Moirésystems have emerged as an ideal platform for exploring interaction effects and correlated states.However,most of the experimental systems are based on either triangular or honeycomb lattices.In this study,b...Moirésystems have emerged as an ideal platform for exploring interaction effects and correlated states.However,most of the experimental systems are based on either triangular or honeycomb lattices.In this study,based on the self-consistent Hartree–Fock calculation,we investigate the phase diagram of the kagomélattice in a recently discovered system with two degenerateΓvalley orbitals and strong spin–orbit coupling.By focusing on the filling factors of 1/2,1/3 and 2/3,we identify various symmetry-breaking states by adjusting the screening length and dielectric constant.At the half filling,we discover that the spin–orbit coupling induces Dzyaloshinskii–Moriya interaction and stabilizes a classical magnetic state with 120°ordering.Additionally,we observe a transition to a ferromagnetic state with out-of-plane ordering.In the case of 1/3 filling,the system is ferromagnetically ordered due to the lattice frustration.Furthermore,for 2/3 filling,the system exhibits a pinned droplet state and a 120°magnetic ordered state at weak and immediate coupling strengths,respectively.For the strong coupling case,when dealing with non-integer filling,the system is always charge ordered with sublattice polarization.Our study serves as a starting point for exploring the effects of correlation in moirékagomésystems.展开更多
We investigate electron mesoscopic transport in a three-terminal setup with coupled quantum dots and a magnetic flux.By mapping the original transport problem into a non-Hermitian Hamiltonian form,we study the interpl...We investigate electron mesoscopic transport in a three-terminal setup with coupled quantum dots and a magnetic flux.By mapping the original transport problem into a non-Hermitian Hamiltonian form,we study the interplay between the coherent couplings between quantum dots,the magnetic flux,and the dissipation due to the tunnel coupling with the reservoirs.展开更多
Hypernuclei,nuclei containing one or more hyperons,serve as unique laboratories for probing the non-perturbative quantum chromodynamics(QCD).Recent progress in hypernuclear physics,driven by advanced experimental tech...Hypernuclei,nuclei containing one or more hyperons,serve as unique laboratories for probing the non-perturbative quantum chromodynamics(QCD).Recent progress in hypernuclear physics,driven by advanced experimental techniques and theoretical innovations,is briefly reviewed with a focus on key findings and unresolved challenges,such as the precise determination of the hypertriton binding energy,investigations of charge symmetry breaking in mirror hypernuclei,and the search for exotic systems,including the neutral nnΛstate.Experimental breakthroughs,including invariant-mass analyses and femtoscopy studies in heavy-ion collisions,as well as high-resolutionγ-spectroscopy,have enabled precise studies of light hypernuclei and offered critical insights into the hyperon–nucleon interaction.Theoretical progress,including ab initio calculations based on chiral effective field theory and lattice QCD,has further enhanced our understanding of hyperon–nucleon and hyperon–hyperon interactions.展开更多
In this study,a straightforward one-step hydrothermal method was successfully utilized to synthesize the solid solution Na_(0.9)Mg_(0.45)Ti_(3.55)O_(8)-Na_(2)Ni_(2)Ti_(6)O_(16)(NNMTO-x),where x denotes the molar perce...In this study,a straightforward one-step hydrothermal method was successfully utilized to synthesize the solid solution Na_(0.9)Mg_(0.45)Ti_(3.55)O_(8)-Na_(2)Ni_(2)Ti_(6)O_(16)(NNMTO-x),where x denotes the molar percentage of Na_(2)Ni_(2)Ti_(6)O_(16)(NNTO)within Na_(0.9)Mg_(0.45)Ti_(3.55)O_(8)(NMTO),with x values of 10,20,30,40,and 50.Both XPS(X-ray Photoelectron Spectroscopy)and EDX(Energy Dispersive X-ray Spectroscopy)analyses unequivocally validated the formation of the NNMTO-x solid solutions.It was observed that when x is below 40,the NNMTO-x solid solution retains the structural characteristics of the original NMTO.However,beyond this threshold,significant alterations in crystal morphology were noted,accompanied by a noticeable decline in photocatalytic activity.Notably,the absorption edge of NNMTO-x(x<40)exhibited a shift towards the visible-light spectrum,thereby substantially broadening the absorption range.The findings highlight that NNMTO-30 possesses the most pronounced photocatalytic activity for the reduction of CO_(2).Specifically,after a 6 h irradiation period,the production rates of CO and CH_(4)were recorded at 42.38 and 1.47μmol/g,respectively.This investigation provides pivotal insights that are instrumental in the advancement of highly efficient and stable photocatalysts tailored for CO_(2)reduction processes.展开更多
BACKGROUND:Hemiplegia,a prevalent stroke-related condition,is often studied for motor dysfunction;however,spasticity remains under-researched.Abnormal muscle tone significantly hinders hemiplegic patients’walking rec...BACKGROUND:Hemiplegia,a prevalent stroke-related condition,is often studied for motor dysfunction;however,spasticity remains under-researched.Abnormal muscle tone significantly hinders hemiplegic patients’walking recovery.OBJECTIVE:To determine whether early suspension-protected training with a personal assistant machine for stroke patients enhances walking ability and prevents muscle spasms.METHODS:Thirty-two early-stage stroke patients from Shenzhen University General Hospital and the China Rehabilitation Research Center were randomly assigned to the experimental group(n=16)and the control group(n=16).Both groups underwent 4 weeks of gait training under the suspension protection system for 30 minutes daily,5 days a week.The experimental group used the personal assistant machine during training.Three-dimensional gait analysis(using the Cortex motion capture system),Brunnstrom staging,Fugl-Meyer Assessment for lower limb motor function,Fugl-Meyer balance function,and the modified Ashworth Scale were evaluated within 1 week before the intervention and after 4 weeks of intervention.RESULTS AND CONCLUSION:After the 4-week intervention,all outcome measures showed significant changes in each group.The experimental group had a small but significant increase in the modified Ashworth Scale score(P<0.05,d=|0.15|),while the control group had a large significant increase(P<0.05,d=|1.48|).The experimental group demonstrated greater improvements in walking speed(16.5 to 38.44 cm/s,P<0.05,d=|4.01|),step frequency(46.44 to 64.94 steps/min,P<0.05,d=|2.32|),stride length(15.50 to 29.81 cm,P<0.05,d=|3.44|),and peak hip and knee flexion(d=|1.82|to|2.17|).After treatment,the experimental group showed significantly greater improvements than the control group in walking speed(38.44 vs.26.63 cm/s,P<0.05,d=|2.75|),stride length,peak hip and knee flexion(d=|1.31|to|1.45|),step frequency(64.94 vs.59.38 steps/min,P<0.05,d=|0.85|),and a reduced support phase(bilateral:24.31%vs.28.38%,P<0.05,d=|0.88|;non-paretic:66.19%vs.70.13%,P<0.05,d=|0.94|).For early hemiplegia,personal assistant machine-assisted gait training under the suspension protection system helps establish a correct gait pattern,prevents muscle spasms,and improves motor function.展开更多
