The primary objective of global studies is to develop the properties and durability of polymers for various applications.When it comes to dental disability,denture base materials must have sufficient mechanical and tr...The primary objective of global studies is to develop the properties and durability of polymers for various applications.When it comes to dental disability,denture base materials must have sufficient mechanical and tribological performance in order to withstand the forces experienced in the mouth.This work aims to investigate the effects of the addition of low content of cellulose nanocrystals(CNC)on the mechanical and tribological performance of the polymethyl methacrylate(PMMA)nanocomposites.Different weight percent of CNC(0,0.2,0.4,0.6,and 0.8 wt%)were added to the PMMA matrix followed by ball milling to evenly distribute the nanoparticles reinforced phase in the matrix phase.The findings emphasize the significant impact of CNC integration on the performance of PMMA nanocomposites.By increasing the content of the CNC nanoparticles,the mechanical properties of PMMA were improved.In addition,the tribological outcomes demonstrated a significant reduction in the friction coefficient besides an enhancement in the wear resistance as the weight percentage of nanoparticles increased.The surface of the worn samples was investigated by utilizing SEM to identify the wear mechanisms corresponding to the different compositions.In addition,a finite elment model(FEM)was developed to ascertain the thickness of the worn layer and the generated stressed on the surfaces of the nanocomposite throughout the friction process.展开更多
Self-assembly of metal halide perovskite nanocrystals(NCs)into superlattices can exhibit unique collective properties,which have significant application values in the display,detector,and solar cell field.This review ...Self-assembly of metal halide perovskite nanocrystals(NCs)into superlattices can exhibit unique collective properties,which have significant application values in the display,detector,and solar cell field.This review discusses the driving forces behind the self-assembly process of perovskite NCs,and the commonly used self-assembly methods and different self-assembly structures are detailed.Subsequently,we summarize the collective optoelectronic properties and application areas of perovskite superlattice structures.Finally,we conclude with an outlook on the potential issues and future challenges in developing perovskite NCs.展开更多
Mn^(2+)doping has been adopted as an efficient approach to regulating the luminescence properties of halide perovskite nano-crystals(NCs).However,it is still difficult to understand the interplay of Mn^(2+)luminescenc...Mn^(2+)doping has been adopted as an efficient approach to regulating the luminescence properties of halide perovskite nano-crystals(NCs).However,it is still difficult to understand the interplay of Mn^(2+)luminescence and the matrix self-trapped exciton(STE)emission therein.In this study,Mn^(2+)-doped CsCdCl_(3) NCs are prepared by hot injection,in which CsCdCl_(3) is selected because of its unique crystal structure suitable for STE emission.The blue emission at 441 nm of undoped CsCdCl_(3) NCs originates from the defect states in the NCs.Mn^(2+)doping promotes lattice distortion of CsCdCl_(3) and generates bright orange-red light emission at 656 nm.The en-ergy transfer from the STEs of CsCdCl_(3) to the excited levels of the Mn^(2+)ion is confirmed to be a significant factor in achieving efficient luminescence in CsCdCl_(3):Mn^(2+)NCs.This work highlights the crucial role of energy transfer from STEs to Mn^(2+)dopants in Mn^(2+)-doped halide NCs and lays the groundwork for modifying the luminescence of other metal halide perovskite NCs.展开更多
Formamidinium lead bromide(FAPbBr_(3))nanocrystals(NCs)have been considered to be a good optoelectronic material due to their pure green emission,excellent stability and superior carrier transport characteristics.Howe...Formamidinium lead bromide(FAPbBr_(3))nanocrystals(NCs)have been considered to be a good optoelectronic material due to their pure green emission,excellent stability and superior carrier transport characteristics.However,two-photon pumped amplified spontaneous emission(ASE)and the corresponding nonlinear optical properties of FAPbBr_(3) NCs are scarcely revealed.Herein,we synthesized colloidal FAPbBr_(3) NCs with different sizes by changing the molar ratio of FABr/PbBr_(2) in the precursor solution,using ligand assisted precipitation(LARP)technology at room temperature.Photoluminescence(PL)and time resolved photoluminescence(TRPL)spectroscopy were measured to characterize their ASE properties.And their nonlinear optical properties were studied through the Zscan technique and the two-photon excited fluorescence method.The stimulated emission properties including oneand two-photon pumped ASE have been realized from FAPbBr_(3) NCs.With large two-photon absorption coefficient(0.27 cm/GW)and high non-linear absorption cross-section(7.52×10^(5) GM),ASE with threshold as low as 9.8μJ/cm^(2) and 487μJ/cm^(2) have been obtained from colloidal FAPbBr_(3) NCs using one-and two-photon excitations.These results indicate that as a new possible green-emitting frequency-upconversion material with low thresholds,FAPbBr_(3) NCs hold great potential in the development of high-performance two-photon pump lasers.展开更多
The exceptional optoelectronic properties of lead halide perovskite nanocrystals(PeNCs)in the ultraviolet and visible spectral regions have positioned them as a promising class of semiconductor materials for diverse o...The exceptional optoelectronic properties of lead halide perovskite nanocrystals(PeNCs)in the ultraviolet and visible spectral regions have positioned them as a promising class of semiconductor materials for diverse optoelectronic and photo-voltaic applications.However,their limited response to near-infrared(NIR)light due to the intrinsic bandgap(>1.5 eV)has hindered their applications in many advanced technologies.To circumvent this limitation,it is of fundamental significance to inte-grate PeNCs with lanthanide-doped upconversion nanoparticles(UCNPs)that are capable of efficiently converting low-energy NIR photons into high-energy ultravi-olet and visible photons.By leveraging the energy transfer from UCNPs to PeNCs,this synergistic combination can not only expand the NIR responsivity range of PeNCs but also introduce novel emission profiles to upconversion luminescence with multi-dimensional tunability(e.g.,wavelength,lifetime,and polarization)under low-to-medium power NIR irradiation,which breaks through the inherent restric-tions of individual PeNCs and UCNPs and thereby opens up new opportunities for materials and device engineering.In this review,we focus on the latest advance-ments in the development of PeNCs-UCNPs nanocomposites,with an emphasis on the controlled synthesis and optical properties design for advanced optoelectronic applications such as full-spectrum solar cells,NIR photodetectors,and multilevel anticounterfeiting.Some future efforts and prospects toward this active research field are also envisioned.展开更多
