Chalcopyrite is a common copper-bearing mineral with antiferromagnetic properties.However,this property has rarely been considered in previous studies for detailed adsorption behaviors of molecules on chalcopyrite.Bas...Chalcopyrite is a common copper-bearing mineral with antiferromagnetic properties.However,this property has rarely been considered in previous studies for detailed adsorption behaviors of molecules on chalcopyrite.Based on density functional theory(DFT),new adsorption pathways by H_(2)O and O_(2)on the chalcopyrite metal terminated(112)surface((112)-M)is found in this work.First,through simulating the adsorption of an isolated water molecule and monolayer water molecules,it is confirmed that H_(2)O molecules tend to adsorb on the surface Fe atoms more than on the surface Cu atoms.Then,we studied various adsorption behaviors of the O_(2)molecule.It is found that the adsorption on the hollow FeAFe site is the most stable case;however,O_(2)is undissociated.Two adsorption cases will happen when H_(2)OAO_(2)adsorb simultaneously on the surface.For the S site,the H_(2)O molecule thoroughly dissociated and formed SAO species,and the other case is H_(2)O undissociated adsorbing at the Cu site.For the former case,it is interesting that H_(2)O is dissociated before O_(2).展开更多
In petroleum industry, crude oil emulsions are commonly formed in oilfields. The asphaltenes and fine particles in crude oil may affect the stability of the emulsions by adsorbing at the water/oil interface. In this r...In petroleum industry, crude oil emulsions are commonly formed in oilfields. The asphaltenes and fine particles in crude oil may affect the stability of the emulsions by adsorbing at the water/oil interface. In this research, the effect of silica nanoparticles and asphaltenes on emulsion stability is explored first. The asphaltenes are proved to benefit emulsion stability. Unlike the asphaltenes, however, the modified silica nanoparticles may have positive or negative effect on emulsion stability, depending on the asphaltene concentration and aggregation degree in the emulsions. Further, it is confirmed by conducting interfacial experiment that the asphaltenes and particles can adsorb at the interface simultaneously and determine the properties of the interfacial layer. More in-depth experiments concerning contact angle and asphaltene adsorption amount on the particles indicate that the asphaltenes can modify the wettability of the particles. Higher concentration and lower aggregation degree of the asphaltenes can increase their adsorption amount on the surface of particles and then improve the modification effectiveness of the particles. Resultantly, the particles with good modification effectiveness can enhance the emulsion stability while the particles with poor modification effectiveness will weaken the emulsion stability.展开更多
First-principles calculations based on density functional theory corrected by Hubbard parameter U （DFT＋U） are applied to the study on the co-adsorption of O2 and H2O molecules to a-U（110） surface. The calculation...First-principles calculations based on density functional theory corrected by Hubbard parameter U （DFT＋U） are applied to the study on the co-adsorption of O2 and H2O molecules to a-U（110） surface. The calculation results show that DFT＋U method with Ueff = 1.5 eV can yield the experimental results of lattice constant and elastic modulus of a-uranium bulk well. Of all 7 low index surfaces of a-uranium, the （001） surface is the most stable with lowest surface energy while the （110） surface possesses the strongest activity with the highest surface energy. The adsorptions of O2 and H2O molecules are investigated separated. The O2 dissociates spontaneously in all initial configurations. For the adsorption of H2O molecule, both molecular and dissociative adsorptionsoccur. Through calculations of co-adsorption, it can be confirmed that the inhibition effect of O2 on the corrosion of uranium by water vapor originates from the preferential adsorption mechanism, while the consumption of H atoms by O atoms exerted little influence on the corrosion of uranium.展开更多
We herein used Fe3O4 nanoparticles（NPs） as an adsorption interface for the concurrent removal of gaseous benzene, toluene, ethylbenzene and m-xylene（BTEX） and sulfur dioxide（SO2）, at different relative humiditie...We herein used Fe3O4 nanoparticles（NPs） as an adsorption interface for the concurrent removal of gaseous benzene, toluene, ethylbenzene and m-xylene（BTEX） and sulfur dioxide（SO2）, at different relative humidities（RH）. X-ray diffraction, Brunauer-Emmett-Teller, and transmission electron microscopy were deployed for nanoparticle surface characterization.Mono-dispersed Fe3O4（Fe2O3·Fe O） NPs synthesized with oleic acid（OA） as surfactant, and uncoated poly-dispersed Fe3O4 NPs demonstrated comparable removal efficiencies.Adsorption experiments of BTEX on NPs were measured using gas chromatography equipped with flame ionization detection, which indicated high removal efficiencies（up to（95 ± 2）%） under dry conditions. The humidity effect and competitive adsorption were investigated using toluene as a model compound. It was observed that the removal efficiencies decreased as a function of the increase in RH, yet, under our experimental conditions, we observed（40 ± 4）% toluene removal at supersaturation for Fe3O4 NPs, and toluene removal of（83 ± 4）% to（59 ± 6）%, for OA-Fe3O4 NPs. In the presence of SO2, the toluene uptake was reduced under dry conditions to（89 ± 2）% and（75 ± 1）% for the uncoated and coated NPs, respectively, depicting competitive adsorption. At RH 〉 100%,competitive adsorption reduced the removal efficiency to（27 ± 1）% for uncoated NPs whereas OA-Fe3O4 NPs exhibited moderate efficiency loss of（55 ± 2）% at supersaturation.Results point to heterogeneous water coverage on the NP surface. The magnetic property of magnetite facilitated the recovery of both types of NPs, without the loss in efficiency when recycled and reused.展开更多
基金The authors are grateful for the financial support provided by the National Natural Science Foundation of China(NSFC)(Nos.51974094,51964004,and U20A20269).
