Lead iodide(PbI2) is a vital raw material for preparing perovskite solar cells(PSCs),and it not only takes part in forming the light absorption layer but also remains in the grain boundary as a passivator.In other wor...Lead iodide(PbI2) is a vital raw material for preparing perovskite solar cells(PSCs),and it not only takes part in forming the light absorption layer but also remains in the grain boundary as a passivator.In other words,the PbI2 content in the precursor and as formed film will affect the efficiency and stability of the PSCs.With moderate residual PbI2,it passivates the bulk/surface defects of perovskite,reduces the interfacial recombination,promotes the perovskite stability,minimizes the device hysteresis,and so on.Deficient PbI2 residue will reduce the interfacial passivation effect and device performance.In addition to facilitating the non-radiative recombination,over PbI2 residue can also lead to electronic insulation in the grain boundary and deteriorate the device performance.However,the impact and regulation of PbI2 residue on the device performance and stability is still not fully understood.Herein,a comprehensive and detailed review is presented by discussing the PbI2 residue impact and its regulation strategies(i.e., elimination,facilitation and conversion of the residue PbI2) to manipulate the PbI2 content,distribution and forms.Finally,we also show future outlooks in this field,with an aim to help further the progression of high-efficiency and stable PSCs.展开更多
Tin-based perovskite solar cells(TPSCs)have received great attention due to their eco-friendly properties and high theoretical efficiencies.However,the fast crystallization feature of tin-based perovskites leads to po...Tin-based perovskite solar cells(TPSCs)have received great attention due to their eco-friendly properties and high theoretical efficiencies.However,the fast crystallization feature of tin-based perovskites leads to poor film quality and limits the corresponding device performance.Herein,a chlorofullerene,C_(60)Cl_(6),with six chlorine attached to the C_(60)cage,is applied to modulate the crystallization process and passivate grain boundary defects of the perovskite film.The chemical interactions between C_(60)Cl_(6)and perovskite components retard the transforming process of precursors to perovskite crystals and obtain a high-quality tin-based perovskite film.It is also revealed that the C_(60)Cl_(6)located at the surfaces and grain boundaries can not only passivate the defects but also offer a role in suturing grain boundaries to suppress the detrimental effects of water and oxygen on perovskite films,especially the oxidation of Sn^(2+)to Sn^(4+).As a result,the C_(60)Cl_(6)-based device yields a remarkably improved device efficiency from 10.03%to 13.30%with enhanced stability.This work provides a new strategy to regulate the film quality and stability of TPSCs using functional fullerene materials.展开更多
Charge transport materials constitute a relatively large portion of the cost in the production of perovskite solar cells(PSCs).Therefore,developing cheap and efficient charge transport materials is of great significan...Charge transport materials constitute a relatively large portion of the cost in the production of perovskite solar cells(PSCs).Therefore,developing cheap and efficient charge transport materials is of great significance for the commercialization of PSCs.In this study,three low-cost hole transport materials(HTMs),specifically 4,4'-(3,3'-bis(4-methoxy-2,6-dimethylphenyl)-[2,2'-bithiophene]-5,5'-diyl)bis(N,N-bis(4-methoxyphenyl)aniline)(TP-H),4,4'-(3,3'-bis(4-methoxy-2,6-dimethylphenyl)-[2,2'-bithiophene]-5,5'-diyl)bis(3-methoxy-N,N-bis(4-methoxy-phenyl)aniline)(TP-OMe),and 4,4'-(3,3'-bis(4-methoxy-2,6-dimethylphenyl)-[2,2'-bithiophene]-5,5'-diyl)bis(3-fluoro-N,N-bis(4-methoxyphenyl)aniline)(TP-F),were designed and synthesized using a bulky group-substi-tuted 2,2'-bithiophene core and methoxy-or F-functionalized triphenylamine derivatives.Compared to the HTMs without F atoms,TP-F using F substitution exhibited enhanced intermolecular packing,a lower highest occupied molecular orbital energy level,and increased hole mobility and conductivity.The PSC incorporating the doped TP-F as the hole transport layer achieved the highest power conversion efficiency(over 24%)among the three devices.The high performance of TP-F can be attributed to the passivation effect of S and F atoms on uncoordinated Pb2+within the perovskite(PVSK)film,which significantly reduces the density of defect states and the incidence of trap-mediated recombination in PSCs.This study demonstrates the effec-tiveness of the 3,3'-bis(4-methoxy-2,6-dimethylphenyl)-2,2'-bithiophene building block for constructing cost-effective HTMs and highlights the impact of F substitution on enhancing the photovoltaic performance of PSCs.展开更多
Wide-bandgap(WBG)perovskite solar cells suffer from severe non-radiative recombination and exhibit relatively large opencircuit voltage(V_(OC))deficits,limiting their photovoltaic performance.Here,we address these iss...Wide-bandgap(WBG)perovskite solar cells suffer from severe non-radiative recombination and exhibit relatively large opencircuit voltage(V_(OC))deficits,limiting their photovoltaic performance.Here,we address these issues by in-situ forming a well-defined 2D perovskite(PMA)_(2)PbCl_(4)(phenmethylammonium is referred to as PMA)passivation layer on top of the WBG active layer.The 2D layer with highly pure dimensionality and halide components is realized by intentionally tailoring the side-chain substituent at the aryl ring of the post-treatment reagent.First-principle calculation and single-crystal X-ray diffraction results reveal that weak intermolecular interactions between bulky PMA cations and relatively low cation-halide hydrogen bonding strength are crucial in forming the well-defined 2D phase.The(PMA)_(2)PbCl_(4)forms improved type-I energy level alignment with the WBG perovskite,reducing the electron recombination at the perovskite/hole-transport-layer interface.Applying this strategy in fabricating semi-transparent WBG perovskite solar cells(indium tin oxide as the back electrode),the V_(OC)deficits can be reduced to 0.49 V,comparable with the reported state-of-the-art WBG perovskite solar cells using metal electrodes.Consequently,we obtain hysteresis-free 18.60%-efficient WBG perovskite solar cells with a high V_(OC)of 1.23 V.展开更多
