Wide-bandgap(WBG)perovskite solar cells(PSCs)have gained remarkable interest owing to their latent applications in tandem solar cells(TSCs).Among them,four-terminal(4T)all-perovskite TSCs have received extensive atten...Wide-bandgap(WBG)perovskite solar cells(PSCs)have gained remarkable interest owing to their latent applications in tandem solar cells(TSCs).Among them,four-terminal(4T)all-perovskite TSCs have received extensive attention as its do without need to consider current matching,surface roughness,and fabrication processes.However,low open-circuit voltage(VOC)and efficiency of WBG PSCs obstacles their applications in 4T allperovskite TSCs.Hence,this review firstly discussed the optimizing strategy in perovskite materials layer and properties.Specifically,we assessed the effect of composition,additive and interface engineering on the efficiency and VOC of WBG PSCs.Secondly,the demonstrated applications of different passivation layers designing for intensifying the efficiency of WBG PSCs and 4T all-perovskite TSCs is discussed.Finally,we put forward three specific approaches for future research,in our view,which would offer appropriate guidance for the exploitation of highly efficient and stable 4T all-perovskite TSCs.展开更多
[4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid(Me-4PACz)self-assembled monolayer(SAM)as the hole transport materials have been demonstrated remarkable potential in perovskite solar cells(PSCs).However,the hyd...[4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid(Me-4PACz)self-assembled monolayer(SAM)as the hole transport materials have been demonstrated remarkable potential in perovskite solar cells(PSCs).However,the hydrophobicity of Me-4PACz presents a critical challenge for the fabrication of high-quality perovskite films due to its poor wettability.Here,a doped Al_(2)O_(3)with Me-4PACz to modify the Me-4PACz surface was proposed.On one hand,this approach improved the wettability of the Me-4PACz film,enhancing the coverage,uniformity,and buried interface properties of the perovskite film.On the other hand,compared to Al_(2)O_(3)modification alone,doping Al_(2)O_(3)with Me-4PACz allowed direct contact between the perovskite and Me-4PACz,resulting in better buried interface passivation.As a result,we achieved an efficiency of 22.71%for single-junction wide-bandgap perovskite solar cells(1.68 eV).Additionally,the efficiency of perovskite/silicon tandem solar cells was improved from 28.68%to 30.92%,with a significant reduction in hysteresis.Furthermore,the tandem cells demonstrated no degradation after 4200 s of operation at the maximum power point.展开更多
The CO_(2)-assisted oxidative dehydrogenation of ethane(CO_(2)-ODHE)provides a promising way to produce ethylene and utilize CO_(2).Simultaneous upgrading of ethane into the high value-added chemical products and the ...The CO_(2)-assisted oxidative dehydrogenation of ethane(CO_(2)-ODHE)provides a promising way to produce ethylene and utilize CO_(2).Simultaneous upgrading of ethane into the high value-added chemical products and the reduction of greenhouse gas CO_(2)emissions could be achieved.However,the targeted breaking of the C-C/C-H bonds of ethane is still a challenge for the designed catalysts.In this paper,ZnO-doped ZrO_(2)bifunctional catalysts(Zn_(x)ZrO)with different Zn/Zr molar ratios were prepared by the deposition-precipitation method,and the functions of various sites for CO_(2)-ODHE reaction were revealed by in situ characterizations and ethane pulse experiment:the medium-strength acidic Zn-O-Zr sites are responsible for the purposefully cracking of ethane C-H bonds to ethylene,while the more oxygen vacancies(OV)created by the introduction of Zn^(2+)are responsible for the efficient activation C=O bonds of CO_(2),thus promoting the RWGS reaction.In addition,the Zn0.2ZrO catalyst demonstrated excellent catalytic performances,with C_(2)H_(6)conversion,C_(2)H_(4)yield,and CO_(2)conversion about 19.1%,10.5%,and 10.6%within 5 h,respectively(600℃,GHSV=3000 mL/(g·h)).Especially,the initial ethylene space-time yield of 355.5μmol/(min·g)was obtained under 6000 mL/(g·h);Finally,the tandem reaction mechanism of ethane dehydrogenation and RWGS was revealed.展开更多
Solar energy, as a renewable resource, is an effective solution to the current global energy shortage problem. To actively respond to the call for "carbon peak" and "carbon neutrality", solar cell ...Solar energy, as a renewable resource, is an effective solution to the current global energy shortage problem. To actively respond to the call for "carbon peak" and "carbon neutrality", solar cell industry has experienced unprecedented development. The full utilization of solar energy resources remains an urgent issue to be addressed.展开更多
All-perovskite tandem solar cells(ATSCs) have the potential to surpass the Shockley-Queisser efficiency limit of conventional single-junction devices. However, the performance and stability of mixed tin–lead(Sn–Pb) ...All-perovskite tandem solar cells(ATSCs) have the potential to surpass the Shockley-Queisser efficiency limit of conventional single-junction devices. However, the performance and stability of mixed tin–lead(Sn–Pb) perovskite solar cells(PSCs), which are crucial components of ATSCs, are much lower than those of lead-based perovskites. The primary challenges include the high crystallization rate of perovskite materials and the susceptibility of Sn^(2+) oxidation, which leads to rough morphology and unfavorable p-type self-doping. To address these issues, we introduced ethylhydrazine oxalate(EDO) at the perovskite interface, which effectively inhibits the oxidation of Sn^(2+) and simultaneously enhances the crystallinity of the perovskite. Consequently, the EDO-modified mixed tin-lead PSCs reached a power conversion efficiency(PCE) of 21.96% with high reproducibility. We further achieved a 27.58% efficient ATSCs by using EDO as interfacial passivator in the Sn-Pb PSCs.展开更多
This study first demonstrates the potential of organic photoabsorbing blends in overcoming a critical limitation of metal oxide photoanodes in tandem modules:insufficient photogenerated current.Various organic blends,...This study first demonstrates the potential of organic photoabsorbing blends in overcoming a critical limitation of metal oxide photoanodes in tandem modules:insufficient photogenerated current.Various organic blends,including PTB7-Th:FOIC,PTB7-Th:O6T-4F,PM6:Y6,and PM6:FM,were systematically tested.When coupled with electron transport layer(ETL)contacts,these blends exhibit exceptional charge separation and extraction,with PM6:Y6 achieving saturation photocurrents up to 16.8 mA cm^(-2) at 1.23 VRHE(oxygen evolution thermodynamic potential).For the first time,a tandem structure utilizing organic photoanodes has been computationally designed and fabricated and the implementation of a double PM6:Y6 photoanode/photovoltaic structure resulted in photogenerated currents exceeding 7mA cm^(-2) at 0 VRHE(hydrogen evolution thermodynamic potential)and anodic current onset potentials as low as-0.5 VRHE.The herein-presented organic-based approach paves the way for further exploration of different blend combinations to target specific oxidative reactions by selecting precise donor/acceptor candidates among the multiple existing ones.展开更多
