Rechargeable batteries currently hold the largest share of the electrochemical energy storage market,and they play a major role in the sustainable energy transition and industrial decarbonization to respond to global ...Rechargeable batteries currently hold the largest share of the electrochemical energy storage market,and they play a major role in the sustainable energy transition and industrial decarbonization to respond to global climate change.Due to the increased popularity of consumer electronics and electric vehicles,lithium-ion batteries have quickly become the most successful rechargeable batteries in the past three decades,yet growing demands in diversified application scenarios call for new types of rechargeable batteries.Tremendous efforts are made to developing the next-generation post-Li-ion rechargeable batteries,which include,but are not limited to solid-state batteries,lithium–sulfur batteries,sodium-/potassium-ion batteries,organic batteries,magnesium-/zinc-ion batteries,aqueous batteries and flow batteries.Despite the great achievements,challenges persist in precise understandings about the electrochemical reaction and charge transfer process,and optimal design of key materials and interfaces in a battery.This roadmap tends to provide an overview about the current research progress,key challenges and future prospects of various types of rechargeable batteries.New computational methods for materials development,and characterization techniques will also be discussed as they play an important role in battery research.展开更多
High-energy-density lithium metal batteries are the next-generation battery systems of choice,and replacing the flammable liquid electrolyte with a polymer solid-state electrolyte is a prominent conduct towards realiz...High-energy-density lithium metal batteries are the next-generation battery systems of choice,and replacing the flammable liquid electrolyte with a polymer solid-state electrolyte is a prominent conduct towards realizing the goal of high-safety and high-specific-energy devices.Unfortunately,the inherent intractable problems of poor solid-solid contacts between the electrode/electrolyte and the growth of Li dendrites hinder their practical applications.The in-situ solidification has demonstrated a variety of advantages in the application of polymer electrolytes and artificial interphase,including the design of integrated polymer electrolytes and asymmetric polymer electrolytes to enhance the compatibility of solid–solid contact and compatibility between various electrolytes,and the construction of artificial interphase between the Li anode and cathode to suppress the formation of Li dendrites and to enhance the high-voltage stability of polymer electrolytes.This review firstly elaborates the history of in-situ solidification for solid-state batteries,and then focuses on the synthetic methods of solidified electrolytes.Furthermore,the recent progress of in-situ solidification technology from both the design of polymer electrolytes and the construction of artificial interphase is summarized,and the importance of in-situ solidification technology in enhancing safety is emphasized.Finally,prospects,emerging challenges,and practical applications of in-situ solidification are envisioned.展开更多
The energy crisis and environmental pollution drive more attention to the development and utilization of renewable energy.Considering the capricious nature of renewable energy resource,it has difficulty supplying elec...The energy crisis and environmental pollution drive more attention to the development and utilization of renewable energy.Considering the capricious nature of renewable energy resource,it has difficulty supplying electricity directly to consumers stably and efficiently,which calls for energy storage systems to collect energy and release electricity at peak periods.Due to their flexible power and energy,quick response,and high energy conversion efficiency,lithium-ion batteries stand out among multiple energy storage technologies and are rapidly deployed in the grid.Pursuing superior performance and ensuring the safety of energy storage systems,intrinsically safe solid-state electrolytes are expected as an ideal alternative to liquid electrolytes.In this review,we systematically evaluate the priorities and issues of traditional lithium-ion batteries in grid energy storage.Beyond lithium-ion batteries containing liquid electrolytes,solid-state lithium-ion batteries have the potential to play a more significant role in grid energy storage.The challenges of developing solid-state lithium-ion batteries,such as low ionic conductivity of the electrolyte,unstable electrode/electrolyte interface,and complicated fabrication process,are discussed in detail.Additionally,the safety of solid-state lithium-ion batteries is re-examined.Following the obtained insights,inspiring prospects for solid-state lithium-ion batteries in grid energy storage are depicted.展开更多
Because of the low price and abundant reserves of sodium compared with lithium,the research of sodium-ion batteries(SIBs)in the field of large-scale energy storage has returned to the research spotlight.Layered oxides...Because of the low price and abundant reserves of sodium compared with lithium,the research of sodium-ion batteries(SIBs)in the field of large-scale energy storage has returned to the research spotlight.Layered oxides distinguish themselves from the mains cathode materials of SIBs owing to their advantages such as high specific capacity,simple synthesis route,and environmental benignity.However,the commercial development of the layered oxides is limited by sluggish kinetics,complex phase transition and poor air stability.Based on the research ideas from macro-to micro-scale,this review systematically summarizes the current optimization strategies of sodium-ion layered oxide cathodes(SLOC)from different dimensions:microstructure design,local chemistry regulation and structural unit construction.In the dimension of microstructure design,the various structures such as the microspheres,nanoplates,nanowires and exposed active facets are prepared to improve the slow kinetics and electrochemical performance.Besides,from the view of local chemistry regulation by chemical element substitution,the intrinsic electron/ion properties of SLOC have been enhanced to strengthen the structural stability.Furthermore,the optimization idea of endeavors to regulate the physical and chemical properties of cathode materials essentially is put forward from the dimension of structural unit construction.The opinions and strategies proposed in this review will provide some inspirations for the design of new SLOC in the future.展开更多
Lithium-sulfur(Li-S)batteries have been regarded as a promising next-generation energy storage system owing to the high theoretical energy density and natural abundance of sulfur.Abundant fundamental researches have p...Lithium-sulfur(Li-S)batteries have been regarded as a promising next-generation energy storage system owing to the high theoretical energy density and natural abundance of sulfur.Abundant fundamental researches have pushed the flourishing development on electrochemical behaviors in recent 20 years.It is time to evolve into post-Li-S battery era with the pursuit towards practical application.During the landmark leap,numerous new challenges appear under harsh conditions,such as high sulfur loading,low cathode density,lean electrolyte and limited lithium reservoir.Herein,we summarize the considerable parameters of pouch Li-S cells and review the pioneering studies focused on the cathode structure,conversion kinetics,electrode interphase and battery safety.The interwoven relationship of these key points is concluded and discussed,which provides guidance to future researches aiming to safe and long-lifespan Li-S batteries with high energy density.展开更多
