Two-dimensional covalent organic frameworks(2D COFs)feature extendedπ-conjugation and ordered stacking sequence,showing great promise for high-performance photocatalysis.Periodic atomic frameworks of 2D COFs facilita...Two-dimensional covalent organic frameworks(2D COFs)feature extendedπ-conjugation and ordered stacking sequence,showing great promise for high-performance photocatalysis.Periodic atomic frameworks of 2D COFs facilitate the in-plane photogenerated charge transfer,but the precise ordered alignment is limited due to the non-covalentπ-stacking of COF layers,accordingly hindering out-of-plane transfer kinetics.Herein,we address a chiral induction method to construct a parallelly superimposed stacking chiral COF ultrathin shell on the support of SiO_(2) microsphere.Compared to the achiral COF analogues,the chiral COF shell with the parallel AA-stacking structure is more conducive to enhance the built-in electric field and accumulates photogenerated electrons for the rapid migration,thereby affording superior photocatalytic performance in hydrogen evolution from water splitting.Taking the simplest ketoenamine-linked chiral COF as a shell of SiO_(2) particle,the resulting composite exhibits an impressive hydrogen evolution rate of 107.1 mmol g^(-1)h^(-1)along with the apparent quantum efficiency of 14.31% at 475 nm.Furthermore,the composite photocatalysts could be fabricated into a film device,displaying a remarkable photocatalytic performance of 178.0 mmol m^(-2)h^(-1)for hydrogen evolution.Our work underpins the surface engineering of organic photocatalysts and illustrates the significance of COF stacking structures in regulating electronic properties.展开更多
The concentration of total nitrogen (TN), total phosphorus (TP) and organic material (OM) at sixty grid division in Lake Chaohu basin around the lake was studied, in order to investigate their spatial distribution cha...The concentration of total nitrogen (TN), total phosphorus (TP) and organic material (OM) at sixty grid division in Lake Chaohu basin around the lake was studied, in order to investigate their spatial distribution characteristics. The results showed that the average concentrations of TN, TP and OM were 1027 mg/kg, 483 mg/kg, 1.95%, and their concentrations ranged from 253 mg/kg to 2273 mg/kg, 223 mg/kg to 1173 mg/kg and 0.291% to 5.48%, respectively. The high concentration areas were located at the basins of Tuogao river and Zhao river while the low concentration areas were located at basins of Pai river, Nanfei river and Dianpu river. The concentrations of TN and OM were higher in East part than in West part. The spatial distribution of TN, TP and OM concentrations of the surface soil showed inconsistent with those of the water quality of the inflow rivers and the lake and the TN and TP of lake sediment studied.展开更多
Multiple earth observing satellites need to communicate with each other to observe plenty of targets on the Earth together. The factors, such as external interference, result in satellite information interaction delay...Multiple earth observing satellites need to communicate with each other to observe plenty of targets on the Earth together. The factors, such as external interference, result in satellite information interaction delays, which is unable to ensure the integrity and timeliness of the information on decision making for satellites. And the optimization of the planning result is affected. Therefore, the effect of communication delay is considered during the multi-satel ite coordinating process. For this problem, firstly, a distributed cooperative optimization problem for multiple satellites in the delayed communication environment is formulized. Secondly, based on both the analysis of the temporal sequence of tasks in a single satellite and the dynamically decoupled characteristics of the multi-satellite system, the environment information of multi-satellite distributed cooperative optimization is constructed on the basis of the directed acyclic graph(DAG). Then, both a cooperative optimization decision making framework and a model are built according to the decentralized partial observable Markov decision process(DEC-POMDP). After that, a satellite coordinating strategy aimed at different conditions of communication delay is mainly analyzed, and a unified processing strategy on communication delay is designed. An approximate cooperative optimization algorithm based on simulated annealing is proposed. Finally, the effectiveness and robustness of the method presented in this paper are verified via the simulation.展开更多
