Carbon nanotubes(CNTs)have been far and wide employed as the counter electrodes(CEs)in dyesensitized solar cells because of their individual physical and chemical properties.However,the techniques available now,such a...Carbon nanotubes(CNTs)have been far and wide employed as the counter electrodes(CEs)in dyesensitized solar cells because of their individual physical and chemical properties.However,the techniques available now,such as chemical vapor deposition,arc discharge and laser ablation for synthesizing CNTs,commonly suffer from rigorous operations and complicated steps,which make the process difficult to be controlled.Herein,we present a simple and facile glutamic acid-assisted hydrothermal recrystallization strategy to construct bamboo-like CNTs(GHP-BC-x).Generally,the conventional organic dye3,4,9,10-perylene tetracarboxylic dianhydride(PTCDA)is used as a precursor and glutamic acid efficiently promotes the recrystallization of the perylene cores'planarπ-conjugated system in PTCDA under hydrothermal conditions and then self-assembles into one-dimensio nal nano rods with improved crystallization degree,finally resulting in the morphology of bamboo-like CNTs after carbonization.When applied as the counter electrodes,the GHP-BC-3 displays a remarkable power conversion efficiency of8.25%,benefiting from the superb electrical conductivity and mass transfer dynamics,superior to that of Pt CE(7.62%).展开更多
A molecular structural mechanics approach combining with finite element analysis(MSM/FEA) was applied to study the microstructure and tensile behaviors of bamboo-like carbon nanotubes(BCNTs). The mathematical model of...A molecular structural mechanics approach combining with finite element analysis(MSM/FEA) was applied to study the microstructure and tensile behaviors of bamboo-like carbon nanotubes(BCNTs). The mathematical model of tensile behaviors of BCNTs was established based on molecular structural mechanics theory. The deformations of BCNTs, with different diameters and compartments set based on the experimental investigation on BCNT structures synthesized by chemical vapor depositon, under tensile load, were analyzed with ANSYS programmed. Results show that the BCNTs have good tensile properties, and those Young's modulus can reach 0.84 Tpa. Through the analysis, it can be found that the Young's modulus of BCNTs depends on the diameters and the length of compartment, which is in good agreement with our experimental tests for the tensile performances of individual BCNT.展开更多
Electrochemical cyclic voltammetric（CV） scan was applied to inducing the partial oxidation and defects of carbon nanotubes（CNTs）.The electrochemically induced functional groups and physical defects were demonstrat...Electrochemical cyclic voltammetric（CV） scan was applied to inducing the partial oxidation and defects of carbon nanotubes（CNTs）.The electrochemically induced functional groups and physical defects were demonstrated to show positive effects on the nanotube capacitance,as exemplified by super-long CNT arrays as model for the easy fabrication of CNT electrodes.Specifically,the initial hydrophobic nanotube surface becomes hydrophilic and a ten-time enhancement in capacitance is observed with respect to the pristine CNT sample.Thus,the electrochemical CV pretreatment can be used as an effective approach to activate the CNT surface for an enhanced electrochemical performance in capacitors,and many other advanced devices beyond capacitors,such as electrochemical sensors and batteries.展开更多
Bamboo-like nitrogen-doped carbon（CNx） nanotubes were synthesized by chemical vapor deposition （CVD） at a high reaction temperature of 600―900 °C. The butylamine and Fe/SBA-15 molecular sieve have been used ...Bamboo-like nitrogen-doped carbon（CNx） nanotubes were synthesized by chemical vapor deposition （CVD） at a high reaction temperature of 600―900 °C. The butylamine and Fe/SBA-15 molecular sieve have been used as precursor and catalyst, respectively. Transmission electron microscopy（TEM） and high resolution transmission electron microscopy（HRTEM） observations show that the outer diameter and wall thickness as well as the inner diameter were increased with increasing reaction temperature in a temperature range of 600―800 °C. A synergism mechanism of the growth through bulk diffusion and the competitive growth through surface diffusion functions during the synthesis of CNx nanotubes was proposed.展开更多
