The proper bandgap and exceptional photostability enable CsPbI_(3) as a potential candidate for indoor photovoltaics(IPVs),but indoor power conversion efficiency(PCE) is impeded by serious nonradiative recombination s...The proper bandgap and exceptional photostability enable CsPbI_(3) as a potential candidate for indoor photovoltaics(IPVs),but indoor power conversion efficiency(PCE) is impeded by serious nonradiative recombination stemming from challenges in incomplete DMAPbI_(3) conversion and lattice structure distortion.Here,the coplanar symmetric structu re of hexyl sulfide(HS) is employed to functionalize the CsPbI_(3) layer for fabricating highly efficient IPVs.The hydrogen bond between HS and DMAI promotes the conversion of DMAPbI_(3) to CsPbI_(3),while the copianar symmetric structure enhances crystalline order.Simultaneously,surface sulfidation during HS-induced growth results in the in situ formation of PbS,spontaneously creating a CsPbI_(3) N-P homojunction to enhance band alignment and carrier mobility.As a result,the CsPbI_(3)&HS devices achieve an impressive indoor PCE of 39.90%(P_(in):334.6 μW cm^(-2),P_(out):133.5 μW cm^(-2)) under LED@2968 K,1062 lux,and maintain over 90% initial PCE for 800 h at ^(3)0% air ambient humidity.展开更多
A considerable efficiency gap exists between large-area perovskite solar modules and small-area perovskite solar cells.The control of forming uniform and large-area film and perovskite crystallization is still the mai...A considerable efficiency gap exists between large-area perovskite solar modules and small-area perovskite solar cells.The control of forming uniform and large-area film and perovskite crystallization is still the main obstacle restricting the efficiency of PSMs.In this work,we adopted a solid-liquid two-step film formation technique,which involved the evaporation of a lead iodide film and blade coating of an organic ammonium halide solution to prepare perovskite films.This method possesses the advantages of integrating vapor deposition and solution methods,which could apply to substrates with different roughness and avoid using toxic solvents to achieve a more uniform,large-area perovskite film.Furthermore,modification of the NiO_(x)/perovskite buried interface and introduction of Urea additives were utilized to reduce interface recombination and regulate perovskite crystallization.As a result,a large-area perovskite film possessing larger grains,fewer pinholes,and reduced defects could be achieved.The inverted PSM with an active area of 61.56 cm^(2)(10×10 cm^(2)substrate)achieved a champion power conversion efficiency of 20.56%and significantly improved stability.This method suggests an innovative approach to resolving the uniformity issue associated with large-area film fabrication.展开更多
On May 6, 2009, the X-ray imaging and biomedical application beamline(BL13W1) at Shanghai Synchrotron Radiation Facility(SSRF) officially opened to users, with 8–72.5 ke V X-rays. The experimental station is equipped...On May 6, 2009, the X-ray imaging and biomedical application beamline(BL13W1) at Shanghai Synchrotron Radiation Facility(SSRF) officially opened to users, with 8–72.5 ke V X-rays. The experimental station is equipped with four sets of X-ray CCD detectors of different pixel size(0.19–24 μm) for on-line phase-contrast imaging and micro-CT imaging with 0.8 μm spatial resolution and 1 ms temporal resolution. An in vivo microCT experiment for a living insect was realized in 4 s. An X-ray fluorescence detector is equipped for X-ray fluorescence mapping imaging and X-ray fluorescence micro-CT imaging with 50 μm spatial resolution. In order to meet different requirements from the users, several experimental methods, such as X-ray spiral micro-CT, Xray local micro-CT, X-ray fast micro-CT, X-ray grating-based differential micro-CT, X-ray fluorescence microCT and X-ray quantitative micro-CT have been developed, and nearly 60 papers related to those developments for this beamline have been published. Moreover, the beamline has realized the remote fast CT reconstruction,providing a great convenience for the users to process experimental data at their offices. As of August 2014,the beamline has offered the user beamtime of(23 145 h), from which 232 user papers have been published,including 151 SCI papers and 55 papers with SCI impact factor > 3. The quantity and quality of the user paper outcome keep a steady increase. Some typical user experimental results are introduced.展开更多
This paper introduces some latest developments regarding the X-ray imaging methodology and applications of the X-ray imaging and biomedical application beamline(BL13W1)at Shanghai Synchrotron Radiation Facility in the...This paper introduces some latest developments regarding the X-ray imaging methodology and applications of the X-ray imaging and biomedical application beamline(BL13W1)at Shanghai Synchrotron Radiation Facility in the past 5 years.The photon energy range of the beamline is 8–72.5 keV.Several sets of X-ray imaging detectors with different pixel sizes(0.19–24 lm)are used to realize X-ray microcomputed tomography(X-ray micro-CT)and X-ray in-line phase-contrast imaging.To satisfy the requirements of user experiments,new X-ray imaging methods and image processing techniques are developed.In vivo dynamic micro-CT experiments with living insects are performed in 0.5 s(sampling rate of 2 Hz,2 tomograms/s)with a monochromatic beam from a wiggler source and in 40 ms(sampling rate of 25 Hz,25 tomograms/s)with a white beam from a bending magnet source.A new X-ray imaging method known as move contrast X-ray imaging is proposed,with which blood flow and moving tissues in raw images can be distinguished according to their moving frequencies in the time domain.Furthermore,X-ray speckle-tracking imaging with twice exposures to eliminate the edge enhancement effect is developed.A high-precision quantification method is realized to measure complex three-dimensional blood vessels obtained via X-ray micro-CT.X-ray imaging methods such as three-dimensional X-ray diffraction microscopy,small-angle X-ray scattering CT,and X-ray fluorescence CT are developed,in which the X-ray micro-CT imaging method is combined with other contrast mechanisms such as diffraction,scattering,and fluorescence contrasts respectively.Moreover,an X-ray nano-CT experiment is performed with a 100 nm spatial resolution.Typical user experimental results from the fields of material science,biomedicine,paleontology,physics,chemistry,and environmental science obtained on the beamline are provided.展开更多
With the rapid rise in perovskite solar cells(PSCs)performance,it is imperative to develop scalable fabrication techniques to accelerate potential commercialization.However,the power conversion efficiencies(PCEs)of PS...With the rapid rise in perovskite solar cells(PSCs)performance,it is imperative to develop scalable fabrication techniques to accelerate potential commercialization.However,the power conversion efficiencies(PCEs)of PSCs fabricated via scalable two-step sequential deposition lag far behind the state-of-the-art spin-coated ones.Herein,the additive methylammonium chloride(MACl)is introduced to modulate the crystallization and orientation of a two-step sequential doctorbladed perovskite film in ambient conditions.MACl can significantly improve perovskite film quality and increase grain size and crystallinity,thus decreasing trap density and suppressing nonradiative recombination.Meanwhile,MACl also promotes the preferred face-up orientation of the(100)plane of perovskite film,which is more conducive to the transport and collection of carriers,thereby significantly improving the fill factor.As a result,a champion PCE of 23.14%and excellent longterm stability are achieved for PSCs based on the structure of ITO/SnO_(2)/FA_(1-x)MA_xPb(I_(1-y)Br_y)_3/Spiro-OMeTAD/Ag.The superior PCEs of 21.20%and 17.54%are achieved for 1.03 cm~2 PSC and 10.93 cm~2 mini-module,respectively.These results represent substantial progress in large-scale two-step sequential deposition of high-performance PSCs for practical applications.展开更多
