Parking in a small parking lot within limited space poses a difficult task. It often leads to deviations between the final parking posture and the target posture. These deviations can lead to partial occupancy of adja...Parking in a small parking lot within limited space poses a difficult task. It often leads to deviations between the final parking posture and the target posture. These deviations can lead to partial occupancy of adjacent parking lots, which poses a safety threat to vehicles parked in these parking lots. However, previous studies have not addressed this issue. In this paper, we aim to evaluate the impact of parking deviation of existing vehicles next to the target parking lot(PDEVNTPL) on the automatic ego vehicle(AEV) parking, in terms of safety, comfort, accuracy, and efficiency of parking. A segmented parking training framework(SPTF) based on soft actor-critic(SAC) is proposed to improve parking performance. In the proposed method, the SAC algorithm incorporates strategy entropy into the objective function, to enable the AEV to learn parking strategies based on a more comprehensive understanding of the environment. Additionally, the SPTF simplifies complex parking tasks to maintain the high performance of deep reinforcement learning(DRL). The experimental results reveal that the PDEVNTPL has a detrimental influence on the AEV parking in terms of safety, accuracy, and comfort, leading to reductions of more than 27%, 54%, and 26%respectively. However, the SAC-based SPTF effectively mitigates this impact, resulting in a considerable increase in the parking success rate from 71% to 93%. Furthermore, the heading angle deviation is significantly reduced from 2.25 degrees to 0.43degrees.展开更多
Actor-Critic是一种强化学习方法,通过与环境在线试错交互收集样本来学习策略,是求解序贯感知决策问题的有效手段.但是,这种在线交互的主动学习范式在一些复杂真实环境中收集样本时会带来成本和安全问题离线强化学习作为一种基于数据驱...Actor-Critic是一种强化学习方法,通过与环境在线试错交互收集样本来学习策略,是求解序贯感知决策问题的有效手段.但是,这种在线交互的主动学习范式在一些复杂真实环境中收集样本时会带来成本和安全问题离线强化学习作为一种基于数据驱动的强化学习范式,强调从静态样本数据集中学习策略,与环境无探索交互,为机器人、自动驾驶、健康护理等真实世界部署应用提供了可行的解决方案,是近年来的研究热点.目前,离线强化学习方法存在学习策略和行为策略之间的分布偏移挑战,针对这个挑战,通常采用策略约束或值函数正则化来限制访问数据集分布之外(Out-Of-Distribution,OOD)的动作,从而导致学习性能过于保守,阻碍了值函数网络的泛化和学习策略的性能提升.为此,本文利用不确定性估计和OOD采样来平衡值函数学习的泛化性和保守性,提出一种基于不确定性估计的离线确定型Actor-Critic方法(Offline Deterministic Actor-Critic based on UncertaintyEstimation,ODACUE).首先,针对确定型策略,给出一种Q值函数的不确定性估计算子定义,理论证明了该算子学到的Q值函数是最优Q值函数的一种悲观估计.然后,将不确定性估计算子应用于确定型Actor-Critic框架中,通过对不确定性估计算子进行凸组合构造Critic学习的目标函数.最后,D4RL基准数据集任务上的实验结果表明:相较于对比算法,ODACUE在11个不同质量等级数据集任务中的总体性能提升最低达9.56%,最高达64.92%.此外,参数分析和消融实验进一步验证了ODACUE的稳定性和泛化能力.展开更多
In this study,a novel residential virtual power plant(RVPP)scheduling method that leverages a gate recurrent unit(GRU)-integrated deep reinforcement learning(DRL)algorithm is proposed.In the proposed scheme,the GRU-in...In this study,a novel residential virtual power plant(RVPP)scheduling method that leverages a gate recurrent unit(GRU)-integrated deep reinforcement learning(DRL)algorithm is proposed.In the proposed scheme,the GRU-integrated DRL algorithm guides the RVPP to participate effectively in both the day-ahead and real-time markets,lowering the electricity purchase costs and consumption risks for end-users.The Lagrangian relaxation technique is introduced to transform the constrained Markov decision process(CMDP)into an unconstrained optimization problem,which guarantees that the constraints are strictly satisfied without determining the penalty coefficients.Furthermore,to enhance the scalability of the constrained soft actor-critic(CSAC)-based RVPP scheduling approach,a fully distributed scheduling architecture was designed to enable plug-and-play in the residential distributed energy resources(RDER).Case studies performed on the constructed RVPP scenario validated the performance of the proposed methodology in enhancing the responsiveness of the RDER to power tariffs,balancing the supply and demand of the power grid,and ensuring customer comfort.展开更多
Metal-organic framework(MOF)and covalent organic framework(COF)are a huge group of advanced porous materials exhibiting attractive and tunable microstructural features,such as large surface area,tunable pore size,and ...Metal-organic framework(MOF)and covalent organic framework(COF)are a huge group of advanced porous materials exhibiting attractive and tunable microstructural features,such as large surface area,tunable pore size,and functional surfaces,which have significant values in various application areas.The emerging 3D printing technology further provides MOF and COFs(M/COFs)with higher designability of their macrostructure and demonstrates large achievements in their performance by shaping them into advanced 3D monoliths.However,the currently available 3D printing