MnO2-10aded D301 weak basic anion exchange resin has been used as adsorbent to simultaneously remove lead and cadmium ions from aqueous solution.The effects of adsorbent dosage,solution pH and the coexistent ions on t...MnO2-10aded D301 weak basic anion exchange resin has been used as adsorbent to simultaneously remove lead and cadmium ions from aqueous solution.The effects of adsorbent dosage,solution pH and the coexistent ions on the adsorption were investigated.Experimental results showed that with the adsorbent dosage more than 0.6 g/L,both Pb^2+and Cd^2+were simultaneously removed at pH range 5-6.Except for HPO4^2-,the high concentration coexistent ions such as Na^+,K^+,Cl^-,NO3^-,SO4^2-and HCO3^-,showed no significant effect on the removal efficiency of both Pb^2+and Cd^2+under the experimental conditions.The coexistence of Mg^2+,Ca^2+caused the reduction of Cd^2+removal,but not for Pb^2+.The adsorption equilibrium for Pb^2+and Cd^2+could be excellently described by the Langmuir isotherm model with R^2〉0.99.The maximum adsorption capacity was calculated as 80.64 mg/g for Pb^2+and 21.45 mg/g for Cd^2+.The adsorption processes followed the pseudo first-order kinetics model.MnO2-loaded D301 resin has been shown to have a potential to be used as an effective adsorbent for simultaneous removal of lead and cadmium ions from aqueous solution.展开更多
We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-...We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-step pyrolysis as the cathode electrode for Li-O2batteries.It is observed that the intermediate LiMnO4rather than Li2O2is formed when LiO2interactes with MnO(111)during the discharge process.It is precisely because of LiMnO4that reduces its charge overpotential to 0.29 V.The novel reaction mechanism dominated by LiMnO4further facilitates the lower charge overpotential,thereby enhancing the energy efficiency of the batteries.展开更多
The adsorption properties of Cu 2+ -loaded montmorillonite clays (MMT-Cu) for Escherichia coli K 88 as a function of time,bacteria concentrations,pH,ionic strength and temperature were investigated.The results show...The adsorption properties of Cu 2+ -loaded montmorillonite clays (MMT-Cu) for Escherichia coli K 88 as a function of time,bacteria concentrations,pH,ionic strength and temperature were investigated.The results showed that the bacteria adsorption onto MMT-Cu surface reached equilibrium after 90 min.The percentages of E.coli K 88 adsorbed onto the surfaces of MMT-Cu and montmorillonite clays (MMT) at equilibrium were 88.9% and 56.5%,respectively.Scanning electron microscopy revealed that a lot of E.coli K 88 adhered to the surface of MMT-Cu.The zeta potential of MMT-Cu was relatively high as compared to that of MMT.The adsorptive ability of MMT-Cu for E.coli K 88 was higher than that of MMT (P 0.05).Moreover,pH,ionic strength and temperature produced a strong influence on the extent of E.coli K 88 adsorption to surface of MMT-Cu and MMT.The mechanism of adsorption of E.coli onto MMT-Cu may involve electrostatic attraction and physiochemical properties of bacterial cell walls and minerals surfaces.展开更多
Titanium dioxide (TiO2) loaded tungsten trioxide (WO3) composite films are prepared by an E-beam vapor system. Associated with the existence of a heterojunction at the interface of TiO2 and WO3, the prepared TiO2-...Titanium dioxide (TiO2) loaded tungsten trioxide (WO3) composite films are prepared by an E-beam vapor system. Associated with the existence of a heterojunction at the interface of TiO2 and WO3, the prepared TiO2-WO3 composite film shows enhanced photocurrent density, four times than the pure WO3 film illuminated under xenon lamp, and higher incident-photon-to-current conversion e^ciency. By varying the initial TiO2 film thickness, such composite structures could be optimized to obtain the highest photocurrent density. We believe that thin TiO2 films improve the light response and increase the surface roughness of WO3 films. Furthermore, the existence of the heterojunction results in the e^cient charge carriers' separation, transfer process, and a lower recombination of electron-hole pairs, which is beneficial for the enhancement of photocurrent density.展开更多
