The damage characteristics and occurrence regularity of radish alternaria leaf spot, black rot, soft rot, virus disease and hollowness are introduced in the paper, and the corresponding control method is proposed from...The damage characteristics and occurrence regularity of radish alternaria leaf spot, black rot, soft rot, virus disease and hollowness are introduced in the paper, and the corresponding control method is proposed from two aspects of agricultural control and chemical control.展开更多
Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology r...Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.展开更多
Microwave absorbing materials(MAMs)characterized by high absorption efficiency and good environmental tolerance are highly desirable in practical applications.Both silicon carbide and carbon are considered as stable M...Microwave absorbing materials(MAMs)characterized by high absorption efficiency and good environmental tolerance are highly desirable in practical applications.Both silicon carbide and carbon are considered as stable MAMs under some rigorous conditions,while their composites still fail to produce satisfactory microwave absorption performance regardless of the improvements as compared with the individuals.Herein,we have successfully implemented compositional and structural engineering to fabricate hollow Si C/C microspheres with controllable composition.The simultaneous modulation on dielectric properties and impedance matching can be easily achieved as the change in the composition of these composites.The formation of hollow structure not only favors lightweight feature,but also generates considerable contribution to microwave attenuation capacity.With the synergistic effect of composition and structure,the optimized SiC/C composite exhibits excellent performance,whose the strongest reflection loss intensity and broadest effective absorption reach-60.8 dB and 5.1 GHz,respectively,and its microwave absorption properties are actually superior to those of most SiC/C composites in previous studies.In addition,the stability tests of microwave absorption capacity after exposure to harsh conditions and Radar Cross Section simulation data demonstrate that hollow SiC/C microspheres from compositional and structural optimization have a bright prospect in practical applications.展开更多
Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optim...Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optimized electron distribution holds great promise.Here,we have designed a threedimensional(3D)hollow Ni/NiMoN hierarchical structure with arrayed-sheet surface based on a onepot hydrothermal route for efficient urea-assisted HER based on a simple hydrothermal process.The Ni/NiMoN catalyst exhibits super-hydrophilic/aerophobic properties with a small droplet contact angle of 6.07°and an underwater bubble contact angle of 155.7°,thus facilitating an escape of bubbles from the electrodes.Density functional theory calculations and X-ray photoelectron spectroscopy results indicate the optimized electronic structure at the interface of Ni and NiMoN,which can promote the adsorption/desorption of reactants and intermediates.The virtues combining with a large specific surface area endow Ni/NiMoN with efficient catalytic activity of low potentials of 25 mV for HER and 1.33 V for UOR at10 mA cm^(-2).The coupled HER and UOR system demonstrates a low cell voltage of 1.42 V at 10 mA cm^(-2),which is approximately 209 mV lower than water electrolysis.展开更多
The plasma density enhancement outside hollow electrodes in capacitively coupled radio-frequency(RF) discharges is investigated by a two-dimensional(2D) particle-in-cell/Monte-Carlo collision(PIC/MCC) model. Results s...The plasma density enhancement outside hollow electrodes in capacitively coupled radio-frequency(RF) discharges is investigated by a two-dimensional(2D) particle-in-cell/Monte-Carlo collision(PIC/MCC) model. Results show that plasma exists inside the cavity when the sheath inside the hollow electrode hole is fully collapsed, which is an essential condition for the plasma density enhancement outside hollow electrodes. In addition, the existence of the electron density peak at the orifice is generated via the hollow cathode effect(HCE), which plays an important role in the density enhancement. It is also found that the radial width of bulk plasma at the orifice affects the magnitude of the density enhancement, and narrow radial plasma bulk width at the orifice is not beneficial to obtain high-density plasma outside hollow electrodes.Higher electron density at the orifice, combined with larger radial plasma bulk width at the orifice,causes higher electron density outside hollow electrodes. The results also imply that the HCE strength inside the cavity cannot be determined by the magnitude of the electron density outside hollow electrodes.展开更多
Radio frequency capacitively coupled plasma source(RF-CCP)with a hollow electrode can increase the electron density through the hollow cathode effect(HCE),which offers a method to modify the spatial profiles of the pl...Radio frequency capacitively coupled plasma source(RF-CCP)with a hollow electrode can increase the electron density through the hollow cathode effect(HCE),which offers a method to modify the spatial profiles of the plasma density.In this work,the variations of the HCE in one RF period are investigated by using a two-dimensional particle-in-cell/Monte-Carlo collision(PIC/MCC)model.The results show that the sheath electric field,the sheath potential drop,the sheath thickness,the radial plasma bulk width,the electron energy distribution function(EEDF),and the average electron energy in the cavity vary in one RF period.During the hollow electrode sheath's expansion phase,the secondary electron heating and sheath oscillation heating in the cavity are gradually enhanced,and the frequency of the electron pendular motion in the cavity gradually increases,hence the HCE is gradually enhanced.However,during the hollow electrode sheath's collapse phase,the secondary electron heating is gradually attenuated.In addition,when interacting with the gradually collapsed hollow electrode sheaths,high-energy plasma bulk electrons in the cavity will lose some energy.Furthermore,the frequency of the electron pendular motion in the cavity gradually decreases.Therefore,during the hollow electrode sheath's collapse phase,the HCE is gradually attenuated.展开更多