Safety issues related to flammable electrolytes in lithium-ion batteries(LIBs) remain a major challenge for their extended applications.The use of non-flammable phosphate-based electrolytes has proved the validity in ...Safety issues related to flammable electrolytes in lithium-ion batteries(LIBs) remain a major challenge for their extended applications.The use of non-flammable phosphate-based electrolytes has proved the validity in inhibiting the combustion of LIBs.However,the strong interaction between Li^(+) and phosphate leads to a dominant solid electrolyte interphase(SEI) with limited electronic shielding,resulting in the poor Li^(+) intercalation at the graphite(Gr) anode when using high-phosphate-content electrolytes.To mitigate this issue and improve Li^(+) insertion,we propose an “In-N-Out” strategy to render phosphates “noncoordinative”.By employing a combination of strongly polar solvents for a “block effect” and weakly polar solvents for a “drag effect”,we reduce the Li^(+)–phosphate interaction.As a result,phosphates remain in the electrolyte phase(“In”),minimizing their impact on the incompatibility with the Gr electrode(“Out”).We have developed a non-flammable electrolyte with high triethyl phosphate(TEP) content(>60 wt.%),demonstrating the excellent ion conductivity(5.94 mS cm^(-1) at 30 ℃) and reversible Li^(+) intercalation at a standard concentration(~1 mol L^(-1)).This approach enables the manipulation of multiple electrolyte functions and holds the promise for the development of safe electrochemical energy storage systems using non-flammable electrolytes.展开更多
Lithium-ion batteries(LIBs)have become one of the most successful energy storage systems due to their high operating voltage,high energy density,and long cycle life.However,with the widespread use of LIBs in recent de...Lithium-ion batteries(LIBs)have become one of the most successful energy storage systems due to their high operating voltage,high energy density,and long cycle life.However,with the widespread use of LIBs in recent decades,lithium resources are at risk of being exhausted.Therefore,it is necessary to find a substitute for LIBs to meet the needs of future large-scale energy storage systems.Because of their competitiveness,low cost,and high safety,aqueous rechargeable zinc-ion batteries(ARZIBs)are regarded as promising components in the post-lithium-ion-battery era.Given the tunable composition,ordered porous channels,and controllable structure of metal-organic frameworks(MOFs)and covalent organic frameworks(COFs),these frameworks are viewed as potential materials for developing high-performance ARZIBs.In this review,we focus on the recent developments in the applications of MOF-/COF-based materials in ARZIBs,including in electrode materials,anode modifications,separators,and solid electrolytes.We then focus on the critical factors and optimization techniques of MOF-/COF-based materials that affect the performance of ARZIBs.Finally,we conclude with some projections for the expansion of ARZIBs containing MOF-/COF-based materials.展开更多
N-heterocyclic carbene-catalyzed enantioselective kinetic resolutions,dynamic kinetic resolutions,and desymmetrization reactions are systematically reviewed.The content is organized according to the activation modes i...N-heterocyclic carbene-catalyzed enantioselective kinetic resolutions,dynamic kinetic resolutions,and desymmetrization reactions are systematically reviewed.The content is organized according to the activation modes involved in these transformations.Future advances within this highly active research field are discussed from our perspectives on the topic.展开更多
Rechargeable aqueous metal-ion batteries(AMBs)have attracted extensive scientific and commercial interest due to their potential for cost-effective,highly safe,and scalable stationary energy storage.However,their limi...Rechargeable aqueous metal-ion batteries(AMBs)have attracted extensive scientific and commercial interest due to their potential for cost-effective,highly safe,and scalable stationary energy storage.However,their limited output voltage,inadequate energy density,and poor reversibility of ambiguous electrode reactions in aqueous electrolytes strongly limit their practical viability.This review aims to elucidate the challenges of existing AMBs from the material design to whole device applications.We summarize the emerging electrochemistry,fundamental properties,and key issues in interfacial behaviors of various classes of prevailing AMBs,including aqueous alkali metal-ion batteries and multivalent-ion batteries,and present an appraisal of recent advances for addressing the performance deficiency.Specifically,the progress of zinc-ion batteries is highlighted to provide a ubiquitous guideline for their commercialization in the grid-scale energy storage.Finally,we figure out the dominating general challenges for achieving high-performance AMBs,laying out a perspective for future breakthroughs.展开更多
Lithium-sulfur(Li-S) batteries have shown promises for the next-generation, high-energy electrochemical storage, yet are hindered by rapid performance decay due to the polysulfide shuttle in the cathode and safety con...Lithium-sulfur(Li-S) batteries have shown promises for the next-generation, high-energy electrochemical storage, yet are hindered by rapid performance decay due to the polysulfide shuttle in the cathode and safety concerns about potential thermal runaway. To address the above challenges, herein, we show a flame-retardant cathode binder that simultaneously improves the electrochemical stability and safety of batteries. The combination of soft and hard segments in the polymer framework of binders allows high flexibility and mechanical strength for adapting to the drastic volume change during the Li(de)intercalation of the S cathode. The binder contains a large number of polar groups, which show the high affinity to polysulfides so that they help to anchor active S species at the cathode. These polar groups also help to regulate and facilitate the Li-ion transport, promoting the kinetics of polysulfide conversion reaction. The binder contains abundant phosphine oxide groups, which, in the case of battery's thermal runaway, decompose and release PO· radicals to quench the combustion reactions and stop the fire. Consequently, Li-S batteries using the new cathode binder show the improved electrochemical performance, including a low-capacity decay of 0.046% per cycle for 800 cycles at 1 C and favorable rate capabilities of up to 3 C. This work offers new insights on the practical realization of high-energy rechargeable batteries with stable storage electrochemistry and high safety.展开更多
Energy storage technologies have been identified as the key in constructing new electric power systems and achieving carbon neutrality,as they can absorb and smooth the renewables-generated electricity.Alkaline zinc-b...Energy storage technologies have been identified as the key in constructing new electric power systems and achieving carbon neutrality,as they can absorb and smooth the renewables-generated electricity.Alkaline zinc-based flow batteries are well suitable for stationary energy storage applications,since they feature the advantages of high safety,high cell voltage and low cost.Currently,many alkaline zinc-based flow batteries have been proposed and developed,e.g.,the alkaline zinc–iron flow battery and alkaline zinc–nickel flow battery.Their development and application are closely related to advanced materials and battery configurations.In this perspective,we will first provide a brief introduction and discussion of alkaline zinc-based flow batteries.Then we focus on these batteries from the perspective of their current status,challenges and prospects.The bottlenecks for these batteries are briefly analyzed.Combined with the practical requirements and development trends of alkaline zinc-based flow battery technologies,their future development and research direction will be summarized.展开更多