Quasi-2D perovskites have attracted tremendous interest for application as lightemission layers in light-emitting diodes(LEDs).However,the heterogeneous n phase and non-uniform distribution still severely limit the fu...Quasi-2D perovskites have attracted tremendous interest for application as lightemission layers in light-emitting diodes(LEDs).However,the heterogeneous n phase and non-uniform distribution still severely limit the further development of quasi-2D perovskite LEDs(Pero-LEDs).Meanwhile,the increased defect density caused by the reduced dimension and grain size induces non-radiative recombination and further deteriorates the device performance.Here,we found that a series of molecules containing phosphoryl chloride functional groups have noticeable enhancement effects on the device performance of quasi-2D Pero-LEDs.Then,we studied the modification mechanism by focusing on the bis(2-oxo-3-oxazolidinyl)phosphinic chloride(BOPCl).It is concluded that the BOPCl can not only regulate the phase distribution by decreasing the crystallization rate but also remain in the grain boundaries and passivate the defects.As a result,the corresponding quasi-2D Pero-LEDs obtained a maximum external quantum efficiency(EQE_(max))of 20.82%and an average EQE(EQE_(ave))of around 20%on the optimal 50 devices,proving excellent reproducibility.Our work provides a new selection of molecular types for regulating the crystallization and passivating the defects of quasi-2D perovskite films.展开更多
Semiconductor photocatalysis is a potential pathway to solve the problems of global energy shortage and environmental pollution.Black phosphorus(BP)has been widely used in the field of photocatalysis owing to its feat...Semiconductor photocatalysis is a potential pathway to solve the problems of global energy shortage and environmental pollution.Black phosphorus(BP)has been widely used in the field of photocatalysis owing to its features of high hole mobility,adjustable bandgap,and wide optical absorption range.Nevertheless,pristine BP still exhibits unsatisfactory photocatalytic activity due to the low separation efficiency of photoinduced charge carriers.In recent years,the construction of heterostructured photocatalysts based on BP has become a research hotspot in photocatalysis with the remarkable improvement of photoexcited charge-separation efficiency.Herein,progress on the design,synthesis,properties,and applications of BP and its corresponding heterostructured photocatalysts is summarized.Furthermore,the photocatalytic applications of BP-based heterostructured photocatalysts in water splitting,pollutant degradation,carbon dioxide reduction,nitrogen fixation,bacterial disinfection,and organic synthesis are reviewed.Opportunities and challenges for the exploration of advanced BP-based heterostructured photocatalysts are presented.This review will promote the development and applications of BP-based heterostructured photocatalysts in energy conversion and environmental remediation.展开更多
SnO_(2)is widely used as the electron transport layer(ETL)in perovskite solar cells(PSCs)due to its excellent electron mobility,low processing temperature,and low cost.And the most common way of preparing the SnO_(2)E...SnO_(2)is widely used as the electron transport layer(ETL)in perovskite solar cells(PSCs)due to its excellent electron mobility,low processing temperature,and low cost.And the most common way of preparing the SnO_(2)ETL is spincoating using the corresponding colloid solution.However,the spin-coated SnO_(2)layer is sometimes not so compact and contains pinholes,weakening the hole blocking capability.Here,a SnO_(2)thin film prepared through magnetron-sputtering was inserted between ITO and the spin-coated SnO_(2)acted as an interlayer.This strategy can combine the advantages of efficient electron extraction and hole blocking due to the high compactness of the sputtered film and the excellent electronic property of the spin-coated SnO_(2).Therefore,the recombination of photo-generated carriers at the interface is significantly reduced.As a result,the semitransparent perovskite solar cells(with a bandgap of 1.73 eV)based on this double-layered SnO_(2)demonstrate a maximum efficiency of 17.7%(stabilized at 17.04%)with negligible hysteresis.Moreover,the shelf stability of the device is also significantly improved,maintaining 95%of the initial efficiency after 800-hours of aging.展开更多
Main observation and conclusion In this article,we report a base-promoted sequential cyclization/aldol-type condensation/isomerization cascade reaction of N-propargyl-β-enaminones with aryl aldehydes.The key step in ...Main observation and conclusion In this article,we report a base-promoted sequential cyclization/aldol-type condensation/isomerization cascade reaction of N-propargyl-β-enaminones with aryl aldehydes.The key step in this protocol is the generation of 1,4-oxazepine anions from N-propargyl-β-enaminones under basic conditions,which are captured by aryl aldehydes.The method allows the formation of one pyridone core and one C—C double bond in“one pot”,and the preparation of a variety of densely decorated pyridone derivatives in moderate to good yields with broad functional group tolerance.展开更多
Magnesium rechargeable batteries(MRBs)present opportunities for grid-scale energy storage applications as a complement to Li-ion batteries(LIBS).The major challenges are the low reversible capacity,inferior cycling st...Magnesium rechargeable batteries(MRBs)present opportunities for grid-scale energy storage applications as a complement to Li-ion batteries(LIBS).The major challenges are the low reversible capacity,inferior cycling stability and unsatisfactory energy densities.Na_(3)VCr_(0.5)Fe_(0.5)(PO_(4))_(3) with a well-defined NASIONtype structure is used as cathode in Mg cell.Two-electrons reaction(~116 m Ah/g),1.5 V average voltage and 65%of capacity retention over 100 cycles are accomplished.Mg is inserted by a biphasic reaction with the participation of V3+/V4+/V5+redox couples in the electrochemical reaction while the non-active redox couples such as Cr^(3+)/Cr^(4+)and Fe^(2+)/Fe^(3+)served as stabilizer to buffer the volume variation.A thermal stability up to~412℃ is also exhibited.Therefore,incorporating a mixture of three transition metal(V/Cr/Fe)in this type of structures will broaden new perspectives for realizing high performance cathodes for MRBs.展开更多