M/COFs strategy faces a major challenge of severe destruction of M/COFs’microstructural features,both during and after 3D printing.It is envisioned that preserving the microstructure of M/COFs in the 3D-printed monolith will bring a great improvement to the related applications.In this overview,the 3D-printed M/COFs are categorized into M/COF-mixed monoliths and M/COF-covered monoliths.Their differences in the properties,applications,and current research states are discussed.The up-to-date advancements in paste/scaffold composition and printing/covering methods to preserve the superior M/COF microstructure during 3D printing are further discussed for the two types of 3D-printed M/COF.Throughout the analysis of the current states of 3D-printed M/COFs,the expected future research direction to achieve a highly preserved microstructure in the 3D monolith is proposed.展开更多
Dear Editor,Light fields give relatively complete description of scenes from perspective of angles and positions of rays. At present time, most of the computer vision algorithms take 2D images as input which are simpl...Dear Editor,Light fields give relatively complete description of scenes from perspective of angles and positions of rays. At present time, most of the computer vision algorithms take 2D images as input which are simplified expression of light fields with depth information discarded. In theory, computer vision tasks may achieve better performance as long as complete light fields are acquired.展开更多
Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in superca...Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in supercapacitors.The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors(LICs).Herein,for the first time,custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode,respectively,for an all-COF nanofilm-structured LIC.The COFBTMB-TP nanofilm with strong electronegative–CF3 groups enables tuning the partial electron cloud density for Li^(+) migration to ensure the rapid anode kinetic process.The thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the capacity.Due to the aligned 1D channel,2D aromatic skeleton and accessible active sites of COF nanofilms,the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm^(−3) at a high-power density of 6 W cm^(−3),excellent rate capability,good cycle stability with the capacity retention rate of 77%after 5000-cycle.The COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type supercapacitors.After being comprehensively explored via ex situ XPS,7Li solid-state NMR analyses,and DFT calculation,it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C–F bonds during lithium storage.COFBTMB-TP exhibits a strong interaction with Li^(+) due to the C–F,C=O,and C–N bonds,facilitating Li^(+) desolation and absorption from the electrolyte.This work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.展开更多
Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hamper...Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water splitting.Herein,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water splitting.AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 h.After integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 V.Experimental investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high activity.Theoretical calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.展开更多
Anticipating the imminent surge of retired lithium-ion batteries(R-LIBs)from electric vehicles,the need for safe,cost-effective and environmentally friendly disposal technologies has escalated.This paper seeks to offe...Anticipating the imminent surge of retired lithium-ion batteries(R-LIBs)from electric vehicles,the need for safe,cost-effective and environmentally friendly disposal technologies has escalated.This paper seeks to offer a comprehensive overview of the entire disposal framework for R-LIBs,encompassing a broad spectrum of activities,including screening,repurposing and recycling.Firstly,we delve deeply into a thorough examination of current screening technologies,shifting the focus from a mere enumeration of screening methods to the exploration of the strategies for enhancing screening efficiency.Secondly,we outline battery repurposing with associated key factors,summarizing stationary applications and sizing methods for R-LIBs in their second life.A particular light is shed on available reconditioning solutions,demonstrating their great potential in facilitating battery safety and lifetime in repurposing scenarios and identifying their techno-economic issues.In the realm of battery recycling,we present an extensive survey of pre-treatment options and subsequent material recovery technologies.Particularly,we introduce several global leading recyclers to illustrate their industrial processes and technical intricacies.Furthermore,relevant challenges and evolving trends are investigated in pursuit of a sustainable end-of-life management and disposal framework.We hope that this study can serve as a valuable resource for researchers,industry professionals and policymakers in this field,ultimately facilitating the adoption of proper disposal practices.展开更多
