Developing high-performance anodes for potassium ion batteries(KIBs) is of paramount significance but remains challenging.In the normal sense,electrode materials are prepared by ubiquitous wet chemical routes,which ot...Developing high-performance anodes for potassium ion batteries(KIBs) is of paramount significance but remains challenging.In the normal sense,electrode materials are prepared by ubiquitous wet chemical routes,which otherwise might not be versatile enough to create desired heterostructures and/or form clean interfacial areas for fast transport of K-ions and electrons.Along this line,rate capability/cycling stability of resulting KIBs are greatly handicapped.Herein we present an all-chemical vapor deposition approach to harness the direct synthesis of nitrogen-doped graphene(NG)/rhenium diselenide(ReSe_2)hybrids over three-dimensional MXene supports as superior heterostructure anode material for KIBs.In such an innovative design,1 T'-ReSe2 nanoparticles are sandwiched in between the NG coatings and MXene frameworks via strong interfacial interactions,thereby affording facile K~+ diffusion,enhancing overall conductivity,boosting high-power performance and reinforcing structural stability of electrodes.Thus-constructed anode delivers an excellent rate performance of 138 mAh g^(-1) at 10.0 A g^(-1) and a high reversible capacity of 90 mAh g^(-1) at 5 A g^(-1) after 300 cycles.Furthermore,the potassium storage mechanism has been systematically probed by advanced in situlex situ characterization techniques in combination with first principles computations.展开更多
A simple strategy of Cu modification was proposed to broaden the operation temperature window for NbCe catalyst.The best catalyst Cu0.010/Nb1Ce3 presented over 90%NO conversion in a wide temperature range of 200-400℃...A simple strategy of Cu modification was proposed to broaden the operation temperature window for NbCe catalyst.The best catalyst Cu0.010/Nb1Ce3 presented over 90%NO conversion in a wide temperature range of 200-400℃and exhibited an excellent H_(2)O or/and SO_(2) resistance at 275℃.To understand the promotional mechanism of Cu modification,the correlation among the"activity-structure-property"were tried to establish systematically.Cu species highly dispersed on NbCe catalyst to serve as the active component.The strong interaction among Cu,Nb and Ce promoted the emergence of NbO4 and induced more Bronsted acid sites.And Cu modification obviously enhanced the redox behavior of the NbCe catalyst.Besides,EPR probed the Cu species exited in the form of monomeric and dimeric Cu^(2+),the isolated Cu^(2+)acted as catalytic active sites to promote the reaction:Cu^(2+)-NO_(3)^(-)+NO(g)→Cu^(2+)-NO_(2)^(-)+NO_(2)(g).Then the generated NO_(2) would accelerate the fast-SCR reaction process and thus facilitated the lowtemperature deNO_(x) efficiency.Moreover,surface nitrates became unstable and easy to decompose after Cu modification,thus providing additional adsorption and activation sites for NH3,and ensuring the improvement of catalytic activity at high temperature.Since the NH3-SCR reaction followed by E-R reaction pathway efficaciously over Cu_(0.010)/Nb_(1)Ce_(3) catalyst,the excellent H_(2)O and SO_(2) resistance was as expected.展开更多
Few-layer graphene grown on Ni thin films has been studied by scanning tunneling microscopy. In most areas on the surfaces, moir′e patterns resulted from rotational stacking faults were observed. At a bias lower than...Few-layer graphene grown on Ni thin films has been studied by scanning tunneling microscopy. In most areas on the surfaces, moir′e patterns resulted from rotational stacking faults were observed. At a bias lower than 200 mV, only one sublattice shows up in regions without moir′e patterns while both sublattices are seen in regions with moir′e pattens. This phenomenon can be used to identify AB stacked regions. The scattering characteristics at various types of step edges are different from those of monolayer graphene edges, either armchair or zigzag.展开更多
The electronic Fabry–Pérot interferometer operating in the quantum Hall regime may be a promising tool for probing edge state interferences and studying the non-Abelian statistics of fractionally charged quasipa...The electronic Fabry–Pérot interferometer operating in the quantum Hall regime may be a promising tool for probing edge state interferences and studying the non-Abelian statistics of fractionally charged quasiparticles. Here we report on realizing a quantum Hall Fabry–Pérot interferometer based on monolayer graphene. We observe resistance oscillations as a function of perpendicular magnetic field and gate voltage both on the electron and hole sides. Their Coulomb-dominated origin is revealed by the positive(negative) slope of the constant phase lines in the plane of magnetic field and gate voltage on the electron(hole) side. Our work demonstrates that the graphene interferometer is feasible and paves the way for the studies of edge state interferences since high-Landau-level and even denominator fractional quantum Hall states have been found in graphene.展开更多