Aqueous rechargeable Zn/MnO2 zinc-ion batteries(ZIBs)are reviving recently due to their low cost,non-toxicity,and natural abundance.However,their energy storage mechanism remains controversial due to their complicated...Aqueous rechargeable Zn/MnO2 zinc-ion batteries(ZIBs)are reviving recently due to their low cost,non-toxicity,and natural abundance.However,their energy storage mechanism remains controversial due to their complicated electrochemical reactions.Meanwhile,to achieve satisfactory cyclic stability and rate performance of the Zn/MnO2 ZIBs,Mn2+ is introduced in the electrolyte(e.g.,ZnSO4 solution),which leads to more complicated reactions inside the ZIBs systems.Herein,based on comprehensive analysis methods including electrochemical analysis and Pourbaix diagram,we provide novel insights into the energy storage mechanism of Zn/MnO2 batteries in the presence of Mn2+.A complex series of electrochemical reactions with the coparticipation of Zn2+,H+,Mn2+,SO42-,and OH-were revealed.During the first discharge process,co-insertion of Zn2+ and H+ promotes the transformation of MnO2 into ZnxMnO4,MnOOH,and Mn2O3,accompanying with increased electrolyte pH and the formation of ZnSO4·3 Zn(OH)2-5 H2O.During the subsequent charge process,ZnxMnO4,MnOOH,and Mn2O3 revert to a-MnO2 with the extraction of Zn2+ and H+,while ZnSO4·3Zn(OH)2·5H2O reacts with Mn2+ to form ZnMn3O7·3 H2O.In the following charge/discharge processes,besides aforementioned electrochemical reactions,Zn2+ reversibly insert into/extract from α-MnO2,ZnxMnO4,and ZnMn3O7·3H2O hosts;ZnSO4·3Zn(OH)2·5 H2O,Zn2Mn3O8,and ZnMn2O4 convert mutually with the participation of Mn2+.This work is believed to provide theoretical guidance for further research on high-performance ZIBs.展开更多
Various MnO2 structures have been extensively applied in catalysis. In this study,γ-MnO2,α-MnO2, and δ-MnO2 with corresponding rod, tube, and hierarchical architecture morphologies were prepared and applied for the...Various MnO2 structures have been extensively applied in catalysis. In this study,γ-MnO2,α-MnO2, and δ-MnO2 with corresponding rod, tube, and hierarchical architecture morphologies were prepared and applied for the catalytic oxidation of chlorobenzene (CB). The redox ability, H2O activation behavior, and acidity of MnO2 were analyzed using a range of techniques, including TPR, H2O-TPD, XPS, and pyridine-IR. The catalytic activities in CB oxidation were assessed;this revealed that γ-MnO2 exhibited the highest activity and best stability, owing to its enriched surface oxygen vacancies that functioned to activate O2 and H2O, and capture labile chlorine, which reacted with dissociated H2O to form HCl. All the MnO2 phases generated toxic polychlorinated by-products, including CHCl3, CCl4, C2HCl3, and C2Cl4, indicating the occurrence of electrophilic chlorination during CB oxidation. In particular, the dichlorobenzene detected in the effluents of α-MnO2 might generate unintended dioxins via a nucleophilic substitution reaction.展开更多
α‐,β‐,γ‐andδ‐MnO2catalysts were synthesized by a one‐step hydrothermal method,and were utilized for the catalytic oxidation of toluene in a combined plasma‐catalytic process.The relationship between catalyti...α‐,β‐,γ‐andδ‐MnO2catalysts were synthesized by a one‐step hydrothermal method,and were utilized for the catalytic oxidation of toluene in a combined plasma‐catalytic process.The relationship between catalytic performance and MnO2crystal structures was investigated.It was noted that the toluene removal efficiency was32.5%at the specific input energy of160J/L when non‐thermal plasma was used alone.Theα‐MnO2catalyst showed the best activity among the investigated catalysts,yielding a toluene conversion of78.1%at the specific input energy of160J/L.Forβ‐MnO2,γ‐MnO2andδ‐MnO2,removal efficiencies of47.4%,66.1%and50.0%,respectively,were achieved.By powder X‐ray diffraction,Raman spectroscopy,transmission electron microscopy,scanning electron microscopy,Brunauer‐Emmett‐Teller,H2temperature‐programmed