Predicting tropical cyclone(TC)genesis is of great societal importance but scientifically challenging.It requires fineresolution coupled models that properly represent air−sea interactions in the atmospheric responses...Predicting tropical cyclone(TC)genesis is of great societal importance but scientifically challenging.It requires fineresolution coupled models that properly represent air−sea interactions in the atmospheric responses to local warm sea surface temperatures and feedbacks,with aid from coherent coupled initialization.This study uses three sets of highresolution regional coupled models(RCMs)covering the Asia−Pacific(AP)region initialized with local observations and dynamically downscaled coupled data assimilation to evaluate the predictability of TC genesis in the West Pacific.The APRCMs consist of three sets of high-resolution configurations of the Weather Research and Forecasting−Regional Ocean Model System(WRF-ROMS):27-km WRF with 9-km ROMS,and 9-km WRF with 3-km ROMS.In this study,a 9-km WRF with 9-km ROMS coupled model system is also used in a case test for the predictability of TC genesis.Since the local sea surface temperatures and wind shear conditions that favor TC formation are better resolved,the enhanced-resolution coupled model tends to improve the predictability of TC genesis,which could be further improved by improving planetary boundary layer physics,thus resolving better air−sea and air−land interactions.展开更多
Zeolites Y,A and mordenite(ZY,ZA and ZM)were obtained from diatomite in a template-free system,and the products were modified by thiourea(TU).Characterization studies results indicated that the TU molecules were loade...Zeolites Y,A and mordenite(ZY,ZA and ZM)were obtained from diatomite in a template-free system,and the products were modified by thiourea(TU).Characterization studies results indicated that the TU molecules were loaded onto the exterior surfaces of the synthetic zeolites as well as the channels.Elemental analysis and energy-dispersive X-ray spectrometer proved that the TU molecules loaded on to ZA were more than ZY and ZM.Removal of Cd(Ⅱ)was investigated,and itwas found that themodified zeolites have higher removal capacity,modified ZA is especially noticeable.In the adsorption experiments,the effects of various parameters such as sorbent content,contact time,concentration of cadmium solution,pH,selectivity and regeneration were discussed.At the best removal efficiency by modified zeolites,the maximum adsorption capacity is 94.3 mg·g^−1,103.2 mg·g^−1 and 89.7 mg·g^−1 at 25℃,respectively.The sorbents show good efficiency for the removal of Cd(Ⅱ)in the presence of different multivalent cations and have good regeneration effect.For the modified samples,removal experiments take place via ion exchange and complexation processes.展开更多
Compared to regular conjugated polymers,the random conjugated terpolymers are usually not beneficial to achieve highly efficient non-fullerene(NF)-based polymer solar cells(PSCs)due to their disordered chemical struct...Compared to regular conjugated polymers,the random conjugated terpolymers are usually not beneficial to achieve highly efficient non-fullerene(NF)-based polymer solar cells(PSCs)due to their disordered chemical structures.In this work,we report two random terpolymer donors(PBNB80 and PBNB50)by tuning the molar ratio of electron-accepting units of 1,3-di(thiophen-2-yl)naphtho[2,3-c]thiophene-4,9-dione(NTD)and 1,3-bis(4-chlorothiophen-2-yl)-4 H,8 H-benzo[1,2-c:4,5-c’]dithiophene-4,8-dione(ClBDD),at the same time,the parent polymers(PBNB100 and PBNB00)are also compared to study.These four polymer donors exhibit similar optical bandgaps and gradually deepen highest occupied molecular orbital levels.Importantly,aggregation and self-organization properties of the random terpolymer donors are optimized,which result in the better morphology and crystal coherence length after blending with NF acceptor of BO-4 Cl.Particularly,a PBNB80:BO-4 Cl blend forms an optimal nanoscale phase-separation morphology,thereby producing an outstanding power conversion efficiency of 16.0%,which is much higher than those(12.8%and 10.7%)of their parent binary polymer donor-based devices.This work demonstrates that rational using terpolymerization strategy to prepare random terpolymer is a very important method to achieve highly efficient NF-PSCs.展开更多
To further explore enthalpy-based sea-ice assimilation, a one-dimensional (1D) enthalpy sea-ice model is implemented into a simple pycnocline prediction model. The 1D enthalpy sea-ice model includes the physical pro...To further explore enthalpy-based sea-ice assimilation, a one-dimensional (1D) enthalpy sea-ice model is implemented into a simple pycnocline prediction model. The 1D enthalpy sea-ice model includes the physical processes such as brine expulsion, flushing, and salt diffusion. After being coupled with the atmosphere and ocean components, the enthalpy sea-ice model can be integrated stably and serves as an important modulator of model variability. Results from a twin experiment show that the sea-ice data assimilation in the enthalpy space can produce smaller root-mean-square errors of model variables than the traditional scheme that assimilates the observations of ice concentration, especially for slow-varying states. This study provides some insights into the improvement of sea-ice data assimilation in a coupled general circulation model.展开更多
That a model has sensitivity responses to parameter uncertainties is a key concept in implementing model parameter es- timation using filtering theory and methodology. Depending on the nature of associated physics and...That a model has sensitivity responses to parameter uncertainties is a key concept in implementing model parameter es- timation using filtering theory and methodology. Depending on the nature of associated physics and characteristic variability of the fluid in a coupled system, the response time scales of a model to parameters can be different, from hourly to decadal. Unlike state estimation, where the update frequency is usually linked with observational frequency, the update frequency for parameter estimation must be associated with the time scale of the model sensitivity response to the parameter being esti- mated. Here, with a simple coupled model, the impact of model sensitivity response time scales on coupled model parameter estimation is studied. The model includes characteristic synoptic to decadal scales by coupling a long-term varying deep ocean with a slow-varying upper ocean forced by a chaotic atmosphere. Results show that, using the update frequency deter- mined by the model sensitivity response time scale, both the reliability and quality of parameter estimation can be improved significantly, and thus the estimated parameters make the model more consistent with the observation. These simple model results provide a guideline for when real observations are used to optimize the parameters in a coupled general circulation model for improving climate analysis and prediction initialization.展开更多
