N-doped TiO2 nanoparticle photocatalysts were prepared through a sol-gel procedure using NH4C1 as the nitrogen source and followed by calcination at certain temperature. Systematic studies for the preparation paramete...N-doped TiO2 nanoparticle photocatalysts were prepared through a sol-gel procedure using NH4C1 as the nitrogen source and followed by calcination at certain temperature. Systematic studies for the preparation parameters and their impact on the structure and photocatalytic activity under ultraviolet （UV） and visible light irra-diation were carried out. Multiple techniques （XRD, TEM, DRIF, DSC, and XPS） were commanded to characterize the crystal structures and chemical binding of N-doped TiO2. Its photocatalytic activity was examined by the deg- radation of organic compounds. The catalytic activity of the prepared N-doped TiO2 nanoparticles under visible light （λ〉400nm） irradiation is evidenced by the decomposition of 4-chlorophenol, showing that nitrogen atoms in the N-doped TiO2 nanoparticle catalyst are responsible for the visible light catalytic activity. The N-doped TiO2 nanoparticle catalyst prepared with this modified route exhibits higher catalytic activity under UV irradiation in contrast to TiO2 without N-doping. It is suggested that the doped nitrogen here is located at the interstitial site of TiO2 lattice.展开更多
The recycling of plastics is a significant global concern.Due to the thermosetting properties of melamineformaldehyde(MF)resin plastics,which make heating and melting difficult,their recycling and reuse pose substanti...The recycling of plastics is a significant global concern.Due to the thermosetting properties of melamineformaldehyde(MF)resin plastics,which make heating and melting difficult,their recycling and reuse pose substantial challenges.In this study,we developed nitrogen-doped(N-doped)carbon materials through scalable carbonization of MF resin plastic waste.This metal-free N-doped carbon catalyst achieved a hydrogen peroxide(H_(2)O_(2))production rate of 971.6 mmol gcatalyst^(-1)h^(-1)with a Faradaic efficiency for H_(2)O_(2)(FEH_(2)O_(2))exceeding 90%under acidic conditions.Additionally,a flow cell utilizing this carbon catalyst demonstrated a production rate of 11.3 mol cm^(-2)h^(-1)(22.5 mol g_(catalyst)^(-1)h^(-1))and maintained a record-high current density of approximately 530 mA cm^(-2)over 300 h.In-situ electrochemical surface-enhanced Raman spectroscopy and density functional theory calculations revealed the presence of porphyrin-like carbon defects,which serve as active sites for the continuous and stable generation of^(*)OOH species.The nitrogen-doped carbon materials obtained from large-scale carbonization of MF plastic waste exhibit abundant active sites,making them highly promising electrocatalysts for the two-electron oxygen reduction reaction(2e^(-)ORR).展开更多
The N-doped TiO2 polycrystalline powder was synthesized through calcining the hydrolysis prodact of tetra-butyl titanate with ammonia. The photocatalytic activity of N-doped TiO2 powder with anatase phone calcined at ...The N-doped TiO2 polycrystalline powder was synthesized through calcining the hydrolysis prodact of tetra-butyl titanate with ammonia. The photocatalytic activity of N-doped TiO2 powder with anatase phone calcined at 400℃ was 2.7 times higher than that of Degussa P25 for phenol decomposition under visible light. All samples had mesoporoas structures. X- ray photoelectron spectroscopy confirmed that a trace amount of N atoms remained in the anatase polycrystaUine TiO2 powder when calcined at 400 ℃ as substitutional atoms at the oxygen sites. UV-Vis and EPR analyses indicated that oxygen vacancy states were created during the course of N-doped TiO2 powder formation. It is considered that substitutional N atoms, oxygen vacancy, states, large BET surface areas and mesoporoas structure are important facwrs for the N-doped photocatalyst to present a high vis-activity.展开更多
The steel industry produces many byproducts, requiring extensive land for storage and causing significant environmental contamination. Industrial effluents discharged into water bodies negatively impact both aquatic e...The steel industry produces many byproducts, requiring extensive land for storage and causing significant environmental contamination. Industrial effluents discharged into water bodies negatively impact both aquatic ecosystems and human health. To solve this problem, this study synthesized a composite of titanium dioxide (TiO2) and steel slag nanocomposites (SSNC) at a 1:2 mass ratio to create a robust photocatalyst for the treatment of synthetic wastewater. The efficacy of this catalyst in degrading