Pyrazinoquinoxaline-based graphdiyne (PQ-GDY) contains a fixed number of sp-sp2hybridized carbon atoms and pyrazine-like sp2hybridized N atoms.In this paper,NH_(2)-UIO-66(Zr) on PQ-GDY substrate was successfully const...Pyrazinoquinoxaline-based graphdiyne (PQ-GDY) contains a fixed number of sp-sp2hybridized carbon atoms and pyrazine-like sp2hybridized N atoms.In this paper,NH_(2)-UIO-66(Zr) on PQ-GDY substrate was successfully constructed with the help of microwaveassisted heating.PQ-GDY surface acts as a microwave antenna under microwave irradiation to rapidly absorb microwave energy and form hot spots (hot spot effect),which facilitates the formation of well-dispersed NH2-UIO-66(Zr) with good crystallinity.Transient absorption spectra show that high hole transport property of PQ-GDY can accelerate the migration of photogenerated holes from NH2-UIO-66(Zr) to PQ-GDY and greatly reduce the recombination rate of photogenerated electrons and holes due to the strong interaction between PQ-GDY and NH2-UIO-66(Zr).Under visible light (λ≥420 nm),PQ-GDY@NH_(2)-UIO-66(Zr) shows high photocatalytic stability and high NO_(x)removal rate up to 74%,which is 44% higher than that of primitive NH_(2)-UIO-66(Zr).At the same time,it inhibits the formation of toxic byproducts (NO2) and limits its concentration to a low level.展开更多
Despite rapid advances in fluorescence detectors over the past decade,the development of a highly stable,sensitive,and selective fluorescence platform for molecular recognition remains a considerable challenge.Here we...Despite rapid advances in fluorescence detectors over the past decade,the development of a highly stable,sensitive,and selective fluorescence platform for molecular recognition remains a considerable challenge.Here we report a stable carbazole-based sp2 carbon fluorescence covalent organic framework(COF)nanosheet,termed a JUC-557 nanosheet.Owing to the synergistic effect of aggregation-induced emission-and aggregation-caused quenching-based chromophores,the architecture of the JUC-577 shows high absolute quantum yields(up to 23.0%)in the solid state and when dispersed in various solvents as well as excellent sensing performance toward specific analytes,such as iodine(Ka:2.10×10^(5)M−1 and LOD:302 ppb),2,4,6-trinitrotoluene(Ka:4.38×10^(5)M−1 and LOD:129 ppb),and especially nitrobenzene(Ka:6.18×10^(6)M−1 and LOD:5 ppb)that is superior to that of fluorescence detection materials reported so far.Furthermore,the JUC-557 nanosheet preserves strong luminescence and sensitive recognition,even under harsh conditions,and allows trace detection of various analytes via a handheld UV lamp.These findings pave the way for developing stable ultrathin COF nanomaterials for highly sensitive and selective molecular detection.展开更多
基金supported by the National Natural Science Foundation of China (Nos. 22022608, 21876112, 21876113, 22176127, 21261140333 and 92034301)National Key Research and Development Program of China (No. 2020YFA0211004)+2 种基金the Shanghai Engineering Research Center of Green Energy Chemical Engineering (No. 18DZ2254200)“111” Innovation and Talent Recruitment Base on Photochemical and Energy Materials (No. D18020)Shanghai Government (Nos. 22010503400 and 18SG41)。
文摘Pyrazinoquinoxaline-based graphdiyne (PQ-GDY) contains a fixed number of sp-sp2hybridized carbon atoms and pyrazine-like sp2hybridized N atoms.In this paper,NH_(2)-UIO-66(Zr) on PQ-GDY substrate was successfully constructed with the help of microwaveassisted heating.PQ-GDY surface acts as a microwave antenna under microwave irradiation to rapidly absorb microwave energy and form hot spots (hot spot effect),which facilitates the formation of well-dispersed NH2-UIO-66(Zr) with good crystallinity.Transient absorption spectra show that high hole transport property of PQ-GDY can accelerate the migration of photogenerated holes from NH2-UIO-66(Zr) to PQ-GDY and greatly reduce the recombination rate of photogenerated electrons and holes due to the strong interaction between PQ-GDY and NH2-UIO-66(Zr).Under visible light (λ≥420 nm),PQ-GDY@NH_(2)-UIO-66(Zr) shows high photocatalytic stability and high NO_(x)removal rate up to 74%,which is 44% higher than that of primitive NH_(2)-UIO-66(Zr).At the same time,it inhibits the formation of toxic byproducts (NO2) and limits its concentration to a low level.
基金supported by the National Natural Science Foundation of China(grant nos.22025504,21621001,21390394,22105082,21772123,21761142011,51502173,and 21702095)the 111 Project(grant nos.BP0719036 and B17020)+3 种基金the China Postdoctoral Science Foundation(grant nos.2020TQ0118 and 2020M681034)the program for the JLU Science and Technology Innovative Research Team,Shanghai Engineering Research Center of Green Energy Chemical Engineering(grant no.18DZ2254200)the 111 Innovation and Talent Recruitment Base on Photochemical and Energy Materials(grant no.D18020),the Shanghai Government(grant nos.21010503400 and 18JC1412900)the International Joint Laboratory of Resource Chemistry(IJLRC).
文摘Despite rapid advances in fluorescence detectors over the past decade,the development of a highly stable,sensitive,and selective fluorescence platform for molecular recognition remains a considerable challenge.Here we report a stable carbazole-based sp2 carbon fluorescence covalent organic framework(COF)nanosheet,termed a JUC-557 nanosheet.Owing to the synergistic effect of aggregation-induced emission-and aggregation-caused quenching-based chromophores,the architecture of the JUC-577 shows high absolute quantum yields(up to 23.0%)in the solid state and when dispersed in various solvents as well as excellent sensing performance toward specific analytes,such as iodine(Ka:2.10×10^(5)M−1 and LOD:302 ppb),2,4,6-trinitrotoluene(Ka:4.38×10^(5)M−1 and LOD:129 ppb),and especially nitrobenzene(Ka:6.18×10^(6)M−1 and LOD:5 ppb)that is superior to that of fluorescence detection materials reported so far.Furthermore,the JUC-557 nanosheet preserves strong luminescence and sensitive recognition,even under harsh conditions,and allows trace detection of various analytes via a handheld UV lamp.These findings pave the way for developing stable ultrathin COF nanomaterials for highly sensitive and selective molecular detection.