The elastic thickness of the lithosphere(Te)is a key parameter used to describe the strength of the lithosphere.It is usually estimated by a spectral analysis between gravity and topography.In previous research on the...The elastic thickness of the lithosphere(Te)is a key parameter used to describe the strength of the lithosphere.It is usually estimated by a spectral analysis between gravity and topography.In previous research on the estimation of Te,altimetry data were used on both the gravity data and topography data,which could lead to deviations.The study described in this paper analyzed the effects of using gravity anomalies derived from different data sources on the estimation of Te,Taking the western Pacific region as an example,this study analyzed the impact of the repeated presence of altimetry satellite data on the calculation of the effective elastic thickness and found that if gravity anomalies and topography model both contain altimetry satellite data,they systematically overestimate effective elasticity.For a uniform area,the difference in Te can reach up to 30%.For a Te distribution,the difference can reach up to about16%.After eliminating this effect,the effective elastic thickness of the western Pacific region was found to be 10 km,and the statistical results of the effective elastic thickness distribution showed that the effective elastic thickness of the lithosphere in most areas of the western Pacific is about 12 km.The paper shows the importance of choosing the appropriate gravity model in evaluating the elastic thickness of lithosphere in the oceans.A figure of Te at seamounts with loading ages demonstrates that Te in the western Pacific is generally distributed within the 100-300℃isotherm depth and does not increase with loading age.展开更多
Developing organic room-temperature phosphorescence(RTP)materials with a wide range of tunable-emission is significant in expanding the applications of RTP materials.Herein,we rationally designed amphiphilic alternati...Developing organic room-temperature phosphorescence(RTP)materials with a wide range of tunable-emission is significant in expanding the applications of RTP materials.Herein,we rationally designed amphiphilic alternating copolymers poly(1,2-bis(4-alkoxyphenyl)ethane-1,2-dione-alt-(ethylene glycol)x)(P(Bz-alt-EGx))that combined the advantage of alternating benzil and EGxskeleton,and tunable mainchain conformation.Through a mainchain conformation ordering assembly(COA)process,P(Bz-alt-EGx)self-assembled into well-defined platelets,and such assemblies emitted blue RTP at ca.425 nm due to the ordered folded-chain conformation and confined microenvironment.In contrast,traditional self-assembly(TA)of P(Bz-alt-EGx)obtained less ordered aggregates,such as asymmetric worms,vesicles,and rod-like micelles.The resultant less ordered aggregates exhibited yellow-green RTP at ca.550 nm.The wide-tuning RTP emission in solution(between blue and yellow-green,over125 nm)is realized using the P(Bz-alt-EG_(x))alternating copolymers under the treatment of different self-assembly conditions.This study uncovers a new strategy to tailor the RTP emission through different self-assembly pathways and holds great promise for the fabrication of advanced optical materials.展开更多
Stretchable and self-healable materials with excellent mechanical performance hold great promise for applications in flexible functional devices.Despite rapid developments,achieving high mechanical strength,extreme st...Stretchable and self-healable materials with excellent mechanical performance hold great promise for applications in flexible functional devices.Despite rapid developments,achieving high mechanical strength,extreme stretchability,and rapid selfhealing capability in self-healing materials remains challenging.Here,inspired by the hierarchical structure and unique network of connective tissue,we fabricated a class of bionic nanocomposites with high stretchability,outstanding mechanical strength,and rapid self-healing ability by integrating the bottlebrush copolymer functionalized graphene oxide(BCP@GO)into a polyurethane(PU)matrix via in-situ polymerization.The bottlebrush copolymer(BCP)acted as a bond bridge for linking the GO nanosheets(noncovalent interaction)and PU chains(covalent and hydrogen-bond interaction).The covalent interactions were responsible for providing high mechanical strength,and the abundant hydrogen-bond-based cross-links realized extreme stretchability and rapid self-healing capability.The resultant BCP@GO/PU nanocomposite with only 0.5 wt.%GO loading exhibited excellent mechanical properties(tensile strength increased by 52.1%,up to 28.6 MPa;toughness increased by 70.8%,up to 256.9 MJ/m^(3);elongation at break increased by 12.8%,up to 1847.2%),exceptional rapid and efficient self-healing ability(~99%with 20 s NIR irradiation),as well as superior shape memory and recyclable capability.This study develops a new strategy for designing highperformance self-healing nanocomposites and unfolds broad application prospects in smart materials.展开更多