Short tandem repeats(STRs)modulate gene expression and contribute to trait variation.However,a systematic evaluation of the genomic characteristics of STRs has not been conducted,and their influence on gene expression...Short tandem repeats(STRs)modulate gene expression and contribute to trait variation.However,a systematic evaluation of the genomic characteristics of STRs has not been conducted,and their influence on gene expression in rice remains unclear.Here,we construct a map of 137,629 polymorphic STRs in the rice(Oryza sativa L.)genome using a population-scale resequencing dataset.A genome-wide survey encompassing 4726 accessions shows that the occurrence frequency,mutational patterns,chromosomal distribution,and functional properties of STRs are correlated with the sequences and lengths of repeat motifs.Leveraging a transcriptome dataset from 127 rice accessions,we identify 44,672 expression STRs(eSTRs)by modeling gene expression in response to the length variation of STRs.These eSTRs are notably enriched in the regulatory regions of genes with active transcriptional signatures.Population analysis identifies numerous STRs that have undergone genetic divergence among different rice groups and 1726 tagged STRs that may be associated with agronomic traits.By editing the(ACT)_(7) STR in OsFD1 promoter,we further experimentally validate its role in regulating gene expression and phenotype.Our study highlights the contribution of STRs to transcriptional regulation in plants and establishes the foundation for their potential use as alternative targets for genetic improvement.展开更多
Tandem solar cells(TSCs)represent an attractive technology that can overcome the single-junction Shockdey-Queisser limit.Recently,a tandem structure combining wide-bandgap metal halide perovskite with complementary ba...Tandem solar cells(TSCs)represent an attractive technology that can overcome the single-junction Shockdey-Queisser limit.Recently,a tandem structure combining wide-bandgap metal halide perovskite with complementary bandgap copper indium gallium selenide(CIGS)photovoltaic technology has demonstrated a realistic pathway to achieve the industrialization goal of pushing power conversion efficiency(PCE)approaching 30% at low-cost.In this review,we first pinpoint the unique advantage of perovskite/CIGS tandems with respect to the other mainstream photovoltaic technologies and retrospect the research progress of perovskite/CIGS TSCs from both PCE and stability perspective in the last years.Next,we comprehensively discuss the major advancements in absorbers,functional layers of the individual sub-cell,and the interconnection layer between them in the recent decade.Finally,we outline several essential scientific and engineering challenges that are to be solved toward the development of efficient,long-term stable,and large-area perovskite/CIGS TSCs in the future.展开更多
Traditional electrospray ionization tandem mass spectrometry(ESI-MS^(n))has been a powerful tool in diverse research areas,however,it faces great limitations in the study of protein-small molecule interactions.In this...Traditional electrospray ionization tandem mass spectrometry(ESI-MS^(n))has been a powerful tool in diverse research areas,however,it faces great limitations in the study of protein-small molecule interactions.In this article,the state-of-the-art temperature-controlled electrospray ionization tandem mass spectrometry(TC-ESI-MS^(n))is applied to investigate interactions between ubiquitin and two flavonol molecules,respectively.The combination of collision-induced dissociation(CID)and MS solution-melting experiments facilitates the understanding of flavonol-protein interactions in a new dimension across varying temperature ranges.While structural changes of proteins disturbed by small molecules are unseen in ESI-MS^(n),TC-ESI-MS^(n)allows a simultaneous assessment of the stability of the complex in both gas and liquid phases under various temperature conditions,meanwhile investigating the impact on the protein’s structure and tracking changes in thermodynamic data,and the characteristics of structural intermediates.展开更多
All-perovskite tandem solar cells have the potential to surpass the theoretical efficiency limit of single junction solar cells by reducing thermalization losses.However,the challenges encompass the oxidation of Sn^(2...All-perovskite tandem solar cells have the potential to surpass the theoretical efficiency limit of single junction solar cells by reducing thermalization losses.However,the challenges encompass the oxidation of Sn^(2+)to Sn^(4+)and uncontrolled crystallization kinetics in Sn-Pb perovskites,leading to nonradiative recombination and compositional heterogeneity to decrease photovoltaic efficiency and operational stability.Herein,we introduced an ionic liquid additive,1-ethyl-3-methylimidazolium iodide (EMIMI) into Sn-Pb perovskite precursor to form low-dimensional Sn-rich/pure-Sn perovskites at grain boundaries,which mitigates oxidation of Sn^(2+)to Sn^(4+)and regulates the film-forming dynamics of Sn/Pb-based perovskite films.The optimized single-junction Sn-Pb perovskite devices incorporating EMIMI achieved a high efficiency of 22.87%.Furthermore,combined with wide-bandgap perovskite sub-cells in tandem device,we demonstrate 2-terminal all-perovskite tandem solar cells with a power conversion efficiency of 28.34%,achieving improved operational stability.展开更多
The development of high-voltage tandem thin-film supercapacitors(TFSCs)has been limited by the issues such as expensive electrode materials,indispensable commercial separators and metal current collectors,and complex ...The development of high-voltage tandem thin-film supercapacitors(TFSCs)has been limited by the issues such as expensive electrode materials,indispensable commercial separators and metal current collectors,and complex manufacturing processes.Herein,we develop a potentially scalable approach to address all these issues by using CO_(2) laser pyrolysis of polyimide(PI)paper into the three-dimensional(3D)morphology of graphene paper in air.The formation process and mechanism of PI to graphene were clarified by microstructure and chemical characterizations and reaction molecular dynamics.The influences of laser scan density,power,defocus,and scan speed on the sheet resistance,longitudinal resistance,Raman spectra,and electrochemical performance of graphene papers were systematically investigated.Results indicate that high-quality graphene papers with ultralow sheet resistance(4.88Ω·square^(-1))and longitudinal resistance(3.46Ω)and extra-large crystalline size(96.1 nm)were achieved under optimized process parameters.The graphene papers can simultaneously serve as active electrode materials,current collectors,and interconnectors.The active area of electrodes is defined by a PI mask,with the help of which a hydrogel electrolyte functions as a separator.The assembled graphene paper-based TFSCs demonstrate outstanding electrochemical performance and mechanical flexibility,with the areal capacitance of 54.5 mF·cm^(-2),energy density of 10.9µWh·cm^(-2),and cycle stability retention of 86.9%over 15000 cycles.Moreover,all the tandem metal-free TFSCs,ranging from 1 to 160 cells,show excellent performance uniformity.The output voltage increases linearly from 1.2 V to 200 V.Significantly,the 160-tandem TFSCs exhibit a high voltage density within a compact volume of∼3.8 cm^(3).This work provides an avenue for achieving tandem metal-free TFSCs in a simple and efficient manner.展开更多
