In the realm of large-scale power system energy storage,sodium-based batteries represent a cost-effective post-lithium energy storage technology,making inorganic solid-state sodium batteries(ISSSB)a critical branch of...In the realm of large-scale power system energy storage,sodium-based batteries represent a cost-effective post-lithium energy storage technology,making inorganic solid-state sodium batteries(ISSSB)a critical branch of this development.Inorganic solid-state electrolytes(ISSEs)are the core components of sodium batteries;however,they face significant challenges such as insufficient ionic conductivity,interfacial instability,and dendrite growth,all of which severely hinder practical application.This review critically assesses experimental protocols and theoretical frameworks related to mainstream ISSEs and systematizes optimization strategies aimed at overcoming these challenges.Leveraging integrated insights from both experimental and computational studies,the review first categorizes and summarizes the primary types of ISSEs,namely oxide-,sulfide-,and halide-based electrolytes.It then details interfacial optimization strategies focused on addressing three core interfacial issues:ion transport barriers resulting from mechanical incompatibility,side reactions stemming from electrochemical mismatch,and dendrite formation.Finally,the review advocates prioritizing in-depth research that integrates experimental and theoretical approaches to establish a closed-loop methodology encompassing predictive design,multiscale investigation,mechanistic exploration,and high-throughput automated experimentation,with feedback-driven refinement.This work serves as a comprehensive reference and systematic roadmap for future research on solid-state electrolytes(SSEs).展开更多
Solar-driven Fenton-like reactions are promising strategies for degrading pharmaceutical wastewater to address environmental challenges and antibiotic pollution.However,its efficacy is limited by suboptimal light abso...Solar-driven Fenton-like reactions are promising strategies for degrading pharmaceutical wastewater to address environmental challenges and antibiotic pollution.However,its efficacy is limited by suboptimal light absorption efficiency,rapid charge recombination,and inadequate interfacial charge transfer.In this study,an inorganic/organic S-scheme photo-Fenton system of pseudobrookite/carbon nitride(FTOCN)was synthesized via a hydrothermally coupled calcination process for the effective purification of tetracycline antibiotics under visible-light irradiation.The optimized FTOCN-2 heterostructure exhibits a significantly enhanced TC degradation capacity of 90%within 60 min.The rate constant of FTOCN-2 is 1.6 and 5.2 times greater than those of FTO and CN,respectively.Furthermore,FTOCN exhibits high antibacterial efficacy,highlighting its potential application in the purification of natural water.Measurements via a range of analytical techniques,including Kelvin probe force microscopy,density functional theory calculations,in situ X-ray photoelectron spectroscopy,and femtosecond transient absorption spectroscopy,corroborate the S-scheme mechanism.This study provides a novel perspective for the development of photo-Fenton systems with S-scheme heterojunctions for water purification.展开更多
CsPbBr_(3)perovskite solar cells(PSCs)have attracted significant interest for their remarkable stability under high temperatures and humidity.However,challenges such as energy loss at the CsPbBr_(3)/oxide buried inter...CsPbBr_(3)perovskite solar cells(PSCs)have attracted significant interest for their remarkable stability under high temperatures and humidity.However,challenges such as energy loss at the CsPbBr_(3)/oxide buried interface and imperfect band alignment have impeded further efficiency enhancements.In this study,TiO_(2),SnO_(2),or ZnO was employed as electron transport layer(ETL)materials,respectively,in CsPbBr_(3)-based PSCs to optimize the band alignment at the ETL/CsPbBr_(3)interface and enhance the film quality of CsPbBr_(3)materials.The research findings indicate that the power conversion efficiency(PCE)of PSCs is influenced by the choice of ETL material.Specifically,TiO_(2)-based PSCs achieved a PCE of 10.37%efficiency,higher than SnO_(2)-or ZnO-based PSCs.This disparity in PCE can be attributed to variations in open-circuit voltage,which stem from different band alignments at the ETL/CsPbBr_(3)interface.Notably,superior photovoltaic performance was consistently observed in TiO_(2)-based PSCs due to the substantial conduction band offset(∆Ec)at the TiO_(2)/CsPbBr_(3)interface and the high quality of the CsPbBr_(3)film.This not only enhances electron extraction at the TiO_(2)/CsPbBr_(3)interface but also diminishes non-radiative recombination at the interface,as confirmed by density functional theory(DFT)calculations and experiments.Furthermore,photodetectors(PDs)based on TiO_(2)/CsPbBr_(3)heterojunction exhibit high photoresponse and photodetectivity.In conclusion,this study underscores the critical importance of the buried interface contact in CsPbBr_(3)and offers a direct approach for fabricating efficient and stable inorganic PSCs and PDs.展开更多
Organic-inorganic metal halides(OIMHs)have emerged as highly promising novel multifunctional optoelectronic materials,owing to their easily adjustable properties from a variety of combinations of different components....Organic-inorganic metal halides(OIMHs)have emerged as highly promising novel multifunctional optoelectronic materials,owing to their easily adjustable properties from a variety of combinations of different components.But it is still difficult and rare to realize highly tunable multicolor luminescence within the same material.In this work,we successfully incorporated three adjustable emission centers in OIMHs to synthesize a novel OIMH(NEA)_(2)MnBr_(4),with each emission center capable of emitting one of the primary colors—red,green,and blue.The green and red emissions originate from the tetrahedron and octahedron structures in the Mn-based frame,while the blue can be attributed to the contribution of organic components.Additionally,to achieve comparable emission intensity among the three primary colors,we enhanced the blue emission performance by optimizing the ratio of organic structure components and incorporating chirality in the OIMHs.The resulting high-quality films can be obtained by spin-coating method with a photoluminescence quantum yields of up to 96%.More interestingly,by the dual manipulation of excitation wavelength and temperature,the sample can be emitted at least seven distinct colors including a standard white luminescence at(0.33,0.33),opening up promising prospects for multicolor luminescence applications such as high-end anti-counterfeiting technology,light-emitting diodes,X-ray imaging,latent fingerprints,humidity detection,and so on.Therefore,based on application scenarios and requirements,our research on this highly tunable luminescent OIMH material lays a solid foundation for further development of various functional properties of related materials.展开更多
For the further improvement of the power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs),the buried interface between the perovskite and the electron transport layer is crucial.However,it is ch...For the further improvement of the power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs),the buried interface between the perovskite and the electron transport layer is crucial.However,it is challenging to effectively optimize this interface as it is buried beneath the perovskite film.Herein,we have designed and synthesized a series of multifunctional organic-inorganic(OI)complexes as buried interfacial material to promote electron extraction,as well as the crystal growth of the perovskite.The OI complex with BF4−group not only eliminates oxygen vacancies on the SnO_(2) surface but also balances energy level alignment between SnO_(2) and perovskite,providing a favorable environment for charge carrier extraction.Moreover,OI complex with amine(−NH_(2))functional group can regulate the crystallization of the perovskite film via interaction with PbI2,resulting in highly crystallized perovskite film with large grains and low defect density.Consequently,with rational molecular design,the PSCs with optimal OI complex buried interface layer which contains both BF4−and−NH_(2) functional groups yield a champion device efficiency of 23.69%.More importantly,the resulting unencapsulated device performs excellent ambient stability,maintaining over 90%of its initial efficiency after 2000 h storage,and excellent light stability of 91.5%remaining PCE in the maximum power point tracking measurement(under continuous 100 mW cm−2 light illumination in N2 atmosphere)after 500 h.展开更多