Living crystallization-driven self-assembly(CDSA)provides robust access to uniformπ-conjugated nanostructures(CNSs)from block copolymers(BCPs)containing a crystallineπ-conjugated segment with controlled dimension,mo...Living crystallization-driven self-assembly(CDSA)provides robust access to uniformπ-conjugated nanostructures(CNSs)from block copolymers(BCPs)containing a crystallineπ-conjugated segment with controlled dimension,morphology and composition,which show appealing applications in biomedicine,photocatalysis and microelectronics.To further expand the application spectrum of these CNSs,the development of facile strategies toward diverse CNSs with varying structures/functionalities is highly desired.Herein,BCPs consisting of oligo(p-phenylene ethynylene)-b-poly(polypropyl-3-methanethiol acrylate)(OPE_(9)-bPMTPA35and OPE_(9)-b-PMTPA_(58);the subscript represents the number of repeat unit of each block)consisting of a crystallineπ-conjugated core-forming OPE_(9)segment and a corona-forming PMTPA block are synthesized.By efficient“click-type”alkylation of methylthio groups,OPE_(9)-b-PMTPA with varying contents of sulfonium unit is obtained.Uniform ribbon-like micelles with different widths and lengths can then be generated in a controlled manner via the self-seeding approach of living CDSA.Additionally,negatively charged polymeric and Ag nanoparticles can be immobilized on sulfonium/methylthio-containing shells by taking advantage of electrostatic attraction and coordination interaction,respectively.Interestingly,the ribbon-like micelles with positively charged shells exhibit antibacterial activity against E.coli.Given the ease of modification of PMTPA-based shell and attractive opto-electronic/photocatalytic properties ofπ-conjugated units,the combination of methylthio-chemistry and living CDSA opens a new avenue to generate multi-functional CNSs for widespread applications from biomedicine to photocatalysis.展开更多
This paper reports an overpotential-dependent shape evolution of gold nano-crystals （Au NCs） in a choline chloride-urea （ChCl-urea） based deep eutectic solvent （DES）. It was found that the growth overpotentials ...This paper reports an overpotential-dependent shape evolution of gold nano-crystals （Au NCs） in a choline chloride-urea （ChCl-urea） based deep eutectic solvent （DES）. It was found that the growth overpotentials play a key role in tuning the shape of Au NCs. The shape evolution of Au NCs successively from concave rhombic dodecahedra （RD） to concave cubes, octopods, cuboctahedral boxes, and finally, to hollow octahedra （OH） was achieved by carefully controlling the growth overpotentials in the range from -0.50 to -0.95 V （vs. Pt quasi-reference electrode）. In addition, the presence of urea was important in the shape evolution of Au NCs. The surface structure of the as-prepared Au NCs was comprehensively characterized by scanning electron microscopy （SEM）, transmission electron microscopy （TEM） and electrochemical studies. It was demonstrated that the electrocatalytic activity of the as-prepared Au NCs for D-glucose electrooxidation was sensitively dependent on their morphologies. The results illustrated that the dehydrogenated glucose adsorbed on concave RD and concave cubic Au NCs was preferentially transformed to gluconolactone at low electrode potentials. Subsequent gluconolactone oxidation occurred favorably on octopods with {111}-truncated arms and hollow OH at high electrode potential. This study opens up a new approach to develop the surface-structure-controlled growth of Au NCs by combining DES with electrochemical techniques. In addition, it is significant for the tuning of the electrocatalytic properties of NCs.展开更多
Comprehensive Summary Starting from an organic multiyne,three steps are normally needed for the preparation of non-βphosphonium functionalized rhodaand irida-carbolong complexes.Herein,a one-pot strategy,by mixing a ...Comprehensive Summary Starting from an organic multiyne,three steps are normally needed for the preparation of non-βphosphonium functionalized rhodaand irida-carbolong complexes.Herein,a one-pot strategy,by mixing a multiyne,a nucleophile,and Rhcl(CO)(PPh_(3))_(2)/AgBF_(4)or[Ir(CH:CN)(CO)(PPh_(3))_(2)]BF_(4),was developed to achieve a series ofβfunctionalized rhoda-and irida-carbolong complexes.Theβ-substituents in these complexes can be various C-,N-and O-centered groups,dependent on the nucleophiles used.This strategy provides a new convenient route to construct carbolong complexes,which is important for the further development of carbolong chemistry.展开更多
基金funded by Guangdong Province Introduced Innovative R&D Team of Geological Processes and Natural Disasters around the South China Sea,China(No.2016ZT06N331)the National key Research and Development Program of China,China(No.2017YFC1500101)Guangdong Province Natural Science Foundation,China(No.2018A030310314)。
文摘The elastic thickness of the lithosphere(Te)is a key parameter used to describe the strength of the lithosphere.It is usually estimated by a spectral analysis between gravity and topography.In previous research on the estimation of Te,altimetry data were used on both the gravity data and topography data,which could lead to deviations.The study described in this paper analyzed the effects of using gravity anomalies derived from different data sources on the estimation of Te,Taking the western Pacific region as an example,this study analyzed the impact of the repeated presence of altimetry satellite data on the calculation of the effective elastic thickness and found that if gravity anomalies and topography model both contain altimetry satellite data,they systematically overestimate effective elasticity.For a uniform area,the difference in Te can reach up to 30%.For a Te distribution,the difference can reach up to about16%.After eliminating this effect,the effective elastic thickness of the western Pacific region was found to be 10 km,and the statistical results of the effective elastic thickness distribution showed that the effective elastic thickness of the lithosphere in most areas of the western Pacific is about 12 km.The paper shows the importance of choosing the appropriate gravity model in evaluating the elastic thickness of lithosphere in the oceans.A figure of Te at seamounts with loading ages demonstrates that Te in the western Pacific is generally distributed within the 100-300℃isotherm depth and does not increase with loading age.