To facilitate the low-noise design of tandem lift bodies as applied in aeroengines and aircraft,the acoustic features of tandem blades are investigated by wind-tunnel experiments.This is further specialized for the ro...To facilitate the low-noise design of tandem lift bodies as applied in aeroengines and aircraft,the acoustic features of tandem blades are investigated by wind-tunnel experiments.This is further specialized for the rotating blades applied in contra-rotating open rotors under the concept of frozen-rotor.A 70-channel phased microphone array and nine high-precision free-field microphones are employed.The beamforming method,enhanced by a source filtering technique,is employed to locate noise sources,providing insights into the source patterns of blade-blade interaction noise concerning flow speed,blade spacing,and aft blade clipping.The results show the following:(A)Sources of tandem-blade noise exist in the form of concentrated source clusters,resulting in two major clusters:the mid-span interaction noise and the tip-induced noise.(B)These source clusters tend to separate as flow speed or blade spacing increases.(C)By increasing blade spacing,the band-pass filtered overall sound pressure level is reduced by 2.9 dB.(D)A two-phase noise suppression pattern is observed with blade clipping,resulting in a total reduction of 3.0 dB for the interaction noise through the removal of tip-induced noise sources and the replacement of mid-span noise sources.Based on these findings,suggestions concerning blade spacing and clipping are discussed.展开更多
All-inorganic perovskite materials exhibit exceptional thermal stability and promising candidates for tandem devices,while their application is still in the initial stage.Here,a metal halide doping strategy was implem...All-inorganic perovskite materials exhibit exceptional thermal stability and promising candidates for tandem devices,while their application is still in the initial stage.Here,a metal halide doping strategy was implemented to enhance device performance and stability for inverted CsPbI_(3)perovskite solar cells(PSCs),which are ideal for integration into perovskite/silicon tandem solar cells.The lanthanide compound terbium chloride(TbCl_(3))was employed to improve buried interface between[4-(3,6-Dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid(Me-4PACz)and perovskite layer,thereby enhancing the crystallinity of CsPbI_(3)films and passivating non-radiative recombination defects.Thus,the inverted CsPbI_(3)PSCs achieved an efficiency of 18.68%and demonstrated excellent stability against water and oxygen.Meanwhile,remarkable efficiencies of 29.40%and 25.44%were,respectively,achieved in four-terminal(4T)and two-terminal(2T)perovskite/silicon mechanically tandem devices,which are higher efficiencies among reported all-inorganic perovskite-based tandem solar cells.This study presents a novel approach for fabricating highly efficient and stable inverted all-inorganic PSCs and perovskite/silicon tandem solar cells.展开更多
Electrochemical CO_(2) reduction(ECR)driven by intermittent renewable energy sources is an emerging technology to achieve net-zero CO_(2) emissions.Tandem electrochemical CO_(2) reduction(T-ECR),employs tandem catalys...Electrochemical CO_(2) reduction(ECR)driven by intermittent renewable energy sources is an emerging technology to achieve net-zero CO_(2) emissions.Tandem electrochemical CO_(2) reduction(T-ECR),employs tandem catalysts with synergistic or complementary functions to efficiently convert CO_(2) into multi-carbon(C^(2+))products in a succession of reactions within single or sequentially coupled reactors.However,the lack of clear interpretation and systematic understanding of T-ECR mechanisms has resulted in suboptimal current outcomes.This review presents new perspectives and summarizes recent advancements in efficient T-ECR across various scales,including synergistic tandem catalysis at the microscopic scale,relay tandem catalysis at the mesoscopic scale,and tandem reactors at the macroscopic scale.We begin by outlining the principle of tandem catalysis,followed by discuss on tandem catalyst design,the electrode construction,and reactor configuration.Additionally,we address the challenges and prospects of tandem strategies,emphasizing the integration of machine learning,theoretical calculations,and advanced characterization techniques for developing industry-scale CO_(2) valorization.展开更多
Selective synthesis of value-added xylenes and para-xylene(PX)by CO_(2)hydrogenation reduces the dependence on fossil resource and relieves the environment burden derived from the greenhouse gas CO_(2).Herein,modified...Selective synthesis of value-added xylenes and para-xylene(PX)by CO_(2)hydrogenation reduces the dependence on fossil resource and relieves the environment burden derived from the greenhouse gas CO_(2).Herein,modified MCM-22 zeolite combined with ZnCeZrOx solid solution is reported to catalyze the tandem CO_(2)hydrogenation and toluene methylation reaction at a relatively low temperature(<603 K),showing xylene selectivity of 92.4%and PX selectivity of 62%(PX/X,67%)in total aromatics at a CO_(2)conversion of 7.7%,toluene conversion of 23.6%and low CO selectivity of 11.6%,as well as giving high STY of xylene(302.0 mg·h^(–1)·gcat^(–1))and PX(201.6 mg·h^(–1)·gcat^(–1)).The outstanding catalytic performances are closely related to decreased pore sizes and eliminated external surface acid sites in modified MCM-22,which promoted zeolite shape-selectivity and suppressed secondary reactions.展开更多
