There has been a continuous need for high active, excellently durable and low-cost electrocatalysts for rechargeable zinc-air batteries. Among many low-cost metal based candidates, transition metal oxides with the CNT...There has been a continuous need for high active, excellently durable and low-cost electrocatalysts for rechargeable zinc-air batteries. Among many low-cost metal based candidates, transition metal oxides with the CNTs composite have gained increasing attention. In this paper, the 3-D hollow sphere MnO_2 nanotube-supported Co_3O_4 nanoparticles and its carbon nanotubes hybrid material(Co_3 O_4/MnO_2-CNTs) have been synthesized via a simple co-precipitation method combined with post-heat treatment. The morphology and composition of the catalysts are thoroughly analyzed through SEM, TEM, TEM-mapping, XRD, EDX and XPS. In comparison with the commercial 20% Pt/C, Co_3O_4/MnO_2,bare MnO_2 nanotubes and CNTs, the hybrid Co_3O_4/MnO_2-CNTs-350 exhibits perfect bi-functional catalytic activity toward oxygen reduction reaction and oxygen evolution reaction under alkaline condition(0.1 M KOH). Therefore, high cell performances are achieved which result in an appropriate open circuit voltage(～1.47 V),a high discharge peak power density(340 mW cm^(-2)) and a large specific capacity(775 mAh g^(-1) at 10 mA cm^(-2)) for the primary Zn-air battery, a small charge-discharge voltage gap and a high cycle-life(504 cycles at 10 mA cm^(-2) with 10 min per cycle) for the rechargeable Zn-air battery. In particular, the simple synthesis method is suitable for a large-scale production of this bifunctional material due to a green, cost effective and readily available process.展开更多
One of the critical challenges that limit broad commercialization of proton exchange membrane fuel cells(PEMFC)is to reduce the usage of Pt while maintaining high power output and sufficient durability.Herein,a novel ...One of the critical challenges that limit broad commercialization of proton exchange membrane fuel cells(PEMFC)is to reduce the usage of Pt while maintaining high power output and sufficient durability.Herein,a novel bifunctional layer consisting of vertically aligned carbon nanotubes(VACNTs)and nanoparticles of Pt-Co catalysts(Pt-Co/VACNTs)is reported for highperformance PEMFCs.Readily prepared by a two-step process,the Pt-Co/VACNTs layer with a hydrophilic catalyst-loaded side and a hydrophobic gas diffusion side enables a PTFE-free electrode structure with fully exposed catalyst active sites and superior gas–water diffusion capability.When tested in a PEMFC,the bi-functional Pt-Co/VACNTs layer with ultralow Pt loading(~65μgcathodecm-2)demonstrates a power density of 19.5 kW gPt cathode-1 at 0.6 V,more than seven times that of a cell with commercial Pt/C catalyst(2.7 kW gPt cathode-1 at 0.6 V)at a loading of 400μgcathodecm-2 tested under similar conditions.This remarkable design of VACNTs-based catalyst with dual functionalities enables much lower Pt loading,faster mass transport,and higher electrochemical performance and stability.Further,the preparation procedure can be easily scaled up for low-cost fabrication and commercialization.展开更多
The synthesis of ultrasmall metal nanoclusters(NCs) with high catalytic activities is of great importance for the development of clean and renewable energy technologies but remains a challenge. Here we report a facile...The synthesis of ultrasmall metal nanoclusters(NCs) with high catalytic activities is of great importance for the development of clean and renewable energy technologies but remains a challenge. Here we report a facile wet-chemical method to prepare ~1.0 nm Au Pd NCs supported on amine-functionalized carbon blacks. The Au Pd NCs exhibit a specific activity of 5.98 mA cm_(AuPd)^(-2)and mass activity of 5.25 A mg_(auPd)^(-1) for ethanol electrooxidation, which are far better than those of commercial Pd/C catalysts(1.74 mAcm_(AuPd)^(-2) and 0.54 A mg_(Pd)^(-1) ). For formic acid dehydrogenation, the Au Pd NCs have an initial turn over frequency of 49339 h^(-1) at 298 K without any additive, which is much higher than those obtained for most of reported Au Pd catalysts. The reported synthesis may represent a facile and low-cost approach to prepare other ultrasmall metal NCs with high catalytic activities for various applications.展开更多
