查看更多>>摘要：The electrocatalytic oxidation of biomass-derived furfural(FF)feedstocks into 2-furoic acid(FA)holds immense industrial potential in optics,cosmetics,polymers,and food.Herein,we fabricated CoO/NiO/nickel foam(NF)and Cu2O/NiO/NF electrodes via in situ pulsed laser irradiation in liquids(PLIL)for the bifunctional electrocatalysis of oxygen evolution reaction(OER)and furfural oxidation reaction(FOR),respectively.Simultaneous oxidation of NF surface to NiO and deposition of CoO and/or Cu2O on NF during PLIL offer distinct advantages for enhancing both the OER and FOR.CoO/NiO/NF electrocatalyst provides a consistently low overpotential of～359 mV(OER)at 10 mA/cm2,achieving the maximum FA yield(～16.37 mM)with 61.5％selectivity,79.5％carbon balance,and a remarkable Faradaic efficiency of～90.1％during 2 h of FOR at 1.43 V(vs.reversible hydrogen electrode).Mechanistic pathway via in situ electrochemical-Raman spectroscopy on CoO/NiO/NF reveals the involvement of phase transition inter-mediates(NiOOH and CoOOH)as surface-active centers during electrochemical oxidation.The carbonyl carbon in FF is attacked by hydroxyl groups to form unstable hydrates that subsequently undergo further oxidation to yield FA products.This method holds promise for large-scale applications,enabling simulta-neous production of renewable building materials and fuel.
查看更多>>摘要：To address climate change and promote environmental sustainability,electrochemical energy conversion and storage systems emerge as promising alternative to fossil fuels,catering to the escalating demand for energy.Achieving optimal energy efficiency and cost competitiveness in these systems requires the strategic design of electrocatalysts,coupled with a thorough comprehension of the underlying mecha-nisms and degradation behavior occurring during the electrocatalysis processes.Scanning electrochem-ical microscopy(SECM),an analytical technique for studying surface electrochemically,stands out as a powerful tool offering electrochemical insights.It possesses remarkable spatiotemporal resolution,enabling the visualization of the localized electrochemical activity and surface topography.This review compiles crucial research findings and recent breakthroughs in electrocatalytic processes utilizing the SECM methodology,specifically focusing on applications in electrolysis,fuel cells,and metal-oxygen bat-teries within the realm of energy conversion and storage systems.Commencing with an overview of each energy system,the review introduces the fundamental principles of SECM,and aiming to provide new perspectives and broadening the scope of applied research by describing the major research categories within SECM.
查看更多>>摘要：Exploring effective energy storage systems is critical to alleviate energy scarcity.Rechargeable zinc-air batteries are promising energy storage devices.However,conventional rechargeable zinc-air battery sys-tems face many challenges associated with electrolytes and electrodes,causing inferior electrochemistry performance.The light-assisted strategy represents a novel and innovative approach to conventional zinc-air battery technology that uses only electrical energy.This strategy effectively combines both light and electrical energy conversion/storage mechanisms.In addition,light-assisted rechargeable zinc-air batteries can achieve photocharging with or without applied electrical bias by partially using solar energy and the acceleration of oxygen reduction/evolution reaction kinetics.In this paper,the working mecha-nism and structural design of the light-assisted rechargeable zinc-air batteries are introduced based on the theory of photoelectrochemistry and its characteristics.Then,the latest advances in electrolyte and photocathode design strategies are discussed in detail.The performance enhancement of aqueous light-assisted rechargeable zinc-air batteries using photoelectric materials is explained.Finally,a sum-mary and outlook on the further modification of properties of light-assisted rechargeable zinc-air batter-ies,especially the photovoltaic electrode catalyst design strategies,are illustrated.This review provides insights and guidance for the design of high-performance light-assisted rechargeable Zn-air batteries for next-generation energy storage devices.
