Two-dimensional Ruddlesden-Popper(2DRP)perovskite exhibits excellent stability in perovskite solar cells(PSCs)due to introducing hydrophobic long-chain organic spacers.However,the poor charge transporting property of ...Two-dimensional Ruddlesden-Popper(2DRP)perovskite exhibits excellent stability in perovskite solar cells(PSCs)due to introducing hydrophobic long-chain organic spacers.However,the poor charge transporting property of bulky organic cation spacers limits the performance of 2DRP PSCs.Inspired by the Asite cation alloying strategy in 3D perovskites,2DRP perovskites with a binary spacer can promote charge transporting compared to the unary spacer counterparts.Herein,the superior MA-based 2DRP perovskite films with a binary spacer,including 3-guanidinopropanoic acid(GPA)and 4-fluorophenethylamine(FPEA)are realized.These films(GPA_(0.85)FPEA_(0.15))_(2)MA_(4)Pb_5I_(16)show good morphology,large grain size,decreased trap state density,and preferential orientation of the as-prepared film.Accordingly,the present 2DRP-based PSC with the binary spacer achieves a remarkable efficiency of 18.37%with a V_(OC)of1.15 V,a J_(SC)of 20.13 mA cm^(-2),and an FF of 79.23%.To our knowledge,the PCE value should be the highest for binary spacer MA-based 2DRP(n≤5)PSCs to date.Importantly,owing to the hydrophobic fluorine group of FPEA and the enhanced interlayer interaction by FPEA,the unencapsulated 2DRP PSCs based on binary spacers exhibit much excellent humidity stability and thermal stability than the unary spacer counterparts.展开更多
Perovskite solar cells(PSCs)offer low costs and high power conversion efficiency.However,the lack of long-term stability,primarily stemming from the interfacial defects and the sus-ceptible metal electrodes,hinders th...Perovskite solar cells(PSCs)offer low costs and high power conversion efficiency.However,the lack of long-term stability,primarily stemming from the interfacial defects and the sus-ceptible metal electrodes,hinders their practical application.In the past few years,two-dimensional(2D)materials(e.g.,graphene and its derivatives,transitional metal dichalcogenides,MXenes,and black phosphorus)have been identified as a promising solution to solving these problems because of their dangling bond-free surfaces,layer-dependent electronic band structures,tunable functional groups,and inherent compactness.Here,recent progress of 2D material toward efficient and stable PSCs is summarized,including its role as both interface materials and electrodes.We discuss their beneficial effects on perovskite growth,energy level alignment,defect passivation,as well as blocking external stimulus.In particular,the unique properties of 2D materials to form van der Waals heterojunction at the bottom interface are emphasized.Finally,perspectives on the further development of PSCs using 2D materials are provided,such as designing high-quality van der Waals heterojunction,enhancing the uniformity and coverage of 2D nanosheets,and developing new 2D materials-based electrodes.展开更多
Nanoparticles anchored on the perovskite surface have gained considerable attention for their wide-ranging applications in heterogeneous catalysis and energy conversion due to their robust and integrated structural co...Nanoparticles anchored on the perovskite surface have gained considerable attention for their wide-ranging applications in heterogeneous catalysis and energy conversion due to their robust and integrated structural configuration.Herein,we employ controlled Co doping to effectively enhance the nanoparticle exsolution process in layered perovskite ferrites materials.CoFe alloy nanoparticles with ultra-high-density are exsolved on the(PrBa)_(0.95)(Fe_(0.8)Co_(0.1)Nb_(0.1))2O_(5+δ)(PBFCN_(0.1))surface under reducing atmosphere,providing significant amounts of reaction sites and good durability for hydrocarbon catalysis.Under a reducing atmosphere,cobalt facilitates the reduction of iron cations within PBFCN_(0.1),leading to the formation of CoFe alloy nanoparticles.This formation is accompanied by a cation exchange process,wherein,with the increase in temperature,partial cobalt ions are substituted by iron.Meanwhile,Co doping significantly enhance the electrical conductivity due to the stronger covalency of the Cosingle bondO bond compared with Fesingle bondO bond.A single cell with the configuration of PBFCN_(0.1)-Sm_(0.2)Ce_(0.8)O_(1.9)(SDC)|SDC|Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF)-SDC achieves an extremely low polarization resistance of 0.0163Ωcm^(2)and a high peak power density of 740 mW cm^(−2)at 800℃.The cell also shows stable operation for 120 h in H_(2)with a constant current density of 285 mA cm^(−2).Furthermore,employing wet C_(2)H_(6)as fuel,the cell demonstrates remarkable performance,achieving peak power densities of 455 mW cm^(−2)at 800℃and 320 mW cm^(−2)at 750℃,marking improvements of 36%and 70%over the cell with(PrBa)_(0.95)(Fe_(0.9)Nb_(0.1))_(2)O_(5+δ)(PBFN)-SDC at these respective temperatures.This discovery emphasizes how temperature influences alloy nanoparticles exsolution within doped layered perovskite ferrites materials,paving the way for the development of high-performance ceramic fuel cell anodes.展开更多
Scintillation semiconductors play increasingly important medical diagnosis and industrial inspection roles.Recently,two-dimensional(2D)perovskites have been shown to be promising materials for medical X-ray imaging,bu...Scintillation semiconductors play increasingly important medical diagnosis and industrial inspection roles.Recently,two-dimensional(2D)perovskites have been shown to be promising materials for medical X-ray imaging,but they are mostly used in low-energy(≤130 keV)regions.Direct detection of MeV X-rays,which ensure thorough penetration of the thick shell walls of containers,trucks,and aircraft,is also highly desired in practical industrial applications.Unfortunately,scintillation semiconductors for high-energy X-ray detection are currently scarce.Here,This paper reports a 2D(C_(4)H_(9)NH_(3))_(2)PbBr_(4)single crystal with outstanding sensitivity and stability toward X-ray radiation that provides an ultra-wide detectable X-ray range of between 8.20 nGy_(air)s^(-1)(50 keV)and 15.24 mGy_(air)s^(-1)(9 MeV).The(C_(4)H_(9)NH_(3))_(2)PbBr_(4)single-crystal detector with a vertical structure is used for high-performance X-ray imaging,delivering a good spatial resolution of 4.3 Ip mm^(-1)in a plane-scan imaging system.Low ionic migration in the 2D perovskite enables the vertical device to be operated with hundreds of keV to MeV X-ray radiation at high bias voltages,leading to a sensitivity of 46.90μC Gy_(air)-1 cm^(-2)(-1.16 Vμm^(-1))with 9 MeV X-ray radiation,demonstrating that 2D perovskites have enormous potential for high-energy industrial applications.展开更多
Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the...Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the use of Ca_(2)MnO_(4)-layered perovskites modified with NaNO_(3) dopants,serving as redox catalysts(also known as oxygen carriers),for the CL-ODH of ethane within a temperature range of 700-780℃.Our findings revealed that the incorporation of NaNO_(3) as a modifier significantly-nhanced the selectivity for-thylene generation from Ca_(2)MnO_(4).At 750℃and a gas hourly space velocity of 1300 h^(-1),we achieved an-thane conversion up to 68.17%,accompanied by a corresponding-thylene yield of 57.39%.X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO_(3) onto Ca_(2)MnO_(4) not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox catalyst.Furthermore,formation of NaNO_(3) shell on the surface of Ca_(2)MnO_(4) led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise manner.This modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO_(3)-doped Ca_(2)MnO_(4) catalyst.These findings provide compelling evidence for the potential of Ca_(2)MnO_(4)-layered perovskites as promising redox catalysts in the context of CL-ODH reactions.展开更多
