Photocatalytic hydrogen(H_(2))evolution using covalent organic frameworks(COFs)is an attractive and promising avenue for exploration,but one of its big challenges is low photo-induced charge separation.In this study,w...Photocatalytic hydrogen(H_(2))evolution using covalent organic frameworks(COFs)is an attractive and promising avenue for exploration,but one of its big challenges is low photo-induced charge separation.In this study,we present a straightforward and facile dipole polarization engineering strategy to enhance charge separation efficiency,achieved through atomic modulation(O,S,and Se)of the COF monomer.Our findings demonstrate that incorporating atoms with varying electronegativities into the COF matrix significantly influences the local dipole moment,thereby affecting charge separation efficiency and photostability,which in turn affects the rates of photocatalytic H_(2) evolution.As a result,the newly developed TMT-BO-COF,which contains highly electronegative O atoms,exhibits the lowest exciton binding energy,the highest efficiency in charge separation and transportation,and the longest lifetime of the active charges.This leads to an impressive average H_(2) production rate of 23.7 mmol g^(−1) h^(−1),which is 2.5 and 24.5 times higher than that of TMT-BS-COF(containing S atoms)and TMT-BSe-COF(containing Se atoms),respectively.A novel photocatalytic hydrogen evolution mechanism based on proton-coupled electron transfer on N in the structure of triazine rings in vinylene-linked COFs is proposed by theoretical calculations.Our findings provide new insights into the design of highly photoactive organic framework materials for H_(2) evolution and beyond.展开更多
A major challenge is to construct ceramic membranes with tunable structures and functions for water treatment.Herein,a novel corrosion-resistant polymer-derived silicon oxycarbide(SiOC)ceramic membrane with designed a...A major challenge is to construct ceramic membranes with tunable structures and functions for water treatment.Herein,a novel corrosion-resistant polymer-derived silicon oxycarbide(SiOC)ceramic membrane with designed architectures was fabricated by a phase separation method and was applied in organic removal via adsorption and oxidation for the first time.The pore structure of the as-prepared SiOC ceramic membranes was well controlled by changing the sintering temperature and polydimethylsiloxane content,leading to a pore size of 0.84–1.62μm and porosity of 25.0–43.8%.Corrosion resistance test results showed that the SiOC membranes sustained minimal damage during 24 h exposure to high-intensity acid–base conditions,which could be attributed to the chemical inertness of SiOC.With rhodamine 6G(R6G)as the model pollutant,the SiOC membrane demonstrated an initial eff ective removal rate of 99%via adsorption;however,the removal rate decreased as the system approached adsorption saturation.When peroxymonosulfate was added into the system,efficient and continuous degradation of R6G was observed throughout the entire period,indicating the potential of the as-prepared SiOC membrane in oxidation-related processes.Thus,this work provides new insights into the construction of novel polymer-derived ceramic membranes with well-defined structures and functions.展开更多
Background:Acute ankle injury causes damage to joint mechanoreceptors and deafferentation and contributes to proprioception deficits in patients with chronic ankle instability(CAI).We aimed to explore whether deficits...Background:Acute ankle injury causes damage to joint mechanoreceptors and deafferentation and contributes to proprioception deficits in patients with chronic ankle instability(CAI).We aimed to explore whether deficits of proprioception,including kinesthesia and joint position sense(JPS),exist in patients with CAI when compared with the uninjured contralateral side and healthy people.We hypothesized that proprioception deficits did exist in patients with CAI and that the deficits varied by test methodologies.Methods:The study was a systematic review and meta-analysis.We identified studies that compared kinesthesia or JPS in patients with CAI with the uninjured contralateral side or with healthy controls.Meta-analyses were conducted for the studies with similar test procedures,and narrative syntheses were undertaken for the rest.Results:A total of 7731 studies were identified,of which 30 were included for review.A total of 21 studies were eligible for meta-analysis.Compared with the contralateral side,patients with CAI had ankle kinesthesia deficits in inversion and plantarflexion,with a standardized mean difference(SMD)of 0.41 and 0.92,respectively,and active and passive JPS deficits in inversion(SMD=0.92 and 0.72,respectively).Compared with healthy people,patients with CAI had ankle kinesthesia deficits in inversion and eversion(SMD=0.64 and 0.76,respectively),and active JPS deficits in inversion and eversion(SMD=1.00 and 4.82,respectively).Proprioception deficits in the knee and shoulder of patients with CAI were not statistically significant.Conclusion:Proprioception,including both kinesthesia and JPS,of the injured ankle of patients with CAI was impaired,compared with the uninjured contralateral limbs and healthy people.Proprioception varied depending on different movement directions and test methodologies.The use of more detailed measurements of proprioception and interventions for restoring the deficits are recommended in the clinical management of CAI.展开更多
Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellentconductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we ...Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellentconductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we reported a novel well-designed hierarchically porous nitrogen-doped carbon (HPNC) via acombination of salt template (ZnC12) and hard template (SiO2) as sulfur host for lithium-sulfur batter-ies. The low-melting ZnC12 is boiled off and leaves behind micropores and small size mesopores duringpyrolysis process, while the silica spheres are removed by acid leaching to generate interconnected 3Dnetwork of macropores. The HPNC-S electrode exhibits an initial specific capacity of 1355 mAh g^-l at 0.IC (IC= 1675 mAh g^-1 ), a high-rate capability of 623 mAh g-l at 2 C, and a small decay of 0.13% per cycleover 300 cycles at 0.2 C. This excellent rate capability and remarkable long-term cyclability of the HPNC-Selectrode are attributed to its hierarchical porous structures for confining the soluble lithium polysulfideas well as the nitrogen doping for high absorbability of lithium polysulfide.展开更多
The development of surface modification technology for temperature sensitive fibers has been a huge challenge.In this work,a novel technique based on cold plasma treatment was developed for the preparation of anti-bac...The development of surface modification technology for temperature sensitive fibers has been a huge challenge.In this work,a novel technique based on cold plasma treatment was developed for the preparation of anti-bacterial polypropylene(PP)fibers.The results showed that plasma treatment introduced a rough surface and polar groups,which acted as the anchor point and initiators for diallyldimethyl ammonium chloride(DADMAC)graft-polymerization.The fabricated PP membranes presented a high bacterial sterilization rate,as well as excellent adhesion force and washing durability.After ultrasonic treatment for 30 min,the physical coating sample had lost anti-bacterial effect,while the plasma grafted sample still showed a sterilization rate of 91.67%.This work provided a clean and novel DADMAC grafting method and it is also applicable for anti-bacterial material fabrication.展开更多
Surfactants were used to assist in the crystallization of lysozyme.Three types of surfactants with different structures(sodium dodecyl sulfate,cetyltrimethylammonium bromide,or betaine hydrochloride[BH])were used.The ...Surfactants were used to assist in the crystallization of lysozyme.Three types of surfactants with different structures(sodium dodecyl sulfate,cetyltrimethylammonium bromide,or betaine hydrochloride[BH])were used.The study indicated that three surfactants were all capable of shortening the crystallization induction time of lysozyme,with BH inducing the shortest crystallization induction time(t=1 min)and the largest crystal size(37μm).The molecular interactions among each of the three surfactants aforementioned and lysozyme were also investigated by simulations.It was found that hydrogen bonding dominantly acted between the carboxyl structure of the surfactant BH and the lysozyme,which produced the most favorable conformation for the self-assembly of lysozyme(promote lysozyme orderly aggregation and shorten the crystallization induction time).On this basis,the mechanism of surfactant-promoted lysozyme crystallization was proposed.展开更多
文摘Photocatalytic hydrogen(H_(2))evolution using covalent organic frameworks(COFs)is an attractive and promising avenue for exploration,but one of its big challenges is low photo-induced charge separation.In this study,we present a straightforward and facile dipole polarization engineering strategy to enhance charge separation efficiency,achieved through atomic modulation(O,S,and Se)of the COF monomer.Our findings demonstrate that incorporating atoms with varying electronegativities into the COF matrix significantly influences the local dipole moment,thereby affecting charge separation efficiency and photostability,which in turn affects the rates of photocatalytic H_(2) evolution.As a result,the newly developed TMT-BO-COF,which contains highly electronegative O atoms,exhibits the lowest exciton binding energy,the highest efficiency in charge separation and transportation,and the longest lifetime of the active charges.This leads to an impressive average H_(2) production rate of 23.7 mmol g^(−1) h^(−1),which is 2.5 and 24.5 times higher than that of TMT-BS-COF(containing S atoms)and TMT-BSe-COF(containing Se atoms),respectively.A novel photocatalytic hydrogen evolution mechanism based on proton-coupled electron transfer on N in the structure of triazine rings in vinylene-linked COFs is proposed by theoretical calculations.Our findings provide new insights into the design of highly photoactive organic framework materials for H_(2) evolution and beyond.
基金supported by the National Key R&D Program of China(Grant No.2021YFB3200500)Natural Science Foundation of China(Grant No.52370014)+2 种基金Ningbo 3315 plan(Grant No.2018A-03-A)Natural Science Foundation of Tianjin City(Grant No.63241631)the financial support of Joint Lab for Advanced Organosilicon Precursors with Zhejiang Xinshichen New Materials Ltd.Co.
文摘A major challenge is to construct ceramic membranes with tunable structures and functions for water treatment.Herein,a novel corrosion-resistant polymer-derived silicon oxycarbide(SiOC)ceramic membrane with designed architectures was fabricated by a phase separation method and was applied in organic removal via adsorption and oxidation for the first time.The pore structure of the as-prepared SiOC ceramic membranes was well controlled by changing the sintering temperature and polydimethylsiloxane content,leading to a pore size of 0.84–1.62μm and porosity of 25.0–43.8%.Corrosion resistance test results showed that the SiOC membranes sustained minimal damage during 24 h exposure to high-intensity acid–base conditions,which could be attributed to the chemical inertness of SiOC.With rhodamine 6G(R6G)as the model pollutant,the SiOC membrane demonstrated an initial eff ective removal rate of 99%via adsorption;however,the removal rate decreased as the system approached adsorption saturation.When peroxymonosulfate was added into the system,efficient and continuous degradation of R6G was observed throughout the entire period,indicating the potential of the as-prepared SiOC membrane in oxidation-related processes.Thus,this work provides new insights into the construction of novel polymer-derived ceramic membranes with well-defined structures and functions.