Booming low-power electric propulsion systems require 1–2 A hollow cathodes.Such cathodes are expected to go through more frequent ignitions in the low orbit,but the impact of cyclic ignitions on such 1–2 A barium t...Booming low-power electric propulsion systems require 1–2 A hollow cathodes.Such cathodes are expected to go through more frequent ignitions in the low orbit,but the impact of cyclic ignitions on such 1–2 A barium tungsten hollow cathodes with a heater was not clear.In this study,a 12,638-cyclic ignition test and a 6,000-hour-long life test on two identical cathodes were carried out.The discharge voltage of the cathode and the erosion of the orifice after cyclic ignition were all larger than that of the cathode after stable operation.This indicated that the impact of cycle ignition on the discharge performance of a low current BaO-W cathode with a heater was higher than that of stable operation.The results of the ion energy distribution function measured during the ignition period indicated that the main reason for the orifice expansion was ion bombardment.Therefore,it was necessary to pay attention to the number of ignitions for the lifetime of this kind of cathode.展开更多
Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult...Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult decomposition of discharge products at present.Here,we have developed N-doped carbon anchored atomically dispersed Ru sites cathode catalyst with open hollow structure(h-RuNC)for Lithium–oxygen battery.On one hand,the abundance of atomically dispersed Ru sites can effectively catalyze the formation and decomposition of discharge products,thereby greatly enhancing the redox kinetics.On the other hand,the open hollow structure not only enhances the mass activity of atomically dispersed Ru sites but also improves the diffusion efficiency of catalytic molecules.Therefore,the excellent activity from atomically dispersed Ru sites and the enhanced diffusion from open hollow structure respectively improve the redox kinetics and cycling stability,ultimately achieving a high-performance lithium–oxygen battery.展开更多
With the rapid development of flexible wearable electronics,the demand for stretchable energy storage devices has surged.In this work,a novel gradient-layered architecture was design based on single-pore hollow lignin...With the rapid development of flexible wearable electronics,the demand for stretchable energy storage devices has surged.In this work,a novel gradient-layered architecture was design based on single-pore hollow lignin nanospheres(HLNPs)-intercalated two-dimensional transition metal carbide(Ti_(3)C_(2)T_(x) MXene)for fabricating highly stretchable and durable supercapacitors.By depositing and inserting HLNPs in the MXene layers with a bottom-up decreasing gradient,a multilayered porous MXene structure with smooth ion channels was constructed by reducing the overstacking of MXene lamella.Moreover,the micro-chamber architecture of thin-walled lignin nanospheres effectively extended the contact area between lignin and MXene to improve ion and electron accessibility,thus better utilizing the pseudocapacitive property of lignin.All these strategies effectively enhanced the capacitive performance of the electrodes.In addition,HLNPs,which acted as a protective phase for MXene layer,enhanced mechanical properties of the wrinkled stretchable electrodes by releasing stress through slip and deformation during the stretch-release cycling and greatly improved the structural integrity and capacitive stability of the electrodes.Flexible electrodes and symmetric flexible all-solid-state supercapacitors capable of enduring 600%uniaxial tensile strain were developed with high specific capacitances of 1273 mF cm^(−2)(241 F g^(−1))and 514 mF cm^(−2)(95 F g^(−1)),respectively.Moreover,their capacitances were well preserved after 1000 times of 600%stretch-release cycling.This study showcased new possibilities of incorporating biobased lignin nanospheres in energy storage devices to fabricate stretchable devices leveraging synergies among various two-dimensional nanomaterials.展开更多
Sodium-sulfur(Na-S)and potassium-sulfur(K-S)batteries for use at room temperature have received widespread attention because of the abundance and low cost of their raw materials and their high energy density.However,t...Sodium-sulfur(Na-S)and potassium-sulfur(K-S)batteries for use at room temperature have received widespread attention because of the abundance and low cost of their raw materials and their high energy density.However,their development is restricted by the shuttling of polysulfides,large volume expansion and poor conductivity.To overcome these obstacles,an effective approach is to use carbon-based materials with abundant space for the sulfur that has sulfiphilic sites to immobilize it,and a high electrical conductivity.Hollow carbon spheres(HCSs)with a controllable structure and composition are promising for this purpose.We consider recent progress in optimizing the electrochemical performance of Na-/K-S batteries by using these materials.First,the advantages of HCSs,their synthesis methods,and strategies for preparing HCSs/sulfur composite materials are reviewed.Second,the use of HCSs in Na-/K-S batteries,along with mechanisms underlying the resulting performance improvement,are discussed.Finally,prospects for the further development of HCSs for metal−S batteries are presented.展开更多
The separation of aromatic/aliphatic hydrocarbon mixtures is crucial in the petrochemical industry.Pervaporation is regarded as a promising approach for the separation of aromatic compounds from alkanes. Developing me...The separation of aromatic/aliphatic hydrocarbon mixtures is crucial in the petrochemical industry.Pervaporation is regarded as a promising approach for the separation of aromatic compounds from alkanes. Developing membrane materials with efficient separation performance is still the main task since the membrane should provide chemical stability, high permeation flux, and selectivity. In this study, the hyperbranched polymer(HBP) was deposited on the outer surface of a polyvinylidene fluoride(PVDF)hollow-fiber ultrafiltration membrane by a facile dip-coating method. The dip-coating rate, HBP concentration, and thermal cross-linking temperature were regulated to optimize the membrane structure.The obtained HBP/PVDF hollow-fiber-composite membrane had a good separation performance for aromatic/aliphatic hydrocarbon mixtures. For the 50%/50%(mass) toluene/n-heptane mixture, the permeation flux of optimized composite membranes could reach 1766 g·m^(-2)·h^(-1), with a separation factor of 4.1 at 60℃. Therefore, the HBP/PVDF hollow-fiber-composite membrane has great application prospects in the pervaporation separation of aromatic/aliphatic hydrocarbon mixtures.展开更多
