Asymmetric supercapacitors(ASCs)are promising candidates for high-power output applications;however,their theoretical capacity remains largely unrealized owing to the low specific capacity of carbon negative electrode...Asymmetric supercapacitors(ASCs)are promising candidates for high-power output applications;however,their theoretical capacity remains largely unrealized owing to the low specific capacity of carbon negative electrodes.Traditional strategies for enhancing the specific capacity of carbon via structural optimization often compromise the tap density,electrical conductivity,and rate performance of the material.In this study,we address this bottleneck by incorporating 4-hydroxy-2,2,6,6-tetramethylpiperidinyloxyl(4OT)as a redox mediator into the electrolyte to construct ASCs with well-matched capacities and potential windows between the two electrodes.With 50,100,and 200 mM 4OT added in electrolytes,the activated carbon electrodes achieve specific capacities of 113,181,and 263 mAh·g-1at 2 A·g-1.The Ni3S2/CoNi2S4positive electrode exhibited a specific capacity of 415 mAh·g-1,benefiting from its superior electrical conductivity,abundant active sites,and enhanced electrochemical activity.Notably,introducing 4OT to the electrolyte effectively balances the capacity and potential window of the two electrodes.Consequently,the as-assembled ASCs deliver a maximum energy density of55 Wh·kg-1,which surpasses previously reported values.Our work demonstrates that the rational selection and application of redox mediators have great potential for balancing electrode capacity and boosting the energy density of high-performance ASCs.展开更多
Exploring and designing bi-functional catalysts with earth-abundant elements that can work well for both hydrogen evolution reaction(HER) and oxygen evolution reaction(OER) in alkaline medium are of significance f...Exploring and designing bi-functional catalysts with earth-abundant elements that can work well for both hydrogen evolution reaction(HER) and oxygen evolution reaction(OER) in alkaline medium are of significance for producing clean fuel to relieve energy and environment crisis.Here,a novel Ni/NiO monolithic electrode was developed by a facile and cost-effective acid promoted activation of Ni foam.After the treatment,this obtained monolithic electrode with a layer of NiO on its surface demonstrates rough and sheet-like morphology,which not only possesses larger accessible surface area but also provides more reactive active sites. Compared with powder catalysts,this monolithic electrode can achieve intimate contact between the electrocatalyst and the current collector,which will alleviate the problem of pulverization and enable the stable function of the electrode. It can be served as an efficient bi-functional electrocatalyst with an overpotential of 160 mV for HER and 290 mV for OER to produce current densities of 10 mA cm^(-2) in the alkaline medium. And it maintains benign stability after 5,000 cycles,which rivals many recent reported noble-metal free catalysts in 1.0mol L^(-1) KOH solution. Attributed to the easy,scalable methodology and high catalytic efficiency,this work not only offers a promising monolithic catalyst but also inspires us to exploit other inexpensive,highly efficient and self-standing noble metalfree electrocatalysts for scale-up electrochemical water-splitting technology.展开更多
Electrocatalysis plays a central role in electrochemical energy storage and conversion systems,providing a number of sustainable processes for future technologies.As a green,renewable,and abundant natural polymer mate...Electrocatalysis plays a central role in electrochemical energy storage and conversion systems,providing a number of sustainable processes for future technologies.As a green,renewable,and abundant natural polymer material,the unique structure and physicochemical properties of wood and its derivatives provide a unique application advantage in the field of electrocatalysis,which has aroused intense attention from researchers.At present,researchers have developed many wood-based catalytic electrodes by taking advantage of the anisotropic hierarchical porous structure of wood and abundant active functional groups on the cell wall surface of wood.Here,a comprehensive review of recent progress in the design and synthesis of woodinspired electrodes for electrocatalytic reactions is summarized.Starting from the role and importance of the electrocatalytic process in the whole energy conversion system,this review highlights the composition and structure of wood,analyzes the mechanisms of electrocatalytic hydrogen evolution reaction(HER),oxygen evolution reaction(OER),urea oxidation reaction(UOR),and oxygen reduction reaction(ORR),and discusses the structure-activity relationship between the structural properties and electrochemical activity of wood-inspired electrodes.Finally,the opportunities,challenges,and future directions in the application of wood and its derivatives in the field of electrocatalysis are prospected.展开更多
Piezoresistive sensors,as an indispensable part of electronic and intelligent wearable devices,are often hindered by nonrenewable resources(graphene,conventional metal,or silicon).Biomass-derived carbonaceous material...Piezoresistive sensors,as an indispensable part of electronic and intelligent wearable devices,are often hindered by nonrenewable resources(graphene,conventional metal,or silicon).Biomass-derived carbonaceous materials boast many advantages such as their light weight,renewability,and excellent chemical stabilization.However,a major challenge is that the strength and resilience of carbon-based piezoresistive materials still falls short of requirements due to their random microarchitectures which cannot provide sufficiently good stress distribution.Encouraged by the excellent compressible properties and extraordinary strength of the Thalia dealbata stem,we propose a wood biomassderived carbon piezoresistive sensor with an artificial interconnected lamellar structure like the stem itself.By introducing a freezing-induced assembly process,a wood-based,completely delignified,nano-lignocellulose material can be built into a“bridges supported lamellar”type architecture,where subsequent freeze-drying and pyrolysis results in carbon aerogel monoliths.The resultant bioinspired carbon sponge has high compressibility and strength,of the order of two to five times higher than that of conventional metal,carbon,and organic materials.Combined with excellent biocompatible properties and chemical durability,these are useful properties for intelligent wearable devices and human-motion detection.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22579071 and 22109056)the Postgraduate Research&Practice Innovation Program of Jiangsu Province,China(No.KYCX24_4119)。
摘要Asymmetric supercapacitors(ASCs)are promising candidates for high-power output applications;however,their theoretical capacity remains largely unrealized owing to the low specific capacity of carbon negative electrodes.Traditional strategies for enhancing the specific capacity of carbon via structural optimization often compromise the tap density,electrical conductivity,and rate performance of the material.In this study,we address this bottleneck by incorporating 4-hydroxy-2,2,6,6-tetramethylpiperidinyloxyl(4OT)as a redox mediator into the electrolyte to construct ASCs with well-matched capacities and potential windows between the two electrodes.With 50,100,and 200 mM 4OT added in electrolytes,the activated carbon electrodes achieve specific capacities of 113,181,and 263 mAh·g-1at 2 A·g-1.The Ni3S2/CoNi2S4positive electrode exhibited a specific capacity of 415 mAh·g-1,benefiting from its superior electrical conductivity,abundant active sites,and enhanced electrochemical activity.Notably,introducing 4OT to the electrolyte effectively balances the capacity and potential window of the two electrodes.Consequently,the as-assembled ASCs deliver a maximum energy density of55 Wh·kg-1,which surpasses previously reported values.Our work demonstrates that the rational selection and application of redox mediators have great potential for balancing electrode capacity and boosting the energy density of high-performance ASCs.
