The pore structure of coal plays a key role in controlling the storage and migration of CH4/N2.The pore structure of coal is an important indicator to measure the gas extraction capability and the gas displacement efe...The pore structure of coal plays a key role in controlling the storage and migration of CH4/N2.The pore structure of coal is an important indicator to measure the gas extraction capability and the gas displacement efect of N2 injection.The deformation characteristic of coal during adsorption–desorption of CH4/N2 is an important factor afecting CH4 pumpability and N2 injectability.The pore structure characteristics of low-permeability coal were obtained by fuid intrusion method and photoelectric radiation technology.The multistage and connectivity of coal pores were analyzed.Subsequently,a simultaneous test experiment of CH4/N2 adsorption–desorption and coal deformation was carried out.The deformation characteristics of coal were clarifed and a coal strain model was constructed.Finally,the applicability of low-permeability coal to N2 injection for CH4 displacement technology was investigated.The results show that the micropores and transition pores of coal samples are relatively developed.The pore morphology of coal is dominated by semi-open pores.The pore structure of coal is highly complex and heterogeneous.Transition pores,mesopores and macropores of coal have good connectivity,while micropores have poor connectivity.Under constant triaxial stress,the adsorption capacity of the coal for CH4 is greater than that for N2,and the deformation capacity of the coal for CH4 adsorption is greater than that for N2 adsorption.The axial strain,circumferential strain,and volumetric strain during the entire process of CH4 and N2 adsorption/desorption in the coal can be divided into three stages.Coal adsorption–desorption deformation has the characteristics of anisotropy and gas-diference.A strain model for the adsorption–desorption of CH4/N2 from coal was established by considering the expansion stress of adsorbed gas on the coal matrix,the compression stress of free gas on the coal matrix,and the expansion stress of free gas on micropore fractures.N2 has good injectability in low-permeability coal seams and has the dual functions of improving coal seam permeability and enhancing gas fow,which can signifcantly improve the efectiveness of low-permeability coal seam gas control and promote the efcient utilization of gas resources.展开更多
The durability of cement-based materials is related to water transport and storage in their pore network under different humidity conditions.To understand the mechanism and characteristics of water adsorption and deso...The durability of cement-based materials is related to water transport and storage in their pore network under different humidity conditions.To understand the mechanism and characteristics of water adsorption and desorption processes from the microscopic scale,this study introduces different points of view for the pore space model generation and numerical simulation of water transport by considering the“ink-bottle”effect.On the basis of the pore structure parameters(i.e.,pore size distribution and porosity)of cement paste and mortar with water-binder ratios of 0.3,0.4 and 0.5 obtained via mercury intrusion porosimetry,randomly formed 3D pore space models are generated using two-phase transformation on Gaussian random fields and verified via image analysis method of mathematical morphology.Considering the Kelvin-Laplace equation and the influence of“ink-bottle”pores,two numerical calculation scenarios based on mathematical morphology are proposed and applied to the generated model to simulate the adsorption-desorption process.The simulated adsorption and desorption curves are close to those of the experiment,verifying the effectiveness of the developed model and methods.The obtained results characterize water transport in cement-based materials during the variation of relative humidity and further explain the hysteresis effect due to“ink-bottle”pores from the microscopic scale.展开更多