On the basis of making clear diversity characteristics of soil functions and multiple characteristics of income, this paper points out that the monetization of soil functions based functional maintenance and change de...On the basis of making clear diversity characteristics of soil functions and multiple characteristics of income, this paper points out that the monetization of soil functions based functional maintenance and change decision process can be regarded as a game process of different utilization methods at the background of different functions. The balance of this game process will determine monetary value of soil functions. After understanding money and monetization concepts, it introduces that measurability and exchangeability of soil functions provide objective conditions for monetization of soil functions. Finally, it discusses that usefulness value of soil functions provide basis for monetization of soil functions.展开更多
Organic photovoltaic(OPV)cells have demonstrated remarkable performance in small,spin-coated areas.Nevertheless significant challenges persist in the form of large efficiency losses due to the fact that the ideal morp...Organic photovoltaic(OPV)cells have demonstrated remarkable performance in small,spin-coated areas.Nevertheless significant challenges persist in the form of large efficiency losses due to the fact that the ideal morphology cannot be preserved in the transition of small-area cells to large-scale panels.Herein,the ternary strategy of incorporating the third component FTCC-Br into the active layer of PB2:BTP-eC9 is employed to improve absorption response,optimize morphology,and reduce charge recombination,leading to a power conversion efficiency(PCE)of 19.5%(certified as 19.1%by the National Institute of Metrology,China).Moreover,the addition of FTCC-Br can control the aggregation kinetics of the active layer during the film formation process,transferring the optimal morphology to the blade-coated large-area films.Based on the highly efficient ternary bulk heterojunction,the 50 cm^(2) OPVmodules exhibited a PCE of 15.2%with respect to the active area.Importantly,the ternary OPV cells retain 80%of its initial PCE after 4000 h under continuous illumination.Our work demonstrates that the addition of a third component has the potential to improve the efficiency and stability of large-area organic solar cells.展开更多
The discovery of single-atom catalysts(SACs)represents a groundbreaking advancement in the field of catalysis over the past decades.With the in-depth exploration of relevant structure-activity relationships,the metal−...The discovery of single-atom catalysts(SACs)represents a groundbreaking advancement in the field of catalysis over the past decades.With the in-depth exploration of relevant structure-activity relationships,the metal−support interaction(MSI)is widely adopted to elucidate variations in electronic structure and coordination configuration of atomic active sites on various kinds of supports.Herein,we briefly summarize the metal oxide supports for SACs fabrication,including the distinctive characteristics of metal oxide supports,enlightening advancements in metal oxide support-based SACs(MO-SACs),feasible preparation methods for MO-SACs and effective regulation strategies of MSI effect in MO-SACs.In addition,we present our viewpoints and outlook in this field to stimulate rational design and construction of novel MO-SACs applied in diverse renewable energy devices,while some universal suggestions are sincerely given to provoke thoughtful considerations during the research process.展开更多
Owing to the function of manipulating light absorption distribution,tandem organic solar cells containing multiple sub-cells exhibit high power conversion efficiencies.However,there is a substantial challenge in preci...Owing to the function of manipulating light absorption distribution,tandem organic solar cells containing multiple sub-cells exhibit high power conversion efficiencies.However,there is a substantial challenge in precisely controlling the inter-subcells carrier migration which determines the balance of charge transport across the entire device.The conductivity of"nanowires"-like conducting channel in interconnecting layer between sub-cells should be improved which calls for fine engineering on the morphology of polyelectrolyte in interconnecting layer.Here,we develop a simple method to effectively manipulating the domains of conductive components in commercially available polyelectrolyte PEDOT:PSs.The use of poor solvent could effectively modify the configuration of polystyrene sulfonic acid and thus the space for conductive components.Based on our strategy,the insulated shells wrapping conductive domains are thinned and the efficiencies of tandem organic solar cells are improved.We believe our method might provide guidance for the manufacture of tandem organic solar cells.展开更多
In the context of global efforts to reduce carbon(C)emissions,several studies have examined the effects of agricultural practices such as straw returning and fertilization on C sequestration by microorganisms.However,...In the context of global efforts to reduce carbon(C)emissions,several studies have examined the effects of agricultural practices such as straw returning and fertilization on C sequestration by microorganisms.However,our understanding of the specific microbial groups and their roles in long-term C increase remains limited.In this study,a 36-year(1984-2020)farmland experiment was conducted to investigate the impact of bacterial C metabolism on the augmentation of organic C in a Typic Hapludoll(Mollisol)in the black soil region of Jilin Province,Northeast China.Our results demonstrated a noteworthy increase in the diversity of microorganisms in the farmland as a result of long-term straw returning and application of mixed chemical fertilizers.However,by examining the functions of microorganisms involved in C metabolism,it was observed that the effects of fertilization on C metabolism were relatively consistent.This consistency was attributed to a deterministic competitive exclusion process,which minimized the differences between treatment groups.On the other hand,the influence of straw addition on C metabolism appeared to follow a more random pattern.These changes in microbial activity were closely linked to the downregulation of core metabolic pathways related to C metabolism.Notably,long-term fertilization had a negative impact on soil organic C levels,while long-term straw returning plus fertilization resulted in a positive increase in soil organic C.These findings have important implications for enhancing soil organic C and grain yield in the regions with typical black soil.展开更多
