查看更多>>摘要：Considerable research efforts have been dedicated to investigating the side reactions and the growth of Zn dendritic in aqueous zinc-ion batteries(AZIBs).The incorporation of organic solvents as additives in electrolytes has yielded highly promising results.Nevertheless,their pervasive use has been hindered by concerns regarding their toxicity,flammability,and economic viability.Herein,we propose the utiliza-tion of γ-valerolactone(γ-V),a novel eco-friendly solvent,as an alternative for conventional organic additives to improve the performance of Zn anode.Experimental investigations and theoretical analyses have verified that γ-V additives can diminish the Zn2+-desolvation energy and enhance Zn2+transport kinetics.The adsorbed y-V molecules modulate the nucleation and diffusion of Zn2+,facilitating Zn growth along the(002)crystal plane,thus inhibiting dendrite formation and side reactions.Consequently,the modified electrolyte with 3％γ-V exhibit highly reversible cycling for 2800 h at 1 mA cm-2 and 1 mA h cm-2 in Zn//Zn symmetric cell.The Zn//KVOH coin cells deliver a capacity reten-tion of 74.7％after 1000 cycles at 5 A g-1.The Zn//KVOH pouch cells maintain a capacity retention of 78.7％over 90 cycles at 3 A g-1.Notably,the γ-V additives also effectively alleviate the self-discharge phe-nomenon.This work provides valuable insights on the development of aqueous zinc-ion batteries with superior safety through the modulation of electrolytes using eco-friendly additives.
查看更多>>摘要：The application of Li-rich Mn-based cathodes,the most promising candidates for high-energy-density Li-ion batteries,in all-solid-state batteries can further enhance the safety and stability of battery systems.However,the utilization of high-capacity Li-rich cathodes has been limited by sluggish kinetics and sev-ere interfacial issues in all-solid-state batteries.Here,a multi-functional interface modification strategy involving dispersed submicron single-crystal structure and multi-functional surface modification layer obtained through in-situ interfacial chemical reactions was designed to improve the electrochemical per-formance of Li-rich Mn-based cathodes in all-solid-state batteries.The design of submicron single-crystal structure promotes the interface contact between the cathode particles and the solid-state electrolyte,and thus constructs a more complete ion and electron conductive network in the composite cathode.Furthermore,the Li-gradient layer and the lithium molybdate coating layer constructed on the surface of single-crystal Li-rich particles accelerate the transport of Li ions at the interface,suppress the side reac-tions between cathodes and electrolyte,and inhibit the oxygen release on the cathode surface.The opti-mized Li-rich cathode materials exhibit excellent electrochemical performance in halide all-solid-state batteries.This study emphasizes the vital importance of reaction kinetics and interfacial stability of Li-rich cathodes in all-solid-state batteries and provides a facile modification strategy to enhance the elec-trochemical performance of all-solid-state batteries based on Li-rich cathodes.
查看更多>>摘要：The extreme volume expansion of the silicon(Si)anodes during repeated cycles seriously induces unde-sirable interfacial side reactions,forming an unstable solid electrolyte interphase(SEI)that degrades the electrode integrity and cycle stability in lithium-ion batteries,limiting their practical applications.Despite considerable efforts to stabilize the SEI through surface modification,challenges persist in the development of high-performance Si anodes that effectively regulate intrinsic SEI properties and simul-taneously facilitate electron/ion transport.Here,a highly conductive and organic electrolyte-compatible lamellar p-toluenesulfonic acid-doped polyaniline(pTAP)layer is proposed for constructing a robust arti-ficial SEI on Si nanoparticles to achieve fast charging,long-term cycle lifespan and high areal capacity.The spatially uniform pTAP layer,formed through a facile direct-encapsulation approach assisted by enriched hydrogen bonding,contributes to the effective formation of in situ SEI with an even distribution of the LiF-rich phase in its interlamination spaces.Furthermore,the integrated artificial SEI facilitates isotropic ion/electron transport,increased robustness,and effectively dissipates stress from volume changes.Consequently,a notably high rate performance of 570 mA h g-1,even at a substantially high current den-sity of 10 A g-1,is achieved with excellent cyclic stability by showing a superior capacity over 1430 mA h g-1 at 1 A g-1 after 250 cycles and a high areal capacity of ca.2 mA h cm-2 at 0.5 C in a full cell system.This study demonstrates that the rational design of conductive polymers with SEI modulation for surface protection has great potential for use in high-energy-density Si anodes.
