Adsorption by solid amine adsorbent is a promising technology for decarbonization of flue gas.However,adsorption properties of many solid amine adsorbents need to be enhanced,and it is necessary to further study the C...Adsorption by solid amine adsorbent is a promising technology for decarbonization of flue gas.However,adsorption properties of many solid amine adsorbents need to be enhanced,and it is necessary to further study the CO_(2)adsorption mechanism.A novel CO_(2)adsorbent with high capacity was obtained by grafting 3-aminopropyltriethoxysilane(APTES)on a micro-mesoporous composite molecular sieve ZSM-5/MCM-48 as the support,and then impregnated with tetraethylenepentamine(TEPA)or polyethyleneimine(PEI).The maximum adsorption capacity of APTES-ZSM-5/MCM-48-TEPA-60(A-ZM-T60),loaded with 60%(in mass)TEPA,for CO_(2)reaches 5.82 mmol·g^(-1) at 60℃in 15%(in volume)CO_(2).Carbamate,alkyl ammonium carbamate and carbonate are generated during the chemical adsorption,which is dominant for CO_(2)adsorption because of the reaction between CO_(2)and amino groups on the adsorbent,simultaneously accompanied by weak physical adsorption.All above data confirm that these composites display an outstanding adsorption performance with a bright future for CO_(2)capture from flue gas after desulfurization.展开更多
Hydroxyapatite nanoparticles(HAP NPs)were synthesized by a one‐step hydrothermal method.The surface of HAP NPs was grafted-SH and-COOH chelating groups via in situ surface‐modification with iminodiacetic acid(IDA)an...Hydroxyapatite nanoparticles(HAP NPs)were synthesized by a one‐step hydrothermal method.The surface of HAP NPs was grafted-SH and-COOH chelating groups via in situ surface‐modification with iminodiacetic acid(IDA)and 3‐mercaptopropyl trimethoxysilane(MPS)to afford dual surface‐capped nano‐amendment HAPIDA/MPS.The structure of HAP‐IDA/MPS was characterized,and its adsorption performance for Hg^(2+),Cu^(2+),Zn^(2+),Ni^(2+),Co^(2+),and Cd^(2+)was evaluated.The total adsorption capacity of 0.10 g HAP‐IDA/MPS nano‐amendment for Hg^(2+),Cu^(2+),Zn^(2+),Ni^(2+),Co^(2+),and Cd^(2+)with an initial mass concentration of 20 mg·L^(-1) reached 13.7 mg·g^(-1),about 4.3 times as much as that of HAP.Notably,HAP‐IDA/MPS nano‐amendment displayed the highest immobilization rate for Hg^(2+),possibly because of its chemical reaction with-SH to form sulfide,possessing the lowest solubility product constant among a variety of metal sulfides.展开更多
Adsorption as an effective technique for the remediation of wastewater has been widely used in industrial wastewater treatment due to the advantage of cost-effectiveness,availability of the adsorbent and ease of opera...Adsorption as an effective technique for the remediation of wastewater has been widely used in industrial wastewater treatment due to the advantage of cost-effectiveness,availability of the adsorbent and ease of operation.However,the low adsorption capacity of the reported adsorbents is still a challenge for wastewater treatment with highefficiency.Here,we developed a super adsorbent(SUA-1),which was a kind of porous carbon nanofibers derived from a composite of PAN-based electrospinning and ZIF-8(PAN/ZIF-8)via simple heat treatment process.The asprepared SUA showed an ultra-high adsorption capacity for adsorbing methyl blue(MB)at nearly three times its own weight,as high as 2998.18 mg/g.A series tests demonstrated that the pore-making effect of ZIF-8 during heat treatment process endowed high BET surface area and generated ZnO components as chemical adsorption center.Under the synergistic effect of bonding and non-bonding forces including ionic bond,electrostatic interaction,andπ-πinteraction,the adsorption capacity has been greatly improved.In view of promising efficiency,this work provides guidance and insights for the preparation of highly efficient adsorbents based on electrospinning derived porous carbon nanofibers.展开更多
Currently,the solid adsorbents with porous structure have been widely applied in CO_(2)capture.However,the unmodified MgO-ZrO_(2)adsorbents appeared to be low adsorption capacity of CO_(2).The solid adsorbent material...Currently,the solid adsorbents with porous structure have been widely applied in CO_(2)capture.However,the unmodified MgO-ZrO_(2)adsorbents appeared to be low adsorption capacity of CO_(2).The solid adsorbent materials were successfully synthesized by loading TEPA onto the pore MgO/ZrO_(2)carriers in the paper.The pore structure and surface characteristic of the samples were analyzed by using XRD,BET,FT-IR and SEM.The adsorbent materials exhibited microcrystalline state,and the crystallinity of all samples gradually decreased as the increase of TEPA content.The pore structure analysis indicated that the modification of MgO-ZrO_(2)adsorbents with TEPA led to the decrease of the specific surface areas,but the narrow micro-mesopore size distributions ranging from 1.8-12 nm in the adsorbents still were maintained.FT-IR spectrum results further verified the successful loading of TEPA.The adsorption capacity of the adsorbents for CO_(2)were tested by using an adsorption apparatus equipped with gas chromatography.The results indicated that when the TEPA loading reached 50%,the sample exhibited the maximum adsorption value for CO_(2),reaching 4.07 mmol/g under the operation condition of 75℃and atmospheric pressure.This result could be assigned to not only the base active sites but also the coexistence of both micropore and mesopore in the adsorbent.After three cycles tests for CO_(2)capture,the adsorption value of the sample for CO_(2)can also reached 95%of its original adsorption capacity,which verified the excellent cyclic operation stability.展开更多