Optical fiber temperature sensors have been widely employed in enormous areas ranging from electric power industry,medical treatment,ocean dynamics to aerospace.Recently,graphene optical fiber temperature sensors attr...Optical fiber temperature sensors have been widely employed in enormous areas ranging from electric power industry,medical treatment,ocean dynamics to aerospace.Recently,graphene optical fiber temperature sensors attract tremendous attention for their merits of simple structure and direct power detecting ability.However,these sensors based on transfer techniques still have limitations in the relatively low sensitivity or distortion of the transmission characteristics,due to the unsuitable Fermi level of graphene and the destruction of fiber structure,respectively.Here,we propose a tunable and highly sensitive temperature sensor based on graphene photonic crystal fiber(Gr-PCF)with the non-destructive integration of graphene into the holes of PCF.This hybrid structure promises the intact fiber structure and transmission mode,which efficiently enhances the temperature detection ability of graphene.From our simulation,we find that the temperature sensitivity can be electrically tuned over four orders of magnitude and achieve up to~3.34×10^(-3) dB/(cm·℃)when the graphene Fermi level is~35 meV higher than half the incident photon energy.Additionally,this sensitivity can be further improved by~10 times through optimizing the PCF structure(such as the fiber hole diameter)to enhance the light–matter interaction.Our results provide a new way for the design of the highly sensitive temperature sensors and broaden applications in all-fiber optoelectronic devices.展开更多
The practical applications of lithium-sulfur(Li-S)battery have been greatly hindered by the severe polysulfide shuttle at the cathode and rampant lithium dendrite growth at the anode.One of the effective solutions dea...The practical applications of lithium-sulfur(Li-S)battery have been greatly hindered by the severe polysulfide shuttle at the cathode and rampant lithium dendrite growth at the anode.One of the effective solutions deals with concurrent management of both electrodes.Nevertheless,this direction remains in a nascent stage due to a lack of material selection and mechanism exploration.Herein,we devise a temperature-mediated direct chemical vapor deposition strategy to realize the controllable synthesis of three-dimensional boron/nitrogen dual-doped graphene(BNG)particulated architectures,which is employed as a light-weighted and multi-functional mediator for both electrodes in Li-S batteries.Benefiting from the“sulfiphilic”and“lithiophilic”features,the BNG modified separator not only enables boosted kinetics of polysulfide transformation to mitigate the shuttle effect but also endows uniform lithium deposition to suppress the dendritic growth.Theoretical calculations in combination with electro-kinetic tests and operando Raman analysis further elucidate the favorable sulfur and lithium electrochemistry of BNG at a molecular level.This work offers direct insight into the mediator design via controllable synthesis of graphene materials to tackle the fundamental challenges of Li-S batteries.展开更多
Being parent materials of two-dimensional (2D) crystals, van der Waals layered materials have received revived interest. In most 2D materials, the interaction between electrons is negligible. Introducing the interacti...Being parent materials of two-dimensional (2D) crystals, van der Waals layered materials have received revived interest. In most 2D materials, the interaction between electrons is negligible. Introducing the interaction can give rise to a variety of exotic properties. Here, via intercalating a van der Waals layered compound VS2, we find evidence for electron correlation by extensive magnetic, thermal, electrical, and thermoelectric characterizations. The low temperature Sommerfeld coefficient is 64 mJ·K-2·mol-1 and the Kadowaki-Woods ratio rKW^0.20a0. Both supports an enhancement of the electron correlation. The temperature dependences of the resistivity and thermopower indicate an important role played by the Kondo effect. The Kondo temperature TK is estimated to be around 8 K. Our results suggest intercalation as a potential means to engineer the electron correlation in van der Waals materials, as well as 2D materials.展开更多
Gaseous promotors have readily been adopted during the direct synthesis of graphene over insulators to enhance the growth quality and/or boost the growth rate.The understanding of the real functions of carbon-containi...Gaseous promotors have readily been adopted during the direct synthesis of graphene over insulators to enhance the growth quality and/or boost the growth rate.The understanding of the real functions of carbon-containing promotors has still remained elusive.In this study,we identify the critical roles of a representative CO_(2)promotor played in the direct growth of graphene.The comparative experimental trials validate CO_(2)as an effective modulator to decrease graphene nucleation density,improve growth kinetics,mitigate adlayer formation.The first-principles calculations illustrate that the generation of gas-phase OH species in CO_(2)-assisted system helps decrease the energy barriers of CH4 decomposition and carbon attachment to the growth front,which might be the key factor to allow high-quality direct growth.Such a CO_(2)-promoted strategy enables the conformal coating of graphene film over curved insulators,where the sheet resistance of grown graphene on quartz reaches as low as 1.26 kΩ·sq^(−1)at an optical transmittance of~95.8%.The fabricated endoscope lens based on our conformal graphene harvests an apoptosis of 82.8%for noninvasive thermal therapy.The work presented here is expected to motivate further investigations in the controllable growth of high-quality graphene on insulating substrates.展开更多