The application potential of cellulosic materials in natural composites and other fields needs to be explored to develop innovative, sustainable, lightweight, functional biomass materials that are also environmentally...The application potential of cellulosic materials in natural composites and other fields needs to be explored to develop innovative, sustainable, lightweight, functional biomass materials that are also environmentally friendly. This study investigated Typha angustifolia (Typha sp.) as a potential new raw material for extracting cellulose nanocrystals (CNCs) for application in wastewater treatment composites. Alkaline treatments and bleaching were used to remove cellulose from the stem fibres. The CNCs were then isolated from the recovered cellulose using acid hydrolysis. The study showed a few distinct functional groups (O-H, -C-H, =C-H and C-O, and C-O-C) in the Fourier Transform Infrared (FTIR) spectra. A scanning electron microscope (SEM) revealed the smooth surface of CPC and CNCs, which resulted from removing lignin and hemicellulose from powdered Typha angustifolia. Based on the crystalline index, the powdered Typha angustifolia, CPC, and CNCs were 42.86%, 66.94% and 77.41%. The loss of the amorphous section of the Typha sp. fibre resulted in a decrease in particle size. It may be inferred from the features of a Typha sp. CNC that CNCs may be employed as reinforcement in composites for wastewater treatment.展开更多
Recently,a Schwarz crystal structure with curved grain boundaries(GBs)constrained by twin-boundary(TB)networks was discovered in nanocrystalline Cu through experiments and atomistic simulations.Nanocrystalline Cu with...Recently,a Schwarz crystal structure with curved grain boundaries(GBs)constrained by twin-boundary(TB)networks was discovered in nanocrystalline Cu through experiments and atomistic simulations.Nanocrystalline Cu with nanosized Schwarz crystals exhibited high strength and excellent thermal stability.However,the grainsize effect and associated deformation mechanisms of Schwarz nanocrystals remain unknown.Here,we performed large-scale atomistic simulations to investigate the deformation behaviors and grain-size effect of nanocrystalline Cu with Schwarz crystals.Our simulations showed that similar to regular nanocrystals,Schwarz nanocrystals exhibit a strengthening-softening transition with decreasing grain size.The critical grain size in Schwarz nanocrystals is smaller than that in regular nanocrystals,leading to a maximum strength higher than that of regular nanocrystals.Our simulations revealed that the softening in Schwarz nanocrystals mainly originates from TB migration(or detwinning)and annihilation of GBs,rather than GB-mediated processes(including GB migration,sliding and diffusion)dominating the softening in regular nanocrystals.Quantitative analyses of simulation data further showed that compared with those in regular nanocrystals,the GB-mediated processes in Schwarz nanocrystals are suppressed,which is related to the low volume fraction of amorphous-like GBs and constraints of TB networks.The smaller critical grain size arises from the suppression of GB-mediated processes.展开更多
To achieve environmentally benign energy conversion with the carbon neutrality target via electrochemical reactions, the innovation of electrocatalysts plays a vital role in the enablement of renewable resources. Nowa...To achieve environmentally benign energy conversion with the carbon neutrality target via electrochemical reactions, the innovation of electrocatalysts plays a vital role in the enablement of renewable resources. Nowadays, Pt-based nanocrystals(NCs) have been identified as one class of the most promising candidates to efficiently catalyze both the half-reactions in hydrogen-and hydrocarbonbased fuel cells. Here, we thoroughly discuss the key achievement in developing shape-controlled Pt and Pt-based NCs, and their electrochemical applications in fuel cells. We begin with a mechanistic discussion on how the morphology can be precisely controlled in a colloidal system, followed by highlighting the advanced development of shape-controlled Pt, Pt-alloy, Pt-based core@shell NCs, Pt-based nanocages, and Pt-based intermetallic compounds. We then select some case studies on models of typical reactions(oxygen reduction reaction at the cathode and small molecular oxidation reaction at the anode) that are enhanced by the shape-controlled Pt-based nanocatalysts. Finally, we provide an outlook on the potential challenges of shape-controlled nanocatalysts and envision their perspective with suggestions.展开更多
The main bottleneck against industrial utilization of sodium ion batteries(SIBs)is the lack of high-capacity electrodes to rival those of the benchmark lithium ion batteries(LIBs).Here in this work,we have developed a...The main bottleneck against industrial utilization of sodium ion batteries(SIBs)is the lack of high-capacity electrodes to rival those of the benchmark lithium ion batteries(LIBs).Here in this work,we have developed an economical method for in situ fabrication of nanocomposites made of crystalline few-layer graphene sheets loaded with ultrafine SnO_(2)nanocrystals,using short exposure of microwave to xerogel of graphene oxide(GO)and tin tetrachloride containing minute catalyzing dispersoids of chemically reduced GO(RGO).The resultant nanocomposites(SnO_(2)@MWG)enabled significantly quickened redox processes as SIB anode,which led to remarkable full anode-specific capacity reaching 538 mAh g^(−1)at 0.05 A g^(−1)(about 1.45 times of the theoretical capacity of graphite for the LIB),in addition to outstanding rate performance over prolonged charge–discharge cycling.Anodes based on the optimized SnO_(2)@MWG delivered stable performance over 2000 cycles even at a high current density of 5 A g^(−1),and capacity retention of over 70.4%was maintained at a high areal loading of 3.4 mg cm^(−2),highly desirable for high energy density SIBs to rival the current benchmark LIBs.展开更多
Polypyrrole(PPy)is wildly used as electrode material in supercapacitors due to its high conductivity,low cost,ease of handling,and ease of fabrication.However,limited capacitance and poor cycling stability hinder its ...Polypyrrole(PPy)is wildly used as electrode material in supercapacitors due to its high conductivity,low cost,ease of handling,and ease of fabrication.However,limited capacitance and poor cycling stability hinder its practical application.After developing carboxylated cellulose nanocrystals(CNC-COO^(-))as immobile dopants for PPy to improve its cycling stability,we investigated the effect of different commonly used salts(KCl,NaCl,KBr,and NaClO_(4))as dopants during electrode fabrication by electropolymerization.The film’s capacitance increased from 160.6 to 183.4 F g^(-1)after adding a combination of KCl and NaClO_(4) into the electrodeposition electrolyte.More importantly,the porous and interconnected PPy/CNC-COO^(-)-Cl-(Cl O_(4)^(-))_0.5 electrode film exhibited an excellent capacitance of 125.0 F g^(-1)(0.78 F cm^(-2))at a high current density of 2.0 Ag^(-1)(20 m A cm^(-2),allowing charging in less than 1 min),increasing almost 204%over PPy/CNC-COO-films.A symmetric PPy/CNC-COO^(-)-Cl-(ClO_(4)^(-))_0.5 supercapacitor retained its full capacitance after 5000 cycles,and displayed a high energy density of 5.2 Wh kg^(-1)at a power density of 25.4 W kg^(-1)(34.5μWh cm^(-2) at 1752.3μW cm^(-2)).These results reveal that the porous structure formed by doping with CNC-COO-and inorganic salts opens up more active reaction areas to store charges in PPy-based films as the stiff and ribbon-like CNC-COO-as permanent dopants improve the strength and stability of PPy-based films.Our demonstration provides a simple and practical way to deposit PPy based supercapacitors with high capacitance,fast charging,and excellent cycling stability.展开更多