various dye pollutants, including methylene blue (MB), was tested under simulated solar light conditions. Comprehensive analyses were conducted to assess the physical and chemical characteristics, crystalline structure, energy gap, and point of zero charge of the composite. The TiO2-SSNC composite catalyst exhibited excellent stability, with a point of zero charge at 8.342 and an energy gap of 2.4 eV. The degradation process conformed to pseudo-first-order kinetics. Optimization of operational parameters was achieved through the response surface methodology. Reusability tests demonstrated that the TiO2-SSNC composite catalyst effectively degraded up to 93.41% of MB in the suspended mode and 92.03% in the coated mode after five cycles. Additionally, the degradation efficiencies for various dyes were significant, highlighting the potential of the composite for broad applications in industrial wastewater treatment. This study also explored the degradation mechanisms and identified byproducts, establishing a pathway for contaminant breakdown. The cost-benefit analysis revealed a total cost of 0.842 8 USD per cubic meter for each treatment activity, indicating low operational and production costs. These findings underscore the promise of the TiO2-SSNC composite as a cost-effective and efficient alternative for wastewater purification.展开更多
Synergistic interplays involving multiple active centers originating from TiO2 nanotube layers(TNT)and ruthenium(Ru)species comprising of both single atoms(SAs)and nanoparticles(NPs)augment the alkaline hydrogen evolu...Synergistic interplays involving multiple active centers originating from TiO2 nanotube layers(TNT)and ruthenium(Ru)species comprising of both single atoms(SAs)and nanoparticles(NPs)augment the alkaline hydrogen evolution reaction(HER)by enhancing Volmer kinetics from rapid water dissociation and improving Tafel kinetics from efficient H*desorption.Atomic layer deposition of Ru with 50 process cycles results in a mixture of Ru SAs and 2.8-0.4 nm NPs present on TNT layers,and it emerges with the highest HER activity among all the electrodes synthesized.A detailed study of the Ti and Ru species using different high-resolution techniques confirmed the presence of Ti^(3+)states and the coexistence of Ru SAs and NPs.With insights from literature,the role of Ti^(3+),appropriate work functions of TNT layers and Ru,and the synergistic effect of Ru SAs and Ru NPs in improving the performance of alkaline HER were elaborated and justified.The aforementioned characteristics led to a remarkable performance by having 9mV onset potentials and 33 mV dec^(-1) of Tafel slopes and a higher turnover frequency of 1.72 H2 s^(-1) at 30 mV.Besides,a notable stability from 28 h staircase chronopotentiometric measurements for TNT@Ru surpasses TNT@Pt in comparison.展开更多
Controllable synthesis of insertion-type anode materials with beneficial micro-and nanostructures is a promising approach for the synthesis of sodium-ion storage devices with high-reactivity and excellent electrochemi...Controllable synthesis of insertion-type anode materials with beneficial micro-and nanostructures is a promising approach for the synthesis of sodium-ion storage devices with high-reactivity and excellent electrochemical performance.In this study,we developed a sacrificial-templating route to synthesize TiO_(2)@N-doped carbon nanotubes(TiO_(2)@NC-NTs)with excellent electrochemical performance.The asprepared mesoporous TiO_(2)@NC-NTs with tiny nanocrystals of anatase TiO_(2) wrapped in N-doped carbon layers showed a well-defined tube structure with a large specific surface area of 198 m^(2) g^(-1) and a large pore size of~5 nm.The TiO_(2)@NC-NTs delivered high reversible capacities of 158 m A h g^(-1) at 2 C(1 C=335 m A g^(-1))for 2200 cycles and 146 m A h g^(-1) at 5 C for 4000 cycles,as well as an ultrahigh rate capability of up to 40 C with a capacity of 98 m A h g^(-1).Even at a high current density of 10 C,a capacity of 138 m A h g^(-1) could be delivered over 10,000 cycles.Thus,the synthesis of mesoporous TiO_(2)@NC-NTs was demonstrated to be an efficient approach for developing electrode materials with high sodium storage and long cycle life.展开更多
