Biomass-derived activated carbon is a highly promising electrode material for supercapacitors.However,its widespread application is often limited by insufficient power density,stemming from low electrical conductivity...Biomass-derived activated carbon is a highly promising electrode material for supercapacitors.However,its widespread application is often limited by insufficient power density,stemming from low electrical conductivity and sluggish ionic transport.To address these challenges,we developed a difluorocarbene-grafted strategy that fluorinates surface carbonyl groups on carbon through a gassolid reaction path.This process effectively induces a redistribution of carbon atomic electron density and concurrently reconfigures the microporous-mesoporous architecture.The resultant synergistic effects significantly enhance both charge transport efficiency and ionic storage capacity.The optimized fluorinated macadamia nut shell-derived activated carbon(F-MNSAC)exhibits a remarkable compaction density of 0.64 g cm-3,an electrical conductivity of 3.34 S mm-1,and a substantial pore volume of1.213 m3g-1.The supercapacitor based on F-MNSAC delivers a higher specific capacitance(33.63 F g-1at 1 A g-1)than commercialized YP-50F(~27 F g-1at 1 A g-1),and outstanding rate capability(86.6%capacity retention at 50 A g-1).Consequently,the device achieves a high energy density of24.1 Wh kg-1at a high power density of 61.2 kW kg-1.This work establishes a new paradigm for developing high-performance carbon materials and lays a firm technological foundation for advancing nextgeneration,high-power supercapacitors.展开更多
The emerging interfacial polarization strategy exhibits applicative potential in piezoelectric enhancement.However,there is an ongoing effort to address the inherent limitations arising from charge bridging phenomena ...The emerging interfacial polarization strategy exhibits applicative potential in piezoelectric enhancement.However,there is an ongoing effort to address the inherent limitations arising from charge bridging phenomena and stochastic interface disorder that plague the improvement of piezoelectric performance.Here,we report a dual structure reinforced MXene/PVDF-TrFE piezoelectric composite,whose piezoelectricity is enhanced under the coupling effect of interfacial polarization and structural design.Synergistically,molecular dynamics simulations,density functional theory calculations and experimental validation revealed the details of interfacial interactions,which promotes the net spontaneous polarization of PVDF-TrFE from the 0.56 to 31.41 Debye.The oriented MXene distribution and porous structure not only tripled the piezoelectric response but also achieved an eightfold increase in sensitivity within the low-pressure region,along with demonstrating cyclic stability exceeding 20,000 cycles.The properties reinforcement originating from dual structure is elucidated through the finite element simulation and experimental validation.Attributed to the excellent piezoelectric response and deep learning algorithm,the sensor can effectively recognize the signals of artery pulse and finger flexion.Finally,a 3×3 sensor array is fabricated to monitor the pressure distribution wirelessly.This study provides an innovative methodology for reinforcing interfacial polarized piezoelectric materials and insight into structural designs.展开更多
Bimodal pressure sensors capable of simultaneously detecting static and dynamic forces are essential to medical detection and bio-robotics.However,conventional pressure sensors typically integrate multiple operating m...Bimodal pressure sensors capable of simultaneously detecting static and dynamic forces are essential to medical detection and bio-robotics.However,conventional pressure sensors typically integrate multiple operating mechanisms to achieve bimodal detection,leading to complex device architectures and challenges in signal decoupling.In this work,we address these limitations by leveraging the unique piezotronic effect of Y-ion-doped ZnO to develop a bimodal piezotronic sensor(BPS)with a simplified structure and enhanced sensitivity.Through a combination of finite element simulations and experimental validation,we demonstrate that the BPS can effectively monitor both dynamic and static forces,achieving an on/off ratio of 1029,a gauge factor of 23,439 and a static force response duration of up to 600 s,significantly outperforming the performance of conventional piezoelectric sensors.As a proof-of-concept,the BPS demonstrates the continuous monitoring of Achilles tendon behavior under mixed dynamic and static loading conditions.Aided by deep learning algorithms,the system achieves 96%accuracy in identifying Achilles tendon movement patterns,thus enabling warnings for dangerous movements.This work provides a viable strategy for bimodal force monitoring,highlighting its potential in wearable electronics.展开更多
Ti3CNTx MXenes with unique electrical conductivity can be widely applied for supercapacitors and electromagnetic shielding.However,its relatively low-yield quaternary nitrogen-containing Ti3AlCN ce ramics precursor(le...Ti3CNTx MXenes with unique electrical conductivity can be widely applied for supercapacitors and electromagnetic shielding.However,its relatively low-yield quaternary nitrogen-containing Ti3AlCN ce ramics precursor(less than 50%),due to the inevitable Al segregation during the synthesizing process,significantly hindered its widely commercial applications.Herein,we employed the controllable AlNoversaturation precursor strategy to precisely tune the phase transition point of quaternary Ti3AlCN ceramics to obtain high-yield Ti3 AlCN precursor for the purpose of high conductivity Ti3 CNTx MXenes.Combined energy dispersive X-ray spectrometer(XRD)with X-ray photoelectron spectroscopy(XPS)characterizations,the yield of the quaternary nitrogen-containing Ti3 AlCN ceramics was evidently proved to be up to 70%,which is 1.4 times than that of previously reported works.Such relatively highyield quaternary Ti3AlCN is mainly ascribed to the elimination of Al segregation.Based on it,we further developed accordion-like two-dimensional(2D)MXene via hydrofluoric acid etch and vacuum freezedry.This novel accordion-like 2D Ti3CNTx MXene possesses high electrochemical capacitive properties(209 F/g).Therefore,this controllable AlN-oversaturation precursor strategy will pave a way to exploit costly high-yield MAX ceramics precursor for high conductivity MXenes and also play a powerful role in promoting their practical applications including electrical and magnetic engineering fields.展开更多