We report an organic/inorganic hybridized nanocomposite consisting of a bi-functional poly（N-vinyl）-3-[p-nitrophenylazo]carbazolyl serves as a polymeric charge-transporting and second-order nonliner optical matrix, ...We report an organic/inorganic hybridized nanocomposite consisting of a bi-functional poly（N-vinyl）-3-[p-nitrophenylazo]carbazolyl serves as a polymeric charge-transporting and second-order nonliner optical matrix, and CdS nanoparticles as photosensitizers to manifest photorefractive （PR） effect. The unpoled PVNPAK film exhibits a second harmonic generation （SHG） coefficient of 4.7 pm/V due to the possibility of self-alignment of the azo chromophore. Significant enhancement of photoconductivity is noticed with the increase of CdS nanoparticles concentration. The photorefractive property of the polymer nanocomposites were determined by two-beam coupling （TBC） experiment. The TBC gain and diffraction efficiency of 11.89 cm-1 and 3.2% were obtained for PVNPAK/CdS at zero electrical field.展开更多
A novel bi-functional photorefractive acrylate polymer with pendant carbazolyl groups and azo derivatives as side chains was synthesized. Photorefractive experiments showed a high two-beam coupling gain coefficient of...A novel bi-functional photorefractive acrylate polymer with pendant carbazolyl groups and azo derivatives as side chains was synthesized. Photorefractive experiments showed a high two-beam coupling gain coefficient of 93 cm(-1), diffraction efficiency of 12% and electro-optic coefficient of 26 pm/V were obtained.展开更多
The aim of this theoretical investigation is the description of the multicomponent mass transfer process in the Nano- Composites (NC)—novel materials with the bi-functional matrix. The new theoretical NC Model is ass...The aim of this theoretical investigation is the description of the multicomponent mass transfer process in the Nano- Composites (NC)—novel materials with the bi-functional matrix. The new theoretical NC Model is assigned for the modern theoretical investigations of the multicomponent mass transfer kinetics in the bi-functional NC materials. This NC Model for the multicomponent mass transfer in the bi-functional NC matrix includes into the consideration the proposed key conception—two co-existing routes: I—chemical reactions onto the active NC centers-sites, and II—diffusion mass transfer inside the bi-functional NC matrix. All the results are presented in the terms of the additional key concept: propagating multicomponent concentration waves (W+) in the NC matrix. The used W+ concept for the description of the multicomponent NC mass transfer kinetics give the clear interpretation of the computerized results. The mass transfer process in the NC matrix has been described theoretically by computerized simulation. The results of the calculations are new and illustrated by author’s animations showing visually the propagation of the multicomponent concentration waves (W) inside the various NC matrixes: r-beads, cylindrical ro-fibers, or planar L-membranes. Two variants of modeling for mass transfer diffusion kinetics in the bi-functional NC matrixes with one (Variant 1), or two (Variant 2) dissociation-association reactions at the active nano-sites (R0) are considered theoretically.展开更多
Carbon nanotubes/graphene hybrid materials with excellent physicochemical properties can be widely ap-plied in the fields of energy storage,electrocatalysis,sensing,etc.Reducing the self-stacking and achiev-ing covale...Carbon nanotubes/graphene hybrid materials with excellent physicochemical properties can be widely ap-plied in the fields of energy storage,electrocatalysis,sensing,etc.Reducing the self-stacking and achiev-ing covalent interaction between carbon nanotubes and graphene are important to ensure a stable hi-erarchical architecture and effective mass transfer.Herein,we propose a one-step strategy to synthesize 3D interconnected carbon nanotubes/graphene hybrids on the easy-to-remove biomass-derived substrate.The calcined natural cuttlebone as bi-functional catalyst precursor can simultaneously grow carbon nan-otubes and graphene by one-step chemical vapor deposition without the addition of extra metal catalysts,while the interconnected structure can act as the porous template for graphene growth.The simultane-ous growth process can obtain covalent bonding between carbon nanotubes and graphene,while the crystalline quality and interlayer space can be adjusted by different carbon sources and growth parame-ters(e.g.,temperature).The one-step grown carbon nanotubes/graphene hybrids with seamless interfaces and hierarchical interconnected 3D structure can effectively enhance the electron transfer as well as the electrolyte infiltration efficiency.When utilized as lithium-ion batteries(LIBs)anode,a high specific ca-pacity(544 mAh g^(-1) at 0.1 A g^(-1)),good rate capability(200 mAh g^(-1) at 6.4 A g^(-1) with an ultrashort charge time of 113 s),and excellent cyclic stability can be achieved.This simple and one-step carbon nanotubes/graphene hybrids fabrication strategy can be easily scale-up and applied in various fields.展开更多
