Determining the adsorption of shale gas on complex surfaces remains a challenge in molecular simulation studies.Difficulties essentially stem from the need to create a realistic shale structure model in terms of miner...Determining the adsorption of shale gas on complex surfaces remains a challenge in molecular simulation studies.Difficulties essentially stem from the need to create a realistic shale structure model in terms of mineral heterogeneityand multiplicity.Moreover,precise characterization of the competitive adsorption of hydrogen andmethane in shale generally requires the experimental determination of the related adsorptive capacity.In thisstudy,the adsorption of adsorbates,methane(CH_(4)),and hydrogen(H_(2))on heterogeneous shale surface modelsof Kaolinite,Orthoclase,Muscovite,Mica,C_(60),and Butane has been simulated in the frame of a moleculardynamic’s numerical technique.The results show that these behaviors are influenced by pressure and potentialenergy.On increasing the pressure from 500 to 2000 psi,the sorption effect for CH_(4)significantly increasesbut shows a decline at a certain stage(if compared to H_(2)).The research findings also indicate that raw shalehas a higher capacity to adsorb CH_(4)compared to hydrogen.However,in shale,this difference is negligible.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 accessibility of tetracycline resistance gene (tetG) into the pores of activated carbon (AC), as well as the impact of the pore size distribution (PSD) of AC on the uptake capacity of tetG, were investigated using...The accessibility of tetracycline resistance gene (tetG) into the pores of activated carbon (AC), as well as the impact of the pore size distribution (PSD) of AC on the uptake capacity of tetG, were investigated using eight types of AC (four coal-based and four wood-based). AC showed the capability to admit tetG and the average reduction of tetG for coal-based and wood-based ACs at the AC dose of 1 g·L<sup>-1</sup> was 3.12 log and 3.65 log, respectively. The uptake kinetic analysis showed that the uptake of the gene followed the pseudo-second-order kinetics reaction, and the uptake rate constant for the coal-based and wood-based ACs was in the range of 5.97 × 10<sup>-12</sup> - 4.64 × 10<sup>-9</sup> and 7.02 × 10<sup>-11</sup> - 1.59 × 10<sup>-8</sup> copies·mg<sup>-1</sup>·min<sup>-1</sup>, respectively. The uptake capacity analysis by fitting the obtained experiment data with the Freundlich isotherm model indicated that the uptake constant (K<sub>F</sub>) values were 1.71 × 10<sup>3</sup> - 8.00 × 10<sup>9</sup> (copies·g<sup>-1</sup>)<sup>1-1/n</sup> for coal-based ACs and 7.00 × 10<sup>8</sup> - 3.00 × 10<sup>10</sup> (copies·g<sup>-1</sup>)<sup>1-1/n</sup> for wood-based ones. In addition, the correlation analysis between K<sub>F</sub> values and pore volume as well as pore surface at different pore size regions of ACs showed that relatively higher positive correlation was found for pores of 50 - 100 Å, suggesting ACs with more pores in this size region can uptake more tetG. The findings of this study are valuable as reference for optimizing the adsorption process regarding antibiotic resistance-related concerns in drinking water treatment.展开更多
Methane adsorption is a critical assessment of the gas storage capacity(GSC)of shales with geological conditions.Although the related research of marine shales has been well-illustrated,the methane adsorption of marin...Methane adsorption is a critical assessment of the gas storage capacity(GSC)of shales with geological conditions.Although the related research of marine shales has been well-illustrated,the methane adsorption of marine-continental transitional(MCT)shales is still ambiguous.In this study,a method of combining experimental data with analytical models was used to investigate the methane adsorption characteristics and GSC of MCT shales collected from the Qinshui Basin,China.The Ono-Kondo model was used to fit the adsorption data to obtain the adsorption parameters.Subsequently,the geological model of GSC based on pore evolution was constructed using a representative shale sample with a total organic carbon(TOC)content of 1.71%,and the effects of reservoir pressure coefficient and water saturation on GSC were explored.In experimental results,compared to the composition of the MCT shale,the pore structure dominates the methane adsorption,and meanwhile,the maturity mainly governs the pore structure.Besides,maturity in the middle-eastern region of the Qinshui Basin shows a strong positive correlation with burial depth.The two parameters,micropore pore volume and non-micropore surface area,induce a good fit for the adsorption capacity data of the shale.In simulation results,the depth,pressure coefficient,and water saturation of the shale all affect the GSC.It demonstrates a promising shale gas potential of the MCT shale in a deeper block,especially with low water saturation.Specifically,the economic feasibility of shale gas could be a major consideration for the shale with a depth of<800 m and/or water saturation>60%in the Yushe-Wuxiang area.This study provides a valuable reference for the reservoir evaluation and favorable block search of MCT shale gas.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