Since the discovery of carbon dots(CDs)in 2004,the unique photoluminescence phenomenon of CDs has attracted widespread attention.However,the molecular weight of CDs has not been adequately quantified at present,due to...Since the discovery of carbon dots(CDs)in 2004,the unique photoluminescence phenomenon of CDs has attracted widespread attention.However,the molecular weight of CDs has not been adequately quantified at present,due to CDs are atomically imprecise and their molecular weight distribution is broad.In this paper,a series of Pluronic-modified CDs were prepared and the structure of the CDs was briefly analyzed.Subsequently,a molecular weight measurement method based on colligative properties was developed,and the correction coefficient in the algorithm was briefly analyzed.The calculated molecular weight was applied to the determination of surface adsorption capacity.This work provided a method for averaging the molecular weight of atomically imprecise particulate materials,which is expected to provide new opportunities in related fields.展开更多
To optimize the CO_(2) adsorption performance of carbon materials,this study proposed a preparation method for biomass-based porous carbon through hydrothermal carbonization coupled with nitrogen source optimization a...To optimize the CO_(2) adsorption performance of carbon materials,this study proposed a preparation method for biomass-based porous carbon through hydrothermal carbonization coupled with nitrogen source optimization and K_(2)CO_(3) activation.The effects of different nitrogen sources(urea,piperazine,melamine,and polyaniline)and activation temperatures on the physicochemical features and CO_(2) adsorption characteristics of the porous carbons were systematically investigated.The results indicated that different nitrogen sources showed varying impacts on the CO_(2) uptake of porous carbons,and not all nitrogen sources enhanced the adsorption performance.The urea and piperazine doped porous carbons exhibited relatively low nitrogen contents and specific surface areas.Whereas the melamine doped carbons showed higher nitrogen contents and specific surface areas,but lacked narrow micropores,limiting their CO_(2) adsorption performance.In contrast,PAC-700,prepared using polyaniline as nitrogen source,featured a well-developed pore structure,abundant narrow micropores and pyrrolic-N groups,endowing it with enhanced CO_(2) adsorption capability.At 0℃/1 bar and 25℃/1 bar,the CO_(2) uptake of PAC-700 reached 6.85 and 4.64 mmol/g,respectively.Additionally,PAC-700 maintained a CO_(2) uptake retention ratio of 99%after 5 adsorption-desorption cycles and exhibited good CO_(2)/N_(2) selectivity of 22.4−51.6.These findings highlighted the advantageous CO_(2) adsorption performance of PAC-700,indicating its substantial application potential in the domain of carbon capture.展开更多
A new adsorbent was successfully prepared by hydrothermal treatment and chemical activation through coal gasification fine slag(CGFS)and blue algae(BA)as raw materials and used for CO_(2)capture.The CO_(2)chemisorptio...A new adsorbent was successfully prepared by hydrothermal treatment and chemical activation through coal gasification fine slag(CGFS)and blue algae(BA)as raw materials and used for CO_(2)capture.The CO_(2)chemisorption capacity of the adsorbent was further enhanced by taking advantage of the nitrogenous bases contained in the BA.In the hydrothermal process,the addition of BA significantly increased the content of pyrrole nitrogen in the adsorbent.In the activation process,pyrrole nitrogen gradually changed into pyridine nitrogen and graphite nitrogen.Increased BA addition result in a higher specific surface area and microporosity of the adsorbent.The CO_(2)adsorption performance test proved that the CGFS-50%-CA sample has the strongest CO_(2)adsorption capacity at low temperature,up to 15.59 cm^(3)/g,which is mainly through physical adsorption,and the CGFS-10%-CA sample has the strongest CO_(2)adsorption capacity at high temperature,up to 7.31 cm^(3)/g,which is mainly through chemical adsorption.CO_(2)uptake of the CGFS-10%-CA sample was well maintained after 10 cycles,with regeneration efficiencies above 99%.The results indicate that the novel adsorbents with coexistence of physical and chemical adsorption have great potential for CO_(2)adsorption applications.展开更多
The adsorption of CO on different lattice oxygen sites in Cu doped CeO_(2)(111)was studied by DFT method,and the geometrical structure and electronic properties of adsorption systems were analyzed.The results showed t...The adsorption of CO on different lattice oxygen sites in Cu doped CeO_(2)(111)was studied by DFT method,and the geometrical structure and electronic properties of adsorption systems were analyzed.The results showed that CO interacted with lattice oxygen on the first layer formed CO_(2).However,when adsorbed on the second layer lattice oxygen,carbonate species were formed with the participation of first layer lattice oxygens,i.e.,CO co-adsorbed on first and second layer lattice oxygens.For the second layer adsorption,the absolute CO adsorption energy was big on the Oss nearby Cu.This kind of carbonates was thermodynamically stable,and it was attributed to the facilitation of Cu on CO adsorption,manifested by an electron migration behavior from the C 2p orbitals to the Cu 3d orbitals.However,the absolute CO adsorption energy on the Oss away from Cu was small.Compared to the formation of carbonates,the formation CO_(2)had very small absolute adsorption energy,suggesting the formed carbonates on second layer was stable.Further,when CO adsorbed on the systems with a carbonate,the absolute CO adsorption energy was significantly smaller than that of the non-carbonated system,indicating that the formation of carbonates inhibited CO oxidation on Cu/CeO_(2)(111).Therefore,the formation of carbonates was unfavorable for CO oxidation reaction on Cu/CeO_(2)(111).The results of this study provide theoretical support for the negative effect of CO_(2)on ceria-based catalysts.展开更多