2D MXene(Ti3CNTx)has been considered as the most promising electrode material for flexible supercapacitors owing to its metallic conductivity,ultra-high capacitance,and excellent flexibility.However,it suffers f...2D MXene(Ti3CNTx)has been considered as the most promising electrode material for flexible supercapacitors owing to its metallic conductivity,ultra-high capacitance,and excellent flexibility.However,it suffers from a severe restacking problem during the electrode fabrication process,limiting the ion transport kinetics and the accessibility of ions in the electrodes,especially in the direction normal to the electrode surface.Herein,we report a NH3-induced in situ etching strategy to fabricate 3D-interconnected porous MXene/carbon dots(p-MC)films for high-performance flexible supercapacitor.The pre-intercalated carbon dots(CDs)first prevent the restacking of MXene to expose more inner electrochemical active sites.The partially decomposed CDs generate NH3for in situ etching of MXene nanosheets toward 3D-interconnected p-MC films.Benefiting from the structural merits and the 3D-interconnected ionic transmission channels,p-MC film electrodes achieve excellent gravimetric capacitance(688.9 F g-1at 2 A g-1)and superior rate capability.Moreover,the optimized p-MC electrode is assembled into an asymmetric solid-state flexible supercapacitor with high energy density and superior cycling stability,demonstrating the great promise of p-MC electrode for practical applications.展开更多
Lithium-ion capacitors(LICs)are becoming important electrochemical energy storage systems due to their great potential to bridge the gap between supercapacitors and lithium-ion batteries.However,capacity lopsidedness ...Lithium-ion capacitors(LICs)are becoming important electrochemical energy storage systems due to their great potential to bridge the gap between supercapacitors and lithium-ion batteries.However,capacity lopsidedness and low output voltage greatly hinder the realization of high-energy-density LICs.Herein,a strategy of balancing capacity towards fastest dynamics is proposed to enable high-voltage LICs.Through electrochemical prelithiation of Nb2C to be 1.1 V with 165 mAh g-1,Nb2C//LiFePO4 LICs show a broadened potential window from 3.0 to 4.2 V and an according high energy density of 420 Wh kg-1.Moreover,the underlying mechanism between prelithiation and high voltage is disclosed by electrochemical dynamic analysis.Prelithiation declines the Nb2C anode potential that facilitates electron transmission in the interlayer of two-dimensional Nb2C MXene.This effect induces small drive force for Li+ions deposition and hence weakens the repulsive force from adsorbed ions on the electrode surface.Benefiting from even more Li+ions deposition,a higher voltage is eventually delivered.In addition,prelithiation significantly increases Coulomb efficiency of the 1st cycle from 74%to 90%,which is crucial to commercial application of LICs.展开更多
Carbon dots(CDs), because of their unique properties, are being rapidly developed as important luminescent materials for imaging, sensing, and use in photonic devices. However, most of the reported fundamental propert...Carbon dots(CDs), because of their unique properties, are being rapidly developed as important luminescent materials for imaging, sensing, and use in photonic devices. However, most of the reported fundamental properties of the CDs are results of investigations conducted in the solution state, which may be completely different from those conducted in the solid state. In this work, we study the luminescence properties, photostability, and the dynamics of CDs in different matrix environments, from ensemble to the single-particle level. We observed that the properties associated with the emission centers and photostability of CDs were extremely sensitive to the local chemical environment. A better understanding of the dependence of the spectroscopic properties of CDs on the complex local chemical environment is an important step toward finding new ways of controlling the optical properties of CDs and optimizing their use in various applications.展开更多
lonic-conductive solid-state polymer electrolytes are promising for the development of advanced lithium batteries yet a deeper understanding of their underlying ion-transfer mechanism is needed to improve performance....lonic-conductive solid-state polymer electrolytes are promising for the development of advanced lithium batteries yet a deeper understanding of their underlying ion-transfer mechanism is needed to improve performance.Here we demonstrate the low-enthalpy and high-entropy(LEHE)electrolytes can intrinsically generate remarkably free ions and high mobility,enabling them to efficiently drive lithium-ion storage.The LEHE electrolytes are constructed on the basis of introducing CsPbl3perovskite quantum dots(PQDs)to strengthen PEO@LiTFSI complexes.An extremely stable cycling>1000 h at 0.3 mA cm-2can be delivered by LEHE electrolytes.Also,the as-developed Li|LEHE|LiFePO4cell retains 92.3%of the initial capacity(160.7 mAh g-1)after 200 cycles.This cycling stability is ascribed to the suppressed charge concentration gradient leading to free lithium dendrites.It is realized by a dramatic increment in lithium-ion transference number(0.57 vs 0.19)and a significant decline in ion-transfer activation energy(0.14 eV vs 0.22 eV)for LEHE electrolytes comparing with PEO@LiTFSI counterpart.The CsPbl3PQDs promote highly structural disorder by inhibiting crystallization and hence endow polymer electrolytes with low melting enthalpy and high structural entropy,which in turn facilitate long-term cycling stability and excellent rate-capability of lithium-metal batteries.展开更多
Owing to the utilization of lithium metal as anode with the ultrahigh theoretical capacity density of 3860 mA h g-1and oxide-based ceramic solid-state electrolytes(SE),e.g.,garnet-type Li7La3Zr2O12(LLZO),a...Owing to the utilization of lithium metal as anode with the ultrahigh theoretical capacity density of 3860 mA h g-1and oxide-based ceramic solid-state electrolytes(SE),e.g.,garnet-type Li7La3Zr2O12(LLZO),all-state-state lithium metal batteries(ASLMBs)have been widely accepted as the promising alternatives for providing the satisfactory energy density and safety.However,its applications are still challenged by plenty of technical and scientific issues.In this contribution,the co-sintering temperature at 500℃is proved as a compromise method to fabricate the composite cathode with structural integrity and declined capacity fading of LiNi0.5Co0.2Mn0.3O2(NCM).On the other hand,it tends to form weaker grain boundary(GB)inside polycrystalline LLZO at inadequate sintering temperature for LLZO,which can induce the intergranular failure of SE during the growth of Li filament inside the unavoidable defect on the interface of SE.Therefore,increasing the strength of GB,refining the grain to 0.4μm,and precluding the interfacial defect are suggested to postpone the electro-chemo-mechanical failure of SE with weak GB.Moreover,the advanced sintering techniques to lower the co-sintering temperature for both NCM-LLZO composite cathode and LLZO SE can be posted out to realize the viability of state-of-the-art ASLMBs with higher energy density as well as the guaranteed safety.展开更多
