Significant progress has been achieved in the field of organic solar cells(OSCs). Most devices with power conversion efficiencies(PCEs) exceeding 20% rely predominantly on active materials that incorporate D18 or its ...Significant progress has been achieved in the field of organic solar cells(OSCs). Most devices with power conversion efficiencies(PCEs) exceeding 20% rely predominantly on active materials that incorporate D18 or its derivatives as the donor. In contrast, the PCEs over 20% have been realized as well for OSCs with the non-D18-based donor materials by simultaneously optimizing material properties, active layer morphologies and interface engineering, thereby demonstrating the potential to outperform D18 counterparts. Therefore, this review summarizes an overview of recent advancements in OSCs with the PCEs over20% utilizing the non-D18-based donor materials, and highlights three critical aspects including molecular design strategies,the active layer morphologies, and the interface optimization. Their synergistic roles are advantageous in enhancing the exciton dissociation, facilitating the charge transport, and suppressing the recombination losses, accordingly supporting the improved PCEs over 20%. Furthermore, the challenges and valuable insights are discussed, which can lead to improved efficiency, scalable fabrication, and enhanced environmental and thermal stability, potentially accelerating the commercialization of OSCs.展开更多
Sulfide-based all-solid-state lithium batteries(ASSLBs) with nickel-rich oxide cathodes are emerging as primary contenders for the next generation rechargeable batteries,owing to their superior safety and energy densi...Sulfide-based all-solid-state lithium batteries(ASSLBs) with nickel-rich oxide cathodes are emerging as primary contenders for the next generation rechargeable batteries,owing to their superior safety and energy density.However,the all-solid-state batteries with nickel-rich oxide cathodes suffer from performance degradation due to the reactions between the highly reactive surface oxygen of the cathode and the electrolyte,as well as the instability of the bulk oxygen structure in the cathode.Herein,we propose a synergistic modification design scheme to adjust the oxygen activity from surface to bulk.The LiBO_(2)coating inhibits the reactivity of surface lattice oxygen ions.Meanwhile,Zr doping in the bulk phase forms strong Zr-O covalent bonds that stabilize the bulk lattice oxygen structure.The synergistic effect of these modifications prevents the release of oxygen,thus avoiding the degradation of the cathode/SE interface.Additionally,the regulation of surface-to-bulk oxygen activity establishes a highly stable interface,thereby enhancing the lithium ion diffusion kinetics and mechanical stability of the cathode.Consequently,cathodes modified with this synergistic strategy exhibit outstanding performance in sulfide-based ASSLBs,including an ultra-long cycle life of 100,000 cycles,ultra-high rate capability at 45C,and 85% high active material content in the composite cathode.Additionally,ASSLB exhibits stable cycling under high loading conditions of 82.82 mg cm^(-2),achieving an areal capacity of 17.90 mA h cm^(-2).These encouraging results pave the way for practical applications of ASSLBs in fast charging,long cycle life,and high energy density in the future.展开更多
Perovskite solar cells(PSCs)based onα-phase FAPbI_(3)(α-FAPbI_(3))microcrystals precursor outperform those withδ-phase mi-crocrystals due to their superior crystallinity and fewer defects,makingα-phase microcrysta...Perovskite solar cells(PSCs)based onα-phase FAPbI_(3)(α-FAPbI_(3))microcrystals precursor outperform those withδ-phase mi-crocrystals due to their superior crystallinity and fewer defects,makingα-phase microcrystals precursor more advantageous for high-per-formance PSCs.However,most reported synthesis methods of perovskite microcrystals,especially for aqueous synthesis,fail to reach the energy threshold required forα-phase transformation and therefore exhibit theδphase.In this study,we introduce a novel aqueous syn-thesis method to fabricateα-FAPbI_(3) microcrystals.Our approach overcomes the energy barrier by properly heating the reaction system,enabling the direct formation ofα-FAPbI_(3) in water.This direct one-step aqueous synthesis route yieldsα-FAPbI_(3) microcrystals with su-perior phase purity,crystallinity,and minimal defect density.Combined with green anti-solvent,the high-qualityα-FAPbI_(3) microcrystals serving as exceptional precursors endow perovskite films with reduced nonradiative recombination.The PSC achieves a remarkable power conversion efficiency(PCE)of 24.43%,which is one of the highest PCE reports for using the green anti-solvent in ambient air condition.This aqueous synthesis approach shows a significant potential for scalable production of high-performance PSCs.展开更多
The effective reuse of iron phosphate residue(IPR)is the key issue in the recycling of spent LiFePO_(4)batteries.Therefore,in this study,the reduction leaching of IPR in H_(2)SO_(4)solution by adding iron powder as re...The effective reuse of iron phosphate residue(IPR)is the key issue in the recycling of spent LiFePO_(4)batteries.Therefore,in this study,the reduction leaching of IPR in H_(2)SO_(4)solution by adding iron powder as reducing agent was investigated and compared with direct leaching.The results show that the leaching rate of IPR reached 97%under the optimum reduction leaching conditions.Kinetic studies show that the activation energy for reduction leaching is 12.71 k J/mol,while that of direct leaching is 21.57 k J/mol.Moreover,the reduction leaching time is reduced by half and the acid consumption is reduced by 30% compared to direct leaching with the same leaching rate.This work provides a scientific guidance to the treatment of iron phosphate residue from the recycling of spent LiFePO_(4)batteries.展开更多