The low band gap polymer based on benzodithiophene(BDT)-thieno[3,4-b]thiophene(TT)backbone,PBDT-TS1,was synthesized following our previous work and the bulk heterojunction(BHJ)material comprising PBDT-TS1/PC71BM was o...The low band gap polymer based on benzodithiophene(BDT)-thieno[3,4-b]thiophene(TT)backbone,PBDT-TS1,was synthesized following our previous work and the bulk heterojunction(BHJ)material comprising PBDT-TS1/PC71BM was optimized and characterized.By processing the active layer with different additives i.e.1,8-diiodooctane(DIO),1-chloronaphthalene(CN)and 1,8-octanedithiol(ODT)and optimizing the ratio of each additive in the host solvent,a high PCE of 9.98%was obtained under the condition of utilizing 3%DIO as processing additive in CB.The effect of varied additives on photovoltaic performance was illustrated with atomic force microscopy(AFM)and transmission electron microscope(TEM)measurements that explained changes in photovoltaic parameters.These results provide valuable information of solvent additive choice in device optimization of PBDTTT polymers,and the systematic device optimization could be applied in other efficient photovoltaic polymers.Apparently,this work presents a great advance in single junction PSCs,especially in PSCs with conventional architecture.展开更多
Halogenation is a very efficient chemical modification method to tune the molecular energy levels, absorption spectra and molecular packing of organic semiconductors. Recently, in the field of organic solar cells(OSCs...Halogenation is a very efficient chemical modification method to tune the molecular energy levels, absorption spectra and molecular packing of organic semiconductors. Recently, in the field of organic solar cells(OSCs), both fluorine-and chlorinesubstituted photovoltaic materials, including donors and acceptors, demonstrated their great potentials in achieving high power conversion efficiencies(PCEs), raising a question that how to make a decision between fluorination and chlorination when designing materials. Herein, we systemically studied the impact of fluorination and chlorination on the properties of resulting donors(PBDB-T-2 F and PBDB-T-2 Cl) and acceptors(IT-4 F and IT-4 Cl). The results suggest that all the OSCs based on different donor and acceptor combinations can deliver good PCEs around 13%–14%. Chlorination is more effective than fluorination in downshifting the molecular energy levels and broadening the absorption spectra. The influence of chlorination and fluorination on the crystallinity of the resulting materials is dependent on their introduction positions. As chlorination has the advantage of easy synthesis, it is more attractive in designing low-cost photovoltaic materials and therefore may have more potential in largescale applications.展开更多
In this work, photovoltaic properties of the PBDB-T:ITIC based-NF-PSCs were fully optimized and characterized by tuning the morphology of the active layers and changing the device architecture. First, donor/acceptor(D...In this work, photovoltaic properties of the PBDB-T:ITIC based-NF-PSCs were fully optimized and characterized by tuning the morphology of the active layers and changing the device architecture. First, donor/acceptor(D/A) weight ratios were scanned,and then further optimization was performed by using different additives, i.e. 1,8-diiodooctane(DIO), diphenyl ether(DPE),1-chloronaphthalene(CN) and N-methyl-2-pyrrolidone(NMP), on the basis of best D/A ratio(1:1, w/w), respectively. Finally,the conventional or inverted device architectures with different buffer layers were employed to fabricate NF-PSC devices, and meanwhile, the morphology of the active layers was further optimized by controlling annealing temperature and time. As a result,a record efficiency of 11.3% was achieved, which is the highest result for NF-PSCs. It's also remarkable that the inverted NF-PSCs exhibited long-term stability, i.e. the best-performing devices maintain 83% of their initial PCEs after over 4000 h storage.展开更多
Organic solar cells(OSCs)have been developed for few decades since the preparation of the first photovoltaic device,and the record power conversion efficiency(PCE)certified by national renewable energy laboratory(NREL...Organic solar cells(OSCs)have been developed for few decades since the preparation of the first photovoltaic device,and the record power conversion efficiency(PCE)certified by national renewable energy laboratory(NREL)has exceeded 17%.Looking back the whole history of OSCs,its rapid development is inseparable from multi-disciplinary efforts,including the new materials synthesizing,the device physics,and the device engineering,especially the breakthroughs in these disciplines.In this review,we are aiming at reviewing the history of the development of OSCs and summarizing the representative breakthroughs.展开更多
Synergistic optimization of donor-acceptor blend morphologyis a hurdle in the path of realizing efficient non-fullerene small-molecule organic solar cells(NFSMOSCs)due to the anisotropic conjugated backbones of both d...Synergistic optimization of donor-acceptor blend morphologyis a hurdle in the path of realizing efficient non-fullerene small-molecule organic solar cells(NFSMOSCs)due to the anisotropic conjugated backbones of both donor and acceptor.Therefore,developing a facile molecular design strategy to effectively regulate the crystalline properties of photoactive materials,and thus,enable the optimization of blend morphology is of vital importance.In this study,a new donor molecule B1,comprising phenyl-substituted benzodithiophene(BDT)central unit,exhibits strong interaction with the non-fullerene acceptor BO-4 Cl in comparison with its corresponding thiophene-substituted BDT-based material,BTR.As a result,the B1 is affected and induced from an edgeon to a face-on orientation by the acceptor,while the BTR and the acceptor behave individually for the similar molecular orientation in pristine and blend films according to grazing incidence wide angle X-ray scattering results.It means the donor-acceptor blend morphology is synergistically optimized in the B1 system,and the B1:BO-4 Cl-based devices achieve an outstanding power conversion efficiency(PCE)of 15.3%,further certified to be 15.1%by the National Institute of Metrology,China.Our results demonstrate a simple and effective strategy to improve the crystalline properties of the donor molecule as well as synergistically optimize the morphology of the all-small-molecule system,leading to the high-performance NFSM-OSCs.展开更多
