Rechargeable lithium-oxygen(Li-O_(2))batteries are the next generation energy storage devices due to their ultrahigh theoretical capacity.Redox mediators(RMs)are widely used as a homogenous electrocatalyst in non-aque...Rechargeable lithium-oxygen(Li-O_(2))batteries are the next generation energy storage devices due to their ultrahigh theoretical capacity.Redox mediators(RMs)are widely used as a homogenous electrocatalyst in non-aqueous Li-O_(2)batteries to enhance their discharge capacity and reduce charge overpotential.However,the shuttle effect of RMs in the electrolyte solution usually leads to corrosion of the Li metal anode and uneven Li deposition on the anode surface,resulting in unwanted consumption of electrocatalysts and deterioration of the cells.It is therefore necessary to take some measures to prevent the shuttle effect of RMs and fully utilize the soluble electrocatalysts.Herein,we summarize the strategies to suppress the RM shuttle effect reported in recent years,including electrolyte additives,protective separators and electrode modification.The mechanisms of these strategies are analyzed and their corresponding requirements are discussed.The electrochemical properties of Li-O_(2)batteries with different strategies are summarized and compared.The challenges and perspectives on preventing the shuttle effect of RMs are described for future study.This review provides guidance for achieving shuttle-free redox mediation and for designing Li-O_(2)cells with a long cycle life,high energy efficiency and highly reversible electrochemical reactions.展开更多
The inspection of water conveyance tunnels plays an important role in water diversion projects.Siltation is an essential factor threatening the safety of water conveyance tunnels.Accurate and efficient identification ...The inspection of water conveyance tunnels plays an important role in water diversion projects.Siltation is an essential factor threatening the safety of water conveyance tunnels.Accurate and efficient identification of such siltation can reduce risks and enhance safety and reliability of these projects.The remotely operated vehicle(ROV)can detect such siltation.However,it needs to improve its intelligent recognition of image data it obtains.This paper introduces the idea of ensemble deep learning.Based on the VGG16 network,a compact convolutional neural network(CNN)is designed as a primary learner,called Silt-net,which is used to identify the siltation images.At the same time,the fully-connected network is applied as the meta-learner,and stacking ensemble learning is combined with the outputs of the primary classifiers to obtain satisfactory classification results.Finally,several evaluation metrics are used to measure the performance of the proposed method.The experimental results on the siltation dataset show that the classification accuracy of the proposed method reaches 97.2%,which is far better than the accuracy of other classifiers.Furthermore,the proposed method can weigh the accuracy and model complexity on a platform with limited computing resources.展开更多
Lithium-oxygen(Li-O_(2))batteries have a great potential in energy storage and conversion due to their ultra-high theoretical specific energy,but their applications are hindered by sluggish redox reaction kinetics in ...Lithium-oxygen(Li-O_(2))batteries have a great potential in energy storage and conversion due to their ultra-high theoretical specific energy,but their applications are hindered by sluggish redox reaction kinetics in the charge/discharge processes.Redox mediators(RMs),as soluble catalysts,are widely used to facilitate the electrochemical processes in the Li-O_(2)batteries.A drawback of RMs is the shuttle effect due to their solubility and mobility,which leads to the corrosion of a Li metal anode and the degradation of the electrochemical performance of the batteries.Herein,we synthesize a polymer-based composite protective separator containing molecular sieves.The nanopores with a diameter of 4Åin the zeolite powder(4A zeolite)are able to physically block the migration of 2,2,6,6-tetramethylpiperidinyloxy(TEMPO)molecules with a larger size;therefore,the shuttle effect of TEMPO is restrained.With the assistance of the zeolite molecular sieves,the cycle life of the Li-O_(2)batteries is significantly extended from~20 to 170 cycles at a current density of 250 mA·g^(-1)and a limited capacity of 500 mAh·g^(-1).Our work provides a highly effective approach to suppress the shuttle effects of RMs and boost the electrochemical performance of Li-O_(2)batteries.展开更多
基金financially supported by the Tsinghua-Foshan Innovation Special Fund(Grant No.2018THFS0409)the China Postdoctoral Science Foundation(Grant No.2019M650668)the National Key Research and Development Program of China(Grant No.2016YFA0201003)。