Incubation experiments are carried out to study the exchange rates of dissolved inorganic nutrients including silicate, phosphate, ammonium, nitrite, and nitrate (vSiO3-Si, vPO4-P, vNH4-N, vNO2-N and vNO3-N) at the se...Incubation experiments are carried out to study the exchange rates of dissolved inorganic nutrients including silicate, phosphate, ammonium, nitrite, and nitrate (vSiO3-Si, vPO4-P, vNH4-N, vNO2-N and vNO3-N) at the sediment-water interface in the Jiaozhou Bay. Major factors influencing the exchange rates are discussed in detail, which include the dissolved inorganic nutrient concentrations in porewater (Cpw), water and clay contents, and grain size of the sediments (CH2O, Cclay and GSsed). The results may provide insight into the dynamics of nutrient transport and the environmental capacity of nutrients in Jiaozhou Bay, and should be beneficial to solving the problems caused by excessive nutrient input this area.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
This paper reports a template-free method to synthesize a series of inorganic hollow spheres（IHSs）including Cu-1,Cu-2,Ni-1,Ni-2 based on mineralization reactions at water/＂water-brother＂ interfaces. ＂Water-brothe...This paper reports a template-free method to synthesize a series of inorganic hollow spheres（IHSs）including Cu-1,Cu-2,Ni-1,Ni-2 based on mineralization reactions at water/＂water-brother＂ interfaces. ＂Water-brother＂ was defined as a solvent which is miscible with water,such as ethanol and acetone. The water/＂water-brother＂ interfaces are very different from water/oil interfaces. The ＂water-brother＂ solvent will usually form a homogenous phase with water. Interestingly,in our method,these interfaces can be formed,observed and utilized to synthesize hollow spheres. Utilizing the unique porous properties of the spheres,their potential application in water treatment was demonstrated by using Cu-1 IHSs as Fenton-like reagents for adsorption and decomposition of Congo Red from aqueous solution. The final adsorption equilibrium was achieved after 30 min with the maximum adsorption capacity of 86.1 mg/g,and 97.3% removal of the dye in 80 min after adsorption equilibrium. The IHSs can be reused as least 5 times after treatment by Na OH.This method is facile and suitable for large-scale production,and shows great potential for watertreatment. 更多展开更多
Particles of TiO2 modified with poly 3-(2-thienyl) aniline (PThA) and occluded in poly 2,2 bithiophene (PBTh), were subjected to optical, electrochemical impedance spectroscopic (EIS) and photoelectrochemical (PEC) in...Particles of TiO2 modified with poly 3-(2-thienyl) aniline (PThA) and occluded in poly 2,2 bithiophene (PBTh), were subjected to optical, electrochemical impedance spectroscopic (EIS) and photoelectrochemical (PEC) investigation in aqueous, acetate, citrate, and phosphate electrolytes. EIS studies revealed that the assembly film of TiO2/PThA/PBTh possess porous-type structure. They also confirmed the approximate value of Ef obtained from electrochemical studies. Both EIS and optical studies indicated that ac conductivity is much greater than dc conductivity. Guided by the properties of PBTh, no large changes in the energy band structure occurred due to occlusion of TiO2 in PBTh films. Occlusion of TiO2/PThA into the network structure of PBTh inhibits the energy dissipation process and impeded charge polarization process of the material. Photoelectrochemical outcome suggested possible band alignments between the organic film and TiO2 and formation of hybrid sub-bands. Inclusion of TiO2 in the thiophene-based polymers enhanced the charge separation and consequently charge transfer processes and widen the absorption in visible light range.展开更多
Sodium-ion batteries have garnered significant attention due to their abundant sodium resources and low cost,showing great potential for large-scale energy storage.However,traditional sodium-ion batteries,which rely o...Sodium-ion batteries have garnered significant attention due to their abundant sodium resources and low cost,showing great potential for large-scale energy storage.However,traditional sodium-ion batteries,which rely on flammable liquid electrolytes as the ion transport medium,pose safety challenges in practical applications.Using solid-state electrolytes instead of liquid electrolytes can effectively improve the safety and electrochemical performance of battery systems,making solid-state sodium-ion batteries as a highly promising option for energy storage.Solid-state electrolytes are categorized into organic and inorganic types.Inorganic solid-state electrolytes have garnered increased interest for their high ionic conductivity,high ion mobility,excellent mechanical properties,and good thermal stability.This review systematically explores the advancements in various inorganic solid-state electrolytes,includingβ-Al_(2)O_(3),sodium superionic conductor,sulfide,halide,complex hydride,and anti-perovskite.The review focuses on material preparation,ionic conductivity,and electrochemical properties.Additionally,it addresses the interface challenges between inorganic solid-state electrolytes and electrode materials,along with effective strategies to improve these interfaces.展开更多
Organic light-emitting transistors(OLETs)are gaining increasing attention as a promising candidate for nextgeneration display technology.However,due to the limited horizontal charge transport capability in OLETs,enhan...Organic light-emitting transistors(OLETs)are gaining increasing attention as a promising candidate for nextgeneration display technology.However,due to the limited horizontal charge transport capability in OLETs,enhancing their optical performance remains greatly challenging.In this work,an effective strategy is employed to achieve highperformance OLETs by constructing a two-dimensional molecular-scale passivation layer at the dielectric/channel interface using a promising solution-processed small-molecule material,tetratetracontane(TTC).By controlling the microscopic flows driven by intermolecular interactions near the solution meniscus,molecular self-assembly dynamics are effectively regulated,contributing to a significant transformation in molecular layer stacking mode and enabling the formation of large-area TTC thin films with two-dimensional molecular-scale surface structure and uniform morphology.The introduction of high-quality TTC passivation layer film into the dielectric/channel interface optimizes the film morphologies of overlying channel layer,effectively shields the electrostatic dipole effects at dielectric/channel interface,leading to the synergistic optoelectronic regulation and enhanced optical properties of OLETs.Consequently,high brightness of 10,077.3 cd·m^(-2),high external quantum efficiency(EQE)of 20.46%,and low voltage of 15 V are achieved in the lateral OLET.This work presents a promising approach for two-dimensional molecular-scale small molecule interfaces,and provides an effective strategy for achieving high-performance OLET devices.展开更多
