Recently, we reported a series of reversibly interlocked polymer networks(RILNs), whose mechanical robustness and functionalities improvement was believed to be derived from topological interlocking of two sub-network...Recently, we reported a series of reversibly interlocked polymer networks(RILNs), whose mechanical robustness and functionalities improvement was believed to be derived from topological interlocking of two sub-networks, although the direct evidence for the deduction is still lacking. Herein, a specially-designed RILNs system, in which the inter-component hydrogen bonds can be shielded as needed, was prepared and used to study the micro-structures of RILNs, aiming to verify the existence of mechanical interlocking in RILNs. By changing the pH of the swelling solvent, the effect exerted by the inter-component non-covalent bonds was eliminated, so detailed information of the networks structure was exposed. The small angle X-ray scattering(SAXS) and small-angle neutron scattering(SANS) results indicated that swelling-induced structural evolution of the two sub-networks mutually affected each other, even when the inter-component hydrogen bonds were absent, proving the presence of topological interlocking. The findings may help to draw a more accurate physical image and reveal the detailed structureproperty relationship of RILNs.展开更多
An interlocked M_(4) L_(8) coordination cage was synthesized by coordination-driven self-assembly of palladium(Ⅱ)ions with aromatic amide bidentate ligands.The reaction of the ligand and the metal at 2:1 ratio led to...An interlocked M_(4) L_(8) coordination cage was synthesized by coordination-driven self-assembly of palladium(Ⅱ)ions with aromatic amide bidentate ligands.The reaction of the ligand and the metal at 2:1 ratio led to the monomeric M_(2) L_(4) cage as the kinetic product,while the thermodynamic product M_(4) L_(8) cage was obtained by prolongating the reaction.This conve rsion and the interlocked structure was clearly revealed by using~1 H NMR,mass spectrometry and X-ray crystallography.The driving force of interlocking was mainly attributed to the interactions(hydrogen bonding,aromatic stacking and electrostatic interaction)arising from the aptitude of flexibility of the amide ligand.展开更多
Two-dimensional(2D)materials have attracted considerable interest thanks to their unique electronic/physical-chemical characteristics and their potential for use in a large variety of sensing applications.However,few-...Two-dimensional(2D)materials have attracted considerable interest thanks to their unique electronic/physical-chemical characteristics and their potential for use in a large variety of sensing applications.However,few-layered nanosheets tend to agglomerate owing to van der Waals forces,which obstruct internal nanoscale transport channels,resulting in low electrochemical activity and restricting their use for sensing purposes.Here,a hybrid MXene/rGO aerogel with a three-dimensional(3D)interlocked network was fabricated via a freeze-drying method.The porous MXene/rGO aerogel has a lightweight and hierarchical porous architecture,which can be compressed and expanded several times without breaking.Additionally,a flexible pressure sensor that uses the aerogel as the sensitive layer has a wide response range of approximately 0-40 kPa and a considerable response within this range,averaging approximately 61.49 kPa^(-1).The excellent sensing performance endows it with a broad range of applications,including human-computer interfaces and human health monitoring.展开更多
The design and synthesis of two-dimensional(2D)polymers have received notable attention over the past two decades because of their unique structural properties and wide range of applications,such as molecular separati...The design and synthesis of two-dimensional(2D)polymers have received notable attention over the past two decades because of their unique structural properties and wide range of applications,such as molecular separation,nanoelectronics,sensing,and optoelectronics[1].The regularity of 2D polymeric networks,especially when high crystallinity is formed,allows them to control their pore sizes,surface areas,and mechanical properties,keeping them at the forefront of materials chemistry and nanotechnology[2,3].展开更多
The mechanics of structural ceramics,especially the toughness,are crucial to their service reliability and need to be continuously optimized.Inspired by the“brick-mortar”structure and further adjusting the microstru...The mechanics of structural ceramics,especially the toughness,are crucial to their service reliability and need to be continuously optimized.Inspired by the“brick-mortar”structure and further adjusting the microstructure of“mortar”on the interface,ceramic with strength and toughness up to 444.16 MPa and 13.79 MPa⋅m^(1/2) is constructed by hot pressed sintering with alumina(Al_(2)O_(3))as brick and vertical graphene(VG)with active atomic edges as mortar.Relying on the covalent interface between VG grown in-situ and Al_(2)O_(3),the sliding of Al_(2)O_(3)links the shear-deformation process of the crosslinked and interlocked nanointerface formed by VG,making the VG-enhanced Al_(2)O_(3)ceramics(AVG)obtain super toughness.Moreover,the structure of interlocked VG-nanointerface exhibits an excellent high-temperature resistance,which makes AVG still show the excellent strength of 437.66 MPa and toughness of 11.16 MPa⋅m^(1/2)after heat treatment at 1500℃for 100 h and they are respective 2.51 times and 3.18 times higher than Al_(2)O_(3)in the same condition.This work provides a new thought for the preparation of high-strength,ultra-tough and high-temperature mechanical stable ceramics.展开更多
Styrene-butadiene rubber(SBR)is an indispensable material in modern society,and the necessity for enhanced mechanical properties in SBR persists,particularly to withstand the rigors of challenging environmental condit...Styrene-butadiene rubber(SBR)is an indispensable material in modern society,and the necessity for enhanced mechanical properties in SBR persists,particularly to withstand the rigors of challenging environmental conditions.To surmount the limitations of conventional cross-linking modes,mechanical bonds stabilized by host-vip recognition are incorporated as the cross-linking points of SBR to form mechanically interlocked networks(MINs).Compared with covalently cross-linked network,the representative MIN exhibits superior mechanical performance in terms of elongation(1392%)and breaking strength(4.6 MPa),whose toughness has surged by 17 times.Dissociation of host-vip recognition and subsequent sliding motion provide an effective energy dissipation mechanism,and the release of hidden length is also beneficial to enhance toughness.Furthermore,the introduction of the rotaxane cross-links made the network more pliable and possess damping and elastic properties,which can return to initial state with one minute rest interval.We aspire that this direct introduction method can serve as a blueprint,offering valuable insights for the enhancement of mechanical properties in conventional commercial polymer materials.展开更多
