Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains...Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains a confusing topic.Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures(SCSs)for Zn-ion storage with double-high capacitive activity and durability.Tetrachlorobenzoquinone(H-bond acceptor)and dimethylbenzidine(H-bond donator)can interact to form organic nanosheet modules,which are sequentially assembled,orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds(N-H···O).Featured with rich surface-active heterodiatomic motifs,more exposed nanoporous channels,and successive charge migration paths,SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers(3.3Ωs-0.5).Consequently,the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics,including high energy density(166 Wh kg-1),high-rate performance(172 m Ah g^(-1)at 20 A g^(-1)),and long-lasting cycling lifespan(95.5%capacity retention after 500,000 cycles).An opposite chargecarrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage,involving high-kinetics physical Zn^(2+)/CF_(3)SO_(3)-adsorption and chemical Zn^(2+)redox with carbonyl/pyridine groups.This work gives insights into H-bond-guided interfacial superassembly design of superstructural carbons toward advanced energy storage.展开更多
Flexible electronics face critical challenges in achieving monolithic three-dimensional(3D)integration,including material compatibility,structural stability,and scalable fabrication methods.Inspired by the tactile sen...Flexible electronics face critical challenges in achieving monolithic three-dimensional(3D)integration,including material compatibility,structural stability,and scalable fabrication methods.Inspired by the tactile sensing mechanism of the human skin,we have developed a flexible monolithic 3D-integrated tactile sensing system based on a holey MXene paste,where each vertical one-body unit simultaneously functions as a microsupercapacitor and pressure sensor.The in-plane mesopores of MXene significantly improve ion accessibility,mitigate the self-stacking of nanosheets,and allow the holey MXene to multifunctionally act as a sensing material,an active electrode,and a conductive interconnect,thus drastically reducing the interface mismatch and enhancing the mechanical robustness.Furthermore,we fabricate a large-scale device using a blade-coating and stamping method,which demonstrates excellent mechanical flexibility,low-power consumption,rapid response,and stable long-term operation.As a proof-of-concept application,we integrate our sensing array into a smart access control system,leveraging deep learning to accurately identify users based on their unique pressing behaviors.This study provides a promising approach for designing highly integrated,intelligent,and flexible electronic systems for advanced human-computer interactions and personalized electronics.展开更多
Innovative use of HfO_(2)-based high-dielectric-permittivity materials could enable their integration into few-nanometre-scale devices for storing substantial quantities of electrical charges,which have received wides...Innovative use of HfO_(2)-based high-dielectric-permittivity materials could enable their integration into few-nanometre-scale devices for storing substantial quantities of electrical charges,which have received widespread applications in high-storage-density dynamic random access memory and energy-efficient complementary metal-oxide-semiconductor devices.During bipolar high electric-field cycling in numbers close to dielectric breakdown,the dielectric permittivity suddenly increases by 30 times after oxygen-vacancy ordering and ferroelectric-to-nonferroelectric phase transition of near-edge plasma-treated Hf_(0.5)Zr_(0.5)O_(2) thin-film capacitors.Here we report a much higher dielectric permittivity of 1466 during downscaling of the capacitor into the diameter of 3.85μm when the ferroelectricity suddenly disappears without high-field cycling.The stored charge density is as high as 183μC cm^(−2) at an operating voltage/time of 1.2 V/50 ns at cycle numbers of more than 10^(12) without inducing dielectric breakdown.The study of synchrotron X-ray micro-diffraction patterns show missing of a mixed tetragonal phase.The image of electron energy loss spectroscopy shows the preferred oxygen-vacancy accumulation at the regions near top/bottom electrodes as well as grain boundaries.The ultrahigh dielectric-permittivity material enables high-density integration of extremely scaled logic and memory devices in the future.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22272118,22172111,and 22309134)the Science and Technology Commission of Shanghai Municipality,China(Nos.22ZR1464100,20ZR1460300,and 19DZ2271500)+2 种基金the China Postdoctoral Science Foundation(2022M712402),the Shanghai Rising-Star Program(23YF1449200)the Zhejiang Provincial Science and Technology Project(2022C01182)the Fundamental Research Funds for the Central Universities(2023-3-YB-07)。
文摘Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains a confusing topic.Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures(SCSs)for Zn-ion storage with double-high capacitive activity and durability.Tetrachlorobenzoquinone(H-bond acceptor)and dimethylbenzidine(H-bond donator)can interact to form organic nanosheet modules,which are sequentially assembled,orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds(N-H···O).Featured with rich surface-active heterodiatomic motifs,more exposed nanoporous channels,and successive charge migration paths,SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers(3.3Ωs-0.5).Consequently,the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics,including high energy density(166 Wh kg-1),high-rate performance(172 m Ah g^(-1)at 20 A g^(-1)),and long-lasting cycling lifespan(95.5%capacity retention after 500,000 cycles).An opposite chargecarrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage,involving high-kinetics physical Zn^(2+)/CF_(3)SO_(3)-adsorption and chemical Zn^(2+)redox with carbonyl/pyridine groups.This work gives insights into H-bond-guided interfacial superassembly design of superstructural carbons toward advanced energy storage.
