In line with recent studies,where it has been shown that nanofluids containing graphene have a stronger capacity to boost the heat transfer coefficient with respect to ordinary nanofluids,experiments have been conducted ...In line with recent studies,where it has been shown that nanofluids containing graphene have a stronger capacity to boost the heat transfer coefficient with respect to ordinary nanofluids,experiments have been conducted using water with cobalt ferrite/graphene nanoparticles.In particular,a circular channel made of copper subjected to a constant heatflux has been considered.As nanoparticles are sensitive to the presence of a magneticfield,different conditions have been examined,allowing both the strength and the frequency of such afield to span relatively wide ranges and assuming different concentrations of nanoparticles.According to thefindings,the addition of nanoparticles to thefluid causes its rotation speed to increase by a factor of two,whereas ultraviolet radiation plays a negligible role.The amount of time required to attain the maximum rotation speed of the nanofluid and the Nusselt number have been measured under both constant and alternating magneticfields for a ferrofluid with a concentration of 0.5%and atflow Reynolds number of 550 and 1750.展开更多
Coaxial fiber-shaped supercapacitors are a promising class of energy storage devices requiring high performance for flexible and miniature electronic devices.Yet,they are still struggling from inferior energy density,...Coaxial fiber-shaped supercapacitors are a promising class of energy storage devices requiring high performance for flexible and miniature electronic devices.Yet,they are still struggling from inferior energy density,which comes from the limited choices in materials and structure used.Here,Zn-doped CuO nanowires were designed as 3D framework for aligned distributing high mass loading of MnO2 nanosheets.Zn could be introduced into the CuO crystal lattice to tune the covalency character and thus improve charge transport.The Zn–CuO@MnO2 as positive electrode obtained superior performance without sacrificing its areal and gravimetric capacitances with the increasing of mass loading of MnO2 due to 3D Zn–CuO framework enabling efficient electron transport.A novel category of free-standing asymmetric coaxial fiber-shaped supercapacitor based on Zn0.11CuO@MnO2 core electrode possesses superior specific capacitance and enhanced cell potential window.This asymmetric coaxial structure provides superior performance including higher capacity and better stability under deformation because of sufficient contact between the electrodes and electrolyte.Based on these advantages,the as-prepared asymmetric coaxial fiber-shaped supercapacitor exhibits a high specific capacitance of 296.6 mF cm^−2 and energy density of 133.47μWh cm^−2.In addition,its capacitance retention reaches 76.57%after bending 10,000 times,which demonstrates as-prepared device’s excellent flexibility and long-term cycling stability.展开更多
Neutral aqueous rechargeable Co_(3)O_(4)//Zn batteries with high-output voltage and outstanding cycling stability have yielded new insights into wearable energy-storage devices.To meet the increasing demand for a mean...Neutral aqueous rechargeable Co_(3)O_(4)//Zn batteries with high-output voltage and outstanding cycling stability have yielded new insights into wearable energy-storage devices.To meet the increasing demand for a means of powering wearable and portable devices,the development of a high-performance fiber-shaped Co//Zn battery would be highly desirable.However,the intrinsically poor conductivity of C 03O4 significantly restricts the application of these high-capacity and high-rate aqueous rechargeable battery.Encouragingly,density functional theory(DFT)calculations demonstrate that the substitution of Zn for Co^(3+)leads to an insulatormetal transition in the Zn-doped Co_(3)O_(4)(Zn-Co_(3)O_(4)).In this study,we used metallic Zn-Co_(3)O_(4)nanowire arrays(NWAs)as a novel binder-free cathode to successfully fabricate an all-solid-state fiber-shaped aqueous rechargeable(AFAR)Co//Zn battery.The resulting fiber-shaped Co//Zn battery takes advantage of the enhanced conductivity,increased capacity,and improved rate capability of Zn-Co_(3)O_(4)NWAs to yield a remarkable capacity of 1.25 mAh·cm^(-2)at a current density of 0.5 mA·cm^(-2),extraordinary rate capability(60.8%capacity retention at a high current density of 20 mA·cm^(-2))and an admirable energy density of 772.6 mWh·cm^(-3).Thus,the successful construction of Zn-Co_(3)O_(4)NWAs provides valuable insights into the design of high-capacity and high-rate cathode materials for aqueous rechargeable high-voltage batteries.展开更多