reduction and X‐ray photoelectron spectroscopy analyses,it was concluded that the tunnel structure,the stability of the crystal in plasma,the Mn-O bond strength of MnO2and the surface‐chemisorbed oxygen species played important roles in the plasma‐catalytic degradation of toluene.Additionally,the degradation routes of toluene in non‐thermal plasma and in the plasma‐catalytic process were also studied.It was concluded that the introduction of MnO2catalysts enabled O3,O2,electrons and radical species in the gas to be adsorbed on the MnO2surface via a facile interconversion among the Mn4+,Mn3+and Mn2+states.These four species could then be transported to the toluene or intermediate organic by‐products,which greatly improved the toluene removal efficiency and decreased the final output of by‐products.展开更多
α‐,β‐,δ‐,andγ‐MnO2nanocrystals are successfully prepared.We then evaluated the NH3selective catalytic reduction(SCR)performance of the MnO2catalysts with different phases.The NOx conversion efficiency decrease...α‐,β‐,δ‐,andγ‐MnO2nanocrystals are successfully prepared.We then evaluated the NH3selective catalytic reduction(SCR)performance of the MnO2catalysts with different phases.The NOx conversion efficiency decreased in the order:γ‐MnO2>α‐MnO2>δ‐MnO2>β‐MnO2.The NOx conversion with the use ofγ‐MnO2andα‐MnO2catalysts reached90%in the temperature range of140–200°C,while that based onβ‐MnO2reached only40%at200°C.Theγ‐MnO2andα‐MnO2nanowire crystal morphologies enabled good dispersion of the catalysts and resulted in a relatively high specific surface area.We found thatγ‐MnO2andα‐MnO2possessed stronger reducing abilities and more and stronger acidic sites than the other catalysts.In addition,more chemisorbed oxygen existed on the surface of theγ‐MnO2andα‐MnO2catalysts.Theγ‐MnO2andα‐MnO2catalysts showed excellent performance in the low‐temperature SCR of NO to N2with NH3.展开更多
基金supported by the National Mega-Project of Science and Technology of China(No.2008ZX07421-002)the International Cooperation Project of Chinese Ministry of Science and Technology(No.2007DFR90050)
摘要MnO2-10aded D301 weak basic anion exchange resin has been used as adsorbent to simultaneously remove lead and cadmium ions from aqueous solution.The effects of adsorbent dosage,solution pH and the coexistent ions on the adsorption were investigated.Experimental results showed that with the adsorbent dosage more than 0.6 g/L,both Pb^2+and Cd^2+were simultaneously removed at pH range 5-6.Except for HPO4^2-,the high concentration coexistent ions such as Na^+,K^+,Cl^-,NO3^-,SO4^2-and HCO3^-,showed no significant effect on the removal efficiency of both Pb^2+and Cd^2+under the experimental conditions.The coexistence of Mg^2+,Ca^2+caused the reduction of Cd^2+removal,but not for Pb^2+.The adsorption equilibrium for Pb^2+and Cd^2+could be excellently described by the Langmuir isotherm model with R^2〉0.99.The maximum adsorption capacity was calculated as 80.64 mg/g for Pb^2+and 21.45 mg/g for Cd^2+.The adsorption processes followed the pseudo first-order kinetics model.MnO2-loaded D301 resin has been shown to have a potential to be used as an effective adsorbent for simultaneous removal of lead and cadmium ions from aqueous solution.
基金Funded by the National Natural Science Foundation of China(No.22075035)the Technology Planning Project of Liaoning Province(No.2020JH2/10700008)the Dalian Science and Technology Innovation Fund Project(No.2022JJ11CG005)。
摘要We proposed a strategy to address the issue by synthesizing MnO with half-filled 3 d electron orbitals.That is,MnO nanocubes with an edge length of 61.82 nm were successfully prepared through electros-pinning and one-step pyrolysis as the cathode electrode for Li-O2batteries.It is observed that the intermediate LiMnO4rather than Li2O2is formed when LiO2interactes with MnO(111)during the discharge process.It is precisely because of LiMnO4that reduces its charge overpotential to 0.29 V.The novel reaction mechanism dominated by LiMnO4further facilitates the lower charge overpotential,thereby enhancing the energy efficiency of the batteries.