基金supported by the National Natural Science Foundation of China(52272177,12204010)the Foundation for the Introduction of High-Level Talents of Anhui University(S020118002/097)+1 种基金the University Synergy Innovation Program of Anhui Province(GXXT-2023-066)the Scientific Research Project of Anhui Provincial Higher Education Institution(2023AH040008)。
文摘Flexible electronics face critical challenges in achieving monolithic three-dimensional(3D)integration,including material compatibility,structural stability,and scalable fabrication methods.Inspired by the tactile sensing mechanism of the human skin,we have developed a flexible monolithic 3D-integrated tactile sensing system based on a holey MXene paste,where each vertical one-body unit simultaneously functions as a microsupercapacitor and pressure sensor.The in-plane mesopores of MXene significantly improve ion accessibility,mitigate the self-stacking of nanosheets,and allow the holey MXene to multifunctionally act as a sensing material,an active electrode,and a conductive interconnect,thus drastically reducing the interface mismatch and enhancing the mechanical robustness.Furthermore,we fabricate a large-scale device using a blade-coating and stamping method,which demonstrates excellent mechanical flexibility,low-power consumption,rapid response,and stable long-term operation.As a proof-of-concept application,we integrate our sensing array into a smart access control system,leveraging deep learning to accurately identify users based on their unique pressing behaviors.This study provides a promising approach for designing highly integrated,intelligent,and flexible electronic systems for advanced human-computer interactions and personalized electronics.
基金supported by the National Key Basic Research Program of China (2022YFA1402904)Basic Research Project of Shanghai Science and Technology Innovation Action (grant number 24CL2900900)the National Natural Science Foundation of China (grant number 61904034)
文摘Innovative use of HfO_(2)-based high-dielectric-permittivity materials could enable their integration into few-nanometre-scale devices for storing substantial quantities of electrical charges,which have received widespread applications in high-storage-density dynamic random access memory and energy-efficient complementary metal-oxide-semiconductor devices.During bipolar high electric-field cycling in numbers close to dielectric breakdown,the dielectric permittivity suddenly increases by 30 times after oxygen-vacancy ordering and ferroelectric-to-nonferroelectric phase transition of near-edge plasma-treated Hf_(0.5)Zr_(0.5)O_(2) thin-film capacitors.Here we report a much higher dielectric permittivity of 1466 during downscaling of the capacitor into the diameter of 3.85μm when the ferroelectricity suddenly disappears without high-field cycling.The stored charge density is as high as 183μC cm^(−2) at an operating voltage/time of 1.2 V/50 ns at cycle numbers of more than 10^(12) without inducing dielectric breakdown.The study of synchrotron X-ray micro-diffraction patterns show missing of a mixed tetragonal phase.The image of electron energy loss spectroscopy shows the preferred oxygen-vacancy accumulation at the regions near top/bottom electrodes as well as grain boundaries.The ultrahigh dielectric-permittivity material enables high-density integration of extremely scaled logic and memory devices in the future.