Perovskite crystal facets greatly impact the performance and stability of their corresponding photovoltaic devices.Compared to the(001)facet,the(011)facet yields better photoelectric properties,including higher conduc...Perovskite crystal facets greatly impact the performance and stability of their corresponding photovoltaic devices.Compared to the(001)facet,the(011)facet yields better photoelectric properties,including higher conductivity and enhanced charge carrier mobility.Thus,achieving(011)facet-exposed films is a promising way to improve device performance.However,the growth of(011)facets is energetically unfavorable in FAPbI_(3) perovskites due to the influence of methylammonium chloride additive.Here,1-butyl-4-methylpyridinium chloride([4MBP]Cl)was used to expose(011)facets.The[4MBP]^(+)cation selectively decreases the surface energy of the(011)facet enabling the growth of the(011)plane.The[4MBP]^(+)cation causes the perovskite nuclei to rotate by 45°such that(011)crystal facets stack along the out-of-plane direction.The(011)facet has excellent charge transport properties and can achieve better-matched energy level alignment.In addition,[4MBP]Cl increases the activation energy barrier for ion migration,suppressing decomposition of the perovskite.As a result,a small-size device(0.06 cm2)and a module(29.0 cm2)based on exposure of the(011)facet achieved power conversion efficiencies of 25.24%and 21.12%,respectively.展开更多
Multilayer interference mirrors play a pivotal role in spectroscopic diagnostic systems,which probe electron temperature and density during inertial confinement fusion processes.In this study,aperiodic Mo/B_(4)C multi...Multilayer interference mirrors play a pivotal role in spectroscopic diagnostic systems,which probe electron temperature and density during inertial confinement fusion processes.In this study,aperiodic Mo/B_(4)C multilayer mirrors of varied thick-nesses were investigated for X-ray plasma diagnostics at the 9.67-keV W-Lβline.The thickness distribution of the aperiodic multilayers was designed using the first Bragg diffraction condition and then optimized through a simplex algorithm to realize a narrow bandwidth and consistent spectral response.To enhance spectral accuracy,further refinements were undertaken by matching the grazing incidence X-ray reflectivity data with actual structural parameters.X-ray reflectivity measurements from the SSRF synchrotron radiation facility on the optimized sample showed a reflectivity of 29.7±2.6%,flat-band range of 1.3 keV,and bandwidth of 1.7 keV,making it suitable for high-temperature plasma diagnostics.The study explored the potential of predicting the 9.67 keV reflectivity spectrum using the fitting data from the grazing incidence X-ray reflectivity curves at 8.05 keV.Additionally,the short-term thermal stability of an aperiodic multilayer was assessed using temperature-dependent in situ X-ray measurements.Shifts in the reflectivity spectrum during annealing were attributed to interdiffusion and interfacial relaxation.The research team recommends the aperiodic Mo/B_(4)C multilayer mirror for operations below 300℃.展开更多
The interfaces of perovskite solar cells(PSCs)are well known to be rich in deep-level carrier traps,which serve as non-radiative recombination centers and limit the open-circuit voltage(Voc)and power conversion effici...The interfaces of perovskite solar cells(PSCs)are well known to be rich in deep-level carrier traps,which serve as non-radiative recombination centers and limit the open-circuit voltage(Voc)and power conversion efficiency(PCE)of PSCs.Defect chemistry and surface passivators have been researched extensively and mainly focused on the neutralization of uncoordinated lead or anion defects.Herein,a novel brominated passivator 2-bromophenethylammonium iodide(2-Br-PEAI)is introduced for a multi-functional passivation effect at the perovskite interface.The brominated species readily form 2D perovskite on top of the 3D perovskite and multi-interact with the 3D perovskite surface.Apart from the halide vacancy filling and anion bonding ability,the Br atoms on the benzene ring can interact with the FA cations via strong hydrogen bonding N-H…Br and interact with the[PbI_(6)]^(4−)inorganic framework.The interface defects in the PSCs are well passivated,minimizing non-radiative recombination and enhancing device performance.As a result,a champion PCE of 24.22%was achieved with high V_(oc)and fill factor.In addition,modified devices also showed enhanced operational stability(retention of>95%initial PCE after 400 h)and humidity resistance(>90%initial PCE maintained after 1500 h under~50%RH).展开更多
Varying the film thickness is a precise route to tune the interfacial strain to manipulate the properties of the multiferroic materials.Here,to explore the effects of the interfacial strain on the properties of the mu...Varying the film thickness is a precise route to tune the interfacial strain to manipulate the properties of the multiferroic materials.Here,to explore the effects of the interfacial strain on the properties of the multiferroic BiFeO_3films,we investigated thickness-dependent structural and polarization evolutions of the BiFeO_3 films.The epitaxial growth with an atomic stacking sequence of BiO/TiO_2 at the interface was confirmed by scanning transmission electron microscopy.Combining X-ray diffraction experiments and first-principles calculations,a thickness-dependent structural evolution was observed from a fully strained tetragonality to a partially relaxed one without any structural phase transition or rotated twins.The tetragonality(c/a) of the BiFeO_3 films increases as the film thickness decreases,while the polarization is in contrast with this trend,and the size effect including the depolarization field plays a crucial role in this contradiction in thinner films.These findings offer an alternative strategy to manipulate structural and polarization properties by tuning the interfacial strain in epitaxial multiferroic thin films.展开更多
The complete elimination of methylammonium(MA)cations in Sn-Pb composites can extend their light and thermal stabilities.Unfortunately,MA-free Sn-Pb alloyed perovskite thin films suffer from wrinkled surfaces and poor...The complete elimination of methylammonium(MA)cations in Sn-Pb composites can extend their light and thermal stabilities.Unfortunately,MA-free Sn-Pb alloyed perovskite thin films suffer from wrinkled surfaces and poor crystallization,due to the coexistence of mixed intermediate phases.Here,we report an additive strategy for finely regulating the impurities in the intermediate phase of Cs_(0.25)FA_(0.75)Pb_(0.6)Sn_(0.4)I_(3)and,thereby,obtaining high-performance solar cells.We introduced d-homoserine lactone hydrochloride(D-HLH)to form hydrogen bonds and strong Pb-O/Sn-O bonds with perovskite precursors,thereby weakening the incomplete complexation effect between polar aprotic solvents(e.g.,DMSO)and organic(FAI)or inorganic(CsI,PbI_(2),and SnI_(2))components,and balancing their nucleation processes.This treatment completely transformed mixed intermediate phases into pure preformed perovskite nuclei prior to thermal anneal-ing.Besides,this D-HLH substantially inhibited the oxidation of Sn^(2+) species.This strategy generated a record efficiency of 21.61%,with a Voc of 0.88 V for an MA-free Sn-Pb device,and an efficiency of 23.82%for its tandem device.The unencapsulated devices displayed impressive thermal stability at 85℃ for 300 h and much improved continuous operation stability at MPP for 120 h.展开更多