Extensive efforts have recently been devoted to the construction of aqueous rechargeable sodium-ion batteries(ARSIBs)for large-scale energy-storage applications due to their desired properties of abundant sodium resou...Extensive efforts have recently been devoted to the construction of aqueous rechargeable sodium-ion batteries(ARSIBs)for large-scale energy-storage applications due to their desired properties of abundant sodium resources and inherently safer aqueous electrolytes.However,it is still a significant challenge to develop highly flexible ARSIBs ascribing to the lack of flexible electrode materials.In this work,nanocube-like KNiFe(CN)6(KNHCF)and rugby balllike NaTi2(PO4)3(NTP)are grown on carbon nanotube fibers via simple and mild methods as the flexible binder-free cathode(KNHCF@CNTF)and anode(NTP@CNTF),respectively.Taking advantage of their high conductivity,fast charge transport paths,and large accessible surface area,the as-fabricated binder-free electrodes display admirable electrochemical performance.Inspired by the remarkable flexibility of the binder-free electrodes and the synergy of KNHCF@CNTF and NTP@CNTF,a high-performance quasi-solid-state fiber-shaped ARSIB(FARSIB)is successfully assembled for the first time.Significantly,the as-assembled FARSIB possesses a high capacity of 34.21 mAh cm?3 and impressive energy density of 39.32 mWh cm?3.More encouragingly,our FARSIB delivers superior mechanical flexibility with only 5.7%of initial capacity loss after bending at 90°for over 3000 cycles.Thus,this work opens up an avenue to design ultraflexible ARSIBs based on all binder-free electrodes for powering wearable and portable electronics.展开更多
Air-breathing proton exchange membrane fuel cells(PEMFCs) are very promising portable energy with many advantages. However, its power density is low and many additional supporting parts affect its specific power. In t...Air-breathing proton exchange membrane fuel cells(PEMFCs) are very promising portable energy with many advantages. However, its power density is low and many additional supporting parts affect its specific power. In this paper, we aim to improve the air diffusion and fuel cell performance by employing a novel condensing-tower-like curved flow field rather than an additional fan, making the fuel cell more compact and has less internal power consumption. Polarization curve test and galvanostatic discharge test are carried out and proved that curved flow field can strengthen the air diffusion into the PEMFC and improve its performance. With appropriate curved flow field, the fuel cell peak power can be 55.2%higher than that of planar flow field in our study. A four-layer stack with curved cathode flow field is fabricated and has a peak power of 2.35 W(120 W/kg).展开更多
Metal sulfide based materials as photocatalysts for energy conversion are essential to produce value-added chemical fuels,but their intrinsically slow carrier dynamics and low activity are yet to be resolved.Herein,we...Metal sulfide based materials as photocatalysts for energy conversion are essential to produce value-added chemical fuels,but their intrinsically slow carrier dynamics and low activity are yet to be resolved.Herein,we developed a unique heterogeneously nanostructured ZnIn_(2)S_(4)-CdS heterostructure that involves zero-dimensional(0D)CdS quantum dots uniformly confined on three-dimensional(3D)ZnIn_(2)S_(4)nanoflowers,which achieves an excellent catalytic performance of CO_(2) photoconversion under visible-light irradiation.The obtained hierarchical heterostructure can significantly enhance the light harvesting,shorten the migration distance of carriers,and obviously accelerate the transport of electrons.As evidenced by the ultrafast transient absorption spectroscopy,the formed interface can effectively facilitate charge separation and transport.This work opens up a new avenue to carefully design the elaborate heterostructures for achieving optimal charge separation efficiency by lowering interfacial kinetic barriers and energy losses at the interface.展开更多
Flexible electrochemical power sources are attracting increasing attentions for their unique advantages like flexibility, shape diversity, light weight and excellent mechanical properties. In this research, we discove...Flexible electrochemical power sources are attracting increasing attentions for their unique advantages like flexibility, shape diversity, light weight and excellent mechanical properties. In this research, we discover that the current collector can dramatically affect the performance of flexible electrochemical power sources with large size. For flexible air-breathing proton exchange membrane fuel cell (PEMFC), the performance could have more than 8 times increase by only adjusting the directions of current collectors. The different performances of different current collection types are mainly attributed to the diverse lengths of the electron transfer pathways. In addition, the conductivity of current collector can dramatically affect the capability of flexible PEMFCs with large-size. The flexible PEMFCs with thicker carbon nanotube membrane as current collector (low electric resistance) show higher ability. A mathematic model is successfully built in this work to further understand the performance. Moreover, the model and simulation are also applicable to other flexible power sources, such as flexible Li-ion battery and supercapacitor.展开更多
The unveiling of MOF growth mechanism is hampered by the lack of fundamental knowledge about the very early stage of nucleation,especially the form and ratio of molecular species in the solution for crystal growth.Her...The unveiling of MOF growth mechanism is hampered by the lack of fundamental knowledge about the very early stage of nucleation,especially the form and ratio of molecular species in the solution for crystal growth.Herein,we report the detection of growth species for a series of MOFs with mono-linker,CuMOF-2-BDC and Cu-MOF-2-NDC,and two linkers,MTV-MOF-2-(C_(4)H_(4))x,by high resolution ESI-MS,where a large variety of Cu-containing species are identified unambiguously.The solvent molecules such as H_(2)O,methanol and DMF participate in the formation of these species,other than ethanol.Furthermore,in the growth solution of MTV-MOF-2-(C_(4)H_(4))x,growth species containing two different organic linkers are observed.The feeding ratio is not the only factor controlling the distribution of growth species for MTVMOFs,but also the solvent involves in coordination,an aspect usually overlooked previously.展开更多