The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecul...The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecules and{[Co2(BINDI)(DMA)_(2)]·DMA}_(n)(Co-MOF,H4BINDI=N,N'-bis(5-isophthalic acid)naphthalenediimide,DMA=N,N-dimethylacetamide)was synthesized via a one-pot method,leveragingπ-πinteractions between pyrene and Co-MOF to modulate electrical conductivity.Results demonstrate that the Py@Co-MOF catalyst exhibited significantly enhanced OER performance compared to pure Co-MOF or pyrene-based electrodes,achieving an overpotential of 246 mV at a current density of 10 mA·cm^(-2) along with excellent stability.Density functional theory(DFT)calculations reveal that the formation of O*in the second step is the rate-determining step(RDS)during the OER process on Co-MOF,with an energy barrier of 0.85 eV due to the weak adsorption affinity of the OH*intermediate for Co sites.CCDC:2419276.展开更多
CZTS(Cu_(2)ZnSnS_(4))is a quaternary semiconductor that is environmentally friendly,less expensive.In this paper,we report on the optimization and fabrication of CZTS-based heterojunction nanodevices for bifunctional ...CZTS(Cu_(2)ZnSnS_(4))is a quaternary semiconductor that is environmentally friendly,less expensive.In this paper,we report on the optimization and fabrication of CZTS-based heterojunction nanodevices for bifunctional applications such as solar cells and photodetectors.CZTS thin films were deposited on top of(Molybdenum)Mo-coated glass substrates via RF sputtering at 100 and 200 W.Rapid thermal processing(RTP)was used at 300,400,and 500℃temperatures.Cd S(cadmium sulphide)was deposited on CZTS using a chemical bath deposition system with 3-and 5-min deposition times.Zn O(zinc oxide)and AZO(aluminium doped zinc oxide)layers were deposited using RF(radio frequency)sputtering to create the solar device.XRD confirms the formation of a tetragonal structure with increased crystallinity due to the use of RTP.Raman reveals the characteristic Raman shift peak associated with CZTS at 336 and 335 cm^(-1).The FESEM shows a relationship with RTP temperature.Surface features,including grain size,vary with RTP temperature.The ideality factor is nearly 2,indicating imperfection in the Mo/CZTS interface.Schottky barrier height estimates range from 0.6 to 0.7 e V.Absorbance and transmittance show a predictable fluctuation with RTP temperature.Photovoltaic device was built using the higher crystalline feature of CZTS in conjunction with Cd S deposited at 3 and 5 min.The efficiency of Cd S deposited after 3 and 5 min was 1.15 and 0.97 percent,respectively.Fabricated devices were used for wavelength-dependent photodetection.This work demonstrated self-powered photodetection.展开更多
Subcritical reactors(SCRs)or subcritical assemblies(SCAs)are the main infrastructure for designing power reactors.These reactors are widely used for training and research because of their high level of inherent safety...Subcritical reactors(SCRs)or subcritical assemblies(SCAs)are the main infrastructure for designing power reactors.These reactors are widely used for training and research because of their high level of inherent safety.The objective of this study is to design a subcritical reactor using a pressurized water reactor(PWR)conventional fuel following two safety points.In the first approach,deeply placed SCR cores with an infinite multiplication factor(k_(∞))of less than unity were identified using the DRAGON lattice code.In the second approach,subcritical reactor cores with an effective multiplication factor(k_(eff))of less than unity were determined by coupling the cell calculations of the DRAGON lattice code and core calculations of the DONJON code.For the deeply subcritical reactor design,it was found that the reactor would remain inherently subcritical while using fuel rods with ^(235)U enrichment of up to 0.9%,regardless of the pitch of the fuel rods.In the second approach,the optimal pitches(1.3 to 2.3 cm)were determined for different fuel enrichment values from 1 to 5%.Subsequently,the k_(eff) was obtained for a fuel rod arrangement of 8×8 to 80×80,and the states in which the reactor would be subcritical were determined for different fuel enrichments at the corresponding optimal pitch.To validate the models used in the DRAGON and DONJON codes,the k_(eff) of the Isfahan Light Water Subcritical Reactor(LWSCR)was experimentally measured and compared with the results of the calculations.Finally,the effects of fuel and moderator temperature changes were investigated to ensure that the designed assemblies remained in the subcritical state at all operational temperatures.展开更多
We prepared Co_(x)Pt_(100-x)(x=40,45,50,55,60)nanoparticles by the sol-gel method.The phase composition and crystal structure,morphology and microstructure,and magnetic properties of the samples were characterized and...We prepared Co_(x)Pt_(100-x)(x=40,45,50,55,60)nanoparticles by the sol-gel method.The phase composition and crystal structure,morphology and microstructure,and magnetic properties of the samples were characterized and tested using X-ray diffraction(XRD),transmission electron microscopy(TEM),and vibrating sample magnetometer(VSM),respectively.The results demonstrate that the coercivity of CoPt nanoparticles can be effectively controlled by adjusting the atomic ratio of Co and Pt in the samples.Among the compositions studied,the Co_(45)Pt_(55)sample synthesized by the sol-gel method exhibits smaller grain size and a coercivity as high as 6.65×10^(5) A/m is achieved.The morphology and microstructure of the nanoparticles were analyzed by TEM images,indicating that a slight excess of Pt can effectively enhance the coercivity of CoPt nanoparticles.展开更多
Doping in thin-film transistors(TFTs) plays a crucial role in tailoring material properties to enhance device performance, making them essential for advanced electronic applications. This study explores the synthesis ...Doping in thin-film transistors(TFTs) plays a crucial role in tailoring material properties to enhance device performance, making them essential for advanced electronic applications. This study explores the synthesis and characterization of TFTs fabricated using nickel(Ni)-doped indium oxide(In_(2)O_(3)) via a wet-chemical approach. The presented work investigates the effect of "Ni" incorporation in In_(2)O_(3) on the structural and electrical transport properties of In_(2)O_(3), revealing that higher "Ni" content decreases the oxygen vacancies, leading to a reduction in leakage current and a forward shift in threshold potential(V_(th)).Experimental findings reveal that Ni In O-based TFTs(with Ni = 0.5%) showcase enhanced electrical performance, achieving mobility of 7.54 cm^(2)/(V·s), an impressive ON/OFF current ratio of ~10^(7), a V_(th) of 6.26 V, reduced interfacial trap states(D_(it)) of 8.23 ×10^(12) cm^(-2) and enhanced biased stress stability. The efficacy of "Ni" incorporation is attributed to the upgraded Lewis acidity, stable Ni-O bond strength, and small ionic radius of Ni. Negative bias illumination stability(NBIS) measurements further indicate that device stability diminishes with shorter light wavelengths, likely due to the activation of oxygen vacancies. These findings validate the solution-processed techniques' potential for future large-scale, low-cost, energy-efficient, and high-performance electronics.展开更多