Artificial synapses and neurons are crucial milestones for neuromorphic computing hardware,and memristors with resistive and threshold switching characteristics are regarded as the most promising candidates for the co...Artificial synapses and neurons are crucial milestones for neuromorphic computing hardware,and memristors with resistive and threshold switching characteristics are regarded as the most promising candidates for the construction of hardware neural networks.However,most of the memristors can only operate in one mode,that is,resistive switching or threshold switching,and distinct memristors are required to construct fully memristive neuromorphic computing hardware,making it more complex for the fabrication and integration of the hardware.Herein,we propose a flexible dual-mode memristor array based on core–shell CsPbBr3@graphdiyne nanocrystals,which features a 100%transition yield,small cycle-to-cycle and device-to-device variability,excellent flexibility,and environmental stability.Based on this dual-mode memristor,homo-material-based fully memristive neuromorphic computing hardware—a power-free artificial nociceptive signal processing system and a spiking neural network—are constructed for the first time.Our dual-mode memristors greatly simplify the fabrication and integration of fully memristive neuromorphic systems.展开更多
Recently,graphene has drawn considerable attention in the field of electronics,owing to its favorable conductivity and high carrier mobility.Crucial to the industrialization of graphene is its high-quality microfabric...Recently,graphene has drawn considerable attention in the field of electronics,owing to its favorable conductivity and high carrier mobility.Crucial to the industrialization of graphene is its high-quality microfabrication via chemical vapor deposition.However,many problems remain in its preparation,such as the not fully understood cracking mechanism of the carbon source,the mechanism of its substrate oxidation,and insufficient defect repair theory.To help close this capability gap,this study leverages density functional theory to explore the role of O in graphene growth.The effects of Cu substrate oxidation on carbon source cracking,nucleation barriers,crystal nucleus growth,and defect repairs are discussed.OCu was found to reduce energy change during dehydrogenation,rendering the process easier.Moreover,the adsorbed O in graphene or its Cu substrate can promote defect repair and edge growth.展开更多
The chirality structure of a single-walled carbon nanotube(SWNT)strongly depends on the composition of catalyst used in the chemical vapor deposition process.In this study,we develop a porous magnesia supported mangan...The chirality structure of a single-walled carbon nanotube(SWNT)strongly depends on the composition of catalyst used in the chemical vapor deposition process.In this study,we develop a porous magnesia supported manganese-rhenium(MnRe/MgO)catalyst for chirality-selective synthesis of SWNTs.Detailed characterizations reveal that(6,5)tubes with a selectivity higher than 70%are grown from the Re-rich MnRe/MgO catalyst.By comparing the SWNT growth results with those of monometallic Mn or Re,the formation of sigma phase,an intermetallic compound occurring in transition-metal alloy systems,is revealed to be crucial for the dominant synthesis of(6,5)SWNTs.This work not only extends the application of sigma phase alloy for catalytic synthesis of SWNTs,but also sheds lights on the growth of SWNTs with a high chirality selectivity.展开更多
Tin-based compounds are deemed as suitable anode candidates affording promising sodium-ion storages for rechargeable batteries andhybrid capacitors.However,synergistically tailoring the electrical conductivity and str...Tin-based compounds are deemed as suitable anode candidates affording promising sodium-ion storages for rechargeable batteries andhybrid capacitors.However,synergistically tailoring the electrical conductivity and structural stability of tin-based anodes to attain durablesodium-ion storages remains challenging to date for its practical applications.Herein,metal-organic framework(MOF)derived SnSe/C wrappedwithin nitrogen-doped graphene(NG@SnSe/C)is designed targeting durable sodium-ion storage.NG@SnSe/C possesses favorable electricalconductivity and structure stability due to the"inner"carbon framework from the MOF thermal treatment and"outer"graphitic cage from thedirect chemical vapor deposition synthesis.Consequently,NG@SnSe/C electrode can obtain a high reversible capacity of 650 mAh·g^-1 at 0.05 A·g^1,a favorable rate performance of 287.8 mAh·g^1 at 5 A·g^1 and a superior cycle stability with a negligible capacity decay of 0.016%percycle over 3,200 cycles at 0.4 A·g^1.Theoretical calculations reveal that the nitrogen-doping in graphene can stabilize the NG@SnSe/Cstructure and improve the electrical conductivity.The reversible Na-ion storage mechanism of SnSe is further investigated by in-situ X-raydiffraction/ex-s/tu transmission electron microscopy.Furthermore,assembled sodium-ion hybrid capacitor full-cells comprising our NG@SnSe/Canode and an active carbon cathode harvest a high energy/power density of 115.5 Wh·kg^-1/5,742 W·kg^-1,holding promise for next-generationen ergy storages.展开更多
