The development of effective and safe vehicles to deliver small interfering RNA(siRNA) and chemotherapeutics remains a major challenge in RNA interference-based combination therapy with chemotherapeutics,which has eme...The development of effective and safe vehicles to deliver small interfering RNA(siRNA) and chemotherapeutics remains a major challenge in RNA interference-based combination therapy with chemotherapeutics,which has emerged as a powerful platform to treat drug-resistant cancer cells.Herein,we describe the development of novel all-in-one fluorescent silicon nanoparticles(SiNPs)-based nanomedicine platform for imaging-guided co-delivery of siRNA and doxorubicin(DOX).This approach enhanced therapeutic efficacy in multidrug-resistant breast cancer cells(i.e.,MCF-7/ADR cells).Typically,the SiNP-based nanocarriers enhanced the stability of siRNA in a biological environment(i.e.,medium or RNase A) and imparted the responsive release behavior of siRNA,resulting in approximately 80% down-regulation of P-glycoprotein expression.Co-delivery of P-glycoprotein siRNA and DOX led to>35-fold decrease in the half maximal inhibitory concentration of DOX in comparison with free DOX,indicating the pronounced therapeutic efficiency of the resultant nanocomposites for drug-resistant breast cancer cells.The intracellular time-dependent release behaviors of siRNA and DOX were revealed through tracking the strong and stable fluorescence of SiNPs.These data provide valuable information for designing effective RNA interference-based co-delivery carriers.展开更多
The development of electrocatalysts for the oxygen reduction reaction(ORR) that bears high selectivity,exceptional activity,and long-term stability is crucial for advancing various green energy technologies.Intermetal...The development of electrocatalysts for the oxygen reduction reaction(ORR) that bears high selectivity,exceptional activity,and long-term stability is crucial for advancing various green energy technologies.Intermetallics composed of platinum and transition metals are considered to be promising candidates for this purpose.However,they typically face challenges such as unfavorable intrinsic activity and a propensity for particle aggregation,diminishing their ORR performance.Against this backdrop,we present our findings on a N-doped carbon confined Pt_(3)Co intermetallic doped with p-block metal tin(Pt_(3)Co_(x)Sn_(1-x)/NC).The introduction of Sn induces lattice strain due to its larger atomic size,which leads to the distortion of the Pt_(3)Co lattice structure,while the coupling of carbon polyhedra inhibits the particle aggregation.The optimized Pt_(3)Co_(0.8)Sn_(0.2)/NC catalyst demonstrates an impressive half-wave potential of 0.86 V versus RHE,surpassing both Pt_(3)Co/NC and Pt_(3)Sn/NC catalysts.Moreover,the Pt_(3)Co_(0.8)Sn_(0.2)/NC exhibits a mass-specific activity as high as 1.4 A mg_(Pt)^(-1),ranking it in the top level among the intermetallicsbased ORR electrocatalysts.When further employed as a cathode material in a self-assembled zinc-air battery,it shows stable operation for over 80 h.These results underscore the significant impact of lattice strain engineering through the strategic doping of p-block metal in the carbon-confined Pt_(3)Co intermetallic,thereby enhancing the catalytic efficiency for the ORR.展开更多
Organic field-effect transistors(OFETs) based on organic micro-/nanocrystals have been widely reported with charge carrier mobility exceeding 1.0 cm^2V^(-1)s^(-1), demonstrating great potential for high-performance, l...Organic field-effect transistors(OFETs) based on organic micro-/nanocrystals have been widely reported with charge carrier mobility exceeding 1.0 cm^2V^(-1)s^(-1), demonstrating great potential for high-performance, low-cost organic electronic applications. However, fabrication of large-area organic micro-/nanocrystal arrays with consistent crystal growth direction has posed a significant technical challenge. Here, we describe a solution-processed dip-coating technique to grow large-area, aligned 9,10-bis(phenylethynyl) anthracene(BPEA) and 6,13-bis(triisopropylsilylethynyl) pentacene(TIPSPEN) single-crystalline nanoribbon arrays. The method is scalable to a 5 9 10 cm^2 wafer substrate, with around 60% of the wafer surface covered by aligned crystals. The quality of crystals can be easily controlled by tuning the dip-coating speed. Furthermore, OFETs based on well-aligned BPEA and TIPS-PEN single-crystalline nanoribbons were constructed.By optimizing channel lengths and using appropriate metallic electrodes, the BPEA and TIPS-PEN-based OFETs showed hole mobility exceeding 2.0 cm^2V^(-1)s^(-1)(average mobility 1.2 cm^2V^(-1)s^(-1)) and 3.0 cm^2V^(-1)s^(-1)(average mobility2.0 cm^2V^(-1)s^(-1)), respectively. They both have a high on/off ratio(I_(on)/I_(off))>10~9. The performance can well satisfy the requirements for light-emitting diodes driving.展开更多
Continuous deforming always leads to the performance degradation of a flexible triboelectric nanogenerator due to the Young’s modulus mismatch of different functional layers.In this work,we fabricated a fiber-shaped ...Continuous deforming always leads to the performance degradation of a flexible triboelectric nanogenerator due to the Young’s modulus mismatch of different functional layers.In this work,we fabricated a fiber-shaped stretchable and tailorable triboelectric nanogenerator(FST-TENG)based on the geometric construction of a steel wire as electrode and ingenious selection of silicone rubber as triboelectric layer.Owing to the great robustness and continuous conductivity,the FST-TENGs demonstrate high stability,stretchability,and even tailorability.For a single device with ~6 cm in length and ~3 mm in diameter,the open-circuit voltage of ~59.7 V,transferred charge of ~23.7 nC,short-circuit current of ~2.67 μA and average power of ~2.13 μW can be obtained at 2.5 Hz.By knitting several FST-TENGs to be a fabric or a bracelet,it enables to harvest human motion energy and then to drive a wearable electronic device.Finally,it can also be woven on dorsum of glove to monitor the movements of gesture,which can recognize every single finger,different bending angle,and numbers of bent finger by analyzing voltage signals.展开更多
Due to the negative roles of tumor microenvironment(TME)in compromising therapeutic responses of various cancer therapies,it is expected that modulation of TME may be able to enhance the therapeutic responses during c...Due to the negative roles of tumor microenvironment(TME)in compromising therapeutic responses of various cancer therapies,it is expected that modulation of TME may be able to enhance the therapeutic responses during cancer treatment.Herein,we develop a concise strategy to prepare pH-responsive nanoparticles via the CaCO3-assisted double emulsion method,thereby enabling effective co-encapsulation of both doxorubicin(DOX),an immunogenic cell death(ICD)inducer,and alkylated NLG919(aNLG919),an inhibitor of indoleamine 2,3-dioxygenase 1(IDO1).The obtained DOX/aNLG919-loaded CaCO3 nanoparticles(DNCaNPs)are able to cause effective ICD of cancer cells and at the same time restrict the production of immunosuppressive kynurenine by inhibiting IDO1.Upon intravenous injection,such DNCaNPs show efficient tumor accumulation,improved tumor penetration of therapeutics and neutralization of acidic TME.As a result,those DNCaNPs can elicit effective anti-tumor immune responses featured in increased density of tumor-infiltrating CD8+cytotoxic T cells as well as depletion of immunosuppressive regulatory T cells(Tregs),thus effectively suppressing the growth of subcutaneous CT26 and orthotopic 4T1 tumors on the Balb/c mice through combined chemotherapy&immunotherapy.This study presents a compendious strategy for construction of pH-responsive nanoparticles,endowing significantly enhanced chemo-immunotherapy of cancer by overcoming the immunosuppressive TME.展开更多