Microstructure and oxidation behavior of modified Ni-16Mo-7Cr-4Fe alloys by yttrium microalloying were investigated by scanning electron microscopy, transmission electron microscopy, grazing incident Xray diffraction ...Microstructure and oxidation behavior of modified Ni-16Mo-7Cr-4Fe alloys by yttrium microalloying were investigated by scanning electron microscopy, transmission electron microscopy, grazing incident Xray diffraction and synchrotron radiation X-ray fluorescence. M6 C and Ni17Y2 phases were observed and the amount of Ni17Y2 increased with yttrium concentration. When the yttrium concentration increased to 0.43 wt.%,some Ni17Y2 chains and multi phase regions containing Ni17Y2, M6 C and γ phase appeared, which is harmful for the oxidation resistance. The alloy containing 0.05 wt.% yttrium showed the best oxidation resistance, which derives its oxidation resistance from the adequate concentration of yttrium in the solid-solution(γ phase), the formation of the protective layer of YCr O3 and chromia oxide and the strengthening effect of yttrium on oxide boundaries.展开更多
Multifunctional additives are widely used to improve crystallization and to passivate defects in perovskite solar cells. The roles of these additives are usually related to the various functional groups contained in s...Multifunctional additives are widely used to improve crystallization and to passivate defects in perovskite solar cells. The roles of these additives are usually related to the various functional groups contained in such additives. Here, we introduce a serious of analogues of amino acids into methylammonium lead iodide perovskites and find they play different roles in the crystallization process despite the fact that these additives share exactly the same terminal groups, namely one amino group and one carboxyl group. The corresponding crystallization pathways are established for the first time via monitoring the time-resolved phase formation and transformation. We find that avoiding the rapid formation of perovskites from precursor solution can facilitate the uniform nucleation and growth of perovskite crystals with enhanced crystallinity and reduced defects. Further, we find the different crystallization behaviors probably arise from the inherent structural characteristic of these additives, leading to different interactions in the precursors. This study unveils the effects of amino acids on the liquid–solid crystallization process and helps better understand the role of multifunctional additives beyond their functional groups.展开更多
Perovskite film quality is a decisive factor governing the performance and long-term stability of perovskite solar cells(PSCs). To passivate defects for high-quality perovskite films, various additives have been explo...Perovskite film quality is a decisive factor governing the performance and long-term stability of perovskite solar cells(PSCs). To passivate defects for high-quality perovskite films, various additives have been explored in perovskite precursor with notable achievements in the development of highperformance PSCs. Herein, tartaric acid(TA) was applied as additive in perovskite precursor solution to modulate the crystal growth leading to high quality thin films with enhanced multiple preferential orientations favoring efficient charge transport along multiple directions. It is also noticed that TA can improve the energy level alignment in PSCs, which effectively accelerates both carrier extraction and transportation with non-radiative recombination suppressed at the perovskite interfaces. Based on the present perovskite films, the fabricated PSCs achieved an excellent champion power conversion efficiency(PCE) of 21.82% from that of 19.70% for the control device without TA additive. In addition, a PSC with TA additive was shown to exhibit impressive operational stability by retaining 92% of its initial PCE after~1200 h of aging at room temperature in ambient air with a relative humidity of about 10%–25%. In summary, the present work demonstrates a facile and versatile approach by using TA as additive in perovskite precursor to fabricate high quality perovskite films with enhanced multiple preferential orientations for high-efficiency stable PSCs.展开更多
Pb-free Sn-based perovskite solar cells(PSCs) have recently made inspiring progress, and power conversion efficiency(PCE) of 14.8% has been achieved. However, due to the energy-level mismatch and poor interfacial cont...Pb-free Sn-based perovskite solar cells(PSCs) have recently made inspiring progress, and power conversion efficiency(PCE) of 14.8% has been achieved. However, due to the energy-level mismatch and poor interfacial contact between commonly used hole transport layer(i.e., poly(3,4-ethylenedioxythio phene):poly(styrene sulfonate), PEDOT:PSS) and FASnI_(3) film, it is still challenging to effectively extract holes at the interface. Owing to the p-type nature of Sn-based perovskites, the efficient hole extraction is of particular significance to improve the PCE of their solar cells. In this work, for the first time, the role of chiral cations, a-methylbenzylamine(S-/R-/rac-MBA), in promoting hole transportation of FASnI_(3)-based PSCs is demonstrated. The introduction of MBAs is found to form 2D/3D film with lowdimensional structures locating at PEDOT:PSS/FASnI_(3) interface, which facilitates the energy level alignment and efficient charge transfer at the interface. Importantly, chiral-induced spin selectivity(CISS)effect of R-MBA_(2)SnI_(4)induced by chiral R-MBA cation is found to further assist the specific interfacial transport of accumulated holes. As a result, R-MBA-based PSCs achieve decent PCE of 10.73% with much suppressed hysteresis and enhanced device stability. This work opens up a new strategy to efficiently promote the interfacial extraction of accumulated charges in working PSCs.展开更多
The development of efficient perovskite light-emitting diodes(PeLEDs)relies strongly on the fabrication of perovskite films with rationally designed structures(grain size,composition,surface,etc.).Therefore,an underst...The development of efficient perovskite light-emitting diodes(PeLEDs)relies strongly on the fabrication of perovskite films with rationally designed structures(grain size,composition,surface,etc.).Therefore,an understanding of structure-performance relationships is of vital importance for developing high-performance perovskite devices,particularly for devices with in-situ fabricated perovskite nanocrystal films.In this study,we reveal the vertical structure of an in-situ fabricated quasi-two-dimensional perovskite film.By combining time-of-flight secondary ion mass spectrometry,energy dispersive spectroscopy,grazing incidence wide-angle X-ray scattering(GIWAXS),and low-temperature photoluminescence spectra,we illustrate that the resulting in-situ fabricated DPPA_(2)Cs_(n-1)Pb_(n)(Br_(0.3)I_(0.7))_(3n+1)(DPPA^(+):3,3-diphenylpropylammonium)film has a gradient structure with a very thin layer of ligands on the surface,predominantly small-n domains at the top,and predominantly large-n domains at the bottom owing to the solubility difference of the precursors.In addition,GIWAXS measurements show that the domain of n=2 on the top layer has an ordered in-plane alignment.Based on the understanding of the film structure,we developed an in-situ fabrication process with ligand exchange to achieve efficient pure red PeLEDs at 638 nm with an average external quantum efficiency(EQE)of 7.4%.The optimized device had a maximum luminance of 623 cd/m^(2) with a peak EQE of 9.7%.展开更多
