The self-charging concept has drawn considerable attention due to its excellent ability to achieve environmental energy harvesting,conversion and storage without an external power supply.However,most self-charging des...The self-charging concept has drawn considerable attention due to its excellent ability to achieve environmental energy harvesting,conversion and storage without an external power supply.However,most self-charging designs assembled by multiple energy harvesting,conversion and storage materials increase the energy transfer loss;the environmental energy supply is generally limited by climate and meteorological conditions,hindering the potential application of these selfpowered devices to be available at all times.Based on aerobic autoxidation of catechol,which is similar to the electrochemical oxidation of the catechol groups on the carbon materials under an electrical charge,we proposed an air-breathing chemical self-charge concept based on the aerobic autoxidation of catechol groups on oxygen-enriched carbon materials to ortho-quinone groups.Energy harvesting,conversion and storage functions could be integrated on a single carbon material to avoid the energy transfer loss among the different materials.Moreover,the assembled Cu/oxygen-enriched carbon battery confirmed the feasibility of the air-oxidation self-charging/electrical discharging mechanism for potential applications.This air-breathing chemical self-charge concept could facilitate the exploration of high-efficiency sustainable air self-charging devices.展开更多
Non-renewable fossil fuels have led to serious problems such as global warming,environmental pollution,etc.Oxygen electrocatalysis including oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)plays a cent...Non-renewable fossil fuels have led to serious problems such as global warming,environmental pollution,etc.Oxygen electrocatalysis including oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)plays a central role in clean energy conversion,enabling a number of sustainable processes for future air battery technologies.Fluorine,as the most electronegative element(4.0)not only can induce more efficient regulation for the electronic structure,but also can bring more abundant defects and other novel effects in materials selection and preparation for favorable catalysis with respect to the other nonmetal elements.However,an individual and comprehensive overview of fluorine-containing functional materials for oxygen electrocatalysis field is still blank.Therefore,it is very meaningful to review the recent progresses of fluorine-containing oxygen electrocatalysts.In this review,we first systematically summarize the controllable preparation methods and their possible development directions based on fluorine-containing materials from four preparation methods.Due to the strong electron-withdrawing properties of fluorine,its control of the electronic structure can effectively enhance the oxygen electrocatalytic activity of the materials.In addition,the catalytic enhancement effect of fluorine on carbonbased materials also includes the prevent oxidation and the layer peeling,and realizes the precise atomic control.And the catalytic improvement mechanism of fluorine containing metal-based compounds also includes the hydration of metal site,the crystal transformation,and the oxygen vacancy induction.Then,based on their various dimensions(0D–3D),we also have summarized the advantages of different morphologies on oxygen electrocatalytic performances.Finally,the prospects and possible future researching direction of F-containing oxygen electrocatalysts are presented(e.g.,novel pathways,advanced methods for measurement and simulation,field assistance and multi-functions).The review is considered valuable and helpful in exploring the novel designs and mechanism analyses of advanced fluorine-containing electrocatalysts.展开更多
The oxygen evolution reaction(OER) is the basis of various sustainable energy conversion and storage techniques,especially hydrogen production by water electrolysis.To realize the practical application of hydrogen ene...The oxygen evolution reaction(OER) is the basis of various sustainable energy conversion and storage techniques,especially hydrogen production by water electrolysis.To realize the practical application of hydrogen energy and mass-scale hydrogen production via water electrolysis,several obstacles,such as the multi-electron transfer OER process with sluggish kinetics and overall high reaction barrier,should be overcome.Manganese oxide-based(MnOx) materials,especially MnO_(2),have emerged as promising non-noble electrocatalysts for water electro-oxidation under acidic conditions due to their wellbalanced properties between catalytic activity and stability.This review introduces the fundamental understanding of the catalytic OER process on MnOx-based materials,including the conventional adsorbate evolution mechanism(AEM) and emerging lattice oxygen oxidation mechanism(LOM).The rational screening and prediction of MnOx-based catalysts that can stably catalyze OER in acid are summarized based on Pourbaix diagram analysis and thermodynamic density functional theory(DFT) calculations.Then,the up-to-date progress of upgrading the OER catalytic performance of MnOx-based catalysts by composite construction is reviewed.Afterward,feasible strategies to improve the electrocatalytic activity and lifetime of MnOx-based catalysts are systemically discussed in terms of crystal structure control,reasonable setting of working potential and electrolyte environment,optimal selection of acid-stable conductive supports,and self-healing engineering.Finally,future scientific challenges and research directions are outlined to guide the construction of advanced MnOx-based electrocatalysts for OER in acid.展开更多
Rechargeable aluminum batteries(RABs)are attractive cadidates for next-generation energy storage and conversion,due to the low cost and high safety of Al resources,and high capacity of metal Al based on the three-elec...Rechargeable aluminum batteries(RABs)are attractive cadidates for next-generation energy storage and conversion,due to the low cost and high safety of Al resources,and high capacity of metal Al based on the three-electrons reaction mechanism.However,the development of RABs is greatly limited,because of the lack of advanced cathode materials,and their complicated and unclear reaction mechanisms.Exploring the novel nanostructured transition metal and carbon composites is an effective route for obtaining ideal cathode materials.In this work,we synthesize porous CoSnO_(3)/C nanocubes with oxygen vacancies for utilizing as cathodes in RABs for the first time.The intrinsic structure stability of the mixed metal cations and carbon coating can improve the cycling performance of cathodes by regulating the internal strains of the electrodes during volume expansion.The nanocubes with porous structures contribute to fast mass transportation which improves the rate capability.In addition to this,abundant oxygen vacancies promote the adsorption affinity of cathodes,which improves storage capacity.As a result,the CoSnO_(3)/C cathodes display an excellent reversible capacity of 292.1 mAh g^(-1) at 0.1 A g^(-1),a good rate performance with 109 mAh g^(-1) that is maintained even at 1 A g^(-1) and the provided stable cycling behavior for 500 cycles.Besides,a mechanism of intercalation of Al^(3+)within CoSnO_(3)/C cathode is proposed for the electrochemical process.Overall,this work provides a step toward the development of advanced cathode materials for RABs by engineering novel nanostructured mixed transition-metal oxides with carbon composite and proposes novel insights into chemistry for RABs.展开更多