Nitrogen-doped carbon nanotubes （NCNTs） were used as a support for iron （Fe） nanoparticles applied in car- bon dioxide （CO_2） hydrogenation at 633 K and 25 bar （1 bar = 10-5 Pa）. The Fe/NCNT catalyst promoted ...Nitrogen-doped carbon nanotubes （NCNTs） were used as a support for iron （Fe） nanoparticles applied in car- bon dioxide （CO_2） hydrogenation at 633 K and 25 bar （1 bar = 10-5 Pa）. The Fe/NCNT catalyst promoted with both potassium （K） and manganese （Mn） showed high performance in CO_2 hydrogenation, reaching 34.9% conversion with a gas hourly space velocity （GHSV） of 3.1 L-（g·h）-1. Product selectivities were high for olefin products and low for short-chain alkanes for the K-promoted catalysts. When Fe/NCNT catalyst was promot- ed with both K and Mn, the catalytic activity was stable for 60 h of reaction time. The structural effect of the Mn promoter was demonstrated by X-ray diffraction （XRD）, temperature-programmed reduction （TPR） with molecular hydrogen （H2）, and in situ X-ray absorption near-edge structure （XANES） analysis. The Mn pro- moter stabilized wtistite （FeO） as an intermediate and lowered the TPR onset temperature. Catalytic ammo- nia （NH_3） decomposition was used as an additional probe reaction for characterizing the promoter effects. The Fe/NCNT catalyst promoted with both K and Mn had the highest catalytic activity, and the Mn-promoted Fe/NCNT catalysts had the highest thermal stability under reducing conditions.展开更多
Synthesis of spherical carbon beads with effective CO_2 capture capability is highly desirable for large scale application of CO2 sorption, but remains challenging. Herein, a facile and efficient strategy to prepare n...Synthesis of spherical carbon beads with effective CO_2 capture capability is highly desirable for large scale application of CO2 sorption, but remains challenging. Herein, a facile and efficient strategy to prepare nitrogen-doped hierarchically porous carbon spheres was developed via co-pyrolyzation of poly(vinylidene chloride) and melamine in alginate gel beads. In this approach, melamine not only serves as the nitrogen precursor, but also acts as a template for the macropores structures. The nitrogen contents in the hierarchically porous carbon spheres reach a high level, ranging from 11.8 wt% to 14.7 wt%, as the melamine amount increases. Owing to the enriched nitrogen functionalities and the special hierarchical porous structure, the carbon spheres exhibit an outstanding CO_2 capture performance, with the dynamic capacity of as much as about 7 wt% and a separation factor about 49 at 25 °C in a gas mixture of CO_2/N_2(0.5:99.5, v/v).展开更多
Additive Ba（N3）2 as a source of nitrogen is heavily doped into the graphite-Fe-based alloy system to grow nitrogendoped diamond crystals under a relatively high pressure （about 6.0 GPa） by employing the temperatur...Additive Ba（N3）2 as a source of nitrogen is heavily doped into the graphite-Fe-based alloy system to grow nitrogendoped diamond crystals under a relatively high pressure （about 6.0 GPa） by employing the temperature gradient method. Gem-grade diamond crystal with a size of around 5 mm and a nitrogen concentration of about 1173 ppm is successfully synthesised for the first time under high pressure and high temperature in a China-type cubic anvil highpressure apparatus. The growth habit of diamond crystal under the environment with high degree of nitrogen doping is investigated. It is found that the morphologies of heavily nitrogen-doped diamond crystals are all of octahedral shape dominated by {111} facets. The effects of temperature and duration on nitrogen concentration and form are explored by infrared absorption spectra. The results indicate that nitrogen impurity is present in diamond predominantly in the dispersed form accompanied by aggregated form, and the aggregated nitrogen concentration in diamond increases with temperature and duration. In addition, it is indicated that nitrogen donors are more easily incorporated into growing crystals at higher temperature. Strains in nitrogen-doped diamond crystal are characterized by micro-Raman spectroscopy. Measurement results demonstrate that the undoped diamond crystals exhibit the compressive stress, whereas diamond crystals heavily doped with the addition of Ba（N3）2 display the tensile stress.展开更多
The metal oxide/nitrogen-doped carbon(NC)compounds zirconium oxide/NC(ZrO_(2)/NC)and cerium oxide/NC(CeO_(2)/NC)were synthesized via the pyrolysis of polyaniline on the metal oxide surface.The characterization of the ...The metal oxide/nitrogen-doped carbon(NC)compounds zirconium oxide/NC(ZrO_(2)/NC)and cerium oxide/NC(CeO_(2)/NC)were synthesized via the pyrolysis of polyaniline on the metal oxide surface.The characterization of the ZrO_(2)/NC and CeO_(2)/NC catalysts showed more active CO_(2) reduction reaction activity than that of NC catalyst without metal oxide.Gas chromatography analysis revealed that CO and H_(2)were the primary products,and no liquid-phase products were detected via proton nuclear magnetic resonance spectroscopy or high-performance liquid chromatography.The maximum Faraday effi ciency of ZrO_(2)/NC reached 90%at−0.73 V(vs.RHE),with the current density of CO at 5.5 mA/cm^(2);this Faraday effi ciency value was higher than that of NC(41%),with the current density of CO at 3.1 mA/cm^(2).The interaction between the metal oxide and carbon allowed the effi cient formation of defect sites,especially imine-type nitrogen,strengthening the adsorption of the key reaction intermediate CO_(2)^(•−) and thus promoting the CO_(2) reduction reaction.展开更多
