Surface-enhanced Raman Spectroscopy(SERS)is a nondestructive technique for rapid detection of analytes even at the single-molecule level.However,highly sensitive and reliable SERS substrates are mostly fabricated with...Surface-enhanced Raman Spectroscopy(SERS)is a nondestructive technique for rapid detection of analytes even at the single-molecule level.However,highly sensitive and reliable SERS substrates are mostly fabricated with complex nanofabrication techniques,greatly restricting their practical applications.A convenient electrochemical method for transforming the surface of commercial gold wires/foils into silver-alloyed nanostructures is demonstrated in this report.Au substrates are treated with repetitive anodic and cathodic bias in an electrolyte of thiourea,in a one-pot one-step manner.X-rays absorption fine structure(XAFS)spectroscopy confirms that the AuAg alloy is induced at the surface.The unique AuAg alloyed surface nanostructures are particularly advantageous when served as SERS substrates,enabling a remarkably sensitive detection of Rhodamine B(a detection limit of 10^(-14)M,and uniform strong response throughout the substrates at 10^(-12)M).展开更多
The graphitic carbon nitride(g-C_3N_4) which is a two-dimensional conjugated polymer has drawn broad interdisciplinary attention as a low-cost, metal-free, and visible-light-responsive photocatalyst in the area of env...The graphitic carbon nitride(g-C_3N_4) which is a two-dimensional conjugated polymer has drawn broad interdisciplinary attention as a low-cost, metal-free, and visible-light-responsive photocatalyst in the area of environmental remediation. The g-C_3N_4-based materials have excellent electronic band structures, electron-rich properties, basic surface functionalities, high physicochemical stabilities and are ‘‘earth-abundant.'' This review summarizes the latest progress related to the design and construction of g-C_3N_4-based materials and their applications including catalysis, sensing,imaging, and white-light-emitting diodes. An outlook on possible further developments in g-C_3N_4-based research for emerging properties and applications is also included.展开更多
Solution processability and flexibility still remain major challenges for many thermoelectric(TE)materials,including bismuth telluride(Bi_(2)Te_(3)),a typical and commercially available TE material.Here,we report a ne...Solution processability and flexibility still remain major challenges for many thermoelectric(TE)materials,including bismuth telluride(Bi_(2)Te_(3)),a typical and commercially available TE material.Here,we report a new solutionprocessed method to prepare a flexible film of a Bi_(2)Te_(3)/single-walled carbon nanotube(SWCNT)hybrid,where the dissolved Bi_(2)Te_(3) ion precursors are mixed with dispersed SWCNTs in solution and recrystallized on the SWCNT surfaces to form a“cement-rebar”-like architecture.The hybrid film shows an n-type characteristic,with a stable Seebeck coefficient of^(−1)00.00±1.69μVK^(−1) in air.Furthermore,an extremely low in-plane thermal conductivity of∼0.33Wm^(−1) K^(−1) is achieved at 300 K,and the figure of merit(ZT)reaches 0.47±0.02.In addition,the TE performance is independent of mechanical bending.The unique“cement-rebar”-like architecture is believed to be responsible for the excellent TE performances and the high flexibility.The results provide a new avenue for the fabrication of solution-processable and flexible TE hybrid films and will speed up the applications of flexible electronics and energy conversion.展开更多
Based on the transverse Ising model and using decoupling approximation to the Fermi-type Green's function, we study the phase transition properties of the epitaxial ferroeleetric film with one substrate. A general re...Based on the transverse Ising model and using decoupling approximation to the Fermi-type Green's function, we study the phase transition properties of the epitaxial ferroeleetric film with one substrate. A general recursive equation of the ferroelectric thin film with two n-layer materials is obtained, which enables us to study the phase transition properties for any number layers for epitaxial ferroelectric thin film. With the help of this equation, we analyze the effect of the exchange interaction and the transverse field in the phase diagram, the influence to the polarizations and Curie temperature numerically. The results show that epitaxial ferroelectric film are able to induce a strong increase or decrease of Curie temperature to different exchange interactions and transverse fields within the epitaxial film layers. The theoretical results are in reasonable accordance with experimental data of different ferroelectric thin film.展开更多
Here,this work presents an air-stable ultrabright inverted organic lightemitting device(OLED)by using zinc ionchelated polyethylenimine(PEI)as electron injection layer.The zinc chelation is demonstrated to increase th...Here,this work presents an air-stable ultrabright inverted organic lightemitting device(OLED)by using zinc ionchelated polyethylenimine(PEI)as electron injection layer.The zinc chelation is demonstrated to increase the conductivity of the PEI by three orders of magnitude and passivate the polar amine groups.With these physicochemical properties,the inverted OLED shows a record-high external quantum efficiency of 10.0% at a high brightness of 45,610 cd m^(-2) and can deliver a maximum brightness of 121,865 cd m^(-2).Besides,the inverted OLED is also demonstrated to possess an excellent air stability(humidity,35%)with a half-brightness operating time of 541 h@1000 cd m^(-2) without any protection nor encapsulation.展开更多
A new electrochemical sensor for organophosphate pesticide(methyl-paraoxon)detection based on bifunctional cerium oxide(CeO_(2))nanozyme is here reported for the first time.Methyl-paraoxon was degraded into p-nitrophe...A new electrochemical sensor for organophosphate pesticide(methyl-paraoxon)detection based on bifunctional cerium oxide(CeO_(2))nanozyme is here reported for the first time.Methyl-paraoxon was degraded into p-nitrophenol by using CeO_(2) with phosphatase mimicking activity.The CeO_(2) nanozymemodified electrode was then synthesized to detect p-nitrophenol.Cyclic voltammetry was applied to investigate the electrochemical behavior of the modified electrode,which indicates that the signal enhancement effect may attribute to the coating of CeO_(2) nanozyme.The current research also studied and discussed the main parameters affecting the analytical signal,including accumulation potential,accumulation time,and pH.Under the optimum conditions,the present method provided a wider linear range from 0.1 to 100 mmol/L for methyl-paraoxon with a detection limit of 0.06 mmol/L.To validate the proof of concept,the electrochemical sensor was then successfully applied for the determination of methyl-paraoxon in three herb samples,i.e.,Coix lacryma-jobi,Adenophora stricta and Semen nelumbinis.Our findings may provide new insights into the application of bifunctional nanozyme in electrochemical detection of organophosphorus pesticide.展开更多
