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
Recently,reactive oxygen species(ROS)-independent mimetics of oxidase with Au nanoclusters(NCs)as the catalysts and MnO_(2)as electron acceptor have gained attention.In this study,we aim to explore the oxidase-mimicki...Recently,reactive oxygen species(ROS)-independent mimetics of oxidase with Au nanoclusters(NCs)as the catalysts and MnO_(2)as electron acceptor have gained attention.In this study,we aim to explore the oxidase-mimicking potential of bovine serum albumin(BSA)-templated metal nanoclusters(BSA-M NCs,where M=Ag,Pt,Cu,or Cd)beyond Au NCs in boosting the oxidation of 3,3',5,5'-tetramethylbenzidine(TMB)by MnO_(2),denoted as BM@Metal.The oxidase-mimetic activity of BM@Metal is independent of ROS and generally enhanced by the incorporation of metal nanoclusters.Notably,this enhancement varies with the metal species,with BSA-Cd exhibiting the highest activity.The X-ray photoelectron spectroscopy(XPS)analysis confirms mixed valence states(Mn(Ⅳ)/Mn(Ⅱ))in BM@Cd.Given that the catalytic activity is closely linked to the substrate adsorption,the label-free isothermal titration calorimetry was employed to probe the affinity between TMB and BSA-M NCs,which provides a robust approach for probing the interface adsorption.The results reveal that the superior catalytic performance of BSA-Cd correlates with enhanced TMB adsorption,likely facilitated by coordination and hydrophobic interactions.Finally,the superior catalytic performance of BSA-M NCs on the oxidation of TMB by MnO_(2)has inspired us to fabricate the assay for analyzing α-glucosidase’s activity.This work not only demonstrates the versatility of metal NCs in constructing ROS-independent oxidase mimetics but also provides interfacial adsorption engineered strategy for the rational design of superior ROS independent mimetics of natural oxidase.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
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
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
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
In this study,we investigated improving the performance of a layered double hydroxide(LDH)for the adsorption of As(III)and As(V)by controlling the morphology of LDH crystals.The LDH was synthesized via a simple coprec...In this study,we investigated improving the performance of a layered double hydroxide(LDH)for the adsorption of As(III)and As(V)by controlling the morphology of LDH crystals.The LDH was synthesized via a simple coprecipitation method using barely soluble MgO as a precursor and succinic acid(SA)as a morphological control agent.Doping the LDH crystals with carboxylate ions(RCOO−)derived from SA caused the crystals to develop in a radial direction.This changed the pore characteristics and increased the density of active surface sites.Subsequently,SA/MgFe-LDH showed excellent affinity for As(III)and As(V)with maximum sorption densities of 2.42 and 1.60 mmol/g,respectively.By comparison,the pristine MgFe-LDH had sorption capacities of 1.56 and 1.31 mmol/g for As(III)and As(V),respectively.The LDH was effective over a wide pH range for As(III)adsorption(pH 3-8.5)and As(V)adsorption(pH 3-6.5).Using a combination of spectroscopy and sorption modeling calculations,the main sorption mechanism of As(III)and As(V)on SA/MgFe-LDH was identified as inner-sphere complexation via ligand exchangewith hydroxyl group(-OH)and RCOO−.Specifically,bidentate As-Fe complexeswere proposed for both As(III)and As(V)uptake,with the magnitude of formation varying with the initial As concentration.Importantly,the As-laden adsorbent had satisfactory stability in simulated real landfill leachate.These findings demonstrate that SA/MgFe-LDH exhibits considerable potential for remediation of As-contaminated water.展开更多
