SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish ...SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish reaction kinetics,low electronic conductivity,and large volume changes during charge and discharge hinder the practical applications of SnO_(2)-based electrodes for SIBs and PIBs.Engineering rational structures with fast charge/ion transfer and robust stability is important to overcoming these challenges.Herein,S-doped SnO_(2)(S-SnO_(2))quantum dots(QDs)(≈3 nm)encapsulated in an N,S codoped carbon fiber networks(S-SnO_(2)-CFN)are rationally fabricated using a sequential freeze-drying,calcination,and S-doping strategy.Experimental analysis and density functional theory calculations reveal that the integration of S-SnO_(2) QDs with N,S codoped carbon fiber network remarkably decreases the adsorption energies of Na/K atoms in the interlayer of SnO_(2)-CFN,and the S doping can increase the conductivity of SnO_(2),thereby enhancing the ion transfer kinetics.The synergistic interaction between S-SnO_(2) QDs and N,S codoped carbon fiber network results in a composite with fast Na+/K+storage and extraordinary long-term cyclability.Specifically,the S-SnO_(2)-CFN delivers high rate capacities of 141.0 mAh g^(−1) at 20 A g^(−1) in SIBs and 102.8 mAh g^(−1) at 10 A g^(−1) in PIBs.Impressively,it delivers ultra-stable sodium storage up to 10,000 cycles at 5 A g^(−1) and potassium storage up to 5000 cycles at 2 A g^(−1).This study provides insights into constructing metal oxide-based carbon fiber network structures for high-performance electrochemical energy storage and conversion devices.展开更多
LiBH_(4)with high hydrogen storage density,is regarded as one of the most promising hydrogen storage materials.Nevertheless,it suffers from high dehydrogenation temperature and poor reversibility for practical use.Nan...LiBH_(4)with high hydrogen storage density,is regarded as one of the most promising hydrogen storage materials.Nevertheless,it suffers from high dehydrogenation temperature and poor reversibility for practical use.Nanoconfinement is effective in achieving low dehydrogenation temperature and favorable reversibility.Besides,graphene can serve as supporting materials for LiBH_(4)catalysts and also destabilize LiBH_(4)via interfacial reaction.However,graphene has never been used alone as a frame material for nanoconfining LiBH_(4).In this study,graphene microflowers with large pore volumes were prepared and used as nanoconfinement framework material for LiBH_(4),and the nanoconfinement effect of graphene was revealed.After loading 70 wt%of LiBH_(4) and mechanically compressed at 350 MPa,8.0 wt% of H2 can be released within 100 min at 320C,corresponding to the highest volumetric hydrogen storage density of 94.9 g H2 L^(-1)ever reported.Thanks to the nanoconfinement of graphene,the rate-limiting step of dehydrogenation of nanoconfined LiBH_(4) was changed and its apparent activation energy of the dehydrogenation(107.3 kJ mol^(-1))was 42%lower than that of pure LiBH_(4).Moreover,the formation of the intermediate Li_(2)B_(12)H_(12) was effectively inhibited,and the stable nanoconfined structure enhanced the reversibility of LiBH_(4).This work widens the understanding of graphene's nanoconfinement effect and provides new insights for developing high-density hydrogen storage materials.展开更多
While the rechargeable aqueous zinc-ion batteries(AZIBs)have been recognized as one of the most viable batteries for scale-up application,the instability on Zn anode–electrolyte interface bottleneck the further devel...While the rechargeable aqueous zinc-ion batteries(AZIBs)have been recognized as one of the most viable batteries for scale-up application,the instability on Zn anode–electrolyte interface bottleneck the further development dramatically.Herein,we utilize the amino acid glycine(Gly)as an electrolyte additive to stabilize the Zn anode–electrolyte interface.The unique interfacial chemistry is facilitated by the synergistic“anchor-capture”effect of polar groups in Gly molecule,manifested by simultaneously coupling the amino to anchor on the surface of Zn anode and the carboxyl to capture Zn^(2+)in the local region.As such,this robust anode–electrolyte interface inhibits the disordered migration of Zn^(2+),and effectively suppresses both side reactions and dendrite growth.The reversibility of Zn anode achieves a significant improvement with an average Coulombic efficiency of 99.22%at 1 mA cm^(−2)and 0.5 mAh cm^(−2)over 500 cycles.Even at a high Zn utilization rate(depth of discharge,DODZn)of 68%,a steady cycle life up to 200 h is obtained for ultrathin Zn foils(20μm).The superior rate capability and long-term cycle stability of Zn–MnO_(2)full cells further prove the effectiveness of Gly in stabilizing Zn anode.This work sheds light on additive designing from the specific roles of polar groups for AZIBs.展开更多
The development of high-performance binders is a simple but effective approach to address the rapid capacity decay of high-capacity anodes caused by large volume change upon lithiation/delithiation.Herein,we demonstra...The development of high-performance binders is a simple but effective approach to address the rapid capacity decay of high-capacity anodes caused by large volume change upon lithiation/delithiation.Herein,we demonstrate a unique organic/inorganic hybrid binder system that enables an efficient in situ crosslinking of aqueous binders(e.g.,sodium alginate(SA)and carboxymethyl cellulose(CMC))by reacting with an inorganic crosslinker(sodium metaborate hydrate(SMH))upon vacuum drying.The resultant 3D interconnected networks endow the binders with strong adhesion and outstanding self-healing capability,which effectively improve the electrode integrity by preventing fracturing and exfoliation during cycling and facilitate Li^(+)ion transfer.SiO anodes fabricated from the commercial microsized powders with the SA/0.2SMH binder maintain 1470 mAh g^(-1)of specific capacity at 100 mA g^(-1)after 200 cycles,which is 5 times higher than that fabricated with SA binder alone(293 mAh g^(-1)).Nearly,no capacity loss was observed over 500 cycles when limiting discharge capacity at 1500 mAh g^(-1).The new binders also dramatically improved the performance of Fe_(2)O_(3),Fe_(3)O_(4),NiO,and Si electrodes,indicating the excellent applicability.This finding represents a novel strategy in developing high-performance aqueous binders and improves the prospect of using high-capacity anode materials in Li-ion batteries.展开更多
The rapid advance of mild aqueous zinc-ion batteries(ZIBs)is driving the development of the energy storage system market.But the thorny issues of Zn anodes,mainly including dendrite growth,hydrogen evolution,and corro...The rapid advance of mild aqueous zinc-ion batteries(ZIBs)is driving the development of the energy storage system market.But the thorny issues of Zn anodes,mainly including dendrite growth,hydrogen evolution,and corrosion,severely reduce the performance of ZIBs.To commercialize ZIBs,researchers must overcome formidable challenges.Research about mild aqueous ZIBs is still developing.Various technical and scientific obstacles to designing Zn anodes with high stripping efficiency and long cycling life have not been resolved.Moreover,the performance of Zn anodes is a complex scientific issue determined by various parameters,most of which are often ignored,failing to achieve the maximum performance of the cell.This review proposes a comprehensive overview of existing Zn anode issues and the corresponding strategies,frontiers,and development trends to deeply comprehend the essence and inner connection of degradation mechanism and performance.First,the formation mechanism of dendrite growth,hydrogen evolution,corrosion,and their influence on the anode are analyzed.Furthermore,various strategies for constructing stable Zn anodes are summarized and discussed in detail from multiple perspectives.These strategies are mainly divided into interface modification,structural anode,alloying anode,intercalation anode,liquid electrolyte,non-liquid electrolyte,separator design,and other strategies.Finally,research directions and prospects are put forward for Zn anodes.This contribution highlights the latest developments and provides new insights into the advanced Zn anode for future research.展开更多