[Objective]The research aimed to provide scientific reference for reasonable utilization of polyacrylamide(PAM).[Method]After PAM treatment,the soil aggregates were classified through dry sieve analysis and the adsorp...[Objective]The research aimed to provide scientific reference for reasonable utilization of polyacrylamide(PAM).[Method]After PAM treatment,the soil aggregates were classified through dry sieve analysis and the adsorption capacity and desorption capacity of all soil aggregates to phosphorus at different phosphorus concentrations were analyzed.[Result] The phosphorus adsorption and desorption of soil sample treated by PAM declined. The amount of phosphorus adsorption increased with the increase of phosphorus concentration and this increase was fast in low phosphorus concentration area but slow in high phosphorus concentration area.At different phosphorus concentrations,adsorption showed a へ shape changing trend.The phosphorus adsorption was related to phosphorus concentration and the 2-3 mm aggregate had the highest desorption rate while 0.1-0.25 mm aggregate and 0.45-1 mm aggregate had lowest desorption rate.[Conclusion]The PAM treatment generated significant influence on phosphorus adsorption and analytic features of aggregate in all size fractions.展开更多
[Objective] This study aimed to investigate the adsorption and desorption characteristics of cadmium and lead in typical paddy soils of Jiangxi Province. [Method] Gleyed paddy soil and waterloggogenic paddy soil were ...[Objective] This study aimed to investigate the adsorption and desorption characteristics of cadmium and lead in typical paddy soils of Jiangxi Province. [Method] Gleyed paddy soil and waterloggogenic paddy soil were collected from Jiangxi Province and used as experimental materials to investigate single and com- petitive adsorption and desorption behaviors of cadmium and lead by batch equilib- rium method. The environmental risk of the presence of cadmium and lead in paddy soils was assessed using distribution coefficients. [Result] Under equal ratio condi- tions, the adsorption capacity of lead by two types of paddy soils was higher than that of cadmium, and the adsorption rate in waterloggogenic paddy soil was higher than that in gleyed paddy soil. The desorption capacity of cadmium by two types of paddy soils was higher than that of lead, and the desorption rate in gleyed paddy soil was higher than that in waterloggogenic paddy soil. Under competitive condi- tions, the adsorption capacity of cadmium and lead by paddy soils was significantly reduced compared with single ion system, while the desorption rate was remarkably improved. The potential environmental risk of cadmium contamination was greater than that of lead in paddy soils. Moreover, environmental risks of cadmium and lead were reduced with the increase of pH, which increased significantly under the coex- istence state. [Conclusion] In the coexistence of cadmium and lead, cadmium con- tamination should be controlled and avoided compared with lead contamination in paddy soils.展开更多
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
The adsorption and desorption kinetic of natural zeolite on NH4+ was stud-ied by lab analysis. The results showed that the adsorption and desorption kinetic of natural zeolite on NH4+ coincided with the first-order ...The adsorption and desorption kinetic of natural zeolite on NH4+ was stud-ied by lab analysis. The results showed that the adsorption and desorption kinetic of natural zeolite on NH4+ coincided with the first-order kinetics, modified Freundlich equation, parabolic diffusion model, and heterogeneous diffusion model. The desorp-tion of the adsorbed NH4+ was far rapider than the adsorption, which can be fin-ished within 60 min.展开更多
Injecting carbon dioxide(CO_(2))into coal seams may unlock substantial carbon sequestration potential.Since the coal acts like a carbon filter,it can preferentially absorb significant amounts of CO_(2).To explore this...Injecting carbon dioxide(CO_(2))into coal seams may unlock substantial carbon sequestration potential.Since the coal acts like a carbon filter,it can preferentially absorb significant amounts of CO_(2).To explore this further,desorption of the adsorbed gas due to pressure drop is investigated in this paper,to achieve an improved understanding of the long-term fate of injected CO_(2) during post-injection period.This paper presents a dual porosity model coupling gas flow,adsorption and geomechanics for studying coupled processes and effectiveness of CO_(2) sequestration in coals.A new adsorption?desorption model derived based on thermodynamics is incorporated,particularly,the desorption hysteresis is considered.The reliability of the proposed adsorption-desorption isotherm is examined via validation tests.It is indicated that occurrence of desorption hysteresis is attributed to the adsorption-induced pore deformation.After injection ceases,the injected gas continues to propagate further from the injection well,while the pressure in the vicinity of the injection well experiences a significant drop.Although the adsorbed gas near the well also decreases,this decrease is less compared to that in pressure because of desorption hysteresis.The unceasing spread of CO_(2) and drops of pressure and adsorbed gas depend on the degree of desorption hysteresis and heterogeneity of coals,which should be considered when designing CO_(2) sequestration into coal seams.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
