To efficiently remove radioactive nuclides from nuclear industry wastewater and minimize the generation of radioactive secondary waste,this study proposes the concept of a magnetically controlled microchannel adsorber...To efficiently remove radioactive nuclides from nuclear industry wastewater and minimize the generation of radioactive secondary waste,this study proposes the concept of a magnetically controlled microchannel adsorber based on magnetic adsorbents.A novel protocol for achieving high adsorption performance in microchannel adsorbers with periodically distributed particles is developed using the particle-resolved computational fluid dynamics (CFD) method,which addresses the limitations of traditional porous media flow models.To align simulation results more closely with practical scenarios,a typical high-efficiency magnetic adsorbent,magnetic sodium alginate/cobalt-based Prussian blue (M-SA/PB-Co),was synthesized.The M-SA/PB-Co microspheres exhibit a uniform size distribution (300–600 μm),and their Cs^(+) adsorption follows the pseudo-second-order kinetic model with a Langmuir saturated adsorption capacity of 124.84 mg·g^(-1).The performance parameters of M-SA/PB-Co,obtained from characterization and adsorption experiments,were integrated into CFD simulations.CFD results indicate that as the flow velocity increases,the flow field gradually transitions with vortices expanding in scale and streamline bifurcation points shifting rearward.The Cs^(+) concentration decreases progressively along the flow direction,with a more pronounced reduction in the vortex regions downstream of particles.The characteristic velocity and characteristic concentration of specific regions surrounding the particles were extracted based on boundary layer distribution.The amount of concentration reduction of Cs^(+) through particle is positively correlated with the characteristic concentration and negatively correlated with the characteristic velocity.The number of microspheres required in the microchannel adsorber was optimized using the response surface method.Compared with industrial fixed-bed adsorbers,microchannel adsorbers exhibit 8–10 times higher processing capacity,demonstrating significant industrial application potential.展开更多
Economical and sustainable wastewater treatment techniques are highly demanded to alleviate the issues of clearwater scarcity globally.In this work,the acetic acid/H_(2)O_(2) (AHP) was leveraged to enrich oxygenated f...Economical and sustainable wastewater treatment techniques are highly demanded to alleviate the issues of clearwater scarcity globally.In this work,the acetic acid/H_(2)O_(2) (AHP) was leveraged to enrich oxygenated functional groups on the biochar surface for efficient ciprofloxacin (CIP) adsorption and biochar regeneration (In situ degradation of CIP in the spent AHP solution).The AHP-modified biochar exhibited significantly enhanced CIP adsorption capacity,about 22 times that of the pristine biochar.The optimized modification condition (acetic acid/H_(2)O_(2):2.11,temperature:45 ℃,and time:12 h) was screened by the response surface method,reaching the highest CIP adsorption capacity of 86.26 mg·g^(−1).Characterization results revealed that the content of carboxyl —C=O—O was enhanced in AHP-modified biochar,which contributed to efficient CIP adsorption by the electrostatic interaction,hydrogen bonding,and hydrophobic interaction.The adsorption of modified biochar to CIP molecules was a spontaneous endothermic process,and in line with the pseudo-second-order model and the Langmuir isotherm model.Moreover,the biochar modification process enabled the spent AHP solution with a strong oxidizing agent of peracetic acid (PAA),which can be employed to degrade adsorbed CIP for biochar in-situ generation.This work tailored a closed-loop strategy for biochar oxidation,contaminant adsorption,and biochar regeneration,highlighting a viable route for sustainable wastewater treatment.展开更多
Flubendiamide is a commonly used pesticide with low water solubility and a high organic carbon sorption constant,causing it to adhere to soil particles and negatively impact soil ecosystems.First,chili plant stems,typ...Flubendiamide is a commonly used pesticide with low water solubility and a high organic carbon sorption constant,causing it to adhere to soil particles and negatively impact soil ecosystems.First,chili plant stems,typically discarded after the harvest season,represent an abundant local biomass resource with significant potential for utilization,and were converted into biochar through pyrolysis.Here,we describe the synthesis of biochar modified with iron and chitosan to increase the diversity of functions and surface functional groups of biochar.The resulting chitosan-modified magnetic biochar(CMBC)presents a full range of functional groups of chitosan and iron oxide as shown by Fourier-transform infrared spectroscopy.The correlation between flubendiamide concentration and the dose of biochar on adsorption was explored.The flubendiamide adsorption efficiency of CMBC(1%mass ratio of soil)reached 68.03%in 90 min.The highest adsorption capacity achieved was 0.95 mg·g^(−1).The flubendiamide adsorption mechanism by CMBC can be described with a pseudo-second-order kinetic model.The experiment data closely fit a Freundlich isotherm model(R^(2)=0.998),and the low residual sum of squares values demonstrate the high model applicability.In this study,we present a comprehensive overview of pesticides,alongside kinetic and isotherm model studies of flubendiamide adsorption by CMBC.We emphasize the potential of modified biochar to enhance environmental remediation applications.展开更多
In this study,chitosan(CS)was combined with microcrystalline cellulose(MCC)to fabricate composite hydrogel beads.These beads were further modified through blending and grafting with polyethyleneimine(PEI)to develop ch...In this study,chitosan(CS)was combined with microcrystalline cellulose(MCC)to fabricate composite hydrogel beads.These beads were further modified through blending and grafting with polyethyleneimine(PEI)to develop chitosan/microcrystalline cellulose@polyethyleneimine(CS/MCC@PEI)composite gel spheres for the efficient adsorption of diclofenac sodium(DS)from aqueous solutions.The adsorbent was characterized using scanning electron microscopy(SEM),X-ray diffraction(XRD),Fourier-transform infrared spectroscopy(FTIR),X-ray pho-toelectron spectroscopy(XPS),and thermogravimetric analysis(TGA).The CS/MCC@PEI composite exhibited a spherical morphology with a porous structure,abundant surface functional groups,and a high adsorption capac-ity of 274.84 mg/g for DS.Kinetic studies revealed that the adsorption process followed the pseudo-second-order model,dominated by physical adsorption,with both surface and internal diffusion influencing the adsorption rate.The Freundlich isotherm model best described the adsorption behavior,indicating multilayer adsorption on heterogeneous surfaces.Environmental adaptability tests demonstrated minimal interference from co-existing anions and humic acid,while regeneration experiments confirmed excellent reusability(>77%removal after five cycles).The adsorption mechanism involved electrostatic interactions and hydrogen bonding between the hydroxyl/amino groups of the composite and DS.These findings highlight the potential of CS/MCC@PEI as a cost-effective and sustainable adsorbent for DS removal from water.展开更多
The flotation separation of argentite from sphalerite using ammonium dibutyl dithiophosphate(ADD)was studied.Molecular simulation(MS)calculation shows that ADD is chemisorbed on argentite and sphalerite surface in the...The flotation separation of argentite from sphalerite using ammonium dibutyl dithiophosphate(ADD)was studied.Molecular simulation(MS)calculation shows that ADD is chemisorbed on argentite and sphalerite surface in the form of S—P bond.The ADD adsorption on argentite and sphalerite surface in Ag^(+)system was revealed by ICP,Zeta potential and XPS analyses.It is shown that the dissolved Ag^(+)from argentite surface can be absorbed on sphalerite surface in the form of silver hydroxide,and AgOH hydrophilic colloid prevents the adsorption of ADD on sphalerite surface.The ADD adsorption on argentite and sphalerite surface in the pulp containing silver and zinc ions was revealed by adsorption capacity and surface wettability analyses.It is shown that the combined Zn(OH)_(2) and AgOH hydrophilic colloid leads to greater ADD adsorption capacity on argentite surface and stronger surface hydrophobicity than sphalerite.Flotation tests demonstrate that ADD enables efficient separation of argentite from sphalerite in the pulp containing silver and zinc ions.展开更多
