This study aims to enhance the photocatalytic performance of 2D/2D heterojunctions for NO removal from marine vessel effluents.SnS_(2)/g-C_(3)N_(4) composites were successfully constructed via a facile solvothermal me...This study aims to enhance the photocatalytic performance of 2D/2D heterojunctions for NO removal from marine vessel effluents.SnS_(2)/g-C_(3)N_(4) composites were successfully constructed via a facile solvothermal method,demonstrating a significant improvement in photocatalytic NO removal under visible light irradiation.For high-flux simulated flue gas,the composite with 10%SnS_(2)(denoted as SNCN-10)showed exceptional NO removal efficiency,reaching up to 66.8%,along with excellent reusability over five consecutive cycles.Detailed band structure and density of states(DOS)calculations confirmed the formation of a characteristic heterojunction.Spin-trapping ESR spectroscopy identified·O_(2)^(-)−as the key reactive species driving NO oxidation.Additionally,in situ DRIFT spectroscopy revealed that SNCN-10 facilitated the conversion of NO to nitrate through intermediate species,including bridging nitrite and cis-nitrite(N_(2)O_(2)^(2-)).Kinetic studies further indicated that NO oxidation followed the Langmuir-Hinshelwood(L-H)mechanism.Based on density functional theory(DFT)calculations of free energy changes,a comprehensive reaction pathway for NO oxidation was proposed.These findings provide valuable insights for the development of efficient photocatalytic strategies for NO removal.展开更多
It is still challenging for exploring high-active photocatalysts to efficiently remove levofloxacin(LFX)by activating peroxymonosulfate(PMS).Herein,we constructed a novel Z scheme ZnFe_(2)O_(4)/g-C_(3)N_(4)/CQDs(ZCC)h...It is still challenging for exploring high-active photocatalysts to efficiently remove levofloxacin(LFX)by activating peroxymonosulfate(PMS).Herein,we constructed a novel Z scheme ZnFe_(2)O_(4)/g-C_(3)N_(4)/CQDs(ZCC)heterojunction by anchoring ZnFe_(2)O_(4)on tubular-like g-C_(3)N_(4)induced by CQDs(denoted as CNC)using microwave-assisted thermal methods.The ZCC exhibits the highest photocatalytic activity in activating PMS for LFX degradation,endowing a removal rate~95.3%,which is 4.8 and 7.3 times that of pure ZnFe_(2)O_(4)(19.8%)and g-C_(3)N_(4)(13.1%),separately.The enhanced photocatalytic activity of ZCC can be attributed to the distinctive morphology of CNC,enhanced light response,increased specific surface area and abundant pore structure.Besides,the formed Z scheme heterojunction and CQDs acting as a transmission bridge of the photogenerated charges(e−and h+)can accelerate transfer and inhibit recombination of e−and h+.Radical capture experiments and electron spin resonance(ESR)measurements revealed that SO4•-and O2•-play a predominant role in degradation process of LFX.Liquid chromatography-mass spectrometry(LC-MS)was applied to identify intermediates and propose feasible degradation pathways of LFX.In conclusion,this study presents a promising strategy for regulating the photocatalytic activity of g-C_(3)N_(4)by simultaneously integrating CQDs induction and Z scheme heterojunction construction.展开更多
Owing to outstanding hydrophilicity and ionic interaction,layered double hydroxides(LDHs)have emerged as a promising carrier for high performance catalysts.However,the synthesis of new specialized catalytic LDHs for d...Owing to outstanding hydrophilicity and ionic interaction,layered double hydroxides(LDHs)have emerged as a promising carrier for high performance catalysts.However,the synthesis of new specialized catalytic LDHs for degradation of antibiotics still faces some challenges.In this study,a CoFe_(2)O_(4)/MgAl-LDH composite catalyst was synthesized using a hydrothermal coprecipitation method.Comprehensive characterization reveals that the surface of MgAl-LDH is covered with nanometer CoFe_(2)O_(4) particles.The specific surface area of CoFe_(2)O_(4)/MgAl-LDH