This study presents a facile and rapid method for synthesizing novel Layered Double Hydroxide(LDH)nanoflakes,exploring their application as a photocatalyst,and investigating the influence of condensed phosphates'g...This study presents a facile and rapid method for synthesizing novel Layered Double Hydroxide(LDH)nanoflakes,exploring their application as a photocatalyst,and investigating the influence of condensed phosphates'geometric linearity on their photocatalytic properties.Herein,the Mg O film,obtained by plasma electrolysis of AZ31 Mg alloys,was modified by growing an LDH film,which was further functionalized using cyclic sodium hexametaphosphate(CP)and linear sodium tripolyphosphate(LP).CP acted as an enhancer for flake spacing within the LDH structure,while LP changed flake dispersion and orientation.Consequently,CP@LDH demonstrated exceptional efficiency in heterogeneous photocatalysis,effectively degrading organic dyes like Methylene blue(MB),Congo red(CR),and Methyl orange(MO).The unique cyclic structure of CP likely enhances surface reactions and improves the catalyst's interaction with dye molecules.Furthermore,the condensed phosphate structure contributes to a higher surface area and reactivity in CP@LDH,leading to its superior photocatalytic performance compared to LP@LDH.Specifically,LP@LDH demonstrated notable degradation efficiencies of 93.02%,92.89%,and 88.81%for MB,MO,and CR respectively,over a 40 min duration.The highest degradation efficiencies were observed in the case of the CP@LDH sample,reporting 99.99%for MB,98.88%for CR,and 99.70%for MO.This underscores the potential of CP@LDH as a highly effective photocatalyst for organic dye degradation,offering promising prospects for environmental remediation and water detoxification applications.展开更多
A novel photo-catalytic system composed of N-doped biochars(NBCs),MnFe_(2)O_(4) and sulfite activation under ultraviolet(NBCs/MnFe_(2)O_(4)/sulfite/UV)was constructed to realize the efficient eliminate of tetracycline...A novel photo-catalytic system composed of N-doped biochars(NBCs),MnFe_(2)O_(4) and sulfite activation under ultraviolet(NBCs/MnFe_(2)O_(4)/sulfite/UV)was constructed to realize the efficient eliminate of tetracycline(TC).As the carrier of MnFe_(2)O_(4),NBCs were synthesized from alfalfa,which has large specific surface area,graphite like structure and hierarchical porous structure.The adsorption isotherm indicated that NBCs/MnFe_(2)O_(4)-2:1 had the best adsorption performance for TC(347.56 mg g^(-1)).Through synergistic adsorption and photocatalysis,the removal rate of TC reached 84%,which was significantly higher than that of MnFe_(2)O_(4).Electrochemical impedance spectroscopy(EIS)and Photoluminescence(PL)characterization results showed that the introduction of NBCs improved the separation efficiency of photogenerated electron and hole pairs and enhanced the photocatalytic performance.Moreover,the adsorption,degradation mechanism and degradation path of TC by the catalyst were systematically analyzed by coupling HPLC–MS measurement with the theoretical calculation.Considering the advantages of excellent degradation performance,low cost,easy separation and environmental friendliness of NBCs/MnFe_(2)O_(4),this work was expected to provide a new path for the practical application of biochar.展开更多
Temperature-swing adsorption(TSA)is an effective technique for CO_(2) capture,but the temperature swing procedure is energy-intensive.Herein,we report a low-energy-consumption system by combining passive radiative coo...Temperature-swing adsorption(TSA)is an effective technique for CO_(2) capture,but the temperature swing procedure is energy-intensive.Herein,we report a low-energy-consumption system by combining passive radiative cooling and solar heating for the uptake of CO_(2) on commercial activated carbons(CACs).During adsorption,the adsorbents are coated with a layer of hierarchically porous poly(vinylidene fluoride-co-hexafluoropropene)[P(VdF-HFP)HP],which cools the adsorbents to a low temperature under sunlight through radiative cooling.For desorption,CACs with broad absorption of the solar spectrum are exposed to light irradiation for heating.The heating and cooling processes are completely driven by solar energy.Adsorption tests under mimicked sunlight using the CACs show that the performance of this system is comparable to that of the traditional ones.Furthermore,under real sunlight irradiation,the adsorption capacity of the CACs can be well maintained after multiple cycles.The present work may inspire the development of new temperature swing procedures with little energy consumption.展开更多
Poria cocos(PC)is a famous traditional Chinese medicine(TCM)and a widely used healthcare ingredient,which has antiobesity,enhancing immunity and improving sleep effects.Traditionally,only water-soluble poria polysacch...Poria cocos(PC)is a famous traditional Chinese medicine(TCM)and a widely used healthcare ingredient,which has antiobesity,enhancing immunity and improving sleep effects.Traditionally,only water-soluble poria polysaccharide(WSP)is extracted and applied for clinical application,while insoluble polysaccharide(alkali-soluble poria polysaccharide,ASP)is discarded as herb residue.However,the whole PC has also been historically utilized as functional herbal food.Considering the beneficial role of dietary fiber and the traditional use of PC,ASP may also contribute substantially to the therapy function of PC.Compared to WSP,little attention has been paid to ASP and ASP modified product carboxymethyl poria polysaccharide(CMP)which has been used as an antitumor adjuvant drug.In this study,the oil,cholesterol,metal ions and polyphenols adsorption ability,in vitro simulated digestive and the gut microbiota fermentation characteristics of WSP,ASP and CMP were studied to evaluate the functional values of three P.cocos polysaccharides(PCPs).The results showed that all three PCPs had good adsorption capacity on cholesterol,polyphenols and metal ions(Cd^(2+)/Zn^(2+)/Mg^(2+)),among which ASP showed the highest capacity than WSP and CMP.The adsorption capacity of all three PCPs on heavy metal ions(Cd^(2+)/Zn^(2+))was stronger than that of non-heavy metal ions(Mg^(2+));The in vitro digestibility of all three PCPs was very low,but WSP was slightly higher than ASP and CMP;Moreover,the indigestible residue of all three PCPs could improve the richness and diversity of gut microbiota,among which ASP had the greatest influence.In general,ASP and CMP could significantly promote the proliferation of some probiotics and inhibit the growth of some harmful bacteria.The gut microbiota diversity of CMP was reduced,but the richness of probiotics,especially Parabacteroides distasonis was significantly enhanced compared with the ASP group,and the growth of harmful bacteria Klebsiella pneumoniae was inhibited after CMP treatment.The short-chain fatty acids(SCFAs)analysis results showed that all three PCPs could significantly promote the production of acetic acid,propionic acid and the total acid content compared with blank control group,and SCFAs producing activity was positively correlated with the proliferative capacity of probiotics.Taken together,the good adsorption characteristics and gut microbiota regulatory activity of ASP may lay foundation for its lipid-lowering and immune-improving function.Additionally,the probiotic effect of CMP and ASP indicated that except for only use the water extract of PC in clinic,CMP and ASP also can be used in healthcare to take full advantage of this valuable medicine.展开更多