We study the desorption mechanism of hydrogen isotopes from graphene surface using first-principles calculations,with focus on the effects of quantum tunneling.At low temperatures,quantum tunneling plays a dominant ro...We study the desorption mechanism of hydrogen isotopes from graphene surface using first-principles calculations,with focus on the effects of quantum tunneling.At low temperatures,quantum tunneling plays a dominant role in the desorption process of both hydrogen monomers and dimers.In the case of dimer desorption,two types of mechanisms,namely the traditional one-step desorption in the form of molecules(molecular mechanism),and the two-step desorption in the form of individual atoms(atomic mechanism),are studied and compared.For the ortho-dimers,the dominant desorption mechanism is found to switch from the molecular mechanism to the atomic mechanism above a critical temperature,which is∼300K and 200K for H and D,respectively.展开更多
Flotation is the most common method to obtain concentrate through the selective adsorption of collectors on target minerals to make them hydrophobic and floatable.In the hydrometallurgy of concentrate,collectors adsor...Flotation is the most common method to obtain concentrate through the selective adsorption of collectors on target minerals to make them hydrophobic and floatable.In the hydrometallurgy of concentrate,collectors adsorbed on concentrate can damage ion-exchange resin and increase the chemical oxygen demand(COD)value of wastewater.In this work,we proposed a new scheme,i.e.,desorbing the collectors from concentrate in ore dressing plant and reusing them in flotation flowsheet.Lead nitrate and benzohydroxamic acid(Pb-BHA)complex is a common collector in scheelite flotation.In this study,different physical(stirring or ultrasonic waves)and chemical(strong acid or alkali environment)methods for facilitating the desorption of Pb-BHA collector from scheelite concentrate were explored.Single-mineral desorption tests showed that under the condition of pulp pH 13 and ultrasonic treatment for 15 min,the highest desorption rates of Pb and BHA from the scheelite concentrate were 90.48%and 63.75%,respectively.Run-of-mine ore flotation tests revealed that the reuse of desorbed Pb and BHA reduced the collector dosage by 30%for BHA and 25%for Pb.The strong alkali environment broke the chemical bonds between Pb and BHA.The cavitation effect of ultrasonic waves effectively reduced the interaction intensity between Pb-BHA collector and scheelite surfaces.This method combining ultrasonic waves and strong alkali environment can effectively desorb the collectors from concentrate and provide“clean”scheelite concentrate for metallurgic plants;the reuse of desorbed collector in flotation flowsheet can reduce reagent cost for ore dressing plants.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
To identify the species in liquid surface using mass spectrometry,we must eliminate or reduce interferences during the vaporization or desorption of the species from the liquid surface.It is much more challenging to i...To identify the species in liquid surface using mass spectrometry,we must eliminate or reduce interferences during the vaporization or desorption of the species from the liquid surface.It is much more challenging to isolate the ionic,larger species from the liquid surface,because of the frangible structures and the higher solvation energies of those species.Here we demonstrate a new mass spectrometry in which the ionic species at the liquid surface can be desorbed with ultrasoft infrared picosecond laser pulses while the liquid surface is not breached.This laser desorption assisted mass spectrometry is not only a powerful tool to detect the fragile species but also promising to investigate vibrational energy transfer dynamics in the liquid surface.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