Lithium metal anode has become a favorable candidate for next-generation rechargeable batteries.However, the unstable interface between lithium metal and electrolyte leads to the growth of dendrites,resulting in the l...Lithium metal anode has become a favorable candidate for next-generation rechargeable batteries.However, the unstable interface between lithium metal and electrolyte leads to the growth of dendrites,resulting in the low Coulombic efficiency and even the safety concerns. Herein, a rigid-flexible dual-layer vermiculite nanosheet(VN) based organic-inorganic hybrid film on lithium metal anode is proposed to suppress dendrite growth and relieve volume fluctuations. The inner mechanically robust VN layer(3 μm thick) enhances the mechanical properties of the protective layer, while the outer polymer(4 μm thick) can enhance the flexibility of the hybrid layer. The Li | Li symmetric cell with protected lithium shows an extended life of over 670 h. The full cell with Li anode protected by dual-layer interface exhibits a better capacity retention of 80% after 174 cycles in comparison to bare Li anode with 94 cycles.This study provides a novel approach and a significant step towards prolonging lifespan of lithium metal batteries.展开更多
Lithium(Li)metal anodes with the high theoretical specific capacity(3860 mAh g^(-1))and most negative reduction potential(-3.04 V vs.standard hydrogen electrode)have been considered as an ultimate choice for energy st...Lithium(Li)metal anodes with the high theoretical specific capacity(3860 mAh g^(-1))and most negative reduction potential(-3.04 V vs.standard hydrogen electrode)have been considered as an ultimate choice for energy storage devices with high energy density[1-4].However,the practical applications of Li metalbased batteries(LMBs)are confronted with two tough issues:Li dendrite growth induced by uneven Li depositions and unstable solid electrolyte interphase(SEI)(Fig.1a)[5,6].展开更多
After fast developing of single-junction perovskite solar cells and organic solar cells in the past 10 years,it is becoming harder and harder to improve their power conversion efficiencies.Tandem solar cells are recei...After fast developing of single-junction perovskite solar cells and organic solar cells in the past 10 years,it is becoming harder and harder to improve their power conversion efficiencies.Tandem solar cells are receiving more and more attention because they have much higher theoretical efficiency than single-junction solar cells.Good device performance has been achieved for perovskite/silicon and perovskite/perovskite tandem solar cells,including 2-terminal and 4-terminal structures.However,very few studies have been done about 4-terminal inorganic perovskite/organic tandem solar cells.In this work,semi-transparent inorganic perovskite solar cells and organic solar cells are used to fabricate 4-terminal inorganic perovskite/organic tandem solar cells,achieving a power conversion efficiency of 21.25%for the tandem cells with spin-coated perovskite layer.By using drop-coating instead of spin-coating to make the inorganic perovskite films,4-terminal tandem cells with an efficiency of 22.34%are made.The efficiency is higher than the reported 2-terminal and 4-terminal inorganic perovskite/organic tandem solar cells.In addition,equivalent 2-terminal tandem solar cells were fabricated by connecting the sub-cells in series.The stability of organic solar cells under continuous illumination is improved by using semi-transparent perovskite solar cells as filter.展开更多
Sulfide-based all-solid-state batteries(ASSBs)exhibit unparalleled application value due to the high ionic conductivity and good processability of sulfide solid electrolytes(SSEs).Carbon-based conductive agents(CAs)are ...Sulfide-based all-solid-state batteries(ASSBs)exhibit unparalleled application value due to the high ionic conductivity and good processability of sulfide solid electrolytes(SSEs).Carbon-based conductive agents(CAs)are often used in the construction of electronic conductive networks to achieve rapid electron transfer.However,CAs accelerate the formation of decomposition products of SSEs,and their effects on sulfide-based ASSBs are not fully understood.Herein,the effect of CAs(super P,vaper-grown carbonfibers,and carbon nanotubes)on the performance of sulfide-based ASSBs is investigated under different cathode active materials mass loading(8 and 25 mg⋅cm^(-2)).The results show that under low mass loading,the side reaction between the CAs and the SSEs deteriorates the performance of the cell,while the charge transfer promotion caused by the addition of CAs is only manifested under high mass loading.Furthermore,the gradient design strategy(enrichment of CAs near the current collector side and depletion of CAs near the electrolyte side)is applied to maximize the benefits of CAs in electron transport and reduce the adverse effects of CAs.The charge carrier transport barrier inside the high mass loading electrode is significantly reduced through the regulation of electronic conductivity.Consequently,the optimized electrode achieves a high areal capacity of 5.6 mAh⋅cm^(-2)at high current density(1.25 mA⋅cm2,0.2℃)at 25℃with a capacity retention of 87.85%after 100 cycles.This work provides a promising way for the design of high-mass loading electrodes with practical application value.展开更多
Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells suffer from significant open-circuit voltage(V_(OC))deficits due to severe interfacial and bulk recombination,restricting their power conversion efficiency(PCE)far bel...Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells suffer from significant open-circuit voltage(V_(OC))deficits due to severe interfacial and bulk recombination,restricting their power conversion efficiency(PCE)far below the ShockleyQueisser limit.This work proposes a low-temperature annealing strategy during ITO sputtering(SA)to synergistically address these challenges.The temperature applied during ITO sputtering not only improves the crystallinity,carrier concentration,and optical transmittance of the ITO layer but also promotes the diffusion of In from ITO into both CdS and CZTSSe layers.Consequently,lattice matching at the CZTSSe/CdS interface is optimized,enabling epitaxial growth.And a favorable ITO/In:CdS/In&Cd:CZTSSe structure with optimal band alignment is obtained.As a result,a champion device with a PCE of 1_(4).29%was achieved.The SA-treating also enabled the CZTSSe solar cells to achieve the highest V_(OC)reported to date,exceeding 590 mV.This underscores the essential role of SA processing in optimizing interface engineering and suppressing defects,thus promoting the development of low-cost,high-performance kesterite photovoltaics.展开更多
