Accurate and efficient integration of the equations of motion is indispensable for molecular dynamics(MD)simulations.Despite the massive use of the conventional leapfrog(LF)integrator in modern computational tools wit...Accurate and efficient integration of the equations of motion is indispensable for molecular dynamics(MD)simulations.Despite the massive use of the conventional leapfrog(LF)integrator in modern computational tools within the framework of MD propagation,further development for better performance is still possible.The alternative version of LF in the middle thermostat scheme(LFmiddle)achieves a higher order of accuracy and efficiency and maintains stable dynamics even with the integration time stepsize extended by several folds.In this work,we perform a benchmark test of the two integrators(LF and LF-middle)in extensive conventional and enhanced sampling simulations,aiming at quantifying the time-stepsizeinduced variations of global properties(e.g.,detailed potential energy terms)as well as of local observables(e.g.,free energy changes or bondlengths)in practical simulations of complex systems.The test set is composed of six chemically and biologically relevant systems,including the conformational change of dihedral flipping in the N-methylacetamide and an AT(AdenineThymine)tract,the intra-molecular proton transfer inside malonaldehyde,the binding free energy calculations of benzene and phenol targeting T4 lysozyme L99A,the hydroxyl bond variations in ethaline deep eutectic solvent,and the potential energy of the blue-light using flavin photoreceptor.It is observed that the time-step-induced error is smaller for the LFmiddle scheme.The outperformance of LF-middle over the conventional LF integrator is much more significant for global properties than local observables.Overall,the current work demonstrates that the LF-middle scheme should be preferably applied to obtain accurate thermodynamics in the simulation of practical chemical and biological systems.展开更多
Many electrochemical energy storage devices,such as batteries,supercapacitors,and metal ion capacitors,rely on effective and inexpensive electrode materials.Herein,we have developed highly active nitrogen-doped porous...Many electrochemical energy storage devices,such as batteries,supercapacitors,and metal ion capacitors,rely on effective and inexpensive electrode materials.Herein,we have developed highly active nitrogen-doped porous carbon nanofoams(NPCNs-600-N)for sodium-ion capacitors(SICs).NPCNs-600-N have a highly porous framework,extended interlayer spacing(0.41 nm),and lots of surface functional groups.Accordingly,NPCNs-600-N achieves a high reversible capacity(301 mAh·g^(-1)at 0.05 A·g^(-1)),superior rate capability(112 mAh·g^(-1)at 5.00 A·g^(-1)),and ultra-stable cyclability.The excellent rate and cycling performance originate from the abundant active sites and porous architecture of NPCNs-600-N.Further-more,SICs device is constructed by employing the NPCNs-600-N as the battery-like anode and commercial superconductive carbon black as the capacitive cathode,which delivers high energy/power densities of 92 Wh·kg^(-1)/15984 W·kg^(-1)with a remarkable cyclability(93%reten-tion over 5000 cycles at 1.00 A·g^(-1)).The methodology of the work enables the simultaneous tuning of the porous architectures and surface function groups of carbon for high-performance SICs.展开更多
We produced Wood-Polymer Composites (WPCs) with phenolic resin (PR) filled with saw dust (SD) and rice husks (RH) in a PR:fillerratio of 60:40 wt.%. RH and SD were grinded and sieved into particles μm. The aim of thi...We produced Wood-Polymer Composites (WPCs) with phenolic resin (PR) filled with saw dust (SD) and rice husks (RH) in a PR:fillerratio of 60:40 wt.%. RH and SD were grinded and sieved into particles μm. The aim of this research work was to evaluate sawdust and rice husks as fillers for sustainable phenolic resin based WPCs. Therefore, we investigated the thermal stability of PR/RH and PR/SD WPCs then we studied and compared the tensile, flexural properties of PR/SD and PR/RH WPCs samples, as well as their dimensional stability after water absorption test. Furthermore, through ultraviolet light exposure, we evaluated the effects of photo-oxidation on the water stability and mechanical properties of PR/RH and PR/SD WPCs samples compared to unexposed ones. PR filled with SD presented better mechanical properties compared to PR/RH WPCs samples. However, PR/RH WPCs showed good mechanical properties, and better thermal resistance and better water repulsion capabilities compared to PR/SD WPCs samples. Although, long time UV exposure ended up lowering considerably the mechanical properties and water resistance of PR/SD and PR/RH WPCs, both RH and SD offer great added value as fillers for PR based WPCs;SD having better interactions with PR matrix compared to RH.展开更多