Two-dimensional Ruddlesden-Popper(2DRP)perovskites have attracted intense research interest for optoelectronic applications,due to their tunable optoelectronic properties and better environmental stability than their ...Two-dimensional Ruddlesden-Popper(2DRP)perovskites have attracted intense research interest for optoelectronic applications,due to their tunable optoelectronic properties and better environmental stability than their threedimensional counterparts.Furthermore,high-performance photodetectors based on single-crystal and polycrystalline thin-films 2DRP perovskites have shown great potential for practical application.However,the complex growth process of single-crystal membranes and uncontrollable phase distribution of polycrystalline films hinder the further development of 2DRP perovskites photodetectors.Herein,we report a series of high-performance photodetectors based on single-crystal-like phase-pure 2DRP perovskite films by designing a novel spacer source.Experimental and theoretical evidence demonstrates that phase-pure films substantially suppress defect states and ion migration.These highly sensitive photodetectors show I_(light)/I_(dark) ratio exceeding 3×10^(4),responsivities exceeding 16 A/W,and detectivities exceeding 3×10^(13) Jones,which are higher at least by 1 order than those of traditional mixed-phase thinfilms 2DRP devices(close to the reported single-crystal devices).More importantly,this strategy can significantly enhance the operational stability of optoelectronic devices and pave the way to large-area flexible productions.展开更多
Low-temperature processed electron transport layer(ETL)of TiO_(2)that is widely used in planar perovskite solar cells(PSCs)has inherent low carrier mobility,resulting in insufficient photogenerated elec-tron transport...Low-temperature processed electron transport layer(ETL)of TiO_(2)that is widely used in planar perovskite solar cells(PSCs)has inherent low carrier mobility,resulting in insufficient photogenerated elec-tron transport and thus recombination loss at buried interface.Herein,we demonstrate an effective strategy of laser embedding of p-n homojunctions in the TiO_(2)ETL to accelerate electron transport in PSCs,through localized build-in electric fields that enables boosted electron mobility by two orders of magnitude.Such embedding is found significantly helpful for not only the enhanced crystallization quality of TiO_(2)ETL,but the fabrication of perovskite films with larger-grain and the less-trap-states.The embedded p-n homojunction enables also the modulation of interfacial energy level between perovskite layers and ETLs,favoring for the reduced voltage deficit of PSCs.Benefiting from these merits,the formamidinium lead iodide(FAPbI_(3))PSCs employing such ETLs deliver a champion efficiency of 25.50%,along with much-improved device stability under harsh conditions,i.e.,maintain over 95%of their initial efficiency after operation at maximum power point under continuous heat and illumination for 500 h,as well as mixed-cation PSCs with a champion efficiency of 22.02%and over 3000 h of ambient storage under humidity stability of 40%.Present study offers new possibilities of regulating charge transport layers via p-n homojunction embedding for high performance optoelectronics.展开更多
Nickel oxide(NiO_(x))has been established as a highly efficient and stable holetransporting layer(HTL)in perovskite solar cells(PSCs).However,existing deposition methods for NiO_(x)have been restricted by high-vacuum ...Nickel oxide(NiO_(x))has been established as a highly efficient and stable holetransporting layer(HTL)in perovskite solar cells(PSCs).However,existing deposition methods for NiO_(x)have been restricted by high-vacuum processes and fail to address the energy level mismatch at the NiO_(x)/perovskite interface,which has impeded the development of PSCs.Accordingly,we explored the application of NiO_(x)as a hybrid HTL through a sol-gel process,where a NiO_(x)film was pre-doped with Ag ions,forming a p/p^(+)homojunction in the NiO_(x)-based inverted PSCs.This innovative approach offers two synergistic advantages,including the enlargement of the built-in electric field for facilitating charge separation,optimizing energy level alignment,and charge transfer efficiency at the interface between the perovskite and HTL.Incorporating this hybrid HTL featuring the p/p^(+)homojunction in the inverted PSCs resulted in a high-power conversion efficiency(PCE)of up to 19.25%,significantly narrowing the efficiency gap compared to traditional n-i-p devices.Furthermore,this innovative strategy for the HTL enhanced the environmental stability to 30 days,maintaining 90%of the initial efficiency.展开更多
Solid oxide electrolysis cell(SOEC) could be a potential technology to afford chemical storage of renewable electricity by converting water and carbon dioxide.In this work,we present the Ni-doped layered perovskite ox...Solid oxide electrolysis cell(SOEC) could be a potential technology to afford chemical storage of renewable electricity by converting water and carbon dioxide.In this work,we present the Ni-doped layered perovskite oxides,(La_(4)Sr_(n-4))_(0.9)Ti_(0.9n)Ni_(0.1n)O_(3n+2) with n=5,8,and 12(LSTNn) for application as catalysts of CO_(2) electrolysis with the exsolution of Ni nanoparticles through a simple in-situ growth method.It is found that the density,size,and distribution of exsolved Ni nanoparticles are determined by the number of n in LSTNn due to the different stack structures of TiO_6 octahedra along the c axis.The Ni doping in LSTNn significantly improved the electrochemical activity by increasing oxygen vacancies,and the Ni metallic nanoparticles afford much more active sites.The results show that LSTNn cathodes can successfully be manipulated the activity by controlling both the n number and Ni exsolution.Among these LSTNn(n=5,8,and 12),LSTN8 renders a higher activity for electrolysis of CO_(2) with a current density of 1.50A cm^(-2)@2.0 V at 800℃ It is clear from these results that the number of n in(La_(4)Sr_(n-4))_(0.9)Ti_(0.9n)Ni_(0.1n)O_(3n+2)with Ni-doping is a key factor in controlling the electrochemical performance and catalytic activity in SOEC.展开更多
Layered two dimensional(2D) or quasi-2D perovskites are emerging photovoltaic materials due to their superior environment and structure stability in comparison with their 3D counterparts. The typical 2D perovskites ca...Layered two dimensional(2D) or quasi-2D perovskites are emerging photovoltaic materials due to their superior environment and structure stability in comparison with their 3D counterparts. The typical 2D perovskites can be obtained by cutting 3D perovskites along < 100 > orientation by incorporation of bulky organic spacers, which play a key role in the performance of 2D perovskite solar cells(PSCs). Compared with aliphatic spacers, aromatic spacers with high dielectric constant have the potential to decrease the dielectric and quantum confinement effect of 2D perovskites, promote efficient charge transport and reduce the exciton binding energy, all of which are beneficial for the photovoltaic performance of 2D PSCs. In this review, we aim to provide useful guidelines for the design of aromatic spacers for 2D perovskites. We systematically reviewed the recent progress of aromatic spacers used in 2D PSCs. Finally, we propose the possible design strategies for aromatic spacers that may lead to more efficient and stable 2D PSCs.展开更多
