Aqueous Zinc-ion batteries(ZIB) are attracting immense attention because of their merits of excellent safety and quite cheap properties compared with lithium-ion batteries(LIB).Manganese oxide is one of the most impor...Aqueous Zinc-ion batteries(ZIB) are attracting immense attention because of their merits of excellent safety and quite cheap properties compared with lithium-ion batteries(LIB).Manganese oxide is one of the most important cathode materials of ZIB.In this paper,α-Mn2O3 used as cathode of ZIB is synthesized via Metal-Organic Framework(MOF)-derived method,which delivers a high specific capacity of225 mAh g^(-1) at 0.05 A g^(-1) and 92.7 mAh g^(-1) after 1700 cycles at 2 A g^(-1).The charge storage mechanism of α-Mn2O3 cathode is found to greatly depend on the discharge current density.At lower current density discharging,the H+ and Zn2+ are successively intercalated into the α-Mn2O3 before and after the "turning point" of discharge voltage and their discharging products present obviously different morphologies changing from flower-like to large plate-like products.At a higher current density,the low-voltage plateau after the turning point disappears due to the decrease of amount of Zn2+ intercalation and the H+intercalation is dominated in α-Mn2 O3.This study provides significant understanding for future design and research of high-performance Mn-based cathodes of ZIB.展开更多
Organic light-emitting diodes （OLEDs） have been extensively studied since the first efficient device based on small molecular luminescent materials was reported by Tang. Organic electroluminescent material, one of t...Organic light-emitting diodes （OLEDs） have been extensively studied since the first efficient device based on small molecular luminescent materials was reported by Tang. Organic electroluminescent material, one of the centerpieces of OLEDs, has been the focus of studies by many material scientists. To obtain high luminosity and to keep material costs low, a few remarkable design concepts have been developed. Aggregation-induced emission （AIE） materials were invented to overcome the common fluorescence-quenching problem, and cross-dipole stacking of fluorescent molecules was shown to be an effective method to get high solid-state luminescence. To exceed the limit of internal quantum efficiency of conventional fluorescent materials, phosphorescent materials were successfully applied in highly efficient electroluminescent devices. Most recently, delayed flu- orescent materials via reverse-intersystem crossing （RISC） from triplet to singlet and the ＂hot exciton＂ materials based on hy- bridized local and charge-transfer （HLCT） states were developed to he a new generation of low-cost luminescent materials as efficient as phosphorescent materials. In terms of the device-fabrication process, solution-processible small molecular lumi- nescent materials possess the advantages of high purity （vs. polymers） and low procession cost （vs. vacuum deposition）, which are garnering them increasing attention. Herein, we review the progress of the development of small-molecule luminescent materials with different design concepts and features, and also briefly examine future development tendencies of luminescent materials.展开更多
Since 1986,the donor-acceptor (D:A) heterojunction has been regarded a necessity for high-efficiency organic photovoltaics (OPVs),due to its unique advantage in compensating the intrinsic limitations of organic semico...Since 1986,the donor-acceptor (D:A) heterojunction has been regarded a necessity for high-efficiency organic photovoltaics (OPVs),due to its unique advantage in compensating the intrinsic limitations of organic semiconductors,such as high exciton binding energy and poor ambipolar charge mobility. While this adversely causes tremendous non-radiative charge recombination and instability issues,which currently become the most critical limits for commercialization of OPVs. Here,we present a concept-to-proof study on the potential of D:A heterojunction free OPV by taking advantage of recent progress of non-fullerene acceptors. First,we demonstrate that the “free carriers” can be spontaneously generated upon illumination in an NFA,i.e.,the 6TIC-4F single layer. Second,the 6TIC-4F layer also exhibits good ambipolar charge transporting property. These exceptional characteristics distinguish it from the traditional organic semiconductors,and relieve it from the reliance of D:A heterojunction to independently work as active layer. As a result,the subsequent OPV by simply sandwiching the 6TIC-4F layer between the cathode and anode yields a considerably high power conversion efficiency ~1%. Moreover,we find the D:A heterojunction free device exhibits two order of magnitude higher electroluminescence quantum efficiency and significantly reduced VOC loss by 0.16 eV compared to those of the D:A BHJ structure,validating its promise for higher efficiency in the future. Therefore,our work demonstrates the possibility of using D:A heterojunction-free device structure for high performance,that can potentially become the next game changer of OPV.展开更多
