The electrocatalytic oxidation of glycerol toward formic acid is one of the most promising pathways for transformation and utilization of glycerol.Herein,a series of well-defined Ni_(n)(SR)_(2n) nanoclusters(n=4,5,6;d...The electrocatalytic oxidation of glycerol toward formic acid is one of the most promising pathways for transformation and utilization of glycerol.Herein,a series of well-defined Ni_(n)(SR)_(2n) nanoclusters(n=4,5,6;denoted as Ni NCs)were prepared for the electrocatalytic glycerol oxidation toward formic acid,in which Ni_(6)-PET-50CV afforded the most excellent electrocatalytic performance with a high formic acid selectivity of 93% and a high glycerol conversion of 86%.This was attributed to the lowest charge transfer impedance and the most rapid reaction kinetics.Combined electrochemical measurements and X-ray absorption fine structure measurements revealed that the structures of Ni NCs remained intact after CV scanning pretreatment and electrocatalysis via forming the Ni–O bond.Additionally,the kinetic studies and in-situ Fourier transformed infrared suggested a sequential oxidation mechanism,in which the main reaction steps of glycerol→glyceraldehyde→glyceric acid were very rapid to produce a high selectivity of formic acid even though the low glycerol conversion.This work presents an opportunity to study Ni NCs for the efficient electrocatalytic oxidation of biomass-derived polyhydroxyl platform molecules to produce value-added carboxylic acids.展开更多
It is still a huge challenge for traditional Pareto-dominatedmany-objective optimization algorithms to solve manyobjective optimization problems because these algorithms hardly maintain the balance between convergence...It is still a huge challenge for traditional Pareto-dominatedmany-objective optimization algorithms to solve manyobjective optimization problems because these algorithms hardly maintain the balance between convergence and diversity and can only find a group of solutions focused on a small area on the Pareto front,resulting in poor performance of those algorithms.For this reason,we propose a reference vector-assisted algorithmwith an adaptive niche dominance relation,for short MaOEA-AR.The new dominance relation forms a niche based on the angle between candidate solutions.By comparing these solutions,the solutionwith the best convergence is found to be the non-dominated solution to improve the selection pressure.In reproduction,a mutation strategy of k-bit crossover and hybrid mutation is used to generate high-quality offspring.On 23 test problems with up to 15-objective,we compared the proposed algorithm with five state-of-the-art algorithms.The experimental results verified that the proposed algorithm is competitive.展开更多
Two structurally analogous self-assembled bowl-shaped hosts were obtained in close to quantitative yields via hydrazone condensation in acidic aqueous media,where the dynamic nature of hydrazone bonds was activated.Ea...Two structurally analogous self-assembled bowl-shaped hosts were obtained in close to quantitative yields via hydrazone condensation in acidic aqueous media,where the dynamic nature of hydrazone bonds was activated.Each bowl bears nine positive charges,endowing it with good water solubility.The bowls can thus take advantage of the hydrophobic effect and/or electrostatic forces to recognize neu-tral or anionic vips.Upon being accommodated within the host cavity,an anthracene derivative was protected from UV-stimulated oxidation.展开更多
Background: Many studies have emphasized that selective resection of epileptic lesions in temoral lobe is associated with better preservation of cognition function;whether this applies to patients with refractory mesi...Background: Many studies have emphasized that selective resection of epileptic lesions in temoral lobe is associated with better preservation of cognition function;whether this applies to patients with refractory mesial temporal lobe epilepsy (MTLE) remains unknown. The objective of this study was to evaluate changes in cognitive functions, mood status, and quality of life after anterior temporal lobectomy in patients with refractory MTLE. Methods: This single-arm cohort study assessed cognitive function, mood status, and quality of life, as well as electroencephalography findings, in patients with refractory MTLE who underwent anterior temporal lobectomy at Xuanwu Hospital from January 2018 to March 2019. Pre- and post-operative characteristics were compared to evaluate the effects of surgery. Results: Anterior temporal lobectomy significantly reduced the frequencies of epileptiform discharges. The overall success rate of surgery was acceptable. Anterior temporal lobectomy did not result in significant changes in overall cognitive functions (P > 0.05), although changes in certain domains, including visuospatial ability, executive ability, and abstract thinking, were detected. Anterior temporal lobectomy resulted in improvements in anxiety and depression symptoms and quality of life. Conclusions: Anterior temporal lobectomy reduced epileptiform discharges and incidence of post-operative seizures as well as resulted in improved mood status and quality of life without causing significant changes in cognitive function.展开更多
