming agent,and sodium polyacrylate(PAAS)as the dispersant.The effects of the activated carbon additions(1.5%,3.0%,5.2%,and 7.8%,by mass)and PAAS additions(1%,2%,and 3%,extra adding,by mass)on the physical properties,phase composition and microstructure of the porous ceramics were studied.The results show that:(1)as a pore-forming agent,activated carbon promotes the formation of pores inside the samples,while the apparent porosity of the samples increases significantly with the increasing activated carbon addition;when the activated carbon addition is 7.8%,the apparent porosity of the sample is 65.7%,the cold compressive strength is 4.62 MPa,the peak pore size is around 3.5μm,and the pore size distribution is uniform;(2)appropriate PAAS helps to improve the dispersion of activated carbon in the samples and the comprehensive performance of the porous mullite ceramics;when the PAAS addition is 2%,the apparent porosity of the sample is 71.8%,the cold compressive strength is 5.53 MPa,the peak pore size is around 3μm,and the pore size distribution is optimized;however,excessive PAAS increases the liquid phase in the system,resulting in over sintering of mullite and a decrease in the porosity.展开更多
The development of polymeric materials that exhibit blue thermally activated delayed fluorescence(TADF)is of great interest for optoelectronic applications.However,achieving TADF in polymers often requires an elaborat...The development of polymeric materials that exhibit blue thermally activated delayed fluorescence(TADF)is of great interest for optoelectronic applications.However,achieving TADF in polymers often requires an elaborate monomer design.The high-energy local triplet state(^(3)LE)of carbazole complicates its application despite the molecular orbital arrangement being suitable for blue emission.Here,we present an approach to polymer design that makes it possible to solve this problem.We demonstrate the in situ formation of a TADF donor-acceptor system during Suzuki polycondensation,creating an extended carbazole-based donor matrix coupled with a triazine acceptor.The resulting polymer exhibited efficient TADF with a low energy gap(ΔE_(ST))value if a phenyl N-substituent,enabling essential electron delocalization,was present in the carbazole moiety.This work establishes a versatile platform for developing carbazole-based TADF polymers,overcoming the fundamental limitations that hinder their widespread application.展开更多
Although activated carbon filters are thought to be the best way to remove per-and polyfluorinated alkyl substances(PFAS),it is yet unknown how biofilms affect PFAS removal.This study first examined how the removal of...Although activated carbon filters are thought to be the best way to remove per-and polyfluorinated alkyl substances(PFAS),it is yet unknown how biofilms affect PFAS removal.This study first examined how the removal of PFAS in full-scale drinking water treatment plants(DWTPs)was impacted by biofilm from biological activated carbon(BAC)of varying depths and carbon ages.PFAS desorption from BAC was visible,but at this point,BAC could still remove dissolved organic matter(DOM)efficiently.Studies have demonstrated that the use of activated carbon filters can dramatically lower the content of PFAS in water,with the amount of PFAS reducing as the filter’s depth grows and its use duration increases.Additionally,pore-clogging becomes more noticeable as the biofilm ages,which reduces BAC’s capacity to eliminate PFAS and hinders PFAS desorption.Furthermore,the adsorption process of PFAS may be impeded by the secretion of biofilms,which are composed of proteins and polysaccharides.Based on the analysis above,it can be the adsorption of PFAS by BAC is significantly inhibited by biofilms,according to another research.This provides theoretical direction for improving the removal effectiveness of PFAS in DWTPs.展开更多