Ligand assisted reprecipitation(LARP)is a widely used method for cesium lead halide perovskite nanocrystals(NCs)synthesis.Nevertheless,the ultrafast kinetics of LARP,as well as the inefficient transport properties and...Ligand assisted reprecipitation(LARP)is a widely used method for cesium lead halide perovskite nanocrystals(NCs)synthesis.Nevertheless,the ultrafast kinetics of LARP,as well as the inefficient transport properties and discontinuity of batch reactors,challenge the particle size control and experimental repeatability.To address these issues,an ultrasonic cavitation-enabled microfluidic approach was developed to achieve the continuous synthesis of cesium lead halide perovskite via LARP.It was found that the mixing between the good solvent and antisolvent in the microchannel was greatly enhanced by intensive ultrasonic cavitation.The mixing time could be reduced to below 10 ms under the irradiation of 35 W ultrasound.By modulating the mixing degree,LARP was proved to be a mixing-sensitive process.The effects of ultrasonic power,ultrasonic treatment time,total flow rate,water additive,and reprecipitation temperature on the synthesis of CsPbBr_(3) NCs were systematically investigated.As compared to CsPbBr_(3) NCs synthesized in the batch reactor,the sample synthesized via the ultrasonic cavitation-enabled microfluidic approach possessed stronger photoluminescence intensity and better repeatability.Moreover,the ultrasonic cavitation-enabled microfluidic approach could also realize the continuous synthesis of cesium lead halide perovskite NCs with different halide compositions to cover a wide visible spectrum(426-661 nm).The ultrasonic cavitation-enabled microfluidic approach paved the way for the large-scale of high-quality cesium lead halide perovskite NCs.展开更多
Nanocellulose,a natural polymeric nanomaterial,has attracted significant attention in enhanced oil recovery(EOR)applications due to its abundance,nanoscale,high oil-water interfacial adsorption ef-ficiency.In this stu...Nanocellulose,a natural polymeric nanomaterial,has attracted significant attention in enhanced oil recovery(EOR)applications due to its abundance,nanoscale,high oil-water interfacial adsorption ef-ficiency.In this study,surface-functionalized cellulose nanocrystals(SF-CNCs)were prepared via hy-drochloric acid hydrolysis and chemical modification,with adaptable nanosize and considerable dispersion stability in low-permeability reservoirs.The SF-CNCs were structurally characterized by FT-IR,Cryo-TEM,which have a diameter of 5-10 nm and a length of 100-200 nm.The SF-CNC dispersions possessed higher stability and stronger salt-tolerance than those of corresponding CNC dispersions,due to the strong hydrophilicity of the sulfonic acid group.It was synergistically used with a non-ionic surfactant(APG1214)to formulate a combined flooding system(0.1 wt%SF-CNC+0.2 wt%APG1214).The combined flooding system exhibits strong emulsification stability,low oil-water interfacial tension of o.03 mN/m,and the ability to alter the wettability for oil-wetting rocks.Furthermore,the combined system was_able to provide an optimum EOR efficiency of 20.2%in low-permeability cores with 30.13×10^(-3)μm^(2).Notably.it can enlarge the sweep volume and increase the displacement efficiency simultaneously.Overall,the newly formulated nanocellulose/surfactant combined system exhibits a remarkable EoR performance in low-permeability reservoirs.展开更多
In recent years,photocatalytic CO_(2)reduction reaction(CRR) has attracted much scientific attention to overcome energy and environmental issues by converting CO_(2)into high-value-added chemicals utilizing solar ener...In recent years,photocatalytic CO_(2)reduction reaction(CRR) has attracted much scientific attention to overcome energy and environmental issues by converting CO_(2)into high-value-added chemicals utilizing solar energy.Metal halide perovskite(MHP) nanocrystals(NCs) are recognized as an ideal choice for CRR owing to their outstanding optoelectronic properties.Although great efforts have been devoted to designing more effective photocatalysts to optimize CRR performance,severe charge recombination,instability,and unsatisfactory activity have become major bottlenecks in developing perovskite-based photocatalysts.In this review,we mainly focus on the recent research progress in the areas of relevance.First,a brief insight into reaction mechanisms for CRR and structural features of MHPs are introduced.Second,efficient modification approaches for the improvement of the photocatalytic activity and stability of the perovskite-based catalysts are comprehensively reviewed.Third,the state-of-the-art achievements of perovskite-based photocatalysts for CRR are systematically summarized and discussed,which are focused on the modification approaches,structure design,and the mechanism of the CO_(2)reduction process.Lastly,the current challenges and future research perspectives in the design and application of perovskite materials are highlighted from our point of view to provide helpful insights for seeking breakthroughs in the field of CRR.This review may provide a guide for scientists interested in applying perovskite-based catalysts for solar-to-chemical energy conversion.展开更多
Perovskite nanocrystals(NCs) with high two-photon absorption(TPA) cross-section are of great interest due to their potential applications in three-dimensional optical data storage and multiphoton fluorescence microsco...Perovskite nanocrystals(NCs) with high two-photon absorption(TPA) cross-section are of great interest due to their potential applications in three-dimensional optical data storage and multiphoton fluorescence microscopy. Among various perovskite materials, FAPbBr_(3) NCs show a better development prospect due to their excellent stability. However, there are few reports on their nonlinear optical properties. In this work, the nonlinear optical behavior of FAPbBr_(3) NCs is studied.The methods of multiphoton absorption photoluminescence saturation and open aperture Z-scan technique were applied to determine the TPA cross-section of FAPbBr_(3)NCs, which was around 2.76 × 10^(-45)cm^(4)·s·photon^(-1) at 800 nm. In addition,temperature-dependent photoluminescence induced by TPA was investigated, and the small longitudinal optical phonon energy and electron–phonon coupling strength was obtained, which confirm the weak Pb–Br interaction. Meanwhile, it is found that the exciton binding energy in FAPbBr_(3) NCs was 69.668 me V, which may be ascribed to the strong hydrogen bond interaction. It is expected that our findings will promote the application of FAPbBr_(3) NCs in optoelectronic devices.展开更多
Sodium-ion hybrid capacitor(SIHC)is one of the most promising alternatives for large-scale energy storage due to its high energy and power densities,natural abundance,and low cost.However,overcoming the imbalance betw...Sodium-ion hybrid capacitor(SIHC)is one of the most promising alternatives for large-scale energy storage due to its high energy and power densities,natural abundance,and low cost.However,overcoming the imbalance between slow Na^(+)reaction kinetics of battery-type anodes and rapid ion adsorption/desorption of capacitive cathodes is a significant challenge.Here,we propose the high-rate-performance NiS_(2)@OMGC anode material composed of monodispersed NiS_(2) nanocrystals(8.8±1.7 nm in size)and N,S-co-doped graphenic carbon(GC).The NiS_(2)@OMGC material has a three-dimensionally ordered macroporous(3DOM)morphology,and numerous NiS_(2) nanocrystals are uniformly embedded in GC,forming a core-shell structure in the local area.Ultrafine NiS_(2) nanocrystals and their nano-microstructure demonstrate high pseudocapacitive Na-storage capability and thus excellent rate performance(355.7 mAh/g at 20.0 A/g).A SIHC device fabricated using NiS_(2)@OMGC and commercial activated carbon(AC)cathode exhibits ultrahigh energy densities(197.4 Wh/kg at 398.8 W/kg)and power densities(43.9 kW/kg at 41.3 Wh/kg),together with a long life span.This outcome exemplifies the rational architecture and composition design of this type of anode material.This strategy can be extended to the design and synthesis of a wide range of high-performance electrode materials for energy storage applications.展开更多