Particulate materials possessing dual functionalities have received tremendous investigations in many fields,owing to their superiority over mono-functional counterparts and their potential for process integration and...Particulate materials possessing dual functionalities have received tremendous investigations in many fields,owing to their superiority over mono-functional counterparts and their potential for process integration and intensification.This review focuses on bi-functional catalytic particles which also serve as sorbents/adsorbents or heat suppliers in the scheme of various thermo-chemical processes,enabling inherent separation or energy conservation within single-step operation.Bi-functional particles applied for integration of reaction and separation including sorption-enhanced hydrogen production and integrated capture and catalytic conversion processes are reviewed in detail,providing insights into material design and key performance indicators.On the other hand,bi-functional particles applied for integration of reaction and non-thermal radiation heating,including electrothermal and photothermal assisted heterogeneously catalyzed reactions,are also reviewed,with emphasis on the material property and energy efficiency improvement.These bi-functional particles show broad adaptability and feasibility in various reactions operated in integrated and intensified schemes,affording huge potentials for further improving productivity and efficiency in thermo-chemical processes.展开更多
A series of Ni/HZSM-5 and Ni/HIM-5 bi-functional catalysts were synthesized and applied to the aqueous-phase hydrodeoxygenation(HDO)of phenol.The Ni dispersibility and particle sizes were shown to be directly related ...A series of Ni/HZSM-5 and Ni/HIM-5 bi-functional catalysts were synthesized and applied to the aqueous-phase hydrodeoxygenation(HDO)of phenol.The Ni dispersibility and particle sizes were shown to be directly related to the porosity and crystal sizes of the parent zeolites,which further influenced the catalytic performances.The large pores and small crystal sizes of the parent zeolites were beneficial for dispersing Ni and forming small Ni particles,and the corresponding Ni/zeolite catalyst exhibited a higher phenol conversion and selectivity towards hydrocarbons.Importantly,the Ni/HIM-5 bi-functional catalyst exhibited a high activity(98.3%)and high selectivity for hydrocarbons(98.8%)when heated at 220°C for 1 h and is thus a new potential catalyst for the HDO of phenolics to form hydrocarbons in the aqueous phase.展开更多
Simultaneous broadband absorption and polarization conversion are crucial in many practical applications,especially in terahertz communications.Thus,actively tunable metamaterial systems can exploit the graphene-based...Simultaneous broadband absorption and polarization conversion are crucial in many practical applications,especially in terahertz communications.Thus,actively tunable metamaterial systems can exploit the graphene-based nanomaterials derived from renewable resources because of the flexible surface conductivity and selective permeability of the nanomaterials at terahertz frequencies.In this paper,we propose a graphene-based active tunable bifunctional metasurface for dynamic terahertz absorption and polarization conversion.The graphene ring presents a certain opening angle(A)along the diagonal of the xoy plane.When A=0°,the proposed metasurface behaves as a broadband absorber.Numerical results show the feasibility of achieving this polarization-insensitive absorber with nearly 100%absorptance,and the bandwidth of its 90%absorptance is 1.22 THz under normal incidence.Alternatively,when A=40°after optimization,the proposed metasurface serves as a broadband polarization convertor,resulting in robust broadband polarization conversion ratio(PCR)curves with a bandwidth surpassing 0.5 THz in the reflection spectrum.To tune the PCR response or the broad absorption spectrum of graphene,we change the Fermi energy of graphene dynamically from 0 to 0.9 eV.Furthermore,both the broadband absorption and the linear polarization conversion spectra of the proposed metasurface exhibit insensitivity to the incident angle,allowing large incident angles within 40°under high-performance operating conditions.To demonstrate the physical process,we present the impedance matching theory and measure electric field distributions.This architecture in the THz frequency range has several applications,such as in modulators,sensors,stealth,and optoelectronic switches.THz wave polarization and beam steering also have broad application prospects in the field of intelligent systems.展开更多