Achieving a highly robust zinc(Zn)metal anode is extremely important for improving the performance of aqueous Zn-ion batteries(AZIBs)for advancing“carbon neutrality”society,which is hampered by the uncontrollable gr...Achieving a highly robust zinc(Zn)metal anode is extremely important for improving the performance of aqueous Zn-ion batteries(AZIBs)for advancing“carbon neutrality”society,which is hampered by the uncontrollable growth of Zn dendrite and severe side reactions including hydrogen evolution reaction,corrosion,and passivation,etc.Herein,an interlayer containing fluorinated zincophilic covalent organic framework with sulfonic acid groups(COF-S-F)is developed on Zn metal(Zn@COF-S-F)as the artificial solid electrolyte interface(SEI).Sulfonic acid group(-SO_(3)H)in COF-S-F can effectively ameliorate the desolvation process of hydrated Zn ions,and the three-dimensional channel with fluoride group(-F)can provide interconnected channels for the favorable transport of Zn ions with ion-confinement effects,endowing Zn@COF-S-F with dendrite-free morphology and suppressed side reactions.Consequently,Zn@COF-S-F symmetric cell can stably cycle for 1,000 h with low average hysteresis voltage(50.5 m V)at the current density of 1.5 m A cm^(-2).Zn@COF-S-F|Mn O_(2)cell delivers the discharge specific capacity of 206.8 m Ah g^(-1)at the current density of 1.2 A g^(-1)after 800 cycles with high-capacity retention(87.9%).Enlightening,building artificial SEI on metallic Zn surface with targeted design has been proved as the effective strategy to foster the practical application of high-performance AZIBs.展开更多
This research aims to propose a practical framework designed for the automatic analysis of a product’s comprehensive functionality and security vulnerabilities,generating applicable guidelines based on real-world sof...This research aims to propose a practical framework designed for the automatic analysis of a product’s comprehensive functionality and security vulnerabilities,generating applicable guidelines based on real-world software.The existing analysis of software security vulnerabilities often focuses on specific features or modules.This partial and arbitrary analysis of the security vulnerabilities makes it challenging to comprehend the overall security vulnerabilities of the software.The key novelty lies in overcoming the constraints of partial approaches.The proposed framework utilizes data from various sources to create a comprehensive functionality profile,facilitating the derivation of real-world security guidelines.Security guidelines are dynamically generated by associating functional security vulnerabilities with the latest Common Vulnerabilities and Exposure(CVE)and Common Vulnerability Scoring System(CVSS)scores,resulting in automated guidelines tailored to each product.These guidelines are not only practical but also applicable in real-world software,allowing for prioritized security responses.The proposed framework is applied to virtual private network(VPN)software,wherein a validated Level 2 data flow diagram is generated using the Spoofing,Tampering,Repudiation,Information Disclosure,Denial of Service,and Elevation of privilege(STRIDE)technique with references to various papers and examples from related software.The analysis resulted in the identification of a total of 121 vulnerabilities.The successful implementation and validation demonstrate the framework’s efficacy in generating customized guidelines for entire systems,subsystems,and selected modules.展开更多
The unique and interesting physical and chemical properties of metal–organic framework(MOF)materials have recently attracted extensive attention in a new generation of photoelectric applications.In this review,we sum...The unique and interesting physical and chemical properties of metal–organic framework(MOF)materials have recently attracted extensive attention in a new generation of photoelectric applications.In this review,we summarized and discussed the research progress on MOF-based photodetectors.The methods of preparing MOF-based photodetectors and various types of MOF single crystals and thin film as well as MOF composites are introduced in details.Additionally,the photodetectors applications for X-ray,ultraviolet and infrared light,biological detectors,and circularly polarized light photodetectors are discussed.Furthermore,summaries and challenges are provided for this important research field.展开更多
Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical composition.For ins...Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical composition.For instance,their unique porous structures promote electrolyte penetration,ions transport,and make them ideal for battery separators.Regulating the chemical composition of MOF can introduce more active sites for electrochemical reactions.Therefore,MOFs and their related composites have been extensively and thoroughly explored for LIBs.However,the reported reviews solely include the applications of MOFs in the electrode materials of LIBs and rarely involve other aspects.A systematic review of the application of MOFs in LIBs is essential for understanding the mechanism of MOFs and better designing related MOFs battery materials.This review systematically evaluates the latest developments in pristine MOFs and MOF composites for LIB applications,including MOFs as the main materials(anode,cathode,separators,and electrolytes)to auxiliary materials(coating layers and additives for electrodes).Furthermore,the synthesis,modification methods,challenges,and prospects for the application of MOFs in LIBs are discussed.展开更多
Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore mic...Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.展开更多
With the continuous advancement of communication technology,the escalating demand for electromagnetic shielding interference(EMI)materials with multifunctional and wideband EMI performance has become urgent.Controllin...With the continuous advancement of communication technology,the escalating demand for electromagnetic shielding interference(EMI)materials with multifunctional and wideband EMI performance has become urgent.Controlling the electrical and magnetic components and designing the EMI material structure have attracted extensive interest,but remain a huge challenge.Herein,we reported the alternating electromagnetic structure composite films composed of hollow metal-organic frameworks/layered MXene/nanocellulose(HMN)by alternating vacuum-assisted filtration process.The HMN composite films exhibit excellent EMI shielding effectiveness performance in the GHz frequency(66.8 dB at Kaband)and THz frequency(114.6 dB at 0.1-4.0 THz).Besides,the HMN composite films also exhibit a high reflection loss of 39.7 dB at 0.7 THz with an effective absorption bandwidth up to 2.1 THz.Moreover,HMN composite films show remarkable photothermal conversion performance,which can reach 104.6℃under 2.0 Sun and 235.4℃under 0.8 W cm^(−2),respectively.The unique micro-and macrostructural design structures will absorb more incident electromagnetic waves via interfacial polarization/multiple scattering and produce more heat energy via the local surface plasmon resonance effect.These features make the HMN composite film a promising candidate for advanced EMI devices for future 6G communication and the protection of electronic equipment in cold environments.展开更多
基金supported by National Natural Science Foundation of China(52222215, 52272420, 52072051)。
文摘Parking in a small parking lot within limited space poses a difficult task. It often leads to deviations between the final parking posture and the target posture. These deviations can lead to partial occupancy of adjacent parking lots, which poses a safety threat to vehicles parked in these parking lots. However, previous studies have not addressed this issue. In this paper, we aim to evaluate the impact of parking deviation of existing vehicles next to the target parking lot(PDEVNTPL) on the automatic ego vehicle(AEV) parking, in terms of safety, comfort, accuracy, and efficiency of parking. A segmented parking training framework(SPTF) based on soft actor-critic(SAC) is proposed to improve parking performance. In the proposed method, the SAC algorithm incorporates strategy entropy into the objective function, to enable the AEV to learn parking strategies based on a more comprehensive understanding of the environment. Additionally, the SPTF simplifies complex parking tasks to maintain the high performance of deep reinforcement learning(DRL). The experimental results reveal that the PDEVNTPL has a detrimental influence on the AEV parking in terms of safety, accuracy, and comfort, leading to reductions of more than 27%, 54%, and 26%respectively. However, the SAC-based SPTF effectively mitigates this impact, resulting in a considerable increase in the parking success rate from 71% to 93%. Furthermore, the heading angle deviation is significantly reduced from 2.25 degrees to 0.43degrees.