We report a robust pillar-layered metal-organic framework,Zn‑tfbdc‑dabco(tfbdc:tetrafluoroterephthal-ate,dabco:1,4-diazabicyclo[2.2.2]octane),featuring the fluorinated pore environment,for the preferential binding of ...We report a robust pillar-layered metal-organic framework,Zn‑tfbdc‑dabco(tfbdc:tetrafluoroterephthal-ate,dabco:1,4-diazabicyclo[2.2.2]octane),featuring the fluorinated pore environment,for the preferential binding of propane over propylene and thus highly inverse selective separation of propane/propylene mixture.The inverse propane-selective performance of Zn‑tfbdc‑dabco for the propane/propylene separation was validated by single-component gas adsorption isotherms,isosteric enthalpy of adsorption calculations,ideal adsorbed solution theory calculations,along with the breakthrough experiment.The customized fluorinated networks served as a propane-trap to form more interactions with the exposed hydrogen atoms of propane,as unveiled by the simulation studies at the molecular level.With the advantage of inverse propane-selective adsorption behavior,high adsorption capacity,good cycling stability,and low isosteric enthalpy of adsorption,Zn‑tfbdc‑dabco can be a promising candidate adsorbent for the challenging propane/propylene separation to realize one-step purification of the target propylene substance.展开更多
The novel magnetic sepiolite/Fe_(3)O_(4)/zero-valent iron(nZVI)nanocomposite(nZVI@SepH-Mag)was prepared and used to achieve the removal of Cr(VI)in this work.The nZVI@SepH-Mag composites were characterized by XRD,FTIR...The novel magnetic sepiolite/Fe_(3)O_(4)/zero-valent iron(nZVI)nanocomposite(nZVI@SepH-Mag)was prepared and used to achieve the removal of Cr(VI)in this work.The nZVI@SepH-Mag composites were characterized by XRD,FTIR,BET,SEM and TEM.The characterization results indicated that the structure of the composite consisted of small nanoscale nZVI and magnetite(Mag)particles uniformly anchoring on the surface of acid-activated sepiolite(SepH).Batch experiments were used to analyze the effects of main factors on Cr(VI)removal.A 100%removal efficiency in 60 min and enhanced reaction ratio were reached by the composite comparing other existing materials.The kinetic of the adsorption and possible Cr(VI)removal mechanism of the hybrids were also evaluated and proposed.Based on the removal products identified by Raman,XRD and XPS,a reduction mechanism was proposed.The results indicated that the SepH and Mag can inhibit the agglomeration and enhance the dispersibility of nZVI,and Mag and nZVI displayed good synergetic effects.展开更多
Removing copper from nickel electrolysis anode solution has been a major keypoint in the nickel metallurgy industry.In this study,we proposed a novel process flow to promote removing copper from nickel electrolysis an...Removing copper from nickel electrolysis anode solution has been a major keypoint in the nickel metallurgy industry.In this study,we proposed a novel process flow to promote removing copper from nickel electrolysis anode solution.A simulated nickel anode solution was designed,and static and dynamic adsorption experiments were conducted to determine the best of solution pH,adsorption time and temperature,resin dosage and particle size,and stirring speed.The optimal conditions were explored for copper removal from nickel electrolysis anode solution.Based on the optimal experimental conditions and the relevant experimental data,a novel process for copper removal from nickel electrolysis anodes was designed and verified.This novel process of copper removal from nickel electrolysis anodes was confirmed with nickel anolyte solution with nickel 50−60 g/L and copper 0.5 g/L.After finishing the novel process of copper removal,the nickel in the purified nickel anolyte became undetectable and copper concentration was 3 mg/L,the novel process of resin adsorption to remove copper from nickel anode solution through static and dynamic adsorptions has an efficacious copper removal.It is a beneficial supplement to traditional methods.展开更多
With the growing awareness of environmental protection and the increasing demand for rare earth elements(REEs),it has become necessary to efficiently remove and recover REEs from mine wastewater.In this study,jarosite...With the growing awareness of environmental protection and the increasing demand for rare earth elements(REEs),it has become necessary to efficiently remove and recover REEs from mine wastewater.In this study,jarosite(Jar)and schwertmannite(Sch)were biosynthesized using Acidithiobacillus ferrooxidans for the adsorption of REEs.Additionally,the adsorption capacities of Jar and Sch for La^(3+),Ce^(3+),Pr^(3+),Nd^(3+),Sm^(3+),Gd^(3+),Dy^(3+),and Y^(3+)in mine wastewater were improved by mechanical activation.XRD,FTIR,BET,and SEM-EDS analyses revealed that mechanical activation did not alter the phase of the material,but increased the amount of surface-OH and SO42−groups,as well as the specific surface area.This significantly enhanced the adsorption performance of Jar and Sch for REEs.The optimum adsorption time and pH were determined through batch adsorption experiments.Besides,the adsorption kinetics were studied and found to align well with the pseudo-second-order model.Furthermore,the thermodynamic parameters(ΔG^(Θ),ΔH^(Θ)andΔS^(Θ))and adsorption isotherms were analyzed.The results indicated that mechanically activated schwertmannite(M-Sch)exhibited superior adsorption performance for REEs compared to mechanically activated jarosite(M-Jar).Moreover,M-Sch was reusable and exhibited high adsorption efficiency of REEs in actual mine wastewater,exceeding 92%.展开更多