All-solid-state batteries(ASSBs)are considered to be the most promising candidates for improving battery safety and energy density.Sulfide electrolytes have a narrow electrochemical window,which hinders their applicat...All-solid-state batteries(ASSBs)are considered to be the most promising candidates for improving battery safety and energy density.Sulfide electrolytes have a narrow electrochemical window,which hinders their applications coupled with high-voltage cathodes.Halide electrolytes with high-voltage endurance can help solve this problem.Herein,the combination of spraying and slurry-coating methods was adopted as a practical route to process a free-standing Li_(6)PS_5Cl(LPSCl)asymmetrical electrolyte membrane(19.23Ωcm~2,75μm)decorated with a 10μm Li_(3)In Cl_(6)(LICl)layer.The LICl-LPSCl asymmetrical electrolyte membranes enhanced the high-voltage stabilities to match those of LiNi_(0.83)Co_(0.11)Mn_(0.06)O_(2)(NCM811)and Li_(1.2)Ni_(0.13)Co_(0.13)Mn_(0.54)O_(2)(LRMO)cathodes.The NCM811|LICl-LPSCl|n Si ASSB achieved an initial coulombic efficiency(ICE)of 85.13%and a capacity retention of 77.16%after 200 cycles.Compared with the LPSCl membrane,the LICl-LPSCl membrane displayed high stability with the LRMO cathode as the charging cut-off voltage increased to 4.7 V,which improved the initial charge capacity from 143 to 270 mAh g^(-1)and achieved stable cycling of 160 m Ah g^(-1)at 0.5 C.Additionally,we attempted continuous LICl-LPSCl membrane production and utilized the product to fabricate a pouch-type ASSB based on LRMO.The fabrication of the LICl-LPSCl electrolyte membrane demonstrated its potential for controllable and industryadaptable applications in ASSBs.展开更多
In perovskite solar cells(PSCs)with a wide bandgap(E_(g)≥1.65 eV),mixed halides generate poor-quality perovskite films and lead to a low power conversion efficiency(PCE)due to uncontrolled fast perovskite crystalliza...In perovskite solar cells(PSCs)with a wide bandgap(E_(g)≥1.65 eV),mixed halides generate poor-quality perovskite films and lead to a low power conversion efficiency(PCE)due to uncontrolled fast perovskite crystallization.Herein,we propose a strategy to regulate the grain growth of perovskite wet films by fumigating them in a dimethyl sulfoxide(DMSO)atmosphere.Due to the better coordination of DMSO with lead halides and organic halides,DMso fumigation effectively prolongs the existence time of intermediate phases,which slows the crystallization of perovskites,generating perovskite flms with large grains and a low defect density.Such high-quality perovskite flms were used to fabricate 1.65-evand 1.68-eV-bandgap PSCs,which achieved champion PCEs of 23.19%and 22.38%,respectively.The former PsC showed a V_(oc)deficit of o.391 V,representing one of the state-of-the-art performances for this bandgap.Monolithic perovskite/tunnelling oxide passivating contact(TOPCon)tandem solar cells(TSCs)were also fabricated using the optimized PSCs as front cells,achieving a champion PCE of 30.9%(certified 30.83%).This study demonstrates an easy-to-operate and effective approach to realize highperformance wide-bandgap PSCs and perovskite/TOPCon TSCs.展开更多
Organic-inorganic perovskite (ABX3) solar cells (PSCs) have attracted wide interest in recent years (1)The power conversion efficiency (PCE) has increased up to 23.7%(NREL Best Research-Cell Efficiency Chart, https://...Organic-inorganic perovskite (ABX3) solar cells (PSCs) have attracted wide interest in recent years (1)The power conversion efficiency (PCE) has increased up to 23.7%(NREL Best Research-Cell Efficiency Chart, https://www.nrel.gov/pv/cell-efficiency.html.展开更多
Organic-inorganic lead halide perovskite solar cells(PSCs)have been marching rapidly in recent years with power conversion efficiency(PCE)boosting from 3.8%to 24.2%(NREL Best Research-Cell Efficiency Chart,https://www...Organic-inorganic lead halide perovskite solar cells(PSCs)have been marching rapidly in recent years with power conversion efficiency(PCE)boosting from 3.8%to 24.2%(NREL Best Research-Cell Efficiency Chart,https://www.nrel.gov/pv/cell-effi ciency.html,Accessed April 2019).However,these solar cells are not stable at high temperatures due to volatile organic cations[1].Allinorganic perovskites with cesium cation like CsPbI1-xBrx present high thermal stabilities[2].By partially replacing I-with Br-,the bandgap for CsPbI1-xBrx can be tuned from 1.73 to 2.36 eV.展开更多
The power conversion efficiency for single-junction solar cells is limited by the Shockley-Quiesser limit.An effective approach to realize high efficiency is to develop multi-junction cells.These years have witnessed ...The power conversion efficiency for single-junction solar cells is limited by the Shockley-Quiesser limit.An effective approach to realize high efficiency is to develop multi-junction cells.These years have witnessed the rapid development of organic–inorganic perovskite solar cells.The excellent optoelectronic properties and tunable bandgaps of perovskite materials make them potential candidates for developing tandem solar cells,by combining with silicon,Cu(In,Ga)Se_(2)and organic solar cells.In this review,we present the recent progress of perovskite-based tandem solar cells,including perovskite/silicon,perovskite/perovskite,perovskite/Cu(In,Ga)Se_(2),and perovskite/organic cells.Finally,the challenges and opportunities for perovskite-based tandem solar cells are discussed.展开更多