文摘Actor-Critic是一种强化学习方法,通过与环境在线试错交互收集样本来学习策略,是求解序贯感知决策问题的有效手段.但是,这种在线交互的主动学习范式在一些复杂真实环境中收集样本时会带来成本和安全问题离线强化学习作为一种基于数据驱动的强化学习范式,强调从静态样本数据集中学习策略,与环境无探索交互,为机器人、自动驾驶、健康护理等真实世界部署应用提供了可行的解决方案,是近年来的研究热点.目前,离线强化学习方法存在学习策略和行为策略之间的分布偏移挑战,针对这个挑战,通常采用策略约束或值函数正则化来限制访问数据集分布之外(Out-Of-Distribution,OOD)的动作,从而导致学习性能过于保守,阻碍了值函数网络的泛化和学习策略的性能提升.为此,本文利用不确定性估计和OOD采样来平衡值函数学习的泛化性和保守性,提出一种基于不确定性估计的离线确定型Actor-Critic方法(Offline Deterministic Actor-Critic based on UncertaintyEstimation,ODACUE).首先,针对确定型策略,给出一种Q值函数的不确定性估计算子定义,理论证明了该算子学到的Q值函数是最优Q值函数的一种悲观估计.然后,将不确定性估计算子应用于确定型Actor-Critic框架中,通过对不确定性估计算子进行凸组合构造Critic学习的目标函数.最后,D4RL基准数据集任务上的实验结果表明:相较于对比算法,ODACUE在11个不同质量等级数据集任务中的总体性能提升最低达9.56%,最高达64.92%.此外,参数分析和消融实验进一步验证了ODACUE的稳定性和泛化能力.
基金supported by the Sichuan Science and Technology Program(grant number 2022YFG0123).
文摘In this study,a novel residential virtual power plant(RVPP)scheduling method that leverages a gate recurrent unit(GRU)-integrated deep reinforcement learning(DRL)algorithm is proposed.In the proposed scheme,the GRU-integrated DRL algorithm guides the RVPP to participate effectively in both the day-ahead and real-time markets,lowering the electricity purchase costs and consumption risks for end-users.The Lagrangian relaxation technique is introduced to transform the constrained Markov decision process(CMDP)into an unconstrained optimization problem,which guarantees that the constraints are strictly satisfied without determining the penalty coefficients.Furthermore,to enhance the scalability of the constrained soft actor-critic(CSAC)-based RVPP scheduling approach,a fully distributed scheduling architecture was designed to enable plug-and-play in the residential distributed energy resources(RDER).Case studies performed on the constructed RVPP scenario validated the performance of the proposed methodology in enhancing the responsiveness of the RDER to power tariffs,balancing the supply and demand of the power grid,and ensuring customer comfort.