In this study, biochars from rice straw （Oryza sativa L.） were prepared at 200-600 ℃ by oxygen-limited pyrolysis to investigate the changes in properties of rice straw biochars produced at different temperatures, a...In this study, biochars from rice straw （Oryza sativa L.） were prepared at 200-600 ℃ by oxygen-limited pyrolysis to investigate the changes in properties of rice straw biochars produced at different temperatures, and to examine the adsorption capacities of the biochars for a heavy metal, copper（II） （Cu（II））, and an organic insecticide of cyromazine, as well as to further reveal the adsorption mechanisms. The results obtained with batch experiments showed that the amount of Cu（II） adsorbed varied with the pyrolysis temperatures of rice straw biochar. The biochar produced at 400 ~C had the largest adsorption capacity for Cu（II） （0.37 mol kg-1） among the biochars, with the non-electrostatic adsorption as the main adsorption mechanism. The highest adsorption capacity for cyromazine （156.42 g kg-1） was found in the rice straw biochar produced at 600 ℃, and cyromazine adsorption was exclusively predominated by surface adsorption. An obvious competitive adsorption was found between 5 mmol L-1 Cu（II） and 2 g L-1 cyromazine when they were in the binary solute system. Biochar may be used to remediate heavy metal- and organic insecticide-contaminated water, while the pyrolysis temperature of feedstocks for producing biochar should be considered for the restoration of multi-contamination.展开更多
Low-molecular-weight (LMW) organic acids exist widely in soils and have beenimplicated in many soil processes. The objective of the present paper was to evaluate effect of twoLMW organic acids, citric acid and oxalic ...Low-molecular-weight (LMW) organic acids exist widely in soils and have beenimplicated in many soil processes. The objective of the present paper was to evaluate effect of twoLMW organic acids, citric acid and oxalic acid, on Cl^-adsorption by three variable charge soils, alatosol, a lateritic red soil and a red soil, using a batch method. The results showed that thepresence of citric acid and oxalic acid led to a decrease in Cl^- adsorption with larger decreasesfor citric acid. Among the different soils Cl^- adsorption in the lateritic red soil and the redsoil was more affected by both the LMW organic acids than that in the latosol.展开更多
Organic scintillators that efficiently generate bright triplet excitons are of critical importance for highperformance X-ray-excited luminescence in radiation detection.However,the nature of triplet-singlet spinforbid...Organic scintillators that efficiently generate bright triplet excitons are of critical importance for highperformance X-ray-excited luminescence in radiation detection.However,the nature of triplet-singlet spinforbidden transitions in these materials often result in long-lived phosphorescence,which is undesirable for ultrafast X-ray detection and imaging.Here we demonstrate that the effect of hybridized local and charge-transfer(HLCT)excited states enables organic scintillators to exhibit highly efficient and fast radioluminescence(RL)in response to X-ray irradiation.Our experimental and theoretical investigation shows that the oxidized 1,8-naphthalimide-phenothiazine dyad(OMNI-PTZ 2)with HLCT-excited states has an enhanced overlap integral of the highest occupied molecular orbital(HOMO)and lowest unoccupied molecular orbital(LUMO)on MNIπ-orbitals,and moderate donor–acceptor electron interactions.As a result,the RL of these crystals exhibits a 61-fold increase and its monoexponential decay lifetime is three orders of magnitude faster compared to its corresponding thermally activated delayed fluorescence(TADF)molecule MNI-PTZ 1.We further demonstrate the practical utility of the OMNI-PTZ 2(G)in high-performance X-ray detection and imaging,achieving an X-ray dose sensitivity of 97 nGy s−1 and an exceptional spatial resolution of 20 lp/mm.Our study provides a promising molecular design principle for utilizing triplet excitons to develop high-efficiency and fast X-ray scintillators for the development of next-generation flexible and stretchable X-ray imaging detectors.展开更多
Batch equilibrium experiments were conducted to investigate cadmium （Cd） sorption by two permanent-charge soils, a yellow-cinnamon soil and a yellow-brown soil, and two variable-charge soils, a red soil and a latoso...Batch equilibrium experiments were conducted to investigate cadmium （Cd） sorption by two permanent-charge soils, a yellow-cinnamon soil and a yellow-brown soil, and two variable-charge soils, a red soil and a latosol, with addition of selected organic acids （acetate, tartrate, and citrate）. Results showed that with an increase in acetate concentrations from 0 to 3.0 mmol L^-1, Cd sorption percentage by the yellow-cinnamon soil, the yellow-brown soil, and the latosol decreased. The sorption percentage of Cd by the yellow-clnnamon soil and generally the yellow-brown soil （permanent-charge soils） decreased with an increase in tartrate concentration, but increased at low tartrate concentrations for the red soil and the latosol. Curves of percentage of Cd sorption for citrate were similar to those for tartrate. For the variable-charge soils with tartrate and citrate, there were obvious peaks in Cd sorption percentage. These peaks, where organic acids had maximum influence, changed with soil type, and were at a higher organic acid concentration for the variable-charge soils than for the permanent charge soils. Addition of cadmium after tartrate adsorption resulted in higher sorption increase for the varlable-charge soils than permanent-charge soils. When tartrate and Cd solution were added together, sorption of Cd decreased with tartrate concentration for the yellow-brown soil, but increased at low tartrate concentrations and then decreased with tartrate concentration for the red soil and the latosol.展开更多