基金the National Natural Science Foundation of China(Grant No.81871823).
文摘Background:Acute ankle injury causes damage to joint mechanoreceptors and deafferentation and contributes to proprioception deficits in patients with chronic ankle instability(CAI).We aimed to explore whether deficits of proprioception,including kinesthesia and joint position sense(JPS),exist in patients with CAI when compared with the uninjured contralateral side and healthy people.We hypothesized that proprioception deficits did exist in patients with CAI and that the deficits varied by test methodologies.Methods:The study was a systematic review and meta-analysis.We identified studies that compared kinesthesia or JPS in patients with CAI with the uninjured contralateral side or with healthy controls.Meta-analyses were conducted for the studies with similar test procedures,and narrative syntheses were undertaken for the rest.Results:A total of 7731 studies were identified,of which 30 were included for review.A total of 21 studies were eligible for meta-analysis.Compared with the contralateral side,patients with CAI had ankle kinesthesia deficits in inversion and plantarflexion,with a standardized mean difference(SMD)of 0.41 and 0.92,respectively,and active and passive JPS deficits in inversion(SMD=0.92 and 0.72,respectively).Compared with healthy people,patients with CAI had ankle kinesthesia deficits in inversion and eversion(SMD=0.64 and 0.76,respectively),and active JPS deficits in inversion and eversion(SMD=1.00 and 4.82,respectively).Proprioception deficits in the knee and shoulder of patients with CAI were not statistically significant.Conclusion:Proprioception,including both kinesthesia and JPS,of the injured ankle of patients with CAI was impaired,compared with the uninjured contralateral limbs and healthy people.Proprioception varied depending on different movement directions and test methodologies.The use of more detailed measurements of proprioception and interventions for restoring the deficits are recommended in the clinical management of CAI.
基金financially supported by the National Key Research and Development Program of China (2016YFB0101202)the NSFC of China (Grants 91534205,21436003 and 21576031)Graduate Research and Innovation Foundation of Chongqing China (Grant No.CYB17021)
文摘Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellentconductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we reported a novel well-designed hierarchically porous nitrogen-doped carbon (HPNC) via acombination of salt template (ZnC12) and hard template (SiO2) as sulfur host for lithium-sulfur batter-ies. The low-melting ZnC12 is boiled off and leaves behind micropores and small size mesopores duringpyrolysis process, while the silica spheres are removed by acid leaching to generate interconnected 3Dnetwork of macropores. The HPNC-S electrode exhibits an initial specific capacity of 1355 mAh g^-l at 0.IC (IC= 1675 mAh g^-1 ), a high-rate capability of 623 mAh g-l at 2 C, and a small decay of 0.13% per cycleover 300 cycles at 0.2 C. This excellent rate capability and remarkable long-term cyclability of the HPNC-Selectrode are attributed to its hierarchical porous structures for confining the soluble lithium polysulfideas well as the nitrogen doping for high absorbability of lithium polysulfide.
基金supported by National Natural Science Foundation of China(Nos.51877205 and 52011530191)Fundamental Research Funds for the Central Universities(No.buctrc201906)Beijing Nova Program(No.2022015)。
文摘The development of surface modification technology for temperature sensitive fibers has been a huge challenge.In this work,a novel technique based on cold plasma treatment was developed for the preparation of anti-bacterial polypropylene(PP)fibers.The results showed that plasma treatment introduced a rough surface and polar groups,which acted as the anchor point and initiators for diallyldimethyl ammonium chloride(DADMAC)graft-polymerization.The fabricated PP membranes presented a high bacterial sterilization rate,as well as excellent adhesion force and washing durability.After ultrasonic treatment for 30 min,the physical coating sample had lost anti-bacterial effect,while the plasma grafted sample still showed a sterilization rate of 91.67%.This work provided a clean and novel DADMAC grafting method and it is also applicable for anti-bacterial material fabrication.
基金National Natural Science Foundation of China(grant No.21878067).
文摘Surfactants were used to assist in the crystallization of lysozyme.Three types of surfactants with different structures(sodium dodecyl sulfate,cetyltrimethylammonium bromide,or betaine hydrochloride[BH])were used.The study indicated that three surfactants were all capable of shortening the crystallization induction time of lysozyme,with BH inducing the shortest crystallization induction time(t=1 min)and the largest crystal size(37μm).The molecular interactions among each of the three surfactants aforementioned and lysozyme were also investigated by simulations.It was found that hydrogen bonding dominantly acted between the carboxyl structure of the surfactant BH and the lysozyme,which produced the most favorable conformation for the self-assembly of lysozyme(promote lysozyme orderly aggregation and shorten the crystallization induction time).On this basis,the mechanism of surfactant-promoted lysozyme crystallization was proposed.