The practical application of lithium-sulfur batteries is severely hampered by the poor conductivity,polysulfide shuttle effect and sluggish reaction kinetics of sulfur cathodes.Herein,a hierarchi-cally porous three-di...The practical application of lithium-sulfur batteries is severely hampered by the poor conductivity,polysulfide shuttle effect and sluggish reaction kinetics of sulfur cathodes.Herein,a hierarchi-cally porous three-dimension(3D)carbon architecture assembled by cross-linked carbon leaves with implanted atomic Co-N4 has been deli-cately developed as an advanced sulfur host through a SiO_(2)-mediated zeolitic imidazolate framework-L(ZIF-L)strategy.The unique 3D architectures not only provide a highly conductive network for fast electron transfer and buffer the volume change upon lithiation-delithi-ation process but also endow rich interface with full exposure of Co-N4 active sites to boost the lithium polysulfides adsorption and conversion.Owing to the accelerated kinetics and suppressed shuttle effect,the as-prepared sulfur cathode exhibits a superior electrochemical perfor-mance with a high reversible specific capacity of 695 mAh g^(−1) at 5 C and a low capacity fading rate of 0.053%per cycle over 500 cycles at 1 C.This work may provide a promising solution for the design of an advanced sulfur-based cathode toward high-performance Li-S batteries.展开更多
Exploring highly active but inexpensive electrocatalysts for the hydrogen evolution reaction(HER)is of critical importance for hydrogen production from electrochemical water splitting.Herein,we report a multicomponent...Exploring highly active but inexpensive electrocatalysts for the hydrogen evolution reaction(HER)is of critical importance for hydrogen production from electrochemical water splitting.Herein,we report a multicomponent catalyst with exceptional activity and durability for HER,in which cobalt nanoparticles were in-situ confined inside bamboo-like carbon nanotubes(CNTs)while ultralow ruthenium loading(~2.6μg per electrode area~cm^(−2))is uniformly deposited on their exterior walls(Co@CNTsǀRu).The atomic-scale structural investigations and theoretical calculations indicate that the confined inner Co and loaded outer Ru would induce charge redistribution and a synergistic electron coupling,not only optimizing the adsorption energy of H intermediates(ΔGH*)but also facilitating the electron/mass transfer.The as-developed Co@CNTsǀRu composite catalyst requires overpotentials of only 10,32,and 63 mV to afford a current density of 10 mA cm^(−2) in alkaline,acidic and neutral media,respectively,representing top-level catalytic activity among all reported HER catalysts.The current work may open a new insight into the rational design of carbon-supported metal catalysts for practical applications.展开更多
Magnesium hydride(MgH2) is one of the most promising hydrogen storage materials for practical application due to its favorable reversibility, low cost and environmental benign;however, it suffers from high dehydrogena...Magnesium hydride(MgH2) is one of the most promising hydrogen storage materials for practical application due to its favorable reversibility, low cost and environmental benign;however, it suffers from high dehydrogenation temperature and slow sorption kinetics.Exploring proper catalysts with high and sustainable activity is extremely desired for substantially improving the hydrogen storage properties of MgH2. In this work, a composite catalyst with high-loading of ultrafine Ni nanoparticles(NPs) uniformly dispersed on porous hollow carbon nanospheres is developed, which shows superior catalytic activity towards the de-/hydrogenation of MgH2. With an addition of 5wt% of the composite, which contains 90 wt% Ni NPs, the onset and peak dehydrogenation temperatures of MgH2are lowered to 190 and 242 ℃, respectively. 6.2 wt% H2is rapidly released within 30 min at 250 ℃. The amount of H2that the dehydrogenation product can absorb at a low temperature of 150 ℃ in only 250 s is very close to the initial dehydrogenation value. A dehydrogenation capacity of 6.4wt% remains after 50 cycles at a moderate cyclic regime, corresponding to a capacity retention of 94.1%. The Ni NPs are highly active,reacting with MgH2and forming nanosized Mg2Ni/Mg2NiH4. They act as catalysts during hydrogen sorption cycling, and maintain a high dispersibility with the help of the dispersive role of the carbon substrate, leading to sustainably catalytic activity. The present work provides new insight into designing stable and highly active catalysts for promoting the(de)hydrogenation kinetics of MgH2.展开更多
Magnesium metal anode holds great potentials toward future high energy and safe rechargeable magnesium battery technology due to its divalent redox and dendrite-free nature. Electrolytes based on Lewis acid chemistry ...Magnesium metal anode holds great potentials toward future high energy and safe rechargeable magnesium battery technology due to its divalent redox and dendrite-free nature. Electrolytes based on Lewis acid chemistry enable the reversible Mg plating/stripping,while they fail to match most cathode materials toward highvoltage magnesium batteries. Herein,reversible Mg plating/stripping is achieved in conventional carbonate electrolytes enabled by the cooperative solvation/surface engineering. Strongly electronegative Cl from the MgCl_(2) additive of electrolyte impairs the Mg…O = C interaction to reduce the Mg^(2+) desolvation barrier for accelerated redox kinetics,while the Mg^(2+)-conducting polymer coating on the Mg surface ensures the facile Mg^(2+) migration and the e ective isolation of electrolytes. As a result,reversible plating and stripping of Mg is demonstrated with a low overpotential of 0.7 V up to 2000 cycles. Moreover,benefitting from the wide electrochemical window of carbonate electrolytes,high-voltage(> 2.0 V) rechargeable magnesium batteries are achieved through assembling the electrode couple of Mg metal anode and Prussian blue-based cathodes. The present work provides a cooperative engineering strategy to promote the application of magnesium anode in carbonate electrolytes toward high energy rechargeable batteries.展开更多
The ternary amides LiK2(NH2)3, LiK(NH2)2, and Li3 K(NH2)4 are successfully synthesized by ball milling mixtures of LiNH2 and KNH2, and the hydrogen storage properties of Li3K(NH2)4–xMgH2(x = 1, 2, 3,4) are systematic...The ternary amides LiK2(NH2)3, LiK(NH2)2, and Li3 K(NH2)4 are successfully synthesized by ball milling mixtures of LiNH2 and KNH2, and the hydrogen storage properties of Li3K(NH2)4–xMgH2(x = 1, 2, 3,4) are systematically investigated. The Li3K(NH2)4–2 Mg H2 sample displays optimized hydrogen storage properties, releasing 6.37 wt% of hydrogen in a two-stage reaction with an onset temperature of 60 °C.The first dehydrogenation stage exhibits good reaction kinetics and thermodynamic properties because of a lower activation energy and appropriate enthalpy change. After full dehydrogenation at 130 °C, the Li3K(NH2)4–2 MgH2 sample absorbs 3.80 wt% of H2 below 160 °C in a variable temperature hydrogenation mode. Mechanistic investigations indicate that Li3 K(NH2)4 reacts with Mg H2 to produce Mg(NH2)2, LiH,and KH during ball milling. In the heating process, Mg(NH2)2 first reacts with Li H to form Li2 Mg2 N3 H3 and Li NH2, while KH works as a catalyst, and then, KH reacts with Li2Mg2N3H3 and Li NH2 to generate a new K-containing compound.展开更多