A nitrogen-doped titanium dioxide composite photocatalyst（N–TiO2） with heterojunction structures is synthesized by three different approaches： a novel UV-assisted thermal synthesis, annealing, and microwave techni...A nitrogen-doped titanium dioxide composite photocatalyst（N–TiO2） with heterojunction structures is synthesized by three different approaches： a novel UV-assisted thermal synthesis, annealing, and microwave technique. Photocatalytic activities of synthesized photocatalysts are evaluated by the degradation of Methyl Orange under ultraviolet light types A（UV-A）, B（UV-B）, and C（UV-C）, visible light, and direct sunlight irradiation. Results show that by using N–TiO_2 photocatalyst prepared by the UV-assisted thermal synthesis and annealing, the degradation increases by 16.5% and 20.4%, respectively, compared to that by bare TiO2. The best results are obtained at a nitrogen to TiO2 mass ratio of 0.15（N：TiO2）. The enhancement of the photocatalytic activity observed in the visible range is mainly attributed to the increasing separation rate of photogenerated charge carriers. The novel UV-assisted thermal synthesis has produced encouraging results as a preparation method for the nitrogen-doped TiO2 photocatalyst; thus, further studies are recommended for process optimization, immobilization, and scale-up to evaluate its applicability in wastewater treatment.展开更多
基金Supported by the Science and Technology Research Program of Chongqing Education Commission （KJ050702）, and the Natural Science Foundation Project of Chongqing Science and Technology（Commission （No.2007BB7208）.
文摘N-doped TiO2 nanoparticle photocatalysts were prepared through a sol-gel procedure using NH4C1 as the nitrogen source and followed by calcination at certain temperature. Systematic studies for the preparation parameters and their impact on the structure and photocatalytic activity under ultraviolet （UV） and visible light irra-diation were carried out. Multiple techniques （XRD, TEM, DRIF, DSC, and XPS） were commanded to characterize the crystal structures and chemical binding of N-doped TiO2. Its photocatalytic activity was examined by the deg- radation of organic compounds. The catalytic activity of the prepared N-doped TiO2 nanoparticles under visible light （λ〉400nm） irradiation is evidenced by the decomposition of 4-chlorophenol, showing that nitrogen atoms in the N-doped TiO2 nanoparticle catalyst are responsible for the visible light catalytic activity. The N-doped TiO2 nanoparticle catalyst prepared with this modified route exhibits higher catalytic activity under UV irradiation in contrast to TiO2 without N-doping. It is suggested that the doped nitrogen here is located at the interstitial site of TiO2 lattice.
基金supported by the National Natural Science Foundation of China(Grant No.22276123,22025505)the Oceanic Interdisciplinary Program of Shanghai Jiao Tong University(SL2022ZD105)State Key Lab of Metal Matrix Composite。
文摘The recycling of plastics is a significant global concern.Due to the thermosetting properties of melamineformaldehyde(MF)resin plastics,which make heating and melting difficult,their recycling and reuse pose substantial challenges.In this study,we developed nitrogen-doped(N-doped)carbon materials through scalable carbonization of MF resin plastic waste.This metal-free N-doped carbon catalyst achieved a hydrogen peroxide(H_(2)O_(2))production rate of 971.6 mmol gcatalyst^(-1)h^(-1)with a Faradaic efficiency for H_(2)O_(2)(FEH_(2)O_(2))exceeding 90%under acidic conditions.Additionally,a flow cell utilizing this carbon catalyst demonstrated a production rate of 11.3 mol cm^(-2)h^(-1)(22.5 mol g_(catalyst)^(-1)h^(-1))and maintained a record-high current density of approximately 530 mA cm^(-2)over 300 h.In-situ electrochemical surface-enhanced Raman spectroscopy and density functional theory calculations revealed the presence of porphyrin-like carbon defects,which serve as active sites for the continuous and stable generation of^(*)OOH species.The nitrogen-doped carbon materials obtained from large-scale carbonization of MF plastic waste exhibit abundant active sites,making them highly promising electrocatalysts for the two-electron oxygen reduction reaction(2e^(-)ORR).
