Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology r...Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.展开更多
The single-shot readout data process is essential for the realization of high-fidelity qubits and fault-tolerant quantum algorithms in semiconductor quantum dots. However, the fidelity and visibility of the readout pr...The single-shot readout data process is essential for the realization of high-fidelity qubits and fault-tolerant quantum algorithms in semiconductor quantum dots. However, the fidelity and visibility of the readout process are sensitive to the choice of the thresholds and limited by the experimental hardware. By demonstrating the linear dependence between the measured spin state probabilities and readout visibilities along with dark counts, we describe an alternative threshold-independent method for the single-shot readout of spin qubits in semiconductor quantum dots. We can obtain the extrapolated spin state probabilities of the prepared probabilities of the excited spin state through the threshold-independent method. We then analyze the corresponding errors of the method, finding that errors of the extrapolated probabilities cannot be neglected with no constraints on the readout time and threshold voltage. Therefore, by limiting the readout time and threshold voltage, we ensure the accuracy of the extrapolated probability. We then prove that the efficiency and robustness of this method are 60 times larger than those of the most commonly used method. Moreover, we discuss the influence of the electron temperature on the effective area with a fixed external magnetic field and provide a preliminary demonstration for a single-shot readout of up to 0.7K/1.5T in the future.展开更多
This research investigates the hydrothermal synthesis and annealing duration effects on nickel sulfide(NiS_(2)quantum dots(QDs)for catalytic decolorization of methylene blue(MB)dye and antimicrobial efficacy.QD size i...This research investigates the hydrothermal synthesis and annealing duration effects on nickel sulfide(NiS_(2)quantum dots(QDs)for catalytic decolorization of methylene blue(MB)dye and antimicrobial efficacy.QD size increased with longer annealing,reducing catalytic activity.UV–vis,XRD,TEM,and FTIR analyses probed optical structural,morphological,and vibrational features.XRD confirmed NiS2's anorthic structure,with crystallite size growing from 6.53 to 7.81 nm during extended annealing.UV–Vis exhibited a bathochromic shift,reflecting reduced band gap energy(Eg)in NiS_(2).TEM revealed NiS_(2)QD formation,with agglomerated QD average size increasing from 7.13 to 9.65 nm with prolonged annealing.Pure NiS_(2)showed significant MB decolorization(89.85%)in acidic conditions.Annealed NiS_(2) QDs demonstrated notable antibacterial activity,yielding a 6.15mm inhibition zone against Escherichia coli(E.coli)compared to Ciprofloxacin.First-principles computation supported a robust interaction between MB and NiS_(2),evidenced by obtained adsorption energies.This study highlights the nuanced relationship between annealing duration,structural changes,and functional properties in NiS_(2)QDs,emphasizing their potential applications in catalysis and antibacterial interventions.展开更多
As lead halide perovskite(LHP)semiconductors have shown tremendous promise in many application fields,and particularly made strong impact in the solar photovoltaic area,low dimensional quantum dot forms of these perov...As lead halide perovskite(LHP)semiconductors have shown tremendous promise in many application fields,and particularly made strong impact in the solar photovoltaic area,low dimensional quantum dot forms of these perovskites are showing the potential to make distinct marks in the fields of electronics,optoelectronics and photonics.The so-called perovskite quantum dots(PQDs)not only possess the most important features of LHP materials,i.e.,the unusual high defect tolerance,but also demonstrate clear quantum size effects,along with exhibiting desirable optoelectronic properties such as near perfect photoluminescent quantum yield,multiple exciton generation and slow hot-carrier cooling.Here,we review the advantageous properties of these nanoscale perovskites and survey the prospects for diverse applications which include lightemitting devices,solar cells,photocatalysts,lasers,detectors and memristors,emphasizing the distinct superiorities as well as the challenges.展开更多
A composite was created by incorporating the quantum dot-enhanced SiO_(2)nanoparticles within this hydrogel.Based on this composite,a temperature-controlled fluorescent probe for DCP was developed.A meticulous examina...A composite was created by incorporating the quantum dot-enhanced SiO_(2)nanoparticles within this hydrogel.Based on this composite,a temperature-controlled fluorescent probe for DCP was developed.A meticulous examination of this probe revealed its attributes and factors affecting its performance.By using temperature modulation,the probe was adept at detecting DCP concentrations ranging between 1.0×10^(-6)and 9.0×10^(-6)mol/L.Such a probe offers remarkable selectivity,repeatability,and robust stability,so that the detection of DCP can be carried out at different temperatures,and a fast,reliable,sensitive and low-cost intelligent detection method is realized.展开更多
The combination of non-Hermitian physics and Majorana fermions can give rise to new effects in quantum transport systems. In this work, we investigate the interplay of PT-symmetric complex potentials, Majorana tunneli...The combination of non-Hermitian physics and Majorana fermions can give rise to new effects in quantum transport systems. In this work, we investigate the interplay of PT-symmetric complex potentials, Majorana tunneling and interdot tunneling in a non-Hermitian double quantum dots system. It is found that in the weak-coupling regime the Majorana tunneling has pronounced effects on the transport properties of such a system, manifested as splitting of the single peak into three and a reduced 1/4 peak in the transmission function. In the presence of the PT-symmetric complex potentials and interdot tunneling, the 1/4 central peak is robust against them, while the two side peaks are tuned by them. The interdot tunneling only induces asymmetry, instead of moving the conductance peak, due to the robustness of the Majorana modes. There is an exceptional point induced by the union of Majorana tunneling and interdot tunneling. With increased PT-symmetric complex potentials, the two side peaks will move towards each other. When the exceptional point is passed through, these two side peaks will disappear. In the strong-coupling regime, the Majorana fermion induces a 1/4 conductance dip instead of the three-peak structure. PT-symmetric complex potentials induce two conductance dips pinned at the exceptional point. These effects should be accessible in experiments.展开更多