Solution processability is a unique property of organic semiconductors. The compact and regular π-π stacking between molecules is paramount in the performance of organic optoelectronic devices. However, it is still ...Solution processability is a unique property of organic semiconductors. The compact and regular π-π stacking between molecules is paramount in the performance of organic optoelectronic devices. However, it is still a challenge to improve their stacking quality without sacrificing the solution-processability from the aspect of materials design. Here, delicately engineered additives are presented to promote the formation of ordered aggregation of conjugated molecules by regulating their nucleation and growth dynamics. Intriguingly, the long-chain BTP-eC9-4F molecules can realize ordered aggregation comparable to short-chain ones without sacrificing processability. The domain size of BTP-eC9-4F aggregation is enlarged from 24.2 to 32.2 nm in blend films.Thereby exciton diffusion and charge transport become faster, contributing to the suppression of recombination losses. As a result, a power conversion efficiency of 19.2% is achieved in D18:BTP-eC9-4F based organic photovoltaics. Our findings demonstrate a facile strategy to improve the packing quality of solution-processed organic semiconductors for high-efficiency photovoltaics and beyond photovoltaics.展开更多
Constructing a Z-scheme is a significant approach to improve the separation of photogene rated carriers for effective organic pollutant degradation.Herein,a BiVO4/ZnIn2S4(BZ) Z-scheme composite was successfully synthe...Constructing a Z-scheme is a significant approach to improve the separation of photogene rated carriers for effective organic pollutant degradation.Herein,a BiVO4/ZnIn2S4(BZ) Z-scheme composite was successfully synthesized,and applied to photodegrade methyl orange(MO) irradiated by a LED lamp.Anchoring the BiVO4 on the ZnIn2S4 nanoparticles promoted the separation of photogenerated electronholes and broadened the light response range.The detailed characterizations,including surface morphology,elements valence state,and photocurrent performance,demonstrated that the enhanced separation of photogenerated carriers was the pivotal reason for the enhanced photocatalysis reaction.Benefiting from the excellent photocatalytic characteristics,the 5% mass ratio of BZ composite presented the highest MO degradation rate of 0.00997 min^-1,which was 1.9 and 10.3 times greater than the virgin ZnIn2S4 and BiVO4,respectively.Furthermore,the BZ hybrid materials indicated a well photo-stability in the four recycling tests.展开更多
Photoinduced intermolecular charge transfer(PICT)determines the voltage loss in bulk heterojunction(BHJ)organic photovoltaics(OPVs),and this voltage loss can be minimized by inducing efficient PICT,which requires ener...Photoinduced intermolecular charge transfer(PICT)determines the voltage loss in bulk heterojunction(BHJ)organic photovoltaics(OPVs),and this voltage loss can be minimized by inducing efficient PICT,which requires energy-state matching between the donor and acceptor at the BHJ interfaces.Thus,both geometrically and energetically accessible delocalized state matching at the hot energy level is crucial for achieving efficient PICT.In this study,an effective method for quantifying the hot state matching of OPVs was developed.The degree of energy-state matching between the electron donor and acceptor at BHJ interfaces was quantified using a mismatching factor(MF)calculated from the modified optical density of the BHJ.Furthermore,the correlation between the open-circuit voltage(Voc)of the OPV device and energy-state matching at the BHJ interface was investigated using the calculated MF.The OPVs with small absolute MF values exhibited high Voc values.This result clearly indicates that the energy-state matching between the donor and acceptor is crucial for achieving a high Voc in OPVs.Because the MF indicates the degree of energy-state matching,which is a critical factor for suppressing energy loss,it can be used to estimate the Voc loss in OPVs.展开更多
Semitransparent organic photovoltaics(STOPVs)have gained wide attention owing to their promising applications in building-integrated photovoltaics,agrivoltaics,and floating photovoltaics.Organic semiconductors with hi...Semitransparent organic photovoltaics(STOPVs)have gained wide attention owing to their promising applications in building-integrated photovoltaics,agrivoltaics,and floating photovoltaics.Organic semiconductors with high charge carrier mobility usually have planar and conjugated structures,thereby showing strong absorption in visible region.In this work,a new concept of incorporating transparent inorganic semiconductors is proposed for high-performance STOPVs.Copper(I)thiocyanate(CuSCN)is a visible-transparent inorganic semiconductor with an ionization potential of 5.45 eV and high hole mobility.The transparency of CuSCN benefits high average visible transmittance(AVT)of STOPVs.The energy levels of CuSCN as donor match those of near-infrared small molecule acceptor BTP-eC9,and the formed heterojunction exhibits an ability of exciton dissociation.High mobility of CuSCN contributes to a more favorable charge transport channel and suppresses charge recombination.The control STOPVs based on PM6/BTP-eC9 exhibit an AVT of 19.0%with a power conversion efficiency(PCE)of 12.7%.Partial replacement of PM6 with CuSCN leads to a 63%increase in transmittance,resulting in a higher AVT of 30.9%and a comparable PCE of 10.8%.展开更多