Two-dimensional(2D) layered organic-inorganic hybrid perovskites have attracted much more attention for some applications than their three-dimensional(3D) perovskite counterparts due to their promising thermal and moi...Two-dimensional(2D) layered organic-inorganic hybrid perovskites have attracted much more attention for some applications than their three-dimensional(3D) perovskite counterparts due to their promising thermal and moisture stabilities.In particular, the 2D perovskite devices have shown better promise for optoelectronic applications.However, tunability of optoelectronic properties is often demanded to improve the device performance.Herein, we adopt a newly method to tune the electronic properties of 2D perovskite by introducing pseudohalide into the structure.In this work, we designed a pseudohalidesubstituted 2D perovskite by substituting the out-of-plane halide with pseudohalide and studied the electronic and excitonic properties of 2D-BA2MX4 and 2D-BA2MX2Ps2(M=Ge^(2+), Sn^(2+), and Pb^(2+);X=I;Ps=NCO, NCS, OCN, SCN, Se CN).We revealed the dependence of electronic properties including band gaps, composition of band edges, bonding characteristics, work functions, effective masses, and exciton binding energies on different pseudohalides substituted in 2D perovskite.Our results indicate that the substitution of pseudohalide in 2D perovskites is energetically favorable and can significantly affect the bonding characteristics as well as the CBM and VBM that often play major role in determining their performance in optoelectronic devices.It is expected that the pseudohalide substitution will be helpful in developing more advanced optoelectronic device based on 2D perovskite by optimizing band alignment and promoting charge extraction.展开更多
Research on two-dimensional(2D) materials is one of the most active fields in materials science and nanotechnology. Among the members of the 2D family, layered hydroxides(LHs) represent an exceptional case of study du...Research on two-dimensional(2D) materials is one of the most active fields in materials science and nanotechnology. Among the members of the 2D family, layered hydroxides(LHs) represent an exceptional case of study due to their unparalleled chemical versatility which allows the modulation of their physicochemical properties at will. Nowadays, LHs based on earth-abundant metals are key materials in the areas of energy storage and conversion, hybrid materials or magnetism. α-Co hydroxides(Simonkolleite-like structures) are promising phases with tuneable electronic and magnetic properties by ligand modification. However, even in the simple case of α-Co^(Ⅱ) hydroxychlorides, the preparation of well-defined large 2D crystals is not straightforward, hindering the development of fundamental studies. Herein, we present the synthesis of 2D hexagonal crystals with outstanding sizethickness relationship(diameter > 5 μm and thickness of 20 ± 7 nm) by a simple homogeneous synthesis taking place at room temperature. In structural terms, no differences are observed between our layered materials and those obtained hydrothermally. However, dynamic susceptibility measurements alert about different arrangements of the magnetic sublattices, which have been rationalized with structural DFT calculations. This work provides an extremely easy bottom-up method to obtain high-quality 2D crystals based on α-CoIIhydroxides,paving the way for the development of fundamental studies and applications.展开更多
Two-dimensional(2D) layered perovskites have emerged as potential alternates to traditional three-dimensional(3D)analogs to solve the stability issue of perovskite solar cells. In recent years, many efforts have been ...Two-dimensional(2D) layered perovskites have emerged as potential alternates to traditional three-dimensional(3D)analogs to solve the stability issue of perovskite solar cells. In recent years, many efforts have been spent on manipulating the interlayer organic spacing cation to improve the photovoltaic properties of Dion–Jacobson(DJ) perovskites. In this work, a serious of cycloalkane(CA) molecules were selected as the organic spacing cation in 2D DJ perovskites, which can widely manipulate the optoelectronic properties of the DJ perovskites. The underlying relationship between the CA interlayer molecules and the crystal structures, thermodynamic stabilities, and electronic properties of 58 DJ perovskites has been investigated by using automatic high-throughput workflow cooperated with density-functional(DFT) calculations.We found that these CA-based DJ perovskites are all thermodynamic stable. The sizes of the cycloalkane molecules can influence the degree of inorganic framework distortion and further tune the bandgaps with a wide range of 0.9–2.1 eV.These findings indicate the cycloalkane molecules are suitable as spacing cation in 2D DJ perovskites and provide a useful guidance in designing novel 2D DJ perovskites for optoelectronic applications.展开更多
The high efficiency and low production cost enable the halide perovskite solar cells as a promising technology for the next generation photovoltaics.Nevertheless,the relatively poor stability of the organic–inorganic...The high efficiency and low production cost enable the halide perovskite solar cells as a promising technology for the next generation photovoltaics.Nevertheless,the relatively poor stability of the organic–inorganic halide perovskites hinders their commercial applications.In the past few years,two-dimensional(2D)perovskite has emerged as a more stable alternative to the three-dimensional(3D)counterparts and attracted intense research interests.Although many attempts and advances have been made,it is still ambiguous that whether the 2D perovskites could bring closure to the stability issue.To answer this essential question,a systematic study of the nature of 2D halide perovskites is necessary.Here,we focus on the stability investigations of 2D perovskites from different perspectives,especially light,heat,ion migration and strain.Several remaining challenges and opening problems are also discussed.With further material and device engineering,we believe that the 2D perovskites would promote perovskite solar cells to a promising future.展开更多
Taking advantage of the excellent stability and photoelectric properties,two-dimensional(2D)organicinorganic halide perovskites have been widely researched and applied in optoelectronic and photovoltaic devices.The re...Taking advantage of the excellent stability and photoelectric properties,two-dimensional(2D)organicinorganic halide perovskites have been widely researched and applied in optoelectronic and photovoltaic devices.The remarkable properties are attributed to the unique quantum well structures by intercalating large organic ammonium space layers.In this review,we first summarize the crystal structures and growth methods of 2D halide perovskite crystals.Then,the distinctive optical characteristics and enhanced stability under high humidity,phase stability,suppressed ion migration,and high formation energy,are discussed in detail.Furthermore,we discuss orientation control in 2D perovskite films.The applications of 2D perovskites in solar cells,photo detectors and X-ray detectors are discussed in detail.Finally,we propose an outlook and perspectives to overcome the present challenges and broaden this new class of perovskite materials with other 2D nanomaterials.展开更多
The instability of thin ferroelectric films is discussed based on the close similarity of dielectric properties between bulk Bi-layered perovskites and thin BaTiO<sub>3</sub> films. The dielectric properti...The instability of thin ferroelectric films is discussed based on the close similarity of dielectric properties between bulk Bi-layered perovskites and thin BaTiO<sub>3</sub> films. The dielectric properties of pseudo-two-dimensional layered perovskites suggest that the bulk layered ferroelectric is a good model of ultra-thin ferroelectric film with a few perovskite units, free from any misfit lattice strain. It seems plausible that the ferroelectric interaction is still prominent but shows a crossover from ferroelectric to antiferroelectric along the unique c-axis (perpendicular to the film plane);with decreasing thickness, the ferroelectricity appears within the plane, which results in so-called “canted ferroelectricity”. An extra relaxation mode induced by surface effect of thin films correlates with soft mode, which results in a new intermediate phase between the paraelectric and ferroelectric phases. These evidences may indicate no critical thickness even for ferroelectric ultra- thin films.展开更多