基金Funded by National "973"Plan Research Project ( No.2004CB619204)and Educational Ministry Scientific and Technologi-cal Research Key Project(No.02052)
文摘The N-doped TiO2 polycrystalline powder was synthesized through calcining the hydrolysis prodact of tetra-butyl titanate with ammonia. The photocatalytic activity of N-doped TiO2 powder with anatase phone calcined at 400℃ was 2.7 times higher than that of Degussa P25 for phenol decomposition under visible light. All samples had mesoporoas structures. X- ray photoelectron spectroscopy confirmed that a trace amount of N atoms remained in the anatase polycrystaUine TiO2 powder when calcined at 400 ℃ as substitutional atoms at the oxygen sites. UV-Vis and EPR analyses indicated that oxygen vacancy states were created during the course of N-doped TiO2 powder formation. It is considered that substitutional N atoms, oxygen vacancy, states, large BET surface areas and mesoporoas structure are important facwrs for the N-doped photocatalyst to present a high vis-activity.
基金supported by the Department of Chemical and Petrochemical Engineering,Egypt-Japan University of Science and Technology.
文摘The steel industry produces many byproducts, requiring extensive land for storage and causing significant environmental contamination. Industrial effluents discharged into water bodies negatively impact both aquatic ecosystems and human health. To solve this problem, this study synthesized a composite of titanium dioxide (TiO2) and steel slag nanocomposites (SSNC) at a 1:2 mass ratio to create a robust photocatalyst for the treatment of synthetic wastewater. The efficacy of this catalyst in degrading various dye pollutants, including methylene blue (MB), was tested under simulated solar light conditions. Comprehensive analyses were conducted to assess the physical and chemical characteristics, crystalline structure, energy gap, and point of zero charge of the composite. The TiO2-SSNC composite catalyst exhibited excellent stability, with a point of zero charge at 8.342 and an energy gap of 2.4 eV. The degradation process conformed to pseudo-first-order kinetics. Optimization of operational parameters was achieved through the response surface methodology. Reusability tests demonstrated that the TiO2-SSNC composite catalyst effectively degraded up to 93.41% of MB in the suspended mode and 92.03% in the coated mode after five cycles. Additionally, the degradation efficiencies for various dyes were significant, highlighting the potential of the composite for broad applications in industrial wastewater treatment. This study also explored the degradation mechanisms and identified byproducts, establishing a pathway for contaminant breakdown. The cost-benefit analysis revealed a total cost of 0.842 8 USD per cubic meter for each treatment activity, indicating low operational and production costs. These findings underscore the promise of the TiO2-SSNC composite as a cost-effective and efficient alternative for wastewater purification.
基金support from the European Union Horizon 2020 program(project HERMES,nr.952184)the Ministry of Education,Youth and Sports of the Czech Republic for supporting CEMNAT(LM2023037)+1 种基金Czech-NanoLab(LM2023051)infrastructures for providing ALD,SEM,EDX,XPS,TEM,and XRDCzech Science Foundation(project 23-08019X,EXPRO).
文摘Synergistic interplays involving multiple active centers originating from TiO2 nanotube layers(TNT)and ruthenium(Ru)species comprising of both single atoms(SAs)and nanoparticles(NPs)augment the alkaline hydrogen evolution reaction(HER)by enhancing Volmer kinetics from rapid water dissociation and improving Tafel kinetics from efficient H*desorption.Atomic layer deposition of Ru with 50 process cycles results in a mixture of Ru SAs and 2.8-0.4 nm NPs present on TNT layers,and it emerges with the highest HER activity among all the electrodes synthesized.A detailed study of the Ti and Ru species using different high-resolution techniques confirmed the presence of Ti^(3+)states and the coexistence of Ru SAs and NPs.With insights from literature,the role of Ti^(3+),appropriate work functions of TNT layers and Ru,and the synergistic effect of Ru SAs and Ru NPs in improving the performance of alkaline HER were elaborated and justified.The aforementioned characteristics led to a remarkable performance by having 9mV onset potentials and 33 mV dec^(-1) of Tafel slopes and a higher turnover frequency of 1.72 H2 s^(-1) at 30 mV.Besides,a notable stability from 28 h staircase chronopotentiometric measurements for TNT@Ru surpasses TNT@Pt in comparison.