Low salinity water containing sulfate ions can significantly alter the surface wettability of carbonate rocks.Nevertheless,the impact of sulfate concentration on the desorption of oil film on the surface of carbonate ...Low salinity water containing sulfate ions can significantly alter the surface wettability of carbonate rocks.Nevertheless,the impact of sulfate concentration on the desorption of oil film on the surface of carbonate rock is still unknown.This study examines the variations in the wettability of the surface of carbonate rocks in solutions containing varying amounts of sodium sulfate and pure water.The problem is addressed in the framework of molecular dynamics simulation(Material Studio software)and experiments.The experiment’s findings demonstrate that sodium sulfate can increase the rate at which oil moisture is turned into water moisture.The final contact angle is smaller than that of pure water.The results of the simulations show that many water molecules travel down the water channel under the influence of several powerful forces,including the electrostatic force,the van der Waals force and hydrogen bond,crowding out the oil molecules on the calcite’s surface and causing the oil film to separate.The relative concentration curve of water and oil molecules indicates that the separation rate of the oil film on the surface of calcite increases with the number of sulfate ions.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
Confronting the severe health threats and environmental impacts of Cr(Ⅵ)in aquatic environments demands innovative and effective remediation approaches.In this study,Graphene oxide(GO)-decorated poly(dimethyl amino e...Confronting the severe health threats and environmental impacts of Cr(Ⅵ)in aquatic environments demands innovative and effective remediation approaches.In this study,Graphene oxide(GO)-decorated poly(dimethyl amino ethyl methacrylate)(PDMAEMA)brush nanocomposites(GOP1,GOP2,GOP3,and GOP4)were fabricated using atom transfer radical polymerization(ATRP)by the“graft from”method.The resulting nanocomposites were utilized for removing Cr(Ⅵ)with good adsorption performance due to the electrostatic interaction of protonated nitrogen groups in the brush chains with negatively charged particles in the solution.The kinetic model of pseudo-second-order best represented the contaminants'adsorption characteristics.The WebereMorris model further indicated that surface adsorption and intraparticle diffusion mechanisms primarily controlled the adsorption procedure.Additionally,the Langmuir and Temkin isotherm models were found to most accurately represent the adsorption characteristics of the pollutants on the nanocomposites,and GOP4 can achieve the maximum adsorption capacity of 164.4 mg·g^(-1).The adsorbents'capacity maintains above 85%after five cycles of adsorptiondesorption.The nanocomposites in this study demonstrate promising potential for eliminating Cr(VI)from aqueous solutions.展开更多
基金supported by the Natural Science Foundation of China(51874236 and 52174207)Shaanxi Provincial Department of Science and Technology(2020JC-48 and 2022TD-02)China Postdoctoral Science Foundation(2021M693879).
文摘The pore structure of coal plays a key role in controlling the storage and migration of CH4/N2.The pore structure of coal is an important indicator to measure the gas extraction capability and the gas displacement efect of N2 injection.The deformation characteristic of coal during adsorption–desorption of CH4/N2 is an important factor afecting CH4 pumpability and N2 injectability.The pore structure characteristics of low-permeability coal were obtained by fuid intrusion method and photoelectric radiation technology.The multistage and connectivity of coal pores were analyzed.Subsequently,a simultaneous test experiment of CH4/N2 adsorption–desorption and coal deformation was carried out.The deformation characteristics of coal were clarifed and a coal strain model was constructed.Finally,the applicability of low-permeability coal to N2 injection for CH4 displacement technology was investigated.The results show that the micropores and transition pores of coal samples are relatively developed.The pore morphology of coal is dominated by semi-open pores.The pore structure of coal is highly complex and heterogeneous.Transition pores,mesopores and macropores of coal have good connectivity,while micropores have poor connectivity.Under constant triaxial stress,the adsorption capacity of the coal for CH4 is greater than that for N2,and the deformation capacity of the coal for CH4 adsorption is greater than that for N2 adsorption.The axial strain,circumferential strain,and volumetric strain during the entire process of CH4 and N2 adsorption/desorption in the coal can be divided into three stages.Coal adsorption–desorption deformation has the characteristics of anisotropy and gas-diference.A strain model for the adsorption–desorption of CH4/N2 from coal was established by considering the expansion stress of adsorbed gas on the coal matrix,the compression stress of free gas on the coal matrix,and the expansion stress of free gas on micropore fractures.N2 has good injectability in low-permeability coal seams and has the dual functions of improving coal seam permeability and enhancing gas fow,which can signifcantly improve the efectiveness of low-permeability coal seam gas control and promote the efcient utilization of gas resources.