Carbon nanotubes （CNTs） were prepared using different carrier gases, with ferrocene as the catalyst precusor and acetylene as the carbon source. The effects of ammonia and nitrogen as carrier gases on the structure ...Carbon nanotubes （CNTs） were prepared using different carrier gases, with ferrocene as the catalyst precusor and acetylene as the carbon source. The effects of ammonia and nitrogen as carrier gases on the structure and morphology of CNTs were investigated. Transmission electron microscope （TEM）, high-resolution electron microscope （HRTEM）, scanning electron microscope （SEM） and X-ray diffraction （XRD） were employed to characterize the products and the catalyst. Experiment results show that the CNTs grown in N2 gas exhibited cylindrical and tubular structure, while a bamboo-like structure was observed for the CNTs grown in NH3 gas. Moreover, vertically aligned CNTs were obtained on an A12O3 disk when NH3 was used as the carrier gas. The carrier gas also exerted influence on the shape of the catalyst. Based on the theory of active centers of catalysis and combined with the particle shape of the catalyst, a growth model for the vertically aligned CNTs on the substrate is given.展开更多
Interfacial atomic configuration between dual-metal active species and nitrogen-carbon substrates is of great importance for improving the intrinsic activity of catalysts toward oxygen reduction reaction(ORR).Thus,fro...Interfacial atomic configuration between dual-metal active species and nitrogen-carbon substrates is of great importance for improving the intrinsic activity of catalysts toward oxygen reduction reaction(ORR).Thus,from the atomic-scale engineering we develop a high intrinsic activity ORR catalyst in terms of incorporating atomically dispersed dual Fe centers(single Fe atoms and ultra-small Fe atomic clusters)into bamboo-like N-doped carbon nanotubes.Benefiting from atomically dispersed dual-Fe centers on the atomic interface of Fe-Nx/carbon nanotubes,the fabricated dual Fe centers catalyst exhibits an extremely high ORR activity(E_(onset)=1.006 V;E_(1/2)=0.90 V),beyond state-of-the-art Pt/C.Remarkably,this catalyst also shows a superior kinetic current density of 19.690 mA·cm^(−2),which is 7 times that of state-of-the-art Pt/C.Additionally,based on the excellent catalyst,the primary Zn-air battery reveals a high power density up to 137 mW·cm^(−2) and sufficient potential cycling stability(at least 25 h).Undoubtedly,given the unique structure–activity relationship of dual-Fe active species and metal-nitrogen-carbon substrates,the catalyst will show great prospects in highly efficient electrochemical energy conversion devices.展开更多
Very long and open aligned carbon nanotubes that reach about 2 mm long, an order of magnitude longer than previously reached, have been prepared by chemical vapor deposition over silica dioxide substrates on the surfa...Very long and open aligned carbon nanotubes that reach about 2 mm long, an order of magnitude longer than previously reached, have been prepared by chemical vapor deposition over silica dioxide substrates on the surface, where iron/silica nano-composite particles are evenly positioned. The nanotubes are naturally opened at the bottom ends. The growth mechanism of the very long and open-ended nanotubes is also discussed.展开更多
Aqueous rechargeable zinc-ion battery(ZIB)is considered to be a potential energy storage system for large-scale applications due to its environmental friendliness,high safety,and low cost.However,it remains challengin...Aqueous rechargeable zinc-ion battery(ZIB)is considered to be a potential energy storage system for large-scale applications due to its environmental friendliness,high safety,and low cost.However,it remains challenging to develop suitable cathode materials with high specific capacity and long-term cyclic stability.Herein,we have fabricated freestanding Sr0.19V2O51.3H2O/carbon nanotubes(SrVO/CNTs)composite films with different mass ratios by incorporating SrVO into CNTs network.The synthesized SrVO possesses a large interlayer spacing of 1.31 nm,which facilitates Zn(2+)diffusion.Furthermore,the SrVO/CNTs composite film with conductive network structure promotes electron transfer