The shuttle effect of lithium polysulfides(LiPSs)and uncontrollable lithium dendrite growth seriously hinder the practical application of lithium-sulfur(Li-S)batteries.To simultaneously address such issues,monodispers...The shuttle effect of lithium polysulfides(LiPSs)and uncontrollable lithium dendrite growth seriously hinder the practical application of lithium-sulfur(Li-S)batteries.To simultaneously address such issues,monodispersed Nb N quantum dots anchored on nitrogen-doped hollow carbon nanorods(NbN@NHCR)are elaborately developed as efficient Li PSs immobilizer and Li stabilizer for high-performance Li-S full batteries.Density functional theory(DFT)calculations and experimental characterizations demonstrate that the sulfiphilic and lithiophilic NbN@NHCR hybrid can not only efficiently immobilize the soluble Li PSs and facilitate diffusion-conversion kinetics for alleviating the shuttling effect,but also homogenize the distribution of Li+ions and regulate uniform Li deposition for suppressing Li-dendrite growth.As a result,the assembled Li-S full batteries(NbN@NHCR-S||Nb N@NHCR-Li)deliver excellent long-term cycling stability with a low decay rate of 0.031%per cycle over 1000 cycles at high rate of 2 C.Even at a high S loading of 5.8 mg cm^(-2)and a low electrolyte/sulfur ratio of 5.2μL mg^(-1),a large areal capacity of 6.2 mA h cm^(-2)can be achieved in Li-S pouch cell at 0.1 C.This study provides a new perspective via designing a dual-functional sulfiphilic and lithiophilic hybrid to address serious issues of the shuttle effect of S cathode and dendrite growth of Li anode.展开更多
We utilize the calculation of hierarchical equations of motion to demonstrate that the spin-dependent properties between adjacent quantum dots(QDs)can be changed by breaking the internal symmetry configuration,corresp...We utilize the calculation of hierarchical equations of motion to demonstrate that the spin-dependent properties between adjacent quantum dots(QDs)can be changed by breaking the internal symmetry configuration,corresponding to the inversion of dominant chiral states.In the linear triple quantum dots(LTQDs)connected to two electron reservoirs,we can observe that the blockage appears at the triangle triple quantum dots(TTQDs)by gradually increasing the coupling strength between next-nearest double QDs.When the initial coupling between LTQDs has altered,the internal chiral circulation also undergoes the corresponding transform,thus achieving qualitative regulation and detection of the blocking region.We also investigate the response of the chiral circulation to the dot–lead coupling strength,indicating the overall robust chiral circulation of the TTQDs frustration.展开更多
SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish ...SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish reaction kinetics,low electronic conductivity,and large volume changes during charge and discharge hinder the practical applications of SnO_(2)-based electrodes for SIBs and PIBs.Engineering rational structures with fast charge/ion transfer and robust stability is important to overcoming these challenges.Herein,S-doped SnO_(2)(S-SnO_(2))quantum dots(QDs)(≈3 nm)encapsulated in an N,S codoped carbon fiber networks(S-SnO_(2)-CFN)are rationally fabricated using a sequential freeze-drying,calcination,and S-doping strategy.Experimental analysis and density functional theory calculations reveal that the integration of S-SnO_(2) QDs with N,S codoped carbon fiber network remarkably decreases the adsorption energies of Na/K atoms in the interlayer of SnO_(2)-CFN,and the S doping can increase the conductivity of SnO_(2),thereby enhancing the ion transfer kinetics.The synergistic interaction between S-SnO_(2) QDs and N,S codoped carbon fiber network results in a composite with fast Na+/K+storage and extraordinary long-term cyclability.Specifically,the S-SnO_(2)-CFN delivers high rate capacities of 141.0 mAh g^(−1) at 20 A g^(−1) in SIBs and 102.8 mAh g^(−1) at 10 A g^(−1) in PIBs.Impressively,it delivers ultra-stable sodium storage up to 10,000 cycles at 5 A g^(−1) and potassium storage up to 5000 cycles at 2 A g^(−1).This study provides insights into constructing metal oxide-based carbon fiber network structures for high-performance electrochemical energy storage and conversion devices.展开更多
CsPbI_(3)perovskite quantum dots(QDs)are ideal materials for the next generation of red light-emitting diodes.However,the low phase stability of CsPbI_(3)QDs and long-chain insulating capping ligands hinder the improv...CsPbI_(3)perovskite quantum dots(QDs)are ideal materials for the next generation of red light-emitting diodes.However,the low phase stability of CsPbI_(3)QDs and long-chain insulating capping ligands hinder the improvement of device performance.Traditional in-situ ligand replacement and ligand exchange after synthesis were often difficult to control.Here,we proposed a new ligand exchange strategy using a proton-prompted insitu exchange of short 5-aminopentanoic acid ligands with long-chain oleic acid and oleylamine ligands to obtain stable small-size CsPbI_(3)QDs.This exchange strategy maintained the size and morphology of CsPbI_(3)QDs and improved the optical properties and the conductivity of CsPbI_(3)QDs films.As a result,high-efficiency red QD-based light-emitting diodes with an emission wavelength of 645 nm demonstrated a record maximum external quantum efficiency of 24.45%and an operational half-life of 10.79 h.展开更多
Quantum dot-based up-conversion photodetector,in which an infrared photodiode(PD)and a quantum dot light-emitting diode(QLED)are back-to-back connected,is a promising candidate for low-cost infrared imaging.However,th...Quantum dot-based up-conversion photodetector,in which an infrared photodiode(PD)and a quantum dot light-emitting diode(QLED)are back-to-back connected,is a promising candidate for low-cost infrared imaging.However,the huge efficiency losses caused by integrating the PD and QLED together hasn’t been studied sufficiently.This work revealed at least three origins for the efficiency losses.First,the PD unit and QLED unit usually didn’t work under optimal conditions at the same time.Second,the potential barriers and traps at the interconnection between PD and QLED units induced unfavorable carrier recombination.Third,much emitted visible light was lost due to the strong visible absorption in the PD unit.Based on the understandings on the loss mechanisms,the infrared up-conversion photodetectors were optimized and achieved a breakthrough photon-to-photon conversion efficiency of 6.9%.This study provided valuable guidance on how to optimize the way of integration for up-conversion photodetectors.展开更多
Photocatalytic water splitting is beneficial for the effective mitigation of global energy and environmental crises.Owing to multi-exciton generation,impressive light harvesting,and excellent photochemical properties,...Photocatalytic water splitting is beneficial for the effective mitigation of global energy and environmental crises.Owing to multi-exciton generation,impressive light harvesting,and excellent photochemical properties,the quantum dot(QD)-based catalysts reveal a considerable potential in photocatalytic hydrogen(H_(2))production compared with bulk competitors.In this review,we summarize the recent advances in QDs for photocatalytic H_(2) production by enumerating different synthetic and characterization strategies for QDs.Various QDs-based photocatalysts are introduced and summarized in categories,and the role of different QDs in varied systems,as well as the mechanism and key factors that enhance the photocatalytic H_(2) generation performance,is discussed.Finally,conclusions and future perspectives in the exploration of highly efficient QDs-based photocatalysts for innovative applications are highlighted.展开更多