Electrochemical CO_(2)reduction to value-added fuels and chemicals is recognized as a promising strategy to alleviate energy shortages and global warming owing to its high efficiency and economic feasibility.Recently,...Electrochemical CO_(2)reduction to value-added fuels and chemicals is recognized as a promising strategy to alleviate energy shortages and global warming owing to its high efficiency and economic feasibility.Recently,understanding the activity origin,selectivity regulation,and reaction mechanisms of CO_(2)reduction reactions(CO_(2)RRs)has become the focus of efficient electrocatalyst design.Polyoxometalates(POMs),a unique class of nanosized metal-oxo clusters,are promising candidates for the development of efficient CO_(2)RR electrocatalysts and,owing to their well-defined structure,remarkable electron/proton storage and transfer ability,and capacities for adsorption and activation of CO_(2),are ideal models for investigating the activity origin and reaction mechanisms of CO_(2)RR electrocatalysts.In this review,we focus on the activity origin and mechanism of CO_(2)RRs and survey recent advances that were achieved by employing POMs in electrocatalytic CO_(2)RRs.We highlight the significant roles of POMs in the electrocatalytic CO_(2)RR process and the main factors influencing selectivity regulation and catalytic CO_(2)RR performance,including the electrolyte,electron-transfer process,and surface characteristics.Finally,we offer a perspective of the advantages and future challenges of POM-based materials in electrocatalytic CO_(2)reduction that could inform new advancements in this promising research field.展开更多
Lithium–sulfur(Li–S)battery with a new configuration is demonstrated by inserting a flexible nitrogen-doping carbon nanofiber(N-CNFs)interlayer between the sulfur cathode and the separator.The N-CNFs film with high ...Lithium–sulfur(Li–S)battery with a new configuration is demonstrated by inserting a flexible nitrogen-doping carbon nanofiber(N-CNFs)interlayer between the sulfur cathode and the separator.The N-CNFs film with high surface roughness and surface area is fabricated by electrospinning and a subsequent calcination process.The N-CNFs film interlayer not only effectively traps the shuttling migration of polysulfides but also gives the whole battery reliable electronic conductivity,which can effectively enhance the electrochemical performance of Li–S batteries.Finally,Li–S batteries with long cycling stability of 785 mAh/g after 200 cycles and good rate capability of 573 mAh/g at 5 C are achieved.展开更多
Due to the quantum size effect and other unique photoelectric properties,quantum dots(QDs)have attracted tremendous interest in nanoscience,leading a lot of milestone works.Meantime,the scope and scientific connotatio...Due to the quantum size effect and other unique photoelectric properties,quantum dots(QDs)have attracted tremendous interest in nanoscience,leading a lot of milestone works.Meantime,the scope and scientific connotation of QDs are constantly expanding,which demonstrated amazing development vitality.Besides the well-developed Cd-containing Ⅱ-Ⅵ semiconductors,QDs of environmentally friendly Ⅰ-Ⅲ-Ⅵ(Ⅰ=Cu,Ag;Ⅲ=Ga,In;Ⅵ=S,Se)chalcogenides have been a hot spot in the QDs family,which are different from traditional Ⅱ-Ⅵ QDs in terms of multi-composition,complex defect structure,synthetic chemistry and optical properties,bringing a series of new laws,new phenomena and new challenges.The composition of Ⅰ-Ⅲ-Ⅵ chalcogenides and their solid solutions can be adjusted within a very large range while the anion framework remains stable,giving them excellent capability of photoelectric property manipulation.The important features of Ⅰ-Ⅲ-Ⅵ QDs include wide-range bandgap tuning,large Stokes shift and long photoluminescence(PL)lifetime,which are crucial for biological,optoelectronic and energy applications.This is due to the coexistence of two or more metal cations leading to a large number of intrinsic defects within the crystal lattice also known as deep-donor-acceptor states,besides the commonly observed surface defects in all QDs.However,a profound understanding of their structure and optoelectronic properties remains a huge challenge with many key issues unclear.On one hand,the achievements and experience of traditional QD research are expected to provide vital value for further development of Ⅰ-Ⅲ-Ⅵ QDs.On the other hand,the understanding of the emerging new QDs,such as carbon and other 2D materials,are even more challenging because of the dramatically different composition and structure from Ⅱ-Ⅵ semiconductors.For this,Ⅰ-Ⅲ-Ⅵ QDs,as a close relative to Ⅱ-Ⅵ QDs but with much more complex composition and structure variation,provide a great opportunity as a gradual bridge to make up the big gap between traditional QDs and emerging new QDs,such as carbon dots.Here,we hope to compare the research progress of Ⅰ-Ⅲ-Ⅵ QDs and Ⅱ-Ⅵ QDs,in an effort to comprehensively understand their structure,synthetic chemistry,optical electronic and photocatalytic properties.We further give insights on the key potential issues of Ⅰ-Ⅲ-Ⅵ QDs from the perspective of bridging between traditional QDs and emerging carbon dots,especially the profound principles behind synthetic chemistry,PL mechanism and optoelectronic applications.展开更多
We present a straightforward physical approach for synthesizing multiwalled carbon nanotubes(CNTs)-Pd Au/Pt trimetallic nanoparticles(NPs), which allows predesign and control of the metal compositional ratio by simply...We present a straightforward physical approach for synthesizing multiwalled carbon nanotubes(CNTs)-Pd Au/Pt trimetallic nanoparticles(NPs), which allows predesign and control of the metal compositional ratio by simply adjusting the sputtering targets and conditions. The small-sized CNTs-Pd Au/Pt NPs(~3 nm, Pd/Au/Pt ratio of 3:1:2) act as nanocatalysts for the methanol oxidationreaction(MOR), showing excellent performance with electrocatalytic peak current of 4.4 A mg^(-1) Pt and high stability over 7000 s. The electrocatalytic activity and stability of the Pd Au/Pt trimetallic NPs are much superior to those of the corresponding Pd/Pt and Au/Pt bimetallic NPs,as well as a commercial Pt/C catalyst. Systematic investigation of the microscopic, crystalline, and electronic structure of the Pd Au/Pt NPs reveals alloying and charge redistribution in the Pd Au/Pt NPs, which are responsible for the promotion of the electrocatalytic performance.展开更多
Polymeric organic battery materials are promising alternatives to the transition-metal-based ones owing to their enriched chemistries. However, the flammability of organic compounds brings in serious concern on batter...Polymeric organic battery materials are promising alternatives to the transition-metal-based ones owing to their enriched chemistries. However, the flammability of organic compounds brings in serious concern on battery safety. In addition to use flame-retarding electrolyte/electrolyte additives or battery separators,flame retardancy can readily be achieved through the integration of flame-retarding unit into the polymer backbone, imparting the flame retardancy permanently. The as-designed polymer based on phenothiazine shows significantly shortened self-extinguished time without deteriorating its intrinsic thermodynamic and electrochemical properties. Moreover, two electron per phenothiazine molecule is realized for the first time in a highly reversible manner with discharge voltages of 3.52 V and 4.16 V versus Li+/Li and an average capacity of ca. 120 mAh g-1 at a current rate of 2 C. The origin of the reversibility is investigated through density functional theory(DFT) calculations. These findings address the importance of molecular design for safer and more stable organic materials for batteries.展开更多
With the arrival of intelligent terminals,triboelectric nanogenerators,as a new kind of energy converter,are considered one of the most important technologies for the next generation of intelligent electronics.As a se...With the arrival of intelligent terminals,triboelectric nanogenerators,as a new kind of energy converter,are considered one of the most important technologies for the next generation of intelligent electronics.As a self-powered sensor,it can greatly reduce the power consumption of the entire sensing system by transforming external mechanical energy to electricity.However,the fabrication method of triboelectric sensors largely determines their functionality and performance.This review provides an overview of various methods used to fabricate triboelectric sensors,with a focus on the processes of micro-electro-mechanical systems technology,three-dimensional printing,textile methods,template-assisted methods,and material synthesis methods for manufacturing.The working mechanisms and suitable application scenarios of various methods are outlined.Subsequently,the advantages and disadvantages of various methods are summarized,and reference schemes for the subsequent application of these methods are included.Finally,the opportunities and challenges faced by different methods are discussed,as well as their potential for application in various intelligent systems in the Internet of Things.展开更多