Recycling rare earth elements(REEs)from waste is necessary for an environmentally sustainable reuse and wastewater management approach.Na-A zeolite was synthesized from coal fly ash(CFA)and applied for Ce^(3+)adsorpti...Recycling rare earth elements(REEs)from waste is necessary for an environmentally sustainable reuse and wastewater management approach.Na-A zeolite was synthesized from coal fly ash(CFA)and applied for Ce^(3+)adsorption.Fourier transform infrared(FTIR)spectra show peaks at 790,500 and 467 cm^(-1),which are bond vibrations of Si-O-Si,Si with Al-O and Si-O-.The surface area is 15.88 m^(2)/g,with a pore size of 2.14 nm.SEM images show a cubic shape,which indicates the formation of zeolite.Field emission and energy disperse spectroscopy(EDS)shows the formation of Si,Al,Na,and O.Na-A zeolite was applied for Ce^(3+)adsorption.The optimum conditions for Ce^(3+)adsorption are 50 ppm concentration,360 min,and pH 6.The maximum adsorption capacity is 176.49 mg/g.Based on the results,it is found that the adsorption of Ce^(3+)by Na-A zeolite is pseudo-second-order.The desorption test using HNO_(3) is more effective than using HCl and H_(2)SO_(4).A desorption efficiency of 97.22%is obtained at 4 cycles.Adsorption test using real sample wastewater demonstrates an adsorption efficiency of 83.35%.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
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
In order to reveal the effect of 2-hydroxy-3-naphthyl hydroxamic acid(H205)on the flotation behavior and action mechanism of bastnaesite,single-mineral flotation experiments of bastnaesite were conducted.The flotation...In order to reveal the effect of 2-hydroxy-3-naphthyl hydroxamic acid(H205)on the flotation behavior and action mechanism of bastnaesite,single-mineral flotation experiments of bastnaesite were conducted.The flotation recovery of bastnaesites can be achieved more than 90%when the aeration rate is 40 mL/min,the rotational speed is 200 r/min,the H205 dosage is 120 mg/L,and the pulp pH ranges from 7 to 9.The action mechanism of H205 on the surface of bastnaesite was studied by simultaneous thermogravimetry and differential scanning calorimetry(TG-DSC),Zeta potential measurements,Fourier transform-infrared spectra(FT-IR)and X-ray photoelectron spectroscopy(XPS).These analysis results show that under suitable flotation conditions,H205 has an obvious adsorption phenomenon on the surface of bastnaesite.The adsorption involves electrostatic interactions and chemical interactions,namely H205 has a strong collecting ability of bastnaesite due to the synergism of electrostatic adsorption and chemical adsorption.This study systematically reveals the flotation behavior and adsorption mechanism of H205 on the surface of bastnaesite,and provides useful theoretical guidance for efficient flotation separation of bastnaesite.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
Treatment of precious metals in electronic waste has attracted tremendous attention and is essential for both environmental protection and resource sustainable development.In this study,a novel adsorbent for precious ...Treatment of precious metals in electronic waste has attracted tremendous attention and is essential for both environmental protection and resource sustainable development.In this study,a novel adsorbent for precious metal ions,V_(2)O_(3)spiny hollow nanospheres(pV_(2)O_(3)SHN),was synthe sized through a one-step hydrothermal-as sis ted methodology for the adsorption of Au(Ⅲ),Ag(Ⅰ),Pd(Ⅱ),and Pt(Ⅳ) from the leaching solution of electronic waste.The results reveal that the p-V2O3SHN hierarchy was successfully constructed with a hollow structure and dense spiny morphology.The prepared p-V2O3SHN can effectively remove precious metal ions such as Au(Ⅲ),Ag(Ⅰ),Pd(Ⅱ),and Pt(Ⅳ),with the selective capture order being Au(Ⅲ)> Ag(Ⅰ)> Pt(Ⅳ)> Pd(Ⅱ)> other metal ions.This superior adsorption capability can be attributed to the multi-diffusible,intermingled composition,and numerous active sites decorating the p-V2O3SHN hierarchy,facilitating the uptake of Au(Ⅲ),Ag(Ⅰ),Pd(Ⅱ),and Pt(Ⅳ) ions from electronic waste.The Langmuir model provided a better fit for the uptake process,revealing maximum uptake capacities of 833.33 mg/g for Au(Ⅲ),370.37 mg/g for Ag(Ⅰ),42.01 mg/g for Pd(Ⅱ),and 77.51 mg/g for Pt(Ⅳ) on p-V_(2)O_(3)SHN.Remarkably,p-V_(2)O_(3)SHN exhibited a robust affinity for the adsorbate due to the presence of surface defects and reduction reactions.The new p-V2O3SHN also demonstrated good reusability for three sorption cycles,highlighting its potential for electronic waste treatment.Due to its facile synthesis and excellent efficiency,hierarchical p-V2O3SHN presents itself as a promising candidate for the selective uptake of Au(Ⅲ),Ag(Ⅰ),Pt(Ⅳ),and Pd(Ⅱ) from electronic waste.展开更多