To address the low conductivity and easy agglomeration of transition metal sulfide nanoparticles,FeCoS_(4) nanoparticles embedded in S-doped hollow carbon(FeCoS_(4)@S-HC)composites were successfully fabricated through...To address the low conductivity and easy agglomeration of transition metal sulfide nanoparticles,FeCoS_(4) nanoparticles embedded in S-doped hollow carbon(FeCoS_(4)@S-HC)composites were successfully fabricated through a combination of hydrothermal processes and sulfidation treatment.The unique bowlshaped FeCoS_(4)/S-HC composites exhibit excellent structural stability with a high specific surface area of 303.7 m^(2)·g^(-1) and a pore volume of 0.93 cm^(3)·g^(-1).When applied as anode material for lithium-ion batteries,the FeCoS_(4)@S-HC anode exhibits efficient lithium storage with high reversible specific capacity(970.2 mA·h·g^(-1) at 100 mA·g^(-1))and enhanced cycling stability(574 mA·h·g^(-1) at 0.2 A·g^(-1) after 350 cycles,a capacity retention of 84%).The excellent lithium storage is attributed to the fact that the bimetallic FeCoS_(4) nanoparticles with abundant active sites can accelerate the electrochemical reaction kinetics,and the bowl-shaped S-HC structure can provide a stable mechanical structure to suppress volume expansion.展开更多
The selective hydrogenation of highly toxic phenolic compounds to generate alcohols with thermal stability,environmental friendliness,and non-toxicity is of great importance.Herein,a series of Co-based catalysts,named...The selective hydrogenation of highly toxic phenolic compounds to generate alcohols with thermal stability,environmental friendliness,and non-toxicity is of great importance.Herein,a series of Co-based catalysts,named Co@NCNTs,were designed and constructed by direct pyrolysis of hollow ZIF-67(HZIF-67)under H_(2)/Ar atmosphere.The evolution of the catalyst surface from the shell layer assembled by ZIF-67-derived particles to the in situ-grown hollow nitrogen-doped carbon nanotubes(NCNTs)with certain length and density is achieved by adjusting the pyrolysis atmosphere and temperature.Due to the synergistic effects of in situ-formed hollow NCNTs,well-dispersed Co nanoparticles,and intact carbon matrix,the as-prepared Co@NCNTs-0.10-450 catalyst exhibits superior catalytic performance in the hydrogenation of phenolic compounds to alcohols.The turnover frequency value of Co@NCNTs-0.10-450is 3.52 h^(-1),5.9 times higher than that of Co@NCNTs-0.40-450 and 4.5 times higher than that of Co@NCNTs-0.10-550,exceeding most previously reported non-noble metal catalysts.Our findings provide new insights into the development of non-precious metal,efficient,and cost-effective metal-organic framework-derived catalysts for the hydrogenation of phenolic compounds to alcohols.展开更多
The application of Li metal anodes in rechargeable batteries is impeded by safety issues arising from the severe volume changes and formation of dendritic Li deposits.Three‐dimensional hollow carbon is receiving incr...The application of Li metal anodes in rechargeable batteries is impeded by safety issues arising from the severe volume changes and formation of dendritic Li deposits.Three‐dimensional hollow carbon is receiving increasing attention as a host material capable of accommodating Li metal inside its cavity;however,uncontrollable and nonuniform deposition of Li remains a challenge.In this study,we synthesize metal–organic framework‐derived carbon microcapsules with heteroatom clusters(Zn and Ag)on the capsule walls and it is demonstrated that Ag‐assisted nucleation of Li metal alters the outward‐to‐inward growth in the microcapsule host.Zn‐incorporated microcapsules are prepared via chemical etching of zeolitic imidazole framework‐8 polyhedra and are subsequently decorated with Ag by a galvanic displacement reaction between Ag^(+) and metallic Zn.Galvanically introduced Ag significantly reduces the energy barrier and increases the reaction rate for Li nucleation in the microcapsule host upon Li plating.Through combined electrochemical,microstructural,and computational studies,we verify the beneficial role of Ag‐assisted Li nucleation in facilitating inward growth inside the cavity of the microcapsule host and,in turn,enhancing electrochemical performance.This study provides new insights into the design of reversible host materials for practical Li metal batteries.展开更多
Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their mac...Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their macroscopic assembly.The present study employed a gentle and direct self-assembly technique,wherein controlled growth of CNT sheaths occurred on the metal wire’s surface,followed by etching of the remaining metal to obtain the hollow tubes composed of CNTs.By controlling the growth time and temperature,it is possible to alter the thickness of the CNTs sheath.After immersing in a solution containing 1 g/L of CNTs at 60℃ for 24 h,the resulting CNTs layer achieved a thickness of up to 60μm.These hollow CNTs tubes with varying inner diameters were prepared through surface reinforcement using polymers and sacrificing metal wires,thereby exhibiting exceptional attributes such as robustness,flexibility,air tightness,and high adsorption capacity that effectively capture CO_(2) from the gas mixture.展开更多
The disparity in the transfer of carriers(electrons/mass)during the reaction in zinc-air batteries(ZABs)results in sluggish kinetics of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),along with e...The disparity in the transfer of carriers(electrons/mass)during the reaction in zinc-air batteries(ZABs)results in sluggish kinetics of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),along with elevated overpotentials,thereby imposing additional constraints on its utilization.Therefore,the pre-design and target-development of inexpensive,high-performance,and long-term stable bifunctional catalysts are urgently needed.In this work,an apically guiding dual-functional electrocatalyst(Ag-FeN_(x)-N-C)was prepared,in which a hierarchical porous nitrogen-doped carbon with three-dimensional(3D)hollow star-shaped structure is used as a substrate and high-conductivity Ag nanoparticles are coupled with iron nitride(FeN_(x))nanoparticles.Theoretical calculations indicate that the Mott-Schottky heterojunction as an inherent electric field comes from the two-phase bound of Ag and FeN_(x),of which electron accumulation in the FeN_(x)phase region and electron depletion in the Ag phase region promote orientated-guiding charge migration.The effective modulation of local electronic structures felicitously reforms the d-band electron-group distribution,and intellectually tunes the masstransfer reaction energy barriers for both ORR/OER.Additionally,the hollow star-s haped hierarchical porous structure provides an apical region for fast mass transfer.Experimental results show that the halfwave potential for ORR is 0.914 V,and the overpotential for OER is only 327 mV at 10 mA cm^(-2).A rechargeable ZAB with Ag-FeN_(x)-N-C as the air cathode demonstrates long-term cycling performance exceeding 1500 cycles(500 h),with a power density of 180 mW cm^(-2).Moreover,when employing AgFeN_(x)-N-C as the air cathode,flexible ZABs demonstrate a notable open-circuit voltage of 1.42 V and achieve a maximum power density of 65.6 mW cm^(-2).Ag-FeN_(x)-N-C shows guiding electron/mass transfer route and apical reaction microenvironment for the electrocatalyst architecture in the exploration prospects of ZABs.展开更多
Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challen...Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challenges due to the dissolution of intermediate reaction products.In this work,we aim to harness the advantages of Se while reducing its limitations by preparing a core-shell mesoporous carbon hollow sphere with a titanium nitride(C@TiN)host to load 63.9wt%Se as the positive electrode material for Al-Se batteries.Using the physical and chemical confinement offered by the hollow mesoporous carbon and TiN,the obtained core-shell mesoporous carbon hollow spheres coated with Se(Se@C@TiN)display superior utilization of the active material and remarkable cycling stability.As a result,Al-Se batteries equipped with the as-prepared Se@C@TiN composite positive electrodes show an initial discharge specific capacity of 377 mAh·g^(-1)at a current density of 1000 mA·g^(-1)while maintaining a discharge specific capacity of 86.0 mAh·g^(-1)over 200 cycles.This improved cycling performance is ascribed to the high electrical conductivity of the core-shell mesoporous carbon hollow spheres and the unique three-dimensional hierarchical architecture of Se@C@TiN.展开更多
The traditional automotive catalytic converter using commercial ceramic honeycomb carriers has many problems such as high back pressure,low engine efficiency,and high usage of precious metals.This study proposes a fou...The traditional automotive catalytic converter using commercial ceramic honeycomb carriers has many problems such as high back pressure,low engine efficiency,and high usage of precious metals.This study proposes a four-channel catalytic micro-reactor based on alumina hollow fiber membrane,which uses phase inversion method for structural molding and regulation.Due to the advantages of its carrier,it can achieve lower ignition temperature under low noble metal loading.With Pd/CeO_(2) at a loading rate of 2.3%(mass),the result showed that the reaction ignition temperature is even less than 160℃,which is more than 90℃ lower than the data of commercial ceramic substrates under similar catalyst loading and airspeed conditions.The technology in turn significantly reduces the energy consumption of the reaction.And stability tests were conducted under constant conditions for 1000 h,which proved that this catalytic converter has high catalytic efficiency and stability,providing prospects for the design of innovative catalytic converters in the future.展开更多
Electrochemical CO_(2) reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy conversion.The development of efficient catalysts with high conductivity and readily a...Electrochemical CO_(2) reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy conversion.The development of efficient catalysts with high conductivity and readily accessible active sites for CO_(2) electroreduction remains challenging yet indispensable.In this work,a reliable poly(ethyleneimine)(PEI)-assisted strategy is developed to prepare a hollow carbon nanocomposite comprising a single-site Ni-modified carbon shell and confined Ni nanoparticles(NPs)(denoted as Ni@NHCS),where PEI not only functions as a mediator to induce the highly dispersed growth of Ni NPs within hollow carbon spheres,but also as a nitrogen precursor to construct highly active atomically-dispersed Ni-Nx sites.Benefiting from the unique structural properties of Ni@NHCS,the aggregation and exposure of Ni NPs can be effectively prevented,while the accessibility of abundant catalytically active Ni-Nx sites can be ensured.As a result,Ni@NHCS exhibits a high CO partial current density of 26.9 mA cm^(-2) and a Faradaic efficiency of 93.0% at-1.0 V vs.RHE,outperforming those of its PEI-free analog.Apart from the excellent activity and selectivity,the shell confinement effect of the hollow carbon sphere endows this catalyst with long-term stability.The findings here are anticipated to help understand the structure-activity relationship in Ni-based carbon catalyst systems for electrocatalytic CO_(2) reduction.Furthermore,the PEI-assisted synthetic concept is potentially applicable to the preparation of high-performance metal-based nanoconfined materials tailored for diverse energy conversion applications and beyond.展开更多
Designing a step-scheme(S-scheme)heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H_(2)production activity.Herein,a hollow ZnO/ZnS S-scheme hetero...Designing a step-scheme(S-scheme)heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H_(2)production activity.Herein,a hollow ZnO/ZnS S-scheme heterojunction with O and Zn vacancies(VO,Zn-ZnO/ZnS)is rationally constructed via ion-exchange and calcination treatments.In such a photocatalytic system,the hollow structure combined with the introduction of dual vacancies endows the adequate light absorption.Moreover,the O and Zn vacancies serve as the trapping sites for photo-induced electrons and holes,respectively,which are beneficial for promoting the photo-induced carrier separation.Meanwhile,the S-scheme charge transfer mechanism can not only improve the separation and transfer efficiencies of photo-induced carrier but also retain the strong redox capacity.As expected,the optimized VO,Zn-ZnO/ZnS heterojunction exhibits a superior photocatalytic H_(2) production rate of 160.91 mmol g^(-1)h^(-1),approximately 643.6 times and 214.5 times with respect to that obtained on pure ZnO and ZnS,respectively.Simultaneously,the experimental results and density functional theory calculations disclose that the photo-induced carrier transfer pathway follows the S-scheme heterojunction mechanism and the introduction of O and Zn vacancies reduces the surface reaction barrier.This work provides an innovative strategy of vacancy engineering in S-scheme heterojunction for solar-to-fuel energy conversion.展开更多
文摘The damage characteristics and occurrence regularity of radish alternaria leaf spot, black rot, soft rot, virus disease and hollowness are introduced in the paper, and the corresponding control method is proposed from two aspects of agricultural control and chemical control.