A regional coupled prediction system for the Asia-Pacific(AP-RCP)(38°E-180°,20°S-60°N) area has been established.The AP-RCP system consists of WRF-ROMS(Weather Research and Forecast,and Regional Oc...A regional coupled prediction system for the Asia-Pacific(AP-RCP)(38°E-180°,20°S-60°N) area has been established.The AP-RCP system consists of WRF-ROMS(Weather Research and Forecast,and Regional Ocean Model System) coupled models combined with local observational information through dynamically downscaling coupled data assimilation(CDA).The system generates 18-day forecasts for the atmosphere and ocean environment on a daily quasi-operational schedule at Pilot National Laboratory for Marine Science and Technology(Qingdao)(QNLM),consisting of 2 different-resolution coupled models:27 km WRF coupled with 9 km ROMS,9 km WRF coupled with 3 km ROMS,while a version of 3 km WRF coupled with 3 km ROMS is in a test mode.This study is a first step to evaluate the impact of high-resolution coupled model with dynamically downscaling CDA on the extended-range predictions,focusing on forecasts of typhoon onset,improved precipitation and typhoon intensity forecasts as well as simulation of the Kuroshio current variability associated with mesoscale oceanic activities.The results show that for realizing the extended-range predictability of atmospheric and oceanic environment characterized by statistics of mesoscale activities,a fine resolution coupled model resolving local mesoscale phenomena with balanced and coherent coupled initialization is a necessary first step.The next challenges include improving the planetary boundary physics and the representation of air-sea and air-land interactions to enable the model to resolve kilometer or sub-kilometer processes.展开更多
The printable electrode interlayer with excellent thickness tolerance is crucial for mass production of organic solar cells(OSCs)by solution-based print techniques. Herein, high-quality printable SnO2 films are simply...The printable electrode interlayer with excellent thickness tolerance is crucial for mass production of organic solar cells(OSCs)by solution-based print techniques. Herein, high-quality printable SnO2 films are simply fabricated by spin-coating or bladecoating the chemical precipitated SnO2 colloid precursor with post thermal annealing treatment. The SnO2 films possess outstanding optical and electrical properties, especially extreme thickness-insensitivity. The interfacial electron trap density of SnO2 cathode interlayers(CILs) are very low and show negligible increase as the thicknesses increase from 10 to 160 nm,resulting in slight change of the power conversion efficiencies(PCEs) of the PM6:Y6 based OSCs from 16.10% to 13.07%. For blade-coated SnO2 CIL, the PCE remains high up to 12.08% even the thickness of SnO2 CIL is high up to 530 nm. More strikingly, the large-area OSCs of 100 mm2 with printed SnO2 CILs obtain a high efficiency of 12.74%. To the best of our knowledge, this work presents the first example for the high-performance and large-area OSCs with the thickness-insensitive SnO2 CIL.展开更多
In order to meet the requirements for making organic solar cells(OSCs)through solution printing techniques,great efforts have been devoted into developing high performance OSCs with relatively thicker active layers.In...In order to meet the requirements for making organic solar cells(OSCs)through solution printing techniques,great efforts have been devoted into developing high performance OSCs with relatively thicker active layers.In this work,a thick-film(300 nm)ternary OSC with a power conversion efficiency of 14.3%is fabricated by introducing phenyl-C61-butyric-acid-methyl ester(PC61BM)into a PBDB-T-2Cl:BTP-4 F host blend.The addition of PC61BM is found to be helpful for improving the hole and electron mobilities,and thus facilitates charge transport as well as suppresses charge recombination in the active layers,leading to the improved efficiencies of OSCs with relatively thicker active layers.Our results demonstrate the feasibility of employing fullerene derivative PC61BM to construct a high-efficiency thick-film ternary device,which would promote the development of thick layer ternary OSCs to fulfill the requirements of future roll to roll production.展开更多
To achieve fabrication and cost competitiveness in organic optoelectronic devices that include organic solar cells(OSCs)and organic light-emitting diodes(OLEDs),it is desirable to have one type of material that can si...To achieve fabrication and cost competitiveness in organic optoelectronic devices that include organic solar cells(OSCs)and organic light-emitting diodes(OLEDs),it is desirable to have one type of material that can simultaneously function as both the electron and hole transport layers(ETLs and HTLs)of the organic devices in all device architectures(i.e.,normal and inverted architectures).We address this issue by proposing and demonstrating Cs-intercalated metal oxides(with various Cs mole ratios)as both the ETL and HTL of an organic optoelectronic device with normal and inverted device architectures.Our results demonstrate that the new approach works well for widely used transition metal oxides of molybdenum oxide(MoOx)and vanadium oxide(V_(2)O_(x)).Moreover,the Cs-intercalated metaloxide-based ETL and HTL can be easily formed under the conditions of a room temperature,water-free and solution-based process.These conditions favor practical applications of OSCs and OLEDs.Notably,with the analyses of the Kelvin Probe System,our approach of Cs-intercalated metal oxides with a wide mole ratio range of transition metals(Mo or V)/Cs from 1:0 to 1:0.75 can offer significant and continuous work function tuning as large as 1.31 eV for functioning as both an ETL and HTL.Consequently,our method of intercalated metal oxides can contribute to the emerging large-scale and low-cost organic optoelectronic devices.展开更多
基金supported by the National Key Research&Development Program of China(Grant Nos.2017YFC1404100 and 2017YFC1404104)the National Natural Science Foundation of China(Grant Nos.41775100 and 41830964)。
文摘Predicting tropical cyclone(TC)genesis is of great societal importance but scientifically challenging.It requires fineresolution coupled models that properly represent air−sea interactions in the atmospheric responses to local warm sea surface temperatures and feedbacks,with aid from coherent coupled initialization.This study uses three sets of highresolution regional coupled models(RCMs)covering the Asia−Pacific(AP)region initialized with local observations and dynamically downscaled coupled data assimilation to evaluate the predictability of TC genesis in the West Pacific.The APRCMs consist of three sets of high-resolution configurations of the Weather Research and Forecasting−Regional Ocean Model System(WRF-ROMS):27-km WRF with 9-km ROMS,and 9-km WRF with 3-km ROMS.In this study,a 9-km WRF with 9-km ROMS coupled model system is also used in a case test for the predictability of TC genesis.Since the local sea surface temperatures and wind shear conditions that favor TC formation are better resolved,the enhanced-resolution coupled model tends to improve the predictability of TC genesis,which could be further improved by improving planetary boundary layer physics,thus resolving better air−sea and air−land interactions.