Defective layered Mn-based materials were synthesized by Li/Na ion exchange to improve their electrochemical activity and Coulombic efficiency.The annealing temperature of the Na precursors was important to control th...Defective layered Mn-based materials were synthesized by Li/Na ion exchange to improve their electrochemical activity and Coulombic efficiency.The annealing temperature of the Na precursors was important to control the P3-P2 phase transition,which directly affected the structure and electrochemical characteristics of the final products obtained by ion exchange.The O3-Li_(0.78)[Li_(0.25)Fe_(0.075)Mn_(0.675)]O_(δ) cathode made from a P3-type precursor calcined at 700℃ was analyzed using X-ray photoelectron spectrometry and electron paramagnetic resonance.The results showed that the presence of abundant trivalent manganese and defects resulted in a discharge capacity of 230 mAh/g with an initial Coulombic efficiency of about 109%.Afterward,galvanostatic intermittent titration was performed to examine the Li^(+) ion diffusion coefficients,which affected the reversible capacity.First principles calculations suggested that the charge redistribution induced by oxygen vacancies(OV_(s))greatly affected the local Mn coordination environment and enhanced the structural activity.Moreover,the Li-deficient cathode was a perfect match for the pre-lithiation anode,providing a novel approach to improve the initial Coulombic efficiency and activity of Mn-based materials in the commercial application.展开更多
A novel process for synthesis gas production over Circulating Fluidized Bed (CFB) using oxygen storage materials as oxygen carder was reported. First, oxygen in the air was chemically fixed and converted to lattice ...A novel process for synthesis gas production over Circulating Fluidized Bed (CFB) using oxygen storage materials as oxygen carder was reported. First, oxygen in the air was chemically fixed and converted to lattice oxygen of oxygen storage materials over regenerator, and then methane was selectively oxidized to synthesis gas with lattice oxygen of oxygen storage materials over riser reactor. The results from simulation reaction of CFB by sequential redox reaction on a fixed bed reactor using lanthanum-based perovskite LaFeO3 and La0.8Sr0.2Fe0.9CO0.1O3 oxides prepared by sol-gel, suggested that the depleted oxygen species could be regenerated, and methane could be oxidized to synthesis gas by lattice oxygen with high selectivity. The partial oxidation of methane to synthesis gas over CFB using lattice oxygen of the oxygen storage materials instead of gaseous oxygen should be possibly applicable.展开更多
The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional ...The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.展开更多
Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and ...Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and mitigate climate change.In this process,a metal oxide is used as oxygen carrier in a dual fluidized bed to generate clean CO_(2) via combustion of biomass.Most commonly,natural ores or synthetic materials are used as oxygen carrier whereas both must meet special requirements for the conversion of solid fuels.Synthetic oxygen carriers are characterized by higher reactivity at the expense of higher costs versus the lower-cost natural ores.To determine the viability of both possibilities,a techno-economic comparison of a synthetic material based on manganese,iron,and copper to the natural ore ilmenite was conducted.The synthetic oxygen carrier was characterized and tested in a pilot plant,where high combustion efficiencies up to 98.4%and carbon capture rates up to 98.5%were reached.The techno-economic assessment resulted in CO_(2) capture costs of 75 and 40€/tCO_(2) for the synthetic and natural ore route respectively,whereas a sensitivity analysis showed the high impact of production costs and attrition rates of the synthetic material.The synthetic oxygen carrier could break even with the natural ore in case of lower production costs and attrition rates,which could be reached by adapting the production process and recycling material.By comparison to state-of-the-art technologies,it is demonstrated that both routes are viable and the capture cost of CO_(2) could be reduced by implementing the chemical looping combustion technology.展开更多
Dynamic oxygen storage and release capability (OSC) measurement apparatus was designed to evaluate the OSC performance of ceria-based oxygen storage material. The optimum measurement condition was at a frequency of ...Dynamic oxygen storage and release capability (OSC) measurement apparatus was designed to evaluate the OSC performance of ceria-based oxygen storage material. The optimum measurement condition was at a frequency of 0.1 Hz with the inlet gas-flow sequence CO (5S)→O2(5S)→CO→O2 and a flow rate of 300 ml·min^-1. Under this condition, similar regular square wave in the inlet and outlet of the reactor was obtained to guarantee the reliability of the dynamic OSC results. The dynamic OSC performance of the CeO2 and Ce0.67Zr0.33O2 mixed oxide prepared using the citric sol-gel method was studied at the optimum measurement condition with focus on both quantitative and qualitative analyses, The results reveal distinctly that Ce0.67Zr0.33O2 had better dynamic OSC performance because of its higher oxygen migration rate than CeO2. Under dynamic conditions, two CO2 production peaks occurred corresponding to the CO pulse and the O2 pulse, respectively, during the entire cycle. The intensity and ratio between the two CO2 productions were highly influenced by temperature and frequency indicating complex surface phenomena during the oxygen storage/release process, As a result, this set-up can be applied to the evaluation of ceria-based material on the OSC performance.展开更多
Nanostructured materials have received tremendous interest due to their unique mechanical/electrical properties and overall behavior contributed by the complex synergy of bulk and interfacial properties for efficient ...Nanostructured materials have received tremendous interest due to their unique mechanical/electrical properties and overall behavior contributed by the complex synergy of bulk and interfacial properties for efficient and effective energy conversion and storage. The booming development of nanotechnology affords emerging but effective tools in designing advanced energy material. We reviewed the significant progress and dominated nanostructured energy materials in electrochemical energy conversion and storage devices, including lithium ion batteries, lithium-sulfur batteries, lithium-oxygen batteries, lithium metal batteries, and supercapacitors. The use of nanostructured electrocatalyst for effective electrocatalysis in oxygen reduction and oxygen evolution reactions for fuel cells and metal-air batteries was also included. The challenges in the undesirable side reactions between electrolytes and electrode due to high electrode/electrolyte contact area, low volumetric energy density of electrode owing to low tap density, and uniform production of complex energy materials in working devices should be overcome to fully demonstrate the advanced energy nanostructures for electrochemical energy conversion and storage. The energy chemistry at the interfaces of nanostructured electrode/electrolyte is highly expected to guide the rational design and full demonstration of energy materials in a working device. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.展开更多