Metal phthalocyanines(MPcs) have gained considerable research attention as hole-transport materials(HTMs) in perovskite solar cells(PSCs) because of their superb stability. However, the photovoltaic performance of MPc...Metal phthalocyanines(MPcs) have gained considerable research attention as hole-transport materials(HTMs) in perovskite solar cells(PSCs) because of their superb stability. However, the photovoltaic performance of MPc-based HTMs in PSCs is still lagging behind their small molecule and polymeric counterparts, largely due to their relatively low hole mobility. Here, we report for the first time the application of a copper naphthalocyanine derivative(namely t Bu-Cu Nc) as a hole-transport material(HTM)in perovskite solar cells(PSCs), and systematically study its optoelectronic and photovoltaic property compared with its Cu Pc analog(t Bu-Cu Pc). Combined experiments disclose that the extension of π-conjugation from Pc to Nc core leads to not only an enhanced hole-carrier mobility associated with a stronger intermolecular interaction, but also an elevated glass transition temperature(T_g) of 252 °C. The resultant PSCs employing t Bu-Cu Nc deliver an excellent power conversion efficiency of 24.03%, which is the record efficiency reported for metal complex-based HTMs in PSCs. More importantly, the encapsulated t Bu-Cu Nc-based devices also show dramatically improved thermal stability than the devices using the well-known SpiroOMe TAD, with a T_(80)lifetime for more than 1,000 h under damp-heat stress. This study unfolds a new avenue for developing efficient and stable HTMs in PSCs.展开更多
Inkjet-printed quantum dot light-emitting diodes(QLEDs)are emerging as a promising technology for next-generation displays.However,the progress in fabricating QLEDs using inkjet printing technique has been slower comp...Inkjet-printed quantum dot light-emitting diodes(QLEDs)are emerging as a promising technology for next-generation displays.However,the progress in fabricating QLEDs using inkjet printing technique has been slower compared to spin-coated devices,particularly in terms of efficiency and stability.The key to achieving high performance QLEDs lies in creating a highly ordered and uniform inkjet-printed quantum dot(QD)thin film.In this study,we present a highly effective strategy to significantly improve the quality of inkjet-printed CdZnSe/CdZnS/ZnS QD thin films through a pressure-assisted thermal annealing(PTA)approach.Benefiting from this PTA process,a high quality QD thin film with ordered packing,low surface roughness,high photoluminescence and excellent electrical property is obtained.The mechanism behind the PTA process and its profound impact on device performance have been thoroughly investigated and understood.Consequently,a record high external quantum efficiency(EQE)of 23.08%with an impressive operational lifetime(T50)of up to 343,342h@100cdm−2,and a record EQE of 22.43%with T50 exceeding to 1,500,463h@100cdm−2 are achieved in inkjet-printed red and green CdZnSe-based QLEDs,respectively.This work highlights the PTA process as an important approach to realize highly efficient and stable inkjet-printed QLEDs,thus advancing QLED technology to practical applications.展开更多
Small Ag clusters confined in the channels of ordered mesoporous anatase TiO2 have been fabricated via a vacuum-assisted wet-impregnation method, utilizing well-ordered mesoporous anatase TiO2 with high thermal stabil...Small Ag clusters confined in the channels of ordered mesoporous anatase TiO2 have been fabricated via a vacuum-assisted wet-impregnation method, utilizing well-ordered mesoporous anatase TiO2 with high thermal stability as the host. The composites have been characterized in detail by X-ray diffraction, X-ray photoelectron spectroscopy X-ray absorption fine structure (XAFS) spectroscopy, N2 adsorption, UV-visible diffuse reflectance spectroscopy and transmission electron microscopy. The results indicate that small Ag clusters are formed and uniformly confined in the channels of mesoporous TiO2 with an obvious confinement effect. The presence of strong AgO interactions involving the Ag clusters in intimate contact with the pore walls of mesoporous TiO2 is confirmed by XAFS analysis, and favors the separation of photogenerated electron-hole pairs, as shown by steady-state surface photovoltage spectroscopy and transient-state surface photovoltage measurements. The ordered mesoporous Ag/TiO2 composites exhibit excellent solar-light-driven photocatalytic performance for the degradation of phenol. This is attributed to the synergistic effects between the small Ag clusters acting as traps to effectively capture the photogenerated electrons, and the surface plasmon resonance of the Ag clusters promoting the absorption of visible light. This study clearly demonstrates the high-efficiency utilization of noble metals in the fabrication of high-performance solar-light-driven photocatalysts.展开更多
The introduction of nitrogen significantly decreases the metal particle size and improves the performance of metal-based graphene-supported catalysts. In this work, the density functional theory is used to understand ...The introduction of nitrogen significantly decreases the metal particle size and improves the performance of metal-based graphene-supported catalysts. In this work, the density functional theory is used to understand the interaction between nitrogen-doped graphene and Pd@PdO clusters. Experiments show that small size Pd@PdO clusters (1-2 nm) can be grown uniformly on nitrogen-doped graphene sheets by a facile oxidation-reduction method. The nanoscale interaction relationship between nitrogen-doped graphene and Pd@PdO clusters is investigated through X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectra (XAS). The composite catalysts are applied in Suzuki-Miyaura reactions giving high yields and good structural stability. These results have potential impact in design and optimization of future high performance catalyst materials for cross coupling reactions.展开更多
In this paper, the macroscopic interaction method and high resolution EXAFS technique with a bent crystal analyzer were combined to study Eu(III) interaction mechanism and microstructure with y-MnOOH as a function o...In this paper, the macroscopic interaction method and high resolution EXAFS technique with a bent crystal analyzer were combined to study Eu(III) interaction mechanism and microstructure with y-MnOOH as a function of pH. The results indicated that Eu(III) interaction with y-MnOOH was apparently dependent on pH but independent of ionic strength, suggesting the for- mation of inner-sphere surface complexation for Eu(III) onto y-MnOOH. Results of EXAFS analysis indicated that Eu was surrounded by -9.00 atoms in first coordination shell at REu-O =2.40A, and second shell of Mn atoms at REu-Mn ≈ 3.60 was observed for the three adsorption samples. These findings suggested formation of a bidentate surface complex with Eu(III) bonding by edge sharing to MnO6-octahedron on y-MnOOH surface. Both the macroscopic interaction data and the molecular level evidence of Eu(III) microstructure at the 3,-MnOOH-water interface should be factored into better understanding the fate and mobility of Eu(III) and related radionuclides in the natural soil and water environment.展开更多
基金financial support from the Natural Science Foundation of Guizhou Province (Grant No. ZK 2024-087)Natural Science Foundation of China (no. 22005071)。
文摘The proper bandgap and exceptional photostability enable CsPbI_(3) as a potential candidate for indoor photovoltaics(IPVs),but indoor power conversion efficiency(PCE) is impeded by serious nonradiative recombination stemming from challenges in incomplete DMAPbI_(3) conversion and lattice structure distortion.Here,the coplanar symmetric structu re of hexyl sulfide(HS) is employed to functionalize the CsPbI_(3) layer for fabricating highly efficient IPVs.The hydrogen bond between HS and DMAI promotes the conversion of DMAPbI_(3) to CsPbI_(3),while the copianar symmetric structure enhances crystalline order.Simultaneously,surface sulfidation during HS-induced growth results in the in situ formation of PbS,spontaneously creating a CsPbI_(3) N-P homojunction to enhance band alignment and carrier mobility.As a result,the CsPbI_(3)&HS devices achieve an impressive indoor PCE of 39.90%(P_(in):334.6 μW cm^(-2),P_(out):133.5 μW cm^(-2)) under LED@2968 K,1062 lux,and maintain over 90% initial PCE for 800 h at ^(3)0% air ambient humidity.
