Six new lanthanide complexes:[Ln(3,4-DEOBA)3(4,4'-DM-2,2'-bipy)]2·2C_(2)H_(5)OH,[Ln=Dy(1),Eu(2),Tb(3),Sm(4),Ho(5),Gd(6);3,4-DEOBA-=3,4-diethoxybenzoate,4,4'-DM-2,2'-bipy=4,4'-dimethyl-2,2'...Six new lanthanide complexes:[Ln(3,4-DEOBA)3(4,4'-DM-2,2'-bipy)]2·2C_(2)H_(5)OH,[Ln=Dy(1),Eu(2),Tb(3),Sm(4),Ho(5),Gd(6);3,4-DEOBA-=3,4-diethoxybenzoate,4,4'-DM-2,2'-bipy=4,4'-dimethyl-2,2'-bipyridine]were successfully synthesized by the volatilization of the solution at room temperature.The crystal structures of six complexes were determined by single-crystal X-ray diffraction technology.The results showed that the complexes all have a binuclear structure,and the structures contain free ethanol molecules.Moreover,the coordination number of the central metal of each structural unit is eight.Adjacent structural units interact with each other through hydrogen bonds and further expand to form 1D chain-like and 2D planar structures.After conducting a systematic study on the luminescence properties of complexes 1-4,their emission and excitation spectra were obtained.Experimental results indicated that the fluorescence lifetimes of complexes 2 and 3 were 0.807 and 0.845 ms,respectively.The emission spectral data of complexes 1-4 were imported into the CIE chromaticity coordinate system,and their corre sponding luminescent regions cover the yellow light,red light,green light,and orange-red light bands,respectively.Within the temperature range of 299.15-1300 K,the thermal decomposition processes of the six complexes were comprehensively analyzed by using TG-DSC/FTIR/MS technology.The hypothesis of the gradual loss of ligand groups during the decomposition process was verified by detecting the escaped gas,3D infrared spectroscopy,and ion fragment information detected by mass spectrometry.The specific decomposition path is as follows:firstly,free ethanol molecules and neutral ligands are removed,and finally,acidic ligands are released;the final product is the corresponding metal oxide.CCDC:2430420,1;2430422,2;2430419,3;2430424,4;2430421,5;2430423,6.展开更多
采用水热法成功将镁(Mg)引入ZSM-5分子筛骨架结构中,系统考察了Mg含量对分子筛孔的结构、酸性质、骨架铝(framework aluminum,Al_(F))分布及催化生物乙醇制丙烯(bioethanol to propylene,ETP)反应性能的影响。结果表明,随着Mg含量的增加...采用水热法成功将镁(Mg)引入ZSM-5分子筛骨架结构中,系统考察了Mg含量对分子筛孔的结构、酸性质、骨架铝(framework aluminum,Al_(F))分布及催化生物乙醇制丙烯(bioethanol to propylene,ETP)反应性能的影响。结果表明,随着Mg含量的增加,分子筛介孔体积显著增大,结晶度略有下降。氨气程序升温脱附(NH3-TPD)和吡啶红外(Py-IR)分析结果显示,Mg的引入有效降低了分子筛总酸量和强酸强度,同时提高了Brønsted酸的比例。固体核磁共振(^(27)Al MAS NMR)和紫外可见漫反射光谱(UV-Vis DRS)表明,Mg的引入促使Al_(F)从通道交叉处向正弦或直通道迁移,并减少了铝对(aluminum pair,Al_(pair))的形成。催化反应评价结果显示,适量Mg改性的分子筛(2-MgHZ5)表现出最优的ETP性能,丙烯选择性从改性前的ZSM-5(HZ5)的26.8%提高至29.5%,丙烯选择性维持在不低于10%的时间更是从HZ5的15 h显著延长至30 h,这归因于其适中的酸强度、丰富的介孔结构以及Al分布的优化有效抑制了芳烃循环和积碳生成,促进了烯烃-环戊二烯循环路径。展开更多
In this study,using 3,5‑di(3′,5′‑dicarboxylphenyl)‑1H‑1,2,4‑triazole(H4L)as ligands,a gadolinia‑based organic framework complex{[GdNa(L)(H_(2)O)3]·2H_(2)O}_(n)(Gd‑Na‑MOF)was successfully designed and synthesize...In this study,using 3,5‑di(3′,5′‑dicarboxylphenyl)‑1H‑1,2,4‑triazole(H4L)as ligands,a gadolinia‑based organic framework complex{[GdNa(L)(H_(2)O)3]·2H_(2)O}_(n)(Gd‑Na‑MOF)was successfully designed and synthesized by hydrothermal method.The structure and properties were systematically characterized and tested by techniques such as single‑crystal X‑ray diffraction,powder X‑ray diffraction,thermogravimetric analysis,infrared spectroscopy,and fluorescence spectroscopy.The results indicate that this complex has a unique 3D structure,excellent thermal stability,and outstanding luminescent performance.Based on its luminescent properties,a polymer‑embedding method was employed to fabricate the Gd‑Na‑MOF into a flexible,washable composite fluorescent film,Gd‑Na‑MOF@PMMA/BMA(PMMA=polymethyl methacrylate,BMA=butyl methacrylate).This fluorescent film exhibited highly sensitive recognition capability for tyramine,with a low detection limit of 1.66μmol·L^(-1).It was used for the detection of tyramine in bananas,with a recovery rate of 96.92%‑100.26%.CCDC:2466949.展开更多
