查看更多>>摘要：Ammonia serves both as a widely used fertilizer and environmentally friendly energy source due to its high energy density,rich hydrogen content,and emissions-free combustion.Additionally,it offers conve-nient transportation and storage as a hydrogen carrier.The dominant method used for large-scale ammo-nia production is the Haber-Bosch process,which requires high temperatures and pressures and is energy-intensive.However,non-thermal plasma offers an eco-friendly alternative for ammonia synthe-sis,gaining significant attention.It enables ammonia production at lower temperatures and pressures using plasma technology.This review provides insights into the catalyst and reactor developments,which are pivotal for promoting ammonia efficiency and addressing existing challenges.At first,the reac-tion kinetics and mechanisms are introduced to gain a comprehensive understanding of the reaction pathways involved in plasma-assisted ammonia synthesis.Thereafter,the enhancement of ammonia syn-thesis efficiency is discussed by developing and optimizing plasma reactors and effective catalysts.The effect of other feeding sources,such as water and methane,instead of hydrogen is also presented.Finally,the challenges and possible solutions are outlined to facilitate energy-saving and enhance ammo-nia efficiency in the future.
查看更多>>摘要：Nanoparticles anchored on the perovskite surface have gained considerable attention for their wide-ranging applications in heterogeneous catalysis and energy conversion due to their robust and integrated structural configuration.Herein,we employ controlled Co doping to effectively enhance the nanoparticle exsolution process in layered perovskite ferrites materials.CoFe alloy nanoparticles with ultra-high-density are exsolved on the(PrBa)0.95(Fe0.8Co0.1Nb0.1)2O5+δ(PBFCN0.1)surface under reducing atmo-sphere,providing significant amounts of reaction sites and good durability for hydrocarbon catalysis.Under a reducing atmosphere,cobalt facilitates the reduction of iron cations within PBFCN0.1,leading to the formation of CoFe alloy nanoparticles.This formation is accompanied by a cation exchange process,wherein,with the increase in temperature,partial cobalt ions are substituted by iron.Meanwhile,Co dop-ing significantly enhance the electrical conductivity due to the stronger covalency of the Co-O bond compared with Fe-O bond.A single cell with the configuration of PBFCN0.1-Sm0.2Ce0.8O1.9(SDC)|SDC|Ba0.5Sr0.5Co0.8Fe0.2O3-δ(BSCF)-SDC achieves an extremely low polarization resistance of 0.0163 Ω cm2 and a high peak power density of 740 mW cm-2 at 800 ℃.The cell also shows stable operation for 120 h in H2 with a constant current density of 285 mA cm-2.Furthermore,employing wet C2H6 as fuel,the cell demonstrates remarkable performance,achieving peak power densities of 455 mW cm-2 at 800 ℃ and 320 mW cm-2 at 750 ℃,marking improvements of 36％and 70％over the cell with(PrBa)0.95(Fe0.9Nb0.1)2O5+a(PBFN)-SDC at these respective temperatures.This discovery emphasizes how temperature influences alloy nanoparticles exsolution within doped layered perovskite ferrites materials,paving the way for the development of high-performance ceramic fuel cell anodes.
查看更多>>摘要：Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction reaction.The nature of the active functional group and underlying reaction mechanism,however,remain unclear.Here,a comprehensive workflow was established to identify the active sites from the numerous possible structures.The com-mon hydroxyl group at the notched edge demonstrates a key role in the two-electron process.The local chemical environment weakens the binding of OOH intermediate to substrate while enhancing interac-tion with solution,thereby promoting the H2O2 production.With increasing pH,the intramolecular hydrogen bond between OOH intermediate and hydroxyl decreases,facilitating OOH desorption.Furthermore,the rise in selectivity with increasing potential stems from the suppression of the four-electron process.The active site was further validated through experiments.Guided by theoretical under-standing,optimal performance was achieved with high selectivity(＞95％)and current density(2.06 mA/cm2)in experiment.