The lack of stable p-type van der Waals(vdW)semiconductors with high hole mobility severely impedes the step of low-dimensional materials entering the industrial circle.Although p-type black phosphorus(bP)and telluriu...The lack of stable p-type van der Waals(vdW)semiconductors with high hole mobility severely impedes the step of low-dimensional materials entering the industrial circle.Although p-type black phosphorus(bP)and tellurium(Te)have shown promising hole mobilities,the instability under ambient conditions of bP and relatively low hole mobility of Te remain as daunting issues.Here we report the growth of high-quality Te nanobelts on atomically flat hexagonal boron nitride(h-BN)for high-performance p-type field-effect transistors(FETs).Importantly,the Te-based FET exhibits an ultrahigh hole mobility up to 1370 cm^(2) V^(−1) s^(−1) at room temperature,that may lay the foundation for the future high-performance p-type 2D FET and metal-oxide-semiconductor(p-MOS)inverter.The vdW h-BN dielectric substrate not only provides an ultra-flat surface without dangling bonds for growth of high-quality Te nanobelts,but also reduces the scattering centers at the interface between the channel material and the dielectric layer,thus resulting in the ultrahigh hole mobility.展开更多
The construction of electrode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has gradually been an appealing and attractive technology in energy storage research field.In the present work,a fac...The construction of electrode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has gradually been an appealing and attractive technology in energy storage research field.In the present work,a facile strategy of synthesizing ultrathin amorphous/nanocrystal dual-phase P-doped Bi_(2)MoO_(6)(denoted as P-BiMO)nanosheets via a one-step wet-chemical synthesis approach is explored.Quite distinct from conventional two-dimensional(2D)nanosheets,our newly developed ultrathin P-BiMO nanosheets exhibit a unique tunable amorphous/nanocrystalline dual-phase structure with several compelling advantages including fast ion exchange ability and superb volume change buffer capability.The experimental results reveal that our prepared P-BiMO-6 electrode delivers an excellent reversible capacity of 509.6 mA·g^(−1) after continuous 1,500 cycles at the current densities of 1,500 mA·g^(−1) and improved rate performance for LIBs.In the meanwhile,the P-BiMO-6 electrode also shows a reversible capacity of 300.6 mA·g^(−1) after 100 cycles at 50 mA·g^(−1) when being used as the SIBs electrodes.This present work uncovers an effective dual-phase nanosheet structure to improve the performance of batteries,providing an attractive paradigm to develop superior electrode materials.展开更多
Lead sulfide(PbS),a typical functional semiconductor material,has attracted serious attention due to its great potential in optoelectronics applications.However,controllable growth of PbS single-crystal film still rem...Lead sulfide(PbS),a typical functional semiconductor material,has attracted serious attention due to its great potential in optoelectronics applications.However,controllable growth of PbS single-crystal film still remains a great challenge.Here,we report heteroepitaxial growth of large-scale highly crystalline PbS films on alkali salt(NaCl and KCl)substrates via chemical vapor deposition(CVD).Structural characterizations demonstrate that the as-grown PbS films exhibit an atomically sharp interface with the underlying substrates.The epitaxial relationships between the epilayers and substrates were determined to be PbS(100)//NaCl(100)or KCl(100),PbS[010]//NaCl[010]or KCl[010].Owing to the high solubility of alkali salt,the epitaxial PbS films can be rapidly released from the underlying substrates and transferred to other substrates of interest while maintaining good integrity and crystallinity,the process of which is particularly attractive in the fields of electronics and optoelectronics.Furthermore,photodetectors based on the transferred PbS films were fabricated,exhibiting a high photoresponsivity of 7.5 A/W,a detectivity of 1.44×10^(12)Jones,and a rapid response time of approximately 0.25 s.This work sheds light on the batch production,green transfer,and optoelectronic application of PbS films.展开更多
Owing to the shortcomings of traditional electrode materials in alkalimetal-ion batteries(AIBs),such as limited reversible specific capacity,low power density,and poor cycling performance,it is particularly important ...Owing to the shortcomings of traditional electrode materials in alkalimetal-ion batteries(AIBs),such as limited reversible specific capacity,low power density,and poor cycling performance,it is particularly important to develop new electrode materials.Covalent organic frameworks(COFs)are crystalline porous polymers that incorporate organic building blocks into their periodic structures through dynamic covalent bonds.COFs are superior to organic materials because of their high designability,regular channels,and stable topology.Since the first report of D_(TP)-A_(NDI)-COF as a cathode material for lithium-ion batteries in 2015,research on COF electrode materials has made continuous progress and breakthroughs.This review briefly introduces the characteristics and current challenges associated with COF electrode materials.Furthermore,we summarize the basic reaction types and active sites according to the categories of covalent bonds,including B–O,C=N,C–N,and C=C.Finally,we emphasize the perspectives on basic structure and morphology design,dimension and size design,and conductivity improvement of COFs based on the latest progress in AIBs.We believe that this review provides important guidelines for the development of high-efficiency COF electrode materials and devices for AIBs.展开更多
First principles calculations of structural, electronic, mechanical, and thermodynamic properties of different poly- morphs of BiVO4 are performed using Bender-type plane/wave ultrasoft pseudopotentials within the gen...First principles calculations of structural, electronic, mechanical, and thermodynamic properties of different poly- morphs of BiVO4 are performed using Bender-type plane/wave ultrasoft pseudopotentials within the generalized gradient approximation (GGA) in the flame of density functional theory (DFT). The calculated structural and electronic properties are consistent with the previous theoretical and experimental results. The electronic structures reveal that m-BiVO4, op- BiVO4, and st-BiVO4 have indirect band gaps, on the other hand, zt-BiVO4 has a direct band gap. From the DOS and Mulliken's charge analysis, it is observed that only m-BiVO4 has 6s2 Bi lone pair. Bond population analysis indicates that st-BiVO4 shows a more ionic nature and a similar result is obtained from the elastic properties. From the elastic prop- erties, it is observed that st-BiVO4 is more mechanically stable than the others, st-BiVO4 is more ductile and useful for high electro-optical and electro-mechanical coupling devices. Our calculated thermodynamic properties confirm the similar characteristics found from electronic and elastic properties, m-BiVO4 is useful as photocatalysts, solid state electrolyte, and electrode and other polymorphs are applicable in electronic device fabrications.展开更多