Designing high-efficiency photocatalysts by the construction of organic/inorganic heterojunctions is considered to be an effective approach for improving photocatalytic hydrogen evolution reaction(HER)activity.This wo...Designing high-efficiency photocatalysts by the construction of organic/inorganic heterojunctions is considered to be an effective approach for improving photocatalytic hydrogen evolution reaction(HER)activity.This work designed and built unique S-scheme heterojunctions by in-situ growing inorganic WO_(3) nanoparticles with excellent oxidation ability on fused-sulfone-modified covalent organic frameworks(FS-COF)with strong reduction ability.It is found that FS-COF and WO_(3) have a well-matched staggered band alignment.The best-designed FS-COF/WO_(3)-20%exhibits a maximum photocatalytic HER rate of 24.7 mmol g^(-1) h^(-1) under visible light irradiation,which is 1.4 times greater than the pure FS-COF.Moreover,photogenerated electron-hole pairs can be separated and utilized more efficiently thanks to the FS-COF/WO_(3) heterojunction's ability to create a favorable internal electric field resulting from the difference in work functions between FS-COF and WO_(3),which speeds up the transfer dynamics of photoinduced electrons from WO_(3) to FS-COF through an additional interfacial electron-transfer channel obeying the directional S-scheme migration mechanism.Furthermore,the S-scheme migration mechanism of photoinduced charge carriers instead of the type-II mechanism was confirmed by the signal intensity of•O_(2)−species from spin-trapping electron paramagnetic resonance spectra over the single component and the formed heterojunction.It ensures the photoexcited electrons maintain on the lowest unoccupied molecular orbital of FS-COF with a strong reduction ability to participate in photocatalytic HER,resulting in a significantly boosted H_(2) evolution rate.Based on organic/inorganic coupling,this work offers a strategy for creating particular S-scheme heterojunction photocatalysts.展开更多
The water adsorption performance of shale gas reservoirs is a very important factor affecting their gas in place(GIP)contents,but the water-holding capacity and mechanism of over-mature shale,especially organic pores,...The water adsorption performance of shale gas reservoirs is a very important factor affecting their gas in place(GIP)contents,but the water-holding capacity and mechanism of over-mature shale,especially organic pores,are still not fully understood.In this study,systematic water vapor adsorption(WVA)experiments were carried out on the Lower Cambrian over-mature shale and its kerogen from the Sichuan Basin,China to characterize their WVA behaviors,and combined with the low-pressure gas(N_(2) and CO_(2))adsorption experiments,the main influencing factors of WVA capacity of the shale and the absorbed-water distribution in its organic and inorganic nanopores were investigated.The results show that the WVA isotherms of shale and kerogen are all typeⅡ,with an obvious hysteresis loop in the multilayer adsorption range,and that the positive relationship of the shale TOC content with the WVA capacity(including total adsorption capacity,primary adsorption capacity and secondary adsorption capacity)and WVA hysteresis index(AHIW),and the greater adsorption capacity and AHIW of kerogen than the shale,all indicate that the hydrophilicity of organic matter(OM)in the over-mature shale was underestimated in previous research.Although both the shale OM and clay minerals have a significant positive effect on the WVA,the former has a stronger adsorption ability than the latter.The WVA capacity of the studied Lower Cambrian shale is significantly greater than that of the Longmaxi shale reported in literatures,which was believed to be mainly attributed to its higher maturity,with a significant graphitization of OM.The shale micropores and non-micropores play an important role in WVA,especially OM pores.There are primary and secondary adsorption for water vapor in both the micropores and non-micropores of OM,while these adsorptions of minerals mainly occur in their non-micropores.These results have important guides for understanding the gas storage mechanism and exploration and development potential of marine over-mature shale in southern China,especially the Lower Cambrian shale.展开更多
The exchange of inorganic nutrients at the coastal sediment-water interface(SWI)plays a crucial role in regulating the nutrient budget in overlying water.The related studies mainly focus on the mid-to high-latitude re...The exchange of inorganic nutrients at the coastal sediment-water interface(SWI)plays a crucial role in regulating the nutrient budget in overlying water.The related studies mainly focus on the mid-to high-latitude regions,leaving a significant gap in the quantitative assessment of nutrient exchange and environmental controls at the SWI in lowlatitude coastal regions.We quantitatively assess the exchange of inorganic nutrients at the SWI in three tropical bays(Dongzhai Harbor,Xiaohai Lagoon,Qinglan Harbor).Sediments act as a source of ammonium,phosphate,and silicate,but for nitrate,sediments can be both a source and sink,although with substantial spatial and temporal variations in their fluxes.Labile organic matter is a critical regulator for the fluxes of inorganic nutrients at the SWI.The sedimentary nutrients input with high N/P molar ratio will alter the nutrient stoichiometry to mitigate the nitrogen limitation in coastal waters.However,the internal sediment release in these tropical bays plays a relative weak role in contributing to the nutrient addition in comparison with the other external nutrient sources including riverine input,submarine groundwater discharge,and atmospheric deposition.According to the global compilation on SWI nutrient fluxes,we propose that water column primary production and external inputs to interpret the variation in exchange and fluxes of nutrients at the SWI in different ecosystems.Such a conceptual understanding of these chain biogeochemical processes involving external nutrient input,primary production,particulate organic matter settling,and the accumulation and release of inorganic nutrients in sediments will be helpful for the scientific-based pollution prevent and control in coastal waters.展开更多
High-energy-density lithium metal batteries hold great promise for advancing low-altitude economic development.However,the practical application of ultrathin lithium anodes remains challenging due to significant inter...High-energy-density lithium metal batteries hold great promise for advancing low-altitude economic development.However,the practical application of ultrathin lithium anodes remains challenging due to significant interfacial side reactions,dendrite formation,and substantial volume fluctuations.In this study,lithium metal electrodes were fabricated using a spin-coating process,enabling an in situ reaction between lithium and phenyl disulfide(PDS).The resulting robust organic sulfurization interface,composed of lithium thiophenoxide,facilitates rapid lithium-ion transport and effectively suppresses dendrite formation.Symmetric cells with a 50μm Li@PDS anode exhibited an impressive lifespan exceeding3000 h at 1 mA cm^(-2)and 1 mAh cm^(-2).The Li@PDS anode demonstrated excellent structural stability in a practical LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)lILi@PDS pouch cell,maintaining 94.8%of its initial capacity(1.45 Ah)over 260 cycles at a 0.4C rate and 87.30%of its initial capacity(1.1 Ah)over 360 cycles at a 2C rate(1C=200 mA g^(-1)).This work provides a promising pathway for developing durable lithium metal anodes suitable for scalable practical applications.展开更多
Poly(3-hexylthiophene)(P3HT)is one of the most promising hole-transporting materials in the pursuit of efficient and stable perovskite solar cells due to its outstanding stability and low cost.However,the intrinsic lo...Poly(3-hexylthiophene)(P3HT)is one of the most promising hole-transporting materials in the pursuit of efficient and stable perovskite solar cells due to its outstanding stability and low cost.However,the intrinsic low carrier density of P3 HT and poor contact between the P3HT/perovskite interface always lead to a low performance of the solar cell,while conventional chemical doping always makes the films unstable and limits the scalability.In this work,for the first time,we simultaneously enhanced the hole transporting properties of P3HT film and the interface of perovskite by doping it with a judiciously designed oxidized small molecule organic semiconductor.The organic salt not only can promote the lamellar crystallinity of P3HT to obtain better charge transport properties,but also reduce the defects of perovskite.As a result,we achieved champion efficiencies of 23.0%for small-area solar cells and 18.8%for larger-area modules(48.0 cm^(2)).This efficiency is the highest value for P3HT-based perovskite modules.Moreover,the solar cells show excellent operational stability,retaining over 95%of their initial efficiencies after1200 h of continuous operation.展开更多