Although the synthesis of novel nanostructured metal sulfides has been well established,further size-controllable optimization is still valuable to enhance their performance for various applications.Herein,a self-temp...Although the synthesis of novel nanostructured metal sulfides has been well established,further size-controllable optimization is still valuable to enhance their performance for various applications.Herein,a self-template method to size-controllably synthesize the hollow NiCo2S4 nanospheres is reported.Uniformly monodisperse Ni Co precursors with diameter widely ranging from 97 to 550 nm are controllably synthesized and subsequently transformed into hollow NiCo2S4 nanospheres through in situ sulfidation.Smaller nanoparticles’diameter results in the hollow NiCo2S4 nanospheres larger surface area and thinner shell thickness and hence provides much more electrochemical active sites as well as facilitate the ion and electron transfer.Consequently,the hollow NiCo2S4 nanospheres—used as the electrode materials in supercapacitors—achieve 19%enhancement of specific capacity from 484.8 to 575.1 C g-1 through lowering the 42.5%diameter of hollow NiCo2S4 nanospheres from 407 to 234 nm.Moreover,the hollow NiCo2S4 nanospheres with 234 nm diameter exhibit superior rate capacity indicated by 49%capacity retention from 1 to 50 A g-1 and excellent cycling stability(77%after 2000 cycles).Furthermore,this method is a potentially general strategy in the size-controllable synthesis of the metal sulfides hollow nanostructures and results in the remarkable electrochemical applications.展开更多
The Schrödinger equation for the 2S and 2P states of the lithium-like ions Z=5–7,9–10 is solved by using the Rayleigh-Ritz variational method in Hylleraas coordinates.The leading-order relativistic and QED corr...The Schrödinger equation for the 2S and 2P states of the lithium-like ions Z=5–7,9–10 is solved by using the Rayleigh-Ritz variational method in Hylleraas coordinates.The leading-order relativistic and QED corrections are calculated perturbatively and higher-order corrections are estimated.The transition frequencies between the 2S1/2and 2PJ(J=1/2,3/2)states are determined and compared with experimental and other theoretical results.Specifically,isotope shifts are also calculated for B2+.展开更多
Bioinspired soft robots hold great potential to perform tasks in unstructured terrains.Ferroelectric polymers are highly valued in soft robots for their flexibility,lightweight,and electrically controllable deformatio...Bioinspired soft robots hold great potential to perform tasks in unstructured terrains.Ferroelectric polymers are highly valued in soft robots for their flexibility,lightweight,and electrically controllable deformation.However,achieving large strains in ferroelectric polymers typically requires high driving voltages,posing a significant challenge for practical applications.In this study,we investigate the role of crystalline domain size in enhancing the electrostrain performance of the relaxor ferroelectric polymer poly(vinylidene fluoride-trifluoroethylene-chlorofluoroethylene-fluorinated alkynes)(P(VDFTrFE-CFE-FA)).Leveraging its remarkable inverse piezoelectric coefficient(|d33*|=701 pm V-1),we demonstrate that the planar films exhibit a five times larger bending angle than that of commercial PVDF films at low electric fields.Based on this material,we design a petal-structured soft robot that achieves a curvature of up to 4.5 cm-1 at a DC electric field of 30 Vμm-1.When integrated into a bipedal soft robot,it manifests outstanding electrostrain performance,achieving rapid locomotion of~19 body lengths per second(BL s-1)at 10 Vμm-1(560 Hz).Moreover,the developed robot demonstrates remarkable abilities in climbing slopes and carrying heavy loads.These findings open new avenues for developing low-voltage-driven soft robots with significant promise for practical applications.展开更多
Triboelectric nanogenerators (TENG), a unique technology for harvesting ambient mechanical energy based on triboelectric effect, have been proven to be a cost-effective, simple and robust approach for self-powered s...Triboelectric nanogenerators (TENG), a unique technology for harvesting ambient mechanical energy based on triboelectric effect, have been proven to be a cost-effective, simple and robust approach for self-powered systems. Here, we demonstrate a rationally designed triple-cantilever based TENG for harvesting vibration energy. With the assistance of nanowire arrays fabricated onto the surfaces of beryllium-copper alloy foils, the newly designed TENG produces an open-circuit voltage up to 101 V and a short-circuit current of 55.7 ~tA with a peak power density of 252.3 mW/m2. The TENG was systematically investigated and demonstrated as a direct power source for instantaneously lighting up 40 commercial light-emitting diodes. For the first time, a TENG device has been designed for harvesting vibration energy, especially at low frequencies, opening its application as a new energy technologv.展开更多
Piezoelectric nanofibers have received extensive attention in the field of electronic devices,but they are still restricted for further development,due to their limited dipole arrangement.Herein,we propose spatially c...Piezoelectric nanofibers have received extensive attention in the field of electronic devices,but they are still restricted for further development,due to their limited dipole arrangement.Herein,we propose spatially confined MXene/polyvinylidene fluoride(PVDF)nanofibers for piezoelectric application,with dual functions of pressure sensing and energy harvesting.The spatial confinement of MXene/PVDF nanofibers can actively induce the optimally aligned-CH2-/-CF2-dipoles of PVDF and dramatically boost spontaneous polarization for piezoelectric enhancement.The voltage and current generated by fabricated MXene/PVDF(0.8 wt%)nanofiber piezoelectric electronic devices are respectively 3.97 times and 10.1 times higher than those generated by pure PVDF nanofibers.Based on these results,the developed bifunctional electronic devices are applied to monitor various human movements and to harvest energy.Notably,the results of this work allow for the development of nanofibers with excellent piezoelectric performance using a spatial confinement mechanism.展开更多
The development of triboelectric nanogenerator(TENG)technology which can directly convert ambient mechanical energy into electric energy may affect areas from green energy harvesting to emerging wearing electronics.An...The development of triboelectric nanogenerator(TENG)technology which can directly convert ambient mechanical energy into electric energy may affect areas from green energy harvesting to emerging wearing electronics.And,the material of triboelectric layer is critical to the mechanical robustness and electrical output characteristics of the TENGs.Herein,a MXene enhanced electret polytetrafluoroethylene(PTFE)film with a high mechanical property and surface charge density is developed.The MXene/PTFE composite film was synthesized by spraying and annealing treatment.With the doping of MXene,the crystallinity of composite film could be tuned,leading to an enhancement in the tensile property of 450%and reducing the wear volume about 80%in the friction test.Furthermore,the as-fabricated TENG with this composite film outputs 397 V of open-circuit voltage,21µA of short-circuit current,and 232 nC of transfer charge quantity,which are 4,6,and 6 times higher than that of the TENG made by pure PTFE film,respectively.Therefore,this work provides a creative strategy to simultaneously improve the mechanical property and electrical performance of the TENGs,which have great potential in improving device stability under a complex mechanical environment.展开更多