Natural biopolymers feature natural abundance,diverse chemical compositions,tunable properties,easy processability,excellent biocompatibility and biodegradability,as well as nontoxicity,providing new opportunities for...Natural biopolymers feature natural abundance,diverse chemical compositions,tunable properties,easy processability,excellent biocompatibility and biodegradability,as well as nontoxicity,providing new opportunities for the development of flexible sensing and energy devices.Generally,biopolymers are utilized as the passive and active building blocks to endow the flexible devices with mechanical robustness and good biocompatibility.This review aims to provide a comprehensive review on natural biopolymer-based sensing and energy devices.The diverse structures and fabrication processes of three typical biopolymers,including silk,cellulose,and chitin/chitosan,are presented.We review their utilities as the supporting substrates/matrix,active middle layers,separators,electrolytes,and active components of flexible sensing devices(sensors,actuators,transistors)and energy devices(batteries,supercapacitors,triboelectric nanogenerators).Finally,the remaining challenges and future research opportunities are discussed.展开更多
The booming of wearable electronics has nourished the progress on developing multifunctional energy storage systems with versatile flexibility, which enable the continuous and steady power supply even under various de...The booming of wearable electronics has nourished the progress on developing multifunctional energy storage systems with versatile flexibility, which enable the continuous and steady power supply even under various deformed states. In this sense, the synergy of flexible energy and electronic devices to construct integrative wearable microsystems is meaningful but remains quite challenging by far. Herein, we devise an innovative supercapacitor/sensor integrative wearable device that is based upon our designed vanadium nitride-graphene (VN-G) architectures. Flexible quasi-solid-state VN-G supercapacitor with ultralight and binder-free features deliver a specific capacitance of^53 F·g^-1 with good cycle stability. On the other hand, VN-G derived pressure sensors fabricated throughout a spray-printing process also manifest favorably high sensitivity (40 kPa^-1 at the range of 2-10 kPa), fast response time (~130 ms), perfect skin conformability, and outstanding stability under static and dynamic pressure conditions. In tum, their complementary unity into a self-powered wearable sensor enables the precise detecti on of physiological motions ranging from pulse rate to phonetic recognition, holding promise for in-practical health monitoring applications.展开更多
基金supported by the National Natural Science Foundation of China (51702225)the National Key Research and Development Program (2016YFA0200103)+2 种基金the Natural Science Foundation of Jiangsu Province (BK20170336)the support from Suzhou Key Laboratory for Advanced Carbon MaterialsWearable Energy Technologies, Suzhou, China。
文摘Developing high-performance anodes for potassium ion batteries(KIBs) is of paramount significance but remains challenging.In the normal sense,electrode materials are prepared by ubiquitous wet chemical routes,which otherwise might not be versatile enough to create desired heterostructures and/or form clean interfacial areas for fast transport of K-ions and electrons.Along this line,rate capability/cycling stability of resulting KIBs are greatly handicapped.Herein we present an all-chemical vapor deposition approach to harness the direct synthesis of nitrogen-doped graphene(NG)/rhenium diselenide(ReSe_2)hybrids over three-dimensional MXene supports as superior heterostructure anode material for KIBs.In such an innovative design,1 T'-ReSe2 nanoparticles are sandwiched in between the NG coatings and MXene frameworks via strong interfacial interactions,thereby affording facile K~+ diffusion,enhancing overall conductivity,boosting high-power performance and reinforcing structural stability of electrodes.Thus-constructed anode delivers an excellent rate performance of 138 mAh g^(-1) at 10.0 A g^(-1) and a high reversible capacity of 90 mAh g^(-1) at 5 A g^(-1) after 300 cycles.Furthermore,the potassium storage mechanism has been systematically probed by advanced in situlex situ characterization techniques in combination with first principles computations.