Understanding the adsorption behavior of heavy metals and metalloids on clay minerals is essential for remediating heavy metal-contaminated soils.The adsorption of heavy metals and metalloids on illite(001)and sodium ...Understanding the adsorption behavior of heavy metals and metalloids on clay minerals is essential for remediating heavy metal-contaminated soils.The adsorption of heavy metals and metalloids on illite(001)and sodium montmorillonite(Na-MMT)(001)surfaces was investigated using first-principles calculations in this study,especially As atom and H_(3)AsO_(3) molecule.The adsorption energies of the As atom were−1.94 eV on the illite(001)and−0.56 eV on the Na-MMT(001),whereas,the adsorption energies of the H_(3)AsO_(3) molecule were−1.40 eV on illite(001)and−1.01 eV on Na-MMT(001).The above results indicate that the adsorption was more energetically favorable on illite(001).Additionally,compared to Na-MMT(001),there were more significant interactions between the atoms/molecules on the illite(001).After As atom and H_(3)AsO_(3) molecule adsorption,the electrons were transferred from mineral surface atoms to the adsorbates on both illite(001)and Na-MMT(001)surfaces.Moreover,the adsorption of As atom on illite(001)and Na-MMT(001)surfaces were more energy favorable compared to Hg,Cd,and Cr atoms.Overall,this work provides new insights into the adsorption behavior of As atoms and As molecules on illite and Na-MMT.The results indicate that illite rich soils are more prone to contamination by arsenic compared to soils primarily composed of Na-MMT minerals.展开更多
The intricate grinding process exposes various cleavage surfaces of mineral particles.This paper systematically investigates the structural characteristics of exposed malachite crystal surfaces and the adsorption beha...The intricate grinding process exposes various cleavage surfaces of mineral particles.This paper systematically investigates the structural characteristics of exposed malachite crystal surfaces and the adsorption behavior and mechanism of hydroxamic acid and water molecules using first-principle density functional theory.The study reveals anisotropic surface energies among crystal surfaces,ranked as(201)>(100)>(110)>(001)>(010)>(201).The adsorption of hydroxamic acid and water molecules on malachite surfaces also exhibited anisotropy.The difference in adsorption strength between hydroxamic acid and water molecules on the six exposed surfaces followed the order of(110)>(100)>(010)>(001)>(201)>(201),and the resistance of water molecules to the adsorption of hydroxamic acid on the six exposed surfaces was(110)>(201)>(010)>(201)>(001)>(100).It indicates that the reagent exhibits a strong competitive advantage in adsorption on the(100)surface,and the hindrance of water molecules to reagent adsorption is relatively small,which is favorable for flotation.This study provides theoretical references and innovative insights for the precise design of flotation reagents,as well as for the meticulous optimization of mineral surface interfaces,with the objective of enhancing flotation separation.展开更多
In this study,Schwertmannite,Akaganéite and ammoniojarosite were biosynthesized by different bacteria and characterized.The results showed that bacteria are critical in mediating the mineral formation process:the...In this study,Schwertmannite,Akaganéite and ammoniojarosite were biosynthesized by different bacteria and characterized.The results showed that bacteria are critical in mediating the mineral formation process:the morphology,crystallinity,grain size and specific surface area of each mineral varied upon different bacteria and culturing conditions.In addition,the formed minerals’elemental composition and group disparity lead to different morphology,crystallinity and subsequent adsorption performance.In particular,adsorption difference existed in iron minerals biosynthesized by different bacteria.The maximal adsorption capacities of Akaganéite,Schwertmannite and ammoniojarosite were 26.6 mg/g,17.5 mg/g and 3.90 mg/g respectively.Cr(VI)adsorption on iron-minerals involves hydrogen bonding,electrostatic interaction,and ligand exchange.The adsorption only occurred on the surface of ammoniojarosite,while for Akaganéite and Schwertmannite,the tunnel structure greatly facilitated the adsorption process and improved adsorption capacity.Thus,the molecular structure is the primary determining factor for adsorption performance.Collectively,the results can provide useful information in selecting suitable bacteria for synthesizing heavy-metal scavenging minerals according to different environmental conditions.展开更多
基金National Natural Science Foundation of China(51966002)Natural Science Foundation of Guangxi Province(2020GXNSFAA159144)。
文摘Adsorption by solid amine adsorbent is a promising technology for decarbonization of flue gas.However,adsorption properties of many solid amine adsorbents need to be enhanced,and it is necessary to further study the CO_(2)adsorption mechanism.A novel CO_(2)adsorbent with high capacity was obtained by grafting 3-aminopropyltriethoxysilane(APTES)on a micro-mesoporous composite molecular sieve ZSM-5/MCM-48 as the support,and then impregnated with tetraethylenepentamine(TEPA)or polyethyleneimine(PEI).The maximum adsorption capacity of APTES-ZSM-5/MCM-48-TEPA-60(A-ZM-T60),loaded with 60%(in mass)TEPA,for CO_(2)reaches 5.82 mmol·g^(-1) at 60℃in 15%(in volume)CO_(2).Carbamate,alkyl ammonium carbamate and carbonate are generated during the chemical adsorption,which is dominant for CO_(2)adsorption because of the reaction between CO_(2)and amino groups on the adsorbent,simultaneously accompanied by weak physical adsorption.All above data confirm that these composites display an outstanding adsorption performance with a bright future for CO_(2)capture from flue gas after desulfurization.