Superior catalyst supports are crucial to developing advanced electrocatalysts toward heterogeneous catalytic reactions.Herein,we systematically investigate the role of transition metal‐functionalized N‐doped carbon...Superior catalyst supports are crucial to developing advanced electrocatalysts toward heterogeneous catalytic reactions.Herein,we systematically investigate the role of transition metal‐functionalized N‐doped carbon nanosheets(M‐N‐C,M=Mn,Fe,Co,Ni,Cu,Mo,and Ag)as the multifunctional electrocatalyst supports toward hydrogen evolution/oxidation reactions(HER/HOR)in alkaline media.The results demonstrate that all the M‐N‐C nanosheets,except Cu‐N‐C and Ag‐N‐C,can promote the alkaline HER/HOR electrocatalytic activity of Pt by accelerating the sluggish Volmer step,among which Mn plays a more significant role.Analyses reveal that the promotion effect of M‐N‐C support is closely associated with the electronegativity of the metal dopants and the relative filling degree of their d‐orbitals.For one,the metal dopant in M‐N‐C with smaller electronegativity would provide more electrons to oxygen and hence tune the electronic structure of Pt via the M‐O‐Pt bonds at the interface.For another,the transition metal in M‐N4 moieties with more empty d orbitals would hybridize with O 2p orbitals more strongly that promotes the adsorption of water/hydroxyl species.The results demonstrate the conceptual significance of multifunctional supports and would inspire the future development of advanced electrocatalysts.展开更多
In recent years,a series of aqueous metal ion batteries(AMIBs)has been developed to improve the safety and cost-efficiency of portable electronics and electric vehicles.However,the significant gaps in energy density,p...In recent years,a series of aqueous metal ion batteries(AMIBs)has been developed to improve the safety and cost-efficiency of portable electronics and electric vehicles.However,the significant gaps in energy density,power density,and cycle stability of AMIBs directly hinder them from replacing the currently widely used non-aqueous metal ion batteries,which stems from the lack of reasonable configuration and performance optimization of electrode materials.First-row transition metal compounds(FRTMCs),with the advantages of optional voltage ranges(from low to high),adjustable crystal structures(layered and tunnel types with large spacing),and designable morphology(multi-dimensional nanostructures),are widely used to construct high-performance AMIBs.However,no comprehensive review papers were generated to highlight their specific and significant roles in AMIBs.In this review,we first summarize the superiority and characteristics of FRTMCs in AMIBs.Then,we put forward control strategies of FRTMCs from subsurface engineering to inner construction to promote capacitance control and diffusion control energy storage.After that,the electrochemical performance of the FRTMCs regulation strategies in AMIBs is reviewed.Finally,we present potential directions and challenges for further enhancements of FRTMCs in AMIBs.The review aims to provide an in-depth understanding of regulation strategies for enhancing energy storage to build high-performance AMIBs that meet practical applications.展开更多
Solid-state sodium metal batteries utilizing inorganic solid electrolytes(SEs)hold immense potentials such as intrinsical safety,high energy density,and environmental sustainability.However,the interfacial inhomogenei...Solid-state sodium metal batteries utilizing inorganic solid electrolytes(SEs)hold immense potentials such as intrinsical safety,high energy density,and environmental sustainability.However,the interfacial inhomogeneity/instability at the anode-SE interface usually triggers the penetration of sodium dendrites into the electrolyte,leading to short circuit and battery failure.Herein,confronting with the original nonuniform and high-resistance solid electrolyte interphase(SEI)at the Na-Na_(3)Zr_(2)Si_(2)PO_(12)interface,an oxygen-regulated SEI innovative approach is proposed to enhance the cycling stability of anode-SEs interface,through a spontaneous reaction between the metallic sodium(containing trace amounts of oxygen)and the Na_(3)Zr_(2)Si_(2)POi_(2)SE.The oxygen-regulated spontaneous SEI is thin,uniform,and kinetically stable to facilitate homogenous interfacial Na^+transportation,Benefitting from the optimized SEI,the assembled symmetric cell exhibits an ultra-stable sodium plating/stripping cycle for over 6600 h under a practical capacity of 3 mAh cm^(-2).Qua si-sol id-state batteries with Na_(3)V_(2)(PO_(4))_(3)cathode deliver excellent cyclability over 500 cycles at a rate of 0.5 C(1 C=117 mA cm^(-2))with a high capacity retention of95.4%.This oxygen-regulated SEI strategy may offer a potential avenue for the future development of high-energy-density solid-state metal batteries.展开更多
The sluggish reaction kinetics of alkaline hydrogen oxidation reaction(HOR)is one of the key challenges for anion exchange membrane fuel cells(AEMFCs).To achieve robust alkaline HOR with minimized cost,we developed a ...The sluggish reaction kinetics of alkaline hydrogen oxidation reaction(HOR)is one of the key challenges for anion exchange membrane fuel cells(AEMFCs).To achieve robust alkaline HOR with minimized cost,we developed a single atom-cluster multiscale structure with isolated Pt single atoms anchored on Ru nanoclusters supported on nitrogen-doped carbon nanosheets(Pt1-Ru/NC).The well-defined structure not only provides multiple sites with varied affinity with the intermediates but also enables simultaneous modulation of different sites via interfacial interaction.In addition to weakening Ru–H bond strength,the isolated Pt sites are heavily involved in hydrogen adsorption and synergistically accelerate the Volmer step with the help of Ru sites.Furthermore,this catalyst configuration inhibits the excessive occupancy of oxygen-containing species on Ru sites and facilitates the HOR at elevated potentials.The Pt1-Ru/NC catalyst exhibits superior alkaline HOR performance with extremely high activity and excellent CO-tolerance.An AEMFC with a 0.1 mg·cmPGM^(−2)loading of Pt1-Ru/NC anode catalyst achieves a peak powder density of 1172 mW·cm^(−2),which is 2.17 and 1.55 times higher than that of Pt/C and PtRu/C,respectively.This work provides a new catalyst concept to address the sluggish kinetics of electrocatalytic reactions containing multiple intermediates and elemental steps.展开更多
Solid-state batteries(SSBs)have received widespread attention with their high safety and high energy density characteristics.However,solid-solid contacts in the internal electrode material and the electrode material/s...Solid-state batteries(SSBs)have received widespread attention with their high safety and high energy density characteristics.However,solid-solid contacts in the internal electrode material and the electrode material/solid electrolyte(SE)interfaces,as well as the severe electrochemo-mechanical effects caused by the internal stress due to the volume change of the active material,these problems hinder ion/electron transport within the SSBs,which significantly deteriorates the electrochemical performance.Applying fabrication pressures and stack pressures are effective measures to improve solid-solid contact and solve electrochemo-mechanical problems.Herein,the influences of different pressures on cathode material,anode material,SEs,and electrode/SEs interface are briefly summarized from the perspective of interface ion diffusion,transmission of electrons and ions in internal particles,current density and ion diffusion kinetics,and the volume changes of Li^(+)stripping/plating based on two physical contact models,and point out the direction for the future research direction of SSBs and advancing industrialization by building the relationship between pressures and SSBs electrochemistry.展开更多