is 82.84 m^(2)·g^(-)1,which is 2.34 times that of CoFe_(2)O_(4).CoFe_(2)O_(4)/MgAl-LDH has a saturation magnetic strength of 22.24 A·m^(2)·kg^(-1) facilitating efficient solid-liquid separation.The composite catalyst was employed to activate peroxymonosulfate(PMS)for the efficient degradation of tetracycline hydrochloride(TCH).It is found that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH significantly exceeds that of CoFe_(2)O_(4).The maximum TCH removal reaches 98.2%under the optimal conditions([TCH]=25 mg/L,[PMS]=1.5 mmol/L,CoFe_(2)O_(4)/MgAl-LDH=0.20 g/L,pH 7,and T=25℃).Coexisting ions in the solution,such as SO_(4)^(2-),Cl-,H_(2)PO_(4)^(-),and CO_(3)^(2-),have a negligible effect on catalytic performance.Cyclic tests demonstrate that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH remains 67.2%after five cycles.Mechanism investigations suggest that O_(2)^(•-)and ^(1)O_(2) produced by CoFe_(2)O_(4)/MgAl-LDH play a critical role in the catalytic degradation.展开更多
Tin phosphide(Sn_(x)P_(y))is an anode for sodium-ion batteries resulting from its exceptionally high theoretical capacity in future.Nevertheless,its application will be hindered by significant volume expansion during ...Tin phosphide(Sn_(x)P_(y))is an anode for sodium-ion batteries resulting from its exceptionally high theoretical capacity in future.Nevertheless,its application will be hindered by significant volume expansion during charge discharge cycles and poor electrical conductivity.This study employs a Sn-based metal-organic framework(Sn-MOF)as a precursor for synthesizing tin phosphide nanoparticles.Then Solidago Canadensis L.,commonly known as Canadian Goldenrod,is utilized as a biomass carbon carrier to form a composite with tin phosphide nanoparticles.The biomass derived porous carbon provides additional sodium ion storage sites and serves as a structural scaffold that constrains the volumetric expansion of tin phosphide,thereby enhancing the material’s stability.The fabricated composite exhibits superior electrode electrochemical performance for sodium-ion batteries.It retains a high capacity(489.5 mA·h/g)after 100 cycles at 0.2 A/g.Even after 500 cycles at a high current density of 2 A/g,it still maintains a stable reversible capacity.This study offers a comprehensive exploration of innovative design strategies essential for the development of novel anode materials,paving the way for more sustainable and efficient sodium-ion-based energy storage systems.展开更多
基金The project was supported by Natural Science Foundation of Shandong Province(ZR2021MB104)National Natural Science Foundation of China(22078174).
文摘This study aims to enhance the photocatalytic performance of 2D/2D heterojunctions for NO removal from marine vessel effluents.SnS_(2)/g-C_(3)N_(4) composites were successfully constructed via a facile solvothermal method,demonstrating a significant improvement in photocatalytic NO removal under visible light irradiation.For high-flux simulated flue gas,the composite with 10%SnS_(2)(denoted as SNCN-10)showed exceptional NO removal efficiency,reaching up to 66.8%,along with excellent reusability over five consecutive cycles.Detailed band structure and density of states(DOS)calculations confirmed the formation of a characteristic heterojunction.Spin-trapping ESR spectroscopy identified·O_(2)^(-)−as the key reactive species driving NO oxidation.Additionally,in situ DRIFT spectroscopy revealed that SNCN-10 facilitated the conversion of NO to nitrate through intermediate species,including bridging nitrite and cis-nitrite(N_(2)O_(2)^(2-)).Kinetic studies further indicated that NO oxidation followed the Langmuir-Hinshelwood(L-H)mechanism.Based on density functional theory(DFT)calculations of free energy changes,a comprehensive reaction pathway for NO oxidation was proposed.These findings provide valuable insights for the development of efficient photocatalytic strategies for NO removal.
