As one of the important components of high-effi-ciency perovskite/silicon series devices,wide-bandgap(WBG)perovskite solar cells(PSCs)have been suffering from serious carrier transport barriers and huge open-circuit v...As one of the important components of high-effi-ciency perovskite/silicon series devices,wide-bandgap(WBG)perovskite solar cells(PSCs)have been suffering from serious carrier transport barriers and huge open-circuit voltage deficit de-rived from non-radiative recombination,especial-ly at the buried interface that are often overlooked.Herein,we combined cationic and anion passiva-tion strategies via ammonium tetra-n-butyl tetrafluoroborate(TBABF_(4))pre-treating the buried interface.Theoretical calculation predicts that the tetrabutylammonium(TBA^(+))organic cations and(tetrafluoroborate)BF_(4)^(−)anions can easily interact with charged interfacial defect.Characterizations further confirm the enhance-ment of carrier transport performance and decrease in defect density upon TBABF4 pre-treat-ment.Consequently,a power conversion efficiency of 21.35%with an ultrahigh filling factor of 84.12%is obtained for 1.68 eV-WBG inverted PSCs.In addition,the device with TBABF4 pre-treatment demonstrates excellent shelf,thermal,and operational stability.展开更多
An amorphous SiO2/4 H–Si C（0001） interface model with carbon dimer defects is established based on density functional theory of the first-principle plane wave pseudopotential method.The structures of carbon dimer d...An amorphous SiO2/4 H–Si C（0001） interface model with carbon dimer defects is established based on density functional theory of the first-principle plane wave pseudopotential method.The structures of carbon dimer defects after passivation by H2 and NO molecules are established,and the interface states before and after passivation are calculated by the Heyd–Scuseria–Ernzerhof（HSE06） hybrid functional scheme.Calculation results indicate that H2 can be adsorbed on the O2–C = C–O2 defect and the carbon–carbon double bond is converted into a single bond.However,H2 cannot be adsorbed on the O2–（C = C）′ –O2 defect.The NO molecules can be bonded by N and C atoms to transform the carbon–carbon double bonds,thereby passivating the two defects.This study shows that the mechanism for the passivation of Si O2/4 H–SiC（0001） interface carbon dimer defects is to convert the carbon–carbon double bonds into carbon dimers.Moreover,some intermediate structures that can be introduced into the interface state in the band gap should be avoided.展开更多
Electrochemical nitrogen reduction reaction(e-NRR)under ambient conditions is an emerging strategy to tackle the hydrogen-and energy-intensive operations for traditional Haber-Bosch process in industrial ammonia(NH_(3...Electrochemical nitrogen reduction reaction(e-NRR)under ambient conditions is an emerging strategy to tackle the hydrogen-and energy-intensive operations for traditional Haber-Bosch process in industrial ammonia(NH_(3))synthesis.However,the e-NRR performance is currently impeded by the inherent inertness of N_(2) molecules,the extremely slow kinetics and the overwhelming competition from the hydrogen evolution reaction(HER),all of which cause unsatisfied yield and ammonia selectivity(Faradaic efficiency,FE).Defect and interface engineering are capable of achieving novel physical and chemical properties as well as superior synergistic effects for various electrocatalysts.In this review,we first provide a general introduction to the NRR mechanism.We then focus on the recent progress in defect and interface engineering and summarize how defect and interface can be rationally designed and functioned in NRR catalysts.Particularly,the origin of superior NRR catalytic activity by applying these approaches was discussed from both theoretical and experimental perspectives.Finally,the remaining challenges and future perspectives in this emerging area are highlighted.It is expected that this review will shed some light on designing NRR electrocatalysts with excellent activity,selectivity and stability.展开更多
Bulk and interface carrier nonradiative recombination losses impede the further improvement of power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs).It is highly necessary to develop multifunct...Bulk and interface carrier nonradiative recombination losses impede the further improvement of power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs).It is highly necessary to develop multifunctional strategy to minimize surface and interface nonradiative recombination losses.Herein,we report a bulk and interface defect passivation strategy via the synergistic effect of anions and cations,where multifunctional potassium sulphate(K_(2)SO_(4))is incorporated at SnO_(2)/perovskite interface.We find that K^(+)ions in K_(2)SO_(4)diffuse into perovskite layer and suppress the formation of bulk defects in perovskite films,and the SO_(4)^(2-)ions remain located at interface via the strong chemical interaction with SnO_(2)layer and perovskite layer,respectively.Through this synergistic modification strategy,effective defect passivation and improved energy band alignment are achieved simultaneously.These beneficial effects are translated into an efficiency increase from 19.45%to 21.18%with a low voltage deficit of0.53 V mainly as a result of boosted open-circuit voltage(V_(oc))after K_(2)SO_(4)modification.In addition,the K_(2)SO_(4)modification contributes to ameliorated stability.The present work provides a route to minimize bulk and interface nonradiative recombination losses for the simultaneous realization of PCE and stability enhancement by rational anion and cation synergistic engineering.展开更多
The buried interface in the perovskite solar cell(PSC)has been regarded as a breakthrough to boost the power conversion efficiency and stability.However,a comprehensive manipulation of the buried interface in terms of...The buried interface in the perovskite solar cell(PSC)has been regarded as a breakthrough to boost the power conversion efficiency and stability.However,a comprehensive manipulation of the buried interface in terms of the transport layer,buried interlayer,and perovskite layer has been largely overlooked.Herein,we propose the use of a volatile heterocyclic compound called 2-thiopheneacetic acid(TPA)as a pre-buried additive in the buried interface to achieve cross-layer all-interface defect passivation through an in situ bottom-up infiltration diffusion strategy.TPA not only suppresses the serious interfacial nonradiative recombination losses by precisely healing the interfacial and underlying defects but also effectively enhances the quality of perovskite film and releases the residual strain of perovskite film.Owing to this versatility,TPA-tailored CsPbBr3 PSCs deliver a record efficiency of 11.23% with enhanced long-term stability.This breakthrough in manipulating the buried interface using TPA opens new avenues for further improving the performance and reliability of PSC.展开更多