Employing cathode materials with multiple redox couples and electrolytes with efficient cation transport kinetics are two effective approaches to improving the electrochemical performance of batteries.In this work,for...Employing cathode materials with multiple redox couples and electrolytes with efficient cation transport kinetics are two effective approaches to improving the electrochemical performance of batteries.In this work,for the first time,we present a design strategy of simultaneously realizing reversible cationic and anionic redox chemistries as well as selective anion/cation transport in the viologen-based COFs(BAVCOF:X,coordinated anions of X=Cl^(-),Br^(-),I^(-),and ClO_(4)^(-))for high-performance Na-ion cathodes.Besides the cationic redox of viologen segments,the different redox activities of anions effectively tune the total capacities of the COFs.Meanwhile,electrochemical analysis and ab-initial molecular dynamics(AIMD)calculation illustrate that the anion/cation transport kinetics of electrolytes caged in the COFs'channels can be selectively tuned by the coordinated anions.As a result,combining high-potential Br-/Br_(2)redox couple,cationic redox of viologen segments,and enhanced Na+transport kinetics,the BAV-COF:Brdemonstrates stable performance with energy densities of 358.7 and 145.2 Wh kg^(-1)at power densities of 116.5 and 2124.1 W kg^(-1),respectively.This study offers new insight into the fabrication of organic cathodes with anionic redox and the advantages of COFs electrode materials in anion/cation transport selectivity for energy storage applications.展开更多
Silver nanoclusters(NCs) embedded in soda-lime glass was synthesized by the electric fieldassisted diffusion(EFAD) and successive annealing. The samples were characterized by UV-Vis absorption spectroscopy, photol...Silver nanoclusters(NCs) embedded in soda-lime glass was synthesized by the electric fieldassisted diffusion(EFAD) and successive annealing. The samples were characterized by UV-Vis absorption spectroscopy, photoluminescence spectroscopy, X-ray photoelectron spectroscopy(XPS), and lifetime measurements. The experimental results show that the growth of silver clusters is favored by the annealing temperature and dwell time. The as-diffused and annealed glass samples show photoluminescence around 550 nm under UV excitation, which can be associated with the presence of L-center and Ag3~+ cluster. And the increasing of the annealing temperature and dwell time results in an appearance of the SPR peak and the decreasing of the luminescence intensities because the Ag3~+ clusters grow up into the Ag nanoparticles.展开更多
Over the last decades,bone tissue engineering has increasingly become a research focus in the field of biomedical engineering,in which biomaterials play an important role because they can provide both biomechanical su...Over the last decades,bone tissue engineering has increasingly become a research focus in the field of biomedical engineering,in which biomaterials play an important role because they can provide both biomechanical support and osteogenic microenvironment in the process of bone regeneration.Among these biomaterials,two-dimensional(2D)nanomaterials have recently attracted considerable interest owing to their fantastic physicochemical and biological properties including great biocompatibility,excellent osteogenic capability,large specific surface area,and outstanding drug loading capacity.In this review,we summarize the state-of-the-art advances in 2D nanomaterials for bone tissue engineering.Firstly,we introduce the most explored biomaterials used in bone tissue engineering and their advantages.We then highlight the advances of cutting-edge 2D nanomaterials such as graphene and its derivatives,layered double hydroxides,black phosphorus,transition metal dichalcogenides,montmorillonite,hexagonal boron nitride,graphite phase carbon nitride,and transition metal carbonitrides(MXenes)used in bone tissue engineering.Finally,the current challenges and future prospects of 2D nanomaterials for bone tissue regeneration in process of clinical translation are discussed.展开更多
Using density functional theory, we study high hydrogenated zigzag single-walled carbon nanotubes from (7,0) to (11,0). Two structure transitions are classified: type A is a metallic transition and type B is a "...Using density functional theory, we study high hydrogenated zigzag single-walled carbon nanotubes from (7,0) to (11,0). Two structure transitions are classified: type A is a metallic transition and type B is a "semiconductive transition" according to the energy band structure. The charge density transforms only at the C-C bonds without hydrogenated sites. The sp^3 hybridization is mainly enhanced for all the C-C bonds in the vertical axial direction for type-A configurations, and the sp^3 hybridization mainly increases for all C-C bonds along the axial direction for the type-B case.展开更多
Anion-hosting cathodes capable of reversibly storing large-size anions play a leading role in dual-ion batteries(DIBs). The purpose of the present review is to summarize the most promising anion-hosting cathodes for c...Anion-hosting cathodes capable of reversibly storing large-size anions play a leading role in dual-ion batteries(DIBs). The purpose of the present review is to summarize the most promising anion-hosting cathodes for current and late-stage DIBs. This review first summarizes the developments in conventional graphite cathodes, especially the latest advances in the graphiterelated research. Next, organic cathodes for the anion storage are discussed, including aromatic amine polymers, heterocyclic polymers, bipolar compounds, and all-carbon-unsaturated compounds. Then, the review focuses on the conversion-type cathodes with high theoretical specific capacities. Finally, the future research directions of the cathodes of DIBs are proposed.展开更多