Among various architectures of polymers,end-group-free rings have attracted growing interests due to their distinct physicochemical performances over the linear counterparts which are exemplified by reduced hydrodynam...Among various architectures of polymers,end-group-free rings have attracted growing interests due to their distinct physicochemical performances over the linear counterparts which are exemplified by reduced hydrodynamic size and slower degradation.It is key to develop facile methods to large-scale synthesis of polymer rings with tunable compositions and microstructures.Recent progresses in large-scale synthesis of polymer rings against single-chain dynamic nanoparticles,and the example applications in synchronous enhancing toughness and strength of polymer nanocomposites are summarized.Once there is the breakthrough in rational design and effective large-scale synthesis of polymer rings and their functional derivatives,a family of cyclic functional hybrids would be available,thus providing a new paradigm in developing polymer science and engineering.展开更多
Metal halide perovskites(MHPs)with striking electrical and optical properties have appeared at the forefront of semiconductor materials for photocatalytic redox reactions but still suffer from some intrinsic drawbacks...Metal halide perovskites(MHPs)with striking electrical and optical properties have appeared at the forefront of semiconductor materials for photocatalytic redox reactions but still suffer from some intrinsic drawbacks such as inferior stability,severe charge-carrier recombination,and limited active sites.Heterojunctions have recently been widely constructed to improve light absorption,passivate surface for enhanced stability,and promote charge-carrier dynamics of MHPs.However,little attention has been paid to the review of MHPs-based heterojunctions for photocatalytic redox reactions.Here,recent advances of MHPs-based heterojunctions for photocatalytic redox reactions are highlighted.The structure,synthesis,and photophysical properties of MHPs-based heterojunctions are first introduced,including basic principles,categories(such as Schottky junction,type-I,type-II,Z-scheme,and S-scheme junction),and synthesis strategies.MHPs-based heterojunctions for photocatalytic redox reactions are then reviewed in four categories:H2evolution,CO_(2)reduction,pollutant degradation,and organic synthesis.The challenges and prospects in solar-light-driven redox reactions with MHPs-based heterojunctions in the future are finally discussed.展开更多
Electrocatalytic oxidation of glycerol for value-added chemicals is a superior strategy to utilize the excess glycerol produced in the biodiesel industry.Pd is one of the few active catalysts for alkaline glycerol oxi...Electrocatalytic oxidation of glycerol for value-added chemicals is a superior strategy to utilize the excess glycerol produced in the biodiesel industry.Pd is one of the few active catalysts for alkaline glycerol oxidation reaction(GOR);however,glycerol inevitably dissociates and converts to carbon dioxide on the Pd surface,which results in its low total Faradaic efficiency(FE)for high-value-added products.Herein,a series of Pd/C and Pd10Bix/C catalysts were synthesized to investigate the GOR pathway.The Pd10Bi3/C catalyst with optimal Bi content achieved an excellent GOR mass activity of 7.5±0.2 A mgPd−1 and an outstanding total FE of 90%±3%,which are much higher than those values on Pd/C(1.2±0.2 A mgPd−1 for mass activity and 63%±4%for total FE).Combined results of in-situ attenuated total reflection surface enhanced infrared absorption spectroscopy and density functional theory calculations show that Bi suppresses the dissociation of glycerol through the“shielding effect”of Bi to the adjacent Pd sites,which weakens the adsorption strength of GOR intermediates on those sites.This work provides a new insight into the GOR mechanism and puts forward a valid strategy for the rational design of catalysts to enable the transformation of glycerol into high-value-added products.展开更多
Organic-inorganic metal halides(OIMHs)have emerged as highly promising novel multifunctional optoelectronic materials,owing to their easily adjustable properties from a variety of combinations of different components....Organic-inorganic metal halides(OIMHs)have emerged as highly promising novel multifunctional optoelectronic materials,owing to their easily adjustable properties from a variety of combinations of different components.But it is still difficult and rare to realize highly tunable multicolor luminescence within the same material.In this work,we successfully incorporated three adjustable emission centers in OIMHs to synthesize a novel OIMH(NEA)_(2)MnBr_(4),with each emission center capable of emitting one of the primary colors—red,green,and blue.The green and red emissions originate from the tetrahedron and octahedron structures in the Mn-based frame,while the blue can be attributed to the contribution of organic components.Additionally,to achieve comparable emission intensity among the three primary colors,we enhanced the blue emission performance by optimizing the ratio of organic structure components and incorporating chirality in the OIMHs.The resulting high-quality films can be obtained by spin-coating method with a photoluminescence quantum yields of up to 96%.More interestingly,by the dual manipulation of excitation wavelength and temperature,the sample can be emitted at least seven distinct colors including a standard white luminescence at(0.33,0.33),opening up promising prospects for multicolor luminescence applications such as high-end anti-counterfeiting technology,light-emitting diodes,X-ray imaging,latent fingerprints,humidity detection,and so on.Therefore,based on application scenarios and requirements,our research on this highly tunable luminescent OIMH material lays a solid foundation for further development of various functional properties of related materials.展开更多
This study investigates the impact of vegetation-climate feedback on the global land monsoon system during the Last Interglacial(LIG,127000 years BP)and the mid-Holocene(MH,6000 years BP)using the earth system model E...This study investigates the impact of vegetation-climate feedback on the global land monsoon system during the Last Interglacial(LIG,127000 years BP)and the mid-Holocene(MH,6000 years BP)using the earth system model EC-Earth3.Our findings indicate that vegetation changes significantly influence the global monsoon area and precipitation patterns,especially in the North African and Indian monsoon regions.The North African monsoon region experienced the most substantial increase in vegetation during both the LIG and MH,resulting in significant increases in monsoonal precipitation by 9.8%and 6.0%,respectively.The vegetation feedback also intensified the Saharan Heat Low,strengthened monsoonal flows,and enhanced precipitation over the North African monsoon region.In contrast,the Indian monsoon region exhibited divergent responses to vegetation changes.During the LIG,precipitation in the Indian monsoon region decreased by 2.2%,while it increased by 1.6%during the MH.These differences highlight the complex and region-specific impacts of vegetation feedback on monsoon systems.Overall,this study demonstrates that vegetation feedback exerts distinct influences on the global monsoon during the MH and LIG.These findings highlight the importance of considering vegetation-climate feedback in understanding past monsoon variability and in predicting future climate change impacts on monsoon systems.展开更多