基金Project(32272823) supported by the National Natural Science Foundation of ChinaProject(145309315) supported by the Research Foundation of Education Bureau of Heilongjiang Province of ChinaProject(YSTSXK202309) supported by the Plant Food Processing Technology Advantages Characteristic Discipline “Science and Technology Research” Special Project in Heilongjiang Province,China。
文摘It is still challenging for exploring high-active photocatalysts to efficiently remove levofloxacin(LFX)by activating peroxymonosulfate(PMS).Herein,we constructed a novel Z scheme ZnFe_(2)O_(4)/g-C_(3)N_(4)/CQDs(ZCC)heterojunction by anchoring ZnFe_(2)O_(4)on tubular-like g-C_(3)N_(4)induced by CQDs(denoted as CNC)using microwave-assisted thermal methods.The ZCC exhibits the highest photocatalytic activity in activating PMS for LFX degradation,endowing a removal rate~95.3%,which is 4.8 and 7.3 times that of pure ZnFe_(2)O_(4)(19.8%)and g-C_(3)N_(4)(13.1%),separately.The enhanced photocatalytic activity of ZCC can be attributed to the distinctive morphology of CNC,enhanced light response,increased specific surface area and abundant pore structure.Besides,the formed Z scheme heterojunction and CQDs acting as a transmission bridge of the photogenerated charges(e−and h+)can accelerate transfer and inhibit recombination of e−and h+.Radical capture experiments and electron spin resonance(ESR)measurements revealed that SO4•-and O2•-play a predominant role in degradation process of LFX.Liquid chromatography-mass spectrometry(LC-MS)was applied to identify intermediates and propose feasible degradation pathways of LFX.In conclusion,this study presents a promising strategy for regulating the photocatalytic activity of g-C_(3)N_(4)by simultaneously integrating CQDs induction and Z scheme heterojunction construction.
基金University Synergy Innovation Program of Anhui Province(GXXT-2022-083)Science and Technology Plan Project of Wuhu City,China(2023kx12)Anhui Provincial Department of Education New Era Education Project(2023xscx070)。
文摘Owing to outstanding hydrophilicity and ionic interaction,layered double hydroxides(LDHs)have emerged as a promising carrier for high performance catalysts.However,the synthesis of new specialized catalytic LDHs for degradation of antibiotics still faces some challenges.In this study,a CoFe_(2)O_(4)/MgAl-LDH composite catalyst was synthesized using a hydrothermal coprecipitation method.Comprehensive characterization reveals that the surface of MgAl-LDH is covered with nanometer CoFe_(2)O_(4) particles.The specific surface area of CoFe_(2)O_(4)/MgAl-LDH is 82.84 m^(2)·g^(-)1,which is 2.34 times that of CoFe_(2)O_(4).CoFe_(2)O_(4)/MgAl-LDH has a saturation magnetic strength of 22.24 A·m^(2)·kg^(-1) facilitating efficient solid-liquid separation.The composite catalyst was employed to activate peroxymonosulfate(PMS)for the efficient degradation of tetracycline hydrochloride(TCH).It is found that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH significantly exceeds that of CoFe_(2)O_(4).The maximum TCH removal reaches 98.2%under the optimal conditions([TCH]=25 mg/L,[PMS]=1.5 mmol/L,CoFe_(2)O_(4)/MgAl-LDH=0.20 g/L,pH 7,and T=25℃).Coexisting ions in the solution,such as SO_(4)^(2-),Cl-,H_(2)PO_(4)^(-),and CO_(3)^(2-),have a negligible effect on catalytic performance.Cyclic tests demonstrate that the catalytic performance of CoFe_(2)O_(4)/MgAl-LDH remains 67.2%after five cycles.Mechanism investigations suggest that O_(2)^(•-)and ^(1)O_(2) produced by CoFe_(2)O_(4)/MgAl-LDH play a critical role in the catalytic degradation.
文摘Tin phosphide(Sn_(x)P_(y))is an anode for sodium-ion batteries resulting from its exceptionally high theoretical capacity in future.Nevertheless,its application will be hindered by significant volume expansion during charge discharge cycles and poor electrical conductivity.This study employs a Sn-based metal-organic framework(Sn-MOF)as a precursor for synthesizing tin phosphide nanoparticles.Then Solidago Canadensis L.,commonly known as Canadian Goldenrod,is utilized as a biomass carbon carrier to form a composite with tin phosphide nanoparticles.The biomass derived porous carbon provides additional sodium ion storage sites and serves as a structural scaffold that constrains the volumetric expansion of tin phosphide,thereby enhancing the material’s stability.The fabricated composite exhibits superior electrode electrochemical performance for sodium-ion batteries.It retains a high capacity(489.5 mA·h/g)after 100 cycles at 0.2 A/g.Even after 500 cycles at a high current density of 2 A/g,it still maintains a stable reversible capacity.This study offers a comprehensive exploration of innovative design strategies essential for the development of novel anode materials,paving the way for more sustainable and efficient sodium-ion-based energy storage systems.