文摘Hydroxyapatite nanoparticles(HAP NPs)were synthesized by a one‐step hydrothermal method.The surface of HAP NPs was grafted-SH and-COOH chelating groups via in situ surface‐modification with iminodiacetic acid(IDA)and 3‐mercaptopropyl trimethoxysilane(MPS)to afford dual surface‐capped nano‐amendment HAPIDA/MPS.The structure of HAP‐IDA/MPS was characterized,and its adsorption performance for Hg^(2+),Cu^(2+),Zn^(2+),Ni^(2+),Co^(2+),and Cd^(2+)was evaluated.The total adsorption capacity of 0.10 g HAP‐IDA/MPS nano‐amendment for Hg^(2+),Cu^(2+),Zn^(2+),Ni^(2+),Co^(2+),and Cd^(2+)with an initial mass concentration of 20 mg·L^(-1) reached 13.7 mg·g^(-1),about 4.3 times as much as that of HAP.Notably,HAP‐IDA/MPS nano‐amendment displayed the highest immobilization rate for Hg^(2+),possibly because of its chemical reaction with-SH to form sulfide,possessing the lowest solubility product constant among a variety of metal sulfides.
基金Natural Science Foundation of China(22134005,22204011)Chongqing Talents Program for Outstanding Scientists(cstc2021ycjh-bgzxm0179)。
文摘Adsorption as an effective technique for the remediation of wastewater has been widely used in industrial wastewater treatment due to the advantage of cost-effectiveness,availability of the adsorbent and ease of operation.However,the low adsorption capacity of the reported adsorbents is still a challenge for wastewater treatment with highefficiency.Here,we developed a super adsorbent(SUA-1),which was a kind of porous carbon nanofibers derived from a composite of PAN-based electrospinning and ZIF-8(PAN/ZIF-8)via simple heat treatment process.The asprepared SUA showed an ultra-high adsorption capacity for adsorbing methyl blue(MB)at nearly three times its own weight,as high as 2998.18 mg/g.A series tests demonstrated that the pore-making effect of ZIF-8 during heat treatment process endowed high BET surface area and generated ZnO components as chemical adsorption center.Under the synergistic effect of bonding and non-bonding forces including ionic bond,electrostatic interaction,andπ-πinteraction,the adsorption capacity has been greatly improved.In view of promising efficiency,this work provides guidance and insights for the preparation of highly efficient adsorbents based on electrospinning derived porous carbon nanofibers.
基金supported by Shanxi Provincial Key Research and Development Project(202102090301026)Graduate Education Innovation Project of Taiyuan University of Science and Technology(SY2023024)。
文摘Currently,the solid adsorbents with porous structure have been widely applied in CO_(2)capture.However,the unmodified MgO-ZrO_(2)adsorbents appeared to be low adsorption capacity of CO_(2).The solid adsorbent materials were successfully synthesized by loading TEPA onto the pore MgO/ZrO_(2)carriers in the paper.The pore structure and surface characteristic of the samples were analyzed by using XRD,BET,FT-IR and SEM.The adsorbent materials exhibited microcrystalline state,and the crystallinity of all samples gradually decreased as the increase of TEPA content.The pore structure analysis indicated that the modification of MgO-ZrO_(2)adsorbents with TEPA led to the decrease of the specific surface areas,but the narrow micro-mesopore size distributions ranging from 1.8-12 nm in the adsorbents still were maintained.FT-IR spectrum results further verified the successful loading of TEPA.The adsorption capacity of the adsorbents for CO_(2)were tested by using an adsorption apparatus equipped with gas chromatography.The results indicated that when the TEPA loading reached 50%,the sample exhibited the maximum adsorption value for CO_(2),reaching 4.07 mmol/g under the operation condition of 75℃and atmospheric pressure.This result could be assigned to not only the base active sites but also the coexistence of both micropore and mesopore in the adsorbent.After three cycles tests for CO_(2)capture,the adsorption value of the sample for CO_(2)can also reached 95%of its original adsorption capacity,which verified the excellent cyclic operation stability.