基金supported in part by“The National Natural Science Foundation of China (No.52168038)”“Applied Basic Research Foundation of Yunnan Province (No.2019FD125)”“Applied Basic Research Foundation of Yunnan Province (No.202201AT070159)”.
文摘The durability of cement-based materials is related to water transport and storage in their pore network under different humidity conditions.To understand the mechanism and characteristics of water adsorption and desorption processes from the microscopic scale,this study introduces different points of view for the pore space model generation and numerical simulation of water transport by considering the“ink-bottle”effect.On the basis of the pore structure parameters(i.e.,pore size distribution and porosity)of cement paste and mortar with water-binder ratios of 0.3,0.4 and 0.5 obtained via mercury intrusion porosimetry,randomly formed 3D pore space models are generated using two-phase transformation on Gaussian random fields and verified via image analysis method of mathematical morphology.Considering the Kelvin-Laplace equation and the influence of“ink-bottle”pores,two numerical calculation scenarios based on mathematical morphology are proposed and applied to the generated model to simulate the adsorption-desorption process.The simulated adsorption and desorption curves are close to those of the experiment,verifying the effectiveness of the developed model and methods.The obtained results characterize water transport in cement-based materials during the variation of relative humidity and further explain the hysteresis effect due to“ink-bottle”pores from the microscopic scale.
文摘[Objective]The research aimed to provide scientific reference for reasonable utilization of polyacrylamide(PAM).[Method]After PAM treatment,the soil aggregates were classified through dry sieve analysis and the adsorption capacity and desorption capacity of all soil aggregates to phosphorus at different phosphorus concentrations were analyzed.[Result] The phosphorus adsorption and desorption of soil sample treated by PAM declined. The amount of phosphorus adsorption increased with the increase of phosphorus concentration and this increase was fast in low phosphorus concentration area but slow in high phosphorus concentration area.At different phosphorus concentrations,adsorption showed a へ shape changing trend.The phosphorus adsorption was related to phosphorus concentration and the 2-3 mm aggregate had the highest desorption rate while 0.1-0.25 mm aggregate and 0.45-1 mm aggregate had lowest desorption rate.[Conclusion]The PAM treatment generated significant influence on phosphorus adsorption and analytic features of aggregate in all size fractions.
基金Supported by Science and Technology Research Project of Jiangxi Education Department(GJJ14289)Science and Technology Research Project of Environmental Protection Department of Jiangxi Province(JXHBKJ2013-4)Special Fund for Visiting Scholars from the Development Program for Middle-aged and Young Teachers in Colleges of Jiangxi Province(GJGH[2014]N0.15)
文摘[Objective] This study aimed to investigate the adsorption and desorption characteristics of cadmium and lead in typical paddy soils of Jiangxi Province. [Method] Gleyed paddy soil and waterloggogenic paddy soil were collected from Jiangxi Province and used as experimental materials to investigate single and com- petitive adsorption and desorption behaviors of cadmium and lead by batch equilib- rium method. The environmental risk of the presence of cadmium and lead in paddy soils was assessed using distribution coefficients. [Result] Under equal ratio condi- tions, the adsorption capacity of lead by two types of paddy soils was higher than that of cadmium, and the adsorption rate in waterloggogenic paddy soil was higher than that in gleyed paddy soil. The desorption capacity of cadmium by two types of paddy soils was higher than that of lead, and the desorption rate in gleyed paddy soil was higher than that in waterloggogenic paddy soil. Under competitive condi- tions, the adsorption capacity of cadmium and lead by paddy soils was significantly reduced compared with single ion system, while the desorption rate was remarkably improved. The potential environmental risk of cadmium contamination was greater than that of lead in paddy soils. Moreover, environmental risks of cadmium and lead were reduced with the increase of pH, which increased significantly under the coex- istence state. [Conclusion] In the coexistence of cadmium and lead, cadmium con- tamination should be controlled and avoided compared with lead contamination in paddy soils.