基金the support by National Research Foundation of Singapore(NRF,Project:NRF-CRP262021RS-0002),for research conducted at the National University of Singapore(NUS)。
文摘Metal-organic framework(MOF)and covalent organic framework(COF)are a huge group of advanced porous materials exhibiting attractive and tunable microstructural features,such as large surface area,tunable pore size,and functional surfaces,which have significant values in various application areas.The emerging 3D printing technology further provides MOF and COFs(M/COFs)with higher designability of their macrostructure and demonstrates large achievements in their performance by shaping them into advanced 3D monoliths.However,the currently available 3D printing M/COFs strategy faces a major challenge of severe destruction of M/COFs’microstructural features,both during and after 3D printing.It is envisioned that preserving the microstructure of M/COFs in the 3D-printed monolith will bring a great improvement to the related applications.In this overview,the 3D-printed M/COFs are categorized into M/COF-mixed monoliths and M/COF-covered monoliths.Their differences in the properties,applications,and current research states are discussed.The up-to-date advancements in paste/scaffold composition and printing/covering methods to preserve the superior M/COF microstructure during 3D printing are further discussed for the two types of 3D-printed M/COF.Throughout the analysis of the current states of 3D-printed M/COFs,the expected future research direction to achieve a highly preserved microstructure in the 3D monolith is proposed.
文摘Dear Editor,Light fields give relatively complete description of scenes from perspective of angles and positions of rays. At present time, most of the computer vision algorithms take 2D images as input which are simplified expression of light fields with depth information discarded. In theory, computer vision tasks may achieve better performance as long as complete light fields are acquired.
基金We are grateful to National Natural Science Foundation of China(Grant No.22375056,52272163)the Key R&D Program of Hebei(Grant No.216Z1201G)+1 种基金Natural Science Foundation of Hebei Province(Grant No.E2022208066,B2021208014)Key R&D Program of Hebei Technological Innovation Center of Chiral Medicine(Grant No.ZXJJ20220105).
文摘Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in supercapacitors.The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors(LICs).Herein,for the first time,custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode,respectively,for an all-COF nanofilm-structured LIC.The COFBTMB-TP nanofilm with strong electronegative–CF3 groups enables tuning the partial electron cloud density for Li^(+) migration to ensure the rapid anode kinetic process.The thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the capacity.Due to the aligned 1D channel,2D aromatic skeleton and accessible active sites of COF nanofilms,the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm^(−3) at a high-power density of 6 W cm^(−3),excellent rate capability,good cycle stability with the capacity retention rate of 77%after 5000-cycle.The COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type supercapacitors.After being comprehensively explored via ex situ XPS,7Li solid-state NMR analyses,and DFT calculation,it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C–F bonds during lithium storage.COFBTMB-TP exhibits a strong interaction with Li^(+) due to the C–F,C=O,and C–N bonds,facilitating Li^(+) desolation and absorption from the electrolyte.This work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.
基金supported by the National Key Research and Development Program of China (2022YFB4002100)the development project of Zhejiang Province's "Jianbing" and "Lingyan" (2023C01226)+4 种基金the National Natural Science Foundation of China (22278364, U22A20432, 22238008, 22211530045, and 22178308)the Fundamental Research Funds for the Central Universities (226-2022-00044 and 226-2022-00055)the Science Foundation of Donghai Laboratory (DH-2022ZY0009)the Startup Foundation for Hundred-Talent Program of Zhejiang UniversityScientific Research Fund of Zhejiang Provincial Education Department.
文摘Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water splitting.Herein,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water splitting.AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 h.After integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 V.Experimental investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high activity.Theoretical calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.
基金supported by an Australian Government Research Training Program Scholarship offered to the first author of this study。
文摘Anticipating the imminent surge of retired lithium-ion batteries(R-LIBs)from electric vehicles,the need for safe,cost-effective and environmentally friendly disposal technologies has escalated.This paper seeks to offer a comprehensive overview of the entire disposal framework for R-LIBs,encompassing a broad spectrum of activities,including screening,repurposing and recycling.Firstly,we delve deeply into a thorough examination of current screening technologies,shifting the focus from a mere enumeration of screening methods to the exploration of the strategies for enhancing screening efficiency.Secondly,we outline battery repurposing with associated key factors,summarizing stationary applications and sizing methods for R-LIBs in their second life.A particular light is shed on available reconditioning solutions,demonstrating their great potential in facilitating battery safety and lifetime in repurposing scenarios and identifying their techno-economic issues.In the realm of battery recycling,we present an extensive survey of pre-treatment options and subsequent material recovery technologies.Particularly,we introduce several global leading recyclers to illustrate their industrial processes and technical intricacies.Furthermore,relevant challenges and evolving trends are investigated in pursuit of a sustainable end-of-life management and disposal framework.We hope that this study can serve as a valuable resource for researchers,industry professionals and policymakers in this field,ultimately facilitating the adoption of proper disposal practices.