Antibacterial ceramic was prepared by doping enamel slurry with composite phosphate inorganic antibacterial materials containing rare earth (inorganic antibacterial additives), and then the mechanisms for activating w...Antibacterial ceramic was prepared by doping enamel slurry with composite phosphate inorganic antibacterial materials containing rare earth (inorganic antibacterial additives), and then the mechanisms for activating water and improving seed germinative property were tested by nuclear magnetic resonance (NMR) and the method of testing oxygen dissolved in activated water. Results show that the half peak width of (()^(17)O-NMR) for tap water activated by the antibacterial ceramic drops from 115.36 to 99.15 Hz, and oxygen concentrations of activated water increase by 20%, germinate rate of horsebean and earthnut seeds increases by 12.5% and 7.5%, respectively. Therefore antibacterial ceramic doped enamel slurry with inorganic antibacterial additives containing rare earth can reduce the volume of clusters of water molecules, improve activation of tap water, and promote plant seeds germinate.展开更多
MXenes,as an emerging 2D material,are expected to exert a great influence on future energy storage and conversion technologies.In this review,we systematically summarize recent advances in MXene-based materials in ele...MXenes,as an emerging 2D material,are expected to exert a great influence on future energy storage and conversion technologies.In this review,we systematically summarize recent advances in MXene-based materials in electrocatalysis,particularly in the hydrogen evolution,oxygen evolution,oxygen reduction,nitrogen reduction,and CO2 reduction reactions.Crucial factors influencing the properties of these materials,such as functional groups,conductivity,and interface,are discussed,and challenges to the future development of MXene-based electrocatalysts are presented.展开更多
The chromium oxide materials were prepared using Cr2O3 micropowder as main starting material, TiO2 micropowder as sintering aid, polyvinyl alcohol as binder, by a series of processes such as slurrying, spraying granul...The chromium oxide materials were prepared using Cr2O3 micropowder as main starting material, TiO2 micropowder as sintering aid, polyvinyl alcohol as binder, by a series of processes such as slurrying, spraying granulation, machine moulding and cold isostatic pressing, and firing at 1 500 ℃ for 3 h in air ( oxygen partial pressure was 2. 1× 10^4 Pa ), industrial nitrogen ( oxygen partial pressure was 1×10^3 Pa ) , pure nitrogen ( oxygen partial pressure was 10 Pa) , high purity nitrogen ( oxygen partial pressure was 0.1 Pa ) , and carbon cake embedded atmosphere ( oxygen partial pressure wtas 2.3×10-12 Pa ). Effects of oxygen partial pressures on the sintering behavior of Cr2 O3 materials were investiga- ted. The results show that ( 1 ) for 3 wt% TiO2-doped specimeas, there is a substantial dependence of sintering on oxygen partial pressure (0. 1 Pa - 2. 1 ×10^4 Pa ) , and the bulk density increases and apparent porosity decreases with oxygen partial pressure decreasing; (2) even if the oxygen partial pressure is 0. 1 Pa, the specimen without TiO2 cannot reach densification sintering; (3) under very low oxygen partial pressure of carbon embedded atmosphere, Cr2O3 materials containing TiO2 or not can attain denzification.展开更多
Defect-engineered carbon materials have been emerged as promising electrocatalysts for oxygen reduction reaction(ORR)in metal-air batteries.Developing a facile strategy for the preparation of highly active nanocarbon ...Defect-engineered carbon materials have been emerged as promising electrocatalysts for oxygen reduction reaction(ORR)in metal-air batteries.Developing a facile strategy for the preparation of highly active nanocarbon electrocatalysts remains challenging.Herein,a low-cost and simple route is developed to synthesize defective graphene by pyrolyzing the mixture of glucose and carbon nitride.Molecular dynamics simulations reveal that the graphene formation is ascribed to two-dimensional layered feature of carbon nitride,and high compatibility of carbon nitride/glucose systems.Structural measurements suggest that the graphene possesses rich edge and topological defects.The graphene catalyst exhibits higher power density than commercial Pt/C catalyst in a primary Zn-air battery.Combining experimental results and theoretical thermodynamic analysis,it is identified that graphitic nitrogen-modified topological defects at carbon framework edges are responsible for the decent ORR performance.The strategy presented in this work can be can be scaled up readily to fabricate defective carbon materials.展开更多
OER catalyst of Ni_(3)Fe/Ni_(4)S_(3)/Ni/C(NiFeSC series)mixed crystal composite nanofibers was prepared by electrospinning and atmospheric heat treatment process.The testing results indicate that the diameters of Ni_(...OER catalyst of Ni_(3)Fe/Ni_(4)S_(3)/Ni/C(NiFeSC series)mixed crystal composite nanofibers was prepared by electrospinning and atmospheric heat treatment process.The testing results indicate that the diameters of Ni_(3)Fe/Ni_(4)S_(3)/Ni/C composite nanofibers is about 200 nm,the grains size is about 1-3 nm,and the fiber surface is rough.The electrochemical test results show that the heterojunction of the prepared Ni_(3)Fe/Ni_(4)S_(3)/Ni/C hybrid crystal composite nanofiber has synergistic effect with sulfide,and exhibits good electrocatalytic activity of water decomposition and OER in alkaline system.The OER electrocatalytic performance of Ni_(3)Fe/Ni_(4)S_(3)/Ni/C composite electrode prepared via a heat treatment at 1000℃process was tested in 1 mol/L KOH electrolytes.The results show that the overpotential is about 298 mV,the Tafel slope is about 74 mV?dec-1,and the surface resistance is about 1.69Ω·cm^(2),at the current density of 10 mA·cm^(-2).展开更多
Understanding the crystal phase evolution of bimetallic oxide anodes is the main concern to profoundly reveal the conversion reaction kinetics and sodium-ion storage mechanisms.Herein,an integrated selfsupporting anod...Understanding the crystal phase evolution of bimetallic oxide anodes is the main concern to profoundly reveal the conversion reaction kinetics and sodium-ion storage mechanisms.Herein,an integrated selfsupporting anode of the Cu-decorated Cu-Mn bimetallic oxides with oxygen vacancies(Ov-BMO-Cu)are in-situ generated by phase separation and hydrogen etching using nanoporous Cu-Mn alloy as selfsacrificial templates.On this basis,we have elucidated the relationship between the phase evolution,oxygen vacancies and sodium-ion storage mechanisms,further demonstrating the evolution of oxygen vacancies and the inhibition effect of manganese oxides as an“anchor”on grain aggregation of copper oxides.The kinetic analyses confirm that the expanded lattice space and increased oxygen vacancies of cycled Ov-BMO-Cu synergistically guarantee effective sodium-ion diffusion and storage mechanisms.Therefore,the Ov-BMO-Cu electrode exhibits higher reversible capacities of 4.04 mA h cm^(-2)at 0.2 mA cm^(-2)after 100 cycles and 2.20 m A h cm^(-2)at 1.0 mA cm^(-2)after 500 cycles.Besides,the presodiated Ov-BMO-Cu anode delivers a considerable reversible capacity of 0.79 m A h cm^(-2)at 1.0 mA cm^(-2)after 60 cycles in full cells with Na_(3)V_(2)(PO_(4))_(3)cathode,confirming its outstanding practicality.Thus,this work is expected to provide enlightenment for designing high-capacity bimetallic oxide anodes.展开更多