Lithium metal is one of the most promising anodes for next-generation batteries due to its high capacity and low reduction potential.However,the notorious Li dendrites can cause the short life span and safety issues,h...Lithium metal is one of the most promising anodes for next-generation batteries due to its high capacity and low reduction potential.However,the notorious Li dendrites can cause the short life span and safety issues,hindering the extensive application of lithium batteries.Herein,Li_(7)La_(3)Zr_(2)O_(12)(LLZO)ceramics are integrated into polyethylene oxide(PEO)to construct a facile polymer/inorganic composite solid-state electrolyte(CSSE)to inhibit the growth of Li dendrites and widen the electrochemical stability window.Given the feasibility of our strategy,the designed PEO-LLZO-LiTFSI composite solid-state electrolyte(PLLCSSE)exhibits an outstanding cycling property of 134.2 mAh g^(-1) after 500 cycles and the Coulombic efficiency of 99.1%after 1000 cycles at 1 C in LiFePO_(4)-Li cell.When cooperated with LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622)cathode,the PLL-CSSE renders a capacity retention of 82.4%after 200 cycles at 0.2 C.More importantly,the uniform dispersion of LLZO in PEO matrix is tentative tested via Raman and FT-IR spectra and should be responsible for the improved electrochemical performance.The same conclusion can be drawn from the interface investigation after cycling.This work presents an intriguing solid-state electrolyte with high electrochemical performance,which will boost the development of all-solid-state lithium batteries with high energy density.展开更多
All-solid-state batteries potentially exhibit high specific energy and high safety,which is one of the development directions for nextgeneration lithium-ion batteries.The compatibility of all-solid composite electrode...All-solid-state batteries potentially exhibit high specific energy and high safety,which is one of the development directions for nextgeneration lithium-ion batteries.The compatibility of all-solid composite electrodes with high-nickel layered cathodes and inorganic solid electrolytes is one of the important problems to be solved.In addition,the interface and mechanical problems of high-nickel layered cathodes and inorganic solid electrolyte composite electrodes have not been thoroughly addressed.In this paper,the possible interface and mechanical problems in the preparation of high-nickel layered cathodes and inorganic solid electrolytes and their interface reaction during charge–discharge and cycling are reviewed.The mechanical contact problems from phenomena to internal causes are also analyzed.Uniform contact between the high-nickel cathode and solid electrolyte in space and the ionic conductivity of the solid electrolyte are the prerequisites for the good performance of a high-nickel layered cathode.The interface reaction and contact loss between the high-nickel layered cathode and solid electrolyte in the composite electrode directly affect the passage of ions and electrons into the active material.The buffer layer constructed on the high-nickel cathode surface can prevent direct contact between the active material and electrolyte and slow down their interface reaction.An appropriate protective layer can also slow down the interface contact loss by reducing the volume change of the high-nickel layered cathode during charge and discharge.Finally,the following recommendations are put forward to realize the development vision of high-nickel layered cathodes:(1)develop electrochemical systems for high-nickel layered cathodes and inorganic solid electrolytes;(2)elucidate the basic science of interface and electrode processes between high-nickel layered cathodes and inorganic solid electrolytes,clarify the mechanisms of the interfacial chemical and electrochemical reactions between the two materials,and address the intrinsic safety issues;(3)strengthen the development of research and engineering technologies and their preparation methods for composite electrodes with high-nickel layered cathodes and solid electrolytes and promote the industrialization of all-solid-state batteries.展开更多
The self-assembled monolayer(SAM),functioning as a hole transport layer,holds the potential to substantially elevate the efficiency of perovskite and organic solar cells.Nevertheless,incomplete SAM coverage may result...The self-assembled monolayer(SAM),functioning as a hole transport layer,holds the potential to substantially elevate the efficiency of perovskite and organic solar cells.Nevertheless,incomplete SAM coverage may result in interface defects lurking between the photovoltaic layer and the electrode,thereby causing non-radiative recombination losses of interfacial charges.To tackle this issue,we introduced 4-bromobutyric acid to co-assemble with the SAM,yielding a more compact co-assembled monolayer(co-SAM)that effectively repairs these defective zones.Confocal laser scanning microscopy and Kelvin Probe Force Microscopy show that co-SAMs successfully mitigate interface defects in the previously uncovered electrode regions.Furthermore,the work function of the electrodes is elevated to 5.6 eV,facilitating efficient hole extraction.Consequently,devices incorporating co-SAMs exhibit notably reduced non-radiative recombination losses.The power conversion efficiency(PCE)of the devices is enhanced to 20.0% in binary organic solar cells,and an even more remarkable breakthrough PCE of 25.8% is achieved in perovskite/organic tandem devices.This study introduces a straightforward strategy to improve the hole-selective contact of electrodes,ultimately boosting the overall efficiency of the devices.展开更多
Doping is essential for modulating semiconductor conductivity,forming p-n junctions,and reducing contact resistance[1].Notably,as organic semiconductors(OSCs)advance toward high performance,flexibility,and miniaturiza...Doping is essential for modulating semiconductor conductivity,forming p-n junctions,and reducing contact resistance[1].Notably,as organic semiconductors(OSCs)advance toward high performance,flexibility,and miniaturization,achieving precise regionally selective doping becomes critical for building complex,highly integrated devices[2].In inorganic semiconductors(e.g.,silicon),sub-100-nanometer regional doping is achievable through photolithography and ion implantation—techniques foundational to modern complementary metaloxide-semiconductor(CMOS)technology[3].展开更多
基金the National Natural Science Foundation of China (52076076, 52006065)Fundamental Research Funds for Central Universities (2025JC003)Beijing Municipal Natural Science Foundation (3242022)
文摘In the realm of large-scale power system energy storage,sodium-based batteries represent a cost-effective post-lithium energy storage technology,making inorganic solid-state sodium batteries(ISSSB)a critical branch of this development.Inorganic solid-state electrolytes(ISSEs)are the core components of sodium batteries;however,they face significant challenges such as insufficient ionic conductivity,interfacial instability,and dendrite growth,all of which severely hinder practical application.This review critically assesses experimental protocols and theoretical frameworks related to mainstream ISSEs and systematizes optimization strategies aimed at overcoming these challenges.Leveraging integrated insights from both experimental and computational studies,the review first categorizes and summarizes the primary types of ISSEs,namely oxide-,sulfide-,and halide-based electrolytes.It then details interfacial optimization strategies focused on addressing three core interfacial issues:ion transport barriers resulting from mechanical incompatibility,side reactions stemming from electrochemical mismatch,and dendrite formation.Finally,the review advocates prioritizing in-depth research that integrates experimental and theoretical approaches to establish a closed-loop methodology encompassing predictive design,multiscale investigation,mechanistic exploration,and high-throughput automated experimentation,with feedback-driven refinement.This work serves as a comprehensive reference and systematic roadmap for future research on solid-state electrolytes(SSEs).