Atomically precise water-soluble gold nanoclusters(Au NCs)protected by organic ligands have attracted growing attention in serving as unique nanomaterials with the potential to generate theranostic tools(bioimaging,bi...Atomically precise water-soluble gold nanoclusters(Au NCs)protected by organic ligands have attracted growing attention in serving as unique nanomaterials with the potential to generate theranostic tools(bioimaging,biosensing,and biotherapy),due to their ultrasmall size,superior photoluminescence,good biocompatibility,and nontoxicity.More importantly,Au NCs afford a well-defined atomic packing structure and molecular purity,providing a superior platform to unravel the structure−performance correlations for biodistribution,biological pharmacokinetics,and excretion of Au NCs.In this Review,we mainly survey the synthesis of water-soluble Au NCs and the recent progress in biomedicine of Au NCs,including bioimaging,biosensing,and biotherapy.The effects of ligand and size on the biomedical properties are discussed in detail.We hope that the advances in this research area can expand the applications of Au NCs in biomedicine.展开更多
Ligand engineering for well-defined gold nanoclusters(Au NCs) is getting more extensive attention. Organizing the Au-ligand interfaces on gold NCs can achieve the structural and functional control. This review focuses...Ligand engineering for well-defined gold nanoclusters(Au NCs) is getting more extensive attention. Organizing the Au-ligand interfaces on gold NCs can achieve the structural and functional control. This review focuses on the Au-ligand interfaces including gold-phosphorus(Au-P), gold-sulfur(Au-S), gold-selenium(Au-Se), gold-carbon(Au-C), and gold-nitrogen(Au-N), derived from the bonding between Au atoms and the different ligands(e.g., organic phosphine, thiolate, selenolate, alkynyl,n-heterocyclic carbene and nitrogenous ligands). The formation mechanism of Au-ligand interfaces is well discussed. In addition, the effects of Au-ligand interfaces on the stability, optical property, and catalysis are also presented. We hope the advances in this research area can boost the development of Au NC sciences.展开更多
文摘The electrocatalytic oxidation of glycerol toward formic acid is one of the most promising pathways for transformation and utilization of glycerol.Herein,a series of well-defined Ni_(n)(SR)_(2n) nanoclusters(n=4,5,6;denoted as Ni NCs)were prepared for the electrocatalytic glycerol oxidation toward formic acid,in which Ni_(6)-PET-50CV afforded the most excellent electrocatalytic performance with a high formic acid selectivity of 93% and a high glycerol conversion of 86%.This was attributed to the lowest charge transfer impedance and the most rapid reaction kinetics.Combined electrochemical measurements and X-ray absorption fine structure measurements revealed that the structures of Ni NCs remained intact after CV scanning pretreatment and electrocatalysis via forming the Ni–O bond.Additionally,the kinetic studies and in-situ Fourier transformed infrared suggested a sequential oxidation mechanism,in which the main reaction steps of glycerol→glyceraldehyde→glyceric acid were very rapid to produce a high selectivity of formic acid even though the low glycerol conversion.This work presents an opportunity to study Ni NCs for the efficient electrocatalytic oxidation of biomass-derived polyhydroxyl platform molecules to produce value-added carboxylic acids.
基金supported by the National Natural Science Foundation of China(Grant No.61976101)the University Natural Science Research Project of Anhui Province(Grant No.2023AH040056)+4 种基金the Natural Science Research Project of Anhui Province(Graduate Research Project,Grant No.YJS20210463)the Funding Plan for Scientic Research Activities of Academic and Technical Leaders and Reserve Candidates in Anhui Province(Grant No.2021H264)the Top Talent Project of Disciplines(Majors)in Colleges and Universities in Anhui Province(Grant No.gxbjZD2022021)the University Synergy Innovation Program of Anhui Province,China(GXXT-2022-033)supported by the Innovation Fund for Postgraduates of Huaibei Normal University(Grant Nos.cx2022041,yx2021023,CX2023043).
文摘It is still a huge challenge for traditional Pareto-dominatedmany-objective optimization algorithms to solve manyobjective optimization problems because these algorithms hardly maintain the balance between convergence and diversity and can only find a group of solutions focused on a small area on the Pareto front,resulting in poor performance of those algorithms.For this reason,we propose a reference vector-assisted algorithmwith an adaptive niche dominance relation,for short MaOEA-AR.The new dominance relation forms a niche based on the angle between candidate solutions.By comparing these solutions,the solutionwith the best convergence is found to be the non-dominated solution to improve the selection pressure.In reproduction,a mutation strategy of k-bit crossover and hybrid mutation is used to generate high-quality offspring.On 23 test problems with up to 15-objective,we compared the proposed algorithm with five state-of-the-art algorithms.The experimental results verified that the proposed algorithm is competitive.