文摘Chalcopyrite is a common copper-bearing mineral with antiferromagnetic properties.However,this property has rarely been considered in previous studies for detailed adsorption behaviors of molecules on chalcopyrite.Based on density functional theory(DFT),new adsorption pathways by H_(2)O and O_(2)on the chalcopyrite metal terminated(112)surface((112)-M)is found in this work.First,through simulating the adsorption of an isolated water molecule and monolayer water molecules,it is confirmed that H_(2)O molecules tend to adsorb on the surface Fe atoms more than on the surface Cu atoms.Then,we studied various adsorption behaviors of the O_(2)molecule.It is found that the adsorption on the hollow FeAFe site is the most stable case;however,O_(2)is undissociated.Two adsorption cases will happen when H_(2)OAO_(2)adsorb simultaneously on the surface.For the S site,the H_(2)O molecule thoroughly dissociated and formed SAO species,and the other case is H_(2)O undissociated adsorbing at the Cu site.For the former case,it is interesting that H_(2)O is dissociated before O_(2).
基金Support from the National Natural Science Foundation of China(Grant No. 51704315)。
文摘In petroleum industry, crude oil emulsions are commonly formed in oilfields. The asphaltenes and fine particles in crude oil may affect the stability of the emulsions by adsorbing at the water/oil interface. In this research, the effect of silica nanoparticles and asphaltenes on emulsion stability is explored first. The asphaltenes are proved to benefit emulsion stability. Unlike the asphaltenes, however, the modified silica nanoparticles may have positive or negative effect on emulsion stability, depending on the asphaltene concentration and aggregation degree in the emulsions. Further, it is confirmed by conducting interfacial experiment that the asphaltenes and particles can adsorb at the interface simultaneously and determine the properties of the interfacial layer. More in-depth experiments concerning contact angle and asphaltene adsorption amount on the particles indicate that the asphaltenes can modify the wettability of the particles. Higher concentration and lower aggregation degree of the asphaltenes can increase their adsorption amount on the surface of particles and then improve the modification effectiveness of the particles. Resultantly, the particles with good modification effectiveness can enhance the emulsion stability while the particles with poor modification effectiveness will weaken the emulsion stability.
基金Project supported by the National Nature Science Foundation of China(Grant Nos.51401237,11474358,and 51271198)
文摘First-principles calculations based on density functional theory corrected by Hubbard parameter U （DFT＋U） are applied to the study on the co-adsorption of O2 and H2O molecules to a-U（110） surface. The calculation results show that DFT＋U method with Ueff = 1.5 eV can yield the experimental results of lattice constant and elastic modulus of a-uranium bulk well. Of all 7 low index surfaces of a-uranium, the （001） surface is the most stable with lowest surface energy while the （110） surface possesses the strongest activity with the highest surface energy. The adsorptions of O2 and H2O molecules are investigated separated. The O2 dissociates spontaneously in all initial configurations. For the adsorption of H2O molecule, both molecular and dissociative adsorptionsoccur. Through calculations of co-adsorption, it can be confirmed that the inhibition effect of O2 on the corrosion of uranium by water vapor originates from the preferential adsorption mechanism, while the consumption of H atoms by O atoms exerted little influence on the corrosion of uranium.
基金the support of the following Canadian funding agencies: NSERC, FRQNT and CFI
文摘We herein used Fe3O4 nanoparticles（NPs） as an adsorption interface for the concurrent removal of gaseous benzene, toluene, ethylbenzene and m-xylene（BTEX） and sulfur dioxide（SO2）, at different relative humidities（RH）. X-ray diffraction, Brunauer-Emmett-Teller, and transmission electron microscopy were deployed for nanoparticle surface characterization.Mono-dispersed Fe3O4（Fe2O3·Fe O） NPs synthesized with oleic acid（OA） as surfactant, and uncoated poly-dispersed Fe3O4 NPs demonstrated comparable removal efficiencies.Adsorption experiments of BTEX on NPs were measured using gas chromatography equipped with flame ionization detection, which indicated high removal efficiencies（up to（95 ± 2）%） under dry conditions. The humidity effect and competitive adsorption were investigated using toluene as a model compound. It was observed that the removal efficiencies decreased as a function of the increase in RH, yet, under our experimental conditions, we observed（40 ± 4）% toluene removal at supersaturation for Fe3O4 NPs, and toluene removal of（83 ± 4）% to（59 ± 6）%, for OA-Fe3O4 NPs. In the presence of SO2, the toluene uptake was reduced under dry conditions to（89 ± 2）% and（75 ± 1）% for the uncoated and coated NPs, respectively, depicting competitive adsorption. At RH 〉 100%,competitive adsorption reduced the removal efficiency to（27 ± 1）% for uncoated NPs whereas OA-Fe3O4 NPs exhibited moderate efficiency loss of（55 ± 2）% at supersaturation.Results point to heterogeneous water coverage on the NP surface. The magnetic property of magnetite facilitated the recovery of both types of NPs, without the loss in efficiency when recycled and reused.