Single molecule catalysis is very powerful in revealing catalytic mechanism at the single molecule level.But fluorescent molecule is always necessary to take part into the catalysis directly in previous research.In or...Single molecule catalysis is very powerful in revealing catalytic mechanism at the single molecule level.But fluorescent molecule is always necessary to take part into the catalysis directly in previous research.In order to study the single molecule electro-catalysis of non-fluorescent molecule(SMECNFM) on nanocatalyst, we couple the SMECNFM with a single molecule fluorescence reaction. A certain number of fluorescent molecules will be generated and detected when the SMECNFM happens. Through this method, we can detect the electro-oxidation reaction of one HCOONa molecule. The stability of Pt nanocatalyst supported on active carbon is studied at the single molecule level by this method. This paper also provides a general way to make ultra-sensitive sensor, and to study the SMECNFM for the molecules,such as formic acid, hydrogen, oxygen, etc., on single nanoparticle.展开更多
A novel iron-hydrogen battery system, whose Fe^(3+)/Fe^(2+)cathode circumvents slowly dynamic oxygen reduction reaction and anode is fed with clean and cordial hydrogen, is systematically investigated. The maximum dis...A novel iron-hydrogen battery system, whose Fe^(3+)/Fe^(2+)cathode circumvents slowly dynamic oxygen reduction reaction and anode is fed with clean and cordial hydrogen, is systematically investigated. The maximum discharge power density of the iron-hydrogen battery reaches to 96.0 m W/cm^(2) under the room temperature. The capacity reaches to 17.2 Ah/L and the coulombic and energy efficiency are achieved to99% and 86%, respectively, during the galvanostatic charge-discharge test. Moreover, stable cycling test is observed for more than 240 h and 100 cycles with the iron sulfate in the sulfuric acid solutions. It is found that air plasma treatment onto the cathode carbon paper can generate the oxygen-containing groups and increase the hydrophilic pores proportion to ca. 40%, enlarging nearly 6-fold effective diffusion coefficient and improving the mass transfer in the battery performance. The simple iron-hydrogen energy storage battery design offers us a new strategy for the large-scale energy storage and hydrogen involved economy.展开更多
Fiber-based supercapacitors (FSCs) are new members of the energy storage family. They present excellent flexibility and have promising applications in lightweight, flexible, and wearable devices. One of the existing...Fiber-based supercapacitors (FSCs) are new members of the energy storage family. They present excellent flexibility and have promising applications in lightweight, flexible, and wearable devices. One of the existing challenges of FSCs is enhancing their energy density while retaining the flexibility. We developed a facile and cost-effective method to fabricate a highly capacitive positive electrode based on hierarchical ferric-cobalt-nickel ternary oxide nanowire arrays/graphene fibers and a negative electrode based on polyaniline-derived carbon nanorods/graphene fibers. The elegant microstructures and excellent electrochemical performances of both electrodes enabled us to construct a high- performance flexible asymmetric graphene fiber-based supercapacitor device with an operating voltage of 1.4 V, a specific capacitance up to 61.58 mF.cm-2, and an energy density reaching 16.76 μW·h·cm-2. Moreover, the optimal device presents an outstanding cycling stability with 87.5% initial capacitance retention after 8,000 cycles, and an excellent flexibility with a capacitance retention of 90.9% after 4,000 cycles of repetitive bending.展开更多
Fiber-shaped energy storage devices are indispensable parts of wearable and portable electronics.Aqueous rechargeable Ni/Fe battery is a very appropriate energy storage device due to their good safety without organic ...Fiber-shaped energy storage devices are indispensable parts of wearable and portable electronics.Aqueous rechargeable Ni/Fe battery is a very appropriate energy storage device due to their good safety without organic electrolytes, high ionic conductivity, and low cost. Unfortunately, the low energy density,poor power density and cycling performance hinder its further practical applications. In this study, in order to obtain high performance negative iron-based material, we first synthesized a-iron oxide(α-Fe2O3) nanorods(NRs) with superstructures on the surface of highly conductive carbon nanotube fibers(CNTFs), then electrically conductive polypyrrole(PPy) was coated to enhance the electron, ion diffusion and cycle stability. The as-prepared α-Fe2O3@PPy NRs/CNTF electrode shows a high specific capacity of 0.62 Ah cm-3 at the current density of 1 A cm-3. Furthermore, the Ni/Fe battery that was assembled by the above negative electrode shows a maximum volumetric energy density of 15.47 mWh cm-3 with228.2 mW cm-3 at a current density of 1 A cm-3. The cycling durability and mechanical flexibility of the Ni/Fe battery were tested, which show good prospect for practical application. In summary, these merits make it possible for our Ni/Fe battery to have practical applications in next generation flexible energy storage devices.展开更多