基金financially supported by the National Natural Science Foundation of China (Nos.U2002212,52102058,52204414,52204413,and 52204412)the National Key R&D Program of China (Nos.2021YFC1910504,2019YFC1907101,2019YFC1907103,and 2017YFB0702304)+7 种基金the Key R&D Program of Ningxia Hui Autonomous Region,China (Nos.2021BEG01003 and2020BCE01001)the Xijiang Innovation and Entrepreneurship Team,China (No.2017A0109004)the Macao Young Scholars Program (No.AM2022024),Chinathe Beijing Natural Science Foundation (Nos.L212020 and 2214073),Chinathe Guangdong Basic and Applied Basic Research Foundation,China (Nos.2021A1515110998 and 2020A1515110408)the China Postdoctoral Science Foundation (No.2022M710349)the Fundamental Research Funds for the Central Universities,China (Nos.FRF-BD-20-24A,FRF-TP-20-031A1,FRF-IC-19-017Z,and 06500141)the Integration of Green Key Process Systems MIIT and Scientific and Technological Innovation Foundation of Foshan,China(Nos.BK22BE001 and BK21BE002)。
文摘Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.
基金supported by the National Natural Science Foundation of China(No.21676065 and No.52373262)China Postdoctoral Science Foundation(2021MD703944,2022T150782).
文摘Microwave absorbing materials(MAMs)characterized by high absorption efficiency and good environmental tolerance are highly desirable in practical applications.Both silicon carbide and carbon are considered as stable MAMs under some rigorous conditions,while their composites still fail to produce satisfactory microwave absorption performance regardless of the improvements as compared with the individuals.Herein,we have successfully implemented compositional and structural engineering to fabricate hollow Si C/C microspheres with controllable composition.The simultaneous modulation on dielectric properties and impedance matching can be easily achieved as the change in the composition of these composites.The formation of hollow structure not only favors lightweight feature,but also generates considerable contribution to microwave attenuation capacity.With the synergistic effect of composition and structure,the optimized SiC/C composite exhibits excellent performance,whose the strongest reflection loss intensity and broadest effective absorption reach-60.8 dB and 5.1 GHz,respectively,and its microwave absorption properties are actually superior to those of most SiC/C composites in previous studies.In addition,the stability tests of microwave absorption capacity after exposure to harsh conditions and Radar Cross Section simulation data demonstrate that hollow SiC/C microspheres from compositional and structural optimization have a bright prospect in practical applications.
基金financially supported by the National Key R&D Program of China(2022YFA1503003)the National Natural Science Foundation of China(91961111,22271081)+3 种基金the Natural Science Foundation of Heilongjiang Province(ZD2021B003)the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(UNPYSCT-2020004)The Basic Research Fund of Heilongjiang University in Heilongjiang Province(2021-KYYWF-0039)the Heilongjiang University Excellent Youth Foundation。
文摘Hydrogen evolution reaction(HER)and urea oxidation reaction(UOR)are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optimized electron distribution holds great promise.Here,we have designed a threedimensional(3D)hollow Ni/NiMoN hierarchical structure with arrayed-sheet surface based on a onepot hydrothermal route for efficient urea-assisted HER based on a simple hydrothermal process.The Ni/NiMoN catalyst exhibits super-hydrophilic/aerophobic properties with a small droplet contact angle of 6.07°and an underwater bubble contact angle of 155.7°,thus facilitating an escape of bubbles from the electrodes.Density functional theory calculations and X-ray photoelectron spectroscopy results indicate the optimized electronic structure at the interface of Ni and NiMoN,which can promote the adsorption/desorption of reactants and intermediates.The virtues combining with a large specific surface area endow Ni/NiMoN with efficient catalytic activity of low potentials of 25 mV for HER and 1.33 V for UOR at10 mA cm^(-2).The coupled HER and UOR system demonstrates a low cell voltage of 1.42 V at 10 mA cm^(-2),which is approximately 209 mV lower than water electrolysis.
文摘The plasma density enhancement outside hollow electrodes in capacitively coupled radio-frequency(RF) discharges is investigated by a two-dimensional(2D) particle-in-cell/Monte-Carlo collision(PIC/MCC) model. Results show that plasma exists inside the cavity when the sheath inside the hollow electrode hole is fully collapsed, which is an essential condition for the plasma density enhancement outside hollow electrodes. In addition, the existence of the electron density peak at the orifice is generated via the hollow cathode effect(HCE), which plays an important role in the density enhancement. It is also found that the radial width of bulk plasma at the orifice affects the magnitude of the density enhancement, and narrow radial plasma bulk width at the orifice is not beneficial to obtain high-density plasma outside hollow electrodes.Higher electron density at the orifice, combined with larger radial plasma bulk width at the orifice,causes higher electron density outside hollow electrodes. The results also imply that the HCE strength inside the cavity cannot be determined by the magnitude of the electron density outside hollow electrodes.
文摘Radio frequency capacitively coupled plasma source(RF-CCP)with a hollow electrode can increase the electron density through the hollow cathode effect(HCE),which offers a method to modify the spatial profiles of the plasma density.In this work,the variations of the HCE in one RF period are investigated by using a two-dimensional particle-in-cell/Monte-Carlo collision(PIC/MCC)model.The results show that the sheath electric field,the sheath potential drop,the sheath thickness,the radial plasma bulk width,the electron energy distribution function(EEDF),and the average electron energy in the cavity vary in one RF period.During the hollow electrode sheath's expansion phase,the secondary electron heating and sheath oscillation heating in the cavity are gradually enhanced,and the frequency of the electron pendular motion in the cavity gradually increases,hence the HCE is gradually enhanced.However,during the hollow electrode sheath's collapse phase,the secondary electron heating is gradually attenuated.In addition,when interacting with the gradually collapsed hollow electrode sheaths,high-energy plasma bulk electrons in the cavity will lose some energy.Furthermore,the frequency of the electron pendular motion in the cavity gradually decreases.Therefore,during the hollow electrode sheath's collapse phase,the HCE is gradually attenuated.
基金supported by the Key Projects of Schoolenterprise Joint Fund(No.U22B20120)the National Science Fund for Distinguished Young Scholars(No.52107141)。
文摘Booming low-power electric propulsion systems require 1–2 A hollow cathodes.Such cathodes are expected to go through more frequent ignitions in the low orbit,but the impact of cyclic ignitions on such 1–2 A barium tungsten hollow cathodes with a heater was not clear.In this study,a 12,638-cyclic ignition test and a 6,000-hour-long life test on two identical cathodes were carried out.The discharge voltage of the cathode and the erosion of the orifice after cyclic ignition were all larger than that of the cathode after stable operation.This indicated that the impact of cycle ignition on the discharge performance of a low current BaO-W cathode with a heater was higher than that of stable operation.The results of the ion energy distribution function measured during the ignition period indicated that the main reason for the orifice expansion was ion bombardment.Therefore,it was necessary to pay attention to the number of ignitions for the lifetime of this kind of cathode.