Three-dimensional(3D)interlocking frameworks are attracting increasing research attention owing to their intriguing mechanical properties,large surface areas,and rich open sites.The study in this paper entailed the fi...Three-dimensional(3D)interlocking frameworks are attracting increasing research attention owing to their intriguing mechanical properties,large surface areas,and rich open sites.The study in this paper entailed the first use of tuning solvents to realize the synthesis of metal-organic frameworks(MOFs)and metallosalen-based covalent-organic frameworks(COFs)with similar 3D interlocked structures from the same precursors.These interlocking crystalline frameworks are efficient catalysts for CO_(2)photoreduction.Our study is the first to investigate the impact of differences in the metal coordination environment within structurally similar COFs and MOFs in CO_(2)photoreduction activity.Among the materials tested,the photocatalytic performance of the M-N2O4-MOFs(M=Zn,Co,and Ni)was found to be superior to that of their M-N2O_(2)-COF counterparts.Notably,the Ni-N2O4-MOF achieved a CO production rate of 3.96 mmol g^(-1)h^(-1)and a CO selectivity of 93.7%.In contrast,the Ni-N2O_(2)-COF exhibited a production rate of only 0.64 mmol g^(-1)h^(-1)with a 61.1%CO selectivity.Furthermore,a descriptor for the CO evolution rate was derived from the conduction band minimum and the reaction energy of the rate-determining step,which are two key factors influencing photocatalytic activity.This study opens up new avenues for employing interlocking crystalline frameworks in the efficient photoreduction of CO_(2).展开更多
The performance degradation and even damage of the e-textiles caused by sweat,water,or submersion during all-weather health monitoring are the main reasons that e-textiles have not been commercialized and routinized s...The performance degradation and even damage of the e-textiles caused by sweat,water,or submersion during all-weather health monitoring are the main reasons that e-textiles have not been commercialized and routinized so far.Herein,we developed an amphibious,high-performance,air-permeable,and comfortable all-textile triboelectric sensor for continuous and precise measurement of epidermal pulse waves during full-day activities.Based on the principle of preparing gas by acid-base neutralization reaction,a one-piece preparation process of amphibious conductive yarn(ACY)with densely porous structures is proposed.An innovative three-dimensional(3D)interlocking fabric knitted from ACYs(0.6 mm in diameter)and polytetrafluoroethylene yarns exhibit high sensitivity(0.433 V·kPa^(-1)),wide bandwidth(up to 10 Hz),and stability(>30,000 cycles).With these benefits,98.8%agreement was achieved between wrist pulse waves acquired by the sensor and a high-precision laser vibrometer.Furthermore,the polytetrafluoroethylene yarn with good compression resilience provides sufficient mechanical support for the contact separation of the ACYs.Meanwhile,the unique skeletonized design of the 3D interlocking structure can effectively relieve the water pressure on the sensor surface to obtain stable and accurate pulse waves(underwater depth of 5 cm).This achievement represents an important step in improving the practicality of e-textiles and early diagnosis of cardiovascular diseases.展开更多
Smart electromagnetic functional devices prepared based on electromagnetic wave responsive materials will provide more convenience for human life in the future.Here,we prepare oriented magnetic liquid metal droplet-fi...Smart electromagnetic functional devices prepared based on electromagnetic wave responsive materials will provide more convenience for human life in the future.Here,we prepare oriented magnetic liquid metal droplet-filled polydimethylsiloxane films with micropillar array patterned surfaces,and further assemble them into bilayer films with interlocked structures.Once compressed,the increase in conductivity of the film due to the tunneling effect between microarrays and the elongation of liquid metal droplets leads to a rapid increase in electromagnetic interference shielding performance.Accordingly,a tunable electromagnetic interference shielding material with high sensitivity and wide control range is obtained,which has potential applications in electromagnetic wave control systems and intelligent electromagnetic protection systems.Meanwhile,we assemble a strain sensor and a magnetic sensor,which can precisely sense pressure and magnetic field according to changes in electromagnetic signal and electrical signal,respectively.展开更多
The construction of interlocked topologies by metal-cation-template methods has been extensively explored.However,construction of these species using template-free chemical self-assembly methods is hard to rationally ...The construction of interlocked topologies by metal-cation-template methods has been extensively explored.However,construction of these species using template-free chemical self-assembly methods is hard to rationally achieve due to the inherent unpredictability of self-assembly processes.In this work,a strategy to construct interlocked[2]catenanes by coordination-driven template-free self-assembly is demonstrated,whereby combining rigid bidentate ligands with large conjugated-πarea units and building blocks with appropriate lengths facilitated construction of interlocked[2]catenane compounds.Two rigid bidentate ligands,L1 and L2,were chosen to self-assemble with three dinuclear building blocks B1,B2 and B3.Ultimately,the successful construction of three[2]catenanes demonstrated the validity of the strategy.Although[2]catenanes are the simplest of all interlocked topologies,this motif is the basis for constructing more intricate topologies.This successful strategy may therefore lead to construction of other,more intricate topologies in the future.展开更多
The concept of“robust dynamics”describes the incorporation of mechanically interlocked molecules(MIMs)into metal-organic framework(MOF)materials such that large amplitude motions(e.g.,rotation or translation of a ma...The concept of“robust dynamics”describes the incorporation of mechanically interlocked molecules(MIMs)into metal-organic framework(MOF)materials such that large amplitude motions(e.g.,rotation or translation of a macrocycle)can occur inside the free volume pore of the MOF.To aid in the preparation of such materials,reticular synthesis was used herein to design rigid molecular building blocks with predetermined ordered structures starting from the well-known MOF NOTT-101.New linkers were synthesized that have a T-shape,based on a triphenylene tetra-carboxylate strut,and their incorporation into Cu(II)-based MOFs was investigated.The single-crystal structures of three new MOFs,UWCM-12(fof),β-UWCM-13(loz),UWCM-14(lil),with naked T-shaped linkers were determined;β-UWCM-13 is the first reported example of the loz topology.A fourth MOF,UWDM-14(lil)is analogous to UWCM-14(lil)but contains a[2]rotaxane linker.Variable-temperature,^(2)H solid-state NMR was used to probe the dynamics of a 24-membered macrocycle threaded onto the MOF skeleton.展开更多