Different from studies where less defective platinum(Pt)-based nanomaterials have been widely used to improve the catalysis of the oxygen reduction reaction(ORR)for proton-exchange membrane fuel cells(PEMFCs),herein w...Different from studies where less defective platinum(Pt)-based nanomaterials have been widely used to improve the catalysis of the oxygen reduction reaction(ORR)for proton-exchange membrane fuel cells(PEMFCs),herein we have demonstrated that a new class of Pt nanorods(NRs)with a highly distorted configuration can be applied as an advanced,high-efficiency fuel cell catalyst,as transformed from spongy Pt–tellurium NRs(PtTe2 NRs)through sequential chemical and electrochemical aging procedures.The resulting highly distorted Pt NRs exhibit excellent ORR-specific and mass activities of 4.70mA cm−2 and 2.77 Amg−1 Pt at 0.90 V versus the reversible hydrogen electrode(RHE),which are 18.8 and 16.3 times higher than those of commercial Pt/C catalyst,and the mass activity is 6.3 times higher than 2020 U.S.Department of Energy target.Additionally,negligible activity decays were observed after 30,000 cycles.The high ORR performance endows these unique Pt NRs with enhanced activity and lifetimes for practical fuel cell catalysis in comparison with commercial Pt/C,which is consistent with the experimental results.It has been demonstrated that the anomaly of strong electron–lattice coupling suppresses Coulombic repulsion for barrier-free electron transfer while concurrently exposing a large number of active sites,which is a key to superior high-performance fuel cell reactions.展开更多
A homogeneous catalyst [Cp*Rh(NH3)(H2O)2]-(3+) has been found for the clean conversion of methanol and water to hydrogen and carbon dioxide. The simple and easily available reaction steps can circumvent the fo...A homogeneous catalyst [Cp*Rh(NH3)(H2O)2]-(3+) has been found for the clean conversion of methanol and water to hydrogen and carbon dioxide. The simple and easily available reaction steps can circumvent the formation of CO, therefore, making it possible to avoid inactivating catalysts and contaminating the hydrogen fuel. Different from conventional reforming method for hydrogen production, no additional alkaline or organic substances are required in this method. Valuable hydrogen can be obtained under ambient pressure at 70 C, corresponding TOF is 83.2 h 1. This is an unprecedented success in reforming methanol to hydrogen. Effects of reaction conditions, such as reaction temperature, initial methanol concentration and the initial p H value of buffer solution on the hydrogen evolution are all systematically investigated. In a certain range, higher reaction temperature will accelerate reaction rate. The slightly acidic condition is conducive to rapid hydrogen production. These findings are of great significance to the present establishment of the carbon-neutral methanol economy.展开更多
Formic acid(FA) dehydrogenation has attracted a lot of attentions since it is a convenient method for H_2 production. In this work, we designed a self-supporting fuel cell system, in which H_2 from FA is supplied in...Formic acid(FA) dehydrogenation has attracted a lot of attentions since it is a convenient method for H_2 production. In this work, we designed a self-supporting fuel cell system, in which H_2 from FA is supplied into the fuel cell, and the exhaust heat from the fuel cell supported the FA dehydrogenation. In order to realize the system, we synthesized a highly active and selective homogeneous catalyst Ir Cp*Cl_2 bpym for FA dehydrogenation. The turnover frequency(TOF) of the catalyst for FA dehydrogenation is as high as7150 h^(-1)at 50°C, and is up to 144,000 h^(-1)at 90°C. The catalyst also shows excellent catalytic stability for FA dehydrogenation after several cycles of test. The conversion ratio of FA can achieve 93.2%, and no carbon monoxide is detected in the evolved gas. Therefore, the evolved gas could be applied in the proton exchange membrane fuel cell(PEMFC) directly. This is a potential technology for hydrogen storage and generation. The power density of the PEMFC driven by the evolved gas could approximate to that using pure hydrogen.展开更多
文摘In line with recent studies,where it has been shown that nanofluids containing graphene have a stronger capacity to boost the heat transfer coefficient with respect to ordinary nanofluids,experiments have been conducted using water with cobalt ferrite/graphene nanoparticles.In particular,a circular channel made of copper subjected to a constant heatflux has been considered.As nanoparticles are sensitive to the presence of a magneticfield,different conditions have been examined,allowing both the strength and the frequency of such afield to span relatively wide ranges and assuming different concentrations of nanoparticles.According to thefindings,the addition of nanoparticles to thefluid causes its rotation speed to increase by a factor of two,whereas ultraviolet radiation plays a negligible role.The amount of time required to attain the maximum rotation speed of the nanofluid and the Nusselt number have been measured under both constant and alternating magneticfields for a ferrofluid with a concentration of 0.5%and atflow Reynolds number of 550 and 1750.
基金the National Natural Science Foundation of China(Nos.21975281,21773293,21603264)CAS Pioneer Hundred Talents Program,the National Key Research and Development Program of China(2016YFA0203301)+1 种基金Jiangsu Planned Projects for Postdoctoral Research Funds(2019K048)Suzhou Science and Technology Plan Project(SYG201926).