Niobium pentoxide(Nb2O5)has attracted much attention in lithium batteries due to its advantages of high operating voltage,large theoretical capacity,environmental friendliness and cost-effectiveness.However,the intrin...Niobium pentoxide(Nb2O5)has attracted much attention in lithium batteries due to its advantages of high operating voltage,large theoretical capacity,environmental friendliness and cost-effectiveness.However,the intrinsic poor electrical conductivity,sluggish kinetics,and large volume changes hinder its electrochemical performance at high power density,making it away from the requirements for practical applications.In this research work,we regulate the electron transport of niobium-nickel oxide(NiNbO)anode material with enhanced structural stability at high power density by constructing the two-phase boundaries between niobium pentoxide(Nb2O5)and nickel niobate(NiNb2O6)through simple solid phase reaction.In addition,the presence of lattice defects in NiNbO-F further speeds up the transport of Li+and promotes the electrochemical reaction kinetics more effectively.The two-phase boundaries and defect modulated anode material displays high Li+diffusion coefficient of 1.63×10^(−10) cm^(2) s^(−1),pretty high initial discharge capacity of 222.8 mAh g^(−1) at 1 C,extraordinary high rate performance(66.7 mAh g^(−1))at an ultrahigh rate(100 C)and ultra-long cycling stability under high rate of 25 C(83.4 mAh g^(−1) after 2000 cycles)with only 0.016%attenuation per cycle.These results demonstrate an effective approach for developing electrode materials that greatly improve rate performance and durability.展开更多
Previous results revealed that the defect and/or interface had a great impact on the electromagnetic pa-rameters of materials.In order to understand the main physical mechanisms and effectively utilize these strategie...Previous results revealed that the defect and/or interface had a great impact on the electromagnetic pa-rameters of materials.In order to understand the main physical mechanisms and effectively utilize these strategies,in this study,M Fe_(2)O_(4)and flower-like core@shell M Fe_(2)O_(4)@MoS_(2)(M=Mn,Ni,and Zn)sam-ples with different categories were elaborately designed and selectively produced in large scale through a simple two-step hydrothermal reaction.We conducted the systematical investigation on their microstruc-tures,electromagnetic parameters and microwave absorption performances(MAPs).The obtained results revealed that the large radius of M^(2+)cation could effectively boost the concentration of oxygen vacancy in the M Fe_(2)O_(4)and M Fe_(2)O_(4)@MoS_(2)samples,which resulted in the improvement of dielectric loss capabil-ities and MAPs.Furthermore,the introduction of MoS_(2)nanosheets greatly improved the interfacial effect and enhanced the polarization loss capabilities,which also boosted the MAPs.By taking full advantage of the defect and interface,the designed M Fe_(2)O_(4)@MoS_(2)samples displayed tunable and excellent com-prehensive MAPs including strong absorption capability,wide absorption bandwidth and thin matching thicknesses.Therefore,the clear understanding of defect and interface engineering made these strategies well elaborately designed and applicable to improving MAPs.展开更多
Focusing on the low open circuit voltage(V_(OC))and fill factor(FF)in flexible Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells,indium(In)ions are introduced into the CZTSSe absorbers near Mo foils to modify the back interface...Focusing on the low open circuit voltage(V_(OC))and fill factor(FF)in flexible Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells,indium(In)ions are introduced into the CZTSSe absorbers near Mo foils to modify the back interface and passivate deep level defects in CZTSSe bulk concurrently for improving the performance of flexible device.The results show that In doping effectively inhibits the formation of secondary phase(Cu(S,Se)_(2))and VSndefects.Further studies demonstrate that the barrier height at the back interface is decreased and the deep level defects(Cu_(Sn)defects)in CZTSSe bulk are passivated.Moreover,the carrier concentration is increased and the V_(OC) deficit(V_(OC,def))is decreased significantly due to In doping.Finally,the flexible CZTSSe solar cell with 10.01%power conversion efficiency(PCE)has been obtained.The synergistic strategy of interface modification and bulk defects passivation through In incorporation provides a new thought for the fabrication of efficient flexible kesterite-based solar cells.展开更多
Organic molecule passivation of perovskite surfaces has emerged as a promising strategy for efficient and durable perovskite solar cells(PSCs).While many materials have been reported,the optimization of molecular stru...Organic molecule passivation of perovskite surfaces has emerged as a promising strategy for efficient and durable perovskite solar cells(PSCs).While many materials have been reported,the optimization of molecular structure for the best passivation effect remains of significant interest but lacks sufficient study.In this work,we designed and synthesized three novel donor–acceptor-donor(D-A-D)type conjugated organic small molecules with varying alkyl chain lengths to regulate the interface between perovskite and Spiro-OMeTAD.Among them,the OSIT molecule,which features an n-octyl side chain of optimal length,demonstrated a balanced interfacial contact and interaction with the perovskite surface.Beyond the passivation effect of the electron-rich C=O group on undercoordinated Pb2+defects,OSIT optimizes energy level alignment and improves charge extraction by acting as an efficient hole transport channel.As a result,PSCs with OSIT interfacial layer achieved an exceptional efficiency of 25.48%and a high open-circuit voltage of 1.18 V.Furthermore,the durability of unencapsulated devices was significantly enhanced under various environmental conditions,maintaining 93.7%of their initial efficiency after 1000 h of maximum power point tracking in a nitrogen atmosphere.This study provides valuable insights into the rational design of D-A-D type materials for effective interface modification in PSCs.展开更多
Numerous defects at the buried interface of perovskite film and the exacerbated oxidation and degradation of tin-lead(Sn-Pb)perovskites induced by poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS),du...Numerous defects at the buried interface of perovskite film and the exacerbated oxidation and degradation of tin-lead(Sn-Pb)perovskites induced by poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS),due to its hygroscopic and acidic nature,limit performance improvement of SnPb perovskite solar cells(PSCs).To address these issues,1-Ethyl-3-Guanidinothiourea-Hydrochloride(EGH)was employed as a multifunctional modifier at the PEDOT:PSS/perovskite interface to regulate the buried interface behaviors of Sn-Pb PSCs.EGH can not only passivate the defects of the perovskite buried interface and regulate the work function of PEDOT:PSS for a more matched interface energy level,but also prevent the perovskite film from erosion damage by the acidic PEDOT:PSS for a more stable PEDOT:PSS/perovskite interface.Moreover,the interfacial charge transport dynamics were significantly improved by obviously suppressing interfacial non-radiative recombination losses.As a consequence,EGH-tailored 1.25 eV Sn-Pb PSCs yielded a champion PCE of 23.20%,featuring enhanced long-term stability.展开更多