Despite significant advancements in the power conversion efficiency(PCE)of perovskite/silicon tandem solar cells,improving carrier management in top cells remains challenging due to the defective dual interfaces of wi...Despite significant advancements in the power conversion efficiency(PCE)of perovskite/silicon tandem solar cells,improving carrier management in top cells remains challenging due to the defective dual interfaces of wide-bandgap perovskite,particularly on textured silicon surfaces.Herein,a series of halide ions(Cl^(-),Br^(-),I^(-))substituted piperazinium salts are designed and synthesized as post-treatment modifiers for perovskite surfaces.Notably,piperazinium chloride induces an asymmetric bidirectional ions distribution from the top to the bottom surface,with large piperazinium cations concentrating at the perovskite surface and small chloride anions migrating downward to accumulate at the buried interface.This results in effective dual-interface defect passivation and energy band modulation,enabling wide-bandgap(1.68 eV)perovskite solar cells to achieve a PCE of 22.3%and a record product of open-circuit voltage×fill factor(84.4%relative to the Shockley-Queisser limit).Furthermore,the device retains 91.3%of its initial efficiency after 1200 h of maximum power point tracking without encapsulation.When integrated with double-textured silicon heterojunction solar cells,a remarkable PCE of 31.5%is achieved for a 1.04 cm^(2) monolithic perovskite/silicon tandem solar cell,exhibiting excellent long-term operational stability(T_(80)=755 h)without encapsulation in ambient air.This work provides a convenient strategy on dual-interface engineering for making high-efficiency and stable perovskite platforms.展开更多
The production of renewable methanol(CH_(3)OH)via the photocatalytic hydrogenation of CO_(2) is an ideal method to ameliorate energy shortages and mitigate CO_(2) emissions:however,the highly selective synthesis of me...The production of renewable methanol(CH_(3)OH)via the photocatalytic hydrogenation of CO_(2) is an ideal method to ameliorate energy shortages and mitigate CO_(2) emissions:however,the highly selective synthesis of methanol at atmospheric pressure remains challenging owing to the competing reverse water-gas shift(RWGS)reaction.Herein,we present a novel approach for the synthesis of CH_(3)OH via photocatalytic CO_(2) hydrogenation using a catalyst featuring highly dispersed Au nanoparticles loaded on oxygen vacancy(OV)-rich molybdenum dioxide(MoO_(2)),resulting in a remarkable selectivity of 43.78%.The active sites in the Au/MoO_(2) catalyst are high-density Au-oxygen vacancies,which synergistically promote the tandem methanol synthesis via an initial RWGS reaction and subsequent CO hydrogenation.This work provides comprehensive insights into the design of metal-vacancy synergistic sites for the highly selective photocatalytic hydrogenation of CO_(2) to CH_(3)OH.展开更多
Developing high-performance narrow-bandgap (NBG) perovskite solar cells based on tin-lead (Sn-Pb) perovskite is critical for the advancement of all-perovskite tandem solar cells. However, the limitations of the device...Developing high-performance narrow-bandgap (NBG) perovskite solar cells based on tin-lead (Sn-Pb) perovskite is critical for the advancement of all-perovskite tandem solar cells. However, the limitations of the device current density and efficiency are magnified by the issues concerning poor carrier transport caused by a substantial number of defects in thick NBG films. This problem is further exacerbated by the quality of film crystallization, which is associated with the rapid and uncontrolled crystallization of Sn-rich perovskite chemistry using the antisolvent approach. We regulate the crystallization of Sn-contained perovskite with a mild gas-quench approach to fabricate a highly crystal-oriented and well-arranged NBG perovskite absorber. This strategy effectively boosts electron transport and light absorption of the NBG perovskite. Consequently, the average power conversion efficiency (PCE) of the NBG perovskite solar cells increases from 19.50% to 21.18%, with the best device achieving an excellent PCE of 21.84%. Furthermore, when combined with a wide-bandgap perovskite subcell to form an all-perovskite tandem solar cell, a PCE of 25.23% is achieved. After being stored in the glovebox for 1000 h, the unencapsulated device maintains over 90% of its initial PCE, demonstrating long-term stability and durability. This work presents a promising approach for developing high-efficiency NBG perovskite solar cells.展开更多
The CO_(2) reduction reaction(CO_(2)RR)is notable for itsmultiple advantages,such as mild reaction conditions,controllable product output,and ease of operation.The chemistry of CO_(2)RR to producemulticarbon products ...The CO_(2) reduction reaction(CO_(2)RR)is notable for itsmultiple advantages,such as mild reaction conditions,controllable product output,and ease of operation.The chemistry of CO_(2)RR to producemulticarbon products involvesmultiple electron-proton transfer steps,in which the adsorption of CO intermediates is usually the key rate-determining step of the reaction.Currently,Cu is the only metal catalyst known to efficiently reduce CO_(2) tomulticarbon products,mainly due to its appropriate adsorption energy for CO intermediates.However,single Cu catalysts often face challenges such as excessively high overpotentials and poor selectivity,which limit their potential application in CO_(2) reduction.In recent years,electrochemical CO_(2) reduction using copper-based tandem catalysts has become an effective strategy to enhance the overall performance of CO_(2)RR and a hot topic in the research field.Here we review recent research advances in the field of electrochemical CO_(2)RR where tandemmethods have been applied.Themajor points are the following:(1)the tandem process allows for more precise control of the electrochemical reduction pathway,thereby increasing the yield of the target product while reducing the generation of by-products;(2)Mass transportation of *CO intermediates and spatial management is important for the generation of multicarbon products;(3)a variety of tandem means for upgrading the product to a deeply reduced product are reviewed.展开更多
基金supported by Chongqing Key Laboratory of New Energy Materials and Devices,and Wuhan University Key Lab of Artificial Micro-and Nano-Structures of Ministry of Education of China.The authors also acknowledge the financial support from the Chongqing University of Technology(2024ZDZ029).
文摘Wide-bandgap(WBG)perovskite solar cells(PSCs)have gained remarkable interest owing to their latent applications in tandem solar cells(TSCs).Among them,four-terminal(4T)all-perovskite TSCs have received extensive attention as its do without need to consider current matching,surface roughness,and fabrication processes.However,low open-circuit voltage(VOC)and efficiency of WBG PSCs obstacles their applications in 4T allperovskite TSCs.Hence,this review firstly discussed the optimizing strategy in perovskite materials layer and properties.Specifically,we assessed the effect of composition,additive and interface engineering on the efficiency and VOC of WBG PSCs.Secondly,the demonstrated applications of different passivation layers designing for intensifying the efficiency of WBG PSCs and 4T all-perovskite TSCs is discussed.Finally,we put forward three specific approaches for future research,in our view,which would offer appropriate guidance for the exploitation of highly efficient and stable 4T all-perovskite TSCs.