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 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
Cyanobacteria-based activated carbon(CBAC)was successfully prepared by pyrolysis-activation of Taihu cyanobacteria.When the impregnation ratio and activated temperature were 2 and 800-C,respectively,the optimal CBACs ...Cyanobacteria-based activated carbon(CBAC)was successfully prepared by pyrolysis-activation of Taihu cyanobacteria.When the impregnation ratio and activated temperature were 2 and 800-C,respectively,the optimal CBACs possessed an ultra-high specific surface(2178.90 m^(2)·g^(-1))and plenty of micro-and meso-pores,as well as a high pore volume(1.01 cm^(3)·g^(-1)).Ascribed to ultra-high surface area,π-π interaction,electrostatic interaction,as well as hydrogen-bonding interactions,the CBACs displayed huge superiority in efficient dye removal.The saturated methylene blue adsorption capacity by CBACs could be as high as 1143.4 mg·g^(-1),superior to that of other reported biomass-activated carbons.The adsorption was endothermic and modeled well by the pseudo-second-order kinetic,intra-particle diffusion,and Langmuir models.This work presented the effectiveness of Taihu cyanobacteria adsorbent ascribed to its super large specific surface area and high adsorption ability.展开更多
A major challenge is to construct ceramic membranes with tunable structures and functions for water treatment.Herein,a novel corrosion-resistant polymer-derived silicon oxycarbide(SiOC)ceramic membrane with designed a...A major challenge is to construct ceramic membranes with tunable structures and functions for water treatment.Herein,a novel corrosion-resistant polymer-derived silicon oxycarbide(SiOC)ceramic membrane with designed architectures was fabricated by a phase separation method and was applied in organic removal via adsorption and oxidation for the first time.The pore structure of the as-prepared SiOC ceramic membranes was well controlled by changing the sintering temperature and polydimethylsiloxane content,leading to a pore size of 0.84–1.62μm and porosity of 25.0–43.8%.Corrosion resistance test results showed that the SiOC membranes sustained minimal damage during 24 h exposure to high-intensity acid–base conditions,which could be attributed to the chemical inertness of SiOC.With rhodamine 6G(R6G)as the model pollutant,the SiOC membrane demonstrated an initial eff ective removal rate of 99%via adsorption;however,the removal rate decreased as the system approached adsorption saturation.When peroxymonosulfate was added into the system,efficient and continuous degradation of R6G was observed throughout the entire period,indicating the potential of the as-prepared SiOC membrane in oxidation-related processes.Thus,this work provides new insights into the construction of novel polymer-derived ceramic membranes with well-defined structures and functions.展开更多
In this study,the ZIF-8 membrane(ZIF-8/PP-g-MAH)is prepared by in situ synthesis of ZIF-8 on irradiation-pretreated polymer substrates to improve the uranium adsorption performance and address the recycling problems o...In this study,the ZIF-8 membrane(ZIF-8/PP-g-MAH)is prepared by in situ synthesis of ZIF-8 on irradiation-pretreated polymer substrates to improve the uranium adsorption performance and address the recycling problems of ZIF-8 powder.The effects of pH,contact time,and uranium concentration on the adsorption of ZIF-8/PP-g-MAH were investigated.Adsorption isotherm and kinetics analysis show that ZIF-8/PP-g-MAH has a high adsorption capacity of 478.5 mg/g,which is 1.26 times higher than that of ZIF-8,and a rapid adsorption equilibrium of 120 min,which is shortened to one-third of that required for ZIF-8(360 min).The adsorption process of ZIF-8/PP-g-MAH is consistent with that of the Langmuir isotherm and pseudo-second-order dynamic model.ZIF-8/PP-g-MAH also exhibits good selectivity for uranium in simulated seawater.The high adsorption performance of ZIF-8/PP-g-MAH is attributed to its membrane structure,which improves the utilization of coordination sites,including Zn-OH,C-N,and C=N.This study provides an efficient adsorption material for rapid uranium extraction,thus promoting the development of uranium extraction technologies.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
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