To the Editor:Malignant pleural effusion(MPE)is a collection of a large amount of exudativeuid in the pleural cavity that mainly originates from pleural metastases in patients with malignant tumors.The formation of MP...To the Editor:Malignant pleural effusion(MPE)is a collection of a large amount of exudativeuid in the pleural cavity that mainly originates from pleural metastases in patients with malignant tumors.The formation of MPE is related to angiogenesis,increased vascular permeability,lymphatic obstruction,immune reactions,and the tumor metastasis microenvironment,but molecular-based diagnostic and next-generation therapeutic strategies for MPE are still lacking.Exosomes are vesicles with a double-layered lipid membrane structure that are widely distributed in bodyuids and can be produced by almost all cells.Increased evidence has shown that exosomes are related to the development of MPE and are correlated with the efcacy of and response to targeted therapy or immunotherapy.Although exosomes are one of the main components of MPE,the source and functional role of exosomes in MPE are still unclear.展开更多
A facile approach has been adopted for coating cross-linked polystyrene(PS) shells on the surface of Fe304 magnetic clusters using reflux-precipitation polymerization(RPP).Treating the PS shell with chlorosulfonic aci...A facile approach has been adopted for coating cross-linked polystyrene(PS) shells on the surface of Fe304 magnetic clusters using reflux-precipitation polymerization(RPP).Treating the PS shell with chlorosulfonic acid yields magnetic composite particles with acid functionality.By adjusting the amount and proportion of monomers(styrene and divinylbenzene),the obtained magnetic composite particle solid acid(MPM-5 S) exhibits a saturation magnetization value of 18 emu/g,a specific surface area of 243 m^2/g and an acid density of 2.113 mmol/g.The MPM-5 S magnetic solid acid catalyst was evaluated for esterification of oleic acid with methanol to prepare biodiesel.Under mild conditions,the conversion of oleic acid reached 91%,which was much higher than the catalytic activity of Amberlyst-15 and close to the catalytic activity of concentrated H2 SO4.The solid acid catalyst can be recovered by magnetic separation and reused three times maintaining over 95% of its initial catalytic activity.Additionally,the solid acid can be used to catalyze the dehydration of fructose to 5-hydroxymethylfurfural.展开更多
Two-dimensional covalent organic frameworks(2D COFs)have sparkled wide-ranging research to explore proton-conducting materials.However,the powder-pressed pellets or continuous membranes of 2D COFs are composed of rand...Two-dimensional covalent organic frameworks(2D COFs)have sparkled wide-ranging research to explore proton-conducting materials.However,the powder-pressed pellets or continuous membranes of 2D COFs are composed of randomly arranged crystallites,which are undesirable for proton transport via a shortcut pathway.We report a controlled strategy for preparing a conformably oriented free-standing COF membrane to address the critical challenge.A monofunctional aldehyde precursor is used as a modulator to enhance reversible association and optimize growth orientation in an interfacial polymerization system.The preferred face-on alignment is achieved throughout the membrane from its flat side to the nanoflake-standing side and,in turn,generates the unidirectional pore channels for accommodating 1,2,4-triazole as proton carriers.The composite merges distinctive features including orientation,crystallinity,porosity,and mechanical strength into one system,exhibiting ultrafast and stable anhydrous proton conduction at high operating temperatures with low activation energy.Our findings offer an innovative strategy for the oriented crystallization of free-standing COF membranes for energy conversion applications.展开更多