Looking toward world technology trends over the next few decades, self-powered sensing networks are a key field of technological and economic driver for global industries. Since 2006, Zhong Lin Wang's group has pr...Looking toward world technology trends over the next few decades, self-powered sensing networks are a key field of technological and economic driver for global industries. Since 2006, Zhong Lin Wang's group has proposed a novel concept of nanogenerators(NGs), including piezoelectric nanogenerator and triboelectric nanogenerator, which could convert a mechanical trigger into an electric output. Considering motion ubiquitously exists in the surrounding environment and for any most common materials used every day, NGs could be inherently served as an energy source for our daily increasing requirements or as one of self-powered environmental sensors. In this regard, by coupling the piezoelectric or triboelectric properties with semiconducting gas sensing characterization, a new research field of self-powered gas sensing has been proposed. Recent works have shown promising concept to realize NG-based self-powered gas sensors that are capable of detecting gas environment without the need of external power sources to activate the gas sensors or to actively generate a readout signal. Compared with conventional sensors, these self-powered gas sensors keep the approximate performance.Meanwhile, these sensors drastically reduce power consumption and additionally reduce the required space for integration,which are significantly suitable for the wearable devices. This paper gives a brief summary about the establishment and latest progress in the fundamental principle, updated progress and potential applications of NG-based self-powered gas sensing system. The development trend in this field is envisaged, and the basic configurations are also introduced.展开更多
Photoelectrochemical hydrogen generation is a promising approach to address the environmental pollution and energy crisis.In this work,we present a hybridized mechanical and solar energy-driven selfpowered hydrogen pr...Photoelectrochemical hydrogen generation is a promising approach to address the environmental pollution and energy crisis.In this work,we present a hybridized mechanical and solar energy-driven selfpowered hydrogen production system.A rotatory disc-shaped triboelectric nanogenerator was employed to harvest mechanical energy from water and functions as a su cient external power source.WO3/BiVO4 heterojunction photoanode was synthesized in a PEC water-splitting cell to produce H2.After transformation and rectification,the peak current reaches 0.1 m A at the rotation speed of 60 rpm.In this case,the H2 evolution process only occurs with sunlight irradiation.When the rotation speed is over 130 rpm,the peak photocurrent and peak dark current have nearly equal value.Direct electrolysis of water is almost simultaneous with photoelectrocatalysis of water.It is worth noting that the hydrogen production rate increases to 5.45 and 7.27μL min-1 without or with light illumination at 160 rpm.The corresponding energy conversion e ciency is calculated to be 2.43%and 2.59%,respectively.All the results demonstrate such a self-powered system can successfully achieve the PEC hydrogen generation,exhibiting promising possibility of energy conversion.展开更多
Traditional triboelectric tactile sensors based on solid–solid interface have illustrated promising application prospects through optimization approach.However,the poor sensitivity and reliability caused by hard cont...Traditional triboelectric tactile sensors based on solid–solid interface have illustrated promising application prospects through optimization approach.However,the poor sensitivity and reliability caused by hard contact-electrification still poses challenges for the practical applications.In this work,a liquid–solid interface ferrofluid-based triboelectric tactile sensor(FTTS)with ultrahigh sensitivity is proposed.Relying on the fluidity and magnetism of ferrofluid,the topography of microstructure can be flexibly adjusted by directly employing ferrofluid as triboelectric material and controlling the position of outward magnet.To date,an ultrahigh sensitivity of 21.48 k Pa;for the triboelectric sensors can be achieved due to the high spike microstructure,low Young’s modulus of ferrofluid and efficient solid–liquid interface contact-electrification.The detection limit of FTTS of 1.25 Pa with a wide detection range to 390 k Pa was also obtained.In addition,the oleophobic property between ferrofluid and poly-tetra-fluoro-ethylene triboelectric layer can greatly reduce the wear and tear,resulting in the great improvement of stability.Finally,a strategy for personalized password lock with high security level has been demonstrated,illustrating a great perspective for practical application in smart home,artificial intelligence,Internet of things,etc.展开更多
Efficient and durable oxygen evolution reaction(OER)requires the electrocatalyst to bear abundant active sites,optimized electronic structure as well as robust component and mechanical stability.Herein,a bimetallic la...Efficient and durable oxygen evolution reaction(OER)requires the electrocatalyst to bear abundant active sites,optimized electronic structure as well as robust component and mechanical stability.Herein,a bimetallic lanthanum-nickel oxysulfide with rich oxygen vacancies based on the La_(2)O_(2)S prototype is fabricated as a binder-free precatalyst for alkaline OER.The combination of advanced in situ and ex situ characterizations with theoretical calculation uncovers the synergistic effect among La,Ni,O,and S species during OER,which assures the adsorption and stabilization of the oxyanion SO_(4)^(2-)onto the surface of the deeply reconstructed porous heterostructure composed of confining Ni OOH nanodomains by La(OH)_3 barrier.Such coupling,confinement,porosity and immobilization enable notable improvement in active site accessibility,phase stability,mass diffusion capability and the intrinsic Gibbs free energy of oxygen-containing intermediates.The optimized electrocatalyst delivers exceptional alkaline OER activity and durability,outperforming most of the Ni-based benchmark OER electrocatalysts.展开更多
Sulfurized polyacrylonitrile(SPAN)represents a unique class of cathode material for lithium sulfur(Li-S)batteries as it eradicates the polysulfides shuttling issue in carbonate-based electrolyte.However,due to the ess...Sulfurized polyacrylonitrile(SPAN)represents a unique class of cathode material for lithium sulfur(Li-S)batteries as it eradicates the polysulfides shuttling issue in carbonate-based electrolyte.However,due to the essential chemical S-linking and organic nature of SPAN,the active mass percentage and rate capability are two bottleneck issues preventing its ultimate deployment outside of laboratories.In the current work,aiming to endow both the charge conductivity and catalytic activity to SPAN for maximizing the redox kinetics of S conversion,a freestanding nanofibrous SPAN cathode embedding conductive CNTs and atomically dispersed Co centers is fabricated via multivariate electrospinning.While the CNTs enable dramatically enhancing the fiber conductivity and generating mesoscopic porosity for facilitating charge and mass transportation,the cross-linking of SPAN by Co-N_(4) S motifs creates extra charge conduction pathways and further serves as the catalytic active sites for expediting redox S conversion.As a result,an extraordinary Li-SPAN performance is achieved with a high specific capacity up to 1856 mAh g^(-1)@0.2 C,a superb rate capability up to 10 C,and an ultra-long battery life up to 1500 cycles@1 C.Consequently,our study here provides insights into the adoption of coordination chemistry to maximize the sulfur utilization by ensuring a more complete redox conversion from SPAN to Li2 S,and vice versa.展开更多