文摘Coaxial fiber-shaped supercapacitors are a promising class of energy storage devices requiring high performance for flexible and miniature electronic devices.Yet,they are still struggling from inferior energy density,which comes from the limited choices in materials and structure used.Here,Zn-doped CuO nanowires were designed as 3D framework for aligned distributing high mass loading of MnO2 nanosheets.Zn could be introduced into the CuO crystal lattice to tune the covalency character and thus improve charge transport.The Zn–CuO@MnO2 as positive electrode obtained superior performance without sacrificing its areal and gravimetric capacitances with the increasing of mass loading of MnO2 due to 3D Zn–CuO framework enabling efficient electron transport.A novel category of free-standing asymmetric coaxial fiber-shaped supercapacitor based on Zn0.11CuO@MnO2 core electrode possesses superior specific capacitance and enhanced cell potential window.This asymmetric coaxial structure provides superior performance including higher capacity and better stability under deformation because of sufficient contact between the electrodes and electrolyte.Based on these advantages,the as-prepared asymmetric coaxial fiber-shaped supercapacitor exhibits a high specific capacitance of 296.6 mF cm^−2 and energy density of 133.47μWh cm^−2.In addition,its capacitance retention reaches 76.57%after bending 10,000 times,which demonstrates as-prepared device’s excellent flexibility and long-term cycling stability.
基金the National Natural Science Foundation of China(No.51703241)the Fundamental Research Funds for the Central Universities(No.020514380183)+1 种基金the Key Research Program of Frontier Science of Chinese Academy of Sciences(No.QYZDB-SSW-SLH031)the Science and Technology Project of Nanchang(No.2017-SJSYS-008).
文摘Neutral aqueous rechargeable Co_(3)O_(4)//Zn batteries with high-output voltage and outstanding cycling stability have yielded new insights into wearable energy-storage devices.To meet the increasing demand for a means of powering wearable and portable devices,the development of a high-performance fiber-shaped Co//Zn battery would be highly desirable.However,the intrinsically poor conductivity of C 03O4 significantly restricts the application of these high-capacity and high-rate aqueous rechargeable battery.Encouragingly,density functional theory(DFT)calculations demonstrate that the substitution of Zn for Co^(3+)leads to an insulatormetal transition in the Zn-doped Co_(3)O_(4)(Zn-Co_(3)O_(4)).In this study,we used metallic Zn-Co_(3)O_(4)nanowire arrays(NWAs)as a novel binder-free cathode to successfully fabricate an all-solid-state fiber-shaped aqueous rechargeable(AFAR)Co//Zn battery.The resulting fiber-shaped Co//Zn battery takes advantage of the enhanced conductivity,increased capacity,and improved rate capability of Zn-Co_(3)O_(4)NWAs to yield a remarkable capacity of 1.25 mAh·cm^(-2)at a current density of 0.5 mA·cm^(-2),extraordinary rate capability(60.8%capacity retention at a high current density of 20 mA·cm^(-2))and an admirable energy density of 772.6 mWh·cm^(-3).Thus,the successful construction of Zn-Co_(3)O_(4)NWAs provides valuable insights into the design of high-capacity and high-rate cathode materials for aqueous rechargeable high-voltage batteries.
基金supported by the Fundamental Research Funds for the Central Universities(No.020514380183)the National Natural Science Foundation of China(No.51703241)+1 种基金the Key Research Program of Frontier Science of Chinese Academy of Sciences(No.QYZDB-SSW-SLH031)the Thousand Youth Talents Plan,and the Science and Technology Project of Nanchang(2017-SJSYS-008).
文摘Extensive efforts have recently been devoted to the construction of aqueous rechargeable sodium-ion batteries(ARSIBs)for large-scale energy-storage applications due to their desired properties of abundant sodium resources and inherently safer aqueous electrolytes.However,it is still a significant challenge to develop highly flexible ARSIBs ascribing to the lack of flexible electrode materials.In this work,nanocube-like KNiFe(CN)6(KNHCF)and rugby balllike NaTi2(PO4)3(NTP)are grown on carbon nanotube fibers via simple and mild methods as the flexible binder-free cathode(KNHCF@CNTF)and anode(NTP@CNTF),respectively.Taking advantage of their high conductivity,fast charge transport paths,and large accessible surface area,the as-fabricated binder-free electrodes display admirable electrochemical performance.Inspired by the remarkable flexibility of the binder-free electrodes and the synergy of KNHCF@CNTF and NTP@CNTF,a high-performance quasi-solid-state fiber-shaped ARSIB(FARSIB)is successfully assembled for the first time.Significantly,the as-assembled FARSIB possesses a high capacity of 34.21 mAh cm?3 and impressive energy density of 39.32 mWh cm?3.More encouragingly,our FARSIB delivers superior mechanical flexibility with only 5.7%of initial capacity loss after bending at 90°for over 3000 cycles.Thus,this work opens up an avenue to design ultraflexible ARSIBs based on all binder-free electrodes for powering wearable and portable electronics.