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 Program for Excellent Talents in Liaoning Higher Education Institutions(LJQ2012103)~~
文摘The adsorption and desorption kinetic of natural zeolite on NH4+ was stud-ied by lab analysis. The results showed that the adsorption and desorption kinetic of natural zeolite on NH4+ coincided with the first-order kinetics, modified Freundlich equation, parabolic diffusion model, and heterogeneous diffusion model. The desorp-tion of the adsorbed NH4+ was far rapider than the adsorption, which can be fin-ished within 60 min.
基金The research was conducted as part of the“Establishing a Research Observatory to Unlock European Coal Seams for CO_(2) Storage(ROCCS)”project(Grant No.899336)The work of the second author is also sponsored by Shanghai Pujiang Program(Grant No.23PJ1412600)。
文摘Injecting carbon dioxide(CO_(2))into coal seams may unlock substantial carbon sequestration potential.Since the coal acts like a carbon filter,it can preferentially absorb significant amounts of CO_(2).To explore this further,desorption of the adsorbed gas due to pressure drop is investigated in this paper,to achieve an improved understanding of the long-term fate of injected CO_(2) during post-injection period.This paper presents a dual porosity model coupling gas flow,adsorption and geomechanics for studying coupled processes and effectiveness of CO_(2) sequestration in coals.A new adsorption?desorption model derived based on thermodynamics is incorporated,particularly,the desorption hysteresis is considered.The reliability of the proposed adsorption-desorption isotherm is examined via validation tests.It is indicated that occurrence of desorption hysteresis is attributed to the adsorption-induced pore deformation.After injection ceases,the injected gas continues to propagate further from the injection well,while the pressure in the vicinity of the injection well experiences a significant drop.Although the adsorbed gas near the well also decreases,this decrease is less compared to that in pressure because of desorption hysteresis.The unceasing spread of CO_(2) and drops of pressure and adsorbed gas depend on the degree of desorption hysteresis and heterogeneity of coals,which should be considered when designing CO_(2) sequestration into coal seams.
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financially supported by the National Natural Science Foundation of China(Grant Nos.12074382 and 11474285).
文摘We study the desorption mechanism of hydrogen isotopes from graphene surface using first-principles calculations,with focus on the effects of quantum tunneling.At low temperatures,quantum tunneling plays a dominant role in the desorption process of both hydrogen monomers and dimers.In the case of dimer desorption,two types of mechanisms,namely the traditional one-step desorption in the form of molecules(molecular mechanism),and the two-step desorption in the form of individual atoms(atomic mechanism),are studied and compared.For the ortho-dimers,the dominant desorption mechanism is found to switch from the molecular mechanism to the atomic mechanism above a critical temperature,which is∼300K and 200K for H and D,respectively.
基金financially supported by the National Natural Science Foundation of China(Nos.52304314 and U23A20602)the Leading Talents of S&T Innovation of Hunan Province,China(No.2021RC4002)+2 种基金the Open Foundation of State Key Laboratory of Mineral Processing(No.BGRIMM-KJSKL-2024-16)the Open Foundation of Key Laboratory of Green Separation and Enrichment of Strategic Metal Mineral Resources(No.2023-02)the Fundamental Research Funds for the Central Universities of Central South University(No.2024ZZTS0008).