Perovskite nanocrystals(PNCs)have recently become promising optoelectronic materials due to their excellent photophysical properties.However,the highly dynamic binding state between ligands and the surface of PNCs has...Perovskite nanocrystals(PNCs)have recently become promising optoelectronic materials due to their excellent photophysical properties.However,the highly dynamic binding state between ligands and the surface of PNCs has severely restricted their luminescent properties and stabilities.In this work,1,3-bisbenzyl-2-oxoimidazolidine-4,5-dicarboxylic acid(cycle acid,CA)is introduced as both an etchant and a ligand upon post-synthetic surface treatment of PNCs.By removing the imperfect octahedrons[Pb X_(6)]^(4-)and passivating the surface defects synergistically,this treatment improves photoluminescence quantum yields from 76%to 95%and enhances the stability of PNCs against polar solvent,moisture,heat,and illumination.Meanwhile,CA can effectively and instantly recover the luminescence emission for aged PNCs.As a result,the CA-Cs Pb Br_(3)PNCs and CA-Cs Pb IxBr_(3-x)PNCs are applied as color-converting layers on a blue LED chip for warm white light-emitting diodes(WLEDs)with a color coordinate of(0.41,0.40).Importantly,the CA-based WLED device exhibits superior stability in operational conditions.展开更多
Doping in Si nanocrystals is an interesting topic and directly studying the distribution of dopants in phosphorous/boron co-doping is an important issue facing the scientific community.In this study,atom probe tomogra...Doping in Si nanocrystals is an interesting topic and directly studying the distribution of dopants in phosphorous/boron co-doping is an important issue facing the scientific community.In this study,atom probe tomography is performed to study the structures and distribution of impurity in phosphorous/boron co-doped Si nanocrystals/SiO_(2) multilayers.Compared with phosphorous singly doped Si nanocrystals,it is interesting to find that the concentration of phosphorous in co-doped samples can be significantly improved.Theoretical simulation suggests that phosphorous-boron pairs are formed in co-doped Si nanocrystals with the lowest formation energy,which also reduces the formation energy of phosphorous in Si nanocrystals.The results indicate that co-doping can promote the entry of phosphorous impurities into the near-surface and inner sites of Si nanocrystals,which provides an interesting way to regulate the electronic and optical properties of Si nanocrystals such as the observed enhancement of conductivity and sub-band light emission.展开更多
We investigate the transfer of phosphorescent energy between co-assembled metallophosphors in crystalline nanostructures [Angew. Chem. Int. Ed. 57 7820(2018) and J. Am. Chem. Soc. 140 4269(2018)]. Neither Dexter's...We investigate the transfer of phosphorescent energy between co-assembled metallophosphors in crystalline nanostructures [Angew. Chem. Int. Ed. 57 7820(2018) and J. Am. Chem. Soc. 140 4269(2018)]. Neither Dexter's nor Forster's mechanism of resonance energy transfer(RET) could account fully for the observed rates, which exceed 85% with significant temperature dependence. But there exists an alternative pathway on RET mediated by intermediate states of resonantly confined exciton–polaritons. Such a mechanism was used to analyze artificial photosynthesis in organic fluorescents [Phys.Rev. Lett. 122 257402(2019)]. For metallophosphors, the confined modes act as extended states lying between the molecular S_(1) and T_(1) states, offering a bridge for the long-lived T_(1) excitons to migrate from donors to acceptors. Population dynamics with parameters taken entirely based on experiments fits the observed lifetimes of phosphorescence across a broad range of doping and temperature.展开更多
Transformation of greenhouse gas(CO_(2))into valuable chemicals and fuels is a promising route to address the global issues of climate change and the energy crisis.Metal halide perovskite catalysts have shown their po...Transformation of greenhouse gas(CO_(2))into valuable chemicals and fuels is a promising route to address the global issues of climate change and the energy crisis.Metal halide perovskite catalysts have shown their potential in promoting CO_(2)reduction reaction(CO_(2)RR),however,their low phase stability has limited their application perspective.Herein,we present a reduced graphene oxide(rGO)wrapped CsPbI_3 perovskite nanocrystal(NC)CO_(2)RR catalyst(CsPbI_3/rGO),demonstrating enhanced stability in the aqueous electrolyte.The CsPbI_3/rGO catalyst exhibited>92%Faradaic efficiency toward formate production at a CO_(2)RR current density of~12.7 mA cm^(-2).Comprehensive characterizations revealed the superior performance of the CsPbI_3/rGO catalyst originated from the synergistic effects between the CsPbI_3 NCs and rGO,i.e.,rGO stabilized theα-CsPbI_3 phase and tuned the charge distribution,thus lowered the energy barrier for the protonation process and the formation of~*HCOO intermediate,which resulted in high CO_(2)RR selectivity toward formate.This work shows a promising strategy to rationally design robust metal halide perovskites for achieving efficient CO_(2)RR toward valuable fuels.展开更多
In this article, we report the results of our detailed investigations of the growth kinetics of zero-dimensional nanocrystals as well as one-dimensional nanorods by the combined use of small angel X-ray scattering (S...In this article, we report the results of our detailed investigations of the growth kinetics of zero-dimensional nanocrystals as well as one-dimensional nanorods by the combined use of small angel X-ray scattering (SAXS), transmission electron microscopy (TEM) along with other physical techniques. The study includes growth kinetics of gold nanocrystals formed by the reduction of HAuCl4 by tetrakis(hydroxymethyl) phosphonium chloride in aqueous solution, of CdSe nanocrystals formed by the reaction of cadmium stearate and selenium under solvothermal conditions, and of ZnO nanorods formed by the reaction of zinc acetate with sodium hydroxide under solvothermal conditions in the absence and presence of capping agents. The growth of gold nanocrystals does not follow the diffusion-limited Ostwald ripening, and instead follows a Sigmoidal rate curve. The heat change associated with the growth determined by isothermal titration calorimetry is about 10 kcal·mol^-1 per I nm increase in the diameter of the nanocrystals. In the case of CdSe nanocrystals also, the growth mechanism deviates from diffusion-limited growth and follows a combined model containing both diffusion and surface reaction terms. Our study of the growth kinetics of uncapped and poly(vinyl pyrollidone) (PVP)-capped ZnO nanorods has yielded interesting insights. We observe small nanocrystals next to the ZnO nanorods after a lapse of time in addition to periodic focusing and defocusing of the width of the length distribution. These observations lend support to the diffusion-limited growth model for the growth of uncapped ZnO nanorods. Accordingly, the time dependence on the length of uncapped nanorods follows the L3 law as required for diffusion-limited Ostwald ripening. The PVP-capped nanorods, however, show a time dependence, which is best described by a combination of diffusion (L^3) and surface reaction (L^2) terms.展开更多
基金the King Salman Center for Disability Research for funding this work through Research Group(No.KSRG-2023-538).