基金the financial support provided by internal reseach funding of Khalifa University of Science and Technology,United Arab Emirates(Grant No.CIRA-2018-16)。
文摘Controllable synthesis of insertion-type anode materials with beneficial micro-and nanostructures is a promising approach for the synthesis of sodium-ion storage devices with high-reactivity and excellent electrochemical performance.In this study,we developed a sacrificial-templating route to synthesize TiO_(2)@N-doped carbon nanotubes(TiO_(2)@NC-NTs)with excellent electrochemical performance.The asprepared mesoporous TiO_(2)@NC-NTs with tiny nanocrystals of anatase TiO_(2) wrapped in N-doped carbon layers showed a well-defined tube structure with a large specific surface area of 198 m^(2) g^(-1) and a large pore size of~5 nm.The TiO_(2)@NC-NTs delivered high reversible capacities of 158 m A h g^(-1) at 2 C(1 C=335 m A g^(-1))for 2200 cycles and 146 m A h g^(-1) at 5 C for 4000 cycles,as well as an ultrahigh rate capability of up to 40 C with a capacity of 98 m A h g^(-1).Even at a high current density of 10 C,a capacity of 138 m A h g^(-1) could be delivered over 10,000 cycles.Thus,the synthesis of mesoporous TiO_(2)@NC-NTs was demonstrated to be an efficient approach for developing electrode materials with high sodium storage and long cycle life.
基金supported by the Synchrotron Light Research Institute(Public Organization)Thailand(GS-54-D01)+7 种基金the Commission on Higher EducationMinistry of EducationThailandperformed under the project"Sustainable Chemical Synthesis(Sus Chem Sys)"which is co-financed by the European Regional Development Fund(ERDF)the state of North Rhine-WestphaliaGermanyunder the Operational Programme"Regional Competitiveness and Employment"2007–2013
文摘Nitrogen-doped carbon nanotubes （NCNTs） were used as a support for iron （Fe） nanoparticles applied in car- bon dioxide （CO_2） hydrogenation at 633 K and 25 bar （1 bar = 10-5 Pa）. The Fe/NCNT catalyst promoted with both potassium （K） and manganese （Mn） showed high performance in CO_2 hydrogenation, reaching 34.9% conversion with a gas hourly space velocity （GHSV） of 3.1 L-（g·h）-1. Product selectivities were high for olefin products and low for short-chain alkanes for the K-promoted catalysts. When Fe/NCNT catalyst was promot- ed with both K and Mn, the catalytic activity was stable for 60 h of reaction time. The structural effect of the Mn promoter was demonstrated by X-ray diffraction （XRD）, temperature-programmed reduction （TPR） with molecular hydrogen （H2）, and in situ X-ray absorption near-edge structure （XANES） analysis. The Mn pro- moter stabilized wtistite （FeO） as an intermediate and lowered the TPR onset temperature. Catalytic ammo- nia （NH_3） decomposition was used as an additional probe reaction for characterizing the promoter effects. The Fe/NCNT catalyst promoted with both K and Mn had the highest catalytic activity, and the Mn-promoted Fe/NCNT catalysts had the highest thermal stability under reducing conditions.
基金supported by the National Key R&D Program of China (2016YFB0600902)the Dalian National Laboratory for Clean Energy (DNL180401)the National Natural Science Foundation of China (21925803)。
文摘Synthesis of spherical carbon beads with effective CO_2 capture capability is highly desirable for large scale application of CO2 sorption, but remains challenging. Herein, a facile and efficient strategy to prepare nitrogen-doped hierarchically porous carbon spheres was developed via co-pyrolyzation of poly(vinylidene chloride) and melamine in alginate gel beads. In this approach, melamine not only serves as the nitrogen precursor, but also acts as a template for the macropores structures. The nitrogen contents in the hierarchically porous carbon spheres reach a high level, ranging from 11.8 wt% to 14.7 wt%, as the melamine amount increases. Owing to the enriched nitrogen functionalities and the special hierarchical porous structure, the carbon spheres exhibit an outstanding CO_2 capture performance, with the dynamic capacity of as much as about 7 wt% and a separation factor about 49 at 25 °C in a gas mixture of CO_2/N_2(0.5:99.5, v/v).