Aromatic nitro compounds present substantial health and environmental concerns due to their toxic nature and potential explosive properties.Consequently,the development of host–vip molecular recognition systems for...Aromatic nitro compounds present substantial health and environmental concerns due to their toxic nature and potential explosive properties.Consequently,the development of host–vip molecular recognition systems for these compounds serves a dual-purpose:enabling the fabrication of high-performance sensors for detection and guiding the design of efficient adsorbents for environmental remediation.This study investigated the host–vip recognition behavior of perethylated pillar[n]arenes toward two aromatic nitro molecules,1-chloro-2,4-dinitrobenzene and picric acid.Various techniques including^(1)H NMR,2D NOESY NMR,and UV-vis spectroscopy were employed to explore the binding behavior between pillararenes and aromatic nitro vips in solution.Moreover,valuable single crystal structures were obtained to elucidate the distinct solid-state assembly behaviors of these vips with different pillararenes.The assembled solid-state supramolecular structures observed encompassed a 1:1 host–vip inclusion complex,an external binding complex,and an exo-wall tessellation complex.Furthermore,based on the findings from these systems,a pillararene-based test paper was developed for efficient picric acid detection,and the removal of picric acid from solution was also achieved using pillararenes powder.This research provides novel insights into the development of diverse host–vip systems toward hazardous compounds,offering potential applications in environmental protection and explosive detection domains.展开更多
Adsorption by solid amine adsorbent is a promising technology for decarbonization of flue gas.However,adsorption properties of many solid amine adsorbents need to be enhanced,and it is necessary to further study the C...Adsorption by solid amine adsorbent is a promising technology for decarbonization of flue gas.However,adsorption properties of many solid amine adsorbents need to be enhanced,and it is necessary to further study the CO_(2)adsorption mechanism.A novel CO_(2)adsorbent with high capacity was obtained by grafting 3-aminopropyltriethoxysilane(APTES)on a micro-mesoporous composite molecular sieve ZSM-5/MCM-48 as the support,and then impregnated with tetraethylenepentamine(TEPA)or polyethyleneimine(PEI).The maximum adsorption capacity of APTES-ZSM-5/MCM-48-TEPA-60(A-ZM-T60),loaded with 60%(in mass)TEPA,for CO_(2)reaches 5.82 mmol·g^(-1) at 60℃in 15%(in volume)CO_(2).Carbamate,alkyl ammonium carbamate and carbonate are generated during the chemical adsorption,which is dominant for CO_(2)adsorption because of the reaction between CO_(2)and amino groups on the adsorbent,simultaneously accompanied by weak physical adsorption.All above data confirm that these composites display an outstanding adsorption performance with a bright future for CO_(2)capture from flue gas after desulfurization.展开更多
Hydroxyapatite nanoparticles(HAP NPs)were synthesized by a one‐step hydrothermal method.The surface of HAP NPs was grafted-SH and-COOH chelating groups via in situ surface‐modification with iminodiacetic acid(IDA)an...Hydroxyapatite nanoparticles(HAP NPs)were synthesized by a one‐step hydrothermal method.The surface of HAP NPs was grafted-SH and-COOH chelating groups via in situ surface‐modification with iminodiacetic acid(IDA)and 3‐mercaptopropyl trimethoxysilane(MPS)to afford dual surface‐capped nano‐amendment HAPIDA/MPS.The structure of HAP‐IDA/MPS was characterized,and its adsorption performance for Hg^(2+),Cu^(2+),Zn^(2+),Ni^(2+),Co^(2+),and Cd^(2+)was evaluated.The total adsorption capacity of 0.10 g HAP‐IDA/MPS nano‐amendment for Hg^(2+),Cu^(2+),Zn^(2+),Ni^(2+),Co^(2+),and Cd^(2+)with an initial mass concentration of 20 mg·L^(-1) reached 13.7 mg·g^(-1),about 4.3 times as much as that of HAP.Notably,HAP‐IDA/MPS nano‐amendment displayed the highest immobilization rate for Hg^(2+),possibly because of its chemical reaction with-SH to form sulfide,possessing the lowest solubility product constant among a variety of metal sulfides.展开更多
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the financial support from the National Natural Science Foundation of China(Nos.22073025,21603067,and U23A2089)the Program of Science and Technology Plan of the City of Tianjin(No.24JRRCRC00040)+1 种基金Opening Fund of Hubei Key Laboratory of Bioinorganic Chemistry&Materia Medica(No.BCMM202507)the Open Fund of Hubei Key Laboratory of Resources and Chemistry of Chinese Medicine(No.KLRCCM2404).