Fullerene materials have been widely used to fabricate efficient and stable perovskite solar cells(PSCs)due to their excellent electron transport ability,defect passivation effect,and beyond.Recent studies have shown ...Fullerene materials have been widely used to fabricate efficient and stable perovskite solar cells(PSCs)due to their excellent electron transport ability,defect passivation effect,and beyond.Recent studies have shown that fullerene-related chemical interaction has played a crucial role in determining device performance.However,the corresponding fullerene-related chemical interactions are yet well understood.Herein,a comprehensive review of fullerene materials in regulating carrier transport,passivating the surface and grain boundary defects,and enhancing device stability is provided.Specifically,the influence of the fullerene-related chemical interactions,including fullerene-perovskite,fullerene-inorganic electron transport layer(IETL),and fullerene-fullerene,on the device performance is well discussed.Finally,we outline some perspectives for further design and application of fullerene materials to enhance the performance and commercial application of PSCs.展开更多
Semi-transparent perovskite solar cells(ST-PSCs)are promising in building-integrated photovoltaics(BIPVs)and tandem solar cells(TSCs).One of the keys to fabricate high-performance ST-PSCs is depositing efficient trans...Semi-transparent perovskite solar cells(ST-PSCs)are promising in building-integrated photovoltaics(BIPVs)and tandem solar cells(TSCs).One of the keys to fabricate high-performance ST-PSCs is depositing efficient transparent electrodes.Indium tin oxide(ITO)is an excellent transparent conductive oxide with good light transmittance and high conductivity.However,the high sheet resistance of ITO sputtered at room temperature leads to the low fill factor(FF)and poor power conversion efficiency(PCE)of the ST-PSCs.Here,we study the effect of the sputtering temperature on the properties of ITO and the performance of ST-PSCs.We find that when the sputtering temperature increases from the room temperature to 70℃,the crystallinity of the sputtered ITO gradually improves.Therefore,the sheet resistance decreases and the corresponding device performance improves.However,once the sputtering temperature further increases over 70℃,the underlying hole transport layer will be damaged,leading to poor device performance.Therefore,the optimized mild heating temperature of 70℃is applied and we obtain ST-PSCs with a champion PCE of 15.21%.We believe this mild heating assisted sputtering method is applicable in fabricating BIPVs and TSCs.展开更多
Two-dimensional(2D)graphdiyne(GDY)-based materials have attracted attention in the solar cell research community owing to their unique physicochemical properties and hydrophobic nature which can serve as moisture resi...Two-dimensional(2D)graphdiyne(GDY)-based materials have attracted attention in the solar cell research community owing to their unique physicochemical properties and hydrophobic nature which can serve as moisture resistance from the surrounding medium.Benefiting from these,the performance and stability ofperovskite solar cells(PSCs)can be greatly improved via the addition of 2D GDY-based materials.This mini-review summarizes the recent development of 2D GDY-based materials for PSC application.The roles of 2D GDY-based materials,such as hole transporting material,electron transporting material,dopant material in perovskite film and interfacial layer,are discussed in detail.Moreover,we provide future perspectives in this field,aiming to help further progress efficient and stable 2D GDY-based materials in PSCs.展开更多
This highlight mainly focuses on the recent meaningful research progress of single crystals(SCs)perovskite lightemitting diodes(LEDs)made by Xiao et al.[1],published in Nature Photonics.They made a breakthrough in the...This highlight mainly focuses on the recent meaningful research progress of single crystals(SCs)perovskite lightemitting diodes(LEDs)made by Xiao et al.[1],published in Nature Photonics.They made a breakthrough in the in-situ preparation of micron-thick SCs-based perovskite films on the ITO/hole-transporter layer and successfully fabricated the LEDs.展开更多
Semi-transparent perovskite solar cells(ST-PSCs)have broad applications in building integrated photovoltaics.However,the stability of ST-PSCs needs to be improved,especially in n-i-p ST-PSCs since the doped 2,2',7...Semi-transparent perovskite solar cells(ST-PSCs)have broad applications in building integrated photovoltaics.However,the stability of ST-PSCs needs to be improved,especially in n-i-p ST-PSCs since the doped 2,2',7,7'-tetrakis(N,N-di-p-methoxyphenyl-amine)-9,9'-spirobifluorene(Spiro-OMeTAD)is unstable at elevated temperatures and high humidity.In this work,aπ-conjugated polymer poly[(2,6-(4,8-bis(5-(2-ethylhexyl)thiophene-2-yl)-benzo[1,2-b:4,5-b']dithiophene))-alt-(5,5-(1',3'-di-2-thienyl-5',7'-bis(2-ethylhexyl)benzo[1',2'-c:4',5'-c']dithiophene-4,8-dione)](PBDB-T)is selected to form a polymer composite hole transport layer(HTL)with Spiro-OMeTAD.The sulfur atom of the thiophene unit and the carbonyl group of the polymer interact with the undercoordinated Pb2+at the perovskite surface,which stabilizes the perovskite/HTL interface and passivates the interfacial defects.The incorporation of the polymer also increases the glass transition temperature and the moisture resistance of Spiro-OMeTAD.As a result,we obtain ST-PSCs with a champion efficiency of 13.71%and an average visible light transmittance of 36.04%.Therefore,a high light utilization efficiency of 4.94%can be obtained.Moreover,the encapsulated device can maintain 84%of the initial efficiency after 751 h under continuous one-sun illumination(at 30%relative humidity)at the open circuit and the unencapsulated device can maintain 80%of the initial efficiency after maximum power tracking for more than 1250 h under continuous one-sun illumination.展开更多