基金the financial support from Shanxi Province Science and Technology Department(20201101012,202101060301016)the support from the APRC Grant of the City University of Hong Kong(9380086)+5 种基金the TCFS Grant(GHP/018/20SZ)MRP Grant(MRP/040/21X)from the Innovation and Technology Commission of Hong Kongthe Green Tech Fund(202020164)from the Environment and Ecology Bureau of Hong Kongthe GRF grants(11307621,11316422)from the Research Grants Council of Hong KongGuangdong Major Project of Basic and Applied Basic Research(2019B030302007)Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials(2019B121205002).
文摘A considerable efficiency gap exists between large-area perovskite solar modules and small-area perovskite solar cells.The control of forming uniform and large-area film and perovskite crystallization is still the main obstacle restricting the efficiency of PSMs.In this work,we adopted a solid-liquid two-step film formation technique,which involved the evaporation of a lead iodide film and blade coating of an organic ammonium halide solution to prepare perovskite films.This method possesses the advantages of integrating vapor deposition and solution methods,which could apply to substrates with different roughness and avoid using toxic solvents to achieve a more uniform,large-area perovskite film.Furthermore,modification of the NiO_(x)/perovskite buried interface and introduction of Urea additives were utilized to reduce interface recombination and regulate perovskite crystallization.As a result,a large-area perovskite film possessing larger grains,fewer pinholes,and reduced defects could be achieved.The inverted PSM with an active area of 61.56 cm^(2)(10×10 cm^(2)substrate)achieved a champion power conversion efficiency of 20.56%and significantly improved stability.This method suggests an innovative approach to resolving the uniformity issue associated with large-area film fabrication.
基金Supported by the National Natural Science Foundation of China(Nos.11475248 and 11105213)
文摘On May 6, 2009, the X-ray imaging and biomedical application beamline(BL13W1) at Shanghai Synchrotron Radiation Facility(SSRF) officially opened to users, with 8–72.5 ke V X-rays. The experimental station is equipped with four sets of X-ray CCD detectors of different pixel size(0.19–24 μm) for on-line phase-contrast imaging and micro-CT imaging with 0.8 μm spatial resolution and 1 ms temporal resolution. An in vivo microCT experiment for a living insect was realized in 4 s. An X-ray fluorescence detector is equipped for X-ray fluorescence mapping imaging and X-ray fluorescence micro-CT imaging with 50 μm spatial resolution. In order to meet different requirements from the users, several experimental methods, such as X-ray spiral micro-CT, Xray local micro-CT, X-ray fast micro-CT, X-ray grating-based differential micro-CT, X-ray fluorescence microCT and X-ray quantitative micro-CT have been developed, and nearly 60 papers related to those developments for this beamline have been published. Moreover, the beamline has realized the remote fast CT reconstruction,providing a great convenience for the users to process experimental data at their offices. As of August 2014,the beamline has offered the user beamtime of(23 145 h), from which 232 user papers have been published,including 151 SCI papers and 55 papers with SCI impact factor > 3. The quantity and quality of the user paper outcome keep a steady increase. Some typical user experimental results are introduced.
基金This work was supported by the National Key Research and Development Program of China(Nos.2017YFA0403801,2016YFA0401302,2017YFA0206004,2018YFC1200204)the National Major Scientific Instruments and Equipment Development Project of China(No.11627901).
文摘This paper introduces some latest developments regarding the X-ray imaging methodology and applications of the X-ray imaging and biomedical application beamline(BL13W1)at Shanghai Synchrotron Radiation Facility in the past 5 years.The photon energy range of the beamline is 8–72.5 keV.Several sets of X-ray imaging detectors with different pixel sizes(0.19–24 lm)are used to realize X-ray microcomputed tomography(X-ray micro-CT)and X-ray in-line phase-contrast imaging.To satisfy the requirements of user experiments,new X-ray imaging methods and image processing techniques are developed.In vivo dynamic micro-CT experiments with living insects are performed in 0.5 s(sampling rate of 2 Hz,2 tomograms/s)with a monochromatic beam from a wiggler source and in 40 ms(sampling rate of 25 Hz,25 tomograms/s)with a white beam from a bending magnet source.A new X-ray imaging method known as move contrast X-ray imaging is proposed,with which blood flow and moving tissues in raw images can be distinguished according to their moving frequencies in the time domain.Furthermore,X-ray speckle-tracking imaging with twice exposures to eliminate the edge enhancement effect is developed.A high-precision quantification method is realized to measure complex three-dimensional blood vessels obtained via X-ray micro-CT.X-ray imaging methods such as three-dimensional X-ray diffraction microscopy,small-angle X-ray scattering CT,and X-ray fluorescence CT are developed,in which the X-ray micro-CT imaging method is combined with other contrast mechanisms such as diffraction,scattering,and fluorescence contrasts respectively.Moreover,an X-ray nano-CT experiment is performed with a 100 nm spatial resolution.Typical user experimental results from the fields of material science,biomedicine,paleontology,physics,chemistry,and environmental science obtained on the beamline are provided.
基金supported by the National Key Research and Development Program of China(2022YFB3803300)the National Natural Science Foundation of China(51673214)the State Key Laboratory of Powder Metallurgy,Central South University,China。
文摘With the rapid rise in perovskite solar cells(PSCs)performance,it is imperative to develop scalable fabrication techniques to accelerate potential commercialization.However,the power conversion efficiencies(PCEs)of PSCs fabricated via scalable two-step sequential deposition lag far behind the state-of-the-art spin-coated ones.Herein,the additive methylammonium chloride(MACl)is introduced to modulate the crystallization and orientation of a two-step sequential doctorbladed perovskite film in ambient conditions.MACl can significantly improve perovskite film quality and increase grain size and crystallinity,thus decreasing trap density and suppressing nonradiative recombination.Meanwhile,MACl also promotes the preferred face-up orientation of the(100)plane of perovskite film,which is more conducive to the transport and collection of carriers,thereby significantly improving the fill factor.As a result,a champion PCE of 23.14%and excellent longterm stability are achieved for PSCs based on the structure of ITO/SnO_(2)/FA_(1-x)MA_xPb(I_(1-y)Br_y)_3/Spiro-OMeTAD/Ag.The superior PCEs of 21.20%and 17.54%are achieved for 1.03 cm~2 PSC and 10.93 cm~2 mini-module,respectively.These results represent substantial progress in large-scale two-step sequential deposition of high-performance PSCs for practical applications.
基金This work was funded by the European Union’s Horizon 2020 program,through a FET Proactive research and innovation action under grant agreement No.101084124(DIAMOND)supported by the 111 Project(B16016),and the Project of Scientific and Technological Support Program in Jiang Su Province(BE2022026-2)+2 种基金K.Z.thanks to the China Scholarship Council(no.202206730056)X.F.Z.thanks to the China Scholarship Council(no.202206730058)R.W.acknowledges the grant(LD22E020002)by the Natural Science Foundation of Zhejiang Province of China.