Single-molecule luminophores with dual-thermally activated delayed fluorescence(TADF)properties are receiving increasing attention.However,how to achieve these goals requires more in-depth studies.Herein,we demonstrat...Single-molecule luminophores with dual-thermally activated delayed fluorescence(TADF)properties are receiving increasing attention.However,how to achieve these goals requires more in-depth studies.Herein,we demonstrate a novel example emitter,10-(5-(2-(pyridin-3-yl)-[4,5′-bipyrimidin]-6-yl)pyridin-2-yl)-10Hphenoxazine(PmPy-PXZ),enabling dual-TADF properties due to its key feature of conformational isomerization.Introducing a pyridine bridge can greatly reduce the steric hindrance and facilitate dual-stable conformations in the ground state,where the quasi-axial(QA)forms predominate.Moreover,unlike previously reported TADF molecules with dual confirmations,both theoretical and experimental measurements show that not only the quasi-equatorial(QE)forms but also the QA forms exhibit distinct TADF characteristics,which can be attributed to an additional higher reverse intersystem crossing pathway.This is the first time that dual-TADF properties of single molecules have been achieved based on conformational isomerism.Its applications in“self-doping”organic light-emitting diode and biomedical imaging have further been investigated.All these results show the good potential of such dual-band TADF emitters based on molecular conformational isomerization.展开更多
Combining photodynamic therapy(PDT)with chemodynamic therapy(CDT)has been proven to be a promising strategy to improve the treatment efficiency of cancer,because of the synergistic therapeutic effect arising between t...Combining photodynamic therapy(PDT)with chemodynamic therapy(CDT)has been proven to be a promising strategy to improve the treatment efficiency of cancer,because of the synergistic therapeutic effect arising between the two modalities.Herein,we report an inorganic nanoagent based on ternary NiCoTi-layered double hydroxide(NiCoTi-LDH)nanosheets to realize highly efficient photodynamic/chemodynamic synergistic therapy.The NiCoTi-LDH nanosheets exhibit oxygen vacancy-promoted electron-hole separation and photogenerated holeinduced O_(2)-independent reactive oxygen species(ROS)generation under acidic circumstances,realizing in situ pH-responsive PDT.Moreover,due to the effective conversion between Co^(3+)and Co^(2+)caused by photogenerated electrons,the NiCoTi-LDH nanosheets catalyze the release of hydroxyl radicals(-OH)from H_(2)O_(2)through Fenton reactions,resulting in CDT.Laser irradiation enhances the catalyzed ability of the NiCoTi-LDH nanosheets to promote the ROS generation,resulting in a better performance than TiO_(2)nanoparticles at pH 6.5.In vitro and in vivo experimental results show conclusively that NiCoTi-LDH nanosheets plus irradiation lead to efficient cell apoptosis and significant inhibition of tumor growth.This study reports a new pH-responsive inorganic nanoagent with oxygen vacancy-promoted photodynamic/chemodynamic synergistic performance,offering a potentially appealing clinical strategy for selective tumor elimination.展开更多
Memristors have recently emerged as promising contenders for in-memory computing and artificial neural networks,attributed to their analogies to biological synapses and neurons in structural and electrical behaviors.F...Memristors have recently emerged as promising contenders for in-memory computing and artificial neural networks,attributed to their analogies to biological synapses and neurons in structural and electrical behaviors.From the diversity level,a variety of materials have been demonstrated to have great potential for memristor applications.Herein,we focus on one class of crystalline materials(CMs)-based flexible memristors with state-of-the-art experimental demonstrations.Firstly,the typical device structure and switching mechanisms are introduced.Secondly,the recent advances on CMs-based flexible memristors,including 2 D materials,metal-organic frameworks,covalent organic frameworks,and perovskites,as well as their applications for data storage and neuromorphic devices are comprehensively summarized.Finally,the future challenges and perspectives of CMs-based flexible memristors are presented.展开更多
Covalent organic frameworks(COFs)with periodic channels and tunable chemical structures have been widely considered as promising electrode materials in rechargeable batteries.However,the design and construction of hig...Covalent organic frameworks(COFs)with periodic channels and tunable chemical structures have been widely considered as promising electrode materials in rechargeable batteries.However,the design and construction of high-performance COFs-based electrodes still face some challenges in the introduction of multiple efficient redox centers as well as the reduction of dead mass.To address these issues,a unique COF containing double active centers(C═N and N═N)is developed as an anode in rechargeable lithium-ion batteries(LIBs).The as-prepared COF displays excellent electrochemical performance due to its remarkable structural stability and the existence of many active groups.Meanwhile,its electrochemical performance is significantly better than that of the small molecule compound or the linear polymer with the same construction units.Even at a high current density of 5 A/g,the LIBs with COF electrodes remain at a high discharge capacity of 227 mAh/g after 2000 cycles.Moreover,the distinction in electrochemical performances of these three materials is further revealed by calculation.This study illustrates the importance of molecular structure design for improving the performance of organic electrodes.展开更多
基金supported by Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone Shenzhen Park (Project HZQBKCZYB-2020030)National Key R&D Program of China (Project 2017YFA0204403)+2 种基金the National Natural Science Foundation of China (Project 51590892)the Major Program of Changsha Science and Technology (Project kh2003023)the Innovation and Technology Commission of HKSAR through Hong Kong Branch of National Precious Metals Material Engineering Research Centre,and the City University of Hong Kong (Project 9667207)。
文摘Surface-enhanced Raman Spectroscopy(SERS)is a nondestructive technique for rapid detection of analytes even at the single-molecule level.However,highly sensitive and reliable SERS substrates are mostly fabricated with complex nanofabrication techniques,greatly restricting their practical applications.A convenient electrochemical method for transforming the surface of commercial gold wires/foils into silver-alloyed nanostructures is demonstrated in this report.Au substrates are treated with repetitive anodic and cathodic bias in an electrolyte of thiourea,in a one-pot one-step manner.X-rays absorption fine structure(XAFS)spectroscopy confirms that the AuAg alloy is induced at the surface.The unique AuAg alloyed surface nanostructures are particularly advantageous when served as SERS substrates,enabling a remarkably sensitive detection of Rhodamine B(a detection limit of 10^(-14)M,and uniform strong response throughout the substrates at 10^(-12)M).