文摘Zeolites Y,A and mordenite(ZY,ZA and ZM)were obtained from diatomite in a template-free system,and the products were modified by thiourea(TU).Characterization studies results indicated that the TU molecules were loaded onto the exterior surfaces of the synthetic zeolites as well as the channels.Elemental analysis and energy-dispersive X-ray spectrometer proved that the TU molecules loaded on to ZA were more than ZY and ZM.Removal of Cd(Ⅱ)was investigated,and itwas found that themodified zeolites have higher removal capacity,modified ZA is especially noticeable.In the adsorption experiments,the effects of various parameters such as sorbent content,contact time,concentration of cadmium solution,pH,selectivity and regeneration were discussed.At the best removal efficiency by modified zeolites,the maximum adsorption capacity is 94.3 mg·g^−1,103.2 mg·g^−1 and 89.7 mg·g^−1 at 25℃,respectively.The sorbents show good efficiency for the removal of Cd(Ⅱ)in the presence of different multivalent cations and have good regeneration effect.For the modified samples,removal experiments take place via ion exchange and complexation processes.
基金the financial support from the National Natural Science Foundation of China(Grant Nos.51703228,51673201,21835006)Beijing National Laboratory for Molecular Sciences(BNLMS-CXXM-201903)。
文摘Compared to regular conjugated polymers,the random conjugated terpolymers are usually not beneficial to achieve highly efficient non-fullerene(NF)-based polymer solar cells(PSCs)due to their disordered chemical structures.In this work,we report two random terpolymer donors(PBNB80 and PBNB50)by tuning the molar ratio of electron-accepting units of 1,3-di(thiophen-2-yl)naphtho[2,3-c]thiophene-4,9-dione(NTD)and 1,3-bis(4-chlorothiophen-2-yl)-4 H,8 H-benzo[1,2-c:4,5-c’]dithiophene-4,8-dione(ClBDD),at the same time,the parent polymers(PBNB100 and PBNB00)are also compared to study.These four polymer donors exhibit similar optical bandgaps and gradually deepen highest occupied molecular orbital levels.Importantly,aggregation and self-organization properties of the random terpolymer donors are optimized,which result in the better morphology and crystal coherence length after blending with NF acceptor of BO-4 Cl.Particularly,a PBNB80:BO-4 Cl blend forms an optimal nanoscale phase-separation morphology,thereby producing an outstanding power conversion efficiency of 16.0%,which is much higher than those(12.8%and 10.7%)of their parent binary polymer donor-based devices.This work demonstrates that rational using terpolymerization strategy to prepare random terpolymer is a very important method to achieve highly efficient NF-PSCs.
基金co-sponsored by grants from the National Natural Science Foundation (Grant Nos. 41206178, 41306006, 41376015, 41376013 and 41176003)the National Basic Research Program (Grant No. 2013CB430304)+1 种基金the National HighTech R&D Program (Grant No. 2013AA09A505)the Global Change and Air–Sea Interaction Program (Grant No. GASI-01-0112) of China
文摘To further explore enthalpy-based sea-ice assimilation, a one-dimensional (1D) enthalpy sea-ice model is implemented into a simple pycnocline prediction model. The 1D enthalpy sea-ice model includes the physical processes such as brine expulsion, flushing, and salt diffusion. After being coupled with the atmosphere and ocean components, the enthalpy sea-ice model can be integrated stably and serves as an important modulator of model variability. Results from a twin experiment show that the sea-ice data assimilation in the enthalpy space can produce smaller root-mean-square errors of model variables than the traditional scheme that assimilates the observations of ice concentration, especially for slow-varying states. This study provides some insights into the improvement of sea-ice data assimilation in a coupled general circulation model.
基金funded by the National Natural Science Foundation of China (Grant No.41676088)the National Key Research and Development Project of China (2016YFC1401800,2017YFC1404100,2017YFC1404102)+1 种基金the Fundamental Research Funds for the Central Universities (HEUCF 041705)the Foundation of the Key Laboratory of Marine Environmental Information Technology
文摘That a model has sensitivity responses to parameter uncertainties is a key concept in implementing model parameter es- timation using filtering theory and methodology. Depending on the nature of associated physics and characteristic variability of the fluid in a coupled system, the response time scales of a model to parameters can be different, from hourly to decadal. Unlike state estimation, where the update frequency is usually linked with observational frequency, the update frequency for parameter estimation must be associated with the time scale of the model sensitivity response to the parameter being esti- mated. Here, with a simple coupled model, the impact of model sensitivity response time scales on coupled model parameter estimation is studied. The model includes characteristic synoptic to decadal scales by coupling a long-term varying deep ocean with a slow-varying upper ocean forced by a chaotic atmosphere. Results show that, using the update frequency deter- mined by the model sensitivity response time scale, both the reliability and quality of parameter estimation can be improved significantly, and thus the estimated parameters make the model more consistent with the observation. These simple model results provide a guideline for when real observations are used to optimize the parameters in a coupled general circulation model for improving climate analysis and prediction initialization.
基金Supported by Hebei Provincial Social Science Foundation Project in 2012(HB12YJ055)
文摘On the basis of making clear diversity characteristics of soil functions and multiple characteristics of income, this paper points out that the monetization of soil functions based functional maintenance and change decision process can be regarded as a game process of different utilization methods at the background of different functions. The balance of this game process will determine monetary value of soil functions. After understanding money and monetization concepts, it introduces that measurability and exchangeability of soil functions provide objective conditions for monetization of soil functions. Finally, it discusses that usefulness value of soil functions provide basis for monetization of soil functions.