文摘Perovskite crystal facets greatly impact the performance and stability of their corresponding photovoltaic devices.Compared to the(001)facet,the(011)facet yields better photoelectric properties,including higher conductivity and enhanced charge carrier mobility.Thus,achieving(011)facet-exposed films is a promising way to improve device performance.However,the growth of(011)facets is energetically unfavorable in FAPbI_(3) perovskites due to the influence of methylammonium chloride additive.Here,1-butyl-4-methylpyridinium chloride([4MBP]Cl)was used to expose(011)facets.The[4MBP]^(+)cation selectively decreases the surface energy of the(011)facet enabling the growth of the(011)plane.The[4MBP]^(+)cation causes the perovskite nuclei to rotate by 45°such that(011)crystal facets stack along the out-of-plane direction.The(011)facet has excellent charge transport properties and can achieve better-matched energy level alignment.In addition,[4MBP]Cl increases the activation energy barrier for ion migration,suppressing decomposition of the perovskite.As a result,a small-size device(0.06 cm2)and a module(29.0 cm2)based on exposure of the(011)facet achieved power conversion efficiencies of 25.24%and 21.12%,respectively.
基金This work was supported by the National Natural Science Foundation of China(NSFC)(Nos.11875204 and U1932167)Fundamental Research Funds for the Central Universities(Nos.22120210446 and 22120180070)the Presidential Foundation of China Academy of Engineering Physics(No.YZJJLX2019011).
文摘Multilayer interference mirrors play a pivotal role in spectroscopic diagnostic systems,which probe electron temperature and density during inertial confinement fusion processes.In this study,aperiodic Mo/B_(4)C multilayer mirrors of varied thick-nesses were investigated for X-ray plasma diagnostics at the 9.67-keV W-Lβline.The thickness distribution of the aperiodic multilayers was designed using the first Bragg diffraction condition and then optimized through a simplex algorithm to realize a narrow bandwidth and consistent spectral response.To enhance spectral accuracy,further refinements were undertaken by matching the grazing incidence X-ray reflectivity data with actual structural parameters.X-ray reflectivity measurements from the SSRF synchrotron radiation facility on the optimized sample showed a reflectivity of 29.7±2.6%,flat-band range of 1.3 keV,and bandwidth of 1.7 keV,making it suitable for high-temperature plasma diagnostics.The study explored the potential of predicting the 9.67 keV reflectivity spectrum using the fitting data from the grazing incidence X-ray reflectivity curves at 8.05 keV.Additionally,the short-term thermal stability of an aperiodic multilayer was assessed using temperature-dependent in situ X-ray measurements.Shifts in the reflectivity spectrum during annealing were attributed to interdiffusion and interfacial relaxation.The research team recommends the aperiodic Mo/B_(4)C multilayer mirror for operations below 300℃.
基金supported by the National Natural Science Foundation of China(21872080)State Key Laboratory of Power System and Generation Equipment(No.SKLD21Z03,SKLD20M03)China Postdoctoral Science Foundation(No.043240004).
文摘The interfaces of perovskite solar cells(PSCs)are well known to be rich in deep-level carrier traps,which serve as non-radiative recombination centers and limit the open-circuit voltage(Voc)and power conversion efficiency(PCE)of PSCs.Defect chemistry and surface passivators have been researched extensively and mainly focused on the neutralization of uncoordinated lead or anion defects.Herein,a novel brominated passivator 2-bromophenethylammonium iodide(2-Br-PEAI)is introduced for a multi-functional passivation effect at the perovskite interface.The brominated species readily form 2D perovskite on top of the 3D perovskite and multi-interact with the 3D perovskite surface.Apart from the halide vacancy filling and anion bonding ability,the Br atoms on the benzene ring can interact with the FA cations via strong hydrogen bonding N-H…Br and interact with the[PbI_(6)]^(4−)inorganic framework.The interface defects in the PSCs are well passivated,minimizing non-radiative recombination and enhancing device performance.As a result,a champion PCE of 24.22%was achieved with high V_(oc)and fill factor.In addition,modified devices also showed enhanced operational stability(retention of>95%initial PCE after 400 h)and humidity resistance(>90%initial PCE maintained after 1500 h under~50%RH).
基金supported by the National Basic Research Program of China(Grant Nos.2012CB921403 and 2013CB328706)the National Natural Science Foundation of China(Grant Nos.10904030,11004238,11205235,11134012, 11404380,and 11474349)the Strategic Priority Research Program(B) of the Chinese Academy of Sciences(Grant No. XDB07030200)
文摘Varying the film thickness is a precise route to tune the interfacial strain to manipulate the properties of the multiferroic materials.Here,to explore the effects of the interfacial strain on the properties of the multiferroic BiFeO_3films,we investigated thickness-dependent structural and polarization evolutions of the BiFeO_3 films.The epitaxial growth with an atomic stacking sequence of BiO/TiO_2 at the interface was confirmed by scanning transmission electron microscopy.Combining X-ray diffraction experiments and first-principles calculations,a thickness-dependent structural evolution was observed from a fully strained tetragonality to a partially relaxed one without any structural phase transition or rotated twins.The tetragonality(c/a) of the BiFeO_3 films increases as the film thickness decreases,while the polarization is in contrast with this trend,and the size effect including the depolarization field plays a crucial role in this contradiction in thinner films.These findings offer an alternative strategy to manipulate structural and polarization properties by tuning the interfacial strain in epitaxial multiferroic thin films.
基金funded by the Natural Science Foundation of Shanghai(22ZR1428200)the National Natural Science Foundation of China(51950410581)+1 种基金the Shanghai Government(20JC141500)and CATL-SJTU joint funding.
文摘The complete elimination of methylammonium(MA)cations in Sn-Pb composites can extend their light and thermal stabilities.Unfortunately,MA-free Sn-Pb alloyed perovskite thin films suffer from wrinkled surfaces and poor crystallization,due to the coexistence of mixed intermediate phases.Here,we report an additive strategy for finely regulating the impurities in the intermediate phase of Cs_(0.25)FA_(0.75)Pb_(0.6)Sn_(0.4)I_(3)and,thereby,obtaining high-performance solar cells.We introduced d-homoserine lactone hydrochloride(D-HLH)to form hydrogen bonds and strong Pb-O/Sn-O bonds with perovskite precursors,thereby weakening the incomplete complexation effect between polar aprotic solvents(e.g.,DMSO)and organic(FAI)or inorganic(CsI,PbI_(2),and SnI_(2))components,and balancing their nucleation processes.This treatment completely transformed mixed intermediate phases into pure preformed perovskite nuclei prior to thermal anneal-ing.Besides,this D-HLH substantially inhibited the oxidation of Sn^(2+) species.This strategy generated a record efficiency of 21.61%,with a Voc of 0.88 V for an MA-free Sn-Pb device,and an efficiency of 23.82%for its tandem device.The unencapsulated devices displayed impressive thermal stability at 85℃ for 300 h and much improved continuous operation stability at MPP for 120 h.
