2,3-Dichloro-5,6-dicyano-1,4-benzoquinone (DDQ) is a stoichiometric oxidant that is frequently used in traditional organic synthesis. Recently, the rapid development of organic electrochemistry has led to new advancem...2,3-Dichloro-5,6-dicyano-1,4-benzoquinone (DDQ) is a stoichiometric oxidant that is frequently used in traditional organic synthesis. Recently, the rapid development of organic electrochemistry has led to new advancements in DDQ-catalyzed C—H bonds functionalization. Moreover, the challenging C—H functionalization of electron-deficient arenes has been achieved through the merger of electrochemical DDQ catalysis and photoirradiation. In addition, the synthetic utility of electrophotochemical DDQ catalysis was further demonstrated by the nucleophilic aromatic substitution (SNAr) reaction of unactivated aryl fluorides. The recent developments in electro- and electrophotochemical DDQ-catalyzed C—H/C—F func- tionalizations with attention to their strategies and mechanistic insights are summarized. It is hoped that this not only deepens the understanding of this field, but also helps relevant researchers expand the application scope of DDQ catalysis.展开更多
Hydrogel scaffolds have numerous potential applications in the tissue engineering field.However,tough hydrogel scaffolds implanted in vivo are seldom reported because it is difficult to balance biocompatibility and hi...Hydrogel scaffolds have numerous potential applications in the tissue engineering field.However,tough hydrogel scaffolds implanted in vivo are seldom reported because it is difficult to balance biocompatibility and high mechanical properties.Inspired by Chinese ramen,we propose a universal fabricating method(printing-P,training-T,cross-linking-C,PTC&PCT)for tough hydrogel scaffolds to fill this gap.First,3D printing fabricates a hydrogel scaffold with desired structures(P).Then,the scaffold could have extraordinarily high mechanical properties and functional surface structure by cycle mechanical training with salting-out assistance(T).Finally,the training results are fixed by photo-cross-linking processing(C).The tough gelatin hydrogel scaffolds exhibit excellent tensile strength of 6.66 MPa(622-fold untreated)and have excellent biocompatibility.Furthermore,this scaffold possesses functional surface structures from nanometer to micron to millimeter,which can efficiently induce directional cell growth.Interestingly,this strategy can produce bionic human tissue with mechanical properties of 10 kPa-10 MPa by changing the type of salt,and many hydrogels,such as gelatin and silk,could be improved with PTC or PCT strategies.Animal experiments show that this scaffold can effectively promote the new generation of muscle fibers,blood vessels,and nerves within 4 weeks,prompting the rapid regeneration of large-volume muscle loss injuries.展开更多
Listeria monocytogenes(LM)is a dangerous foodborne pathogen for humans.One emerging and validated method of indirectly assessing LM in food is detecting 3-hydroxy-2-butanone(3H2B)gas.In this study,the synthesis of 3-(...Listeria monocytogenes(LM)is a dangerous foodborne pathogen for humans.One emerging and validated method of indirectly assessing LM in food is detecting 3-hydroxy-2-butanone(3H2B)gas.In this study,the synthesis of 3-(2-aminoethylamino)propyltrimethoxysilane(AAPTMS)functionalized hierarchical hollow TiO_(2)nanospheres was achieved via precise controlling of solvothermal reaction temperature and post-grafting route.The sensors based on as-prepared materials exhibited excellent sensitivity(480 Hz@50 ppm),low detection limit(100 ppb),and outstanding selectivity.Moreover,the evaluation of LM with high sensitivity and specificity was achieved using the sensors.Such stable three-dimensional spheres,whose distinctive hierarchical and hollow nanostructure simultaneously improved both sensitivity and response/recovery speed dramatically,were spontaneously assembled by nanosheets.Meanwhile,the moderate loadings of AAPTMS significantly improved the selectivity of sensors.Then,the gas-sensing mechanism was explored by utilizing thermodynamic investigation,Gaussian 16 software,and in situ diffuse reflectance infrared transform spectroscopy,illustrating the weak chemisorption between the-NHgroup and 3H2B molecules.These portable sensors are promising for real-time assessment of LM at room temperature,which will make a magnificent contribution to food safety.展开更多
文摘2,3-Dichloro-5,6-dicyano-1,4-benzoquinone (DDQ) is a stoichiometric oxidant that is frequently used in traditional organic synthesis. Recently, the rapid development of organic electrochemistry has led to new advancements in DDQ-catalyzed C—H bonds functionalization. Moreover, the challenging C—H functionalization of electron-deficient arenes has been achieved through the merger of electrochemical DDQ catalysis and photoirradiation. In addition, the synthetic utility of electrophotochemical DDQ catalysis was further demonstrated by the nucleophilic aromatic substitution (SNAr) reaction of unactivated aryl fluorides. The recent developments in electro- and electrophotochemical DDQ-catalyzed C—H/C—F func- tionalizations with attention to their strategies and mechanistic insights are summarized. It is hoped that this not only deepens the understanding of this field, but also helps relevant researchers expand the application scope of DDQ catalysis.