This study presents a thorough investigation into the use of single and twin-tailed cationic and anionic surfactant-modified chitosan(SMCS)hydrogel beads as effective adsorbents for the elimination of hazardous polycy...This study presents a thorough investigation into the use of single and twin-tailed cationic and anionic surfactant-modified chitosan(SMCS)hydrogel beads as effective adsorbents for the elimination of hazardous polycyclic aromatic hydrocarbons(PAHs)from aqueous solutions.The Chitosan(CS)hydrogel beads were modified with single/twin-tailed anionic surfactants,sodium dodecyl sulfate(SDS)and sodium bis(2-ethylhexyl)sulfosuccinate(AOT),and cationic surfactants,dodecyltrimethylammonium bromide(DTAB)and didodecyldimethylammonium bromide(DDAB),to enhance their adsorption capacity of PAHs.The CS and SMCS beads were evaluated for their structural,mechanical,and adsorption properties using a range of techniques,including infrared spectroscopy(IR),energy-dispersive X-ray spectroscopy(EDX),rheometry,and field emission scanning electron microscopy(FESEM).Adsorption experiments of naphthalene(Nap),acenaphthene(Ace),and phenanthrene(Phe)on SMCS beads demonstrate that they have significantly higher adsorption capacities than CS beads,due to increase in hydrophobic interactions.Adsorption capacity followed the trend,Phen>Ace>Nap for all the beads revealing that twin-tailed SMCS bead possess much higher adsorption capacities(Qmax)compared to single-tailed SMCS beads.For twin tailed surfactants,the maximum adsorption capacities for Nap,Ace and Phe varied as CS-AOT(CS-DDAB):430.0(323.8)611.60(538.18)633.39(536.99)mg/g respectively,outperforming other reported hydrogel beads.The study highlights the simplicity,eco-friendliness,and enhanced performance of surfactant modification for developing high-efficiency adsorbents,paving the way for cost-effective solutions in water re-mediation.展开更多
In order to address the evolving emission characteristics of oxygenated volatile organic compounds(OVOCs),it is essential to develop adsorbent materials specifically designed for the efficient adsorption of OVOCs with...In order to address the evolving emission characteristics of oxygenated volatile organic compounds(OVOCs),it is essential to develop adsorbent materials specifically designed for the efficient adsorption of OVOCs with large kinetic diameters.In this study,we used co-pyrolysis to prepare a series of graded porous carbon materials with well-developed micropores by adjusting the doping ratios of root nodules and pretreated cellulose.The material with root nodule to cellulose mass ratio of 1:1(TCC-RN-1)exhibited the highest saturated adsorption capacity for butyl acetate(834 mg/g).This can be attributed to enhanced pore size distribution from nodule doping,which facilitates the development of a micropore-graded structure.Additionally,the nodules acted as auxiliary activating agents that enhanced the KOH micropore regulation effect during the activation stage,resulting in the highest micropore volume(0.863 cm^(3)/g).The doping of root nodules facilitated the formation of additional defects on the surface of the porous carbon material,leading to a more disordered arrangement that improved pollutant adsorption.Furthermore,TCC-RN-1 demonstrated good thermal stability in an air atmosphere,main-taining a butyl acetate adsorption capacity exceeding 95%after five adsorption-desorption cycles.This indicates its favorable potential for industrial applications.展开更多
Aqueous zinc-ion batteries(AZIBs) are regarded as one of the most promising energy conversion and storage devices.Nevertheless,side reactions and dendrite growth on the zinc metal anode hinder their widespread applica...Aqueous zinc-ion batteries(AZIBs) are regarded as one of the most promising energy conversion and storage devices.Nevertheless,side reactions and dendrite growth on the zinc metal anode hinder their widespread application.In this study,hemin was employed as a multi-functional artificial interface for the first time to inhibit the disordered growth of zinc dendrites and mitigate side reactions.Theoretical calculations indicate that hemin is preferentially adsorbed onto the zinc anode,thus blocking the interaction between the active zinc anode and electrolyte.Compared with zinc foil,the Hemin@Zn anode demonstrates enhanced corrosion resistance,a decrease in hydrogen evolution,and more orderly deposition of zinc.As expected,the symmetric cell with Hemin@Zn anode can sustain up to 4000 h at 0.2 mA/cm^(2),0.2 mAh/cm^(2).Asymmetric Zn//Cu cells exhibit an average coulombic efficiency exceeding 99.72 % during 500 cycles.Moreover,the full cell Hemin@Zn//NH_(4)V_(4)O_(10) delivers a superior capacity up to 367 m Ah/g and the discharge capacity retention reaches 124 mAh/g after 1200 cycles even at a current density of 5 A/g.This work provides a simple and effective method for constructing a robust artificial interface to promote the application of long-life AZIBs.展开更多
The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightfor...The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightforward reduction approach was employed to design three bimetallic alloy nanoparticles(FeNi,FeCo,and NiCo)supported on multistage porous carbon substrates.Experimental and theoretical calculations reveal that the charge transfer within the alloy catalyst influences the position of its d-band center and its degree of hybridization with sodium polysulfides(NaPSs).An increased charge transfer leads to a shift of the alloy’s d-band center closer to the Fermi energy level,thereby enhancing its adsorption and catalytic capabilities.Among the three alloy compositions,the FeNi alloy exhibits the highest charge transfer.Consequently,the FeNi alloy demonstrates the superior electrochemical performance,achieving a high reversible specific capacity of 848.2 mA h g^(−1),with an average capacity degradation rate of only 0.037%per cycle over 1000 cycles at 1.2 C.The S/FeNi/NC cathode exhibits a low electrolyte-to-sulfur(E/S)ratio of 6.6µL mg^(−1),while maintaining a high reversible specific capacity of 568.1 mA h g^(−1).This offers valuable insights for the application of alloy catalysts in the S/FeNi/NC cathode of RT Na-S batteries.展开更多
Injecting impure CO_(2)for enhanced gas recovery(CO_(2)-EGR)offers a dual benefit by improving natural gas extraction while enabling CO_(2)sequestration.However,the interactions between CO_(2),N_(2),and CH_(4)under re...Injecting impure CO_(2)for enhanced gas recovery(CO_(2)-EGR)offers a dual benefit by improving natural gas extraction while enabling CO_(2)sequestration.However,the interactions between CO_(2),N_(2),and CH_(4)under reservoir conditions require further investigation.This study employs Grand Canonical Monte Carlo(GCMC)and Molecular Dynamics(MD)simulations to quantify the adsorption and diffusion behaviors of CO_(2),N_(2),and CH_(4)in quartz nanopores over a pressure range of 1-24 MPa under varying water saturations and gas compositions.The results indicate that:(1)CO_(2)exhibits the broadest energy distribution and the strongest adsorption stability,occupying about 20%-30%more adsorption sites than CH_(4)or N_(2)and showing the least sensitivity to water saturation,with only a 30%reduction at 50%saturation,compared to 60%for CH_(4),giving CO_(2)a clear competitive advantage.(2)The adsorption and desorption behaviors are strongly pressure dependent,as increasing pressure reduces the adsorption layer area and shifts gas distribution from adsorption dominated to free phase.Competitive adsorption analysis reveals that while CO_(2)dominates displacement at low pressures,mixtures that contain N_(2)achieve higher CH_(4)desorption efficiency above 13 MPa by mitigating diffusion resistance.(3)A higher N_(2)fraction improves CH_(4)diffusion coefficients,thereby facilitating gas mobility and ensuring superior recovery performance under high-pressure conditions.This study advances the fundamental knowledge of microscale gas behavior in tight sandstones and supports the feasibility of impure CO_(2)injection as a practical strategy for sustainable gas production.展开更多