Inspired by brick-and-mortar architectures and suture interfaces,we propose a design of bioinspired nacre-like materials with interlocking sutures to improve the toughness of brittle materials.Laser-engraved glass int...Inspired by brick-and-mortar architectures and suture interfaces,we propose a design of bioinspired nacre-like materials with interlocking sutures to improve the toughness of brittle materials.Laser-engraved glass interlockers are laminated with soft interlayers in a staggered arrangement,and the fundamental mechanical properties of the structure are investigated through experiments and numerical modeling.It is found that the tensile performance,such as the strength and toughness,is strongly affected by the interlocking angle and suture line spacing.The geometric interlocking originated from suture interfaces as well as tablet sliding arising from the staggered arrangement of interlockers cooperatively contribute to enhancing the strength and toughness of this bioinspired design.Additionally,the finite element modeling shows the interfacial failure and plastic deformation,revealing the interplay of the geometric interlocking mechanism and the sliding mechanism.This novel bioinspired design paves a new path for fabrication of structural materials combining high stiffness,high strength,and enhanced toughness.展开更多
Metallic nanowires have served as novel materials for soft electronics due to their outstanding mechanical compliance and electrical properties.However,weak adhesion and low mechanical robustness of nanowire networks ...Metallic nanowires have served as novel materials for soft electronics due to their outstanding mechanical compliance and electrical properties.However,weak adhesion and low mechanical robustness of nanowire networks to substrates significantly undermine their reliability,necessitating the use of an insulating protective layer,which greatly limits their utility.Herein,we present a versatile and generalized laser-based process that simultaneously achieves strong adhesion and mechanical robustness of nanowire networks on diverse substrates without the need for a protective layer.In this method,the laser-induced photothermal energy at the interface between the nanowire network and the substrate facilitates the interpenetration of the nanowire network and the polymer matrix,resulting in mechanical interlocking through percolation.This mechanism is broadly applicable across different metallic nanowires and thermoplastic substrates,significantly enhancing its universality in diverse applications.Thereby,we demonstrated the mechanical robustness of nanowires in reusable wearable physiological sensors on the skin without compromising the performance of the sensor.Furthermore,enhanced robustness and electrical conductivity by the laser-induced interlocking enables a stable functionalization of conducting polymers in a wet environment,broadening its application into various electrochemical devices.展开更多
Brittle rock has the mechanical characteristics of a high ratio of uniaxial compressive strength to tensilestrength, brittle-ductile transition, and so on. The mineral meso-structure of brittle rock shows theinterlock...Brittle rock has the mechanical characteristics of a high ratio of uniaxial compressive strength to tensilestrength, brittle-ductile transition, and so on. The mineral meso-structure of brittle rock shows theinterlocking behavior and there are some microcracks between the mineral grains, so it is difficult toanalyze the mechanical characteristics accurately with a regular constitutive model. The previous numericalmodels have some limitations when applied to brittle rock, that they cannot provide sufficientinternal interlocking and are incapable of considering the microcracks. These limitations are addressedby using the updated flat-joint contact model to join notional polygonal particles with an initial gap andincreasing the particle coordination number by adding flat-joint contacts to more particles that arewithin some non-zero distance of one another via the range coefficient contact identification method. Acomparison of experimental and numerical results confirms that the updated flat-jointed model providesa good match with the mechanical properties of brittle rock. In this paper, we investigate the influence ofmineral meso-structure (micro-cracks, range coefficient, and radius multiplier) on the meso-mechanicalproperties of Jinping dolomitic marble via the updated flat-joint contact model under direct-tension testsand compression tests. It is found that the updated model can reproduce the microstructure effect ofbrittle rock and can better simulate the mechanical characteristics of the brittle rock than conventionalmodels, such as high strength ratio, brittle-ductile transition, initial nonlinearity, and different modulusin compression and tension.展开更多
To understand the specific behaviors of coastal coral sand slope foundations,discrete element method(DEM)was employed to examine the effect of breakable particle corners on the performance of coral sand slope foundati...To understand the specific behaviors of coastal coral sand slope foundations,discrete element method(DEM)was employed to examine the effect of breakable particle corners on the performance of coral sand slope foundations under a strip footing,from macro to micro scales.The results demonstrate that the bearing characteristics of coral sand slope foundations can be successfully modeled by utilizing breakable corner particles in simulations.The dual effects of interlocking and breakage of corners well explained the specific shallower load transmission and narrower shear stress zones in breakable corner particle slopes.Additionally,the study revealed the significant influence of breakable corners on soil behaviors on slopes.Furthermore,progressive corner breakage within slip bands was successfully identified as the underling mechanism in determining the unique bearing characteristics and the distinct failure patterns of breakable corner particle slopes.This study provides a new perspective to clarify the behaviors of slope foundations composed of breakable corner particle materials.展开更多
Mechanically interlocked molecules(MIMs)and host–vip chemistry have received great attention in the past few decades.However,it remains challenging to design architectures with mechanically interlocked features and...Mechanically interlocked molecules(MIMs)and host–vip chemistry have received great attention in the past few decades.However,it remains challenging to design architectures with mechanically interlocked features and construct cavities for vip molecule recognition using similar building blocks.In this study,we designed and constructed a series of novel twisted supramolecular structures by assembling various multitopic terpyridine(tpy)ligands with the same diameter and Zn(II)ions.The obtained complexes exhibited evolutional architectures and showed distinctively different space-constraint effects.Specifically,the assembled dimer SA,SB,and SBH displayed mechanically interlocked phenomena,including[2]catenane and[3]catenane,with an increase in concentration.However,no interlocked structures were observed in complexes SC and SCH constructed by hexatopic tpy ligands due to the significant space constraints.The single-crystal data of complex SCH further proved significant space constraints and illustrated the formation of a relatively closed cavity,which showed excellent host–vip properties for different calixarenes,especially high affinity for calix[6]arene.展开更多
