This paper shows that for a supercritical contact process in one dimension, if the initial distribution satisfies reasonable hypothesis, then the first hitting time of certain set with anomalous small density is asymp...This paper shows that for a supercritical contact process in one dimension, if the initial distribution satisfies reasonable hypothesis, then the first hitting time of certain set with anomalous small density is asymptotically exponentially distributed. We also show the similar result for the contact process on the finite set [0, N].展开更多
The nonequilibrium composition and its formation process are critical aspects of nanoparticle production technology.Understanding the dynamics of nanoparticle formation under nonequilibrium conditions is essential.In ...The nonequilibrium composition and its formation process are critical aspects of nanoparticle production technology.Understanding the dynamics of nanoparticle formation under nonequilibrium conditions is essential.In this study,Crdoped CeO_(2) nanoparticles are synthesized via continuous-flow hydrothermal synthesis at various temperatures(300,350,400℃)with reaction times precisely controlled on the order of seconds.At the initial stage of particle formation,Cr-rich CeO_(2) particles form due to a low surface energy.Over time,the Cr content decreases as the particles relax toward the equilibrium structure.This process yields an unusual nonequilibrium composition through rapid heating and short residence times.Similar nonequilibrium compositions are also observed for other dopants,such as Fe and Eu.Continuous-flow hydrothermal synthesis thus presents an efficient method for fabricating nanomaterials with unique compositions that are unattainable using conventional batch methods.展开更多
Chemically active motion is ubiquitous in many nature and artificial systems where each unit can move directionally by converting chemical energy into kinetic energy.Since the systems are driven by activity far from e...Chemically active motion is ubiquitous in many nature and artificial systems where each unit can move directionally by converting chemical energy into kinetic energy.Since the systems are driven by activity far from equilibrium,many dynamical behaviors forbidden in equilibrium systems may be induced.Nonequilibrium dynamics of such systems is then a hot multidisciplinary topic with great challenges.Here,we review our recent theoretical advances in some fundamental problems at the single active particle level,the collective behavior level,as well as in systems where active particles act as baths.展开更多
Classical strength criteria are developed based on some empirical assumptions and have been widely used in engineering to predict material strength owing to their simplicity. In some cases, however, considerable discr...Classical strength criteria are developed based on some empirical assumptions and have been widely used in engineering to predict material strength owing to their simplicity. In some cases, however, considerable discrepancies arise between classicalstrength-criteria-based theoretical predictions and experimental results. Recently, a global nonequilibrium thermodynamics model has made important progress over classical models without resorting to any empirical assumptions. A prominent advance of this rational energy model is that it straightforwardly determines the dissipation energy density function, which is pertinent to inherent material ductility, through simple uniaxial and equi-biaxial tensions. In this study, a brief introduction of the nonequilibrium energy model was followed by systematic experimental investigation to determine the dissipation energy function and predict the material strength of pristine 316 L stainless steel-commonly used in engineering-under complex loadings. The results indicated that the strength contours predicted by the nonequilibrium energy criterion for complex loadings are consistent with the experimental results obtained for biaxial tension, implying that the nonequilibrium thermodynamics model is both reasonable and reliable. The prediction error was presumed to be induced by the anisotropy of the 316 L stainless steel sheets.展开更多
In nature, biological systems maintain their unique structures and functions by using nonequilibrium processes driven by chemical fuels. Inspired by natural systems, transient hydrogel systems based on chemical reacti...In nature, biological systems maintain their unique structures and functions by using nonequilibrium processes driven by chemical fuels. Inspired by natural systems, transient hydrogel systems based on chemical reaction networks have been developed that are in thermodynamically nonequilibrium states. The formation of dynamic covalent bonds is an effective tool for designing analogous systems. Herein, we design a transient polymer hydrogel based on fuel-mediated covalent borate ester bonds. The pH-sensitive covalent borate ester bond is formed by the reaction between polyvinyl alcohol (PVA) and boric acid (B(OH)_(3)). Sodium hydroxide (NaOH) and 1,3-propanesulfonate (PrS) are used together as the chemical fuels to temporally control the pH of the system. Meanwhile, the lifetime of the transient hydrogel can be simply controlled by adjusting the composition of the chemical fuel, and the cyclic phase transitions can also be achieved. These programmable transient hydrogels have potential applications in the fields of information transmission and fluid guidance.展开更多