Charge-based studies,in particular investigations of mass distribution,are still almost absent,although the efficiency of the organic Rankine cycle(ORC)has attracted a great deal of scholarly attention.This paper aims...Charge-based studies,in particular investigations of mass distribution,are still almost absent,although the efficiency of the organic Rankine cycle(ORC)has attracted a great deal of scholarly attention.This paper aims to provide a new perspective on the intrinsic relationship among the mass distribution,phase-zone distribution in the heat exchanger(HEX),charge of working fuid(WF),rotation speed of the pump(RSP),and system performance.A comprehensive ORC simulation model is presented by linking each component's sub-models,including the independent models for HEX,pump,and expander in an object-oriented fashion.The visualization study of mass distribution of the WF in the system is investigated under different working conditions.Furthermore,the volume and mass of the gas phase,two-phase and liquid phase of WF in the HEX and their variation rules are analyzed in-depth.Finally,the strategies of charge reduction considering HEX areas and pipe sizes are investigated.The results show that the model based on the interior-point method provides high levels of accuracy and robustness.The mass ratio of the WF is concentrated in the liquid receiver,especially in the regenerator,which is 32.9%and 21.9%of the total mass,respectively.Furthermore,2.4 kg(6.9%)WF in the system gradually migrates to the high-temperature side as the RSP increases while 6.1 kg(17.4%)WF migrates to the low-temperature side,especially to the condenser,as the charge in the system increases.Output power and efficiency both decrease gradually after the peak due to changes in RSP and charge.Last,reducing heat transfer areas of the condenser and regenerator is the most effective way to reduce WF charge.展开更多
The organic cocrystal strategy has provided a convenient and efficient platform for preparing organic photothermal materials.However,the rapidly directional preparation of cocrystals with desirable photothermal proper...The organic cocrystal strategy has provided a convenient and efficient platform for preparing organic photothermal materials.However,the rapidly directional preparation of cocrystals with desirable photothermal properties remains challenging due to a lack of suitable design ideas.Here,two new photothermal cocrystals,MTC and MFC,based on acceptor molecules(TCNQ and F4TCNQ)with different electron-withdrawing capacities were quickly prepared by the coprecipitation method,aiming to explore the effect of charge transfer(CT)interaction on photothermal properties.Compared with MTC,the stronger intermolecular CT interaction in MFC facilitates extending the absorption range(from the NIR-I to the NIR-II region)and enhancing the non-radiative transition process.Under the 808 nm laser irradiation,the photothermal conversion efficiency(PCE)of MFC is 54.6%,whereas MTC displays a mere 36.8%.The MFC cocrystal was further combined with a flexible polymer substrate(HPDMS)to prepare a flexible wearable heater(HPDMS@MFC),which exhibits excellent NIR-II photothermal performance.This work points out a research direction for the rapid assembly of efficient photothermal cocrystals and additionally provides an extensive application prospect for organic photothermal cocrystals in the field of wearable devices.展开更多
基金supported by the National Natural Science Foundation of China (51672156)Local Innovative Research Teams Project of Guangdong Pearl River Talents Program (No. 2017BT01N111)+2 种基金Guangdong Province Technical Plan Project (2017B010119001)Shenzhen Technical Plan Project (JCYJ20170817161221958 and JCYJ20170412170706047)Shenzhen Graphene Manufacturing Innovation Center (201901161513)。
文摘Aqueous Zinc-ion batteries(ZIB) are attracting immense attention because of their merits of excellent safety and quite cheap properties compared with lithium-ion batteries(LIB).Manganese oxide is one of the most important cathode materials of ZIB.In this paper,α-Mn2O3 used as cathode of ZIB is synthesized via Metal-Organic Framework(MOF)-derived method,which delivers a high specific capacity of225 mAh g^(-1) at 0.05 A g^(-1) and 92.7 mAh g^(-1) after 1700 cycles at 2 A g^(-1).The charge storage mechanism of α-Mn2O3 cathode is found to greatly depend on the discharge current density.At lower current density discharging,the H+ and Zn2+ are successively intercalated into the α-Mn2O3 before and after the "turning point" of discharge voltage and their discharging products present obviously different morphologies changing from flower-like to large plate-like products.At a higher current density,the low-voltage plateau after the turning point disappears due to the decrease of amount of Zn2+ intercalation and the H+intercalation is dominated in α-Mn2 O3.This study provides significant understanding for future design and research of high-performance Mn-based cathodes of ZIB.