基金This work was supported by National Key R&D Program of China(2021YFF0500503)National Natural Science Foundation of China(21925202,U22B2071)International Joint Mission on Climate Change and Carbon Neutrality.
文摘Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult decomposition of discharge products at present.Here,we have developed N-doped carbon anchored atomically dispersed Ru sites cathode catalyst with open hollow structure(h-RuNC)for Lithium–oxygen battery.On one hand,the abundance of atomically dispersed Ru sites can effectively catalyze the formation and decomposition of discharge products,thereby greatly enhancing the redox kinetics.On the other hand,the open hollow structure not only enhances the mass activity of atomically dispersed Ru sites but also improves the diffusion efficiency of catalytic molecules.Therefore,the excellent activity from atomically dispersed Ru sites and the enhanced diffusion from open hollow structure respectively improve the redox kinetics and cycling stability,ultimately achieving a high-performance lithium–oxygen battery.
基金supported by Natural Science and Engineering Research Council of Canada(RGPIN-2017-06737)Canada Research Chairs program,the National Key Research and Development Program of China(2017YFD0601005,2022YFD0904201)+1 种基金the National Natural Science Foundation of China(51203075)the China Scholarship Council(Grant No.CSC202208320361).
文摘With the rapid development of flexible wearable electronics,the demand for stretchable energy storage devices has surged.In this work,a novel gradient-layered architecture was design based on single-pore hollow lignin nanospheres(HLNPs)-intercalated two-dimensional transition metal carbide(Ti_(3)C_(2)T_(x) MXene)for fabricating highly stretchable and durable supercapacitors.By depositing and inserting HLNPs in the MXene layers with a bottom-up decreasing gradient,a multilayered porous MXene structure with smooth ion channels was constructed by reducing the overstacking of MXene lamella.Moreover,the micro-chamber architecture of thin-walled lignin nanospheres effectively extended the contact area between lignin and MXene to improve ion and electron accessibility,thus better utilizing the pseudocapacitive property of lignin.All these strategies effectively enhanced the capacitive performance of the electrodes.In addition,HLNPs,which acted as a protective phase for MXene layer,enhanced mechanical properties of the wrinkled stretchable electrodes by releasing stress through slip and deformation during the stretch-release cycling and greatly improved the structural integrity and capacitive stability of the electrodes.Flexible electrodes and symmetric flexible all-solid-state supercapacitors capable of enduring 600%uniaxial tensile strain were developed with high specific capacitances of 1273 mF cm^(−2)(241 F g^(−1))and 514 mF cm^(−2)(95 F g^(−1)),respectively.Moreover,their capacitances were well preserved after 1000 times of 600%stretch-release cycling.This study showcased new possibilities of incorporating biobased lignin nanospheres in energy storage devices to fabricate stretchable devices leveraging synergies among various two-dimensional nanomaterials.
文摘Sodium-sulfur(Na-S)and potassium-sulfur(K-S)batteries for use at room temperature have received widespread attention because of the abundance and low cost of their raw materials and their high energy density.However,their development is restricted by the shuttling of polysulfides,large volume expansion and poor conductivity.To overcome these obstacles,an effective approach is to use carbon-based materials with abundant space for the sulfur that has sulfiphilic sites to immobilize it,and a high electrical conductivity.Hollow carbon spheres(HCSs)with a controllable structure and composition are promising for this purpose.We consider recent progress in optimizing the electrochemical performance of Na-/K-S batteries by using these materials.First,the advantages of HCSs,their synthesis methods,and strategies for preparing HCSs/sulfur composite materials are reviewed.Second,the use of HCSs in Na-/K-S batteries,along with mechanisms underlying the resulting performance improvement,are discussed.Finally,prospects for the further development of HCSs for metal−S batteries are presented.
基金financially supported by the National Natural Science Foundation of China (22178008, 22125801)Petrochina (2022DJ6004)。
文摘The separation of aromatic/aliphatic hydrocarbon mixtures is crucial in the petrochemical industry.Pervaporation is regarded as a promising approach for the separation of aromatic compounds from alkanes. Developing membrane materials with efficient separation performance is still the main task since the membrane should provide chemical stability, high permeation flux, and selectivity. In this study, the hyperbranched polymer(HBP) was deposited on the outer surface of a polyvinylidene fluoride(PVDF)hollow-fiber ultrafiltration membrane by a facile dip-coating method. The dip-coating rate, HBP concentration, and thermal cross-linking temperature were regulated to optimize the membrane structure.The obtained HBP/PVDF hollow-fiber-composite membrane had a good separation performance for aromatic/aliphatic hydrocarbon mixtures. For the 50%/50%(mass) toluene/n-heptane mixture, the permeation flux of optimized composite membranes could reach 1766 g·m^(-2)·h^(-1), with a separation factor of 4.1 at 60℃. Therefore, the HBP/PVDF hollow-fiber-composite membrane has great application prospects in the pervaporation separation of aromatic/aliphatic hydrocarbon mixtures.