High concentrations of copper ions(Cu(Ⅱ)) in water will pose health risks to humans and the ecological environment. Therefore, this study aims to utilize ultrasonic-cured modified municipal solid waste incineration(M...High concentrations of copper ions(Cu(Ⅱ)) in water will pose health risks to humans and the ecological environment. Therefore, this study aims to utilize ultrasonic-cured modified municipal solid waste incineration(MSWI) fly ash for Cu(Ⅱ) adsorption to achieve the purpose of “treating waste by waste.” The effects of p H, adsorption time, initial concentration, and temperature on the modified MSWI fly ash’s adsorption efficiency were systematically studied in this article. The adsorption performance of the modified MSWI fly ash can be enhanced by the ultrasonic modification. At pH = 2, 3 and 4, the adsorption capacity of the modified MSWI fly ash for Cu(Ⅱ) increased by 2.7, 1.9 and 1.2 times, respectively. Furthermore, it was suggested that the adsorption process of the modified MSWI fly ash can be better simulated by the pseudo-second-order kinetic model, with a maximum adsorption capacity calculated by the Langmuir model of 24.196 mg.g-1. Additionally, the adsorption process is spontaneous,endothermic, and chemisorption-dominated from the thermodynamic studies(ΔH and ΔS > 0, ΔG < 0).Finally, the enhanced adsorption performance of the modified MSWI fly ash for Cu(Ⅱ) may be attributed to electrostatic interaction and chelation effects.展开更多
Balancing electron transfer and intermediate adsorption ability of bifunctional catalysts via tailoring electronic structures is crucial for green hydrogen production,while it still remains challenging due to lacking ...Balancing electron transfer and intermediate adsorption ability of bifunctional catalysts via tailoring electronic structures is crucial for green hydrogen production,while it still remains challenging due to lacking efficient strategies.Herein,one efficient and universal strategy is developed to greatly regulate electronic structures of the metallic Ni-Fe-P catalysts via in-situ introducing the rare earth(RE)atoms(Ni-Fe-RE-P,RE=La,Ce,Pr,and Nd).Accordingly,the as-prepared optimal Ni-Fe-Ce-P/CC self-supported bifunctional electrodes exhibited superior electrocatalytic activity and excellent stability with the low overpotentials of 247 and 331 mV at 100 mA cm^(-2) for HER and OER,respectively.In the assembled electrolyzer,the Ni-Fe-Ce-P/CC as bifunctional electrodes displayed low operation potential of 1.49 V to achieve a current density of 10 mA cm^(-2),and the catalytic performance can be maintained for 100 h.Experimental results combined with density functional theory(DFT)calculation reveal that Ce doping leads to electron decentralization and crystal structure distortion,which can tailor the band structures and d-band center of Ni-Fe-P,further increasing conductivity and optimizing intermediate adsorption energy.Our work not only proposes a valuable strategy to regulate the electron transfer and intermediate adsorption of electrocatalysts via RE atoms doping,but also provides a deep under-standing of regulation mechanism of metallic electrocatalysts for enhanced water splitting.展开更多
As drilling wells continue to move into deep ultra-deep layers,the requirements for temperature resistance of drilling fluid treatments are getting higher and higher.Among them,blocking agent,as one of the key treatme...As drilling wells continue to move into deep ultra-deep layers,the requirements for temperature resistance of drilling fluid treatments are getting higher and higher.Among them,blocking agent,as one of the key treatment agents,has also become a hot spot of research.In this study,a high temperature resistant strong adsorption rigid blocking agent(QW-1)was prepared using KH570 modified silica,acrylamide(AM)and allyltrimethylammonium chloride(TMAAC).QW-1 has good thermal stability,average particle size of 1.46μm,water contact angle of 10.5.,has a strong hydrophilicity,can be well dispersed in water.The experimental results showed that when 2 wt%QW-1 was added to recipe A(4 wt%bentonite slurry+0.5 wt%DSP-1(filtration loss depressant)),the API filtration loss decreased from 7.8to 6.4 m L.After aging at 240.C,the API loss of filtration was reduced from 21 to 14 m L,which has certain performance of high temperature loss of filtration.At the same time,it is effective in sealing 80-100mesh and 100-120 mesh sand beds as well as 3 and 5μm ceramic sand discs.Under the same conditions,the blocking performance was superior to silica(5μm)and calcium carbonate(2.6μm).In addition,the mechanism of action of QW-1 was further investigated.The results show that QW-1 with amide and quaternary ammonium groups on the molecular chain can be adsorbed onto the surface of clay particles through hydrogen bonding and electrostatic interaction to form a dense blocking layer,thus preventing further intrusion of drilling fluid into the formation.展开更多