基金supported by the National Natural Science Foundation of China(21334002,51303057,51373054,91233113)the National Basic Research Program of China(2013CB834705,2014CB643504,2015CB655003)+1 种基金the Fundamental Research Funds for the Central Universities(2013ZZ0001)the Introduced Innovative R&D Team of Guangdong(201101C0105067115)
文摘Organic light-emitting diodes （OLEDs） have been extensively studied since the first efficient device based on small molecular luminescent materials was reported by Tang. Organic electroluminescent material, one of the centerpieces of OLEDs, has been the focus of studies by many material scientists. To obtain high luminosity and to keep material costs low, a few remarkable design concepts have been developed. Aggregation-induced emission （AIE） materials were invented to overcome the common fluorescence-quenching problem, and cross-dipole stacking of fluorescent molecules was shown to be an effective method to get high solid-state luminescence. To exceed the limit of internal quantum efficiency of conventional fluorescent materials, phosphorescent materials were successfully applied in highly efficient electroluminescent devices. Most recently, delayed flu- orescent materials via reverse-intersystem crossing （RISC） from triplet to singlet and the ＂hot exciton＂ materials based on hy- bridized local and charge-transfer （HLCT） states were developed to he a new generation of low-cost luminescent materials as efficient as phosphorescent materials. In terms of the device-fabrication process, solution-processible small molecular lumi- nescent materials possess the advantages of high purity （vs. polymers） and low procession cost （vs. vacuum deposition）, which are garnering them increasing attention. Herein, we review the progress of the development of small-molecule luminescent materials with different design concepts and features, and also briefly examine future development tendencies of luminescent materials.
基金supported by the National Key Research and Development Program of China(No.2022YFB4200600)the National Natural Science Foundation of China(Nos.52173185 and 52127806)+1 种基金the Fundamental Research Funds for the Central Universities(Nos.226-2022-00133 and 226-2022-00209)L.Z.thanks the research start-up fund from Zhejiang University.
文摘Since 1986,the donor-acceptor (D:A) heterojunction has been regarded a necessity for high-efficiency organic photovoltaics (OPVs),due to its unique advantage in compensating the intrinsic limitations of organic semiconductors,such as high exciton binding energy and poor ambipolar charge mobility. While this adversely causes tremendous non-radiative charge recombination and instability issues,which currently become the most critical limits for commercialization of OPVs. Here,we present a concept-to-proof study on the potential of D:A heterojunction free OPV by taking advantage of recent progress of non-fullerene acceptors. First,we demonstrate that the “free carriers” can be spontaneously generated upon illumination in an NFA,i.e.,the 6TIC-4F single layer. Second,the 6TIC-4F layer also exhibits good ambipolar charge transporting property. These exceptional characteristics distinguish it from the traditional organic semiconductors,and relieve it from the reliance of D:A heterojunction to independently work as active layer. As a result,the subsequent OPV by simply sandwiching the 6TIC-4F layer between the cathode and anode yields a considerably high power conversion efficiency ~1%. Moreover,we find the D:A heterojunction free device exhibits two order of magnitude higher electroluminescence quantum efficiency and significantly reduced VOC loss by 0.16 eV compared to those of the D:A BHJ structure,validating its promise for higher efficiency in the future. Therefore,our work demonstrates the possibility of using D:A heterojunction-free device structure for high performance,that can potentially become the next game changer of OPV.