Bi-functional electrocatalysts for acid overall water splitting reactions are crucial but still challenging to the development of proton exchange membrane water electrolysis.Herein,an efficient bi-functional catalyst ...Bi-functional electrocatalysts for acid overall water splitting reactions are crucial but still challenging to the development of proton exchange membrane water electrolysis.Herein,an efficient bi-functional catalyst of Ir/MoS_(2) nanoflowers(Ir/MoS_(2) NFs) catalyst was reported for acidic water electrolysis which can be constructed by coupling three-dimensionally interconnected MoS_(2) NFs with ultrafine Ir nanoparticles.A more suitable adsorption ability for the H* and *OOH intermediates was revealed,where the Ir sites were proposed as the main active center and MoS_(2) promoted the charge relocation to electronically modify the interfacial structure.The significant interfacial charge redistribution between the MoS_(2) NFs and the Ir active sites synergistically induced excellent catalytic activity and stability for the water electrolysis reaction.Specifically,the catalyst required overpotentials of 270 and 35 mV to reach a kinetic current density of 10 mA cm^(-2)for OER and HER,respectively,loading on the glass carbon electrode,with high catalytic kinetics,stability,and catalytic efficiency.A two-electrode system constructed by Ir/MoS_(2) NFs drove 10 mA cm^(-2)at a cell voltage of 1.55 V,about 70 mV lower than that of the commercial Pt/C||IrO_(2) system.In addition,partial surface oxidation of Ir nanoparticles to generate high-valent Ir species was also found significant to accelerate OER.The enhanced catalytic performance was attributed to the strong metal-support interaction in the Ir/MoS_(2) NFs catalyst system that changed the electronic structure of Ir metal and promoted the synergistic catalytic effect between Ir and MoS_(2) NFs.The work presented a novel platform of Ir-catalyst for proton exchange membrane water electrolysis.展开更多
基金financial support from the National Natural Science Foundation of China (U1510120, 91645110)the Project of Introducing Overseas Intelligence High Education of China (2017-2018)+1 种基金the Graduate Thesis Innovation Foundation of Donghua University (EG2016034)the College of Environmental Science and Engineering, State Environmental Protection Engineering Center for Pollution Treatment and Control in Textile Industry, Donghua University
文摘There has been a continuous need for high active, excellently durable and low-cost electrocatalysts for rechargeable zinc-air batteries. Among many low-cost metal based candidates, transition metal oxides with the CNTs composite have gained increasing attention. In this paper, the 3-D hollow sphere MnO_2 nanotube-supported Co_3O_4 nanoparticles and its carbon nanotubes hybrid material(Co_3 O_4/MnO_2-CNTs) have been synthesized via a simple co-precipitation method combined with post-heat treatment. The morphology and composition of the catalysts are thoroughly analyzed through SEM, TEM, TEM-mapping, XRD, EDX and XPS. In comparison with the commercial 20% Pt/C, Co_3O_4/MnO_2,bare MnO_2 nanotubes and CNTs, the hybrid Co_3O_4/MnO_2-CNTs-350 exhibits perfect bi-functional catalytic activity toward oxygen reduction reaction and oxygen evolution reaction under alkaline condition(0.1 M KOH). Therefore, high cell performances are achieved which result in an appropriate open circuit voltage(～1.47 V),a high discharge peak power density(340 mW cm^(-2)) and a large specific capacity(775 mAh g^(-1) at 10 mA cm^(-2)) for the primary Zn-air battery, a small charge-discharge voltage gap and a high cycle-life(504 cycles at 10 mA cm^(-2) with 10 min per cycle) for the rechargeable Zn-air battery. In particular, the simple synthesis method is suitable for a large-scale production of this bifunctional material due to a green, cost effective and readily available process.