Due to their unique photoelectric properties,nontoxic tin-based perovskites are emerging candidates for efficient near-infrared LEDs.However,the facile oxidation of Sn2+and the rapid crystallization rate of tin-based ...Due to their unique photoelectric properties,nontoxic tin-based perovskites are emerging candidates for efficient near-infrared LEDs.However,the facile oxidation of Sn2+and the rapid crystallization rate of tin-based perovskites result in suboptimal film quality,leading to inferior efficiencies of tin-based perovskite light-emitting diodes(Pero-LEDs).In this study,we investigate the influence of commonly used solvents on the quality of the CsSnI3 films.Remarkably,DMSO exhibits a stronger interaction with SnI2,forming a stable intermediate phase of SnI2·3DMSO.This intermediate effectively inhibits the oxidation of Sn2+and slows down the crystallization rate,bringing in lower defect state density and higher photoluminescence quantum yield of the pre-pared perovskite films.Consequently,the corresponding Pero-LEDs achieve a maximum external quantum efficiency(EQE)of 5.6%,among the most effi-cient near-infrared Pero-LEDs.In addition,the device processes ultra-low effi-ciency roll-off and high reproducibility.Our research underscores the crucial role of solvent-perovskite coordination in determining film quality.These find-ings offer valuable guidance for screening solvents to prepare highly efficient and stable tin-based perovskites.展开更多
Carrier recombination at the buried SnO_(2)/perovskite interface limits the efficiency and stability of n-i-p-structured perovskite solar cells(PSCs).Herein,we report an In_(2)O_(3)interfacial layer with the distincti...Carrier recombination at the buried SnO_(2)/perovskite interface limits the efficiency and stability of n-i-p-structured perovskite solar cells(PSCs).Herein,we report an In_(2)O_(3)interfacial layer with the distinctive structure of the monolithic compact/nanostructured bilayer.The partial hydrolysis nature of the In^(3+)ion enables the formation of nanorods on top of the compact In_(2)O_(3)layer when spin-coating the In(NO_(3))_(3) aqueous solution.This novel interfacial layer reduces the pinholes of the SnO_(2)film and increases the contact area between the perovskite and electron transport material.Therefore,PSCs with the incorporation of the interfacial layer demonstrate enhanced electron extraction and suppressed carrier recombination.Consequently,the champion device achieves a power conversion efficiency of 23.87%with a high fill factor of 82.14%.The optimized device also shows robust operational stability,retaining over 80%of the initial power conversion efficiency after working at the maximum power point for over 500 h under continuous one-sun illumination.展开更多
Exploration of bifunctional electrocatalysts toward effective oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is pivotal for developing high-efficiency and rechargeable metal-air batteries but remains ...Exploration of bifunctional electrocatalysts toward effective oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is pivotal for developing high-efficiency and rechargeable metal-air batteries but remains great challenging.Here we elaborately synthesize lamellar-assembled PdNi super-nanosheets(SNSs)with an optimized Pd/Ni molar ratio to serve as attractive ORR and OER bifunctional electrocatalysts for rechargeable high-powered Zn-air batteries(ZABs).The products are layer-by-layer stackings of ultrathin PdNi nanosheet motifs.On the drastically extended two-dimensional(2D)surface,the inserted Ni atoms can substantially lower down the d-band center of surface Pd toward improved ORR kinetics and concurrently create oxytropic NiOx sites to adsorb–OH groups for promoting the reverse OER electrocatalysis.Specifically,the ORR mass activity and specific activity of the primary Pd_(92)Ni_(8)SNSs attain 2.5 A·mg^(−1)and 3.15 mA·cm^(−2),which are respectively 14 and 9 times those of commercial Pt/C.Meanwhile,the OER activity and stability of Pd_(92)Ni_(8)SNSs/C distinctly outperform those of the RuO_(2)benchmark,suggesting excellent reversible oxygen electrocatalysis.The power density of the ZAB with Pd_(92)Ni_(8)SNSs/C as the air cathode is 2.7 times higher than that by Pt/C benchmark.Significantly,it can last for over 150 h without significant performance degradation during the charge–discharge cycle test.This work showcases a feasible strategy for developing self-assembled multimetallic 2D nanomaterials with excellent bifunctional catalytic performances toward energy conversion applications.展开更多
基金financially supported by the National Natural Science Foundation of China(U21A2078,22179042,and 12104170)the Natural Science Foundation of Fujian Province(2020J06021 and 2020J01064)Scientific Research Funds of Huaqiao University(23BS109)。
文摘Lead iodide(PbI2) is a vital raw material for preparing perovskite solar cells(PSCs),and it not only takes part in forming the light absorption layer but also remains in the grain boundary as a passivator.In other words,the PbI2 content in the precursor and as formed film will affect the efficiency and stability of the PSCs.With moderate residual PbI2,it passivates the bulk/surface defects of perovskite,reduces the interfacial recombination,promotes the perovskite stability,minimizes the device hysteresis,and so on.Deficient PbI2 residue will reduce the interfacial passivation effect and device performance.In addition to facilitating the non-radiative recombination,over PbI2 residue can also lead to electronic insulation in the grain boundary and deteriorate the device performance.However,the impact and regulation of PbI2 residue on the device performance and stability is still not fully understood.Herein,a comprehensive and detailed review is presented by discussing the PbI2 residue impact and its regulation strategies(i.e., elimination,facilitation and conversion of the residue PbI2) to manipulate the PbI2 content,distribution and forms.Finally,we also show future outlooks in this field,with an aim to help further the progression of high-efficiency and stable PSCs.