Flue gas and coal bed methane are two important sources of greenhouse gases.Pressure swing adsorption process has a wide range of application in the field of gas separation,and the selection of adsorbent is crucial.In...Flue gas and coal bed methane are two important sources of greenhouse gases.Pressure swing adsorption process has a wide range of application in the field of gas separation,and the selection of adsorbent is crucial.In this regard,in order to assess the better adsorbent for separating CO_(2) from flue gas and CH_(4) from coal bed methane,adsorption isotherms of CO_(2),CH_(4) and N_(2) on activated carbon and carbon molecular sieve are measured at 303.15,318.15 and 333.15 K,and up to 250 kPa.The experimental data fit better with Langmuir 2 compared to Langmuir 3 and Langmuir-Freundlich models,and Clausius-Clapeyron equation was used to calculate the isosteric heat.Both the order of the adsorbed amount and the adsorption heat on the two adsorbents are CO_(2)>CH_(4)>N_(2).The adsorption kinetics are calculated by the pseudo-first kinetic model,and the order of adsorption rates on activated carbon is N_(2)-CH_(4)>CO_(2),while on carbon molecular sieve,it is CO_(2)-N_(2)>CH_(4).It is shown that relative molecular mass and adsorption heat are the primary effect on kinetics for activated carbon,while kinetic diameter is the main resistance factor for carbon molecular sieve.Moreover,the adsorption selectivity of CH_(4)/N_(2) and CO_(2)/N_(2) were estimated with the ideal adsorption solution theory,and carbon molecular sieve performed best at 318.15 K for both CO_(2) and CH_(4) separation.The study suggested that activated carbon is a better choice for separating flue gas and carbon molecular sieve can be a strong candidate for separating coal bed methane.展开更多
The adsorption process of droplets on the liquid-liquid interface and phase separation process can regulate the spatial distribution of the fluid system,which are crucial for chemical engineering.However,the cross-lin...The adsorption process of droplets on the liquid-liquid interface and phase separation process can regulate the spatial distribution of the fluid system,which are crucial for chemical engineering.However,the cross-linking reaction,which is widely used in the field of polymers,can change the physical properties of the fluids and affect the flow behavior accordingly.A configuration of microchannels is designed to conveniently generate uniform droplets in one phase of the parallel flow.The flow behavior of the adsorption process of sodium alginate droplets on the liquid-liquid interface is investigated,and the subsequent process of phase separation is studied.In the process of droplet adsorption,the crosslinking reaction occurs synchronously,which makes the droplet viscosity and the elasticity modules of the droplet surface increase,thus affecting the dynamics of the adsorption process and the equilibrium shape of the droplet.The variation of the adsorption length with time is divided into three stages,which all conform to power law relationship.The exponents of the second and third stages deviate from the results of the Tanner's law.The flow pattern maps of droplet adsorption and phase separation are drawn,and the operating ranges of complete adsorption and complete separation are provided.This study provides a theoretical basis for further studying the flow behavior of droplets with cross-linking reaction in a microchannel.展开更多
A core-shell composite consisting of ZSM-5 zeolite as the core and ordered mesoporous silica as the shell was prepared by a surfactant-controlled sol-gel process and using tetradecylamine(TDA) as the template and Tetr...A core-shell composite consisting of ZSM-5 zeolite as the core and ordered mesoporous silica as the shell was prepared by a surfactant-controlled sol-gel process and using tetradecylamine(TDA) as the template and Tetraethylorthosilicate(TEOS) as the silica precursor.The pores of the silica shell were found to be ordered and perpendicular to the crystal faces of the zeolite core.The thickness of the shell in the coreshell structured composite can be adjusted in the range of 20-90 nm,while the surface morphology and the pore size distribution were modified by changing the mass ratio of TEOS to zeolite.The composite molecular sieves have higher surface area for capturing molecules than ZSM-5,and with the increase of mesoporous shell layer,the ZSM-5@SiO_(2)-x composites show stronger adsorption capacity of butyraldehyde.However,when the shell thickness exceeds 90 nm,the adsorption capacity of butyraldehyde decreases instead.The composites have a huge potential for environmental applications.展开更多
Three kinds of iron nanoparticles(FeNPs)were prepared via green route based on pomegranate(PG),green tea(GT),and mulberry(ML)extracts under ambient conditions.The obtained materials were characterized by scanning elec...Three kinds of iron nanoparticles(FeNPs)were prepared via green route based on pomegranate(PG),green tea(GT),and mulberry(ML)extracts under ambient conditions.The obtained materials were characterized by scanning electron microscopy(SEM),transmission electronic microscopy(TEM),X-ray energy-dispersive spectrometer(EDS),X-ray diffraction(XRD),fourier transform infrared spectroscopy(FTIR),and X-ray photoelectron spectroscopy(XPS)techniques.The experimental results show that FeNPs were in the form of amorphous iron(Ⅱ,Ⅲ)-polyphenol complex with different dispersity and morphologies.GT-Fe has the smallest size range of 25-35 nm,PG-Fe has a moderate size-distribution of 30-40 nm,while ML-Fe formed a tuberous net-type with a sheeting structure.PG-Fe displays the highest removal efficiency of 90.2%in 20 min towards cationic dye of malachite green(16.6%by ML-Fe and 69.3%by GT-Fe),which is attributed to its highest polyphenol content,lowest zeta potential,as well as the most Fe^(2+)on the surface of FeNPs.The removal mechanism was mainly induced by electrostatic adsorption based on pH and zeta potential tests.展开更多
The flotation of complex solid–liquid multiphase systems involve interactions among multiple components,the core problem facing flotation theory.Meanwhile,the combined use of multicomponent flotation reagents to impr...The flotation of complex solid–liquid multiphase systems involve interactions among multiple components,the core problem facing flotation theory.Meanwhile,the combined use of multicomponent flotation reagents to improve mineral flotation has become an important issue in studies on the efficient use of refractory mineral resources.However,studying the flotation of complex solid–liquid systems is extremely difficult,and no systematic theory has been developed to date.In addition,the physical mechanism associated with combining reagents to improve the flotation effect has not been unified,which limits the development of flotation theory and the progress of flotation technology.In this study,we applied theoretical thermodynamics to a solid–liquid flotation system and used changes in the entropy and Gibbs free energy of the reagents adsorbed on the mineral surface to establish thermodynamic equilibrium equations that de-scribe interactions among various material components while also introducing adsorption equilibrium constants for the flotation reagents adsorbed on the mineral surface.The homogenization effect on the mineral surface in pulp solution was determined using the chemical potentials of the material components of the various mineral surfaces required to maintain balance.The flotation effect can be improved through synergy among multicomponent flotation reagents;its physical essence is the thermodynamic law that as the number of compon-ents of flotation reagents on the mineral surface increases,the surface adsorption entropy change increases,and the Gibbs free energy change of adsorption decreases.According to the results obtained using flotation thermodynamics theory,we established high-entropy flotation theory and a technical method in which increasing the types of flotation reagents adsorbed on the mineral surface,increasing the adsorption entropy change of the flotation reagents,decreasing the Gibbs free energy change,and improving the adsorption efficiency and stability of the flotation reagents improves refractory mineral flotation.展开更多