Supramolecular polymers,as a type of dynamic polymers,are subordinate to the interdisciplinary field of polymer chemistry and supramolecular chemistry,whose development has greatly promoted the prosperity of new mater...Supramolecular polymers,as a type of dynamic polymers,are subordinate to the interdisciplinary field of polymer chemistry and supramolecular chemistry,whose development has greatly promoted the prosperity of new materials.Notably,molecular weight is one of the most important parameters of supramolecular polymers,which affects the physical/chemical properties and processing applications of materials.Developing new methods for characterizing the molecular weight of supramolecular polymers is crucial for advancing the development of supramolecular polymers.In this review,we elaborate and summarize three strategies for characterizing the molecular weight of supramolecular polymers that recently reported by our research group according to the characteristics of supramolecular polymers,including(1)the molecular weight distinction corresponding to variable fluorescence colors,(2)matching different molecular weights with different fluorescence lifetime,(3)transforming supramolecular polymers into mechanically interlocked polymers or covalent polymers.Besides,we also discuss the limitations of current methods for characterizing supramolecular polymers.We hope that this review can promote the development of supramolecular polymers and significantly inspire to exploit new methods to characterizing molecular weight of supramolecular polymers.展开更多
Oligo[n]rotaxanes are one of the most extensively studied categories of mechanically bonded macromolecules.In this study,a supramolecular oligo[2]rotaxane is successfully constructed driven by platinum(Ⅱ)metallacycle...Oligo[n]rotaxanes are one of the most extensively studied categories of mechanically bonded macromolecules.In this study,a supramolecular oligo[2]rotaxane is successfully constructed driven by platinum(Ⅱ)metallacycle and pillar[5]arene-based host–vip interactions in an orthogonal way.The supramolecular oligo[2]rotaxane is further applied in fabricating a light harvesting system.展开更多
In this study,the cold-spraying process was utilized to deposit Al particles onto an Al slab,an Mg slab,and both Al and Mg slabs to form an ultra-thin interlayer,and then the clad slabs were rolled at 400℃,developing...In this study,the cold-spraying process was utilized to deposit Al particles onto an Al slab,an Mg slab,and both Al and Mg slabs to form an ultra-thin interlayer,and then the clad slabs were rolled at 400℃,developing three roll-bonding processes:the roll-bonding process with cold-sprayed Al powder on the Al slab(CS-Al),the roll-bonding process with cold-sprayed Al powder on the Mg slab(CS-Mg),and the rollbonding process with cold-sprayed Al powder on both the Al slab and the Mg slab(CS-Both).The effects of three different cold-sprayed Al particle interlayer processes on the mechanical properties of rolled Mg/Al clad plates were investigated to improve the mechanical properties.The microstructure,texture evolution,intermetallic compound formation,mechanical properties,and mechanisms involved in the Mg/Al clad plate rolling were systematically investigated.The results showed that the pre-bonding between the particles and the substrates through coldspraying had a significant impact on the bonding strength of the Mg/Al clad plates,and the CS-Both process can increase the average shear strength of the Mg/Al clad plates to 49.24 MPa at a medium reduction rate of 37.5%,2.5 times that of the conventional rolling process.The CS-Both process constructed more evident dual microscopic three-dimensional interfaces and promoted more thorough atomic diffusion at the interface through the double-sided cold-spraying process.Meanwhile,the dual cold-sprayed Al coatings on both the Mg slab and Al slab underwent dynamic recrystallization during rolling to form a homogeneous unit with no additional coating interfaces.Fine grain strengthening and dislocation strengthening were judged to be important mechanisms for improving the mechanical performance of the interfacial layer.展开更多
A bottleneck in biomimetic synthesis consists in the full copy of,for example,the hierarchical structure of proteins directed by weak interactions.By contrast with covalent bonds bearing definite orientation and high ...A bottleneck in biomimetic synthesis consists in the full copy of,for example,the hierarchical structure of proteins directed by weak interactions.By contrast with covalent bonds bearing definite orientation and high stability,weak intermolecular forces within a continuous dynamic equilibrium can be hardly tamed for molecular design.In this endeavor,a ligand-dominated strategy that embodies tunable electrostatic repulsion andπ···πstacking was first employed to shape polyoxovanadate-based metal-organic polyhedra(VMOPs).Structural evolution involving transformation,interlock,and discovery of an unprecedented prototype of the Star of David was hence achievable.Not only as a handy tool for the primary structural control over VMOPs,these weak forces allow for an advanced management on the spatial distribution of such manmade macromolecules as well as the associated physicochemical behaviors,representing an ideal model for simulating and interpreting the conformation-function relationship of proteins.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos. 52033011, 52173092 and 51973237)Natural Science Foundation of Guangdong Province(Nos. 2019B1515120038, 2020A1515011276 and 2021A1515010417)+4 种基金Science and Technology Planning Project of Guangzhou City (No. 202201011568)the Talented Program of Guizhou University (No. X2022008)Fundamental Research Funds for the Central Universities,Sun Yat-sen University (No. 23yxqntd002)GBRCE for Functional Molecular Engineering,the Youth Innovation Promotion Association,CAS(No. 2020010)Guangdong Basic and Applied Basic Research Foundation (No. 2021A1515110908)。
文摘Recently, we reported a series of reversibly interlocked polymer networks(RILNs), whose mechanical robustness and functionalities improvement was believed to be derived from topological interlocking of two sub-networks, although the direct evidence for the deduction is still lacking. Herein, a specially-designed RILNs system, in which the inter-component hydrogen bonds can be shielded as needed, was prepared and used to study the micro-structures of RILNs, aiming to verify the existence of mechanical interlocking in RILNs. By changing the pH of the swelling solvent, the effect exerted by the inter-component non-covalent bonds was eliminated, so detailed information of the networks structure was exposed. The small angle X-ray scattering(SAXS) and small-angle neutron scattering(SANS) results indicated that swelling-induced structural evolution of the two sub-networks mutually affected each other, even when the inter-component hydrogen bonds were absent, proving the presence of topological interlocking. The findings may help to draw a more accurate physical image and reveal the detailed structureproperty relationship of RILNs.