基金supported by the Starry Night Science Fund of Zhejiang University,Shanghai Institute for Advanced Study(grant no.SN-ZJU-SIAS-006)support from the Leading Innovation Team grant from the Department of Science and Technology of Zhejiang Province(grant no.2022R01005)+1 种基金the Natural Science Foundation of Zhejiang Province(grant no.LZ24B020002)the National Natural Science Foundation of China(grant nos.22273082 and 22250610196).
文摘Two structurally analogous self-assembled bowl-shaped hosts were obtained in close to quantitative yields via hydrazone condensation in acidic aqueous media,where the dynamic nature of hydrazone bonds was activated.Each bowl bears nine positive charges,endowing it with good water solubility.The bowls can thus take advantage of the hydrophobic effect and/or electrostatic forces to recognize neu-tral or anionic vips.Upon being accommodated within the host cavity,an anthracene derivative was protected from UV-stimulated oxidation.
文摘Background: Many studies have emphasized that selective resection of epileptic lesions in temoral lobe is associated with better preservation of cognition function;whether this applies to patients with refractory mesial temporal lobe epilepsy (MTLE) remains unknown. The objective of this study was to evaluate changes in cognitive functions, mood status, and quality of life after anterior temporal lobectomy in patients with refractory MTLE. Methods: This single-arm cohort study assessed cognitive function, mood status, and quality of life, as well as electroencephalography findings, in patients with refractory MTLE who underwent anterior temporal lobectomy at Xuanwu Hospital from January 2018 to March 2019. Pre- and post-operative characteristics were compared to evaluate the effects of surgery. Results: Anterior temporal lobectomy significantly reduced the frequencies of epileptiform discharges. The overall success rate of surgery was acceptable. Anterior temporal lobectomy did not result in significant changes in overall cognitive functions (P > 0.05), although changes in certain domains, including visuospatial ability, executive ability, and abstract thinking, were detected. Anterior temporal lobectomy resulted in improvements in anxiety and depression symptoms and quality of life. Conclusions: Anterior temporal lobectomy reduced epileptiform discharges and incidence of post-operative seizures as well as resulted in improved mood status and quality of life without causing significant changes in cognitive function.
基金financial support from the Foundation of the Jiangsu Higher Education Institutions of China(22KJB150026)the National Natural Science Foundation of China(22178161,22101128).
文摘Atomically precise water-soluble gold nanoclusters(Au NCs)protected by organic ligands have attracted growing attention in serving as unique nanomaterials with the potential to generate theranostic tools(bioimaging,biosensing,and biotherapy),due to their ultrasmall size,superior photoluminescence,good biocompatibility,and nontoxicity.More importantly,Au NCs afford a well-defined atomic packing structure and molecular purity,providing a superior platform to unravel the structure−performance correlations for biodistribution,biological pharmacokinetics,and excretion of Au NCs.In this Review,we mainly survey the synthesis of water-soluble Au NCs and the recent progress in biomedicine of Au NCs,including bioimaging,biosensing,and biotherapy.The effects of ligand and size on the biomedical properties are discussed in detail.We hope that the advances in this research area can expand the applications of Au NCs in biomedicine.
基金supported by the Jiangsu Natural Science Foundation of China(BK20230329)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(22KJB150026)+1 种基金the Foundation of the National Natural Science Foundation of China(21802070 and 2217816)the National Key R&D Program of China(2018YFE0122600)。
文摘Ligand engineering for well-defined gold nanoclusters(Au NCs) is getting more extensive attention. Organizing the Au-ligand interfaces on gold NCs can achieve the structural and functional control. This review focuses on the Au-ligand interfaces including gold-phosphorus(Au-P), gold-sulfur(Au-S), gold-selenium(Au-Se), gold-carbon(Au-C), and gold-nitrogen(Au-N), derived from the bonding between Au atoms and the different ligands(e.g., organic phosphine, thiolate, selenolate, alkynyl,n-heterocyclic carbene and nitrogenous ligands). The formation mechanism of Au-ligand interfaces is well discussed. In addition, the effects of Au-ligand interfaces on the stability, optical property, and catalysis are also presented. We hope the advances in this research area can boost the development of Au NC sciences.