文摘Recently,reactive oxygen species(ROS)-independent mimetics of oxidase with Au nanoclusters(NCs)as the catalysts and MnO_(2)as electron acceptor have gained attention.In this study,we aim to explore the oxidase-mimicking potential of bovine serum albumin(BSA)-templated metal nanoclusters(BSA-M NCs,where M=Ag,Pt,Cu,or Cd)beyond Au NCs in boosting the oxidation of 3,3',5,5'-tetramethylbenzidine(TMB)by MnO_(2),denoted as BM@Metal.The oxidase-mimetic activity of BM@Metal is independent of ROS and generally enhanced by the incorporation of metal nanoclusters.Notably,this enhancement varies with the metal species,with BSA-Cd exhibiting the highest activity.The X-ray photoelectron spectroscopy(XPS)analysis confirms mixed valence states(Mn(Ⅳ)/Mn(Ⅱ))in BM@Cd.Given that the catalytic activity is closely linked to the substrate adsorption,the label-free isothermal titration calorimetry was employed to probe the affinity between TMB and BSA-M NCs,which provides a robust approach for probing the interface adsorption.The results reveal that the superior catalytic performance of BSA-Cd correlates with enhanced TMB adsorption,likely facilitated by coordination and hydrophobic interactions.Finally,the superior catalytic performance of BSA-M NCs on the oxidation of TMB by MnO_(2)has inspired us to fabricate the assay for analyzing α-glucosidase’s activity.This work not only demonstrates the versatility of metal NCs in constructing ROS-independent oxidase mimetics but also provides interfacial adsorption engineered strategy for the rational design of superior ROS independent mimetics of natural oxidase.
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 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 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.
文摘In this study,we investigated improving the performance of a layered double hydroxide(LDH)for the adsorption of As(III)and As(V)by controlling the morphology of LDH crystals.The LDH was synthesized via a simple coprecipitation method using barely soluble MgO as a precursor and succinic acid(SA)as a morphological control agent.Doping the LDH crystals with carboxylate ions(RCOO−)derived from SA caused the crystals to develop in a radial direction.This changed the pore characteristics and increased the density of active surface sites.Subsequently,SA/MgFe-LDH showed excellent affinity for As(III)and As(V)with maximum sorption densities of 2.42 and 1.60 mmol/g,respectively.By comparison,the pristine MgFe-LDH had sorption capacities of 1.56 and 1.31 mmol/g for As(III)and As(V),respectively.The LDH was effective over a wide pH range for As(III)adsorption(pH 3-8.5)and As(V)adsorption(pH 3-6.5).Using a combination of spectroscopy and sorption modeling calculations,the main sorption mechanism of As(III)and As(V)on SA/MgFe-LDH was identified as inner-sphere complexation via ligand exchangewith hydroxyl group(-OH)and RCOO−.Specifically,bidentate As-Fe complexeswere proposed for both As(III)and As(V)uptake,with the magnitude of formation varying with the initial As concentration.Importantly,the As-laden adsorbent had satisfactory stability in simulated real landfill leachate.These findings demonstrate that SA/MgFe-LDH exhibits considerable potential for remediation of As-contaminated water.