Single-atom materials(SAMs)have become one of the most important power sources to push the field of energy conversion forward.Among the main types of energy,including thermal energy,electrical energy,solar energy,and ...Single-atom materials(SAMs)have become one of the most important power sources to push the field of energy conversion forward.Among the main types of energy,including thermal energy,electrical energy,solar energy,and biomass energy,SAMs have realized ultra-high efficiency and show an appealing future in practical application.More than high activity,the uniform active sites also provide a convincible model for chemists to design and comprehend the mechanism behind the phenomenon.Therefore,we presented an insightful review of the application of the single-atom material in the field of energy conversion.The challenges(e.g.,accurate synthesis and practical application)and future directions(e.g.,machine learning and efficient design)of the applications of SAMs in energy conversion are included,aiming to provide guidance for the research in the next step.展开更多
Nanoscaled catalysts have attracted much more attention due to their more abundant active sites and better dispersion than their bulky counterparts.In this work,VH_(x) nanoparticles smaller than 10 nm in average size ...Nanoscaled catalysts have attracted much more attention due to their more abundant active sites and better dispersion than their bulky counterparts.In this work,VH_(x) nanoparticles smaller than 10 nm in average size are successfully synthesized by a simple solid-state ball milling coupled with THF washing process,which are proved to be highly effective in enhancing the hydrogen absorption/desorption kinetics of MgH_(2) at moderate temperatures.The nano-VH_(x)-modified MgH_(2) releases hydrogen from 182℃,which is 88℃ lower than additive-free MgH_(2).The release of hydrogen amounts to 6.3 wt%H within 10 min at 230℃ and 5.6 wt%H after 30 min at 215℃ with initial vacuum.More importantly,the dehydro-genated MgH_(2)+10 wt.%nano-VH_(x) rapidly absorbs 5.2 wt%H within 3 min at 50℃ under 50 bar H_(2).It even takes up 4.3 wt%H within 30 min at room temperature(25℃)under 10 bar H_(2),exhibiting supe-rior hydrogenation kinetics to most of the previous reports.Mechanistic analyzes disclose the reversible transformation between V and V-H species during the hydrogen desorption-absorption process.The ho-mogeneously distributed V-based species is believed to act as hydrogen pump and nucleation sites for MgH_(2) and Mg,respectively,thus triggering fast hydrogenation/dehydrogenation kinetics.展开更多
Proton exchange membrane water electrolyzer(PEMWE)driven by renewable electricity is a promising technique toward green hydrogen production,but the corrosive environment and high working potential pose severe challeng...Proton exchange membrane water electrolyzer(PEMWE)driven by renewable electricity is a promising technique toward green hydrogen production,but the corrosive environment and high working potential pose severe challenges for developing advanced electrocatalysts for the oxygen evolution reaction(OER).Although Ir-based materials possess relatively balanced activity and stability for the OER,their dissolution behavior cannot be neglected,in particular under high working potentials.In this work,iridium dioxide(IrO_(2))nanoparticles(NPs)were anchored on the surface of exfoliated h-boron nitride(BN)nanosheets(NSs)toward the OER reaction in acid media.Highly active Ir(V)species were stabilized by the epitaxial interface between IrO_(2)and h-BN,and therefore the IrO_(2)/BN delivered stable performance at increased working potentials,while the activity of bare IrO_(2)NPs without h-BN support decreased rapidly.Also,the smaller lattice spacing of h-BN induced compressive strain for IrO_(2),resulting in improved activity.Our results demonstrate the feasibility of stabilizing highly active Ir(V)species for the OER in acid media by constructing robust interface and provide new possibilities toward designing advanced heterostructured electrocatalysts.展开更多
The storage of hydrogen in a compact,safe and cost-effective manner can be one of the key enabling technologies to power a more sustainable society.Magnesium hydride(MgH_(2))has attracted strong research interest as a...The storage of hydrogen in a compact,safe and cost-effective manner can be one of the key enabling technologies to power a more sustainable society.Magnesium hydride(MgH_(2))has attracted strong research interest as a hydrogen carrier because of its high gravimetric and volumetric hydrogen densities.However,the practical use of MgH_(2)for hydrogen storage has been limited due to high operation temperatures and sluggish kinetics.Catalysis is of crucial importance for the enhancement of hydrogen cycling kinetics of Mg/MgH_(2)and considerable work has been focused on designing,fabricating and optimizing catalysts.This review covers the recent advances in catalyzed Mg-based hydrogen storage materials.The fundamental properties and the syntheses of MgH_(2)as a hydrogen carrier are first briefly reviewed.After that,the general catalysis mechanisms and the catalysts developed for hydrogen storage in MgH_(2)are summarized in detail.Finally,the challenges and future research focus are discussed.Literature studies indicate that transition metals,rare-earth metals and their compounds are quite effective in catalyzing hydrogen storage in Mg/MgH_(2).Most metal-containing compounds were converted in situ to elemental metal or their magnesium alloys,and their particle sizes and dispersion affect their catalytic activity.The in-situ construction of catalyzed ultrasmall Mg/MgH_(2)nanostructures(<10 nm in size)is believed to be the future research focus.These important insights will help with the design and development of high-performance catalysts for hydrogen storage in Mg/MgH_(2).展开更多
基金National Natural Science Foundation of China,Grant/Award Number:51971065Innovation Program of Shanghai Municipal Education Commission,Grant/Award Number:2019-01-07-00-07-E00028。
文摘SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish reaction kinetics,low electronic conductivity,and large volume changes during charge and discharge hinder the practical applications of SnO_(2)-based electrodes for SIBs and PIBs.Engineering rational structures with fast charge/ion transfer and robust stability is important to overcoming these challenges.Herein,S-doped SnO_(2)(S-SnO_(2))quantum dots(QDs)(≈3 nm)encapsulated in an N,S codoped carbon fiber networks(S-SnO_(2)-CFN)are rationally fabricated using a sequential freeze-drying,calcination,and S-doping strategy.Experimental analysis and density functional theory calculations reveal that the integration of S-SnO_(2) QDs with N,S codoped carbon fiber network remarkably decreases the adsorption energies of Na/K atoms in the interlayer of SnO_(2)-CFN,and the S doping can increase the conductivity of SnO_(2),thereby enhancing the ion transfer kinetics.The synergistic interaction between S-SnO_(2) QDs and N,S codoped carbon fiber network results in a composite with fast Na+/K+storage and extraordinary long-term cyclability.Specifically,the S-SnO_(2)-CFN delivers high rate capacities of 141.0 mAh g^(−1) at 20 A g^(−1) in SIBs and 102.8 mAh g^(−1) at 10 A g^(−1) in PIBs.Impressively,it delivers ultra-stable sodium storage up to 10,000 cycles at 5 A g^(−1) and potassium storage up to 5000 cycles at 2 A g^(−1).This study provides insights into constructing metal oxide-based carbon fiber network structures for high-performance electrochemical energy storage and conversion devices.
