查看更多>>摘要：A fast-charging policy is widely employed to alleviate the inconvenience caused by the extended charging time of electric vehicles.However,fast charging exacerbates battery degradation and shortens battery lifespan.In addition,there is still a lack of tailored health estimations for fast-charging batteries;most existing methods are applicable at lower charging rates.This paper proposes a novel method for estimat-ing the health of lithium-ion batteries,which is tailored for multi-stage constant current-constant voltage fast-charging policies.Initially,short charging segments are extracted by monitoring current switches,followed by deriving voltage sequences using interpolation techniques.Subsequently,a graph generation layer is used to transform the voltage sequence into graphical data.Furthermore,the integration of a graph convolution network with a long short-term memory network enables the extraction of informa-tion related to inter-node message transmission,capturing the key local and temporal features during the battery degradation process.Finally,this method is confirmed by utilizing aging data from 185 cells and 81 distinct fast-charging policies.The 4-minute charging duration achieves a balance between high accu-racy in estimating battery state of health and low data requirements,with mean absolute errors and root mean square errors of 0.34％and 0.66％,respectively.
查看更多>>摘要：The thermodynamic instability of zinc anodes in aqueous electrolytes leads to issues such as corrosion,hydrogen evolution reactions(HER),and dendrite growth,severely hindering the practical application of zinc-based aqueous energy storage devices.To address these challenges,this work proposes a dual-function zinc anode protective layer,composed of Zn-Al-In layered double oxides(ILDO)by rationally designing Zn-Al layered double hydroxides(Zn-Al LDHs)for the first time.Differing from previous works on the LDHs coatings,firstly,the ILDO layer accelerates zinc-ion desolvation and also captures and anchors SO4-.Secondly,the in-situ formation of the Zn-In alloy phase effectively lowers the nucleation energy barrier,thereby regulating zinc nucleation.Consequently,the zinc anode with the ILDO protective layer demonstrates long-term stability exceeding 1900 h and low voltage hysteresis of 7.5 mV at 0.5 mA cm-2 and 0.5 mA h cm-2.Additionally,it significantly enhances the rate capability and cycling perfor-mance of Zn@ILDO//MnO2 full batteries and Zn@ILDO//activated carbon zinc-ion hybrid capacitors.This simple and effective dual-function protective layer strategy offers a promising approach for achiev-ing high-performance zinc-ion batteries.
查看更多>>摘要：The electrochemical oxidation of 5-hydroxymethylfurfural(HMF)represents a significant avenue for sus-tainable chemical synthesis,owing to its potential to generate high-value derivatives from biomass feed-stocks.Transition metal catalysts offer a cost-effective alternative to precious metals for catalyzing HMF oxidation,with transition bimetallic catalysts emerging as particularly promising candidates.In this review,we delve into the intricate reaction pathways and electrochemical mechanisms underlying HMF oxidation,emphasizing the pivotal role of transition bimetallic catalysts in enhancing catalytic effi-ciency.Subsequently,various types of transition bimetallic catalysts are explored,detailing their synthe-sis methods and structural modulation strategies.By elucidating the mechanisms behind catalyst modification and performance enhancement,this review sets the stage for upcoming advancements in the field,ultimately advancing the electrochemical HMF conversion and facilitating the transition towards sustainable chemical production.
查看更多>>摘要：Lead sulfide quantum dots(PbS QDs)hold unique characteristics,including bandgap tunability,solution-processability etc.,which make them highly applicable in tandem solar cells(TSCs).In all QD TSCs,its effi-ciency lags much behind to their single junction counterparts due to the deficient interconnection layer(ICL)and defective subcells.To improve TSCs performance,we developed three kinds of ICL structures based on 1.34 and 0.96 eV PbS QDs subcells.The control,1,2-ethanedithiol capped PbS QDs(PbS-EDT)/Au/tin dioxide(SnO2)/zinc oxide(ZnO),utilized SnO2 layer to obtain high surface compactness.However,its energy level mismatch causes incomplete recombination.Bypassing it,the second ICL(PbS-EDT/Au/ZnO)removed SnO2 and boosted the power conversion efficiency(PCE)from 5.75％to 8.69％.In the third ICL(PbS-EDT/poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine](PTAA)/Au/ZnO),a thin layer of PTAA can effectively fill fissures on the surface of PbS-EDT and also protect the front cells from solvent penetration.This TSC obtained a PCE of 9.49％with an open circuit voltage of 0.91 V,a short circuit current density of 15.47 mA/cm2,and a fill factor of 67.7％.To the best of our knowledge,this was the highest PCE achieved by all PbS QD TSCs reported to date.These TSCs maintained stable performance for a long working time under ambient conditions.