Microbes are microscopic living organisms that surround us which include bacteria, archaea, most protozoa, and some fungi and algae. In recent years, microbes have been explored as novel precursors to synthesize carbo...Microbes are microscopic living organisms that surround us which include bacteria, archaea, most protozoa, and some fungi and algae. In recent years, microbes have been explored as novel precursors to synthesize carbon-based(nano)materials and as substrates or templates to produce carbon-containing(nano)composites. Being greener and more affordable, microbe-derived carbons(MDCs) offer good potential for energy applications. In this review, we describe the unique advantages of MDCs and outline the common procedures to prepare them. We also extensively discuss the energy applications of MDCs including their use as electrodes in supercapacitors and lithium-ion batteries, and as electrocatalysts for processes such as oxygen reduction, oxygen evolution, and hydrogen evolution reactions which are essential for fuel cell and water electrochemical splitting cells. Based on the literature trend and our group's expertise, we propose potential research directions for developing new types of MDCs. This review, therefore, provides the state-of-the-art of a new energy chemistry concept. We expect to stimulate future research on the applications of MDCs that may address energy and environmental challenges that our societies are facing.展开更多
The growth of electrochemically inert segregation layers on the surface of solid oxide fuel cell cathodes has become a bottleneck restricting the development of perovskite-structured oxygen reduction catalysts.Here,we...The growth of electrochemically inert segregation layers on the surface of solid oxide fuel cell cathodes has become a bottleneck restricting the development of perovskite-structured oxygen reduction catalysts.Here,we report a new discovery in which enriched Ba and Fe ions on the near-surface of Nd_(1/2)Ba_(1/2)Co_(1/3)Fe_(1/3)Mn_(1/3)O_(3-δ)spontaneously agglomerate into dispersed Ba_(5)Fe_(2)O_(8) nanoparticles and maintain a highly active and durable perovskite structure on the surface.This unique surface selfcleaning phenomenon is related to the low average potential energy of Ba_(5)Fe_(2)O_(8),which is grown on the near-surface layer.The electrochemically inert Ba_(5)Fe_(2)O_(8) segregation layer on the near-surface of the perovskite catalyst achieves self-cleaning by regulating the formation energy of enriched metal oxides.This self-cleaned perovskite surface exhibits an ultrafast oxygen exchange rate,high catalytic activity for the oxygen reduction reaction,and good adaptability to the actual working conditions of solid oxide fuel cell stacks.This study paves a new way for overcoming the stubborn problem of perovskite catalyst surface deactivation and enriches the scientific knowledge of surface catalysis.展开更多
Combustion within small motors is key in the application-specific development of nanothermite-based micro-energetic systems. This study evaluates the performance of nanothermite mixtures in a converging-diverging nozz...Combustion within small motors is key in the application-specific development of nanothermite-based micro-energetic systems. This study evaluates the performance of nanothermite mixtures in a converging-diverging nozzle and an open tube. Mixtures were prepared using nano-aluminum(n-Al),potassium perchlorate(KClO_(4)), and different carbon nanomaterials(CNMs) including graphene-oxide(GO), reduced GO, carbon nanotubes(CNTs) and nanofibers(CNFs). The mixtures were packed at different densities and ignited by laser beam. Performance was measured using thrust measurement,high-speed imaging, and computational fluid dynamics modeling, respectively. Thrust, specific impulse(ISP), volumetric impulse(ISV), as well as normalized energy were found to increase notably with CNM content. Two distinctive reaction regimes(fast and slow) were observed in combustion of low and high packing densities(20% and 55%TMD), respectively. Total impulse(IFT) and ISPwere maximized in the 5%GO/Al/KClO_4 mixture, producing 7.95 m N·s and 135.20 s respectively at 20%TMD, an improvement of 57%compared to a GO-free sample(5.05 m N·s and 85.88 s). CFD analysis of the motors over predicts the thrust generated but trends in nozzle layout and packing density agree with those observed experimentally;peak force was maximized by reducing packing density and using an open tube. The numerical force profiles fit better for the nozzle cases than the open tube scenarios due to the rapid nature of combustion. This study reveals the potential of GO in improving oxygenated salt-based nanothermites,and further demonstrates their applicability for micro-propulsion and micro-energetic applications.展开更多
In recent years,manganese-based oxides as an advanced class of cathode materials for zinc-ion batteries(ZIBs)have attracted a great deal of attentions from numerous researchers.However,their slow reaction kinetics,lim...In recent years,manganese-based oxides as an advanced class of cathode materials for zinc-ion batteries(ZIBs)have attracted a great deal of attentions from numerous researchers.However,their slow reaction kinetics,limited active sites and poor electrical conductivity inevitably give rise to the severe performance degradation.To solve these problems,herein,we introduce abundant oxygen vacancies into the flower-likeδ-MnO_(2)nanostructure and effectively modulate the vacancy defects to reach the optimal level(δ-MnO_(2)-x-2.0).The smart design intrinsically tunes the electronic structure,guarantees ion chemisorption-desorption equilibrium and increases the electroactive sites,which not only effectively accelerates charge transfer rate during reaction processes,but also endows more redox reactions,as verified by first-principle calculations.These merits can help the fabricatedδ-MnO_(2)-x-2.0 cathode to present a large specific capacity of 551.8 mAh g^(-1) at 0.5 A g^(-1),high-rate capability of 262.2 mAh g^(-1) at 10 A g^(-1) and an excellent cycle lifespan(83%of capacity retention after 1500 cycles),which is far superior to those of the other metal compound cathodes.In addition,the charge/discharge mechanism of theδ-MnO_(2)-x-2.0 cathode has also been elaborated through ex situ techniques.This work opens up a new pathway for constructing the next-generation high-performance ZIBs cathode materials.展开更多
基金financially supported by the National Natural Science Foundation of China(51503178,52202048,52027801)National Key R&D Program of China(2017YFA0206301)+1 种基金China-Germany Collaboration Project(M-0199)Natural Science Foundation of Hebei Province(B2021203012,E2022203082)。
文摘The self-charging concept has drawn considerable attention due to its excellent ability to achieve environmental energy harvesting,conversion and storage without an external power supply.However,most self-charging designs assembled by multiple energy harvesting,conversion and storage materials increase the energy transfer loss;the environmental energy supply is generally limited by climate and meteorological conditions,hindering the potential application of these selfpowered devices to be available at all times.Based on aerobic autoxidation of catechol,which is similar to the electrochemical oxidation of the catechol groups on the carbon materials under an electrical charge,we proposed an air-breathing chemical self-charge concept based on the aerobic autoxidation of catechol groups on oxygen-enriched carbon materials to ortho-quinone groups.Energy harvesting,conversion and storage functions could be integrated on a single carbon material to avoid the energy transfer loss among the different materials.Moreover,the assembled Cu/oxygen-enriched carbon battery confirmed the feasibility of the air-oxidation self-charging/electrical discharging mechanism for potential applications.This air-breathing chemical self-charge concept could facilitate the exploration of high-efficiency sustainable air self-charging devices.
