A plastic may degrade in response to a trigger.The kinetics of degradation have long been characterized by the loss of weight and strength over time.These methods of gross characterization,however,are misleading when ...A plastic may degrade in response to a trigger.The kinetics of degradation have long been characterized by the loss of weight and strength over time.These methods of gross characterization,however,are misleading when plastic degrades heterogeneously.Here,we study heterogeneous degradation in an extreme form:the growth of a crack under the combined action of chemistry and mechanics.An applied load opens the crack,exposes the crack front to chemical attack,and causes the crack to outrun gross degradation.We studied the crack growth in polylactic acid(PLA),a polyester in which ester bonds break by hydrolysis.We cut a crack in a PLA film using scissors,tore it using an apparatus,and recorded the crack growth using a camera through a microscope.In our testing range,the crack velocity was insensitive to load but was sensitive to humidity and pH.These findings will aid the development of degradable plastics for healthcare and sustainability.展开更多
Multivariate metal-organic frameworks（MTV-MOFs） with different ratios of terephthalate（BDC） linker and amino-benzenedicarboxylate（BDC-NH2） linker were synthesized through both direct synthesis from linker mixtur...Multivariate metal-organic frameworks（MTV-MOFs） with different ratios of terephthalate（BDC） linker and amino-benzenedicarboxylate（BDC-NH2） linker were synthesized through both direct synthesis from linker mixture and linker exchange of activated single-linker MOFs. Functionality proportion was impacted by the thermodynamics during the one-pot MOF construction, resulting in preference of BDC over BDC-NH2 in the MTV-MOF, in agreement with the quantum mechanics calculations. The functionality difference also affects the thermodynamics in the linker exchange process, as indicated by the more effective linker exchange in BDC-NH2-based IRMOF-3 than in BDC-based MOF-5. Furthermore,the thermal decomposition temperatures and chemical integrity upon ambient air exposure of these MOFs with variate functionalities were investigated, and it reveals that higher proportion of BDC in the MTV-MOF crystals contribute to both higher thermal and higher chemical stabilities.展开更多
基金The work at Harvard University,USA was supported by National Science Foundation(NSF)Materials Research Science and Engineering Centers(MRSEC)(DMR-2011754)X.Yang was a visiting student at Harvard University supported by the China Scholarship Council.J.Steck acknowledges support from the NSF Graduate Research Fellowship(DGE1745303).
文摘A plastic may degrade in response to a trigger.The kinetics of degradation have long been characterized by the loss of weight and strength over time.These methods of gross characterization,however,are misleading when plastic degrades heterogeneously.Here,we study heterogeneous degradation in an extreme form:the growth of a crack under the combined action of chemistry and mechanics.An applied load opens the crack,exposes the crack front to chemical attack,and causes the crack to outrun gross degradation.We studied the crack growth in polylactic acid(PLA),a polyester in which ester bonds break by hydrolysis.We cut a crack in a PLA film using scissors,tore it using an apparatus,and recorded the crack growth using a camera through a microscope.In our testing range,the crack velocity was insensitive to load but was sensitive to humidity and pH.These findings will aid the development of degradable plastics for healthcare and sustainability.
基金supported by the "Top-Notch Students Training in Basic Disciplines" undergraduate program of Ministry of Education of China
文摘Multivariate metal-organic frameworks（MTV-MOFs） with different ratios of terephthalate（BDC） linker and amino-benzenedicarboxylate（BDC-NH2） linker were synthesized through both direct synthesis from linker mixture and linker exchange of activated single-linker MOFs. Functionality proportion was impacted by the thermodynamics during the one-pot MOF construction, resulting in preference of BDC over BDC-NH2 in the MTV-MOF, in agreement with the quantum mechanics calculations. The functionality difference also affects the thermodynamics in the linker exchange process, as indicated by the more effective linker exchange in BDC-NH2-based IRMOF-3 than in BDC-based MOF-5. Furthermore,the thermal decomposition temperatures and chemical integrity upon ambient air exposure of these MOFs with variate functionalities were investigated, and it reveals that higher proportion of BDC in the MTV-MOF crystals contribute to both higher thermal and higher chemical stabilities.