The interest in curtailing environmental pollution issues through physical separation processes has inspired an extensive search for novel nanoporous materials with exceptional adsorption capabilities.Covalent triazin...The interest in curtailing environmental pollution issues through physical separation processes has inspired an extensive search for novel nanoporous materials with exceptional adsorption capabilities.Covalent triazine frameworks(CTFs),emerged as a class of crystalline covalent organic frameworks(COFs),have been widely examined for various separation applications,owing to their large porosity,high stability,and rich nitrogen(N)doping.The development of CTFs for efficient adsorption of mercury(Ⅱ)(Hg^(2+))is of great importance for the field,whereas it is rarely attempted,on account of limited synthetic strategies and unknown structural-property relations of conventional CTFs derived from ionothermal approaches.Herein,we report rational synthesis of a crystalline CTF with methylthio pendant arms for efficient removal of Hg^(2+)with an exceptional capacity of 751 mg·g^(-1),ranking at the top among previously-reported adsorbents.This work may open up new possibility in the synthesis of COFs for various separations.展开更多
A well-known hazardous metal and top contaminant in wastewater is hexavalent chromium. The two forms of most commonly found chromium are chromate ( CrO 4 2− ) and dichromate ( Cr 2 O 7 2− ). Leather tanning, cooling t...A well-known hazardous metal and top contaminant in wastewater is hexavalent chromium. The two forms of most commonly found chromium are chromate ( CrO 4 2− ) and dichromate ( Cr 2 O 7 2− ). Leather tanning, cooling tower blow-down, plating, electroplating, rinse water sources, anodizing baths etc. are the main sources of Cr (VI) contamination. The Cr (VI) is not only non-biodegradable in the environment but also carcinogenic to living population. It is still difficult to treat Cr contaminated waste water effectively, safely, eco-friendly, and economically. As a result, many techniques have been used to treat Cr (VI)-polluted wastewater, including adsorption, chemical precipitation, coagulation, ion-exchange, and filtration. Among these practices, the most practical method is adsorption for the removal of Cr (VI) from aqueous solutions, which has gained widespread acceptance due to the ease of use and affordability of the equipment and adsorbent. It has been revealed that Fe-based adsorbents’ oxides and hydroxides have high adsorptive potential to lower Cr (VI) content below the advised threshold. Fe-based adsorbents were also discovered to be relatively cheap and toxic-free in Cr (VI) treatment. Fe-based adsorbents are commonly utilized in industry. It has been discovered that nanoparticles of Fe-, Ti-, and Cu-based adsorbents have a better capacity to remove Cr (VI). Cr (VI) was effectively removed from contaminated water using mixed element-based adsorbents (Fe-Mn, Fe-Ti, Fe-Cu, Fe-Zr, Fe-Cu-Y, Fe-Mg, etc.). Initial findings suggest that Cr (VI) removal from wastewater may be accomplished by using magnesium ferrite nanomaterials as an efficient adsorbent.展开更多
Ni^(2+)and Cd^(2+)in wastewater accumulated through the ecological chain and could jeopardize human health.Adsorption of Ni^(2+)and Cd^(2+)from wastewater using recovered perlite was an important way to solve the prob...Ni^(2+)and Cd^(2+)in wastewater accumulated through the ecological chain and could jeopardize human health.Adsorption of Ni^(2+)and Cd^(2+)from wastewater using recovered perlite was an important way to solve the problem of resource utilization of solid waste from agar production.Our previous study confirmed that recovered perlite from agar extraction residue had better pore size and specific surface area than commercial perlite.However,the adsorption efficiency and adsorption mechanism of recovered perlite were the main factors limiting its adsorption application.The adsorption process of Ni^(2+)and Cd^(2+)by recovered perlite in aqueous solution was described by the pseudo-second-order kinetic equation,and the relevant adsorption mechanism was mainly chemisorption.Compared with commercial perlite,the adsorption removal rate of Ni^(2+)and Cd^(2+)by enzymatic recovered perlite could reach 92.9%and 89.2%,respectively,and were improved by 12.63%and 13.03%.Langmuir isothermal adsorption model could better describe the isothermal adsorption process of recovered perlite on heavy metal Ni^(2+)and Cd^(2+),and the relevant adsorption mechanism was mainly monolayer adsorption.The X-ray photoelectron spectroscopy(XPS)results indicated that the decrease of Si—O Si^(2+)hydroxyl coordination bond and the increase of C—Si bond might make the binding effect of recovered perlite with heavy metals stronger.The competitive adsorption of Ni^(2+)and Cd^(2+)by recovered perlite was still dominated by chemisorption and monolayer adsorption.This study was expected to provide a theoretical basis and technical support for the removal of Ni^(2+)and Cd^(2+)from wastewater using recovered perlite from seaweed residue.展开更多
基金PETRONAS Research fund(PRF)under PETRONAS Teknologi Transfer(PTT)Pre-Commercialization—External:YUTP-PRG Cycle 2022(015PBC-020).