基金supported by National Key Research and Development Program of China(2021YFB4000602)National Natural Science Foundation of PR China(Nos.52071287,52072342,52271227)+3 种基金National Outstanding Youth Foundation of China(No.52125104)Natural Science Foundation of Zhejiang Province,PR China(No.LZ23E010002)Young Talent Fund of Association for Science and Technology in Shaanxi,China(No.20220456)Young Star Project of Science and Technology of Shaanxi Province(2022KJXX-43).
文摘LiBH_(4)with high hydrogen storage density,is regarded as one of the most promising hydrogen storage materials.Nevertheless,it suffers from high dehydrogenation temperature and poor reversibility for practical use.Nanoconfinement is effective in achieving low dehydrogenation temperature and favorable reversibility.Besides,graphene can serve as supporting materials for LiBH_(4)catalysts and also destabilize LiBH_(4)via interfacial reaction.However,graphene has never been used alone as a frame material for nanoconfining LiBH_(4).In this study,graphene microflowers with large pore volumes were prepared and used as nanoconfinement framework material for LiBH_(4),and the nanoconfinement effect of graphene was revealed.After loading 70 wt%of LiBH_(4) and mechanically compressed at 350 MPa,8.0 wt% of H2 can be released within 100 min at 320C,corresponding to the highest volumetric hydrogen storage density of 94.9 g H2 L^(-1)ever reported.Thanks to the nanoconfinement of graphene,the rate-limiting step of dehydrogenation of nanoconfined LiBH_(4) was changed and its apparent activation energy of the dehydrogenation(107.3 kJ mol^(-1))was 42%lower than that of pure LiBH_(4).Moreover,the formation of the intermediate Li_(2)B_(12)H_(12) was effectively inhibited,and the stable nanoconfined structure enhanced the reversibility of LiBH_(4).This work widens the understanding of graphene's nanoconfinement effect and provides new insights for developing high-density hydrogen storage materials.
基金supported by National Key R&D Program(2022YFB2502000)Zhejiang Provincial Natural Science Foundation of China(LZ23B030003)+1 种基金the Fundamental Research Funds for the Central Universities(2021FZZX001-09)the National Natural Science Foundation of China(52175551).
文摘While the rechargeable aqueous zinc-ion batteries(AZIBs)have been recognized as one of the most viable batteries for scale-up application,the instability on Zn anode–electrolyte interface bottleneck the further development dramatically.Herein,we utilize the amino acid glycine(Gly)as an electrolyte additive to stabilize the Zn anode–electrolyte interface.The unique interfacial chemistry is facilitated by the synergistic“anchor-capture”effect of polar groups in Gly molecule,manifested by simultaneously coupling the amino to anchor on the surface of Zn anode and the carboxyl to capture Zn^(2+)in the local region.As such,this robust anode–electrolyte interface inhibits the disordered migration of Zn^(2+),and effectively suppresses both side reactions and dendrite growth.The reversibility of Zn anode achieves a significant improvement with an average Coulombic efficiency of 99.22%at 1 mA cm^(−2)and 0.5 mAh cm^(−2)over 500 cycles.Even at a high Zn utilization rate(depth of discharge,DODZn)of 68%,a steady cycle life up to 200 h is obtained for ultrathin Zn foils(20μm).The superior rate capability and long-term cycle stability of Zn–MnO_(2)full cells further prove the effectiveness of Gly in stabilizing Zn anode.This work sheds light on additive designing from the specific roles of polar groups for AZIBs.
基金support from the National Outstanding Youth Foundation of China(52125104)the National Natural Science Foundation of China(52071285 and 51831009)+1 种基金the Fundamental Research Funds for the Central Universities(2021FZZX001-09)the National Youth Top-Notch Talent Support Program.Z.H.acknowledges support under the Australian Research Council's Future Fellowship(FT190100658).
文摘The development of high-performance binders is a simple but effective approach to address the rapid capacity decay of high-capacity anodes caused by large volume change upon lithiation/delithiation.Herein,we demonstrate a unique organic/inorganic hybrid binder system that enables an efficient in situ crosslinking of aqueous binders(e.g.,sodium alginate(SA)and carboxymethyl cellulose(CMC))by reacting with an inorganic crosslinker(sodium metaborate hydrate(SMH))upon vacuum drying.The resultant 3D interconnected networks endow the binders with strong adhesion and outstanding self-healing capability,which effectively improve the electrode integrity by preventing fracturing and exfoliation during cycling and facilitate Li^(+)ion transfer.SiO anodes fabricated from the commercial microsized powders with the SA/0.2SMH binder maintain 1470 mAh g^(-1)of specific capacity at 100 mA g^(-1)after 200 cycles,which is 5 times higher than that fabricated with SA binder alone(293 mAh g^(-1)).Nearly,no capacity loss was observed over 500 cycles when limiting discharge capacity at 1500 mAh g^(-1).The new binders also dramatically improved the performance of Fe_(2)O_(3),Fe_(3)O_(4),NiO,and Si electrodes,indicating the excellent applicability.This finding represents a novel strategy in developing high-performance aqueous binders and improves the prospect of using high-capacity anode materials in Li-ion batteries.
基金supported by the National Natural Science Foundation of China(No.52071171)Liaoning Revitalization Talents Program-Pan Deng Scholars(XLYC1802005)+5 种基金Liaoning BaiQianWan Talents Program(LNBQW2018B0048)Natural Science Fund of Liaoning Province for Excellent Young Scholars(2019-YQ-04)Key Project of Scientific Research of the Education Department of Liaoning Province(LZD201902)Foundation for Young Scholars of Liaoning University(a252102001)Australian Research Council(ARC)Future Fellowship(FT210100298)CSIRO Energy Centre,Kick-Start Project and the Victorian Government’s support through the provision of a grant from veski-Study Melbourne Research Partnerships(SMRP)project.