Negative thermal expansion(NTE) behavior has roused wide interest for the control of thermomechanical properties of functional materials.Although NTE behaviors have been found in kinds of compounds,it remains challeng...Negative thermal expansion(NTE) behavior has roused wide interest for the control of thermomechanical properties of functional materials.Although NTE behaviors have been found in kinds of compounds,it remains challenging for polymers to achieve intrinsic NTE property.In this work,we systematically studied the conformational change of dibenzocyclooctadiene(DBCOD) derivatives between chair(C) and twist-boat(TB) forms based on density-functional theo ry(DFT) calculations,and found clear evidence of the relationship between the structure of DBCOD units and the thermal contraction behavior of the related polymers.In order to obtain the polymer with NTE property,two conditions should be met for the thermal contracting DBCOD related units as follows:(i) the TB conformation can turn into C conformation as the temperature increases,and(ii) the volume of C conformation is smaller than that of TB conformation.This rule should offer a guidance to exploration of the new intrinsic NTE polymers in the future.展开更多
This special column is dedicated to Professor Shou-Kuan Fu on the occasion of his 80thbirthday.Prof. Shou-Kuan Fu, born in July, 1940 in Jiangsu Province. He obtained his B.S. in Chemistry from Department of Chemistry...This special column is dedicated to Professor Shou-Kuan Fu on the occasion of his 80thbirthday.Prof. Shou-Kuan Fu, born in July, 1940 in Jiangsu Province. He obtained his B.S. in Chemistry from Department of Chemistry,Fudan University in 1962, then, he graduated from graduate school of Fudan University in 1966, under the supervision of Prof. TongYin Yu, a distinguished pioneer of polymer science in China and the founder of Department of Macromolecular Science at Fudan University.展开更多
Biocompatible magnetic nanoparticles were prepared by co-precipitation method in the presence of poly(aspartic acid)(PAsp)as stabilizer,which was one of the most extensively studied and used poly(amino acids).As a bio...Biocompatible magnetic nanoparticles were prepared by co-precipitation method in the presence of poly(aspartic acid)(PAsp)as stabilizer,which was one of the most extensively studied and used poly(amino acids).As a biocompatible dispersant,PAsp was successfully attached to the Fe_(3)O_(4) nanoparticles,which was approved by Fourier transform infrared spectroscopy(FTIR),transmission electron microscopy(TEM)and thermogravimetric analysis(TGA).From X-ray diffraction(XRD)and vibrating sample magnetometry(VSM)measurement results,it was found that PAsp stabilized iron oxide nanoparticles possess excellent Fe_(3)O_(4) crystal structure and superparamagnetic property.Compared with trisodium citrate stabilized magnetic nanoparticles,PAsp stabilized magnetic nanoparticles were biocompatible and with lower cytotoxicity,which makes it more applicable in medicine,biology and biomaterial science.展开更多
文摘Two-dimensional covalent organic frameworks(2D COFs)feature extendedπ-conjugation and ordered stacking sequence,showing great promise for high-performance photocatalysis.Periodic atomic frameworks of 2D COFs facilitate the in-plane photogenerated charge transfer,but the precise ordered alignment is limited due to the non-covalentπ-stacking of COF layers,accordingly hindering out-of-plane transfer kinetics.Herein,we address a chiral induction method to construct a parallelly superimposed stacking chiral COF ultrathin shell on the support of SiO_(2) microsphere.Compared to the achiral COF analogues,the chiral COF shell with the parallel AA-stacking structure is more conducive to enhance the built-in electric field and accumulates photogenerated electrons for the rapid migration,thereby affording superior photocatalytic performance in hydrogen evolution from water splitting.Taking the simplest ketoenamine-linked chiral COF as a shell of SiO_(2) particle,the resulting composite exhibits an impressive hydrogen evolution rate of 107.1 mmol g^(-1)h^(-1)along with the apparent quantum efficiency of 14.31% at 475 nm.Furthermore,the composite photocatalysts could be fabricated into a film device,displaying a remarkable photocatalytic performance of 178.0 mmol m^(-2)h^(-1)for hydrogen evolution.Our work underpins the surface engineering of organic photocatalysts and illustrates the significance of COF stacking structures in regulating electronic properties.