文摘Determining the adsorption of shale gas on complex surfaces remains a challenge in molecular simulation studies.Difficulties essentially stem from the need to create a realistic shale structure model in terms of mineral heterogeneityand multiplicity.Moreover,precise characterization of the competitive adsorption of hydrogen andmethane in shale generally requires the experimental determination of the related adsorptive capacity.In thisstudy,the adsorption of adsorbates,methane(CH_(4)),and hydrogen(H_(2))on heterogeneous shale surface modelsof Kaolinite,Orthoclase,Muscovite,Mica,C_(60),and Butane has been simulated in the frame of a moleculardynamic’s numerical technique.The results show that these behaviors are influenced by pressure and potentialenergy.On increasing the pressure from 500 to 2000 psi,the sorption effect for CH_(4)significantly increasesbut shows a decline at a certain stage(if compared to H_(2)).The research findings also indicate that raw shalehas a higher capacity to adsorb CH_(4)compared to hydrogen.However,in shale,this difference is negligible.
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.
文摘The accessibility of tetracycline resistance gene (tetG) into the pores of activated carbon (AC), as well as the impact of the pore size distribution (PSD) of AC on the uptake capacity of tetG, were investigated using eight types of AC (four coal-based and four wood-based). AC showed the capability to admit tetG and the average reduction of tetG for coal-based and wood-based ACs at the AC dose of 1 g·L<sup>-1</sup> was 3.12 log and 3.65 log, respectively. The uptake kinetic analysis showed that the uptake of the gene followed the pseudo-second-order kinetics reaction, and the uptake rate constant for the coal-based and wood-based ACs was in the range of 5.97 × 10<sup>-12</sup> - 4.64 × 10<sup>-9</sup> and 7.02 × 10<sup>-11</sup> - 1.59 × 10<sup>-8</sup> copies·mg<sup>-1</sup>·min<sup>-1</sup>, respectively. The uptake capacity analysis by fitting the obtained experiment data with the Freundlich isotherm model indicated that the uptake constant (K<sub>F</sub>) values were 1.71 × 10<sup>3</sup> - 8.00 × 10<sup>9</sup> (copies·g<sup>-1</sup>)<sup>1-1/n</sup> for coal-based ACs and 7.00 × 10<sup>8</sup> - 3.00 × 10<sup>10</sup> (copies·g<sup>-1</sup>)<sup>1-1/n</sup> for wood-based ones. In addition, the correlation analysis between K<sub>F</sub> values and pore volume as well as pore surface at different pore size regions of ACs showed that relatively higher positive correlation was found for pores of 50 - 100 Å, suggesting ACs with more pores in this size region can uptake more tetG. The findings of this study are valuable as reference for optimizing the adsorption process regarding antibiotic resistance-related concerns in drinking water treatment.
基金jointly supported by the Science and Technology Department of Shanxi Province,China (20201101003)the National Natural Science Foundation of China (U1810201)the China Scholarship Council (202206400012)。
文摘Methane adsorption is a critical assessment of the gas storage capacity(GSC)of shales with geological conditions.Although the related research of marine shales has been well-illustrated,the methane adsorption of marine-continental transitional(MCT)shales is still ambiguous.In this study,a method of combining experimental data with analytical models was used to investigate the methane adsorption characteristics and GSC of MCT shales collected from the Qinshui Basin,China.The Ono-Kondo model was used to fit the adsorption data to obtain the adsorption parameters.Subsequently,the geological model of GSC based on pore evolution was constructed using a representative shale sample with a total organic carbon(TOC)content of 1.71%,and the effects of reservoir pressure coefficient and water saturation on GSC were explored.In experimental results,compared to the composition of the MCT shale,the pore structure dominates the methane adsorption,and meanwhile,the maturity mainly governs the pore structure.Besides,maturity in the middle-eastern region of the Qinshui Basin shows a strong positive correlation with burial depth.The two parameters,micropore pore volume and non-micropore surface area,induce a good fit for the adsorption capacity data of the shale.In simulation results,the depth,pressure coefficient,and water saturation of the shale all affect the GSC.It demonstrates a promising shale gas potential of the MCT shale in a deeper block,especially with low water saturation.Specifically,the economic feasibility of shale gas could be a major consideration for the shale with a depth of<800 m and/or water saturation>60%in the Yushe-Wuxiang area.This study provides a valuable reference for the reservoir evaluation and favorable block search of MCT shale gas.