基金supported by the National Natural Science Foundation of China (21571073 and 21673090)the National Basic Research Program of China (2015CB932600)+2 种基金Hubei Provincial Natural Science Foundation of China (2016CFA031)the Program for HUST Interdisciplinary Innovation Team (2015ZDTD038)the Fundamental Research Funds for the Central Universities
摘要Exploring and designing bi-functional catalysts with earth-abundant elements that can work well for both hydrogen evolution reaction(HER) and oxygen evolution reaction(OER) in alkaline medium are of significance for producing clean fuel to relieve energy and environment crisis.Here,a novel Ni/NiO monolithic electrode was developed by a facile and cost-effective acid promoted activation of Ni foam.After the treatment,this obtained monolithic electrode with a layer of NiO on its surface demonstrates rough and sheet-like morphology,which not only possesses larger accessible surface area but also provides more reactive active sites. Compared with powder catalysts,this monolithic electrode can achieve intimate contact between the electrocatalyst and the current collector,which will alleviate the problem of pulverization and enable the stable function of the electrode. It can be served as an efficient bi-functional electrocatalyst with an overpotential of 160 mV for HER and 290 mV for OER to produce current densities of 10 mA cm^(-2) in the alkaline medium. And it maintains benign stability after 5,000 cycles,which rivals many recent reported noble-metal free catalysts in 1.0mol L^(-1) KOH solution. Attributed to the easy,scalable methodology and high catalytic efficiency,this work not only offers a promising monolithic catalyst but also inspires us to exploit other inexpensive,highly efficient and self-standing noble metalfree electrocatalysts for scale-up electrochemical water-splitting technology.
基金supported by the National Key R&D Program of China(2023YFD2201403)the National Natural Science Foundation of China(32371508,32401265)+1 种基金the Scientific Research Foundation of Zhejiang A&F University(2019FR009)the Science Research and Technology Development Plan of Nanning(20231033).
摘要Electrocatalysis plays a central role in electrochemical energy storage and conversion systems,providing a number of sustainable processes for future technologies.As a green,renewable,and abundant natural polymer material,the unique structure and physicochemical properties of wood and its derivatives provide a unique application advantage in the field of electrocatalysis,which has aroused intense attention from researchers.At present,researchers have developed many wood-based catalytic electrodes by taking advantage of the anisotropic hierarchical porous structure of wood and abundant active functional groups on the cell wall surface of wood.Here,a comprehensive review of recent progress in the design and synthesis of woodinspired electrodes for electrocatalytic reactions is summarized.Starting from the role and importance of the electrocatalytic process in the whole energy conversion system,this review highlights the composition and structure of wood,analyzes the mechanisms of electrocatalytic hydrogen evolution reaction(HER),oxygen evolution reaction(OER),urea oxidation reaction(UOR),and oxygen reduction reaction(ORR),and discusses the structure-activity relationship between the structural properties and electrochemical activity of wood-inspired electrodes.Finally,the opportunities,challenges,and future directions in the application of wood and its derivatives in the field of electrocatalysis are prospected.
基金Hubei Provincial Natural Science Foundation of China,Grant/Award Number:2019CFA002National Basic Research Program of China,Grant/Award Number:2015CB932600+1 种基金the Fundamental Research Funds for the Central University,Grant/Award Number:2019kfyXMBZ018Zhejiang Provincial Natural Science Foundation for Distinguished Young Scholars of China,Grant/Award Number:LR19C160001。
摘要Piezoresistive sensors,as an indispensable part of electronic and intelligent wearable devices,are often hindered by nonrenewable resources(graphene,conventional metal,or silicon).Biomass-derived carbonaceous materials boast many advantages such as their light weight,renewability,and excellent chemical stabilization.However,a major challenge is that the strength and resilience of carbon-based piezoresistive materials still falls short of requirements due to their random microarchitectures which cannot provide sufficiently good stress distribution.Encouraged by the excellent compressible properties and extraordinary strength of the Thalia dealbata stem,we propose a wood biomassderived carbon piezoresistive sensor with an artificial interconnected lamellar structure like the stem itself.By introducing a freezing-induced assembly process,a wood-based,completely delignified,nano-lignocellulose material can be built into a“bridges supported lamellar”type architecture,where subsequent freeze-drying and pyrolysis results in carbon aerogel monoliths.The resultant bioinspired carbon sponge has high compressibility and strength,of the order of two to five times higher than that of conventional metal,carbon,and organic materials.Combined with excellent biocompatible properties and chemical durability,these are useful properties for intelligent wearable devices and human-motion detection.