Over the past decades,the emergence of photovoltaics(PV)alleviates the energy crisis and environmental pollution of fossil fuels.Compared to the large-scale silicon-based PV technology,thin-film PV technology is still...Over the past decades,the emergence of photovoltaics(PV)alleviates the energy crisis and environmental pollution of fossil fuels.Compared to the large-scale silicon-based PV technology,thin-film PV technology is still just a newcomer.展开更多
Kesterite Cu2ZnSn(S,Se)4(CZTSSe)is one of the most promising next-generation thin-film photovoltaic materials due to its environmental friendliness and earthabundant constitutions,excellent optoelectronic properties(h...Kesterite Cu2ZnSn(S,Se)4(CZTSSe)is one of the most promising next-generation thin-film photovoltaic materials due to its environmental friendliness and earthabundant constitutions,excellent optoelectronic properties(high absorption coefficient>104/cm and tunable band gap 1.0–1.5 eV)and high theoretical efficiency(32%).1,2 In 2014,12.6%3 efficiency was achieved by the IBM group using the hydrazine method.Based on the sputtering process,12.62%4 efficiency for CZTSSe and 12.5%5 efficiency for CZTSe have been achieved in recent years.However,the highest efficiency has stuck around 12.6%for several years.Lately,a breakthrough with certified 13%power conversion efficiency(PCE)has been demonstrated for CZTSSe thin-film solar cells,surpassing the dust-covered efficiency record since 2014.3,6 Along with the efficiency advancement of kesterite solar cells,a cost-effective fabrication process with low carbon footprint plays an increasingly important role considering the near-future industrialisation of this kind of solar cell with low energy payback time.展开更多
Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)thin films are attractive due to environmental-friendly and earth-abundant constituents,and superior optoelectronic properties such as high absorption coeffi-cient and tunable ban...Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)thin films are attractive due to environmental-friendly and earth-abundant constituents,and superior optoelectronic properties such as high absorption coeffi-cient and tunable bandgaps(1.0-1.5 eV).In the past several years,profound progress has been made in CZTSSe via addressing the issues of massive deep defects[1,2],severe band tailing[3],uncon-trollable grain growth[4,5].and unoptimized interfaces[6,7].展开更多
In recent years,all-inorganic perovskite solar cells(PSCs)have attracted tremendous interest due to their excellent thermal stability[1-3].Unlike organic-inorganic halide perovskites,whose organic component is volatil...In recent years,all-inorganic perovskite solar cells(PSCs)have attracted tremendous interest due to their excellent thermal stability[1-3].Unlike organic-inorganic halide perovskites,whose organic component is volatile at temperatures higher than 2000C,all-inorganic perovskites can tolerate temperatures over 400℃without deterioration[4].However,the power conversion efficiency(PCE)for all-inorganic PSCs is much lower than that of organic-inorganic halide PSCs mainly due to its wider bandgap,which leads to limited light absorption and low short-circuit current density(Jsc).At present,the most studied all-inorganic perovskites are CsPbI3 and CsPbI2Br.Partly replacing I with Br can decrease the preparation temperature,but the bandgap will increase[5,6].To improve the performance of inorganic PSCs,many researches focused on crystallinity control and interfacial engineering[7-10].Few works were done to broaden the photoresponse to improve Jsc,thus improving the PCE.Developing tandem or integrated solar cells is an effective approach to make full use of sunlight[11,12].For tandem solar cells,the preparation process is very complicated.展开更多
Over the past few years, there have been significant advancements in uncovering previously sealed records in the kesterite solar cell. This also has led to substantial growth marked by multiple groups achieving succes...Over the past few years, there have been significant advancements in uncovering previously sealed records in the kesterite solar cell. This also has led to substantial growth marked by multiple groups achieving successive efficiency breakthroughs, shining a renewed spotlight on this promising photovoltaic material that had previously been overlooked due to its low efficiency.展开更多
基金support from the National Key Research and Development Program of China (2022YFB3803300)the National Natural Science Foundation of China (U23A20138 and 52173192)Hunan Provincial Major Basic Research Project (2025JC0004)。
文摘Significant progress has been achieved in the field of organic solar cells(OSCs). Most devices with power conversion efficiencies(PCEs) exceeding 20% rely predominantly on active materials that incorporate D18 or its derivatives as the donor. In contrast, the PCEs over 20% have been realized as well for OSCs with the non-D18-based donor materials by simultaneously optimizing material properties, active layer morphologies and interface engineering, thereby demonstrating the potential to outperform D18 counterparts. Therefore, this review summarizes an overview of recent advancements in OSCs with the PCEs over20% utilizing the non-D18-based donor materials, and highlights three critical aspects including molecular design strategies,the active layer morphologies, and the interface optimization. Their synergistic roles are advantageous in enhancing the exciton dissociation, facilitating the charge transport, and suppressing the recombination losses, accordingly supporting the improved PCEs over 20%. Furthermore, the challenges and valuable insights are discussed, which can lead to improved efficiency, scalable fabrication, and enhanced environmental and thermal stability, potentially accelerating the commercialization of OSCs.
