CO_(2)reformation of methane(CRM)and CO_(2)methanation are two interconnected processes with significant implications for greenhouse gas reduction and sustainable energy production for industrial purposes.While Nibase...CO_(2)reformation of methane(CRM)and CO_(2)methanation are two interconnected processes with significant implications for greenhouse gas reduction and sustainable energy production for industrial purposes.While Nibased catalysis suffers from poor stability due to coke formation or sintering,we report a super stable remedy.The active sites of mesoporous MgO were loaded using wet impregnation.The incorporation of Ni and promoters altered the physical features of the catalysts.Sm–Ni/MgO showed the smallest crystallite size,specific surface area,and pore volume.The Sm–Ni/MgO catalyst was selected as the most suitable candidate for CRM,with 82%CH4 and H2/CO ratio of approximately 100%and also for CO_(2)methanation with the conversion of carbon dioxide(82%)and the selectivity toward methane reaches 100%at temperatures above 300ᵒC.Furthermore,the Sm–Ni/MgO catalyst was stable for 900 min of continuous reaction,without significant carbon deposition.This stability was largely due to the high oxygen mobility on the catalyst surface in the presence of Sm.Overall,we demonstrated the efficacy of using promoted Ni catalysts supported by mesoporous magnesia for the improved reformation of greenhouse gases.展开更多
Novel graphitic carbon nitride(g-C_(3)N_(4))nanosheet/Bi_(5)O_(7)Br/NH_(2)-MIL-88B(Fe)photocatalysts(denoted as GCN-NSh/Bi_(5)O_(7)Br/FeMOF,in which MOF is metal–organic framework)with double S-scheme heterojunctions...Novel graphitic carbon nitride(g-C_(3)N_(4))nanosheet/Bi_(5)O_(7)Br/NH_(2)-MIL-88B(Fe)photocatalysts(denoted as GCN-NSh/Bi_(5)O_(7)Br/FeMOF,in which MOF is metal–organic framework)with double S-scheme heterojunctions were synthesized by a facile solvothermal route.The resultant materials were examined by X-ray photoelectron spectrometer(XPS),X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDX),transmission electron microscopy(TEM),high-resolution transmission electron microscopy(HRTEM),photoluminescence spectroscopy(PL),Fourier transform infrared spectroscopy(FT-IR),UV-Vis diffuse reflection spectroscopy(UV-vis DRS),photocurrent density,electrochemical impedance spectroscopy(EIS),and Brunauer–Emmett–Teller(BET)analyses.After the integration of Fe-MOF with GCN-NSh/Bi_(5)O_(7)Br,the removal constant of tetracycline over the optimal GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite was promoted 33 times compared with that of the pristine GCN.The GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite showed superior photoactivity to azithromycin,metronidazole,and cephalexin removal that was 36.4,20.2,and 14.6 times higher than that of pure GCN,respectively.Radical quenching tests showed that·O_(2)-and h+mainly contributed to the elimination reaction.In addition,the nanocomposite maintained excellent activity after 4 successive cycles.Based on the developed n–n heterojunctions among n-GCN-NSh,n-Bi_(5)O_(7)Br,and n-Fe-MOF semiconductors,the double S-scheme charge transfer mechanism was proposed for the destruction of the selected antibiotics.展开更多
The photocatalytic activity of carbon nitride(CN)materials is mainly limited to small specific surface areas,limited solar absorption,and low separation and mobility of photoinduced carriers.In this study,we developed...The photocatalytic activity of carbon nitride(CN)materials is mainly limited to small specific surface areas,limited solar absorption,and low separation and mobility of photoinduced carriers.In this study,we developed a precursor-modified strategy for the synthesis of graphitic CN with highly efficient photocatalytic performance.The precursor dicyandiamide reformed by different acids undergoes a basic structural change and transforms into diverse new precursors.The thin porous amino-rich HNO_(3)-CN(5H-CN)was calcined by dicyandiamidine nitrate,formed by concentrated nitric acid modified dicyandiamide,and presented the best photocatalytic degradation rate of Rh B,more than 34 times that of bulk graphitic CN.Moreover,the photocatalytic hydrogen evolution rate of 5H-CN significantly improved.The TG-DSC-FTIR analyses indicated that the distinguishing thermal polymerization process of 5H-CN led to its thin porous amino-rich structure,and the theoretical calculations revealed that the negative conduction band potential of 5H-CN was attributed to its amino-rich structure.It is anticipated that the thin porous structure and the negative conduction band position of 5H-CN play important roles in the improvement of the photocatalytic performance.This study demonstrates that precursor modification is a promising project to induce a new thermal polycondensation process for the synthesis of CN with enhanced photocatalytic performance.展开更多