Amorphous materials represent a promising platform for advancing CO_(2)electrochemical reduction due to their inherently diverse coordination environments.In this study,we demonstrate computationally the superior perf...Amorphous materials represent a promising platform for advancing CO_(2)electrochemical reduction due to their inherently diverse coordination environments.In this study,we demonstrate computationally the superior performance of amorphous CuNi alloys for CO_(2)electrochemical reduction.By integrating machine learning forcefields for efficient structure generation and density functional theory for subsequent structural refinement and property calculations,we reveal the potential of these disordered systems to outperform their crystalline counterparts.Machine learning forcefields can generate a bulk structure containing a mixture of Cu and Ni atoms,resulting in enhanced catalytic performance.Effective screening of the amorphous surfaces is used to identify undercoordinated Cu and Ni sites in the amorphous structure to synergistically promote selective CO production and favor ethanol formation over ethylene via the stabilization of the*COCHO intermediate,resulting in significantly lower Gibbs free energy changes compared to the crystalline counterpart.The varying atomic coordination environments on amorphous surfaces promote both C–C bond formation and subsequent proton-electron transfer,leading to ethanol formation.These findings demonstrate the superior catalytic performance of amorphous CuNi,highlighting its potential for efficient and selective electroreduction of CO_(2).展开更多
Inorganic materials can solve transportable and on-site hydrolytic hydrogen generation issues.CaH_(2)/(Al/Si)composites are preferable due to their notable chemical properties.However,these composites require pretreat...Inorganic materials can solve transportable and on-site hydrolytic hydrogen generation issues.CaH_(2)/(Al/Si)composites are preferable due to their notable chemical properties.However,these composites require pretreatments,an inert environment,and long hours of physical ball milling for high homogeneity and synergistic effects.CaH_(2)also inhibits the hydrolysis reaction by forming its products on the Al/Si surface,which hinders the direct utilization of composites.This work represents the first investigation of NaH-CaH_(2)(Al/Si)fuel composites,which greatly overcome these limitations and can be directly used for on-site hydrogen generation and proton exchange membrane(PEM)fuel cells.The NaH-CaH_(2)(Al/Si)fuel composites were prepared by using a straightforward mixing method with variable composition ratios,showing high H_(2)yield and fuel cell(FC)performance.NaH addition provides the bridge effect,which opens up a new way to enable efficient hydrolysis and greatly enhances the hydrolysis activity of CaH_(2)/(Al/Si)composites.The novel fuel composites(NaH-CaH_(2)/Al)have extraordinary FC performance and a 0.42 W/cm2 peak power density greater than commercial hydrogen generators.It provides high H_(2)yield 84.4%for NaH-CaH_(2)/Al and 82%for NaH-CaH_(2)/Si compared to NaOH-CaH_(2)(Al/Si),NaCl-CaH_(2)(Al/Si),and KCl-CaH_(2)(Al/Si)composites.The NaH bridge effect hinders the direct water contact and stops the formation of Ca(OH)2 around Al/Si,which provides adequate pathways for the CaH_(2)(Al/Si)hydrolysis.The impressive capabilities of novel fuel composites are anticipated to offer practical uses in fuel cells,automobile applications,and portable/on-board H_(2)generation.展开更多
The solution processibility of perovskites provides a costeffective and high-throughput route for fabricating state-of-the-art solar cells.However,the fast kinetics of precursor-to-perovskite transformation is suscept...The solution processibility of perovskites provides a costeffective and high-throughput route for fabricating state-of-the-art solar cells.However,the fast kinetics of precursor-to-perovskite transformation is susceptible to processing conditions,resulting in an uncontrollable variance in device performance.Here,we demonstrate a supramolecule confined approach to reproducibly fabricate perovskite films with an ultrasmooth,electronically homogeneous surface.The assembly of a calixarene capping layer on precursor surface can induce host-vip interactions with solvent molecules to tailor the desolvation kinetics,and initiate the perovskite crystallization from the sharp molecule-precursor interface.These combined effects significantly reduced the spatial variance and extended the processing window of perovskite films.As a result,the standard efficiency deviations of device-to-device and batch-to-batch devices were reduced from 0.64-0.26%to 0.67-0.23%,respectively.In addition,the perovskite films with ultrasmooth top surfaces exhibited photoluminescence quantum yield>10%and surface recombination velocities<100 cm s^(-1)for both interfaces that yielded p-i-n structured solar cells with power conversion efficiency over 25%.展开更多
Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implem...Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implementation remains a significant challenge.Herein,we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs.Specifically,polypyrrole(PPy)is in situ vapor-phase polymerized on the surface of N-doped TiO_(2) nanorods supported on carbon cloth(N-TiO_(2)/CC),thereby forming a well-defined p–n heterojunction.This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field.Thus,the PPy@N-TiO_(2)/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur,enabling ultrafast sulfur redox dynamics,as convincingly validated by both theoretical simulations and experimental results.Consequently,the PPy@N-TiO_(2)/CC PALSB achieves a high discharge capacity of 1653 mAh g^(−1),reaching 98.7%of the theoretical value.Furthermore,5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g^(−1),achieving dual-mode energy harvesting capabilities.This work successfully integrates solar energy conversion and storage within a rechargeable battery system,providing a promising strategy for sustainable energy storage technologies.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12350404 and 12174066)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0302600)+1 种基金the National Key Research and Development Program of China(Grant No.2019YFA0308404)the Science and Technology Commission of Shanghai Municipality(Grant Nos.23JC1400600 and 2019SHZDZX01)。
文摘Moirésystems have emerged as an ideal platform for exploring interaction effects and correlated states.However,most of the experimental systems are based on either triangular or honeycomb lattices.In this study,based on the self-consistent Hartree–Fock calculation,we investigate the phase diagram of the kagomélattice in a recently discovered system with two degenerateΓvalley orbitals and strong spin–orbit coupling.By focusing on the filling factors of 1/2,1/3 and 2/3,we identify various symmetry-breaking states by adjusting the screening length and dielectric constant.At the half filling,we discover that the spin–orbit coupling induces Dzyaloshinskii–Moriya interaction and stabilizes a classical magnetic state with 120°ordering.Additionally,we observe a transition to a ferromagnetic state with out-of-plane ordering.In the case of 1/3 filling,the system is ferromagnetically ordered due to the lattice frustration.Furthermore,for 2/3 filling,the system exhibits a pinned droplet state and a 120°magnetic ordered state at weak and immediate coupling strengths,respectively.For the strong coupling case,when dealing with non-integer filling,the system is always charge ordered with sublattice polarization.Our study serves as a starting point for exploring the effects of correlation in moirékagomésystems.