Current electrochemical energy storage technology has evolved a variety of rechargeable battery systems.Recently,the resource shortage of raw materials in commercially available lithium-ion batteries has attracted wid...Current electrochemical energy storage technology has evolved a variety of rechargeable battery systems.Recently,the resource shortage of raw materials in commercially available lithium-ion batteries has attracted widespread attention.The requirements to meet resourcefulness,sustainability,safety,and high energy density have motivated the development of rechargeable magnesium-ion batteries(RMBs).Although RMBs have made significant progress so far,there are still many obstacles to practical orientation.We systematically summarize the significant progress and the latest research on RMBs,including Mg^(2+)-conducting electrolytes,Mg^(2+)-storage cathodes,and Mg-based anodes.In this review,we mainly introduce the properties and features of various Mg^(2+)-conductive electrolytes,the mainstream cathode materials,and their respective Mg^(2+)-storage mechanisms,as well as the Mg metal(or alloy)anodes and the corresponding modification strategies.Finally,the future directions in various key components for RMBs are highlighted.展开更多
Organic solar cells(OSCs) have drawn considerable attention in the last decade due to the great potential of light weight,flexibility, and low-cost solution processing. Particularly, Y-series non-fullerene acceptors(N...Organic solar cells(OSCs) have drawn considerable attention in the last decade due to the great potential of light weight,flexibility, and low-cost solution processing. Particularly, Y-series non-fullerene acceptors(NFAs) including small molecular acceptors(SMAs) and polymerized small molecular acceptors(PSMAs) have become research hot spots due to their excellent power conversion efficiency. Side chain engineering is crucial to adjust the solubility and crystallinity of NFAs, which will significantly affect the morphology of active layers and the efficiency of OSCs. However, the understanding of side chain engineering on NFAs is still limited and lacks a systematic review. This review aims to provide a brief summary of the recent developments in side chain engineering of NFAs, with a special focus on the design and application of Y-series SMAs and PSMAs for high-efficiency non-fullerene organic solar cells(NF-OSCs). In addition, the review also points out challenges and provides useful guidance regarding side chain regulation for Y-series NFAs.展开更多
Highly reduced polyoxometalates(POMs) are predicted to be used as rather high energy density materials;however,it still suffers from the limited cluster species and reduction ratio.Here we demonstrate that it is possi...Highly reduced polyoxometalates(POMs) are predicted to be used as rather high energy density materials;however,it still suffers from the limited cluster species and reduction ratio.Here we demonstrate that it is possible to employ the building block strategy to generate a highly reduced polyoxomolybdate(C_(2)H_(8)N)_(14)(NH_(4))_(4)H_(14)[Mo_(48)-ⅤMo_(26)ⅥO_(202)(OH)_(12)(SO_(4))_(6)]·46H_(2)O(Mo_(74)).The fundamental Mo-based{Mo_x}(x=4,5,and 6) building blocks,which are templated by tetra-coordinated anions{MoO_(4)}or{SO_(4)},not only lay foundation for the formation of Mo_(74) featuring an unprecedented reduction ratio of 65%,but also give rise to SBBs-mediated(secondary building blocks) supramolecular dense packing interactions among the isolated Mo_(74) clusters that are favorable for proton conduction.Remarkably,high proton conductivity(2.04×10^(-2)S cm^(-1)) had been realized at 50℃ and 90% relative humidity,revealing one of the well-known POMs-based crystalline proton conducting materials.This result highlights that this building block approach possesses great potential in producing highly reduced POM systems that can achieve controllable reduced ratio and desirable properties.展开更多
Spin-crossover(SCO)materials that reversibly switch between high-and low-spin states have potential for the storage of spin state-relative information,and have gained much attention incorporating secondary physical pr...Spin-crossover(SCO)materials that reversibly switch between high-and low-spin states have potential for the storage of spin state-relative information,and have gained much attention incorporating secondary physical properties,such as fluorescence and magneto-optical switching.In this study,we synthesized three octanuclear metal-organic cages(MOCs)using tetraphenylethylene-based luminophores,aldehydes,and Fe^(Ⅱ)salts,by subcomponent self-assembly approach,namely[Fe1]-[Fe3].By controlling the ligand-field strength and guest encapsulation,we finely tuned their SCO properties.Among them,MOC[Fe2]displayed nearly complete SCO behavior in the solid state,which is rare for high-nuclearity complexes.We also demonstrated the coupling of SCO with fluorescence emission in these MOCs by using isostructural Zn^(Ⅱ)complexes([Zn1]-[Zn3])as control experiments,for the first time.Theoretical calculations revealed the energy-transfer mechanism between fluorophores and SCOactive centers,which emphasizes the significant contribution of d-d transitions in the interplay between the occurrence of SCO and fluorescence emission.展开更多
A nickel-hydride(Ni H)-catalyzed migratory and nonmigratory hydroalkylation reaction of 2-alkenyl azaarenes with alkyl iodines has been established through strategic modulation of N-or P-donor ligands.This method enab...A nickel-hydride(Ni H)-catalyzed migratory and nonmigratory hydroalkylation reaction of 2-alkenyl azaarenes with alkyl iodines has been established through strategic modulation of N-or P-donor ligands.This method enables the synthesis of diverseβ-orγ-branched aromatic N-heterocycles.The mild regiodivergent protocols exhibit wide substrate scope,excellent functional tolerance,and great reaction yield with remarkable regioselectivity.Importantly,deuterium labeling studies reveal Ni H-catalyzed interrupted chain-walking mode as the mechanism behind remotedβ-selective hydroalkylation reaction—an interesting phenomenon mediated through aromatic imine directing groups.展开更多
An asymmetric catalytic strategy in photocatalysis utilizing a chirality-induced approach through an organocatalytic/photoredox relay catalysis strategy is successfully achieved for the rapid construction of polycycli...An asymmetric catalytic strategy in photocatalysis utilizing a chirality-induced approach through an organocatalytic/photoredox relay catalysis strategy is successfully achieved for the rapid construction of polycyclic compounds containing vicinal amino alcohols in a one-pot protocol. This methodology facilitates the efficient synthesis of diverse substituted polycyclic tetrahydroquinoline and benzofuran-derived vicinal amino alcohols, each containing five consecutive chiral centers, with high yields,excellent diastereoselectivities and enantioselectivities(up to 95% yield, >20:1 dr and 98% ee), under mild reaction conditions driven by sequential bifunctional squaramide organocatalyst-catalyzed [4+2] annulation and photocatalyst-catalyzed ketyl radical addition cyclization reaction process. Furthermore, investigations into the stereoselectivity mechanism and high-resolution mass spectrometry(HRMS) experiments on free radical trapping have provided evidence for elucidating the detailed mechanism of chirality-induced processes and chiral intermediate conversions in this procedure.展开更多
β-Chiral sulfones are structural motifs widely found in natural products and bioactive molecules, while also serving as important intermediates for the synthesis of valuable chiral scaffolds. In contrast to the rapid...β-Chiral sulfones are structural motifs widely found in natural products and bioactive molecules, while also serving as important intermediates for the synthesis of valuable chiral scaffolds. In contrast to the rapid growth of sulfur dioxide insertion chemistry over the last decade, enantioselective catalytic variants for accessing β-chiral sulfones, especially those bearing a quaternary carbon stereocenter, remain rare. Herein, we report an enantioselective copper/bisoxazoline catalyzed oxysulfonylation of alkenes to yield isoxazolinyl-containing β-chiral sulfones bearing quaternary carbon stereocenters with moderate to excellent yields and up to 96:4 er. The advantage and irreplaceability of this sulfur dioxide insertion catalytic system have been demonstrated by achieving transformations clearly unavailable with the previously reported sulfonyl chloride system. Additionally,the recoverability of the new-developed bisoxazoline ligand L9 and its reusability without any erosion of the catalytic activity and enantioselectivity further demonstrate the usefulness of the protocol.展开更多