基金supported by the National Natural Science Foundation of China(No.21871101)the Natural Science Foundation of Hubei Scientific Committee(Nos.2017CFA036,2019ACA125)。
文摘An interlocked M_(4) L_(8) coordination cage was synthesized by coordination-driven self-assembly of palladium(Ⅱ)ions with aromatic amide bidentate ligands.The reaction of the ligand and the metal at 2:1 ratio led to the monomeric M_(2) L_(4) cage as the kinetic product,while the thermodynamic product M_(4) L_(8) cage was obtained by prolongating the reaction.This conve rsion and the interlocked structure was clearly revealed by using~1 H NMR,mass spectrometry and X-ray crystallography.The driving force of interlocking was mainly attributed to the interactions(hydrogen bonding,aromatic stacking and electrostatic interaction)arising from the aptitude of flexibility of the amide ligand.
基金financial support from the National Natural Science Foundation of China(NSFC Grant No.61625404,61888102,62174152)Young Elite Scientists Sponsorship Program by CAST(2018QNRC001)+1 种基金the Strategic Priority Program of the Chinese Academy of Sciences,Grant No XDA16021100the Science and Technology Development Plan of Jilin Province(20210101168JC).
文摘Two-dimensional(2D)materials have attracted considerable interest thanks to their unique electronic/physical-chemical characteristics and their potential for use in a large variety of sensing applications.However,few-layered nanosheets tend to agglomerate owing to van der Waals forces,which obstruct internal nanoscale transport channels,resulting in low electrochemical activity and restricting their use for sensing purposes.Here,a hybrid MXene/rGO aerogel with a three-dimensional(3D)interlocked network was fabricated via a freeze-drying method.The porous MXene/rGO aerogel has a lightweight and hierarchical porous architecture,which can be compressed and expanded several times without breaking.Additionally,a flexible pressure sensor that uses the aerogel as the sensitive layer has a wide response range of approximately 0-40 kPa and a considerable response within this range,averaging approximately 61.49 kPa^(-1).The excellent sensing performance endows it with a broad range of applications,including human-computer interfaces and human health monitoring.
文摘The design and synthesis of two-dimensional(2D)polymers have received notable attention over the past two decades because of their unique structural properties and wide range of applications,such as molecular separation,nanoelectronics,sensing,and optoelectronics[1].The regularity of 2D polymeric networks,especially when high crystallinity is formed,allows them to control their pore sizes,surface areas,and mechanical properties,keeping them at the forefront of materials chemistry and nanotechnology[2,3].
基金supported by the National Natural Science Foundation of China under Grant Nos.52222204,52172103,52293371,52072304,and Natural Science Basic Research Program in Shaanxi(2022JC-25).
文摘The mechanics of structural ceramics,especially the toughness,are crucial to their service reliability and need to be continuously optimized.Inspired by the“brick-mortar”structure and further adjusting the microstructure of“mortar”on the interface,ceramic with strength and toughness up to 444.16 MPa and 13.79 MPa⋅m^(1/2) is constructed by hot pressed sintering with alumina(Al_(2)O_(3))as brick and vertical graphene(VG)with active atomic edges as mortar.Relying on the covalent interface between VG grown in-situ and Al_(2)O_(3),the sliding of Al_(2)O_(3)links the shear-deformation process of the crosslinked and interlocked nanointerface formed by VG,making the VG-enhanced Al_(2)O_(3)ceramics(AVG)obtain super toughness.Moreover,the structure of interlocked VG-nanointerface exhibits an excellent high-temperature resistance,which makes AVG still show the excellent strength of 437.66 MPa and toughness of 11.16 MPa⋅m^(1/2)after heat treatment at 1500℃for 100 h and they are respective 2.51 times and 3.18 times higher than Al_(2)O_(3)in the same condition.This work provides a new thought for the preparation of high-strength,ultra-tough and high-temperature mechanical stable ceramics.
基金the financial support of the National Natural Science Foundation of China(22071152 and 22122105)the financial support of the National Natural Science Foundation of China(22305150)+4 种基金the financial support from the National Natural Science Foundation of China(22101175 and 52333001)Natural Science Foundation of Shanghai(22dz1207603)supported by the Starry Night Science Fund of Zhejiang University Shanghai Institute for Advanced Study(SN-ZJU-SIAS-006)State Key Laboratory of Polyolefins and Catalysis and Shanghai Key Laboratory of Catalysis Technology for Polyolefins(SKL-LCTP-202301)the Shuguang Program of Shanghai Education Development Foundation and Shanghai Municipal Education Commission(22SG11)。
文摘Styrene-butadiene rubber(SBR)is an indispensable material in modern society,and the necessity for enhanced mechanical properties in SBR persists,particularly to withstand the rigors of challenging environmental conditions.To surmount the limitations of conventional cross-linking modes,mechanical bonds stabilized by host-vip recognition are incorporated as the cross-linking points of SBR to form mechanically interlocked networks(MINs).Compared with covalently cross-linked network,the representative MIN exhibits superior mechanical performance in terms of elongation(1392%)and breaking strength(4.6 MPa),whose toughness has surged by 17 times.Dissociation of host-vip recognition and subsequent sliding motion provide an effective energy dissipation mechanism,and the release of hidden length is also beneficial to enhance toughness.Furthermore,the introduction of the rotaxane cross-links made the network more pliable and possess damping and elastic properties,which can return to initial state with one minute rest interval.We aspire that this direct introduction method can serve as a blueprint,offering valuable insights for the enhancement of mechanical properties in conventional commercial polymer materials.
基金the National Natural Science Foundation of China(grant nos.22373058,22003031,and 22273050)the National Key Research and Development Program of China(grant no.2022YFA1503100)+2 种基金the Natural Science Foundation of Shandong Province(grant no.ZR2020QB080)the Program of Young Scholars Future Program of Shandong University for its financial support.Wei Zhou gratefully acknowledges support from the Scientific Research Staring Foundation of Hainan University(grant no.KYQD(ZR)23171)Weiqiao Deng gratefully acknowledges the financial support from the Program of Taishan Scholars Project(grant no.tspd20230601).