文摘Since the discovery of carbon dots(CDs)in 2004,the unique photoluminescence phenomenon of CDs has attracted widespread attention.However,the molecular weight of CDs has not been adequately quantified at present,due to CDs are atomically imprecise and their molecular weight distribution is broad.In this paper,a series of Pluronic-modified CDs were prepared and the structure of the CDs was briefly analyzed.Subsequently,a molecular weight measurement method based on colligative properties was developed,and the correction coefficient in the algorithm was briefly analyzed.The calculated molecular weight was applied to the determination of surface adsorption capacity.This work provided a method for averaging the molecular weight of atomically imprecise particulate materials,which is expected to provide new opportunities in related fields.
基金supported by the National Key R&D Program(2022YFC3902403)Fundamental Research Funds for the Central Universities(2024JC001,2019JG002)Technology Innovation Special Fund of Jiangsu Province for Carbon Dioxide Emission Peaking and Carbon Neutrality(BE2022307)。
文摘To optimize the CO_(2) adsorption performance of carbon materials,this study proposed a preparation method for biomass-based porous carbon through hydrothermal carbonization coupled with nitrogen source optimization and K_(2)CO_(3) activation.The effects of different nitrogen sources(urea,piperazine,melamine,and polyaniline)and activation temperatures on the physicochemical features and CO_(2) adsorption characteristics of the porous carbons were systematically investigated.The results indicated that different nitrogen sources showed varying impacts on the CO_(2) uptake of porous carbons,and not all nitrogen sources enhanced the adsorption performance.The urea and piperazine doped porous carbons exhibited relatively low nitrogen contents and specific surface areas.Whereas the melamine doped carbons showed higher nitrogen contents and specific surface areas,but lacked narrow micropores,limiting their CO_(2) adsorption performance.In contrast,PAC-700,prepared using polyaniline as nitrogen source,featured a well-developed pore structure,abundant narrow micropores and pyrrolic-N groups,endowing it with enhanced CO_(2) adsorption capability.At 0℃/1 bar and 25℃/1 bar,the CO_(2) uptake of PAC-700 reached 6.85 and 4.64 mmol/g,respectively.Additionally,PAC-700 maintained a CO_(2) uptake retention ratio of 99%after 5 adsorption-desorption cycles and exhibited good CO_(2)/N_(2) selectivity of 22.4−51.6.These findings highlighted the advantageous CO_(2) adsorption performance of PAC-700,indicating its substantial application potential in the domain of carbon capture.
基金supported by the National Natural Science Foundation of China(22168032)the National Key Research and Development Program of China(2023YFC3904302,2023YFB4103500)the Key Projects of Ning Dong Energy and Chemical Industry Base(2023NDKJXMLX022).
文摘A new adsorbent was successfully prepared by hydrothermal treatment and chemical activation through coal gasification fine slag(CGFS)and blue algae(BA)as raw materials and used for CO_(2)capture.The CO_(2)chemisorption capacity of the adsorbent was further enhanced by taking advantage of the nitrogenous bases contained in the BA.In the hydrothermal process,the addition of BA significantly increased the content of pyrrole nitrogen in the adsorbent.In the activation process,pyrrole nitrogen gradually changed into pyridine nitrogen and graphite nitrogen.Increased BA addition result in a higher specific surface area and microporosity of the adsorbent.The CO_(2)adsorption performance test proved that the CGFS-50%-CA sample has the strongest CO_(2)adsorption capacity at low temperature,up to 15.59 cm^(3)/g,which is mainly through physical adsorption,and the CGFS-10%-CA sample has the strongest CO_(2)adsorption capacity at high temperature,up to 7.31 cm^(3)/g,which is mainly through chemical adsorption.CO_(2)uptake of the CGFS-10%-CA sample was well maintained after 10 cycles,with regeneration efficiencies above 99%.The results indicate that the novel adsorbents with coexistence of physical and chemical adsorption have great potential for CO_(2)adsorption applications.
基金supported by National Natural Science Foundation of China(22379059)Applied Basic Research Program Project of Liaoning Province(2023JH2/101300224)+4 种基金Service Local Project of the Education Department of Liaoning Province(Enlisting and Leading)(LJKFZ20220201)General Project of the Educational Department of Liaoning Province(LJKMZ20220728)supported by Talent Scientific Research Fund of Liaoning Petrochemical University(2019-XJJL-028)Collaborative Innovation Project of Beijing-Tianjin-Hebei(Tianjin)(22PTXTHZ00020)Basic scientific research project of Liaoning Provincial Department of Education(LJ212410148019)。
文摘The adsorption of CO on different lattice oxygen sites in Cu doped CeO_(2)(111)was studied by DFT method,and the geometrical structure and electronic properties of adsorption systems were analyzed.The results showed that CO interacted with lattice oxygen on the first layer formed CO_(2).However,when adsorbed on the second layer lattice oxygen,carbonate species were formed with the participation of first layer lattice oxygens,i.e.,CO co-adsorbed on first and second layer lattice oxygens.For the second layer adsorption,the absolute CO adsorption energy was big on the Oss nearby Cu.This kind of carbonates was thermodynamically stable,and it was attributed to the facilitation of Cu on CO adsorption,manifested by an electron migration behavior from the C 2p orbitals to the Cu 3d orbitals.However,the absolute CO adsorption energy on the Oss away from Cu was small.Compared to the formation of carbonates,the formation CO_(2)had very small absolute adsorption energy,suggesting the formed carbonates on second layer was stable.Further,when CO adsorbed on the systems with a carbonate,the absolute CO adsorption energy was significantly smaller than that of the non-carbonated system,indicating that the formation of carbonates inhibited CO oxidation on Cu/CeO_(2)(111).Therefore,the formation of carbonates was unfavorable for CO oxidation reaction on Cu/CeO_(2)(111).The results of this study provide theoretical support for the negative effect of CO_(2)on ceria-based catalysts.