Porous carbon microspheres are widely regarded as a superior CO_(2) adsorbent due to their exceptional efficiency and affordability.However,better adsorption performance is very attractive for porous carbon microspher...Porous carbon microspheres are widely regarded as a superior CO_(2) adsorbent due to their exceptional efficiency and affordability.However,better adsorption performance is very attractive for porous carbon microspheres.And modification of the pore structure is one of the effective strategies.In this study,multi-cavity mesoporous carbon microspheres were successfully synthesized by the synergistic method of soft and hard templates,during which a phenolic resin with superior thermal stability was employed as the carbon precursor and a mixture of silica sol and F108 as the mesoporous template.Carbon microspheres with multi-cavity mesoporous structures were prepared,and all the samples showed highly even mesopores,with diameters around 12 nm.The diameter of these microspheres decreased from 396.8 nm to about 182.5 nm with the increase of silica sol.After CO_(2) activation,these novel carbon microspheres(APCF0.5-S1.75)demonstrated high specific surface area(983.3 m^(2)/g)and remarkable CO_(2) uptake of 4.93 mmol/g at 0℃ and1 bar.This could be attributed to the unique multi-cavity structure,which offers uniform mesoporous pore channels,minimal CO_(2) transport of and a greater number of active sites for CO_(2) adsorption.展开更多
Metal hydrides with high hydrogen density provide promising hydrogen storage paths for hydrogen transportation.However,the requirement of highly pure H_(2)for re-hydrogenation limits its wide application.Here,amorphou...Metal hydrides with high hydrogen density provide promising hydrogen storage paths for hydrogen transportation.However,the requirement of highly pure H_(2)for re-hydrogenation limits its wide application.Here,amorphous Al_(2)O_(3)shells(10 nm)were deposited on the surface of highly active hydrogen storage material particles(MgH_(2)-ZrTi)by atomic layer deposition to obtain MgH_(2)-ZrTi@Al_(2)O_(3),which have been demonstrated to be air stable with selective adsorption of H_(2)under a hydrogen atmosphere with different impurities(CH_(4),O_(2),N_(2),and CO_(2)).About 4.79 wt% H_(2)was adsorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)at 75℃under 10%CH_(4)+90%H_(2)atmosphere within 3 h with no kinetic or density decay after 5 cycles(~100%capacity retention).Furthermore,about 4 wt%of H_(2)was absorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)under 0.1%O_(2)+0.4%N_(2)+99.5%H_(2)and 0.1%CO_(2)+0.4%N_(2)+99.5%H_(2)atmospheres at 100℃within 0.5 h,respectively,demonstrating the selective hydrogen absorption of MgH_(2)-ZrTi@10nmAl_(2)O_(3)in both oxygen-containing and carbon dioxide-containing atmospheres hydrogen atmosphere.The absorption and desorption curves of MgH_(2)-ZrTi@10nmAl_(2)O_(3)with and without absorption in pure hydrogen and then in 21%O_(2)+79%N_(2)for 1 h were found to overlap,further confirming the successful shielding effect of Al_(2)O_(3)shells against O_(2)and N_(2).The MgH_(2)-ZrTi@10nmAl_(2)O_(3)has been demonstrated to be air stable and have excellent selective hydrogen absorption performance under the atmosphere with CH_(4),O_(2),N_(2),and CO_(2).展开更多
In observation of efficiently utilizing the boil off gas(BOG)from onboard liquefied natural gas(LNG),storage by adsorption is employed to construct an auxiliary system for fuel storage.A typical LNG powered ship was s...In observation of efficiently utilizing the boil off gas(BOG)from onboard liquefied natural gas(LNG),storage by adsorption is employed to construct an auxiliary system for fuel storage.A typical LNG powered ship was selected,and the storage by adsorption system was designed as per the amount of BOG released during the process of charging and that from daily evaporation on the LNG storage tank.Researches were conducted experimentally and numerically on a 1 L conformable vessel typically designed for adsorbing BOG.Verification of the accuracy of the results from simulations was performed by comparing the data recorded during the charging and discharging process of methane on the vessel packed with one kind of commercially available activated carbon SAC-01(S_(BET)=1507 m^(2)·g^(-1)).Simulations were conducted further to evaluate the performance of the vessel respectively filled with activated carbon AX-21,HKUST-1,MIL-101(Cr),MOF-5.It shows that the mean relative error between the data from simulations and the experimental data is less than 5%.Results also reveal that,within the flow rates range in correspondence with the fuel consumed by the model ship's power unit under its typical working conditions,the mean temperature fluctuation within the vessel is the weakest while packing HKUST-1,which results in the largest accumulated amount of discharge.It suggests that HKUST-1 is a suitable adsorbent for storage by adsorption of BOG from on board LNG.展开更多
Solvation structures fundamentally control the ion-transport dynamics and mechanical properties of polymer electrolytes.However,there is a lack of strategies to rationally regulate the solvation structures and fundame...Solvation structures fundamentally control the ion-transport dynamics and mechanical properties of polymer electrolytes.However,there is a lack of strategies to rationally regulate the solvation structures and fundamental understanding on how they control the electrochemical performances.Herein,by harnessing the electrostatic adsorption of one-dimensional nanofiller(i.e.,surface-charged halloysite nanotubes,d-HNTs),we successfully fabricate a high-performance polymer nanocomposite electrolyte enabled by strong surface adsorption,referred as adsorption-state polymer electrolyte(ASPE).This ASPE shows fast ion transport(0.71±0.05 mS cm^(-1)at room temperature),high mechanical strength and toughness(10.3±0.05 MPa;15.73 MJ m^(-3)),improved lithium-ion transference number,and long cycle life with lithium metal anode,in comparison with the sample without the d-HNT adsorption effect.To fundamentally understand these high performances,an anion-rich asymmetric solvent structure model is further proposed and evidenced by both experiments and simulation studies.Results show that the electrostatic adsorption among the d-HNT,ionic liquid electrolyte,and polymer chain generates a nano filler-supported fast ion-conduction pathway with asymmetric Li+-coordination microenvironment.Meanwhile,the anion-rich asymmetric solvent structure model of ASPE also generates a fast de-solvation and anion-derived stable solid-electrolyte interphase for lithium metal anode.The high performance and understanding of the mechanism for ASPE provide a promising path to develop advanced polymer electrolytes.展开更多
During thewater treatment process,chlorination and ultraviolet(UV)sterilization can modify microplastics(MPs)and alter their physicochemical properties,causing various changes between MPs and other pollutants.In this ...During thewater treatment process,chlorination and ultraviolet(UV)sterilization can modify microplastics(MPs)and alter their physicochemical properties,causing various changes between MPs and other pollutants.In this study,the impact of chlorination and UV modification on the physicochemical properties of polystyrene(PS)and polyvinyl chloride(PVC)were investigated,and the adsorption behavior of pefloxacin(PEF)before and after modificationwas examined.The effect of pH,ionic strength,dissolved organicmatter,heavymetal ions and other water environmental conditions on adsorption behavior was revealed.The results showed that PS had a higher adsorption capacity of PEF than PVC,and the modification increased the presence of O-containing functional groups in the MPs,thereby enhancing the adsorption capacity of both materials.Chlorination had a more significant impact on the physicochemical properties of MPs compared to UV irradiation within the same time period,leading to better adsorption performance of chlorination.The optimal pH for adsorption was found to be 6,and NaCl,sodium alginate and Cu2+would inhibit adsorption to varying degrees,among which the inhibition caused by pH was the strongest.Chlorination and UV modification would weaken the inhibitory effect of environmental factors on the adsorption of PEF by MPs.The main mechanisms of adsorption involved electrostatic interaction and hydrogen bonding.The study clarified the effects of modification on the physicochemical properties of MPs,providing reference for subsequent biotoxicity analysis and environmental protection studies.展开更多