Monitoring physiological signals of the human body can provide extremely important information for sports healthcare,preventing injuries and providing efficient guidance for individual sports.However,the signals relat...Monitoring physiological signals of the human body can provide extremely important information for sports healthcare,preventing injuries and providing efficient guidance for individual sports.However,the signals related to human healthcare involve both subtle and vigorous signals,making it difficult for a sensor to satisfy the full-scale monitoring at the same time.Here,a novel conductive elastomer featuring homogeneously micropyramid-structured PDMS/CNT composite is used to fabricate highperformance piezoresistive sensors by a drop-casting method.Benefiting from the significant increase in the contact area of microstructure during deformation,the flexible sensor presents a broad detection range(up to 185.5 kPa),fast responseecovery time(44/13 ms),ultrahigh sensitivity(242.4 kPa–1)and excellent durability over 8,000 cycles.As a proof of concept,the as-fabricated pressure sensor can be used for body-area sports healthcare,and enable the detection of full-scale pressure distribution.Considering the fabulous sensing performance,the sensor may potentially become promising in personal sports healthcare and telemedicine monitoring.展开更多
Respiration is a critical physiological process of the body and plays an essential role in maintaining human health.Wearable piezoelectric nanofiber-based respiratory monitoring has attracted much attention due to its...Respiration is a critical physiological process of the body and plays an essential role in maintaining human health.Wearable piezoelectric nanofiber-based respiratory monitoring has attracted much attention due to its self-power,high linearity,noninvasiveness,and convenience.However,the limited sensitivity of conventional piezoelectric nanofibers makes it difficult to meet medical and daily respiratory monitoring requirements due to their low electromechanical conversion efficiency.Here,we present a universally applicable,highly sensitive piezoelectric nanofiber characterized by a coaxial composite structure of polyvinylidene fluoride(PVDF)and carbon nanotube(CNT),which is denoted as PS-CC.Based on elucidating the enhancement mechanism from the percolation effect,PS-CC exhibits excellent sensing performance with a high sensitivity of 3.7 V/N and a fast response time of 20 ms for electromechanical conversion.As a proof-of-concept,the nanofiber membrane is seamlessly integrated into a facial mask,facilitating accurate recognition of respiratory states.With the assistance of a one-dimensional convolutional neural network(CNN),a PS-CC-based smart mask can recognize respiratory tracts and multiple breathing patterns with a classification accuracy of up to 97.8%.Notably,this work provides an effective strategy for monitoring respiratory diseases and offers widespread utility for daily health monitoring and clinical applications.展开更多
The wide-spread proliferation of aqueous MXene-based supercapacitor has been largely shadowed by the limited cell potential window(typically in the range of 0-0.6 V).To address this baffling issue,designing asymmetric...The wide-spread proliferation of aqueous MXene-based supercapacitor has been largely shadowed by the limited cell potential window(typically in the range of 0-0.6 V).To address this baffling issue,designing asymmetric supercapacitor(ASC)is proposed as a rational strategy to enlarge the potential window(thus energy density)of individual cell in aqueous electrolytes.To this date,however,it still remains a great challenge to develop easy fabricating,3D nanostructured,and pseudocapacitive cathode materials that can perfectly match with MXene anodematerials.In this work,we propose a supramolecular strategy to construct conducting polymer hydrogel(CPH)with highly interconnected 3D nanostructures and large pseudocapacitance,which can finely match with 2D Ti3C2Tx.The as-assembled CPH//Ti3C2Tx ASCwith CPH cathode and MXene anode can operate in a broadened potential window of 1.15 V in aqueous PVA/H2SO4 gel electrolyte with remarkably improved energy density of 16.6μWh/cm2(nine times higher than that of symmetric MXene supercapacitor).Additionally,this ASC exhibits outstanding cyclic stability with no trackable performance decay over 30,000 galvanostatic charge and discharge cycles.It is demonstrated in this work that employing positive CPH electrode is a feasible yet promising strategy to enhance the potential window and energy density of aqueous MXene supercapacitors.展开更多
基金supported by the National Natural Science Foundation of China(No.52372228,No.22309203)the Science and Technology Department project of Sichuan Province of China(No.2024ZYD0013)+2 种基金the China Postdoctoral Science Foundation(2024M752669)the Sichuan Science and Technology Program(No.2026NSFSC0896)the Fundamental Research Funds for the Central Universities(Grant Number:2682025CX003)。
摘要Biomass-derived activated carbon is a highly promising electrode material for supercapacitors.However,its widespread application is often limited by insufficient power density,stemming from low electrical conductivity and sluggish ionic transport.To address these challenges,we developed a difluorocarbene-grafted strategy that fluorinates surface carbonyl groups on carbon through a gassolid reaction path.This process effectively induces a redistribution of carbon atomic electron density and concurrently reconfigures the microporous-mesoporous architecture.The resultant synergistic effects significantly enhance both charge transport efficiency and ionic storage capacity.The optimized fluorinated macadamia nut shell-derived activated carbon(F-MNSAC)exhibits a remarkable compaction density of 0.64 g cm-3,an electrical conductivity of 3.34 S mm-1,and a substantial pore volume of1.213 m3g-1.The supercapacitor based on F-MNSAC delivers a higher specific capacitance(33.63 F g-1at 1 A g-1)than commercialized YP-50F(~27 F g-1at 1 A g-1),and outstanding rate capability(86.6%capacity retention at 50 A g-1).Consequently,the device achieves a high energy density of24.1 Wh kg-1at a high power density of 61.2 kW kg-1.This work establishes a new paradigm for developing high-performance carbon materials and lays a firm technological foundation for advancing nextgeneration,high-power supercapacitors.