文摘Solar-driven Fenton-like reactions are promising strategies for degrading pharmaceutical wastewater to address environmental challenges and antibiotic pollution.However,its efficacy is limited by suboptimal light absorption efficiency,rapid charge recombination,and inadequate interfacial charge transfer.In this study,an inorganic/organic S-scheme photo-Fenton system of pseudobrookite/carbon nitride(FTOCN)was synthesized via a hydrothermally coupled calcination process for the effective purification of tetracycline antibiotics under visible-light irradiation.The optimized FTOCN-2 heterostructure exhibits a significantly enhanced TC degradation capacity of 90%within 60 min.The rate constant of FTOCN-2 is 1.6 and 5.2 times greater than those of FTO and CN,respectively.Furthermore,FTOCN exhibits high antibacterial efficacy,highlighting its potential application in the purification of natural water.Measurements via a range of analytical techniques,including Kelvin probe force microscopy,density functional theory calculations,in situ X-ray photoelectron spectroscopy,and femtosecond transient absorption spectroscopy,corroborate the S-scheme mechanism.This study provides a novel perspective for the development of photo-Fenton systems with S-scheme heterojunctions for water purification.
基金supported by the National Natural Science Foundation of China(Nos.62304171 and 62374128)the China Postdoctoral Science Foundation(No.2022M722500)+2 种基金the Key Research and Development Program of Shaanxi Province(No.2024GX-YBXM-512)Xidian University Specially Funded Project for Interdisciplinary Exploration(Nos.TZJH2024052 and TZJH2024050)the Fundamental Research Funds for the Central Universities,the open fund of State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan University of Technology(No.2024-KF-12).
文摘CsPbBr_(3)perovskite solar cells(PSCs)have attracted significant interest for their remarkable stability under high temperatures and humidity.However,challenges such as energy loss at the CsPbBr_(3)/oxide buried interface and imperfect band alignment have impeded further efficiency enhancements.In this study,TiO_(2),SnO_(2),or ZnO was employed as electron transport layer(ETL)materials,respectively,in CsPbBr_(3)-based PSCs to optimize the band alignment at the ETL/CsPbBr_(3)interface and enhance the film quality of CsPbBr_(3)materials.The research findings indicate that the power conversion efficiency(PCE)of PSCs is influenced by the choice of ETL material.Specifically,TiO_(2)-based PSCs achieved a PCE of 10.37%efficiency,higher than SnO_(2)-or ZnO-based PSCs.This disparity in PCE can be attributed to variations in open-circuit voltage,which stem from different band alignments at the ETL/CsPbBr_(3)interface.Notably,superior photovoltaic performance was consistently observed in TiO_(2)-based PSCs due to the substantial conduction band offset(∆Ec)at the TiO_(2)/CsPbBr_(3)interface and the high quality of the CsPbBr_(3)film.This not only enhances electron extraction at the TiO_(2)/CsPbBr_(3)interface but also diminishes non-radiative recombination at the interface,as confirmed by density functional theory(DFT)calculations and experiments.Furthermore,photodetectors(PDs)based on TiO_(2)/CsPbBr_(3)heterojunction exhibit high photoresponse and photodetectivity.In conclusion,this study underscores the critical importance of the buried interface contact in CsPbBr_(3)and offers a direct approach for fabricating efficient and stable inorganic PSCs and PDs.
基金supported by supported by the Basic Research Project of State Key Laboratory of Photovoltaic Science and Technology(No.202401020302)funding support from the National Natural Science Foundation of China(No.62274040 and No.62304046)Shanghai science and technology innovation action plan(No.24DZ3001200)。
文摘Organic-inorganic metal halides(OIMHs)have emerged as highly promising novel multifunctional optoelectronic materials,owing to their easily adjustable properties from a variety of combinations of different components.But it is still difficult and rare to realize highly tunable multicolor luminescence within the same material.In this work,we successfully incorporated three adjustable emission centers in OIMHs to synthesize a novel OIMH(NEA)_(2)MnBr_(4),with each emission center capable of emitting one of the primary colors—red,green,and blue.The green and red emissions originate from the tetrahedron and octahedron structures in the Mn-based frame,while the blue can be attributed to the contribution of organic components.Additionally,to achieve comparable emission intensity among the three primary colors,we enhanced the blue emission performance by optimizing the ratio of organic structure components and incorporating chirality in the OIMHs.The resulting high-quality films can be obtained by spin-coating method with a photoluminescence quantum yields of up to 96%.More interestingly,by the dual manipulation of excitation wavelength and temperature,the sample can be emitted at least seven distinct colors including a standard white luminescence at(0.33,0.33),opening up promising prospects for multicolor luminescence applications such as high-end anti-counterfeiting technology,light-emitting diodes,X-ray imaging,latent fingerprints,humidity detection,and so on.Therefore,based on application scenarios and requirements,our research on this highly tunable luminescent OIMH material lays a solid foundation for further development of various functional properties of related materials.
基金The authors acknowledge the financial support from the Natural Science Foundation of China(Nos.21931002 and 22101123)the National Key Research and Development Program of China(2018YFB0704100)+4 种基金the Shenzhen Science and Technology Innovation Committee(no.JCYJ20200109140812302)the Leading talents of Guangdong province program(2016LJ06N507)the Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(no.2018B030322001)the Guangdong Provincial Key Laboratory of Catalysis(no.2020B121201002)Outstanding Talents Training Fund in Shenzhen.