基金financial support granted by National Key R&D Program of China from Ministry of Science and Technology of China (Nos. 2020YFB1505700, 2016YFA0200700)China Postdoctoral Science Foundation (No. 2021M702408)+4 种基金the National Natural Science Foundation of China (No. 22172191)Dongyue Polymer Material Company of Dongyue FederationState Key Laboratory of Fluorinated Functional Membrane Materials(Dongyue Group institute)Dongyue Future Hydrogen Energy Materials Companysponsored by the Collaborative Innovation Center of Suzhou Nano Science and Technology。
文摘Air-breathing proton exchange membrane fuel cells(PEMFCs) are very promising portable energy with many advantages. However, its power density is low and many additional supporting parts affect its specific power. In this paper, we aim to improve the air diffusion and fuel cell performance by employing a novel condensing-tower-like curved flow field rather than an additional fan, making the fuel cell more compact and has less internal power consumption. Polarization curve test and galvanostatic discharge test are carried out and proved that curved flow field can strengthen the air diffusion into the PEMFC and improve its performance. With appropriate curved flow field, the fuel cell peak power can be 55.2%higher than that of planar flow field in our study. A four-layer stack with curved cathode flow field is fabricated and has a peak power of 2.35 W(120 W/kg).
基金the National Natural Science Foundation of China(Nos.21573211,21633007,21671180)the National Key R&D Program of China(Nos.2016YFA0200602,2017YFA0208300,2017YFA0700104,2018YFA0208702)the Anhui Initiative in Quantum Information Technologies(No.AHY090200).We also thank the funding support from the CAS Fujian Institute of Innovation.
文摘Metal sulfide based materials as photocatalysts for energy conversion are essential to produce value-added chemical fuels,but their intrinsically slow carrier dynamics and low activity are yet to be resolved.Herein,we developed a unique heterogeneously nanostructured ZnIn_(2)S_(4)-CdS heterostructure that involves zero-dimensional(0D)CdS quantum dots uniformly confined on three-dimensional(3D)ZnIn_(2)S_(4)nanoflowers,which achieves an excellent catalytic performance of CO_(2) photoconversion under visible-light irradiation.The obtained hierarchical heterostructure can significantly enhance the light harvesting,shorten the migration distance of carriers,and obviously accelerate the transport of electrons.As evidenced by the ultrafast transient absorption spectroscopy,the formed interface can effectively facilitate charge separation and transport.This work opens up a new avenue to carefully design the elaborate heterostructures for achieving optimal charge separation efficiency by lowering interfacial kinetic barriers and energy losses at the interface.
基金financial support granted by Ministry of Science and Technology of China(Nos. 2016YFE0105700, 2016YFA0200700)the National Natural Science Foundation of China (Nos. 21373264, 21573275)+2 种基金China Postdoctoral Science Foundation(No. 2018M632406)the Science and Technology Project of Nanchang(No. 2017-SJSYS-008)the Collaborative Innovation Center of Suzhou Nano Science and Technology
文摘Flexible electrochemical power sources are attracting increasing attentions for their unique advantages like flexibility, shape diversity, light weight and excellent mechanical properties. In this research, we discover that the current collector can dramatically affect the performance of flexible electrochemical power sources with large size. For flexible air-breathing proton exchange membrane fuel cell (PEMFC), the performance could have more than 8 times increase by only adjusting the directions of current collectors. The different performances of different current collection types are mainly attributed to the diverse lengths of the electron transfer pathways. In addition, the conductivity of current collector can dramatically affect the capability of flexible PEMFCs with large-size. The flexible PEMFCs with thicker carbon nanotube membrane as current collector (low electric resistance) show higher ability. A mathematic model is successfully built in this work to further understand the performance. Moreover, the model and simulation are also applicable to other flexible power sources, such as flexible Li-ion battery and supercapacitor.
基金the National Natural Science Foundation of China(Nos.91545205,91622103,21971199 and 22025106)National Key Research and Development Project(Nos.2020YFB1505700,2016YFA0200700 and 2018YFA-0704000)+1 种基金Innovation Team of Wuhan University(No.2042017kf0232)the Fundamental Research Funds for the Central Universities(No.2042020kf0214)。
文摘The unveiling of MOF growth mechanism is hampered by the lack of fundamental knowledge about the very early stage of nucleation,especially the form and ratio of molecular species in the solution for crystal growth.Herein,we report the detection of growth species for a series of MOFs with mono-linker,CuMOF-2-BDC and Cu-MOF-2-NDC,and two linkers,MTV-MOF-2-(C_(4)H_(4))x,by high resolution ESI-MS,where a large variety of Cu-containing species are identified unambiguously.The solvent molecules such as H_(2)O,methanol and DMF participate in the formation of these species,other than ethanol.Furthermore,in the growth solution of MTV-MOF-2-(C_(4)H_(4))x,growth species containing two different organic linkers are observed.The feeding ratio is not the only factor controlling the distribution of growth species for MTVMOFs,but also the solvent involves in coordination,an aspect usually overlooked previously.