基金Financial support from the National Natural Science Foundation of China,China(Nos.21972062,21976081,21976111)。
文摘A simple strategy of Cu modification was proposed to broaden the operation temperature window for NbCe catalyst.The best catalyst Cu0.010/Nb1Ce3 presented over 90%NO conversion in a wide temperature range of 200-400℃and exhibited an excellent H_(2)O or/and SO_(2) resistance at 275℃.To understand the promotional mechanism of Cu modification,the correlation among the"activity-structure-property"were tried to establish systematically.Cu species highly dispersed on NbCe catalyst to serve as the active component.The strong interaction among Cu,Nb and Ce promoted the emergence of NbO4 and induced more Bronsted acid sites.And Cu modification obviously enhanced the redox behavior of the NbCe catalyst.Besides,EPR probed the Cu species exited in the form of monomeric and dimeric Cu^(2+),the isolated Cu^(2+)acted as catalytic active sites to promote the reaction:Cu^(2+)-NO_(3)^(-)+NO(g)→Cu^(2+)-NO_(2)^(-)+NO_(2)(g).Then the generated NO_(2) would accelerate the fast-SCR reaction process and thus facilitated the lowtemperature deNO_(x) efficiency.Moreover,surface nitrates became unstable and easy to decompose after Cu modification,thus providing additional adsorption and activation sites for NH3,and ensuring the improvement of catalytic activity at high temperature.Since the NH3-SCR reaction followed by E-R reaction pathway efficaciously over Cu_(0.010)/Nb_(1)Ce_(3) catalyst,the excellent H_(2)O and SO_(2) resistance was as expected.
基金supported by the National Basic Research Program of China(Grant No.2012CB921300)the National Natural Science Foundation of China(Grant Nos.11074005 and 91021007)the Chinese Ministry of Education
文摘Few-layer graphene grown on Ni thin films has been studied by scanning tunneling microscopy. In most areas on the surfaces, moir′e patterns resulted from rotational stacking faults were observed. At a bias lower than 200 mV, only one sublattice shows up in regions without moir′e patterns while both sublattices are seen in regions with moir′e pattens. This phenomenon can be used to identify AB stacked regions. The scattering characteristics at various types of step edges are different from those of monolayer graphene edges, either armchair or zigzag.
基金Project supported by the National Key Research and Development Program of China(Grant Nos.2016YFA0300601 and 2017YFA0303304)the National Natural Science Foundation of China(Grant Nos.11874071,11774005,and 11974026)Beijing Academy of Quantum Information Sciences,China(Grant No.Y18G22)
文摘The electronic Fabry–Pérot interferometer operating in the quantum Hall regime may be a promising tool for probing edge state interferences and studying the non-Abelian statistics of fractionally charged quasiparticles. Here we report on realizing a quantum Hall Fabry–Pérot interferometer based on monolayer graphene. We observe resistance oscillations as a function of perpendicular magnetic field and gate voltage both on the electron and hole sides. Their Coulomb-dominated origin is revealed by the positive(negative) slope of the constant phase lines in the plane of magnetic field and gate voltage on the electron(hole) side. Our work demonstrates that the graphene interferometer is feasible and paves the way for the studies of edge state interferences since high-Landau-level and even denominator fractional quantum Hall states have been found in graphene.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.52021006,52025023,51991342,and 11888101)the Key R&D Program of Guangdong Province,China(Grant Nos.2019B010931001,2020B010189001,and 2018B030327001)+6 种基金the Pearl River Talent Recruitment Program of Guangdong Province,China(Grant No.2019ZT08C321)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB33000000)Beijing Natural Science Foundation,China(Grant No.JQ19004)Beijing Municipal Science&Technology Commission,China(Grant No.Z181100004818003)the China Postdoctoral Science Foundation(Grant No.2020M680177)National Postdoctoral Program for Innovative Talents of China(Grant No.BX20190016)China Postdoctoral Science Foundation(Grant No.2019M660280).
文摘Optical fiber temperature sensors have been widely employed in enormous areas ranging from electric power industry,medical treatment,ocean dynamics to aerospace.Recently,graphene optical fiber temperature sensors attract tremendous attention for their merits of simple structure and direct power detecting ability.However,these sensors based on transfer techniques still have limitations in the relatively low sensitivity or distortion of the transmission characteristics,due to the unsuitable Fermi level of graphene and the destruction of fiber structure,respectively.Here,we propose a tunable and highly sensitive temperature sensor based on graphene photonic crystal fiber(Gr-PCF)with the non-destructive integration of graphene into the holes of PCF.This hybrid structure promises the intact fiber structure and transmission mode,which efficiently enhances the temperature detection ability of graphene.From our simulation,we find that the temperature sensitivity can be electrically tuned over four orders of magnitude and achieve up to~3.34×10^(-3) dB/(cm·℃)when the graphene Fermi level is~35 meV higher than half the incident photon energy.Additionally,this sensitivity can be further improved by~10 times through optimizing the PCF structure(such as the fiber hole diameter)to enhance the light–matter interaction.Our results provide a new way for the design of the highly sensitive temperature sensors and broaden applications in all-fiber optoelectronic devices.