文摘Three-dimensional(3D)interlocking frameworks are attracting increasing research attention owing to their intriguing mechanical properties,large surface areas,and rich open sites.The study in this paper entailed the first use of tuning solvents to realize the synthesis of metal-organic frameworks(MOFs)and metallosalen-based covalent-organic frameworks(COFs)with similar 3D interlocked structures from the same precursors.These interlocking crystalline frameworks are efficient catalysts for CO_(2)photoreduction.Our study is the first to investigate the impact of differences in the metal coordination environment within structurally similar COFs and MOFs in CO_(2)photoreduction activity.Among the materials tested,the photocatalytic performance of the M-N2O4-MOFs(M=Zn,Co,and Ni)was found to be superior to that of their M-N2O_(2)-COF counterparts.Notably,the Ni-N2O4-MOF achieved a CO production rate of 3.96 mmol g^(-1)h^(-1)and a CO selectivity of 93.7%.In contrast,the Ni-N2O_(2)-COF exhibited a production rate of only 0.64 mmol g^(-1)h^(-1)with a 61.1%CO selectivity.Furthermore,a descriptor for the CO evolution rate was derived from the conduction band minimum and the reaction energy of the rate-determining step,which are two key factors influencing photocatalytic activity.This study opens up new avenues for employing interlocking crystalline frameworks in the efficient photoreduction of CO_(2).
基金supported by the National Key Research and Development Program of China(No.2021YFA1201600)the Natural Science Foundation Projects of Chongqing(No.cstc2022ycjh-bgzxm0206)the Natural Science Foundation of Innovative Research Groups(No.cstc2020jcyj-cxttX0005).
文摘The performance degradation and even damage of the e-textiles caused by sweat,water,or submersion during all-weather health monitoring are the main reasons that e-textiles have not been commercialized and routinized so far.Herein,we developed an amphibious,high-performance,air-permeable,and comfortable all-textile triboelectric sensor for continuous and precise measurement of epidermal pulse waves during full-day activities.Based on the principle of preparing gas by acid-base neutralization reaction,a one-piece preparation process of amphibious conductive yarn(ACY)with densely porous structures is proposed.An innovative three-dimensional(3D)interlocking fabric knitted from ACYs(0.6 mm in diameter)and polytetrafluoroethylene yarns exhibit high sensitivity(0.433 V·kPa^(-1)),wide bandwidth(up to 10 Hz),and stability(>30,000 cycles).With these benefits,98.8%agreement was achieved between wrist pulse waves acquired by the sensor and a high-precision laser vibrometer.Furthermore,the polytetrafluoroethylene yarn with good compression resilience provides sufficient mechanical support for the contact separation of the ACYs.Meanwhile,the unique skeletonized design of the 3D interlocking structure can effectively relieve the water pressure on the sensor surface to obtain stable and accurate pulse waves(underwater depth of 5 cm).This achievement represents an important step in improving the practicality of e-textiles and early diagnosis of cardiovascular diseases.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.51971008,U1832138,51731002,and 51671010)Natural Science Foundation of Beijing Municipality(No.2212033).
文摘Smart electromagnetic functional devices prepared based on electromagnetic wave responsive materials will provide more convenience for human life in the future.Here,we prepare oriented magnetic liquid metal droplet-filled polydimethylsiloxane films with micropillar array patterned surfaces,and further assemble them into bilayer films with interlocked structures.Once compressed,the increase in conductivity of the film due to the tunneling effect between microarrays and the elongation of liquid metal droplets leads to a rapid increase in electromagnetic interference shielding performance.Accordingly,a tunable electromagnetic interference shielding material with high sensitivity and wide control range is obtained,which has potential applications in electromagnetic wave control systems and intelligent electromagnetic protection systems.Meanwhile,we assemble a strain sensor and a magnetic sensor,which can precisely sense pressure and magnetic field according to changes in electromagnetic signal and electrical signal,respectively.
基金This work was supported by the National Natural Science Foundation of China(Nos.22031003 and 21720102004)the Shanghai Science Technology Committee(No.19DZ2270100).
文摘The construction of interlocked topologies by metal-cation-template methods has been extensively explored.However,construction of these species using template-free chemical self-assembly methods is hard to rationally achieve due to the inherent unpredictability of self-assembly processes.In this work,a strategy to construct interlocked[2]catenanes by coordination-driven template-free self-assembly is demonstrated,whereby combining rigid bidentate ligands with large conjugated-πarea units and building blocks with appropriate lengths facilitated construction of interlocked[2]catenane compounds.Two rigid bidentate ligands,L1 and L2,were chosen to self-assemble with three dinuclear building blocks B1,B2 and B3.Ultimately,the successful construction of three[2]catenanes demonstrated the validity of the strategy.Although[2]catenanes are the simplest of all interlocked topologies,this motif is the basis for constructing more intricate topologies.This successful strategy may therefore lead to construction of other,more intricate topologies in the future.
基金S.J.L.acknowledges the Natural Sciences and Engineering Research Council of Canada for support of a Discovery Grant(101694)and a Canada Research Chair.R.W.S.is also grateful for support from NSERC,the Canadian Foundation for Innovation,the Ontario Innovation Trust,the University of Windsor for the development and maintenance of the SSNMR centre,and for funding from the Florida State University and the National High Magnetic Field Laboratory(NHMFL),which is funded by the National Science Foundation Cooperative Agreement(DM R-1644779)and by the State of Florida.The authors acknowledge M.Revington for technical assistance with solution NM Rspectroscopy and J.Auld for technical assistance with high resolution mass spectrometry.