基金supported by the National Key R&D Program of China(Grant No.2022YFA1404400)the National Natural Science Foundation of China(Grant No.12125504 and 12305050)+2 种基金Zhejiang Provincial Natural Science Foundation of China(Grant No.LZ25A050001)the Hundred Talents Program of the Chinese Academy of Sciencesthe Natural Science Foundation of Jiangsu Higher Education Institutions of China(Grant No.23KJB140017)。
文摘We investigate electron mesoscopic transport in a three-terminal setup with coupled quantum dots and a magnetic flux.By mapping the original transport problem into a non-Hermitian Hamiltonian form,we study the interplay between the coherent couplings between quantum dots,the magnetic flux,and the dissipation due to the tunnel coupling with the reservoirs.
基金supported by the the National Key R&D Program of China(Grant Nos.2022YFA1604900 and 2023YFA1606703)the National Natural Science Foundation of China(Grant Nos.12025501,12435007,12405133,and 12347180)+1 种基金China Postdoctoral Science Foundation(Grant No.2023M740189)the Postdoctoral Fellowship Program of CPSF(Grant No.GZC20233381).
文摘Hypernuclei,nuclei containing one or more hyperons,serve as unique laboratories for probing the non-perturbative quantum chromodynamics(QCD).Recent progress in hypernuclear physics,driven by advanced experimental techniques and theoretical innovations,is briefly reviewed with a focus on key findings and unresolved challenges,such as the precise determination of the hypertriton binding energy,investigations of charge symmetry breaking in mirror hypernuclei,and the search for exotic systems,including the neutral nnΛstate.Experimental breakthroughs,including invariant-mass analyses and femtoscopy studies in heavy-ion collisions,as well as high-resolutionγ-spectroscopy,have enabled precise studies of light hypernuclei and offered critical insights into the hyperon–nucleon interaction.Theoretical progress,including ab initio calculations based on chiral effective field theory and lattice QCD,has further enhanced our understanding of hyperon–nucleon and hyperon–hyperon interactions.
基金Supported by the Doctoral Research Start-up Project of Yuncheng University(YQ-2023067)Project of Shanxi Natural Science Foundation(202303021211189)+1 种基金Fund Program for the Scientific Activities of Selected Returned Overseas Professionals in Shanxi Provinces(20220036)Shanxi ProvinceIntelligent Optoelectronic Sensing Application Technology Innovation Center and Shanxi Province Optoelectronic Information Science and TechnologyLaboratory,Yuncheng University.
文摘In this study,a straightforward one-step hydrothermal method was successfully utilized to synthesize the solid solution Na_(0.9)Mg_(0.45)Ti_(3.55)O_(8)-Na_(2)Ni_(2)Ti_(6)O_(16)(NNMTO-x),where x denotes the molar percentage of Na_(2)Ni_(2)Ti_(6)O_(16)(NNTO)within Na_(0.9)Mg_(0.45)Ti_(3.55)O_(8)(NMTO),with x values of 10,20,30,40,and 50.Both XPS(X-ray Photoelectron Spectroscopy)and EDX(Energy Dispersive X-ray Spectroscopy)analyses unequivocally validated the formation of the NNMTO-x solid solutions.It was observed that when x is below 40,the NNMTO-x solid solution retains the structural characteristics of the original NMTO.However,beyond this threshold,significant alterations in crystal morphology were noted,accompanied by a noticeable decline in photocatalytic activity.Notably,the absorption edge of NNMTO-x(x<40)exhibited a shift towards the visible-light spectrum,thereby substantially broadening the absorption range.The findings highlight that NNMTO-30 possesses the most pronounced photocatalytic activity for the reduction of CO_(2).Specifically,after a 6 h irradiation period,the production rates of CO and CH_(4)were recorded at 42.38 and 1.47μmol/g,respectively.This investigation provides pivotal insights that are instrumental in the advancement of highly efficient and stable photocatalysts tailored for CO_(2)reduction processes.
文摘BACKGROUND:Hemiplegia,a prevalent stroke-related condition,is often studied for motor dysfunction;however,spasticity remains under-researched.Abnormal muscle tone significantly hinders hemiplegic patients’walking recovery.OBJECTIVE:To determine whether early suspension-protected training with a personal assistant machine for stroke patients enhances walking ability and prevents muscle spasms.METHODS:Thirty-two early-stage stroke patients from Shenzhen University General Hospital and the China Rehabilitation Research Center were randomly assigned to the experimental group(n=16)and the control group(n=16).Both groups underwent 4 weeks of gait training under the suspension protection system for 30 minutes daily,5 days a week.The experimental group used the personal assistant machine during training.Three-dimensional gait analysis(using the Cortex motion capture system),Brunnstrom staging,Fugl-Meyer Assessment for lower limb motor function,Fugl-Meyer balance function,and the modified Ashworth Scale were evaluated within 1 week before the intervention and after 4 weeks of intervention.RESULTS AND CONCLUSION:After the 4-week intervention,all outcome measures showed significant changes in each group.The experimental group had a small but significant increase in the modified Ashworth Scale score(P<0.05,d=|0.15|),while the control group had a large significant increase(P<0.05,d=|1.48|).The experimental group demonstrated greater improvements in walking speed(16.5 to 38.44 cm/s,P<0.05,d=|4.01|),step frequency(46.44 to 64.94 steps/min,P<0.05,d=|2.32|),stride length(15.50 to 29.81 cm,P<0.05,d=|3.44|),and peak hip and knee flexion(d=|1.82|to|2.17|).After treatment,the experimental group showed significantly greater improvements than the control group in walking speed(38.44 vs.26.63 cm/s,P<0.05,d=|2.75|),stride length,peak hip and knee flexion(d=|1.31|to|1.45|),step frequency(64.94 vs.59.38 steps/min,P<0.05,d=|0.85|),and a reduced support phase(bilateral:24.31%vs.28.38%,P<0.05,d=|0.88|;non-paretic:66.19%vs.70.13%,P<0.05,d=|0.94|).For early hemiplegia,personal assistant machine-assisted gait training under the suspension protection system helps establish a correct gait pattern,prevents muscle spasms,and improves motor function.