Heavy-metal-free ternary Cu–In–Se quantum dots(CISe QDs)are promising for solar fuel production because of their low toxicity,tunable band gap,and high light absorption coefficient.Although defects significantly aff...Heavy-metal-free ternary Cu–In–Se quantum dots(CISe QDs)are promising for solar fuel production because of their low toxicity,tunable band gap,and high light absorption coefficient.Although defects significantly affect the photophysical properties of QDs,the influence on photoelectrochemical hydrogen production is not well understood.Herein,we present the defect engineering of CISe QDs for efficient solar-energy conversion.Lewis acid–base reactions between metal halide–oleylamine complexes and oleylammonium selenocarbamate are modulated to achieve CISe QDs with the controlled amount of Cu vacancies without changing their morphology.Among them,CISe QDs with In/Cu=1.55 show the most outstanding photoelectrochemical hydrogen generation with excellent photocurrent density of up to 10.7 mA cm-2(at 0.6 VRHE),attributed to the suitable electronic band structures and enhanced carrier concentrations/lifetimes of the QDs.The proposed method,which can effectively control the defects in heavy-metal-free ternary QDs,offers a deeper understanding of the effects of the defects and provides a practical approach to enhance photoelectrochemical hydrogen generation.展开更多
Metal halide perovskites have generated significant attention in recent years because of their extraordinary physical properties and photovoltaic performance.Among these,inorganic perovskite quantum dots(QDs)stand out...Metal halide perovskites have generated significant attention in recent years because of their extraordinary physical properties and photovoltaic performance.Among these,inorganic perovskite quantum dots(QDs)stand out for their prominent merits,such as quantum confinement effects,high photoluminescence quantum yield,and defect-tolerant structures.Additionally,ligand engineering and an all-inorganic composition lead to a robust platform for ambient-stable QD devices.This review presents the state-of-the-art research progress on inorganic perovskite QDs,emphasizing their electronic applications.In detail,the physical properties of inorganic perovskite QDs will be introduced first,followed by a discussion of synthesis methods and growth control.Afterwards,the emerging applications of inorganic perovskite QDs in electronics,including transistors and memories,will be presented.Finally,this review will provide an outlook on potential strategies for advancing inorganic perovskite QD technologies.展开更多
Organometal halide perovskites are promising semiconducting materials for photodetectors because of their favorable optoelectrical properties.Although nanoscale perovskite materials such as quantum dots(QDs)show novel...Organometal halide perovskites are promising semiconducting materials for photodetectors because of their favorable optoelectrical properties.Although nanoscale perovskite materials such as quantum dots(QDs)show novel behavior,they have intrinsic stability issues.In this study,an effectively silane barrier-capped quantum dot(QD@APDEMS)is thinly applied onto a bulk perovskite photosensitive layer for use in photodetectors.QD@APDEMS is synthesized with a silane ligand with hydrophobic CH_(3)-terminal groups,resulting in excellent dispersibility and durability to enable effective coating.The introduction of the QD@APDEMS layer results in the formation of a lowdefect perovskite film with enlarged grains.This is attributed to the grain boundary interconnection effect via interaction between the functional groups of QD@APDEMS and uncoordinated Pb^(2+)in grain boundaries.By passivating the grain boundaries,where various trap sites are distributed,hole chargecarrier injection and shunt leakage can be suppressed.Also,from the energy point of view,the deep highest occupied molecular orbital(HOMO)level of QD@APDEMS can work as a hole charge injection barrier.Improved charge dynamics(generation,transfer,and recombination properties)and reduced trap density of QD@APDEMS are demonstrated.When this perovskite film is used in a photodetector,the device performance(especially the detectivity)stands out among existing perovskites evaluated for energy sensing device applications.展开更多
The mercury species in the ocean(MeHg,Hg^(2+))will be enriched in marine organisms and threaten human health through the food chain.While the excessive H_(2)O_(2)in the metabolic process will produce hydroxyl radicals...The mercury species in the ocean(MeHg,Hg^(2+))will be enriched in marine organisms and threaten human health through the food chain.While the excessive H_(2)O_(2)in the metabolic process will produce hydroxyl radicals and accelerate the aging of human cells,causing a series of diseases.Hence,the cost-effective and rapid detection of mercury and H_(2)O_(2)is of urgent requirement and significance.Here,we synthesized emerging graphitic carbon nitride quantum dots(g-CNQDs)with high fluorescence quantum yield(FLQY)of 42.69%via a bottom-up strategy by a facile one-step hydrothermal method.The g-CNQDs can detect the H_(2)O_(2)and Hg^(2+)through the fluorescence quenching effect between g-CNQDs and detected substances.With the presence of KI,g-CNQDs show concentration-dependent fluorescence toward H_(2)O_(2),with a wide detection range of 1–1000μmolL^(-1)and a low detection limit of 0.23μmolL^(-1).The g-CNQDs also show sensitivity toward Hg^(2+)with a detection range of 0–0.1μmolL^(-1)and a detection limit of 0.038μmolL^(-1).This dual-function detection of g-CNQDs has better practical application capability compared to other quantum dot detection.This study may provide a new strategy for g-CNQDs preparation and construct a fluorescence probe that can be used in various systems involving H_(2)O_(2)and Hg^(2+),providing better support for future bifunctional or multifunction studies.展开更多
The development of lithium-sulfur(Li-S) battery as one of the most attractive energy storage systems among lithium metal batteries is seriously hindered by low sulfur utilization, poor cycle stability and uneven redep...The development of lithium-sulfur(Li-S) battery as one of the most attractive energy storage systems among lithium metal batteries is seriously hindered by low sulfur utilization, poor cycle stability and uneven redeposition of Li anode. It is necessary to propose strategies to address the problems as well as improve the electrochemical performance. One of the effective solutions is to improve the sulfiphilicity of sulfur cathode and the lithiophilicity of the Li anode. Herein, we reported that a synergistic functional separator(graphene quantum dots(GQDs)-polyacrylonitrile(PAN) @polypropylene(PP) separator)improved the electrochemical activity of sulfur cathode as well as the stability of Li anode. GQDs induced uniform Li^(+)nucleation and deposition, which slowed down the passivation of Li anode and avoided shortcircuit. Further, three-dimensional network constructed by electrospinning nanofibers and the polar functional groups of GQDs could both effectively inhibit the shuttle of LiPSs and improve the sulfur utilization. The stability of Li-S battery was improved by the synergistic effect. In addition, GQDs and electrospinning nanofibers protector increased lifetime of separators. Benefiting from the unique design strategy, Li//Li symmetric battery with GQDs-PAN@PP separators exhibited stably cycling for over 600 h. More importantly, the Li-S full batteries based GQDs-PAN@PP separators enabled high stability and desirable sulfur electrochemistry, including high reversibility of 558.09 mA h g^(-1)for 200 cycles and durable life with a low fading rate of 0.075% per cycle after 500 cycles at 0.5 C. Moreover, an impressive areal capacity of 3.23 mA h cm^(-2)was maintained under high sulfur loading of 5.10 mg cm^(-2). This work provides a new insight for modification separator to improve the electrochemical performance of Li-S/Li metal batteries.展开更多
