Organic solar cells(OSCs)processed without halogenated solvents and complex treatments are essential for future commercialization.Herein,we report three novel small molecule acceptors(NFAs)consisting of a Y6-like core...Organic solar cells(OSCs)processed without halogenated solvents and complex treatments are essential for future commercialization.Herein,we report three novel small molecule acceptors(NFAs)consisting of a Y6-like core but withπ-extended naphthalene with progressively more chlorinated end-capping groups and a longer branched chain on the Nitrogen atom.These NFAs exhibit good solubilities in nonchlorinated organic solvents,broad optical absorptions,closeπ-πstacking distances(3.63–3.84A),and high electron mobilities(~10^(-3)cm^(2)V^(-1)s^(-1)).The o-xylene processed and as-cast binary devices using PM6 as the donor polymer exhibit a PCE increasing upon progressive chlorination of the naphthalene end-capping group from 8.93%for YN to 14.38%for YN-Cl to 15.00%for YN-2Cl.Furthermore similarly processed ternary OSCs were fabricated by employing YN-Cl and YN-2Cl as the third component of PM6:CH1007 blends(PCE=15.75%).Compared to all binary devices,the ternary PM6:CH1007:YN-Cl(1:1:0.2)and PM6:CH1007:YN-2Cl(1:1:0.2)cells exhibit significantly improved PCEs of 16.49%and15.88%,respectively,which are among the highest values reported to date for non-halogenated solvent processed OSCs without using any additives and blend post-deposition treatments.展开更多
The oxidative dehydrogenation of isobutane to isobutene was examined for the use in the preparation of FSM-16 and related compounds doped by chromium with expectations that a yield of isobutene of greater than 8% coul...The oxidative dehydrogenation of isobutane to isobutene was examined for the use in the preparation of FSM-16 and related compounds doped by chromium with expectations that a yield of isobutene of greater than 8% could be achieved. The activity depended on the molding procedure of the catalyst and the doping method of the chromium species. In the present study, 8.8% and 8.3% of the yield of isobutene were obtained at 0.75 h and 6 h on-stream for the catalyst (Cr-loading; 6.2 wt.%) molded using wet treatment hut not pressurization treatment, in which the chromium species were directly added into the aqueous solution containing raw FSM-16 (hydrated sodium silicate powder) at an initial stage of the catalyst preparation. The structure information was based on XRD (X-ray diffraction), the specific surface area was determined using a conventional BET (Brunauer-Emmett-Teller) nitrogen adsorption and the loading of chromium was estimated using ICP (inductively coupled plasma). All those parameters combined with the molding method indicated that the catalytic activity was more influenced by the loading of chromium into bulk but not on surface of the catalyst rather than by the hexagonal structure of FSM-16 and the surface area.展开更多
The phase transition behavior and aggregating states of [smectic LCP, PS(4BC/DM)/nematic LC, E7/chiral dopant, CB 15] ternary composite system were investigated on the basis of differential scanning calorimetry (DSC)...The phase transition behavior and aggregating states of [smectic LCP, PS(4BC/DM)/nematic LC, E7/chiral dopant, CB 15] ternary composite system were investigated on the basis of differential scanning calorimetry (DSC) measurement, polarizing optical microscopy (POM) observation and wide angle X ray diffraction (WAXD) patterns. It was demonstrated that if the weight ratio of the chiral dopant was fixed as 4.8wt%, an induced chiral nematic (N *) phase existed in the ternary system when PS(4BC/DM) ratio was below 47.6 wt%. Moreover, smectic like long range ordering appeared in the induced N * phase in a certain temperature range just above the smectic A(S A) N * phase transition when PS(4BC/DM) ratio was between 19.1wt% and 47.6wt%.展开更多