文摘The graphitic carbon nitride(g-C_3N_4) which is a two-dimensional conjugated polymer has drawn broad interdisciplinary attention as a low-cost, metal-free, and visible-light-responsive photocatalyst in the area of environmental remediation. The g-C_3N_4-based materials have excellent electronic band structures, electron-rich properties, basic surface functionalities, high physicochemical stabilities and are ‘‘earth-abundant.'' This review summarizes the latest progress related to the design and construction of g-C_3N_4-based materials and their applications including catalysis, sensing,imaging, and white-light-emitting diodes. An outlook on possible further developments in g-C_3N_4-based research for emerging properties and applications is also included.
基金We thank the National Natural Science Foundation of China(No.51973122)for financial support.
文摘Solution processability and flexibility still remain major challenges for many thermoelectric(TE)materials,including bismuth telluride(Bi_(2)Te_(3)),a typical and commercially available TE material.Here,we report a new solutionprocessed method to prepare a flexible film of a Bi_(2)Te_(3)/single-walled carbon nanotube(SWCNT)hybrid,where the dissolved Bi_(2)Te_(3) ion precursors are mixed with dispersed SWCNTs in solution and recrystallized on the SWCNT surfaces to form a“cement-rebar”-like architecture.The hybrid film shows an n-type characteristic,with a stable Seebeck coefficient of^(−1)00.00±1.69μVK^(−1) in air.Furthermore,an extremely low in-plane thermal conductivity of∼0.33Wm^(−1) K^(−1) is achieved at 300 K,and the figure of merit(ZT)reaches 0.47±0.02.In addition,the TE performance is independent of mechanical bending.The unique“cement-rebar”-like architecture is believed to be responsible for the excellent TE performances and the high flexibility.The results provide a new avenue for the fabrication of solution-processable and flexible TE hybrid films and will speed up the applications of flexible electronics and energy conversion.
基金Supported partly by SRF for ROCS,SEM under Grant No.20071108
文摘Based on the transverse Ising model and using decoupling approximation to the Fermi-type Green's function, we study the phase transition properties of the epitaxial ferroeleetric film with one substrate. A general recursive equation of the ferroelectric thin film with two n-layer materials is obtained, which enables us to study the phase transition properties for any number layers for epitaxial ferroelectric thin film. With the help of this equation, we analyze the effect of the exchange interaction and the transverse field in the phase diagram, the influence to the polarizations and Curie temperature numerically. The results show that epitaxial ferroelectric film are able to induce a strong increase or decrease of Curie temperature to different exchange interactions and transverse fields within the epitaxial film layers. The theoretical results are in reasonable accordance with experimental data of different ferroelectric thin film.
基金supported by the National Natural Science Foundation of China(Grant Nos.61905086,62174067,62175085)Science and Technology Development Planning of Jilin Province(Project Nos.20190101024JH,20200201296JC)+1 种基金the Hong Kong Scholars Program(Project No.XJ2020028)grants from the Research Grants Council of the Hong Kong Special Administrative Region,China(Project Nos.11300418 and 11300419).
文摘Here,this work presents an air-stable ultrabright inverted organic lightemitting device(OLED)by using zinc ionchelated polyethylenimine(PEI)as electron injection layer.The zinc chelation is demonstrated to increase the conductivity of the PEI by three orders of magnitude and passivate the polar amine groups.With these physicochemical properties,the inverted OLED shows a record-high external quantum efficiency of 10.0% at a high brightness of 45,610 cd m^(-2) and can deliver a maximum brightness of 121,865 cd m^(-2).Besides,the inverted OLED is also demonstrated to possess an excellent air stability(humidity,35%)with a half-brightness operating time of 541 h@1000 cd m^(-2) without any protection nor encapsulation.
基金This work was supported by Macao Science and Technology Development Fund(Grant No.:0147/2019/A3)Guangxi Innovation-driven Development Special Foundation Project(Project No.:GuiKe AA18118049)+1 种基金China Postdoctoral Science Foundation(Grant No.:2019M653299)the National Natural Science Foundation of China(Grant No.:81903794).
文摘A new electrochemical sensor for organophosphate pesticide(methyl-paraoxon)detection based on bifunctional cerium oxide(CeO_(2))nanozyme is here reported for the first time.Methyl-paraoxon was degraded into p-nitrophenol by using CeO_(2) with phosphatase mimicking activity.The CeO_(2) nanozymemodified electrode was then synthesized to detect p-nitrophenol.Cyclic voltammetry was applied to investigate the electrochemical behavior of the modified electrode,which indicates that the signal enhancement effect may attribute to the coating of CeO_(2) nanozyme.The current research also studied and discussed the main parameters affecting the analytical signal,including accumulation potential,accumulation time,and pH.Under the optimum conditions,the present method provided a wider linear range from 0.1 to 100 mmol/L for methyl-paraoxon with a detection limit of 0.06 mmol/L.To validate the proof of concept,the electrochemical sensor was then successfully applied for the determination of methyl-paraoxon in three herb samples,i.e.,Coix lacryma-jobi,Adenophora stricta and Semen nelumbinis.Our findings may provide new insights into the application of bifunctional nanozyme in electrochemical detection of organophosphorus pesticide.