Two-dimensional(2D)lead halide perovskites have attracted tremendous attention due to their outstanding physical properties.However,the presence of toxic lead is a major problem for large-scale applications.Here,we re...Two-dimensional(2D)lead halide perovskites have attracted tremendous attention due to their outstanding physical properties.However,the presence of toxic lead is a major problem for large-scale applications.Here,we report the synthesis,phase transition,dielectric and photoluminescence(PL)properties of a lead-free 2D Ge-based perovskite(BIM)_(2)GeI_(4)(BIM=benzimidazolium)which experiences a phase transition at 405 K accompanied by an order-disorder change of organic spacer.Moreover,the step-like dielectric transition near the phase transition temperature makes it suitable for dielectric switching.Meanwhile,(BIM)_(2)GeI_(4)has a direct bandgap of 2.23 eV and broadband emission from 550 to 1000 nm,implying its unique optical property for potential near-infrared lighting and displaying.This work provides a fresh example for the development of lead-free 2D Ge-based perovskite with potential applications in the fields of optoelectronics and high temperature dielectric switching.展开更多
Atomically thin two-dimensional(2D) materials are the building bricks for next-generation electronics and optoelectronics, which demand plentiful functional properties in mechanics, transport, magnetism and photorespo...Atomically thin two-dimensional(2D) materials are the building bricks for next-generation electronics and optoelectronics, which demand plentiful functional properties in mechanics, transport, magnetism and photoresponse.For electronic devices, not only metals and high-performance semiconductors but also insulators and dielectric materials are highly desirable. Layered structures composed of 2D materials of different properties can be delicately designed as various useful heterojunction or homojunction devices, in which the designs on the same material(namely homojunction) are of special interest because preparation techniques can be greatly simplified and atomically seamless interfaces can be achieved. We demonstrate that the insulating pristine ZnPS_3, a ternary transition-metal phosphorus trichalcogenide, can be transformed into a highly conductive metal and an n-type semiconductor by intercalating Co and Cu atoms, respectively. The field-effect-transistor(FET) devices are prepared via an ultraviolet exposure lithography technique. The Co-ZnPS_3 device exhibits an electrical conductivity of 8 × 10^(4) S/m, which is comparable to the conductivity of graphene. The Cu-ZnPS_3 FET reveals a current ON/OFF ratio of 1-05 and a mobility of 3 × 10^(-2 )cm^(2)·V^(-1)·s^(-1). The realization of an insulator, a typical semiconductor and a metallic state in the same 2D material provides an opportunity to fabricate n-metal homojunctions and other in-plane electronic functional devices.展开更多
To achieve high power conversion efficiency(PCE) and long-term stability of perovskite solar cells(PSCs), a hole transport layer(HTL) with persistently high conductivity, good moisture/oxygen barrier ability, and adeq...To achieve high power conversion efficiency(PCE) and long-term stability of perovskite solar cells(PSCs), a hole transport layer(HTL) with persistently high conductivity, good moisture/oxygen barrier ability, and adequate passivation capability is important. To achieve enough conductivity and effective hole extraction, spiro-OMe TAD, one of the most frequently used HTL in optoelectronic devices, often needs chemical doping with a lithium compound(LiTFSI). However, the lithium salt dopant induces crystallization and has a negative impact on the performance and lifetime of the device due to its hygroscopic nature. Here, we provide an easy method for creating a gel by mixing a natural small molecule additive(thioctic acid, TA) with spiro-OMe TAD. We discover that gelation effectively improves the compactness of resultant HTL and prevents moisture and oxygen infiltration. Moreover, the gelation of HTL improves not only the conductivity of spiro-OMe TAD, but also the operational robustness of the devices in the atmospheric environment. In addition, TA passivates the perovskite defects and facilitates the charge transfer from the perovskite layer to HTL. As a consequence, the optimized PSCs based on the gelated HTL exhibit an improved PCE(22.52%) with excellent device stability.展开更多
Three kinds of new layered perovskite compounds with Ruddlesden-Popper (R-P) phase, AgrNa2-xLa2Ti3O10 (x = 0.2, 0.3 and 0.5), were synthesized by an ion-exchange reaction of Na2La2Ti3O10 with AgNO3 solution. The s...Three kinds of new layered perovskite compounds with Ruddlesden-Popper (R-P) phase, AgrNa2-xLa2Ti3O10 (x = 0.2, 0.3 and 0.5), were synthesized by an ion-exchange reaction of Na2La2Ti3O10 with AgNO3 solution. The structures of the compounds were characterized by EDX and XRD, and their antibacterial activity and light-resistance property were evaluated. The results indicated that the molecular formula of AgxNa2-xLa2Ti3O10 (x = 0.2, 0.3 and 0.5) was confirmed, and that the crystalline structure of Na2La2Ti3O10 was not obviously affected by exchange of silver ion. The minimum inhibitory concentrations (MICs) of Ag0.3Na1.7La2Ti3O10 against Escherichia coli (E. coli), Staphylococcus aureus (S. aureus) were 180 μg/mL and 240 μg/mL, respectively, while its discoloration was not observed after 24 h light ageing test.展开更多
基金financially supported by the Natural Science Foundation of China(Grant Nos.52372226,52173263,62004167)the Natural Science Basic Research Plan in Shaanxi Province of China(Grant Nos.2022JM-315,2023-JC-QN-0643)+4 种基金the National Key R&D Program of China(Grant No.2022YFB3603703)the Qinchuangyuan High-level Talent Project of Shaanxi(Grant No.QCYRCXM-2022-219)the Ningbo Natural Science Foundation(Grant No.2022J061)the Key Research and Development Program of Shaanxi(Grant No.2023GXLH-091)the Shccig-Qinling Program and the Fundamental Research Funds for the Central Universities。
文摘Two-dimensional Ruddlesden-Popper(2DRP)perovskite exhibits excellent stability in perovskite solar cells(PSCs)due to introducing hydrophobic long-chain organic spacers.However,the poor charge transporting property of bulky organic cation spacers limits the performance of 2DRP PSCs.Inspired by the Asite cation alloying strategy in 3D perovskites,2DRP perovskites with a binary spacer can promote charge transporting compared to the unary spacer counterparts.Herein,the superior MA-based 2DRP perovskite films with a binary spacer,including 3-guanidinopropanoic acid(GPA)and 4-fluorophenethylamine(FPEA)are realized.These films(GPA_(0.85)FPEA_(0.15))_(2)MA_(4)Pb_5I_(16)show good morphology,large grain size,decreased trap state density,and preferential orientation of the as-prepared film.Accordingly,the present 2DRP-based PSC with the binary spacer achieves a remarkable efficiency of 18.37%with a V_(OC)of1.15 V,a J_(SC)of 20.13 mA cm^(-2),and an FF of 79.23%.To our knowledge,the PCE value should be the highest for binary spacer MA-based 2DRP(n≤5)PSCs to date.Importantly,owing to the hydrophobic fluorine group of FPEA and the enhanced interlayer interaction by FPEA,the unencapsulated 2DRP PSCs based on binary spacers exhibit much excellent humidity stability and thermal stability than the unary spacer counterparts.