文摘We report a robust pillar-layered metal-organic framework,Zn‑tfbdc‑dabco(tfbdc:tetrafluoroterephthal-ate,dabco:1,4-diazabicyclo[2.2.2]octane),featuring the fluorinated pore environment,for the preferential binding of propane over propylene and thus highly inverse selective separation of propane/propylene mixture.The inverse propane-selective performance of Zn‑tfbdc‑dabco for the propane/propylene separation was validated by single-component gas adsorption isotherms,isosteric enthalpy of adsorption calculations,ideal adsorbed solution theory calculations,along with the breakthrough experiment.The customized fluorinated networks served as a propane-trap to form more interactions with the exposed hydrogen atoms of propane,as unveiled by the simulation studies at the molecular level.With the advantage of inverse propane-selective adsorption behavior,high adsorption capacity,good cycling stability,and low isosteric enthalpy of adsorption,Zn‑tfbdc‑dabco can be a promising candidate adsorbent for the challenging propane/propylene separation to realize one-step purification of the target propylene substance.
基金Projects(52474138,52104261,52525401)supported by the National Natural Science Foundation of ChinaProject supported by the New Cornerstone Science Foundation through the XPLORER PRIZE,ChinaProject supported by the Shanxi Key Laboratory Funds of Mine Rock Strata Control and Disaster Prevention,China。
文摘The novel magnetic sepiolite/Fe_(3)O_(4)/zero-valent iron(nZVI)nanocomposite(nZVI@SepH-Mag)was prepared and used to achieve the removal of Cr(VI)in this work.The nZVI@SepH-Mag composites were characterized by XRD,FTIR,BET,SEM and TEM.The characterization results indicated that the structure of the composite consisted of small nanoscale nZVI and magnetite(Mag)particles uniformly anchoring on the surface of acid-activated sepiolite(SepH).Batch experiments were used to analyze the effects of main factors on Cr(VI)removal.A 100%removal efficiency in 60 min and enhanced reaction ratio were reached by the composite comparing other existing materials.The kinetic of the adsorption and possible Cr(VI)removal mechanism of the hybrids were also evaluated and proposed.Based on the removal products identified by Raman,XRD and XPS,a reduction mechanism was proposed.The results indicated that the SepH and Mag can inhibit the agglomeration and enhance the dispersibility of nZVI,and Mag and nZVI displayed good synergetic effects.
基金Project(2019yff0216502)supported by the National Key Research&Development Plan of Ministry of Science and Technology of ChinaProject(2021SK1020-4)supported by the Major Science and Technological Innovation Project of Hunan Province,China。
文摘Removing copper from nickel electrolysis anode solution has been a major keypoint in the nickel metallurgy industry.In this study,we proposed a novel process flow to promote removing copper from nickel electrolysis anode solution.A simulated nickel anode solution was designed,and static and dynamic adsorption experiments were conducted to determine the best of solution pH,adsorption time and temperature,resin dosage and particle size,and stirring speed.The optimal conditions were explored for copper removal from nickel electrolysis anode solution.Based on the optimal experimental conditions and the relevant experimental data,a novel process for copper removal from nickel electrolysis anodes was designed and verified.This novel process of copper removal from nickel electrolysis anodes was confirmed with nickel anolyte solution with nickel 50−60 g/L and copper 0.5 g/L.After finishing the novel process of copper removal,the nickel in the purified nickel anolyte became undetectable and copper concentration was 3 mg/L,the novel process of resin adsorption to remove copper from nickel anode solution through static and dynamic adsorptions has an efficacious copper removal.It is a beneficial supplement to traditional methods.
基金Project(2022YFC2105300) supported by the National Key Research and Development Program of ChinaProject(52274288) supported by the National Natural Science Foundation of China。
文摘With the growing awareness of environmental protection and the increasing demand for rare earth elements(REEs),it has become necessary to efficiently remove and recover REEs from mine wastewater.In this study,jarosite(Jar)and schwertmannite(Sch)were biosynthesized using Acidithiobacillus ferrooxidans for the adsorption of REEs.Additionally,the adsorption capacities of Jar and Sch for La^(3+),Ce^(3+),Pr^(3+),Nd^(3+),Sm^(3+),Gd^(3+),Dy^(3+),and Y^(3+)in mine wastewater were improved by mechanical activation.XRD,FTIR,BET,and SEM-EDS analyses revealed that mechanical activation did not alter the phase of the material,but increased the amount of surface-OH and SO42−groups,as well as the specific surface area.This significantly enhanced the adsorption performance of Jar and Sch for REEs.The optimum adsorption time and pH were determined through batch adsorption experiments.Besides,the adsorption kinetics were studied and found to align well with the pseudo-second-order model.Furthermore,the thermodynamic parameters(ΔG^(Θ),ΔH^(Θ)andΔS^(Θ))and adsorption isotherms were analyzed.The results indicated that mechanically activated schwertmannite(M-Sch)exhibited superior adsorption performance for REEs compared to mechanically activated jarosite(M-Jar).Moreover,M-Sch was reusable and exhibited high adsorption efficiency of REEs in actual mine wastewater,exceeding 92%.