基金financially supported by the National Natural Science Foundation of China (52474338,22109084 and 52304338)the Hunan Provincial Key Research and Development Program (2024JK2093,2023GK2016)supported in part by the High Performance Computing Center of Central South University.
文摘Sulfide-based all-solid-state lithium batteries(ASSLBs) with nickel-rich oxide cathodes are emerging as primary contenders for the next generation rechargeable batteries,owing to their superior safety and energy density.However,the all-solid-state batteries with nickel-rich oxide cathodes suffer from performance degradation due to the reactions between the highly reactive surface oxygen of the cathode and the electrolyte,as well as the instability of the bulk oxygen structure in the cathode.Herein,we propose a synergistic modification design scheme to adjust the oxygen activity from surface to bulk.The LiBO_(2)coating inhibits the reactivity of surface lattice oxygen ions.Meanwhile,Zr doping in the bulk phase forms strong Zr-O covalent bonds that stabilize the bulk lattice oxygen structure.The synergistic effect of these modifications prevents the release of oxygen,thus avoiding the degradation of the cathode/SE interface.Additionally,the regulation of surface-to-bulk oxygen activity establishes a highly stable interface,thereby enhancing the lithium ion diffusion kinetics and mechanical stability of the cathode.Consequently,cathodes modified with this synergistic strategy exhibit outstanding performance in sulfide-based ASSLBs,including an ultra-long cycle life of 100,000 cycles,ultra-high rate capability at 45C,and 85% high active material content in the composite cathode.Additionally,ASSLB exhibits stable cycling under high loading conditions of 82.82 mg cm^(-2),achieving an areal capacity of 17.90 mA h cm^(-2).These encouraging results pave the way for practical applications of ASSLBs in fast charging,long cycle life,and high energy density in the future.
基金financially supported by the National Key Research and Development Program of China(No.2022YFB3803300)the Major Scientific and Technological Project in 2022 of Changsha,China(No.kq2301002).
文摘Perovskite solar cells(PSCs)based onα-phase FAPbI_(3)(α-FAPbI_(3))microcrystals precursor outperform those withδ-phase mi-crocrystals due to their superior crystallinity and fewer defects,makingα-phase microcrystals precursor more advantageous for high-per-formance PSCs.However,most reported synthesis methods of perovskite microcrystals,especially for aqueous synthesis,fail to reach the energy threshold required forα-phase transformation and therefore exhibit theδphase.In this study,we introduce a novel aqueous syn-thesis method to fabricateα-FAPbI_(3) microcrystals.Our approach overcomes the energy barrier by properly heating the reaction system,enabling the direct formation ofα-FAPbI_(3) in water.This direct one-step aqueous synthesis route yieldsα-FAPbI_(3) microcrystals with su-perior phase purity,crystallinity,and minimal defect density.Combined with green anti-solvent,the high-qualityα-FAPbI_(3) microcrystals serving as exceptional precursors endow perovskite films with reduced nonradiative recombination.The PSC achieves a remarkable power conversion efficiency(PCE)of 24.43%,which is one of the highest PCE reports for using the green anti-solvent in ambient air condition.This aqueous synthesis approach shows a significant potential for scalable production of high-performance PSCs.
基金financial support from the Hunan Provincial Natural Science Foundation,China(No.2022JJ10074)。
文摘The effective reuse of iron phosphate residue(IPR)is the key issue in the recycling of spent LiFePO_(4)batteries.Therefore,in this study,the reduction leaching of IPR in H_(2)SO_(4)solution by adding iron powder as reducing agent was investigated and compared with direct leaching.The results show that the leaching rate of IPR reached 97%under the optimum reduction leaching conditions.Kinetic studies show that the activation energy for reduction leaching is 12.71 k J/mol,while that of direct leaching is 21.57 k J/mol.Moreover,the reduction leaching time is reduced by half and the acid consumption is reduced by 30% compared to direct leaching with the same leaching rate.This work provides a scientific guidance to the treatment of iron phosphate residue from the recycling of spent LiFePO_(4)batteries.