文摘The rapid advance of mild aqueous zinc-ion batteries(ZIBs)is driving the development of the energy storage system market.But the thorny issues of Zn anodes,mainly including dendrite growth,hydrogen evolution,and corrosion,severely reduce the performance of ZIBs.To commercialize ZIBs,researchers must overcome formidable challenges.Research about mild aqueous ZIBs is still developing.Various technical and scientific obstacles to designing Zn anodes with high stripping efficiency and long cycling life have not been resolved.Moreover,the performance of Zn anodes is a complex scientific issue determined by various parameters,most of which are often ignored,failing to achieve the maximum performance of the cell.This review proposes a comprehensive overview of existing Zn anode issues and the corresponding strategies,frontiers,and development trends to deeply comprehend the essence and inner connection of degradation mechanism and performance.First,the formation mechanism of dendrite growth,hydrogen evolution,corrosion,and their influence on the anode are analyzed.Furthermore,various strategies for constructing stable Zn anodes are summarized and discussed in detail from multiple perspectives.These strategies are mainly divided into interface modification,structural anode,alloying anode,intercalation anode,liquid electrolyte,non-liquid electrolyte,separator design,and other strategies.Finally,research directions and prospects are put forward for Zn anodes.This contribution highlights the latest developments and provides new insights into the advanced Zn anode for future research.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.51871060,52071084 and 51831009)Recruit Program of Global Youth Experts and Fudan’s Undergraduate Research Opportunities Program(FDUROP)。
文摘The practical application of lithium-sulfur batteries is severely hampered by the poor conductivity,polysulfide shuttle effect and sluggish reaction kinetics of sulfur cathodes.Herein,a hierarchi-cally porous three-dimension(3D)carbon architecture assembled by cross-linked carbon leaves with implanted atomic Co-N4 has been deli-cately developed as an advanced sulfur host through a SiO_(2)-mediated zeolitic imidazolate framework-L(ZIF-L)strategy.The unique 3D architectures not only provide a highly conductive network for fast electron transfer and buffer the volume change upon lithiation-delithi-ation process but also endow rich interface with full exposure of Co-N4 active sites to boost the lithium polysulfides adsorption and conversion.Owing to the accelerated kinetics and suppressed shuttle effect,the as-prepared sulfur cathode exhibits a superior electrochemical perfor-mance with a high reversible specific capacity of 695 mAh g^(−1) at 5 C and a low capacity fading rate of 0.053%per cycle over 500 cycles at 1 C.This work may provide a promising solution for the design of an advanced sulfur-based cathode toward high-performance Li-S batteries.
基金supported by“Shuguang Program”supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission Shaanxi Outstanding Youth Fund(2020JC-49)Youth Innovation Team of University in Shaanxi Province(20SG03)+2 种基金State Key Laboratory of New Textile Materials and Advanced Processing Technologies(No.FZ2021001)Guangdong Basic and Applied Basic Research Foundation(2021A1515110496)the Natural Science Basic Research Plan in Shaanxi Province of China(No.2022JQ-438).
文摘Exploring highly active but inexpensive electrocatalysts for the hydrogen evolution reaction(HER)is of critical importance for hydrogen production from electrochemical water splitting.Herein,we report a multicomponent catalyst with exceptional activity and durability for HER,in which cobalt nanoparticles were in-situ confined inside bamboo-like carbon nanotubes(CNTs)while ultralow ruthenium loading(~2.6μg per electrode area~cm^(−2))is uniformly deposited on their exterior walls(Co@CNTsǀRu).The atomic-scale structural investigations and theoretical calculations indicate that the confined inner Co and loaded outer Ru would induce charge redistribution and a synergistic electron coupling,not only optimizing the adsorption energy of H intermediates(ΔGH*)but also facilitating the electron/mass transfer.The as-developed Co@CNTsǀRu composite catalyst requires overpotentials of only 10,32,and 63 mV to afford a current density of 10 mA cm^(−2) in alkaline,acidic and neutral media,respectively,representing top-level catalytic activity among all reported HER catalysts.The current work may open a new insight into the rational design of carbon-supported metal catalysts for practical applications.
基金supported by the National Key Research and Development Program of the Ministry of Science and Technology of PR China (No. 2018YFB1502103)National Natural Science Foundation of PR China (Nos. 52071287, 51571175, U1601212, 51831009)。
文摘Magnesium hydride(MgH2) is one of the most promising hydrogen storage materials for practical application due to its favorable reversibility, low cost and environmental benign;however, it suffers from high dehydrogenation temperature and slow sorption kinetics.Exploring proper catalysts with high and sustainable activity is extremely desired for substantially improving the hydrogen storage properties of MgH2. In this work, a composite catalyst with high-loading of ultrafine Ni nanoparticles(NPs) uniformly dispersed on porous hollow carbon nanospheres is developed, which shows superior catalytic activity towards the de-/hydrogenation of MgH2. With an addition of 5wt% of the composite, which contains 90 wt% Ni NPs, the onset and peak dehydrogenation temperatures of MgH2are lowered to 190 and 242 ℃, respectively. 6.2 wt% H2is rapidly released within 30 min at 250 ℃. The amount of H2that the dehydrogenation product can absorb at a low temperature of 150 ℃ in only 250 s is very close to the initial dehydrogenation value. A dehydrogenation capacity of 6.4wt% remains after 50 cycles at a moderate cyclic regime, corresponding to a capacity retention of 94.1%. The Ni NPs are highly active,reacting with MgH2and forming nanosized Mg2Ni/Mg2NiH4. They act as catalysts during hydrogen sorption cycling, and maintain a high dispersibility with the help of the dispersive role of the carbon substrate, leading to sustainably catalytic activity. The present work provides new insight into designing stable and highly active catalysts for promoting the(de)hydrogenation kinetics of MgH2.
基金supported by National Key Research and Development Program (2019YFE0111200)the National Natural Science Foundation of China (51722105)+1 种基金Zhejiang Provincial Natural Science Foundation of China (LR18B030001)the Fundamental Research Funds for the Central Universities and the Fundamental Research Funds for the Central Universities。
文摘Magnesium metal anode holds great potentials toward future high energy and safe rechargeable magnesium battery technology due to its divalent redox and dendrite-free nature. Electrolytes based on Lewis acid chemistry enable the reversible Mg plating/stripping,while they fail to match most cathode materials toward highvoltage magnesium batteries. Herein,reversible Mg plating/stripping is achieved in conventional carbonate electrolytes enabled by the cooperative solvation/surface engineering. Strongly electronegative Cl from the MgCl_(2) additive of electrolyte impairs the Mg…O = C interaction to reduce the Mg^(2+) desolvation barrier for accelerated redox kinetics,while the Mg^(2+)-conducting polymer coating on the Mg surface ensures the facile Mg^(2+) migration and the e ective isolation of electrolytes. As a result,reversible plating and stripping of Mg is demonstrated with a low overpotential of 0.7 V up to 2000 cycles. Moreover,benefitting from the wide electrochemical window of carbonate electrolytes,high-voltage(> 2.0 V) rechargeable magnesium batteries are achieved through assembling the electrode couple of Mg metal anode and Prussian blue-based cathodes. The present work provides a cooperative engineering strategy to promote the application of magnesium anode in carbonate electrolytes toward high energy rechargeable batteries.
