Monolithic carbon electrodes with robust mechanical integrity and porous architecture are highly desired for capacitive deionization but remain challenging.Owing to the excellent mechanical strength and electroconduct...Monolithic carbon electrodes with robust mechanical integrity and porous architecture are highly desired for capacitive deionization but remain challenging.Owing to the excellent mechanical strength and electroconductivity,commercial carbon fibers cloth demonstrates great potential as high-performance electrodes for ions storage.Despite this,its direct application on capacitive deionization is rarely reported in terms of limited pore structure and natural hydrophobicity.Herein,a powerful metal-organic framework-engaged structural regulation strategy is developed to boost the desalination properties of carbon fibers.The obtained porous carbon fibers features hierarchical porous structure and hydrophilic surface providing abundant ions-accessible sites,and continuous graphitized carbon core ensuring rapid electrons transport.The catalytic-etching mechanism involving oxidation of Co and subsequent carbonthermal reduction is proposed and highly relies on annealing temperature and holding time.When directly evaluated as a current collector-free capacitive deionization electrode,the porous carbon fibers demonstrates much superior desalination capability than pristine carbon fibers,and remarkable cyclic stability up to 20 h with negligible degeneration.Particularly,the PCF-1000 showcases the highest areal salt adsorption capacity of 0.037 mg cm^(−2) among carbon microfibers.Moreover,monolithic porous carbon fibers-carbon nanotubes with increased active sites and good structural integrity by in-situ growth of carbon nanotubes are further fabricated to enhance the desalination performance(0.051 mg cm^(−2)).This work demonstrates the great potential of carbon fibers in constructing high-efficient and robust monolithic electrode for capacitive deionization.展开更多
Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple ...Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple pyrolysis of biomass always generates inadequate porosity with limited surface area.Moreover,biomass-derived carbon also suffers from poor wettability and single physical adsorption of ions,resulting in limited desalination performance.Herein,pore structure optimization and element co-doping are integrated on banana peels(BP)-derived carbon to construct hierarchically porous and B,N co-doped carbon with large ions-accessible surface area.A unique expansionactivation(EA)strategy is proposed to modulate the porosity and specific surface area of carbon.Furthermore,B,N co-doping could increase the ions-accessible sites with improved hydrophilicity,and promote ions adsorption.Benefitting from the synergistic effect of hierarchical porosity and B,N co-doping,the resultant electrode manifest enhanced CDI performance for NaCl with large desalination capacity(29.5 mg g^(-1)),high salt adsorption rate(6.2 mg g^(-1)min^(-1)),and versatile adsorption ability for other salts.Density functional theory reveals the enhanced deionization mechanism by pore and B,N co-doping.This work proposes a facile EA strategy for pore structure modulation of biomass-derived carbon,and demonstrates great potentials of integrating pore and heteroatoms-doping on constructing high-performance CDI electrode.展开更多
Non-layered two-dimensional(2 D)carbon complexes manifest great potential in energy-related applications owing to their exotic electronic structures,large electrochemically active surface,and intriguing synergistic ef...Non-layered two-dimensional(2 D)carbon complexes manifest great potential in energy-related applications owing to their exotic electronic structures,large electrochemically active surface,and intriguing synergistic effects.However,reliable method for mass production and thickness manipulation of 2 D carbon complexes remains great challenges.Here,inspired by blowing chewing gum into bubbles,a“tailored gel expanding"strategy is proposed for high-yield synthesis of non-layered 2 D carbon complexes with tailored thickness from~12 nm to~1 lm,by controllable pyrolysis of metal-polymeric gel with adequate crosslinking degree.The key feature for thickness manipulation is introducing NH4 NO3 in sol-gel process,which tailors the expansion behavior of gel precursor during subsequent pyrolysis.Various of 2 D sheets with intimately coupled N,O-doped carbon(NOC)and Ni Co-based(Ni Co,(Ni Co)S_(2),(Ni Co)Se_(2),Ni Co_(2)O_(4),(Ni Co)(PO_(3))_(2))nanocrystals are obtained on a large scale and without any impurities.Moreover,these 2 D products are branched with in-situ grown CNTs on the surface,accelerating electrons transfer and preventing the nanosheets from stacking.As a demonstration,the 2 D(Ni Co)S_(2)/NOC with optimized thickness manifests excellent lithium storage properties in both half and full cells.This method paves a new path for massive and controlled production of non-layered 2 D materials with tailored thickness and robust structure stability for energy-related applications.展开更多