This research discusses the separation of methane gas from three different gas mixtures,CH4/H2 S,CH4/N2 and CH4/CO2,using a modified silicon carbide nanosheet(Si CNS)membrane using both molecular dynamics(MD)and compu...This research discusses the separation of methane gas from three different gas mixtures,CH4/H2 S,CH4/N2 and CH4/CO2,using a modified silicon carbide nanosheet(Si CNS)membrane using both molecular dynamics(MD)and computational fluid dynamics(CFD)methods.The research examines the effects of different structures of the Si CNSs on the separation of these gas mixtures.Various parameters including the potential of the mean force,separation factor,permeation rate,selectivity and diffusivity are discussed in detail.Our MD simulations showed that the separation of CH4/H2 S,and CH4/CO2 mixtures was successful,while simulation demonstrated a poor result for the CH4/N2 mixture.The effect of temperature on the diffusivity of gas is also discussed,and a correlation is introduced for diffusivity as a function of temperature.The evaluated value for diffusivity is then used in the CFD method to investigate the permeation rate of gas mixtures.展开更多
Li^(+) transport in solid electrolyte interphase is recognized as important factor,which has become a research hotspot.Recently,an one-step pore diffusion mechanism for Li^(+) transport through solid electrolyte inter...Li^(+) transport in solid electrolyte interphase is recognized as important factor,which has become a research hotspot.Recently,an one-step pore diffusion mechanism for Li^(+) transport through solid electrolyte interphase was proposed,which was different from previous two-step mechanism.Such one-step pore diffusion process could effectively eliminate the dynamic limitations of Li^(+) transport in solid electrolyte interphase (SEI) for rapid charging process.The work will contribute to the development of rapid charging lithium-ion batteries.展开更多
Plants are essential components of all ecosystems and play a critical role in environmental fate of nanoparticles. However, the toxicological impacts of nanoparticles on plants are not well documented. Titanium dioxid...Plants are essential components of all ecosystems and play a critical role in environmental fate of nanoparticles. However, the toxicological impacts of nanoparticles on plants are not well documented. Titanium dioxide nanoparticles(TiO2-NPs) are produced worldwide in large quantities for a wide range of purposes. In the present study, the uptake of TiO2-NPs by the aquatic plant Spirodela polyrrhiza and the consequent effects on the plant were evaluated.Initially, structural and morphological characteristics of the used TiO2-NPs were determined using XRD, SEM, TEM and BET techniques. As a result, an anatase structure with the average crystalline size of 8 nm was confirmed for the synthesized TiO2-NPs. Subsequently, entrance of TiO2-NPSto plant roots was verified by fluorescence microscopic images. Activity of a number of antioxidant enzymes, as well as, changes in growth parameters and photosynthetic pigment contents as physiological indices were assessed to investigate the effects of TiO2-NPs on S. polyrrhiza. The increasing concentration of TiO2-NPs led to the significant decrease in all of the growth parameters and changes in antioxidant enzyme activities. The activity of superoxide dismutase enhanced significantly by the increasing concentration of TiO2-NPs. Enhancement of superoxide dismutase activity could be explained as promoting antioxidant system to scavenging the reactive oxygen species. In contrast, the activity of peroxidase was notably decreased in the treated plants. Reduced peroxidase activity could be attributed to either direct effect of these particles on the molecular structure of the enzyme or plant defense system damage due to reactive oxygen species.展开更多