基金supported by the National Natural Science Foundation of China (No.30471255)the Program for New Century Excellent Talents in University(No.NCET-06-0913)
摘要The adsorption properties of Cu 2+ -loaded montmorillonite clays (MMT-Cu) for Escherichia coli K 88 as a function of time,bacteria concentrations,pH,ionic strength and temperature were investigated.The results showed that the bacteria adsorption onto MMT-Cu surface reached equilibrium after 90 min.The percentages of E.coli K 88 adsorbed onto the surfaces of MMT-Cu and montmorillonite clays (MMT) at equilibrium were 88.9% and 56.5%,respectively.Scanning electron microscopy revealed that a lot of E.coli K 88 adhered to the surface of MMT-Cu.The zeta potential of MMT-Cu was relatively high as compared to that of MMT.The adsorptive ability of MMT-Cu for E.coli K 88 was higher than that of MMT (P 0.05).Moreover,pH,ionic strength and temperature produced a strong influence on the extent of E.coli K 88 adsorption to surface of MMT-Cu and MMT.The mechanism of adsorption of E.coli onto MMT-Cu may involve electrostatic attraction and physiochemical properties of bacterial cell walls and minerals surfaces.
基金Supported by the National Natural Science Foundation of China under Grant Nos 11174137,11474215 and 21204058the Natural Science Foundation for the Youth of Jiangsu Province under Grant No BK20130284the Priority Academic Program Development of Jiangsu Higher Education Institutions
摘要Titanium dioxide (TiO2) loaded tungsten trioxide (WO3) composite films are prepared by an E-beam vapor system. Associated with the existence of a heterojunction at the interface of TiO2 and WO3, the prepared TiO2-WO3 composite film shows enhanced photocurrent density, four times than the pure WO3 film illuminated under xenon lamp, and higher incident-photon-to-current conversion e^ciency. By varying the initial TiO2 film thickness, such composite structures could be optimized to obtain the highest photocurrent density. We believe that thin TiO2 films improve the light response and increase the surface roughness of WO3 films. Furthermore, the existence of the heterojunction results in the e^cient charge carriers' separation, transfer process, and a lower recombination of electron-hole pairs, which is beneficial for the enhancement of photocurrent density.
基金the financial support from the International Science & Technology Cooperation Program of China (No. 2016YFE0102200)Shenzhen Technical Plan Project (No. JCYJ20160301154114273)+1 种基金National Key Basic Research(973) Program of China (No. 2014CB932400)Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (2017BT01N111)
摘要Aqueous rechargeable Zn/MnO2 zinc-ion batteries(ZIBs)are reviving recently due to their low cost,non-toxicity,and natural abundance.However,their energy storage mechanism remains controversial due to their complicated electrochemical reactions.Meanwhile,to achieve satisfactory cyclic stability and rate performance of the Zn/MnO2 ZIBs,Mn2+ is introduced in the electrolyte(e.g.,ZnSO4 solution),which leads to more complicated reactions inside the ZIBs systems.Herein,based on comprehensive analysis methods including electrochemical analysis and Pourbaix diagram,we provide novel insights into the energy storage mechanism of Zn/MnO2 batteries in the presence of Mn2+.A complex series of electrochemical reactions with the coparticipation of Zn2+,H+,Mn2+,SO42-,and OH-were revealed.During the first discharge process,co-insertion of Zn2+ and H+ promotes the transformation of MnO2 into ZnxMnO4,MnOOH,and Mn2O3,accompanying with increased electrolyte pH and the formation of ZnSO4·3 Zn(OH)2-5 H2O.During the subsequent charge process,ZnxMnO4,MnOOH,and Mn2O3 revert to a-MnO2 with the extraction of Zn2+ and H+,while ZnSO4·3Zn(OH)2·5H2O reacts with Mn2+ to form ZnMn3O7·3 H2O.In the following charge/discharge processes,besides aforementioned electrochemical reactions,Zn2+ reversibly insert into/extract from α-MnO2,ZnxMnO4,and ZnMn3O7·3H2O hosts;ZnSO4·3Zn(OH)2·5 H2O,Zn2Mn3O8,and ZnMn2O4 convert mutually with the participation of Mn2+.This work is believed to provide theoretical guidance for further research on high-performance ZIBs.