查看更多>>摘要：Typical application scenarios,such as vehicle to grid(V2G)and frequency regulation,have imposed sig-nificant long-life demands on lithium-ion batteries.Herein,we propose an advanced battery life-extension method employing bidirectional pulse charging(BPC)strategy.Unlike traditional constant cur-rent charging methods,BPC strategy not only achieves comparable charging speeds but also facilitates V2G frequency regulation simultaneously.It significantly enhances battery cycle ampere-hour through-put and demonstrates remarkable life extension capabilities.For this interesting conclusion,adopting model identification and postmortem characterization to reveal the life regulation mechanism of BPC:it mitigates battery capacity loss attributed to loss of lithium-ion inventory(LLI)in graphite anodes by intermittently regulating the overall battery voltage and anode potential using a negative charging cur-rent.Then,from the perspective of internal side reaction,the life extension mechanism is further revealed as inhibition of solid electrolyte interphase(SEI)and lithium dendrite growth by regulating voltage with a bidirectional pulse current,and a semi-empirical life degradation model combining SEI and lithium dendrite growth is developed for BPC scenarios health management,the model parameters are identified by genetic algorithm with the life simulation exhibiting an accuracy exceeding 99％.This finding indicates that under typical rate conditions,adaptable BPC strategies can extend the service life of LFP battery by approximately 123％.Consequently,the developed advanced BPC strategy offers innovative perspectives and insights for the development of long-life battery applications in the future.
查看更多>>摘要：Nickel-rich layered oxide cathode(LiNixCoyMn1-x-yO2,x＞0.5,NCM)shows substantial potential for applications in longer-range electrical vehicles.However,the rapid capacity decay and serious safety con-cerns impede its practical viability.This work provides a hydrogen-bonded organic framework(HOF)modification strategy to simultaneously improve the electrochemical performance,thermal stability and incombustibility of separator.Melamine cyanurate(MCA),as a low-cost and reliable flame-retardant HOF,was implemented in the separator modification layer,which can prevent the battery short circuit even at a high temperature.In addition,the supermolecule properties of MCA provide unique physical and chemical microenvironment for regulating ion-transport behavior in electrolyte.The MCA coating layer enabled the nickel-rich layered oxide cathode with a high-capacity retention of 90.3％after 300 cycles at 1.0 C.Collectively,the usage of MCA in lithium-ion batteries(LIBs)affords a simple,low-cost and efficient strategy to improve the security and service life of nickel-rich layered cathodes.
查看更多>>摘要：Magnesium ion batteries(MIBs)are a potential field for the energy storage of the future but are restricted by insufficient rate capability and rapid capacity degradation.Magnesium-sodium hybrid ion batteries(MSHBs)are an effective way to address these problems.Here,we report a new type of MSHBs that use layered sodium vanadate((Na,Mn)V8O20·5H2O,Mn-NVO)cathodes coupled with an organic 3,4,9,10-perylenetetracarboxylic diimide(PTCDI)anode in Mg2+/Na+hybrid electrolytes.During electro-chemical cycling,Mg2+and Na+co-participate in the cathode reactions,and the introduction of Na+pro-motes the structural stability of the Mn-NVO cathode,as cleared by several ex-situ characterizations.Consequently,the Mn-NVO cathode presents great specific capacity(249.9 mA h g-1 at 300 mA g-1)and cycling(1500 cycles at 1500 mA g-1)in the Mg2+/Na+hybrid electrolytes.Besides,full battery dis-plays long lifespan with 10,000 cycles at 1000 mA g-1.The rate performance and cycling stability of MSHBs have been improved by an economical and scalable method,and the mechanism for these improvements is discussed.
查看更多>>摘要：Aqueous organic redox flow batteries(AORFBs),which exploit the reversible electrochemical reactions of water-soluble organic electrolytes to store electricity,have emerged as an efficient electrochemical energy storage technology for the grid-scale integration of renewable electricity.pH-neutral AORFBs that feature high safety,low corrosivity,and environmental benignity are particularly promising,and their battery performance is significantly impacted by redox-active molecules and ion-exchange membranes(IEMs).Here,representative anolytes and catholytes engineered for use in pH-neutral AORFBs are out-lined and summarized,as well as their side reactions that cause irreversible battery capacity fading.In addition,the recent achievements of IEMs for pH-neutral AORFBs are discussed,with a focus on the con-struction and tuning of ion transport channels.Finally,the critical challenges and potential research opportunities for developing practically relevant pH-neutral AORFBs are presented.
