The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly co...The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.展开更多
Rational architecture design has turned out to be an effective strategy in improving the electrochemical performance of electrode materials for batteries.However,an elaborate structure that could simultaneously endow ...Rational architecture design has turned out to be an effective strategy in improving the electrochemical performance of electrode materials for batteries.However,an elaborate structure that could simultaneously endow active materials with promoted reaction reversibility,accelerated kinetic and restricted volume change still remains a huge challenge.Herein,a novel chemical interaction motivated structure design strategy has been proposed,and a chemically bonded Co(CO_(3))_(0.5)OH·0.11 H_(2)O@MXene(CoCH@MXene)layered-composite was fabricated for the first time.In such a composite,the chemical interaction between Co^(2+)and MXene drives the growth of smaller-sized CoCH crystals and the subsequent formation of interwoven CoCH wires sandwiched in-between MXene nanosheets.This unique layered structure not only encourages charge transfer for faster reaction dynamics,but buffers the volume change of CoCH during lithiation-delithiation process,owing to the confined crystal growth between conductive MXene layers with the help of chemical bonding.Besides,the sandwiched interwoven CoCH wires also prevent the stacking of MXene layers,further conducive to the electrochemical performance of the composite.As a result,the as-prepared CoCH@MXene anode demonstrates a high reversible capacity(903.1 mAh g^(-1)at 100 mA g^(-1))and excellent cycling stability(maintains 733.6 mAh g^(-1)at1000 mA g^(-1)after 500 cycles)for lithium ion batteries.This work highlights a novel concept of layerby-layer chemical interaction motivated architecture design for futuristic high performance electrode materials in energy storage systems.展开更多
Living in a world of heavy industrialization and confronted by the ever-deteriorating environment,the human race is now undertaking serious efforts to reach the target of carbon neutrality.One major step is to promote...Living in a world of heavy industrialization and confronted by the ever-deteriorating environment,the human race is now undertaking serious efforts to reach the target of carbon neutrality.One major step is to promote the development of sustainable electrochemical energy storage and conversion technologies based on green resources instead of the traditional nonreusable petroleum-based technologies.As an almost inexhaustible bioresource,nanocellulose derived from natural biomass exhibits outstanding physiochemical properties that could be well leveraged to bring about numerous opportunities for electrochemical processes.Through structure engineering,nanocellulose with a width of a few tens of nanometers and a length of up to micrometers could be realized.The drastic reduction in dimensions leads to superior mechanical,optical,and functional properties inaccessible to the bulky cellulose counterpart.In this review,different types of nanocellulose with distinctive physiochemical properties and their respective preparation methods are first examined.This is followed by a detailed and insightful analysis of the superiority and unprecedented performance gains that nanocellulose imparts to different electrochemical energy storage and conversion applications as a result of nanosizing.Finally,we humbly put forward our perspectives on the problems regarding current studies as well as on the future research direction for nanocellulose-mediated electrochemical processes to enable practical applications.This review is intended as guidance to initiate cross-disciplinary research effort in this engaging field and help evoke inspiration to effect solutions to critical energy issues of the day.展开更多
Lithium-sulfur batteries(LSBs)have emerged as a promising high energy density system in miniaturized energy storage devices.However,serious issues rooted in large volume change(80%),poor intrinsic conductivity,“shutt...Lithium-sulfur batteries(LSBs)have emerged as a promising high energy density system in miniaturized energy storage devices.However,serious issues rooted in large volume change(80%),poor intrinsic conductivity,“shuttle effect”of S cathode,and limited mass loading of traditional electrode still make it a big challenge to achieve high energy density LSBs in a limited footprint.Herein,an innovative carbon dioxide(CO_(2))assisted three-dimensional(3D)printing strategy is proposed to fabricate threedimensional lattice structured CO_(2)activated single-walled carbon nanotubes/S composite thick electrode(3DP S@CNTs-CO_(2))for high areal capacity LSBs.The 3D lattice structure formed by interwoven CNTs and printed regular macropores can not only act as fast electron transfer networks,ensuring good electronic conductivity of thick electrode,but is beneficial to electrolyte infiltration,effectively boosting ion diffusion kinetics even under a high-mass loading.In addition,the subsequent hightemperature CO_(2)in-situ etching can induce abundant nanopores on the wall of CNTs,which significantly promotes the sulfur loading as well as its full utilization as a result of shortened ion diffusion paths.Owing to these merits,the 3DP S@CNTs-CO_(2)electrode delivers an impressive mass loading of 10 mg·cm^(−2).More importantly,a desired attribute of linearly scale up in areal capacitance with increased layers is observed,up to an outstanding value of 5.74 mAh·cm^(−2),outperforming most reported LSBs that adopt strategies that physically inhibit polysulfides.This work provides a thrilling drive that stimulates the application of LSBs in new generation miniaturized electronic devices.展开更多