基金supported by the National Natural Science Foundation(Grant number 51501175 and 51671172)the Zhejiang Provincial Natural Science Foundation of China(Grant number LQ16E010001 and LR16E010002)the Hubei Provincial Natural Science Foundation of China(Grant number 2015CFB498)
文摘The ternary amides LiK2(NH2)3, LiK(NH2)2, and Li3 K(NH2)4 are successfully synthesized by ball milling mixtures of LiNH2 and KNH2, and the hydrogen storage properties of Li3K(NH2)4–xMgH2(x = 1, 2, 3,4) are systematically investigated. The Li3K(NH2)4–2 Mg H2 sample displays optimized hydrogen storage properties, releasing 6.37 wt% of hydrogen in a two-stage reaction with an onset temperature of 60 °C.The first dehydrogenation stage exhibits good reaction kinetics and thermodynamic properties because of a lower activation energy and appropriate enthalpy change. After full dehydrogenation at 130 °C, the Li3K(NH2)4–2 MgH2 sample absorbs 3.80 wt% of H2 below 160 °C in a variable temperature hydrogenation mode. Mechanistic investigations indicate that Li3 K(NH2)4 reacts with Mg H2 to produce Mg(NH2)2, LiH,and KH during ball milling. In the heating process, Mg(NH2)2 first reacts with Li H to form Li2 Mg2 N3 H3 and Li NH2, while KH works as a catalyst, and then, KH reacts with Li2Mg2N3H3 and Li NH2 to generate a new K-containing compound.
文摘Superior catalyst supports are crucial to developing advanced electrocatalysts toward heterogeneous catalytic reactions.Herein,we systematically investigate the role of transition metal‐functionalized N‐doped carbon nanosheets(M‐N‐C,M=Mn,Fe,Co,Ni,Cu,Mo,and Ag)as the multifunctional electrocatalyst supports toward hydrogen evolution/oxidation reactions(HER/HOR)in alkaline media.The results demonstrate that all the M‐N‐C nanosheets,except Cu‐N‐C and Ag‐N‐C,can promote the alkaline HER/HOR electrocatalytic activity of Pt by accelerating the sluggish Volmer step,among which Mn plays a more significant role.Analyses reveal that the promotion effect of M‐N‐C support is closely associated with the electronegativity of the metal dopants and the relative filling degree of their d‐orbitals.For one,the metal dopant in M‐N‐C with smaller electronegativity would provide more electrons to oxygen and hence tune the electronic structure of Pt via the M‐O‐Pt bonds at the interface.For another,the transition metal in M‐N4 moieties with more empty d orbitals would hybridize with O 2p orbitals more strongly that promotes the adsorption of water/hydroxyl species.The results demonstrate the conceptual significance of multifunctional supports and would inspire the future development of advanced electrocatalysts.
基金supported by the National Natural Science Foundation of China(Nos.52071171,22109060)the Liaoning Revitalization Talents Program-Pan Deng Scholars(XLYC1802005)+5 种基金the Liaoning Bai Qian Wan Talents Program(LNBQW2018B0048)the Natural Science Fund of Liaoning Province for Excellent Young Scholars(2019-YQ-04)the Key Project of Scientific Research of the Education Department of Liaoning Province(LZD201902)the Research Fund for the Doctoral Program of Liaoning Province(2020-BS-085)the Australian Research Council(ARC)Future Fellowship(FT210100298)the CSIRO Energy Centre。
文摘In recent years,a series of aqueous metal ion batteries(AMIBs)has been developed to improve the safety and cost-efficiency of portable electronics and electric vehicles.However,the significant gaps in energy density,power density,and cycle stability of AMIBs directly hinder them from replacing the currently widely used non-aqueous metal ion batteries,which stems from the lack of reasonable configuration and performance optimization of electrode materials.First-row transition metal compounds(FRTMCs),with the advantages of optional voltage ranges(from low to high),adjustable crystal structures(layered and tunnel types with large spacing),and designable morphology(multi-dimensional nanostructures),are widely used to construct high-performance AMIBs.However,no comprehensive review papers were generated to highlight their specific and significant roles in AMIBs.In this review,we first summarize the superiority and characteristics of FRTMCs in AMIBs.Then,we put forward control strategies of FRTMCs from subsurface engineering to inner construction to promote capacitance control and diffusion control energy storage.After that,the electrochemical performance of the FRTMCs regulation strategies in AMIBs is reviewed.Finally,we present potential directions and challenges for further enhancements of FRTMCs in AMIBs.The review aims to provide an in-depth understanding of regulation strategies for enhancing energy storage to build high-performance AMIBs that meet practical applications.
基金Zhejiang Provincial Natural Science Foundation of China(LZ23B030003)the National Key R&D Program(2022YFB2502000)+1 种基金the National Key R&D Program(2022YFB2502000)the Fundamental Research Funds for the Central Universities(2021FZZX001-09)。
文摘Solid-state sodium metal batteries utilizing inorganic solid electrolytes(SEs)hold immense potentials such as intrinsical safety,high energy density,and environmental sustainability.However,the interfacial inhomogeneity/instability at the anode-SE interface usually triggers the penetration of sodium dendrites into the electrolyte,leading to short circuit and battery failure.Herein,confronting with the original nonuniform and high-resistance solid electrolyte interphase(SEI)at the Na-Na_(3)Zr_(2)Si_(2)PO_(12)interface,an oxygen-regulated SEI innovative approach is proposed to enhance the cycling stability of anode-SEs interface,through a spontaneous reaction between the metallic sodium(containing trace amounts of oxygen)and the Na_(3)Zr_(2)Si_(2)POi_(2)SE.The oxygen-regulated spontaneous SEI is thin,uniform,and kinetically stable to facilitate homogenous interfacial Na^+transportation,Benefitting from the optimized SEI,the assembled symmetric cell exhibits an ultra-stable sodium plating/stripping cycle for over 6600 h under a practical capacity of 3 mAh cm^(-2).Qua si-sol id-state batteries with Na_(3)V_(2)(PO_(4))_(3)cathode deliver excellent cyclability over 500 cycles at a rate of 0.5 C(1 C=117 mA cm^(-2))with a high capacity retention of95.4%.This oxygen-regulated SEI strategy may offer a potential avenue for the future development of high-energy-density solid-state metal batteries.
基金financially supported by the National Natural Science Foundation of China(Nos.52171224 and 92261119)J.M.W.acknowledges support from Zhejiang Province Postdoctoral Science Foundation(No.ZJ2022003)China Postdoctoral Science Foundation(No.2023M733020).
文摘The sluggish reaction kinetics of alkaline hydrogen oxidation reaction(HOR)is one of the key challenges for anion exchange membrane fuel cells(AEMFCs).To achieve robust alkaline HOR with minimized cost,we developed a single atom-cluster multiscale structure with isolated Pt single atoms anchored on Ru nanoclusters supported on nitrogen-doped carbon nanosheets(Pt1-Ru/NC).The well-defined structure not only provides multiple sites with varied affinity with the intermediates but also enables simultaneous modulation of different sites via interfacial interaction.In addition to weakening Ru–H bond strength,the isolated Pt sites are heavily involved in hydrogen adsorption and synergistically accelerate the Volmer step with the help of Ru sites.Furthermore,this catalyst configuration inhibits the excessive occupancy of oxygen-containing species on Ru sites and facilitates the HOR at elevated potentials.The Pt1-Ru/NC catalyst exhibits superior alkaline HOR performance with extremely high activity and excellent CO-tolerance.An AEMFC with a 0.1 mg·cmPGM^(−2)loading of Pt1-Ru/NC anode catalyst achieves a peak powder density of 1172 mW·cm^(−2),which is 2.17 and 1.55 times higher than that of Pt/C and PtRu/C,respectively.This work provides a new catalyst concept to address the sluggish kinetics of electrocatalytic reactions containing multiple intermediates and elemental steps.