Observation under high resolution electron microscope shows that the continuous bombing of high speed ions produces a great amount of vacant site defects.The assembly of vacancies forms vacant dish,and the collapase o...Observation under high resolution electron microscope shows that the continuous bombing of high speed ions produces a great amount of vacant site defects.The assembly of vacancies forms vacant dish,and the collapase of vacant dish forms stacking fault tetrahedrons and oth- er crystal defects.The interfaces between phase ε(Fe_(2-3)N)and phase γ'(Fe_4N)are smooth, straight and coherent,and they have the orientation relationships of(11)//(0001)and [110]/[110] .展开更多
Antimony trisulfide(Sb_(2)S_(3)) solar cells suffer from large open circuit voltage deficits due to their intrinsic defects which limit the power conversion efficiency.Thus,it is important to elucidate these defects’...Antimony trisulfide(Sb_(2)S_(3)) solar cells suffer from large open circuit voltage deficits due to their intrinsic defects which limit the power conversion efficiency.Thus,it is important to elucidate these defects’ origin and defects at the interface.Here,we discover that sulfide radical defects have a significant impact on the performance of Sb_(2)S_(3)solar cells.Moreover,it has been illustrated that these defects at the CdS/Sb_(2)S_(3)interface can be reduced by optimizing the deposition process.A trap distribution model is used to quantify the defect density at the CdS/Sb_(2)S_(3)interface.It shows that the interface defects can be reduced by24% by improving the deposition process.This work reveals the importance of interface defects and guides the future optimization of Sb_(2)S_(3)solar cells.展开更多
Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells suffer from severe carrier recombination,limiting the photovoltaic performance.Unfavorable energy band alignment at the p-n junction and defective front interface are ...Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells suffer from severe carrier recombination,limiting the photovoltaic performance.Unfavorable energy band alignment at the p-n junction and defective front interface are two main causes.Herein,oxygen incorporation in CZTSSe via absorber air-annealing was developed as a strategy to optimize its surface photoelectric property and reduce the defects.With optimized oxygen incorporation conditions,the carrier separation and collection behavior at the front interface of the device is improved.In particular,it is found that oxygen incorporated absorber exhibits increased band bending,larger depletion region width,and suppressed absorber defects.These indicate the dynamic factors for carrier separation become stronger.Meanwhile,the increased potential difference between grain boundaries and intra grains combined with the decreased concentration of interface deep level defect in the absorber provide a better path for carrier transport.As a consequence,the champion efficiency of CZTSSe solar cells has been improved from 9.74%to 12.04%with significantly improved open-circuit voltage after optimized air-annealing condition.This work provides a new insight for interface engineering to improve the photoelectric conversion efficiency of CZTSSe devices.展开更多
The buried interface defects severely affect the further enhancements of efficiency and stability of SnO_(2)-based planar perovskite solar cells(PSCs).To well tackle this problem,we propose a passivation strategy empl...The buried interface defects severely affect the further enhancements of efficiency and stability of SnO_(2)-based planar perovskite solar cells(PSCs).To well tackle this problem,we propose a passivation strategy employing NH_(4)PF_6 to modify the buried interface of perovskite layer((FAPbI_(3))_(0.85)(MAPbBr_(3))_(0.15) composition) in planar PSCs.After introducing NH_(4)PF_(6),the oxygen defects on the surface of SnO_(2) film are greatly restricted due to the coordinate interaction between fluorine atoms(F) in PF_(6)^(-)and undercoordinated Sn^(4+).Meanwhile,the hydrogen bonding interaction(N-H…I) between NH_(4)PF_(6) and PbI_(2) can passivate the non-radiative charge recombination sites,significantly optimizing the quality of perovskite film,as well as the charge transfer process at the SnO_(2)/perovskite interface.As a result,the NH_(4)PF_(6)-modified PSC obtains a champion power conversion efficiency(PCE) of 21.11%superior to the reference device(18.46%),and the device with an active area of 1 cm^(2) achieves a PCE as high as17.38%.Furthermore,the unencapsulated NH_(4)PF_(6)-modified PSCs show good humidity stability and retain about80% of the initial PCE after 1080 h aging at the relative humidity(RH) of 35% ± 5%.展开更多
Defects have a significant impact on the performance of semiconductor devices.Using the first-principles combined with one-dimensional static coupling theory approach,we have calculated the variation of carrier captur...Defects have a significant impact on the performance of semiconductor devices.Using the first-principles combined with one-dimensional static coupling theory approach,we have calculated the variation of carrier capture coefficients with temperature for the interfacial defects P_(b0) and P_(b1) in amorphous-SiO_(2)/Si(100)interface.It is found that the geometrical shapes of P_(b0) and P_(b1) defects undergo large deformations after capturing carriers to form charged defects,especially for the Si atoms containing a dangling bond.The hole capture coefficients of neutral P_(b0) and P_(b1) defects are largest than the other capture coefficients,indicating that these defects have a higher probability of forming positively charged centres.Meanwhile,the calculated results of non-radiative recombination coefficient of these defects show that both P_(b0) and P_(b1) defects are the dominant non-radiative recombination centers in the interface of a-SiO_(2)/Si(100).展开更多
Based on the first-principles method, the structural stability and the contribution of point defects such as O, Sr or Ti vacancies on two-dimensional electron gas of n- and p-type LaAlO3/SrTiO3 interfaces are investig...Based on the first-principles method, the structural stability and the contribution of point defects such as O, Sr or Ti vacancies on two-dimensional electron gas of n- and p-type LaAlO3/SrTiO3 interfaces are investigated. The results show that O vacancies at p-type interfaces have much lower formation energies, and Sr or Ti vacancies at n-type interfaces are more stable than the ones at p-type interfaces under O-rich conditions. The calculated densities of states indicate that O vacancies act as donors and give a significant compensation to hole carriers, resulting in insulating behavior at p-type interfaces. In contrast, Sr or Ti vacancies tend to trap electrons and behave as acceptors. Sr vacancies are the most stable defects at high oxygen partial pressures, and the Sr vacancies rather than Ti vacancies are responsible for the insulator-metal transition of n-type interface. The calculated results can be helpful to understand the tuned electronic properties of LaAlO3 /SrTiO3 heterointerfaces.展开更多