Fuel-driven dissipative self-assembly,which is a well-established concept in recent years,refers to out-of-equilibrium molecular self-assembly initiated and supported by the addition of active molecules (chemical fuel...Fuel-driven dissipative self-assembly,which is a well-established concept in recent years,refers to out-of-equilibrium molecular self-assembly initiated and supported by the addition of active molecules (chemical fuel).It widely exists in nature since many temporary,active micro- or nanostructures in living bodies are generated by the dissipative self-assembly of biomolecules.Therefore,the study on dissipative self-assembly provides a good opportunity to have an insight into the microscopic mechanism of living organisms.In the meantime,dissipative assembly is thought to be a potential pathway to achieve dynamic,temporary supramolecular materials.Recently,a number of temporary materials have been developed with the aid of strategies for realizing dissipative self-assembly.Some of their properties,including solubility,stiffness,turbidity,color,or self-healing ability,change upon the addition of chemical fuel but spontaneously restore with chemical fuel consumption.The dynamic of these materials brings them various unprecedented functions.In this review,the principles of fabricating a fuel-driven temporary material are first reviewed.Subsequently,recent examples of fuel-driven temporary materials are emphatically summarized,including gels,self-erased inks,nanoreactors,self-healing materials,nanochannels,and droplets.Finally,the challenges of developing fuel-driven temporary materials and some perspectives on the function and application of such kind of materials are discussed.展开更多
Developing chemical systems capable of executing multipath nonequilibrium processes provides valuable insights into the study of multistage dissipative structures in living systems.Here,we report a nonequilibrium mult...Developing chemical systems capable of executing multipath nonequilibrium processes provides valuable insights into the study of multistage dissipative structures in living systems.Here,we report a nonequilibrium multipath evolution in a three-state supramolecular system,which is clarified by associating it with a multibranch selection structure.This system is constructed by synergistically combining an assembly-induced sol-gel transition with the color change of an acid-base indicator.Depending on the initial condition and chemical fuel composition,this system can execute five distinct nonequilibrium processes.In addition,the set of structured programming can be replayed by repeatedly introducing the chemical fuel.It is further utilized to explore the applications of information encryption and establish its universality.These findings offer novel avenues for future transient material design and may make significant contributions to systems chemistry.展开更多
基金Supported in part by the National Natural Science Foundation of China.
文摘This paper shows that for a supercritical contact process in one dimension, if the initial distribution satisfies reasonable hypothesis, then the first hitting time of certain set with anomalous small density is asymptotically exponentially distributed. We also show the similar result for the contact process on the finite set [0, N].
基金support from the Japan Science and Technology Agency(JST)[MIRAI,Grant No.JPMJMI17E4,and CREST,Grant No.JPMJCR16P3]the New Energy and Industrial Technology Development Organization of Japan(NEDO)+1 种基金JSPS KAKENHI(Grant Numbers JP16H06367,JP20K20548,and JP21H05010)the Materials Processing Science Project(Materealize,Grant No.JPMXP0219192801).
文摘The nonequilibrium composition and its formation process are critical aspects of nanoparticle production technology.Understanding the dynamics of nanoparticle formation under nonequilibrium conditions is essential.In this study,Crdoped CeO_(2) nanoparticles are synthesized via continuous-flow hydrothermal synthesis at various temperatures(300,350,400℃)with reaction times precisely controlled on the order of seconds.At the initial stage of particle formation,Cr-rich CeO_(2) particles form due to a low surface energy.Over time,the Cr content decreases as the particles relax toward the equilibrium structure.This process yields an unusual nonequilibrium composition through rapid heating and short residence times.Similar nonequilibrium compositions are also observed for other dopants,such as Fe and Eu.Continuous-flow hydrothermal synthesis thus presents an efficient method for fabricating nanomaterials with unique compositions that are unattainable using conventional batch methods.
基金MOST(2018YFA0208702)NSFC(32090044,21973085,21833007,21790350,21521001)+1 种基金Anhui Initiative in Quantum Information Technologies(AHY090200)the Fundamental Research Funds for the Central Universities(WK2340000104).
文摘Chemically active motion is ubiquitous in many nature and artificial systems where each unit can move directionally by converting chemical energy into kinetic energy.Since the systems are driven by activity far from equilibrium,many dynamical behaviors forbidden in equilibrium systems may be induced.Nonequilibrium dynamics of such systems is then a hot multidisciplinary topic with great challenges.Here,we review our recent theoretical advances in some fundamental problems at the single active particle level,the collective behavior level,as well as in systems where active particles act as baths.