In this paper, we consider a class of Banach space valued singular integrals. The Lp boundedness of these operators has already been obtained. We shall discuss their boundedness from BMO to BMO. As applications, we ge...In this paper, we consider a class of Banach space valued singular integrals. The Lp boundedness of these operators has already been obtained. We shall discuss their boundedness from BMO to BMO. As applications, we get BMO boundedness for the classic g-function and the Marcinkiewicz integral. Some known results are improved.展开更多
As persulfate(S_(2)O_(8)^(2-))is being increasingly used as an alternative oxidizing agent,developing lowcost and eco-friendly catalysts for efficient S_(2)O_(8)^(2-)activation is potentially useful for the treatment ...As persulfate(S_(2)O_(8)^(2-))is being increasingly used as an alternative oxidizing agent,developing lowcost and eco-friendly catalysts for efficient S_(2)O_(8)^(2-)activation is potentially useful for the treatment of wastewater containing refractory organic pollutant.In this study,the degradative features and mechanisms of carbamazepine(CBZ)were systematically investigated in a novel FeS-S_(2)O_(8)^(2-)process under near-neutral conditions.The results exhibited that CBZ can be effectively eliminated by the FeS-S_(2)O_(8)^(2-)process and the optimal conditions were:250 mg/L FeS,0.5 mmol/L S_(2)O_(8)^(2-),and pH=6.0.The existence of Cl^(−)(1 and 50 mmol/L)has little influence on the CBZ elimination,while both HCO_(3)^(−) and HPO_(4)^(2−)(1 and 50 mmol/L)significantly suppressed the CBZ removal in the FeS-S_(2)O_(8)^(2-)process.CBZ could be degraded via a radical mechanism in the FeS-S_(2)O_(8)^(2-)process,the working radical species(i.e.,SO_(4)•−and•OH)were efficiently formed via the promoted decomposition of S_(2)O_(8)^(2-)by the surface Fe2+on the FeS and the dissolved ferrous ions in solution.Based on the identified oxidized products and Fukui index calculations,a possible degradation pathway of CBZ was speculated.More importantly,a two-stage oxidation mechanism of CBZ elimination was speculated in the FeS-S_(2)O_(8)^(2-)process,the activation of S_(2)O_(8)^(2-)by the surface-active Fe(II)of FeS dominated in the initial 5 min,while homogeneous oxidation reactions played more essential parts than others in the following reaction stage(5–60 min).Overall,this study demonstrated that the FeS-S_(2)O_(8)^(2-)process is capable of removing CBZ from water efficiently.展开更多
Hydrogenation of CO_(2) to value-added chemicals has attracted much attention all through the world.In2 O_(3) with cubic bixbyite-type(denoted as c-In2O_(3))is well known for its high CO_(2) hydrogenation activity and...Hydrogenation of CO_(2) to value-added chemicals has attracted much attention all through the world.In2 O_(3) with cubic bixbyite-type(denoted as c-In2O_(3))is well known for its high CO_(2) hydrogenation activity and CH3 OH selectivity at high temperature.However,the other structure of In2O_(3) with rhombohedral corundum-type(denoted as rh-In2O_(3))rarely been investigated as catalyst.Herein,c-In2O_(3) and rh-In2O_(3) were prepared and comparatively studied for CO_(2) hydrogenation.The results indicated that c-In2O_(3) showed higher CO_(2) conversion activity than rh-In2O_(3) due to the impressive reducibility and reactivity.Whereas rh-In2O_(3) had higher CH3 OH selectivity due to weaker CH3 OH and stronger CO adsorption on rhIn2O_(3).Although c-In2O_(3) and rh-In2O_(3) catalysts showed different CO_(2) hydrogenation perfo rmance,in-situ diffuse reflectance infrared Fourier transform spectroscopy showed CO_(2) can be reduced to CO through redox cycling and hydrogenation to CH3 OH through formate path.展开更多
基金We gratefully acknowledge financial supports from the Natural Science Founda-tion of Shandong Province (No.ZR2020QE066)Taishan Scholar Project (No.ts201511080)+1 种基金the fellowship of China Postdoctoral Science Foundation (No.2020M672081)Opening Project of State Key Laboratory of Advanced Tech-nology for Float Glass (No.2020KF08).