Although ionic liquids(ILs)have been widely employed to heal the defects in perovskite solar cells(PSCs),the corresponding defect passivation mechanisms are not thoroughly understood up to now.Herein,we first reveal a...Although ionic liquids(ILs)have been widely employed to heal the defects in perovskite solar cells(PSCs),the corresponding defect passivation mechanisms are not thoroughly understood up to now.Herein,we first reveal an abnormal buried interface anion defect passivation mechanism depending on cationinduced steric hindrance.The IL molecules containing the same anion([BF4]^(-))and different sizes of imidazolium cations induced by substituent size are used to manipulate buried interface.It was revealed what passivated interfacial defects is mainly anions instead of cations.Theoretical and experimental results demonstrate that the large-sized cations can weaken the ionic bond strength between anions and cations,and facilitate the interaction between anions and SnO2as well as perovskites,which is conducive to interfacial defect passivation and ameliorating interfacial contact.It can be concluded that interfacial chemical interaction strength and defect passivation effect are positively correlated with the size of cations.The discovery breaks conventional thinking that large-sized modification molecules would weaken their chemical interaction with perovskite.Compared with the control device(21.54%),the device based on 1,3-Bis(1-adamantyl)-imidazolium tetrafluoroborate(BAIMBF4)with maximum size cations achieves a significantly enhanced efficiency of 23.61%along with much increased moisture,thermal and light stabilities.展开更多
It is well known that in the process of thermal oxidation of silicon,there are P_(b)-type defects at amorphous silicon dioxide/silicon(a-SiO_(2)/Si)interface due to strain.These defects have a very important impact on...It is well known that in the process of thermal oxidation of silicon,there are P_(b)-type defects at amorphous silicon dioxide/silicon(a-SiO_(2)/Si)interface due to strain.These defects have a very important impact on the performance and reliability of semiconductor devices.In the process of passivation,hydrogen is usually used to inactivate P_(b)-type defects by the reaction P_(b)+H_(2)→P_(b)H+H.At the same time,P_(b)H centers dissociate according to the chemical reaction P_(b)H→P_(b)+H.Therefore,it is of great significance to study the balance of the passivation and dissociation.In this work,the reaction mechanisms of passivation and dissociation of the P_(b)-type defects are investigated by first-principles calculations.The reaction rates of the passivation and dissociation are calculated by the climbing image-nudged elastic band(CI-NEB)method and harmonic transition state theory(HTST).By coupling the rate equations of the passivation and dissociation reactions,the equilibrium density ratio of the saturated interfacial dangling bonds and interfacial defects(P_(b),P_(b)0,and P_(b)1)at different temperatures is calculated.展开更多
Sb_(2)Se_(3) with unique one-dimensional(1D) crystal structure exhibits exceptional deformation tolerance,demonstrating great application potential in flexible devices.However,the power conversion efficiency(PCE) of f...Sb_(2)Se_(3) with unique one-dimensional(1D) crystal structure exhibits exceptional deformation tolerance,demonstrating great application potential in flexible devices.However,the power conversion efficiency(PCE) of flexible Sb_(2)Se_(3) photovoltaic devices is temporarily limited by the complicated intrinsic defects and the undesirable contact interfaces.Herein,a high-quality Sb_(2)Se_(3) absorber layer with large crystal grains and benign [hkl] growth orientation can be first prepared on a Mo foil substrate.Then NaF intermediate layer is introduced between Mo and Sb_(2)Se_(3),which can further optimize the growth of Sb_(2)Se_(3)thin film.Moreover,positive Na ion diffusion enables it to dramatically lower barrier height at the back contact interface and passivate harmful defects at both bulk and heterojunction.As a result,the champion substrate structured Mo-foil/Mo/NaF/Sb_(2)Se_(3)/CdS/ITO/Ag flexible thin-film solar cell delivers an obviously higher efficiency of 8.03% and a record open-circuit voltage(V_(OC)) of 0.492 V.This flexible Sb_(2)Se_(3) device also exhibits excellent stability and flexibility to stand large bending radius and multiple bending times,as well as superior weak light photo-response with derived efficiency of 12.60%.This work presents an effective strategy to enhance the flexible Sb_(2)Se_(3) device performance and expand its potential photovoltaic applications.展开更多
This scientific paper presents a study investigating the effects of defects at the CdS/CIGS and CdS/SDL interfaces on the performance of CIGS solar cells. The objective of this study is to analyze the influence of def...This scientific paper presents a study investigating the effects of defects at the CdS/CIGS and CdS/SDL interfaces on the performance of CIGS solar cells. The objective of this study is to analyze the influence of defects at the interface between the CdS buffer layer and the CIGS absorber, as well as the surface defect layer (SDL), on CIGS solar cell performance. The study explores three key aspects: the impact of the conduction band offset (CBO) at the CdS/CIGS interface, the effects of interface defects and defect density on performance, and the combined influence of CBO and defect density at the CdS/ SDL and SDL/CIGS interfaces. For interface defects not exceeding 10<sup>13</sup> cm<sup>-2</sup>, we obtained a good efficiency of 22.9% when -0.1 eV analyzing the quality of CdS/SDL and SDL/CIGS junctions, it appears that defects at the SDL/CIGS interface have very little impact on the performances of the CIGS solar cell. By optimizing the electrical parameters of the CdS/SDL interface defects, we achieved a conversion efficiency of 23.1% when -0.05 eV < CBO < 0.05 eV.展开更多
文摘As one of the important components of high-effi-ciency perovskite/silicon series devices,wide-bandgap(WBG)perovskite solar cells(PSCs)have been suffering from serious carrier transport barriers and huge open-circuit voltage deficit de-rived from non-radiative recombination,especial-ly at the buried interface that are often overlooked.Herein,we combined cationic and anion passiva-tion strategies via ammonium tetra-n-butyl tetrafluoroborate(TBABF_(4))pre-treating the buried interface.Theoretical calculation predicts that the tetrabutylammonium(TBA^(+))organic cations and(tetrafluoroborate)BF_(4)^(−)anions can easily interact with charged interfacial defect.Characterizations further confirm the enhance-ment of carrier transport performance and decrease in defect density upon TBABF4 pre-treat-ment.Consequently,a power conversion efficiency of 21.35%with an ultrahigh filling factor of 84.12%is obtained for 1.68 eV-WBG inverted PSCs.In addition,the device with TBABF4 pre-treatment demonstrates excellent shelf,thermal,and operational stability.