查看更多>>摘要：The unstable electrolyte/lithium(Li)anode interface has been one of the key challenges in realizing high energy density solid-state lithium metal batteries(LMBs)applications.Herein,a dense and uniform silver(Ag)nano interlayer with a thickness of～35 nm is designed accurately by magnetron sputtering technol-ogy to optimize the electrolyte/Li anode interface.This Ag nano layer reacts with Li metal anode to in-situ form Li-Ag alloy,thus enhancing the physical interfacial contact,and further improving the interfacial wettability and compatibility.In particular,the Li-Ag alloy is inclined to form AgLi phase proved by cryo-TEM and DFT,effectively preventing SN from continuously"attacking"the Li metal anode due to the lower adsorption of succinonitrile(SN)molecules on AgLi than that of pure Li metal,thereby signif-icantly reinforcing the interfacial stability.Hence,the enhanced physical and chemical stability of elec-trolyte/Li anode interface promotes the homogeneous deposition of Li+and inhibits the dendrite growth.The Li-symmetric cell maintains stable operation for up to 1700 h and the cycling stability of LiFePO4|SPE|Li full cell is remarkably improved at room temperature(capacity retention rate of 91.9％for 200 cycles).This work opens an effective way for accurate and controllable interface design of long lifespan solid-state LMBs.
查看更多>>摘要：Wide-bandgap(＞1.7 eV)perovskites suffer from severe light-induced phase segregation due to high bro-mine content,causing irreversible damage to devices stability.However,the strategies of suppressing photoinduced phase segregation and related mechanisms have not been fully disclosed.Here,we report a new passivation agent 4-aminotetrahydrothiopyran hydrochloride(4-ATpHCl)with multifunctional groups for the interface treatment of a 1.77-eV wide-bandgap perovskite film.4-ATpH+impeded halogen ion migration by anchoring on the perovskite surface,leading to the inhibition of phase segregation and thus the passivation of defects,which is ascribed to the interaction of 4-ATpH+with perovskite and the formation of low-dimensional perovskites.Finally,the champion device achieved an efficiency of 19.32％with an open-circuit voltage(Voc)of 1.314 V and a fill factor of 83.32％.Moreover,4-ATpHCl modified device exhibited significant improved stability as compared with control one.The target device main-tained 80％of its initial efficiency after 519 h of maximum power output(MPP)tracking under 1 sun illu-mination,however,the control device showed a rapid decrease in efficiency after 267 h.Finally,an efficiency of 27.38％of the champion 4-terminal all-perovskite tandem solar cell was achieved by mechanically stacking this wide-bandgap top subcell with a 1.25-eV low-bandgap perovskite bottom subcell.
查看更多>>摘要：In recent years,water evaporation-induced electricity has attracted a great deal of attention as an emerg-ing green and renewable energy harvesting technology.Although abundant materials have been devel-oped to fabricate hydrovoltaic devices,the limitations of high costs,inconvenient storage and transport,low environmental benefits,and unadaptable shape have restricted their wide applications.Here,an electricity generator driven by water evaporation has been engineered based on natural biomass leather with inherent properties of good moisture permeability,excellent wettability,physicochemical stability,flexibility,and biocompatibility.Including numerous nano/microchannels together with rich oxygen-bearing functional groups,the natural leather-based water evaporator,LeatherEmblic-NPs-SA/CB,could continuously produce electricity even staying outside,achieving a maximum output voltage of～3 V with six-series connection.Furthermore,the leather-based water evaporator has enormous poten-tial for use as a flexible self-powered electronic floor and seawater demineralizer due to its sensitive pres-sure sensing ability as well as its excellent photothermal conversion efficiency(96.3％)and thus fast water evaporation rate(2.65 kg m-2 h-1).This work offers a new and functional material for the con-struction of hydrovoltaic devices to harvest the sustained green energy from water evaporation in arbi-trary ambient environments,which shows great promise in their widespread applications.
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