The biological properties of therapeutic peptides,such as their pharmacokinetics and pharmacodynamics,are correlated with their structure and aggregation properties.Herein,we studied the aggregation properties of a th...The biological properties of therapeutic peptides,such as their pharmacokinetics and pharmacodynamics,are correlated with their structure and aggregation properties.Herein,we studied the aggregation properties of a therapeutic peptide(CIGB-814),currently in phase 2 clinical trial,for the treatment of rheumatoid arthritis over a wide range of concentrations(μM-mM).We applied spectroscopic techniques(fluorescence,circular dichro-ism,resonance,and dynamic light scattering),atomic force microscopy,and molecular dynamics simulations to determine the aggregation mechanism of CIGB-814.We found that the hierarchical aggregation of CIGB-814 at micromolar concentrations was initiated by the formation of peptide oligomers.Subsequently,the peptide oligomers trigger the nucleation and growth of peptide nanostructures(cac=123μM),ultimately leading to the fibrillization of CIGB-814(cac’=508μM).These results pave the way for a deeper understanding of the CIGB-814 therapeutic activity and may give important insights on its pharmacokinetics.展开更多
Main observation and conclusion Two new uranium(VI)phosphonate compounds,namely K_(8)[N(C_(2)H_(5))_(4)]_(2)(UO_(2))_(17)(H_(2)O)_(4)[CH_(2)(PO_(3))_(2)]_(8)[CH_(2)(PO_(3))(PO_(3)H)]_(4)·16(H_(2)O)(1)and[N(C_(2)H...Main observation and conclusion Two new uranium(VI)phosphonate compounds,namely K_(8)[N(C_(2)H_(5))_(4)]_(2)(UO_(2))_(17)(H_(2)O)_(4)[CH_(2)(PO_(3))_(2)]_(8)[CH_(2)(PO_(3))(PO_(3)H)]_(4)·16(H_(2)O)(1)and[N(C_(2)H_(5))_(4)]_(4)(H_(3)O)_(2)(UO_(2))_(10)[CH_(2)(PO_(3))_(2)]_(5)[CH_(2)(PO_(3))(PO_(3)H)]_(2)·10H_(2)O(2),have been synthesized under mild hydro/solvothermal condition.The structural analysis of the two compounds reveals that they both contain all three typical coordination geometries of the U(VI)ions,including UO;tetragonal,UO,pentagonal,and UOg hexagonal bipyramids.Moreover,compound 1 displays a tempera-ture-induced single crystal to single crystal phase transformation as confirmed by the Single-crystal X-ray diffraction data collected at different temperatures.Temperature-dependent fluorescence spectra presented herein illustrate the perturbation of the electronic structure of uranyl centers.展开更多
J-aggregation and H-aggregation are identified as two classical models of function-ally oriented non-covalent interactions,and significant attention has been drawn by researchers.However,due to the scarcity of single-...J-aggregation and H-aggregation are identified as two classical models of function-ally oriented non-covalent interactions,and significant attention has been drawn by researchers.However,due to the scarcity of single-crystal examples of H-aggregation,a comprehensive understanding of the relationship between its stacking mode and optical behaviour has been hindered.In recent studies,two polyaromatic Schiff base compounds,Cl-Salmphen and H-Salmphen,were successfully synthe-sized,and both were found to exhibit H-aggregation.In thefindings,H-Salmphen was shown to display typical C─H···πinteractions,characteristic of Aggregation-Induced Emission(AIE)active molecules,whereas its halogenated counterpart was identified as behaving similar to Aggregation-Caused Quenching(ACQ)active molecules.These types of results suggest that identical intermolecular interactions can produce differing optical behaviours.Light was shed,at least in part,on the for-mation mechanisms of H-type aggregates and their luminescence properties from these observations.Additionally,the high optical signal-to-noise ratio inherent to H-aggregates was utilized for the exploration of water content detection.As an outcome,a high-performancefluorescentfilter paper was developed,enabling easy real-time detection using a smartphone.展开更多
A nonmetal doping strategy was exploited for the conventional La_(0.5)Sr_(0.5)FeO_(3-δ)(LSF)cathode,allowing high performance for proton-conducting solid oxide fuel cells(H-SOFCs).Unlike previous studies focusing on ...A nonmetal doping strategy was exploited for the conventional La_(0.5)Sr_(0.5)FeO_(3-δ)(LSF)cathode,allowing high performance for proton-conducting solid oxide fuel cells(H-SOFCs).Unlike previous studies focusing on the utilization of metal oxides as dopants,phosphorus,which is a nonmetal element,was used as the cation dopant for LSF by partially replacing Fe ions to form the new La_(0.5)Sr_(0.5)Fe_(0.9)P_(0.1)O_(3-δ)(LSFP)compound.The H-SOFC using the LSFP cathode showed a two-fold peak power density as compared to that using the LSF cathode.Both experimental studies and first-principle calculations were used to unveil the mechanisms for the high performance of the LSFP cells.展开更多