Sonochemical synthesis has flourished significantly in the last few decades for the preparation of photocatalysts.A large number of photocatalysts have been prepared through sonochemical techniques.This review highlig...Sonochemical synthesis has flourished significantly in the last few decades for the preparation of photocatalysts.A large number of photocatalysts have been prepared through sonochemical techniques.This review highlights the scope of sonochemistry in the preparation of photocatalysts,and their applications in energy production and environmental remediation.Beside,the sonochemical degradation of pollutants is discussed in detail.The progress made in sonochemical synthesis and the future perspective for this technique are summarized here.This review may create more enthusiasm among researchers to pay extra attention to the sonochemical synthesis of materials and add their useful contribution to the investigation of new materials for photocatalytic and other applications.This will propel this technique toward commercial sonosynthesis of nanomaterials.展开更多
The potential of pennywort (Hydrocotyle vulgaris) for phytoremediation of C.I. Acid Blue 92 (AB92) was evaluated. The effects of various experimental parameters including pH, temperature, dye concentration and pla...The potential of pennywort (Hydrocotyle vulgaris) for phytoremediation of C.I. Acid Blue 92 (AB92) was evaluated. The effects of various experimental parameters including pH, temperature, dye concentration and plant weight on dye removal efficiency were investigated. The results showed that the optimal condition for dye removal were pH 3.5 and temperature 25~C. Moreover, the absolute dye removal enhanced with increase in the initial dye concentration and plant weight. Pennywort showed the same removal efficiency in repeated experiments (four runs) as that obtained from the first run (a 6-day period). Therefore, the ability of the plant in consecutive removal of AB92 confirmed the biodegradation process. Accordingly, a number of produced intermediate compounds were identified. The effect of treatment on photosynthesis and antioxidant defense system including superoxide dismutase, peroxidase and catalase in plant roots and leaves were evaluated. The results revealed a reduction in photosynthetic pigments content under dye treatments. Antioxidant enzyme responses showed marked variations with respect to the plant organ and dye concentration in the liquid medium. Overall, the increase in antioxidant enzyme activity under AB92 stress in the roots was much higher than that in the leaves. Nevertheless, no significant increase in malondialdehyde content was detected in roots or leaves, implying that the high efficiency of antioxidant system in the elimination of reactive oxygen species. Based on these results, pennywort was founded to be a capable species for phytoremediation of AB92-contaminated water, may be effective for phytoremediation dye-contaminated polluted aquatic ecosystems.展开更多
Chromium(Cr)-contaminated soils pose a great environmental risk, with high solubility and persistent leaching of Cr(Ⅵ). In this study, hydroxysulfate green rust(GR_(SO4)), with the general formula Fe(Ⅱ)_(4) Fe(Ⅲ)_(...Chromium(Cr)-contaminated soils pose a great environmental risk, with high solubility and persistent leaching of Cr(Ⅵ). In this study, hydroxysulfate green rust(GR_(SO4)), with the general formula Fe(Ⅱ)_(4) Fe(Ⅲ)_(2)(OH)_(12) SO_(4)·8 H_(2) O, was evaluated for its efficiency in Cr(Ⅵ) stabilization via Cr(Ⅵ) reduction to Cr(Ⅲ) in four representative Cr(Ⅵ)-spiked soils. The initial concentrations of phosphate buffer-extractable Cr(Ⅵ)(Cr(Ⅵ)b) in soils 1, 2, 3, and 4 were 382.4, 575.9, 551.3, and 483.7 mg kg^(-1), respectively. Reduction of Cr(Ⅵ) to Cr(Ⅲ) by structural Fe(Ⅱ)(Fe(Ⅱ)s) in GR_(SO4) in all studied soils was fast,wherein the application of GR_(SO4) markedly decreased the amount of Cr(Ⅵ)bat the Cr(Ⅵ)b/Fe(Ⅱ)s stoichiometric mole ratio of 0.33. The kinetics of Cr(Ⅵ)reduction by GR_(SO4) could not be determined as this reaction coincided with the release of Cr(Ⅵ) from soil during the experiment. The concentration of Cr(Ⅵ)bdecreased, as the Cr(Ⅵ)b/Fe(Ⅱ)s ratio decreased from 0.46 to 0.20, generally to below 10 mg kg^(-1). Back-transformation of the generated Cr(Ⅲ)was examined in the presence of manganese oxide birnessite at the birnessite/initial Cr(Ⅲ) mole ratio of 4.5. The results of batch tests showed that only 5.2% of the initial Cr(Ⅲ) was converted to Cr(Ⅵ) after two months, while under field capacity moisture conditions, less than 0.05% of the initial Cr(Ⅲ) was oxidized to Cr(Ⅵ) after six months. The results illustrated that remediation of Cr(Ⅵ)-contaminated soils would be fast, successful, and irreversible with an appropriate quantity of fresh GR_(SO_(4)).展开更多
基金supports rendered by Zhejiang Normal University(Grant No.YS304221928)Iran National Science Foundation.No.:4002219Yonsei University Mirae Campus.