基金supported by National Natural Science Foundation of China (22179070, U1932220)。
文摘Lithium metal anode has become a favorable candidate for next-generation rechargeable batteries.However, the unstable interface between lithium metal and electrolyte leads to the growth of dendrites,resulting in the low Coulombic efficiency and even the safety concerns. Herein, a rigid-flexible dual-layer vermiculite nanosheet(VN) based organic-inorganic hybrid film on lithium metal anode is proposed to suppress dendrite growth and relieve volume fluctuations. The inner mechanically robust VN layer(3 μm thick) enhances the mechanical properties of the protective layer, while the outer polymer(4 μm thick) can enhance the flexibility of the hybrid layer. The Li | Li symmetric cell with protected lithium shows an extended life of over 670 h. The full cell with Li anode protected by dual-layer interface exhibits a better capacity retention of 80% after 174 cycles in comparison to bare Li anode with 94 cycles.This study provides a novel approach and a significant step towards prolonging lifespan of lithium metal batteries.
基金supported by National Key Research and Development Program,China(2016YFA0202500 and 2016YFA0200102)National Natural Science Foundation of China,China(21805161,21808124,U1932220)Fundamental Research Funds for the Central Universites of Central South University,China(2020zzts471)。
文摘Lithium(Li)metal anodes with the high theoretical specific capacity(3860 mAh g^(-1))and most negative reduction potential(-3.04 V vs.standard hydrogen electrode)have been considered as an ultimate choice for energy storage devices with high energy density[1-4].However,the practical applications of Li metalbased batteries(LMBs)are confronted with two tough issues:Li dendrite growth induced by uneven Li depositions and unstable solid electrolyte interphase(SEI)(Fig.1a)[5,6].
基金the National Key Research and Development Program of China (2017YFA0206600)the National Natural Science Foundation of China (51773045, 21772030, 51922032 and 21961160720)the Fundamental Research Funds for the Central Universities (2020CDJQY-A055) for financial support。
文摘Inorganic perovskites (CsPbX_3, X=halide anion), containing no volatile organic cations, exhibit better thermal stability than organic–inorganic hybrid perovskites~([1, 2]). Among inorganic perovskites,α-Cs Pb I3(cubic phase) possesses a relatively suitable bandgap of~1.7 eV. CsPbI_3 perovskite solar cells (PSCs) have demonstrated power conversion efficiencies (PCEs) over 20%~([3-5]).
基金We thank the National Key Research and Development Program of China(2022YFB3803300)the open research fund of Songshan Lake Materials Laboratory(2021SLABFK02)+1 种基金the National Natural Science Foundation of China(21961160720 and 52203217)the China Postdoctoral Science Foundation(2021M690805)for financial support.
文摘After fast developing of single-junction perovskite solar cells and organic solar cells in the past 10 years,it is becoming harder and harder to improve their power conversion efficiencies.Tandem solar cells are receiving more and more attention because they have much higher theoretical efficiency than single-junction solar cells.Good device performance has been achieved for perovskite/silicon and perovskite/perovskite tandem solar cells,including 2-terminal and 4-terminal structures.However,very few studies have been done about 4-terminal inorganic perovskite/organic tandem solar cells.In this work,semi-transparent inorganic perovskite solar cells and organic solar cells are used to fabricate 4-terminal inorganic perovskite/organic tandem solar cells,achieving a power conversion efficiency of 21.25%for the tandem cells with spin-coated perovskite layer.By using drop-coating instead of spin-coating to make the inorganic perovskite films,4-terminal tandem cells with an efficiency of 22.34%are made.The efficiency is higher than the reported 2-terminal and 4-terminal inorganic perovskite/organic tandem solar cells.In addition,equivalent 2-terminal tandem solar cells were fabricated by connecting the sub-cells in series.The stability of organic solar cells under continuous illumination is improved by using semi-transparent perovskite solar cells as filter.
基金supported by Hunan Provincial Science and Technology Department(No.2021JJ10058).
文摘Sulfide-based all-solid-state batteries(ASSBs)exhibit unparalleled application value due to the high ionic conductivity and good processability of sulfide solid electrolytes(SSEs).Carbon-based conductive agents(CAs)are often used in the construction of electronic conductive networks to achieve rapid electron transfer.However,CAs accelerate the formation of decomposition products of SSEs,and their effects on sulfide-based ASSBs are not fully understood.Herein,the effect of CAs(super P,vaper-grown carbonfibers,and carbon nanotubes)on the performance of sulfide-based ASSBs is investigated under different cathode active materials mass loading(8 and 25 mg⋅cm^(-2)).The results show that under low mass loading,the side reaction between the CAs and the SSEs deteriorates the performance of the cell,while the charge transfer promotion caused by the addition of CAs is only manifested under high mass loading.Furthermore,the gradient design strategy(enrichment of CAs near the current collector side and depletion of CAs near the electrolyte side)is applied to maximize the benefits of CAs in electron transport and reduce the adverse effects of CAs.The charge carrier transport barrier inside the high mass loading electrode is significantly reduced through the regulation of electronic conductivity.Consequently,the optimized electrode achieves a high areal capacity of 5.6 mAh⋅cm^(-2)at high current density(1.25 mA⋅cm2,0.2℃)at 25℃with a capacity retention of 87.85%after 100 cycles.This work provides a promising way for the design of high-mass loading electrodes with practical application value.