基金Supported by the program of International S&T Cooperation(No.2014D FG60230)the National Natural Science Foundation of China(Nos.51371189 and 51371188)+1 种基金Science and Technology Commis sion of Shanghai Municipality(No.11JC1414900)the Scientific Research Foundation for the Returned Overseas Chinese Scholars,State Education Ministry
文摘Microstructure and oxidation behavior of modified Ni-16Mo-7Cr-4Fe alloys by yttrium microalloying were investigated by scanning electron microscopy, transmission electron microscopy, grazing incident Xray diffraction and synchrotron radiation X-ray fluorescence. M6 C and Ni17Y2 phases were observed and the amount of Ni17Y2 increased with yttrium concentration. When the yttrium concentration increased to 0.43 wt.%,some Ni17Y2 chains and multi phase regions containing Ni17Y2, M6 C and γ phase appeared, which is harmful for the oxidation resistance. The alloy containing 0.05 wt.% yttrium showed the best oxidation resistance, which derives its oxidation resistance from the adequate concentration of yttrium in the solid-solution(γ phase), the formation of the protective layer of YCr O3 and chromia oxide and the strengthening effect of yttrium on oxide boundaries.
基金financial support from the National Natural Science Foundation of China (Grant No. 22075094, 12075303 and 11675252)the National Key Research and Development Program of China (Grant No. 2016YFA0201101)the Fundamental Research Funds for the Central Universities。
文摘Multifunctional additives are widely used to improve crystallization and to passivate defects in perovskite solar cells. The roles of these additives are usually related to the various functional groups contained in such additives. Here, we introduce a serious of analogues of amino acids into methylammonium lead iodide perovskites and find they play different roles in the crystallization process despite the fact that these additives share exactly the same terminal groups, namely one amino group and one carboxyl group. The corresponding crystallization pathways are established for the first time via monitoring the time-resolved phase formation and transformation. We find that avoiding the rapid formation of perovskites from precursor solution can facilitate the uniform nucleation and growth of perovskite crystals with enhanced crystallinity and reduced defects. Further, we find the different crystallization behaviors probably arise from the inherent structural characteristic of these additives, leading to different interactions in the precursors. This study unveils the effects of amino acids on the liquid–solid crystallization process and helps better understand the role of multifunctional additives beyond their functional groups.
基金supported by the National Key Research and Development Program of China 2017YFA0403403 and 2017YFB0701901the Natural Science Foundation of China 12075303, 11675252 and U1632265。
文摘Perovskite film quality is a decisive factor governing the performance and long-term stability of perovskite solar cells(PSCs). To passivate defects for high-quality perovskite films, various additives have been explored in perovskite precursor with notable achievements in the development of highperformance PSCs. Herein, tartaric acid(TA) was applied as additive in perovskite precursor solution to modulate the crystal growth leading to high quality thin films with enhanced multiple preferential orientations favoring efficient charge transport along multiple directions. It is also noticed that TA can improve the energy level alignment in PSCs, which effectively accelerates both carrier extraction and transportation with non-radiative recombination suppressed at the perovskite interfaces. Based on the present perovskite films, the fabricated PSCs achieved an excellent champion power conversion efficiency(PCE) of 21.82% from that of 19.70% for the control device without TA additive. In addition, a PSC with TA additive was shown to exhibit impressive operational stability by retaining 92% of its initial PCE after~1200 h of aging at room temperature in ambient air with a relative humidity of about 10%–25%. In summary, the present work demonstrates a facile and versatile approach by using TA as additive in perovskite precursor to fabricate high quality perovskite films with enhanced multiple preferential orientations for high-efficiency stable PSCs.
基金financially supported by the Natural Science Foundation of China (Grants 51802253, 51972172, 61705102,61904152, and 91833304)the China Postdoctoral Science Foundation (Grant 2021M692630)+6 种基金the Natural Science Basic Research Plan in Shaanxi Province of China (2019JM-326)the Joint Research Funds of Department of Science&Technology of Shaanxi Province and Northwestern Polytechnical University (No. 2020GXLH-Z-007)the Natural Science Foundation of Jiangsu Province for Distinguished Young Scholars,China (Grant BK20200034)the Young 1000 Talents Global Recruitment Program of Chinathe Jiangsu Specially Appointed Professor programthe “Six talent peaks” Project in Jiangsu Province,Chinathe Fundamental Research Funds for the Central Universities。
文摘Pb-free Sn-based perovskite solar cells(PSCs) have recently made inspiring progress, and power conversion efficiency(PCE) of 14.8% has been achieved. However, due to the energy-level mismatch and poor interfacial contact between commonly used hole transport layer(i.e., poly(3,4-ethylenedioxythio phene):poly(styrene sulfonate), PEDOT:PSS) and FASnI_(3) film, it is still challenging to effectively extract holes at the interface. Owing to the p-type nature of Sn-based perovskites, the efficient hole extraction is of particular significance to improve the PCE of their solar cells. In this work, for the first time, the role of chiral cations, a-methylbenzylamine(S-/R-/rac-MBA), in promoting hole transportation of FASnI_(3)-based PSCs is demonstrated. The introduction of MBAs is found to form 2D/3D film with lowdimensional structures locating at PEDOT:PSS/FASnI_(3) interface, which facilitates the energy level alignment and efficient charge transfer at the interface. Importantly, chiral-induced spin selectivity(CISS)effect of R-MBA_(2)SnI_(4)induced by chiral R-MBA cation is found to further assist the specific interfacial transport of accumulated holes. As a result, R-MBA-based PSCs achieve decent PCE of 10.73% with much suppressed hysteresis and enhanced device stability. This work opens up a new strategy to efficiently promote the interfacial extraction of accumulated charges in working PSCs.
基金supported by the National Natural Science Foundation of China(61735004).
文摘The development of efficient perovskite light-emitting diodes(PeLEDs)relies strongly on the fabrication of perovskite films with rationally designed structures(grain size,composition,surface,etc.).Therefore,an understanding of structure-performance relationships is of vital importance for developing high-performance perovskite devices,particularly for devices with in-situ fabricated perovskite nanocrystal films.In this study,we reveal the vertical structure of an in-situ fabricated quasi-two-dimensional perovskite film.By combining time-of-flight secondary ion mass spectrometry,energy dispersive spectroscopy,grazing incidence wide-angle X-ray scattering(GIWAXS),and low-temperature photoluminescence spectra,we illustrate that the resulting in-situ fabricated DPPA_(2)Cs_(n-1)Pb_(n)(Br_(0.3)I_(0.7))_(3n+1)(DPPA^(+):3,3-diphenylpropylammonium)film has a gradient structure with a very thin layer of ligands on the surface,predominantly small-n domains at the top,and predominantly large-n domains at the bottom owing to the solubility difference of the precursors.In addition,GIWAXS measurements show that the domain of n=2 on the top layer has an ordered in-plane alignment.Based on the understanding of the film structure,we developed an in-situ fabrication process with ligand exchange to achieve efficient pure red PeLEDs at 638 nm with an average external quantum efficiency(EQE)of 7.4%.The optimized device had a maximum luminance of 623 cd/m^(2) with a peak EQE of 9.7%.