文摘The concept of“robust dynamics”describes the incorporation of mechanically interlocked molecules(MIMs)into metal-organic framework(MOF)materials such that large amplitude motions(e.g.,rotation or translation of a macrocycle)can occur inside the free volume pore of the MOF.To aid in the preparation of such materials,reticular synthesis was used herein to design rigid molecular building blocks with predetermined ordered structures starting from the well-known MOF NOTT-101.New linkers were synthesized that have a T-shape,based on a triphenylene tetra-carboxylate strut,and their incorporation into Cu(II)-based MOFs was investigated.The single-crystal structures of three new MOFs,UWCM-12(fof),β-UWCM-13(loz),UWCM-14(lil),with naked T-shaped linkers were determined;β-UWCM-13 is the first reported example of the loz topology.A fourth MOF,UWDM-14(lil)is analogous to UWCM-14(lil)but contains a[2]rotaxane linker.Variable-temperature,^(2)H solid-state NMR was used to probe the dynamics of a 24-membered macrocycle threaded onto the MOF skeleton.
基金Project supported by the National Natural Science Foundation of China(Nos.12202257,12072184,12002197)。
文摘Inspired by brick-and-mortar architectures and suture interfaces,we propose a design of bioinspired nacre-like materials with interlocking sutures to improve the toughness of brittle materials.Laser-engraved glass interlockers are laminated with soft interlayers in a staggered arrangement,and the fundamental mechanical properties of the structure are investigated through experiments and numerical modeling.It is found that the tensile performance,such as the strength and toughness,is strongly affected by the interlocking angle and suture line spacing.The geometric interlocking originated from suture interfaces as well as tablet sliding arising from the staggered arrangement of interlockers cooperatively contribute to enhancing the strength and toughness of this bioinspired design.Additionally,the finite element modeling shows the interfacial failure and plastic deformation,revealing the interplay of the geometric interlocking mechanism and the sliding mechanism.This novel bioinspired design paves a new path for fabrication of structural materials combining high stiffness,high strength,and enhanced toughness.
基金supported by the National Research Foundation of Korea(NRF)Grant(RS-2024-00343512,RS-2024-00416938).
文摘Metallic nanowires have served as novel materials for soft electronics due to their outstanding mechanical compliance and electrical properties.However,weak adhesion and low mechanical robustness of nanowire networks to substrates significantly undermine their reliability,necessitating the use of an insulating protective layer,which greatly limits their utility.Herein,we present a versatile and generalized laser-based process that simultaneously achieves strong adhesion and mechanical robustness of nanowire networks on diverse substrates without the need for a protective layer.In this method,the laser-induced photothermal energy at the interface between the nanowire network and the substrate facilitates the interpenetration of the nanowire network and the polymer matrix,resulting in mechanical interlocking through percolation.This mechanism is broadly applicable across different metallic nanowires and thermoplastic substrates,significantly enhancing its universality in diverse applications.Thereby,we demonstrated the mechanical robustness of nanowires in reusable wearable physiological sensors on the skin without compromising the performance of the sensor.Furthermore,enhanced robustness and electrical conductivity by the laser-induced interlocking enables a stable functionalization of conducting polymers in a wet environment,broadening its application into various electrochemical devices.
基金funding support from the National Natural Science Foundation of China(NSFC,Grant No.51428902)the China Scholarship Council(CSC,Grant No.202306270120).
文摘Brittle rock has the mechanical characteristics of a high ratio of uniaxial compressive strength to tensilestrength, brittle-ductile transition, and so on. The mineral meso-structure of brittle rock shows theinterlocking behavior and there are some microcracks between the mineral grains, so it is difficult toanalyze the mechanical characteristics accurately with a regular constitutive model. The previous numericalmodels have some limitations when applied to brittle rock, that they cannot provide sufficientinternal interlocking and are incapable of considering the microcracks. These limitations are addressedby using the updated flat-joint contact model to join notional polygonal particles with an initial gap andincreasing the particle coordination number by adding flat-joint contacts to more particles that arewithin some non-zero distance of one another via the range coefficient contact identification method. Acomparison of experimental and numerical results confirms that the updated flat-jointed model providesa good match with the mechanical properties of brittle rock. In this paper, we investigate the influence ofmineral meso-structure (micro-cracks, range coefficient, and radius multiplier) on the meso-mechanicalproperties of Jinping dolomitic marble via the updated flat-joint contact model under direct-tension testsand compression tests. It is found that the updated model can reproduce the microstructure effect ofbrittle rock and can better simulate the mechanical characteristics of the brittle rock than conventionalmodels, such as high strength ratio, brittle-ductile transition, initial nonlinearity, and different modulusin compression and tension.
基金Projects(51878103,52208370)supported by the National Natural Science Foundation of ChinaProject(cstc2020jcyjcxtt X0003)supported by the Innovation Group Science Foundation of the Natural Science Foundation of Chongqing,ChinaProject(2022CDJQY-012)supported by the Fundamental Research Funds for the Central Universities,China。
文摘To understand the specific behaviors of coastal coral sand slope foundations,discrete element method(DEM)was employed to examine the effect of breakable particle corners on the performance of coral sand slope foundations under a strip footing,from macro to micro scales.The results demonstrate that the bearing characteristics of coral sand slope foundations can be successfully modeled by utilizing breakable corner particles in simulations.The dual effects of interlocking and breakage of corners well explained the specific shallower load transmission and narrower shear stress zones in breakable corner particle slopes.Additionally,the study revealed the significant influence of breakable corners on soil behaviors on slopes.Furthermore,progressive corner breakage within slip bands was successfully identified as the underling mechanism in determining the unique bearing characteristics and the distinct failure patterns of breakable corner particle slopes.This study provides a new perspective to clarify the behaviors of slope foundations composed of breakable corner particle materials.
基金supported by the National Natural Science Foundation of China(grant no.22071079 for M.W.)Guangdong Natural Science Foundation(grant no.2019A1515011358 for Z.Z.)Science and Technology Research Project of Guangzhou(grant no.202002030257 for Z.Z).