文摘The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecules and{[Co2(BINDI)(DMA)_(2)]·DMA}_(n)(Co-MOF,H4BINDI=N,N'-bis(5-isophthalic acid)naphthalenediimide,DMA=N,N-dimethylacetamide)was synthesized via a one-pot method,leveragingπ-πinteractions between pyrene and Co-MOF to modulate electrical conductivity.Results demonstrate that the Py@Co-MOF catalyst exhibited significantly enhanced OER performance compared to pure Co-MOF or pyrene-based electrodes,achieving an overpotential of 246 mV at a current density of 10 mA·cm^(-2) along with excellent stability.Density functional theory(DFT)calculations reveal that the formation of O*in the second step is the rate-determining step(RDS)during the OER process on Co-MOF,with an energy barrier of 0.85 eV due to the weak adsorption affinity of the OH*intermediate for Co sites.CCDC:2419276.
文摘CZTS(Cu_(2)ZnSnS_(4))is a quaternary semiconductor that is environmentally friendly,less expensive.In this paper,we report on the optimization and fabrication of CZTS-based heterojunction nanodevices for bifunctional applications such as solar cells and photodetectors.CZTS thin films were deposited on top of(Molybdenum)Mo-coated glass substrates via RF sputtering at 100 and 200 W.Rapid thermal processing(RTP)was used at 300,400,and 500℃temperatures.Cd S(cadmium sulphide)was deposited on CZTS using a chemical bath deposition system with 3-and 5-min deposition times.Zn O(zinc oxide)and AZO(aluminium doped zinc oxide)layers were deposited using RF(radio frequency)sputtering to create the solar device.XRD confirms the formation of a tetragonal structure with increased crystallinity due to the use of RTP.Raman reveals the characteristic Raman shift peak associated with CZTS at 336 and 335 cm^(-1).The FESEM shows a relationship with RTP temperature.Surface features,including grain size,vary with RTP temperature.The ideality factor is nearly 2,indicating imperfection in the Mo/CZTS interface.Schottky barrier height estimates range from 0.6 to 0.7 e V.Absorbance and transmittance show a predictable fluctuation with RTP temperature.Photovoltaic device was built using the higher crystalline feature of CZTS in conjunction with Cd S deposited at 3 and 5 min.The efficiency of Cd S deposited after 3 and 5 min was 1.15 and 0.97 percent,respectively.Fabricated devices were used for wavelength-dependent photodetection.This work demonstrated self-powered photodetection.
文摘Subcritical reactors(SCRs)or subcritical assemblies(SCAs)are the main infrastructure for designing power reactors.These reactors are widely used for training and research because of their high level of inherent safety.The objective of this study is to design a subcritical reactor using a pressurized water reactor(PWR)conventional fuel following two safety points.In the first approach,deeply placed SCR cores with an infinite multiplication factor(k_(∞))of less than unity were identified using the DRAGON lattice code.In the second approach,subcritical reactor cores with an effective multiplication factor(k_(eff))of less than unity were determined by coupling the cell calculations of the DRAGON lattice code and core calculations of the DONJON code.For the deeply subcritical reactor design,it was found that the reactor would remain inherently subcritical while using fuel rods with ^(235)U enrichment of up to 0.9%,regardless of the pitch of the fuel rods.In the second approach,the optimal pitches(1.3 to 2.3 cm)were determined for different fuel enrichment values from 1 to 5%.Subsequently,the k_(eff) was obtained for a fuel rod arrangement of 8×8 to 80×80,and the states in which the reactor would be subcritical were determined for different fuel enrichments at the corresponding optimal pitch.To validate the models used in the DRAGON and DONJON codes,the k_(eff) of the Isfahan Light Water Subcritical Reactor(LWSCR)was experimentally measured and compared with the results of the calculations.Finally,the effects of fuel and moderator temperature changes were investigated to ensure that the designed assemblies remained in the subcritical state at all operational temperatures.
基金Funded by the National Natural Science Foundation of China(No.52371169)。
文摘We prepared Co_(x)Pt_(100-x)(x=40,45,50,55,60)nanoparticles by the sol-gel method.The phase composition and crystal structure,morphology and microstructure,and magnetic properties of the samples were characterized and tested using X-ray diffraction(XRD),transmission electron microscopy(TEM),and vibrating sample magnetometer(VSM),respectively.The results demonstrate that the coercivity of CoPt nanoparticles can be effectively controlled by adjusting the atomic ratio of Co and Pt in the samples.Among the compositions studied,the Co_(45)Pt_(55)sample synthesized by the sol-gel method exhibits smaller grain size and a coercivity as high as 6.65×10^(5) A/m is achieved.The morphology and microstructure of the nanoparticles were analyzed by TEM images,indicating that a slight excess of Pt can effectively enhance the coercivity of CoPt nanoparticles.
基金funded by the research startup funding of National Research Foundation (NRF) of Korea through the Ministry of Science and ICT 2022R1G1A1009887Part of this study was supported by research start-up funding of Anhui University (S202418001/078)。
文摘Doping in thin-film transistors(TFTs) plays a crucial role in tailoring material properties to enhance device performance, making them essential for advanced electronic applications. This study explores the synthesis and characterization of TFTs fabricated using nickel(Ni)-doped indium oxide(In_(2)O_(3)) via a wet-chemical approach. The presented work investigates the effect of "Ni" incorporation in In_(2)O_(3) on the structural and electrical transport properties of In_(2)O_(3), revealing that higher "Ni" content decreases the oxygen vacancies, leading to a reduction in leakage current and a forward shift in threshold potential(V_(th)).Experimental findings reveal that Ni In O-based TFTs(with Ni = 0.5%) showcase enhanced electrical performance, achieving mobility of 7.54 cm^(2)/(V·s), an impressive ON/OFF current ratio of ~10^(7), a V_(th) of 6.26 V, reduced interfacial trap states(D_(it)) of 8.23 ×10^(12) cm^(-2) and enhanced biased stress stability. The efficacy of "Ni" incorporation is attributed to the upgraded Lewis acidity, stable Ni-O bond strength, and small ionic radius of Ni. Negative bias illumination stability(NBIS) measurements further indicate that device stability diminishes with shorter light wavelengths, likely due to the activation of oxygen vacancies. These findings validate the solution-processed techniques' potential for future large-scale, low-cost, energy-efficient, and high-performance electronics.