Cost-effective,safe,and highly performing energy storage devices require rechargeable batteries,and among various options,aqueous zinc-ion batteries(ZIBs)have shown high promise in this regard.As a cathode material fo...Cost-effective,safe,and highly performing energy storage devices require rechargeable batteries,and among various options,aqueous zinc-ion batteries(ZIBs)have shown high promise in this regard.As a cathode material for the aqueous ZIBs,manganese dioxide(MnO_(2))has been found to be promising,but certain drawbacks of this cathode material are slow charge-transfer capability and poor cycling performance.Herein,a novel design of graphene quantum dots(GQDs)integrated with Zn-intercalated MnO_(2)nanosheets is put forward to construct a 3D nanoflower-like GQDs@ZnxMnO_(2)composite cathode for aqueous ZIBs.The synergistic coupling of GQDs modification with Zn intercalation provides abundant active sites and conductive medium to facilitate the ion/electron transmission,as well as ensure the GQDs@ZnxMnO_(2)composite cathode with enhanced charge-transfer capability and high electrochemical reversibility,which are elucidated by experiment results and in-situ Raman investigation.These impressive properties endow the GQDs@ZnxMnO_(2)composite cathode with superior aqueous Zn^(2+) storage capacity(~403.6 mAh·g^(−1)),excellent electrochemical kinetics,and good structural stability.For actual applications,the fabricated aqueous ZIBs can deliver a substantial energy density(226.8 W·h·kg^(−1)),a remarkable power density(650 W·kg^(−1)),and long-term cycle performance,further stimulating their potential application as efficient electrochemical storage devices for various energy-related fields.展开更多
The commercial viability of lithium-sulfur batteries is still challenged by the notorious lithium polysulfides(Li PSs)shuttle effect on the sulfur cathode and uncontrollable Li dendrites growth on the Li anode.Herein,...The commercial viability of lithium-sulfur batteries is still challenged by the notorious lithium polysulfides(Li PSs)shuttle effect on the sulfur cathode and uncontrollable Li dendrites growth on the Li anode.Herein,a bi-service host with Co-Fe binary-metal selenide quantum dots embedded in three-dimensional inverse opal structured nitrogen-doped carbon skeleton(3DIO FCSe-QDs@NC)is elaborately designed for both sulfur cathode and Li metal anode.The highly dispersed FCSe-QDs with superb adsorptive-catalytic properties can effectively immobilize the soluble Li PSs and improve diffusion-conversion kinetics to mitigate the polysulfide-shutting behaviors.Simultaneously,the 3D-ordered porous networks integrated with abundant lithophilic sites can accomplish uniform Li deposition and homogeneous Li-ion flux for suppressing the growth of dendrites.Taking advantage of these merits,the assembled Li-S full batteries with 3DIO FCSe-QDs@NC host exhibit excellent rate performance and stable cycling ability(a low decay rate of 0.014%over 2,000 cycles at 2C).Remarkably,a promising areal capacity of 8.41 mAh cm^(-2)can be achieved at the sulfur loading up to 8.50 mg cm^(-2)with an ultra-low electrolyte/sulfur ratio of 4.1μL mg^(-1).This work paves the bi-serve host design from systematic experimental and theoretical analysis,which provides a viable avenue to solve the challenges of both sulfur and Li electrodes for practical Li-S full batteries.展开更多
The hydrogen evolution reaction performance of semiconducting 2H-phase molybdenum disulfide(2H-MoS_(2))presents a significant hurdle in realizing its full potential applications.Here,we utilize theoretical calculation...The hydrogen evolution reaction performance of semiconducting 2H-phase molybdenum disulfide(2H-MoS_(2))presents a significant hurdle in realizing its full potential applications.Here,we utilize theoretical calculations to predict possible functionalized graphene quantum dots(GQDs),which can enhance HER activity of bulk MoS_(2).Subsequently,we design a functionalized GQD-induced in-situ bottom-up strategy to fabricate near atom-layer 2H-MoS_(2) nanosheets mediated with GQDs(ALQD)by modulating the concentration of electron withdrawing/donating functional groups.Experimental results reveal that the introduction of a series of functionalized GQDs during the synthesis of ALQD plays a crucial role.Notably,the higher the concentration and strength of electron-withdrawing functional groups on GQDs,the thinner and more active the resulting ALQD are.Remarkably,the synthesized near atom-layer ALQD-SO_(3)demonstrate significantly improved HER performance.Our GQD-induced strategy provides a simple and efficient approach for expanding the catalytic application of MoS_(2).Furthermore,it holds substantial potential for developing nanosheets in other transition-metal dichalcogenide materials.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos.U2002212,52102058,52204414,52204413,and 52204412)the National Key R&D Program of China (Nos.2021YFC1910504,2019YFC1907101,2019YFC1907103,and 2017YFB0702304)+7 种基金the Key R&D Program of Ningxia Hui Autonomous Region,China (Nos.2021BEG01003 and2020BCE01001)the Xijiang Innovation and Entrepreneurship Team,China (No.2017A0109004)the Macao Young Scholars Program (No.AM2022024),Chinathe Beijing Natural Science Foundation (Nos.L212020 and 2214073),Chinathe Guangdong Basic and Applied Basic Research Foundation,China (Nos.2021A1515110998 and 2020A1515110408)the China Postdoctoral Science Foundation (No.2022M710349)the Fundamental Research Funds for the Central Universities,China (Nos.FRF-BD-20-24A,FRF-TP-20-031A1,FRF-IC-19-017Z,and 06500141)the Integration of Green Key Process Systems MIIT and Scientific and Technological Innovation Foundation of Foshan,China(Nos.BK22BE001 and BK21BE002)。
文摘Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.12074368,92165207,12034018,and 62004185)the Anhui Province Natural Science Foundation (Grant No.2108085J03)the USTC Tang Scholarship。
文摘The single-shot readout data process is essential for the realization of high-fidelity qubits and fault-tolerant quantum algorithms in semiconductor quantum dots. However, the fidelity and visibility of the readout process are sensitive to the choice of the thresholds and limited by the experimental hardware. By demonstrating the linear dependence between the measured spin state probabilities and readout visibilities along with dark counts, we describe an alternative threshold-independent method for the single-shot readout of spin qubits in semiconductor quantum dots. We can obtain the extrapolated spin state probabilities of the prepared probabilities of the excited spin state through the threshold-independent method. We then analyze the corresponding errors of the method, finding that errors of the extrapolated probabilities cannot be neglected with no constraints on the readout time and threshold voltage. Therefore, by limiting the readout time and threshold voltage, we ensure the accuracy of the extrapolated probability. We then prove that the efficiency and robustness of this method are 60 times larger than those of the most commonly used method. Moreover, we discuss the influence of the electron temperature on the effective area with a fixed external magnetic field and provide a preliminary demonstration for a single-shot readout of up to 0.7K/1.5T in the future.