基金supported by the financial supports from National Natural Science Foundation of China(Grant No.61904110)Young Teachers’Startup Fund for Scientific Research of Shenzhen University(Grant No.860-000002110426)+2 种基金the funding support from the National Natural Science Foundation of China(52122002)the Start-Up Grant(Project No.9610495)from City University of Hong KongECS scheme(City U 21201821)from the Research Grant Council of Hong Kong。
文摘The lack of stable p-type van der Waals(vdW)semiconductors with high hole mobility severely impedes the step of low-dimensional materials entering the industrial circle.Although p-type black phosphorus(bP)and tellurium(Te)have shown promising hole mobilities,the instability under ambient conditions of bP and relatively low hole mobility of Te remain as daunting issues.Here we report the growth of high-quality Te nanobelts on atomically flat hexagonal boron nitride(h-BN)for high-performance p-type field-effect transistors(FETs).Importantly,the Te-based FET exhibits an ultrahigh hole mobility up to 1370 cm^(2) V^(−1) s^(−1) at room temperature,that may lay the foundation for the future high-performance p-type 2D FET and metal-oxide-semiconductor(p-MOS)inverter.The vdW h-BN dielectric substrate not only provides an ultra-flat surface without dangling bonds for growth of high-quality Te nanobelts,but also reduces the scattering centers at the interface between the channel material and the dielectric layer,thus resulting in the ultrahigh hole mobility.
基金supported by Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone Shenzhen Park Project:HZQB-KCZYB-2020030the National Key R&D Program of China(Project No.2017YFA0204403)Hong Kong Innovation and Technology Commission via the Hong Kong Branch of National Precious Metals Material Engineering Research Center.
文摘The construction of electrode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has gradually been an appealing and attractive technology in energy storage research field.In the present work,a facile strategy of synthesizing ultrathin amorphous/nanocrystal dual-phase P-doped Bi_(2)MoO_(6)(denoted as P-BiMO)nanosheets via a one-step wet-chemical synthesis approach is explored.Quite distinct from conventional two-dimensional(2D)nanosheets,our newly developed ultrathin P-BiMO nanosheets exhibit a unique tunable amorphous/nanocrystalline dual-phase structure with several compelling advantages including fast ion exchange ability and superb volume change buffer capability.The experimental results reveal that our prepared P-BiMO-6 electrode delivers an excellent reversible capacity of 509.6 mA·g^(−1) after continuous 1,500 cycles at the current densities of 1,500 mA·g^(−1) and improved rate performance for LIBs.In the meanwhile,the P-BiMO-6 electrode also shows a reversible capacity of 300.6 mA·g^(−1) after 100 cycles at 50 mA·g^(−1) when being used as the SIBs electrodes.This present work uncovers an effective dual-phase nanosheet structure to improve the performance of batteries,providing an attractive paradigm to develop superior electrode materials.
基金The authors gratefully acknowledge Beijing Advanced Innovation Center for Intelligent Robots and Systems in Beijing Institute of Technology for the use of FIB and TEM.Financial support was provided by the National Natural Science Foundation of China(No.11704389)the Scientific Equipment Development Project and Youth Innovation Promotion Association Project of Chinese Academy of Sciences.
文摘Lead sulfide(PbS),a typical functional semiconductor material,has attracted serious attention due to its great potential in optoelectronics applications.However,controllable growth of PbS single-crystal film still remains a great challenge.Here,we report heteroepitaxial growth of large-scale highly crystalline PbS films on alkali salt(NaCl and KCl)substrates via chemical vapor deposition(CVD).Structural characterizations demonstrate that the as-grown PbS films exhibit an atomically sharp interface with the underlying substrates.The epitaxial relationships between the epilayers and substrates were determined to be PbS(100)//NaCl(100)or KCl(100),PbS[010]//NaCl[010]or KCl[010].Owing to the high solubility of alkali salt,the epitaxial PbS films can be rapidly released from the underlying substrates and transferred to other substrates of interest while maintaining good integrity and crystallinity,the process of which is particularly attractive in the fields of electronics and optoelectronics.Furthermore,photodetectors based on the transferred PbS films were fabricated,exhibiting a high photoresponsivity of 7.5 A/W,a detectivity of 1.44×10^(12)Jones,and a rapid response time of approximately 0.25 s.This work sheds light on the batch production,green transfer,and optoelectronic application of PbS films.
基金This work was supported by the National Natural Science Foundation of China(grant no.22179063)Q.Z.gratefully acknowledges the funding support from the City University of Hong Kong(grant nos.9380117,7005620,and 7020040)and Hong Kong Institute for Advanced Study,City University of Hong Kong,Hong Kong,China.
文摘Owing to the shortcomings of traditional electrode materials in alkalimetal-ion batteries(AIBs),such as limited reversible specific capacity,low power density,and poor cycling performance,it is particularly important to develop new electrode materials.Covalent organic frameworks(COFs)are crystalline porous polymers that incorporate organic building blocks into their periodic structures through dynamic covalent bonds.COFs are superior to organic materials because of their high designability,regular channels,and stable topology.Since the first report of D_(TP)-A_(NDI)-COF as a cathode material for lithium-ion batteries in 2015,research on COF electrode materials has made continuous progress and breakthroughs.This review briefly introduces the characteristics and current challenges associated with COF electrode materials.Furthermore,we summarize the basic reaction types and active sites according to the categories of covalent bonds,including B–O,C=N,C–N,and C=C.Finally,we emphasize the perspectives on basic structure and morphology design,dimension and size design,and conductivity improvement of COFs based on the latest progress in AIBs.We believe that this review provides important guidelines for the development of high-efficiency COF electrode materials and devices for AIBs.