基金supported by the National Key Research and Development Program of China(2024YFB4205000)the National Natural Science Foundation of China(52525405,62504071,and 52572217)+1 种基金the Natural Science Foundation of Henan Province(252300421255 and242300420313)the Key Research Projects of Higher Education Institutions in Henan Province(24A430003)。
文摘Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells suffer from significant open-circuit voltage(V_(OC))deficits due to severe interfacial and bulk recombination,restricting their power conversion efficiency(PCE)far below the ShockleyQueisser limit.This work proposes a low-temperature annealing strategy during ITO sputtering(SA)to synergistically address these challenges.The temperature applied during ITO sputtering not only improves the crystallinity,carrier concentration,and optical transmittance of the ITO layer but also promotes the diffusion of In from ITO into both CdS and CZTSSe layers.Consequently,lattice matching at the CZTSSe/CdS interface is optimized,enabling epitaxial growth.And a favorable ITO/In:CdS/In&Cd:CZTSSe structure with optimal band alignment is obtained.As a result,a champion device with a PCE of 1_(4).29%was achieved.The SA-treating also enabled the CZTSSe solar cells to achieve the highest V_(OC)reported to date,exceeding 590 mV.This underscores the essential role of SA processing in optimizing interface engineering and suppressing defects,thus promoting the development of low-cost,high-performance kesterite photovoltaics.
基金financially supported by Hunan Provincial Key R&D Project(Grant No.2023GK2016)the National Key Research and Development Program of China(Grant No.2023YFC2909100)the National Natural Science Foundation of China(Grant Nos.52304376 and 22109084)。
文摘All-solid-state batteries(ASSBs)are considered to be the most promising candidates for improving battery safety and energy density.Sulfide electrolytes have a narrow electrochemical window,which hinders their applications coupled with high-voltage cathodes.Halide electrolytes with high-voltage endurance can help solve this problem.Herein,the combination of spraying and slurry-coating methods was adopted as a practical route to process a free-standing Li_(6)PS_5Cl(LPSCl)asymmetrical electrolyte membrane(19.23Ωcm~2,75μm)decorated with a 10μm Li_(3)In Cl_(6)(LICl)layer.The LICl-LPSCl asymmetrical electrolyte membranes enhanced the high-voltage stabilities to match those of LiNi_(0.83)Co_(0.11)Mn_(0.06)O_(2)(NCM811)and Li_(1.2)Ni_(0.13)Co_(0.13)Mn_(0.54)O_(2)(LRMO)cathodes.The NCM811|LICl-LPSCl|n Si ASSB achieved an initial coulombic efficiency(ICE)of 85.13%and a capacity retention of 77.16%after 200 cycles.Compared with the LPSCl membrane,the LICl-LPSCl membrane displayed high stability with the LRMO cathode as the charging cut-off voltage increased to 4.7 V,which improved the initial charge capacity from 143 to 270 mAh g^(-1)and achieved stable cycling of 160 m Ah g^(-1)at 0.5 C.Additionally,we attempted continuous LICl-LPSCl membrane production and utilized the product to fabricate a pouch-type ASSB based on LRMO.The fabrication of the LICl-LPSCl electrolyte membrane demonstrated its potential for controllable and industryadaptable applications in ASSBs.
基金supported by the National Key Research and Development Program of China(2022YFB3803300)Major Scientific and Technological Project of Changsha(kq2301002)。
文摘In perovskite solar cells(PSCs)with a wide bandgap(E_(g)≥1.65 eV),mixed halides generate poor-quality perovskite films and lead to a low power conversion efficiency(PCE)due to uncontrolled fast perovskite crystallization.Herein,we propose a strategy to regulate the grain growth of perovskite wet films by fumigating them in a dimethyl sulfoxide(DMSO)atmosphere.Due to the better coordination of DMSO with lead halides and organic halides,DMso fumigation effectively prolongs the existence time of intermediate phases,which slows the crystallization of perovskites,generating perovskite flms with large grains and a low defect density.Such high-quality perovskite flms were used to fabricate 1.65-evand 1.68-eV-bandgap PSCs,which achieved champion PCEs of 23.19%and 22.38%,respectively.The former PsC showed a V_(oc)deficit of o.391 V,representing one of the state-of-the-art performances for this bandgap.Monolithic perovskite/tunnelling oxide passivating contact(TOPCon)tandem solar cells(TSCs)were also fabricated using the optimized PSCs as front cells,achieving a champion PCE of 30.9%(certified 30.83%).This study demonstrates an easy-to-operate and effective approach to realize highperformance wide-bandgap PSCs and perovskite/TOPCon TSCs.
基金the National Key Research and Development Program of China (2017YFA0206600)the National Natural Science Foundation of China (51773045, 21572041 and 21772030) for financial support
文摘Organic-inorganic perovskite (ABX3) solar cells (PSCs) have attracted wide interest in recent years (1)The power conversion efficiency (PCE) has increased up to 23.7%(NREL Best Research-Cell Efficiency Chart, https://www.nrel.gov/pv/cell-efficiency.html.