基金supported by the National Natural Science Foundation of China under(No.21878158,2182880,51678291)Jiangsu Natural Science Foundation for Distinguished Young Scholars(No.BK20170043)+3 种基金the National Key R&D Program of China(2018YFB1502903)Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)China Postdoctoral Science Foundation(2019M660112)the Jiangsu Postdoctoral Science Funding Project
文摘One of the critical challenges that limit broad commercialization of proton exchange membrane fuel cells(PEMFC)is to reduce the usage of Pt while maintaining high power output and sufficient durability.Herein,a novel bifunctional layer consisting of vertically aligned carbon nanotubes(VACNTs)and nanoparticles of Pt-Co catalysts(Pt-Co/VACNTs)is reported for highperformance PEMFCs.Readily prepared by a two-step process,the Pt-Co/VACNTs layer with a hydrophilic catalyst-loaded side and a hydrophobic gas diffusion side enables a PTFE-free electrode structure with fully exposed catalyst active sites and superior gas–water diffusion capability.When tested in a PEMFC,the bi-functional Pt-Co/VACNTs layer with ultralow Pt loading(~65μgcathodecm-2)demonstrates a power density of 19.5 kW gPt cathode-1 at 0.6 V,more than seven times that of a cell with commercial Pt/C catalyst(2.7 kW gPt cathode-1 at 0.6 V)at a loading of 400μgcathodecm-2 tested under similar conditions.This remarkable design of VACNTs-based catalyst with dual functionalities enables much lower Pt loading,faster mass transport,and higher electrochemical performance and stability.Further,the preparation procedure can be easily scaled up for low-cost fabrication and commercialization.
基金supported by the National Natural Science Foundation of China (51901083)the Fundamental Research Funds for the Central Universities。
文摘The synthesis of ultrasmall metal nanoclusters(NCs) with high catalytic activities is of great importance for the development of clean and renewable energy technologies but remains a challenge. Here we report a facile wet-chemical method to prepare ~1.0 nm Au Pd NCs supported on amine-functionalized carbon blacks. The Au Pd NCs exhibit a specific activity of 5.98 mA cm_(AuPd)^(-2)and mass activity of 5.25 A mg_(auPd)^(-1) for ethanol electrooxidation, which are far better than those of commercial Pd/C catalysts(1.74 mAcm_(AuPd)^(-2) and 0.54 A mg_(Pd)^(-1) ). For formic acid dehydrogenation, the Au Pd NCs have an initial turn over frequency of 49339 h^(-1) at 298 K without any additive, which is much higher than those obtained for most of reported Au Pd catalysts. The reported synthesis may represent a facile and low-cost approach to prepare other ultrasmall metal NCs with high catalytic activities for various applications.
基金Funded by the National Natural Science Foundation of China (No.50802069)the Natural Science Foundation of Wuhan University of Tech-nology (471-38650378)
文摘We report an organic/inorganic hybridized nanocomposite consisting of a bi-functional poly（N-vinyl）-3-[p-nitrophenylazo]carbazolyl serves as a polymeric charge-transporting and second-order nonliner optical matrix, and CdS nanoparticles as photosensitizers to manifest photorefractive （PR） effect. The unpoled PVNPAK film exhibits a second harmonic generation （SHG） coefficient of 4.7 pm/V due to the possibility of self-alignment of the azo chromophore. Significant enhancement of photoconductivity is noticed with the increase of CdS nanoparticles concentration. The photorefractive property of the polymer nanocomposites were determined by two-beam coupling （TBC） experiment. The TBC gain and diffraction efficiency of 11.89 cm-1 and 3.2% were obtained for PVNPAK/CdS at zero electrical field.
文摘A novel bi-functional photorefractive acrylate polymer with pendant carbazolyl groups and azo derivatives as side chains was synthesized. Photorefractive experiments showed a high two-beam coupling gain coefficient of 93 cm(-1), diffraction efficiency of 12% and electro-optic coefficient of 26 pm/V were obtained.