基金financially supported by the National Natural Science Foundation of China(51902110,U21A2078,and 22179042)Natural Science Foundation of Fujian Province(2020J01064 and 2020J06021)Scientific Research Funds of Huaqiao University,and the Promotion Program for Young and Middle-aged Teacher in Science and Technology Research of Huaqiao University(ZQN-806,ZQNPY607)
文摘Tin-based perovskite solar cells(TPSCs)have received great attention due to their eco-friendly properties and high theoretical efficiencies.However,the fast crystallization feature of tin-based perovskites leads to poor film quality and limits the corresponding device performance.Herein,a chlorofullerene,C_(60)Cl_(6),with six chlorine attached to the C_(60)cage,is applied to modulate the crystallization process and passivate grain boundary defects of the perovskite film.The chemical interactions between C_(60)Cl_(6)and perovskite components retard the transforming process of precursors to perovskite crystals and obtain a high-quality tin-based perovskite film.It is also revealed that the C_(60)Cl_(6)located at the surfaces and grain boundaries can not only passivate the defects but also offer a role in suturing grain boundaries to suppress the detrimental effects of water and oxygen on perovskite films,especially the oxidation of Sn^(2+)to Sn^(4+).As a result,the C_(60)Cl_(6)-based device yields a remarkably improved device efficiency from 10.03%to 13.30%with enhanced stability.This work provides a new strategy to regulate the film quality and stability of TPSCs using functional fullerene materials.
基金supported by the National Natural Science Foundation of China(Grant Nos.U23A20371,U21A2078,and 22179042)the Natural Science Foundation of Fujian Province(Grant No.2023J06034)+1 种基金the Natural Science Foundation of Xiamen,China(Grant No.3502Z20227036)the Scientific Research Funds of Huaqiao University(Grant No.605-50Y23024).
文摘Charge transport materials constitute a relatively large portion of the cost in the production of perovskite solar cells(PSCs).Therefore,developing cheap and efficient charge transport materials is of great significance for the commercialization of PSCs.In this study,three low-cost hole transport materials(HTMs),specifically 4,4'-(3,3'-bis(4-methoxy-2,6-dimethylphenyl)-[2,2'-bithiophene]-5,5'-diyl)bis(N,N-bis(4-methoxyphenyl)aniline)(TP-H),4,4'-(3,3'-bis(4-methoxy-2,6-dimethylphenyl)-[2,2'-bithiophene]-5,5'-diyl)bis(3-methoxy-N,N-bis(4-methoxy-phenyl)aniline)(TP-OMe),and 4,4'-(3,3'-bis(4-methoxy-2,6-dimethylphenyl)-[2,2'-bithiophene]-5,5'-diyl)bis(3-fluoro-N,N-bis(4-methoxyphenyl)aniline)(TP-F),were designed and synthesized using a bulky group-substi-tuted 2,2'-bithiophene core and methoxy-or F-functionalized triphenylamine derivatives.Compared to the HTMs without F atoms,TP-F using F substitution exhibited enhanced intermolecular packing,a lower highest occupied molecular orbital energy level,and increased hole mobility and conductivity.The PSC incorporating the doped TP-F as the hole transport layer achieved the highest power conversion efficiency(over 24%)among the three devices.The high performance of TP-F can be attributed to the passivation effect of S and F atoms on uncoordinated Pb2+within the perovskite(PVSK)film,which significantly reduces the density of defect states and the incidence of trap-mediated recombination in PSCs.This study demonstrates the effec-tiveness of the 3,3'-bis(4-methoxy-2,6-dimethylphenyl)-2,2'-bithiophene building block for constructing cost-effective HTMs and highlights the impact of F substitution on enhancing the photovoltaic performance of PSCs.
基金supported by the National Natural Science Foundation of China(22179042,U21A2078,and 51902110)the Natural Science Foundation of Fujian Province(2020J06021 and 2020J01064).
文摘Wide-bandgap(WBG)perovskite solar cells suffer from severe non-radiative recombination and exhibit relatively large opencircuit voltage(V_(OC))deficits,limiting their photovoltaic performance.Here,we address these issues by in-situ forming a well-defined 2D perovskite(PMA)_(2)PbCl_(4)(phenmethylammonium is referred to as PMA)passivation layer on top of the WBG active layer.The 2D layer with highly pure dimensionality and halide components is realized by intentionally tailoring the side-chain substituent at the aryl ring of the post-treatment reagent.First-principle calculation and single-crystal X-ray diffraction results reveal that weak intermolecular interactions between bulky PMA cations and relatively low cation-halide hydrogen bonding strength are crucial in forming the well-defined 2D phase.The(PMA)_(2)PbCl_(4)forms improved type-I energy level alignment with the WBG perovskite,reducing the electron recombination at the perovskite/hole-transport-layer interface.Applying this strategy in fabricating semi-transparent WBG perovskite solar cells(indium tin oxide as the back electrode),the V_(OC)deficits can be reduced to 0.49 V,comparable with the reported state-of-the-art WBG perovskite solar cells using metal electrodes.Consequently,we obtain hysteresis-free 18.60%-efficient WBG perovskite solar cells with a high V_(OC)of 1.23 V.