文摘The concentration of total nitrogen (TN), total phosphorus (TP) and organic material (OM) at sixty grid division in Lake Chaohu basin around the lake was studied, in order to investigate their spatial distribution characteristics. The results showed that the average concentrations of TN, TP and OM were 1027 mg/kg, 483 mg/kg, 1.95%, and their concentrations ranged from 253 mg/kg to 2273 mg/kg, 223 mg/kg to 1173 mg/kg and 0.291% to 5.48%, respectively. The high concentration areas were located at the basins of Tuogao river and Zhao river while the low concentration areas were located at basins of Pai river, Nanfei river and Dianpu river. The concentrations of TN and OM were higher in East part than in West part. The spatial distribution of TN, TP and OM concentrations of the surface soil showed inconsistent with those of the water quality of the inflow rivers and the lake and the TN and TP of lake sediment studied.
基金supported by the National Science Foundation for Young Scholars of China(6130123471401175)
文摘Multiple earth observing satellites need to communicate with each other to observe plenty of targets on the Earth together. The factors, such as external interference, result in satellite information interaction delays, which is unable to ensure the integrity and timeliness of the information on decision making for satellites. And the optimization of the planning result is affected. Therefore, the effect of communication delay is considered during the multi-satel ite coordinating process. For this problem, firstly, a distributed cooperative optimization problem for multiple satellites in the delayed communication environment is formulized. Secondly, based on both the analysis of the temporal sequence of tasks in a single satellite and the dynamically decoupled characteristics of the multi-satellite system, the environment information of multi-satellite distributed cooperative optimization is constructed on the basis of the directed acyclic graph(DAG). Then, both a cooperative optimization decision making framework and a model are built according to the decentralized partial observable Markov decision process(DEC-POMDP). After that, a satellite coordinating strategy aimed at different conditions of communication delay is mainly analyzed, and a unified processing strategy on communication delay is designed. An approximate cooperative optimization algorithm based on simulated annealing is proposed. Finally, the effectiveness and robustness of the method presented in this paper are verified via the simulation.
基金Key R&D Plan of Jiangxi Province(No.2021BBG71006)Zhejiang Provincial Basic Public Welfare Research Project(No.GF19H160028)Key project of Science and Technology Innovation of Health Commission of Jiangxi Province(Nos.2023ZD005 and 2024ZD008)
文摘To the Editor:Malignant pleural effusion(MPE)is a collection of a large amount of exudativeuid in the pleural cavity that mainly originates from pleural metastases in patients with malignant tumors.The formation of MPE is related to angiogenesis,increased vascular permeability,lymphatic obstruction,immune reactions,and the tumor metastasis microenvironment,but molecular-based diagnostic and next-generation therapeutic strategies for MPE are still lacking.Exosomes are vesicles with a double-layered lipid membrane structure that are widely distributed in bodyuids and can be produced by almost all cells.Increased evidence has shown that exosomes are related to the development of MPE and are correlated with the efcacy of and response to targeted therapy or immunotherapy.Although exosomes are one of the main components of MPE,the source and functional role of exosomes in MPE are still unclear.
基金financially supported by the National Natural Science Foundation of China(No.21802039)Hunan Provincial Natural Science Foundation of China(No.2019JJ40061)+3 种基金Scientific Research Fund of Hunan Provincial Education Department (No.18A422)the National College Students’ Innovation and Entrepreneurship Training Program Project,Hunan Province College Students’ Research Learning and Innovative Experiment Projectthe Acteristic Application Discipline of Material Science Engineering in Hunan Province(Hunan Provincial Education Department Notice(No.[2018]469)funding from Dow through the University Partnership Initiative
文摘A facile approach has been adopted for coating cross-linked polystyrene(PS) shells on the surface of Fe304 magnetic clusters using reflux-precipitation polymerization(RPP).Treating the PS shell with chlorosulfonic acid yields magnetic composite particles with acid functionality.By adjusting the amount and proportion of monomers(styrene and divinylbenzene),the obtained magnetic composite particle solid acid(MPM-5 S) exhibits a saturation magnetization value of 18 emu/g,a specific surface area of 243 m^2/g and an acid density of 2.113 mmol/g.The MPM-5 S magnetic solid acid catalyst was evaluated for esterification of oleic acid with methanol to prepare biodiesel.Under mild conditions,the conversion of oleic acid reached 91%,which was much higher than the catalytic activity of Amberlyst-15 and close to the catalytic activity of concentrated H2 SO4.The solid acid catalyst can be recovered by magnetic separation and reused three times maintaining over 95% of its initial catalytic activity.Additionally,the solid acid can be used to catalyze the dehydration of fructose to 5-hydroxymethylfurfural.