文摘The aim of this theoretical investigation is the description of the multicomponent mass transfer process in the Nano- Composites (NC)—novel materials with the bi-functional matrix. The new theoretical NC Model is assigned for the modern theoretical investigations of the multicomponent mass transfer kinetics in the bi-functional NC materials. This NC Model for the multicomponent mass transfer in the bi-functional NC matrix includes into the consideration the proposed key conception—two co-existing routes: I—chemical reactions onto the active NC centers-sites, and II—diffusion mass transfer inside the bi-functional NC matrix. All the results are presented in the terms of the additional key concept: propagating multicomponent concentration waves (W+) in the NC matrix. The used W+ concept for the description of the multicomponent NC mass transfer kinetics give the clear interpretation of the computerized results. The mass transfer process in the NC matrix has been described theoretically by computerized simulation. The results of the calculations are new and illustrated by author’s animations showing visually the propagation of the multicomponent concentration waves (W) inside the various NC matrixes: r-beads, cylindrical ro-fibers, or planar L-membranes. Two variants of modeling for mass transfer diffusion kinetics in the bi-functional NC matrixes with one (Variant 1), or two (Variant 2) dissociation-association reactions at the active nano-sites (R0) are considered theoretically.
基金the financially supported from the National Nat-ural Science Foundation of China(Nos.21978178,22008157,and 21776187)the Distinguished Young Scholars for the Natural Science Foundation of Sichuan Province(No.2023NSFSC1915)。
文摘Carbon nanotubes/graphene hybrid materials with excellent physicochemical properties can be widely ap-plied in the fields of energy storage,electrocatalysis,sensing,etc.Reducing the self-stacking and achiev-ing covalent interaction between carbon nanotubes and graphene are important to ensure a stable hi-erarchical architecture and effective mass transfer.Herein,we propose a one-step strategy to synthesize 3D interconnected carbon nanotubes/graphene hybrids on the easy-to-remove biomass-derived substrate.The calcined natural cuttlebone as bi-functional catalyst precursor can simultaneously grow carbon nan-otubes and graphene by one-step chemical vapor deposition without the addition of extra metal catalysts,while the interconnected structure can act as the porous template for graphene growth.The simultane-ous growth process can obtain covalent bonding between carbon nanotubes and graphene,while the crystalline quality and interlayer space can be adjusted by different carbon sources and growth parame-ters(e.g.,temperature).The one-step grown carbon nanotubes/graphene hybrids with seamless interfaces and hierarchical interconnected 3D structure can effectively enhance the electron transfer as well as the electrolyte infiltration efficiency.When utilized as lithium-ion batteries(LIBs)anode,a high specific ca-pacity(544 mAh g^(-1) at 0.1 A g^(-1)),good rate capability(200 mAh g^(-1) at 6.4 A g^(-1) with an ultrashort charge time of 113 s),and excellent cyclic stability can be achieved.This simple and one-step carbon nanotubes/graphene hybrids fabrication strategy can be easily scale-up and applied in various fields.
基金supported by the National Natural Science Foundation of China(Grant Nos.22078106,22008044)Guangdong Natural Science Foundation(Grant No.2017A030312005).
文摘Particulate materials possessing dual functionalities have received tremendous investigations in many fields,owing to their superiority over mono-functional counterparts and their potential for process integration and intensification.This review focuses on bi-functional catalytic particles which also serve as sorbents/adsorbents or heat suppliers in the scheme of various thermo-chemical processes,enabling inherent separation or energy conservation within single-step operation.Bi-functional particles applied for integration of reaction and separation including sorption-enhanced hydrogen production and integrated capture and catalytic conversion processes are reviewed in detail,providing insights into material design and key performance indicators.On the other hand,bi-functional particles applied for integration of reaction and non-thermal radiation heating,including electrothermal and photothermal assisted heterogeneously catalyzed reactions,are also reviewed,with emphasis on the material property and energy efficiency improvement.These bi-functional particles show broad adaptability and feasibility in various reactions operated in integrated and intensified schemes,affording huge potentials for further improving productivity and efficiency in thermo-chemical processes.
基金This work was supported by the National Natural Science Foundation of China(Grant No.21908225)the National Key Research and Development Program of China(Grant No.2016YFB0600505)Youth Innovation Promotion Association,CAS(2014037).