Comparative experiments and theoretical analysis of the surface chemistry changes of goethite(GT)and goethite containing Ni(GTN)in the lattice in the presence of salicylhydroxamic acid(SA)were performed.It was reveale...Comparative experiments and theoretical analysis of the surface chemistry changes of goethite(GT)and goethite containing Ni(GTN)in the lattice in the presence of salicylhydroxamic acid(SA)were performed.It was revealed that in the presence of 100 g·t^(-1)of SA,the flotation recovery of GTN and GT increased with increasing pH,achieving a maximum recovery of 98.9%for both minerals at p H 8.3 and decreasing beyond that pH,with GTN having a slightly higher recovery than GT,except at pH 8.3.This was further confirmed by the higher complexation energies of GTN···SA(-883.87 kJ·mol^(-1))compared with GT···SA(-604.23 kJ·mol^(-1))resulting from covalent,closed-shell,and conventional hydrogen bonding.The higher adsorption of SA onto GTN relative to GT was due to the formation of aπ-hole in GTN,thereby promoting a higher interaction of the collector with the mineral.Thus,the presence of Ni in the GT lattice improves and decreases the adsorption and desorption of SA onto and from the mineral,respectively,compared with those onto and from GT.展开更多
The nitrite(NO_(2)^(−))to ammonia(NH3)electroreduction reaction(NO_(2)^(−)RR)would be impeded by sluggish proton-coupled electron transfer kinetics and competitive hydrogen evolution reaction(HER).A key to improving t...The nitrite(NO_(2)^(−))to ammonia(NH3)electroreduction reaction(NO_(2)^(−)RR)would be impeded by sluggish proton-coupled electron transfer kinetics and competitive hydrogen evolution reaction(HER).A key to improving the NH_(3) selectivity is to facilitate adsorption and activation of NO_(2)^(−),which is generally undesirable in unitary species.In this work,an efficient NO_(2)^(−)RR catalyst is constructed by cooperating Pd with In2O3,in which NO_(2)^(−)could adsorb on interfacial dual-site through“Pd–N–O–In”linkage,leading to strengthened NO_(2)^(−)adsorption and easier N=O bond cleavage than that on unitary Pd or In2O3.Moreover,the Pd/In_(2)O_(3)composite exhibits moderate H^(*)adsorption,which may facilitate protonation kinetics while inhibiting competitive HER.As a result,it exhibits a fairly high NH_(3)yield rate of 622.76 mmol h^(−1)g^(−1)cat with a Faradaic efficiency(FE)of 95.72%,good selectivity of 91.96%,and cycling stability towards the NO_(2)^(−)RR,surpassing unitary In_(2)O_(3)and Pd/C electrocatalysts.Besides,computed results indicate that NH_(3)production on Pd/In_(2)O_(3)follows the deoxidation to hydrogenation pathway.This work highlights the significance of H^(*)and NO_(2)^(−)adsorption modulation and N=O activation in NO_(2)^(−)RR electrochemistry by creating synergy between a mediocre catalyst with an appropriate cooperator.展开更多
It is quite important to ensure the safety and sustainable development of nuclear energy for the treatment of radioactive wastewater. To treat radioactive wastewater efficiently and rapidly, two multi-amine β-cyclode...It is quite important to ensure the safety and sustainable development of nuclear energy for the treatment of radioactive wastewater. To treat radioactive wastewater efficiently and rapidly, two multi-amine β-cyclodextrin polymers(diethylenetriamine β-cyclodextrin polymer(DETA-TFCDP) and triethylenetetramine β-cyclodextrin polymer(TETA-TFCDP)) were prepared and applied to capture uranium. Results exhibited that DETA-TFCDP and TETA-TFCDP displayed the advantages of high adsorption amounts(612.2and 628.2 mg·g-1, respectively) and rapid adsorption rates, which can reach(88 ± 1)% of their equilibrium adsorption amounts in 10 min. Moreover, the adsorbent processes of DETA-TFCDP and TETATFCDP on uranium(Ⅵ) followed the Langmuir model and pseudo-second-order model, stating they were mainly chemisorption and self-endothermic. Besides, TETA-TFCDP also showed excellent selectivity in the presence of seven competing cations and could be effectively reused five times via Na2CO3as the desorption reagent. Meanwhile, X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy illustrated that the enriched multi-amine groups and oxygen-containing functional groups on the surface of TETA-TFCDP were the main active sites for capturing uranium(Ⅵ). Hence, multi-amine β-cyclodextrin polymers are a highly efficient, rapid, and promising adsorbent for capturing uranium(Ⅵ)from radioactive wastewater.展开更多
Investigating zeolites as hydrogen storage scaffolds is imperative due to their porous nature and favorable physicochemical properties.Nevertheless,the storage capacity of the unmodified zeolites has been rather unsat...Investigating zeolites as hydrogen storage scaffolds is imperative due to their porous nature and favorable physicochemical properties.Nevertheless,the storage capacity of the unmodified zeolites has been rather unsatisfactory(0.224%-1.082%(mass))compared to its modified counterpart.Thus,the contemporary focus on enhancing hydrogen storage capacities has led to significant attention towards the utilization of modified zeolites,with studies exploring surface modifications through physical and chemical treatments,as well as the integration of various active metals.The enhanced hydrogen storage properties of zeolites are attributed to the presence of aluminosilicates from alkaline and alkaline-earth metals,resulting in increased storage capacity through interactions with the charge density of these aluminosilicates.Therefore,there is a great demand to critically review their role such as well-defined topology,pore structure,good thermal stability,and tunable hydrophilicity in enhanced hydrogen storage.This article aimed to critically review the recent research findings based on modified zeolite performance for enhanced hydrogen storage.Some of the factors affecting the hydrogen storage capacities of zeolites that can affect the rate of reaction and the stability of the adsorbent,like pressure,structure,and morphology were studied,and examined.Then,future perspectives,recommendations,and directions for modified zeolites were discussed.展开更多
Graphene-based materials possess significant potential for the treatment of dye wastewater due to their exceptional adsorption properties toward stubborn pollutants.However,their utilization is hindered by high prepar...Graphene-based materials possess significant potential for the treatment of dye wastewater due to their exceptional adsorption properties toward stubborn pollutants.However,their utilization is hindered by high preparation costs,low yields,environmental pollution during synthesis,and challenges in regenerating the adsorbent.This study proposes a novel approach to address these limitations by developing nitrogen-doped three-dimensional(3D)polyvinyl alcohol(PVA)crosslinked graphene sponges(N-PGA)using a cross-linking method with ammonium carbonate.This method offers a relatively mild,environmentally friendly approach.Ammonium carbonate serves as both a reducing and modifying agent,facilitating the formation of the intrinsic structure of N-PGA and acting as a nitrogen source.Meanwhile,PVA is utilized as the cross-linking agent.The results demonstrate that N-PGA exhibits a favorable internal 3D hierarchical porous structure and possesses robust mechanical properties.The measured specific surface area(BET)of N-PGA was as high as406.538 m^(2)·g^(-1),which was favorable for its efficient adsorption of Congo red(CR)dye molecules.At an initial concentration of 50 mg·L^(-1),N-PGA achieved an impressive removal rate of 89.6%and an adsorption capacity of 112 mg·g^(-1)for CR dye.Furthermore,it retained 79%of its initial adsorption capacity after 10 cycles,demonstrating excellent regeneration performance.In summary,the synthesized N-PGA displays remarkable efficacy in the adsorption of CR dye in wastewater,opening up new possibilities for utilizing 3D porous graphene nanomaterials as efficient adsorbents in wastewater treatment.展开更多