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.
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 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financially supported by the Key Research&Development program of Zhejiang Province(2021C03196)the National Key Research and Development Program of China(2022YFE0128600)the Natural Science Foundation of Zhejiang Province(LY22B060011).
文摘Cyanobacteria-based activated carbon(CBAC)was successfully prepared by pyrolysis-activation of Taihu cyanobacteria.When the impregnation ratio and activated temperature were 2 and 800-C,respectively,the optimal CBACs possessed an ultra-high specific surface(2178.90 m^(2)·g^(-1))and plenty of micro-and meso-pores,as well as a high pore volume(1.01 cm^(3)·g^(-1)).Ascribed to ultra-high surface area,π-π interaction,electrostatic interaction,as well as hydrogen-bonding interactions,the CBACs displayed huge superiority in efficient dye removal.The saturated methylene blue adsorption capacity by CBACs could be as high as 1143.4 mg·g^(-1),superior to that of other reported biomass-activated carbons.The adsorption was endothermic and modeled well by the pseudo-second-order kinetic,intra-particle diffusion,and Langmuir models.This work presented the effectiveness of Taihu cyanobacteria adsorbent ascribed to its super large specific surface area and high adsorption ability.
基金supported by the National Key R&D Program of China(Grant No.2021YFB3200500)Natural Science Foundation of China(Grant No.52370014)+2 种基金Ningbo 3315 plan(Grant No.2018A-03-A)Natural Science Foundation of Tianjin City(Grant No.63241631)the financial support of Joint Lab for Advanced Organosilicon Precursors with Zhejiang Xinshichen New Materials Ltd.Co.
文摘A major challenge is to construct ceramic membranes with tunable structures and functions for water treatment.Herein,a novel corrosion-resistant polymer-derived silicon oxycarbide(SiOC)ceramic membrane with designed architectures was fabricated by a phase separation method and was applied in organic removal via adsorption and oxidation for the first time.The pore structure of the as-prepared SiOC ceramic membranes was well controlled by changing the sintering temperature and polydimethylsiloxane content,leading to a pore size of 0.84–1.62μm and porosity of 25.0–43.8%.Corrosion resistance test results showed that the SiOC membranes sustained minimal damage during 24 h exposure to high-intensity acid–base conditions,which could be attributed to the chemical inertness of SiOC.With rhodamine 6G(R6G)as the model pollutant,the SiOC membrane demonstrated an initial eff ective removal rate of 99%via adsorption;however,the removal rate decreased as the system approached adsorption saturation.When peroxymonosulfate was added into the system,efficient and continuous degradation of R6G was observed throughout the entire period,indicating the potential of the as-prepared SiOC membrane in oxidation-related processes.Thus,this work provides new insights into the construction of novel polymer-derived ceramic membranes with well-defined structures and functions.
文摘In this study,the ZIF-8 membrane(ZIF-8/PP-g-MAH)is prepared by in situ synthesis of ZIF-8 on irradiation-pretreated polymer substrates to improve the uranium adsorption performance and address the recycling problems of ZIF-8 powder.The effects of pH,contact time,and uranium concentration on the adsorption of ZIF-8/PP-g-MAH were investigated.Adsorption isotherm and kinetics analysis show that ZIF-8/PP-g-MAH has a high adsorption capacity of 478.5 mg/g,which is 1.26 times higher than that of ZIF-8,and a rapid adsorption equilibrium of 120 min,which is shortened to one-third of that required for ZIF-8(360 min).The adsorption process of ZIF-8/PP-g-MAH is consistent with that of the Langmuir isotherm and pseudo-second-order dynamic model.ZIF-8/PP-g-MAH also exhibits good selectivity for uranium in simulated seawater.The high adsorption performance of ZIF-8/PP-g-MAH is attributed to its membrane structure,which improves the utilization of coordination sites,including Zn-OH,C-N,and C=N.This study provides an efficient adsorption material for rapid uranium extraction,thus promoting the development of uranium extraction technologies.
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supported by the key program of the National Natural Science Foundation of China(52236008).