文摘CO_(2)reformation of methane(CRM)and CO_(2)methanation are two interconnected processes with significant implications for greenhouse gas reduction and sustainable energy production for industrial purposes.While Nibased catalysis suffers from poor stability due to coke formation or sintering,we report a super stable remedy.The active sites of mesoporous MgO were loaded using wet impregnation.The incorporation of Ni and promoters altered the physical features of the catalysts.Sm–Ni/MgO showed the smallest crystallite size,specific surface area,and pore volume.The Sm–Ni/MgO catalyst was selected as the most suitable candidate for CRM,with 82%CH4 and H2/CO ratio of approximately 100%and also for CO_(2)methanation with the conversion of carbon dioxide(82%)and the selectivity toward methane reaches 100%at temperatures above 300ᵒC.Furthermore,the Sm–Ni/MgO catalyst was stable for 900 min of continuous reaction,without significant carbon deposition.This stability was largely due to the high oxygen mobility on the catalyst surface in the presence of Sm.Overall,we demonstrated the efficacy of using promoted Ni catalysts supported by mesoporous magnesia for the improved reformation of greenhouse gases.
文摘Novel graphitic carbon nitride(g-C_(3)N_(4))nanosheet/Bi_(5)O_(7)Br/NH_(2)-MIL-88B(Fe)photocatalysts(denoted as GCN-NSh/Bi_(5)O_(7)Br/FeMOF,in which MOF is metal–organic framework)with double S-scheme heterojunctions were synthesized by a facile solvothermal route.The resultant materials were examined by X-ray photoelectron spectrometer(XPS),X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDX),transmission electron microscopy(TEM),high-resolution transmission electron microscopy(HRTEM),photoluminescence spectroscopy(PL),Fourier transform infrared spectroscopy(FT-IR),UV-Vis diffuse reflection spectroscopy(UV-vis DRS),photocurrent density,electrochemical impedance spectroscopy(EIS),and Brunauer–Emmett–Teller(BET)analyses.After the integration of Fe-MOF with GCN-NSh/Bi_(5)O_(7)Br,the removal constant of tetracycline over the optimal GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite was promoted 33 times compared with that of the pristine GCN.The GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite showed superior photoactivity to azithromycin,metronidazole,and cephalexin removal that was 36.4,20.2,and 14.6 times higher than that of pure GCN,respectively.Radical quenching tests showed that·O_(2)-and h+mainly contributed to the elimination reaction.In addition,the nanocomposite maintained excellent activity after 4 successive cycles.Based on the developed n–n heterojunctions among n-GCN-NSh,n-Bi_(5)O_(7)Br,and n-Fe-MOF semiconductors,the double S-scheme charge transfer mechanism was proposed for the destruction of the selected antibiotics.