基金Supported by the National Natural Science Foundation of China(Nos.52293472,22473096 and 22471164)。
文摘Among various architectures of polymers,end-group-free rings have attracted growing interests due to their distinct physicochemical performances over the linear counterparts which are exemplified by reduced hydrodynamic size and slower degradation.It is key to develop facile methods to large-scale synthesis of polymer rings with tunable compositions and microstructures.Recent progresses in large-scale synthesis of polymer rings against single-chain dynamic nanoparticles,and the example applications in synchronous enhancing toughness and strength of polymer nanocomposites are summarized.Once there is the breakthrough in rational design and effective large-scale synthesis of polymer rings and their functional derivatives,a family of cyclic functional hybrids would be available,thus providing a new paradigm in developing polymer science and engineering.
基金financially supported by National Natural Science Foundation of China(No.22302155)the Fundamental Research Funds of the Center Universities(No.D5000240188)the research program of ZJUT(YJY-ZS-20240001)。
文摘Metal halide perovskites(MHPs)with striking electrical and optical properties have appeared at the forefront of semiconductor materials for photocatalytic redox reactions but still suffer from some intrinsic drawbacks such as inferior stability,severe charge-carrier recombination,and limited active sites.Heterojunctions have recently been widely constructed to improve light absorption,passivate surface for enhanced stability,and promote charge-carrier dynamics of MHPs.However,little attention has been paid to the review of MHPs-based heterojunctions for photocatalytic redox reactions.Here,recent advances of MHPs-based heterojunctions for photocatalytic redox reactions are highlighted.The structure,synthesis,and photophysical properties of MHPs-based heterojunctions are first introduced,including basic principles,categories(such as Schottky junction,type-I,type-II,Z-scheme,and S-scheme junction),and synthesis strategies.MHPs-based heterojunctions for photocatalytic redox reactions are then reviewed in four categories:H2evolution,CO_(2)reduction,pollutant degradation,and organic synthesis.The challenges and prospects in solar-light-driven redox reactions with MHPs-based heterojunctions in the future are finally discussed.
基金supported by the National Natural Science Foundation of China(Grant number 22172112)and the Fundamental Research Funds for the Central Universities.
文摘Electrocatalytic oxidation of glycerol for value-added chemicals is a superior strategy to utilize the excess glycerol produced in the biodiesel industry.Pd is one of the few active catalysts for alkaline glycerol oxidation reaction(GOR);however,glycerol inevitably dissociates and converts to carbon dioxide on the Pd surface,which results in its low total Faradaic efficiency(FE)for high-value-added products.Herein,a series of Pd/C and Pd10Bix/C catalysts were synthesized to investigate the GOR pathway.The Pd10Bi3/C catalyst with optimal Bi content achieved an excellent GOR mass activity of 7.5±0.2 A mgPd−1 and an outstanding total FE of 90%±3%,which are much higher than those values on Pd/C(1.2±0.2 A mgPd−1 for mass activity and 63%±4%for total FE).Combined results of in-situ attenuated total reflection surface enhanced infrared absorption spectroscopy and density functional theory calculations show that Bi suppresses the dissociation of glycerol through the“shielding effect”of Bi to the adjacent Pd sites,which weakens the adsorption strength of GOR intermediates on those sites.This work provides a new insight into the GOR mechanism and puts forward a valid strategy for the rational design of catalysts to enable the transformation of glycerol into high-value-added products.
基金supported by supported by the Basic Research Project of State Key Laboratory of Photovoltaic Science and Technology(No.202401020302)funding support from the National Natural Science Foundation of China(No.62274040 and No.62304046)Shanghai science and technology innovation action plan(No.24DZ3001200)。
文摘Organic-inorganic metal halides(OIMHs)have emerged as highly promising novel multifunctional optoelectronic materials,owing to their easily adjustable properties from a variety of combinations of different components.But it is still difficult and rare to realize highly tunable multicolor luminescence within the same material.In this work,we successfully incorporated three adjustable emission centers in OIMHs to synthesize a novel OIMH(NEA)_(2)MnBr_(4),with each emission center capable of emitting one of the primary colors—red,green,and blue.The green and red emissions originate from the tetrahedron and octahedron structures in the Mn-based frame,while the blue can be attributed to the contribution of organic components.Additionally,to achieve comparable emission intensity among the three primary colors,we enhanced the blue emission performance by optimizing the ratio of organic structure components and incorporating chirality in the OIMHs.The resulting high-quality films can be obtained by spin-coating method with a photoluminescence quantum yields of up to 96%.More interestingly,by the dual manipulation of excitation wavelength and temperature,the sample can be emitted at least seven distinct colors including a standard white luminescence at(0.33,0.33),opening up promising prospects for multicolor luminescence applications such as high-end anti-counterfeiting technology,light-emitting diodes,X-ray imaging,latent fingerprints,humidity detection,and so on.Therefore,based on application scenarios and requirements,our research on this highly tunable luminescent OIMH material lays a solid foundation for further development of various functional properties of related materials.
基金supported by the Swedish Research Council(Vetenskapsradet,Grant No.202203129)the Project of Youth Science and Technology Fund of Gansu Province(Grant No.24JRRA439)partially funded by the Swedish Research Council(Vetenskapsradet,Grant No.2022-06725)。
文摘This study investigates the impact of vegetation-climate feedback on the global land monsoon system during the Last Interglacial(LIG,127000 years BP)and the mid-Holocene(MH,6000 years BP)using the earth system model EC-Earth3.Our findings indicate that vegetation changes significantly influence the global monsoon area and precipitation patterns,especially in the North African and Indian monsoon regions.The North African monsoon region experienced the most substantial increase in vegetation during both the LIG and MH,resulting in significant increases in monsoonal precipitation by 9.8%and 6.0%,respectively.The vegetation feedback also intensified the Saharan Heat Low,strengthened monsoonal flows,and enhanced precipitation over the North African monsoon region.In contrast,the Indian monsoon region exhibited divergent responses to vegetation changes.During the LIG,precipitation in the Indian monsoon region decreased by 2.2%,while it increased by 1.6%during the MH.These differences highlight the complex and region-specific impacts of vegetation feedback on monsoon systems.Overall,this study demonstrates that vegetation feedback exerts distinct influences on the global monsoon during the MH and LIG.These findings highlight the importance of considering vegetation-climate feedback in understanding past monsoon variability and in predicting future climate change impacts on monsoon systems.
基金the UK Materials and Molecular Modelling Hub for computational resources,which is partially funded by EPSRC(EP/T022213/1,EP/W032260/1 and EP/P020194/1)via our membership of the UK’s HEC Materials Chemistry Consortium,which is funded by EPSRC(EP/L000202)This work used the ARCHER UK National Super-computing Service(https://www.archer.ac.uk).This research utilized Queen Mary’s Apocrita HPC facility,supported by QMUL Research-IT(https://doi.org/10.5281/zenodo.438045)+1 种基金These results are part of the“Advancing Solid Interface and Lubricants by First Principles Material Design(SLIDE)”project that has received funding from the European Research Council(ERC)under the European Union’s Horizon 2020 research and innovation program(Grant agreement No.865633)Furthermore,D.D.T.thanks the Leverhulme Trust,United Kingdom(RPG-2023-239)for resources supporting projects advancing materials characterization by computational means.