基金supported by the National Key Research and Development Program of China(2023YFB4202503)the cooperation project between Three Gorges Corporation and Nankai University(202103571)+6 种基金the National Natural Science Foundation Joint Fund(U21A2072)the National Science Foundation(62274099,62104115)Tianjin Science and Technology Project(24ZXZSSS00160)Yunnan Provincial Science and Technology Project at Southwest United Graduate School(202302A0370009)the China Higher Education Discipline Innovation Overseas Expert Introduction Project(B16027)the Haihe Laboratory of Sustainable Chemical Transformationsthe Fundamental Research Funds for the Central Universities,Nankai University。
文摘[4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid(Me-4PACz)self-assembled monolayer(SAM)as the hole transport materials have been demonstrated remarkable potential in perovskite solar cells(PSCs).However,the hydrophobicity of Me-4PACz presents a critical challenge for the fabrication of high-quality perovskite films due to its poor wettability.Here,a doped Al_(2)O_(3)with Me-4PACz to modify the Me-4PACz surface was proposed.On one hand,this approach improved the wettability of the Me-4PACz film,enhancing the coverage,uniformity,and buried interface properties of the perovskite film.On the other hand,compared to Al_(2)O_(3)modification alone,doping Al_(2)O_(3)with Me-4PACz allowed direct contact between the perovskite and Me-4PACz,resulting in better buried interface passivation.As a result,we achieved an efficiency of 22.71%for single-junction wide-bandgap perovskite solar cells(1.68 eV).Additionally,the efficiency of perovskite/silicon tandem solar cells was improved from 28.68%to 30.92%,with a significant reduction in hysteresis.Furthermore,the tandem cells demonstrated no degradation after 4200 s of operation at the maximum power point.
文摘The CO_(2)-assisted oxidative dehydrogenation of ethane(CO_(2)-ODHE)provides a promising way to produce ethylene and utilize CO_(2).Simultaneous upgrading of ethane into the high value-added chemical products and the reduction of greenhouse gas CO_(2)emissions could be achieved.However,the targeted breaking of the C-C/C-H bonds of ethane is still a challenge for the designed catalysts.In this paper,ZnO-doped ZrO_(2)bifunctional catalysts(Zn_(x)ZrO)with different Zn/Zr molar ratios were prepared by the deposition-precipitation method,and the functions of various sites for CO_(2)-ODHE reaction were revealed by in situ characterizations and ethane pulse experiment:the medium-strength acidic Zn-O-Zr sites are responsible for the purposefully cracking of ethane C-H bonds to ethylene,while the more oxygen vacancies(OV)created by the introduction of Zn^(2+)are responsible for the efficient activation C=O bonds of CO_(2),thus promoting the RWGS reaction.In addition,the Zn0.2ZrO catalyst demonstrated excellent catalytic performances,with C_(2)H_(6)conversion,C_(2)H_(4)yield,and CO_(2)conversion about 19.1%,10.5%,and 10.6%within 5 h,respectively(600℃,GHSV=3000 mL/(g·h)).Especially,the initial ethylene space-time yield of 355.5μmol/(min·g)was obtained under 6000 mL/(g·h);Finally,the tandem reaction mechanism of ethane dehydrogenation and RWGS was revealed.
文摘Solar energy, as a renewable resource, is an effective solution to the current global energy shortage problem. To actively respond to the call for "carbon peak" and "carbon neutrality", solar cell industry has experienced unprecedented development. The full utilization of solar energy resources remains an urgent issue to be addressed.
基金financially supported by National Key R&D Program of China (2025YFE0100300)the National Natural Science Foundation of China (52202293 and 52330004)the Fundamental Research Funds for the Central Universities (WUT: 2023IVA075 and 2023IVB009)。
文摘All-perovskite tandem solar cells(ATSCs) have the potential to surpass the Shockley-Queisser efficiency limit of conventional single-junction devices. However, the performance and stability of mixed tin–lead(Sn–Pb) perovskite solar cells(PSCs), which are crucial components of ATSCs, are much lower than those of lead-based perovskites. The primary challenges include the high crystallization rate of perovskite materials and the susceptibility of Sn^(2+) oxidation, which leads to rough morphology and unfavorable p-type self-doping. To address these issues, we introduced ethylhydrazine oxalate(EDO) at the perovskite interface, which effectively inhibits the oxidation of Sn^(2+) and simultaneously enhances the crystallinity of the perovskite. Consequently, the EDO-modified mixed tin-lead PSCs reached a power conversion efficiency(PCE) of 21.96% with high reproducibility. We further achieved a 27.58% efficient ATSCs by using EDO as interfacial passivator in the Sn-Pb PSCs.
基金partly funded by a BIST Ignite Programme grant from the Barcelona Institute of Science and Technology(Code:MOLOPEC)financial support from LICROX and SOREC2 EUFunded projects(Codes:951843 and 101084326)+7 种基金the BIST Program,and Severo Ochoa Programpartially funded by CEX2019-000910-S(MCIN/AEI/10.13039/501100011033 and PID2020-112650RBI00),Fundació Cellex,Fundació Mir-PuigGeneralitat de Catalunya through CERCAfunding from the European Union’s Horizon Europe research and innovation programme under the Marie Skłodowska-Curie grant agreement No 101081441financial support by the Agencia Estatal de Investigación(grant PRE2018-084881)the financial support by from the European Union’s Horizon Europe research and innovation programme under the Marie Skłodowska-Curie grant agreement No 101081441support from the MCIN/AEI JdC-F Fellowship(FJC2020-043223-I)the Severo Ochoa Excellence Postdoctoral Fellowship(CEX2019-000910-S).