基金Project supported by the National Natural Science Foundation of China(Grant No.61474013)
文摘An amorphous SiO2/4 H–Si C（0001） interface model with carbon dimer defects is established based on density functional theory of the first-principle plane wave pseudopotential method.The structures of carbon dimer defects after passivation by H2 and NO molecules are established,and the interface states before and after passivation are calculated by the Heyd–Scuseria–Ernzerhof（HSE06） hybrid functional scheme.Calculation results indicate that H2 can be adsorbed on the O2–C = C–O2 defect and the carbon–carbon double bond is converted into a single bond.However,H2 cannot be adsorbed on the O2–（C = C）′ –O2 defect.The NO molecules can be bonded by N and C atoms to transform the carbon–carbon double bonds,thereby passivating the two defects.This study shows that the mechanism for the passivation of Si O2/4 H–SiC（0001） interface carbon dimer defects is to convert the carbon–carbon double bonds into carbon dimers.Moreover,some intermediate structures that can be introduced into the interface state in the band gap should be avoided.
基金supported by the National Natural Science Foundation of China(grant no.21904071 and 22071115)。
文摘Electrochemical nitrogen reduction reaction(e-NRR)under ambient conditions is an emerging strategy to tackle the hydrogen-and energy-intensive operations for traditional Haber-Bosch process in industrial ammonia(NH_(3))synthesis.However,the e-NRR performance is currently impeded by the inherent inertness of N_(2) molecules,the extremely slow kinetics and the overwhelming competition from the hydrogen evolution reaction(HER),all of which cause unsatisfied yield and ammonia selectivity(Faradaic efficiency,FE).Defect and interface engineering are capable of achieving novel physical and chemical properties as well as superior synergistic effects for various electrocatalysts.In this review,we first provide a general introduction to the NRR mechanism.We then focus on the recent progress in defect and interface engineering and summarize how defect and interface can be rationally designed and functioned in NRR catalysts.Particularly,the origin of superior NRR catalytic activity by applying these approaches was discussed from both theoretical and experimental perspectives.Finally,the remaining challenges and future perspectives in this emerging area are highlighted.It is expected that this review will shed some light on designing NRR electrocatalysts with excellent activity,selectivity and stability.
基金financially supported by the Defense Industrial Technology Development Program(JCKY2017110C0654)the National Natural Science Foundation of China(11974063,61904023)the Chongqing Special Postdoctoral Science Foundation(cstc2019jcyj-bsh0026)。
文摘Bulk and interface carrier nonradiative recombination losses impede the further improvement of power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs).It is highly necessary to develop multifunctional strategy to minimize surface and interface nonradiative recombination losses.Herein,we report a bulk and interface defect passivation strategy via the synergistic effect of anions and cations,where multifunctional potassium sulphate(K_(2)SO_(4))is incorporated at SnO_(2)/perovskite interface.We find that K^(+)ions in K_(2)SO_(4)diffuse into perovskite layer and suppress the formation of bulk defects in perovskite films,and the SO_(4)^(2-)ions remain located at interface via the strong chemical interaction with SnO_(2)layer and perovskite layer,respectively.Through this synergistic modification strategy,effective defect passivation and improved energy band alignment are achieved simultaneously.These beneficial effects are translated into an efficiency increase from 19.45%to 21.18%with a low voltage deficit of0.53 V mainly as a result of boosted open-circuit voltage(V_(oc))after K_(2)SO_(4)modification.In addition,the K_(2)SO_(4)modification contributes to ameliorated stability.The present work provides a route to minimize bulk and interface nonradiative recombination losses for the simultaneous realization of PCE and stability enhancement by rational anion and cation synergistic engineering.
基金This work was supported by the National Natural Science Foundation of China(62104136,22179051)the National Key Research and Development Program of China(2021YFE0111000)+3 种基金Project of Shandong Province Higher Educational Young Innovative Team(2022KJ218)China Postdoctoral Science Foundation(2023M732104)Qingdao Postdoctoral Funding Program(QDBSH20220201002)Postdoctoral Innovation Project of Shandong Province(SDCX-ZG-202303032).
文摘The buried interface in the perovskite solar cell(PSC)has been regarded as a breakthrough to boost the power conversion efficiency and stability.However,a comprehensive manipulation of the buried interface in terms of the transport layer,buried interlayer,and perovskite layer has been largely overlooked.Herein,we propose the use of a volatile heterocyclic compound called 2-thiopheneacetic acid(TPA)as a pre-buried additive in the buried interface to achieve cross-layer all-interface defect passivation through an in situ bottom-up infiltration diffusion strategy.TPA not only suppresses the serious interfacial nonradiative recombination losses by precisely healing the interfacial and underlying defects but also effectively enhances the quality of perovskite film and releases the residual strain of perovskite film.Owing to this versatility,TPA-tailored CsPbBr3 PSCs deliver a record efficiency of 11.23% with enhanced long-term stability.This breakthrough in manipulating the buried interface using TPA opens new avenues for further improving the performance and reliability of PSC.
基金supported by the National Natural Science Foundation of China(Nos.52002119 and 52102346)the National Key R&D Program of China(No.2021YFB3400800)the Startup Funds from the Henan University of Science and Technology(Nos.13480095,13480096,13554031 and 13554032).