查看更多>>摘要：In the pursuit of ultrathin polymer electrolyte(＜20 μm)for lithium metal batteries,achieving a balance between mechanical strength and interfacial stability is crucial for the longevity of the electrolytes.Herein,11 μm-thick gel polymer electrolyte is designed via an integrated electrode/electrolyte structure supported by lithium metal anode.Benefiting from an exemplary superiority of excellent mechanical property,high ionic conductivity,and robust interfacial adhesion,the in-situ formed polymer electrolyte reinforced by titanosiloxane networks(ISPTS)embodies multifunctional roles of physical barrier,ionic carrier,and artificial protective layer at the interface.The potent interfacial interactions foster a seamless fusion of the electrode/electrolyte interfaces and enable continuous ion transport.Moreover,the built-in ISPTS electrolyte participates in the formation of gradient solid-electrolyte interphase(SEI)layer,which enhances the SEI's structural integrity against the strain induced by volume fluctuations of lithium anode.Consequently,the resultant 11 μm-thick ISPTS electrolyte enables lithium symmetric cells with cycling stability over 600 h and LiFePO4 cells with remarkable capacity retention of 96.6％after 800 cycles.This study provides a new avenue for designing ultrathin polymer electrolytes towards stable,safe,and high-energy-density lithium metal batteries.
查看更多>>摘要：Single-crystal Nickel-rich layered oxides has been recognized as one of the promising cathodes for next-generation lithium batteries on account of their high capacity,while its practical application was hin-dered by structural instability and slow Li+transfer kinetics.Herein,a surface-to-bulk engineered single-crystal LiNio.9Coo.05Mno.05O2(Ni90)cathode,which features W-doped bulk and Li2WO4 surface layer,was successfully achieved by a one-step high-valence W6+modification.The as-obtained W-modified Ni90 delivers excellent cycling stability(89.8％capacity retention after 300 cycles at 0.5 C)and rate capability.The enhanced electrochemical performance was ascribed to the doped-W induced stabilized lattice oxygen,reduced Li+/Ni2+mixing and inhibited H2-H3 phase transition in the bulk,and Li2WO4 layer generated stabilized cathode/electrolyte interface.In addition,the thinner LiF-rich cathode electrolyte interphase(CEI)on surface and smaller grain size for W-modified Ni90 benefit to its Li+diffusion dynamics.The effect of high-valence W6+on single-crystal Ni-rich cathode was firstly revealed in detail,which deepens the understanding of electrochemical behavior of Ni-rich cathode with high-valence cations modification,and provides clues for design of high-performance layered cathodes.
查看更多>>摘要：Hydrogen energy is one of the ideal energy alternatives and the upstream of the hydrogen industry chain is hydrogen production,which can be achieved via the reaction of inorganic materials with water,known as hydrolysis.Among inorganic materials,the high hydrogen capacity for hydrolysis of MgH2(15.2 wt％)makes it a promising material for hydrogen production via hydrolysis.However,the dense Mg(OH)2 passi-vation layer will block the reaction between MgH2 and the solution,resulting in low hydrogen yield and sluggish hydrolysis kinetics.In this work,the hydrogen yield and hydrogen generation rate of MgH2 are con-siderably enhanced by adding Ti-Zr-Fe-Mn-Cr-V high-entropy alloys(HEAs)for the first time.In particular,the MgH2-3 wt％TiZrFe1.5MnCrV0.5(labelled as MgH2-3 wt％Fe1.5)composite releases 1526.70 mL/g H2 within 5 min at 40 ℃,and the final hydrolysis conversion rate reaches 95.62％within 10 min.The mean hydrogen generation rate of the MgH2-3 wt％Fe1.5 composite is 289.16 mL/g/min,which is 2.38 times faster than that of pure MgH2.Meanwhile,the activation energy of the MgH2-3 wt％Fe1.5 composite is calculated to be 12.53 kJ/mol.The density functional theory(DFT)calculation reveals that the addition of HEAs weak-ens the Mg-H bonds and accelerates the electron transfer between MgH2 and HEAs.Combined with the cocktail effect of HEAs as well as the formation of more interfaces and micro protocells,the hydrolysis per-formance of MgH2 is considerably improved.This work provides an appealing prospect for real-time hydro-gen supply and offers a new effective strategy for improving the hydrolysis performance of MgH2.