基金supported by the National Natural Science Foundation of China,China(52203066,51973157,51673148 and 51678411)the Science and Technology Plans of Tianjin,China(19PTSYJC00010)+3 种基金China Postdoctoral Science Foundation Grant,China(2019M651047)the Tianjin Research Innovation Project for Postgraduate Students,China(2020YJSB062)the Tianjin Municipal College Student’Innovation And Entrepreneurship Training Program,China(202110058052)the National Innovation and Entrepreneurship Training Program for College Students,China(202110058017)。
文摘Non-renewable fossil fuels have led to serious problems such as global warming,environmental pollution,etc.Oxygen electrocatalysis including oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)plays a central role in clean energy conversion,enabling a number of sustainable processes for future air battery technologies.Fluorine,as the most electronegative element(4.0)not only can induce more efficient regulation for the electronic structure,but also can bring more abundant defects and other novel effects in materials selection and preparation for favorable catalysis with respect to the other nonmetal elements.However,an individual and comprehensive overview of fluorine-containing functional materials for oxygen electrocatalysis field is still blank.Therefore,it is very meaningful to review the recent progresses of fluorine-containing oxygen electrocatalysts.In this review,we first systematically summarize the controllable preparation methods and their possible development directions based on fluorine-containing materials from four preparation methods.Due to the strong electron-withdrawing properties of fluorine,its control of the electronic structure can effectively enhance the oxygen electrocatalytic activity of the materials.In addition,the catalytic enhancement effect of fluorine on carbonbased materials also includes the prevent oxidation and the layer peeling,and realizes the precise atomic control.And the catalytic improvement mechanism of fluorine containing metal-based compounds also includes the hydration of metal site,the crystal transformation,and the oxygen vacancy induction.Then,based on their various dimensions(0D–3D),we also have summarized the advantages of different morphologies on oxygen electrocatalytic performances.Finally,the prospects and possible future researching direction of F-containing oxygen electrocatalysts are presented(e.g.,novel pathways,advanced methods for measurement and simulation,field assistance and multi-functions).The review is considered valuable and helpful in exploring the novel designs and mechanism analyses of advanced fluorine-containing electrocatalysts.
基金the financial support of the National Natural Science Foundation of China(21962008)the Yunnan Province Excellent Youth Fund Project(202001AW070005)the Yunnan Ten Thousand Talents Plan Young & Elite Talents Project(YNWR-QNBJ-2018-346)。
文摘The oxygen evolution reaction(OER) is the basis of various sustainable energy conversion and storage techniques,especially hydrogen production by water electrolysis.To realize the practical application of hydrogen energy and mass-scale hydrogen production via water electrolysis,several obstacles,such as the multi-electron transfer OER process with sluggish kinetics and overall high reaction barrier,should be overcome.Manganese oxide-based(MnOx) materials,especially MnO_(2),have emerged as promising non-noble electrocatalysts for water electro-oxidation under acidic conditions due to their wellbalanced properties between catalytic activity and stability.This review introduces the fundamental understanding of the catalytic OER process on MnOx-based materials,including the conventional adsorbate evolution mechanism(AEM) and emerging lattice oxygen oxidation mechanism(LOM).The rational screening and prediction of MnOx-based catalysts that can stably catalyze OER in acid are summarized based on Pourbaix diagram analysis and thermodynamic density functional theory(DFT) calculations.Then,the up-to-date progress of upgrading the OER catalytic performance of MnOx-based catalysts by composite construction is reviewed.Afterward,feasible strategies to improve the electrocatalytic activity and lifetime of MnOx-based catalysts are systemically discussed in terms of crystal structure control,reasonable setting of working potential and electrolyte environment,optimal selection of acid-stable conductive supports,and self-healing engineering.Finally,future scientific challenges and research directions are outlined to guide the construction of advanced MnOx-based electrocatalysts for OER in acid.
基金supported by the National Natural Science Foundation of China (Grant No.22075028).
文摘Rechargeable aluminum batteries(RABs)are attractive cadidates for next-generation energy storage and conversion,due to the low cost and high safety of Al resources,and high capacity of metal Al based on the three-electrons reaction mechanism.However,the development of RABs is greatly limited,because of the lack of advanced cathode materials,and their complicated and unclear reaction mechanisms.Exploring the novel nanostructured transition metal and carbon composites is an effective route for obtaining ideal cathode materials.In this work,we synthesize porous CoSnO_(3)/C nanocubes with oxygen vacancies for utilizing as cathodes in RABs for the first time.The intrinsic structure stability of the mixed metal cations and carbon coating can improve the cycling performance of cathodes by regulating the internal strains of the electrodes during volume expansion.The nanocubes with porous structures contribute to fast mass transportation which improves the rate capability.In addition to this,abundant oxygen vacancies promote the adsorption affinity of cathodes,which improves storage capacity.As a result,the CoSnO_(3)/C cathodes display an excellent reversible capacity of 292.1 mAh g^(-1) at 0.1 A g^(-1),a good rate performance with 109 mAh g^(-1) that is maintained even at 1 A g^(-1) and the provided stable cycling behavior for 500 cycles.Besides,a mechanism of intercalation of Al^(3+)within CoSnO_(3)/C cathode is proposed for the electrochemical process.Overall,this work provides a step toward the development of advanced cathode materials for RABs by engineering novel nanostructured mixed transition-metal oxides with carbon composite and proposes novel insights into chemistry for RABs.