基金supported by the National Natural Science Foundation of China(61804073)the Center for Light Energy Activated Redox Processes(LEAP),an Energy Frontier Research Center funded by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences,under award DE-SC0001059+3 种基金the Mat CI Facility which receives support from the National Science Foundation MRSEC Program(NSF DMR-1720139)of the Materials Research Center at Northwestern Universitysupport from the US Office of Naval Research Contract N00014-20-1-2116the U.S.Department of Energy under contract No.DE-AC02-05CH11231at beamline 8-ID-E of the Advanced Photon Source,a U.S.Department of Energy(DOE)Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No.DE-AC0206CH11357。
文摘Organic solar cells(OSCs)processed without halogenated solvents and complex treatments are essential for future commercialization.Herein,we report three novel small molecule acceptors(NFAs)consisting of a Y6-like core but withπ-extended naphthalene with progressively more chlorinated end-capping groups and a longer branched chain on the Nitrogen atom.These NFAs exhibit good solubilities in nonchlorinated organic solvents,broad optical absorptions,closeπ-πstacking distances(3.63–3.84A),and high electron mobilities(~10^(-3)cm^(2)V^(-1)s^(-1)).The o-xylene processed and as-cast binary devices using PM6 as the donor polymer exhibit a PCE increasing upon progressive chlorination of the naphthalene end-capping group from 8.93%for YN to 14.38%for YN-Cl to 15.00%for YN-2Cl.Furthermore similarly processed ternary OSCs were fabricated by employing YN-Cl and YN-2Cl as the third component of PM6:CH1007 blends(PCE=15.75%).Compared to all binary devices,the ternary PM6:CH1007:YN-Cl(1:1:0.2)and PM6:CH1007:YN-2Cl(1:1:0.2)cells exhibit significantly improved PCEs of 16.49%and15.88%,respectively,which are among the highest values reported to date for non-halogenated solvent processed OSCs without using any additives and blend post-deposition treatments.
文摘The oxidative dehydrogenation of isobutane to isobutene was examined for the use in the preparation of FSM-16 and related compounds doped by chromium with expectations that a yield of isobutene of greater than 8% could be achieved. The activity depended on the molding procedure of the catalyst and the doping method of the chromium species. In the present study, 8.8% and 8.3% of the yield of isobutene were obtained at 0.75 h and 6 h on-stream for the catalyst (Cr-loading; 6.2 wt.%) molded using wet treatment hut not pressurization treatment, in which the chromium species were directly added into the aqueous solution containing raw FSM-16 (hydrated sodium silicate powder) at an initial stage of the catalyst preparation. The structure information was based on XRD (X-ray diffraction), the specific surface area was determined using a conventional BET (Brunauer-Emmett-Teller) nitrogen adsorption and the loading of chromium was estimated using ICP (inductively coupled plasma). All those parameters combined with the molding method indicated that the catalytic activity was more influenced by the loading of chromium into bulk but not on surface of the catalyst rather than by the hexagonal structure of FSM-16 and the surface area.
文摘The phase transition behavior and aggregating states of [smectic LCP, PS(4BC/DM)/nematic LC, E7/chiral dopant, CB 15] ternary composite system were investigated on the basis of differential scanning calorimetry (DSC) measurement, polarizing optical microscopy (POM) observation and wide angle X ray diffraction (WAXD) patterns. It was demonstrated that if the weight ratio of the chiral dopant was fixed as 4.8wt%, an induced chiral nematic (N *) phase existed in the ternary system when PS(4BC/DM) ratio was below 47.6 wt%. Moreover, smectic like long range ordering appeared in the induced N * phase in a certain temperature range just above the smectic A(S A) N * phase transition when PS(4BC/DM) ratio was between 19.1wt% and 47.6wt%.
基金Russian Foundation for Basic Research and Japan Society for the Promotion of Science for support within the grantRFBR(12-02-92107-ЯФ)Israeli Ministry of Science&Technology(3-9754)
基金This project received funding from the European Union Horizon 2020 Research and Innovation Program under the Marie Skłodowska-Curie grant agreement no.872233(“PEPSA-MATE”).GB acknowledges CINECA and the EU-PRACE program for the CPU time.FC acknowledges the funding received as an award of an RMIT senior vice chancellor fel-lowship.