文摘For the further improvement of the power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs),the buried interface between the perovskite and the electron transport layer is crucial.However,it is challenging to effectively optimize this interface as it is buried beneath the perovskite film.Herein,we have designed and synthesized a series of multifunctional organic-inorganic(OI)complexes as buried interfacial material to promote electron extraction,as well as the crystal growth of the perovskite.The OI complex with BF4−group not only eliminates oxygen vacancies on the SnO_(2) surface but also balances energy level alignment between SnO_(2) and perovskite,providing a favorable environment for charge carrier extraction.Moreover,OI complex with amine(−NH_(2))functional group can regulate the crystallization of the perovskite film via interaction with PbI2,resulting in highly crystallized perovskite film with large grains and low defect density.Consequently,with rational molecular design,the PSCs with optimal OI complex buried interface layer which contains both BF4−and−NH_(2) functional groups yield a champion device efficiency of 23.69%.More importantly,the resulting unencapsulated device performs excellent ambient stability,maintaining over 90%of its initial efficiency after 2000 h storage,and excellent light stability of 91.5%remaining PCE in the maximum power point tracking measurement(under continuous 100 mW cm−2 light illumination in N2 atmosphere)after 500 h.
基金This research was partially supported by the National Natural Science Foundation of China (Nos 40136020 and 49976027)the Key Project of Chinese Ministry of Education (No.01110).
文摘Incubation experiments are carried out to study the exchange rates of dissolved inorganic nutrients including silicate, phosphate, ammonium, nitrite, and nitrate (vSiO3-Si, vPO4-P, vNH4-N, vNO2-N and vNO3-N) at the sediment-water interface in the Jiaozhou Bay. Major factors influencing the exchange rates are discussed in detail, which include the dissolved inorganic nutrient concentrations in porewater (Cpw), water and clay contents, and grain size of the sediments (CH2O, Cclay and GSsed). The results may provide insight into the dynamics of nutrient transport and the environmental capacity of nutrients in Jiaozhou Bay, and should be beneficial to solving the problems caused by excessive nutrient input this area.
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.21273059,21528501,21511130060)the HIT Environment and Ecology Innovation Special Funds(No.HSCJ201617)
文摘This paper reports a template-free method to synthesize a series of inorganic hollow spheres（IHSs）including Cu-1,Cu-2,Ni-1,Ni-2 based on mineralization reactions at water/＂water-brother＂ interfaces. ＂Water-brother＂ was defined as a solvent which is miscible with water,such as ethanol and acetone. The water/＂water-brother＂ interfaces are very different from water/oil interfaces. The ＂water-brother＂ solvent will usually form a homogenous phase with water. Interestingly,in our method,these interfaces can be formed,observed and utilized to synthesize hollow spheres. Utilizing the unique porous properties of the spheres,their potential application in water treatment was demonstrated by using Cu-1 IHSs as Fenton-like reagents for adsorption and decomposition of Congo Red from aqueous solution. The final adsorption equilibrium was achieved after 30 min with the maximum adsorption capacity of 86.1 mg/g,and 97.3% removal of the dye in 80 min after adsorption equilibrium. The IHSs can be reused as least 5 times after treatment by Na OH.This method is facile and suitable for large-scale production,and shows great potential for watertreatment. 更多
文摘Particles of TiO2 modified with poly 3-(2-thienyl) aniline (PThA) and occluded in poly 2,2 bithiophene (PBTh), were subjected to optical, electrochemical impedance spectroscopic (EIS) and photoelectrochemical (PEC) investigation in aqueous, acetate, citrate, and phosphate electrolytes. EIS studies revealed that the assembly film of TiO2/PThA/PBTh possess porous-type structure. They also confirmed the approximate value of Ef obtained from electrochemical studies. Both EIS and optical studies indicated that ac conductivity is much greater than dc conductivity. Guided by the properties of PBTh, no large changes in the energy band structure occurred due to occlusion of TiO2 in PBTh films. Occlusion of TiO2/PThA into the network structure of PBTh inhibits the energy dissipation process and impeded charge polarization process of the material. Photoelectrochemical outcome suggested possible band alignments between the organic film and TiO2 and formation of hybrid sub-bands. Inclusion of TiO2 in the thiophene-based polymers enhanced the charge separation and consequently charge transfer processes and widen the absorption in visible light range.
基金supported by the National Natural Science Foundation of China(No.22205182)National Science Fund for Distinguished Young Scholars(No.52025034)+1 种基金China Postdoctoral Science Foundation(Nos.2022M722594 and 2024T171170)Basic and Applied Basic Research Foundation of Guangdong(No.2024A1515011516).
文摘Sodium-ion batteries have garnered significant attention due to their abundant sodium resources and low cost,showing great potential for large-scale energy storage.However,traditional sodium-ion batteries,which rely on flammable liquid electrolytes as the ion transport medium,pose safety challenges in practical applications.Using solid-state electrolytes instead of liquid electrolytes can effectively improve the safety and electrochemical performance of battery systems,making solid-state sodium-ion batteries as a highly promising option for energy storage.Solid-state electrolytes are categorized into organic and inorganic types.Inorganic solid-state electrolytes have garnered increased interest for their high ionic conductivity,high ion mobility,excellent mechanical properties,and good thermal stability.This review systematically explores the advancements in various inorganic solid-state electrolytes,includingβ-Al_(2)O_(3),sodium superionic conductor,sulfide,halide,complex hydride,and anti-perovskite.The review focuses on material preparation,ionic conductivity,and electrochemical properties.Additionally,it addresses the interface challenges between inorganic solid-state electrolytes and electrode materials,along with effective strategies to improve these interfaces.
基金supported by the National Natural Science Foundation of China(Nos.62474011 and 62204006)Shenzhen Science and Technology Program(No.RCBS20231211090701006)+2 种基金Development and Reform Commission of Shenzhen Municipality(No.XMHT20220106002)Guangdong Key Laboratory of Flexible Optoelectronic Materials and Devices,Guangdong International Science Collaboration Base(No.2019A050505003)Shenzhen Key Laboratory of Organic Opto-electromagnetic Functional Materials of Shenzhen Science and Technology Plan(No.ZDSYS20140509094114164).
文摘Organic light-emitting transistors(OLETs)are gaining increasing attention as a promising candidate for nextgeneration display technology.However,due to the limited horizontal charge transport capability in OLETs,enhancing their optical performance remains greatly challenging.In this work,an effective strategy is employed to achieve highperformance OLETs by constructing a two-dimensional molecular-scale passivation layer at the dielectric/channel interface using a promising solution-processed small-molecule material,tetratetracontane(TTC).By controlling the microscopic flows driven by intermolecular interactions near the solution meniscus,molecular self-assembly dynamics are effectively regulated,contributing to a significant transformation in molecular layer stacking mode and enabling the formation of large-area TTC thin films with two-dimensional molecular-scale surface structure and uniform morphology.The introduction of high-quality TTC passivation layer film into the dielectric/channel interface optimizes the film morphologies of overlying channel layer,effectively shields the electrostatic dipole effects at dielectric/channel interface,leading to the synergistic optoelectronic regulation and enhanced optical properties of OLETs.Consequently,high brightness of 10,077.3 cd·m^(-2),high external quantum efficiency(EQE)of 20.46%,and low voltage of 15 V are achieved in the lateral OLET.This work presents a promising approach for two-dimensional molecular-scale small molecule interfaces,and provides an effective strategy for achieving high-performance OLET devices.