Phosphate was removed from aqueous environment by corundum-hollow-spheres supported caclined hydrotalcite (cHT) thin films. Mg-Al-CO3 hydrotalcite (HT) thin films were deposited on corundumhollow-sphere substrates by ...Phosphate was removed from aqueous environment by corundum-hollow-spheres supported caclined hydrotalcite (cHT) thin films. Mg-Al-CO3 hydrotalcite (HT) thin films were deposited on corundumhollow-sphere substrates by hydrothermal homogeneous precipitation at 120℃for 30-240 min and cHT thin films were obtained by annealing of the HT thin films at 500℃for 180 min. Their crystal phase, morphology and microstructure were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM).The results show that homogeneous, well-crystallized and hierarchical flower-like thin films were deposited firmly on the surface of the corundum. The mechanism of nucleation and growth of the HT thin films was fitted well with the anion coordination polyhedron growth unit model. To determine the absorption of phosphate by this adsorbent, different bed depth (10-30 cm) and flow rate (1.0-3.0 m L/min) were examined by column experiments. The highest removal efficiency of phosphate amounted to 98.5%under optimum condition (pH=7.2). The adsorption capacity increased as the bed depth increased and decreased as the flow rate increased.展开更多
Understanding the adsorption interactions between carbon materials and sulfur compounds has far-reaching impacts,in addition to their well-known important role in energy storage and conversion,such as lithium-ion batt...Understanding the adsorption interactions between carbon materials and sulfur compounds has far-reaching impacts,in addition to their well-known important role in energy storage and conversion,such as lithium-ion batteries.In this paper,properties of intrinsic B or Si single-atom doped,and B-Si codoped graphene(GR)and graphdiyne(GDY)were investigated by using density functional theory-based calculations,in which the optimal doping configurations were explored for potential applications in adsorbing sulfur compounds.Results showed that both B or Si single-atom doping and B-Si codoping could substantially enhance the electron transport properties of GR and GDY,improving their surface activity.Notably,B and Si atoms displayed synergistic effects for the codoped configurations,where B-Si codoped GR/GDY exhibited much better performance in the adsorption of sulfurcontaining chemicals than single-atom doped systems.In addition,results demonstrated that,after B-Si codoping,the adsorption energy and charge transfer amounts of GDY with sulfur compounds were much larger than those of GR,indicating that B-Si codoped GDY might be a favorable material for more effectively interacting with sulfur reagents.展开更多
Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performan...Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performance for hydrogen evolution reaction(HER). With the VS concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS_(2)-VS 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential(68 m V) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy(ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S-H* peak of the Ni S_(2)-VS 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the Ni S_(2)-VS 5.9% has the optimal |ΔG^(H*)| of 0.17 e V. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy.展开更多
A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structur...A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structure and the defective sites of h-BNNS not only are beneficial to the stabilization of Pt NPs but also favor the adsorption of aromatic sulfides.By employing Pt/h-BNNS with a Pt loading amount of 1.19 wt%as the active adsorbent and air as an oxidant,a 98.0%sulfur removal over dibenzothiophene(DBT)is achieved along with a total conversion of the DBT to the corresponding sulfones(DBTO_(2)).Detailed experiments show that the excellent desulfurization activity originates from the few-layered structure of h-BNNS and the high catalytic activity of Pt NPs.In addition,the OPADS system with Pt/h-BNNS as the active adsorbent shows remarkable stability in desulfurization performance with the existence of different interferents such as olefin,and aromatic hydrocarbons.Besides,the Pt/h-BNNS can be recycled 12 times without a significant decrease in desulfurization performance.Also,a process flow diagram is proposed for deep desulfurization of fuel oil and recovery of high value-added products,which would promote the industrial application of such OPADS strategy.展开更多
Lignocellulose has the potential to become a bio-based adsorbent due to its biodegradability and renewability.In this study,a novel polydopamine functionalized-lignin(lignin@PDA),prepared via self-polymerization of do...Lignocellulose has the potential to become a bio-based adsorbent due to its biodegradability and renewability.In this study,a novel polydopamine functionalized-lignin(lignin@PDA),prepared via self-polymerization of dopamine(PDA)on lignin,was used as a bio-based adsorbent for rapid scavenging of hexavalent chromium(Cr(VI)).The morphology,functional groups,crystalline structure,and chemical composition of lignin@PDA were characterized with a scanning electron microscope-energy dispersive spectrometer,Fourier transform infrared spectroscopy,X-ray diffraction,and X-ray photoelectron spectroscopy.The Cr(VI)adsorption process of lignin@PDA was studied using batch experiments as a function of pH,ionic strength,adsorbent dose,and contact time at room temperature.The adsorption rate of lignin@PDA was five times greater than that of the unmodified lignin,with a maximum adsorption capacity of 102.6 mg/g in an acidic medium.The adsorption of Cr(VI)on lignin@PDA fit the pseudo-secondorder equation and the Freundlich model,indicating that the adsorption process was mainly dominated by chemisorption and surface complexation.The thermodynamic parameters showed that adsorption of Cr(VI)on lignin@PDA was an endothermic and spontaneous process.The X-ray absorption fine structure results showed that sorption and reduction of Cr(VI)into Cr(II)occurred simultaneously on lignin.Moreover,PDA coating not only improved the reactivity of lignin but also promoted the complete reduction of Cr(VI)by lignin.According to these results,polydopamine functionalized-lignin is a promising bio-based adsorbent for immobilization of Cr(VI)from wastewater.展开更多
基金the National Research Foundation of Korea(NRF)funded by the Korean Government(MSIT)(No.2022R1A2C1006743)。
文摘This study presents a facile and rapid method for synthesizing novel Layered Double Hydroxide(LDH)nanoflakes,exploring their application as a photocatalyst,and investigating the influence of condensed phosphates'geometric linearity on their photocatalytic properties.Herein,the Mg O film,obtained by plasma electrolysis of AZ31 Mg alloys,was modified by growing an LDH film,which was further functionalized using cyclic sodium hexametaphosphate(CP)and linear sodium tripolyphosphate(LP).CP acted as an enhancer for flake spacing within the LDH structure,while LP changed flake dispersion and orientation.Consequently,CP@LDH demonstrated exceptional efficiency in heterogeneous photocatalysis,effectively degrading organic dyes like Methylene blue(MB),Congo red(CR),and Methyl orange(MO).The unique cyclic structure of CP likely enhances surface reactions and improves the catalyst's interaction with dye molecules.Furthermore,the condensed phosphate structure contributes to a higher surface area and reactivity in CP@LDH,leading to its superior photocatalytic performance compared to LP@LDH.Specifically,LP@LDH demonstrated notable degradation efficiencies of 93.02%,92.89%,and 88.81%for MB,MO,and CR respectively,over a 40 min duration.The highest degradation efficiencies were observed in the case of the CP@LDH sample,reporting 99.99%for MB,98.88%for CR,and 99.70%for MO.This underscores the potential of CP@LDH as a highly effective photocatalyst for organic dye degradation,offering promising prospects for environmental remediation and water detoxification applications.