文摘The biological properties of therapeutic peptides,such as their pharmacokinetics and pharmacodynamics,are correlated with their structure and aggregation properties.Herein,we studied the aggregation properties of a therapeutic peptide(CIGB-814),currently in phase 2 clinical trial,for the treatment of rheumatoid arthritis over a wide range of concentrations(μM-mM).We applied spectroscopic techniques(fluorescence,circular dichro-ism,resonance,and dynamic light scattering),atomic force microscopy,and molecular dynamics simulations to determine the aggregation mechanism of CIGB-814.We found that the hierarchical aggregation of CIGB-814 at micromolar concentrations was initiated by the formation of peptide oligomers.Subsequently,the peptide oligomers trigger the nucleation and growth of peptide nanostructures(cac=123μM),ultimately leading to the fibrillization of CIGB-814(cac’=508μM).These results pave the way for a deeper understanding of the CIGB-814 therapeutic activity and may give important insights on its pharmacokinetics.
基金the National Natural Science Foundation of China(21906113,21561018,21790374,and 22066014)the Priority Academic Pro-gram Development of Jiangsu Higher Education Institutions(PAPD)the Applied Basic Research Foundation of Yunnan Province(2017FH001-023).
文摘Main observation and conclusion Two new uranium(VI)phosphonate compounds,namely K_(8)[N(C_(2)H_(5))_(4)]_(2)(UO_(2))_(17)(H_(2)O)_(4)[CH_(2)(PO_(3))_(2)]_(8)[CH_(2)(PO_(3))(PO_(3)H)]_(4)·16(H_(2)O)(1)and[N(C_(2)H_(5))_(4)]_(4)(H_(3)O)_(2)(UO_(2))_(10)[CH_(2)(PO_(3))_(2)]_(5)[CH_(2)(PO_(3))(PO_(3)H)]_(2)·10H_(2)O(2),have been synthesized under mild hydro/solvothermal condition.The structural analysis of the two compounds reveals that they both contain all three typical coordination geometries of the U(VI)ions,including UO;tetragonal,UO,pentagonal,and UOg hexagonal bipyramids.Moreover,compound 1 displays a tempera-ture-induced single crystal to single crystal phase transformation as confirmed by the Single-crystal X-ray diffraction data collected at different temperatures.Temperature-dependent fluorescence spectra presented herein illustrate the perturbation of the electronic structure of uranyl centers.
基金the Program for Innovative Research Team(in Science and Technology)in Universities of Yunnan Province(IRTSTYN),the Recruitment Program of Yunnan Province Experts Provincial Young Talents(2019HB098)the Ten-Thousand Talents Program of Yunnan Province(YNWR-QNBJ-2018-273).
文摘J-aggregation and H-aggregation are identified as two classical models of function-ally oriented non-covalent interactions,and significant attention has been drawn by researchers.However,due to the scarcity of single-crystal examples of H-aggregation,a comprehensive understanding of the relationship between its stacking mode and optical behaviour has been hindered.In recent studies,two polyaromatic Schiff base compounds,Cl-Salmphen and H-Salmphen,were successfully synthe-sized,and both were found to exhibit H-aggregation.In thefindings,H-Salmphen was shown to display typical C─H···πinteractions,characteristic of Aggregation-Induced Emission(AIE)active molecules,whereas its halogenated counterpart was identified as behaving similar to Aggregation-Caused Quenching(ACQ)active molecules.These types of results suggest that identical intermolecular interactions can produce differing optical behaviours.Light was shed,at least in part,on the for-mation mechanisms of H-type aggregates and their luminescence properties from these observations.Additionally,the high optical signal-to-noise ratio inherent to H-aggregates was utilized for the exploration of water content detection.As an outcome,a high-performancefluorescentfilter paper was developed,enabling easy real-time detection using a smartphone.
基金the National Natural Science Foundation of China,Grant/Award Number:51972183the Hundred Youth Talents Program of Hunanthe Startup Funding for Talents at University of South China。
文摘A nonmetal doping strategy was exploited for the conventional La_(0.5)Sr_(0.5)FeO_(3-δ)(LSF)cathode,allowing high performance for proton-conducting solid oxide fuel cells(H-SOFCs).Unlike previous studies focusing on the utilization of metal oxides as dopants,phosphorus,which is a nonmetal element,was used as the cation dopant for LSF by partially replacing Fe ions to form the new La_(0.5)Sr_(0.5)Fe_(0.9)P_(0.1)O_(3-δ)(LSFP)compound.The H-SOFC using the LSFP cathode showed a two-fold peak power density as compared to that using the LSF cathode.Both experimental studies and first-principle calculations were used to unveil the mechanisms for the high performance of the LSFP cells.