文摘This research investigates the hydrothermal synthesis and annealing duration effects on nickel sulfide(NiS_(2)quantum dots(QDs)for catalytic decolorization of methylene blue(MB)dye and antimicrobial efficacy.QD size increased with longer annealing,reducing catalytic activity.UV–vis,XRD,TEM,and FTIR analyses probed optical structural,morphological,and vibrational features.XRD confirmed NiS2's anorthic structure,with crystallite size growing from 6.53 to 7.81 nm during extended annealing.UV–Vis exhibited a bathochromic shift,reflecting reduced band gap energy(Eg)in NiS_(2).TEM revealed NiS_(2)QD formation,with agglomerated QD average size increasing from 7.13 to 9.65 nm with prolonged annealing.Pure NiS_(2)showed significant MB decolorization(89.85%)in acidic conditions.Annealed NiS_(2) QDs demonstrated notable antibacterial activity,yielding a 6.15mm inhibition zone against Escherichia coli(E.coli)compared to Ciprofloxacin.First-principles computation supported a robust interaction between MB and NiS_(2),evidenced by obtained adsorption energies.This study highlights the nuanced relationship between annealing duration,structural changes,and functional properties in NiS_(2)QDs,emphasizing their potential applications in catalysis and antibacterial interventions.
基金supported by the National Natural Science Foundation of China(Grant No.52102266,12204167)the China Postdoctoral Science Foundation(2020M680861)+4 种基金the support from the Department of Science and Technology-Science and Engineering Research Board(DST-SERB),Government of India(project no.SRG/2020/000258)CSIR-Indian Institute of Chemical Technology,Hyderabadsupported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2022R1A5A1032539,2022R1C1C1008282)Industrial Strategic Technology Development Program-Alchemist Project(1415180859,Chiral perovskite LED smart contact lens based hyper vision metaverse)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)Korea Evaluation Institute of Industrial Technology(KEIT,Korea).
文摘As lead halide perovskite(LHP)semiconductors have shown tremendous promise in many application fields,and particularly made strong impact in the solar photovoltaic area,low dimensional quantum dot forms of these perovskites are showing the potential to make distinct marks in the fields of electronics,optoelectronics and photonics.The so-called perovskite quantum dots(PQDs)not only possess the most important features of LHP materials,i.e.,the unusual high defect tolerance,but also demonstrate clear quantum size effects,along with exhibiting desirable optoelectronic properties such as near perfect photoluminescent quantum yield,multiple exciton generation and slow hot-carrier cooling.Here,we review the advantageous properties of these nanoscale perovskites and survey the prospects for diverse applications which include lightemitting devices,solar cells,photocatalysts,lasers,detectors and memristors,emphasizing the distinct superiorities as well as the challenges.
基金Funded by the Natural Science Foundation of Hubei Province(No.2022CFB861)the Wenhua College Research and Innovation Team(No.2022T01)。
文摘A composite was created by incorporating the quantum dot-enhanced SiO_(2)nanoparticles within this hydrogel.Based on this composite,a temperature-controlled fluorescent probe for DCP was developed.A meticulous examination of this probe revealed its attributes and factors affecting its performance.By using temperature modulation,the probe was adept at detecting DCP concentrations ranging between 1.0×10^(-6)and 9.0×10^(-6)mol/L.Such a probe offers remarkable selectivity,repeatability,and robust stability,so that the detection of DCP can be carried out at different temperatures,and a fast,reliable,sensitive and low-cost intelligent detection method is realized.
基金Project supported by the National Natural Science Foundation of China (Grant No.11834005)。
文摘The combination of non-Hermitian physics and Majorana fermions can give rise to new effects in quantum transport systems. In this work, we investigate the interplay of PT-symmetric complex potentials, Majorana tunneling and interdot tunneling in a non-Hermitian double quantum dots system. It is found that in the weak-coupling regime the Majorana tunneling has pronounced effects on the transport properties of such a system, manifested as splitting of the single peak into three and a reduced 1/4 peak in the transmission function. In the presence of the PT-symmetric complex potentials and interdot tunneling, the 1/4 central peak is robust against them, while the two side peaks are tuned by them. The interdot tunneling only induces asymmetry, instead of moving the conductance peak, due to the robustness of the Majorana modes. There is an exceptional point induced by the union of Majorana tunneling and interdot tunneling. With increased PT-symmetric complex potentials, the two side peaks will move towards each other. When the exceptional point is passed through, these two side peaks will disappear. In the strong-coupling regime, the Majorana fermion induces a 1/4 conductance dip instead of the three-peak structure. PT-symmetric complex potentials induce two conductance dips pinned at the exceptional point. These effects should be accessible in experiments.
基金supported by the open research fund of Songshan Lake Materials Laboratory (2022SLABFN26)the National Natural Science Foundation of China (21773024)+1 种基金the Sichuan Science and Technology program (2020YJ0324,2020YJ0262)the Reformation and Development Funds for Local Region Universities from China Government in 2020 (ZCKJ 2020-11)。
文摘The shuttle effect of lithium polysulfides(LiPSs)and uncontrollable lithium dendrite growth seriously hinder the practical application of lithium-sulfur(Li-S)batteries.To simultaneously address such issues,monodispersed Nb N quantum dots anchored on nitrogen-doped hollow carbon nanorods(NbN@NHCR)are elaborately developed as efficient Li PSs immobilizer and Li stabilizer for high-performance Li-S full batteries.Density functional theory(DFT)calculations and experimental characterizations demonstrate that the sulfiphilic and lithiophilic NbN@NHCR hybrid can not only efficiently immobilize the soluble Li PSs and facilitate diffusion-conversion kinetics for alleviating the shuttling effect,but also homogenize the distribution of Li+ions and regulate uniform Li deposition for suppressing Li-dendrite growth.As a result,the assembled Li-S full batteries(NbN@NHCR-S||Nb N@NHCR-Li)deliver excellent long-term cycling stability with a low decay rate of 0.031%per cycle over 1000 cycles at high rate of 2 C.Even at a high S loading of 5.8 mg cm^(-2)and a low electrolyte/sulfur ratio of 5.2μL mg^(-1),a large areal capacity of 6.2 mA h cm^(-2)can be achieved in Li-S pouch cell at 0.1 C.This study provides a new perspective via designing a dual-functional sulfiphilic and lithiophilic hybrid to address serious issues of the shuttle effect of S cathode and dendrite growth of Li anode.