Carbon dots(CDs),as a unique zero-dimensional member of carbon materials,have attracted numerous attentions for their potential applications in optoelectronic,biological,and energy related fields.Recently,CDs as catal...Carbon dots(CDs),as a unique zero-dimensional member of carbon materials,have attracted numerous attentions for their potential applications in optoelectronic,biological,and energy related fields.Recently,CDs as catalysts for energy conversion reactions under multi-physical conditions such as light and/or electricity have grown into a research frontier due to their advantages of high visible light utilization,fast migration of charge carriers,efficient surface redox reactions and good electrical conductivity.In this review,we summarize the fabrication methods of CDs and corresponding CD nanocomposites,including the strategies of surface modification and heteroatom doping.The properties of CDs that concerned to the photo-and electro-catalysis are highlighted and detailed corresponding applications are listed.More importantly,as new non-contact detection technologies,transient photo-induced voltage/current have been developed to detect and study the charge transfer kinetics,which can sensitively reflect the complex electron separation and transfer behavior in photo-/electro-catalysts.The development and application of the techniques are reviewed.Finally,we discuss and outline the major challenges and opportunities for future CD-based catalysts,and the needs and expectations for the development of novel characterization technologies.展开更多
Hematite is regarded as a promising photoanode for photoelectrochemical(PEC) water splitting.However,the charge recombination occurred at the interface of FTO/hematite strictly limits the PEC performance of hematite.H...Hematite is regarded as a promising photoanode for photoelectrochemical(PEC) water splitting.However,the charge recombination occurred at the interface of FTO/hematite strictly limits the PEC performance of hematite.Herein,we reported a Ti3C2 MXene underlayer modified hematite(Ti-Fe2O3) photoanode via a simple drop-casting followed by hydrothermal and annealing processes.Owing to the bifunctional role of Ti3C2 MXene underlayer in improving the interfacial properties of FTO/hematite and providing Ti source for the construction of Fe2 TiO5/Fe2O3 heterostructure in hematite nanostructure,the bulk and interfacial charge transfer dynamics of hematite are significantly enhanced,and consequently enhancing the PEC performance.Compared with the pristine hematite,the as-prepared Ti-Fe2O3 photoanode shows an increased photocurrent density from 0.80 mA/cm^(2) to 1.30 mA/cm^(2) at 1.23 V vs.RHE.Moreover,a further promoted PEC performance including a dramatically increased photocurrent density of 2.49 mA/cm^(2) at1.23 V vs.RHE and an obviously lowered onset potential is achieved for the Ti-Fe2O3 sample after the subsequent surface F-treatment and the loading of FeNiOOH cocatalyst.Such results suggest that the introduction of Ti3C2 MXene underlayer is a facile but effective approach to improve the PEC water splitting activity of hematite.展开更多
Seawater photoelectrolysis is showing huge potential in green energy conversion field,yet it is still a formidable challenge to develop one catalyst that can drive the electrolysis reaction stably,economically and eff...Seawater photoelectrolysis is showing huge potential in green energy conversion field,yet it is still a formidable challenge to develop one catalyst that can drive the electrolysis reaction stably,economically and efficiently.Motivated by this point,the inorganic–organic hybridization strategy is proposed to insitu construct one hierarchical electrode via concurrent electroless plating and polymerization,which assures the growth of boron-modulated nickel–cobalt oxyhydroxide nanoballs and photosensitive polyaniline nanochains on the self-supporting Ti-based foil(B-Co Ni OOH/PANI@TiO_(2)/Ti).Upon inducing photoelectric effect(PEE),the designed target electrode delivers overpotentials as low as 196 and 398 mV at 100 mA cm^(-2)for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),respectively,corresponding to an activity enhancement by about 15%as compared to those without PEE.Inspiringly,when served as bifunctional electrocatalysts for overall seawater electrolysis,it can stably maintain at 200 mA cm^(-2)with negligible decay over 72 h.Further analysis reveals that the exceptional catalytic performance can be credit to the B-CoNiOOH,polyaniline(PANI)and TiO_(2)subunit coupling-induced physically and chemically synergistic catalysis effect such as admirable composition stability,photoelectric function and adhesion capability.The finding in this contribution may trigger much more broad interest to the novel hybrid catalysts consisting of photosensitive polymer and transition metal-based electrocatalysts.展开更多
Efficient electrocatalysts for hydrogen evolution reaction(HER) in alkaline solution are highly required for water splitting.Here we design an ultra-small PtOx nanoparticle with hybrid Pt chemical states on carbon nan...Efficient electrocatalysts for hydrogen evolution reaction(HER) in alkaline solution are highly required for water splitting.Here we design an ultra-small PtOx nanoparticle with hybrid Pt chemical states on carbon nanotubes as highly efficient alkaline HER catalyst,which shows a low overpotential of 19.4 mV at 10 mA cm^(-2),a high mass activity of 5.56 A mg_(Pt)^(-1) at 0.1 V, and a stable durability for at least 20 h.The HER performance is better than that of the benchmark 20 wt% Pt/C while the Pt content in the catalyst is only about one tenth of that in Pt/C.It also represents one of the best catalysts ever reported for HER in alkaline solution.Synchrotron radiation X-ray absorption spectroscopy reveals that the efficient and stable alkaline HER performance can be attributed to the favorable design of hybrid chemical states of Pt with carbon nanotubes,which exhibits abundant surface Pt-O as active catalytic sites and forms stable Pt-C interfacial interaction to both anchor the NPs and improve the synergistic effect between catalyst and substrate.展开更多
基金financial support from the National Basic Research Program of China(973 Program,2013CB934400)the National Natural Science Foundation of China(Nos.21825402,31400860,21575096,and 21605109)+3 种基金the Natural Science Foundation of Jiangsu Province of China(BK20170061)a Project funded by Collaborative Innovation Center of Suzhou Nano Science&Technology(NANO-CIC)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)the 111 Project as well as Joint International Research Laboratory of Carbon-Based Functional Materials and Devices
文摘The development of effective and safe vehicles to deliver small interfering RNA(siRNA) and chemotherapeutics remains a major challenge in RNA interference-based combination therapy with chemotherapeutics,which has emerged as a powerful platform to treat drug-resistant cancer cells.Herein,we describe the development of novel all-in-one fluorescent silicon nanoparticles(SiNPs)-based nanomedicine platform for imaging-guided co-delivery of siRNA and doxorubicin(DOX).This approach enhanced therapeutic efficacy in multidrug-resistant breast cancer cells(i.e.,MCF-7/ADR cells).Typically,the SiNP-based nanocarriers enhanced the stability of siRNA in a biological environment(i.e.,medium or RNase A) and imparted the responsive release behavior of siRNA,resulting in approximately 80% down-regulation of P-glycoprotein expression.Co-delivery of P-glycoprotein siRNA and DOX led to>35-fold decrease in the half maximal inhibitory concentration of DOX in comparison with free DOX,indicating the pronounced therapeutic efficiency of the resultant nanocomposites for drug-resistant breast cancer cells.The intracellular time-dependent release behaviors of siRNA and DOX were revealed through tracking the strong and stable fluorescence of SiNPs.These data provide valuable information for designing effective RNA interference-based co-delivery carriers.