基金This work was financially supported by the National Natural Science Foundation of China(Grant No.52201277).
文摘Solid-state batteries(SSBs)have received widespread attention with their high safety and high energy density characteristics.However,solid-solid contacts in the internal electrode material and the electrode material/solid electrolyte(SE)interfaces,as well as the severe electrochemo-mechanical effects caused by the internal stress due to the volume change of the active material,these problems hinder ion/electron transport within the SSBs,which significantly deteriorates the electrochemical performance.Applying fabrication pressures and stack pressures are effective measures to improve solid-solid contact and solve electrochemo-mechanical problems.Herein,the influences of different pressures on cathode material,anode material,SEs,and electrode/SEs interface are briefly summarized from the perspective of interface ion diffusion,transmission of electrons and ions in internal particles,current density and ion diffusion kinetics,and the volume changes of Li^(+)stripping/plating based on two physical contact models,and point out the direction for the future research direction of SSBs and advancing industrialization by building the relationship between pressures and SSBs electrochemistry.
基金National Natural Science Foundation of China,Grant/Award Number:22325101。
文摘Single-atom materials(SAMs)have become one of the most important power sources to push the field of energy conversion forward.Among the main types of energy,including thermal energy,electrical energy,solar energy,and biomass energy,SAMs have realized ultra-high efficiency and show an appealing future in practical application.More than high activity,the uniform active sites also provide a convincible model for chemists to design and comprehend the mechanism behind the phenomenon.Therefore,we presented an insightful review of the application of the single-atom material in the field of energy conversion.The challenges(e.g.,accurate synthesis and practical application)and future directions(e.g.,machine learning and efficient design)of the applications of SAMs in energy conversion are included,aiming to provide guidance for the research in the next step.
基金supported by the National Out-standing Youth Foundation of China (No.52125104)the Natural Science Foundation of Zhejiang Province (No.LD21E010002)+2 种基金the National Natural Science Foundation of China (No.52001277)the Fundamental Research Funds for the Central Universities (No.2021FZZX001-09)the National Youth Top-Notch Talent Support Program.
文摘Nanoscaled catalysts have attracted much more attention due to their more abundant active sites and better dispersion than their bulky counterparts.In this work,VH_(x) nanoparticles smaller than 10 nm in average size are successfully synthesized by a simple solid-state ball milling coupled with THF washing process,which are proved to be highly effective in enhancing the hydrogen absorption/desorption kinetics of MgH_(2) at moderate temperatures.The nano-VH_(x)-modified MgH_(2) releases hydrogen from 182℃,which is 88℃ lower than additive-free MgH_(2).The release of hydrogen amounts to 6.3 wt%H within 10 min at 230℃ and 5.6 wt%H after 30 min at 215℃ with initial vacuum.More importantly,the dehydro-genated MgH_(2)+10 wt.%nano-VH_(x) rapidly absorbs 5.2 wt%H within 3 min at 50℃ under 50 bar H_(2).It even takes up 4.3 wt%H within 30 min at room temperature(25℃)under 10 bar H_(2),exhibiting supe-rior hydrogenation kinetics to most of the previous reports.Mechanistic analyzes disclose the reversible transformation between V and V-H species during the hydrogen desorption-absorption process.The ho-mogeneously distributed V-based species is believed to act as hydrogen pump and nucleation sites for MgH_(2) and Mg,respectively,thus triggering fast hydrogenation/dehydrogenation kinetics.
基金supported by the Natural Science Foundation of Zhejiang Province(No.LZ22B030006)the National Natural Science Foundation of China(No.52171224)+2 种基金G.Q.Z.acknowledges the financial support from the China Postdoctoral Science Foundation(Nos.2021M690132 and 2021T140588)the Office of China Postdoc Council(No.YJ20200160)Natural Science Foundation of Zhejiang Province(No.LQ22B030005).
文摘Proton exchange membrane water electrolyzer(PEMWE)driven by renewable electricity is a promising technique toward green hydrogen production,but the corrosive environment and high working potential pose severe challenges for developing advanced electrocatalysts for the oxygen evolution reaction(OER).Although Ir-based materials possess relatively balanced activity and stability for the OER,their dissolution behavior cannot be neglected,in particular under high working potentials.In this work,iridium dioxide(IrO_(2))nanoparticles(NPs)were anchored on the surface of exfoliated h-boron nitride(BN)nanosheets(NSs)toward the OER reaction in acid media.Highly active Ir(V)species were stabilized by the epitaxial interface between IrO_(2)and h-BN,and therefore the IrO_(2)/BN delivered stable performance at increased working potentials,while the activity of bare IrO_(2)NPs without h-BN support decreased rapidly.Also,the smaller lattice spacing of h-BN induced compressive strain for IrO_(2),resulting in improved activity.Our results demonstrate the feasibility of stabilizing highly active Ir(V)species for the OER in acid media by constructing robust interface and provide new possibilities toward designing advanced heterostructured electrocatalysts.
基金the financial support received from the National Key R&D Program of China(No.2022YFB3803700)the National Outstanding Youth Foundation of China(No.52125104)+3 种基金the Natural Science Foundation of Zhejiang Province(No.LD21E010002)the National Natural Science Foundation of China(Nos.52001277 and U22A20120)the Fundamental Research Funds for the Central Universities(Nos.2021FZZX001-09 and 226-2022-00246)the National Youth Top-Notch Talent Support Program.
文摘The storage of hydrogen in a compact,safe and cost-effective manner can be one of the key enabling technologies to power a more sustainable society.Magnesium hydride(MgH_(2))has attracted strong research interest as a hydrogen carrier because of its high gravimetric and volumetric hydrogen densities.However,the practical use of MgH_(2)for hydrogen storage has been limited due to high operation temperatures and sluggish kinetics.Catalysis is of crucial importance for the enhancement of hydrogen cycling kinetics of Mg/MgH_(2)and considerable work has been focused on designing,fabricating and optimizing catalysts.This review covers the recent advances in catalyzed Mg-based hydrogen storage materials.The fundamental properties and the syntheses of MgH_(2)as a hydrogen carrier are first briefly reviewed.After that,the general catalysis mechanisms and the catalysts developed for hydrogen storage in MgH_(2)are summarized in detail.Finally,the challenges and future research focus are discussed.Literature studies indicate that transition metals,rare-earth metals and their compounds are quite effective in catalyzing hydrogen storage in Mg/MgH_(2).Most metal-containing compounds were converted in situ to elemental metal or their magnesium alloys,and their particle sizes and dispersion affect their catalytic activity.The in-situ construction of catalyzed ultrasmall Mg/MgH_(2)nanostructures(<10 nm in size)is believed to be the future research focus.These important insights will help with the design and development of high-performance catalysts for hydrogen storage in Mg/MgH_(2).