Radical-polar crossover(RPC) reaction bridges the gap between one-and two-electron reactivities,thus providing an ideal solution to overcome the limitations of both radical and polar chemistry.In this manifold,organic...Radical-polar crossover(RPC) reaction bridges the gap between one-and two-electron reactivities,thus providing an ideal solution to overcome the limitations of both radical and polar chemistry.In this manifold,organic electrochemistry provides a uniquely facile strategy to access a diverse array of radical intermediates,thus broadening the chemical space of the RPC concept.This review highlights the synthetic advances in the field of electrochemical RPC reactions since 2020,with an emphasis on the substrate scope,reaction limitation and mechanistic aspect.The related RPC reactions are categorized as netoxidative,net-reductive,or redox neutral transformations.展开更多
Styrene-butadiene rubber(SBR)is an indispensable material in modern society,and the necessity for enhanced mechanical properties in SBR persists,particularly to withstand the rigors of challenging environmental condit...Styrene-butadiene rubber(SBR)is an indispensable material in modern society,and the necessity for enhanced mechanical properties in SBR persists,particularly to withstand the rigors of challenging environmental conditions.To surmount the limitations of conventional cross-linking modes,mechanical bonds stabilized by host-guest recognition are incorporated as the cross-linking points of SBR to form mechanically interlocked networks(MINs).Compared with covalently cross-linked network,the representative MIN exhibits superior mechanical performance in terms of elongation(1392%)and breaking strength(4.6 MPa),whose toughness has surged by 17 times.Dissociation of host-guest recognition and subsequent sliding motion provide an effective energy dissipation mechanism,and the release of hidden length is also beneficial to enhance toughness.Furthermore,the introduction of the rotaxane cross-links made the network more pliable and possess damping and elastic properties,which can return to initial state with one minute rest interval.We aspire that this direct introduction method can serve as a blueprint,offering valuable insights for the enhancement of mechanical properties in conventional commercial polymer materials.展开更多
基金supported by the CAS Project for Young Scientists in Basic Research(YSBR-058)the Basic Science Center Project of National Natural Science Foundation of China(52388201)+57 种基金the Beijing Natural Science Foundation(JQ22005)financially supported by the National Key R&D Program of China(2022YFB2404400)the National Natural Science Foundation of China(92263206,21875007,21975006,21974007,and U19A2018)the Youth Beijing Scholars program(PXM2021_014204_000023)the Beijing Natural Science Foundation(2222001 and KZ202010005007)supported by the National Key R&D Program of China(2021YFB2400200)the Youth Innovation Promotion Association CAS(2023040)the National Natural Science Foundation of China(22279148 and 21905286)the Beijing Natural Science Foundation(Z220021)supported by Beijing Municipal Natural Science Foundation(Z200011)National Key Research and Development Program(2021YFB2500300,2021YFB2400300)National Natural Science Foundation of China(22308190,22109084,22108151,22075029,and 22061132002)Key Research and Development Program of Yunnan Province(202103AA080019)the S&T Program of Hebei Province(22344402D)China Postdoctoral Science Foundation(2022TQ0165)Tsinghua-Jiangyin Innovation Special Fund(TJISF)Tsinghua-Toyota Joint Research Fundthe Institute of Strategic Research,Huawei Technologies Co.,LtdOrdos-Tsinghua Innovative&Collaborative Research Program in Carbon Neutralitythe Shuimu Tsinghua Scholar Program of Tsinghua Universityfinancially supported by the National Key R&D Program of China(2021YFB2400300)National Natural Science Foundation of China(22179083)Program of Shanghai Academic Research Leader(20XD1401900)Key-Area Research and Development Program of Guangdong Province(2019B090908001)financially supported by the National Key R&D Program of China(2020YFE0204500)the National Natural Science Foundation of China(52071311,52271140)Jilin Province Science and Technology Development Plan Funding Project(20220201112GX)Changchun Science and Technology Development Plan Funding Project(21ZY06)Youth Innovation Promotion Association CAS(2020230,2021223)supported by the National Natural Science Foundation of China(51971124,52171217,52202284 and 52250710680)the State Key Laboratory of Electrical Insulation and Power Equipment,Xi’an Jiaotong University(EIPE22208)Zhejiang Natural Science Foundation(LZ21E010001,LQ23E020002)Wenzhou Natural Science Foundation(G20220019,G20220021,ZG2022032,G2023027)Science and Technology Project of State Grid Corporation of China(5419-202158503A-0-5-ZN)Wenzhou Key Scientific and Technological Innovation Research Projects(ZG2023053)Cooperation between industry and education project of Ministry of Education(220601318235513)supported by the Australian Research Council(DP210101486 and FL210100050)supported by the National Natural Science Foundation of China(22179135,22109168,52072195,and 21975271)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA22010603,XDA22010600)Taishan Scholars Program for Young Expert of Shandong Province(tsqn202103145)Shandong Energy Institute(SEI I202108 and SEI I202127)the China Postdoctoral Science Foundation(BX20200344,2020M682251)supported by the National Key R&D Program of China(2022YFB2402200)the National Natural Science Foundation of China(22121005,22020102002,and 21835004)the Frontiers Science Center for New Organic Matter of Nankai University(63181206)the Haihe Laboratory of Sustainable Chemical Transformationssupported by National Key Research and Development Program of China(2022YFB2404500)Shenzhen Outstanding Talents Training Fundsupported by the National Key R&D Program of China(2019YFA0705104)GRF under the project number City U 11305218supported from National Natural Science Foundation of China(22078313,21925804)Free exploring basic research project of Liaoning(2022JH6/100100005)Youth Innovation Promotion Association CAS(2019182)supported from the Research Center for industries of the Future(RCIF)at Westlake Universitythe start-up fund from Westlake Universitysupported by the National Key R&D Program of China(2020YFB2007400)the National Natural Science Foundation of China(22075317)the Strategic Priority Research Program(B)(XDB07030200)of Chinese Academy of Sciences。
文摘Rechargeable batteries currently hold the largest share of the electrochemical energy storage market,and they play a major role in the sustainable energy transition and industrial decarbonization to respond to global climate change.Due to the increased popularity of consumer electronics and electric vehicles,lithium-ion batteries have quickly become the most successful rechargeable batteries in the past three decades,yet growing demands in diversified application scenarios call for new types of rechargeable batteries.Tremendous efforts are made to developing the next-generation post-Li-ion rechargeable batteries,which include,but are not limited to solid-state batteries,lithium–sulfur batteries,sodium-/potassium-ion batteries,organic batteries,magnesium-/zinc-ion batteries,aqueous batteries and flow batteries.Despite the great achievements,challenges persist in precise understandings about the electrochemical reaction and charge transfer process,and optimal design of key materials and interfaces in a battery.This roadmap tends to provide an overview about the current research progress,key challenges and future prospects of various types of rechargeable batteries.New computational methods for materials development,and characterization techniques will also be discussed as they play an important role in battery research.
