For poly(9,9-dioctylfluorene)(PFO),β phase (coplanar conformation with the intra-chain torsion angle of 165°) has a greater conjugation length and higher degree of order compared to those of α phase, which favo...For poly(9,9-dioctylfluorene)(PFO),β phase (coplanar conformation with the intra-chain torsion angle of 165°) has a greater conjugation length and higher degree of order compared to those of α phase, which favors charge carrier transport. However, the highest content of β phase obtained so far is 45%. We propose to increase the content of β phase by promoting the solution aggregation of PFO molecules and extending film-forming time. For this purpose, 1,8-diiodooctane (DIO) is added to PFO o-xylene solution, which enhances the interaction of PFO chains and improves the planarity of PFO backbone, resulting in the formation of ordered aggregation. The aggregates act as nucleation centers to promote the formation of β phase. The content of β phase increases with increasing DIO concentration and reaches a platform of 39% as DIO is more than 4 vol%. Furthermore, the film is kept in a sealed environment with oxylene atmosphere for 3 h, thus the PFO molecules have enough time to diffuse to the crystallization front and achieve disorder-order transition. As a result, the crystallinity of PFO is improved significantly and the content of β phase increases to 52%, reaching the highest value reported so far.展开更多
Super-fine L1_(0)-Fe Pt nanoparticles(NPs)with high ordering degree were successfully prepared by a modified two-step sintering method,which includes low-temperature pre-sintering,and the high magnetic field(HMF)assis...Super-fine L1_(0)-Fe Pt nanoparticles(NPs)with high ordering degree were successfully prepared by a modified two-step sintering method,which includes low-temperature pre-sintering,and the high magnetic field(HMF)assisted post-sintering processes.The particle size of the L1_(0)-FePt NPs was obviously refined by lowering the sintering temperature.By applying the HMF during the post-sintering process,the fine size characteristics of L1_(0)-Fe Pt NPs were retained,and the ordering degree was significantly improved.The L1_(0)-Fe Pt NPs with sizes of about 4.5 nm,ordering degree of 0.940,and coercivity of 22.01 k Oe were obtained by this two-step sintering under a magnetic field of 12 T.The mechanism investigation of HMF enhancing the ordering degree indicates that the HMF enhances lattice distortion and magnetization energy(Zeeman energy).The enhanced lattice distortions cause high stress existing in the lattice,which can effectively promote the disordered-order transition.When the magnetic field reaches to 3 T,the Zeeman energy of the NPs is higher than the thermal disturbing energy of the NPs,and the magnetization effect is stronger.Therefore,the HMF(higher than 3 T)can obviously improve the disorder-order transition by lowering the energy barrier and accelerating the orderly diffusions of atoms.The HMF is a promising assistant to synthesize the L1_(0)-phase NPs with both of high ordering degree and super-fine size.展开更多
The crowding agent induced phase transition of amphiphilic block copolymers in solution was explicitly considered. The influence of the size and the volume fraction of the crowding agent on the phase separation of amp...The crowding agent induced phase transition of amphiphilic block copolymers in solution was explicitly considered. The influence of the size and the volume fraction of the crowding agent on the phase separation of ampbiphilic diblock copolymers is investigated by using self-consistent field theory （SCFT） method. The concentration of the disorder to order transition of the block copolymer decreases when the size of the crowding agent is larger than that of the solvent. The higher volume fraction of the crowding agent will induce the transition of the block copolymer from disorder to order state at a lower concentration. The relation between the size and the volume fraction of the crowding agent is elucidated. When the size of the crowding agent is larger, its volume fraction of the disorder to order transition of the block copolymer will be lower. The conformation of the crowding agent considered as a polymer chain is also studied and compared.展开更多
Tuberculosis drug resistance continues to threaten global health but the underline molecular mechanisms are not clear.Ethambutol(EMB),one of the well-known first-line drugs in tuberculosis treatment is,unfortunately,n...Tuberculosis drug resistance continues to threaten global health but the underline molecular mechanisms are not clear.Ethambutol(EMB),one of the well-known first-line drugs in tuberculosis treatment is,unfortunately,not free from drug resistance problems.Genomic studies have shown that some genetic mutations in Mycobacterium tuberculosis(Mtb)EmbR,and EmbC/A/B genes cause EMB resistance.EmbR-PknH pair controls embC/A/B operon,which encodes EmbC/A/B genes,and EMB interacts with EmbA/B proteins.However,the EmbR binding site on PknH was unknown.We conducted molecular simulation on the EmbR-peptides binding structures and discovered phosphorylated PknH 273-280(N′-HEALS^(P)DPD-C′)makesβstrand with the EmbR FHA domain,asβ-MoRF(MoRF;molecular recognition feature)does at its binding site.Hydrogen bond number analysis also supported the peptides’β-MoRF forming activity at the EmbR FHA domain.Also,we discovered that previously known phosphorylation residues might have their chronological order according to the phosphorylation status.The discovery validated that Mtb PknH 273-280(N′-HEALSDPD-C′)has reliable EmbR binding affinity.This approach is revolutionary in the computer-aided drug discovery field,because it is the first trial to discover the protein-protein interaction site,and find binding partner in nature from this site.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos. 51890871, 91833306, and 51573185)the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB12020300)
文摘For poly(9,9-dioctylfluorene)(PFO),β phase (coplanar conformation with the intra-chain torsion angle of 165°) has a greater conjugation length and higher degree of order compared to those of α phase, which favors charge carrier transport. However, the highest content of β phase obtained so far is 45%. We propose to increase the content of β phase by promoting the solution aggregation of PFO molecules and extending film-forming time. For this purpose, 1,8-diiodooctane (DIO) is added to PFO o-xylene solution, which enhances the interaction of PFO chains and improves the planarity of PFO backbone, resulting in the formation of ordered aggregation. The aggregates act as nucleation centers to promote the formation of β phase. The content of β phase increases with increasing DIO concentration and reaches a platform of 39% as DIO is more than 4 vol%. Furthermore, the film is kept in a sealed environment with oxylene atmosphere for 3 h, thus the PFO molecules have enough time to diffuse to the crystallization front and achieve disorder-order transition. As a result, the crystallinity of PFO is improved significantly and the content of β phase increases to 52%, reaching the highest value reported so far.