基金supported by the National Natural Science Foundation of China (Nos.41371245 and 41230855)the National Key Technology R&D Program of China (No.2012BAJ24B06)
文摘In this study, biochars from rice straw （Oryza sativa L.） were prepared at 200-600 ℃ by oxygen-limited pyrolysis to investigate the changes in properties of rice straw biochars produced at different temperatures, and to examine the adsorption capacities of the biochars for a heavy metal, copper（II） （Cu（II））, and an organic insecticide of cyromazine, as well as to further reveal the adsorption mechanisms. The results obtained with batch experiments showed that the amount of Cu（II） adsorbed varied with the pyrolysis temperatures of rice straw biochar. The biochar produced at 400 ~C had the largest adsorption capacity for Cu（II） （0.37 mol kg-1） among the biochars, with the non-electrostatic adsorption as the main adsorption mechanism. The highest adsorption capacity for cyromazine （156.42 g kg-1） was found in the rice straw biochar produced at 600 ℃, and cyromazine adsorption was exclusively predominated by surface adsorption. An obvious competitive adsorption was found between 5 mmol L-1 Cu（II） and 2 g L-1 cyromazine when they were in the binary solute system. Biochar may be used to remediate heavy metal- and organic insecticide-contaminated water, while the pyrolysis temperature of feedstocks for producing biochar should be considered for the restoration of multi-contamination.
基金Project supported by the Knowledge Innovation Program Foundation of the Chinese Academy of Sciences (No. ISSASIP0108) the National Natural Science Foundation of China (No. 40271062).
文摘Low-molecular-weight (LMW) organic acids exist widely in soils and have beenimplicated in many soil processes. The objective of the present paper was to evaluate effect of twoLMW organic acids, citric acid and oxalic acid, on Cl^-adsorption by three variable charge soils, alatosol, a lateritic red soil and a red soil, using a batch method. The results showed that thepresence of citric acid and oxalic acid led to a decrease in Cl^- adsorption with larger decreasesfor citric acid. Among the different soils Cl^- adsorption in the lateritic red soil and the redsoil was more affected by both the LMW organic acids than that in the latosol.
基金the National Natural Science Foundation of China(22378148,21975084,51672089)the Natural Science Foundation of Guangdong Province(2021A1515010075)for their supports。
基金supported by the National Key R&D Program of China(grant no.2020YFA0709900)the National Natural Science Foundation of China(grant nos.21971041,22201042,22027805,62134003,and 22104016)+2 种基金the Natural Science Foundation of Fujian Province(grant nos.2020J01447,2022J06008,and 2022J0121)the Research Foundation of Education Bureau of Fujian Province(grant no.JAT210001)the Fuzhou University Testing Fund of Precious Apparatus(grant no.2022T001).
文摘Organic scintillators that efficiently generate bright triplet excitons are of critical importance for highperformance X-ray-excited luminescence in radiation detection.However,the nature of triplet-singlet spinforbidden transitions in these materials often result in long-lived phosphorescence,which is undesirable for ultrafast X-ray detection and imaging.Here we demonstrate that the effect of hybridized local and charge-transfer(HLCT)excited states enables organic scintillators to exhibit highly efficient and fast radioluminescence(RL)in response to X-ray irradiation.Our experimental and theoretical investigation shows that the oxidized 1,8-naphthalimide-phenothiazine dyad(OMNI-PTZ 2)with HLCT-excited states has an enhanced overlap integral of the highest occupied molecular orbital(HOMO)and lowest unoccupied molecular orbital(LUMO)on MNIπ-orbitals,and moderate donor–acceptor electron interactions.As a result,the RL of these crystals exhibits a 61-fold increase and its monoexponential decay lifetime is three orders of magnitude faster compared to its corresponding thermally activated delayed fluorescence(TADF)molecule MNI-PTZ 1.We further demonstrate the practical utility of the OMNI-PTZ 2(G)in high-performance X-ray detection and imaging,achieving an X-ray dose sensitivity of 97 nGy s−1 and an exceptional spatial resolution of 20 lp/mm.Our study provides a promising molecular design principle for utilizing triplet excitons to develop high-efficiency and fast X-ray scintillators for the development of next-generation flexible and stretchable X-ray imaging detectors.
基金Project supported by the National Natural Sciences Foundation of China (No. 40371065).