文摘Niobium pentoxide(Nb2O5)has attracted much attention in lithium batteries due to its advantages of high operating voltage,large theoretical capacity,environmental friendliness and cost-effectiveness.However,the intrinsic poor electrical conductivity,sluggish kinetics,and large volume changes hinder its electrochemical performance at high power density,making it away from the requirements for practical applications.In this research work,we regulate the electron transport of niobium-nickel oxide(NiNbO)anode material with enhanced structural stability at high power density by constructing the two-phase boundaries between niobium pentoxide(Nb2O5)and nickel niobate(NiNb2O6)through simple solid phase reaction.In addition,the presence of lattice defects in NiNbO-F further speeds up the transport of Li+and promotes the electrochemical reaction kinetics more effectively.The two-phase boundaries and defect modulated anode material displays high Li+diffusion coefficient of 1.63×10^(−10) cm^(2) s^(−1),pretty high initial discharge capacity of 222.8 mAh g^(−1) at 1 C,extraordinary high rate performance(66.7 mAh g^(−1))at an ultrahigh rate(100 C)and ultra-long cycling stability under high rate of 25 C(83.4 mAh g^(−1) after 2000 cycles)with only 0.016%attenuation per cycle.These results demonstrate an effective approach for developing electrode materials that greatly improve rate performance and durability.
基金This work was supported by the Fund of Fok Ying Tung Edu-cation Foundation,the Major Research Project of Innovative Group of Guizhou province(No.2018-013)Open Fund from Henan Uni-versity of Science and Technology,the National Science Foundation of China(Nos.11964006 and 11774156)the Foundation of the National Key Project for Basic Research(No.2012CB932304)for fi-nancial support。
文摘Previous results revealed that the defect and/or interface had a great impact on the electromagnetic pa-rameters of materials.In order to understand the main physical mechanisms and effectively utilize these strategies,in this study,M Fe_(2)O_(4)and flower-like core@shell M Fe_(2)O_(4)@MoS_(2)(M=Mn,Ni,and Zn)sam-ples with different categories were elaborately designed and selectively produced in large scale through a simple two-step hydrothermal reaction.We conducted the systematical investigation on their microstruc-tures,electromagnetic parameters and microwave absorption performances(MAPs).The obtained results revealed that the large radius of M^(2+)cation could effectively boost the concentration of oxygen vacancy in the M Fe_(2)O_(4)and M Fe_(2)O_(4)@MoS_(2)samples,which resulted in the improvement of dielectric loss capabil-ities and MAPs.Furthermore,the introduction of MoS_(2)nanosheets greatly improved the interfacial effect and enhanced the polarization loss capabilities,which also boosted the MAPs.By taking full advantage of the defect and interface,the designed M Fe_(2)O_(4)@MoS_(2)samples displayed tunable and excellent com-prehensive MAPs including strong absorption capability,wide absorption bandwidth and thin matching thicknesses.Therefore,the clear understanding of defect and interface engineering made these strategies well elaborately designed and applicable to improving MAPs.
基金supported by the National Natural Science Foundation of China(62074037)the Science and Technology Department of Fujian Province(2020I0006)the Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZZ124)。
文摘Focusing on the low open circuit voltage(V_(OC))and fill factor(FF)in flexible Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells,indium(In)ions are introduced into the CZTSSe absorbers near Mo foils to modify the back interface and passivate deep level defects in CZTSSe bulk concurrently for improving the performance of flexible device.The results show that In doping effectively inhibits the formation of secondary phase(Cu(S,Se)_(2))and VSndefects.Further studies demonstrate that the barrier height at the back interface is decreased and the deep level defects(Cu_(Sn)defects)in CZTSSe bulk are passivated.Moreover,the carrier concentration is increased and the V_(OC) deficit(V_(OC,def))is decreased significantly due to In doping.Finally,the flexible CZTSSe solar cell with 10.01%power conversion efficiency(PCE)has been obtained.The synergistic strategy of interface modification and bulk defects passivation through In incorporation provides a new thought for the fabrication of efficient flexible kesterite-based solar cells.
基金supported by the National Natural Science Foundation of China(22179053,22279046)Natural Science Excellent Youth Foundation of Jiangsu Provincial(BK20220112)+1 种基金Special Foundation for Carbon Peak Carbon Neutralization Technology Innovation Program of Jiangsu Province(BE2022026-2)JSPS KAKENHI(20K15385,20H02817,and 24H00486)。
文摘Organic molecule passivation of perovskite surfaces has emerged as a promising strategy for efficient and durable perovskite solar cells(PSCs).While many materials have been reported,the optimization of molecular structure for the best passivation effect remains of significant interest but lacks sufficient study.In this work,we designed and synthesized three novel donor–acceptor-donor(D-A-D)type conjugated organic small molecules with varying alkyl chain lengths to regulate the interface between perovskite and Spiro-OMeTAD.Among them,the OSIT molecule,which features an n-octyl side chain of optimal length,demonstrated a balanced interfacial contact and interaction with the perovskite surface.Beyond the passivation effect of the electron-rich C=O group on undercoordinated Pb2+defects,OSIT optimizes energy level alignment and improves charge extraction by acting as an efficient hole transport channel.As a result,PSCs with OSIT interfacial layer achieved an exceptional efficiency of 25.48%and a high open-circuit voltage of 1.18 V.Furthermore,the durability of unencapsulated devices was significantly enhanced under various environmental conditions,maintaining 93.7%of their initial efficiency after 1000 h of maximum power point tracking in a nitrogen atmosphere.This study provides valuable insights into the rational design of D-A-D type materials for effective interface modification in PSCs.
基金financially supported by the National Key R&D Program of China(2022YFB4200303 to D.Zhao)the National Natural Science Foundation of China(62174112,52461160298 to D.Zhao and E30853YM19 to C.Xiao)+2 种基金the Natural Science Foundation of Sichuan Province(2024NSFSC1011 to C.Chen)the Fundamental Research Funds for the Central Universities(YJ2021157 to C.Chen)the Engineering Featured Team Fund of Sichuan University(2020SCUNG102 to D.Zhao)。
文摘Numerous defects at the buried interface of perovskite film and the exacerbated oxidation and degradation of tin-lead(Sn-Pb)perovskites induced by poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS),due to its hygroscopic and acidic nature,limit performance improvement of SnPb perovskite solar cells(PSCs).To address these issues,1-Ethyl-3-Guanidinothiourea-Hydrochloride(EGH)was employed as a multifunctional modifier at the PEDOT:PSS/perovskite interface to regulate the buried interface behaviors of Sn-Pb PSCs.EGH can not only passivate the defects of the perovskite buried interface and regulate the work function of PEDOT:PSS for a more matched interface energy level,but also prevent the perovskite film from erosion damage by the acidic PEDOT:PSS for a more stable PEDOT:PSS/perovskite interface.Moreover,the interfacial charge transport dynamics were significantly improved by obviously suppressing interfacial non-radiative recombination losses.As a consequence,EGH-tailored 1.25 eV Sn-Pb PSCs yielded a champion PCE of 23.20%,featuring enhanced long-term stability.