基金gratefully acknowledge the financial support for this research from the National Natural Science Foundation of China(Grant No.:21978047,21776046)the Six Talent Climax Foundation of Jiangsu(Grant No.:XCL-079).
文摘A novel photo-catalytic system composed of N-doped biochars(NBCs),MnFe_(2)O_(4) and sulfite activation under ultraviolet(NBCs/MnFe_(2)O_(4)/sulfite/UV)was constructed to realize the efficient eliminate of tetracycline(TC).As the carrier of MnFe_(2)O_(4),NBCs were synthesized from alfalfa,which has large specific surface area,graphite like structure and hierarchical porous structure.The adsorption isotherm indicated that NBCs/MnFe_(2)O_(4)-2:1 had the best adsorption performance for TC(347.56 mg g^(-1)).Through synergistic adsorption and photocatalysis,the removal rate of TC reached 84%,which was significantly higher than that of MnFe_(2)O_(4).Electrochemical impedance spectroscopy(EIS)and Photoluminescence(PL)characterization results showed that the introduction of NBCs improved the separation efficiency of photogenerated electron and hole pairs and enhanced the photocatalytic performance.Moreover,the adsorption,degradation mechanism and degradation path of TC by the catalyst were systematically analyzed by coupling HPLC–MS measurement with the theoretical calculation.Considering the advantages of excellent degradation performance,low cost,easy separation and environmental friendliness of NBCs/MnFe_(2)O_(4),this work was expected to provide a new path for the practical application of biochar.
基金supported by the National Science Fund for Distinguished Young Scholars(22125804)the National Natural Science Foundation of China(21808110,22078155,and 21878149).
文摘Temperature-swing adsorption(TSA)is an effective technique for CO_(2) capture,but the temperature swing procedure is energy-intensive.Herein,we report a low-energy-consumption system by combining passive radiative cooling and solar heating for the uptake of CO_(2) on commercial activated carbons(CACs).During adsorption,the adsorbents are coated with a layer of hierarchically porous poly(vinylidene fluoride-co-hexafluoropropene)[P(VdF-HFP)HP],which cools the adsorbents to a low temperature under sunlight through radiative cooling.For desorption,CACs with broad absorption of the solar spectrum are exposed to light irradiation for heating.The heating and cooling processes are completely driven by solar energy.Adsorption tests under mimicked sunlight using the CACs show that the performance of this system is comparable to that of the traditional ones.Furthermore,under real sunlight irradiation,the adsorption capacity of the CACs can be well maintained after multiple cycles.The present work may inspire the development of new temperature swing procedures with little energy consumption.
基金supported by the Province Natural Science Foundation of Hunan,China (2022JJ5410)Special Project on Modern Agricultural Industrial Technology System Construction of Hunan,China (2022-67)。
文摘Poria cocos(PC)is a famous traditional Chinese medicine(TCM)and a widely used healthcare ingredient,which has antiobesity,enhancing immunity and improving sleep effects.Traditionally,only water-soluble poria polysaccharide(WSP)is extracted and applied for clinical application,while insoluble polysaccharide(alkali-soluble poria polysaccharide,ASP)is discarded as herb residue.However,the whole PC has also been historically utilized as functional herbal food.Considering the beneficial role of dietary fiber and the traditional use of PC,ASP may also contribute substantially to the therapy function of PC.Compared to WSP,little attention has been paid to ASP and ASP modified product carboxymethyl poria polysaccharide(CMP)which has been used as an antitumor adjuvant drug.In this study,the oil,cholesterol,metal ions and polyphenols adsorption ability,in vitro simulated digestive and the gut microbiota fermentation characteristics of WSP,ASP and CMP were studied to evaluate the functional values of three P.cocos polysaccharides(PCPs).The results showed that all three PCPs had good adsorption capacity on cholesterol,polyphenols and metal ions(Cd^(2+)/Zn^(2+)/Mg^(2+)),among which ASP showed the highest capacity than WSP and CMP.The adsorption capacity of all three PCPs on heavy metal ions(Cd^(2+)/Zn^(2+))was stronger than that of non-heavy metal ions(Mg^(2+));The in vitro digestibility of all three PCPs was very low,but WSP was slightly higher than ASP and CMP;Moreover,the indigestible residue of all three PCPs could improve the richness and diversity of gut microbiota,among which ASP had the greatest influence.In general,ASP and CMP could significantly promote the proliferation of some probiotics and inhibit the growth of some harmful bacteria.The gut microbiota diversity of CMP was reduced,but the richness of probiotics,especially Parabacteroides distasonis was significantly enhanced compared with the ASP group,and the growth of harmful bacteria Klebsiella pneumoniae was inhibited after CMP treatment.The short-chain fatty acids(SCFAs)analysis results showed that all three PCPs could significantly promote the production of acetic acid,propionic acid and the total acid content compared with blank control group,and SCFAs producing activity was positively correlated with the proliferative capacity of probiotics.Taken together,the good adsorption characteristics and gut microbiota regulatory activity of ASP may lay foundation for its lipid-lowering and immune-improving function.Additionally,the probiotic effect of CMP and ASP indicated that except for only use the water extract of PC in clinic,CMP and ASP also can be used in healthcare to take full advantage of this valuable medicine.