The mass production and widespread use of Pharmaceuticals and Personal Care Products(PPCPs)have posed a serious threat to the water environment and public health.In this work,a green metal-based Metal Organic Framewor...The mass production and widespread use of Pharmaceuticals and Personal Care Products(PPCPs)have posed a serious threat to the water environment and public health.In this work,a green metal-based Metal Organic Framework(MOF)Bi-NH_(2)-BDC was prepared and characterized,and the adsorption characteristics of Bi-NH_(2)-BDCwere investigated with typical PPCPs-diclofenac sodium(DCF).It was found that DCF mainly covered the adsorbent surface as a single molecular layer,the adsorption reaction was a spontaneous,entropyincreasing exothermic process and the adsorption mechanisms between Bi-NH_(2)-BDC and DCF were hydrogen bonding,π-πinteractions and electrostatic interactions.In addition,Bi-NH_(2)-BDC also had considerable photocatalytic properties,and its application in adsor-bent desorption treatment effectively solved the problem of secondary pollution,achieving a green and sustainable adsorption desorption cycle.展开更多
This study investigates the adsorption mechanism,the film formation process,and the inhibition performance of benzotriazole(BTAH)on carbon steels with different grain sizes(i.e.,24.5,4.3,and 0.6μm)in 3.5 wt.%NaCl sol...This study investigates the adsorption mechanism,the film formation process,and the inhibition performance of benzotriazole(BTAH)on carbon steels with different grain sizes(i.e.,24.5,4.3,and 0.6μm)in 3.5 wt.%NaCl solution.The results demonstrate that grain refinement significantly impacts the adsorption and inhibition performance of BTAH on carbon steels.Ultra-refinement of steel grains to 0.6μm improves the maximum inhibition efficiency of BTAH to 90.0%within 168 h of immersion,which was much higher than that of the steels with 24.5μm(73.6%)and 4.3μm grain sizes(81.7%).Notably,grain sizes of 4.3 and 0.6μm facilitate a combination of physisorption and chemisorption of BTAH after 120 h of immersion,as evidenced by the X-ray photoelectron spectroscopy(XPS)results and Langmuir adsorption isotherms,while BTAH adsorbed on carbon steels with a grain size of 24.5μm through physisorption during the 168 h of immersion.Ultra-refinement of grains has beneficial impacts on promoting the formation of a stable and dense corrosion inhibitor film,leading to improved corrosion resistance and the mitigation of non-uniform corrosion.These advantageous effects can be attributed to the higher adsorption energy at grain boundaries(approximately-3.12 eV)compared to grain interiors(ranging from-0.79 to 2.47 eV),promoting both the physisorption and chemisorption of organic corrosion inhibitors.The investigation comprehensively illustrates,for the first time,the effects of grain size on the adsorption mechanism,film formation process,and inhibition performance of organic corrosion inhibitors on carbon steels.This study demonstrates a promising approach to enhancing corrosion inhibition performance through microstructural design.展开更多
Electrocatalytic urea wastewater treatment technology has emerged as a promising method for environmental remediation.However,the realization of highly efficient and scalable electrocatalytic urea wastewater treatment...Electrocatalytic urea wastewater treatment technology has emerged as a promising method for environmental remediation.However,the realization of highly efficient and scalable electrocatalytic urea wastewater treatment(SEUWT)is still an enormous challenge.Herein,through regulating the adsorption behavior of urea functional groups,the efficient SEUWT coupled hydrogen production is realized in anion exchange membrane water electrolyzer(AEMWE).Density functional theory calculations indicate that self-driven electron transfer at the heterogeneous interface(NiO/Co_(3)O_(4))can induce charge redistribution,resulting in electron-rich NiO and electron-deficient Co_(3)O_(4),which are superior to adsorbing C=O(electron-withdrawing group)and–NH_(2)(electron-donating group),respectively,regulating the adsorption behavior of urea molecule and accelerating the reaction kinetics of urea oxidation.This viewpoint is further verified by temperature-programmed desorption experiments.The SEUWT coupled hydrogen production in AEMWE assembled with NiO/Co_(3)O_(4)(anode)and NiCoP(cathode)can continuously treat urea wastewater at an initial current density of 600 mA cm^(-2),with the average urea treatment efficiency about 53%.Compared with overall water splitting,the H_(2) production rate(8.33 mmol s^(-1))increases by approximately 3.5 times.This work provides a cost-effective strategy for scalable purifying urea-rich wastewater and energy-saving hydrogen production.展开更多
Current research on heterogeneous advanced oxidation processes(HAOPs)predominantly emphasizes catalyst iteration and innovation.Significant efforts have been made to regulate the electron structure and optimize the el...Current research on heterogeneous advanced oxidation processes(HAOPs)predominantly emphasizes catalyst iteration and innovation.Significant efforts have been made to regulate the electron structure and optimize the electron distribution,thereby increasing the catalytic activity.However,this focus often overshadows an equally essential aspect of HAOPs:the adsorption effect.Adsorption is a critical initiator for triggering the interaction of oxidants and contaminants with heterogeneous catalysts.The efficacy of these interactions is influenced by a variety of physicochemical properties,including surface chemistry and pore sizes,which determine the affinities between contaminants and material surfaces.This dispar ity in affinity is pivotal because it underpins the selective removal of contaminants,especially in complex waste streams containing diverse contaminants and competing matrices.Consequently,understanding and mastering these interfacial interactions is fundamentally indispensable not only for improving pro cess efficiency but also for enhancing the selectivity of contaminant removal.Herein,we highlight the importance of adsorption-driven interfacial interactions for fundamentally elucidating the catalytic mechanisms of HAOPs.Such interactions dictate the overall performance of the treatment processes by balancing the adsorption,reaction,and desorption rates on the catalyst surfaces.Elucidating the adsorption effect not only shifts the paradigm in understanding HAOPs but also improves their practical ity in water treatment and wastewater decontamination.Overall,we propose that revisiting adsorption driven interfacial interactions holds great promise for optimizing catalytic processes to develop effective HAOP strategies.展开更多
Carbon dioxide(CO_(2))geological sequestration represents a critical technology in mitigating climate change.Shale reservoirs demonstrate a pronounced affinity for CO_(2),resulting in adsorption-induced swelling that ...Carbon dioxide(CO_(2))geological sequestration represents a critical technology in mitigating climate change.Shale reservoirs demonstrate a pronounced affinity for CO_(2),resulting in adsorption-induced swelling that significantly impacts permeability,mechanical strength,injection efficiency,and sequestration safety.For this,we tried to explore the key factors driving the swelling of shale upon CO_(2)injection and its subsequent impact on reservoir properties.Utilizing a self-developed high-temperature-pressure gas adsorption apparatus,we measured strain in Jurassic shale at 308 K under constant hydrostatic pressure with helium(He)at 1300 psi(1 psi=6.895 kPa)and CO_(2)at 850 psi.Next,we investigated the influence of CO_(2)concentration on swelling protentional while maintaining constant pressure,uncovering the anisotropic deformation in relation to pressure.It shows that CO_(2)adsorption induces significant swelling in shale,following a Langmuir-type pressure relationship.Deformation is more pronounced perpendicular than that parallel to the bedding plane.At low pressure,vertical swelling is 2.28 times greater than the horizontal;while at high pressure,the vertical compression is 31.26 times greater than the horizontal.It seems that the anisotropic swelling enhances permeability predictions during CO_(2)injection.Mixed gases under constant compression can prompt gas desorption,stress redistribution,and alterations in pore structure,amplifying He compression effect.The strain induced after replacing CO_(2)with He exceeds that from pure He injection.The asynchronous response of CO_(2)-induced swelling and mechanical compression can precipitate crack propagation and fracturing.Overall,anisotropic swelling from CO_(2)adsorption changes pore structure and permeability,affecting fluid flow and storage.Considering CO_(2)concentration and anisotropic characteristics in reservoir modeling is essential for optimizing injection strategies and enhancing reservoir efficiency.展开更多
基金Dalian distinguished young scholars program(2022RJ17)the Dalian excellent young talents program(2023RY037)provided funding for this study.