The limitation of areal energy density of rechargeable aqueous hybrid batteries(RAHBs)has been a significant longstanding problem that impedes the application of RAHBs in miniaturized energy storage.Constructing thick...The limitation of areal energy density of rechargeable aqueous hybrid batteries(RAHBs)has been a significant longstanding problem that impedes the application of RAHBs in miniaturized energy storage.Constructing thick electrodes with optimized geometrical properties is a promising strategy for achieving high areal energy density,but the sluggish ion/electron transfer and poor mechanical stability,as well as the increased electrode thickness,itself present well-known problems.In this work,a 3D printing technique is introduced to construct an ultra-thick lithium iron phosphate(LFP)/carboxylated carbon nanotube(CNT)/carboxyl terminated cellulose nanofiber(CNF)composite electrode with uncompromised reaction kinetics for high areal energy density Li–Zn RAHBs.The uniformly dispersed CNTs and CNFs form continuous interconnected 3D networks that encapsulate LFP nanoparticles,guaranteeing fast electron transfer and efficient stress relief as the electrode thickness increases.Additionally,multistage ion diffusion channels generated from the hierarchical porous structure assure accelerated ion diffusion.As a result,LFP/Zn hybrid pouch cells assembled with 3D printed electrodes deliver a well-retained reversible gravimetric capacity of about 143.5 mAh g^(-1) at 0.5 C as the electrode thickness increases from 0.52 to 1.56 mm,and establish a record-high areal energy density of 5.25 mWh cm^(-2) with an impressive utilization of active material up to 30 mg cm^(-2) for an ultra-thick(2.08 mm)electrode,which outperforms almost all reported zinc-based hybrid-ion and single-ion batteries.This work opens up exciting prospects for developing high areal energy density energy storage devices using 3D printing.展开更多
基金financially supported by the National Natural Science Foundation of China(No.51933007,No.52373047,No.52302106)the Sichuan Youth Science and Technology Innovation Research Team Project(No.2022JDTD0012)+2 种基金the Program for Featured Directions of Engineering Multidisciplines of Sichuan University(No.2020SCUNG203)the Natural Science Foundation of Sichuan Province(No.2023NSFSC0418)the Program for State Key Laboratory of Polymer Materials Engineering(No.sklpme2022-3-10)。
文摘The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.
基金financially supported by the National Natural Science Foundation of China(No.51933007,No.51673123 and No.22005346)the National Key R&D Program of China(No.2017YFE0111500)+1 种基金the State Key Laboratory of Polymer Materials Engineering(Grant No.:sklpme2020-1-02)Financial support provided by the Fundamental Research Funds for the Central Universities(No.YJ202118)。
文摘Rational architecture design has turned out to be an effective strategy in improving the electrochemical performance of electrode materials for batteries.However,an elaborate structure that could simultaneously endow active materials with promoted reaction reversibility,accelerated kinetic and restricted volume change still remains a huge challenge.Herein,a novel chemical interaction motivated structure design strategy has been proposed,and a chemically bonded Co(CO_(3))_(0.5)OH·0.11 H_(2)O@MXene(CoCH@MXene)layered-composite was fabricated for the first time.In such a composite,the chemical interaction between Co^(2+)and MXene drives the growth of smaller-sized CoCH crystals and the subsequent formation of interwoven CoCH wires sandwiched in-between MXene nanosheets.This unique layered structure not only encourages charge transfer for faster reaction dynamics,but buffers the volume change of CoCH during lithiation-delithiation process,owing to the confined crystal growth between conductive MXene layers with the help of chemical bonding.Besides,the sandwiched interwoven CoCH wires also prevent the stacking of MXene layers,further conducive to the electrochemical performance of the composite.As a result,the as-prepared CoCH@MXene anode demonstrates a high reversible capacity(903.1 mAh g^(-1)at 100 mA g^(-1))and excellent cycling stability(maintains 733.6 mAh g^(-1)at1000 mA g^(-1)after 500 cycles)for lithium ion batteries.This work highlights a novel concept of layerby-layer chemical interaction motivated architecture design for futuristic high performance electrode materials in energy storage systems.
基金supported by the National Natural Science Foundation of China(Nos.51933007,51673123,51803141)National Key R&D Program of China(No.2017YFE0111500).