and ensures good contact between SrVO and CNTs during the long-term cycling process.As a result,the battery based on the SrVO/CNTs composite cathode with a mass ratio of 7:3 delivers a specific capacity of 326 mAh·g^(-1)at 0.1 A·g^(-1)and 145 mAh·g^(-1)at 5 A·g^(-1),demonstrating a high capacity and excellent rate capability.Remarkably,the assembled ZIB shows good capacity retention of 91%even after ultra-long cycling for 7500 cycles at a high current rate of 5 Ag^(-1).More importantly,the battery also delivers a high energy density and power density,as 290 Wh·kg^(-1)at 125 W·kg^(-1)(0.1 A·g^(-1)),or 115 Wh·kg^(-1)at 6078 W·kg^(-1)(5 Ag^(-1)).The results demonstrate that the SrVO/CNTs composite is a promising cathode toward large-scale energy storage applications.展开更多
Efficient selective oxidation of hydrocarbons to corresponding ketones has been a significant but challenging work in the past decades.Here,a nitrogen-doped bamboo-like carbon nanotubes encapsulating cobalt catalyst(N...Efficient selective oxidation of hydrocarbons to corresponding ketones has been a significant but challenging work in the past decades.Here,a nitrogen-doped bamboo-like carbon nanotubes encapsulating cobalt catalyst(NCNTs-X)using citric acid,melamine and CoCl_(2)·6H_(2)O as precursors was synthesized by a simple pyrolysis method.A series of characterization techniques were employed to investigate the physicochemical properties of samples.And the results show that the as-prepared catalysts achieve a high catalytic performance for selective ethylbenzene oxidation(78.3% ethylbenzene conversion)using molecular oxygen as oxidant,especially giving a high selectivity(93.8% selectivity to acetophenone).According to the investigation of the structure-activity relationship of the catalysts,it can be deduced that the Co-N_(x) sites have an obvious positive effect on catalytic performance thanks to the synergistic effect between metallic cobalt and pyridinic N.展开更多
基金partly supported by the National Natural Science Foundation of China(51872035 and 22078052)Talent Program of Rejuvenation of the Liaoning(XLYC1807002)Innovation Program of Dalian City(2019RJ03)。
文摘Carbon nanotubes(CNTs)have been far and wide employed as the counter electrodes(CEs)in dyesensitized solar cells because of their individual physical and chemical properties.However,the techniques available now,such as chemical vapor deposition,arc discharge and laser ablation for synthesizing CNTs,commonly suffer from rigorous operations and complicated steps,which make the process difficult to be controlled.Herein,we present a simple and facile glutamic acid-assisted hydrothermal recrystallization strategy to construct bamboo-like CNTs(GHP-BC-x).Generally,the conventional organic dye3,4,9,10-perylene tetracarboxylic dianhydride(PTCDA)is used as a precursor and glutamic acid efficiently promotes the recrystallization of the perylene cores'planarπ-conjugated system in PTCDA under hydrothermal conditions and then self-assembles into one-dimensio nal nano rods with improved crystallization degree,finally resulting in the morphology of bamboo-like CNTs after carbonization.When applied as the counter electrodes,the GHP-BC-3 displays a remarkable power conversion efficiency of8.25%,benefiting from the superb electrical conductivity and mass transfer dynamics,superior to that of Pt CE(7.62%).
基金Funded by the National Natural Science Foundation of China(Nos.51472203,51221001,U1435202)
文摘A molecular structural mechanics approach combining with finite element analysis(MSM/FEA) was applied to study the microstructure and tensile behaviors of bamboo-like carbon nanotubes(BCNTs). The mathematical model of tensile behaviors of BCNTs was established based on molecular structural mechanics theory. The deformations of BCNTs, with different diameters and compartments set based on the experimental investigation on BCNT structures synthesized by chemical vapor depositon, under tensile load, were analyzed with ANSYS programmed. Results show that the BCNTs have good tensile properties, and those Young's modulus can reach 0.84 Tpa. Through the analysis, it can be found that the Young's modulus of BCNTs depends on the diameters and the length of compartment, which is in good agreement with our experimental tests for the tensile performances of individual BCNT.