文摘The primary objective of global studies is to develop the properties and durability of polymers for various applications.When it comes to dental disability,denture base materials must have sufficient mechanical and tribological performance in order to withstand the forces experienced in the mouth.This work aims to investigate the effects of the addition of low content of cellulose nanocrystals(CNC)on the mechanical and tribological performance of the polymethyl methacrylate(PMMA)nanocomposites.Different weight percent of CNC(0,0.2,0.4,0.6,and 0.8 wt%)were added to the PMMA matrix followed by ball milling to evenly distribute the nanoparticles reinforced phase in the matrix phase.The findings emphasize the significant impact of CNC integration on the performance of PMMA nanocomposites.By increasing the content of the CNC nanoparticles,the mechanical properties of PMMA were improved.In addition,the tribological outcomes demonstrated a significant reduction in the friction coefficient besides an enhancement in the wear resistance as the weight percentage of nanoparticles increased.The surface of the worn samples was investigated by utilizing SEM to identify the wear mechanisms corresponding to the different compositions.In addition,a finite elment model(FEM)was developed to ascertain the thickness of the worn layer and the generated stressed on the surfaces of the nanocomposite throughout the friction process.
基金financially supported by the National Key Research and Development Program of China (2021YFB3600403)the Fundamental Research Funds for the Central Universities (000-0903069032)。
文摘Self-assembly of metal halide perovskite nanocrystals(NCs)into superlattices can exhibit unique collective properties,which have significant application values in the display,detector,and solar cell field.This review discusses the driving forces behind the self-assembly process of perovskite NCs,and the commonly used self-assembly methods and different self-assembly structures are detailed.Subsequently,we summarize the collective optoelectronic properties and application areas of perovskite superlattice structures.Finally,we conclude with an outlook on the potential issues and future challenges in developing perovskite NCs.
基金supported by the Guangdong Provincial Science&Technology Project(No.2023A0505050084)the National Natural Science Foundation of China(No.22361132525)+1 种基金the Fundamental Research Funds for the Central Universities(No.2023ZYGXZR002)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01X137).
文摘Mn^(2+)doping has been adopted as an efficient approach to regulating the luminescence properties of halide perovskite nano-crystals(NCs).However,it is still difficult to understand the interplay of Mn^(2+)luminescence and the matrix self-trapped exciton(STE)emission therein.In this study,Mn^(2+)-doped CsCdCl_(3) NCs are prepared by hot injection,in which CsCdCl_(3) is selected because of its unique crystal structure suitable for STE emission.The blue emission at 441 nm of undoped CsCdCl_(3) NCs originates from the defect states in the NCs.Mn^(2+)doping promotes lattice distortion of CsCdCl_(3) and generates bright orange-red light emission at 656 nm.The en-ergy transfer from the STEs of CsCdCl_(3) to the excited levels of the Mn^(2+)ion is confirmed to be a significant factor in achieving efficient luminescence in CsCdCl_(3):Mn^(2+)NCs.This work highlights the crucial role of energy transfer from STEs to Mn^(2+)dopants in Mn^(2+)-doped halide NCs and lays the groundwork for modifying the luminescence of other metal halide perovskite NCs.
文摘Formamidinium lead bromide(FAPbBr_(3))nanocrystals(NCs)have been considered to be a good optoelectronic material due to their pure green emission,excellent stability and superior carrier transport characteristics.However,two-photon pumped amplified spontaneous emission(ASE)and the corresponding nonlinear optical properties of FAPbBr_(3) NCs are scarcely revealed.Herein,we synthesized colloidal FAPbBr_(3) NCs with different sizes by changing the molar ratio of FABr/PbBr_(2) in the precursor solution,using ligand assisted precipitation(LARP)technology at room temperature.Photoluminescence(PL)and time resolved photoluminescence(TRPL)spectroscopy were measured to characterize their ASE properties.And their nonlinear optical properties were studied through the Zscan technique and the two-photon excited fluorescence method.The stimulated emission properties including oneand two-photon pumped ASE have been realized from FAPbBr_(3) NCs.With large two-photon absorption coefficient(0.27 cm/GW)and high non-linear absorption cross-section(7.52×10^(5) GM),ASE with threshold as low as 9.8μJ/cm^(2) and 487μJ/cm^(2) have been obtained from colloidal FAPbBr_(3) NCs using one-and two-photon excitations.These results indicate that as a new possible green-emitting frequency-upconversion material with low thresholds,FAPbBr_(3) NCs hold great potential in the development of high-performance two-photon pump lasers.
基金National Key R&D Program of China,Grant/Award Number:2022YFB3503700National Natural Science Foundation of China,Grant/Award Numbers:12074379,12174391,U22A20398,22135008+1 种基金Youth Innovation Promotion Association of CAS,Grant/Award Number:2020305Self-deployment Project Research Program of Haixi Institutes,CAS,Grant/Award Numbers:CXZX-2022-GS01,GCXZX-2022-GH10。
文摘The exceptional optoelectronic properties of lead halide perovskite nanocrystals(PeNCs)in the ultraviolet and visible spectral regions have positioned them as a promising class of semiconductor materials for diverse optoelectronic and photo-voltaic applications.However,their limited response to near-infrared(NIR)light due to the intrinsic bandgap(>1.5 eV)has hindered their applications in many advanced technologies.To circumvent this limitation,it is of fundamental significance to inte-grate PeNCs with lanthanide-doped upconversion nanoparticles(UCNPs)that are capable of efficiently converting low-energy NIR photons into high-energy ultravi-olet and visible photons.By leveraging the energy transfer from UCNPs to PeNCs,this synergistic combination can not only expand the NIR responsivity range of PeNCs but also introduce novel emission profiles to upconversion luminescence with multi-dimensional tunability(e.g.,wavelength,lifetime,and polarization)under low-to-medium power NIR irradiation,which breaks through the inherent restric-tions of individual PeNCs and UCNPs and thereby opens up new opportunities for materials and device engineering.In this review,we focus on the latest advance-ments in the development of PeNCs-UCNPs nanocomposites,with an emphasis on the controlled synthesis and optical properties design for advanced optoelectronic applications such as full-spectrum solar cells,NIR photodetectors,and multilevel anticounterfeiting.Some future efforts and prospects toward this active research field are also envisioned.
文摘The application potential of cellulosic materials in natural composites and other fields needs to be explored to develop innovative, sustainable, lightweight, functional biomass materials that are also environmentally friendly. This study investigated Typha angustifolia (Typha sp.) as a potential new raw material for extracting cellulose nanocrystals (CNCs) for application in wastewater treatment composites. Alkaline treatments and bleaching were used to remove cellulose from the stem fibres. The CNCs were then isolated from the recovered cellulose using acid hydrolysis. The study showed a few distinct functional groups (O-H, -C-H, =C-H and C-O, and C-O-C) in the Fourier Transform Infrared (FTIR) spectra. A scanning electron microscope (SEM) revealed the smooth surface of CPC and CNCs, which resulted from removing lignin and hemicellulose from powdered Typha angustifolia. Based on the crystalline index, the powdered Typha angustifolia, CPC, and CNCs were 42.86%, 66.94% and 77.41%. The loss of the amorphous section of the Typha sp. fibre resulted in a decrease in particle size. It may be inferred from the features of a Typha sp. CNC that CNCs may be employed as reinforcement in composites for wastewater treatment.