基金supported by the National Natural Science Foundation of China (51973039,52173197,52131308)
文摘Two-dimensional covalent organic frameworks(2D COFs)have sparkled wide-ranging research to explore proton-conducting materials.However,the powder-pressed pellets or continuous membranes of 2D COFs are composed of randomly arranged crystallites,which are undesirable for proton transport via a shortcut pathway.We report a controlled strategy for preparing a conformably oriented free-standing COF membrane to address the critical challenge.A monofunctional aldehyde precursor is used as a modulator to enhance reversible association and optimize growth orientation in an interfacial polymerization system.The preferred face-on alignment is achieved throughout the membrane from its flat side to the nanoflake-standing side and,in turn,generates the unidirectional pore channels for accommodating 1,2,4-triazole as proton carriers.The composite merges distinctive features including orientation,crystallinity,porosity,and mechanical strength into one system,exhibiting ultrafast and stable anhydrous proton conduction at high operating temperatures with low activation energy.Our findings offer an innovative strategy for the oriented crystallization of free-standing COF membranes for energy conversion applications.
基金supported by the National Natural Science Foundation of China (Nos.51633001,51721002 and 51873040)National Key R&D Program of China (No.2016YFC1100300)。
文摘Negative thermal expansion(NTE) behavior has roused wide interest for the control of thermomechanical properties of functional materials.Although NTE behaviors have been found in kinds of compounds,it remains challenging for polymers to achieve intrinsic NTE property.In this work,we systematically studied the conformational change of dibenzocyclooctadiene(DBCOD) derivatives between chair(C) and twist-boat(TB) forms based on density-functional theo ry(DFT) calculations,and found clear evidence of the relationship between the structure of DBCOD units and the thermal contraction behavior of the related polymers.In order to obtain the polymer with NTE property,two conditions should be met for the thermal contracting DBCOD related units as follows:(i) the TB conformation can turn into C conformation as the temperature increases,and(ii) the volume of C conformation is smaller than that of TB conformation.This rule should offer a guidance to exploration of the new intrinsic NTE polymers in the future.
文摘This special column is dedicated to Professor Shou-Kuan Fu on the occasion of his 80thbirthday.Prof. Shou-Kuan Fu, born in July, 1940 in Jiangsu Province. He obtained his B.S. in Chemistry from Department of Chemistry,Fudan University in 1962, then, he graduated from graduate school of Fudan University in 1966, under the supervision of Prof. TongYin Yu, a distinguished pioneer of polymer science in China and the founder of Department of Macromolecular Science at Fudan University.
基金This work was supported by the National Natural Science Foundation of China(Grant Nos.20974023,21034003 and 51073040)Shanghai Committee of Science and Technology,China(Grant No.10XD1400500).
文摘Biocompatible magnetic nanoparticles were prepared by co-precipitation method in the presence of poly(aspartic acid)(PAsp)as stabilizer,which was one of the most extensively studied and used poly(amino acids).As a biocompatible dispersant,PAsp was successfully attached to the Fe_(3)O_(4) nanoparticles,which was approved by Fourier transform infrared spectroscopy(FTIR),transmission electron microscopy(TEM)and thermogravimetric analysis(TGA).From X-ray diffraction(XRD)and vibrating sample magnetometry(VSM)measurement results,it was found that PAsp stabilized iron oxide nanoparticles possess excellent Fe_(3)O_(4) crystal structure and superparamagnetic property.Compared with trisodium citrate stabilized magnetic nanoparticles,PAsp stabilized magnetic nanoparticles were biocompatible and with lower cytotoxicity,which makes it more applicable in medicine,biology and biomaterial science.