基金supported by the renewable energy and hydrogen projects in National Key Research and Development Plan of China(2019YFB1505000).
文摘Flue gas and coal bed methane are two important sources of greenhouse gases.Pressure swing adsorption process has a wide range of application in the field of gas separation,and the selection of adsorbent is crucial.In this regard,in order to assess the better adsorbent for separating CO_(2) from flue gas and CH_(4) from coal bed methane,adsorption isotherms of CO_(2),CH_(4) and N_(2) on activated carbon and carbon molecular sieve are measured at 303.15,318.15 and 333.15 K,and up to 250 kPa.The experimental data fit better with Langmuir 2 compared to Langmuir 3 and Langmuir-Freundlich models,and Clausius-Clapeyron equation was used to calculate the isosteric heat.Both the order of the adsorbed amount and the adsorption heat on the two adsorbents are CO_(2)>CH_(4)>N_(2).The adsorption kinetics are calculated by the pseudo-first kinetic model,and the order of adsorption rates on activated carbon is N_(2)-CH_(4)>CO_(2),while on carbon molecular sieve,it is CO_(2)-N_(2)>CH_(4).It is shown that relative molecular mass and adsorption heat are the primary effect on kinetics for activated carbon,while kinetic diameter is the main resistance factor for carbon molecular sieve.Moreover,the adsorption selectivity of CH_(4)/N_(2) and CO_(2)/N_(2) were estimated with the ideal adsorption solution theory,and carbon molecular sieve performed best at 318.15 K for both CO_(2) and CH_(4) separation.The study suggested that activated carbon is a better choice for separating flue gas and carbon molecular sieve can be a strong candidate for separating coal bed methane.
基金supported by the National Natural Science Foundation of China(92034303,21978197)。
文摘The adsorption process of droplets on the liquid-liquid interface and phase separation process can regulate the spatial distribution of the fluid system,which are crucial for chemical engineering.However,the cross-linking reaction,which is widely used in the field of polymers,can change the physical properties of the fluids and affect the flow behavior accordingly.A configuration of microchannels is designed to conveniently generate uniform droplets in one phase of the parallel flow.The flow behavior of the adsorption process of sodium alginate droplets on the liquid-liquid interface is investigated,and the subsequent process of phase separation is studied.In the process of droplet adsorption,the crosslinking reaction occurs synchronously,which makes the droplet viscosity and the elasticity modules of the droplet surface increase,thus affecting the dynamics of the adsorption process and the equilibrium shape of the droplet.The variation of the adsorption length with time is divided into three stages,which all conform to power law relationship.The exponents of the second and third stages deviate from the results of the Tanner's law.The flow pattern maps of droplet adsorption and phase separation are drawn,and the operating ranges of complete adsorption and complete separation are provided.This study provides a theoretical basis for further studying the flow behavior of droplets with cross-linking reaction in a microchannel.
文摘A core-shell composite consisting of ZSM-5 zeolite as the core and ordered mesoporous silica as the shell was prepared by a surfactant-controlled sol-gel process and using tetradecylamine(TDA) as the template and Tetraethylorthosilicate(TEOS) as the silica precursor.The pores of the silica shell were found to be ordered and perpendicular to the crystal faces of the zeolite core.The thickness of the shell in the coreshell structured composite can be adjusted in the range of 20-90 nm,while the surface morphology and the pore size distribution were modified by changing the mass ratio of TEOS to zeolite.The composite molecular sieves have higher surface area for capturing molecules than ZSM-5,and with the increase of mesoporous shell layer,the ZSM-5@SiO_(2)-x composites show stronger adsorption capacity of butyraldehyde.However,when the shell thickness exceeds 90 nm,the adsorption capacity of butyraldehyde decreases instead.The composites have a huge potential for environmental applications.
基金Funded by the Hubei Provincial Natural Science Foundation of China(No.2024AFB946)the Excellent Young and Middle-aged Science and Technology Innovation Team Plan of Hubei Colleges(No.T201824)。
文摘Three kinds of iron nanoparticles(FeNPs)were prepared via green route based on pomegranate(PG),green tea(GT),and mulberry(ML)extracts under ambient conditions.The obtained materials were characterized by scanning electron microscopy(SEM),transmission electronic microscopy(TEM),X-ray energy-dispersive spectrometer(EDS),X-ray diffraction(XRD),fourier transform infrared spectroscopy(FTIR),and X-ray photoelectron spectroscopy(XPS)techniques.The experimental results show that FeNPs were in the form of amorphous iron(Ⅱ,Ⅲ)-polyphenol complex with different dispersity and morphologies.GT-Fe has the smallest size range of 25-35 nm,PG-Fe has a moderate size-distribution of 30-40 nm,while ML-Fe formed a tuberous net-type with a sheeting structure.PG-Fe displays the highest removal efficiency of 90.2%in 20 min towards cationic dye of malachite green(16.6%by ML-Fe and 69.3%by GT-Fe),which is attributed to its highest polyphenol content,lowest zeta potential,as well as the most Fe^(2+)on the surface of FeNPs.The removal mechanism was mainly induced by electrostatic adsorption based on pH and zeta potential tests.
基金supported by the Yunnan Science and Technology Leading Talent Project(No.202305AB350005)National Science Foundation for Young Scientists of China(No.51404118).
文摘The flotation of complex solid–liquid multiphase systems involve interactions among multiple components,the core problem facing flotation theory.Meanwhile,the combined use of multicomponent flotation reagents to improve mineral flotation has become an important issue in studies on the efficient use of refractory mineral resources.However,studying the flotation of complex solid–liquid systems is extremely difficult,and no systematic theory has been developed to date.In addition,the physical mechanism associated with combining reagents to improve the flotation effect has not been unified,which limits the development of flotation theory and the progress of flotation technology.In this study,we applied theoretical thermodynamics to a solid–liquid flotation system and used changes in the entropy and Gibbs free energy of the reagents adsorbed on the mineral surface to establish thermodynamic equilibrium equations that de-scribe interactions among various material components while also introducing adsorption equilibrium constants for the flotation reagents adsorbed on the mineral surface.The homogenization effect on the mineral surface in pulp solution was determined using the chemical potentials of the material components of the various mineral surfaces required to maintain balance.The flotation effect can be improved through synergy among multicomponent flotation reagents;its physical essence is the thermodynamic law that as the number of compon-ents of flotation reagents on the mineral surface increases,the surface adsorption entropy change increases,and the Gibbs free energy change of adsorption decreases.According to the results obtained using flotation thermodynamics theory,we established high-entropy flotation theory and a technical method in which increasing the types of flotation reagents adsorbed on the mineral surface,increasing the adsorption entropy change of the flotation reagents,decreasing the Gibbs free energy change,and improving the adsorption efficiency and stability of the flotation reagents improves refractory mineral flotation.