基金Natural Science Foundation of Jiangsu Province (BK20210735)National Natural Science Foundation of China (52201269, 52302296)+4 种基金Collaborative Innovation Center of Suzhou Nano Science and Technologythe 111 Projectthe Suzhou Key Laboratory of Functional Nano and Soft MaterialsJiangsu Key Laboratory for Carbon-Based Functional Materials & Devicesthe funding from the Gusu leading talent plan for scientific and technological innovation and entrepreneurship (ZXL2022487)。
文摘The development of electrocatalysts for the oxygen reduction reaction(ORR) that bears high selectivity,exceptional activity,and long-term stability is crucial for advancing various green energy technologies.Intermetallics composed of platinum and transition metals are considered to be promising candidates for this purpose.However,they typically face challenges such as unfavorable intrinsic activity and a propensity for particle aggregation,diminishing their ORR performance.Against this backdrop,we present our findings on a N-doped carbon confined Pt_(3)Co intermetallic doped with p-block metal tin(Pt_(3)Co_(x)Sn_(1-x)/NC).The introduction of Sn induces lattice strain due to its larger atomic size,which leads to the distortion of the Pt_(3)Co lattice structure,while the coupling of carbon polyhedra inhibits the particle aggregation.The optimized Pt_(3)Co_(0.8)Sn_(0.2)/NC catalyst demonstrates an impressive half-wave potential of 0.86 V versus RHE,surpassing both Pt_(3)Co/NC and Pt_(3)Sn/NC catalysts.Moreover,the Pt_(3)Co_(0.8)Sn_(0.2)/NC exhibits a mass-specific activity as high as 1.4 A mg_(Pt)^(-1),ranking it in the top level among the intermetallicsbased ORR electrocatalysts.When further employed as a cathode material in a self-assembled zinc-air battery,it shows stable operation for over 80 h.These results underscore the significant impact of lattice strain engineering through the strategic doping of p-block metal in the carbon-confined Pt_(3)Co intermetallic,thereby enhancing the catalytic efficiency for the ORR.
基金supported by the National Basic Research Program of China(2013CB933500)National Natural Science Foundation of China(Grant Nos.61422403,51672180,51622306,21673151)+2 种基金Qing Lan ProjectCollaborative Innovation Center of Suzhou Nano Science and Technology(NANO-CIC)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)
文摘Organic field-effect transistors(OFETs) based on organic micro-/nanocrystals have been widely reported with charge carrier mobility exceeding 1.0 cm^2V^(-1)s^(-1), demonstrating great potential for high-performance, low-cost organic electronic applications. However, fabrication of large-area organic micro-/nanocrystal arrays with consistent crystal growth direction has posed a significant technical challenge. Here, we describe a solution-processed dip-coating technique to grow large-area, aligned 9,10-bis(phenylethynyl) anthracene(BPEA) and 6,13-bis(triisopropylsilylethynyl) pentacene(TIPSPEN) single-crystalline nanoribbon arrays. The method is scalable to a 5 9 10 cm^2 wafer substrate, with around 60% of the wafer surface covered by aligned crystals. The quality of crystals can be easily controlled by tuning the dip-coating speed. Furthermore, OFETs based on well-aligned BPEA and TIPS-PEN single-crystalline nanoribbons were constructed.By optimizing channel lengths and using appropriate metallic electrodes, the BPEA and TIPS-PEN-based OFETs showed hole mobility exceeding 2.0 cm^2V^(-1)s^(-1)(average mobility 1.2 cm^2V^(-1)s^(-1)) and 3.0 cm^2V^(-1)s^(-1)(average mobility2.0 cm^2V^(-1)s^(-1)), respectively. They both have a high on/off ratio(I_(on)/I_(off))>10~9. The performance can well satisfy the requirements for light-emitting diodes driving.
基金supported by National Natural Science Foundation of China (NSFC) (No. 61804103)National Key R&D Program of China (No. 2017YFA0205002)+8 种基金Natural Science Foundation of the Jiangsu Higher Education Institutions of China (Nos. 18KJA535001 and 14KJB 150020)Natural Science Foundation of Jiangsu Province of China (Nos. BK20170343 and BK20180242)China Postdoctoral Science Foundation (No. 2017M610346)State Key Laboratory of Silicon Materials, Zhejiang University (No. SKL2018-03)Nantong Municipal Science and Technology Program (No. GY12017001)Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University (KSL201803)supported by Collaborative Innovation Center of Suzhou Nano Science & Technology, the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)the 111 ProjectJoint International Research Laboratory of Carbon-Based Functional Materials and Devices
文摘Continuous deforming always leads to the performance degradation of a flexible triboelectric nanogenerator due to the Young’s modulus mismatch of different functional layers.In this work,we fabricated a fiber-shaped stretchable and tailorable triboelectric nanogenerator(FST-TENG)based on the geometric construction of a steel wire as electrode and ingenious selection of silicone rubber as triboelectric layer.Owing to the great robustness and continuous conductivity,the FST-TENGs demonstrate high stability,stretchability,and even tailorability.For a single device with ~6 cm in length and ~3 mm in diameter,the open-circuit voltage of ~59.7 V,transferred charge of ~23.7 nC,short-circuit current of ~2.67 μA and average power of ~2.13 μW can be obtained at 2.5 Hz.By knitting several FST-TENGs to be a fabric or a bracelet,it enables to harvest human motion energy and then to drive a wearable electronic device.Finally,it can also be woven on dorsum of glove to monitor the movements of gesture,which can recognize every single finger,different bending angle,and numbers of bent finger by analyzing voltage signals.
基金partially supported by the National Natural Science Foundation of China(51802209,22077093,51761145041,51525203)the National Research Programs from Ministry of Science and Technology(MOST)of China(2016YFA0201200)+3 种基金the Natural Science Foundation of Jiangsu Province(BK20180848)the Jiangsu Social Development Project(BE2019658)Collaborative Innovation Center of Suzhou Nano Science and Technologythe 111 Program from the Ministry of Education of China.
文摘Due to the negative roles of tumor microenvironment(TME)in compromising therapeutic responses of various cancer therapies,it is expected that modulation of TME may be able to enhance the therapeutic responses during cancer treatment.Herein,we develop a concise strategy to prepare pH-responsive nanoparticles via the CaCO3-assisted double emulsion method,thereby enabling effective co-encapsulation of both doxorubicin(DOX),an immunogenic cell death(ICD)inducer,and alkylated NLG919(aNLG919),an inhibitor of indoleamine 2,3-dioxygenase 1(IDO1).The obtained DOX/aNLG919-loaded CaCO3 nanoparticles(DNCaNPs)are able to cause effective ICD of cancer cells and at the same time restrict the production of immunosuppressive kynurenine by inhibiting IDO1.Upon intravenous injection,such DNCaNPs show efficient tumor accumulation,improved tumor penetration of therapeutics and neutralization of acidic TME.As a result,those DNCaNPs can elicit effective anti-tumor immune responses featured in increased density of tumor-infiltrating CD8+cytotoxic T cells as well as depletion of immunosuppressive regulatory T cells(Tregs),thus effectively suppressing the growth of subcutaneous CT26 and orthotopic 4T1 tumors on the Balb/c mice through combined chemotherapy&immunotherapy.This study presents a compendious strategy for construction of pH-responsive nanoparticles,endowing significantly enhanced chemo-immunotherapy of cancer by overcoming the immunosuppressive TME.
文摘Electrochemical CO_(2)reduction to value-added fuels and chemicals is recognized as a promising strategy to alleviate energy shortages and global warming owing to its high efficiency and economic feasibility.Recently,understanding the activity origin,selectivity regulation,and reaction mechanisms of CO_(2)reduction reactions(CO_(2)RRs)has become the focus of efficient electrocatalyst design.Polyoxometalates(POMs),a unique class of nanosized metal-oxo clusters,are promising candidates for the development of efficient CO_(2)RR electrocatalysts and,owing to their well-defined structure,remarkable electron/proton storage and transfer ability,and capacities for adsorption and activation of CO_(2),are ideal models for investigating the activity origin and reaction mechanisms of CO_(2)RR electrocatalysts.In this review,we focus on the activity origin and mechanism of CO_(2)RRs and survey recent advances that were achieved by employing POMs in electrocatalytic CO_(2)RRs.We highlight the significant roles of POMs in the electrocatalytic CO_(2)RR process and the main factors influencing selectivity regulation and catalytic CO_(2)RR performance,including the electrolyte,electron-transfer process,and surface characteristics.Finally,we offer a perspective of the advantages and future challenges of POM-based materials in electrocatalytic CO_(2)reduction that could inform new advancements in this promising research field.