It is with great sadness for us that Professor Wei Jiang, a young and well-known supramolecular chemist, passed away on Sunday25 December 2022. He created a series of supramolecular hosts including Oxatubarenes [1] an...It is with great sadness for us that Professor Wei Jiang, a young and well-known supramolecular chemist, passed away on Sunday25 December 2022. He created a series of supramolecular hosts including Oxatubarenes [1] and Naphthotubes [2] with inner functionalized groups [3–6] and applied them into materials, catalysis,molecular machines and drug recognition and delivery fields [7–10] during his independent research career.展开更多
The recognition function based on host-vip chemistry of molecular cages represents one of the primary origins of supramolecular chemistry.The utilization of host-vip interactions allows the artificially designed s...The recognition function based on host-vip chemistry of molecular cages represents one of the primary origins of supramolecular chemistry.The utilization of host-vip interactions allows the artificially designed supramolecular hosts for a wide range of applications in binding recognition,drug delivery,molecular separation,confined catalysis,etc[1-3].展开更多
Sequence-activated chemiluminescence(CL)technique offers a unique approach to detecting specific biomolecules or cellular events with high sensitivity and spatial resolution.The fundamental principle behind sequence-a...Sequence-activated chemiluminescence(CL)technique offers a unique approach to detecting specific biomolecules or cellular events with high sensitivity and spatial resolution.The fundamental principle behind sequence-activated CL probes involves tailoring highly-controllable CL signals in response to specific sequences or events of interest,thus enabling high-contrast signals under complex physiological conditions.This sequential activation could be triggered by enzymes,reactive oxygen species(ROS),biothiols or changes in the microenvironment.These unique sequence-activated CL probes bestow several advantages,including minimal background,deep-tissue penetration,and the ability of non-invasive or minimally invasive detection.The sequence-activated CL techniques represent a significant advancement in molecular imaging and diagnostics.In this mini-review,we focus on the latest developments in sequential CL probes,addressing the technical challenges and discussing the future trajectory by harnessing CL signaling and molecular recognition.展开更多
Electroluminescence of f-f transition lanthanide complex is a traditional topic for display over decades.Here we report highly efficient organic light-emitting diodes based on a new terbium(III)complex with novel liga...Electroluminescence of f-f transition lanthanide complex is a traditional topic for display over decades.Here we report highly efficient organic light-emitting diodes based on a new terbium(III)complex with novel ligand CPMIP(1-(4-cyanophenyl)-3-methyl-4-isobutyryl-pyrazoline-5-one).The high triplet energy level of CPMIP(3.0 e V)and inhibited quenching effects in the solid-state lead to a nearly 100%photoluminescent quantum efficiency of Tb(CPMIP)3.The best Tb(CPMIP)3 device exhibited maximum external quantum efficiency up to 19.7%,setting a new record of OLEDs based on f-f transition lanthanide complexes.展开更多
Precise and early detection ofβ-amyloid(Aβ)deposits in situ and in real time is pivotal to the diagnosis and early intervention of Alzheimer’s disease(AD).Optical imaging stands out to be a promising technique for ...Precise and early detection ofβ-amyloid(Aβ)deposits in situ and in real time is pivotal to the diagnosis and early intervention of Alzheimer’s disease(AD).Optical imaging stands out to be a promising technique for such a task;however,it still remains a big challenge,due to the lack of high-performance imaging contrast agent.Restricted by poor blood-brain barrier(BBB)penetrability,short-wavelength excitation and emission,as well as the aggregation-caused quenching effect,the widely used goldstandard probes cannot be used for early in-vivo imaging of Aβdeposits.Herein,we integrate the Aβdeposits-favored geometry,amphiphilic and zwitterionic molecular structure,extended D-π-A electronic structure,and 3 D conformation into one molecule,facilely establishing a simple and economic imaging contrast agent that enjoys high specificity and affinity to Aβdeposits,good BBB penetrability,bright red/near-infrared fluorescence,low interference from autofluorescence,aggregation-induced emission(AIE)feature,high signal-to-noise ratio(SNR),and high contrast.In-vitro,ex-vivo,and in-vivo experiments with different strains of mice indicate that AIE-CNPy-AD holds the universality to Aβdeposits identification.Noteworthily,AIE-CNPy-AD is even able to precisely trace the small and sparsely-distributed Aβdeposits in AD model mice as young as 4-month-old APP/PS1 mice,the youngest having Aβdeposits.Moreover,the present probe could clearly reveal the increase and enlargement of Aβdeposits as the mice grow.Therefore,AIE-CNPy-AD might be an ideal alternative for early AD diagnosis and highly reliable monitoring of AD progression.展开更多
基金supported by the National Natural Science Foundation of China(No.21961142017)the Ministry of Science and Technology of China(No.2017YFA0204901)。