查看更多>>摘要：Electrocatalytic water splitting is crucial for H2 generation via hydrogen evolution reaction(HER)but subject to the sluggish dynamics of oxygen evolution reaction(OER).In this work,single Fe atom-doped MoS2 nanosheets(SFe-DMNs)were prepared based on the high-throughput density functional the-ory(DFT)calculation screening.Due to the synergistic effect between Fe atom and MoS2 and optimized intermediate binding energy,the SFe-DMNs could deliver outstanding activity for both HER and OER.When assembled into a two-electrode electrolytic cell,the SFe-DMNs could achieve the current density of 50 mA cm-2 at a low cell voltage of 1.55 V under neutral condition.These results not only confirmed the effectiveness of high-throughput screening,but also revealed the excellent activity and thus the potential applications in fuel cells of SFe-DMNs.
查看更多>>摘要：Zincophilic property and high electrical conductivity are both very important parameters to design novel Zn anode for aqueous Zn-ion batteries(AZIBs).However,single material is difficult to exhibit zincophilic property and high electrical conductivity at the same time.Herein,originating from theoretical calcula-tion,a zincophilic particle regulation strategy is proposed to address these limitations and carbon coated Na3V2(PO4)3 is taken as an example to be a protective layer on zinc metal(NVPC@Zn).Na3V2(PO4)3(NVP)is a common cathode material for Zn-ion batteries,which is zincophilic.Carbon materials not only offer an electron pathway to help Zn deposition onto NVPC surface,but also enhance the zinc nucleophilicity of Na3V2(PO4)3.Hence,this hybrid coating layer can tune zincdeposition and resist side reactions such as hydrogen generation and Zn metal corrosion.Experimentally,a symmetrical battery with NVPC@Zn elec-trode displays highly reversible plating/stripping behavior with a long cycle lifespan over 1800 h at 2 mA cm-2,much better than carbon and Na3V2(PO4)3 solely modified Zn electrodes.When the Na3V2(PO4)3 is replaced with zincophobic Al2O3 or zincophilic V2O3,the stability of the modified zinc anodes is also prolonged.This strategy expands the option of zincophilic materials and provides a general and effective way to stabilize the Zn electrode.
查看更多>>摘要：An in-depth mechanism in zonal activation of CO2 and H2 molecular over dual-active sites has not been revealed yet.Here,Ni-Co-MgO was rationally constructed to elucidate the CO2 methanation mechanism.The abundant surface nickel and cobalt components as active sites led to strong Ni-Co interaction with charge transfer from nickel to cobalt.Notably,electron-enriched Coδ-species participated in efficient chemisorption and activation of CO2 to generate monodentate carbonate.Simultaneously,plentiful avail-able Ni0 sites facilitated H2 dissociation,thus CO2 and H2 were smoothly activated at zones of Coδ-species and Ni0,respectively.Detailed in situ DRIFTS,quasi situ XPS,TPSR,and DFT calculations substantiated a new formate evolution mechanism via monodentate carbonate instead of traditional bidentate carbonate based on synergistic catalysis of Coδ-species and Ni0.The zonal activation of CO2 and H2 by tuning elec-tron behaviors of double-center catalysts can boost heterogeneous catalytic hydrogenation performance.
查看更多>>摘要：Urea holds promise as an alternative water-oxidation substrate in electrolytic cells.High-valence nickel-based spinel,especially after heteroatom doping,excels in urea oxidation reactions(UOR).However,traditional spinel synthesis methods with prolonged high-temperature reactions lack kinetic precision,hindering the balance between controlled doping and highly active two-dimensional(2D)porous struc-tures design.This significantly impedes the identification of electron configuration-dependent active sites in doped 2D nickel-based spinels.Herein,we present a microwave shock method for the preparation of 2D porous NiCo2O4 spinel.Utilizing the transient on-off property of microwave pulses for precise heteroatom doping and 2D porous structural design,non-metal doping(boron,phosphorus,and sulfur)with distinct extranuclear electron disparities serves as straightforward examples for investigation.Precise tuning of lattice parameter reveals the impact of covalent bond strength on NiCo2O4 structural stability.The introduced defect levels induce unpaired d-electrons in transition metals,enhancing the adsorption of electron-donating amino groups in urea molecules.Simultaneously,Bode plots confirm the impact mechanism of rapid electron migration caused by reduced band gaps on UOR activity.The pre-pared phosphorus-doped 2D porous NiCo2O4,with optimal electron configuration control,outperforms most reported spinels.This controlled modification strategy advances understanding theoretical structure-activity mechanisms of high-performance 2D spinels in UOR.