基金supported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)and the Ministry of Trade,Industry&Energy(MOTIE)of the Republic of Korea(No.20227A10100010)。
文摘Comparative experiments and theoretical analysis of the surface chemistry changes of goethite(GT)and goethite containing Ni(GTN)in the lattice in the presence of salicylhydroxamic acid(SA)were performed.It was revealed that in the presence of 100 g·t^(-1)of SA,the flotation recovery of GTN and GT increased with increasing pH,achieving a maximum recovery of 98.9%for both minerals at p H 8.3 and decreasing beyond that pH,with GTN having a slightly higher recovery than GT,except at pH 8.3.This was further confirmed by the higher complexation energies of GTN···SA(-883.87 kJ·mol^(-1))compared with GT···SA(-604.23 kJ·mol^(-1))resulting from covalent,closed-shell,and conventional hydrogen bonding.The higher adsorption of SA onto GTN relative to GT was due to the formation of aπ-hole in GTN,thereby promoting a higher interaction of the collector with the mineral.Thus,the presence of Ni in the GT lattice improves and decreases the adsorption and desorption of SA onto and from the mineral,respectively,compared with those onto and from GT.
基金supported by the National Key R&D Program of China(Nos.2022YFA1503104 and 2022YFA1503102)the Natural Science Foundation of Shandong Province(No.2022HWYQ-009)+2 种基金the Natural Science Foundation of Jiangsu Province(No.BK20230243)Taishan Scholars Project(No.tspd20230601)Qilu Young Scholars Program of Shandong University.
文摘The nitrite(NO_(2)^(−))to ammonia(NH3)electroreduction reaction(NO_(2)^(−)RR)would be impeded by sluggish proton-coupled electron transfer kinetics and competitive hydrogen evolution reaction(HER).A key to improving the NH_(3) selectivity is to facilitate adsorption and activation of NO_(2)^(−),which is generally undesirable in unitary species.In this work,an efficient NO_(2)^(−)RR catalyst is constructed by cooperating Pd with In2O3,in which NO_(2)^(−)could adsorb on interfacial dual-site through“Pd–N–O–In”linkage,leading to strengthened NO_(2)^(−)adsorption and easier N=O bond cleavage than that on unitary Pd or In2O3.Moreover,the Pd/In_(2)O_(3)composite exhibits moderate H^(*)adsorption,which may facilitate protonation kinetics while inhibiting competitive HER.As a result,it exhibits a fairly high NH_(3)yield rate of 622.76 mmol h^(−1)g^(−1)cat with a Faradaic efficiency(FE)of 95.72%,good selectivity of 91.96%,and cycling stability towards the NO_(2)^(−)RR,surpassing unitary In_(2)O_(3)and Pd/C electrocatalysts.Besides,computed results indicate that NH_(3)production on Pd/In_(2)O_(3)follows the deoxidation to hydrogenation pathway.This work highlights the significance of H^(*)and NO_(2)^(−)adsorption modulation and N=O activation in NO_(2)^(−)RR electrochemistry by creating synergy between a mediocre catalyst with an appropriate cooperator.
基金National Natural Science Foundation of China(21603064,52102214)Natural Science Foundation of Jiangxi Province(20202BABL203026,20212BAB203001,20202BABL214016)College Student Innovation and Enterprise Programme of Jiangxi Province(S202310405010)provided funding for this study.
文摘It is quite important to ensure the safety and sustainable development of nuclear energy for the treatment of radioactive wastewater. To treat radioactive wastewater efficiently and rapidly, two multi-amine β-cyclodextrin polymers(diethylenetriamine β-cyclodextrin polymer(DETA-TFCDP) and triethylenetetramine β-cyclodextrin polymer(TETA-TFCDP)) were prepared and applied to capture uranium. Results exhibited that DETA-TFCDP and TETA-TFCDP displayed the advantages of high adsorption amounts(612.2and 628.2 mg·g-1, respectively) and rapid adsorption rates, which can reach(88 ± 1)% of their equilibrium adsorption amounts in 10 min. Moreover, the adsorbent processes of DETA-TFCDP and TETATFCDP on uranium(Ⅵ) followed the Langmuir model and pseudo-second-order model, stating they were mainly chemisorption and self-endothermic. Besides, TETA-TFCDP also showed excellent selectivity in the presence of seven competing cations and could be effectively reused five times via Na2CO3as the desorption reagent. Meanwhile, X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy illustrated that the enriched multi-amine groups and oxygen-containing functional groups on the surface of TETA-TFCDP were the main active sites for capturing uranium(Ⅵ). Hence, multi-amine β-cyclodextrin polymers are a highly efficient, rapid, and promising adsorbent for capturing uranium(Ⅵ)from radioactive wastewater.
基金supported by the Ministry of Higher Education Malaysia through the Fundamental Research Grant Scheme(FRGS)No.FRGS/1/2021/TK0/UMP/02/37(University Ref.RDU210135).
文摘Investigating zeolites as hydrogen storage scaffolds is imperative due to their porous nature and favorable physicochemical properties.Nevertheless,the storage capacity of the unmodified zeolites has been rather unsatisfactory(0.224%-1.082%(mass))compared to its modified counterpart.Thus,the contemporary focus on enhancing hydrogen storage capacities has led to significant attention towards the utilization of modified zeolites,with studies exploring surface modifications through physical and chemical treatments,as well as the integration of various active metals.The enhanced hydrogen storage properties of zeolites are attributed to the presence of aluminosilicates from alkaline and alkaline-earth metals,resulting in increased storage capacity through interactions with the charge density of these aluminosilicates.Therefore,there is a great demand to critically review their role such as well-defined topology,pore structure,good thermal stability,and tunable hydrophilicity in enhanced hydrogen storage.This article aimed to critically review the recent research findings based on modified zeolite performance for enhanced hydrogen storage.Some of the factors affecting the hydrogen storage capacities of zeolites that can affect the rate of reaction and the stability of the adsorbent,like pressure,structure,and morphology were studied,and examined.Then,future perspectives,recommendations,and directions for modified zeolites were discussed.