基金supported by the Innovative Research Group Project of the National Natural Science Foundation of China(T2121004)Key Programme(52235007)National Outstanding Youth Foundation of China(52325504).
文摘Hydrogel scaffolds have numerous potential applications in the tissue engineering field.However,tough hydrogel scaffolds implanted in vivo are seldom reported because it is difficult to balance biocompatibility and high mechanical properties.Inspired by Chinese ramen,we propose a universal fabricating method(printing-P,training-T,cross-linking-C,PTC&PCT)for tough hydrogel scaffolds to fill this gap.First,3D printing fabricates a hydrogel scaffold with desired structures(P).Then,the scaffold could have extraordinarily high mechanical properties and functional surface structure by cycle mechanical training with salting-out assistance(T).Finally,the training results are fixed by photo-cross-linking processing(C).The tough gelatin hydrogel scaffolds exhibit excellent tensile strength of 6.66 MPa(622-fold untreated)and have excellent biocompatibility.Furthermore,this scaffold possesses functional surface structures from nanometer to micron to millimeter,which can efficiently induce directional cell growth.Interestingly,this strategy can produce bionic human tissue with mechanical properties of 10 kPa-10 MPa by changing the type of salt,and many hydrogels,such as gelatin and silk,could be improved with PTC or PCT strategies.Animal experiments show that this scaffold can effectively promote the new generation of muscle fibers,blood vessels,and nerves within 4 weeks,prompting the rapid regeneration of large-volume muscle loss injuries.
基金supported by the National Natural Science Foundation of China(No.32272399)the Shanghai Natural Science Foundation(No.21ZR1427500).
文摘Listeria monocytogenes(LM)is a dangerous foodborne pathogen for humans.One emerging and validated method of indirectly assessing LM in food is detecting 3-hydroxy-2-butanone(3H2B)gas.In this study,the synthesis of 3-(2-aminoethylamino)propyltrimethoxysilane(AAPTMS)functionalized hierarchical hollow TiO_(2)nanospheres was achieved via precise controlling of solvothermal reaction temperature and post-grafting route.The sensors based on as-prepared materials exhibited excellent sensitivity(480 Hz@50 ppm),low detection limit(100 ppb),and outstanding selectivity.Moreover,the evaluation of LM with high sensitivity and specificity was achieved using the sensors.Such stable three-dimensional spheres,whose distinctive hierarchical and hollow nanostructure simultaneously improved both sensitivity and response/recovery speed dramatically,were spontaneously assembled by nanosheets.Meanwhile,the moderate loadings of AAPTMS significantly improved the selectivity of sensors.Then,the gas-sensing mechanism was explored by utilizing thermodynamic investigation,Gaussian 16 software,and in situ diffuse reflectance infrared transform spectroscopy,illustrating the weak chemisorption between the-NHgroup and 3H2B molecules.These portable sensors are promising for real-time assessment of LM at room temperature,which will make a magnificent contribution to food safety.