基金the financial support from National Natural Science Foundation of China (Grants Nos.12325203,91963117,and 11921002)。
文摘Recently,a Schwarz crystal structure with curved grain boundaries(GBs)constrained by twin-boundary(TB)networks was discovered in nanocrystalline Cu through experiments and atomistic simulations.Nanocrystalline Cu with nanosized Schwarz crystals exhibited high strength and excellent thermal stability.However,the grainsize effect and associated deformation mechanisms of Schwarz nanocrystals remain unknown.Here,we performed large-scale atomistic simulations to investigate the deformation behaviors and grain-size effect of nanocrystalline Cu with Schwarz crystals.Our simulations showed that similar to regular nanocrystals,Schwarz nanocrystals exhibit a strengthening-softening transition with decreasing grain size.The critical grain size in Schwarz nanocrystals is smaller than that in regular nanocrystals,leading to a maximum strength higher than that of regular nanocrystals.Our simulations revealed that the softening in Schwarz nanocrystals mainly originates from TB migration(or detwinning)and annihilation of GBs,rather than GB-mediated processes(including GB migration,sliding and diffusion)dominating the softening in regular nanocrystals.Quantitative analyses of simulation data further showed that compared with those in regular nanocrystals,the GB-mediated processes in Schwarz nanocrystals are suppressed,which is related to the low volume fraction of amorphous-like GBs and constraints of TB networks.The smaller critical grain size arises from the suppression of GB-mediated processes.
基金supported by the National Science Foundation (DMR 1808383)partially supported by S3IP at the State University of New York at Binghamton。
文摘To achieve environmentally benign energy conversion with the carbon neutrality target via electrochemical reactions, the innovation of electrocatalysts plays a vital role in the enablement of renewable resources. Nowadays, Pt-based nanocrystals(NCs) have been identified as one class of the most promising candidates to efficiently catalyze both the half-reactions in hydrogen-and hydrocarbonbased fuel cells. Here, we thoroughly discuss the key achievement in developing shape-controlled Pt and Pt-based NCs, and their electrochemical applications in fuel cells. We begin with a mechanistic discussion on how the morphology can be precisely controlled in a colloidal system, followed by highlighting the advanced development of shape-controlled Pt, Pt-alloy, Pt-based core@shell NCs, Pt-based nanocages, and Pt-based intermetallic compounds. We then select some case studies on models of typical reactions(oxygen reduction reaction at the cathode and small molecular oxidation reaction at the anode) that are enhanced by the shape-controlled Pt-based nanocatalysts. Finally, we provide an outlook on the potential challenges of shape-controlled nanocatalysts and envision their perspective with suggestions.
基金funded by the Zhengzhou Materials Genome Institute,the National Talents Program of China,and Key Innovation Projects of the Zhengzhou Municipal City of China.
文摘The main bottleneck against industrial utilization of sodium ion batteries(SIBs)is the lack of high-capacity electrodes to rival those of the benchmark lithium ion batteries(LIBs).Here in this work,we have developed an economical method for in situ fabrication of nanocomposites made of crystalline few-layer graphene sheets loaded with ultrafine SnO_(2)nanocrystals,using short exposure of microwave to xerogel of graphene oxide(GO)and tin tetrachloride containing minute catalyzing dispersoids of chemically reduced GO(RGO).The resultant nanocomposites(SnO_(2)@MWG)enabled significantly quickened redox processes as SIB anode,which led to remarkable full anode-specific capacity reaching 538 mAh g^(−1)at 0.05 A g^(−1)(about 1.45 times of the theoretical capacity of graphite for the LIB),in addition to outstanding rate performance over prolonged charge–discharge cycling.Anodes based on the optimized SnO_(2)@MWG delivered stable performance over 2000 cycles even at a high current density of 5 A g^(−1),and capacity retention of over 70.4%was maintained at a high areal loading of 3.4 mg cm^(−2),highly desirable for high energy density SIBs to rival the current benchmark LIBs.
基金supported by the Research Foundation Flanders(grant 3E181170)supported by the China Scholarship Council(CSC,201806220066)。
文摘Polypyrrole(PPy)is wildly used as electrode material in supercapacitors due to its high conductivity,low cost,ease of handling,and ease of fabrication.However,limited capacitance and poor cycling stability hinder its practical application.After developing carboxylated cellulose nanocrystals(CNC-COO^(-))as immobile dopants for PPy to improve its cycling stability,we investigated the effect of different commonly used salts(KCl,NaCl,KBr,and NaClO_(4))as dopants during electrode fabrication by electropolymerization.The film’s capacitance increased from 160.6 to 183.4 F g^(-1)after adding a combination of KCl and NaClO_(4) into the electrodeposition electrolyte.More importantly,the porous and interconnected PPy/CNC-COO^(-)-Cl-(Cl O_(4)^(-))_0.5 electrode film exhibited an excellent capacitance of 125.0 F g^(-1)(0.78 F cm^(-2))at a high current density of 2.0 Ag^(-1)(20 m A cm^(-2),allowing charging in less than 1 min),increasing almost 204%over PPy/CNC-COO-films.A symmetric PPy/CNC-COO^(-)-Cl-(ClO_(4)^(-))_0.5 supercapacitor retained its full capacitance after 5000 cycles,and displayed a high energy density of 5.2 Wh kg^(-1)at a power density of 25.4 W kg^(-1)(34.5μWh cm^(-2) at 1752.3μW cm^(-2)).These results reveal that the porous structure formed by doping with CNC-COO-and inorganic salts opens up more active reaction areas to store charges in PPy-based films as the stiff and ribbon-like CNC-COO-as permanent dopants improve the strength and stability of PPy-based films.Our demonstration provides a simple and practical way to deposit PPy based supercapacitors with high capacitance,fast charging,and excellent cycling stability.
基金the financial supports from National Natural Science Foundation of China(22178336 and 21991103).
文摘Ligand assisted reprecipitation(LARP)is a widely used method for cesium lead halide perovskite nanocrystals(NCs)synthesis.Nevertheless,the ultrafast kinetics of LARP,as well as the inefficient transport properties and discontinuity of batch reactors,challenge the particle size control and experimental repeatability.To address these issues,an ultrasonic cavitation-enabled microfluidic approach was developed to achieve the continuous synthesis of cesium lead halide perovskite via LARP.It was found that the mixing between the good solvent and antisolvent in the microchannel was greatly enhanced by intensive ultrasonic cavitation.The mixing time could be reduced to below 10 ms under the irradiation of 35 W ultrasound.By modulating the mixing degree,LARP was proved to be a mixing-sensitive process.The effects of ultrasonic power,ultrasonic treatment time,total flow rate,water additive,and reprecipitation temperature on the synthesis of CsPbBr_(3) NCs were systematically investigated.As compared to CsPbBr_(3) NCs synthesized in the batch reactor,the sample synthesized via the ultrasonic cavitation-enabled microfluidic approach possessed stronger photoluminescence intensity and better repeatability.Moreover,the ultrasonic cavitation-enabled microfluidic approach could also realize the continuous synthesis of cesium lead halide perovskite NCs with different halide compositions to cover a wide visible spectrum(426-661 nm).The ultrasonic cavitation-enabled microfluidic approach paved the way for the large-scale of high-quality cesium lead halide perovskite NCs.