基金Supported by the Scientific Research Foundation for the Returned Overseas Chinese Scholars,Ministry of Education of China(No.20100732002)the National Natural Science Foundation of China(No.21004006)+2 种基金the Research Foundation for the Doctoral Program of Higher Education of China(No.20101101120036)the 111 Project in China(No.B07012)the Program for the New Century Excellent Talents in Universities of China(No.NCET-10-0047)
文摘Electrochemical cyclic voltammetric（CV） scan was applied to inducing the partial oxidation and defects of carbon nanotubes（CNTs）.The electrochemically induced functional groups and physical defects were demonstrated to show positive effects on the nanotube capacitance,as exemplified by super-long CNT arrays as model for the easy fabrication of CNT electrodes.Specifically,the initial hydrophobic nanotube surface becomes hydrophilic and a ten-time enhancement in capacitance is observed with respect to the pristine CNT sample.Thus,the electrochemical CV pretreatment can be used as an effective approach to activate the CNT surface for an enhanced electrochemical performance in capacitors,and many other advanced devices beyond capacitors,such as electrochemical sensors and batteries.
基金Supported by the National Natural Science Foundation of China(No.21101105)NSFC-Shenhua Group(No.51174274)+1 种基金the "Shu Guang"Project,China(No.09SG54)the Innovation Program of Shanghai Municipal Education Commission,China(No.12ZZ195)
文摘Bamboo-like nitrogen-doped carbon（CNx） nanotubes were synthesized by chemical vapor deposition （CVD） at a high reaction temperature of 600―900 °C. The butylamine and Fe/SBA-15 molecular sieve have been used as precursor and catalyst, respectively. Transmission electron microscopy（TEM） and high resolution transmission electron microscopy（HRTEM） observations show that the outer diameter and wall thickness as well as the inner diameter were increased with increasing reaction temperature in a temperature range of 600―800 °C. A synergism mechanism of the growth through bulk diffusion and the competitive growth through surface diffusion functions during the synthesis of CNx nanotubes was proposed.
基金This work was supported by the National Natural Science Foundation of China (No. 50228203 and 20425619) and CheungKong Scholar Program.
文摘Carbon nanotubes （CNTs） were prepared using different carrier gases, with ferrocene as the catalyst precusor and acetylene as the carbon source. The effects of ammonia and nitrogen as carrier gases on the structure and morphology of CNTs were investigated. Transmission electron microscope （TEM）, high-resolution electron microscope （HRTEM）, scanning electron microscope （SEM） and X-ray diffraction （XRD） were employed to characterize the products and the catalyst. Experiment results show that the CNTs grown in N2 gas exhibited cylindrical and tubular structure, while a bamboo-like structure was observed for the CNTs grown in NH3 gas. Moreover, vertically aligned CNTs were obtained on an A12O3 disk when NH3 was used as the carrier gas. The carrier gas also exerted influence on the shape of the catalyst. Based on the theory of active centers of catalysis and combined with the particle shape of the catalyst, a growth model for the vertically aligned CNTs on the substrate is given.
基金the National Natural Science Foundation of China(NSFC)(Nos.21501096 and 22075223)Natural Science Foundation of Jiangsu(Nos.BK20150086 and BK20201120)+2 种基金Foundation of the Jiangsu Education Committee(No.15KJB150020)the Six Talent Peaks Project in Jiangsu Province(No.JY-087)Innovation Project of Jiangsu Province.
文摘Interfacial atomic configuration between dual-metal active species and nitrogen-carbon substrates is of great importance for improving the intrinsic activity of catalysts toward oxygen reduction reaction(ORR).Thus,from the atomic-scale engineering we develop a high intrinsic activity ORR catalyst in terms of incorporating atomically dispersed dual Fe centers(single Fe atoms and ultra-small Fe atomic clusters)into bamboo-like N-doped carbon nanotubes.Benefiting from atomically dispersed dual-Fe centers on the atomic interface of Fe-Nx/carbon nanotubes,the fabricated dual Fe centers catalyst exhibits an extremely high ORR activity(E_(onset)=1.006 V;E_(1/2)=0.90 V),beyond state-of-the-art Pt/C.Remarkably,this catalyst also shows a superior kinetic current density of 19.690 mA·cm^(−2),which is 7 times that of state-of-the-art Pt/C.Additionally,based on the excellent catalyst,the primary Zn-air battery reveals a high power density up to 137 mW·cm^(−2) and sufficient potential cycling stability(at least 25 h).Undoubtedly,given the unique structure–activity relationship of dual-Fe active species and metal-nitrogen-carbon substrates,the catalyst will show great prospects in highly efficient electrochemical energy conversion devices.