基金supported by Beijing Municipal Natural Science Foundation(Z200011)National Key Research and Development Program of China(2021YFB2500300,2021YFB2400300)+8 种基金National Natural Science Foundation of China(22308190,22109084,22108151,22075029,and 22061132002)Key Research and Development Program of Yunnan Province(202103AA080019)the S&T Program of Hebei Province(22344402D)China Postdoctoral Science Foundation(2022TQ0165)Tsinghua-Jiangyin Innovation Special Fund(TJISF)Tsinghua-Toyota Joint Research Fundthe Institute of Strategic Research,Huawei Technologies Co.,LtdOrdos-Tsinghua Innovative&Collaborative Research Program in Carbon Neutralitythe Shuimu Tsinghua Scholar Program of Tsinghua University。
文摘High-energy-density lithium metal batteries are the next-generation battery systems of choice,and replacing the flammable liquid electrolyte with a polymer solid-state electrolyte is a prominent conduct towards realizing the goal of high-safety and high-specific-energy devices.Unfortunately,the inherent intractable problems of poor solid-solid contacts between the electrode/electrolyte and the growth of Li dendrites hinder their practical applications.The in-situ solidification has demonstrated a variety of advantages in the application of polymer electrolytes and artificial interphase,including the design of integrated polymer electrolytes and asymmetric polymer electrolytes to enhance the compatibility of solid–solid contact and compatibility between various electrolytes,and the construction of artificial interphase between the Li anode and cathode to suppress the formation of Li dendrites and to enhance the high-voltage stability of polymer electrolytes.This review firstly elaborates the history of in-situ solidification for solid-state batteries,and then focuses on the synthetic methods of solidified electrolytes.Furthermore,the recent progress of in-situ solidification technology from both the design of polymer electrolytes and the construction of artificial interphase is summarized,and the importance of in-situ solidification technology in enhancing safety is emphasized.Finally,prospects,emerging challenges,and practical applications of in-situ solidification are envisioned.
基金supported by the National Key R&D Program of China(2021YFB2400200)the CAS Project for Young Scientists in Basic Research(YSBR-058)+4 种基金the“Transformational Technologies for Clean Energy and Demonstration”,Strategic Priority Research Program of the Chinese Academy of Sciences(XDA21070300)the National Natural Science Foundation of China(22279148,21905286 and 22005314)the China Postdoctoral Science Foundation(2019M660805)the Special Financial Grant from the China Postdoctoral Science Foundation(2020T130658)Beijing National Laboratory for Molecular Sciences(2019BMS20022)。
文摘The energy crisis and environmental pollution drive more attention to the development and utilization of renewable energy.Considering the capricious nature of renewable energy resource,it has difficulty supplying electricity directly to consumers stably and efficiently,which calls for energy storage systems to collect energy and release electricity at peak periods.Due to their flexible power and energy,quick response,and high energy conversion efficiency,lithium-ion batteries stand out among multiple energy storage technologies and are rapidly deployed in the grid.Pursuing superior performance and ensuring the safety of energy storage systems,intrinsically safe solid-state electrolytes are expected as an ideal alternative to liquid electrolytes.In this review,we systematically evaluate the priorities and issues of traditional lithium-ion batteries in grid energy storage.Beyond lithium-ion batteries containing liquid electrolytes,solid-state lithium-ion batteries have the potential to play a more significant role in grid energy storage.The challenges of developing solid-state lithium-ion batteries,such as low ionic conductivity of the electrolyte,unstable electrode/electrolyte interface,and complicated fabrication process,are discussed in detail.Additionally,the safety of solid-state lithium-ion batteries is re-examined.Following the obtained insights,inspiring prospects for solid-state lithium-ion batteries in grid energy storage are depicted.
基金supported by the National Natural Science Foundation of China(51971124,52171217)the State Key Laboratory of Electrical Insulation and Power Equipment,Xi’an Jiaotong University(EIPE22208)+5 种基金the National Postdoctoral Program for Innovative Talents(BX20200222)the China Postdoctoral Science Foundation(2020M682878)Zhejiang Natural Science Foundation(LQ23E020002)Wenzhou Natural Science Foundation(G20220019)Cooperation between industry and education project of Ministry of Education(220601318235513)National Natural Science Foundation of China(52202284)。
文摘Because of the low price and abundant reserves of sodium compared with lithium,the research of sodium-ion batteries(SIBs)in the field of large-scale energy storage has returned to the research spotlight.Layered oxides distinguish themselves from the mains cathode materials of SIBs owing to their advantages such as high specific capacity,simple synthesis route,and environmental benignity.However,the commercial development of the layered oxides is limited by sluggish kinetics,complex phase transition and poor air stability.Based on the research ideas from macro-to micro-scale,this review systematically summarizes the current optimization strategies of sodium-ion layered oxide cathodes(SLOC)from different dimensions:microstructure design,local chemistry regulation and structural unit construction.In the dimension of microstructure design,the various structures such as the microspheres,nanoplates,nanowires and exposed active facets are prepared to improve the slow kinetics and electrochemical performance.Besides,from the view of local chemistry regulation by chemical element substitution,the intrinsic electron/ion properties of SLOC have been enhanced to strengthen the structural stability.Furthermore,the optimization idea of endeavors to regulate the physical and chemical properties of cathode materials essentially is put forward from the dimension of structural unit construction.The opinions and strategies proposed in this review will provide some inspirations for the design of new SLOC in the future.