基金supported by the National Natural Science Foundation of China(52073094,52273291,52273008)the Shanghai Scientific and Technological Innovation Project(22ZR1479300)the Shanghai Rising-Star Program(23QA1402500)。
文摘Developing organic room-temperature phosphorescence(RTP)materials with a wide range of tunable-emission is significant in expanding the applications of RTP materials.Herein,we rationally designed amphiphilic alternating copolymers poly(1,2-bis(4-alkoxyphenyl)ethane-1,2-dione-alt-(ethylene glycol)x)(P(Bz-alt-EGx))that combined the advantage of alternating benzil and EGxskeleton,and tunable mainchain conformation.Through a mainchain conformation ordering assembly(COA)process,P(Bz-alt-EGx)self-assembled into well-defined platelets,and such assemblies emitted blue RTP at ca.425 nm due to the ordered folded-chain conformation and confined microenvironment.In contrast,traditional self-assembly(TA)of P(Bz-alt-EGx)obtained less ordered aggregates,such as asymmetric worms,vesicles,and rod-like micelles.The resultant less ordered aggregates exhibited yellow-green RTP at ca.550 nm.The wide-tuning RTP emission in solution(between blue and yellow-green,over125 nm)is realized using the P(Bz-alt-EG_(x))alternating copolymers under the treatment of different self-assembly conditions.This study uncovers a new strategy to tailor the RTP emission through different self-assembly pathways and holds great promise for the fabrication of advanced optical materials.
基金supported by the National Natural Science Foundation of China(Nos.22278140,U22B20143,and 52273008)the Science and Technology Commission of Shanghai Municipality(Nos.22DZ1205900 and 22ZR1479300)+1 种基金Shanghai Rising-Star Program(No.23QA1402500)Project supported by Shanghai Municipal Science and Technology Major Project,and the Fundamental Research Funds for the Central Universities.
文摘Stretchable and self-healable materials with excellent mechanical performance hold great promise for applications in flexible functional devices.Despite rapid developments,achieving high mechanical strength,extreme stretchability,and rapid selfhealing capability in self-healing materials remains challenging.Here,inspired by the hierarchical structure and unique network of connective tissue,we fabricated a class of bionic nanocomposites with high stretchability,outstanding mechanical strength,and rapid self-healing ability by integrating the bottlebrush copolymer functionalized graphene oxide(BCP@GO)into a polyurethane(PU)matrix via in-situ polymerization.The bottlebrush copolymer(BCP)acted as a bond bridge for linking the GO nanosheets(noncovalent interaction)and PU chains(covalent and hydrogen-bond interaction).The covalent interactions were responsible for providing high mechanical strength,and the abundant hydrogen-bond-based cross-links realized extreme stretchability and rapid self-healing capability.The resultant BCP@GO/PU nanocomposite with only 0.5 wt.%GO loading exhibited excellent mechanical properties(tensile strength increased by 52.1%,up to 28.6 MPa;toughness increased by 70.8%,up to 256.9 MJ/m^(3);elongation at break increased by 12.8%,up to 1847.2%),exceptional rapid and efficient self-healing ability(~99%with 20 s NIR irradiation),as well as superior shape memory and recyclable capability.This study develops a new strategy for designing highperformance self-healing nanocomposites and unfolds broad application prospects in smart materials.