文摘High concentrations of copper ions(Cu(Ⅱ)) in water will pose health risks to humans and the ecological environment. Therefore, this study aims to utilize ultrasonic-cured modified municipal solid waste incineration(MSWI) fly ash for Cu(Ⅱ) adsorption to achieve the purpose of “treating waste by waste.” The effects of p H, adsorption time, initial concentration, and temperature on the modified MSWI fly ash’s adsorption efficiency were systematically studied in this article. The adsorption performance of the modified MSWI fly ash can be enhanced by the ultrasonic modification. At pH = 2, 3 and 4, the adsorption capacity of the modified MSWI fly ash for Cu(Ⅱ) increased by 2.7, 1.9 and 1.2 times, respectively. Furthermore, it was suggested that the adsorption process of the modified MSWI fly ash can be better simulated by the pseudo-second-order kinetic model, with a maximum adsorption capacity calculated by the Langmuir model of 24.196 mg.g-1. Additionally, the adsorption process is spontaneous,endothermic, and chemisorption-dominated from the thermodynamic studies(ΔH and ΔS > 0, ΔG < 0).Finally, the enhanced adsorption performance of the modified MSWI fly ash for Cu(Ⅱ) may be attributed to electrostatic interaction and chelation effects.
基金support from the National Key Technology R&D Program of China(2021YFB3500801,2022YFC3901503,2022YFB3504302)the Natural Science Foundation and Overseas Talent Projects of Jiangxi Province(20232BAB214025,20232BCJ25044).
文摘Balancing electron transfer and intermediate adsorption ability of bifunctional catalysts via tailoring electronic structures is crucial for green hydrogen production,while it still remains challenging due to lacking efficient strategies.Herein,one efficient and universal strategy is developed to greatly regulate electronic structures of the metallic Ni-Fe-P catalysts via in-situ introducing the rare earth(RE)atoms(Ni-Fe-RE-P,RE=La,Ce,Pr,and Nd).Accordingly,the as-prepared optimal Ni-Fe-Ce-P/CC self-supported bifunctional electrodes exhibited superior electrocatalytic activity and excellent stability with the low overpotentials of 247 and 331 mV at 100 mA cm^(-2) for HER and OER,respectively.In the assembled electrolyzer,the Ni-Fe-Ce-P/CC as bifunctional electrodes displayed low operation potential of 1.49 V to achieve a current density of 10 mA cm^(-2),and the catalytic performance can be maintained for 100 h.Experimental results combined with density functional theory(DFT)calculation reveal that Ce doping leads to electron decentralization and crystal structure distortion,which can tailor the band structures and d-band center of Ni-Fe-P,further increasing conductivity and optimizing intermediate adsorption energy.Our work not only proposes a valuable strategy to regulate the electron transfer and intermediate adsorption of electrocatalysts via RE atoms doping,but also provides a deep under-standing of regulation mechanism of metallic electrocatalysts for enhanced water splitting.
基金supported by the National Natural Science Foundation of China (No.52074330,No.52288101)。
文摘As drilling wells continue to move into deep ultra-deep layers,the requirements for temperature resistance of drilling fluid treatments are getting higher and higher.Among them,blocking agent,as one of the key treatment agents,has also become a hot spot of research.In this study,a high temperature resistant strong adsorption rigid blocking agent(QW-1)was prepared using KH570 modified silica,acrylamide(AM)and allyltrimethylammonium chloride(TMAAC).QW-1 has good thermal stability,average particle size of 1.46μm,water contact angle of 10.5.,has a strong hydrophilicity,can be well dispersed in water.The experimental results showed that when 2 wt%QW-1 was added to recipe A(4 wt%bentonite slurry+0.5 wt%DSP-1(filtration loss depressant)),the API filtration loss decreased from 7.8to 6.4 m L.After aging at 240.C,the API loss of filtration was reduced from 21 to 14 m L,which has certain performance of high temperature loss of filtration.At the same time,it is effective in sealing 80-100mesh and 100-120 mesh sand beds as well as 3 and 5μm ceramic sand discs.Under the same conditions,the blocking performance was superior to silica(5μm)and calcium carbonate(2.6μm).In addition,the mechanism of action of QW-1 was further investigated.The results show that QW-1 with amide and quaternary ammonium groups on the molecular chain can be adsorbed onto the surface of clay particles through hydrogen bonding and electrostatic interaction to form a dense blocking layer,thus preventing further intrusion of drilling fluid into the formation.
