查看更多>>摘要：Despite the presence of LiF components in the solid electrolyte interphase(SEI)formed on the graphite anode surface by conventional electrolyte,these LiF components primarily exist in an amorphous state,rendering them incapable of effectively inhibiting the exchange reaction between lithium ions and tran-sition metal ions in the electrolyte.Consequently,nearly all lithium ions within the SEI film are replaced by transition metal ions,resulting in an increase in interphacial impedance and a decrease in stability.Herein,we demonstrate that the SEI film,constructed by fluoroethylene carbonate(FEC)additive rich in crystalline LiF,effectively inhibits the undesired Li+/Co2+ion exchange reaction,thereby suppressing the deposition of cobalt compounds and metallic cobalt.Furthermore,the deposited cobalt compounds exhibit enhanced structural stability and reduced catalytic activity with minimal impact on the interpha-cial stability of the graphite anode.Our findings reveal the crucial influence of SEI film composition and structure on the deposition and hazards associated with transition metal ions,providing valuable guid-ance for designing next-generation electrolytes.
查看更多>>摘要：Lithium-sulfur battery(LSB)has brought much attention and concern because of high theoretical specific capacity and energy density as one of main competitors for next-generation energy storage systems.The widely commercial application and development of LSB is mainly hindered by serious"shuttle effect"of lithium polysulfides(LiPSs),slow reaction kinetics,notorious lithium dendrites,etc.In various structures of LSB materials,array structured materials,possessing the composition of ordered micro units with the same or similar characteristics of each unit,present excellent application potential for various secondary cells due to some merits such as immobilization of active substances,high specific surface area,appro-priate pore sizes,easy modification of functional material surface,accommodated huge volume change,enough facilitated transportation for electrons/lithium ions,and special functional groups strongly adsorbing LiPSs.Thus many novel array structured materials are applied to battery for tackling thorny problems mentioned above.In this review,recent progresses and developments on array structured materials applied in LSBs including preparation ways,collaborative structural designs based on array structures,and action mechanism analyses in improving electrochemical performance and safety are summarized.Meanwhile,we also have detailed discussion for array structured materials in LSBs and con-structed the structure-function relationships between array structured materials and battery perfor-mances.Lastly,some directions and prospects about preparation ways,functional modifications,and practical applications of array structured materials in LSBs are generalized.We hope the review can attract more researchers'attention and bring more studying on array structured materials for other sec-ondary batteries including LSB.
查看更多>>摘要：Rational design of efficient and robust earth-abundant alkaline hydrogen evolution reaction(HER)cata-lysts is a key factor for developing energy conversion technologies.Currently,antiperovskite nitride CuNMn3 has garnered significant interest due to its remarkable properties such as negative/zero thermal expansion and magnetocaloric effects.However,when utilized as hydrogen evolution catalysts,it encounters large challenge resulting from excessively strong/weak interactions with adsorbed H on Mn/Cu active sites,which leads to low HER activity.In this study,we introduce an asymmetric orbital hybridization strategy in Zn-doped Cu1-xZnxNMn3 by leveraging the localization of Zn electronic states to reconfigure the electronic structures of Cu and Mn,thereby reducing the energy barrier for water dis-sociation and optimizing Cu and Mn active sites for hydrogen adsorption and H2 production.Electrochemical evaluations reveal that Cu0.85Zn0.15NMn3 with x=0.15 demonstrates exceptional elec-trocatalytic activity in alkaline electrolytes.A low overpotential of 52 mV at 10 mA cm-2 and outstanding stability over a 150-h test period are achieved,surpassing commercial Pt/C.This research offers a novel strategy for enhancing HER performance by modulating asymmetric hybridization of electron orbitals between multiple metal atoms within a material structure.
查看更多>>摘要：Lithium-sulfur(Li-S)batteries are one of the most promising modern-day energy supply systems because of their high theoretical energy density and low cost.However,the development of high-energy density Li-S batteries with high loading of flammable sulfur faces the challenges of electrochemical performance degradation owing to the shuttle effect and safety issues related to fire or explosion accidents.In this work,we report a three-dimensional(3D)conductive nitrogen-doped carbon foam supported electro-static self-assembled MXene-ammonium polyphosphate(NCF-MXene-APP)layer as a heat-resistant,thermally-insulated,flame-retardant,and freestanding host for Li-S batteries with a facile and cost-effective synthesis method.Consequently,through the use of NCF-MXene-APP hosts that strongly anchor polysulfides,the Li-S batteries demonstrate outstanding electrochemical properties,including a high ini-tial discharge capacity of 1191.6 mA h g-1,excellent rate capacity of 755.0 mA h g-1 at 1 C,and long-term cycling stability with an extremely low-capacity decay rate of 0.12％per cycle at 2 C.More importantly,these batteries can continue to operate reliably under high temperature or flame attack conditions.Thus,this study provides valuable insights into the design of safe high-performance Li-S batteries.