文摘Batch equilibrium experiments were conducted to investigate cadmium （Cd） sorption by two permanent-charge soils, a yellow-cinnamon soil and a yellow-brown soil, and two variable-charge soils, a red soil and a latosol, with addition of selected organic acids （acetate, tartrate, and citrate）. Results showed that with an increase in acetate concentrations from 0 to 3.0 mmol L^-1, Cd sorption percentage by the yellow-cinnamon soil, the yellow-brown soil, and the latosol decreased. The sorption percentage of Cd by the yellow-clnnamon soil and generally the yellow-brown soil （permanent-charge soils） decreased with an increase in tartrate concentration, but increased at low tartrate concentrations for the red soil and the latosol. Curves of percentage of Cd sorption for citrate were similar to those for tartrate. For the variable-charge soils with tartrate and citrate, there were obvious peaks in Cd sorption percentage. These peaks, where organic acids had maximum influence, changed with soil type, and were at a higher organic acid concentration for the variable-charge soils than for the permanent charge soils. Addition of cadmium after tartrate adsorption resulted in higher sorption increase for the varlable-charge soils than permanent-charge soils. When tartrate and Cd solution were added together, sorption of Cd decreased with tartrate concentration for the yellow-brown soil, but increased at low tartrate concentrations and then decreased with tartrate concentration for the red soil and the latosol.
基金supported by the National Natural Science Foundation of China(52303239)the Natural Science Foundation of Shandong Province(ZR2022QB141,2023HWYQ-087)+1 种基金Jiangsu Key Laboratory for Carbon-Based Functional Materials&Devices,Soochow University(KJS2209)Sichuan Science and Technology Program(2023NSFSC0990)。
文摘Solution processability is a unique property of organic semiconductors. The compact and regular π-π stacking between molecules is paramount in the performance of organic optoelectronic devices. However, it is still a challenge to improve their stacking quality without sacrificing the solution-processability from the aspect of materials design. Here, delicately engineered additives are presented to promote the formation of ordered aggregation of conjugated molecules by regulating their nucleation and growth dynamics. Intriguingly, the long-chain BTP-eC9-4F molecules can realize ordered aggregation comparable to short-chain ones without sacrificing processability. The domain size of BTP-eC9-4F aggregation is enlarged from 24.2 to 32.2 nm in blend films.Thereby exciton diffusion and charge transport become faster, contributing to the suppression of recombination losses. As a result, a power conversion efficiency of 19.2% is achieved in D18:BTP-eC9-4F based organic photovoltaics. Our findings demonstrate a facile strategy to improve the packing quality of solution-processed organic semiconductors for high-efficiency photovoltaics and beyond photovoltaics.
基金financial supports from the National Natural Science Foundation of China(Nos.51908485 and 51608468)the China Postdoctoral Science Foundation(No.2019T120194)the University Science and Technology Program Project of Hebei Provincial Department of Education(No.QN2018258)。
文摘Constructing a Z-scheme is a significant approach to improve the separation of photogene rated carriers for effective organic pollutant degradation.Herein,a BiVO4/ZnIn2S4(BZ) Z-scheme composite was successfully synthesized,and applied to photodegrade methyl orange(MO) irradiated by a LED lamp.Anchoring the BiVO4 on the ZnIn2S4 nanoparticles promoted the separation of photogenerated electronholes and broadened the light response range.The detailed characterizations,including surface morphology,elements valence state,and photocurrent performance,demonstrated that the enhanced separation of photogenerated carriers was the pivotal reason for the enhanced photocatalysis reaction.Benefiting from the excellent photocatalytic characteristics,the 5% mass ratio of BZ composite presented the highest MO degradation rate of 0.00997 min^-1,which was 1.9 and 10.3 times greater than the virgin ZnIn2S4 and BiVO4,respectively.Furthermore,the BZ hybrid materials indicated a well photo-stability in the four recycling tests.
基金National Research Foundation of Korea,Grant/Award Number:2022R1A6A1A03051158BrainLink Program,Grant/Award Number:2022H1D3A3A01077343Nano Material Technology Development Program,Grant/Award Number:2021M3H4A1A02057007。
文摘Photoinduced intermolecular charge transfer(PICT)determines the voltage loss in bulk heterojunction(BHJ)organic photovoltaics(OPVs),and this voltage loss can be minimized by inducing efficient PICT,which requires energy-state matching between the donor and acceptor at the BHJ interfaces.Thus,both geometrically and energetically accessible delocalized state matching at the hot energy level is crucial for achieving efficient PICT.In this study,an effective method for quantifying the hot state matching of OPVs was developed.The degree of energy-state matching between the electron donor and acceptor at BHJ interfaces was quantified using a mismatching factor(MF)calculated from the modified optical density of the BHJ.Furthermore,the correlation between the open-circuit voltage(Voc)of the OPV device and energy-state matching at the BHJ interface was investigated using the calculated MF.The OPVs with small absolute MF values exhibited high Voc values.This result clearly indicates that the energy-state matching between the donor and acceptor is crucial for achieving a high Voc in OPVs.Because the MF indicates the degree of energy-state matching,which is a critical factor for suppressing energy loss,it can be used to estimate the Voc loss in OPVs.