基金financially supported by National Natural Science Foundation of China(Nos.51872090,51772097,52372252)Hebei Natural Science Fund for Distinguished Young Scholar(No.E2019209433)+1 种基金Youth Talent Program of Hebei Provincial Education Department(No.BJ2018020)Natural Science Foundation of Hebei Province(No.E2020209151)。
文摘Achieving a highly robust zinc(Zn)metal anode is extremely important for improving the performance of aqueous Zn-ion batteries(AZIBs)for advancing“carbon neutrality”society,which is hampered by the uncontrollable growth of Zn dendrite and severe side reactions including hydrogen evolution reaction,corrosion,and passivation,etc.Herein,an interlayer containing fluorinated zincophilic covalent organic framework with sulfonic acid groups(COF-S-F)is developed on Zn metal(Zn@COF-S-F)as the artificial solid electrolyte interface(SEI).Sulfonic acid group(-SO_(3)H)in COF-S-F can effectively ameliorate the desolvation process of hydrated Zn ions,and the three-dimensional channel with fluoride group(-F)can provide interconnected channels for the favorable transport of Zn ions with ion-confinement effects,endowing Zn@COF-S-F with dendrite-free morphology and suppressed side reactions.Consequently,Zn@COF-S-F symmetric cell can stably cycle for 1,000 h with low average hysteresis voltage(50.5 m V)at the current density of 1.5 m A cm^(-2).Zn@COF-S-F|Mn O_(2)cell delivers the discharge specific capacity of 206.8 m Ah g^(-1)at the current density of 1.2 A g^(-1)after 800 cycles with high-capacity retention(87.9%).Enlightening,building artificial SEI on metallic Zn surface with targeted design has been proved as the effective strategy to foster the practical application of high-performance AZIBs.
基金This work is the result of commissioned research project supported by the Affiliated Institute of ETRI(2022-086)received by Junho AhnThis research was supported by the National Research Foundation of Korea(NRF)Basic Science Research Program funded by the Ministry of Education(No.2020R1A6A1A03040583)this work was supported by Korea Institute for Advancement of Technology(KIAT)Grant funded by the Korea government(MOTIE)(P0008691,HRD Program for Industrial Innovation).
文摘This research aims to propose a practical framework designed for the automatic analysis of a product’s comprehensive functionality and security vulnerabilities,generating applicable guidelines based on real-world software.The existing analysis of software security vulnerabilities often focuses on specific features or modules.This partial and arbitrary analysis of the security vulnerabilities makes it challenging to comprehend the overall security vulnerabilities of the software.The key novelty lies in overcoming the constraints of partial approaches.The proposed framework utilizes data from various sources to create a comprehensive functionality profile,facilitating the derivation of real-world security guidelines.Security guidelines are dynamically generated by associating functional security vulnerabilities with the latest Common Vulnerabilities and Exposure(CVE)and Common Vulnerability Scoring System(CVSS)scores,resulting in automated guidelines tailored to each product.These guidelines are not only practical but also applicable in real-world software,allowing for prioritized security responses.The proposed framework is applied to virtual private network(VPN)software,wherein a validated Level 2 data flow diagram is generated using the Spoofing,Tampering,Repudiation,Information Disclosure,Denial of Service,and Elevation of privilege(STRIDE)technique with references to various papers and examples from related software.The analysis resulted in the identification of a total of 121 vulnerabilities.The successful implementation and validation demonstrate the framework’s efficacy in generating customized guidelines for entire systems,subsystems,and selected modules.