查看更多>>摘要：Building well-developed ion-conductive highways is highly desirable for anion exchange membranes(AEMs).Grafting side chain is a highly effective approach for constructing a well-defined phase-separated morphological structure and forming unblocked ion pathways in AEMs for fast ion transport.Fluorination of side chains can further enhance phase separation due to the superhydrophobic nature of fluorine groups.However,their electronic effect on the alkaline stability of side chains and membranes is rarely reported.Here,fluorine-containing and fluorine-free side chains are introduced into the polyaro-matic backbone in proper configuration to investigate the impact of the fluorine terminal group on the stability of the side chains and membrane properties.The poly(binaphthyl-co-p-terphenyl piperidinium)AEM(QBNpTP)has the highest molecular weight and most dimensional stability due to its favorable backbone arrangement among ortho-and meta-terphenyl based AEMs.Importantly,by introducing both a fluorinated piperidinium side chain and a hexane chain into the p-terphenyl-based backbone,the pre-pared AEM(QBNpTP-QFC)presents an enhanced conductivity(150.6 mS cm1)and a constrained swel-ling at 80 ℃.The electronic effect of fluorinated side chains is contemplated by experiments and simulations.The results demonstrate that the presence of strong electro-withdrawing fluorine groups weakens the electronic cloud of adjacent C atoms,increasing OH-attack on the C atom and improving the stability of piperidinium cations.Hence QBNpTP-QFC possesses a robust alkaline stability at 80 ℃(95.3％conductivity retention after testing in 2 M NaOH for 2160 h).An excellent peak power density of 1.44 W cm-2 and a remarkable durability at 80 ℃(4.5％voltage loss after 100 h)can be observed.
查看更多>>摘要：Electrocatalytic overall water splitting(OWS),a pivotal approach in addressing the global energy crisis,aims to produce hydrogen and oxygen.However,most of the catalysts in powder form are adhesively bounding to the electrodes,resulting in catalyst detachment by bubble generation and other uncertain interference,and eventually reducing the OWS performance.To surmount this challenge,we synthesized a hybrid material of Co3S4-pyrolysis lotus fiber(labeled as Co3S4-pLF)textile by hydrothermal and high-temperature pyrolysis processes for electrocatalytic OWS.Owing to the natural LF textile exposing the uniformly distributed functional groups(-OH,-NH2,etc.)to anchor Co3S4 nanoparticles with hierarchi-cal porous structure and outstanding hydrophily,the hybrid Co3S4-pLF catalyst shows low overpotentials at 10mA cm-2(η11.HER=100 mV η10.OER=240 mV)alongside prolonged operational stability during elec-trocatalytic reactions.Theoretical calculations reveal that the electron transfer from pLF to Co3S4 in the hybrid Co3S4-pLF is beneficial to the electrocatalytic process.This work will shed light on the develop-ment of nature-inspired carbon-based materials in hybrid electrocatalysts for OWS.
查看更多>>摘要：For large-scale in-service electric vehicles(EVs)that undergo potential maintenance,second-hand trans-actions,and retirement,it is crucial to rapidly evaluate the health status of their battery packs.However,existing methods often rely on lengthy battery charging/discharging data or extensive training samples,which hinders their implementation in practical scenarios.To address this issue,a rapid health estima-tion method based on short-time charging data and limited labels for in-service battery packs is proposed in this paper.First,a digital twin of battery pack is established to emulate its dynamic behavior across various aging levels and inconsistency degrees.Then,increment capacity sequences(△Q)within a short voltage span are extracted from charging process to indicate battery health.Furthermore,data-driven models based on deep convolutional neural network(DCNN)are constructed to estimate battery state of health(SOH),where the synthetic data is employed to pre-train the models,and transfer learning strategies by using fine-tuning and domain adaptation are utilized to enhance the model adaptability.Finally,field data of 10 EVs exhibiting different SOHs are used to verify the proposed methods.By using the △Q with 100 mV voltage change,the SOH of battery packs can be accurately estimated with an error around 3.2％.