基金supported by the National Natural Science Foundation of China(U21A2078)Natural Science Foundation of Fujian Province(2020J06021,2019J01057,and 2020J01064)Scientific Research Funds of Huaqiao University.
文摘Quasi-2D perovskites have attracted tremendous interest for application as lightemission layers in light-emitting diodes(LEDs).However,the heterogeneous n phase and non-uniform distribution still severely limit the further development of quasi-2D perovskite LEDs(Pero-LEDs).Meanwhile,the increased defect density caused by the reduced dimension and grain size induces non-radiative recombination and further deteriorates the device performance.Here,we found that a series of molecules containing phosphoryl chloride functional groups have noticeable enhancement effects on the device performance of quasi-2D Pero-LEDs.Then,we studied the modification mechanism by focusing on the bis(2-oxo-3-oxazolidinyl)phosphinic chloride(BOPCl).It is concluded that the BOPCl can not only regulate the phase distribution by decreasing the crystallization rate but also remain in the grain boundaries and passivate the defects.As a result,the corresponding quasi-2D Pero-LEDs obtained a maximum external quantum efficiency(EQE_(max))of 20.82%and an average EQE(EQE_(ave))of around 20%on the optimal 50 devices,proving excellent reproducibility.Our work provides a new selection of molecular types for regulating the crystallization and passivating the defects of quasi-2D perovskite films.
基金financially supported by the National Natural Science Foundation of China(21902051,21861130353,U1905214,21961142019,22032002,21761132002,and 21425309)the Fundamental Research Funds for the Central Universities(ZQN-807)+7 种基金the Natural Science Foundation of Fujian Province(2019J05090 and 2017J01014)the Graphene Powder and Composite Research Center of Fujian Province(2017H2001)the Scientific Research Funds of Huaqiao University(20171XD033)the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment of Fuzhou University(SKLPEE-KF201803)the National Key Technologies R&D Program of China(2018YFA0209301)the National Basic Research Program of China(2013CB632405)the Chang Jiang Scholars Program of China(T2016147)the 111 Project(D16008).
文摘Semiconductor photocatalysis is a potential pathway to solve the problems of global energy shortage and environmental pollution.Black phosphorus(BP)has been widely used in the field of photocatalysis owing to its features of high hole mobility,adjustable bandgap,and wide optical absorption range.Nevertheless,pristine BP still exhibits unsatisfactory photocatalytic activity due to the low separation efficiency of photoinduced charge carriers.In recent years,the construction of heterostructured photocatalysts based on BP has become a research hotspot in photocatalysis with the remarkable improvement of photoexcited charge-separation efficiency.Herein,progress on the design,synthesis,properties,and applications of BP and its corresponding heterostructured photocatalysts is summarized.Furthermore,the photocatalytic applications of BP-based heterostructured photocatalysts in water splitting,pollutant degradation,carbon dioxide reduction,nitrogen fixation,bacterial disinfection,and organic synthesis are reviewed.Opportunities and challenges for the exploration of advanced BP-based heterostructured photocatalysts are presented.This review will promote the development and applications of BP-based heterostructured photocatalysts in energy conversion and environmental remediation.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.22179042,U21A2078,and 51902110)the Natural Science Foundation of Fujian Province,China(Grant Nos.2020J06021,2019J01057,and 2020J01064)+1 种基金Scientific Research Funds of Huaqiao UniversityPromotion Program for Young and Middle-aged Teacher in Science and Technology Research of Huaqiao University(Grant Nos.ZQN-PY607 and ZQN-806)。
文摘SnO_(2)is widely used as the electron transport layer(ETL)in perovskite solar cells(PSCs)due to its excellent electron mobility,low processing temperature,and low cost.And the most common way of preparing the SnO_(2)ETL is spincoating using the corresponding colloid solution.However,the spin-coated SnO_(2)layer is sometimes not so compact and contains pinholes,weakening the hole blocking capability.Here,a SnO_(2)thin film prepared through magnetron-sputtering was inserted between ITO and the spin-coated SnO_(2)acted as an interlayer.This strategy can combine the advantages of efficient electron extraction and hole blocking due to the high compactness of the sputtered film and the excellent electronic property of the spin-coated SnO_(2).Therefore,the recombination of photo-generated carriers at the interface is significantly reduced.As a result,the semitransparent perovskite solar cells(with a bandgap of 1.73 eV)based on this double-layered SnO_(2)demonstrate a maximum efficiency of 17.7%(stabilized at 17.04%)with negligible hysteresis.Moreover,the shelf stability of the device is also significantly improved,maintaining 95%of the initial efficiency after 800-hours of aging.
文摘Main observation and conclusion In this article,we report a base-promoted sequential cyclization/aldol-type condensation/isomerization cascade reaction of N-propargyl-β-enaminones with aryl aldehydes.The key step in this protocol is the generation of 1,4-oxazepine anions from N-propargyl-β-enaminones under basic conditions,which are captured by aryl aldehydes.The method allows the formation of one pyridone core and one C—C double bond in“one pot”,and the preparation of a variety of densely decorated pyridone derivatives in moderate to good yields with broad functional group tolerance.
