Organic radical as a powerful tool has been extensively applied in synthetic chemistry. However, harnessing radical-mediated noncovalent interactions to fabricate soft materials remains elusive. Here we report a new c...Organic radical as a powerful tool has been extensively applied in synthetic chemistry. However, harnessing radical-mediated noncovalent interactions to fabricate soft materials remains elusive. Here we report a new category of supramolecular hydrogel system held by multiple radical-radical(polyradical) interactions, and its photosensitive cross-linking structure. A simple polyacrylamide with triarylamine(TAA)pendants is designed as the precursor. The TAA units in polymer can be converted into active TAA^(·+)radical cations with light and further associate each other via TAA^(·+)–TAA^(·+)stacking interactions to form stable supramolecular network. Temporal control of the light irradiation dictates the degree of radical stacks, thus regulating the mechanical performance of the resulting hydrogel materials on-demand. Moreover, the reversible collapse of this hydrogels can be promoted by adding radical scavenger or exerting reduction voltage.展开更多
Energy transition,and the related chemistry transition due to their strong nexus,is creating a major worldwide change in the current production system,driven initially by social and environmental pressures(cleaner pro...Energy transition,and the related chemistry transition due to their strong nexus,is creating a major worldwide change in the current production system,driven initially by social and environmental pressures(cleaner production,reduced greenhouse gas emissions),but today instead is pushed by economic(renewable energy sources are becoming progressively the more economic energy form)and geopolitical(energy security)motivations.Oil and natural gases are the building blocks of the current refinery and(petro)chemistry,but going beyond fossil fuels is the challenge associated with this transition.This has also major implications on the technologies and processes actually in use,further pushed from another emerging direction associated with the progressive change from centralized to delocalized productions,for a better link with the territory and the local resources.The combined effect of these two emerging directions determines a radical change in the energy and chemical production systems,with major technological implications.Current process technologies in the area of chemical and fuel production cannot just be adapted,they need to be fully redesigned(also in terms of concepts,materials,engineering)to address the new challenges of using renewable energy sources in delocalized productions(small‐scale production at the regional level using local resources and in strong symbiosis to other local productions).展开更多
基金supported by the National Science Fund for Distinguished Young Scholars(22125804)the National Natural Science Foundation of China(22078155)the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions。
基金fund support of the National Natural Science Foundation of China (Nos. 21674022 and 51703034)the National Defense Science and Technology Innovation Zone (No. 163 Program)the Shanghai Rising-Star Program (No. 19QA1400700)。
文摘Organic radical as a powerful tool has been extensively applied in synthetic chemistry. However, harnessing radical-mediated noncovalent interactions to fabricate soft materials remains elusive. Here we report a new category of supramolecular hydrogel system held by multiple radical-radical(polyradical) interactions, and its photosensitive cross-linking structure. A simple polyacrylamide with triarylamine(TAA)pendants is designed as the precursor. The TAA units in polymer can be converted into active TAA^(·+)radical cations with light and further associate each other via TAA^(·+)–TAA^(·+)stacking interactions to form stable supramolecular network. Temporal control of the light irradiation dictates the degree of radical stacks, thus regulating the mechanical performance of the resulting hydrogel materials on-demand. Moreover, the reversible collapse of this hydrogels can be promoted by adding radical scavenger or exerting reduction voltage.
文摘Energy transition,and the related chemistry transition due to their strong nexus,is creating a major worldwide change in the current production system,driven initially by social and environmental pressures(cleaner production,reduced greenhouse gas emissions),but today instead is pushed by economic(renewable energy sources are becoming progressively the more economic energy form)and geopolitical(energy security)motivations.Oil and natural gases are the building blocks of the current refinery and(petro)chemistry,but going beyond fossil fuels is the challenge associated with this transition.This has also major implications on the technologies and processes actually in use,further pushed from another emerging direction associated with the progressive change from centralized to delocalized productions,for a better link with the territory and the local resources.The combined effect of these two emerging directions determines a radical change in the energy and chemical production systems,with major technological implications.Current process technologies in the area of chemical and fuel production cannot just be adapted,they need to be fully redesigned(also in terms of concepts,materials,engineering)to address the new challenges of using renewable energy sources in delocalized productions(small‐scale production at the regional level using local resources and in strong symbiosis to other local productions).