基金Project supported by Rumah Program 2023 and Net Zero Emission Program(1507/Ⅱ.7/HK.01.00/6/2023)a research facility from the National Research and Innovation Agency of Republic of Indonesia。
文摘Recycling rare earth elements(REEs)from waste is necessary for an environmentally sustainable reuse and wastewater management approach.Na-A zeolite was synthesized from coal fly ash(CFA)and applied for Ce^(3+)adsorption.Fourier transform infrared(FTIR)spectra show peaks at 790,500 and 467 cm^(-1),which are bond vibrations of Si-O-Si,Si with Al-O and Si-O-.The surface area is 15.88 m^(2)/g,with a pore size of 2.14 nm.SEM images show a cubic shape,which indicates the formation of zeolite.Field emission and energy disperse spectroscopy(EDS)shows the formation of Si,Al,Na,and O.Na-A zeolite was applied for Ce^(3+)adsorption.The optimum conditions for Ce^(3+)adsorption are 50 ppm concentration,360 min,and pH 6.The maximum adsorption capacity is 176.49 mg/g.Based on the results,it is found that the adsorption of Ce^(3+)by Na-A zeolite is pseudo-second-order.The desorption test using HNO_(3) is more effective than using HCl and H_(2)SO_(4).A desorption efficiency of 97.22%is obtained at 4 cycles.Adsorption test using real sample wastewater demonstrates an adsorption efficiency of 83.35%.
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 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Project supported by the Natural Science Foundation Innovation Group Project of Hubei Province(2023AFA044)the National Natural Science Foundation of China(52222405)+1 种基金the Science and Technology Research Project of Education Department of Hubei Province(Q20221505)the China Postdoctoral Science(2023M731041)。
文摘In order to reveal the effect of 2-hydroxy-3-naphthyl hydroxamic acid(H205)on the flotation behavior and action mechanism of bastnaesite,single-mineral flotation experiments of bastnaesite were conducted.The flotation recovery of bastnaesites can be achieved more than 90%when the aeration rate is 40 mL/min,the rotational speed is 200 r/min,the H205 dosage is 120 mg/L,and the pulp pH ranges from 7 to 9.The action mechanism of H205 on the surface of bastnaesite was studied by simultaneous thermogravimetry and differential scanning calorimetry(TG-DSC),Zeta potential measurements,Fourier transform-infrared spectra(FT-IR)and X-ray photoelectron spectroscopy(XPS).These analysis results show that under suitable flotation conditions,H205 has an obvious adsorption phenomenon on the surface of bastnaesite.The adsorption involves electrostatic interactions and chemical interactions,namely H205 has a strong collecting ability of bastnaesite due to the synergism of electrostatic adsorption and chemical adsorption.This study systematically reveals the flotation behavior and adsorption mechanism of H205 on the surface of bastnaesite,and provides useful theoretical guidance for efficient flotation separation of bastnaesite.
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 Open Project of State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology(No.ES202306).
文摘Treatment of precious metals in electronic waste has attracted tremendous attention and is essential for both environmental protection and resource sustainable development.In this study,a novel adsorbent for precious metal ions,V_(2)O_(3)spiny hollow nanospheres(pV_(2)O_(3)SHN),was synthe sized through a one-step hydrothermal-as sis ted methodology for the adsorption of Au(Ⅲ),Ag(Ⅰ),Pd(Ⅱ),and Pt(Ⅳ) from the leaching solution of electronic waste.The results reveal that the p-V2O3SHN hierarchy was successfully constructed with a hollow structure and dense spiny morphology.The prepared p-V2O3SHN can effectively remove precious metal ions such as Au(Ⅲ),Ag(Ⅰ),Pd(Ⅱ),and Pt(Ⅳ),with the selective capture order being Au(Ⅲ)> Ag(Ⅰ)> Pt(Ⅳ)> Pd(Ⅱ)> other metal ions.This superior adsorption capability can be attributed to the multi-diffusible,intermingled composition,and numerous active sites decorating the p-V2O3SHN hierarchy,facilitating the uptake of Au(Ⅲ),Ag(Ⅰ),Pd(Ⅱ),and Pt(Ⅳ) ions from electronic waste.The Langmuir model provided a better fit for the uptake process,revealing maximum uptake capacities of 833.33 mg/g for Au(Ⅲ),370.37 mg/g for Ag(Ⅰ),42.01 mg/g for Pd(Ⅱ),and 77.51 mg/g for Pt(Ⅳ) on p-V_(2)O_(3)SHN.Remarkably,p-V_(2)O_(3)SHN exhibited a robust affinity for the adsorbate due to the presence of surface defects and reduction reactions.The new p-V2O3SHN also demonstrated good reusability for three sorption cycles,highlighting its potential for electronic waste treatment.Due to its facile synthesis and excellent efficiency,hierarchical p-V2O3SHN presents itself as a promising candidate for the selective uptake of Au(Ⅲ),Ag(Ⅰ),Pt(Ⅳ),and Pd(Ⅱ) from electronic waste.