基金supported by the Scientific Research Funds of Huaqiao University and Xiamen University Foreign Young Talents Program(No.G2022149004L)。
文摘Magnesium rechargeable batteries(MRBs)present opportunities for grid-scale energy storage applications as a complement to Li-ion batteries(LIBS).The major challenges are the low reversible capacity,inferior cycling stability and unsatisfactory energy densities.Na_(3)VCr_(0.5)Fe_(0.5)(PO_(4))_(3) with a well-defined NASIONtype structure is used as cathode in Mg cell.Two-electrons reaction(~116 m Ah/g),1.5 V average voltage and 65%of capacity retention over 100 cycles are accomplished.Mg is inserted by a biphasic reaction with the participation of V3+/V4+/V5+redox couples in the electrochemical reaction while the non-active redox couples such as Cr^(3+)/Cr^(4+)and Fe^(2+)/Fe^(3+)served as stabilizer to buffer the volume variation.A thermal stability up to~412℃ is also exhibited.Therefore,incorporating a mixture of three transition metal(V/Cr/Fe)in this type of structures will broaden new perspectives for realizing high performance cathodes for MRBs.
基金the National Natural Science Foundation of China(Nos.51902110,U21A2078,and 22179042)the Natural Science Foundation of Fujian Province(Nos.2020J01064,2020J06021,and 2019J01057)the Scientific Research Funds of Huaqiao University,and Promotion Program for Young and Middle-aged Teacher in Science and Technology Research of Huaqiao University(Nos.ZQN-806 and ZQNPY607).
文摘Fullerene materials have been widely used to fabricate efficient and stable perovskite solar cells(PSCs)due to their excellent electron transport ability,defect passivation effect,and beyond.Recent studies have shown that fullerene-related chemical interaction has played a crucial role in determining device performance.However,the corresponding fullerene-related chemical interactions are yet well understood.Herein,a comprehensive review of fullerene materials in regulating carrier transport,passivating the surface and grain boundary defects,and enhancing device stability is provided.Specifically,the influence of the fullerene-related chemical interactions,including fullerene-perovskite,fullerene-inorganic electron transport layer(IETL),and fullerene-fullerene,on the device performance is well discussed.Finally,we outline some perspectives for further design and application of fullerene materials to enhance the performance and commercial application of PSCs.
基金the National Natural Science Foundation of China(22179042,U21A2078,and 51902110)Natural Science Foundation of Fujian Province(2020J06021,2019J01057,and 2020J01064)Scientific Research Funds of Huaqiao University,and Promotion Program for Young and Middle-Aged Teacher in Science and Technology Research of Huaqiao University(ZQN-PY607,ZQN-806).
文摘Semi-transparent perovskite solar cells(ST-PSCs)are promising in building-integrated photovoltaics(BIPVs)and tandem solar cells(TSCs).One of the keys to fabricate high-performance ST-PSCs is depositing efficient transparent electrodes.Indium tin oxide(ITO)is an excellent transparent conductive oxide with good light transmittance and high conductivity.However,the high sheet resistance of ITO sputtered at room temperature leads to the low fill factor(FF)and poor power conversion efficiency(PCE)of the ST-PSCs.Here,we study the effect of the sputtering temperature on the properties of ITO and the performance of ST-PSCs.We find that when the sputtering temperature increases from the room temperature to 70℃,the crystallinity of the sputtered ITO gradually improves.Therefore,the sheet resistance decreases and the corresponding device performance improves.However,once the sputtering temperature further increases over 70℃,the underlying hole transport layer will be damaged,leading to poor device performance.Therefore,the optimized mild heating temperature of 70℃is applied and we obtain ST-PSCs with a champion PCE of 15.21%.We believe this mild heating assisted sputtering method is applicable in fabricating BIPVs and TSCs.
基金financially supported by the National Natural Science Foundation of China(U21A2078,22179042,and 12104170)the Natural Science Foundation of Fujian Province(2020J06021,2019J01057,and 2020J01064)Scientific Research Funds of Huaqiao University.
文摘Two-dimensional(2D)graphdiyne(GDY)-based materials have attracted attention in the solar cell research community owing to their unique physicochemical properties and hydrophobic nature which can serve as moisture resistance from the surrounding medium.Benefiting from these,the performance and stability ofperovskite solar cells(PSCs)can be greatly improved via the addition of 2D GDY-based materials.This mini-review summarizes the recent development of 2D GDY-based materials for PSC application.The roles of 2D GDY-based materials,such as hole transporting material,electron transporting material,dopant material in perovskite film and interfacial layer,are discussed in detail.Moreover,we provide future perspectives in this field,aiming to help further progress efficient and stable 2D GDY-based materials in PSCs.
文摘This highlight mainly focuses on the recent meaningful research progress of single crystals(SCs)perovskite lightemitting diodes(LEDs)made by Xiao et al.[1],published in Nature Photonics.They made a breakthrough in the in-situ preparation of micron-thick SCs-based perovskite films on the ITO/hole-transporter layer and successfully fabricated the LEDs.
基金supported by the National Natural Science Foundation of China(Nos.22179042 and U21A2078)the Natural Science Foundation of Fujian Province(Nos.2020J06021 and 2020J01064).