基金the Natural Science Foundation of China(NSFC)(Grant No.U1432249,21203130)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)This work was also supported by the German Research Foundation(DFG:LE2249/5-1).
文摘Lithium–sulfur(Li–S)battery with a new configuration is demonstrated by inserting a flexible nitrogen-doping carbon nanofiber(N-CNFs)interlayer between the sulfur cathode and the separator.The N-CNFs film with high surface roughness and surface area is fabricated by electrospinning and a subsequent calcination process.The N-CNFs film interlayer not only effectively traps the shuttling migration of polysulfides but also gives the whole battery reliable electronic conductivity,which can effectively enhance the electrochemical performance of Li–S batteries.Finally,Li–S batteries with long cycling stability of 785 mAh/g after 200 cycles and good rate capability of 573 mAh/g at 5 C are achieved.
基金the National Natural Science Foundation of China(21908081,21501072,51972216,51725204,21771132 and 52041202)the National MCF Energy R&D Program(2018YFE0306105)+1 种基金Innovative Research Group Project of the National Natural Science Foundation of China(51821002)the Jiangsu Specially-Appointed Professors Program,and the Natural Science Foundation of Jiangsu Province(BK20190041,BK20190828 and BK20150489).
文摘Due to the quantum size effect and other unique photoelectric properties,quantum dots(QDs)have attracted tremendous interest in nanoscience,leading a lot of milestone works.Meantime,the scope and scientific connotation of QDs are constantly expanding,which demonstrated amazing development vitality.Besides the well-developed Cd-containing Ⅱ-Ⅵ semiconductors,QDs of environmentally friendly Ⅰ-Ⅲ-Ⅵ(Ⅰ=Cu,Ag;Ⅲ=Ga,In;Ⅵ=S,Se)chalcogenides have been a hot spot in the QDs family,which are different from traditional Ⅱ-Ⅵ QDs in terms of multi-composition,complex defect structure,synthetic chemistry and optical properties,bringing a series of new laws,new phenomena and new challenges.The composition of Ⅰ-Ⅲ-Ⅵ chalcogenides and their solid solutions can be adjusted within a very large range while the anion framework remains stable,giving them excellent capability of photoelectric property manipulation.The important features of Ⅰ-Ⅲ-Ⅵ QDs include wide-range bandgap tuning,large Stokes shift and long photoluminescence(PL)lifetime,which are crucial for biological,optoelectronic and energy applications.This is due to the coexistence of two or more metal cations leading to a large number of intrinsic defects within the crystal lattice also known as deep-donor-acceptor states,besides the commonly observed surface defects in all QDs.However,a profound understanding of their structure and optoelectronic properties remains a huge challenge with many key issues unclear.On one hand,the achievements and experience of traditional QD research are expected to provide vital value for further development of Ⅰ-Ⅲ-Ⅵ QDs.On the other hand,the understanding of the emerging new QDs,such as carbon and other 2D materials,are even more challenging because of the dramatically different composition and structure from Ⅱ-Ⅵ semiconductors.For this,Ⅰ-Ⅲ-Ⅵ QDs,as a close relative to Ⅱ-Ⅵ QDs but with much more complex composition and structure variation,provide a great opportunity as a gradual bridge to make up the big gap between traditional QDs and emerging new QDs,such as carbon dots.Here,we hope to compare the research progress of Ⅰ-Ⅲ-Ⅵ QDs and Ⅱ-Ⅵ QDs,in an effort to comprehensively understand their structure,synthetic chemistry,optical electronic and photocatalytic properties.We further give insights on the key potential issues of Ⅰ-Ⅲ-Ⅵ QDs from the perspective of bridging between traditional QDs and emerging carbon dots,especially the profound principles behind synthetic chemistry,PL mechanism and optoelectronic applications.
基金supported by the National Natural Science Foundation of China (Nos. 61675143, 11661131002)the Natural Science Foundation of Jiangsu Province (No. BK20160277)+2 种基金the Soochow University-Western University Joint Centre for Synchrotron Radiation Researchthe Collaborative Innovation Center of Suzhou Nano Science & Technologythe Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
文摘We present a straightforward physical approach for synthesizing multiwalled carbon nanotubes(CNTs)-Pd Au/Pt trimetallic nanoparticles(NPs), which allows predesign and control of the metal compositional ratio by simply adjusting the sputtering targets and conditions. The small-sized CNTs-Pd Au/Pt NPs(~3 nm, Pd/Au/Pt ratio of 3:1:2) act as nanocatalysts for the methanol oxidationreaction(MOR), showing excellent performance with electrocatalytic peak current of 4.4 A mg^(-1) Pt and high stability over 7000 s. The electrocatalytic activity and stability of the Pd Au/Pt trimetallic NPs are much superior to those of the corresponding Pd/Pt and Au/Pt bimetallic NPs,as well as a commercial Pt/C catalyst. Systematic investigation of the microscopic, crystalline, and electronic structure of the Pd Au/Pt NPs reveals alloying and charge redistribution in the Pd Au/Pt NPs, which are responsible for the promotion of the electrocatalytic performance.
基金financial support from the National Natural Science Foundation of China (grant no.51772199)the Natural Science Foundation of Jiangsu Province (Grant no.BK20170329)+2 种基金the Collaborative Innovation Center of Suzhou Nano Science & Technologythe Priority Academic Program Development of Jiangsu Higher Education Institutionsthe 111 Project。
文摘Polymeric organic battery materials are promising alternatives to the transition-metal-based ones owing to their enriched chemistries. However, the flammability of organic compounds brings in serious concern on battery safety. In addition to use flame-retarding electrolyte/electrolyte additives or battery separators,flame retardancy can readily be achieved through the integration of flame-retarding unit into the polymer backbone, imparting the flame retardancy permanently. The as-designed polymer based on phenothiazine shows significantly shortened self-extinguished time without deteriorating its intrinsic thermodynamic and electrochemical properties. Moreover, two electron per phenothiazine molecule is realized for the first time in a highly reversible manner with discharge voltages of 3.52 V and 4.16 V versus Li+/Li and an average capacity of ca. 120 mAh g-1 at a current rate of 2 C. The origin of the reversibility is investigated through density functional theory(DFT) calculations. These findings address the importance of molecular design for safer and more stable organic materials for batteries.
基金supported by the National Natural Science Foundation of China(Nos.62174115 and U21A20147)the International Joint Research Center for Intelligent Nano Environmental Protection New Materials and Testing Technology(No.SDGH2108)the Collaborative Innovation Center of Suzhou Nano Science&Technology,the 111 Project and the Joint International Research Laboratory of Carbon-Based Functional Materials and Devices。
文摘With the arrival of intelligent terminals,triboelectric nanogenerators,as a new kind of energy converter,are considered one of the most important technologies for the next generation of intelligent electronics.As a self-powered sensor,it can greatly reduce the power consumption of the entire sensing system by transforming external mechanical energy to electricity.However,the fabrication method of triboelectric sensors largely determines their functionality and performance.This review provides an overview of various methods used to fabricate triboelectric sensors,with a focus on the processes of micro-electro-mechanical systems technology,three-dimensional printing,textile methods,template-assisted methods,and material synthesis methods for manufacturing.The working mechanisms and suitable application scenarios of various methods are outlined.Subsequently,the advantages and disadvantages of various methods are summarized,and reference schemes for the subsequent application of these methods are included.Finally,the opportunities and challenges faced by different methods are discussed,as well as their potential for application in various intelligent systems in the Internet of Things.