The increasing demand for flexible displays and wearable electronics has driven extensive efforts to develop stretchable organic lightemitting diodes(OLEDs).A critical challenge in this field is the creation of emissi...The increasing demand for flexible displays and wearable electronics has driven extensive efforts to develop stretchable organic lightemitting diodes(OLEDs).A critical challenge in this field is the creation of emissive layers that combine high efficiency with mechanical robustness.Thermally activated delayed fluorescence(TADF)materials have attracted significant attention as third-generation emitters capable of achieving 100%internal quantum efficiency;however,their application in stretchable OLEDs has been limited.In this study,we propose an elastomer doping strategy.Polyurethane(PU)is incorporated into TADF polymers to improve their mechanical flexibility while maintaining a high luminescent efficiency.The resulting composite films exhibited excellent TADF characteristics and remarkable stretchability(75%).OLEDs fabricated from these materials achieved a maximum external quantum efficiency(EQE)of 14.26%and a peak luminance of 73570 cd·m^(-2),with the PUdoped devices showing a significantly suppressed efficiency roll-off.Additionally,a fully stretchable OLED architecture was designed and operated under tensile strain to maintain stable electroluminescent performance.These results demonstrate that elastomer doping is an effective strategy for balancing the mechanical compliance with optoelectronic performance,offering a promising pathway for the development of high-performance stretchable OLEDs for flexible electronics.展开更多
Engineering the pore structure of biomass-derived activated carbons is critical for optimizing their performance in adsorptionbased applications.This study demonstrates for the first time that washing hydrochars in so...Engineering the pore structure of biomass-derived activated carbons is critical for optimizing their performance in adsorptionbased applications.This study demonstrates for the first time that washing hydrochars in solvents of different polarity before activation is a simple yet powerful strategy to tailor pore size distribution.Hydrochar is produced from spent coffee grounds via hydrothermal carbonization,followed by washing in various solvents and activation in KOH.This results in carbons with a very large surface area(~2700 m^(2)/g),and washing is demonstrated to significantly increase product yield.Furthermore,washing in non-polar or mixed-polarity solvents removes long-chain carboxylic acids and esters from the hydrochar,promoting the development of narrow micropores while suppressing mesopore formation.To illustrate the impact of this structural control of porous carbons,post-combustion CO_(2)capture is investigated as a case study.Narrower pore size distribution enhances CO_(2)uptake,significantly improving capacity from 2.8 mmol/g for unwashed samples to 3.8 mmol/g for acetone-washed samples.Interestingly,moderate pore size(9-12Å)is shown to be optimal for CO_(2):N2 selectivity,while smaller pores result in lower selectivity due to stronger interactions between N2 and the pore walls.These findings highlight the potential role of solvent washing in directing pore architecture of hydrochars for adsorption-based carbon capture technologies and beyond.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
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
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
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
Nitrogen-doped activated carbon(N-AC)was successfully prepared by KOH-activation and nitrogen doping using ammonia(NH3)heat treatment.Coconut shell-derived activated carbon(AC)was heat-treated under NH3 gas in the tem...Nitrogen-doped activated carbon(N-AC)was successfully prepared by KOH-activation and nitrogen doping using ammonia(NH3)heat treatment.Coconut shell-derived activated carbon(AC)was heat-treated under NH3 gas in the temperature range of 700℃-900℃.Likewise,the mixture of potassium hydroxide(KOH)and AC was heated at 800℃,followed by heat treatment underNH3 gas at 800℃(hereafter referred to asKOH-N-AC800).Scanning electron microscopy(SEM),Raman spectroscopy,X-ray photoelectron spectroscopy(XPS)and Brunauer-Emmett-Teller(BET)method were utilized to analyze morphology,crystallinity,chemical bonding,chemical composition and surface area.The surface area and porosity of N-AC increased with increasing NH3 heat treatment.Similarly,the nitrogen content in the N-AC increased from 3.23%to 4.84 at%when the NH3 heat treatment was raised from 700℃ to 800℃.However,the nitrogen content of N-AC decreased to 3.40 at% after using NH3 heat treatment at 900℃.The nitrogen content of KOH-N-AC800 is 5.43 at%.KOH-N-AC800 and N-AC800 exhibited improvements of 33.66% and 26.24%,respectively,in CO_(2) adsorption compared with AC.The enhancement of CO_(2) adsorption of KOH-N-AC800 is attributed to the synergic effect of the nitrogen doping,high surface area,and porosity.The results exhibited that nitrogen sites on the surface play a more significant role in CO_(2) adsorption than surface area and porosity.This work proposes the potential synergistic effect of KOH-activation and nitrogen doping for enhancing the CO_(2) adsorption capacity of activated carbon.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