基金the China National Postdoctoral Program for Innovative Talents(Bx20200386)China Postdoctoral Science Foundation(2021M703586)+1 种基金Key Program of National Natural Science Foundation of China(52130401)National Natural Science Foundation of China(52204064,52104055)for financial support.
文摘Nanocellulose,a natural polymeric nanomaterial,has attracted significant attention in enhanced oil recovery(EOR)applications due to its abundance,nanoscale,high oil-water interfacial adsorption ef-ficiency.In this study,surface-functionalized cellulose nanocrystals(SF-CNCs)were prepared via hy-drochloric acid hydrolysis and chemical modification,with adaptable nanosize and considerable dispersion stability in low-permeability reservoirs.The SF-CNCs were structurally characterized by FT-IR,Cryo-TEM,which have a diameter of 5-10 nm and a length of 100-200 nm.The SF-CNC dispersions possessed higher stability and stronger salt-tolerance than those of corresponding CNC dispersions,due to the strong hydrophilicity of the sulfonic acid group.It was synergistically used with a non-ionic surfactant(APG1214)to formulate a combined flooding system(0.1 wt%SF-CNC+0.2 wt%APG1214).The combined flooding system exhibits strong emulsification stability,low oil-water interfacial tension of o.03 mN/m,and the ability to alter the wettability for oil-wetting rocks.Furthermore,the combined system was_able to provide an optimum EOR efficiency of 20.2%in low-permeability cores with 30.13×10^(-3)μm^(2).Notably.it can enlarge the sweep volume and increase the displacement efficiency simultaneously.Overall,the newly formulated nanocellulose/surfactant combined system exhibits a remarkable EoR performance in low-permeability reservoirs.
基金supported by the National Natural Science Foundation of China (52102166)the China Postdoctoral Science Foundation under Grant Nos. 2019M663058, 2021M701065,2019M652749, 2021M701071, and 2022T150187+3 种基金the Program for Innovative Research Team in University of Henan Province(21IRTSTHN009)Science and Technology Development Plan of Henan Province (212300410029, 202300410087, 202102210251)the Key Research&Development and Promotion Project of Henan Province (Science and Technology Tackling Key Problems) under Grant Nos. 222102320182, 222102240070Henan Center for Outstanding Overseas Scientists (GZS2022014)。
文摘In recent years,photocatalytic CO_(2)reduction reaction(CRR) has attracted much scientific attention to overcome energy and environmental issues by converting CO_(2)into high-value-added chemicals utilizing solar energy.Metal halide perovskite(MHP) nanocrystals(NCs) are recognized as an ideal choice for CRR owing to their outstanding optoelectronic properties.Although great efforts have been devoted to designing more effective photocatalysts to optimize CRR performance,severe charge recombination,instability,and unsatisfactory activity have become major bottlenecks in developing perovskite-based photocatalysts.In this review,we mainly focus on the recent research progress in the areas of relevance.First,a brief insight into reaction mechanisms for CRR and structural features of MHPs are introduced.Second,efficient modification approaches for the improvement of the photocatalytic activity and stability of the perovskite-based catalysts are comprehensively reviewed.Third,the state-of-the-art achievements of perovskite-based photocatalysts for CRR are systematically summarized and discussed,which are focused on the modification approaches,structure design,and the mechanism of the CO_(2)reduction process.Lastly,the current challenges and future research perspectives in the design and application of perovskite materials are highlighted from our point of view to provide helpful insights for seeking breakthroughs in the field of CRR.This review may provide a guide for scientists interested in applying perovskite-based catalysts for solar-to-chemical energy conversion.
基金Project supported by the National Natural Science Foundation of China (Grant No. 62174079)the Fund from the Science, Technology, and Innovation Commission of Shenzhen Municipality (Grant Nos. JCYJ20220530113015035, JCYJ20210324120204011, JCYJ20190808121211510, and KQTD2015071710313656)。
文摘Perovskite nanocrystals(NCs) with high two-photon absorption(TPA) cross-section are of great interest due to their potential applications in three-dimensional optical data storage and multiphoton fluorescence microscopy. Among various perovskite materials, FAPbBr_(3) NCs show a better development prospect due to their excellent stability. However, there are few reports on their nonlinear optical properties. In this work, the nonlinear optical behavior of FAPbBr_(3) NCs is studied.The methods of multiphoton absorption photoluminescence saturation and open aperture Z-scan technique were applied to determine the TPA cross-section of FAPbBr_(3)NCs, which was around 2.76 × 10^(-45)cm^(4)·s·photon^(-1) at 800 nm. In addition,temperature-dependent photoluminescence induced by TPA was investigated, and the small longitudinal optical phonon energy and electron–phonon coupling strength was obtained, which confirm the weak Pb–Br interaction. Meanwhile, it is found that the exciton binding energy in FAPbBr_(3) NCs was 69.668 me V, which may be ascribed to the strong hydrogen bond interaction. It is expected that our findings will promote the application of FAPbBr_(3) NCs in optoelectronic devices.
基金supported by the National Natural Science Foundation of Tianjin(No.20JCQNJC01280)the National Natural Science Foundation of China(No.21905201)+1 种基金the support of the scientifi c research project from China Three Gorges Corporation(No.202103406)supported by Tohoku University and JSPS KAKENHI(No.JP16J06828).
文摘Sodium-ion hybrid capacitor(SIHC)is one of the most promising alternatives for large-scale energy storage due to its high energy and power densities,natural abundance,and low cost.However,overcoming the imbalance between slow Na^(+)reaction kinetics of battery-type anodes and rapid ion adsorption/desorption of capacitive cathodes is a significant challenge.Here,we propose the high-rate-performance NiS_(2)@OMGC anode material composed of monodispersed NiS_(2) nanocrystals(8.8±1.7 nm in size)and N,S-co-doped graphenic carbon(GC).The NiS_(2)@OMGC material has a three-dimensionally ordered macroporous(3DOM)morphology,and numerous NiS_(2) nanocrystals are uniformly embedded in GC,forming a core-shell structure in the local area.Ultrafine NiS_(2) nanocrystals and their nano-microstructure demonstrate high pseudocapacitive Na-storage capability and thus excellent rate performance(355.7 mAh/g at 20.0 A/g).A SIHC device fabricated using NiS_(2)@OMGC and commercial activated carbon(AC)cathode exhibits ultrahigh energy densities(197.4 Wh/kg at 398.8 W/kg)and power densities(43.9 kW/kg at 41.3 Wh/kg),together with a long life span.This outcome exemplifies the rational architecture and composition design of this type of anode material.This strategy can be extended to the design and synthesis of a wide range of high-performance electrode materials for energy storage applications.