文摘Living in a world of heavy industrialization and confronted by the ever-deteriorating environment,the human race is now undertaking serious efforts to reach the target of carbon neutrality.One major step is to promote the development of sustainable electrochemical energy storage and conversion technologies based on green resources instead of the traditional nonreusable petroleum-based technologies.As an almost inexhaustible bioresource,nanocellulose derived from natural biomass exhibits outstanding physiochemical properties that could be well leveraged to bring about numerous opportunities for electrochemical processes.Through structure engineering,nanocellulose with a width of a few tens of nanometers and a length of up to micrometers could be realized.The drastic reduction in dimensions leads to superior mechanical,optical,and functional properties inaccessible to the bulky cellulose counterpart.In this review,different types of nanocellulose with distinctive physiochemical properties and their respective preparation methods are first examined.This is followed by a detailed and insightful analysis of the superiority and unprecedented performance gains that nanocellulose imparts to different electrochemical energy storage and conversion applications as a result of nanosizing.Finally,we humbly put forward our perspectives on the problems regarding current studies as well as on the future research direction for nanocellulose-mediated electrochemical processes to enable practical applications.This review is intended as guidance to initiate cross-disciplinary research effort in this engaging field and help evoke inspiration to effect solutions to critical energy issues of the day.
基金supported by the National Natural Science Foundation of China(Nos.51933007 and 51673123)the National Key Research and development Program of China(No.2017YFE0111500)the Program for Featured Directions of Engineering Multidisciplines of Sichuan University(No.2020SCUNG203).
文摘Lithium-sulfur batteries(LSBs)have emerged as a promising high energy density system in miniaturized energy storage devices.However,serious issues rooted in large volume change(80%),poor intrinsic conductivity,“shuttle effect”of S cathode,and limited mass loading of traditional electrode still make it a big challenge to achieve high energy density LSBs in a limited footprint.Herein,an innovative carbon dioxide(CO_(2))assisted three-dimensional(3D)printing strategy is proposed to fabricate threedimensional lattice structured CO_(2)activated single-walled carbon nanotubes/S composite thick electrode(3DP S@CNTs-CO_(2))for high areal capacity LSBs.The 3D lattice structure formed by interwoven CNTs and printed regular macropores can not only act as fast electron transfer networks,ensuring good electronic conductivity of thick electrode,but is beneficial to electrolyte infiltration,effectively boosting ion diffusion kinetics even under a high-mass loading.In addition,the subsequent hightemperature CO_(2)in-situ etching can induce abundant nanopores on the wall of CNTs,which significantly promotes the sulfur loading as well as its full utilization as a result of shortened ion diffusion paths.Owing to these merits,the 3DP S@CNTs-CO_(2)electrode delivers an impressive mass loading of 10 mg·cm^(−2).More importantly,a desired attribute of linearly scale up in areal capacitance with increased layers is observed,up to an outstanding value of 5.74 mAh·cm^(−2),outperforming most reported LSBs that adopt strategies that physically inhibit polysulfides.This work provides a thrilling drive that stimulates the application of LSBs in new generation miniaturized electronic devices.
基金supported by the National Natural Science Foundation of China(22005346,51673123,and 51933007)the National Key R&D Program of China(2017YFE0111500)+2 种基金the Program for Featured Directions of Engineering Multidisciplines of Sichuan University(2020SCUNG203)the State Key Laboratory of Polymer Materials Engineering(sklpme2020-1-02)the Fundamental Research Funds for the Central Universities(YJ202118)。
文摘The limitation of areal energy density of rechargeable aqueous hybrid batteries(RAHBs)has been a significant longstanding problem that impedes the application of RAHBs in miniaturized energy storage.Constructing thick electrodes with optimized geometrical properties is a promising strategy for achieving high areal energy density,but the sluggish ion/electron transfer and poor mechanical stability,as well as the increased electrode thickness,itself present well-known problems.In this work,a 3D printing technique is introduced to construct an ultra-thick lithium iron phosphate(LFP)/carboxylated carbon nanotube(CNT)/carboxyl terminated cellulose nanofiber(CNF)composite electrode with uncompromised reaction kinetics for high areal energy density Li–Zn RAHBs.The uniformly dispersed CNTs and CNFs form continuous interconnected 3D networks that encapsulate LFP nanoparticles,guaranteeing fast electron transfer and efficient stress relief as the electrode thickness increases.Additionally,multistage ion diffusion channels generated from the hierarchical porous structure assure accelerated ion diffusion.As a result,LFP/Zn hybrid pouch cells assembled with 3D printed electrodes deliver a well-retained reversible gravimetric capacity of about 143.5 mAh g^(-1) at 0.5 C as the electrode thickness increases from 0.52 to 1.56 mm,and establish a record-high areal energy density of 5.25 mWh cm^(-2) with an impressive utilization of active material up to 30 mg cm^(-2) for an ultra-thick(2.08 mm)electrode,which outperforms almost all reported zinc-based hybrid-ion and single-ion batteries.This work opens up exciting prospects for developing high areal energy density energy storage devices using 3D printing.