基金the National Natural Science Foundation of China(NSFC,grant nos.21835006 and 51961135103)the Bureau of International Cooperation Chinese Academy of Sciences(grant no.121111KYSB20200043)+1 种基金the financial support from China Postdoctoral Science Foundation(grant no.2022M723199)the Beijing National Laboratory for Molecular Sciences Junior Fellow.
文摘Organic photovoltaic(OPV)cells have demonstrated remarkable performance in small,spin-coated areas.Nevertheless significant challenges persist in the form of large efficiency losses due to the fact that the ideal morphology cannot be preserved in the transition of small-area cells to large-scale panels.Herein,the ternary strategy of incorporating the third component FTCC-Br into the active layer of PB2:BTP-eC9 is employed to improve absorption response,optimize morphology,and reduce charge recombination,leading to a power conversion efficiency(PCE)of 19.5%(certified as 19.1%by the National Institute of Metrology,China).Moreover,the addition of FTCC-Br can control the aggregation kinetics of the active layer during the film formation process,transferring the optimal morphology to the blade-coated large-area films.Based on the highly efficient ternary bulk heterojunction,the 50 cm^(2) OPVmodules exhibited a PCE of 15.2%with respect to the active area.Importantly,the ternary OPV cells retain 80%of its initial PCE after 4000 h under continuous illumination.Our work demonstrates that the addition of a third component has the potential to improve the efficiency and stability of large-area organic solar cells.
基金The authors are grateful to the financial support from the Key Research and Development Program sponsored by the Ministry of Science and Technology(MOST)(2022YFA1203400)the National Natural Science Foundation of China(22102172,22372155,22072145,22005294,21925205,21721003)the authors also thank the ZEROVISION company for providing assistance in creating figures for this manuscript.
文摘The discovery of single-atom catalysts(SACs)represents a groundbreaking advancement in the field of catalysis over the past decades.With the in-depth exploration of relevant structure-activity relationships,the metal−support interaction(MSI)is widely adopted to elucidate variations in electronic structure and coordination configuration of atomic active sites on various kinds of supports.Herein,we briefly summarize the metal oxide supports for SACs fabrication,including the distinctive characteristics of metal oxide supports,enlightening advancements in metal oxide support-based SACs(MO-SACs),feasible preparation methods for MO-SACs and effective regulation strategies of MSI effect in MO-SACs.In addition,we present our viewpoints and outlook in this field to stimulate rational design and construction of novel MO-SACs applied in diverse renewable energy devices,while some universal suggestions are sincerely given to provoke thoughtful considerations during the research process.
基金the National Natural Science Foundation of China(NSFC)(22275016,21835006,22122905)Beijing Municipal Science&Technology Commission(2232078)+2 种基金Beijing National Laboratory for Molecular Sciences(BNLMS)Junior Fellow(2019BMS20014,BNLMS-CXXM-201903)National Research Council of Science and Technology of Korea(Global20-004)the Key Research Program of the Chinese Academy of Sciences(XDPB13-3).
文摘Owing to the function of manipulating light absorption distribution,tandem organic solar cells containing multiple sub-cells exhibit high power conversion efficiencies.However,there is a substantial challenge in precisely controlling the inter-subcells carrier migration which determines the balance of charge transport across the entire device.The conductivity of"nanowires"-like conducting channel in interconnecting layer between sub-cells should be improved which calls for fine engineering on the morphology of polyelectrolyte in interconnecting layer.Here,we develop a simple method to effectively manipulating the domains of conductive components in commercially available polyelectrolyte PEDOT:PSs.The use of poor solvent could effectively modify the configuration of polystyrene sulfonic acid and thus the space for conductive components.Based on our strategy,the insulated shells wrapping conductive domains are thinned and the efficiencies of tandem organic solar cells are improved.We believe our method might provide guidance for the manufacture of tandem organic solar cells.
基金funded by the Science and Technology Cooperation Project Between Jilin Province and Chinese Academy of Sciences(No.2022000170)the National Natural Science Foundation of China(Nos.41920104008 and U22A20593)the Strategic Priority Research Program of CAS(No.XDA28020400)。
文摘In the context of global efforts to reduce carbon(C)emissions,several studies have examined the effects of agricultural practices such as straw returning and fertilization on C sequestration by microorganisms.However,our understanding of the specific microbial groups and their roles in long-term C increase remains limited.In this study,a 36-year(1984-2020)farmland experiment was conducted to investigate the impact of bacterial C metabolism on the augmentation of organic C in a Typic Hapludoll(Mollisol)in the black soil region of Jilin Province,Northeast China.Our results demonstrated a noteworthy increase in the diversity of microorganisms in the farmland as a result of long-term straw returning and application of mixed chemical fertilizers.However,by examining the functions of microorganisms involved in C metabolism,it was observed that the effects of fertilization on C metabolism were relatively consistent.This consistency was attributed to a deterministic competitive exclusion process,which minimized the differences between treatment groups.On the other hand,the influence of straw addition on C metabolism appeared to follow a more random pattern.These changes in microbial activity were closely linked to the downregulation of core metabolic pathways related to C metabolism.Notably,long-term fertilization had a negative impact on soil organic C levels,while long-term straw returning plus fertilization resulted in a positive increase in soil organic C.These findings have important implications for enhancing soil organic C and grain yield in the regions with typical black soil.