查看更多>>摘要：Although the performance of perovskite solar cells(PSCs)has been dramatically increased in recent years,stability is still the main obstacle preventing the PSCs from being commercial.PSC device instability can be caused by a variety of reasons,including ions diffusion,surface and grain boundary defects,etc.In this work,the cross-linkable tannic acid(TA)is introduced to modify perovskite film through post-treatment method.The numerous organic functional groups(-OH and C=O)in TA can interact with the uncoordi-nated Pb2+and I- ions in perovskite,thus passivating defects and inhibiting ions diffusion.In addition,the formed TA network can absorb a small amount of the residual moisture inside the device to protect the perovskite layer.Furthermore,TA modification regulates the energy level of perovskite,and reduces interfacial charge recombination.Ultimately,following TA treatment,the device efficiency is increased significantly from 21.31％to 23.11％,with a decreased hysteresis effect.Notably,the treated device shows excellent air,thermal,and operational stability.In light of this,the readily available,inexpensive TA has the potential to operate as a multipurpose interfacial modifier to increase device efficiency while also enhancing device stability.
查看更多>>摘要：It is challenging for aqueous Zn-ion batteries(ZIBs)to achieve comparable low-temperature(low-T)per-formance due to the easy-frozen electrolyte and severe Zn dendrites.Herein,an aqueous electrolyte with a low freezing point and high ionic conductivity is proposed.Combined with molecular dynamics simu-lation and multi-scale interface analysis(time of flight secondary ion mass spectrometry three-dimensional mapping and in-situ electrochemical impedance spectroscopy method),the temperature independence of the V2O5 cathode and Zn anode is observed to be opposite.Surprisingly,dominated by the solvent structure of the designed electrolyte at low temperatures,vanadium dissolution/shuttle is significantly inhibited,and the zinc dendrites caused by this electrochemical crosstalk are greatly relieved,thus showing an abnormal temperature inversion effect.Through the disclosure and improve-ment of the above phenomena,the designed Zn||V2O5 full cell delivers superior low-T performance,main-taining almost 99％capacity retention after 9500 cycles(working more than 2500 h)at-20 ℃.This work proposes a kind of electrolyte suitable for low-T ZIBs and reveals the inverse temperature dependence of the Zn anode,which might offer a novel perspective for the investigation of low-T aqueous battery systems.
查看更多>>摘要：The photoreduction of CO2 into CH4 with simultaneous high activity and selectivity is a promising strat-egy to increase energy supply and alleviate global warming.However,the absence of the active sites that is responsible for the adsorption and activation of CO2 and the generation of CO and H2 via side reactions often lead to poor efficiency and low selectivity of the catalyst.Herein,Cu,Pd,and PdCu metal clusters cocatalyst-anchored defective TiO2 nanotubes(Cu/TiO2-SBO,Pd/TiO2-SBO,and Pd1Cu1/TiO2-SBO)were designed via a simple solution impregnation reduction and applied for photocatalytic conversion of CO2 to CH4.The Pd1Cu1/TiO2-SBO photocatalyst exhibits excellent catalytic performance among the other catalysts for photoreduction of CO2 into CH4.More interestingly,the product selectivity of CH4 reaches up to 100％with a rate of 25 pmol g-1 h-1.In-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)simulations indicate that the main reasons for the high selectivity of CH4 are attributed to the PdCu alloy and oxygen vacancies,which jointly enhance the pho-toinduced carrier separation and lower energy barriers of key intermediates.Moreover,due to the tun-able d-band center of the Cu site in the PdCu alloy,the generated intermediates can be well prevented from poisoning and promoted to participate in further reactions.Hopefully,the current study will provide insight into the development of new,highly selective photocatalysts for the visible light-catalytic reduc-tion of CO2 into CH4.
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