文摘The photocatalytic activity of carbon nitride(CN)materials is mainly limited to small specific surface areas,limited solar absorption,and low separation and mobility of photoinduced carriers.In this study,we developed a precursor-modified strategy for the synthesis of graphitic CN with highly efficient photocatalytic performance.The precursor dicyandiamide reformed by different acids undergoes a basic structural change and transforms into diverse new precursors.The thin porous amino-rich HNO_(3)-CN(5H-CN)was calcined by dicyandiamidine nitrate,formed by concentrated nitric acid modified dicyandiamide,and presented the best photocatalytic degradation rate of Rh B,more than 34 times that of bulk graphitic CN.Moreover,the photocatalytic hydrogen evolution rate of 5H-CN significantly improved.The TG-DSC-FTIR analyses indicated that the distinguishing thermal polymerization process of 5H-CN led to its thin porous amino-rich structure,and the theoretical calculations revealed that the negative conduction band potential of 5H-CN was attributed to its amino-rich structure.It is anticipated that the thin porous structure and the negative conduction band position of 5H-CN play important roles in the improvement of the photocatalytic performance.This study demonstrates that precursor modification is a promising project to induce a new thermal polycondensation process for the synthesis of CN with enhanced photocatalytic performance.
文摘This research discusses the separation of methane gas from three different gas mixtures,CH4/H2 S,CH4/N2 and CH4/CO2,using a modified silicon carbide nanosheet(Si CNS)membrane using both molecular dynamics(MD)and computational fluid dynamics(CFD)methods.The research examines the effects of different structures of the Si CNSs on the separation of these gas mixtures.Various parameters including the potential of the mean force,separation factor,permeation rate,selectivity and diffusivity are discussed in detail.Our MD simulations showed that the separation of CH4/H2 S,and CH4/CO2 mixtures was successful,while simulation demonstrated a poor result for the CH4/N2 mixture.The effect of temperature on the diffusivity of gas is also discussed,and a correlation is introduced for diffusivity as a function of temperature.The evaluated value for diffusivity is then used in the CFD method to investigate the permeation rate of gas mixtures.
基金financially supported by the National Natural Science Foundation of China (Nos.52272287, 22268003 and 22202138)the Science and Technology Project of Yunnan (Nos.202305AF150116,202301AT070027 and 230212526080)。
文摘Li^(+) transport in solid electrolyte interphase is recognized as important factor,which has become a research hotspot.Recently,an one-step pore diffusion mechanism for Li^(+) transport through solid electrolyte interphase was proposed,which was different from previous two-step mechanism.Such one-step pore diffusion process could effectively eliminate the dynamic limitations of Li^(+) transport in solid electrolyte interphase (SEI) for rapid charging process.The work will contribute to the development of rapid charging lithium-ion batteries.
文摘Plants are essential components of all ecosystems and play a critical role in environmental fate of nanoparticles. However, the toxicological impacts of nanoparticles on plants are not well documented. Titanium dioxide nanoparticles(TiO2-NPs) are produced worldwide in large quantities for a wide range of purposes. In the present study, the uptake of TiO2-NPs by the aquatic plant Spirodela polyrrhiza and the consequent effects on the plant were evaluated.Initially, structural and morphological characteristics of the used TiO2-NPs were determined using XRD, SEM, TEM and BET techniques. As a result, an anatase structure with the average crystalline size of 8 nm was confirmed for the synthesized TiO2-NPs. Subsequently, entrance of TiO2-NPSto plant roots was verified by fluorescence microscopic images. Activity of a number of antioxidant enzymes, as well as, changes in growth parameters and photosynthetic pigment contents as physiological indices were assessed to investigate the effects of TiO2-NPs on S. polyrrhiza. The increasing concentration of TiO2-NPs led to the significant decrease in all of the growth parameters and changes in antioxidant enzyme activities. The activity of superoxide dismutase enhanced significantly by the increasing concentration of TiO2-NPs. Enhancement of superoxide dismutase activity could be explained as promoting antioxidant system to scavenging the reactive oxygen species. In contrast, the activity of peroxidase was notably decreased in the treated plants. Reduced peroxidase activity could be attributed to either direct effect of these particles on the molecular structure of the enzyme or plant defense system damage due to reactive oxygen species.