文摘A series of Ni/HZSM-5 and Ni/HIM-5 bi-functional catalysts were synthesized and applied to the aqueous-phase hydrodeoxygenation(HDO)of phenol.The Ni dispersibility and particle sizes were shown to be directly related to the porosity and crystal sizes of the parent zeolites,which further influenced the catalytic performances.The large pores and small crystal sizes of the parent zeolites were beneficial for dispersing Ni and forming small Ni particles,and the corresponding Ni/zeolite catalyst exhibited a higher phenol conversion and selectivity towards hydrocarbons.Importantly,the Ni/HIM-5 bi-functional catalyst exhibited a high activity(98.3%)and high selectivity for hydrocarbons(98.8%)when heated at 220°C for 1 h and is thus a new potential catalyst for the HDO of phenolics to form hydrocarbons in the aqueous phase.
基金supported by the High Level Talent Project of Basic and Applied Basic Research(Natural Science)of Hainan Province in 2019(No.2019RC158)by the Project of the Education Department of Hainan Province(No.Hnky2020ZD-2),all support is gratefully acknowledged.
文摘Simultaneous broadband absorption and polarization conversion are crucial in many practical applications,especially in terahertz communications.Thus,actively tunable metamaterial systems can exploit the graphene-based nanomaterials derived from renewable resources because of the flexible surface conductivity and selective permeability of the nanomaterials at terahertz frequencies.In this paper,we propose a graphene-based active tunable bifunctional metasurface for dynamic terahertz absorption and polarization conversion.The graphene ring presents a certain opening angle(A)along the diagonal of the xoy plane.When A=0°,the proposed metasurface behaves as a broadband absorber.Numerical results show the feasibility of achieving this polarization-insensitive absorber with nearly 100%absorptance,and the bandwidth of its 90%absorptance is 1.22 THz under normal incidence.Alternatively,when A=40°after optimization,the proposed metasurface serves as a broadband polarization convertor,resulting in robust broadband polarization conversion ratio(PCR)curves with a bandwidth surpassing 0.5 THz in the reflection spectrum.To tune the PCR response or the broad absorption spectrum of graphene,we change the Fermi energy of graphene dynamically from 0 to 0.9 eV.Furthermore,both the broadband absorption and the linear polarization conversion spectra of the proposed metasurface exhibit insensitivity to the incident angle,allowing large incident angles within 40°under high-performance operating conditions.To demonstrate the physical process,we present the impedance matching theory and measure electric field distributions.This architecture in the THz frequency range has several applications,such as in modulators,sensors,stealth,and optoelectronic switches.THz wave polarization and beam steering also have broad application prospects in the field of intelligent systems.
基金supported by the National Natural Science Foundation of China (21972124, 22272148)the Priority Academic Program Development of Jiangsu Higher Education Institution。
文摘Bi-functional electrocatalysts for acid overall water splitting reactions are crucial but still challenging to the development of proton exchange membrane water electrolysis.Herein,an efficient bi-functional catalyst of Ir/MoS_(2) nanoflowers(Ir/MoS_(2) NFs) catalyst was reported for acidic water electrolysis which can be constructed by coupling three-dimensionally interconnected MoS_(2) NFs with ultrafine Ir nanoparticles.A more suitable adsorption ability for the H* and *OOH intermediates was revealed,where the Ir sites were proposed as the main active center and MoS_(2) promoted the charge relocation to electronically modify the interfacial structure.The significant interfacial charge redistribution between the MoS_(2) NFs and the Ir active sites synergistically induced excellent catalytic activity and stability for the water electrolysis reaction.Specifically,the catalyst required overpotentials of 270 and 35 mV to reach a kinetic current density of 10 mA cm^(-2)for OER and HER,respectively,loading on the glass carbon electrode,with high catalytic kinetics,stability,and catalytic efficiency.A two-electrode system constructed by Ir/MoS_(2) NFs drove 10 mA cm^(-2)at a cell voltage of 1.55 V,about 70 mV lower than that of the commercial Pt/C||IrO_(2) system.In addition,partial surface oxidation of Ir nanoparticles to generate high-valent Ir species was also found significant to accelerate OER.The enhanced catalytic performance was attributed to the strong metal-support interaction in the Ir/MoS_(2) NFs catalyst system that changed the electronic structure of Ir metal and promoted the synergistic catalytic effect between Ir and MoS_(2) NFs.The work presented a novel platform of Ir-catalyst for proton exchange membrane water electrolysis.