基金supported by the National Basic Research Program of China(2014CB643501)the National Natural Science Foundation of China(21325419,51373181,91333204)+1 种基金the Chinese Academy of Sciences(XDB12030200,KJZD-EW-J01)the Science and Technology Commission of Beijing(Z131100006013002)
文摘The low band gap polymer based on benzodithiophene(BDT)-thieno[3,4-b]thiophene(TT)backbone,PBDT-TS1,was synthesized following our previous work and the bulk heterojunction(BHJ)material comprising PBDT-TS1/PC71BM was optimized and characterized.By processing the active layer with different additives i.e.1,8-diiodooctane(DIO),1-chloronaphthalene(CN)and 1,8-octanedithiol(ODT)and optimizing the ratio of each additive in the host solvent,a high PCE of 9.98%was obtained under the condition of utilizing 3%DIO as processing additive in CB.The effect of varied additives on photovoltaic performance was illustrated with atomic force microscopy(AFM)and transmission electron microscope(TEM)measurements that explained changes in photovoltaic parameters.These results provide valuable information of solvent additive choice in device optimization of PBDTTT polymers,and the systematic device optimization could be applied in other efficient photovoltaic polymers.Apparently,this work presents a great advance in single junction PSCs,especially in PSCs with conventional architecture.
基金supported by the National Natural Science Foundation of China (91333204, 91633301, 51673201)the Ministry of Science and Technology of China (2014CB643501)the Chinese Academy of Sciences (XDB12030200, KJZD-EW-J01)
文摘Halogenation is a very efficient chemical modification method to tune the molecular energy levels, absorption spectra and molecular packing of organic semiconductors. Recently, in the field of organic solar cells(OSCs), both fluorine-and chlorinesubstituted photovoltaic materials, including donors and acceptors, demonstrated their great potentials in achieving high power conversion efficiencies(PCEs), raising a question that how to make a decision between fluorination and chlorination when designing materials. Herein, we systemically studied the impact of fluorination and chlorination on the properties of resulting donors(PBDB-T-2 F and PBDB-T-2 Cl) and acceptors(IT-4 F and IT-4 Cl). The results suggest that all the OSCs based on different donor and acceptor combinations can deliver good PCEs around 13%–14%. Chlorination is more effective than fluorination in downshifting the molecular energy levels and broadening the absorption spectra. The influence of chlorination and fluorination on the crystallinity of the resulting materials is dependent on their introduction positions. As chlorination has the advantage of easy synthesis, it is more attractive in designing low-cost photovoltaic materials and therefore may have more potential in largescale applications.
基金supported by the National Basic Research Program(2014CB643501)the National Natural Science Foundation of China(91333204,21325419)the Chinese Academy of Sciences(XDB12030200)
文摘In this work, photovoltaic properties of the PBDB-T:ITIC based-NF-PSCs were fully optimized and characterized by tuning the morphology of the active layers and changing the device architecture. First, donor/acceptor(D/A) weight ratios were scanned,and then further optimization was performed by using different additives, i.e. 1,8-diiodooctane(DIO), diphenyl ether(DPE),1-chloronaphthalene(CN) and N-methyl-2-pyrrolidone(NMP), on the basis of best D/A ratio(1:1, w/w), respectively. Finally,the conventional or inverted device architectures with different buffer layers were employed to fabricate NF-PSC devices, and meanwhile, the morphology of the active layers was further optimized by controlling annealing temperature and time. As a result,a record efficiency of 11.3% was achieved, which is the highest result for NF-PSCs. It's also remarkable that the inverted NF-PSCs exhibited long-term stability, i.e. the best-performing devices maintain 83% of their initial PCEs after over 4000 h storage.
基金supported by the financial support from the National Natural Science Foundation of China(Nos.21835006,21704004 and 21734008)the Fundamental Research Funds for the Central Universities,China(No.FRF-TP-19-047A2)China Postdoctoral Science Foundation(No.2019M660799).
文摘Organic solar cells(OSCs)have been developed for few decades since the preparation of the first photovoltaic device,and the record power conversion efficiency(PCE)certified by national renewable energy laboratory(NREL)has exceeded 17%.Looking back the whole history of OSCs,its rapid development is inseparable from multi-disciplinary efforts,including the new materials synthesizing,the device physics,and the device engineering,especially the breakthroughs in these disciplines.In this review,we are aiming at reviewing the history of the development of OSCs and summarizing the representative breakthroughs.
基金financially supported by the Basic and Applied Basic Research Major Program of Guangdong Province(2019B030302007)the National Natural Science Foundation of China(51873217,21734008,51703228,51961135103,51773047 and 51903239)。
文摘Synergistic optimization of donor-acceptor blend morphologyis a hurdle in the path of realizing efficient non-fullerene small-molecule organic solar cells(NFSMOSCs)due to the anisotropic conjugated backbones of both donor and acceptor.Therefore,developing a facile molecular design strategy to effectively regulate the crystalline properties of photoactive materials,and thus,enable the optimization of blend morphology is of vital importance.In this study,a new donor molecule B1,comprising phenyl-substituted benzodithiophene(BDT)central unit,exhibits strong interaction with the non-fullerene acceptor BO-4 Cl in comparison with its corresponding thiophene-substituted BDT-based material,BTR.As a result,the B1 is affected and induced from an edgeon to a face-on orientation by the acceptor,while the BTR and the acceptor behave individually for the similar molecular orientation in pristine and blend films according to grazing incidence wide angle X-ray scattering results.It means the donor-acceptor blend morphology is synergistically optimized in the B1 system,and the B1:BO-4 Cl-based devices achieve an outstanding power conversion efficiency(PCE)of 15.3%,further certified to be 15.1%by the National Institute of Metrology,China.Our results demonstrate a simple and effective strategy to improve the crystalline properties of the donor molecule as well as synergistically optimize the morphology of the all-small-molecule system,leading to the high-performance NFSM-OSCs.