文摘To efficiently remove radioactive nuclides from nuclear industry wastewater and minimize the generation of radioactive secondary waste,this study proposes the concept of a magnetically controlled microchannel adsorber based on magnetic adsorbents.A novel protocol for achieving high adsorption performance in microchannel adsorbers with periodically distributed particles is developed using the particle-resolved computational fluid dynamics (CFD) method,which addresses the limitations of traditional porous media flow models.To align simulation results more closely with practical scenarios,a typical high-efficiency magnetic adsorbent,magnetic sodium alginate/cobalt-based Prussian blue (M-SA/PB-Co),was synthesized.The M-SA/PB-Co microspheres exhibit a uniform size distribution (300–600 μm),and their Cs^(+) adsorption follows the pseudo-second-order kinetic model with a Langmuir saturated adsorption capacity of 124.84 mg·g^(-1).The performance parameters of M-SA/PB-Co,obtained from characterization and adsorption experiments,were integrated into CFD simulations.CFD results indicate that as the flow velocity increases,the flow field gradually transitions with vortices expanding in scale and streamline bifurcation points shifting rearward.The Cs^(+) concentration decreases progressively along the flow direction,with a more pronounced reduction in the vortex regions downstream of particles.The characteristic velocity and characteristic concentration of specific regions surrounding the particles were extracted based on boundary layer distribution.The amount of concentration reduction of Cs^(+) through particle is positively correlated with the characteristic concentration and negatively correlated with the characteristic velocity.The number of microspheres required in the microchannel adsorber was optimized using the response surface method.Compared with industrial fixed-bed adsorbers,microchannel adsorbers exhibit 8–10 times higher processing capacity,demonstrating significant industrial application potential.
基金supported by the National Natural Science Foundation of China(22478266 and 32472027)the National Key Research&Development Program of China(2022YFE0207100)the Department of Science and Technology of Sichuan Province(2024ZYD0080 and 2022YFN0027).
文摘Economical and sustainable wastewater treatment techniques are highly demanded to alleviate the issues of clearwater scarcity globally.In this work,the acetic acid/H_(2)O_(2) (AHP) was leveraged to enrich oxygenated functional groups on the biochar surface for efficient ciprofloxacin (CIP) adsorption and biochar regeneration (In situ degradation of CIP in the spent AHP solution).The AHP-modified biochar exhibited significantly enhanced CIP adsorption capacity,about 22 times that of the pristine biochar.The optimized modification condition (acetic acid/H_(2)O_(2):2.11,temperature:45 ℃,and time:12 h) was screened by the response surface method,reaching the highest CIP adsorption capacity of 86.26 mg·g^(−1).Characterization results revealed that the content of carboxyl —C=O—O was enhanced in AHP-modified biochar,which contributed to efficient CIP adsorption by the electrostatic interaction,hydrogen bonding,and hydrophobic interaction.The adsorption of modified biochar to CIP molecules was a spontaneous endothermic process,and in line with the pseudo-second-order model and the Langmuir isotherm model.Moreover,the biochar modification process enabled the spent AHP solution with a strong oxidizing agent of peracetic acid (PAA),which can be employed to degrade adsorbed CIP for biochar in-situ generation.This work tailored a closed-loop strategy for biochar oxidation,contaminant adsorption,and biochar regeneration,highlighting a viable route for sustainable wastewater treatment.
基金supported by research funds of Jeonbuk National University in 2024 and partly supported by the National Research Foundation of Korea(NRF-2019R1A2C1006441)from the Ministry of Education.
文摘Flubendiamide is a commonly used pesticide with low water solubility and a high organic carbon sorption constant,causing it to adhere to soil particles and negatively impact soil ecosystems.First,chili plant stems,typically discarded after the harvest season,represent an abundant local biomass resource with significant potential for utilization,and were converted into biochar through pyrolysis.Here,we describe the synthesis of biochar modified with iron and chitosan to increase the diversity of functions and surface functional groups of biochar.The resulting chitosan-modified magnetic biochar(CMBC)presents a full range of functional groups of chitosan and iron oxide as shown by Fourier-transform infrared spectroscopy.The correlation between flubendiamide concentration and the dose of biochar on adsorption was explored.The flubendiamide adsorption efficiency of CMBC(1%mass ratio of soil)reached 68.03%in 90 min.The highest adsorption capacity achieved was 0.95 mg·g^(−1).The flubendiamide adsorption mechanism by CMBC can be described with a pseudo-second-order kinetic model.The experiment data closely fit a Freundlich isotherm model(R^(2)=0.998),and the low residual sum of squares values demonstrate the high model applicability.In this study,we present a comprehensive overview of pesticides,alongside kinetic and isotherm model studies of flubendiamide adsorption by CMBC.We emphasize the potential of modified biochar to enhance environmental remediation applications.
基金supported by the Open Project Funding of Key Laboratory of Intelligent Health Perception and Ecological Restoration of Rivers and Lakes,Ministry of Education,Hubei University of Technology(No.HGKFZ03).
文摘In this study,chitosan(CS)was combined with microcrystalline cellulose(MCC)to fabricate composite hydrogel beads.These beads were further modified through blending and grafting with polyethyleneimine(PEI)to develop chitosan/microcrystalline cellulose@polyethyleneimine(CS/MCC@PEI)composite gel spheres for the efficient adsorption of diclofenac sodium(DS)from aqueous solutions.The adsorbent was characterized using scanning electron microscopy(SEM),X-ray diffraction(XRD),Fourier-transform infrared spectroscopy(FTIR),X-ray pho-toelectron spectroscopy(XPS),and thermogravimetric analysis(TGA).The CS/MCC@PEI composite exhibited a spherical morphology with a porous structure,abundant surface functional groups,and a high adsorption capac-ity of 274.84 mg/g for DS.Kinetic studies revealed that the adsorption process followed the pseudo-second-order model,dominated by physical adsorption,with both surface and internal diffusion influencing the adsorption rate.The Freundlich isotherm model best described the adsorption behavior,indicating multilayer adsorption on heterogeneous surfaces.Environmental adaptability tests demonstrated minimal interference from co-existing anions and humic acid,while regeneration experiments confirmed excellent reusability(>77%removal after five cycles).The adsorption mechanism involved electrostatic interactions and hydrogen bonding between the hydroxyl/amino groups of the composite and DS.These findings highlight the potential of CS/MCC@PEI as a cost-effective and sustainable adsorbent for DS removal from water.
基金the support from the National Key Research and Development Program of China (No. 2022YFC2904504)the Science and Technology Research Project of Jiangxi Provincial Department of Education, China (No. GJJ2200864)the Gansu Provincial Key Research and Development Project, China (No. 22YF7GA073)。
文摘The flotation separation of argentite from sphalerite using ammonium dibutyl dithiophosphate(ADD)was studied.Molecular simulation(MS)calculation shows that ADD is chemisorbed on argentite and sphalerite surface in the form of S—P bond.The ADD adsorption on argentite and sphalerite surface in Ag^(+)system was revealed by ICP,Zeta potential and XPS analyses.It is shown that the dissolved Ag^(+)from argentite surface can be absorbed on sphalerite surface in the form of silver hydroxide,and AgOH hydrophilic colloid prevents the adsorption of ADD on sphalerite surface.The ADD adsorption on argentite and sphalerite surface in the pulp containing silver and zinc ions was revealed by adsorption capacity and surface wettability analyses.It is shown that the combined Zn(OH)_(2) and AgOH hydrophilic colloid leads to greater ADD adsorption capacity on argentite surface and stronger surface hydrophobicity than sphalerite.Flotation tests demonstrate that ADD enables efficient separation of argentite from sphalerite in the pulp containing silver and zinc ions.
基金the Department of Science and Technology(DST),Govt.of India for providing funds under the FIST program and PURSE grant vide No.SR/PURSE/2020/31 to the department of Chemistry,University of Kashmir.