基金financially supported by the National Key R&D Program of China(2021YFB2400300)National Natural Science Foundation of China(22179083)+1 种基金Program of Shanghai Academic Research Leader(20XD1401900)Key-Area Research and Development Program of Guangdong Province(2019B090908001)。
文摘Lithium-sulfur(Li-S)batteries have been regarded as a promising next-generation energy storage system owing to the high theoretical energy density and natural abundance of sulfur.Abundant fundamental researches have pushed the flourishing development on electrochemical behaviors in recent 20 years.It is time to evolve into post-Li-S battery era with the pursuit towards practical application.During the landmark leap,numerous new challenges appear under harsh conditions,such as high sulfur loading,low cathode density,lean electrolyte and limited lithium reservoir.Herein,we summarize the considerable parameters of pouch Li-S cells and review the pioneering studies focused on the cathode structure,conversion kinetics,electrode interphase and battery safety.The interwoven relationship of these key points is concluded and discussed,which provides guidance to future researches aiming to safe and long-lifespan Li-S batteries with high energy density.
基金supported by the National Key Research and Development Program of China (2022YFB2404800)the National Natural Science Foundation of China (52022013,51974031 and U22A20438)。
文摘Safety issues related to flammable electrolytes in lithium-ion batteries(LIBs) remain a major challenge for their extended applications.The use of non-flammable phosphate-based electrolytes has proved the validity in inhibiting the combustion of LIBs.However,the strong interaction between Li^(+) and phosphate leads to a dominant solid electrolyte interphase(SEI) with limited electronic shielding,resulting in the poor Li^(+) intercalation at the graphite(Gr) anode when using high-phosphate-content electrolytes.To mitigate this issue and improve Li^(+) insertion,we propose an “In-N-Out” strategy to render phosphates “noncoordinative”.By employing a combination of strongly polar solvents for a “block effect” and weakly polar solvents for a “drag effect”,we reduce the Li^(+)–phosphate interaction.As a result,phosphates remain in the electrolyte phase(“In”),minimizing their impact on the incompatibility with the Gr electrode(“Out”).We have developed a non-flammable electrolyte with high triethyl phosphate(TEP) content(>60 wt.%),demonstrating the excellent ion conductivity(5.94 mS cm^(-1) at 30 ℃) and reversible Li^(+) intercalation at a standard concentration(~1 mol L^(-1)).This approach enables the manipulation of multiple electrolyte functions and holds the promise for the development of safe electrochemical energy storage systems using non-flammable electrolytes.
基金supported by the National Key R&D Program of China(2019YFA0705104)GRF under the project number City U 11305218。
文摘Lithium-ion batteries(LIBs)have become one of the most successful energy storage systems due to their high operating voltage,high energy density,and long cycle life.However,with the widespread use of LIBs in recent decades,lithium resources are at risk of being exhausted.Therefore,it is necessary to find a substitute for LIBs to meet the needs of future large-scale energy storage systems.Because of their competitiveness,low cost,and high safety,aqueous rechargeable zinc-ion batteries(ARZIBs)are regarded as promising components in the post-lithium-ion-battery era.Given the tunable composition,ordered porous channels,and controllable structure of metal-organic frameworks(MOFs)and covalent organic frameworks(COFs),these frameworks are viewed as potential materials for developing high-performance ARZIBs.In this review,we focus on the recent developments in the applications of MOF-/COF-based materials in ARZIBs,including in electrode materials,anode modifications,separators,and solid electrolytes.We then focus on the critical factors and optimization techniques of MOF-/COF-based materials that affect the performance of ARZIBs.Finally,we conclude with some projections for the expansion of ARZIBs containing MOF-/COF-based materials.
基金supported by the National Natural Science Foundation of China (21961006,32172459,22371057)Science and Technology Department of Guizhou Province (Qiankehejichu-ZK[2021]Key033)+1 种基金Program of Introducing Talents of Discipline to Universities of China (111 Program,D20023) at Guizhou UniversityFrontiers Science Center for Asymmetric Synthesis and Medicinal Molecules,Department of Education,Guizhou Province (Qianjiaohe KY (2020)004),Guizhou University (China)。
文摘N-heterocyclic carbene-catalyzed enantioselective kinetic resolutions,dynamic kinetic resolutions,and desymmetrization reactions are systematically reviewed.The content is organized according to the activation modes involved in these transformations.Future advances within this highly active research field are discussed from our perspectives on the topic.
基金supported by National Key Research and Development Program of China(2022YFB2404500)Shenzhen Outstanding Talents Training Fund。
文摘Rechargeable aqueous metal-ion batteries(AMBs)have attracted extensive scientific and commercial interest due to their potential for cost-effective,highly safe,and scalable stationary energy storage.However,their limited output voltage,inadequate energy density,and poor reversibility of ambiguous electrode reactions in aqueous electrolytes strongly limit their practical viability.This review aims to elucidate the challenges of existing AMBs from the material design to whole device applications.We summarize the emerging electrochemistry,fundamental properties,and key issues in interfacial behaviors of various classes of prevailing AMBs,including aqueous alkali metal-ion batteries and multivalent-ion batteries,and present an appraisal of recent advances for addressing the performance deficiency.Specifically,the progress of zinc-ion batteries is highlighted to provide a ubiquitous guideline for their commercialization in the grid-scale energy storage.Finally,we figure out the dominating general challenges for achieving high-performance AMBs,laying out a perspective for future breakthroughs.