基金financial from the National Natural Science Foundation of China(22279039 and 20181194)the Chinese National 1000-Talent-Plan program+2 种基金the Innovation Project of Optics Valley Laboratory(OVL2021BG008)the Frontier of the Application Foundation of Wuhan Science and Technology Plan Project(2020010601012202)the Foundation of State Key Laboratory of New Textile Materials and Advanced Processing Technologies(FZ2021011)。
文摘Perovskite nanocrystals(PNCs)have recently become promising optoelectronic materials due to their excellent photophysical properties.However,the highly dynamic binding state between ligands and the surface of PNCs has severely restricted their luminescent properties and stabilities.In this work,1,3-bisbenzyl-2-oxoimidazolidine-4,5-dicarboxylic acid(cycle acid,CA)is introduced as both an etchant and a ligand upon post-synthetic surface treatment of PNCs.By removing the imperfect octahedrons[Pb X_(6)]^(4-)and passivating the surface defects synergistically,this treatment improves photoluminescence quantum yields from 76%to 95%and enhances the stability of PNCs against polar solvent,moisture,heat,and illumination.Meanwhile,CA can effectively and instantly recover the luminescence emission for aged PNCs.As a result,the CA-Cs Pb Br_(3)PNCs and CA-Cs Pb IxBr_(3-x)PNCs are applied as color-converting layers on a blue LED chip for warm white light-emitting diodes(WLEDs)with a color coordinate of(0.41,0.40).Importantly,the CA-based WLED device exhibits superior stability in operational conditions.
基金Project supported by the National Key Research and Development Program of China (Grant No.2018YFB2200101)the National Natural Science Foundation of China (Grant Nos.62004078 and 61921005)+4 种基金Natural Science Foundation of Jiangsu Province (Grant No.BK20201073)Natural Science Foundation of Ningbo (Grant No.2021J068)ANR DONNA (Grant No.ANR-18-CE09-0034)Leading Innovative and Entrepreneur Team Introduction Program of Hangzhou (Grant No.TD2022012)partially supported by the CNRS Federation IRMA-FR 3095。
文摘Doping in Si nanocrystals is an interesting topic and directly studying the distribution of dopants in phosphorous/boron co-doping is an important issue facing the scientific community.In this study,atom probe tomography is performed to study the structures and distribution of impurity in phosphorous/boron co-doped Si nanocrystals/SiO_(2) multilayers.Compared with phosphorous singly doped Si nanocrystals,it is interesting to find that the concentration of phosphorous in co-doped samples can be significantly improved.Theoretical simulation suggests that phosphorous-boron pairs are formed in co-doped Si nanocrystals with the lowest formation energy,which also reduces the formation energy of phosphorous in Si nanocrystals.The results indicate that co-doping can promote the entry of phosphorous impurities into the near-surface and inner sites of Si nanocrystals,which provides an interesting way to regulate the electronic and optical properties of Si nanocrystals such as the observed enhancement of conductivity and sub-band light emission.
基金Project supported by the National Natural Science Foundation of China (Grant No. 16Z103060007) (PA)。
文摘We investigate the transfer of phosphorescent energy between co-assembled metallophosphors in crystalline nanostructures [Angew. Chem. Int. Ed. 57 7820(2018) and J. Am. Chem. Soc. 140 4269(2018)]. Neither Dexter's nor Forster's mechanism of resonance energy transfer(RET) could account fully for the observed rates, which exceed 85% with significant temperature dependence. But there exists an alternative pathway on RET mediated by intermediate states of resonantly confined exciton–polaritons. Such a mechanism was used to analyze artificial photosynthesis in organic fluorescents [Phys.Rev. Lett. 122 257402(2019)]. For metallophosphors, the confined modes act as extended states lying between the molecular S_(1) and T_(1) states, offering a bridge for the long-lived T_(1) excitons to migrate from donors to acceptors. Population dynamics with parameters taken entirely based on experiments fits the observed lifetimes of phosphorescence across a broad range of doping and temperature.
基金financial support by Australian Research Council(ARC)supported by the generous funding from Science and Engineering faculty,QUT。
文摘Transformation of greenhouse gas(CO_(2))into valuable chemicals and fuels is a promising route to address the global issues of climate change and the energy crisis.Metal halide perovskite catalysts have shown their potential in promoting CO_(2)reduction reaction(CO_(2)RR),however,their low phase stability has limited their application perspective.Herein,we present a reduced graphene oxide(rGO)wrapped CsPbI_3 perovskite nanocrystal(NC)CO_(2)RR catalyst(CsPbI_3/rGO),demonstrating enhanced stability in the aqueous electrolyte.The CsPbI_3/rGO catalyst exhibited>92%Faradaic efficiency toward formate production at a CO_(2)RR current density of~12.7 mA cm^(-2).Comprehensive characterizations revealed the superior performance of the CsPbI_3/rGO catalyst originated from the synergistic effects between the CsPbI_3 NCs and rGO,i.e.,rGO stabilized theα-CsPbI_3 phase and tuned the charge distribution,thus lowered the energy barrier for the protonation process and the formation of~*HCOO intermediate,which resulted in high CO_(2)RR selectivity toward formate.This work shows a promising strategy to rationally design robust metal halide perovskites for achieving efficient CO_(2)RR toward valuable fuels.
文摘In this article, we report the results of our detailed investigations of the growth kinetics of zero-dimensional nanocrystals as well as one-dimensional nanorods by the combined use of small angel X-ray scattering (SAXS), transmission electron microscopy (TEM) along with other physical techniques. The study includes growth kinetics of gold nanocrystals formed by the reduction of HAuCl4 by tetrakis(hydroxymethyl) phosphonium chloride in aqueous solution, of CdSe nanocrystals formed by the reaction of cadmium stearate and selenium under solvothermal conditions, and of ZnO nanorods formed by the reaction of zinc acetate with sodium hydroxide under solvothermal conditions in the absence and presence of capping agents. The growth of gold nanocrystals does not follow the diffusion-limited Ostwald ripening, and instead follows a Sigmoidal rate curve. The heat change associated with the growth determined by isothermal titration calorimetry is about 10 kcal·mol^-1 per I nm increase in the diameter of the nanocrystals. In the case of CdSe nanocrystals also, the growth mechanism deviates from diffusion-limited growth and follows a combined model containing both diffusion and surface reaction terms. Our study of the growth kinetics of uncapped and poly(vinyl pyrollidone) (PVP)-capped ZnO nanorods has yielded interesting insights. We observe small nanocrystals next to the ZnO nanorods after a lapse of time in addition to periodic focusing and defocusing of the width of the length distribution. These observations lend support to the diffusion-limited growth model for the growth of uncapped ZnO nanorods. Accordingly, the time dependence on the length of uncapped nanorods follows the L3 law as required for diffusion-limited Ostwald ripening. The PVP-capped nanorods, however, show a time dependence, which is best described by a combination of diffusion (L^3) and surface reaction (L^2) terms.