文摘Six new lanthanide complexes:[Ln(3,4-DEOBA)3(4,4'-DM-2,2'-bipy)]2·2C_(2)H_(5)OH,[Ln=Dy(1),Eu(2),Tb(3),Sm(4),Ho(5),Gd(6);3,4-DEOBA-=3,4-diethoxybenzoate,4,4'-DM-2,2'-bipy=4,4'-dimethyl-2,2'-bipyridine]were successfully synthesized by the volatilization of the solution at room temperature.The crystal structures of six complexes were determined by single-crystal X-ray diffraction technology.The results showed that the complexes all have a binuclear structure,and the structures contain free ethanol molecules.Moreover,the coordination number of the central metal of each structural unit is eight.Adjacent structural units interact with each other through hydrogen bonds and further expand to form 1D chain-like and 2D planar structures.After conducting a systematic study on the luminescence properties of complexes 1-4,their emission and excitation spectra were obtained.Experimental results indicated that the fluorescence lifetimes of complexes 2 and 3 were 0.807 and 0.845 ms,respectively.The emission spectral data of complexes 1-4 were imported into the CIE chromaticity coordinate system,and their corre sponding luminescent regions cover the yellow light,red light,green light,and orange-red light bands,respectively.Within the temperature range of 299.15-1300 K,the thermal decomposition processes of the six complexes were comprehensively analyzed by using TG-DSC/FTIR/MS technology.The hypothesis of the gradual loss of ligand groups during the decomposition process was verified by detecting the escaped gas,3D infrared spectroscopy,and ion fragment information detected by mass spectrometry.The specific decomposition path is as follows:firstly,free ethanol molecules and neutral ligands are removed,and finally,acidic ligands are released;the final product is the corresponding metal oxide.CCDC:2430420,1;2430422,2;2430419,3;2430424,4;2430421,5;2430423,6.
文摘采用水热法成功将镁(Mg)引入ZSM-5分子筛骨架结构中,系统考察了Mg含量对分子筛孔的结构、酸性质、骨架铝(framework aluminum,Al_(F))分布及催化生物乙醇制丙烯(bioethanol to propylene,ETP)反应性能的影响。结果表明,随着Mg含量的增加,分子筛介孔体积显著增大,结晶度略有下降。氨气程序升温脱附(NH3-TPD)和吡啶红外(Py-IR)分析结果显示,Mg的引入有效降低了分子筛总酸量和强酸强度,同时提高了Brønsted酸的比例。固体核磁共振(^(27)Al MAS NMR)和紫外可见漫反射光谱(UV-Vis DRS)表明,Mg的引入促使Al_(F)从通道交叉处向正弦或直通道迁移,并减少了铝对(aluminum pair,Al_(pair))的形成。催化反应评价结果显示,适量Mg改性的分子筛(2-MgHZ5)表现出最优的ETP性能,丙烯选择性从改性前的ZSM-5(HZ5)的26.8%提高至29.5%,丙烯选择性维持在不低于10%的时间更是从HZ5的15 h显著延长至30 h,这归因于其适中的酸强度、丰富的介孔结构以及Al分布的优化有效抑制了芳烃循环和积碳生成,促进了烯烃-环戊二烯循环路径。
文摘In this study,using 3,5‑di(3′,5′‑dicarboxylphenyl)‑1H‑1,2,4‑triazole(H4L)as ligands,a gadolinia‑based organic framework complex{[GdNa(L)(H_(2)O)3]·2H_(2)O}_(n)(Gd‑Na‑MOF)was successfully designed and synthesized by hydrothermal method.The structure and properties were systematically characterized and tested by techniques such as single‑crystal X‑ray diffraction,powder X‑ray diffraction,thermogravimetric analysis,infrared spectroscopy,and fluorescence spectroscopy.The results indicate that this complex has a unique 3D structure,excellent thermal stability,and outstanding luminescent performance.Based on its luminescent properties,a polymer‑embedding method was employed to fabricate the Gd‑Na‑MOF into a flexible,washable composite fluorescent film,Gd‑Na‑MOF@PMMA/BMA(PMMA=polymethyl methacrylate,BMA=butyl methacrylate).This fluorescent film exhibited highly sensitive recognition capability for tyramine,with a low detection limit of 1.66μmol·L^(-1).It was used for the detection of tyramine in bananas,with a recovery rate of 96.92%‑100.26%.CCDC:2466949.