基金financially supported by the National Natural Science Foundation of China(Grant nos.51871045,52071070,and 51690161)the Fundamental Research Funds for the Central Universities(Grant no.N2017003)the Doctoral Start-up Foundation of Liaoning Province(Grant no.2019-BS-116)。
文摘Super-fine L1_(0)-Fe Pt nanoparticles(NPs)with high ordering degree were successfully prepared by a modified two-step sintering method,which includes low-temperature pre-sintering,and the high magnetic field(HMF)assisted post-sintering processes.The particle size of the L1_(0)-FePt NPs was obviously refined by lowering the sintering temperature.By applying the HMF during the post-sintering process,the fine size characteristics of L1_(0)-Fe Pt NPs were retained,and the ordering degree was significantly improved.The L1_(0)-Fe Pt NPs with sizes of about 4.5 nm,ordering degree of 0.940,and coercivity of 22.01 k Oe were obtained by this two-step sintering under a magnetic field of 12 T.The mechanism investigation of HMF enhancing the ordering degree indicates that the HMF enhances lattice distortion and magnetization energy(Zeeman energy).The enhanced lattice distortions cause high stress existing in the lattice,which can effectively promote the disordered-order transition.When the magnetic field reaches to 3 T,the Zeeman energy of the NPs is higher than the thermal disturbing energy of the NPs,and the magnetization effect is stronger.Therefore,the HMF(higher than 3 T)can obviously improve the disorder-order transition by lowering the energy barrier and accelerating the orderly diffusions of atoms.The HMF is a promising assistant to synthesize the L1_(0)-phase NPs with both of high ordering degree and super-fine size.
基金financially supported by the National Natural Science Foundations of China(Nos.20874046,21074053 and 51133002)National Basic Research Program of China(Nos.2010CB923303,2012CB821503)Fundamental Research Funds for the Central Universities(No.1095020515)
文摘The crowding agent induced phase transition of amphiphilic block copolymers in solution was explicitly considered. The influence of the size and the volume fraction of the crowding agent on the phase separation of ampbiphilic diblock copolymers is investigated by using self-consistent field theory （SCFT） method. The concentration of the disorder to order transition of the block copolymer decreases when the size of the crowding agent is larger than that of the solvent. The higher volume fraction of the crowding agent will induce the transition of the block copolymer from disorder to order state at a lower concentration. The relation between the size and the volume fraction of the crowding agent is elucidated. When the size of the crowding agent is larger, its volume fraction of the disorder to order transition of the block copolymer will be lower. The conformation of the crowding agent considered as a polymer chain is also studied and compared.
基金This work was supported by the National Institutes of Health Grant No.7R01GM118467-05the National Natural Science Foundation of China(31720103901).
文摘Tuberculosis drug resistance continues to threaten global health but the underline molecular mechanisms are not clear.Ethambutol(EMB),one of the well-known first-line drugs in tuberculosis treatment is,unfortunately,not free from drug resistance problems.Genomic studies have shown that some genetic mutations in Mycobacterium tuberculosis(Mtb)EmbR,and EmbC/A/B genes cause EMB resistance.EmbR-PknH pair controls embC/A/B operon,which encodes EmbC/A/B genes,and EMB interacts with EmbA/B proteins.However,the EmbR binding site on PknH was unknown.We conducted molecular simulation on the EmbR-peptides binding structures and discovered phosphorylated PknH 273-280(N′-HEALS^(P)DPD-C′)makesβstrand with the EmbR FHA domain,asβ-MoRF(MoRF;molecular recognition feature)does at its binding site.Hydrogen bond number analysis also supported the peptides’β-MoRF forming activity at the EmbR FHA domain.Also,we discovered that previously known phosphorylation residues might have their chronological order according to the phosphorylation status.The discovery validated that Mtb PknH 273-280(N′-HEALSDPD-C′)has reliable EmbR binding affinity.This approach is revolutionary in the computer-aided drug discovery field,because it is the first trial to discover the protein-protein interaction site,and find binding partner in nature from this site.