基金supported by the National Key Research and Development Program of China(2022YFE0106400)the National Natural Science Foundation of China(42122039)special funds from Shandong Province for Qingdao Marine Science and Technology National Laboratory(2022QNLM010203)。
基金supported by the National Key Research and Development Program of China(2017YFC1404100,2017YFC1404104)the National Natural Science Foundation of China(41775100,41830964)+1 种基金the Shandong Province’s"Taishan"Scientist Project(2018012919)the collaborative project between the Ocean University of China(OUC),Texas A&M University(TAMU)and the National Center for Atmospheric Research(NCAR)and completed through the International Laboratory for High Resolution Earth System Prediction(iHESP)-a collaboration among QNLM,TAMU and NCAR。
文摘A regional coupled prediction system for the Asia-Pacific(AP-RCP)(38°E-180°,20°S-60°N) area has been established.The AP-RCP system consists of WRF-ROMS(Weather Research and Forecast,and Regional Ocean Model System) coupled models combined with local observational information through dynamically downscaling coupled data assimilation(CDA).The system generates 18-day forecasts for the atmosphere and ocean environment on a daily quasi-operational schedule at Pilot National Laboratory for Marine Science and Technology(Qingdao)(QNLM),consisting of 2 different-resolution coupled models:27 km WRF coupled with 9 km ROMS,9 km WRF coupled with 3 km ROMS,while a version of 3 km WRF coupled with 3 km ROMS is in a test mode.This study is a first step to evaluate the impact of high-resolution coupled model with dynamically downscaling CDA on the extended-range predictions,focusing on forecasts of typhoon onset,improved precipitation and typhoon intensity forecasts as well as simulation of the Kuroshio current variability associated with mesoscale oceanic activities.The results show that for realizing the extended-range predictability of atmospheric and oceanic environment characterized by statistics of mesoscale activities,a fine resolution coupled model resolving local mesoscale phenomena with balanced and coherent coupled initialization is a necessary first step.The next challenges include improving the planetary boundary physics and the representation of air-sea and air-land interactions to enable the model to resolve kilometer or sub-kilometer processes.
基金supported by the National Natural Science Foundation of China (51873007, 51961165102, 21835006)the Fundamental Research Funds for the Central Universities in China (2019MS025, 2018MS032, 2017MS027, 2017XS084)。
文摘The printable electrode interlayer with excellent thickness tolerance is crucial for mass production of organic solar cells(OSCs)by solution-based print techniques. Herein, high-quality printable SnO2 films are simply fabricated by spin-coating or bladecoating the chemical precipitated SnO2 colloid precursor with post thermal annealing treatment. The SnO2 films possess outstanding optical and electrical properties, especially extreme thickness-insensitivity. The interfacial electron trap density of SnO2 cathode interlayers(CILs) are very low and show negligible increase as the thicknesses increase from 10 to 160 nm,resulting in slight change of the power conversion efficiencies(PCEs) of the PM6:Y6 based OSCs from 16.10% to 13.07%. For blade-coated SnO2 CIL, the PCE remains high up to 12.08% even the thickness of SnO2 CIL is high up to 530 nm. More strikingly, the large-area OSCs of 100 mm2 with printed SnO2 CILs obtain a high efficiency of 12.74%. To the best of our knowledge, this work presents the first example for the high-performance and large-area OSCs with the thickness-insensitive SnO2 CIL.
基金supported by the National Natural Science Foundation of China(21835006,21704004,91633301,51673201)the Chinese Academy of Sciences(KJZD-EW-J01)the Innovation Project supported by Beijing National Laboratory for Molecular Sciences(BNLMS-CXXM-201903)
文摘In order to meet the requirements for making organic solar cells(OSCs)through solution printing techniques,great efforts have been devoted into developing high performance OSCs with relatively thicker active layers.In this work,a thick-film(300 nm)ternary OSC with a power conversion efficiency of 14.3%is fabricated by introducing phenyl-C61-butyric-acid-methyl ester(PC61BM)into a PBDB-T-2Cl:BTP-4 F host blend.The addition of PC61BM is found to be helpful for improving the hole and electron mobilities,and thus facilitates charge transport as well as suppresses charge recombination in the active layers,leading to the improved efficiencies of OSCs with relatively thicker active layers.Our results demonstrate the feasibility of employing fullerene derivative PC61BM to construct a high-efficiency thick-film ternary device,which would promote the development of thick layer ternary OSCs to fulfill the requirements of future roll to roll production.
基金This study was supported by the University Grant Council of the University of Hong Kong(Grant Nos.10401466 and 201111159062)the General Research Fund(Grant Nos.HKU711813 and HKU711612E)+1 种基金an RGC-NSFC grant(N_HKU709/12)grant CAS14601 from the CAS-Croucher Funding Scheme for Joint Laboratories.
文摘To achieve fabrication and cost competitiveness in organic optoelectronic devices that include organic solar cells(OSCs)and organic light-emitting diodes(OLEDs),it is desirable to have one type of material that can simultaneously function as both the electron and hole transport layers(ETLs and HTLs)of the organic devices in all device architectures(i.e.,normal and inverted architectures).We address this issue by proposing and demonstrating Cs-intercalated metal oxides(with various Cs mole ratios)as both the ETL and HTL of an organic optoelectronic device with normal and inverted device architectures.Our results demonstrate that the new approach works well for widely used transition metal oxides of molybdenum oxide(MoOx)and vanadium oxide(V_(2)O_(x)).Moreover,the Cs-intercalated metaloxide-based ETL and HTL can be easily formed under the conditions of a room temperature,water-free and solution-based process.These conditions favor practical applications of OSCs and OLEDs.Notably,with the analyses of the Kelvin Probe System,our approach of Cs-intercalated metal oxides with a wide mole ratio range of transition metals(Mo or V)/Cs from 1:0 to 1:0.75 can offer significant and continuous work function tuning as large as 1.31 eV for functioning as both an ETL and HTL.Consequently,our method of intercalated metal oxides can contribute to the emerging large-scale and low-cost organic optoelectronic devices.