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
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
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The recycling of waste activated carbon is of great significance in environmental protection.Porous mullite ceramics were prepared by impregnating the mullite precursor with activated carbon,adding a pore-forming agent,and adopting aluminum sulfate octahydrate,ammonia and silica micropowder as raw materials,waste activated carbon after heat treatment as the pore-forming agent,and sodium polyacrylate(PAAS)as the dispersant.The effects of the activated carbon additions(1.5%,3.0%,5.2%,and 7.8%,by mass)and PAAS additions(1%,2%,and 3%,extra adding,by mass)on the physical properties,phase composition and microstructure of the porous ceramics were studied.The results show that:(1)as a pore-forming agent,activated carbon promotes the formation of pores inside the samples,while the apparent porosity of the samples increases significantly with the increasing activated carbon addition;when the activated carbon addition is 7.8%,the apparent porosity of the sample is 65.7%,the cold compressive strength is 4.62 MPa,the peak pore size is around 3.5μm,and the pore size distribution is uniform;(2)appropriate PAAS helps to improve the dispersion of activated carbon in the samples and the comprehensive performance of the porous mullite ceramics;when the PAAS addition is 2%,the apparent porosity of the sample is 71.8%,the cold compressive strength is 5.53 MPa,the peak pore size is around 3μm,and the pore size distribution is optimized;however,excessive PAAS increases the liquid phase in the system,resulting in over sintering of mullite and a decrease in the porosity.
基金supported by the Russian Science Foundation (No. 25-13-00300)the Centre for Optical and Laser Materials Research (SPbSU) and Saint Petersburg State University for measuring the quantum yields of luminescence within the framework of research project(No.125021902439-8)。
文摘The development of polymeric materials that exhibit blue thermally activated delayed fluorescence(TADF)is of great interest for optoelectronic applications.However,achieving TADF in polymers often requires an elaborate monomer design.The high-energy local triplet state(^(3)LE)of carbazole complicates its application despite the molecular orbital arrangement being suitable for blue emission.Here,we present an approach to polymer design that makes it possible to solve this problem.We demonstrate the in situ formation of a TADF donor-acceptor system during Suzuki polycondensation,creating an extended carbazole-based donor matrix coupled with a triazine acceptor.The resulting polymer exhibited efficient TADF with a low energy gap(ΔE_(ST))value if a phenyl N-substituent,enabling essential electron delocalization,was present in the carbazole moiety.This work establishes a versatile platform for developing carbazole-based TADF polymers,overcoming the fundamental limitations that hinder their widespread application.
基金supported by the National Key Research and Development Program of China(No.2022YFC3203703)the National Natural Science Foundation of China(No.52270013).
文摘Although activated carbon filters are thought to be the best way to remove per-and polyfluorinated alkyl substances(PFAS),it is yet unknown how biofilms affect PFAS removal.This study first examined how the removal of PFAS in full-scale drinking water treatment plants(DWTPs)was impacted by biofilm from biological activated carbon(BAC)of varying depths and carbon ages.PFAS desorption from BAC was visible,but at this point,BAC could still remove dissolved organic matter(DOM)efficiently.Studies have demonstrated that the use of activated carbon filters can dramatically lower the content of PFAS in water,with the amount of PFAS reducing as the filter’s depth grows and its use duration increases.Additionally,pore-clogging becomes more noticeable as the biofilm ages,which reduces BAC’s capacity to eliminate PFAS and hinders PFAS desorption.Furthermore,the adsorption process of PFAS may be impeded by the secretion of biofilms,which are composed of proteins and polysaccharides.Based on the analysis above,it can be the adsorption of PFAS by BAC is significantly inhibited by biofilms,according to another research.This provides theoretical direction for improving the removal effectiveness of PFAS in DWTPs.