基金financially supported by the National Natural Science Foundation of China(22379056,52102260)the Project funded by China Postdoctoral Science Foundation(2022M711545)the Carbon Peak and Carbon Neutrality Project(Breakthrough for Industry Prospect and Key Technologies)of Zhenjiang City(CG2023003)。
文摘To address the low conductivity and easy agglomeration of transition metal sulfide nanoparticles,FeCoS_(4) nanoparticles embedded in S-doped hollow carbon(FeCoS_(4)@S-HC)composites were successfully fabricated through a combination of hydrothermal processes and sulfidation treatment.The unique bowlshaped FeCoS_(4)/S-HC composites exhibit excellent structural stability with a high specific surface area of 303.7 m^(2)·g^(-1) and a pore volume of 0.93 cm^(3)·g^(-1).When applied as anode material for lithium-ion batteries,the FeCoS_(4)@S-HC anode exhibits efficient lithium storage with high reversible specific capacity(970.2 mA·h·g^(-1) at 100 mA·g^(-1))and enhanced cycling stability(574 mA·h·g^(-1) at 0.2 A·g^(-1) after 350 cycles,a capacity retention of 84%).The excellent lithium storage is attributed to the fact that the bimetallic FeCoS_(4) nanoparticles with abundant active sites can accelerate the electrochemical reaction kinetics,and the bowl-shaped S-HC structure can provide a stable mechanical structure to suppress volume expansion.
基金the National Key Research and Development Program(2021YFC3001103)the National Natural Science Foundation(22278209,22178165,21921006,22208149)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20211262,BK20220354)a project funded by the priority academic program development of Jiangsu higher education institutions(PAPD)of China。
文摘The selective hydrogenation of highly toxic phenolic compounds to generate alcohols with thermal stability,environmental friendliness,and non-toxicity is of great importance.Herein,a series of Co-based catalysts,named Co@NCNTs,were designed and constructed by direct pyrolysis of hollow ZIF-67(HZIF-67)under H_(2)/Ar atmosphere.The evolution of the catalyst surface from the shell layer assembled by ZIF-67-derived particles to the in situ-grown hollow nitrogen-doped carbon nanotubes(NCNTs)with certain length and density is achieved by adjusting the pyrolysis atmosphere and temperature.Due to the synergistic effects of in situ-formed hollow NCNTs,well-dispersed Co nanoparticles,and intact carbon matrix,the as-prepared Co@NCNTs-0.10-450 catalyst exhibits superior catalytic performance in the hydrogenation of phenolic compounds to alcohols.The turnover frequency value of Co@NCNTs-0.10-450is 3.52 h^(-1),5.9 times higher than that of Co@NCNTs-0.40-450 and 4.5 times higher than that of Co@NCNTs-0.10-550,exceeding most previously reported non-noble metal catalysts.Our findings provide new insights into the development of non-precious metal,efficient,and cost-effective metal-organic framework-derived catalysts for the hydrogenation of phenolic compounds to alcohols.
基金National Research Foundation,Grant/Award Numbers:NRF‐2018R1A5A1025594,NRF‐2022M3J1A1062644。
文摘The application of Li metal anodes in rechargeable batteries is impeded by safety issues arising from the severe volume changes and formation of dendritic Li deposits.Three‐dimensional hollow carbon is receiving increasing attention as a host material capable of accommodating Li metal inside its cavity;however,uncontrollable and nonuniform deposition of Li remains a challenge.In this study,we synthesize metal–organic framework‐derived carbon microcapsules with heteroatom clusters(Zn and Ag)on the capsule walls and it is demonstrated that Ag‐assisted nucleation of Li metal alters the outward‐to‐inward growth in the microcapsule host.Zn‐incorporated microcapsules are prepared via chemical etching of zeolitic imidazole framework‐8 polyhedra and are subsequently decorated with Ag by a galvanic displacement reaction between Ag^(+) and metallic Zn.Galvanically introduced Ag significantly reduces the energy barrier and increases the reaction rate for Li nucleation in the microcapsule host upon Li plating.Through combined electrochemical,microstructural,and computational studies,we verify the beneficial role of Ag‐assisted Li nucleation in facilitating inward growth inside the cavity of the microcapsule host and,in turn,enhancing electrochemical performance.This study provides new insights into the design of reversible host materials for practical Li metal batteries.
基金Project(ZCLTGS24B0101)supported by Zhejiang Provincial Natural Science Foundation of ChinaProject(Y202250501)supported by Scientific Research Fund of Zhejiang Provincial Education Department,ChinaProject supported by SRT Research Project of Jiaxing Nanhu University,China。
文摘Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their macroscopic assembly.The present study employed a gentle and direct self-assembly technique,wherein controlled growth of CNT sheaths occurred on the metal wire’s surface,followed by etching of the remaining metal to obtain the hollow tubes composed of CNTs.By controlling the growth time and temperature,it is possible to alter the thickness of the CNTs sheath.After immersing in a solution containing 1 g/L of CNTs at 60℃ for 24 h,the resulting CNTs layer achieved a thickness of up to 60μm.These hollow CNTs tubes with varying inner diameters were prepared through surface reinforcement using polymers and sacrificing metal wires,thereby exhibiting exceptional attributes such as robustness,flexibility,air tightness,and high adsorption capacity that effectively capture CO_(2) from the gas mixture.
基金the financial support of the National Natural Science Foundation of China(52002079,22378074,22179025 and U20A20340)the Guangdong Basic and Applied Basic Research Foundation(2022A1515140085)+2 种基金the Research Fund Program of Guangdong Provincial Key Laboratory of Fuel Cell Technology(FC202209)the Guangzhou Hongmian Project(HMJH-20200012)the Foshan Introducing Innovative and Entrepreneurial Teams(1920001000108)。
文摘The disparity in the transfer of carriers(electrons/mass)during the reaction in zinc-air batteries(ZABs)results in sluggish kinetics of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER),along with elevated overpotentials,thereby imposing additional constraints on its utilization.Therefore,the pre-design and target-development of inexpensive,high-performance,and long-term stable bifunctional catalysts are urgently needed.In this work,an apically guiding dual-functional electrocatalyst(Ag-FeN_(x)-N-C)was prepared,in which a hierarchical porous nitrogen-doped carbon with three-dimensional(3D)hollow star-shaped structure is used as a substrate and high-conductivity Ag nanoparticles are coupled with iron nitride(FeN_(x))nanoparticles.Theoretical calculations indicate that the Mott-Schottky heterojunction as an inherent electric field comes from the two-phase bound of Ag and FeN_(x),of which electron accumulation in the FeN_(x)phase region and electron depletion in the Ag phase region promote orientated-guiding charge migration.The effective modulation of local electronic structures felicitously reforms the d-band electron-group distribution,and intellectually tunes the masstransfer reaction energy barriers for both ORR/OER.Additionally,the hollow star-s haped hierarchical porous structure provides an apical region for fast mass transfer.Experimental results show that the halfwave potential for ORR is 0.914 V,and the overpotential for OER is only 327 mV at 10 mA cm^(-2).A rechargeable ZAB with Ag-FeN_(x)-N-C as the air cathode demonstrates long-term cycling performance exceeding 1500 cycles(500 h),with a power density of 180 mW cm^(-2).Moreover,when employing AgFeN_(x)-N-C as the air cathode,flexible ZABs demonstrate a notable open-circuit voltage of 1.42 V and achieve a maximum power density of 65.6 mW cm^(-2).Ag-FeN_(x)-N-C shows guiding electron/mass transfer route and apical reaction microenvironment for the electrocatalyst architecture in the exploration prospects of ZABs.