文摘Rechargeable lithium-oxygen(Li-O_(2))batteries are the next generation energy storage devices due to their ultrahigh theoretical capacity.Redox mediators(RMs)are widely used as a homogenous electrocatalyst in non-aqueous Li-O_(2)batteries to enhance their discharge capacity and reduce charge overpotential.However,the shuttle effect of RMs in the electrolyte solution usually leads to corrosion of the Li metal anode and uneven Li deposition on the anode surface,resulting in unwanted consumption of electrocatalysts and deterioration of the cells.It is therefore necessary to take some measures to prevent the shuttle effect of RMs and fully utilize the soluble electrocatalysts.Herein,we summarize the strategies to suppress the RM shuttle effect reported in recent years,including electrolyte additives,protective separators and electrode modification.The mechanisms of these strategies are analyzed and their corresponding requirements are discussed.The electrochemical properties of Li-O_(2)batteries with different strategies are summarized and compared.The challenges and perspectives on preventing the shuttle effect of RMs are described for future study.This review provides guidance for achieving shuttle-free redox mediation and for designing Li-O_(2)cells with a long cycle life,high energy efficiency and highly reversible electrochemical reactions.
基金Thanks to South to North Water Diversion Central Route Information Technology Co.,Ltd.for providing the underwater video of the water conveyance tunnels for research purposes.This work was supported by the National Key R&D Program of China(No.2016YFC0401600)the National Natural Science Foundation of China(Grant Nos.51979027,52079022,51769033,and 51779035).It should be understood that none of the authors have any financial or scientific conflicts of interest with regard to the research described in this manuscript.
文摘The inspection of water conveyance tunnels plays an important role in water diversion projects.Siltation is an essential factor threatening the safety of water conveyance tunnels.Accurate and efficient identification of such siltation can reduce risks and enhance safety and reliability of these projects.The remotely operated vehicle(ROV)can detect such siltation.However,it needs to improve its intelligent recognition of image data it obtains.This paper introduces the idea of ensemble deep learning.Based on the VGG16 network,a compact convolutional neural network(CNN)is designed as a primary learner,called Silt-net,which is used to identify the siltation images.At the same time,the fully-connected network is applied as the meta-learner,and stacking ensemble learning is combined with the outputs of the primary classifiers to obtain satisfactory classification results.Finally,several evaluation metrics are used to measure the performance of the proposed method.The experimental results on the siltation dataset show that the classification accuracy of the proposed method reaches 97.2%,which is far better than the accuracy of other classifiers.Furthermore,the proposed method can weigh the accuracy and model complexity on a platform with limited computing resources.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.U21A2080 and 51788104)Beijing Natural Science Foundation(No.L223008)National Key Research and Development Program of China(No.2022YFB2404403).
文摘Lithium-oxygen(Li-O_(2))batteries have a great potential in energy storage and conversion due to their ultra-high theoretical specific energy,but their applications are hindered by sluggish redox reaction kinetics in the charge/discharge processes.Redox mediators(RMs),as soluble catalysts,are widely used to facilitate the electrochemical processes in the Li-O_(2)batteries.A drawback of RMs is the shuttle effect due to their solubility and mobility,which leads to the corrosion of a Li metal anode and the degradation of the electrochemical performance of the batteries.Herein,we synthesize a polymer-based composite protective separator containing molecular sieves.The nanopores with a diameter of 4Åin the zeolite powder(4A zeolite)are able to physically block the migration of 2,2,6,6-tetramethylpiperidinyloxy(TEMPO)molecules with a larger size;therefore,the shuttle effect of TEMPO is restrained.With the assistance of the zeolite molecular sieves,the cycle life of the Li-O_(2)batteries is significantly extended from~20 to 170 cycles at a current density of 250 mA·g^(-1)and a limited capacity of 500 mAh·g^(-1).Our work provides a highly effective approach to suppress the shuttle effects of RMs and boost the electrochemical performance of Li-O_(2)batteries.