基金supported by the fundamental research funds of Zhejiang Sci-Tech University(No.22212286-Y)the Natural Science Foundation of Zhejiang Province(No.LQ24B040003)。
文摘Aromatic nitro compounds present substantial health and environmental concerns due to their toxic nature and potential explosive properties.Consequently,the development of host–vip molecular recognition systems for these compounds serves a dual-purpose:enabling the fabrication of high-performance sensors for detection and guiding the design of efficient adsorbents for environmental remediation.This study investigated the host–vip recognition behavior of perethylated pillar[n]arenes toward two aromatic nitro molecules,1-chloro-2,4-dinitrobenzene and picric acid.Various techniques including^(1)H NMR,2D NOESY NMR,and UV-vis spectroscopy were employed to explore the binding behavior between pillararenes and aromatic nitro vips in solution.Moreover,valuable single crystal structures were obtained to elucidate the distinct solid-state assembly behaviors of these vips with different pillararenes.The assembled solid-state supramolecular structures observed encompassed a 1:1 host–vip inclusion complex,an external binding complex,and an exo-wall tessellation complex.Furthermore,based on the findings from these systems,a pillararene-based test paper was developed for efficient picric acid detection,and the removal of picric acid from solution was also achieved using pillararenes powder.This research provides novel insights into the development of diverse host–vip systems toward hazardous compounds,offering potential applications in environmental protection and explosive detection domains.
基金National Natural Science Foundation of China(51966002)Natural Science Foundation of Guangxi Province(2020GXNSFAA159144)。
文摘Adsorption by solid amine adsorbent is a promising technology for decarbonization of flue gas.However,adsorption properties of many solid amine adsorbents need to be enhanced,and it is necessary to further study the CO_(2)adsorption mechanism.A novel CO_(2)adsorbent with high capacity was obtained by grafting 3-aminopropyltriethoxysilane(APTES)on a micro-mesoporous composite molecular sieve ZSM-5/MCM-48 as the support,and then impregnated with tetraethylenepentamine(TEPA)or polyethyleneimine(PEI).The maximum adsorption capacity of APTES-ZSM-5/MCM-48-TEPA-60(A-ZM-T60),loaded with 60%(in mass)TEPA,for CO_(2)reaches 5.82 mmol·g^(-1) at 60℃in 15%(in volume)CO_(2).Carbamate,alkyl ammonium carbamate and carbonate are generated during the chemical adsorption,which is dominant for CO_(2)adsorption because of the reaction between CO_(2)and amino groups on the adsorbent,simultaneously accompanied by weak physical adsorption.All above data confirm that these composites display an outstanding adsorption performance with a bright future for CO_(2)capture from flue gas after desulfurization.
文摘Hydroxyapatite nanoparticles(HAP NPs)were synthesized by a one‐step hydrothermal method.The surface of HAP NPs was grafted-SH and-COOH chelating groups via in situ surface‐modification with iminodiacetic acid(IDA)and 3‐mercaptopropyl trimethoxysilane(MPS)to afford dual surface‐capped nano‐amendment HAPIDA/MPS.The structure of HAP‐IDA/MPS was characterized,and its adsorption performance for Hg^(2+),Cu^(2+),Zn^(2+),Ni^(2+),Co^(2+),and Cd^(2+)was evaluated.The total adsorption capacity of 0.10 g HAP‐IDA/MPS nano‐amendment for Hg^(2+),Cu^(2+),Zn^(2+),Ni^(2+),Co^(2+),and Cd^(2+)with an initial mass concentration of 20 mg·L^(-1) reached 13.7 mg·g^(-1),about 4.3 times as much as that of HAP.Notably,HAP‐IDA/MPS nano‐amendment displayed the highest immobilization rate for Hg^(2+),possibly because of its chemical reaction with-SH to form sulfide,possessing the lowest solubility product constant among a variety of metal sulfides.