文摘Flotation is the most common method to obtain concentrate through the selective adsorption of collectors on target minerals to make them hydrophobic and floatable.In the hydrometallurgy of concentrate,collectors adsorbed on concentrate can damage ion-exchange resin and increase the chemical oxygen demand(COD)value of wastewater.In this work,we proposed a new scheme,i.e.,desorbing the collectors from concentrate in ore dressing plant and reusing them in flotation flowsheet.Lead nitrate and benzohydroxamic acid(Pb-BHA)complex is a common collector in scheelite flotation.In this study,different physical(stirring or ultrasonic waves)and chemical(strong acid or alkali environment)methods for facilitating the desorption of Pb-BHA collector from scheelite concentrate were explored.Single-mineral desorption tests showed that under the condition of pulp pH 13 and ultrasonic treatment for 15 min,the highest desorption rates of Pb and BHA from the scheelite concentrate were 90.48%and 63.75%,respectively.Run-of-mine ore flotation tests revealed that the reuse of desorbed Pb and BHA reduced the collector dosage by 30%for BHA and 25%for Pb.The strong alkali environment broke the chemical bonds between Pb and BHA.The cavitation effect of ultrasonic waves effectively reduced the interaction intensity between Pb-BHA collector and scheelite surfaces.This method combining ultrasonic waves and strong alkali environment can effectively desorb the collectors from concentrate and provide“clean”scheelite concentrate for metallurgic plants;the reuse of desorbed collector in flotation flowsheet can reduce reagent cost for ore dressing plants.
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supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB0450202).
文摘To identify the species in liquid surface using mass spectrometry,we must eliminate or reduce interferences during the vaporization or desorption of the species from the liquid surface.It is much more challenging to isolate the ionic,larger species from the liquid surface,because of the frangible structures and the higher solvation energies of those species.Here we demonstrate a new mass spectrometry in which the ionic species at the liquid surface can be desorbed with ultrasoft infrared picosecond laser pulses while the liquid surface is not breached.This laser desorption assisted mass spectrometry is not only a powerful tool to detect the fragile species but also promising to investigate vibrational energy transfer dynamics in the liquid surface.
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supported by CNPC-CZU Innovation Alliancethe Research Start-Up Fund of Changzhou University.
文摘Low salinity water containing sulfate ions can significantly alter the surface wettability of carbonate rocks.Nevertheless,the impact of sulfate concentration on the desorption of oil film on the surface of carbonate rock is still unknown.This study examines the variations in the wettability of the surface of carbonate rocks in solutions containing varying amounts of sodium sulfate and pure water.The problem is addressed in the framework of molecular dynamics simulation(Material Studio software)and experiments.The experiment’s findings demonstrate that sodium sulfate can increase the rate at which oil moisture is turned into water moisture.The final contact angle is smaller than that of pure water.The results of the simulations show that many water molecules travel down the water channel under the influence of several powerful forces,including the electrostatic force,the van der Waals force and hydrogen bond,crowding out the oil molecules on the calcite’s surface and causing the oil film to separate.The relative concentration curve of water and oil molecules indicates that the separation rate of the oil film on the surface of calcite increases with the number of sulfate ions.
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the Qatar National Research Fund for funding this work through NPRP(10-0127-170270,acknowledged under the grant code KK-2018-008).
文摘Confronting the severe health threats and environmental impacts of Cr(Ⅵ)in aquatic environments demands innovative and effective remediation approaches.In this study,Graphene oxide(GO)-decorated poly(dimethyl amino ethyl methacrylate)(PDMAEMA)brush nanocomposites(GOP1,GOP2,GOP3,and GOP4)were fabricated using atom transfer radical polymerization(ATRP)by the“graft from”method.The resulting nanocomposites were utilized for removing Cr(Ⅵ)with good adsorption performance due to the electrostatic interaction of protonated nitrogen groups in the brush chains with negatively charged particles in the solution.The kinetic model of pseudo-second-order best represented the contaminants'adsorption characteristics.The WebereMorris model further indicated that surface adsorption and intraparticle diffusion mechanisms primarily controlled the adsorption procedure.Additionally,the Langmuir and Temkin isotherm models were found to most accurately represent the adsorption characteristics of the pollutants on the nanocomposites,and GOP4 can achieve the maximum adsorption capacity of 164.4 mg·g^(-1).The adsorbents'capacity maintains above 85%after five cycles of adsorptiondesorption.The nanocomposites in this study demonstrate promising potential for eliminating Cr(VI)from aqueous solutions.