基金financially supported by the National Key R&D Program of China(2019YFA0705703)Natural Science Foundation of Hubei Province(2021CFB082)+4 种基金Scientific Research Foundation of Wuhan Institute of Technology(K2021042)the Open Key Fund Project of State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology,2022-KF-10)National Natural Science Foundation of China(22275142,U22B6011)China Postdoctoral Science Foundation(2021M703268)the Junior Fellow Program of Beijing National Laboratory for Molecular Sciences(2021BMS20062)。
文摘Lithium-sulfur(Li-S) batteries have shown promises for the next-generation, high-energy electrochemical storage, yet are hindered by rapid performance decay due to the polysulfide shuttle in the cathode and safety concerns about potential thermal runaway. To address the above challenges, herein, we show a flame-retardant cathode binder that simultaneously improves the electrochemical stability and safety of batteries. The combination of soft and hard segments in the polymer framework of binders allows high flexibility and mechanical strength for adapting to the drastic volume change during the Li(de)intercalation of the S cathode. The binder contains a large number of polar groups, which show the high affinity to polysulfides so that they help to anchor active S species at the cathode. These polar groups also help to regulate and facilitate the Li-ion transport, promoting the kinetics of polysulfide conversion reaction. The binder contains abundant phosphine oxide groups, which, in the case of battery's thermal runaway, decompose and release PO· radicals to quench the combustion reactions and stop the fire. Consequently, Li-S batteries using the new cathode binder show the improved electrochemical performance, including a low-capacity decay of 0.046% per cycle for 800 cycles at 1 C and favorable rate capabilities of up to 3 C. This work offers new insights on the practical realization of high-energy rechargeable batteries with stable storage electrochemistry and high safety.
基金supported by the Dalian Institute of Chemical Physics,Chinese Academy of Sciencesthe National Natural Science Foundation of China(22078313,21925804)+1 种基金Free exploring basic research project of Liaoning(2022JH6/100100005)Youth Innovation Promotion Association CAS(2019182)。
文摘Energy storage technologies have been identified as the key in constructing new electric power systems and achieving carbon neutrality,as they can absorb and smooth the renewables-generated electricity.Alkaline zinc-based flow batteries are well suitable for stationary energy storage applications,since they feature the advantages of high safety,high cell voltage and low cost.Currently,many alkaline zinc-based flow batteries have been proposed and developed,e.g.,the alkaline zinc–iron flow battery and alkaline zinc–nickel flow battery.Their development and application are closely related to advanced materials and battery configurations.In this perspective,we will first provide a brief introduction and discussion of alkaline zinc-based flow batteries.Then we focus on these batteries from the perspective of their current status,challenges and prospects.The bottlenecks for these batteries are briefly analyzed.Combined with the practical requirements and development trends of alkaline zinc-based flow battery technologies,their future development and research direction will be summarized.
基金supported by the National Natural Science Foundation of China(22179135,22109168,52072195,and 21975271)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA22010603,XDA22010600)+2 种基金Taishan Scholars Program for Young Expert of Shandong Province(tsqn202103145)Shandong Energy Institute(SEI I202108 and SEI I202127)the China Postdoctoral Science Foundation(BX20200344,2020M682251).
文摘Current electrochemical energy storage technology has evolved a variety of rechargeable battery systems.Recently,the resource shortage of raw materials in commercially available lithium-ion batteries has attracted widespread attention.The requirements to meet resourcefulness,sustainability,safety,and high energy density have motivated the development of rechargeable magnesium-ion batteries(RMBs).Although RMBs have made significant progress so far,there are still many obstacles to practical orientation.We systematically summarize the significant progress and the latest research on RMBs,including Mg^(2+)-conducting electrolytes,Mg^(2+)-storage cathodes,and Mg-based anodes.In this review,we mainly introduce the properties and features of various Mg^(2+)-conductive electrolytes,the mainstream cathode materials,and their respective Mg^(2+)-storage mechanisms,as well as the Mg metal(or alloy)anodes and the corresponding modification strategies.Finally,the future directions in various key components for RMBs are highlighted.
基金supported by the Science Foundation of Henan University of Technology(2021BS044)。
文摘Organic solar cells(OSCs) have drawn considerable attention in the last decade due to the great potential of light weight,flexibility, and low-cost solution processing. Particularly, Y-series non-fullerene acceptors(NFAs) including small molecular acceptors(SMAs) and polymerized small molecular acceptors(PSMAs) have become research hot spots due to their excellent power conversion efficiency. Side chain engineering is crucial to adjust the solubility and crystallinity of NFAs, which will significantly affect the morphology of active layers and the efficiency of OSCs. However, the understanding of side chain engineering on NFAs is still limited and lacks a systematic review. This review aims to provide a brief summary of the recent developments in side chain engineering of NFAs, with a special focus on the design and application of Y-series SMAs and PSMAs for high-efficiency non-fullerene organic solar cells(NF-OSCs). In addition, the review also points out challenges and provides useful guidance regarding side chain regulation for Y-series NFAs.
基金supported by the Natural Science Foundation of Jilin Province-Free Exploration General Project(YDZJ202201ZYTS331)the National Natural Science Foundation of China(21801038)+1 种基金the Science and Technology Research Foundation of Jilin Educational Committee(JJKH20221158KJ)the Fundamental Research Funds for the Central Universities(2412022ZD002,2412022ZD009)。
文摘Highly reduced polyoxometalates(POMs) are predicted to be used as rather high energy density materials;however,it still suffers from the limited cluster species and reduction ratio.Here we demonstrate that it is possible to employ the building block strategy to generate a highly reduced polyoxomolybdate(C_(2)H_(8)N)_(14)(NH_(4))_(4)H_(14)[Mo_(48)-ⅤMo_(26)ⅥO_(202)(OH)_(12)(SO_(4))_(6)]·46H_(2)O(Mo_(74)).The fundamental Mo-based{Mo_x}(x=4,5,and 6) building blocks,which are templated by tetra-coordinated anions{MoO_(4)}or{SO_(4)},not only lay foundation for the formation of Mo_(74) featuring an unprecedented reduction ratio of 65%,but also give rise to SBBs-mediated(secondary building blocks) supramolecular dense packing interactions among the isolated Mo_(74) clusters that are favorable for proton conduction.Remarkably,high proton conductivity(2.04×10^(-2)S cm^(-1)) had been realized at 50℃ and 90% relative humidity,revealing one of the well-known POMs-based crystalline proton conducting materials.This result highlights that this building block approach possesses great potential in producing highly reduced POM systems that can achieve controllable reduced ratio and desirable properties.