基金financially supported by the National Natural Science Foundation of China(51702225)the National Key Research and Development Program(2019YFA0708201)+3 种基金the Beijing Municipal Science and Technology Commission(Z161100002116020)the China Postdoctoral Science Foundation funded project(2020 M681704,2021 T140493)the support from Suzhou Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies,Suzhou,Chinathe support from the Postdoctoral Research Foundation of Jiangsu Province。
文摘The practical applications of lithium-sulfur(Li-S)battery have been greatly hindered by the severe polysulfide shuttle at the cathode and rampant lithium dendrite growth at the anode.One of the effective solutions deals with concurrent management of both electrodes.Nevertheless,this direction remains in a nascent stage due to a lack of material selection and mechanism exploration.Herein,we devise a temperature-mediated direct chemical vapor deposition strategy to realize the controllable synthesis of three-dimensional boron/nitrogen dual-doped graphene(BNG)particulated architectures,which is employed as a light-weighted and multi-functional mediator for both electrodes in Li-S batteries.Benefiting from the“sulfiphilic”and“lithiophilic”features,the BNG modified separator not only enables boosted kinetics of polysulfide transformation to mitigate the shuttle effect but also endows uniform lithium deposition to suppress the dendritic growth.Theoretical calculations in combination with electro-kinetic tests and operando Raman analysis further elucidate the favorable sulfur and lithium electrochemistry of BNG at a molecular level.This work offers direct insight into the mediator design via controllable synthesis of graphene materials to tackle the fundamental challenges of Li-S batteries.
基金Project supported by the National Key Basic Research Program of China(Grant Nos.2013CBA01603,2016YFA0300600,and 2016YFA0300903)the National Natural Science Foundation of China(Grant Nos.11574005,11774009,11222436,and 11574283)the National Postdoctoral Program for Innovative Talents of China(Grant No.BX201700012)funded by China Postdoctoral Science Foundation.
文摘Being parent materials of two-dimensional (2D) crystals, van der Waals layered materials have received revived interest. In most 2D materials, the interaction between electrons is negligible. Introducing the interaction can give rise to a variety of exotic properties. Here, via intercalating a van der Waals layered compound VS2, we find evidence for electron correlation by extensive magnetic, thermal, electrical, and thermoelectric characterizations. The low temperature Sommerfeld coefficient is 64 mJ·K-2·mol-1 and the Kadowaki-Woods ratio rKW^0.20a0. Both supports an enhancement of the electron correlation. The temperature dependences of the resistivity and thermopower indicate an important role played by the Kondo effect. The Kondo temperature TK is estimated to be around 8 K. Our results suggest intercalation as a potential means to engineer the electron correlation in van der Waals materials, as well as 2D materials.
基金the National Key R&D Program of China(Nos.2019YFA0708201 and 2019YFA0708204)the National Natural Science Foundation of China(Nos.T2188101,61527814,and 22179089)+3 种基金the Beijing National Laboratory for Molecular Sciences(No.BNLMS-CXTD-202001)the Beijing Municipal Science and Technology Planning Project(No.Z191100000819004)the Science Fund for Distinguished Young Scholars of Jiangsu Province(No.BK20211503)the Suzhou Science and Technology Project-Prospective Application Research Program(No.SYG202038).
文摘Gaseous promotors have readily been adopted during the direct synthesis of graphene over insulators to enhance the growth quality and/or boost the growth rate.The understanding of the real functions of carbon-containing promotors has still remained elusive.In this study,we identify the critical roles of a representative CO_(2)promotor played in the direct growth of graphene.The comparative experimental trials validate CO_(2)as an effective modulator to decrease graphene nucleation density,improve growth kinetics,mitigate adlayer formation.The first-principles calculations illustrate that the generation of gas-phase OH species in CO_(2)-assisted system helps decrease the energy barriers of CH4 decomposition and carbon attachment to the growth front,which might be the key factor to allow high-quality direct growth.Such a CO_(2)-promoted strategy enables the conformal coating of graphene film over curved insulators,where the sheet resistance of grown graphene on quartz reaches as low as 1.26 kΩ·sq^(−1)at an optical transmittance of~95.8%.The fabricated endoscope lens based on our conformal graphene harvests an apoptosis of 82.8%for noninvasive thermal therapy.The work presented here is expected to motivate further investigations in the controllable growth of high-quality graphene on insulating substrates.