基金supported by the National Natural Science Foundation of China(Nos.21373264 and 21573275)Suzhou Institute of Nano-tech and Nano-bionics(No.Y3AAA11004)Thousand Youth Talents Plan(No.Y3BQA11001)
文摘Single molecule catalysis is very powerful in revealing catalytic mechanism at the single molecule level.But fluorescent molecule is always necessary to take part into the catalysis directly in previous research.In order to study the single molecule electro-catalysis of non-fluorescent molecule(SMECNFM) on nanocatalyst, we couple the SMECNFM with a single molecule fluorescence reaction. A certain number of fluorescent molecules will be generated and detected when the SMECNFM happens. Through this method, we can detect the electro-oxidation reaction of one HCOONa molecule. The stability of Pt nanocatalyst supported on active carbon is studied at the single molecule level by this method. This paper also provides a general way to make ultra-sensitive sensor, and to study the SMECNFM for the molecules,such as formic acid, hydrogen, oxygen, etc., on single nanoparticle.
基金financial support granted by National Key R&D Program of China (No.2020YFB1505704)Dongyue Polymer Material Company of Dongyue Federation+2 种基金State Key Laboratory of Fluorinated Functional Membrane Materials (Dongyue Group institute)Dongyue Future Hydrogen Energy Materials Companysponsored by the Collaborative Innovation Center of Suzhou Nano Science and Technology。
文摘A novel iron-hydrogen battery system, whose Fe^(3+)/Fe^(2+)cathode circumvents slowly dynamic oxygen reduction reaction and anode is fed with clean and cordial hydrogen, is systematically investigated. The maximum discharge power density of the iron-hydrogen battery reaches to 96.0 m W/cm^(2) under the room temperature. The capacity reaches to 17.2 Ah/L and the coulombic and energy efficiency are achieved to99% and 86%, respectively, during the galvanostatic charge-discharge test. Moreover, stable cycling test is observed for more than 240 h and 100 cycles with the iron sulfate in the sulfuric acid solutions. It is found that air plasma treatment onto the cathode carbon paper can generate the oxygen-containing groups and increase the hydrophilic pores proportion to ca. 40%, enlarging nearly 6-fold effective diffusion coefficient and improving the mass transfer in the battery performance. The simple iron-hydrogen energy storage battery design offers us a new strategy for the large-scale energy storage and hydrogen involved economy.
基金This work was supported by the National Key R&D Program of China (No. 2017YFB0406000), the Key Research Program of Frontier Science of Chinese Academy of Sciences (No. QYZDB-SSW-SLH031), the Natural Science Foundation of Jiangsu Province, China (Nos. BK20160399 and BK20140392), the Transformation of Scientific and Technological Achievements in Jiangsu Province (No. BA2016026), the Postdoctoral Foundation of Jiangsu Province (No. 1601065B), and the Science and Technology Project of Suzhou, China (Nos. SZS201508, ZXG201428, and ZXG201401).
文摘Fiber-based supercapacitors (FSCs) are new members of the energy storage family. They present excellent flexibility and have promising applications in lightweight, flexible, and wearable devices. One of the existing challenges of FSCs is enhancing their energy density while retaining the flexibility. We developed a facile and cost-effective method to fabricate a highly capacitive positive electrode based on hierarchical ferric-cobalt-nickel ternary oxide nanowire arrays/graphene fibers and a negative electrode based on polyaniline-derived carbon nanorods/graphene fibers. The elegant microstructures and excellent electrochemical performances of both electrodes enabled us to construct a high- performance flexible asymmetric graphene fiber-based supercapacitor device with an operating voltage of 1.4 V, a specific capacitance up to 61.58 mF.cm-2, and an energy density reaching 16.76 μW·h·cm-2. Moreover, the optimal device presents an outstanding cycling stability with 87.5% initial capacitance retention after 8,000 cycles, and an excellent flexibility with a capacitance retention of 90.9% after 4,000 cycles of repetitive bending.
基金This work was supported by the National Natural Science Foundation of China (51972162 and 51703241)the Postdoctoral Foundation of Jiangsu Province (2019Z203 and 2019K001)the Science and Technology Project of Nanchang (2017-SJSYS008)
文摘Fiber-shaped energy storage devices are indispensable parts of wearable and portable electronics.Aqueous rechargeable Ni/Fe battery is a very appropriate energy storage device due to their good safety without organic electrolytes, high ionic conductivity, and low cost. Unfortunately, the low energy density,poor power density and cycling performance hinder its further practical applications. In this study, in order to obtain high performance negative iron-based material, we first synthesized a-iron oxide(α-Fe2O3) nanorods(NRs) with superstructures on the surface of highly conductive carbon nanotube fibers(CNTFs), then electrically conductive polypyrrole(PPy) was coated to enhance the electron, ion diffusion and cycle stability. The as-prepared α-Fe2O3@PPy NRs/CNTF electrode shows a high specific capacity of 0.62 Ah cm-3 at the current density of 1 A cm-3. Furthermore, the Ni/Fe battery that was assembled by the above negative electrode shows a maximum volumetric energy density of 15.47 mWh cm-3 with228.2 mW cm-3 at a current density of 1 A cm-3. The cycling durability and mechanical flexibility of the Ni/Fe battery were tested, which show good prospect for practical application. In summary, these merits make it possible for our Ni/Fe battery to have practical applications in next generation flexible energy storage devices.