基金supported by Natural Science Foundation of China(NSFC)(Grant No.U1432249)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)+1 种基金supported by Collaborative Innovation Center of Suzhou Nano Science&Technologysponsored by Qing Lan Project
文摘Looking toward world technology trends over the next few decades, self-powered sensing networks are a key field of technological and economic driver for global industries. Since 2006, Zhong Lin Wang's group has proposed a novel concept of nanogenerators(NGs), including piezoelectric nanogenerator and triboelectric nanogenerator, which could convert a mechanical trigger into an electric output. Considering motion ubiquitously exists in the surrounding environment and for any most common materials used every day, NGs could be inherently served as an energy source for our daily increasing requirements or as one of self-powered environmental sensors. In this regard, by coupling the piezoelectric or triboelectric properties with semiconducting gas sensing characterization, a new research field of self-powered gas sensing has been proposed. Recent works have shown promising concept to realize NG-based self-powered gas sensors that are capable of detecting gas environment without the need of external power sources to activate the gas sensors or to actively generate a readout signal. Compared with conventional sensors, these self-powered gas sensors keep the approximate performance.Meanwhile, these sensors drastically reduce power consumption and additionally reduce the required space for integration,which are significantly suitable for the wearable devices. This paper gives a brief summary about the establishment and latest progress in the fundamental principle, updated progress and potential applications of NG-based self-powered gas sensing system. The development trend in this field is envisaged, and the basic configurations are also introduced.
基金supported by National Natural Science Foundation of China(NSFC)(Nos.61804103,U1932124)the National Science and Technology Major Project from Minister of Science and Technology of China(Grant No.2018AAA0103104)+8 种基金Natural Science Foundation of the Jiangsu Higher Education Institutions of China(No.18KJA535001)Natural Science Foundation of Jiangsu Province of China(Nos.BK20170343,BK20180242)Jiangsu Key Laboratory for Carbon Based Functional Materials and Devices,Soochow University(KJS1803)the XJTLU Key Programme Special Fund(KSF-A-18)Jiangsu Province Engineering Laboratory of High Efficient Energy Storage Technology and Equipments,China University of Mining and Technology(CUMT)supported by Collaborative Innovation Center of Suzhou Nano Science and Technologythe Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)the 111 ProjectJoint International Research Laboratory of Carbon-Based Functional Materials and Devices.
文摘Photoelectrochemical hydrogen generation is a promising approach to address the environmental pollution and energy crisis.In this work,we present a hybridized mechanical and solar energy-driven selfpowered hydrogen production system.A rotatory disc-shaped triboelectric nanogenerator was employed to harvest mechanical energy from water and functions as a su cient external power source.WO3/BiVO4 heterojunction photoanode was synthesized in a PEC water-splitting cell to produce H2.After transformation and rectification,the peak current reaches 0.1 m A at the rotation speed of 60 rpm.In this case,the H2 evolution process only occurs with sunlight irradiation.When the rotation speed is over 130 rpm,the peak photocurrent and peak dark current have nearly equal value.Direct electrolysis of water is almost simultaneous with photoelectrocatalysis of water.It is worth noting that the hydrogen production rate increases to 5.45 and 7.27μL min-1 without or with light illumination at 160 rpm.The corresponding energy conversion e ciency is calculated to be 2.43%and 2.59%,respectively.All the results demonstrate such a self-powered system can successfully achieve the PEC hydrogen generation,exhibiting promising possibility of energy conversion.
基金Open access funding provided by Shanghai Jiao Tong University。
文摘Traditional triboelectric tactile sensors based on solid–solid interface have illustrated promising application prospects through optimization approach.However,the poor sensitivity and reliability caused by hard contact-electrification still poses challenges for the practical applications.In this work,a liquid–solid interface ferrofluid-based triboelectric tactile sensor(FTTS)with ultrahigh sensitivity is proposed.Relying on the fluidity and magnetism of ferrofluid,the topography of microstructure can be flexibly adjusted by directly employing ferrofluid as triboelectric material and controlling the position of outward magnet.To date,an ultrahigh sensitivity of 21.48 k Pa;for the triboelectric sensors can be achieved due to the high spike microstructure,low Young’s modulus of ferrofluid and efficient solid–liquid interface contact-electrification.The detection limit of FTTS of 1.25 Pa with a wide detection range to 390 k Pa was also obtained.In addition,the oleophobic property between ferrofluid and poly-tetra-fluoro-ethylene triboelectric layer can greatly reduce the wear and tear,resulting in the great improvement of stability.Finally,a strategy for personalized password lock with high security level has been demonstrated,illustrating a great perspective for practical application in smart home,artificial intelligence,Internet of things,etc.
基金supported by National MCF Energy R&D Program of China(2018YFE0306105)National Key R&D Program of China(2020YFA0406104,2020YFA0406101)+10 种基金Innovative Research Group Project of the National Natural Science Foundation of China(51821002)National Natural Science Foundation of China(52201269,51725204,21771132,51972216,52041202)Natural Science Foundation of Jiangsu Province(BK20210735)Natural Science Foundation of the Higher Education Institutions of Jiangsu Province(21KJB430043)Collaborative Innovation Center of Suzhou Nano Science&Technologythe 111 ProjectSuzhou Key Laboratory of Functional Nano&Soft MaterialsJiangsu Key Laboratory for Advanced Negative Carbon Technologiesthe funding from Alexander von Humboldt(AvH)FoundationGusu leading talent plan for scientific and technological innovation and entrepreneurship(ZXL2022487)support from the German Federal Ministry of Education and Research in the framework of the project Catlab(03EW0015A/B)。
文摘Efficient and durable oxygen evolution reaction(OER)requires the electrocatalyst to bear abundant active sites,optimized electronic structure as well as robust component and mechanical stability.Herein,a bimetallic lanthanum-nickel oxysulfide with rich oxygen vacancies based on the La_(2)O_(2)S prototype is fabricated as a binder-free precatalyst for alkaline OER.The combination of advanced in situ and ex situ characterizations with theoretical calculation uncovers the synergistic effect among La,Ni,O,and S species during OER,which assures the adsorption and stabilization of the oxyanion SO_(4)^(2-)onto the surface of the deeply reconstructed porous heterostructure composed of confining Ni OOH nanodomains by La(OH)_3 barrier.Such coupling,confinement,porosity and immobilization enable notable improvement in active site accessibility,phase stability,mass diffusion capability and the intrinsic Gibbs free energy of oxygen-containing intermediates.The optimized electrocatalyst delivers exceptional alkaline OER activity and durability,outperforming most of the Ni-based benchmark OER electrocatalysts.