基金The Beijing Municipal Education Commission(KZ201910005003)supported this work。
文摘Defective layered Mn-based materials were synthesized by Li/Na ion exchange to improve their electrochemical activity and Coulombic efficiency.The annealing temperature of the Na precursors was important to control the P3-P2 phase transition,which directly affected the structure and electrochemical characteristics of the final products obtained by ion exchange.The O3-Li_(0.78)[Li_(0.25)Fe_(0.075)Mn_(0.675)]O_(δ) cathode made from a P3-type precursor calcined at 700℃ was analyzed using X-ray photoelectron spectrometry and electron paramagnetic resonance.The results showed that the presence of abundant trivalent manganese and defects resulted in a discharge capacity of 230 mAh/g with an initial Coulombic efficiency of about 109%.Afterward,galvanostatic intermittent titration was performed to examine the Li^(+) ion diffusion coefficients,which affected the reversible capacity.First principles calculations suggested that the charge redistribution induced by oxygen vacancies(OV_(s))greatly affected the local Mn coordination environment and enhanced the structural activity.Moreover,the Li-deficient cathode was a perfect match for the pre-lithiation anode,providing a novel approach to improve the initial Coulombic efficiency and activity of Mn-based materials in the commercial application.
基金Project supported by the National Natural Science Foundation of China (20306016, 20322201)
文摘A novel process for synthesis gas production over Circulating Fluidized Bed (CFB) using oxygen storage materials as oxygen carder was reported. First, oxygen in the air was chemically fixed and converted to lattice oxygen of oxygen storage materials over regenerator, and then methane was selectively oxidized to synthesis gas with lattice oxygen of oxygen storage materials over riser reactor. The results from simulation reaction of CFB by sequential redox reaction on a fixed bed reactor using lanthanum-based perovskite LaFeO3 and La0.8Sr0.2Fe0.9CO0.1O3 oxides prepared by sol-gel, suggested that the depleted oxygen species could be regenerated, and methane could be oxidized to synthesis gas by lattice oxygen with high selectivity. The partial oxidation of methane to synthesis gas over CFB using lattice oxygen of the oxygen storage materials instead of gaseous oxygen should be possibly applicable.
基金financial support from the National Natural Science Foundation of China (52203070)the Open Fund of State Key Laboratory of New Textile Materials and Advanced Processing Technologies (FZ2022005)+2 种基金the Open Fund of Hubei Key Laboratory of Biomass Fiber and Ecological Dyeing and Finishing (STRZ202203)the financial support provided by the China Scholarship Council (CSC)Visiting Scholar Programfinancial support from Institute for Sustainability,Energy and Resources,The University of Adelaide,Future Making Fellowship,Australia。
文摘The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.
文摘Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and mitigate climate change.In this process,a metal oxide is used as oxygen carrier in a dual fluidized bed to generate clean CO_(2) via combustion of biomass.Most commonly,natural ores or synthetic materials are used as oxygen carrier whereas both must meet special requirements for the conversion of solid fuels.Synthetic oxygen carriers are characterized by higher reactivity at the expense of higher costs versus the lower-cost natural ores.To determine the viability of both possibilities,a techno-economic comparison of a synthetic material based on manganese,iron,and copper to the natural ore ilmenite was conducted.The synthetic oxygen carrier was characterized and tested in a pilot plant,where high combustion efficiencies up to 98.4%and carbon capture rates up to 98.5%were reached.The techno-economic assessment resulted in CO_(2) capture costs of 75 and 40€/tCO_(2) for the synthetic and natural ore route respectively,whereas a sensitivity analysis showed the high impact of production costs and attrition rates of the synthetic material.The synthetic oxygen carrier could break even with the natural ore in case of lower production costs and attrition rates,which could be reached by adapting the production process and recycling material.By comparison to state-of-the-art technologies,it is demonstrated that both routes are viable and the capture cost of CO_(2) could be reduced by implementing the chemical looping combustion technology.
基金Project supported by the National"973"Project (2004CB719503) and the Programfor New Century Excellent Talents in University
文摘Dynamic oxygen storage and release capability (OSC) measurement apparatus was designed to evaluate the OSC performance of ceria-based oxygen storage material. The optimum measurement condition was at a frequency of 0.1 Hz with the inlet gas-flow sequence CO (5S)→O2(5S)→CO→O2 and a flow rate of 300 ml·min^-1. Under this condition, similar regular square wave in the inlet and outlet of the reactor was obtained to guarantee the reliability of the dynamic OSC results. The dynamic OSC performance of the CeO2 and Ce0.67Zr0.33O2 mixed oxide prepared using the citric sol-gel method was studied at the optimum measurement condition with focus on both quantitative and qualitative analyses, The results reveal distinctly that Ce0.67Zr0.33O2 had better dynamic OSC performance because of its higher oxygen migration rate than CeO2. Under dynamic conditions, two CO2 production peaks occurred corresponding to the CO pulse and the O2 pulse, respectively, during the entire cycle. The intensity and ratio between the two CO2 productions were highly influenced by temperature and frequency indicating complex surface phenomena during the oxygen storage/release process, As a result, this set-up can be applied to the evaluation of ceria-based material on the OSC performance.
基金supported by the National Key Research and Development Program (no.2016YFA0202500)National Basic Research Program of China (2015CB932500)the Natural Scientific Foundation of China (nos.21306102 and 21422604)
文摘Nanostructured materials have received tremendous interest due to their unique mechanical/electrical properties and overall behavior contributed by the complex synergy of bulk and interfacial properties for efficient and effective energy conversion and storage. The booming development of nanotechnology affords emerging but effective tools in designing advanced energy material. We reviewed the significant progress and dominated nanostructured energy materials in electrochemical energy conversion and storage devices, including lithium ion batteries, lithium-sulfur batteries, lithium-oxygen batteries, lithium metal batteries, and supercapacitors. The use of nanostructured electrocatalyst for effective electrocatalysis in oxygen reduction and oxygen evolution reactions for fuel cells and metal-air batteries was also included. The challenges in the undesirable side reactions between electrolytes and electrode due to high electrode/electrolyte contact area, low volumetric energy density of electrode owing to low tap density, and uniform production of complex energy materials in working devices should be overcome to fully demonstrate the advanced energy nanostructures for electrochemical energy conversion and storage. The energy chemistry at the interfaces of nanostructured electrode/electrolyte is highly expected to guide the rational design and full demonstration of energy materials in a working device. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.