文摘Observation under high resolution electron microscope shows that the continuous bombing of high speed ions produces a great amount of vacant site defects.The assembly of vacancies forms vacant dish,and the collapase of vacant dish forms stacking fault tetrahedrons and oth- er crystal defects.The interfaces between phase ε(Fe_(2-3)N)and phase γ'(Fe_4N)are smooth, straight and coherent,and they have the orientation relationships of(11)//(0001)and [110]/[110] .
基金support from the National Key R&D Program of China(2019YFE0120300)the National Natural Science Foundation of China(NSFC,11904266,62204174 and 91850207)the Fundamental Research Funds for the Central Universities(2042021kf0202 and 2042021kf0069)。
文摘Antimony trisulfide(Sb_(2)S_(3)) solar cells suffer from large open circuit voltage deficits due to their intrinsic defects which limit the power conversion efficiency.Thus,it is important to elucidate these defects’ origin and defects at the interface.Here,we discover that sulfide radical defects have a significant impact on the performance of Sb_(2)S_(3)solar cells.Moreover,it has been illustrated that these defects at the CdS/Sb_(2)S_(3)interface can be reduced by optimizing the deposition process.A trap distribution model is used to quantify the defect density at the CdS/Sb_(2)S_(3)interface.It shows that the interface defects can be reduced by24% by improving the deposition process.This work reveals the importance of interface defects and guides the future optimization of Sb_(2)S_(3)solar cells.
基金supported by the National Natural Science Foundation of China(62074052,61974173,52072327)the Joint Talent Cultivation Funds of NSFC-HN(U1904192)the Science and Technology Innovation Talents in Universities of Henan Province(21HASTIT023)。
文摘Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells suffer from severe carrier recombination,limiting the photovoltaic performance.Unfavorable energy band alignment at the p-n junction and defective front interface are two main causes.Herein,oxygen incorporation in CZTSSe via absorber air-annealing was developed as a strategy to optimize its surface photoelectric property and reduce the defects.With optimized oxygen incorporation conditions,the carrier separation and collection behavior at the front interface of the device is improved.In particular,it is found that oxygen incorporated absorber exhibits increased band bending,larger depletion region width,and suppressed absorber defects.These indicate the dynamic factors for carrier separation become stronger.Meanwhile,the increased potential difference between grain boundaries and intra grains combined with the decreased concentration of interface deep level defect in the absorber provide a better path for carrier transport.As a consequence,the champion efficiency of CZTSSe solar cells has been improved from 9.74%to 12.04%with significantly improved open-circuit voltage after optimized air-annealing condition.This work provides a new insight for interface engineering to improve the photoelectric conversion efficiency of CZTSSe devices.
基金financially supported by the National Natural Science Foundation of China (Nos. 22179053, 22279046 and 21905119)the Natural Science Excellent Youth Foundation of Jiangsu Provincial (No. BK20220112)the Six-Peak Top Talents in Jiangsu province (No. XNY066)。
文摘The buried interface defects severely affect the further enhancements of efficiency and stability of SnO_(2)-based planar perovskite solar cells(PSCs).To well tackle this problem,we propose a passivation strategy employing NH_(4)PF_6 to modify the buried interface of perovskite layer((FAPbI_(3))_(0.85)(MAPbBr_(3))_(0.15) composition) in planar PSCs.After introducing NH_(4)PF_(6),the oxygen defects on the surface of SnO_(2) film are greatly restricted due to the coordinate interaction between fluorine atoms(F) in PF_(6)^(-)and undercoordinated Sn^(4+).Meanwhile,the hydrogen bonding interaction(N-H…I) between NH_(4)PF_(6) and PbI_(2) can passivate the non-radiative charge recombination sites,significantly optimizing the quality of perovskite film,as well as the charge transfer process at the SnO_(2)/perovskite interface.As a result,the NH_(4)PF_(6)-modified PSC obtains a champion power conversion efficiency(PCE) of 21.11%superior to the reference device(18.46%),and the device with an active area of 1 cm^(2) achieves a PCE as high as17.38%.Furthermore,the unencapsulated NH_(4)PF_(6)-modified PSCs show good humidity stability and retain about80% of the initial PCE after 1080 h aging at the relative humidity(RH) of 35% ± 5%.
基金Project supported by the Science Challenge Project(Grant No.TZ2016003-1-105)Tianjin Natural Science Fundation(Grant No.20JCZDJC00750)the Fundamental Research Funds for the Central Universities,Nankai University(Grant Nos.63211107 and 63201182).
文摘Defects have a significant impact on the performance of semiconductor devices.Using the first-principles combined with one-dimensional static coupling theory approach,we have calculated the variation of carrier capture coefficients with temperature for the interfacial defects P_(b0) and P_(b1) in amorphous-SiO_(2)/Si(100)interface.It is found that the geometrical shapes of P_(b0) and P_(b1) defects undergo large deformations after capturing carriers to form charged defects,especially for the Si atoms containing a dangling bond.The hole capture coefficients of neutral P_(b0) and P_(b1) defects are largest than the other capture coefficients,indicating that these defects have a higher probability of forming positively charged centres.Meanwhile,the calculated results of non-radiative recombination coefficient of these defects show that both P_(b0) and P_(b1) defects are the dominant non-radiative recombination centers in the interface of a-SiO_(2)/Si(100).