基金financially supported by National Science Foundation of China(No.51602207)。
文摘Sonochemical synthesis has flourished significantly in the last few decades for the preparation of photocatalysts.A large number of photocatalysts have been prepared through sonochemical techniques.This review highlights the scope of sonochemistry in the preparation of photocatalysts,and their applications in energy production and environmental remediation.Beside,the sonochemical degradation of pollutants is discussed in detail.The progress made in sonochemical synthesis and the future perspective for this technique are summarized here.This review may create more enthusiasm among researchers to pay extra attention to the sonochemical synthesis of materials and add their useful contribution to the investigation of new materials for photocatalytic and other applications.This will propel this technique toward commercial sonosynthesis of nanomaterials.
文摘The potential of pennywort (Hydrocotyle vulgaris) for phytoremediation of C.I. Acid Blue 92 (AB92) was evaluated. The effects of various experimental parameters including pH, temperature, dye concentration and plant weight on dye removal efficiency were investigated. The results showed that the optimal condition for dye removal were pH 3.5 and temperature 25~C. Moreover, the absolute dye removal enhanced with increase in the initial dye concentration and plant weight. Pennywort showed the same removal efficiency in repeated experiments (four runs) as that obtained from the first run (a 6-day period). Therefore, the ability of the plant in consecutive removal of AB92 confirmed the biodegradation process. Accordingly, a number of produced intermediate compounds were identified. The effect of treatment on photosynthesis and antioxidant defense system including superoxide dismutase, peroxidase and catalase in plant roots and leaves were evaluated. The results revealed a reduction in photosynthetic pigments content under dye treatments. Antioxidant enzyme responses showed marked variations with respect to the plant organ and dye concentration in the liquid medium. Overall, the increase in antioxidant enzyme activity under AB92 stress in the roots was much higher than that in the leaves. Nevertheless, no significant increase in malondialdehyde content was detected in roots or leaves, implying that the high efficiency of antioxidant system in the elimination of reactive oxygen species. Based on these results, pennywort was founded to be a capable species for phytoremediation of AB92-contaminated water, may be effective for phytoremediation dye-contaminated polluted aquatic ecosystems.
基金the University of Tabriz,Iran for providing support。
文摘Chromium(Cr)-contaminated soils pose a great environmental risk, with high solubility and persistent leaching of Cr(Ⅵ). In this study, hydroxysulfate green rust(GR_(SO4)), with the general formula Fe(Ⅱ)_(4) Fe(Ⅲ)_(2)(OH)_(12) SO_(4)·8 H_(2) O, was evaluated for its efficiency in Cr(Ⅵ) stabilization via Cr(Ⅵ) reduction to Cr(Ⅲ) in four representative Cr(Ⅵ)-spiked soils. The initial concentrations of phosphate buffer-extractable Cr(Ⅵ)(Cr(Ⅵ)b) in soils 1, 2, 3, and 4 were 382.4, 575.9, 551.3, and 483.7 mg kg^(-1), respectively. Reduction of Cr(Ⅵ) to Cr(Ⅲ) by structural Fe(Ⅱ)(Fe(Ⅱ)s) in GR_(SO4) in all studied soils was fast,wherein the application of GR_(SO4) markedly decreased the amount of Cr(Ⅵ)bat the Cr(Ⅵ)b/Fe(Ⅱ)s stoichiometric mole ratio of 0.33. The kinetics of Cr(Ⅵ)reduction by GR_(SO4) could not be determined as this reaction coincided with the release of Cr(Ⅵ) from soil during the experiment. The concentration of Cr(Ⅵ)bdecreased, as the Cr(Ⅵ)b/Fe(Ⅱ)s ratio decreased from 0.46 to 0.20, generally to below 10 mg kg^(-1). Back-transformation of the generated Cr(Ⅲ)was examined in the presence of manganese oxide birnessite at the birnessite/initial Cr(Ⅲ) mole ratio of 4.5. The results of batch tests showed that only 5.2% of the initial Cr(Ⅲ) was converted to Cr(Ⅵ) after two months, while under field capacity moisture conditions, less than 0.05% of the initial Cr(Ⅲ) was oxidized to Cr(Ⅵ) after six months. The results illustrated that remediation of Cr(Ⅵ)-contaminated soils would be fast, successful, and irreversible with an appropriate quantity of fresh GR_(SO_(4)).