文摘First principles calculations of structural, electronic, mechanical, and thermodynamic properties of different poly- morphs of BiVO4 are performed using Bender-type plane/wave ultrasoft pseudopotentials within the generalized gradient approximation (GGA) in the flame of density functional theory (DFT). The calculated structural and electronic properties are consistent with the previous theoretical and experimental results. The electronic structures reveal that m-BiVO4, op- BiVO4, and st-BiVO4 have indirect band gaps, on the other hand, zt-BiVO4 has a direct band gap. From the DOS and Mulliken's charge analysis, it is observed that only m-BiVO4 has 6s2 Bi lone pair. Bond population analysis indicates that st-BiVO4 shows a more ionic nature and a similar result is obtained from the elastic properties. From the elastic prop- erties, it is observed that st-BiVO4 is more mechanically stable than the others, st-BiVO4 is more ductile and useful for high electro-optical and electro-mechanical coupling devices. Our calculated thermodynamic properties confirm the similar characteristics found from electronic and elastic properties, m-BiVO4 is useful as photocatalysts, solid state electrolyte, and electrode and other polymorphs are applicable in electronic device fabrications.
基金supported by the NSFC/RGC Joint Research Scheme 2020/21(Project No:N_City U104/20)。
文摘Employing cathode materials with multiple redox couples and electrolytes with efficient cation transport kinetics are two effective approaches to improving the electrochemical performance of batteries.In this work,for the first time,we present a design strategy of simultaneously realizing reversible cationic and anionic redox chemistries as well as selective anion/cation transport in the viologen-based COFs(BAVCOF:X,coordinated anions of X=Cl^(-),Br^(-),I^(-),and ClO_(4)^(-))for high-performance Na-ion cathodes.Besides the cationic redox of viologen segments,the different redox activities of anions effectively tune the total capacities of the COFs.Meanwhile,electrochemical analysis and ab-initial molecular dynamics(AIMD)calculation illustrate that the anion/cation transport kinetics of electrolytes caged in the COFs'channels can be selectively tuned by the coordinated anions.As a result,combining high-potential Br-/Br_(2)redox couple,cationic redox of viologen segments,and enhanced Na+transport kinetics,the BAV-COF:Brdemonstrates stable performance with energy densities of 358.7 and 145.2 Wh kg^(-1)at power densities of 116.5 and 2124.1 W kg^(-1),respectively.This study offers new insight into the fabrication of organic cathodes with anionic redox and the advantages of COFs electrode materials in anion/cation transport selectivity for energy storage applications.
基金Funded by the Shanghai Science and Technology Committee(12nm0504700)
文摘Silver nanoclusters(NCs) embedded in soda-lime glass was synthesized by the electric fieldassisted diffusion(EFAD) and successive annealing. The samples were characterized by UV-Vis absorption spectroscopy, photoluminescence spectroscopy, X-ray photoelectron spectroscopy(XPS), and lifetime measurements. The experimental results show that the growth of silver clusters is favored by the annealing temperature and dwell time. The as-diffused and annealed glass samples show photoluminescence around 550 nm under UV excitation, which can be associated with the presence of L-center and Ag3~+ cluster. And the increasing of the annealing temperature and dwell time results in an appearance of the SPR peak and the decreasing of the luminescence intensities because the Ag3~+ clusters grow up into the Ag nanoparticles.
基金support from the National Natural Science Foundation of China(NSFC:21971007)and the Beijing Natural Science Foundation(2212044).X.W thanks the funding support from the National Natural Science Foundation of China(Grant IDs:81630064 and 81871786)and National Key R&D Program of China 2018YFF0301105.C.T.thanks the funding support from the National Natural Science Foundation of China(Project Nos.22005259 and 52122002),and the Start-Up Grant(Project No.9610495)from City University of Hong Kong.
文摘Over the last decades,bone tissue engineering has increasingly become a research focus in the field of biomedical engineering,in which biomaterials play an important role because they can provide both biomechanical support and osteogenic microenvironment in the process of bone regeneration.Among these biomaterials,two-dimensional(2D)nanomaterials have recently attracted considerable interest owing to their fantastic physicochemical and biological properties including great biocompatibility,excellent osteogenic capability,large specific surface area,and outstanding drug loading capacity.In this review,we summarize the state-of-the-art advances in 2D nanomaterials for bone tissue engineering.Firstly,we introduce the most explored biomaterials used in bone tissue engineering and their advantages.We then highlight the advances of cutting-edge 2D nanomaterials such as graphene and its derivatives,layered double hydroxides,black phosphorus,transition metal dichalcogenides,montmorillonite,hexagonal boron nitride,graphite phase carbon nitride,and transition metal carbonitrides(MXenes)used in bone tissue engineering.Finally,the current challenges and future prospects of 2D nanomaterials for bone tissue regeneration in process of clinical translation are discussed.
文摘Using density functional theory, we study high hydrogenated zigzag single-walled carbon nanotubes from (7,0) to (11,0). Two structure transitions are classified: type A is a metallic transition and type B is a "semiconductive transition" according to the energy band structure. The charge density transforms only at the C-C bonds without hydrogenated sites. The sp^3 hybridization is mainly enhanced for all the C-C bonds in the vertical axial direction for type-A configurations, and the sp^3 hybridization mainly increases for all C-C bonds along the axial direction for the type-B case.
基金the financial support from National Key R&D Program of China (2022YFB2402600)National Natural Science Foundation of China (52125105, 51972329)+4 种基金NSFC/RGC Joint Research Scheme (Project No:N_City U104/20 and52061160484)Science and Technology Planning Project of Guangdong Province (2021TQ05L894)Shenzhen Science and Technology Planning Project (JSGG20211108092801002, JSGG20220831104004008)Quality and Reform Project of Guangdong province undergraduate teaching(XQSYS-2222873)Key Scientific Research Projects of General Universities in Guangdong Province (2021KCXTD086)。
文摘Anion-hosting cathodes capable of reversibly storing large-size anions play a leading role in dual-ion batteries(DIBs). The purpose of the present review is to summarize the most promising anion-hosting cathodes for current and late-stage DIBs. This review first summarizes the developments in conventional graphite cathodes, especially the latest advances in the graphiterelated research. Next, organic cathodes for the anion storage are discussed, including aromatic amine polymers, heterocyclic polymers, bipolar compounds, and all-carbon-unsaturated compounds. Then, the review focuses on the conversion-type cathodes with high theoretical specific capacities. Finally, the future research directions of the cathodes of DIBs are proposed.