文摘Mechanically interlocked molecules(MIMs)and host–vip chemistry have received great attention in the past few decades.However,it remains challenging to design architectures with mechanically interlocked features and construct cavities for vip molecule recognition using similar building blocks.In this study,we designed and constructed a series of novel twisted supramolecular structures by assembling various multitopic terpyridine(tpy)ligands with the same diameter and Zn(II)ions.The obtained complexes exhibited evolutional architectures and showed distinctively different space-constraint effects.Specifically,the assembled dimer SA,SB,and SBH displayed mechanically interlocked phenomena,including[2]catenane and[3]catenane,with an increase in concentration.However,no interlocked structures were observed in complexes SC and SCH constructed by hexatopic tpy ligands due to the significant space constraints.The single-crystal data of complex SCH further proved significant space constraints and illustrated the formation of a relatively closed cavity,which showed excellent host–vip properties for different calixarenes,especially high affinity for calix[6]arene.
基金supported by the National Natural Science Foundation of China(No.22001087)supported by Fundamental Research Funds for the Central Universities(No.2020kfy XJJS013)Interdisciplinary Research Program of HUST(No.2023JCYJ013)。
文摘Supramolecular polymers,as a type of dynamic polymers,are subordinate to the interdisciplinary field of polymer chemistry and supramolecular chemistry,whose development has greatly promoted the prosperity of new materials.Notably,molecular weight is one of the most important parameters of supramolecular polymers,which affects the physical/chemical properties and processing applications of materials.Developing new methods for characterizing the molecular weight of supramolecular polymers is crucial for advancing the development of supramolecular polymers.In this review,we elaborate and summarize three strategies for characterizing the molecular weight of supramolecular polymers that recently reported by our research group according to the characteristics of supramolecular polymers,including(1)the molecular weight distinction corresponding to variable fluorescence colors,(2)matching different molecular weights with different fluorescence lifetime,(3)transforming supramolecular polymers into mechanically interlocked polymers or covalent polymers.Besides,we also discuss the limitations of current methods for characterizing supramolecular polymers.We hope that this review can promote the development of supramolecular polymers and significantly inspire to exploit new methods to characterizing molecular weight of supramolecular polymers.
基金financially supported by the National Natural Science Foundation of China(Nos.22001214,21662031,21661028,22061039)the Science Fund for Distinguished Young Scholars of Gansu Province(No.22JR5RA131)+3 种基金the Longyuan Innovation and Entrepreneurship Talent Project of Gansu Provincethe Major Project Cultivation Program of Northwest Normal University(No.NWNU-LKZD2022-01)the Top Leading Talents Project of Gansu Province,the Key R&D Program of Gansu Province(No.21YF5GA066)Gansu Province College Industry Support Plan Project(No.2022CYZC-18)。
文摘Oligo[n]rotaxanes are one of the most extensively studied categories of mechanically bonded macromolecules.In this study,a supramolecular oligo[2]rotaxane is successfully constructed driven by platinum(Ⅱ)metallacycle and pillar[5]arene-based host–vip interactions in an orthogonal way.The supramolecular oligo[2]rotaxane is further applied in fabricating a light harvesting system.
基金funded by the National Natural Science Foundation of China(Grant No.52305405,52075359)the Natural Science Foundation Research Program of Shanxi Province(Grant No.202203021222121)+1 种基金the Fund for Shanxi“1331Project”Key Innovative Research Teamthe Chinese Postdoctoral Science Foundation(Grant No.2021M702544)。
文摘In this study,the cold-spraying process was utilized to deposit Al particles onto an Al slab,an Mg slab,and both Al and Mg slabs to form an ultra-thin interlayer,and then the clad slabs were rolled at 400℃,developing three roll-bonding processes:the roll-bonding process with cold-sprayed Al powder on the Al slab(CS-Al),the roll-bonding process with cold-sprayed Al powder on the Mg slab(CS-Mg),and the rollbonding process with cold-sprayed Al powder on both the Al slab and the Mg slab(CS-Both).The effects of three different cold-sprayed Al particle interlayer processes on the mechanical properties of rolled Mg/Al clad plates were investigated to improve the mechanical properties.The microstructure,texture evolution,intermetallic compound formation,mechanical properties,and mechanisms involved in the Mg/Al clad plate rolling were systematically investigated.The results showed that the pre-bonding between the particles and the substrates through coldspraying had a significant impact on the bonding strength of the Mg/Al clad plates,and the CS-Both process can increase the average shear strength of the Mg/Al clad plates to 49.24 MPa at a medium reduction rate of 37.5%,2.5 times that of the conventional rolling process.The CS-Both process constructed more evident dual microscopic three-dimensional interfaces and promoted more thorough atomic diffusion at the interface through the double-sided cold-spraying process.Meanwhile,the dual cold-sprayed Al coatings on both the Mg slab and Al slab underwent dynamic recrystallization during rolling to form a homogeneous unit with no additional coating interfaces.Fine grain strengthening and dislocation strengthening were judged to be important mechanisms for improving the mechanical performance of the interfacial layer.
基金financially supported by the National Natural Science Foundation of China(No.22001066)the Natural Science Foundation of Hunan Province(Nos.2021JJ40049 and 2022JJ20007)+3 种基金the Science and Technology Innovation Program of Hunan Province(No.2022RC1115)J.Du acknowledges the Science and Technology Project of Hebei Education Department(No.QN2023049)Science Foundation of Hebei Normal University(No.L2023B51)TianHe-2(LvLiang,China)Cloud Computing Center for support。
文摘A bottleneck in biomimetic synthesis consists in the full copy of,for example,the hierarchical structure of proteins directed by weak interactions.By contrast with covalent bonds bearing definite orientation and high stability,weak intermolecular forces within a continuous dynamic equilibrium can be hardly tamed for molecular design.In this endeavor,a ligand-dominated strategy that embodies tunable electrostatic repulsion andπ···πstacking was first employed to shape polyoxovanadate-based metal-organic polyhedra(VMOPs).Structural evolution involving transformation,interlock,and discovery of an unprecedented prototype of the Star of David was hence achievable.Not only as a handy tool for the primary structural control over VMOPs,these weak forces allow for an advanced management on the spatial distribution of such manmade macromolecules as well as the associated physicochemical behaviors,representing an ideal model for simulating and interpreting the conformation-function relationship of proteins.