文摘This study first demonstrates the potential of organic photoabsorbing blends in overcoming a critical limitation of metal oxide photoanodes in tandem modules:insufficient photogenerated current.Various organic blends,including PTB7-Th:FOIC,PTB7-Th:O6T-4F,PM6:Y6,and PM6:FM,were systematically tested.When coupled with electron transport layer(ETL)contacts,these blends exhibit exceptional charge separation and extraction,with PM6:Y6 achieving saturation photocurrents up to 16.8 mA cm^(-2) at 1.23 VRHE(oxygen evolution thermodynamic potential).For the first time,a tandem structure utilizing organic photoanodes has been computationally designed and fabricated and the implementation of a double PM6:Y6 photoanode/photovoltaic structure resulted in photogenerated currents exceeding 7mA cm^(-2) at 0 VRHE(hydrogen evolution thermodynamic potential)and anodic current onset potentials as low as-0.5 VRHE.The herein-presented organic-based approach paves the way for further exploration of different blend combinations to target specific oxidative reactions by selecting precise donor/acceptor candidates among the multiple existing ones.
基金supported by the National Natural Science Foundation of China(32172010)the Major Program of Guangdong Basic and Applied Basic Research(2019B030302006).
文摘Short tandem repeats(STRs)modulate gene expression and contribute to trait variation.However,a systematic evaluation of the genomic characteristics of STRs has not been conducted,and their influence on gene expression in rice remains unclear.Here,we construct a map of 137,629 polymorphic STRs in the rice(Oryza sativa L.)genome using a population-scale resequencing dataset.A genome-wide survey encompassing 4726 accessions shows that the occurrence frequency,mutational patterns,chromosomal distribution,and functional properties of STRs are correlated with the sequences and lengths of repeat motifs.Leveraging a transcriptome dataset from 127 rice accessions,we identify 44,672 expression STRs(eSTRs)by modeling gene expression in response to the length variation of STRs.These eSTRs are notably enriched in the regulatory regions of genes with active transcriptional signatures.Population analysis identifies numerous STRs that have undergone genetic divergence among different rice groups and 1726 tagged STRs that may be associated with agronomic traits.By editing the(ACT)_(7) STR in OsFD1 promoter,we further experimentally validate its role in regulating gene expression and phenotype.Our study highlights the contribution of STRs to transcriptional regulation in plants and establishes the foundation for their potential use as alternative targets for genetic improvement.
基金funding support from the National Key Research and Development Program of China(Grant No.2020YFB0408002)the Beijing Natural Science Foundation(Z240024)+2 种基金the National Natural Science Foundation of China(Grant Nos.22279083,22461160281,W2412076)the Guangdong Basic and Applied Basic Research Foundation(Grant No.2022B1515120006)the Central Guiding Local Science and Technology Development Special Fund Project(Grant No.ZYYD2024JD24)。
文摘Tandem solar cells(TSCs)represent an attractive technology that can overcome the single-junction Shockdey-Queisser limit.Recently,a tandem structure combining wide-bandgap metal halide perovskite with complementary bandgap copper indium gallium selenide(CIGS)photovoltaic technology has demonstrated a realistic pathway to achieve the industrialization goal of pushing power conversion efficiency(PCE)approaching 30% at low-cost.In this review,we first pinpoint the unique advantage of perovskite/CIGS tandems with respect to the other mainstream photovoltaic technologies and retrospect the research progress of perovskite/CIGS TSCs from both PCE and stability perspective in the last years.Next,we comprehensively discuss the major advancements in absorbers,functional layers of the individual sub-cell,and the interconnection layer between them in the recent decade.Finally,we outline several essential scientific and engineering challenges that are to be solved toward the development of efficient,long-term stable,and large-area perovskite/CIGS TSCs in the future.
基金supports by the National Natural Science Foundation of China(No.22174037)the Joint Funds of the Hunan Provincial Natural Science Foundation of China(No.2023JJ50255)+1 种基金Changsha Science and Technology Project(No.Z202269490128)National Key Research and Development Program of China(No.2023YFF0613400)are appreciated.
文摘Traditional electrospray ionization tandem mass spectrometry(ESI-MS^(n))has been a powerful tool in diverse research areas,however,it faces great limitations in the study of protein-small molecule interactions.In this article,the state-of-the-art temperature-controlled electrospray ionization tandem mass spectrometry(TC-ESI-MS^(n))is applied to investigate interactions between ubiquitin and two flavonol molecules,respectively.The combination of collision-induced dissociation(CID)and MS solution-melting experiments facilitates the understanding of flavonol-protein interactions in a new dimension across varying temperature ranges.While structural changes of proteins disturbed by small molecules are unseen in ESI-MS^(n),TC-ESI-MS^(n)allows a simultaneous assessment of the stability of the complex in both gas and liquid phases under various temperature conditions,meanwhile investigating the impact on the protein’s structure and tracking changes in thermodynamic data,and the characteristics of structural intermediates.
基金National Key Research and Development Program of China (2022YFB420030)National Natural Science Foundation of China (2227903)+1 种基金Innovation Project of Optics Valley Laboratory (OVL2021BG008)Foundation of State Key Laboratory of New Textile Materials and Advanced Processing Technologies (FZ2021011)。
文摘All-perovskite tandem solar cells have the potential to surpass the theoretical efficiency limit of single junction solar cells by reducing thermalization losses.However,the challenges encompass the oxidation of Sn^(2+)to Sn^(4+)and uncontrolled crystallization kinetics in Sn-Pb perovskites,leading to nonradiative recombination and compositional heterogeneity to decrease photovoltaic efficiency and operational stability.Herein,we introduced an ionic liquid additive,1-ethyl-3-methylimidazolium iodide (EMIMI) into Sn-Pb perovskite precursor to form low-dimensional Sn-rich/pure-Sn perovskites at grain boundaries,which mitigates oxidation of Sn^(2+)to Sn^(4+)and regulates the film-forming dynamics of Sn/Pb-based perovskite films.The optimized single-junction Sn-Pb perovskite devices incorporating EMIMI achieved a high efficiency of 22.87%.Furthermore,combined with wide-bandgap perovskite sub-cells in tandem device,we demonstrate 2-terminal all-perovskite tandem solar cells with a power conversion efficiency of 28.34%,achieving improved operational stability.
基金funded by the National Natural Science Foundation of China(Grant Nos.52205457 and 52422511)the National Key R&D Program of China(Grant No.2022YFB4701000)+3 种基金the Guangdong Basic and Applied Basic Research Foundation,China(Grant Nos.2024A1515010043,2025A1515010890 and 2022B1515120011)the Young Talent Support Project of Guangzhou Association for Science and Technology(Grant No.QT2024-010)the Guangzhou Basic and Applied Basic Research Foundation(Grant No.SL2024A04J01501)the State Key Laboratory of Precision Electronic Manufacturing Technology and Equipment(Grant No.JMDZ202303).