文摘This study presents a thorough investigation into the use of single and twin-tailed cationic and anionic surfactant-modified chitosan(SMCS)hydrogel beads as effective adsorbents for the elimination of hazardous polycyclic aromatic hydrocarbons(PAHs)from aqueous solutions.The Chitosan(CS)hydrogel beads were modified with single/twin-tailed anionic surfactants,sodium dodecyl sulfate(SDS)and sodium bis(2-ethylhexyl)sulfosuccinate(AOT),and cationic surfactants,dodecyltrimethylammonium bromide(DTAB)and didodecyldimethylammonium bromide(DDAB),to enhance their adsorption capacity of PAHs.The CS and SMCS beads were evaluated for their structural,mechanical,and adsorption properties using a range of techniques,including infrared spectroscopy(IR),energy-dispersive X-ray spectroscopy(EDX),rheometry,and field emission scanning electron microscopy(FESEM).Adsorption experiments of naphthalene(Nap),acenaphthene(Ace),and phenanthrene(Phe)on SMCS beads demonstrate that they have significantly higher adsorption capacities than CS beads,due to increase in hydrophobic interactions.Adsorption capacity followed the trend,Phen>Ace>Nap for all the beads revealing that twin-tailed SMCS bead possess much higher adsorption capacities(Qmax)compared to single-tailed SMCS beads.For twin tailed surfactants,the maximum adsorption capacities for Nap,Ace and Phe varied as CS-AOT(CS-DDAB):430.0(323.8)611.60(538.18)633.39(536.99)mg/g respectively,outperforming other reported hydrogel beads.The study highlights the simplicity,eco-friendliness,and enhanced performance of surfactant modification for developing high-efficiency adsorbents,paving the way for cost-effective solutions in water re-mediation.
基金supported by the National Natural Science Foundation of China(No.52370112).
文摘In order to address the evolving emission characteristics of oxygenated volatile organic compounds(OVOCs),it is essential to develop adsorbent materials specifically designed for the efficient adsorption of OVOCs with large kinetic diameters.In this study,we used co-pyrolysis to prepare a series of graded porous carbon materials with well-developed micropores by adjusting the doping ratios of root nodules and pretreated cellulose.The material with root nodule to cellulose mass ratio of 1:1(TCC-RN-1)exhibited the highest saturated adsorption capacity for butyl acetate(834 mg/g).This can be attributed to enhanced pore size distribution from nodule doping,which facilitates the development of a micropore-graded structure.Additionally,the nodules acted as auxiliary activating agents that enhanced the KOH micropore regulation effect during the activation stage,resulting in the highest micropore volume(0.863 cm^(3)/g).The doping of root nodules facilitated the formation of additional defects on the surface of the porous carbon material,leading to a more disordered arrangement that improved pollutant adsorption.Furthermore,TCC-RN-1 demonstrated good thermal stability in an air atmosphere,main-taining a butyl acetate adsorption capacity exceeding 95%after five adsorption-desorption cycles.This indicates its favorable potential for industrial applications.
基金financially supported by the National Natural Science Foundation of China (No.52372188)Natural Science Foundation of Henan (Nos.242300421625,252300421333)+4 种基金CAS Henan Industrial Technology Innovation & Incubation Center (No.2024121)Key Scientific Research Project of Education Department of Henan Province (Nos.22A150042,23A150038,and 24A150019)2023 Introduction of studying abroad talent programthe China Postdoctoral Science Foundation (No.2019 M652546)Key Project of Science and Technology of Henan Province (No.252102240007)。
文摘Aqueous zinc-ion batteries(AZIBs) are regarded as one of the most promising energy conversion and storage devices.Nevertheless,side reactions and dendrite growth on the zinc metal anode hinder their widespread application.In this study,hemin was employed as a multi-functional artificial interface for the first time to inhibit the disordered growth of zinc dendrites and mitigate side reactions.Theoretical calculations indicate that hemin is preferentially adsorbed onto the zinc anode,thus blocking the interaction between the active zinc anode and electrolyte.Compared with zinc foil,the Hemin@Zn anode demonstrates enhanced corrosion resistance,a decrease in hydrogen evolution,and more orderly deposition of zinc.As expected,the symmetric cell with Hemin@Zn anode can sustain up to 4000 h at 0.2 mA/cm^(2),0.2 mAh/cm^(2).Asymmetric Zn//Cu cells exhibit an average coulombic efficiency exceeding 99.72 % during 500 cycles.Moreover,the full cell Hemin@Zn//NH_(4)V_(4)O_(10) delivers a superior capacity up to 367 m Ah/g and the discharge capacity retention reaches 124 mAh/g after 1200 cycles even at a current density of 5 A/g.This work provides a simple and effective method for constructing a robust artificial interface to promote the application of long-life AZIBs.
基金supported by Shaanxi Fundamental Science Research Project for Chemistry and Biology(23JHQ011)Natural Science Foundation of Shaanxi(2024JC-YBMS-115)Natural Science Basic Research Plan in Shaanxi Province of China(2025JC-YBMS-141)。
文摘The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightforward reduction approach was employed to design three bimetallic alloy nanoparticles(FeNi,FeCo,and NiCo)supported on multistage porous carbon substrates.Experimental and theoretical calculations reveal that the charge transfer within the alloy catalyst influences the position of its d-band center and its degree of hybridization with sodium polysulfides(NaPSs).An increased charge transfer leads to a shift of the alloy’s d-band center closer to the Fermi energy level,thereby enhancing its adsorption and catalytic capabilities.Among the three alloy compositions,the FeNi alloy exhibits the highest charge transfer.Consequently,the FeNi alloy demonstrates the superior electrochemical performance,achieving a high reversible specific capacity of 848.2 mA h g^(−1),with an average capacity degradation rate of only 0.037%per cycle over 1000 cycles at 1.2 C.The S/FeNi/NC cathode exhibits a low electrolyte-to-sulfur(E/S)ratio of 6.6µL mg^(−1),while maintaining a high reversible specific capacity of 568.1 mA h g^(−1).This offers valuable insights for the application of alloy catalysts in the S/FeNi/NC cathode of RT Na-S batteries.
基金supported by the National Natural Science Foundation of China(Grant No.U23A2022)the National Natural Science Foundation of China(Grant No.52474047)+2 种基金the Natural Science Foundation of Chongqing(Grant No.CSTB2024NSCQ-MSX0951)the Natural Science Foundation of Sichuan Province(Grant No.2025ZNSFSC1357)the National Science and Technology Major Project(Grant No.2025ZD1404307).
文摘Injecting impure CO_(2)for enhanced gas recovery(CO_(2)-EGR)offers a dual benefit by improving natural gas extraction while enabling CO_(2)sequestration.However,the interactions between CO_(2),N_(2),and CH_(4)under reservoir conditions require further investigation.This study employs Grand Canonical Monte Carlo(GCMC)and Molecular Dynamics(MD)simulations to quantify the adsorption and diffusion behaviors of CO_(2),N_(2),and CH_(4)in quartz nanopores over a pressure range of 1-24 MPa under varying water saturations and gas compositions.The results indicate that:(1)CO_(2)exhibits the broadest energy distribution and the strongest adsorption stability,occupying about 20%-30%more adsorption sites than CH_(4)or N_(2)and showing the least sensitivity to water saturation,with only a 30%reduction at 50%saturation,compared to 60%for CH_(4),giving CO_(2)a clear competitive advantage.(2)The adsorption and desorption behaviors are strongly pressure dependent,as increasing pressure reduces the adsorption layer area and shifts gas distribution from adsorption dominated to free phase.Competitive adsorption analysis reveals that while CO_(2)dominates displacement at low pressures,mixtures that contain N_(2)achieve higher CH_(4)desorption efficiency above 13 MPa by mitigating diffusion resistance.(3)A higher N_(2)fraction improves CH_(4)diffusion coefficients,thereby facilitating gas mobility and ensuring superior recovery performance under high-pressure conditions.This study advances the fundamental knowledge of microscale gas behavior in tight sandstones and supports the feasibility of impure CO_(2)injection as a practical strategy for sustainable gas production.
基金supported by the National Key R&D Program of China(No.2021YFB3501102).