基金the financial support of the National Natural Science Foundation of China(Nos.U21A20171,12074245,and 52102281)National Key R&D Program of China(Nos.2021YFB3800068 and 2020YFB1506400)+1 种基金Shanghai Sailing Program(No.21YF1421600)Young Elite Scientists Sponsorship Program by China Association for Science and Technology(No.2021QNRC001).
文摘Perovskite solar cells(PSCs)offer low costs and high power conversion efficiency.However,the lack of long-term stability,primarily stemming from the interfacial defects and the sus-ceptible metal electrodes,hinders their practical application.In the past few years,two-dimensional(2D)materials(e.g.,graphene and its derivatives,transitional metal dichalcogenides,MXenes,and black phosphorus)have been identified as a promising solution to solving these problems because of their dangling bond-free surfaces,layer-dependent electronic band structures,tunable functional groups,and inherent compactness.Here,recent progress of 2D material toward efficient and stable PSCs is summarized,including its role as both interface materials and electrodes.We discuss their beneficial effects on perovskite growth,energy level alignment,defect passivation,as well as blocking external stimulus.In particular,the unique properties of 2D materials to form van der Waals heterojunction at the bottom interface are emphasized.Finally,perspectives on the further development of PSCs using 2D materials are provided,such as designing high-quality van der Waals heterojunction,enhancing the uniformity and coverage of 2D nanosheets,and developing new 2D materials-based electrodes.
基金supported by National Natural Science Foundation of China Project (Grant No. 52374133, 52262034)the Guangdong Basic and Applied Basic Research Committee Foundation (Grant No. KCXST20221021111601003)Shenzhen Science and Technology Innovation Commission Foundation (Grant No. KCXST20221021111601003)
文摘Nanoparticles anchored on the perovskite surface have gained considerable attention for their wide-ranging applications in heterogeneous catalysis and energy conversion due to their robust and integrated structural configuration.Herein,we employ controlled Co doping to effectively enhance the nanoparticle exsolution process in layered perovskite ferrites materials.CoFe alloy nanoparticles with ultra-high-density are exsolved on the(PrBa)_(0.95)(Fe_(0.8)Co_(0.1)Nb_(0.1))2O_(5+δ)(PBFCN_(0.1))surface under reducing atmosphere,providing significant amounts of reaction sites and good durability for hydrocarbon catalysis.Under a reducing atmosphere,cobalt facilitates the reduction of iron cations within PBFCN_(0.1),leading to the formation of CoFe alloy nanoparticles.This formation is accompanied by a cation exchange process,wherein,with the increase in temperature,partial cobalt ions are substituted by iron.Meanwhile,Co doping significantly enhance the electrical conductivity due to the stronger covalency of the Cosingle bondO bond compared with Fesingle bondO bond.A single cell with the configuration of PBFCN_(0.1)-Sm_(0.2)Ce_(0.8)O_(1.9)(SDC)|SDC|Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF)-SDC achieves an extremely low polarization resistance of 0.0163Ωcm^(2)and a high peak power density of 740 mW cm^(−2)at 800℃.The cell also shows stable operation for 120 h in H_(2)with a constant current density of 285 mA cm^(−2).Furthermore,employing wet C_(2)H_(6)as fuel,the cell demonstrates remarkable performance,achieving peak power densities of 455 mW cm^(−2)at 800℃and 320 mW cm^(−2)at 750℃,marking improvements of 36%and 70%over the cell with(PrBa)_(0.95)(Fe_(0.9)Nb_(0.1))_(2)O_(5+δ)(PBFN)-SDC at these respective temperatures.This discovery emphasizes how temperature influences alloy nanoparticles exsolution within doped layered perovskite ferrites materials,paving the way for the development of high-performance ceramic fuel cell anodes.
基金financial support from the National Natural Science Foundation of China(Nos.22075284,51872287,and U2030118)the Youth Innovation Promotion Association CAS(No.2019304)+1 种基金the Fund of Mindu Innovation Laboratory(No.2021ZR201)the Scientific Instrument Developing Project of the Chinese Academy of Sciences(No.YJKYYQ20210039)
文摘Scintillation semiconductors play increasingly important medical diagnosis and industrial inspection roles.Recently,two-dimensional(2D)perovskites have been shown to be promising materials for medical X-ray imaging,but they are mostly used in low-energy(≤130 keV)regions.Direct detection of MeV X-rays,which ensure thorough penetration of the thick shell walls of containers,trucks,and aircraft,is also highly desired in practical industrial applications.Unfortunately,scintillation semiconductors for high-energy X-ray detection are currently scarce.Here,This paper reports a 2D(C_(4)H_(9)NH_(3))_(2)PbBr_(4)single crystal with outstanding sensitivity and stability toward X-ray radiation that provides an ultra-wide detectable X-ray range of between 8.20 nGy_(air)s^(-1)(50 keV)and 15.24 mGy_(air)s^(-1)(9 MeV).The(C_(4)H_(9)NH_(3))_(2)PbBr_(4)single-crystal detector with a vertical structure is used for high-performance X-ray imaging,delivering a good spatial resolution of 4.3 Ip mm^(-1)in a plane-scan imaging system.Low ionic migration in the 2D perovskite enables the vertical device to be operated with hundreds of keV to MeV X-ray radiation at high bias voltages,leading to a sensitivity of 46.90μC Gy_(air)-1 cm^(-2)(-1.16 Vμm^(-1))with 9 MeV X-ray radiation,demonstrating that 2D perovskites have enormous potential for high-energy industrial applications.
基金support of National Natural Science Foundation of China(22179027)gratefully acknowledged.This work was also supported by the Natural Science Foundation of Guangxi Province(2021GXNSFAA075063,2018GXNSFDA281005)+1 种基金the National Key Research and Development Program of China(2017YFE0105500)Science&Technology Research Project of Guangdong Province(2017A020216009).