基金Natural Science Foundation of Tianjin City,Grant/Award Number:19JCYBJC17300National Natural Science Foundation of China,Grant/Award Numbers:21790052,51802220。
文摘Artificial synapses and neurons are crucial milestones for neuromorphic computing hardware,and memristors with resistive and threshold switching characteristics are regarded as the most promising candidates for the construction of hardware neural networks.However,most of the memristors can only operate in one mode,that is,resistive switching or threshold switching,and distinct memristors are required to construct fully memristive neuromorphic computing hardware,making it more complex for the fabrication and integration of the hardware.Herein,we propose a flexible dual-mode memristor array based on core–shell CsPbBr3@graphdiyne nanocrystals,which features a 100%transition yield,small cycle-to-cycle and device-to-device variability,excellent flexibility,and environmental stability.Based on this dual-mode memristor,homo-material-based fully memristive neuromorphic computing hardware—a power-free artificial nociceptive signal processing system and a spiking neural network—are constructed for the first time.Our dual-mode memristors greatly simplify the fabrication and integration of fully memristive neuromorphic systems.
基金the National Natural Science Foundation of China(Nos.T2188101,52021006,and 52072042)the National Natural Science Foundation Youth Fund(Nos.22105006 and 52202033)+2 种基金Beijing National Laboratory for Molecular Science(No.BNLMS-CXTD-202001)the National Key R&D Program of China(Nos.2016YFA0200101,2016YFA0200103,and 2018YFA0703502)the Beijing Municipal Science&Technology Commission(Nos.Z191100000819005,Z191100000819007,and Z201100008720005).
文摘Recently,graphene has drawn considerable attention in the field of electronics,owing to its favorable conductivity and high carrier mobility.Crucial to the industrialization of graphene is its high-quality microfabrication via chemical vapor deposition.However,many problems remain in its preparation,such as the not fully understood cracking mechanism of the carbon source,the mechanism of its substrate oxidation,and insufficient defect repair theory.To help close this capability gap,this study leverages density functional theory to explore the role of O in graphene growth.The effects of Cu substrate oxidation on carbon source cracking,nucleation barriers,crystal nucleus growth,and defect repairs are discussed.OCu was found to reduce energy change during dehydrogenation,rendering the process easier.Moreover,the adsorbed O in graphene or its Cu substrate can promote defect repair and edge growth.
基金supported by the Key Basic Research Project of Shandong Province,China(No.ZR2019ZD49)the National Natural Science Foundation of China(Nos.51972184 and 51802316)the Natural Science Foundation of Liaoning Province,China(No.2020-MS-009).
文摘The chirality structure of a single-walled carbon nanotube(SWNT)strongly depends on the composition of catalyst used in the chemical vapor deposition process.In this study,we develop a porous magnesia supported manganese-rhenium(MnRe/MgO)catalyst for chirality-selective synthesis of SWNTs.Detailed characterizations reveal that(6,5)tubes with a selectivity higher than 70%are grown from the Re-rich MnRe/MgO catalyst.By comparing the SWNT growth results with those of monometallic Mn or Re,the formation of sigma phase,an intermetallic compound occurring in transition-metal alloy systems,is revealed to be crucial for the dominant synthesis of(6,5)SWNTs.This work not only extends the application of sigma phase alloy for catalytic synthesis of SWNTs,but also sheds lights on the growth of SWNTs with a high chirality selectivity.
基金Acknowledgements This work was financially supported by the National Basic Research Program of China (Nos. 2013CB932603, 2012CB933404, 2011CB921903, and 2013CB934600), the National Natural Science Foundation of China (Nos. 51432002, 51290272, 51121091, 51~201, and 11222434), the Ministry of Education (No. 20120001130010) and the Beijing Municipal Sdence and Technology Planning Project (No. Z151100003315013).
基金This work was supported by the National Natural Science Foundation of China(No.51702225)the National Key Research and Development Program(No.2016YFA0200103)Natural Science Foundation of Jiangsu Province(No.BK20170336).C.L.,乙乙L.,Z.X.,H.N.C.,Y.Z.S.,L.H.Y.,W.J.Y.,J.Y.S.,and Z.F.L.acknowledge the support from Suzhou Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies,Suzhou,China.