基金supported by the National Natural Science Foundation of China(grant nos.52003186,52130304,51821002,and 52003185)the National Key Research and Development Program of China(grant nos.2020YFA0714601 and 2020YFA0714604)+1 种基金the Science and Technology Project of Suzhou(grant no.ZXL2022490)the Suzhou Key Laboratory of Functional Nano&Soft Materials,the Collaborative Innovation Center of Suzhou Nano Science and Technology,and the 111 Project.
文摘Single-molecule luminophores with dual-thermally activated delayed fluorescence(TADF)properties are receiving increasing attention.However,how to achieve these goals requires more in-depth studies.Herein,we demonstrate a novel example emitter,10-(5-(2-(pyridin-3-yl)-[4,5′-bipyrimidin]-6-yl)pyridin-2-yl)-10Hphenoxazine(PmPy-PXZ),enabling dual-TADF properties due to its key feature of conformational isomerization.Introducing a pyridine bridge can greatly reduce the steric hindrance and facilitate dual-stable conformations in the ground state,where the quasi-axial(QA)forms predominate.Moreover,unlike previously reported TADF molecules with dual confirmations,both theoretical and experimental measurements show that not only the quasi-equatorial(QE)forms but also the QA forms exhibit distinct TADF characteristics,which can be attributed to an additional higher reverse intersystem crossing pathway.This is the first time that dual-TADF properties of single molecules have been achieved based on conformational isomerism.Its applications in“self-doping”organic light-emitting diode and biomedical imaging have further been investigated.All these results show the good potential of such dual-band TADF emitters based on molecular conformational isomerization.
基金National Natural Science Foundation of China(21971007)the Beijing Natural Science Foundation(2212044).C.T+1 种基金thanks the funding support from the National Natural Science Foundation of China(52122002 and 22005259)the Start-Up Grant(9610495)from City University of Hong Kong.
文摘Combining photodynamic therapy(PDT)with chemodynamic therapy(CDT)has been proven to be a promising strategy to improve the treatment efficiency of cancer,because of the synergistic therapeutic effect arising between the two modalities.Herein,we report an inorganic nanoagent based on ternary NiCoTi-layered double hydroxide(NiCoTi-LDH)nanosheets to realize highly efficient photodynamic/chemodynamic synergistic therapy.The NiCoTi-LDH nanosheets exhibit oxygen vacancy-promoted electron-hole separation and photogenerated holeinduced O_(2)-independent reactive oxygen species(ROS)generation under acidic circumstances,realizing in situ pH-responsive PDT.Moreover,due to the effective conversion between Co^(3+)and Co^(2+)caused by photogenerated electrons,the NiCoTi-LDH nanosheets catalyze the release of hydroxyl radicals(-OH)from H_(2)O_(2)through Fenton reactions,resulting in CDT.Laser irradiation enhances the catalyzed ability of the NiCoTi-LDH nanosheets to promote the ROS generation,resulting in a better performance than TiO_(2)nanoparticles at pH 6.5.In vitro and in vivo experimental results show conclusively that NiCoTi-LDH nanosheets plus irradiation lead to efficient cell apoptosis and significant inhibition of tumor growth.This study reports a new pH-responsive inorganic nanoagent with oxygen vacancy-promoted photodynamic/chemodynamic synergistic performance,offering a potentially appealing clinical strategy for selective tumor elimination.
基金the support from the starting funding of City University of Hong Kong(9380117)the 111 Project(D20015)+5 种基金the financial support from the National Natural Science Foundation of China(22008164)the Natural Science Foundation of Jiangsu Province(BK20190939)the Natural Science Foundation of Jiangsu Higher Education Institutions of China(19KJB150018)supported by the Natural Science Foundation of Jiangsu Higher Education Institutions(18KJA470004)the Six Talent Peaks Project of Jiangsu Province,China(XCL-078)Suzhou Key Laboratory for Low Dimensional Optoelectronic Materials and Devices(SZS201611)。
文摘Memristors have recently emerged as promising contenders for in-memory computing and artificial neural networks,attributed to their analogies to biological synapses and neurons in structural and electrical behaviors.From the diversity level,a variety of materials have been demonstrated to have great potential for memristor applications.Herein,we focus on one class of crystalline materials(CMs)-based flexible memristors with state-of-the-art experimental demonstrations.Firstly,the typical device structure and switching mechanisms are introduced.Secondly,the recent advances on CMs-based flexible memristors,including 2 D materials,metal-organic frameworks,covalent organic frameworks,and perovskites,as well as their applications for data storage and neuromorphic devices are comprehensively summarized.Finally,the future challenges and perspectives of CMs-based flexible memristors are presented.
基金National Natural Science Foundation of China,Grant/Award Numbers:21875206,21403187。
文摘Covalent organic frameworks(COFs)with periodic channels and tunable chemical structures have been widely considered as promising electrode materials in rechargeable batteries.However,the design and construction of high-performance COFs-based electrodes still face some challenges in the introduction of multiple efficient redox centers as well as the reduction of dead mass.To address these issues,a unique COF containing double active centers(C═N and N═N)is developed as an anode in rechargeable lithium-ion batteries(LIBs).The as-prepared COF displays excellent electrochemical performance due to its remarkable structural stability and the existence of many active groups.Meanwhile,its electrochemical performance is significantly better than that of the small molecule compound or the linear polymer with the same construction units.Even at a high current density of 5 A/g,the LIBs with COF electrodes remain at a high discharge capacity of 227 mAh/g after 2000 cycles.Moreover,the distinction in electrochemical performances of these three materials is further revealed by calculation.This study illustrates the importance of molecular structure design for improving the performance of organic electrodes.