基金supported by the National Natural Science Foundation of China(Grant Nos.12274454,11774418,11374363,11674317,11974348,11834014,and 21373191)the Strategic Priority Research Program of CAS(Grant Nos.XDB28000000 and XDB33000000)+2 种基金the National Natural Science Foundation of China(Grant No.11974348)the Training Program of Major Research Plan of NSFC(Grant No.92165105)the Outstanding Innovative Talents Cultivation Funded Programs 2023 of Renmin University of China。
文摘We utilize the calculation of hierarchical equations of motion to demonstrate that the spin-dependent properties between adjacent quantum dots(QDs)can be changed by breaking the internal symmetry configuration,corresponding to the inversion of dominant chiral states.In the linear triple quantum dots(LTQDs)connected to two electron reservoirs,we can observe that the blockage appears at the triangle triple quantum dots(TTQDs)by gradually increasing the coupling strength between next-nearest double QDs.When the initial coupling between LTQDs has altered,the internal chiral circulation also undergoes the corresponding transform,thus achieving qualitative regulation and detection of the blocking region.We also investigate the response of the chiral circulation to the dot–lead coupling strength,indicating the overall robust chiral circulation of the TTQDs frustration.
基金National Natural Science Foundation of China,Grant/Award Number:51971065Innovation Program of Shanghai Municipal Education Commission,Grant/Award Number:2019-01-07-00-07-E00028。
文摘SnO_(2) has been extensively investigated as an anode material for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs)due to its high Na/K storage capacity,high abundance,and low toxicity.However,the sluggish reaction kinetics,low electronic conductivity,and large volume changes during charge and discharge hinder the practical applications of SnO_(2)-based electrodes for SIBs and PIBs.Engineering rational structures with fast charge/ion transfer and robust stability is important to overcoming these challenges.Herein,S-doped SnO_(2)(S-SnO_(2))quantum dots(QDs)(≈3 nm)encapsulated in an N,S codoped carbon fiber networks(S-SnO_(2)-CFN)are rationally fabricated using a sequential freeze-drying,calcination,and S-doping strategy.Experimental analysis and density functional theory calculations reveal that the integration of S-SnO_(2) QDs with N,S codoped carbon fiber network remarkably decreases the adsorption energies of Na/K atoms in the interlayer of SnO_(2)-CFN,and the S doping can increase the conductivity of SnO_(2),thereby enhancing the ion transfer kinetics.The synergistic interaction between S-SnO_(2) QDs and N,S codoped carbon fiber network results in a composite with fast Na+/K+storage and extraordinary long-term cyclability.Specifically,the S-SnO_(2)-CFN delivers high rate capacities of 141.0 mAh g^(−1) at 20 A g^(−1) in SIBs and 102.8 mAh g^(−1) at 10 A g^(−1) in PIBs.Impressively,it delivers ultra-stable sodium storage up to 10,000 cycles at 5 A g^(−1) and potassium storage up to 5000 cycles at 2 A g^(−1).This study provides insights into constructing metal oxide-based carbon fiber network structures for high-performance electrochemical energy storage and conversion devices.
基金This work was financially supported by the National Key Research and Development Program of China(2022YFB3602902)the Key Projects of National Natural Science Foundation of China(62234004)+5 种基金Innovation and Entrepreneurship Team of Zhejiang Province(2021R01003)Science and Technology Innovation 2025 Major Project of Ningbo(2022Z085)Ningbo 3315 Programme(2020A-01-B)YONGJIANG Talent Introduction Programme(2021A-038-B)Flexible Electronics Zhejiang Province Key Laboratory Fund Project(2022FEO02)Zhejiang Provincial Natural Science Foundation of China(LR21F050001).
文摘CsPbI_(3)perovskite quantum dots(QDs)are ideal materials for the next generation of red light-emitting diodes.However,the low phase stability of CsPbI_(3)QDs and long-chain insulating capping ligands hinder the improvement of device performance.Traditional in-situ ligand replacement and ligand exchange after synthesis were often difficult to control.Here,we proposed a new ligand exchange strategy using a proton-prompted insitu exchange of short 5-aminopentanoic acid ligands with long-chain oleic acid and oleylamine ligands to obtain stable small-size CsPbI_(3)QDs.This exchange strategy maintained the size and morphology of CsPbI_(3)QDs and improved the optical properties and the conductivity of CsPbI_(3)QDs films.As a result,high-efficiency red QD-based light-emitting diodes with an emission wavelength of 645 nm demonstrated a record maximum external quantum efficiency of 24.45%and an operational half-life of 10.79 h.
基金supported by the following research fundings including:the National Natural Science Foundation of China(Nos.62005114,62204078 and U22A2072)Natural Science Foundation of Henan-Excellent Youth Scholar(No.232300421092)Open Fund of the State Key Laboratory of Integrated Optoelectronics+(IOSKL2020KF01).
文摘Quantum dot-based up-conversion photodetector,in which an infrared photodiode(PD)and a quantum dot light-emitting diode(QLED)are back-to-back connected,is a promising candidate for low-cost infrared imaging.However,the huge efficiency losses caused by integrating the PD and QLED together hasn’t been studied sufficiently.This work revealed at least three origins for the efficiency losses.First,the PD unit and QLED unit usually didn’t work under optimal conditions at the same time.Second,the potential barriers and traps at the interconnection between PD and QLED units induced unfavorable carrier recombination.Third,much emitted visible light was lost due to the strong visible absorption in the PD unit.Based on the understandings on the loss mechanisms,the infrared up-conversion photodetectors were optimized and achieved a breakthrough photon-to-photon conversion efficiency of 6.9%.This study provided valuable guidance on how to optimize the way of integration for up-conversion photodetectors.
