The most pronounced β-relaxation was found in the Y-based binary metallic glasses（MGs）. The correlation betweenβ-relaxation and local atomic structure was studied. The dynamic mechanical measurements were performe...The most pronounced β-relaxation was found in the Y-based binary metallic glasses（MGs）. The correlation betweenβ-relaxation and local atomic structure was studied. The dynamic mechanical measurements were performed for three chosen binary systems： Zr-, Ti-, and Y-based MGs. The experimental results show that, in each system,the larger negative enthalpy of mixing（？Hm） between the component elements makes β-relaxation become more pronounced. The less negative value of ？Hm facilitates the formation of icosahedral clusters, which have a pinning effect on the excitation of β-relaxations and correspondingly make the β-relaxation become less pronounced. These chemical effects on β-relaxations can only be compared in the same MG system, and it is not suitable for the comparison between different systems due to the different features of the major metallic elements.展开更多
Introducing small molecule-bridged hydrogen bonds(HBs)between polymer chains has been reported to effectively reduce the interchain cooperativity despite of strengthening the intermolecular interaction.Here,a systemat...Introducing small molecule-bridged hydrogen bonds(HBs)between polymer chains has been reported to effectively reduce the interchain cooperativity despite of strengthening the intermolecular interaction.Here,a systematic investigation on tuning the Johari-Goldsteinβ(βJG)relaxation by adding various low-molecular-weight phenols in poly(n-alkyl methacrylate)s is carried out to further clarify the anomalous dynamics.Given these small molecules capable of coupling the motion with pendent groups of host polymers due to forming at least two HBs per molecule,poly(n-alkyl methacrylate)mixtures exhibit rich dynamic changes in theβJG-properties andα,βJG separations.An increased loading of phenols with a small size and strong inter-HB strength(Δυi)clearly benefits for significant retardation and suppression of theβJG-relaxation,narrows theα,βJG separation and converges theβJG-peak with theα-peak,which demonstrates the alleviation of inter-chain topological constraints.However,small molecules with a relatively big size and weakΔυi are found to amplify the magnitude of theα,βJG separation of poly(butyl methacrylate),even though experimental results of changes inα-dispersion and dynamic fragility confirm a reduction of the coupling factor n in all of these hybrids.The counterintuitive phenomenon suggests that the crossover time tc in the Coupling Model is no longer a universal quantity if the inter-chain interaction of polymers is strengthened by HBs.These compelling findings shed vital insights into the HBinduced anomalous dynamics,and provide essential guidance for tailoring theβJG behavior and designing glassy polymeric materials.展开更多
基金supported by the National Basic Research Program of China(Grant No.2010CB731603)the National Natural Science Foundation of China(Grant Nos.50921091 and 51071170)
文摘The most pronounced β-relaxation was found in the Y-based binary metallic glasses（MGs）. The correlation betweenβ-relaxation and local atomic structure was studied. The dynamic mechanical measurements were performed for three chosen binary systems： Zr-, Ti-, and Y-based MGs. The experimental results show that, in each system,the larger negative enthalpy of mixing（？Hm） between the component elements makes β-relaxation become more pronounced. The less negative value of ？Hm facilitates the formation of icosahedral clusters, which have a pinning effect on the excitation of β-relaxations and correspondingly make the β-relaxation become less pronounced. These chemical effects on β-relaxations can only be compared in the same MG system, and it is not suitable for the comparison between different systems due to the different features of the major metallic elements.
基金financially supported by the National Natural Science Foundation of China(Nos.51873063 and 51373053)。
文摘Introducing small molecule-bridged hydrogen bonds(HBs)between polymer chains has been reported to effectively reduce the interchain cooperativity despite of strengthening the intermolecular interaction.Here,a systematic investigation on tuning the Johari-Goldsteinβ(βJG)relaxation by adding various low-molecular-weight phenols in poly(n-alkyl methacrylate)s is carried out to further clarify the anomalous dynamics.Given these small molecules capable of coupling the motion with pendent groups of host polymers due to forming at least two HBs per molecule,poly(n-alkyl methacrylate)mixtures exhibit rich dynamic changes in theβJG-properties andα,βJG separations.An increased loading of phenols with a small size and strong inter-HB strength(Δυi)clearly benefits for significant retardation and suppression of theβJG-relaxation,narrows theα,βJG separation and converges theβJG-peak with theα-peak,which demonstrates the alleviation of inter-chain topological constraints.However,small molecules with a relatively big size and weakΔυi are found to amplify the magnitude of theα,βJG separation of poly(butyl methacrylate),even though experimental results of changes inα-dispersion and dynamic fragility confirm a reduction of the coupling factor n in all of these hybrids.The counterintuitive phenomenon suggests that the crossover time tc in the Coupling Model is no longer a universal quantity if the inter-chain interaction of polymers is strengthened by HBs.These compelling findings shed vital insights into the HBinduced anomalous dynamics,and provide essential guidance for tailoring theβJG behavior and designing glassy polymeric materials.
基金supported by the Young Talent Program of Guangzhou University(RQ2020077)China Biosafety Research Special Program(20SWAQX40)Guangdong Major Project of Basic and Applied Basic Research,China(2020B1515120092)。