查看更多>>摘要：We report here the in situ electrochemical scanning tunneling microscopy(ECSTM)study of cobalt phthalocyanine(CoPc)-catalyzed O2 evolution reaction(OER)and the dynamics of CoPc-O2 dissociation.The self-assembled CoPc monolayer is fabricated on Au(111)substrate and resolved by ECSTM in 0.1 M KOH electrolyte.The OH-adsorption on CoPc prior to OER is observed in ECSTM images.During OER,the generated O2 adsorbed on CoPc is observed in the CoPc monolayer.Potential step experiment is employed to monitor the desorption of OER-generated O2 from CoPc,which results in the decreasing surface cov-erage of CoPc-O2 with time.The rate constant of O2 desorption is evaluated through data fitting.The insights into the dynamics of Co-O2 dissociation at the molecular level via in situ imaging help under-stand the role of Co-O2 in oxygen reduction reaction(ORR)and OER.
An ChenZhilong WangKarl Luigi Loza VidaurreYanqiang Han...
149-168页
查看更多>>摘要：Leveraging big data analytics and advanced algorithms to accelerate and optimize the process of molec-ular and materials design,synthesis,and application has revolutionized the field of molecular and mate-rials science,allowing researchers to gain a deeper understanding of material properties and behaviors,leading to the development of new materials that are more efficient and reliable.However,the difficulty in constructing large-scale datasets of new molecules/materials due to the high cost of data acquisition and annotation limits the development of conventional machine learning(ML)approaches.Knowledge-reused transfer learning(TL)methods are expected to break this dilemma.The application of TL lowers the data requirements for model training,which makes TL stand out in researches addressing data quality issues.In this review,we summarize recent progress in TL related to molecular and materials.We focus on the application of TL methods for the discovery of advanced molecules/materials,particularly,the con-struction of TL frameworks for different systems,and how TL can enhance the performance of models.In addition,the challenges of TL are also discussed.
查看更多>>摘要：The development of electrocatalysts for the oxygen reduction reaction(ORR)that bears high selectivity,exceptional activity,and long-term stability is crucial for advancing various green energy technologies.Intermetallics composed of platinum and transition metals are considered to be promising candidates for this purpose.However,they typically face challenges such as unfavorable intrinsic activity and a propensity for particle aggregation,diminishing their ORR performance.Against this backdrop,we pre-sent our findings on a N-doped carbon confined Pt3Co intermetallic doped with p-block metal tin(Pt3CoxSn1-x/NC).The introduction of Sn induces lattice strain due to its larger atomic size,which leads to the distortion of the Pt3Co lattice structure,while the coupling of carbon polyhedra inhibits the particle aggregation.The optimized Pt3Co0.8Sn0.2/NC catalyst demonstrates an impressive half-wave potential of 0.86 V versus RHE,surpassing both Pt3Co/NC and Pt3Sn/NC catalysts.Moreover,the Pt3Co0.8Sn0.2/NC exhi-bits a mass-specific activity as high as 1.4 A mgpt1,ranking it in the top level among the intermetallics-based ORR electrocatalysts.When further employed as a cathode material in a self-assembled zinc-air battery,it shows stable operation for over 80 h.These results underscore the significant impact of lattice strain engineering through the strategic doping of p-block metal in the carbon-confined Pt3Co intermetal-lic,thereby enhancing the catalytic efficiency for the ORR.
查看更多>>摘要：Unsatisfactory conductivity and volume effects have hindered the commercial application of silicon-based materials as advanced anode materials for high-performance lithium-ion batteries.Herein,nitro-gen doped carbon silicon matrix composite with atomically dispersed Co sites(Si/Co-N-C)is obtained via the design of the frame structure loaded with nano-components and the multi-element hybrid strat-egy.Co atoms are uniformly fixed to the N-C frame and tightly packed with nanoscale silicon particles as an activation and protection building block.The mechanism of the N-C framework of loaded metal Co in the Si alloying process is revealed by electrochemical kinetic analysis and ex situ characterization tests.Impressively,the nitrogen-doped Co site activates the intercalation of the outer carbon matrix to supple-ment the additional capacity.The Co nanoparticles with high conductivity and support enhance the con-ductivity and structural stability of the composite,accelerating the Li+/Na+diffusion kinetics.Density functional theory(DFT)calculation confirms that the hetero-structure Si/Co-N-C adjusts the electronic structure to obtain good lithium-ion adsorption energy,reduces the Li+/Na+migration energy barrier.This work provides meaningful guidance for the development of high-performance metal/non-metal modified anode materials.