文摘The development of high-voltage tandem thin-film supercapacitors(TFSCs)has been limited by the issues such as expensive electrode materials,indispensable commercial separators and metal current collectors,and complex manufacturing processes.Herein,we develop a potentially scalable approach to address all these issues by using CO_(2) laser pyrolysis of polyimide(PI)paper into the three-dimensional(3D)morphology of graphene paper in air.The formation process and mechanism of PI to graphene were clarified by microstructure and chemical characterizations and reaction molecular dynamics.The influences of laser scan density,power,defocus,and scan speed on the sheet resistance,longitudinal resistance,Raman spectra,and electrochemical performance of graphene papers were systematically investigated.Results indicate that high-quality graphene papers with ultralow sheet resistance(4.88Ω·square^(-1))and longitudinal resistance(3.46Ω)and extra-large crystalline size(96.1 nm)were achieved under optimized process parameters.The graphene papers can simultaneously serve as active electrode materials,current collectors,and interconnectors.The active area of electrodes is defined by a PI mask,with the help of which a hydrogel electrolyte functions as a separator.The assembled graphene paper-based TFSCs demonstrate outstanding electrochemical performance and mechanical flexibility,with the areal capacitance of 54.5 mF·cm^(-2),energy density of 10.9µWh·cm^(-2),and cycle stability retention of 86.9%over 15000 cycles.Moreover,all the tandem metal-free TFSCs,ranging from 1 to 160 cells,show excellent performance uniformity.The output voltage increases linearly from 1.2 V to 200 V.Significantly,the 160-tandem TFSCs exhibit a high voltage density within a compact volume of∼3.8 cm^(3).This work provides an avenue for achieving tandem metal-free TFSCs in a simple and efficient manner.
基金supported by grants from the National Natural Science Foundation of China(Nos.12102451,12072186)the National Science and Technology Major Project,China(No.J2019-II-0006-0026)AVIC Aerodynamics Research Institute,China(No.XFX20220201).
文摘To facilitate the low-noise design of tandem lift bodies as applied in aeroengines and aircraft,the acoustic features of tandem blades are investigated by wind-tunnel experiments.This is further specialized for the rotating blades applied in contra-rotating open rotors under the concept of frozen-rotor.A 70-channel phased microphone array and nine high-precision free-field microphones are employed.The beamforming method,enhanced by a source filtering technique,is employed to locate noise sources,providing insights into the source patterns of blade-blade interaction noise concerning flow speed,blade spacing,and aft blade clipping.The results show the following:(A)Sources of tandem-blade noise exist in the form of concentrated source clusters,resulting in two major clusters:the mid-span interaction noise and the tip-induced noise.(B)These source clusters tend to separate as flow speed or blade spacing increases.(C)By increasing blade spacing,the band-pass filtered overall sound pressure level is reduced by 2.9 dB.(D)A two-phase noise suppression pattern is observed with blade clipping,resulting in a total reduction of 3.0 dB for the interaction noise through the removal of tip-induced noise sources and the replacement of mid-span noise sources.Based on these findings,suggestions concerning blade spacing and clipping are discussed.
基金the financial support from the National Natural Science Foundation of China(62274132,62204189,62274126)the Postdoctoral Fellowship Program of CPSF(GZC20241301)+1 种基金Fundamental Research Funds for the Central Universities(ZYTS25221)the National Key R&D Program of China(2022YFB3605402,2021YFF0500501)。
文摘All-inorganic perovskite materials exhibit exceptional thermal stability and promising candidates for tandem devices,while their application is still in the initial stage.Here,a metal halide doping strategy was implemented to enhance device performance and stability for inverted CsPbI_(3)perovskite solar cells(PSCs),which are ideal for integration into perovskite/silicon tandem solar cells.The lanthanide compound terbium chloride(TbCl_(3))was employed to improve buried interface between[4-(3,6-Dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid(Me-4PACz)and perovskite layer,thereby enhancing the crystallinity of CsPbI_(3)films and passivating non-radiative recombination defects.Thus,the inverted CsPbI_(3)PSCs achieved an efficiency of 18.68%and demonstrated excellent stability against water and oxygen.Meanwhile,remarkable efficiencies of 29.40%and 25.44%were,respectively,achieved in four-terminal(4T)and two-terminal(2T)perovskite/silicon mechanically tandem devices,which are higher efficiencies among reported all-inorganic perovskite-based tandem solar cells.This study presents a novel approach for fabricating highly efficient and stable inverted all-inorganic PSCs and perovskite/silicon tandem solar cells.
文摘Electrochemical CO_(2) reduction(ECR)driven by intermittent renewable energy sources is an emerging technology to achieve net-zero CO_(2) emissions.Tandem electrochemical CO_(2) reduction(T-ECR),employs tandem catalysts with synergistic or complementary functions to efficiently convert CO_(2) into multi-carbon(C^(2+))products in a succession of reactions within single or sequentially coupled reactors.However,the lack of clear interpretation and systematic understanding of T-ECR mechanisms has resulted in suboptimal current outcomes.This review presents new perspectives and summarizes recent advancements in efficient T-ECR across various scales,including synergistic tandem catalysis at the microscopic scale,relay tandem catalysis at the mesoscopic scale,and tandem reactors at the macroscopic scale.We begin by outlining the principle of tandem catalysis,followed by discuss on tandem catalyst design,the electrode construction,and reactor configuration.Additionally,we address the challenges and prospects of tandem strategies,emphasizing the integration of machine learning,theoretical calculations,and advanced characterization techniques for developing industry-scale CO_(2) valorization.
文摘Selective synthesis of value-added xylenes and para-xylene(PX)by CO_(2)hydrogenation reduces the dependence on fossil resource and relieves the environment burden derived from the greenhouse gas CO_(2).Herein,modified MCM-22 zeolite combined with ZnCeZrOx solid solution is reported to catalyze the tandem CO_(2)hydrogenation and toluene methylation reaction at a relatively low temperature(<603 K),showing xylene selectivity of 92.4%and PX selectivity of 62%(PX/X,67%)in total aromatics at a CO_(2)conversion of 7.7%,toluene conversion of 23.6%and low CO selectivity of 11.6%,as well as giving high STY of xylene(302.0 mg·h^(–1)·gcat^(–1))and PX(201.6 mg·h^(–1)·gcat^(–1)).The outstanding catalytic performances are closely related to decreased pore sizes and eliminated external surface acid sites in modified MCM-22,which promoted zeolite shape-selectivity and suppressed secondary reactions.