文摘Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the use of Ca_(2)MnO_(4)-layered perovskites modified with NaNO_(3) dopants,serving as redox catalysts(also known as oxygen carriers),for the CL-ODH of ethane within a temperature range of 700-780℃.Our findings revealed that the incorporation of NaNO_(3) as a modifier significantly-nhanced the selectivity for-thylene generation from Ca_(2)MnO_(4).At 750℃and a gas hourly space velocity of 1300 h^(-1),we achieved an-thane conversion up to 68.17%,accompanied by a corresponding-thylene yield of 57.39%.X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO_(3) onto Ca_(2)MnO_(4) not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox catalyst.Furthermore,formation of NaNO_(3) shell on the surface of Ca_(2)MnO_(4) led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise manner.This modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO_(3)-doped Ca_(2)MnO_(4) catalyst.These findings provide compelling evidence for the potential of Ca_(2)MnO_(4)-layered perovskites as promising redox catalysts in the context of CL-ODH reactions.
基金Shenzhen-Hong Kong-Macao Science and Technology Innovation Project(Category C),Grant/Award Number:SGDX2020110309360100Fundo para o Desenvolvimento das Ciências e da Tecnologia,Grant/Award Numbers:FDCT-0044/2020/A1,0034/2021/APD+3 种基金Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials,Grant/Award Number:2019B121205002Natural Science Foundation of Guangdong Province,Grant/Award Number:2019A1515012186National Natural Science Foundation of China,Grant/Award Numbers:61935017,62175268,62105292UM's research fund,Grant/Award Numbers:MYRG2018-00148-IAPME,MYRG2020-00151-IAPME。
文摘Two-dimensional Ruddlesden-Popper(2DRP)perovskites have attracted intense research interest for optoelectronic applications,due to their tunable optoelectronic properties and better environmental stability than their threedimensional counterparts.Furthermore,high-performance photodetectors based on single-crystal and polycrystalline thin-films 2DRP perovskites have shown great potential for practical application.However,the complex growth process of single-crystal membranes and uncontrollable phase distribution of polycrystalline films hinder the further development of 2DRP perovskites photodetectors.Herein,we report a series of high-performance photodetectors based on single-crystal-like phase-pure 2DRP perovskite films by designing a novel spacer source.Experimental and theoretical evidence demonstrates that phase-pure films substantially suppress defect states and ion migration.These highly sensitive photodetectors show I_(light)/I_(dark) ratio exceeding 3×10^(4),responsivities exceeding 16 A/W,and detectivities exceeding 3×10^(13) Jones,which are higher at least by 1 order than those of traditional mixed-phase thinfilms 2DRP devices(close to the reported single-crystal devices).More importantly,this strategy can significantly enhance the operational stability of optoelectronic devices and pave the way to large-area flexible productions.
基金financially supported by the project of the National Natural Science Foundation of China(52202115 and 52172101)the China Postdoctoral Science Foundation(2022M722586)+2 种基金the Natural Science Foundation of Chongqing,China(CSTB2022NSCQ-MSX1085)the Shaanxi Science and Technology Innovation Team(2023-CX-TD-44)the Fundamental Research Funds for the Central Universities(3102019JC005 and G2022KY0604)。
文摘Low-temperature processed electron transport layer(ETL)of TiO_(2)that is widely used in planar perovskite solar cells(PSCs)has inherent low carrier mobility,resulting in insufficient photogenerated elec-tron transport and thus recombination loss at buried interface.Herein,we demonstrate an effective strategy of laser embedding of p-n homojunctions in the TiO_(2)ETL to accelerate electron transport in PSCs,through localized build-in electric fields that enables boosted electron mobility by two orders of magnitude.Such embedding is found significantly helpful for not only the enhanced crystallization quality of TiO_(2)ETL,but the fabrication of perovskite films with larger-grain and the less-trap-states.The embedded p-n homojunction enables also the modulation of interfacial energy level between perovskite layers and ETLs,favoring for the reduced voltage deficit of PSCs.Benefiting from these merits,the formamidinium lead iodide(FAPbI_(3))PSCs employing such ETLs deliver a champion efficiency of 25.50%,along with much-improved device stability under harsh conditions,i.e.,maintain over 95%of their initial efficiency after operation at maximum power point under continuous heat and illumination for 500 h,as well as mixed-cation PSCs with a champion efficiency of 22.02%and over 3000 h of ambient storage under humidity stability of 40%.Present study offers new possibilities of regulating charge transport layers via p-n homojunction embedding for high performance optoelectronics.
基金funded in part by the National Natural Science Foundation of China(62204210)the Natural Science Foundation of Jiangsu Province(BK20220284)+6 种基金the Natural Science Foundation of the Higher Education Institutions of Jiangsu Province(22KJB510013)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China Program(19KJB510059)the Suzhou Science and Technology Development Planning Project:Key Industrial Technology Innovation(SYG201924)University Research Development Fund(RDF-17-01-13)the Key Program Special Fund in XJTLU(KSF-T-03,KSFA-07)partially supported by the XJTLU AI University Research CentreJiangsu(Provincial)Data Science and Cognitive Computational Engineering Research Centre at XJTLU
文摘Nickel oxide(NiO_(x))has been established as a highly efficient and stable holetransporting layer(HTL)in perovskite solar cells(PSCs).However,existing deposition methods for NiO_(x)have been restricted by high-vacuum processes and fail to address the energy level mismatch at the NiO_(x)/perovskite interface,which has impeded the development of PSCs.Accordingly,we explored the application of NiO_(x)as a hybrid HTL through a sol-gel process,where a NiO_(x)film was pre-doped with Ag ions,forming a p/p^(+)homojunction in the NiO_(x)-based inverted PSCs.This innovative approach offers two synergistic advantages,including the enlargement of the built-in electric field for facilitating charge separation,optimizing energy level alignment,and charge transfer efficiency at the interface between the perovskite and HTL.Incorporating this hybrid HTL featuring the p/p^(+)homojunction in the inverted PSCs resulted in a high-power conversion efficiency(PCE)of up to 19.25%,significantly narrowing the efficiency gap compared to traditional n-i-p devices.Furthermore,this innovative strategy for the HTL enhanced the environmental stability to 30 days,maintaining 90%of the initial efficiency.
基金supported by the National Natural Science Foundation of China (51877173)the Key R&D Project of Shaanxi Province (2023-YBGY-057)+1 种基金the State Key Laboratory of Electrical Insulation and Power Equipment (EIPE22314, EIPE22306)the Natural Science Basic Research Program of Shaanxi (2023-JC-QN-0483)。
文摘Solid oxide electrolysis cell(SOEC) could be a potential technology to afford chemical storage of renewable electricity by converting water and carbon dioxide.In this work,we present the Ni-doped layered perovskite oxides,(La_(4)Sr_(n-4))_(0.9)Ti_(0.9n)Ni_(0.1n)O_(3n+2) with n=5,8,and 12(LSTNn) for application as catalysts of CO_(2) electrolysis with the exsolution of Ni nanoparticles through a simple in-situ growth method.It is found that the density,size,and distribution of exsolved Ni nanoparticles are determined by the number of n in LSTNn due to the different stack structures of TiO_6 octahedra along the c axis.The Ni doping in LSTNn significantly improved the electrochemical activity by increasing oxygen vacancies,and the Ni metallic nanoparticles afford much more active sites.The results show that LSTNn cathodes can successfully be manipulated the activity by controlling both the n number and Ni exsolution.Among these LSTNn(n=5,8,and 12),LSTN8 renders a higher activity for electrolysis of CO_(2) with a current density of 1.50A cm^(-2)@2.0 V at 800℃ It is clear from these results that the number of n in(La_(4)Sr_(n-4))_(0.9)Ti_(0.9n)Ni_(0.1n)O_(3n+2)with Ni-doping is a key factor in controlling the electrochemical performance and catalytic activity in SOEC.