文摘Semi-transparent perovskite solar cells(ST-PSCs)have broad applications in building integrated photovoltaics.However,the stability of ST-PSCs needs to be improved,especially in n-i-p ST-PSCs since the doped 2,2',7,7'-tetrakis(N,N-di-p-methoxyphenyl-amine)-9,9'-spirobifluorene(Spiro-OMeTAD)is unstable at elevated temperatures and high humidity.In this work,aπ-conjugated polymer poly[(2,6-(4,8-bis(5-(2-ethylhexyl)thiophene-2-yl)-benzo[1,2-b:4,5-b']dithiophene))-alt-(5,5-(1',3'-di-2-thienyl-5',7'-bis(2-ethylhexyl)benzo[1',2'-c:4',5'-c']dithiophene-4,8-dione)](PBDB-T)is selected to form a polymer composite hole transport layer(HTL)with Spiro-OMeTAD.The sulfur atom of the thiophene unit and the carbonyl group of the polymer interact with the undercoordinated Pb2+at the perovskite surface,which stabilizes the perovskite/HTL interface and passivates the interfacial defects.The incorporation of the polymer also increases the glass transition temperature and the moisture resistance of Spiro-OMeTAD.As a result,we obtain ST-PSCs with a champion efficiency of 13.71%and an average visible light transmittance of 36.04%.Therefore,a high light utilization efficiency of 4.94%can be obtained.Moreover,the encapsulated device can maintain 84%of the initial efficiency after 751 h under continuous one-sun illumination(at 30%relative humidity)at the open circuit and the unencapsulated device can maintain 80%of the initial efficiency after maximum power tracking for more than 1250 h under continuous one-sun illumination.
基金supported by the National Key Research and Development Program of China(2022YFA1204800)National Natural Science Foundation of China(U21A2078,22179042,and 12104170)+1 种基金the Natural Science Foundation of Fujian Province(2023J06034)Scientific Research Funds and Subsidized Project for Postgraduate's Innovative Fund in Scientific Research of Huaqiao University。
文摘Due to their unique photoelectric properties,nontoxic tin-based perovskites are emerging candidates for efficient near-infrared LEDs.However,the facile oxidation of Sn2+and the rapid crystallization rate of tin-based perovskites result in suboptimal film quality,leading to inferior efficiencies of tin-based perovskite light-emitting diodes(Pero-LEDs).In this study,we investigate the influence of commonly used solvents on the quality of the CsSnI3 films.Remarkably,DMSO exhibits a stronger interaction with SnI2,forming a stable intermediate phase of SnI2·3DMSO.This intermediate effectively inhibits the oxidation of Sn2+and slows down the crystallization rate,bringing in lower defect state density and higher photoluminescence quantum yield of the pre-pared perovskite films.Consequently,the corresponding Pero-LEDs achieve a maximum external quantum efficiency(EQE)of 5.6%,among the most effi-cient near-infrared Pero-LEDs.In addition,the device processes ultra-low effi-ciency roll-off and high reproducibility.Our research underscores the crucial role of solvent-perovskite coordination in determining film quality.These find-ings offer valuable guidance for screening solvents to prepare highly efficient and stable tin-based perovskites.
基金National Natural Science Foundation of China,Grant/Award Numbers:22179042,U21A2078,51902110Promotion Program for Young and Middle-aged Teacher in Science and Technology Research of Huaqiao University,Grant/Award Numbers:ZQN-PY607,ZQN-806Natural Science Foundation of Fujian Province,Grant/Award Numbers:2020J06021,2019J01057,2020J01064。
文摘Carrier recombination at the buried SnO_(2)/perovskite interface limits the efficiency and stability of n-i-p-structured perovskite solar cells(PSCs).Herein,we report an In_(2)O_(3)interfacial layer with the distinctive structure of the monolithic compact/nanostructured bilayer.The partial hydrolysis nature of the In^(3+)ion enables the formation of nanorods on top of the compact In_(2)O_(3)layer when spin-coating the In(NO_(3))_(3) aqueous solution.This novel interfacial layer reduces the pinholes of the SnO_(2)film and increases the contact area between the perovskite and electron transport material.Therefore,PSCs with the incorporation of the interfacial layer demonstrate enhanced electron extraction and suppressed carrier recombination.Consequently,the champion device achieves a power conversion efficiency of 23.87%with a high fill factor of 82.14%.The optimized device also shows robust operational stability,retaining over 80%of the initial power conversion efficiency after working at the maximum power point for over 500 h under continuous one-sun illumination.
基金supported by the National Natural Science Foundation of China(No.22171093)the Natural Science Foundation of Fujian Province(Nos.2022J05058 and 2022J02008)the Scientific Research Funds of Huaqiao University(No.605-50Y21048).
文摘Exploration of bifunctional electrocatalysts toward effective oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is pivotal for developing high-efficiency and rechargeable metal-air batteries but remains great challenging.Here we elaborately synthesize lamellar-assembled PdNi super-nanosheets(SNSs)with an optimized Pd/Ni molar ratio to serve as attractive ORR and OER bifunctional electrocatalysts for rechargeable high-powered Zn-air batteries(ZABs).The products are layer-by-layer stackings of ultrathin PdNi nanosheet motifs.On the drastically extended two-dimensional(2D)surface,the inserted Ni atoms can substantially lower down the d-band center of surface Pd toward improved ORR kinetics and concurrently create oxytropic NiOx sites to adsorb–OH groups for promoting the reverse OER electrocatalysis.Specifically,the ORR mass activity and specific activity of the primary Pd_(92)Ni_(8)SNSs attain 2.5 A·mg^(−1)and 3.15 mA·cm^(−2),which are respectively 14 and 9 times those of commercial Pt/C.Meanwhile,the OER activity and stability of Pd_(92)Ni_(8)SNSs/C distinctly outperform those of the RuO_(2)benchmark,suggesting excellent reversible oxygen electrocatalysis.The power density of the ZAB with Pd_(92)Ni_(8)SNSs/C as the air cathode is 2.7 times higher than that by Pt/C benchmark.Significantly,it can last for over 150 h without significant performance degradation during the charge–discharge cycle test.This work showcases a feasible strategy for developing self-assembled multimetallic 2D nanomaterials with excellent bifunctional catalytic performances toward energy conversion applications.