基金supported by the Outstanding Youth Project of Zhejiang Natural Science Foundation(LR19E080004)the National Natural Science Foundation of China(51478418)~~
摘要Various MnO2 structures have been extensively applied in catalysis. In this study,γ-MnO2,α-MnO2, and δ-MnO2 with corresponding rod, tube, and hierarchical architecture morphologies were prepared and applied for the catalytic oxidation of chlorobenzene (CB). The redox ability, H2O activation behavior, and acidity of MnO2 were analyzed using a range of techniques, including TPR, H2O-TPD, XPS, and pyridine-IR. The catalytic activities in CB oxidation were assessed;this revealed that γ-MnO2 exhibited the highest activity and best stability, owing to its enriched surface oxygen vacancies that functioned to activate O2 and H2O, and capture labile chlorine, which reacted with dissociated H2O to form HCl. All the MnO2 phases generated toxic polychlorinated by-products, including CHCl3, CCl4, C2HCl3, and C2Cl4, indicating the occurrence of electrophilic chlorination during CB oxidation. In particular, the dichlorobenzene detected in the effluents of α-MnO2 might generate unintended dioxins via a nucleophilic substitution reaction.
基金supported by the National Key Research and Development Plan of China(2016YFC0204700)Zhejiang Provincial"151"Talents Program(2013)+2 种基金Key Project of Zhejiang Provincial Science and Technology Program,the Program for Zhejiang Leading Team of S&T Innovation(2013TD07)Special Program for Social Development of Key Science and Technology Project of Zhejiang Province(2014C03025)Changjiang Scholar Incentive Program(2009)~~
摘要α‐,β‐,γ‐andδ‐MnO2catalysts were synthesized by a one‐step hydrothermal method,and were utilized for the catalytic oxidation of toluene in a combined plasma‐catalytic process.The relationship between catalytic performance and MnO2crystal structures was investigated.It was noted that the toluene removal efficiency was32.5%at the specific input energy of160J/L when non‐thermal plasma was used alone.Theα‐MnO2catalyst showed the best activity among the investigated catalysts,yielding a toluene conversion of78.1%at the specific input energy of160J/L.Forβ‐MnO2,γ‐MnO2andδ‐MnO2,removal efficiencies of47.4%,66.1%and50.0%,respectively,were achieved.By powder X‐ray diffraction,Raman spectroscopy,transmission electron microscopy,scanning electron microscopy,Brunauer‐Emmett‐Teller,H2temperature‐programmed reduction and X‐ray photoelectron spectroscopy analyses,it was concluded that the tunnel structure,the stability of the crystal in plasma,the Mn-O bond strength of MnO2and the surface‐chemisorbed oxygen species played important roles in the plasma‐catalytic degradation of toluene.Additionally,the degradation routes of toluene in non‐thermal plasma and in the plasma‐catalytic process were also studied.It was concluded that the introduction of MnO2catalysts enabled O3,O2,electrons and radical species in the gas to be adsorbed on the MnO2surface via a facile interconversion among the Mn4+,Mn3+and Mn2+states.These four species could then be transported to the toluene or intermediate organic by‐products,which greatly improved the toluene removal efficiency and decreased the final output of by‐products.
基金supported by the National Natural Science Foundation of China(51502221)~~
摘要α‐,β‐,δ‐,andγ‐MnO2nanocrystals are successfully prepared.We then evaluated the NH3selective catalytic reduction(SCR)performance of the MnO2catalysts with different phases.The NOx conversion efficiency decreased in the order:γ‐MnO2>α‐MnO2>δ‐MnO2>β‐MnO2.The NOx conversion with the use ofγ‐MnO2andα‐MnO2catalysts reached90%in the temperature range of140–200°C,while that based onβ‐MnO2reached only40%at200°C.Theγ‐MnO2andα‐MnO2nanowire crystal morphologies enabled good dispersion of the catalysts and resulted in a relatively high specific surface area.We found thatγ‐MnO2andα‐MnO2possessed stronger reducing abilities and more and stronger acidic sites than the other catalysts.In addition,more chemisorbed oxygen existed on the surface of theγ‐MnO2andα‐MnO2catalysts.Theγ‐MnO2andα‐MnO2catalysts showed excellent performance in the low‐temperature SCR of NO to N2with NH3.