文摘Accurate and efficient integration of the equations of motion is indispensable for molecular dynamics(MD)simulations.Despite the massive use of the conventional leapfrog(LF)integrator in modern computational tools within the framework of MD propagation,further development for better performance is still possible.The alternative version of LF in the middle thermostat scheme(LFmiddle)achieves a higher order of accuracy and efficiency and maintains stable dynamics even with the integration time stepsize extended by several folds.In this work,we perform a benchmark test of the two integrators(LF and LF-middle)in extensive conventional and enhanced sampling simulations,aiming at quantifying the time-stepsizeinduced variations of global properties(e.g.,detailed potential energy terms)as well as of local observables(e.g.,free energy changes or bondlengths)in practical simulations of complex systems.The test set is composed of six chemically and biologically relevant systems,including the conformational change of dihedral flipping in the N-methylacetamide and an AT(AdenineThymine)tract,the intra-molecular proton transfer inside malonaldehyde,the binding free energy calculations of benzene and phenol targeting T4 lysozyme L99A,the hydroxyl bond variations in ethaline deep eutectic solvent,and the potential energy of the blue-light using flavin photoreceptor.It is observed that the time-step-induced error is smaller for the LFmiddle scheme.The outperformance of LF-middle over the conventional LF integrator is much more significant for global properties than local observables.Overall,the current work demonstrates that the LF-middle scheme should be preferably applied to obtain accurate thermodynamics in the simulation of practical chemical and biological systems.
基金financially supported by the Natural Science Foundation of Jiangsu Province (No. BK20170549)the National Natural Science Foundation of China (Nos. 21706103 and 22075109)+2 种基金Nanjing Tech University Research Start-Up Fund (No. 38274017111)Zhongyan Jilantai Chlor-Alkali Chemical Co., Ltd (No. FZ2019-RWS-027)the Open Fund of the Key Laboratory of Fine Chemical Application Technology of Luzhou (No. HYJH-2101-B)
文摘Many electrochemical energy storage devices,such as batteries,supercapacitors,and metal ion capacitors,rely on effective and inexpensive electrode materials.Herein,we have developed highly active nitrogen-doped porous carbon nanofoams(NPCNs-600-N)for sodium-ion capacitors(SICs).NPCNs-600-N have a highly porous framework,extended interlayer spacing(0.41 nm),and lots of surface functional groups.Accordingly,NPCNs-600-N achieves a high reversible capacity(301 mAh·g^(-1)at 0.05 A·g^(-1)),superior rate capability(112 mAh·g^(-1)at 5.00 A·g^(-1)),and ultra-stable cyclability.The excellent rate and cycling performance originate from the abundant active sites and porous architecture of NPCNs-600-N.Further-more,SICs device is constructed by employing the NPCNs-600-N as the battery-like anode and commercial superconductive carbon black as the capacitive cathode,which delivers high energy/power densities of 92 Wh·kg^(-1)/15984 W·kg^(-1)with a remarkable cyclability(93%reten-tion over 5000 cycles at 1.00 A·g^(-1)).The methodology of the work enables the simultaneous tuning of the porous architectures and surface function groups of carbon for high-performance SICs.
文摘We produced Wood-Polymer Composites (WPCs) with phenolic resin (PR) filled with saw dust (SD) and rice husks (RH) in a PR:fillerratio of 60:40 wt.%. RH and SD were grinded and sieved into particles μm. The aim of this research work was to evaluate sawdust and rice husks as fillers for sustainable phenolic resin based WPCs. Therefore, we investigated the thermal stability of PR/RH and PR/SD WPCs then we studied and compared the tensile, flexural properties of PR/SD and PR/RH WPCs samples, as well as their dimensional stability after water absorption test. Furthermore, through ultraviolet light exposure, we evaluated the effects of photo-oxidation on the water stability and mechanical properties of PR/RH and PR/SD WPCs samples compared to unexposed ones. PR filled with SD presented better mechanical properties compared to PR/RH WPCs samples. However, PR/RH WPCs showed good mechanical properties, and better thermal resistance and better water repulsion capabilities compared to PR/SD WPCs samples. Although, long time UV exposure ended up lowering considerably the mechanical properties and water resistance of PR/SD and PR/RH WPCs, both RH and SD offer great added value as fillers for PR based WPCs;SD having better interactions with PR matrix compared to RH.
文摘It is with great sadness for us that Professor Wei Jiang, a young and well-known supramolecular chemist, passed away on Sunday25 December 2022. He created a series of supramolecular hosts including Oxatubarenes [1] and Naphthotubes [2] with inner functionalized groups [3–6] and applied them into materials, catalysis,molecular machines and drug recognition and delivery fields [7–10] during his independent research career.