基金supported by the National Natural Science Foundation of China (52161145408, 21975038, 22088102)the National Key R&D Program of China (2022YFA0911904)+2 种基金the Fundamental Research Funds for the Central Universities (DUT23LAB611)the Central Guidance for Local Scientific and Technological Development Funds in Liaoning Province (2023JH6/100500006)the Research and Innovation Team Project of Dalian University of Technology(DUT2022TB10)。
文摘Metal phthalocyanines(MPcs) have gained considerable research attention as hole-transport materials(HTMs) in perovskite solar cells(PSCs) because of their superb stability. However, the photovoltaic performance of MPc-based HTMs in PSCs is still lagging behind their small molecule and polymeric counterparts, largely due to their relatively low hole mobility. Here, we report for the first time the application of a copper naphthalocyanine derivative(namely t Bu-Cu Nc) as a hole-transport material(HTM)in perovskite solar cells(PSCs), and systematically study its optoelectronic and photovoltaic property compared with its Cu Pc analog(t Bu-Cu Pc). Combined experiments disclose that the extension of π-conjugation from Pc to Nc core leads to not only an enhanced hole-carrier mobility associated with a stronger intermolecular interaction, but also an elevated glass transition temperature(T_g) of 252 °C. The resultant PSCs employing t Bu-Cu Nc deliver an excellent power conversion efficiency of 24.03%, which is the record efficiency reported for metal complex-based HTMs in PSCs. More importantly, the encapsulated t Bu-Cu Nc-based devices also show dramatically improved thermal stability than the devices using the well-known SpiroOMe TAD, with a T_(80)lifetime for more than 1,000 h under damp-heat stress. This study unfolds a new avenue for developing efficient and stable HTMs in PSCs.
基金This work was supported by NSFC(Nos.62261160392,52131304,61725402,U1605244,22279059)the Fundamental Research Funds for the Central Universities(Nos.30921011106,30919012107)+3 种基金the Research Innovation Program of Nanjing Overseas Returnees(No.AD411025)the start-up funding from the Nanjing University of Science and Technology,the Jiangsu Funding Program for Excellent Postdoctoral Talent(No.2023ZB844)the China Postdoctoral Science Foundation(No.2023M731687)The authors are also thankful for the support from the NJUST large instrument equipment open fund and Vacuum Interconnect Nano X Research Facility(NANO-X)of Suzhou Institute of Nano-Tech and Nano-Bionics,CAS.
文摘Inkjet-printed quantum dot light-emitting diodes(QLEDs)are emerging as a promising technology for next-generation displays.However,the progress in fabricating QLEDs using inkjet printing technique has been slower compared to spin-coated devices,particularly in terms of efficiency and stability.The key to achieving high performance QLEDs lies in creating a highly ordered and uniform inkjet-printed quantum dot(QD)thin film.In this study,we present a highly effective strategy to significantly improve the quality of inkjet-printed CdZnSe/CdZnS/ZnS QD thin films through a pressure-assisted thermal annealing(PTA)approach.Benefiting from this PTA process,a high quality QD thin film with ordered packing,low surface roughness,high photoluminescence and excellent electrical property is obtained.The mechanism behind the PTA process and its profound impact on device performance have been thoroughly investigated and understood.Consequently,a record high external quantum efficiency(EQE)of 23.08%with an impressive operational lifetime(T50)of up to 343,342h@100cdm−2,and a record EQE of 22.43%with T50 exceeding to 1,500,463h@100cdm−2 are achieved in inkjet-printed red and green CdZnSe-based QLEDs,respectively.This work highlights the PTA process as an important approach to realize highly efficient and stable inkjet-printed QLEDs,thus advancing QLED technology to practical applications.
文摘Small Ag clusters confined in the channels of ordered mesoporous anatase TiO2 have been fabricated via a vacuum-assisted wet-impregnation method, utilizing well-ordered mesoporous anatase TiO2 with high thermal stability as the host. The composites have been characterized in detail by X-ray diffraction, X-ray photoelectron spectroscopy X-ray absorption fine structure (XAFS) spectroscopy, N2 adsorption, UV-visible diffuse reflectance spectroscopy and transmission electron microscopy. The results indicate that small Ag clusters are formed and uniformly confined in the channels of mesoporous TiO2 with an obvious confinement effect. The presence of strong AgO interactions involving the Ag clusters in intimate contact with the pore walls of mesoporous TiO2 is confirmed by XAFS analysis, and favors the separation of photogenerated electron-hole pairs, as shown by steady-state surface photovoltage spectroscopy and transient-state surface photovoltage measurements. The ordered mesoporous Ag/TiO2 composites exhibit excellent solar-light-driven photocatalytic performance for the degradation of phenol. This is attributed to the synergistic effects between the small Ag clusters acting as traps to effectively capture the photogenerated electrons, and the surface plasmon resonance of the Ag clusters promoting the absorption of visible light. This study clearly demonstrates the high-efficiency utilization of noble metals in the fabrication of high-performance solar-light-driven photocatalysts.
文摘The introduction of nitrogen significantly decreases the metal particle size and improves the performance of metal-based graphene-supported catalysts. In this work, the density functional theory is used to understand the interaction between nitrogen-doped graphene and Pd@PdO clusters. Experiments show that small size Pd@PdO clusters (1-2 nm) can be grown uniformly on nitrogen-doped graphene sheets by a facile oxidation-reduction method. The nanoscale interaction relationship between nitrogen-doped graphene and Pd@PdO clusters is investigated through X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectra (XAS). The composite catalysts are applied in Suzuki-Miyaura reactions giving high yields and good structural stability. These results have potential impact in design and optimization of future high performance catalyst materials for cross coupling reactions.
基金Financial supports from the National Natural Science Foundation of China(1117524421207092)+1 种基金the project of Chinese Academy of Sciences(KJCX2-YW-N43)973 projects(2011CB933700)are acknowledged
文摘In this paper, the macroscopic interaction method and high resolution EXAFS technique with a bent crystal analyzer were combined to study Eu(III) interaction mechanism and microstructure with y-MnOOH as a function of pH. The results indicated that Eu(III) interaction with y-MnOOH was apparently dependent on pH but independent of ionic strength, suggesting the for- mation of inner-sphere surface complexation for Eu(III) onto y-MnOOH. Results of EXAFS analysis indicated that Eu was surrounded by -9.00 atoms in first coordination shell at REu-O =2.40A, and second shell of Mn atoms at REu-Mn ≈ 3.60 was observed for the three adsorption samples. These findings suggested formation of a bidentate surface complex with Eu(III) bonding by edge sharing to MnO6-octahedron on y-MnOOH surface. Both the macroscopic interaction data and the molecular level evidence of Eu(III) microstructure at the 3,-MnOOH-water interface should be factored into better understanding the fate and mobility of Eu(III) and related radionuclides in the natural soil and water environment.