基金The National Natural Science Foundation of China(22078349,22005319,52170109)Self-deployment Program from Lanzhou Institute of Chemical Physics(E30159SQ).
文摘The interest in curtailing environmental pollution issues through physical separation processes has inspired an extensive search for novel nanoporous materials with exceptional adsorption capabilities.Covalent triazine frameworks(CTFs),emerged as a class of crystalline covalent organic frameworks(COFs),have been widely examined for various separation applications,owing to their large porosity,high stability,and rich nitrogen(N)doping.The development of CTFs for efficient adsorption of mercury(Ⅱ)(Hg^(2+))is of great importance for the field,whereas it is rarely attempted,on account of limited synthetic strategies and unknown structural-property relations of conventional CTFs derived from ionothermal approaches.Herein,we report rational synthesis of a crystalline CTF with methylthio pendant arms for efficient removal of Hg^(2+)with an exceptional capacity of 751 mg·g^(-1),ranking at the top among previously-reported adsorbents.This work may open up new possibility in the synthesis of COFs for various separations.
文摘A well-known hazardous metal and top contaminant in wastewater is hexavalent chromium. The two forms of most commonly found chromium are chromate ( CrO 4 2− ) and dichromate ( Cr 2 O 7 2− ). Leather tanning, cooling tower blow-down, plating, electroplating, rinse water sources, anodizing baths etc. are the main sources of Cr (VI) contamination. The Cr (VI) is not only non-biodegradable in the environment but also carcinogenic to living population. It is still difficult to treat Cr contaminated waste water effectively, safely, eco-friendly, and economically. As a result, many techniques have been used to treat Cr (VI)-polluted wastewater, including adsorption, chemical precipitation, coagulation, ion-exchange, and filtration. Among these practices, the most practical method is adsorption for the removal of Cr (VI) from aqueous solutions, which has gained widespread acceptance due to the ease of use and affordability of the equipment and adsorbent. It has been revealed that Fe-based adsorbents’ oxides and hydroxides have high adsorptive potential to lower Cr (VI) content below the advised threshold. Fe-based adsorbents were also discovered to be relatively cheap and toxic-free in Cr (VI) treatment. Fe-based adsorbents are commonly utilized in industry. It has been discovered that nanoparticles of Fe-, Ti-, and Cu-based adsorbents have a better capacity to remove Cr (VI). Cr (VI) was effectively removed from contaminated water using mixed element-based adsorbents (Fe-Mn, Fe-Ti, Fe-Cu, Fe-Zr, Fe-Cu-Y, Fe-Mg, etc.). Initial findings suggest that Cr (VI) removal from wastewater may be accomplished by using magnesium ferrite nanomaterials as an efficient adsorbent.
基金financially supported by National Natural Science Foundation of China(22038012,32172339,and 22178142)National Key Research and Development Program(2023YF D2100603)。
文摘Ni^(2+)and Cd^(2+)in wastewater accumulated through the ecological chain and could jeopardize human health.Adsorption of Ni^(2+)and Cd^(2+)from wastewater using recovered perlite was an important way to solve the problem of resource utilization of solid waste from agar production.Our previous study confirmed that recovered perlite from agar extraction residue had better pore size and specific surface area than commercial perlite.However,the adsorption efficiency and adsorption mechanism of recovered perlite were the main factors limiting its adsorption application.The adsorption process of Ni^(2+)and Cd^(2+)by recovered perlite in aqueous solution was described by the pseudo-second-order kinetic equation,and the relevant adsorption mechanism was mainly chemisorption.Compared with commercial perlite,the adsorption removal rate of Ni^(2+)and Cd^(2+)by enzymatic recovered perlite could reach 92.9%and 89.2%,respectively,and were improved by 12.63%and 13.03%.Langmuir isothermal adsorption model could better describe the isothermal adsorption process of recovered perlite on heavy metal Ni^(2+)and Cd^(2+),and the relevant adsorption mechanism was mainly monolayer adsorption.The X-ray photoelectron spectroscopy(XPS)results indicated that the decrease of Si—O Si^(2+)hydroxyl coordination bond and the increase of C—Si bond might make the binding effect of recovered perlite with heavy metals stronger.The competitive adsorption of Ni^(2+)and Cd^(2+)by recovered perlite was still dominated by chemisorption and monolayer adsorption.This study was expected to provide a theoretical basis and technical support for the removal of Ni^(2+)and Cd^(2+)from wastewater using recovered perlite from seaweed residue.