基金supported by the National Natural Science Foundation of China(No.52303328)the Postdoctoral Innovation Talents Support Program(No.BX20220257)the Sichuan Science and Technology Program(No.2023NSFSC0313).
摘要The emerging interfacial polarization strategy exhibits applicative potential in piezoelectric enhancement.However,there is an ongoing effort to address the inherent limitations arising from charge bridging phenomena and stochastic interface disorder that plague the improvement of piezoelectric performance.Here,we report a dual structure reinforced MXene/PVDF-TrFE piezoelectric composite,whose piezoelectricity is enhanced under the coupling effect of interfacial polarization and structural design.Synergistically,molecular dynamics simulations,density functional theory calculations and experimental validation revealed the details of interfacial interactions,which promotes the net spontaneous polarization of PVDF-TrFE from the 0.56 to 31.41 Debye.The oriented MXene distribution and porous structure not only tripled the piezoelectric response but also achieved an eightfold increase in sensitivity within the low-pressure region,along with demonstrating cyclic stability exceeding 20,000 cycles.The properties reinforcement originating from dual structure is elucidated through the finite element simulation and experimental validation.Attributed to the excellent piezoelectric response and deep learning algorithm,the sensor can effectively recognize the signals of artery pulse and finger flexion.Finally,a 3×3 sensor array is fabricated to monitor the pressure distribution wirelessly.This study provides an innovative methodology for reinforcing interfacial polarized piezoelectric materials and insight into structural designs.
基金financially supported by the National Natural Science Foundation of China(No.U2330120)the Natural Science Foundation of Sichuan Province of China(No.2023NSFSC0313)the Basic Research Cultivation Project of Southwest Jiaotong University(No.2682023KJ024)。
摘要Bimodal pressure sensors capable of simultaneously detecting static and dynamic forces are essential to medical detection and bio-robotics.However,conventional pressure sensors typically integrate multiple operating mechanisms to achieve bimodal detection,leading to complex device architectures and challenges in signal decoupling.In this work,we address these limitations by leveraging the unique piezotronic effect of Y-ion-doped ZnO to develop a bimodal piezotronic sensor(BPS)with a simplified structure and enhanced sensitivity.Through a combination of finite element simulations and experimental validation,we demonstrate that the BPS can effectively monitor both dynamic and static forces,achieving an on/off ratio of 1029,a gauge factor of 23,439 and a static force response duration of up to 600 s,significantly outperforming the performance of conventional piezoelectric sensors.As a proof-of-concept,the BPS demonstrates the continuous monitoring of Achilles tendon behavior under mixed dynamic and static loading conditions.Aided by deep learning algorithms,the system achieves 96%accuracy in identifying Achilles tendon movement patterns,thus enabling warnings for dangerous movements.This work provides a viable strategy for bimodal force monitoring,highlighting its potential in wearable electronics.
基金supported by the National Natural Science Foundation of China(No.51602265)the Special Fund of China Postdoctoral Science Foundation(No.2018T110992)+1 种基金the Sichuan Science and Technology Program(No.2018RZ0074)the Cultivation Program for the Excellent Doctoral Dissertation of Southwest Jiaotong University(No.D-YB201709)。
摘要Ti3CNTx MXenes with unique electrical conductivity can be widely applied for supercapacitors and electromagnetic shielding.However,its relatively low-yield quaternary nitrogen-containing Ti3AlCN ce ramics precursor(less than 50%),due to the inevitable Al segregation during the synthesizing process,significantly hindered its widely commercial applications.Herein,we employed the controllable AlNoversaturation precursor strategy to precisely tune the phase transition point of quaternary Ti3AlCN ceramics to obtain high-yield Ti3 AlCN precursor for the purpose of high conductivity Ti3 CNTx MXenes.Combined energy dispersive X-ray spectrometer(XRD)with X-ray photoelectron spectroscopy(XPS)characterizations,the yield of the quaternary nitrogen-containing Ti3 AlCN ceramics was evidently proved to be up to 70%,which is 1.4 times than that of previously reported works.Such relatively highyield quaternary Ti3AlCN is mainly ascribed to the elimination of Al segregation.Based on it,we further developed accordion-like two-dimensional(2D)MXene via hydrofluoric acid etch and vacuum freezedry.This novel accordion-like 2D Ti3CNTx MXene possesses high electrochemical capacitive properties(209 F/g).Therefore,this controllable AlN-oversaturation precursor strategy will pave a way to exploit costly high-yield MAX ceramics precursor for high conductivity MXenes and also play a powerful role in promoting their practical applications including electrical and magnetic engineering fields.