文摘The recognition function based on host-vip chemistry of molecular cages represents one of the primary origins of supramolecular chemistry.The utilization of host-vip interactions allows the artificially designed supramolecular hosts for a wide range of applications in binding recognition,drug delivery,molecular separation,confined catalysis,etc[1-3].
基金supported by the National Key Research and Development Program of China(2023YFA1802000,2021YFA0910000)the National Natural Science Foundation of China(22225805,22308101,32394001,32121005)+1 种基金the Shanghai Science and Technology Innovation Action Plan(23J21901600)the Innovation Program of Shanghai Municipal Education Commission,China Postdoctoral Science Foundation(2021M701199)。
文摘Sequence-activated chemiluminescence(CL)technique offers a unique approach to detecting specific biomolecules or cellular events with high sensitivity and spatial resolution.The fundamental principle behind sequence-activated CL probes involves tailoring highly-controllable CL signals in response to specific sequences or events of interest,thus enabling high-contrast signals under complex physiological conditions.This sequential activation could be triggered by enzymes,reactive oxygen species(ROS),biothiols or changes in the microenvironment.These unique sequence-activated CL probes bestow several advantages,including minimal background,deep-tissue penetration,and the ability of non-invasive or minimally invasive detection.The sequence-activated CL techniques represent a significant advancement in molecular imaging and diagnostics.In this mini-review,we focus on the latest developments in sequential CL probes,addressing the technical challenges and discussing the future trajectory by harnessing CL signaling and molecular recognition.
基金supported by the National Basic Research Program of China(2017YFA0205100)the Key Project of Science and Technology Plan of Beijing Education Commission(KZ201910028038)financial support from the China Postdoctoral Science Foundation(2018M641065,2021T140009)。
文摘Electroluminescence of f-f transition lanthanide complex is a traditional topic for display over decades.Here we report highly efficient organic light-emitting diodes based on a new terbium(III)complex with novel ligand CPMIP(1-(4-cyanophenyl)-3-methyl-4-isobutyryl-pyrazoline-5-one).The high triplet energy level of CPMIP(3.0 e V)and inhibited quenching effects in the solid-state lead to a nearly 100%photoluminescent quantum efficiency of Tb(CPMIP)3.The best Tb(CPMIP)3 device exhibited maximum external quantum efficiency up to 19.7%,setting a new record of OLEDs based on f-f transition lanthanide complexes.
基金supported by the National Natural Science Foundation of China(21788102,21875064,81903545,21604023,21790361)Shanghai Science and Technology Commission Basic Project-Shanghai Natural Science Foundation(21ZR1417600)+5 种基金Shanghai Municipal Science and Technology Major Project(2018SHZDZX03)Programme of Introducing Talents of Discipline to Universities(B16017)Shanghai Science and Technology Committee(17520750100)Beijing New-Star Plan of Science and Technology(Z201100006820009)Shanghai Sailing Program(16YF1402200)the Fundamental Research Funds for the Central Universities。
文摘Precise and early detection ofβ-amyloid(Aβ)deposits in situ and in real time is pivotal to the diagnosis and early intervention of Alzheimer’s disease(AD).Optical imaging stands out to be a promising technique for such a task;however,it still remains a big challenge,due to the lack of high-performance imaging contrast agent.Restricted by poor blood-brain barrier(BBB)penetrability,short-wavelength excitation and emission,as well as the aggregation-caused quenching effect,the widely used goldstandard probes cannot be used for early in-vivo imaging of Aβdeposits.Herein,we integrate the Aβdeposits-favored geometry,amphiphilic and zwitterionic molecular structure,extended D-π-A electronic structure,and 3 D conformation into one molecule,facilely establishing a simple and economic imaging contrast agent that enjoys high specificity and affinity to Aβdeposits,good BBB penetrability,bright red/near-infrared fluorescence,low interference from autofluorescence,aggregation-induced emission(AIE)feature,high signal-to-noise ratio(SNR),and high contrast.In-vitro,ex-vivo,and in-vivo experiments with different strains of mice indicate that AIE-CNPy-AD holds the universality to Aβdeposits identification.Noteworthily,AIE-CNPy-AD is even able to precisely trace the small and sparsely-distributed Aβdeposits in AD model mice as young as 4-month-old APP/PS1 mice,the youngest having Aβdeposits.Moreover,the present probe could clearly reveal the increase and enlargement of Aβdeposits as the mice grow.Therefore,AIE-CNPy-AD might be an ideal alternative for early AD diagnosis and highly reliable monitoring of AD progression.