基金supported by the National Natural Science Foundation of China(51671052,51750110513,52250610222)the Fundamental Research Funds for the Central Universities(N182502042)the Liao Ning Revitilization Talents Program(XLYC1902105)。
文摘Graphene-based materials possess significant potential for the treatment of dye wastewater due to their exceptional adsorption properties toward stubborn pollutants.However,their utilization is hindered by high preparation costs,low yields,environmental pollution during synthesis,and challenges in regenerating the adsorbent.This study proposes a novel approach to address these limitations by developing nitrogen-doped three-dimensional(3D)polyvinyl alcohol(PVA)crosslinked graphene sponges(N-PGA)using a cross-linking method with ammonium carbonate.This method offers a relatively mild,environmentally friendly approach.Ammonium carbonate serves as both a reducing and modifying agent,facilitating the formation of the intrinsic structure of N-PGA and acting as a nitrogen source.Meanwhile,PVA is utilized as the cross-linking agent.The results demonstrate that N-PGA exhibits a favorable internal 3D hierarchical porous structure and possesses robust mechanical properties.The measured specific surface area(BET)of N-PGA was as high as406.538 m^(2)·g^(-1),which was favorable for its efficient adsorption of Congo red(CR)dye molecules.At an initial concentration of 50 mg·L^(-1),N-PGA achieved an impressive removal rate of 89.6%and an adsorption capacity of 112 mg·g^(-1)for CR dye.Furthermore,it retained 79%of its initial adsorption capacity after 10 cycles,demonstrating excellent regeneration performance.In summary,the synthesized N-PGA displays remarkable efficacy in the adsorption of CR dye in wastewater,opening up new possibilities for utilizing 3D porous graphene nanomaterials as efficient adsorbents in wastewater treatment.
基金Supported by the Major Program of the Ministry of Education of the People’s Republic of China。
文摘Phosphate was removed from aqueous environment by corundum-hollow-spheres supported caclined hydrotalcite (cHT) thin films. Mg-Al-CO3 hydrotalcite (HT) thin films were deposited on corundumhollow-sphere substrates by hydrothermal homogeneous precipitation at 120℃for 30-240 min and cHT thin films were obtained by annealing of the HT thin films at 500℃for 180 min. Their crystal phase, morphology and microstructure were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM).The results show that homogeneous, well-crystallized and hierarchical flower-like thin films were deposited firmly on the surface of the corundum. The mechanism of nucleation and growth of the HT thin films was fitted well with the anion coordination polyhedron growth unit model. To determine the absorption of phosphate by this adsorbent, different bed depth (10-30 cm) and flow rate (1.0-3.0 m L/min) were examined by column experiments. The highest removal efficiency of phosphate amounted to 98.5%under optimum condition (pH=7.2). The adsorption capacity increased as the bed depth increased and decreased as the flow rate increased.
基金the support of the National Natural Science Foundation of China(Grant No.51472074).
文摘Understanding the adsorption interactions between carbon materials and sulfur compounds has far-reaching impacts,in addition to their well-known important role in energy storage and conversion,such as lithium-ion batteries.In this paper,properties of intrinsic B or Si single-atom doped,and B-Si codoped graphene(GR)and graphdiyne(GDY)were investigated by using density functional theory-based calculations,in which the optimal doping configurations were explored for potential applications in adsorbing sulfur compounds.Results showed that both B or Si single-atom doping and B-Si codoping could substantially enhance the electron transport properties of GR and GDY,improving their surface activity.Notably,B and Si atoms displayed synergistic effects for the codoped configurations,where B-Si codoped GR/GDY exhibited much better performance in the adsorption of sulfurcontaining chemicals than single-atom doped systems.In addition,results demonstrated that,after B-Si codoping,the adsorption energy and charge transfer amounts of GDY with sulfur compounds were much larger than those of GR,indicating that B-Si codoped GDY might be a favorable material for more effectively interacting with sulfur reagents.
基金funded by the National Natural Science Foundation of China (NSFC) (Nos. 22221001, 22201115, 21931001, and 21922105)the Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province (2019ZX–04)+3 种基金the 111 Project (B20027)by the Fundamental Research Funds for the Central Universities (lzujbky-2023-eyt03)support Natural Science Foundation of Gansu Providence (22JR5RA540)Gansu Province Youth Science and Technology Talent Promotion Project (GXH202220530-02)。
文摘Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performance for hydrogen evolution reaction(HER). With the VS concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS_(2)-VS 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential(68 m V) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy(ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S-H* peak of the Ni S_(2)-VS 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the Ni S_(2)-VS 5.9% has the optimal |ΔG^(H*)| of 0.17 e V. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy.
基金financial support from the National Natural Science Foundation of China(22178154,22008094,21908082,21878133)Natural Science Foundation of Jiangsu Province(BK20190852,BK20190854)Natural Science Foundation for Jiangsu Colleges and Universities(19KJB530005).
文摘A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structure and the defective sites of h-BNNS not only are beneficial to the stabilization of Pt NPs but also favor the adsorption of aromatic sulfides.By employing Pt/h-BNNS with a Pt loading amount of 1.19 wt%as the active adsorbent and air as an oxidant,a 98.0%sulfur removal over dibenzothiophene(DBT)is achieved along with a total conversion of the DBT to the corresponding sulfones(DBTO_(2)).Detailed experiments show that the excellent desulfurization activity originates from the few-layered structure of h-BNNS and the high catalytic activity of Pt NPs.In addition,the OPADS system with Pt/h-BNNS as the active adsorbent shows remarkable stability in desulfurization performance with the existence of different interferents such as olefin,and aromatic hydrocarbons.Besides,the Pt/h-BNNS can be recycled 12 times without a significant decrease in desulfurization performance.Also,a process flow diagram is proposed for deep desulfurization of fuel oil and recovery of high value-added products,which would promote the industrial application of such OPADS strategy.
基金supported by the Zhejiang Provincial Natural Science Foundation of China(Grant No.LQ19E030017)the Research Start-up Fund(Grant No.KYS205619042)the Technological Research Project for Public Welfare of Zhejiang Province(Grant No.LGG19E030005).
文摘Lignocellulose has the potential to become a bio-based adsorbent due to its biodegradability and renewability.In this study,a novel polydopamine functionalized-lignin(lignin@PDA),prepared via self-polymerization of dopamine(PDA)on lignin,was used as a bio-based adsorbent for rapid scavenging of hexavalent chromium(Cr(VI)).The morphology,functional groups,crystalline structure,and chemical composition of lignin@PDA were characterized with a scanning electron microscope-energy dispersive spectrometer,Fourier transform infrared spectroscopy,X-ray diffraction,and X-ray photoelectron spectroscopy.The Cr(VI)adsorption process of lignin@PDA was studied using batch experiments as a function of pH,ionic strength,adsorbent dose,and contact time at room temperature.The adsorption rate of lignin@PDA was five times greater than that of the unmodified lignin,with a maximum adsorption capacity of 102.6 mg/g in an acidic medium.The adsorption of Cr(VI)on lignin@PDA fit the pseudo-secondorder equation and the Freundlich model,indicating that the adsorption process was mainly dominated by chemisorption and surface complexation.The thermodynamic parameters showed that adsorption of Cr(VI)on lignin@PDA was an endothermic and spontaneous process.The X-ray absorption fine structure results showed that sorption and reduction of Cr(VI)into Cr(II)occurred simultaneously on lignin.Moreover,PDA coating not only improved the reactivity of lignin but also promoted the complete reduction of Cr(VI)by lignin.According to these results,polydopamine functionalized-lignin is a promising bio-based adsorbent for immobilization of Cr(VI)from wastewater.