基金The authors gratefully acknowledge financial support from the National Natural Science Foundation of China(Grant Nos.21805261 and 51972277)Sichuan Science and Technology Program(Grant Nos.2021YFG0251 and 2022YFG0293)Fundamental Research Funds for the Central Universities(Grant No.2682021CX105)。
摘要2D MXene(Ti3CNTx)has been considered as the most promising electrode material for flexible supercapacitors owing to its metallic conductivity,ultra-high capacitance,and excellent flexibility.However,it suffers from a severe restacking problem during the electrode fabrication process,limiting the ion transport kinetics and the accessibility of ions in the electrodes,especially in the direction normal to the electrode surface.Herein,we report a NH3-induced in situ etching strategy to fabricate 3D-interconnected porous MXene/carbon dots(p-MC)films for high-performance flexible supercapacitor.The pre-intercalated carbon dots(CDs)first prevent the restacking of MXene to expose more inner electrochemical active sites.The partially decomposed CDs generate NH3for in situ etching of MXene nanosheets toward 3D-interconnected p-MC films.Benefiting from the structural merits and the 3D-interconnected ionic transmission channels,p-MC film electrodes achieve excellent gravimetric capacitance(688.9 F g-1at 2 A g-1)and superior rate capability.Moreover,the optimized p-MC electrode is assembled into an asymmetric solid-state flexible supercapacitor with high energy density and superior cycling stability,demonstrating the great promise of p-MC electrode for practical applications.
基金financial supported from the National Natural Science Foundation of China (Nos. 51977185 and 51972277)the financial supported from Southwest Jiaotong University Science and Technology Rising Star Program (No. 2682021CG021)
摘要Lithium-ion capacitors(LICs)are becoming important electrochemical energy storage systems due to their great potential to bridge the gap between supercapacitors and lithium-ion batteries.However,capacity lopsidedness and low output voltage greatly hinder the realization of high-energy-density LICs.Herein,a strategy of balancing capacity towards fastest dynamics is proposed to enable high-voltage LICs.Through electrochemical prelithiation of Nb2C to be 1.1 V with 165 mAh g-1,Nb2C//LiFePO4 LICs show a broadened potential window from 3.0 to 4.2 V and an according high energy density of 420 Wh kg-1.Moreover,the underlying mechanism between prelithiation and high voltage is disclosed by electrochemical dynamic analysis.Prelithiation declines the Nb2C anode potential that facilitates electron transmission in the interlayer of two-dimensional Nb2C MXene.This effect induces small drive force for Li+ions deposition and hence weakens the repulsive force from adsorbed ions on the electrode surface.Benefiting from even more Li+ions deposition,a higher voltage is eventually delivered.In addition,prelithiation significantly increases Coulomb efficiency of the 1st cycle from 74%to 90%,which is crucial to commercial application of LICs.
基金financial support from National Natural Science Foundation of China (No.22073046)Fundamental Research Funds for the Central Universities。
摘要Carbon dots(CDs), because of their unique properties, are being rapidly developed as important luminescent materials for imaging, sensing, and use in photonic devices. However, most of the reported fundamental properties of the CDs are results of investigations conducted in the solution state, which may be completely different from those conducted in the solid state. In this work, we study the luminescence properties, photostability, and the dynamics of CDs in different matrix environments, from ensemble to the single-particle level. We observed that the properties associated with the emission centers and photostability of CDs were extremely sensitive to the local chemical environment. A better understanding of the dependence of the spectroscopic properties of CDs on the complex local chemical environment is an important step toward finding new ways of controlling the optical properties of CDs and optimizing their use in various applications.
基金the National Natural Science Foundation of China(Nos.51977185,51972277)the financial supported from Southwest Jiaotong University Science and Technology Rising Star Program(No.2682021CG021)
摘要lonic-conductive solid-state polymer electrolytes are promising for the development of advanced lithium batteries yet a deeper understanding of their underlying ion-transfer mechanism is needed to improve performance.Here we demonstrate the low-enthalpy and high-entropy(LEHE)electrolytes can intrinsically generate remarkably free ions and high mobility,enabling them to efficiently drive lithium-ion storage.The LEHE electrolytes are constructed on the basis of introducing CsPbl3perovskite quantum dots(PQDs)to strengthen PEO@LiTFSI complexes.An extremely stable cycling>1000 h at 0.3 mA cm-2can be delivered by LEHE electrolytes.Also,the as-developed Li|LEHE|LiFePO4cell retains 92.3%of the initial capacity(160.7 mAh g-1)after 200 cycles.This cycling stability is ascribed to the suppressed charge concentration gradient leading to free lithium dendrites.It is realized by a dramatic increment in lithium-ion transference number(0.57 vs 0.19)and a significant decline in ion-transfer activation energy(0.14 eV vs 0.22 eV)for LEHE electrolytes comparing with PEO@LiTFSI counterpart.The CsPbl3PQDs promote highly structural disorder by inhibiting crystallization and hence endow polymer electrolytes with low melting enthalpy and high structural entropy,which in turn facilitate long-term cycling stability and excellent rate-capability of lithium-metal batteries.
基金the National Natural Science Foundation of China(12102328)for supporting this work。
摘要Owing to the utilization of lithium metal as anode with the ultrahigh theoretical capacity density of 3860 mA h g-1and oxide-based ceramic solid-state electrolytes(SE),e.g.,garnet-type Li7La3Zr2O12(LLZO),all-state-state lithium metal batteries(ASLMBs)have been widely accepted as the promising alternatives for providing the satisfactory energy density and safety.However,its applications are still challenged by plenty of technical and scientific issues.In this contribution,the co-sintering temperature at 500℃is proved as a compromise method to fabricate the composite cathode with structural integrity and declined capacity fading of LiNi0.5Co0.2Mn0.3O2(NCM).On the other hand,it tends to form weaker grain boundary(GB)inside polycrystalline LLZO at inadequate sintering temperature for LLZO,which can induce the intergranular failure of SE during the growth of Li filament inside the unavoidable defect on the interface of SE.Therefore,increasing the strength of GB,refining the grain to 0.4μm,and precluding the interfacial defect are suggested to postpone the electro-chemo-mechanical failure of SE with weak GB.Moreover,the advanced sintering techniques to lower the co-sintering temperature for both NCM-LLZO composite cathode and LLZO SE can be posted out to realize the viability of state-of-the-art ASLMBs with higher energy density as well as the guaranteed safety.