基金Taishan Youth Scholar Program of Shandong ProvinceNational Natural Science Foundation of China,Grant/Award Numbers:21972058,21975110,22088102,51825205+3 种基金Postgraduate Practice Research Innovation Program of Jiangsu Province,Grant/Award Number:SJCX21_1707CAS Project for Young Scientists in Basic Research,Grant/Award Number:YSBR‐004DNL Cooperation Fund,CAS,Grant/Award Number:DNL202016National Key Projects for Fundamental Research and Development of China,Grant/Award Number:2018YFB1502002。
文摘Photocatalytic water splitting is beneficial for the effective mitigation of global energy and environmental crises.Owing to multi-exciton generation,impressive light harvesting,and excellent photochemical properties,the quantum dot(QD)-based catalysts reveal a considerable potential in photocatalytic hydrogen(H_(2))production compared with bulk competitors.In this review,we summarize the recent advances in QDs for photocatalytic H_(2) production by enumerating different synthetic and characterization strategies for QDs.Various QDs-based photocatalysts are introduced and summarized in categories,and the role of different QDs in varied systems,as well as the mechanism and key factors that enhance the photocatalytic H_(2) generation performance,is discussed.Finally,conclusions and future perspectives in the exploration of highly efficient QDs-based photocatalysts for innovative applications are highlighted.
基金the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(grant nos.2021R1C1C1007844,2021M3I3A1085039,2020R1F1A1061505,and 2020R1C1C1012014).
文摘Heavy-metal-free ternary Cu–In–Se quantum dots(CISe QDs)are promising for solar fuel production because of their low toxicity,tunable band gap,and high light absorption coefficient.Although defects significantly affect the photophysical properties of QDs,the influence on photoelectrochemical hydrogen production is not well understood.Herein,we present the defect engineering of CISe QDs for efficient solar-energy conversion.Lewis acid–base reactions between metal halide–oleylamine complexes and oleylammonium selenocarbamate are modulated to achieve CISe QDs with the controlled amount of Cu vacancies without changing their morphology.Among them,CISe QDs with In/Cu=1.55 show the most outstanding photoelectrochemical hydrogen generation with excellent photocurrent density of up to 10.7 mA cm-2(at 0.6 VRHE),attributed to the suitable electronic band structures and enhanced carrier concentrations/lifetimes of the QDs.The proposed method,which can effectively control the defects in heavy-metal-free ternary QDs,offers a deeper understanding of the effects of the defects and provides a practical approach to enhance photoelectrochemical hydrogen generation.
基金The authors thank the support from the Australian Research Council(DP190103316)UNSW SHARP Project(RG163043).
文摘Metal halide perovskites have generated significant attention in recent years because of their extraordinary physical properties and photovoltaic performance.Among these,inorganic perovskite quantum dots(QDs)stand out for their prominent merits,such as quantum confinement effects,high photoluminescence quantum yield,and defect-tolerant structures.Additionally,ligand engineering and an all-inorganic composition lead to a robust platform for ambient-stable QD devices.This review presents the state-of-the-art research progress on inorganic perovskite QDs,emphasizing their electronic applications.In detail,the physical properties of inorganic perovskite QDs will be introduced first,followed by a discussion of synthesis methods and growth control.Afterwards,the emerging applications of inorganic perovskite QDs in electronics,including transistors and memories,will be presented.Finally,this review will provide an outlook on potential strategies for advancing inorganic perovskite QD technologies.
基金Ministry of Trade,Industry and Energy,Grant/Award Numbers:20017439,20021915National Research Foundation of Korea,Grant/Award Number:2019R1A2C1087653。
文摘Organometal halide perovskites are promising semiconducting materials for photodetectors because of their favorable optoelectrical properties.Although nanoscale perovskite materials such as quantum dots(QDs)show novel behavior,they have intrinsic stability issues.In this study,an effectively silane barrier-capped quantum dot(QD@APDEMS)is thinly applied onto a bulk perovskite photosensitive layer for use in photodetectors.QD@APDEMS is synthesized with a silane ligand with hydrophobic CH_(3)-terminal groups,resulting in excellent dispersibility and durability to enable effective coating.The introduction of the QD@APDEMS layer results in the formation of a lowdefect perovskite film with enlarged grains.This is attributed to the grain boundary interconnection effect via interaction between the functional groups of QD@APDEMS and uncoordinated Pb^(2+)in grain boundaries.By passivating the grain boundaries,where various trap sites are distributed,hole chargecarrier injection and shunt leakage can be suppressed.Also,from the energy point of view,the deep highest occupied molecular orbital(HOMO)level of QD@APDEMS can work as a hole charge injection barrier.Improved charge dynamics(generation,transfer,and recombination properties)and reduced trap density of QD@APDEMS are demonstrated.When this perovskite film is used in a photodetector,the device performance(especially the detectivity)stands out among existing perovskites evaluated for energy sensing device applications.
基金support from the Natural Science Foundation of Shandong Province(No.ZR2021 MB075)National Natural Science Foundation of China(No.51602297)the Opening Fund of State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering(No.2021-K53).
文摘The mercury species in the ocean(MeHg,Hg^(2+))will be enriched in marine organisms and threaten human health through the food chain.While the excessive H_(2)O_(2)in the metabolic process will produce hydroxyl radicals and accelerate the aging of human cells,causing a series of diseases.Hence,the cost-effective and rapid detection of mercury and H_(2)O_(2)is of urgent requirement and significance.Here,we synthesized emerging graphitic carbon nitride quantum dots(g-CNQDs)with high fluorescence quantum yield(FLQY)of 42.69%via a bottom-up strategy by a facile one-step hydrothermal method.The g-CNQDs can detect the H_(2)O_(2)and Hg^(2+)through the fluorescence quenching effect between g-CNQDs and detected substances.With the presence of KI,g-CNQDs show concentration-dependent fluorescence toward H_(2)O_(2),with a wide detection range of 1–1000μmolL^(-1)and a low detection limit of 0.23μmolL^(-1).The g-CNQDs also show sensitivity toward Hg^(2+)with a detection range of 0–0.1μmolL^(-1)and a detection limit of 0.038μmolL^(-1).This dual-function detection of g-CNQDs has better practical application capability compared to other quantum dot detection.This study may provide a new strategy for g-CNQDs preparation and construct a fluorescence probe that can be used in various systems involving H_(2)O_(2)and Hg^(2+),providing better support for future bifunctional or multifunction studies.