文摘Porous carbon microspheres are widely regarded as a superior CO_(2) adsorbent due to their exceptional efficiency and affordability.However,better adsorption performance is very attractive for porous carbon microspheres.And modification of the pore structure is one of the effective strategies.In this study,multi-cavity mesoporous carbon microspheres were successfully synthesized by the synergistic method of soft and hard templates,during which a phenolic resin with superior thermal stability was employed as the carbon precursor and a mixture of silica sol and F108 as the mesoporous template.Carbon microspheres with multi-cavity mesoporous structures were prepared,and all the samples showed highly even mesopores,with diameters around 12 nm.The diameter of these microspheres decreased from 396.8 nm to about 182.5 nm with the increase of silica sol.After CO_(2) activation,these novel carbon microspheres(APCF0.5-S1.75)demonstrated high specific surface area(983.3 m^(2)/g)and remarkable CO_(2) uptake of 4.93 mmol/g at 0℃ and1 bar.This could be attributed to the unique multi-cavity structure,which offers uniform mesoporous pore channels,minimal CO_(2) transport of and a greater number of active sites for CO_(2) adsorption.
基金supported by the National Natural Science Foundation of China(22175136)the State Key Laboratory of Electrical Insulation and Power Equipment(EIPE23127)the Fundamental Research Funds for the Central Universities(xtr052024009).
文摘Metal hydrides with high hydrogen density provide promising hydrogen storage paths for hydrogen transportation.However,the requirement of highly pure H_(2)for re-hydrogenation limits its wide application.Here,amorphous Al_(2)O_(3)shells(10 nm)were deposited on the surface of highly active hydrogen storage material particles(MgH_(2)-ZrTi)by atomic layer deposition to obtain MgH_(2)-ZrTi@Al_(2)O_(3),which have been demonstrated to be air stable with selective adsorption of H_(2)under a hydrogen atmosphere with different impurities(CH_(4),O_(2),N_(2),and CO_(2)).About 4.79 wt% H_(2)was adsorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)at 75℃under 10%CH_(4)+90%H_(2)atmosphere within 3 h with no kinetic or density decay after 5 cycles(~100%capacity retention).Furthermore,about 4 wt%of H_(2)was absorbed by MgH_(2)-ZrTi@10nmAl_(2)O_(3)under 0.1%O_(2)+0.4%N_(2)+99.5%H_(2)and 0.1%CO_(2)+0.4%N_(2)+99.5%H_(2)atmospheres at 100℃within 0.5 h,respectively,demonstrating the selective hydrogen absorption of MgH_(2)-ZrTi@10nmAl_(2)O_(3)in both oxygen-containing and carbon dioxide-containing atmospheres hydrogen atmosphere.The absorption and desorption curves of MgH_(2)-ZrTi@10nmAl_(2)O_(3)with and without absorption in pure hydrogen and then in 21%O_(2)+79%N_(2)for 1 h were found to overlap,further confirming the successful shielding effect of Al_(2)O_(3)shells against O_(2)and N_(2).The MgH_(2)-ZrTi@10nmAl_(2)O_(3)has been demonstrated to be air stable and have excellent selective hydrogen absorption performance under the atmosphere with CH_(4),O_(2),N_(2),and CO_(2).
基金supported by National Natural Science Foundation of China(51979121)Natural Science Foundation of Fujian Province(2024J01713,2023J01905)+1 种基金Xiamen Municipal Bureau of Sciences&Technology(3502Z20226011)Educational scientific research project for young and middle-aged teachers in Fujian Province(JAT210300).
文摘In observation of efficiently utilizing the boil off gas(BOG)from onboard liquefied natural gas(LNG),storage by adsorption is employed to construct an auxiliary system for fuel storage.A typical LNG powered ship was selected,and the storage by adsorption system was designed as per the amount of BOG released during the process of charging and that from daily evaporation on the LNG storage tank.Researches were conducted experimentally and numerically on a 1 L conformable vessel typically designed for adsorbing BOG.Verification of the accuracy of the results from simulations was performed by comparing the data recorded during the charging and discharging process of methane on the vessel packed with one kind of commercially available activated carbon SAC-01(S_(BET)=1507 m^(2)·g^(-1)).Simulations were conducted further to evaluate the performance of the vessel respectively filled with activated carbon AX-21,HKUST-1,MIL-101(Cr),MOF-5.It shows that the mean relative error between the data from simulations and the experimental data is less than 5%.Results also reveal that,within the flow rates range in correspondence with the fuel consumed by the model ship's power unit under its typical working conditions,the mean temperature fluctuation within the vessel is the weakest while packing HKUST-1,which results in the largest accumulated amount of discharge.It suggests that HKUST-1 is a suitable adsorbent for storage by adsorption of BOG from on board LNG.
基金financial support from the National Natural Science Foundation of China(52203123)the Sichuan Science and Technology Program(2023NSFSC0991)+2 种基金the State Key Laboratory of Polymer Materials Engineering(sklpme 2023-1-05 and sklpme 2024-2-04)the Fundamental Research Funds for the Central Universitiespartially sponsored by the Double First-Class Construction Funds of Sichuan University。
文摘Solvation structures fundamentally control the ion-transport dynamics and mechanical properties of polymer electrolytes.However,there is a lack of strategies to rationally regulate the solvation structures and fundamental understanding on how they control the electrochemical performances.Herein,by harnessing the electrostatic adsorption of one-dimensional nanofiller(i.e.,surface-charged halloysite nanotubes,d-HNTs),we successfully fabricate a high-performance polymer nanocomposite electrolyte enabled by strong surface adsorption,referred as adsorption-state polymer electrolyte(ASPE).This ASPE shows fast ion transport(0.71±0.05 mS cm^(-1)at room temperature),high mechanical strength and toughness(10.3±0.05 MPa;15.73 MJ m^(-3)),improved lithium-ion transference number,and long cycle life with lithium metal anode,in comparison with the sample without the d-HNT adsorption effect.To fundamentally understand these high performances,an anion-rich asymmetric solvent structure model is further proposed and evidenced by both experiments and simulation studies.Results show that the electrostatic adsorption among the d-HNT,ionic liquid electrolyte,and polymer chain generates a nano filler-supported fast ion-conduction pathway with asymmetric Li+-coordination microenvironment.Meanwhile,the anion-rich asymmetric solvent structure model of ASPE also generates a fast de-solvation and anion-derived stable solid-electrolyte interphase for lithium metal anode.The high performance and understanding of the mechanism for ASPE provide a promising path to develop advanced polymer electrolytes.
基金supported by the Shanxi Scholarship Council of China(No.2023-054)the Applied Basic Research Project of Shanxi Province,China(No.20210302123121)the National Natural Science Foundation of China(No.52170045).
文摘During thewater treatment process,chlorination and ultraviolet(UV)sterilization can modify microplastics(MPs)and alter their physicochemical properties,causing various changes between MPs and other pollutants.In this study,the impact of chlorination and UV modification on the physicochemical properties of polystyrene(PS)and polyvinyl chloride(PVC)were investigated,and the adsorption behavior of pefloxacin(PEF)before and after modificationwas examined.The effect of pH,ionic strength,dissolved organicmatter,heavymetal ions and other water environmental conditions on adsorption behavior was revealed.The results showed that PS had a higher adsorption capacity of PEF than PVC,and the modification increased the presence of O-containing functional groups in the MPs,thereby enhancing the adsorption capacity of both materials.Chlorination had a more significant impact on the physicochemical properties of MPs compared to UV irradiation within the same time period,leading to better adsorption performance of chlorination.The optimal pH for adsorption was found to be 6,and NaCl,sodium alginate and Cu2+would inhibit adsorption to varying degrees,among which the inhibition caused by pH was the strongest.Chlorination and UV modification would weaken the inhibitory effect of environmental factors on the adsorption of PEF by MPs.The main mechanisms of adsorption involved electrostatic interaction and hydrogen bonding.The study clarified the effects of modification on the physicochemical properties of MPs,providing reference for subsequent biotoxicity analysis and environmental protection studies.
基金supported by Liaoning Revitalization Talents Program(No.XLYC1907173)the Science and Technology General Project of Liaoning Provincial Education Department(No.LJKMZ20221835)the National Natural Science Foundation of China(Nos.22006073 and 22205027).