基金financially supported by National Natural Science Foundation of China (Grants Nos. 52273182, 21875122)。
文摘Layered two dimensional(2D) or quasi-2D perovskites are emerging photovoltaic materials due to their superior environment and structure stability in comparison with their 3D counterparts. The typical 2D perovskites can be obtained by cutting 3D perovskites along < 100 > orientation by incorporation of bulky organic spacers, which play a key role in the performance of 2D perovskite solar cells(PSCs). Compared with aliphatic spacers, aromatic spacers with high dielectric constant have the potential to decrease the dielectric and quantum confinement effect of 2D perovskites, promote efficient charge transport and reduce the exciton binding energy, all of which are beneficial for the photovoltaic performance of 2D PSCs. In this review, we aim to provide useful guidelines for the design of aromatic spacers for 2D perovskites. We systematically reviewed the recent progress of aromatic spacers used in 2D PSCs. Finally, we propose the possible design strategies for aromatic spacers that may lead to more efficient and stable 2D PSCs.
基金funded by the National Key Research and Development Program of China (2017YFA0204800/2016YFA0202403)the Fundamental Research Funds for the Central Universities (2018CBLZ006)+5 种基金the National Natural Science Foundation of China (61604091 and 61674098)the 111 Project (B14041)the Changjiang Scholar and Innovative Research Team (IRT_14R33)the Chinese National 1000 Talents Plan program (1110010341)the China Postdoctoral Science foundation (2018M633455)the Fundamental Research Funds for the Central Universities (GK201903055)
文摘Two-dimensional(2D) layered organic-inorganic hybrid perovskites have attracted much more attention for some applications than their three-dimensional(3D) perovskite counterparts due to their promising thermal and moisture stabilities.In particular, the 2D perovskite devices have shown better promise for optoelectronic applications.However, tunability of optoelectronic properties is often demanded to improve the device performance.Herein, we adopt a newly method to tune the electronic properties of 2D perovskite by introducing pseudohalide into the structure.In this work, we designed a pseudohalidesubstituted 2D perovskite by substituting the out-of-plane halide with pseudohalide and studied the electronic and excitonic properties of 2D-BA2MX4 and 2D-BA2MX2Ps2(M=Ge^(2+), Sn^(2+), and Pb^(2+);X=I;Ps=NCO, NCS, OCN, SCN, Se CN).We revealed the dependence of electronic properties including band gaps, composition of band edges, bonding characteristics, work functions, effective masses, and exciton binding energies on different pseudohalides substituted in 2D perovskite.Our results indicate that the substitution of pseudohalide in 2D perovskites is energetically favorable and can significantly affect the bonding characteristics as well as the CBM and VBM that often play major role in determining their performance in optoelectronic devices.It is expected that the pseudohalide substitution will be helpful in developing more advanced optoelectronic device based on 2D perovskite by optimizing band alignment and promoting charge extraction.
基金supported by the European Research Council (ERC Starting Grant No. 2D-Pnicto Chem 804110)the Spanish MICINN (PID2019-111742GA-I00 and Unit of Excellence “María de Maeztu” CEX2019-000919-M)+2 种基金the Deutsche Forschungsgemeinschaft DFG (FLAG-ERA AB694/2-1)the Generalitat Valenciana (CIDEGENT/ 2018/001 and i Di FEDER/2018/061 co-financed by FEDER)CONICET for financial support and CNEA Computing Clusters for computer time (density functional theory calculations).
文摘Research on two-dimensional(2D) materials is one of the most active fields in materials science and nanotechnology. Among the members of the 2D family, layered hydroxides(LHs) represent an exceptional case of study due to their unparalleled chemical versatility which allows the modulation of their physicochemical properties at will. Nowadays, LHs based on earth-abundant metals are key materials in the areas of energy storage and conversion, hybrid materials or magnetism. α-Co hydroxides(Simonkolleite-like structures) are promising phases with tuneable electronic and magnetic properties by ligand modification. However, even in the simple case of α-Co^(Ⅱ) hydroxychlorides, the preparation of well-defined large 2D crystals is not straightforward, hindering the development of fundamental studies. Herein, we present the synthesis of 2D hexagonal crystals with outstanding sizethickness relationship(diameter > 5 μm and thickness of 20 ± 7 nm) by a simple homogeneous synthesis taking place at room temperature. In structural terms, no differences are observed between our layered materials and those obtained hydrothermally. However, dynamic susceptibility measurements alert about different arrangements of the magnetic sublattices, which have been rationalized with structural DFT calculations. This work provides an extremely easy bottom-up method to obtain high-quality 2D crystals based on α-CoIIhydroxides,paving the way for the development of fundamental studies and applications.
基金supported by the National Natural Science Foundation of China (Grant No. 62004080)the Postdoctoral Innovative Talents Supporting Program (Grant No. BX20190143)the China Postdoctoral Science Foundation (Grant No. 2020M670834)。
文摘Two-dimensional(2D) layered perovskites have emerged as potential alternates to traditional three-dimensional(3D)analogs to solve the stability issue of perovskite solar cells. In recent years, many efforts have been spent on manipulating the interlayer organic spacing cation to improve the photovoltaic properties of Dion–Jacobson(DJ) perovskites. In this work, a serious of cycloalkane(CA) molecules were selected as the organic spacing cation in 2D DJ perovskites, which can widely manipulate the optoelectronic properties of the DJ perovskites. The underlying relationship between the CA interlayer molecules and the crystal structures, thermodynamic stabilities, and electronic properties of 58 DJ perovskites has been investigated by using automatic high-throughput workflow cooperated with density-functional(DFT) calculations.We found that these CA-based DJ perovskites are all thermodynamic stable. The sizes of the cycloalkane molecules can influence the degree of inorganic framework distortion and further tune the bandgaps with a wide range of 0.9–2.1 eV.These findings indicate the cycloalkane molecules are suitable as spacing cation in 2D DJ perovskites and provide a useful guidance in designing novel 2D DJ perovskites for optoelectronic applications.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 61805263 and 62104234)。
文摘The high efficiency and low production cost enable the halide perovskite solar cells as a promising technology for the next generation photovoltaics.Nevertheless,the relatively poor stability of the organic–inorganic halide perovskites hinders their commercial applications.In the past few years,two-dimensional(2D)perovskite has emerged as a more stable alternative to the three-dimensional(3D)counterparts and attracted intense research interests.Although many attempts and advances have been made,it is still ambiguous that whether the 2D perovskites could bring closure to the stability issue.To answer this essential question,a systematic study of the nature of 2D halide perovskites is necessary.Here,we focus on the stability investigations of 2D perovskites from different perspectives,especially light,heat,ion migration and strain.Several remaining challenges and opening problems are also discussed.With further material and device engineering,we believe that the 2D perovskites would promote perovskite solar cells to a promising future.