基金supported by Key Program (U20A20235) funded by National Natural Science Foundation of Chinathe National Natural Science Foundation of China (52171127, 51974242)+2 种基金Regional Innovation Capability Guidance Program of Shaanxi Provincial Government (2022QFY10-06)Key R&D Program of Xianyang Science and Technology Bureau (2021ZDYF-GY-0029)Doctoral dissertation innovation fund (310-252072201) by Xi’an University of Technology。
文摘The development of lithium-sulfur(Li-S) battery as one of the most attractive energy storage systems among lithium metal batteries is seriously hindered by low sulfur utilization, poor cycle stability and uneven redeposition of Li anode. It is necessary to propose strategies to address the problems as well as improve the electrochemical performance. One of the effective solutions is to improve the sulfiphilicity of sulfur cathode and the lithiophilicity of the Li anode. Herein, we reported that a synergistic functional separator(graphene quantum dots(GQDs)-polyacrylonitrile(PAN) @polypropylene(PP) separator)improved the electrochemical activity of sulfur cathode as well as the stability of Li anode. GQDs induced uniform Li^(+)nucleation and deposition, which slowed down the passivation of Li anode and avoided shortcircuit. Further, three-dimensional network constructed by electrospinning nanofibers and the polar functional groups of GQDs could both effectively inhibit the shuttle of LiPSs and improve the sulfur utilization. The stability of Li-S battery was improved by the synergistic effect. In addition, GQDs and electrospinning nanofibers protector increased lifetime of separators. Benefiting from the unique design strategy, Li//Li symmetric battery with GQDs-PAN@PP separators exhibited stably cycling for over 600 h. More importantly, the Li-S full batteries based GQDs-PAN@PP separators enabled high stability and desirable sulfur electrochemistry, including high reversibility of 558.09 mA h g^(-1)for 200 cycles and durable life with a low fading rate of 0.075% per cycle after 500 cycles at 0.5 C. Moreover, an impressive areal capacity of 3.23 mA h cm^(-2)was maintained under high sulfur loading of 5.10 mg cm^(-2). This work provides a new insight for modification separator to improve the electrochemical performance of Li-S/Li metal batteries.
基金financially supported by the National Nature Science Foundations of China (Nos. 52002157 and 51873083)the Nature Science Foundations of Jiangsu Province, China (No. BK20190976)
文摘Cost-effective,safe,and highly performing energy storage devices require rechargeable batteries,and among various options,aqueous zinc-ion batteries(ZIBs)have shown high promise in this regard.As a cathode material for the aqueous ZIBs,manganese dioxide(MnO_(2))has been found to be promising,but certain drawbacks of this cathode material are slow charge-transfer capability and poor cycling performance.Herein,a novel design of graphene quantum dots(GQDs)integrated with Zn-intercalated MnO_(2)nanosheets is put forward to construct a 3D nanoflower-like GQDs@ZnxMnO_(2)composite cathode for aqueous ZIBs.The synergistic coupling of GQDs modification with Zn intercalation provides abundant active sites and conductive medium to facilitate the ion/electron transmission,as well as ensure the GQDs@ZnxMnO_(2)composite cathode with enhanced charge-transfer capability and high electrochemical reversibility,which are elucidated by experiment results and in-situ Raman investigation.These impressive properties endow the GQDs@ZnxMnO_(2)composite cathode with superior aqueous Zn^(2+) storage capacity(~403.6 mAh·g^(−1)),excellent electrochemical kinetics,and good structural stability.For actual applications,the fabricated aqueous ZIBs can deliver a substantial energy density(226.8 W·h·kg^(−1)),a remarkable power density(650 W·kg^(−1)),and long-term cycle performance,further stimulating their potential application as efficient electrochemical storage devices for various energy-related fields.
基金financial support from the National Natural Science Foundation of China(Grant Nos.51871188 and 51931006)the Fundamental Research Funds for the Central Universities of China(Xiamen University:Nos.20720200068,20720190007 and 20720220074)+2 种基金Guangdong Basic and Applied Basic Research Foundation(No.2021A1515010139)Science and Technology Projects of Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(HRTP-[2022]-22)the“Double-First Class”Foundation of Materials Intelligent Manufacturing Discipline of Xiamen University。
文摘The commercial viability of lithium-sulfur batteries is still challenged by the notorious lithium polysulfides(Li PSs)shuttle effect on the sulfur cathode and uncontrollable Li dendrites growth on the Li anode.Herein,a bi-service host with Co-Fe binary-metal selenide quantum dots embedded in three-dimensional inverse opal structured nitrogen-doped carbon skeleton(3DIO FCSe-QDs@NC)is elaborately designed for both sulfur cathode and Li metal anode.The highly dispersed FCSe-QDs with superb adsorptive-catalytic properties can effectively immobilize the soluble Li PSs and improve diffusion-conversion kinetics to mitigate the polysulfide-shutting behaviors.Simultaneously,the 3D-ordered porous networks integrated with abundant lithophilic sites can accomplish uniform Li deposition and homogeneous Li-ion flux for suppressing the growth of dendrites.Taking advantage of these merits,the assembled Li-S full batteries with 3DIO FCSe-QDs@NC host exhibit excellent rate performance and stable cycling ability(a low decay rate of 0.014%over 2,000 cycles at 2C).Remarkably,a promising areal capacity of 8.41 mAh cm^(-2)can be achieved at the sulfur loading up to 8.50 mg cm^(-2)with an ultra-low electrolyte/sulfur ratio of 4.1μL mg^(-1).This work paves the bi-serve host design from systematic experimental and theoretical analysis,which provides a viable avenue to solve the challenges of both sulfur and Li electrodes for practical Li-S full batteries.
基金This research was supported by Shanghai Pujiang Program(21PJD022)National Natural Science Foundation of China(21901154).
文摘The hydrogen evolution reaction performance of semiconducting 2H-phase molybdenum disulfide(2H-MoS_(2))presents a significant hurdle in realizing its full potential applications.Here,we utilize theoretical calculations to predict possible functionalized graphene quantum dots(GQDs),which can enhance HER activity of bulk MoS_(2).Subsequently,we design a functionalized GQD-induced in-situ bottom-up strategy to fabricate near atom-layer 2H-MoS_(2) nanosheets mediated with GQDs(ALQD)by modulating the concentration of electron withdrawing/donating functional groups.Experimental results reveal that the introduction of a series of functionalized GQDs during the synthesis of ALQD plays a crucial role.Notably,the higher the concentration and strength of electron-withdrawing functional groups on GQDs,the thinner and more active the resulting ALQD are.Remarkably,the synthesized near atom-layer ALQD-SO_(3)demonstrate significantly improved HER performance.Our GQD-induced strategy provides a simple and efficient approach for expanding the catalytic application of MoS_(2).Furthermore,it holds substantial potential for developing nanosheets in other transition-metal dichalcogenide materials.