查看更多>>摘要：Exploring effective iridium(Ir)-based electrocatalysts with stable iridium centers is highly desirable for oxygen evolution reaction(OER).Herein,we regulated the incorporation manner of Ir in Co3O4 support to stabilize the Ir sites for effective OER.When anchored on the surface of Co3O4 in the form of Ir(OH)6 species,the created Ir-OH-Co interface leads to a limited stability and poor acidic OER due to Ir leaching.When doped into Co3O4 lattice,the analyses of X-ray absorption spectroscopy,in-situ Raman,and OER measurements show that the partially replacement of Co in Co3O4 by Ir atoms inclines to cause strong electronic effect and activate lattice oxygen in the presence of Ir-O-Co interface,and simultaneously mas-ter the reconstruction effect to mitigate Ir dissolution,realizing the improved OER activity and stability in alkaline and acidic environments.As a result,Irlat@Co3O4 with Ir loading of 3.67 wt％requires 294±4 mV/285±3 mV and 326±2 mV to deliver 10 mA cm-2 in alkaline(0.1 M KOH/1.0 M KOH)and acidic(0.5 M H2SO4)solution,respectively,with good stability.
查看更多>>摘要：CsPbI2Br perovskite solar cells(PSCs)have drawn tremendous attention due to their suitable bandgap,excellent photothermal stability,and great potential as an ideal candidate for top cells in tandem solar cells.However,the abundant defects at the buried interface and perovskite layer induce severe charge recombination,resulting in the open-circuit voltage(Voc)output and stability much lower than antici-pated.Herein,a novel buried interface management strategy is developed to regulate interfacial carrier dynamics and CsPbI2Br defects by introducing ammonium tetrafluoroborate(NH4BF4),thereby resulting in both high CsPbl2Br crystallization and minimized interfacial energy losses.Specifically,NH4+ions could preferentially heal hydroxyl groups on the SnO2 surface and balance energy level alignment between SnO2 and CsPbl2Br,enhancing charge transport efficiency,while BF4-anions as a quasi-halogen regulate crystal growth of CsPbI2Br,thus reducing perovskite defects.Additionally,it is proved that eliminating hydroxyl groups at the buried interface enhances the iodide migration activation energy of CsPbI2Br for strengthening the phase stability.As a result,the optimized CsPbl2Br PSCs realize a remarkable effi-ciency of 17.09％and an ultrahigh Voc output of 1.43 V,which is one of the highest values for CsPbI2Br PSCs.
查看更多>>摘要：The unabated carbon dioxide(C02)emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challenges and work toward carbon(C)neutrality and reduced CO2 emissions,the capture and uti-lization of CO2 have become imperative in both scientific research and industry.One cutting-edge approach to achieving efficient catalytic performance involves integrating green bioconversion and chem-ical conversion.This innovative strategy offers several advantages,including environmental friendliness,high efficiency,and multi-selectivity.This study provides a comprehensive review of existing technical routes for carbon sequestration(CS)and introduces two novel CS pathways:the electrochemical-biological hybrid and artificial photosynthesis systems.It also thoroughly examines the synthesis of valu-able Cn products from the two CS systems employing different catalysts and biocatalysts.As both systems heavily rely on electron transfer,direct and mediated electron transfer has been discussed and summarized in detail.Additionally,this study explores the conditions suitable for different catalysts and assesses the strengths and weaknesses of biocatalysts.We also explored the biocompatibility of the electrode materials and developed novel materials.These materials were specifically engineered to combine with enzymes or microbial cells to solve the biocompatibility problem,while improving the electron transfer efficiency of both.Furthermore,this review summarizes the relevant systems developed in recent years for manufac-turing different products,along with their respective production efficiencies,providing a solid database for development in this direction.The novel chemical-biological combination proposed herein holds great promise for the future conversion of CO2 into advanced organic compounds.Additionally,it offers exciting prospects for utilizing CO2 in synthesizing a wide range of industrial products.Ultimately,the present study provides a unique perspective for achieving the vital goals of"peak shaving"and C-neutrality,con-tributing significantly to our collective efforts to combat climate change and its associated challenges.
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