基金Project supported by the National Natural Science Foundation of China (Grant No.50572032)
文摘Additive Ba（N3）2 as a source of nitrogen is heavily doped into the graphite-Fe-based alloy system to grow nitrogendoped diamond crystals under a relatively high pressure （about 6.0 GPa） by employing the temperature gradient method. Gem-grade diamond crystal with a size of around 5 mm and a nitrogen concentration of about 1173 ppm is successfully synthesised for the first time under high pressure and high temperature in a China-type cubic anvil highpressure apparatus. The growth habit of diamond crystal under the environment with high degree of nitrogen doping is investigated. It is found that the morphologies of heavily nitrogen-doped diamond crystals are all of octahedral shape dominated by {111} facets. The effects of temperature and duration on nitrogen concentration and form are explored by infrared absorption spectra. The results indicate that nitrogen impurity is present in diamond predominantly in the dispersed form accompanied by aggregated form, and the aggregated nitrogen concentration in diamond increases with temperature and duration. In addition, it is indicated that nitrogen donors are more easily incorporated into growing crystals at higher temperature. Strains in nitrogen-doped diamond crystal are characterized by micro-Raman spectroscopy. Measurement results demonstrate that the undoped diamond crystals exhibit the compressive stress, whereas diamond crystals heavily doped with the addition of Ba（N3）2 display the tensile stress.
基金The work was supported by the National Key R&D Program of China(No.2016YFB0600901)Changyi Hydrogen Industrial Technology Fund.
文摘The metal oxide/nitrogen-doped carbon(NC)compounds zirconium oxide/NC(ZrO_(2)/NC)and cerium oxide/NC(CeO_(2)/NC)were synthesized via the pyrolysis of polyaniline on the metal oxide surface.The characterization of the ZrO_(2)/NC and CeO_(2)/NC catalysts showed more active CO_(2) reduction reaction activity than that of NC catalyst without metal oxide.Gas chromatography analysis revealed that CO and H_(2)were the primary products,and no liquid-phase products were detected via proton nuclear magnetic resonance spectroscopy or high-performance liquid chromatography.The maximum Faraday effi ciency of ZrO_(2)/NC reached 90%at−0.73 V(vs.RHE),with the current density of CO at 5.5 mA/cm^(2);this Faraday effi ciency value was higher than that of NC(41%),with the current density of CO at 3.1 mA/cm^(2).The interaction between the metal oxide and carbon allowed the effi cient formation of defect sites,especially imine-type nitrogen,strengthening the adsorption of the key reaction intermediate CO_(2)^(•−) and thus promoting the CO_(2) reduction reaction.
基金The financial support of Natural Sciences and Engineering Research Council of Canada (NSERC)Ontario Graduate Scholarship (OGS) programRyerson University is greatly appreciated
文摘A nitrogen-doped titanium dioxide composite photocatalyst（N–TiO2） with heterojunction structures is synthesized by three different approaches： a novel UV-assisted thermal synthesis, annealing, and microwave technique. Photocatalytic activities of synthesized photocatalysts are evaluated by the degradation of Methyl Orange under ultraviolet light types A（UV-A）, B（UV-B）, and C（UV-C）, visible light, and direct sunlight irradiation. Results show that by using N–TiO_2 photocatalyst prepared by the UV-assisted thermal synthesis and annealing, the degradation increases by 16.5% and 20.4%, respectively, compared to that by bare TiO2. The best results are obtained at a nitrogen to TiO2 mass ratio of 0.15（N：TiO2）. The enhancement of the photocatalytic activity observed in the visible range is mainly attributed to the increasing separation rate of photogenerated charge carriers. The novel UV-assisted thermal synthesis has produced encouraging results as a preparation method for the nitrogen-doped TiO2 photocatalyst; thus, further studies are recommended for process optimization, immobilization, and scale-up to evaluate its applicability in wastewater treatment.