基金supported by the Ministry of Science and Technology of China(2016YFA0204100 and 2017YFA0208200)the National Natural Science Foundation of China(21571135)+3 种基金Young Thousand Talented Program,the Natural Science Foundation of Jiangsu Higher Education Institutions(17KJB150032)the Special Funded Project of China Postdoctoral Science Foundation(2019T120453)the project of scientific and technologic infrastructure of Suzhou(SZS201708)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD),and start-up support from Soochow University.
文摘Different from studies where less defective platinum(Pt)-based nanomaterials have been widely used to improve the catalysis of the oxygen reduction reaction(ORR)for proton-exchange membrane fuel cells(PEMFCs),herein we have demonstrated that a new class of Pt nanorods(NRs)with a highly distorted configuration can be applied as an advanced,high-efficiency fuel cell catalyst,as transformed from spongy Pt–tellurium NRs(PtTe2 NRs)through sequential chemical and electrochemical aging procedures.The resulting highly distorted Pt NRs exhibit excellent ORR-specific and mass activities of 4.70mA cm−2 and 2.77 Amg−1 Pt at 0.90 V versus the reversible hydrogen electrode(RHE),which are 18.8 and 16.3 times higher than those of commercial Pt/C catalyst,and the mass activity is 6.3 times higher than 2020 U.S.Department of Energy target.Additionally,negligible activity decays were observed after 30,000 cycles.The high ORR performance endows these unique Pt NRs with enhanced activity and lifetimes for practical fuel cell catalysis in comparison with commercial Pt/C,which is consistent with the experimental results.It has been demonstrated that the anomaly of strong electron–lattice coupling suppresses Coulombic repulsion for barrier-free electron transfer while concurrently exposing a large number of active sites,which is a key to superior high-performance fuel cell reactions.
基金financial support granted by Ministry of Science and Technology of the People's Republic of China(Nos.2016YFA0200700 and 2016YFE0105700)the National Natural Science Foundation of China(Nos.21373264 and 21573275)+2 种基金the Natural Science Foundation of Jiangsu Province(No.BK20150362)Suzhou Institute of Nano-tech and Nanobionics(No.Y3AAA11004)Thousand Youth Talents Plan(No.Y3BQA11001)
文摘A homogeneous catalyst [Cp*Rh(NH3)(H2O)2]-(3+) has been found for the clean conversion of methanol and water to hydrogen and carbon dioxide. The simple and easily available reaction steps can circumvent the formation of CO, therefore, making it possible to avoid inactivating catalysts and contaminating the hydrogen fuel. Different from conventional reforming method for hydrogen production, no additional alkaline or organic substances are required in this method. Valuable hydrogen can be obtained under ambient pressure at 70 C, corresponding TOF is 83.2 h 1. This is an unprecedented success in reforming methanol to hydrogen. Effects of reaction conditions, such as reaction temperature, initial methanol concentration and the initial p H value of buffer solution on the hydrogen evolution are all systematically investigated. In a certain range, higher reaction temperature will accelerate reaction rate. The slightly acidic condition is conducive to rapid hydrogen production. These findings are of great significance to the present establishment of the carbon-neutral methanol economy.
基金financial support granted by Ministry of Science and Technology of China(Nos.2016YFE0105700,2016YFA0200700)the National Natural Science Foundation of China(Nos.21373264,21573275)+2 种基金the Natural Science Foundation of Jiangsu Province(No.BK20150362)Suzhou Institute of Nano-tech and Nano-bionics(No.Y3AAA11004)Thousand Youth Talents Plan(No.Y3BQA11001)
文摘Formic acid(FA) dehydrogenation has attracted a lot of attentions since it is a convenient method for H_2 production. In this work, we designed a self-supporting fuel cell system, in which H_2 from FA is supplied into the fuel cell, and the exhaust heat from the fuel cell supported the FA dehydrogenation. In order to realize the system, we synthesized a highly active and selective homogeneous catalyst Ir Cp*Cl_2 bpym for FA dehydrogenation. The turnover frequency(TOF) of the catalyst for FA dehydrogenation is as high as7150 h^(-1)at 50°C, and is up to 144,000 h^(-1)at 90°C. The catalyst also shows excellent catalytic stability for FA dehydrogenation after several cycles of test. The conversion ratio of FA can achieve 93.2%, and no carbon monoxide is detected in the evolved gas. Therefore, the evolved gas could be applied in the proton exchange membrane fuel cell(PEMFC) directly. This is a potential technology for hydrogen storage and generation. The power density of the PEMFC driven by the evolved gas could approximate to that using pure hydrogen.