查看更多>>摘要：Single atom catalysts(SACs)possessing regulated electronic structure,high atom utilization,and superior catalytic efficiency have been studied in almost all fields in recent years.Carbon-based supporting SACs are becoming popular materials because of their low cost,high electron conductivity,and controllable surface property.At the stage of catalysts preparation,the rational design of active sites is necessary for the substantial improvement of activity of catalysts.To date,the reported design strategies are mainly about synthesis mechanism and synthetic method.The level of understanding of design strategies of carbon-based single atom catalysts is requiring deep to be paved.The design strategies about manufac-turing defects and coordination modulation of catalysts are presented.The design strategies are easy to carry out in the process of drawing up preparation routes.The components of carbon-based SACs can be divided into two parts:active site and carbon skeleton.In this review,the manufacture of defects and coordination modulation of two parts are introduced,respectively.The structure features and design strategies from the active sites and carbon skeletons to the overall catalysts are deeply discussed.Then,the structural design of different nano-carbon SACs is introduced systematically.The characteriza-tion of active site and carbon skeleton and the detailed mechanism of reaction process are summarized and analyzed.Next,the applications in the field of electrocatalysis for oxygen conversion and hydrogen conversion are illustrated.The relationships between the superior performance and the structure of active sites or carbon skeletons are discussed.Finally,the conclusion of this review and prospects on the abundant space for further promotion in broader fields are depicted.This review highlights the design and preparation thoughts from the parts to the whole.The detailed and systematic discussion will pro-vide useful guidance for design of SACs for readers.
查看更多>>摘要：Aqueous proton batteries(APBs)offer a viable and attractive option in the field of affordable and sustain-able energy solutions.Organic polymers are highly favored due to their environmentally friendly manu-facturability and malleable molecular configurations,making them suitable materials for constructing APB electrodes.Nonetheless,their currently limited capacity for proton-associated redox reactions poses a challenge to the widespread usage.Herein,we have developed a highly redox-active organic polymer(PTA)tailored for APB applications.The inclusion of dual redox-active moieties in the extended π-conjugated frameworks not only enhances the redox activity and refines the electronic properties,but also ensures the high structural integrity of the PTA polymer.When used as an electrode,the PTA poly-mer has a notable ability to store protons,with a large capacity of 213.99 mA h g-1 at 1 A g-1 and excep-tional long-term stability,as evidenced by retaining 94.6％of its initial capacity after 20,000 cycles.In situ techniques alongside theoretical calculations have unveiled efficient redox processes occurring at C=N and C=O redox-active sites within the PTA electrode upon proton uptake/removal.Furthermore,a soft-package APB device has been assembled with impressive electrochemical behaviors and excellent oper-ational lifespan,accentuating its significant promise for real-world deployment.
查看更多>>摘要：As the world transitions to green energy,there is a growing focus among many researchers on the requirement for high-efficient and safe batteries.Solid-state lithium metal batteries(SSLMBs)have emerged as a promising alternative to traditional liquid lithium-ion batteries(LIBs),offering higher energy density,enhanced safety,and longer lifespan.The rise of SSLMBs has brought about a transforma-tion in energy storage,with aluminum(Al)-based material dopants playing a crucial role in advancing the next generation of batteries.The review highlights the significance of Al-based material dopants in SSLMBs applications,particularly its contributions to solid-state electrolytes(SSEs),cathodes,anodes,and other components of SSLMBs.Some studies have also shown that Al-based material dopants effec-tively enhance SSE ion conductivity,stabilize electrode and SSE interfaces,and suppress lithium dendrite growth,thereby enhancing the electrochemical performance of SSLMBs.Despite the above mentioned progresses,there are still problems and challenges need to be addressed.The review offers a comprehen-sive insight into the important role of Al in SSLMBs and addresses some of the issues related to its appli-cations,endowing valuable support for the practical implementation of SSLMBs.
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