文摘Amorphous materials represent a promising platform for advancing CO_(2)electrochemical reduction due to their inherently diverse coordination environments.In this study,we demonstrate computationally the superior performance of amorphous CuNi alloys for CO_(2)electrochemical reduction.By integrating machine learning forcefields for efficient structure generation and density functional theory for subsequent structural refinement and property calculations,we reveal the potential of these disordered systems to outperform their crystalline counterparts.Machine learning forcefields can generate a bulk structure containing a mixture of Cu and Ni atoms,resulting in enhanced catalytic performance.Effective screening of the amorphous surfaces is used to identify undercoordinated Cu and Ni sites in the amorphous structure to synergistically promote selective CO production and favor ethanol formation over ethylene via the stabilization of the*COCHO intermediate,resulting in significantly lower Gibbs free energy changes compared to the crystalline counterpart.The varying atomic coordination environments on amorphous surfaces promote both C–C bond formation and subsequent proton-electron transfer,leading to ethanol formation.These findings demonstrate the superior catalytic performance of amorphous CuNi,highlighting its potential for efficient and selective electroreduction of CO_(2).
基金financial support granted by the National Natural Science Foundation of China(No.22402225)the Gusu Innovation and Entrepreneurship Leading Talent Plan(No.ZXL2023193)+2 种基金the Sinano Talents Plan(No.2022000175)the Guangdong Basic and Applied Basic Research Foundation(No.2023A1515111133)the ANSO Scholarship for Young Talents.The authors are grateful for the technical support for Nano-X from Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences (SINANO).
文摘Inorganic materials can solve transportable and on-site hydrolytic hydrogen generation issues.CaH_(2)/(Al/Si)composites are preferable due to their notable chemical properties.However,these composites require pretreatments,an inert environment,and long hours of physical ball milling for high homogeneity and synergistic effects.CaH_(2)also inhibits the hydrolysis reaction by forming its products on the Al/Si surface,which hinders the direct utilization of composites.This work represents the first investigation of NaH-CaH_(2)(Al/Si)fuel composites,which greatly overcome these limitations and can be directly used for on-site hydrogen generation and proton exchange membrane(PEM)fuel cells.The NaH-CaH_(2)(Al/Si)fuel composites were prepared by using a straightforward mixing method with variable composition ratios,showing high H_(2)yield and fuel cell(FC)performance.NaH addition provides the bridge effect,which opens up a new way to enable efficient hydrolysis and greatly enhances the hydrolysis activity of CaH_(2)/(Al/Si)composites.The novel fuel composites(NaH-CaH_(2)/Al)have extraordinary FC performance and a 0.42 W/cm2 peak power density greater than commercial hydrogen generators.It provides high H_(2)yield 84.4%for NaH-CaH_(2)/Al and 82%for NaH-CaH_(2)/Si compared to NaOH-CaH_(2)(Al/Si),NaCl-CaH_(2)(Al/Si),and KCl-CaH_(2)(Al/Si)composites.The NaH bridge effect hinders the direct water contact and stops the formation of Ca(OH)2 around Al/Si,which provides adequate pathways for the CaH_(2)(Al/Si)hydrolysis.The impressive capabilities of novel fuel composites are anticipated to offer practical uses in fuel cells,automobile applications,and portable/on-board H_(2)generation.
基金financially supported by the National Natural Science Foundation of China(22379044,22472053)the Science and Technology Commission of Shanghai Municipality(23520710700)+6 种基金the Key Program of the National Natural Science Foundation of China(22239001)the Shanghai Pilot Program for Basic Research(22TQ1400100-5)the ShanghaiMunicipal Natural Science Foundation(25ZR1401081)the Fundamental Research Funds for the Central Universities(JKD01251505,JKVD1251041)the Postdoctoral Fellowship Program of CPSF(GZC20250071)the Shanghai Engineering Research Center of Hierarchical Nanomaterials(18DZ2252400)the Shanghai Frontiers Science Center of Optogenetic Techniques for Cell Metabolism(Shanghai Municipal Education Commission)。
文摘The solution processibility of perovskites provides a costeffective and high-throughput route for fabricating state-of-the-art solar cells.However,the fast kinetics of precursor-to-perovskite transformation is susceptible to processing conditions,resulting in an uncontrollable variance in device performance.Here,we demonstrate a supramolecule confined approach to reproducibly fabricate perovskite films with an ultrasmooth,electronically homogeneous surface.The assembly of a calixarene capping layer on precursor surface can induce host-vip interactions with solvent molecules to tailor the desolvation kinetics,and initiate the perovskite crystallization from the sharp molecule-precursor interface.These combined effects significantly reduced the spatial variance and extended the processing window of perovskite films.As a result,the standard efficiency deviations of device-to-device and batch-to-batch devices were reduced from 0.64-0.26%to 0.67-0.23%,respectively.In addition,the perovskite films with ultrasmooth top surfaces exhibited photoluminescence quantum yield>10%and surface recombination velocities<100 cm s^(-1)for both interfaces that yielded p-i-n structured solar cells with power conversion efficiency over 25%.
基金the financial support from the National Natural Science Foundation of China (22109127)the Chinese Postdoctoral Science Foundation (2021M702666)+2 种基金the Research Fund of the State Key Laboratory of Solidification Processing (NPU),China (Grant No.2023-TS-02)The financial support from the Youth Project of"Shaanxi High-level Talents Introduction Plan"the Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) are also sincerely appreciated
文摘Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implementation remains a significant challenge.Herein,we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs.Specifically,polypyrrole(PPy)is in situ vapor-phase polymerized on the surface of N-doped TiO_(2) nanorods supported on carbon cloth(N-TiO_(2)/CC),thereby forming a well-defined p–n heterojunction.This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field.Thus,the PPy@N-TiO_(2)/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur,enabling ultrafast sulfur redox dynamics,as convincingly validated by both theoretical simulations and experimental results.Consequently,the PPy@N-TiO_(2)/CC PALSB achieves a high discharge capacity of 1653 mAh g^(−1),reaching 98.7%of the theoretical value.Furthermore,5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g^(−1),achieving dual-mode energy harvesting capabilities.This work successfully integrates solar energy conversion and storage within a rechargeable battery system,providing a promising strategy for sustainable energy storage technologies.