文摘Monolithic carbon electrodes with robust mechanical integrity and porous architecture are highly desired for capacitive deionization but remain challenging.Owing to the excellent mechanical strength and electroconductivity,commercial carbon fibers cloth demonstrates great potential as high-performance electrodes for ions storage.Despite this,its direct application on capacitive deionization is rarely reported in terms of limited pore structure and natural hydrophobicity.Herein,a powerful metal-organic framework-engaged structural regulation strategy is developed to boost the desalination properties of carbon fibers.The obtained porous carbon fibers features hierarchical porous structure and hydrophilic surface providing abundant ions-accessible sites,and continuous graphitized carbon core ensuring rapid electrons transport.The catalytic-etching mechanism involving oxidation of Co and subsequent carbonthermal reduction is proposed and highly relies on annealing temperature and holding time.When directly evaluated as a current collector-free capacitive deionization electrode,the porous carbon fibers demonstrates much superior desalination capability than pristine carbon fibers,and remarkable cyclic stability up to 20 h with negligible degeneration.Particularly,the PCF-1000 showcases the highest areal salt adsorption capacity of 0.037 mg cm^(−2) among carbon microfibers.Moreover,monolithic porous carbon fibers-carbon nanotubes with increased active sites and good structural integrity by in-situ growth of carbon nanotubes are further fabricated to enhance the desalination performance(0.051 mg cm^(−2)).This work demonstrates the great potential of carbon fibers in constructing high-efficient and robust monolithic electrode for capacitive deionization.
基金We gratefully acknowledge financial supports from the National Natural Science Foundation of China(No.52202371,51905125,52102364)the Natural Science Foundation of Shandong Province(No.ZR2020QE066)+2 种基金Opening Project of State Key Laboratory of Advanced Technology for Float Glass(No.2020KF08)SDUT&Zibo City Integration Development Project(No.2021SNPT0045)the fellowship of China Postdoctoral Science Foundation(No.2020M672081).
文摘Biomass-derived carbon has demonstrated great potentials as advanced electrode for capacitive deionization(CDI),owing to good electroconductivity,easy availability,intrinsic pores/channels.However,conventional simple pyrolysis of biomass always generates inadequate porosity with limited surface area.Moreover,biomass-derived carbon also suffers from poor wettability and single physical adsorption of ions,resulting in limited desalination performance.Herein,pore structure optimization and element co-doping are integrated on banana peels(BP)-derived carbon to construct hierarchically porous and B,N co-doped carbon with large ions-accessible surface area.A unique expansionactivation(EA)strategy is proposed to modulate the porosity and specific surface area of carbon.Furthermore,B,N co-doping could increase the ions-accessible sites with improved hydrophilicity,and promote ions adsorption.Benefitting from the synergistic effect of hierarchical porosity and B,N co-doping,the resultant electrode manifest enhanced CDI performance for NaCl with large desalination capacity(29.5 mg g^(-1)),high salt adsorption rate(6.2 mg g^(-1)min^(-1)),and versatile adsorption ability for other salts.Density functional theory reveals the enhanced deionization mechanism by pore and B,N co-doping.This work proposes a facile EA strategy for pore structure modulation of biomass-derived carbon,and demonstrates great potentials of integrating pore and heteroatoms-doping on constructing high-performance CDI electrode.
基金supported by the National Natural Science Foundation of China(Grant Nos.51902102,51672059,21805171)the Taishan Scholars Talent Plan(No.ts201511080)+2 种基金the Natural Science Foundation of Hunan Province(Grant No.2020JJ5042)the Natural Science Foundation of Shandong Province(Grant No.ZR2018BB038)the Qiqihar Science and Technology Project(GYGG-201908)。
文摘Non-layered two-dimensional(2 D)carbon complexes manifest great potential in energy-related applications owing to their exotic electronic structures,large electrochemically active surface,and intriguing synergistic effects.However,reliable method for mass production and thickness manipulation of 2 D carbon complexes remains great challenges.Here,inspired by blowing chewing gum into bubbles,a“tailored gel expanding"strategy is proposed for high-yield synthesis of non-layered 2 D carbon complexes with tailored thickness from~12 nm to~1 lm,by controllable pyrolysis of metal-polymeric gel with adequate crosslinking degree.The key feature for thickness manipulation is introducing NH4 NO3 in sol-gel process,which tailors the expansion behavior of gel precursor during subsequent pyrolysis.Various of 2 D sheets with intimately coupled N,O-doped carbon(NOC)and Ni Co-based(Ni Co,(Ni Co)S_(2),(Ni Co)Se_(2),Ni Co_(2)O_(4),(Ni Co)(PO_(3))_(2))nanocrystals are obtained on a large scale and without any impurities.Moreover,these 2 D products are branched with in-situ grown CNTs on the surface,accelerating electrons transfer and preventing the nanosheets from stacking.As a demonstration,the 2 D(Ni Co)S_(2)/NOC with optimized thickness manifests excellent lithium storage properties in both half and full cells.This method paves a new path for massive and controlled production of non-layered 2 D materials with tailored thickness and robust structure stability for energy-related applications.