基金supported by the National Natural Science Foundation of China(Nos.T2441002,22525506,U24A20137,and U22A6002)Strategic Priority Research Program of CAS(No.XDB0520101)+1 种基金National Key R&D Program of China(No.2023YFB3609000)CAS Project for Young Scientists in Basic Research(No.YSBR-053)。
文摘The increasing demand for flexible displays and wearable electronics has driven extensive efforts to develop stretchable organic lightemitting diodes(OLEDs).A critical challenge in this field is the creation of emissive layers that combine high efficiency with mechanical robustness.Thermally activated delayed fluorescence(TADF)materials have attracted significant attention as third-generation emitters capable of achieving 100%internal quantum efficiency;however,their application in stretchable OLEDs has been limited.In this study,we propose an elastomer doping strategy.Polyurethane(PU)is incorporated into TADF polymers to improve their mechanical flexibility while maintaining a high luminescent efficiency.The resulting composite films exhibited excellent TADF characteristics and remarkable stretchability(75%).OLEDs fabricated from these materials achieved a maximum external quantum efficiency(EQE)of 14.26%and a peak luminance of 73570 cd·m^(-2),with the PUdoped devices showing a significantly suppressed efficiency roll-off.Additionally,a fully stretchable OLED architecture was designed and operated under tensile strain to maintain stable electroluminescent performance.These results demonstrate that elastomer doping is an effective strategy for balancing the mechanical compliance with optoelectronic performance,offering a promising pathway for the development of high-performance stretchable OLEDs for flexible electronics.
基金supported by JST,grant number JPMJFS2132JST SPRING,grant number JPMJSP2136by an external research grant from Mitsubishi Fuso Truck&Bus Corporation。
文摘Engineering the pore structure of biomass-derived activated carbons is critical for optimizing their performance in adsorptionbased applications.This study demonstrates for the first time that washing hydrochars in solvents of different polarity before activation is a simple yet powerful strategy to tailor pore size distribution.Hydrochar is produced from spent coffee grounds via hydrothermal carbonization,followed by washing in various solvents and activation in KOH.This results in carbons with a very large surface area(~2700 m^(2)/g),and washing is demonstrated to significantly increase product yield.Furthermore,washing in non-polar or mixed-polarity solvents removes long-chain carboxylic acids and esters from the hydrochar,promoting the development of narrow micropores while suppressing mesopore formation.To illustrate the impact of this structural control of porous carbons,post-combustion CO_(2)capture is investigated as a case study.Narrower pore size distribution enhances CO_(2)uptake,significantly improving capacity from 2.8 mmol/g for unwashed samples to 3.8 mmol/g for acetone-washed samples.Interestingly,moderate pore size(9-12Å)is shown to be optimal for CO_(2):N2 selectivity,while smaller pores result in lower selectivity due to stronger interactions between N2 and the pore walls.These findings highlight the potential role of solvent washing in directing pore architecture of hydrochars for adsorption-based carbon capture technologies and beyond.
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 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.
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.
基金funded by Burapha University,grant number SDG 4/2568.
文摘Nitrogen-doped activated carbon(N-AC)was successfully prepared by KOH-activation and nitrogen doping using ammonia(NH3)heat treatment.Coconut shell-derived activated carbon(AC)was heat-treated under NH3 gas in the temperature range of 700℃-900℃.Likewise,the mixture of potassium hydroxide(KOH)and AC was heated at 800℃,followed by heat treatment underNH3 gas at 800℃(hereafter referred to asKOH-N-AC800).Scanning electron microscopy(SEM),Raman spectroscopy,X-ray photoelectron spectroscopy(XPS)and Brunauer-Emmett-Teller(BET)method were utilized to analyze morphology,crystallinity,chemical bonding,chemical composition and surface area.The surface area and porosity of N-AC increased with increasing NH3 heat treatment.Similarly,the nitrogen content in the N-AC increased from 3.23%to 4.84 at%when the NH3 heat treatment was raised from 700℃ to 800℃.However,the nitrogen content of N-AC decreased to 3.40 at% after using NH3 heat treatment at 900℃.The nitrogen content of KOH-N-AC800 is 5.43 at%.KOH-N-AC800 and N-AC800 exhibited improvements of 33.66% and 26.24%,respectively,in CO_(2) adsorption compared with AC.The enhancement of CO_(2) adsorption of KOH-N-AC800 is attributed to the synergic effect of the nitrogen doping,high surface area,and porosity.The results exhibited that nitrogen sites on the surface play a more significant role in CO_(2) adsorption than surface area and porosity.This work proposes the potential synergistic effect of KOH-activation and nitrogen doping for enhancing the CO_(2) adsorption capacity of activated carbon.
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 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 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.