基金supported by the National Natural Science Foundation of China(52122314,U22A20131,52273008,52361165657)the Strategic Priority Research Program of Chinese Academy of Sciences(XDB0590000)+1 种基金the Shanghai Scientific and Technological Innovation Project(21520780100,21ZR1481700,22ZR1479300,22JC1401000,22ZR1475400)the Shanghai Rising-Star Program(23QA1402500)。
文摘Living crystallization-driven self-assembly(CDSA)provides robust access to uniformπ-conjugated nanostructures(CNSs)from block copolymers(BCPs)containing a crystallineπ-conjugated segment with controlled dimension,morphology and composition,which show appealing applications in biomedicine,photocatalysis and microelectronics.To further expand the application spectrum of these CNSs,the development of facile strategies toward diverse CNSs with varying structures/functionalities is highly desired.Herein,BCPs consisting of oligo(p-phenylene ethynylene)-b-poly(polypropyl-3-methanethiol acrylate)(OPE_(9)-bPMTPA35and OPE_(9)-b-PMTPA_(58);the subscript represents the number of repeat unit of each block)consisting of a crystallineπ-conjugated core-forming OPE_(9)segment and a corona-forming PMTPA block are synthesized.By efficient“click-type”alkylation of methylthio groups,OPE_(9)-b-PMTPA with varying contents of sulfonium unit is obtained.Uniform ribbon-like micelles with different widths and lengths can then be generated in a controlled manner via the self-seeding approach of living CDSA.Additionally,negatively charged polymeric and Ag nanoparticles can be immobilized on sulfonium/methylthio-containing shells by taking advantage of electrostatic attraction and coordination interaction,respectively.Interestingly,the ribbon-like micelles with positively charged shells exhibit antibacterial activity against E.coli.Given the ease of modification of PMTPA-based shell and attractive opto-electronic/photocatalytic properties ofπ-conjugated units,the combination of methylthio-chemistry and living CDSA opens a new avenue to generate multi-functional CNSs for widespread applications from biomedicine to photocatalysis.
基金This study was supported financially by the National Natural Science Foundation of China （Nos. 21361140374, 21229301, 21378113, and 21573183） and the Natural Science Fund project in Jiangsu Province, China （No. BK20160210）.
文摘This paper reports an overpotential-dependent shape evolution of gold nano-crystals （Au NCs） in a choline chloride-urea （ChCl-urea） based deep eutectic solvent （DES）. It was found that the growth overpotentials play a key role in tuning the shape of Au NCs. The shape evolution of Au NCs successively from concave rhombic dodecahedra （RD） to concave cubes, octopods, cuboctahedral boxes, and finally, to hollow octahedra （OH） was achieved by carefully controlling the growth overpotentials in the range from -0.50 to -0.95 V （vs. Pt quasi-reference electrode）. In addition, the presence of urea was important in the shape evolution of Au NCs. The surface structure of the as-prepared Au NCs was comprehensively characterized by scanning electron microscopy （SEM）, transmission electron microscopy （TEM） and electrochemical studies. It was demonstrated that the electrocatalytic activity of the as-prepared Au NCs for D-glucose electrooxidation was sensitively dependent on their morphologies. The results illustrated that the dehydrogenated glucose adsorbed on concave RD and concave cubic Au NCs was preferentially transformed to gluconolactone at low electrode potentials. Subsequent gluconolactone oxidation occurred favorably on octopods with {111}-truncated arms and hollow OH at high electrode potential. This study opens up a new approach to develop the surface-structure-controlled growth of Au NCs by combining DES with electrochemical techniques. In addition, it is significant for the tuning of the electrocatalytic properties of NCs.
基金We gratefully acknowledge the NSFC(Nos.22071098,21871068,22101123 and 22101115)the Guangdong Provincial Key Laboratory of Catalysis(No.2020B121201002)the Shenzhen Science and Technology Innovation Committee(Nos.JCYJ20200109140812302 and JCYJ20210324105013035),for their financial support.
文摘Comprehensive Summary Starting from an organic multiyne,three steps are normally needed for the preparation of non-βphosphonium functionalized rhodaand irida-carbolong complexes.Herein,a one-pot strategy,by mixing a multiyne,a nucleophile,and Rhcl(CO)(PPh_(3))_(2)/AgBF_(4)or[Ir(CH:CN)(CO)(PPh_(3))_(2)]BF_(4),was developed to achieve a series ofβfunctionalized rhoda-and irida-carbolong complexes.Theβ-substituents in these complexes can be various C-,N-and O-centered groups,dependent on the nucleophiles used.This strategy provides a new convenient route to construct carbolong complexes,which is important for the further development of carbolong chemistry.