查看更多>>摘要：All-solid-state lithium-sulfur batteries(ASSLSBs)have become one of the most potential candidates for the next-generation high-energy systems due to their intrinsic safety and high theoretical energy density.However,PEO-based ASSLSBs face the dilemma of insufficient Coulombic efficiency and long-term stabil-ity caused by the coupling problems of dendrite growth of anode and polysulfide shuttle of cathode.In this work,1,3,5-trioxane(TOX)is used as a functional additive to design a PEO-based composite solid-state electrolyte(denoted as TOX-CSE),which realizes the stable long-term cycle of an ASSLSB.The results show that TOX can in-situ decompose on the anode to form a composite solid electrolyte inter-phase(SEI)layer with rich-organic component.It yields a high average modulus of 5.0 GPa,greatly improving the mechanical stability of the SEI layer and thus inhibiting the growth of dendrites.Also,the robust SEI layer can act as a barrier to block the side reaction between polysulfides and lithium metal.As a result,a Li-Li symmetric cell assembled with a TOX-CSE exhibits prolonged cycling stability over 2000 h at 0.2 mA cm-2.The ASSLSB also shows a stable cycling performance of 500 cycles at 0.5 C.This work reveals the structure-activity relationship between the mechanical property of interface layer and the battery's cycling stability.
查看更多>>摘要：The electrochromic Li-ion batteries(ELIBs)combine the functions of electrochromism and energy storage,realizing the display of energy-storage levels by visual signals.However,the accompanying interfacial issues including physical contact and(electro)chemical stability should be taken into account when the conventional liquid/gel electrolytes are replaced with solid-state counterparts.Herein,the in-situ liquid-solid transitional succinonitrile(SCN)plastic glues are constructed between electrodes and poly(ethylene oxide)(PEO)polymer electrolytes,enabling an interface-reinforced solid-state ELIB.Specifically,the liquid SCN precursor can adequately wet electrode/PEO interfaces at high temperature,while it returns back to solid state at room temperature,leading to seamless interfacial contact and smooth ionic transfer without changing the solid state of the device.Moreover,the SCN interlayer sup-presses the direct contact of PEO with electrodes containing high-valence metal ions,evoking the improved interfacial stability by inhibiting the oxidation of PEO.Therefore,the resultant solid-state ELIB with configuration of LiMn2O4/SCN-PEO-SCN/WO3 delivers an initial discharge capacity of 111 mA h g-1 along with a capacity retention of 88.3％after 200 cycles at 30 ℃.Meanwhile,the elec-trochromic function is integrated into the device by distinguishing its energy-storage levels through dis-tinct color changes.This work proposes a promising solid-state ELIB with greatly reinforced interfacial compatibility by introducing in-situ solidified plastic glues.
查看更多>>摘要：Single metal atoms anchored on nitrogen-doped carbon materials(M-N4)have been identified as effec-tive active sites for catalyzing the two-electron oxygen reduction reaction(2e-ORR).However,the rela-tionship between the local atomic/electronic environments of the M-N4 sites(metal atoms coordinated with different types of N species)and their catalytic activity for 2e-ORR has rarely been elaborated clearly,which imposes significant ambiguity for the rational design of catalysts.Herein,guided by the comprehensive density-functional theory calculations and predictions,a series of Zn-N4 single-atom cat-alysts(SACs)are designed with pyrrole/pyridine-N(NPo/NPd)synergistic coordination and prepared by controlling the pyrolysis temperature(600,700,and 800 ℃).Among them,the dominated Zn-N4 config-urations with rationally combined NPo/NPd coordination show*OOH adsorption strength close to the opti-mal value,much superior to those with mono N species.Thus,the as-prepared catalyst exhibits a high H2O2 selectivity of over 90％both in neutral and alkaline environments,with a superb H2O2 yield of up to 33.63 mol g-1 h-1 in an alkaline with flow cell.More importantly,a new descriptor,dz2+s band center,has been proposed,which is especially feasible for predicting the activity for metal types with fully occu-pied s and d orbitals.This work thus presents clear guidance for the rational design of highly active SACs toward ORR and provides a complement to the d-band theory for more accurately predicting the catalytic activity of the materials.
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