文摘Designing high-efficiency photocatalysts by the construction of organic/inorganic heterojunctions is considered to be an effective approach for improving photocatalytic hydrogen evolution reaction(HER)activity.This work designed and built unique S-scheme heterojunctions by in-situ growing inorganic WO_(3) nanoparticles with excellent oxidation ability on fused-sulfone-modified covalent organic frameworks(FS-COF)with strong reduction ability.It is found that FS-COF and WO_(3) have a well-matched staggered band alignment.The best-designed FS-COF/WO_(3)-20%exhibits a maximum photocatalytic HER rate of 24.7 mmol g^(-1) h^(-1) under visible light irradiation,which is 1.4 times greater than the pure FS-COF.Moreover,photogenerated electron-hole pairs can be separated and utilized more efficiently thanks to the FS-COF/WO_(3) heterojunction's ability to create a favorable internal electric field resulting from the difference in work functions between FS-COF and WO_(3),which speeds up the transfer dynamics of photoinduced electrons from WO_(3) to FS-COF through an additional interfacial electron-transfer channel obeying the directional S-scheme migration mechanism.Furthermore,the S-scheme migration mechanism of photoinduced charge carriers instead of the type-II mechanism was confirmed by the signal intensity of•O_(2)−species from spin-trapping electron paramagnetic resonance spectra over the single component and the formed heterojunction.It ensures the photoexcited electrons maintain on the lowest unoccupied molecular orbital of FS-COF with a strong reduction ability to participate in photocatalytic HER,resulting in a significantly boosted H_(2) evolution rate.Based on organic/inorganic coupling,this work offers a strategy for creating particular S-scheme heterojunction photocatalysts.
基金supported by the National Natural Science Foundation of China(42030804,42330811)the“Deep-time Digital Earth”Science and Technology Leading Talents Team Funds for the Central Universities for the Frontiers Science Center for Deep-time Digital Earth,China University of Geosciences(Fundamental Research Funds for the Central Universities,grant number:2652023001).
文摘The water adsorption performance of shale gas reservoirs is a very important factor affecting their gas in place(GIP)contents,but the water-holding capacity and mechanism of over-mature shale,especially organic pores,are still not fully understood.In this study,systematic water vapor adsorption(WVA)experiments were carried out on the Lower Cambrian over-mature shale and its kerogen from the Sichuan Basin,China to characterize their WVA behaviors,and combined with the low-pressure gas(N_(2) and CO_(2))adsorption experiments,the main influencing factors of WVA capacity of the shale and the absorbed-water distribution in its organic and inorganic nanopores were investigated.The results show that the WVA isotherms of shale and kerogen are all typeⅡ,with an obvious hysteresis loop in the multilayer adsorption range,and that the positive relationship of the shale TOC content with the WVA capacity(including total adsorption capacity,primary adsorption capacity and secondary adsorption capacity)and WVA hysteresis index(AHIW),and the greater adsorption capacity and AHIW of kerogen than the shale,all indicate that the hydrophilicity of organic matter(OM)in the over-mature shale was underestimated in previous research.Although both the shale OM and clay minerals have a significant positive effect on the WVA,the former has a stronger adsorption ability than the latter.The WVA capacity of the studied Lower Cambrian shale is significantly greater than that of the Longmaxi shale reported in literatures,which was believed to be mainly attributed to its higher maturity,with a significant graphitization of OM.The shale micropores and non-micropores play an important role in WVA,especially OM pores.There are primary and secondary adsorption for water vapor in both the micropores and non-micropores of OM,while these adsorptions of minerals mainly occur in their non-micropores.These results have important guides for understanding the gas storage mechanism and exploration and development potential of marine over-mature shale in southern China,especially the Lower Cambrian shale.
基金The Major Science and Technology Plan of Hainan Province under contract No.ZDKJ2021008the Hainan Provincial Natural Science Foundation of China under contract No.623RC456+1 种基金the Hainan Province Science and Technology Special Fund under contract Nos ZDYF2021SHFZ064 and ZDYF2022SHFZ056the Collaborative Innovation Center of Marine Science and Technology in Hainan University under contract No.XTCX2022HYC19.
文摘The exchange of inorganic nutrients at the coastal sediment-water interface(SWI)plays a crucial role in regulating the nutrient budget in overlying water.The related studies mainly focus on the mid-to high-latitude regions,leaving a significant gap in the quantitative assessment of nutrient exchange and environmental controls at the SWI in lowlatitude coastal regions.We quantitatively assess the exchange of inorganic nutrients at the SWI in three tropical bays(Dongzhai Harbor,Xiaohai Lagoon,Qinglan Harbor).Sediments act as a source of ammonium,phosphate,and silicate,but for nitrate,sediments can be both a source and sink,although with substantial spatial and temporal variations in their fluxes.Labile organic matter is a critical regulator for the fluxes of inorganic nutrients at the SWI.The sedimentary nutrients input with high N/P molar ratio will alter the nutrient stoichiometry to mitigate the nitrogen limitation in coastal waters.However,the internal sediment release in these tropical bays plays a relative weak role in contributing to the nutrient addition in comparison with the other external nutrient sources including riverine input,submarine groundwater discharge,and atmospheric deposition.According to the global compilation on SWI nutrient fluxes,we propose that water column primary production and external inputs to interpret the variation in exchange and fluxes of nutrients at the SWI in different ecosystems.Such a conceptual understanding of these chain biogeochemical processes involving external nutrient input,primary production,particulate organic matter settling,and the accumulation and release of inorganic nutrients in sediments will be helpful for the scientific-based pollution prevent and control in coastal waters.
基金financially supported by the National Natural Science Foundation of China (No.52471166)the Central South University Graduate-Student Autonomous Exploration Innovative Programme (No.2024ZZTS0373)
文摘High-energy-density lithium metal batteries hold great promise for advancing low-altitude economic development.However,the practical application of ultrathin lithium anodes remains challenging due to significant interfacial side reactions,dendrite formation,and substantial volume fluctuations.In this study,lithium metal electrodes were fabricated using a spin-coating process,enabling an in situ reaction between lithium and phenyl disulfide(PDS).The resulting robust organic sulfurization interface,composed of lithium thiophenoxide,facilitates rapid lithium-ion transport and effectively suppresses dendrite formation.Symmetric cells with a 50μm Li@PDS anode exhibited an impressive lifespan exceeding3000 h at 1 mA cm^(-2)and 1 mAh cm^(-2).The Li@PDS anode demonstrated excellent structural stability in a practical LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)lILi@PDS pouch cell,maintaining 94.8%of its initial capacity(1.45 Ah)over 260 cycles at a 0.4C rate and 87.30%of its initial capacity(1.1 Ah)over 360 cycles at a 2C rate(1C=200 mA g^(-1)).This work provides a promising pathway for developing durable lithium metal anodes suitable for scalable practical applications.