基金financially supported by the Sichuan Science and Technology Program (2023YFH0086, 2023YFH0085, 2023YFH0087 and 2023NSFSC0990)the State Key Laboratory of Polymer Materials Engineering (sklpme2022-3-02 and sklpme2023-2-11)the Tibet Foreign Experts Program (2022wz002)
文摘Semitransparent organic photovoltaics(STOPVs)have gained wide attention owing to their promising applications in building-integrated photovoltaics,agrivoltaics,and floating photovoltaics.Organic semiconductors with high charge carrier mobility usually have planar and conjugated structures,thereby showing strong absorption in visible region.In this work,a new concept of incorporating transparent inorganic semiconductors is proposed for high-performance STOPVs.Copper(I)thiocyanate(CuSCN)is a visible-transparent inorganic semiconductor with an ionization potential of 5.45 eV and high hole mobility.The transparency of CuSCN benefits high average visible transmittance(AVT)of STOPVs.The energy levels of CuSCN as donor match those of near-infrared small molecule acceptor BTP-eC9,and the formed heterojunction exhibits an ability of exciton dissociation.High mobility of CuSCN contributes to a more favorable charge transport channel and suppresses charge recombination.The control STOPVs based on PM6/BTP-eC9 exhibit an AVT of 19.0%with a power conversion efficiency(PCE)of 12.7%.Partial replacement of PM6 with CuSCN leads to a 63%increase in transmittance,resulting in a higher AVT of 30.9%and a comparable PCE of 10.8%.
文摘Charge-based studies,in particular investigations of mass distribution,are still almost absent,although the efficiency of the organic Rankine cycle(ORC)has attracted a great deal of scholarly attention.This paper aims to provide a new perspective on the intrinsic relationship among the mass distribution,phase-zone distribution in the heat exchanger(HEX),charge of working fuid(WF),rotation speed of the pump(RSP),and system performance.A comprehensive ORC simulation model is presented by linking each component's sub-models,including the independent models for HEX,pump,and expander in an object-oriented fashion.The visualization study of mass distribution of the WF in the system is investigated under different working conditions.Furthermore,the volume and mass of the gas phase,two-phase and liquid phase of WF in the HEX and their variation rules are analyzed in-depth.Finally,the strategies of charge reduction considering HEX areas and pipe sizes are investigated.The results show that the model based on the interior-point method provides high levels of accuracy and robustness.The mass ratio of the WF is concentrated in the liquid receiver,especially in the regenerator,which is 32.9%and 21.9%of the total mass,respectively.Furthermore,2.4 kg(6.9%)WF in the system gradually migrates to the high-temperature side as the RSP increases while 6.1 kg(17.4%)WF migrates to the low-temperature side,especially to the condenser,as the charge in the system increases.Output power and efficiency both decrease gradually after the peak due to changes in RSP and charge.Last,reducing heat transfer areas of the condenser and regenerator is the most effective way to reduce WF charge.
基金financially supported by the National Natural Science Foundation of China(22173008)Beijing Key Laboratory for Chemical Power Source and Green Catalysis(2013CX02031)。
基金the National Key R&D Program(2022YFB3603800)the National Natural Science Foundation of China(52121002,U21A6002)+1 种基金Tianjin Natural Science Foundation(20JCJQJC00300)the Fundamental ResearchFunds forthe Central Universities.
文摘The organic cocrystal strategy has provided a convenient and efficient platform for preparing organic photothermal materials.However,the rapidly directional preparation of cocrystals with desirable photothermal properties remains challenging due to a lack of suitable design ideas.Here,two new photothermal cocrystals,MTC and MFC,based on acceptor molecules(TCNQ and F4TCNQ)with different electron-withdrawing capacities were quickly prepared by the coprecipitation method,aiming to explore the effect of charge transfer(CT)interaction on photothermal properties.Compared with MTC,the stronger intermolecular CT interaction in MFC facilitates extending the absorption range(from the NIR-I to the NIR-II region)and enhancing the non-radiative transition process.Under the 808 nm laser irradiation,the photothermal conversion efficiency(PCE)of MFC is 54.6%,whereas MTC displays a mere 36.8%.The MFC cocrystal was further combined with a flexible polymer substrate(HPDMS)to prepare a flexible wearable heater(HPDMS@MFC),which exhibits excellent NIR-II photothermal performance.This work points out a research direction for the rapid assembly of efficient photothermal cocrystals and additionally provides an extensive application prospect for organic photothermal cocrystals in the field of wearable devices.