基金supported by the National Natural Science Foundation of China(No.52374350)China Postdoctoral Science Foundation(Nos.2020M680347 and 2021T140051)the Fundamental Research Funds for the Central Universities(No.FRF-TP-20-045A1)。
文摘Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challenges due to the dissolution of intermediate reaction products.In this work,we aim to harness the advantages of Se while reducing its limitations by preparing a core-shell mesoporous carbon hollow sphere with a titanium nitride(C@TiN)host to load 63.9wt%Se as the positive electrode material for Al-Se batteries.Using the physical and chemical confinement offered by the hollow mesoporous carbon and TiN,the obtained core-shell mesoporous carbon hollow spheres coated with Se(Se@C@TiN)display superior utilization of the active material and remarkable cycling stability.As a result,Al-Se batteries equipped with the as-prepared Se@C@TiN composite positive electrodes show an initial discharge specific capacity of 377 mAh·g^(-1)at a current density of 1000 mA·g^(-1)while maintaining a discharge specific capacity of 86.0 mAh·g^(-1)over 200 cycles.This improved cycling performance is ascribed to the high electrical conductivity of the core-shell mesoporous carbon hollow spheres and the unique three-dimensional hierarchical architecture of Se@C@TiN.
基金funded by the Natural Science Foundation of Jiangsu Province(BK20210252)。
文摘The traditional automotive catalytic converter using commercial ceramic honeycomb carriers has many problems such as high back pressure,low engine efficiency,and high usage of precious metals.This study proposes a four-channel catalytic micro-reactor based on alumina hollow fiber membrane,which uses phase inversion method for structural molding and regulation.Due to the advantages of its carrier,it can achieve lower ignition temperature under low noble metal loading.With Pd/CeO_(2) at a loading rate of 2.3%(mass),the result showed that the reaction ignition temperature is even less than 160℃,which is more than 90℃ lower than the data of commercial ceramic substrates under similar catalyst loading and airspeed conditions.The technology in turn significantly reduces the energy consumption of the reaction.And stability tests were conducted under constant conditions for 1000 h,which proved that this catalytic converter has high catalytic efficiency and stability,providing prospects for the design of innovative catalytic converters in the future.
文摘Electrochemical CO_(2) reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy conversion.The development of efficient catalysts with high conductivity and readily accessible active sites for CO_(2) electroreduction remains challenging yet indispensable.In this work,a reliable poly(ethyleneimine)(PEI)-assisted strategy is developed to prepare a hollow carbon nanocomposite comprising a single-site Ni-modified carbon shell and confined Ni nanoparticles(NPs)(denoted as Ni@NHCS),where PEI not only functions as a mediator to induce the highly dispersed growth of Ni NPs within hollow carbon spheres,but also as a nitrogen precursor to construct highly active atomically-dispersed Ni-Nx sites.Benefiting from the unique structural properties of Ni@NHCS,the aggregation and exposure of Ni NPs can be effectively prevented,while the accessibility of abundant catalytically active Ni-Nx sites can be ensured.As a result,Ni@NHCS exhibits a high CO partial current density of 26.9 mA cm^(-2) and a Faradaic efficiency of 93.0% at-1.0 V vs.RHE,outperforming those of its PEI-free analog.Apart from the excellent activity and selectivity,the shell confinement effect of the hollow carbon sphere endows this catalyst with long-term stability.The findings here are anticipated to help understand the structure-activity relationship in Ni-based carbon catalyst systems for electrocatalytic CO_(2) reduction.Furthermore,the PEI-assisted synthetic concept is potentially applicable to the preparation of high-performance metal-based nanoconfined materials tailored for diverse energy conversion applications and beyond.
文摘Designing a step-scheme(S-scheme)heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H_(2)production activity.Herein,a hollow ZnO/ZnS S-scheme heterojunction with O and Zn vacancies(VO,Zn-ZnO/ZnS)is rationally constructed via ion-exchange and calcination treatments.In such a photocatalytic system,the hollow structure combined with the introduction of dual vacancies endows the adequate light absorption.Moreover,the O and Zn vacancies serve as the trapping sites for photo-induced electrons and holes,respectively,which are beneficial for promoting the photo-induced carrier separation.Meanwhile,the S-scheme charge transfer mechanism can not only improve the separation and transfer efficiencies of photo-induced carrier but also retain the strong redox capacity.As expected,the optimized VO,Zn-ZnO/ZnS heterojunction exhibits a superior photocatalytic H_(2) production rate of 160.91 mmol g^(-1)h^(-1),approximately 643.6 times and 214.5 times with respect to that obtained on pure ZnO and ZnS,respectively.Simultaneously,the experimental results and density functional theory calculations disclose that the photo-induced carrier transfer pathway follows the S-scheme heterojunction mechanism and the introduction of O and Zn vacancies reduces the surface reaction barrier.This work provides an innovative strategy of vacancy engineering in S-scheme heterojunction for solar-to-fuel energy conversion.