文摘The mass production and widespread use of Pharmaceuticals and Personal Care Products(PPCPs)have posed a serious threat to the water environment and public health.In this work,a green metal-based Metal Organic Framework(MOF)Bi-NH_(2)-BDC was prepared and characterized,and the adsorption characteristics of Bi-NH_(2)-BDCwere investigated with typical PPCPs-diclofenac sodium(DCF).It was found that DCF mainly covered the adsorbent surface as a single molecular layer,the adsorption reaction was a spontaneous,entropyincreasing exothermic process and the adsorption mechanisms between Bi-NH_(2)-BDC and DCF were hydrogen bonding,π-πinteractions and electrostatic interactions.In addition,Bi-NH_(2)-BDC also had considerable photocatalytic properties,and its application in adsor-bent desorption treatment effectively solved the problem of secondary pollution,achieving a green and sustainable adsorption desorption cycle.
基金support of the National Natural Science Foundation of China(Nos.52171063,52274362,and 52371049)the Key R&D projects of Henan Province(No.221111230800)+1 种基金the Doctoral Fund of Henan University of Technology(No.2023BS047)the Natural science Project of Zhengzhou Science and Technology Bureau(No.22ZZRDZX04)。
文摘This study investigates the adsorption mechanism,the film formation process,and the inhibition performance of benzotriazole(BTAH)on carbon steels with different grain sizes(i.e.,24.5,4.3,and 0.6μm)in 3.5 wt.%NaCl solution.The results demonstrate that grain refinement significantly impacts the adsorption and inhibition performance of BTAH on carbon steels.Ultra-refinement of steel grains to 0.6μm improves the maximum inhibition efficiency of BTAH to 90.0%within 168 h of immersion,which was much higher than that of the steels with 24.5μm(73.6%)and 4.3μm grain sizes(81.7%).Notably,grain sizes of 4.3 and 0.6μm facilitate a combination of physisorption and chemisorption of BTAH after 120 h of immersion,as evidenced by the X-ray photoelectron spectroscopy(XPS)results and Langmuir adsorption isotherms,while BTAH adsorbed on carbon steels with a grain size of 24.5μm through physisorption during the 168 h of immersion.Ultra-refinement of grains has beneficial impacts on promoting the formation of a stable and dense corrosion inhibitor film,leading to improved corrosion resistance and the mitigation of non-uniform corrosion.These advantageous effects can be attributed to the higher adsorption energy at grain boundaries(approximately-3.12 eV)compared to grain interiors(ranging from-0.79 to 2.47 eV),promoting both the physisorption and chemisorption of organic corrosion inhibitors.The investigation comprehensively illustrates,for the first time,the effects of grain size on the adsorption mechanism,film formation process,and inhibition performance of organic corrosion inhibitors on carbon steels.This study demonstrates a promising approach to enhancing corrosion inhibition performance through microstructural design.
基金supported by the National Natural Science Foundation of China(Grant Nos.22162025,22168040)the Youth Innovation Team of Shaanxi Universities,the Open and Innovation Fund of Hubei Three Gorges Laboratory(SK232001)the Regional Innovation Capability Leading Program of Shaanxi(2022QFY07-03,2022QFY07-06).
文摘Electrocatalytic urea wastewater treatment technology has emerged as a promising method for environmental remediation.However,the realization of highly efficient and scalable electrocatalytic urea wastewater treatment(SEUWT)is still an enormous challenge.Herein,through regulating the adsorption behavior of urea functional groups,the efficient SEUWT coupled hydrogen production is realized in anion exchange membrane water electrolyzer(AEMWE).Density functional theory calculations indicate that self-driven electron transfer at the heterogeneous interface(NiO/Co_(3)O_(4))can induce charge redistribution,resulting in electron-rich NiO and electron-deficient Co_(3)O_(4),which are superior to adsorbing C=O(electron-withdrawing group)and–NH_(2)(electron-donating group),respectively,regulating the adsorption behavior of urea molecule and accelerating the reaction kinetics of urea oxidation.This viewpoint is further verified by temperature-programmed desorption experiments.The SEUWT coupled hydrogen production in AEMWE assembled with NiO/Co_(3)O_(4)(anode)and NiCoP(cathode)can continuously treat urea wastewater at an initial current density of 600 mA cm^(-2),with the average urea treatment efficiency about 53%.Compared with overall water splitting,the H_(2) production rate(8.33 mmol s^(-1))increases by approximately 3.5 times.This work provides a cost-effective strategy for scalable purifying urea-rich wastewater and energy-saving hydrogen production.
基金supported by the National Key Research and Development Program of China(2022YFC3205300)the National Natural Science Foundation of China(22176124).
文摘Current research on heterogeneous advanced oxidation processes(HAOPs)predominantly emphasizes catalyst iteration and innovation.Significant efforts have been made to regulate the electron structure and optimize the electron distribution,thereby increasing the catalytic activity.However,this focus often overshadows an equally essential aspect of HAOPs:the adsorption effect.Adsorption is a critical initiator for triggering the interaction of oxidants and contaminants with heterogeneous catalysts.The efficacy of these interactions is influenced by a variety of physicochemical properties,including surface chemistry and pore sizes,which determine the affinities between contaminants and material surfaces.This dispar ity in affinity is pivotal because it underpins the selective removal of contaminants,especially in complex waste streams containing diverse contaminants and competing matrices.Consequently,understanding and mastering these interfacial interactions is fundamentally indispensable not only for improving pro cess efficiency but also for enhancing the selectivity of contaminant removal.Herein,we highlight the importance of adsorption-driven interfacial interactions for fundamentally elucidating the catalytic mechanisms of HAOPs.Such interactions dictate the overall performance of the treatment processes by balancing the adsorption,reaction,and desorption rates on the catalyst surfaces.Elucidating the adsorption effect not only shifts the paradigm in understanding HAOPs but also improves their practical ity in water treatment and wastewater decontamination.Overall,we propose that revisiting adsorption driven interfacial interactions holds great promise for optimizing catalytic processes to develop effective HAOP strategies.
基金supported by the Innovative Research Group Project of the National Natural Science Foundation of China(Grant No.52121003)the National Natural Science Foundation of China(Grant No.52104046).
文摘Carbon dioxide(CO_(2))geological sequestration represents a critical technology in mitigating climate change.Shale reservoirs demonstrate a pronounced affinity for CO_(2),resulting in adsorption-induced swelling that significantly impacts permeability,mechanical strength,injection efficiency,and sequestration safety.For this,we tried to explore the key factors driving the swelling of shale upon CO_(2)injection and its subsequent impact on reservoir properties.Utilizing a self-developed high-temperature-pressure gas adsorption apparatus,we measured strain in Jurassic shale at 308 K under constant hydrostatic pressure with helium(He)at 1300 psi(1 psi=6.895 kPa)and CO_(2)at 850 psi.Next,we investigated the influence of CO_(2)concentration on swelling protentional while maintaining constant pressure,uncovering the anisotropic deformation in relation to pressure.It shows that CO_(2)adsorption induces significant swelling in shale,following a Langmuir-type pressure relationship.Deformation is more pronounced perpendicular than that parallel to the bedding plane.At low pressure,vertical swelling is 2.28 times greater than the horizontal;while at high pressure,the vertical compression is 31.26 times greater than the horizontal.It seems that the anisotropic swelling enhances permeability predictions during CO_(2)injection.Mixed gases under constant compression can prompt gas desorption,stress redistribution,and alterations in pore structure,amplifying He compression effect.The strain induced after replacing CO_(2)with He exceeds that from pure He injection.The asynchronous response of CO_(2)-induced swelling and mechanical compression can precipitate crack propagation and fracturing.Overall,anisotropic swelling from CO_(2)adsorption changes pore structure and permeability,affecting fluid flow and storage.Considering CO_(2)concentration and anisotropic characteristics in reservoir modeling is essential for optimizing injection strategies and enhancing reservoir efficiency.