基金Supported by NSFC (No. 10901043, 10871173, 11026104)
文摘In this paper, we consider a class of Banach space valued singular integrals. The Lp boundedness of these operators has already been obtained. We shall discuss their boundedness from BMO to BMO. As applications, we get BMO boundedness for the classic g-function and the Marcinkiewicz integral. Some known results are improved.
基金the National Natural Science Foundation of China(No.52100060)the Natural Science Foundation of Hubei Province,China(No.2020CFB383)for the financial support。
文摘As persulfate(S_(2)O_(8)^(2-))is being increasingly used as an alternative oxidizing agent,developing lowcost and eco-friendly catalysts for efficient S_(2)O_(8)^(2-)activation is potentially useful for the treatment of wastewater containing refractory organic pollutant.In this study,the degradative features and mechanisms of carbamazepine(CBZ)were systematically investigated in a novel FeS-S_(2)O_(8)^(2-)process under near-neutral conditions.The results exhibited that CBZ can be effectively eliminated by the FeS-S_(2)O_(8)^(2-)process and the optimal conditions were:250 mg/L FeS,0.5 mmol/L S_(2)O_(8)^(2-),and pH=6.0.The existence of Cl^(−)(1 and 50 mmol/L)has little influence on the CBZ elimination,while both HCO_(3)^(−) and HPO_(4)^(2−)(1 and 50 mmol/L)significantly suppressed the CBZ removal in the FeS-S_(2)O_(8)^(2-)process.CBZ could be degraded via a radical mechanism in the FeS-S_(2)O_(8)^(2-)process,the working radical species(i.e.,SO_(4)•−and•OH)were efficiently formed via the promoted decomposition of S_(2)O_(8)^(2-)by the surface Fe2+on the FeS and the dissolved ferrous ions in solution.Based on the identified oxidized products and Fukui index calculations,a possible degradation pathway of CBZ was speculated.More importantly,a two-stage oxidation mechanism of CBZ elimination was speculated in the FeS-S_(2)O_(8)^(2-)process,the activation of S_(2)O_(8)^(2-)by the surface-active Fe(II)of FeS dominated in the initial 5 min,while homogeneous oxidation reactions played more essential parts than others in the following reaction stage(5–60 min).Overall,this study demonstrated that the FeS-S_(2)O_(8)^(2-)process is capable of removing CBZ from water efficiently.
基金the National Natural Science Foundation of China(No.21878116)Natural Science Foundation of Hubei Province(No.2019CFA070)。
文摘Hydrogenation of CO_(2) to value-added chemicals has attracted much attention all through the world.In2 O_(3) with cubic bixbyite-type(denoted as c-In2O_(3))is well known for its high CO_(2) hydrogenation activity and CH3 OH selectivity at high temperature.However,the other structure of In2O_(3) with rhombohedral corundum-type(denoted as rh-In2O_(3))rarely been investigated as catalyst.Herein,c-In2O_(3) and rh-In2O_(3) were prepared and comparatively studied for CO_(2) hydrogenation.The results indicated that c-In2O_(3) showed higher CO_(2) conversion activity than rh-In2O_(3) due to the impressive reducibility and reactivity.Whereas rh-In2O_(3) had higher CH3 OH selectivity due to weaker CH3 OH and stronger CO adsorption on rhIn2O_(3).Although c-In2O_(3) and rh-In2O_(3) catalysts showed different CO_(2) hydrogenation perfo rmance,in-situ diffuse reflectance infrared Fourier transform spectroscopy showed CO_(2) can be reduced to CO through redox cycling and hydrogenation to CH3 OH through formate path.