基金supported by the National Natural Science Foundation of China(Grant No.62204245,U23A200098)Baima Lake Laboratory Joint Funds of the Zhejiang Provincial Natural Science Foundation of China(Grant No.LBMHD24E020002)+4 种基金Key Research and Development Program of Zhejiang Province(Grant No.2022C01215,2024C01092)China Postdoctoral Science Foundation(Grant No.2023M743620,2024T170960)Key Research and Development Program of Ningbo(Grant No.2023Z151)National Key Research and Development Program of China(Grant No.2024YFB3817304)Zhejiang Provincial Natural Science Foundation of China(Grant No.LY24F040003).
文摘Despite significant advancements in the power conversion efficiency(PCE)of perovskite/silicon tandem solar cells,improving carrier management in top cells remains challenging due to the defective dual interfaces of wide-bandgap perovskite,particularly on textured silicon surfaces.Herein,a series of halide ions(Cl^(-),Br^(-),I^(-))substituted piperazinium salts are designed and synthesized as post-treatment modifiers for perovskite surfaces.Notably,piperazinium chloride induces an asymmetric bidirectional ions distribution from the top to the bottom surface,with large piperazinium cations concentrating at the perovskite surface and small chloride anions migrating downward to accumulate at the buried interface.This results in effective dual-interface defect passivation and energy band modulation,enabling wide-bandgap(1.68 eV)perovskite solar cells to achieve a PCE of 22.3%and a record product of open-circuit voltage×fill factor(84.4%relative to the Shockley-Queisser limit).Furthermore,the device retains 91.3%of its initial efficiency after 1200 h of maximum power point tracking without encapsulation.When integrated with double-textured silicon heterojunction solar cells,a remarkable PCE of 31.5%is achieved for a 1.04 cm^(2) monolithic perovskite/silicon tandem solar cell,exhibiting excellent long-term operational stability(T_(80)=755 h)without encapsulation in ambient air.This work provides a convenient strategy on dual-interface engineering for making high-efficiency and stable perovskite platforms.
文摘The production of renewable methanol(CH_(3)OH)via the photocatalytic hydrogenation of CO_(2) is an ideal method to ameliorate energy shortages and mitigate CO_(2) emissions:however,the highly selective synthesis of methanol at atmospheric pressure remains challenging owing to the competing reverse water-gas shift(RWGS)reaction.Herein,we present a novel approach for the synthesis of CH_(3)OH via photocatalytic CO_(2) hydrogenation using a catalyst featuring highly dispersed Au nanoparticles loaded on oxygen vacancy(OV)-rich molybdenum dioxide(MoO_(2)),resulting in a remarkable selectivity of 43.78%.The active sites in the Au/MoO_(2) catalyst are high-density Au-oxygen vacancies,which synergistically promote the tandem methanol synthesis via an initial RWGS reaction and subsequent CO hydrogenation.This work provides comprehensive insights into the design of metal-vacancy synergistic sites for the highly selective photocatalytic hydrogenation of CO_(2) to CH_(3)OH.
基金supported by the National Key Research and Development Program of China(Grant No.2020YFB1506400)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB43000000)+3 种基金the CAS Project for Young Scientists in Basic Research(YSBR-090)the National Natural Science Foundation of China(Contract Nos.U20A20206,51972300,62274155,and 62304219)support from the Youth Innovation Promotion Association,the Chi-nese Academy of Sciences(No.2020114)Beijing Natural Sci-ence Foundation(Grant No.JQ24029).
文摘Developing high-performance narrow-bandgap (NBG) perovskite solar cells based on tin-lead (Sn-Pb) perovskite is critical for the advancement of all-perovskite tandem solar cells. However, the limitations of the device current density and efficiency are magnified by the issues concerning poor carrier transport caused by a substantial number of defects in thick NBG films. This problem is further exacerbated by the quality of film crystallization, which is associated with the rapid and uncontrolled crystallization of Sn-rich perovskite chemistry using the antisolvent approach. We regulate the crystallization of Sn-contained perovskite with a mild gas-quench approach to fabricate a highly crystal-oriented and well-arranged NBG perovskite absorber. This strategy effectively boosts electron transport and light absorption of the NBG perovskite. Consequently, the average power conversion efficiency (PCE) of the NBG perovskite solar cells increases from 19.50% to 21.18%, with the best device achieving an excellent PCE of 21.84%. Furthermore, when combined with a wide-bandgap perovskite subcell to form an all-perovskite tandem solar cell, a PCE of 25.23% is achieved. After being stored in the glovebox for 1000 h, the unencapsulated device maintains over 90% of its initial PCE, demonstrating long-term stability and durability. This work presents a promising approach for developing high-efficiency NBG perovskite solar cells.
基金supported by the National Natural Science Foundation of China(No.52270078)the Fundamental Research Funds for the Central Universities(No.xzy022023039).
文摘The CO_(2) reduction reaction(CO_(2)RR)is notable for itsmultiple advantages,such as mild reaction conditions,controllable product output,and ease of operation.The chemistry of CO_(2)RR to producemulticarbon products involvesmultiple electron-proton transfer steps,in which the adsorption of CO intermediates is usually the key rate-determining step of the reaction.Currently,Cu is the only metal catalyst known to efficiently reduce CO_(2) tomulticarbon products,mainly due to its appropriate adsorption energy for CO intermediates.However,single Cu catalysts often face challenges such as excessively high overpotentials and poor selectivity,which limit their potential application in CO_(2) reduction.In recent years,electrochemical CO_(2) reduction using copper-based tandem catalysts has become an effective strategy to enhance the overall performance of CO_(2)RR and a hot topic in the research field.Here we review recent research advances in the field of electrochemical CO_(2)RR where tandemmethods have been applied.Themajor points are the following:(1)the tandem process allows for more precise control of the electrochemical reduction pathway,thereby increasing the yield of the target product while reducing the generation of by-products;(2)Mass transportation of *CO intermediates and spatial management is important for the generation of multicarbon products;(3)a variety of tandem means for upgrading the product to a deeply reduced product are reviewed.