基金Project(22376221)supported by the National Natural Science Foundation of ChinaProject(2024JJ2074)supported by the Natural Science Foundation of Hunan Province,ChinaProject(2023QNRC001)supported by the Young Elite Scientists Sponsorship Program by CAST。
文摘Understanding the adsorption behavior of heavy metals and metalloids on clay minerals is essential for remediating heavy metal-contaminated soils.The adsorption of heavy metals and metalloids on illite(001)and sodium montmorillonite(Na-MMT)(001)surfaces was investigated using first-principles calculations in this study,especially As atom and H_(3)AsO_(3) molecule.The adsorption energies of the As atom were−1.94 eV on the illite(001)and−0.56 eV on the Na-MMT(001),whereas,the adsorption energies of the H_(3)AsO_(3) molecule were−1.40 eV on illite(001)and−1.01 eV on Na-MMT(001).The above results indicate that the adsorption was more energetically favorable on illite(001).Additionally,compared to Na-MMT(001),there were more significant interactions between the atoms/molecules on the illite(001).After As atom and H_(3)AsO_(3) molecule adsorption,the electrons were transferred from mineral surface atoms to the adsorbates on both illite(001)and Na-MMT(001)surfaces.Moreover,the adsorption of As atom on illite(001)and Na-MMT(001)surfaces were more energy favorable compared to Hg,Cd,and Cr atoms.Overall,this work provides new insights into the adsorption behavior of As atoms and As molecules on illite and Na-MMT.The results indicate that illite rich soils are more prone to contamination by arsenic compared to soils primarily composed of Na-MMT minerals.
基金Project(52074356)supported by the National Natural Science Foundation of ChinaProject(BGRIMM-KJSKL-2023-06)supported by the Open Foundation of State Key Laboratory of Mineral Processing,China+4 种基金Project(2022RC1183)supported by the Science and Technology Innovation Program of Hunan Province,ChinaProject(kq2009095)supported by the Changsha Science and Technology Project(Outstanding Innovative Youth Training Program),ChinaProject(2023CXQD002)supported by the Innovation Driven Program of Central South University,ChinaProject(B14034)supported by the National“111”Project,ChinaProject(2024ZZTS0655)supported by the Independent Exploration and Innovation Project for Graduate Students of Central South University,China。
文摘The intricate grinding process exposes various cleavage surfaces of mineral particles.This paper systematically investigates the structural characteristics of exposed malachite crystal surfaces and the adsorption behavior and mechanism of hydroxamic acid and water molecules using first-principle density functional theory.The study reveals anisotropic surface energies among crystal surfaces,ranked as(201)>(100)>(110)>(001)>(010)>(201).The adsorption of hydroxamic acid and water molecules on malachite surfaces also exhibited anisotropy.The difference in adsorption strength between hydroxamic acid and water molecules on the six exposed surfaces followed the order of(110)>(100)>(010)>(001)>(201)>(201),and the resistance of water molecules to the adsorption of hydroxamic acid on the six exposed surfaces was(110)>(201)>(010)>(201)>(001)>(100).It indicates that the reagent exhibits a strong competitive advantage in adsorption on the(100)surface,and the hindrance of water molecules to reagent adsorption is relatively small,which is favorable for flotation.This study provides theoretical references and innovative insights for the precise design of flotation reagents,as well as for the meticulous optimization of mineral surface interfaces,with the objective of enhancing flotation separation.
基金Project(42277256)supported by the National Natural Science Foundation of ChinaProjects(HBKT-2021011,HBKT-2021014)supported by the Hunan Province Environmental Protection Research Program,ChinaProject(CDSKY-2023-05)supported by the Scientific Research of Project Hunan Provincial Urban Geological Survey and Monitoring Institute,China。
文摘In this study,Schwertmannite,Akaganéite and ammoniojarosite were biosynthesized by different bacteria and characterized.The results showed that bacteria are critical in mediating the mineral formation process:the morphology,crystallinity,grain size and specific surface area of each mineral varied upon different bacteria and culturing conditions.In addition,the formed minerals’elemental composition and group disparity lead to different morphology,crystallinity and subsequent adsorption performance.In particular,adsorption difference existed in iron minerals biosynthesized by different bacteria.The maximal adsorption capacities of Akaganéite,Schwertmannite and ammoniojarosite were 26.6 mg/g,17.5 mg/g and 3.90 mg/g respectively.Cr(VI)adsorption on iron-minerals involves hydrogen bonding,electrostatic interaction,and ligand exchange.The adsorption only occurred on the surface of ammoniojarosite,while for Akaganéite and Schwertmannite,the tunnel structure greatly facilitated the adsorption process and improved adsorption capacity.Thus,the molecular structure is the primary determining factor for adsorption performance.Collectively,the results can provide useful information in selecting suitable bacteria for synthesizing heavy-metal scavenging minerals according to different environmental conditions.