文摘Antibacterial ceramic was prepared by doping enamel slurry with composite phosphate inorganic antibacterial materials containing rare earth (inorganic antibacterial additives), and then the mechanisms for activating water and improving seed germinative property were tested by nuclear magnetic resonance (NMR) and the method of testing oxygen dissolved in activated water. Results show that the half peak width of (()^(17)O-NMR) for tap water activated by the antibacterial ceramic drops from 115.36 to 99.15 Hz, and oxygen concentrations of activated water increase by 20%, germinate rate of horsebean and earthnut seeds increases by 12.5% and 7.5%, respectively. Therefore antibacterial ceramic doped enamel slurry with inorganic antibacterial additives containing rare earth can reduce the volume of clusters of water molecules, improve activation of tap water, and promote plant seeds germinate.
文摘MXenes,as an emerging 2D material,are expected to exert a great influence on future energy storage and conversion technologies.In this review,we systematically summarize recent advances in MXene-based materials in electrocatalysis,particularly in the hydrogen evolution,oxygen evolution,oxygen reduction,nitrogen reduction,and CO2 reduction reactions.Crucial factors influencing the properties of these materials,such as functional groups,conductivity,and interface,are discussed,and challenges to the future development of MXene-based electrocatalysts are presented.
文摘The chromium oxide materials were prepared using Cr2O3 micropowder as main starting material, TiO2 micropowder as sintering aid, polyvinyl alcohol as binder, by a series of processes such as slurrying, spraying granulation, machine moulding and cold isostatic pressing, and firing at 1 500 ℃ for 3 h in air ( oxygen partial pressure was 2. 1× 10^4 Pa ), industrial nitrogen ( oxygen partial pressure was 1×10^3 Pa ) , pure nitrogen ( oxygen partial pressure was 10 Pa) , high purity nitrogen ( oxygen partial pressure was 0.1 Pa ) , and carbon cake embedded atmosphere ( oxygen partial pressure wtas 2.3×10-12 Pa ). Effects of oxygen partial pressures on the sintering behavior of Cr2 O3 materials were investiga- ted. The results show that ( 1 ) for 3 wt% TiO2-doped specimeas, there is a substantial dependence of sintering on oxygen partial pressure (0. 1 Pa - 2. 1 ×10^4 Pa ) , and the bulk density increases and apparent porosity decreases with oxygen partial pressure decreasing; (2) even if the oxygen partial pressure is 0. 1 Pa, the specimen without TiO2 cannot reach densification sintering; (3) under very low oxygen partial pressure of carbon embedded atmosphere, Cr2O3 materials containing TiO2 or not can attain denzification.
基金supported by the National Natural Science Foundation of China(21838003,91834301 and 21978278)the Shanghai Scientific and Technological Innovation Project(18JC1410500 and 19JC1410400)the Fundamental Research Funds for the Central Universities(222201718002).
文摘Defect-engineered carbon materials have been emerged as promising electrocatalysts for oxygen reduction reaction(ORR)in metal-air batteries.Developing a facile strategy for the preparation of highly active nanocarbon electrocatalysts remains challenging.Herein,a low-cost and simple route is developed to synthesize defective graphene by pyrolyzing the mixture of glucose and carbon nitride.Molecular dynamics simulations reveal that the graphene formation is ascribed to two-dimensional layered feature of carbon nitride,and high compatibility of carbon nitride/glucose systems.Structural measurements suggest that the graphene possesses rich edge and topological defects.The graphene catalyst exhibits higher power density than commercial Pt/C catalyst in a primary Zn-air battery.Combining experimental results and theoretical thermodynamic analysis,it is identified that graphitic nitrogen-modified topological defects at carbon framework edges are responsible for the decent ORR performance.The strategy presented in this work can be can be scaled up readily to fabricate defective carbon materials.
基金Funded by the Doctoral Fund of Chengdu University (2081919131)the Open Fund of Material Corrosion and Protection Key Laboratory of Sichuan Province (2021CL27)the Sichuan Science and Technology Program (2023YFG0229)。
文摘OER catalyst of Ni_(3)Fe/Ni_(4)S_(3)/Ni/C(NiFeSC series)mixed crystal composite nanofibers was prepared by electrospinning and atmospheric heat treatment process.The testing results indicate that the diameters of Ni_(3)Fe/Ni_(4)S_(3)/Ni/C composite nanofibers is about 200 nm,the grains size is about 1-3 nm,and the fiber surface is rough.The electrochemical test results show that the heterojunction of the prepared Ni_(3)Fe/Ni_(4)S_(3)/Ni/C hybrid crystal composite nanofiber has synergistic effect with sulfide,and exhibits good electrocatalytic activity of water decomposition and OER in alkaline system.The OER electrocatalytic performance of Ni_(3)Fe/Ni_(4)S_(3)/Ni/C composite electrode prepared via a heat treatment at 1000℃process was tested in 1 mol/L KOH electrolytes.The results show that the overpotential is about 298 mV,the Tafel slope is about 74 mV?dec-1,and the surface resistance is about 1.69Ω·cm^(2),at the current density of 10 mA·cm^(-2).
基金supported by the Natural Science Foundation of China(5207123251871165)。
文摘Understanding the crystal phase evolution of bimetallic oxide anodes is the main concern to profoundly reveal the conversion reaction kinetics and sodium-ion storage mechanisms.Herein,an integrated selfsupporting anode of the Cu-decorated Cu-Mn bimetallic oxides with oxygen vacancies(Ov-BMO-Cu)are in-situ generated by phase separation and hydrogen etching using nanoporous Cu-Mn alloy as selfsacrificial templates.On this basis,we have elucidated the relationship between the phase evolution,oxygen vacancies and sodium-ion storage mechanisms,further demonstrating the evolution of oxygen vacancies and the inhibition effect of manganese oxides as an“anchor”on grain aggregation of copper oxides.The kinetic analyses confirm that the expanded lattice space and increased oxygen vacancies of cycled Ov-BMO-Cu synergistically guarantee effective sodium-ion diffusion and storage mechanisms.Therefore,the Ov-BMO-Cu electrode exhibits higher reversible capacities of 4.04 mA h cm^(-2)at 0.2 mA cm^(-2)after 100 cycles and 2.20 m A h cm^(-2)at 1.0 mA cm^(-2)after 500 cycles.Besides,the presodiated Ov-BMO-Cu anode delivers a considerable reversible capacity of 0.79 m A h cm^(-2)at 1.0 mA cm^(-2)after 60 cycles in full cells with Na_(3)V_(2)(PO_(4))_(3)cathode,confirming its outstanding practicality.Thus,this work is expected to provide enlightenment for designing high-capacity bimetallic oxide anodes.