基金supported by the National Natural Science Foundation of China(No.51602265)the Special Funding of China Postdoctoral Science Foundation(No.2018T110992)the Sichuan Science and Technology Program(No.2018RZ0074)
摘要Although the synthesis of novel nanostructured metal sulfides has been well established,further size-controllable optimization is still valuable to enhance their performance for various applications.Herein,a self-template method to size-controllably synthesize the hollow NiCo2S4 nanospheres is reported.Uniformly monodisperse Ni Co precursors with diameter widely ranging from 97 to 550 nm are controllably synthesized and subsequently transformed into hollow NiCo2S4 nanospheres through in situ sulfidation.Smaller nanoparticles’diameter results in the hollow NiCo2S4 nanospheres larger surface area and thinner shell thickness and hence provides much more electrochemical active sites as well as facilitate the ion and electron transfer.Consequently,the hollow NiCo2S4 nanospheres—used as the electrode materials in supercapacitors—achieve 19%enhancement of specific capacity from 484.8 to 575.1 C g-1 through lowering the 42.5%diameter of hollow NiCo2S4 nanospheres from 407 to 234 nm.Moreover,the hollow NiCo2S4 nanospheres with 234 nm diameter exhibit superior rate capacity indicated by 49%capacity retention from 1 to 50 A g-1 and excellent cycling stability(77%after 2000 cycles).Furthermore,this method is a potentially general strategy in the size-controllable synthesis of the metal sulfides hollow nanostructures and results in the remarkable electrochemical applications.
基金Project supported by the National Natural Science Foundation of China (Grant No. 11774080)supported by NSERC of Canada
摘要The Schrödinger equation for the 2S and 2P states of the lithium-like ions Z=5–7,9–10 is solved by using the Rayleigh-Ritz variational method in Hylleraas coordinates.The leading-order relativistic and QED corrections are calculated perturbatively and higher-order corrections are estimated.The transition frequencies between the 2S1/2and 2PJ(J=1/2,3/2)states are determined and compared with experimental and other theoretical results.Specifically,isotope shifts are also calculated for B2+.
基金National Natural Science Foundation of China,Grant/Award Number:U2330120Natural Science Foundation of Sichuan Province of China,Grant/Award Number:2023NSFSC0313Basic Research Cultivation Project of Southwest Jiaotong University,Grant/Award Number:2682023KJ024。
摘要Bioinspired soft robots hold great potential to perform tasks in unstructured terrains.Ferroelectric polymers are highly valued in soft robots for their flexibility,lightweight,and electrically controllable deformation.However,achieving large strains in ferroelectric polymers typically requires high driving voltages,posing a significant challenge for practical applications.In this study,we investigate the role of crystalline domain size in enhancing the electrostrain performance of the relaxor ferroelectric polymer poly(vinylidene fluoride-trifluoroethylene-chlorofluoroethylene-fluorinated alkynes)(P(VDFTrFE-CFE-FA)).Leveraging its remarkable inverse piezoelectric coefficient(|d33*|=701 pm V-1),we demonstrate that the planar films exhibit a five times larger bending angle than that of commercial PVDF films at low electric fields.Based on this material,we design a petal-structured soft robot that achieves a curvature of up to 4.5 cm-1 at a DC electric field of 30 Vμm-1.When integrated into a bipedal soft robot,it manifests outstanding electrostrain performance,achieving rapid locomotion of~19 body lengths per second(BL s-1)at 10 Vμm-1(560 Hz).Moreover,the developed robot demonstrates remarkable abilities in climbing slopes and carrying heavy loads.These findings open new avenues for developing low-voltage-driven soft robots with significant promise for practical applications.
基金This research was supported by the U.S. Department of Energy, Office of Basic Energy Sciences (Award No. DE-FG02-07ER46394), National Science Foundation (NSF) (No. 0946418), and the Knowledge Innovation Program of the Chinese Academy of Sciences (Grant No. KJCX2-YW-M13). Patents have been filed based on the research results presented in this manuscript.
摘要Triboelectric nanogenerators (TENG), a unique technology for harvesting ambient mechanical energy based on triboelectric effect, have been proven to be a cost-effective, simple and robust approach for self-powered systems. Here, we demonstrate a rationally designed triple-cantilever based TENG for harvesting vibration energy. With the assistance of nanowire arrays fabricated onto the surfaces of beryllium-copper alloy foils, the newly designed TENG produces an open-circuit voltage up to 101 V and a short-circuit current of 55.7 ~tA with a peak power density of 252.3 mW/m2. The TENG was systematically investigated and demonstrated as a direct power source for instantaneously lighting up 40 commercial light-emitting diodes. For the first time, a TENG device has been designed for harvesting vibration energy, especially at low frequencies, opening its application as a new energy technologv.
基金supported by the Postdoctoral Innovation Talents Support Program(No.BX20220257)the Multiple Clean Energy Harvesting System(No.YYF20223026)+2 种基金the Sichuan Science and Technology Program(No.2023NSFSC0313)a Catalyst Seeding General Grant administered by the Royal Society of New Zealand(Contract 20-UOA-035-CSG)The authors are grateful for the help from the Analysis and Testing Center of Southwest Jiaotong University.
摘要Piezoelectric nanofibers have received extensive attention in the field of electronic devices,but they are still restricted for further development,due to their limited dipole arrangement.Herein,we propose spatially confined MXene/polyvinylidene fluoride(PVDF)nanofibers for piezoelectric application,with dual functions of pressure sensing and energy harvesting.The spatial confinement of MXene/PVDF nanofibers can actively induce the optimally aligned-CH2-/-CF2-dipoles of PVDF and dramatically boost spontaneous polarization for piezoelectric enhancement.The voltage and current generated by fabricated MXene/PVDF(0.8 wt%)nanofiber piezoelectric electronic devices are respectively 3.97 times and 10.1 times higher than those generated by pure PVDF nanofibers.Based on these results,the developed bifunctional electronic devices are applied to monitor various human movements and to harvest energy.Notably,the results of this work allow for the development of nanofibers with excellent piezoelectric performance using a spatial confinement mechanism.