基金support from the National Natural Science Foundation of China(U23A2095)the National Key R&D Program of China(2022YFA1503300)+3 种基金the Youth Innovation Promotion Association of the Chinese Academy of Sciences(Y2022081)Natural Science Foundation of Fujian Province(2022J06031)the STS Project of Fujian-CAS(2023T3003,2023T3052)Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(Grant No.2021ZR131).
文摘The unique and interesting physical and chemical properties of metal–organic framework(MOF)materials have recently attracted extensive attention in a new generation of photoelectric applications.In this review,we summarized and discussed the research progress on MOF-based photodetectors.The methods of preparing MOF-based photodetectors and various types of MOF single crystals and thin film as well as MOF composites are introduced in details.Additionally,the photodetectors applications for X-ray,ultraviolet and infrared light,biological detectors,and circularly polarized light photodetectors are discussed.Furthermore,summaries and challenges are provided for this important research field.
基金supported by the National Natural Science Foundation of China(22179006)。
文摘Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical composition.For instance,their unique porous structures promote electrolyte penetration,ions transport,and make them ideal for battery separators.Regulating the chemical composition of MOF can introduce more active sites for electrochemical reactions.Therefore,MOFs and their related composites have been extensively and thoroughly explored for LIBs.However,the reported reviews solely include the applications of MOFs in the electrode materials of LIBs and rarely involve other aspects.A systematic review of the application of MOFs in LIBs is essential for understanding the mechanism of MOFs and better designing related MOFs battery materials.This review systematically evaluates the latest developments in pristine MOFs and MOF composites for LIB applications,including MOFs as the main materials(anode,cathode,separators,and electrolytes)to auxiliary materials(coating layers and additives for electrodes).Furthermore,the synthesis,modification methods,challenges,and prospects for the application of MOFs in LIBs are discussed.
基金This research was supported by Natural Science Foundation of Jiangsu Province(BK20220405)National Natural Science Foundation of China(21834004,22276100,22304086)+5 种基金Key Laboratory for Organic Electronics&Information Displays,NJUPT(GZR2022010010,GZR2023010045)Nanjing Science and Technology Innovation Project for Chinese Scholars Studying Abroad(NJKCZYZZ2022-01)Research Fund for Jiangsu Distinguished Professor(RK030STP22001)Natural Science Research Start-up Foundation of Recruiting Talents of NJUPT(NY221006,NY223051)Natural Science Foundation of the Jiangsu Higher Education Institutions of China(23KJB150025)State Key Laboratory of Analytical Chemistry for Life Science,Nanjing University(SKLACLS2311).
文摘Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.
基金the Beijing Nova Program(20230484431)Opening Project of State Silica-Based Materials Laboratory of Anhui Province(2022KF12)is gratefully acknowledged.
文摘With the continuous advancement of communication technology,the escalating demand for electromagnetic shielding interference(EMI)materials with multifunctional and wideband EMI performance has become urgent.Controlling the electrical and magnetic components and designing the EMI material structure have attracted extensive interest,but remain a huge challenge.Herein,we reported the alternating electromagnetic structure composite films composed of hollow metal-organic frameworks/layered MXene/nanocellulose(HMN)by alternating vacuum-assisted filtration process.The HMN composite films exhibit excellent EMI shielding effectiveness performance in the GHz frequency(66.8 dB at Kaband)and THz frequency(114.6 dB at 0.1-4.0 THz).Besides,the HMN composite films also exhibit a high reflection loss of 39.7 dB at 0.7 THz with an effective absorption bandwidth up to 2.1 THz.Moreover,HMN composite films show remarkable photothermal conversion performance,which can reach 104.6℃under 2.0 Sun and 235.4℃under 0.8 W cm^(−2),respectively.The unique micro-and macrostructural design structures will absorb more incident electromagnetic waves via interfacial polarization/multiple scattering and produce more heat energy via the local surface plasmon resonance effect.These features make the HMN composite film a promising candidate for advanced EMI devices for future 6G communication and the protection of electronic equipment in cold environments.