文摘Very long and open aligned carbon nanotubes that reach about 2 mm long, an order of magnitude longer than previously reached, have been prepared by chemical vapor deposition over silica dioxide substrates on the surface, where iron/silica nano-composite particles are evenly positioned. The nanotubes are naturally opened at the bottom ends. The growth mechanism of the very long and open-ended nanotubes is also discussed.
基金This study was financially supported by the National Natural Science Foundation of China(No 21905037)the Doctoral Research Startup Fund of Liaoning Province(No.2020-BS-066)+2 种基金the Doctoral Research Fund of Lanzhou City University(No.LZCU-BS2020-03)the Fundamental Research Funds for the Central Universities(No.3132019328)Q.L.acknowledges the financial support from China Scholarship Council(CSC).
文摘Aqueous rechargeable zinc-ion battery(ZIB)is considered to be a potential energy storage system for large-scale applications due to its environmental friendliness,high safety,and low cost.However,it remains challenging to develop suitable cathode materials with high specific capacity and long-term cyclic stability.Herein,we have fabricated freestanding Sr0.19V2O51.3H2O/carbon nanotubes(SrVO/CNTs)composite films with different mass ratios by incorporating SrVO into CNTs network.The synthesized SrVO possesses a large interlayer spacing of 1.31 nm,which facilitates Zn(2+)diffusion.Furthermore,the SrVO/CNTs composite film with conductive network structure promotes electron transfer and ensures good contact between SrVO and CNTs during the long-term cycling process.As a result,the battery based on the SrVO/CNTs composite cathode with a mass ratio of 7:3 delivers a specific capacity of 326 mAh·g^(-1)at 0.1 A·g^(-1)and 145 mAh·g^(-1)at 5 A·g^(-1),demonstrating a high capacity and excellent rate capability.Remarkably,the assembled ZIB shows good capacity retention of 91%even after ultra-long cycling for 7500 cycles at a high current rate of 5 Ag^(-1).More importantly,the battery also delivers a high energy density and power density,as 290 Wh·kg^(-1)at 125 W·kg^(-1)(0.1 A·g^(-1)),or 115 Wh·kg^(-1)at 6078 W·kg^(-1)(5 Ag^(-1)).The results demonstrate that the SrVO/CNTs composite is a promising cathode toward large-scale energy storage applications.
基金financially supported by the National Natural Science Foundation of China(Nos.21975069 and 21872045)Key Project of Research and Development Plan of Hunan Province(Grant No.2019SK2071)+2 种基金the Innovative Research Groups of Hunan Province(Grant No.2019JJ10001)the Natural Science Foundation of Hunan Province,China(Grant No.2020JJ416)the Science and Technology Planning Project of Hunan Province(Grant No.2019RS3010).
文摘Efficient selective oxidation of hydrocarbons to corresponding ketones has been a significant but challenging work in the past decades.Here,a nitrogen-doped bamboo-like carbon nanotubes encapsulating cobalt catalyst(NCNTs-X)using citric acid,melamine and CoCl_(2)·6H_(2)O as precursors was synthesized by a simple pyrolysis method.A series of characterization techniques were employed to investigate the physicochemical properties of samples.And the results show that the as-prepared catalysts achieve a high catalytic performance for selective ethylbenzene oxidation(78.3% ethylbenzene conversion)using molecular oxygen as oxidant,especially giving a high selectivity(93.8% selectivity to acetophenone).According to the investigation of the structure-activity relationship of the catalysts,it can be deduced that the Co-N_(x) sites have an obvious positive effect on catalytic performance thanks to the synergistic effect between metallic cobalt and pyridinic N.