基金Supported by the National Natural Science Foundation of China Under Grant No 61205180the Natural Science Foundation of Hebei Province under Grant No E2014201188+1 种基金the Hebei University Science Funds for Distinguished Young Scholars under Grant No 2012JQ01the Program for Top Young Talents of Hebei Province
文摘Based on the first-principles method, the structural stability and the contribution of point defects such as O, Sr or Ti vacancies on two-dimensional electron gas of n- and p-type LaAlO3/SrTiO3 interfaces are investigated. The results show that O vacancies at p-type interfaces have much lower formation energies, and Sr or Ti vacancies at n-type interfaces are more stable than the ones at p-type interfaces under O-rich conditions. The calculated densities of states indicate that O vacancies act as donors and give a significant compensation to hole carriers, resulting in insulating behavior at p-type interfaces. In contrast, Sr or Ti vacancies tend to trap electrons and behave as acceptors. Sr vacancies are the most stable defects at high oxygen partial pressures, and the Sr vacancies rather than Ti vacancies are responsible for the insulator-metal transition of n-type interface. The calculated results can be helpful to understand the tuned electronic properties of LaAlO3 /SrTiO3 heterointerfaces.
基金financially supported by the Support Plan for Overseas Students to Return to China for Entrepreneurship and Innovation(cx2020003)the Fundamental Research Funds for the Central Universities(2020CDJ-LHZZ-074 and 2021CDJQY-022)Natural Science Foundation of Chongqing(cstc2020jcyjmsxmX0629)。
文摘Although ionic liquids(ILs)have been widely employed to heal the defects in perovskite solar cells(PSCs),the corresponding defect passivation mechanisms are not thoroughly understood up to now.Herein,we first reveal an abnormal buried interface anion defect passivation mechanism depending on cationinduced steric hindrance.The IL molecules containing the same anion([BF4]^(-))and different sizes of imidazolium cations induced by substituent size are used to manipulate buried interface.It was revealed what passivated interfacial defects is mainly anions instead of cations.Theoretical and experimental results demonstrate that the large-sized cations can weaken the ionic bond strength between anions and cations,and facilitate the interaction between anions and SnO2as well as perovskites,which is conducive to interfacial defect passivation and ameliorating interfacial contact.It can be concluded that interfacial chemical interaction strength and defect passivation effect are positively correlated with the size of cations.The discovery breaks conventional thinking that large-sized modification molecules would weaken their chemical interaction with perovskite.Compared with the control device(21.54%),the device based on 1,3-Bis(1-adamantyl)-imidazolium tetrafluoroborate(BAIMBF4)with maximum size cations achieves a significantly enhanced efficiency of 23.61%along with much increased moisture,thermal and light stabilities.
基金Project supported by the Science Challenge Project,China(Grant No.TZ2016003-1-105)the Tianjin Natural Science Foundation,China(Grant No.20JCZDJC00750)the Fundamental Research Funds for the Central Universities,Nankai University(Grant Nos.63211107 and 63201182).
文摘It is well known that in the process of thermal oxidation of silicon,there are P_(b)-type defects at amorphous silicon dioxide/silicon(a-SiO_(2)/Si)interface due to strain.These defects have a very important impact on the performance and reliability of semiconductor devices.In the process of passivation,hydrogen is usually used to inactivate P_(b)-type defects by the reaction P_(b)+H_(2)→P_(b)H+H.At the same time,P_(b)H centers dissociate according to the chemical reaction P_(b)H→P_(b)+H.Therefore,it is of great significance to study the balance of the passivation and dissociation.In this work,the reaction mechanisms of passivation and dissociation of the P_(b)-type defects are investigated by first-principles calculations.The reaction rates of the passivation and dissociation are calculated by the climbing image-nudged elastic band(CI-NEB)method and harmonic transition state theory(HTST).By coupling the rate equations of the passivation and dissociation reactions,the equilibrium density ratio of the saturated interfacial dangling bonds and interfacial defects(P_(b),P_(b)0,and P_(b)1)at different temperatures is calculated.
基金supported by the National Natural Science Foundation of China(Grant Nos.62104156,62074102)the Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2023A1515011256,2022A1515010979)China+1 种基金Science and Technology plan project of Shenzhen(Grant Nos.20220808165025003,20200812000347001)Chinasupported by the open foundation of Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials,State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures,Guangxi University(Grant No.2022GXYSOF13)。
文摘Sb_(2)Se_(3) with unique one-dimensional(1D) crystal structure exhibits exceptional deformation tolerance,demonstrating great application potential in flexible devices.However,the power conversion efficiency(PCE) of flexible Sb_(2)Se_(3) photovoltaic devices is temporarily limited by the complicated intrinsic defects and the undesirable contact interfaces.Herein,a high-quality Sb_(2)Se_(3) absorber layer with large crystal grains and benign [hkl] growth orientation can be first prepared on a Mo foil substrate.Then NaF intermediate layer is introduced between Mo and Sb_(2)Se_(3),which can further optimize the growth of Sb_(2)Se_(3)thin film.Moreover,positive Na ion diffusion enables it to dramatically lower barrier height at the back contact interface and passivate harmful defects at both bulk and heterojunction.As a result,the champion substrate structured Mo-foil/Mo/NaF/Sb_(2)Se_(3)/CdS/ITO/Ag flexible thin-film solar cell delivers an obviously higher efficiency of 8.03% and a record open-circuit voltage(V_(OC)) of 0.492 V.This flexible Sb_(2)Se_(3) device also exhibits excellent stability and flexibility to stand large bending radius and multiple bending times,as well as superior weak light photo-response with derived efficiency of 12.60%.This work presents an effective strategy to enhance the flexible Sb_(2)Se_(3) device performance and expand its potential photovoltaic applications.
文摘This scientific paper presents a study investigating the effects of defects at the CdS/CIGS and CdS/SDL interfaces on the performance of CIGS solar cells. The objective of this study is to analyze the influence of defects at the interface between the CdS buffer layer and the CIGS absorber, as well as the surface defect layer (SDL), on CIGS solar cell performance. The study explores three key aspects: the impact of the conduction band offset (CBO) at the CdS/CIGS interface, the effects of interface defects and defect density on performance, and the combined influence of CBO and defect density at the CdS/ SDL and SDL/CIGS interfaces. For interface defects not exceeding 10<sup>13</sup> cm<sup>-2</sup>, we obtained a good efficiency of 22.9% when -0.1 eV analyzing the quality of CdS/SDL and SDL/CIGS junctions, it appears that defects at the SDL/CIGS interface have very little impact on the performances of the CIGS solar cell. By optimizing the electrical parameters of the CdS/SDL interface defects, we achieved a conversion efficiency of 23.1% when -0.05 eV < CBO < 0.05 eV.