文摘Tin-based compounds are deemed as suitable anode candidates affording promising sodium-ion storages for rechargeable batteries andhybrid capacitors.However,synergistically tailoring the electrical conductivity and structural stability of tin-based anodes to attain durablesodium-ion storages remains challenging to date for its practical applications.Herein,metal-organic framework(MOF)derived SnSe/C wrappedwithin nitrogen-doped graphene(NG@SnSe/C)is designed targeting durable sodium-ion storage.NG@SnSe/C possesses favorable electricalconductivity and structure stability due to the"inner"carbon framework from the MOF thermal treatment and"outer"graphitic cage from thedirect chemical vapor deposition synthesis.Consequently,NG@SnSe/C electrode can obtain a high reversible capacity of 650 mAh·g^-1 at 0.05 A·g^1,a favorable rate performance of 287.8 mAh·g^1 at 5 A·g^1 and a superior cycle stability with a negligible capacity decay of 0.016%percycle over 3,200 cycles at 0.4 A·g^1.Theoretical calculations reveal that the nitrogen-doping in graphene can stabilize the NG@SnSe/Cstructure and improve the electrical conductivity.The reversible Na-ion storage mechanism of SnSe is further investigated by in-situ X-raydiffraction/ex-s/tu transmission electron microscopy.Furthermore,assembled sodium-ion hybrid capacitor full-cells comprising our NG@SnSe/Canode and an active carbon cathode harvest a high energy/power density of 115.5 Wh·kg^-1/5,742 W·kg^-1,holding promise for next-generationen ergy storages.
基金supported by the National Basic Research Program of China(No.2016YFA0200103)the National Natural Science Foundation of China(Nos.51520105003,51432002,51672153 and 21975141)the China Postdoctoral Science Foundation(No.2019M660322).
文摘Natural biopolymers feature natural abundance,diverse chemical compositions,tunable properties,easy processability,excellent biocompatibility and biodegradability,as well as nontoxicity,providing new opportunities for the development of flexible sensing and energy devices.Generally,biopolymers are utilized as the passive and active building blocks to endow the flexible devices with mechanical robustness and good biocompatibility.This review aims to provide a comprehensive review on natural biopolymer-based sensing and energy devices.The diverse structures and fabrication processes of three typical biopolymers,including silk,cellulose,and chitin/chitosan,are presented.We review their utilities as the supporting substrates/matrix,active middle layers,separators,electrolytes,and active components of flexible sensing devices(sensors,actuators,transistors)and energy devices(batteries,supercapacitors,triboelectric nanogenerators).Finally,the remaining challenges and future research opportunities are discussed.
基金This work was supported by the National Basic Research Program of China (Nos. 2015CB932500 and 2013CB632702) and the National Natural Science Foundation of China (No. 51302141). H. W. acknowledges the support from the 1000 Youth Talents Plan of China.
基金This work was financially supported by the National Natural Science Foundation of China (Nos. 81000441, 21222303, and 21173004), the National Basic Research Program of China (Nos. 2014CB932500), and National Program for Support of Top-Notch Young Professionals.
基金the National Key Research and Development Program of China (No. 2016YFA0200103)the National Natural Science Foundation of China (Nos. 51702225, 21473119, 51675275, 51520105003, and 51432002)Jiangsu Youth Science Foundation (BK20170336).
文摘The booming of wearable electronics has nourished the progress on developing multifunctional energy storage systems with versatile flexibility, which enable the continuous and steady power supply even under various deformed states. In this sense, the synergy of flexible energy and electronic devices to construct integrative wearable microsystems is meaningful but remains quite challenging by far. Herein, we devise an innovative supercapacitor/sensor integrative wearable device that is based upon our designed vanadium nitride-graphene (VN-G) architectures. Flexible quasi-solid-state VN-G supercapacitor with ultralight and binder-free features deliver a specific capacitance of^53 F·g^-1 with good cycle stability. On the other hand, VN-G derived pressure sensors fabricated throughout a spray-printing process also manifest favorably high sensitivity (40 kPa^-1 at the range of 2-10 kPa), fast response time (~130 ms), perfect skin conformability, and outstanding stability under static and dynamic pressure conditions. In tum, their complementary unity into a self-powered wearable sensor enables the precise detecti on of physiological motions ranging from pulse rate to phonetic recognition, holding promise for in-practical health monitoring applications.
基金This work was financially supported by the National Basic Research Program of China (Nos. 2016YFA0200103, 2013CB932603, 2012CB933404, and 2013CB934600), the National Natural Science Foundation of China (Nos. 51520105003 and 51432002), the Ministry of Education (No. 20120001130010), and the Beijing Municipal Science and Technology Planning Project (No. Z151100003315013).