基金supported by the Ministry of Education, Singapore (2013-T1-002132)the iFood program of Nanyang Technological UniversityThe University of Sydney for financial support
文摘Microbes are microscopic living organisms that surround us which include bacteria, archaea, most protozoa, and some fungi and algae. In recent years, microbes have been explored as novel precursors to synthesize carbon-based(nano)materials and as substrates or templates to produce carbon-containing(nano)composites. Being greener and more affordable, microbe-derived carbons(MDCs) offer good potential for energy applications. In this review, we describe the unique advantages of MDCs and outline the common procedures to prepare them. We also extensively discuss the energy applications of MDCs including their use as electrodes in supercapacitors and lithium-ion batteries, and as electrocatalysts for processes such as oxygen reduction, oxygen evolution, and hydrogen evolution reactions which are essential for fuel cell and water electrochemical splitting cells. Based on the literature trend and our group's expertise, we propose potential research directions for developing new types of MDCs. This review, therefore, provides the state-of-the-art of a new energy chemistry concept. We expect to stimulate future research on the applications of MDCs that may address energy and environmental challenges that our societies are facing.
基金financially supported by the National Natural Science Foundation of China (U2032157)the Natural Science Foundation of Jiangsu Province (BK20201425)。
文摘The growth of electrochemically inert segregation layers on the surface of solid oxide fuel cell cathodes has become a bottleneck restricting the development of perovskite-structured oxygen reduction catalysts.Here,we report a new discovery in which enriched Ba and Fe ions on the near-surface of Nd_(1/2)Ba_(1/2)Co_(1/3)Fe_(1/3)Mn_(1/3)O_(3-δ)spontaneously agglomerate into dispersed Ba_(5)Fe_(2)O_(8) nanoparticles and maintain a highly active and durable perovskite structure on the surface.This unique surface selfcleaning phenomenon is related to the low average potential energy of Ba_(5)Fe_(2)O_(8),which is grown on the near-surface layer.The electrochemically inert Ba_(5)Fe_(2)O_(8) segregation layer on the near-surface of the perovskite catalyst achieves self-cleaning by regulating the formation energy of enriched metal oxides.This self-cleaned perovskite surface exhibits an ultrafast oxygen exchange rate,high catalytic activity for the oxygen reduction reaction,and good adaptability to the actual working conditions of solid oxide fuel cell stacks.This study paves a new way for overcoming the stubborn problem of perovskite catalyst surface deactivation and enriches the scientific knowledge of surface catalysis.
基金financial funding from the Egyptian governmentthe financial funding from the NSERC Discovery grant。
文摘Combustion within small motors is key in the application-specific development of nanothermite-based micro-energetic systems. This study evaluates the performance of nanothermite mixtures in a converging-diverging nozzle and an open tube. Mixtures were prepared using nano-aluminum(n-Al),potassium perchlorate(KClO_(4)), and different carbon nanomaterials(CNMs) including graphene-oxide(GO), reduced GO, carbon nanotubes(CNTs) and nanofibers(CNFs). The mixtures were packed at different densities and ignited by laser beam. Performance was measured using thrust measurement,high-speed imaging, and computational fluid dynamics modeling, respectively. Thrust, specific impulse(ISP), volumetric impulse(ISV), as well as normalized energy were found to increase notably with CNM content. Two distinctive reaction regimes(fast and slow) were observed in combustion of low and high packing densities(20% and 55%TMD), respectively. Total impulse(IFT) and ISPwere maximized in the 5%GO/Al/KClO_4 mixture, producing 7.95 m N·s and 135.20 s respectively at 20%TMD, an improvement of 57%compared to a GO-free sample(5.05 m N·s and 85.88 s). CFD analysis of the motors over predicts the thrust generated but trends in nozzle layout and packing density agree with those observed experimentally;peak force was maximized by reducing packing density and using an open tube. The numerical force profiles fit better for the nozzle cases than the open tube scenarios due to the rapid nature of combustion. This study reveals the potential of GO in improving oxygenated salt-based nanothermites,and further demonstrates their applicability for micro-propulsion and micro-energetic applications.
基金supported by the National Natural Science Foundation of China under Grant Nos. 52072196, 52002200, 52102106 and 52002199Major Basic Research Program of the Natural Science Foundation of Shandong Province under Grant No. ZR2020ZD09+2 种基金the Natural Science Foundation of Shandong Province under Grant No. ZR2020QE063the Innovation and Technology Program of Shandong Province under Grant No. 2020KJA004the Taishan Scholars Program of Shandong Province under Grant No. ts201511034
文摘In recent years,manganese-based oxides as an advanced class of cathode materials for zinc-ion batteries(ZIBs)have attracted a great deal of attentions from numerous researchers.However,their slow reaction kinetics,limited active sites and poor electrical conductivity inevitably give rise to the severe performance degradation.To solve these problems,herein,we introduce abundant oxygen vacancies into the flower-likeδ-MnO_(2)nanostructure and effectively modulate the vacancy defects to reach the optimal level(δ-MnO_(2)-x-2.0).The smart design intrinsically tunes the electronic structure,guarantees ion chemisorption-desorption equilibrium and increases the electroactive sites,which not only effectively accelerates charge transfer rate during reaction processes,but also endows more redox reactions,as verified by first-principle calculations.These merits can help the fabricatedδ-MnO_(2)-x-2.0 cathode to present a large specific capacity of 551.8 mAh g^(-1) at 0.5 A g^(-1),high-rate capability of 262.2 mAh g^(-1) at 10 A g^(-1) and an excellent cycle lifespan(83%of capacity retention after 1500 cycles),which is far superior to those of the other metal compound cathodes.In addition,the charge/discharge mechanism of theδ-MnO_(2)-x-2.0 cathode has also been elaborated through ex situ techniques.This work opens up a new pathway for constructing the next-generation high-performance ZIBs cathode materials.