基金The authors thank the support of the National Natural Science Foundation of China(Nos.51922023 and 61874011)National Key Research and Development Program of China(No.2016YFA0202704)+3 种基金Beijing Talents Foundation(No.2017000021223TD04)Tribology Science Fund of State Key Laboratory of Tribology(No.SKLTKF19B02)Open Research Foundation of State Key Laboratory of Digital Manufacturing Equipment&Technology(DMETKF2020014)Young Scientific and Technological Innovation Research Team Funds of Sichuan Province(No.20CXTD0106).
摘要The development of triboelectric nanogenerator(TENG)technology which can directly convert ambient mechanical energy into electric energy may affect areas from green energy harvesting to emerging wearing electronics.And,the material of triboelectric layer is critical to the mechanical robustness and electrical output characteristics of the TENGs.Herein,a MXene enhanced electret polytetrafluoroethylene(PTFE)film with a high mechanical property and surface charge density is developed.The MXene/PTFE composite film was synthesized by spraying and annealing treatment.With the doping of MXene,the crystallinity of composite film could be tuned,leading to an enhancement in the tensile property of 450%and reducing the wear volume about 80%in the friction test.Furthermore,the as-fabricated TENG with this composite film outputs 397 V of open-circuit voltage,21µA of short-circuit current,and 232 nC of transfer charge quantity,which are 4,6,and 6 times higher than that of the TENG made by pure PTFE film,respectively.Therefore,this work provides a creative strategy to simultaneously improve the mechanical property and electrical performance of the TENGs,which have great potential in improving device stability under a complex mechanical environment.
基金This work was financially supported by the National Natural Science Foundation of China(No.61801403)the Sichuan province Foundation for Distinguished Young Team(No.20CXTD0106)the Basic Research Cultivation Project(No.2682021ZTPY004).
摘要Monitoring physiological signals of the human body can provide extremely important information for sports healthcare,preventing injuries and providing efficient guidance for individual sports.However,the signals related to human healthcare involve both subtle and vigorous signals,making it difficult for a sensor to satisfy the full-scale monitoring at the same time.Here,a novel conductive elastomer featuring homogeneously micropyramid-structured PDMS/CNT composite is used to fabricate highperformance piezoresistive sensors by a drop-casting method.Benefiting from the significant increase in the contact area of microstructure during deformation,the flexible sensor presents a broad detection range(up to 185.5 kPa),fast responseecovery time(44/13 ms),ultrahigh sensitivity(242.4 kPa–1)and excellent durability over 8,000 cycles.As a proof of concept,the as-fabricated pressure sensor can be used for body-area sports healthcare,and enable the detection of full-scale pressure distribution.Considering the fabulous sensing performance,the sensor may potentially become promising in personal sports healthcare and telemedicine monitoring.
基金supported by the Sichuan Science and Technology Program(No.2023NSFSC0313)the Basic Research Cultivation Project of Southwest Jiaotong University(No.2682023KJ024).
摘要Respiration is a critical physiological process of the body and plays an essential role in maintaining human health.Wearable piezoelectric nanofiber-based respiratory monitoring has attracted much attention due to its self-power,high linearity,noninvasiveness,and convenience.However,the limited sensitivity of conventional piezoelectric nanofibers makes it difficult to meet medical and daily respiratory monitoring requirements due to their low electromechanical conversion efficiency.Here,we present a universally applicable,highly sensitive piezoelectric nanofiber characterized by a coaxial composite structure of polyvinylidene fluoride(PVDF)and carbon nanotube(CNT),which is denoted as PS-CC.Based on elucidating the enhancement mechanism from the percolation effect,PS-CC exhibits excellent sensing performance with a high sensitivity of 3.7 V/N and a fast response time of 20 ms for electromechanical conversion.As a proof-of-concept,the nanofiber membrane is seamlessly integrated into a facial mask,facilitating accurate recognition of respiratory states.With the assistance of a one-dimensional convolutional neural network(CNN),a PS-CC-based smart mask can recognize respiratory tracts and multiple breathing patterns with a classification accuracy of up to 97.8%.Notably,this work provides an effective strategy for monitoring respiratory diseases and offers widespread utility for daily health monitoring and clinical applications.
基金National Natural Science Foundation of China,Grant/Award Numbers:51977185,51972277Sichuan Science and Technology Program,Grant/Award Numbers:20ZDYF2478,20ZDYF2833,21ZDYF3951。
摘要The wide-spread proliferation of aqueous MXene-based supercapacitor has been largely shadowed by the limited cell potential window(typically in the range of 0-0.6 V).To address this baffling issue,designing asymmetric supercapacitor(ASC)is proposed as a rational strategy to enlarge the potential window(thus energy density)of individual cell in aqueous electrolytes.To this date,however,it still remains a great challenge to develop easy fabricating,3D nanostructured,and pseudocapacitive cathode materials that can perfectly match with MXene anodematerials.In this work,we propose a supramolecular strategy to construct conducting polymer hydrogel(CPH)with highly interconnected 3D nanostructures and large pseudocapacitance,which can finely match with 2D Ti3C2Tx.The as-assembled CPH//Ti3C2Tx ASCwith CPH cathode and MXene anode can operate in a broadened potential window of 1.15 V in aqueous PVA/H2SO4 gel electrolyte with remarkably improved energy density of 16.6μWh/cm2(nine times higher than that of symmetric MXene supercapacitor).Additionally,this ASC exhibits outstanding cyclic stability with no trackable performance decay over 30,000 galvanostatic charge and discharge cycles.It is demonstrated in this work that employing positive CPH electrode is a feasible yet promising strategy to enhance the potential window and energy density of aqueous MXene supercapacitors.