基金funded by the National Key Research and Development Program of China(2017YFA0204800)the National Natural Science Foundation of China(91733301/61674098/51901190)+3 种基金the DNL Cooperation Fund CAS(DNL180311)the 111 Project(B14041)the Changjiang Scholars,Innovative Research Team(IRT_14R33)the China Postdoctoral Science Foundation(2020M673336)。
文摘Taking advantage of the excellent stability and photoelectric properties,two-dimensional(2D)organicinorganic halide perovskites have been widely researched and applied in optoelectronic and photovoltaic devices.The remarkable properties are attributed to the unique quantum well structures by intercalating large organic ammonium space layers.In this review,we first summarize the crystal structures and growth methods of 2D halide perovskite crystals.Then,the distinctive optical characteristics and enhanced stability under high humidity,phase stability,suppressed ion migration,and high formation energy,are discussed in detail.Furthermore,we discuss orientation control in 2D perovskite films.The applications of 2D perovskites in solar cells,photo detectors and X-ray detectors are discussed in detail.Finally,we propose an outlook and perspectives to overcome the present challenges and broaden this new class of perovskite materials with other 2D nanomaterials.
文摘The instability of thin ferroelectric films is discussed based on the close similarity of dielectric properties between bulk Bi-layered perovskites and thin BaTiO<sub>3</sub> films. The dielectric properties of pseudo-two-dimensional layered perovskites suggest that the bulk layered ferroelectric is a good model of ultra-thin ferroelectric film with a few perovskite units, free from any misfit lattice strain. It seems plausible that the ferroelectric interaction is still prominent but shows a crossover from ferroelectric to antiferroelectric along the unique c-axis (perpendicular to the film plane);with decreasing thickness, the ferroelectricity appears within the plane, which results in so-called “canted ferroelectricity”. An extra relaxation mode induced by surface effect of thin films correlates with soft mode, which results in a new intermediate phase between the paraelectric and ferroelectric phases. These evidences may indicate no critical thickness even for ferroelectric ultra- thin films.
基金supported by the National Natural Science Foundation of China(22375082,21975114,and 22105094).
文摘Two-dimensional(2D)lead halide perovskites have attracted tremendous attention due to their outstanding physical properties.However,the presence of toxic lead is a major problem for large-scale applications.Here,we report the synthesis,phase transition,dielectric and photoluminescence(PL)properties of a lead-free 2D Ge-based perovskite(BIM)_(2)GeI_(4)(BIM=benzimidazolium)which experiences a phase transition at 405 K accompanied by an order-disorder change of organic spacer.Moreover,the step-like dielectric transition near the phase transition temperature makes it suitable for dielectric switching.Meanwhile,(BIM)_(2)GeI_(4)has a direct bandgap of 2.23 eV and broadband emission from 550 to 1000 nm,implying its unique optical property for potential near-infrared lighting and displaying.This work provides a fresh example for the development of lead-free 2D Ge-based perovskite with potential applications in the fields of optoelectronics and high temperature dielectric switching.
基金Supported by the National Key Research and Development Program of China (Grant Nos.2017YFA0403600 and 2016YFA0300404)the National Natural Science Foundation of China (Grant Nos.11874363,11974356 and U1932216)the Collaborative Innovation Program of Hefei Science Center,CAS (Grant No.2019HSC-CIP002)。
文摘Atomically thin two-dimensional(2D) materials are the building bricks for next-generation electronics and optoelectronics, which demand plentiful functional properties in mechanics, transport, magnetism and photoresponse.For electronic devices, not only metals and high-performance semiconductors but also insulators and dielectric materials are highly desirable. Layered structures composed of 2D materials of different properties can be delicately designed as various useful heterojunction or homojunction devices, in which the designs on the same material(namely homojunction) are of special interest because preparation techniques can be greatly simplified and atomically seamless interfaces can be achieved. We demonstrate that the insulating pristine ZnPS_3, a ternary transition-metal phosphorus trichalcogenide, can be transformed into a highly conductive metal and an n-type semiconductor by intercalating Co and Cu atoms, respectively. The field-effect-transistor(FET) devices are prepared via an ultraviolet exposure lithography technique. The Co-ZnPS_3 device exhibits an electrical conductivity of 8 × 10^(4) S/m, which is comparable to the conductivity of graphene. The Cu-ZnPS_3 FET reveals a current ON/OFF ratio of 1-05 and a mobility of 3 × 10^(-2 )cm^(2)·V^(-1)·s^(-1). The realization of an insulator, a typical semiconductor and a metallic state in the same 2D material provides an opportunity to fabricate n-metal homojunctions and other in-plane electronic functional devices.
基金supported by the National Natural Science Foundation of China (21975028, U21A20172 and 22011540377)the Special Key Projects (2022-JCJQ-ZD-224-12)。
文摘To achieve high power conversion efficiency(PCE) and long-term stability of perovskite solar cells(PSCs), a hole transport layer(HTL) with persistently high conductivity, good moisture/oxygen barrier ability, and adequate passivation capability is important. To achieve enough conductivity and effective hole extraction, spiro-OMe TAD, one of the most frequently used HTL in optoelectronic devices, often needs chemical doping with a lithium compound(LiTFSI). However, the lithium salt dopant induces crystallization and has a negative impact on the performance and lifetime of the device due to its hygroscopic nature. Here, we provide an easy method for creating a gel by mixing a natural small molecule additive(thioctic acid, TA) with spiro-OMe TAD. We discover that gelation effectively improves the compactness of resultant HTL and prevents moisture and oxygen infiltration. Moreover, the gelation of HTL improves not only the conductivity of spiro-OMe TAD, but also the operational robustness of the devices in the atmospheric environment. In addition, TA passivates the perovskite defects and facilitates the charge transfer from the perovskite layer to HTL. As a consequence, the optimized PSCs based on the gelated HTL exhibit an improved PCE(22.52%) with excellent device stability.
文摘Three kinds of new layered perovskite compounds with Ruddlesden-Popper (R-P) phase, AgrNa2-xLa2Ti3O10 (x = 0.2, 0.3 and 0.5), were synthesized by an ion-exchange reaction of Na2La2Ti3O10 with AgNO3 solution. The structures of the compounds were characterized by EDX and XRD, and their antibacterial activity and light-resistance property were evaluated. The results indicated that the molecular formula of AgxNa2-xLa2Ti3O10 (x = 0.2, 0.3 and 0.5) was confirmed, and that the crystalline structure of Na2La2Ti3O10 was not obviously affected by exchange of silver ion. The minimum inhibitory concentrations (MICs) of Ag0.3Na1.7La2Ti3O10 against Escherichia coli (E. coli), Staphylococcus aureus (S. aureus) were 180 μg/mL and 240 μg/mL, respectively, while its discoloration was not observed after 24 h light ageing test.