基金supported by the National Natural Science Foundation of China(92061106,22101021,22071009)the Ministry of Science and Higher Education of the Russian Federation(State assignment in the field of scientific activity,project No.FENW-2023-0017)。
文摘Spin-crossover(SCO)materials that reversibly switch between high-and low-spin states have potential for the storage of spin state-relative information,and have gained much attention incorporating secondary physical properties,such as fluorescence and magneto-optical switching.In this study,we synthesized three octanuclear metal-organic cages(MOCs)using tetraphenylethylene-based luminophores,aldehydes,and Fe^(Ⅱ)salts,by subcomponent self-assembly approach,namely[Fe1]-[Fe3].By controlling the ligand-field strength and guest encapsulation,we finely tuned their SCO properties.Among them,MOC[Fe2]displayed nearly complete SCO behavior in the solid state,which is rare for high-nuclearity complexes.We also demonstrated the coupling of SCO with fluorescence emission in these MOCs by using isostructural Zn^(Ⅱ)complexes([Zn1]-[Zn3])as control experiments,for the first time.Theoretical calculations revealed the energy-transfer mechanism between fluorophores and SCOactive centers,which emphasizes the significant contribution of d-d transitions in the interplay between the occurrence of SCO and fluorescence emission.
基金supported by the Dalian Institute of Chemical Physics,the Chinese Academy of Sciencesthe National Natural Science Foundation of China(21472186,21272231)。
文摘A nickel-hydride(Ni H)-catalyzed migratory and nonmigratory hydroalkylation reaction of 2-alkenyl azaarenes with alkyl iodines has been established through strategic modulation of N-or P-donor ligands.This method enables the synthesis of diverseβ-orγ-branched aromatic N-heterocycles.The mild regiodivergent protocols exhibit wide substrate scope,excellent functional tolerance,and great reaction yield with remarkable regioselectivity.Importantly,deuterium labeling studies reveal Ni H-catalyzed interrupted chain-walking mode as the mechanism behind remotedβ-selective hydroalkylation reaction—an interesting phenomenon mediated through aromatic imine directing groups.
基金supported by the National Natural Science Foundation of China(21632003,21871116,22071085,U22A20390)the Fundamental Research Funds for the Central Universities(lzujbky-2023-stlt01)the 111 Program from the Ministry of Education of China。
文摘An asymmetric catalytic strategy in photocatalysis utilizing a chirality-induced approach through an organocatalytic/photoredox relay catalysis strategy is successfully achieved for the rapid construction of polycyclic compounds containing vicinal amino alcohols in a one-pot protocol. This methodology facilitates the efficient synthesis of diverse substituted polycyclic tetrahydroquinoline and benzofuran-derived vicinal amino alcohols, each containing five consecutive chiral centers, with high yields,excellent diastereoselectivities and enantioselectivities(up to 95% yield, >20:1 dr and 98% ee), under mild reaction conditions driven by sequential bifunctional squaramide organocatalyst-catalyzed [4+2] annulation and photocatalyst-catalyzed ketyl radical addition cyclization reaction process. Furthermore, investigations into the stereoselectivity mechanism and high-resolution mass spectrometry(HRMS) experiments on free radical trapping have provided evidence for elucidating the detailed mechanism of chirality-induced processes and chiral intermediate conversions in this procedure.
基金supported by the National Natural Science Foundation of China(22171206)the Natural Science Foundation of Zhejiang Province(Z23B020002,LY22B020003,)+1 种基金the Open Foundation of Hunan Provincial Key Laboratory of Controllable Preparation and Functional Application of Fine Polymers(E22307)the Open Research Fund of School of Chemistry and Chemical Engineering,Henan Normal University(2020ZD04)。
文摘β-Chiral sulfones are structural motifs widely found in natural products and bioactive molecules, while also serving as important intermediates for the synthesis of valuable chiral scaffolds. In contrast to the rapid growth of sulfur dioxide insertion chemistry over the last decade, enantioselective catalytic variants for accessing β-chiral sulfones, especially those bearing a quaternary carbon stereocenter, remain rare. Herein, we report an enantioselective copper/bisoxazoline catalyzed oxysulfonylation of alkenes to yield isoxazolinyl-containing β-chiral sulfones bearing quaternary carbon stereocenters with moderate to excellent yields and up to 96:4 er. The advantage and irreplaceability of this sulfur dioxide insertion catalytic system have been demonstrated by achieving transformations clearly unavailable with the previously reported sulfonyl chloride system. Additionally,the recoverability of the new-developed bisoxazoline ligand L9 and its reusability without any erosion of the catalytic activity and enantioselectivity further demonstrate the usefulness of the protocol.
基金supported by the National Natural Science Foundation of China (22171015,22271009)the Beijing Natural Science Foundation (2222003)the Beijing Municipal Education Committee Project (KZ202110005003,KM202110005006)。
文摘Radical-polar crossover(RPC) reaction bridges the gap between one-and two-electron reactivities,thus providing an ideal solution to overcome the limitations of both radical and polar chemistry.In this manifold,organic electrochemistry provides a uniquely facile strategy to access a diverse array of radical intermediates,thus broadening the chemical space of the RPC concept.This review highlights the synthetic advances in the field of electrochemical RPC reactions since 2020,with an emphasis on the substrate scope,reaction limitation and mechanistic aspect.The related RPC reactions are categorized as netoxidative,net-reductive,or redox neutral transformations.
基金the financial support of the National Natural Science Foundation of China(22071152 and 22122105)the financial support of the National Natural Science Foundation of China(22305150)+4 种基金the financial support from the National Natural Science Foundation of China(22101175 and 52333001)Natural Science Foundation of Shanghai(22dz1207603)supported by the Starry Night Science Fund of Zhejiang University Shanghai Institute for Advanced Study(SN-ZJU-SIAS-006)State Key Laboratory of Polyolefins and Catalysis and Shanghai Key Laboratory of Catalysis Technology for Polyolefins(SKL-LCTP-202301)the Shuguang Program of Shanghai Education Development Foundation and Shanghai Municipal Education Commission(22SG11)。
文摘Styrene-butadiene rubber(SBR)is an indispensable material in modern society,and the necessity for enhanced mechanical properties in SBR persists,particularly to withstand the rigors of challenging environmental conditions.To surmount the limitations of conventional cross-linking modes,mechanical bonds stabilized by host-guest recognition are incorporated as the cross-linking points of SBR to form mechanically interlocked networks(MINs).Compared with covalently cross-linked network,the representative MIN exhibits superior mechanical performance in terms of elongation(1392%)and breaking strength(4.6 MPa),whose toughness has surged by 17 times.Dissociation of host-guest recognition and subsequent sliding motion provide an effective energy dissipation mechanism,and the release of hidden length is also beneficial to enhance toughness.Furthermore,the introduction of the rotaxane cross-links made the network more pliable and possess damping and elastic properties,which can return to initial state with one minute rest interval.We aspire that this direct introduction method can serve as a blueprint,offering valuable insights for the enhancement of mechanical properties in conventional commercial polymer materials.