基金supported by the National Natural Science Foundation of China(Grant Nos.11832019,and 12002401)the NSFC Original Exploration Project(Grant No.12150001)+1 种基金the Project of Nuclear Power Technology Innovation Center of Science Technology and Industry for National Defense(Grant No.HDLCXZX-2021-HD-035)the Guangdong International Science and Technology Cooperation Program(Grant No.2020A0505020005)。
文摘Classical strength criteria are developed based on some empirical assumptions and have been widely used in engineering to predict material strength owing to their simplicity. In some cases, however, considerable discrepancies arise between classicalstrength-criteria-based theoretical predictions and experimental results. Recently, a global nonequilibrium thermodynamics model has made important progress over classical models without resorting to any empirical assumptions. A prominent advance of this rational energy model is that it straightforwardly determines the dissipation energy density function, which is pertinent to inherent material ductility, through simple uniaxial and equi-biaxial tensions. In this study, a brief introduction of the nonequilibrium energy model was followed by systematic experimental investigation to determine the dissipation energy function and predict the material strength of pristine 316 L stainless steel-commonly used in engineering-under complex loadings. The results indicated that the strength contours predicted by the nonequilibrium energy criterion for complex loadings are consistent with the experimental results obtained for biaxial tension, implying that the nonequilibrium thermodynamics model is both reasonable and reliable. The prediction error was presumed to be induced by the anisotropy of the 316 L stainless steel sheets.
基金supported by the Shenzhen Fundamental Research Program(grant no.JCYJ20190806154814347)the National Natural Science Foundation of China(grant no.21975145).
文摘In nature, biological systems maintain their unique structures and functions by using nonequilibrium processes driven by chemical fuels. Inspired by natural systems, transient hydrogel systems based on chemical reaction networks have been developed that are in thermodynamically nonequilibrium states. The formation of dynamic covalent bonds is an effective tool for designing analogous systems. Herein, we design a transient polymer hydrogel based on fuel-mediated covalent borate ester bonds. The pH-sensitive covalent borate ester bond is formed by the reaction between polyvinyl alcohol (PVA) and boric acid (B(OH)_(3)). Sodium hydroxide (NaOH) and 1,3-propanesulfonate (PrS) are used together as the chemical fuels to temporally control the pH of the system. Meanwhile, the lifetime of the transient hydrogel can be simply controlled by adjusting the composition of the chemical fuel, and the cyclic phase transitions can also be achieved. These programmable transient hydrogels have potential applications in the fields of information transmission and fluid guidance.
基金financially supported by the Heilongjiang Provincial Natural Science Foundation of China(LH2022B009)National Natural Science Foundation of China(21704023,U20A20339).
文摘Fuel-driven dissipative self-assembly,which is a well-established concept in recent years,refers to out-of-equilibrium molecular self-assembly initiated and supported by the addition of active molecules (chemical fuel).It widely exists in nature since many temporary,active micro- or nanostructures in living bodies are generated by the dissipative self-assembly of biomolecules.Therefore,the study on dissipative self-assembly provides a good opportunity to have an insight into the microscopic mechanism of living organisms.In the meantime,dissipative assembly is thought to be a potential pathway to achieve dynamic,temporary supramolecular materials.Recently,a number of temporary materials have been developed with the aid of strategies for realizing dissipative self-assembly.Some of their properties,including solubility,stiffness,turbidity,color,or self-healing ability,change upon the addition of chemical fuel but spontaneously restore with chemical fuel consumption.The dynamic of these materials brings them various unprecedented functions.In this review,the principles of fabricating a fuel-driven temporary material are first reviewed.Subsequently,recent examples of fuel-driven temporary materials are emphatically summarized,including gels,self-erased inks,nanoreactors,self-healing materials,nanochannels,and droplets.Finally,the challenges of developing fuel-driven temporary materials and some perspectives on the function and application of such kind of materials are discussed.
基金supported by the National Natural Science Foundation of China(grant no.21975145)the Natural Science Foundation of Shandong Province(grant no.ZR2023JQ008).
文摘Developing chemical systems capable of executing multipath nonequilibrium processes provides valuable insights into the study of multistage dissipative structures in living systems.Here,we report a nonequilibrium multipath evolution in a three-state supramolecular system,which is clarified by associating it with a multibranch selection structure.This system is constructed by synergistically combining an assembly-induced sol-gel transition with the color change of an acid-base indicator.Depending on the initial condition and chemical fuel composition,this system can execute five distinct nonequilibrium processes.In addition,the set of structured programming can be replayed by repeatedly introducing the chemical fuel.It is further utilized to explore the applications of information encryption and establish its universality.These findings offer novel avenues for future transient material design and may make significant contributions to systems chemistry.