基金financially supported by the National Natural Science Foundation of China(52472248 and 22075221)the Key Research and Development Project of Shanxi Province(202202060301003 and 202202060301015)the Innovation Program of Wuhan-Shuguang Project(2023010201020367)。
文摘Poly(3-hexylthiophene)(P3HT)is one of the most promising hole-transporting materials in the pursuit of efficient and stable perovskite solar cells due to its outstanding stability and low cost.However,the intrinsic low carrier density of P3 HT and poor contact between the P3HT/perovskite interface always lead to a low performance of the solar cell,while conventional chemical doping always makes the films unstable and limits the scalability.In this work,for the first time,we simultaneously enhanced the hole transporting properties of P3HT film and the interface of perovskite by doping it with a judiciously designed oxidized small molecule organic semiconductor.The organic salt not only can promote the lamellar crystallinity of P3HT to obtain better charge transport properties,but also reduce the defects of perovskite.As a result,we achieved champion efficiencies of 23.0%for small-area solar cells and 18.8%for larger-area modules(48.0 cm^(2)).This efficiency is the highest value for P3HT-based perovskite modules.Moreover,the solar cells show excellent operational stability,retaining over 95%of their initial efficiencies after1200 h of continuous operation.
基金financially supported partly by the National Key Research and Development Program of China(2018YFE0111600)the Tianjin Sci.&Tech.Program(17YFZCGX00560)the Young Elite Scientists Sponsorship Program by Tianjin(TJSQNTJ-2017-05)。
文摘Lithium metal is one of the most promising anodes for next-generation batteries due to its high capacity and low reduction potential.However,the notorious Li dendrites can cause the short life span and safety issues,hindering the extensive application of lithium batteries.Herein,Li_(7)La_(3)Zr_(2)O_(12)(LLZO)ceramics are integrated into polyethylene oxide(PEO)to construct a facile polymer/inorganic composite solid-state electrolyte(CSSE)to inhibit the growth of Li dendrites and widen the electrochemical stability window.Given the feasibility of our strategy,the designed PEO-LLZO-LiTFSI composite solid-state electrolyte(PLLCSSE)exhibits an outstanding cycling property of 134.2 mAh g^(-1) after 500 cycles and the Coulombic efficiency of 99.1%after 1000 cycles at 1 C in LiFePO_(4)-Li cell.When cooperated with LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622)cathode,the PLL-CSSE renders a capacity retention of 82.4%after 200 cycles at 0.2 C.More importantly,the uniform dispersion of LLZO in PEO matrix is tentative tested via Raman and FT-IR spectra and should be responsible for the improved electrochemical performance.The same conclusion can be drawn from the interface investigation after cycling.This work presents an intriguing solid-state electrolyte with high electrochemical performance,which will boost the development of all-solid-state lithium batteries with high energy density.
文摘All-solid-state batteries potentially exhibit high specific energy and high safety,which is one of the development directions for nextgeneration lithium-ion batteries.The compatibility of all-solid composite electrodes with high-nickel layered cathodes and inorganic solid electrolytes is one of the important problems to be solved.In addition,the interface and mechanical problems of high-nickel layered cathodes and inorganic solid electrolyte composite electrodes have not been thoroughly addressed.In this paper,the possible interface and mechanical problems in the preparation of high-nickel layered cathodes and inorganic solid electrolytes and their interface reaction during charge–discharge and cycling are reviewed.The mechanical contact problems from phenomena to internal causes are also analyzed.Uniform contact between the high-nickel cathode and solid electrolyte in space and the ionic conductivity of the solid electrolyte are the prerequisites for the good performance of a high-nickel layered cathode.The interface reaction and contact loss between the high-nickel layered cathode and solid electrolyte in the composite electrode directly affect the passage of ions and electrons into the active material.The buffer layer constructed on the high-nickel cathode surface can prevent direct contact between the active material and electrolyte and slow down their interface reaction.An appropriate protective layer can also slow down the interface contact loss by reducing the volume change of the high-nickel layered cathode during charge and discharge.Finally,the following recommendations are put forward to realize the development vision of high-nickel layered cathodes:(1)develop electrochemical systems for high-nickel layered cathodes and inorganic solid electrolytes;(2)elucidate the basic science of interface and electrode processes between high-nickel layered cathodes and inorganic solid electrolytes,clarify the mechanisms of the interfacial chemical and electrochemical reactions between the two materials,and address the intrinsic safety issues;(3)strengthen the development of research and engineering technologies and their preparation methods for composite electrodes with high-nickel layered cathodes and solid electrolytes and promote the industrialization of all-solid-state batteries.
基金supported by the National Natural Science Foundation of China(52303239,51933001,22475114)the Natural Science Foundation of Shandong Province(ZR2022QB141,2023HWYQ-087)+1 种基金the Shanghai Pujiang Program(23PJ1409700)the Hubei Province Key Research Program(2023BAB109)。
文摘The self-assembled monolayer(SAM),functioning as a hole transport layer,holds the potential to substantially elevate the efficiency of perovskite and organic solar cells.Nevertheless,incomplete SAM coverage may result in interface defects lurking between the photovoltaic layer and the electrode,thereby causing non-radiative recombination losses of interfacial charges.To tackle this issue,we introduced 4-bromobutyric acid to co-assemble with the SAM,yielding a more compact co-assembled monolayer(co-SAM)that effectively repairs these defective zones.Confocal laser scanning microscopy and Kelvin Probe Force Microscopy show that co-SAMs successfully mitigate interface defects in the previously uncovered electrode regions.Furthermore,the work function of the electrodes is elevated to 5.6 eV,facilitating efficient hole extraction.Consequently,devices incorporating co-SAMs exhibit notably reduced non-radiative recombination losses.The power conversion efficiency(PCE)of the devices is enhanced to 20.0% in binary organic solar cells,and an even more remarkable breakthrough PCE of 25.8% is achieved in perovskite/organic tandem devices.This study introduces a straightforward strategy to improve the hole-selective contact of electrodes,ultimately boosting the overall efficiency of the devices.
文摘Doping is essential for modulating semiconductor conductivity,forming p-n junctions,and reducing contact resistance[1].Notably,as organic semiconductors(OSCs)advance toward high performance,flexibility,and miniaturization,achieving precise regionally selective doping becomes critical for building complex,highly integrated devices[2].In inorganic semiconductors(e.g.,silicon),sub-100-nanometer regional doping is achievable through photolithography and ion implantation—techniques foundational to modern complementary metaloxide-semiconductor(CMOS)technology[3].