基金National Key Research and Development Program of China (2017YFA0206600)the National Natural Science Foundation of China (51773045, 21572041 and 21772030) for financial support
文摘Organic-inorganic lead halide perovskite solar cells(PSCs)have been marching rapidly in recent years with power conversion efficiency(PCE)boosting from 3.8%to 24.2%(NREL Best Research-Cell Efficiency Chart,https://www.nrel.gov/pv/cell-effi ciency.html,Accessed April 2019).However,these solar cells are not stable at high temperatures due to volatile organic cations[1].Allinorganic perovskites with cesium cation like CsPbI1-xBrx present high thermal stabilities[2].By partially replacing I-with Br-,the bandgap for CsPbI1-xBrx can be tuned from 1.73 to 2.36 eV.
基金the National Natural Science Foundation of China(51773045,21772030,51922032,and 21961160720)for financial support。
文摘The power conversion efficiency for single-junction solar cells is limited by the Shockley-Quiesser limit.An effective approach to realize high efficiency is to develop multi-junction cells.These years have witnessed the rapid development of organic–inorganic perovskite solar cells.The excellent optoelectronic properties and tunable bandgaps of perovskite materials make them potential candidates for developing tandem solar cells,by combining with silicon,Cu(In,Ga)Se_(2)and organic solar cells.In this review,we present the recent progress of perovskite-based tandem solar cells,including perovskite/silicon,perovskite/perovskite,perovskite/Cu(In,Ga)Se_(2),and perovskite/organic cells.Finally,the challenges and opportunities for perovskite-based tandem solar cells are discussed.
基金financial support from the National Key Research and Development Program of China(2018YFE0203400)the National Key Research and Development Program of China(2017YFA0206600)+1 种基金the National Natural Science Foundation of China(U1902218)the National Natural Science Foundation of China(51773045,21772030,51922032,21961160720)for financial support。
文摘Over the past decades,the emergence of photovoltaics(PV)alleviates the energy crisis and environmental pollution of fossil fuels.Compared to the large-scale silicon-based PV technology,thin-film PV technology is still just a newcomer.
文摘Kesterite Cu2ZnSn(S,Se)4(CZTSSe)is one of the most promising next-generation thin-film photovoltaic materials due to its environmental friendliness and earthabundant constitutions,excellent optoelectronic properties(high absorption coefficient>104/cm and tunable band gap 1.0–1.5 eV)and high theoretical efficiency(32%).1,2 In 2014,12.6%3 efficiency was achieved by the IBM group using the hydrazine method.Based on the sputtering process,12.62%4 efficiency for CZTSSe and 12.5%5 efficiency for CZTSe have been achieved in recent years.However,the highest efficiency has stuck around 12.6%for several years.Lately,a breakthrough with certified 13%power conversion efficiency(PCE)has been demonstrated for CZTSSe thin-film solar cells,surpassing the dust-covered efficiency record since 2014.3,6 Along with the efficiency advancement of kesterite solar cells,a cost-effective fabrication process with low carbon footprint plays an increasingly important role considering the near-future industrialisation of this kind of solar cell with low energy payback time.
基金financially supported by the National Key Research and Development Program of China(2018YFE0203400)the National Key Research and Development Program of China(2017YFA0206600)the National Natural Science Foundation of China(51773045,21772030,51922032 and21961160720)for financial support。
文摘Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)thin films are attractive due to environmental-friendly and earth-abundant constituents,and superior optoelectronic properties such as high absorption coeffi-cient and tunable bandgaps(1.0-1.5 eV).In the past several years,profound progress has been made in CZTSSe via addressing the issues of massive deep defects[1,2],severe band tailing[3],uncon-trollable grain growth[4,5].and unoptimized interfaces[6,7].
基金the National Key Research and Development Program of China(2017YFA0206600)the National Natural Science Foundation of China(51773045,21772030,51922032 and 21961160720)。
文摘In recent years,all-inorganic perovskite solar cells(PSCs)have attracted tremendous interest due to their excellent thermal stability[1-3].Unlike organic-inorganic halide perovskites,whose organic component is volatile at temperatures higher than 2000C,all-inorganic perovskites can tolerate temperatures over 400℃without deterioration[4].However,the power conversion efficiency(PCE)for all-inorganic PSCs is much lower than that of organic-inorganic halide PSCs mainly due to its wider bandgap,which leads to limited light absorption and low short-circuit current density(Jsc).At present,the most studied all-inorganic perovskites are CsPbI3 and CsPbI2Br.Partly replacing I with Br can decrease the preparation temperature,but the bandgap will increase[5,6].To improve the performance of inorganic PSCs,many researches focused on crystallinity control and interfacial engineering[7-10].Few works were done to broaden the photoresponse to improve Jsc,thus improving the PCE.Developing tandem or integrated solar cells is an effective approach to make full use of sunlight[11,12].For tandem solar cells,the preparation process is very complicated.
文摘Over the past few years, there have been significant advancements in uncovering previously sealed records in the kesterite solar cell. This also has led to substantial growth marked by multiple groups achieving successive efficiency breakthroughs, shining a renewed spotlight on this promising photovoltaic material that had previously been overlooked due to its low efficiency.