基金supported by the National Natural Science Foundation of China(No.21805201)the NSFC-NRF China-Korea International Joint Research Project(No.51911540473)+1 种基金the Postdoctoral Research Foundation of China(No.2018T110544 and No.2017 M611899)the support by Suzhou Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies。
文摘Sulfurized polyacrylonitrile(SPAN)represents a unique class of cathode material for lithium sulfur(Li-S)batteries as it eradicates the polysulfides shuttling issue in carbonate-based electrolyte.However,due to the essential chemical S-linking and organic nature of SPAN,the active mass percentage and rate capability are two bottleneck issues preventing its ultimate deployment outside of laboratories.In the current work,aiming to endow both the charge conductivity and catalytic activity to SPAN for maximizing the redox kinetics of S conversion,a freestanding nanofibrous SPAN cathode embedding conductive CNTs and atomically dispersed Co centers is fabricated via multivariate electrospinning.While the CNTs enable dramatically enhancing the fiber conductivity and generating mesoscopic porosity for facilitating charge and mass transportation,the cross-linking of SPAN by Co-N_(4) S motifs creates extra charge conduction pathways and further serves as the catalytic active sites for expediting redox S conversion.As a result,an extraordinary Li-SPAN performance is achieved with a high specific capacity up to 1856 mAh g^(-1)@0.2 C,a superb rate capability up to 10 C,and an ultra-long battery life up to 1500 cycles@1 C.Consequently,our study here provides insights into the adoption of coordination chemistry to maximize the sulfur utilization by ensuring a more complete redox conversion from SPAN to Li2 S,and vice versa.
基金supported by National MCF Energy R&D Program of China(2018YFE0306105)National Key R&D Program of China(2020YFA0406104,2020YFA0406101)+6 种基金Innovative Research Group Project of the National Natural Science Foundation of China(51821002)National Natural Science Foundation of China(51725204,21771132,51972216,52041202,51902217)Natural Science Foundation of Jiangsu Province(BK20190041)Key-Area Research and Development Program of GuangDong Province(2019B010933001)Collaborative Innovation Center of Suzhou Nano Science and Technologythe 111 ProjectSuzhou Key Laboratory of Functional Nano and Soft Materials。
文摘Carbon dots(CDs),as a unique zero-dimensional member of carbon materials,have attracted numerous attentions for their potential applications in optoelectronic,biological,and energy related fields.Recently,CDs as catalysts for energy conversion reactions under multi-physical conditions such as light and/or electricity have grown into a research frontier due to their advantages of high visible light utilization,fast migration of charge carriers,efficient surface redox reactions and good electrical conductivity.In this review,we summarize the fabrication methods of CDs and corresponding CD nanocomposites,including the strategies of surface modification and heteroatom doping.The properties of CDs that concerned to the photo-and electro-catalysis are highlighted and detailed corresponding applications are listed.More importantly,as new non-contact detection technologies,transient photo-induced voltage/current have been developed to detect and study the charge transfer kinetics,which can sensitively reflect the complex electron separation and transfer behavior in photo-/electro-catalysts.The development and application of the techniques are reviewed.Finally,we discuss and outline the major challenges and opportunities for future CD-based catalysts,and the needs and expectations for the development of novel characterization technologies.
基金the support from the high-performance computing platform of Jiangsu UniversityThe Jiangsu University Foundation (18JDG019)+3 种基金the Postdoctoral Foundation of Jiangsu Province (2018K072C)Six Talent Peak Project of Jiangsu Province (XLC-158)the China Postdoctoral Science Foundation (2019M651727, 2019M651719)the National Natural Science Foundation of China (21808090, 51902139, U1932211) financially supported this work。
文摘Hematite is regarded as a promising photoanode for photoelectrochemical(PEC) water splitting.However,the charge recombination occurred at the interface of FTO/hematite strictly limits the PEC performance of hematite.Herein,we reported a Ti3C2 MXene underlayer modified hematite(Ti-Fe2O3) photoanode via a simple drop-casting followed by hydrothermal and annealing processes.Owing to the bifunctional role of Ti3C2 MXene underlayer in improving the interfacial properties of FTO/hematite and providing Ti source for the construction of Fe2 TiO5/Fe2O3 heterostructure in hematite nanostructure,the bulk and interfacial charge transfer dynamics of hematite are significantly enhanced,and consequently enhancing the PEC performance.Compared with the pristine hematite,the as-prepared Ti-Fe2O3 photoanode shows an increased photocurrent density from 0.80 mA/cm^(2) to 1.30 mA/cm^(2) at 1.23 V vs.RHE.Moreover,a further promoted PEC performance including a dramatically increased photocurrent density of 2.49 mA/cm^(2) at1.23 V vs.RHE and an obviously lowered onset potential is achieved for the Ti-Fe2O3 sample after the subsequent surface F-treatment and the loading of FeNiOOH cocatalyst.Such results suggest that the introduction of Ti3C2 MXene underlayer is a facile but effective approach to improve the PEC water splitting activity of hematite.
基金supported by the National Natural Science Foundation of China(22109098)the Shanghai Sailing Program(20YF1432300)+4 种基金the Shanghai Engineering Research Center for Food Rapid Detection(19DZ2251300)the Natural Science Foundation of Jiangsu Province(BK20210735)the Natural Science Foundation of the Higher Education Institutions of Jiangsu Province(21KJB430043)the Collaborative Innovation Center of Suzhou Nano Science&Technology,the 111 Projectthe Suzhou Key Laboratory of Functional Nano&Soft Materials。
文摘Seawater photoelectrolysis is showing huge potential in green energy conversion field,yet it is still a formidable challenge to develop one catalyst that can drive the electrolysis reaction stably,economically and efficiently.Motivated by this point,the inorganic–organic hybridization strategy is proposed to insitu construct one hierarchical electrode via concurrent electroless plating and polymerization,which assures the growth of boron-modulated nickel–cobalt oxyhydroxide nanoballs and photosensitive polyaniline nanochains on the self-supporting Ti-based foil(B-Co Ni OOH/PANI@TiO_(2)/Ti).Upon inducing photoelectric effect(PEE),the designed target electrode delivers overpotentials as low as 196 and 398 mV at 100 mA cm^(-2)for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),respectively,corresponding to an activity enhancement by about 15%as compared to those without PEE.Inspiringly,when served as bifunctional electrocatalysts for overall seawater electrolysis,it can stably maintain at 200 mA cm^(-2)with negligible decay over 72 h.Further analysis reveals that the exceptional catalytic performance can be credit to the B-CoNiOOH,polyaniline(PANI)and TiO_(2)subunit coupling-induced physically and chemically synergistic catalysis effect such as admirable composition stability,photoelectric function and adhesion capability.The finding in this contribution may trigger much more broad interest to the novel hybrid catalysts consisting of photosensitive polymer and transition metal-based electrocatalysts.
基金supported by the National Natural Science Foundation of China(U1932211,U1732110)the Collaborative Innovation Center of Suzhou Nano Science&Technology+3 种基金the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)the 111 Projectthe support from Users with Excellence Program of Hefei Science Center CAS(2019HSC-UE002)Post graduate Research&Practice Innovation Program of Jiangsu Province(Grant No.KYCX19_1921)。
文摘Efficient electrocatalysts for hydrogen evolution reaction(HER) in alkaline solution are highly required for water splitting.Here we design an ultra-small PtOx nanoparticle with hybrid Pt chemical states on carbon nanotubes as highly efficient alkaline HER catalyst,which shows a low overpotential of 19.4 mV at 10 mA cm^(-2),a high mass activity of 5.56 A mg_(Pt)^(-1) at 0.1 V, and a stable durability for at least 20 h.The HER performance is better than that of the benchmark 20 wt% Pt/C while the Pt content in the catalyst is only about one tenth of that in Pt/C.It also represents one of the best catalysts ever reported for HER in alkaline solution.Synchrotron radiation X-ray absorption spectroscopy reveals that the efficient and stable alkaline HER performance can be attributed to the favorable design of hybrid chemical states of Pt with carbon nanotubes,which exhibits abundant surface Pt-O as active catalytic sites and forms stable Pt-C interfacial interaction to both anchor the NPs and improve the synergistic effect between catalyst and substrate.
