π-Conjugated donor-acceptor-donor-acceptor-donor(D-A-D-A-D)type pyrenoviologens(PyV^(2+)),with the 2,7 positions of pyrene serving as connection bridges,were synthesized through SN2 reactions.Specifically,pyrenoviolo...π-Conjugated donor-acceptor-donor-acceptor-donor(D-A-D-A-D)type pyrenoviologens(PyV^(2+)),with the 2,7 positions of pyrene serving as connection bridges,were synthesized through SN2 reactions.Specifically,pyrenoviologen 3c was modified with a methylnaphthalene group,while 3a and 3b were modified with methyl and benzyl groups,respectively,for comparison.These pyrenoviologens exhibit reversible redox properties and strong fluorescence emission.Electrochromic devices(ECDs)were prepared using pyrenoviologens as the active materials.Notably,naphthalene-containing pyrenoviologen 3c,with its DA-D-A-D conjugated structure,possesses more stable free radicals,enabling it to maintain the radical color for a longer duration after power loss.A series of color-changing devices were successfully assembled.Due to the strong fluorescence of pyrenoviologens and the unique electron transfer effect between them and picric acid(PA),a sensor film with good selectivity and high sensitivity for PA in aqueous solution was prepared using pyrenoviologens as the fluorescent probe.Specifically,3c exhibited the highest sensitivity to PA due to its lowest energy gap.The introduction of the D-A-D-A-D structure is a strategic approach to enhancing photoelectric performance and broadening the application of viologens.展开更多
An electronic circular dichroism(ECD)-based chiroptical sensing method has been developed forβ-andγ-chiral primary amines via a C-H activation reaction.With the addition of Pd(OAc)_(2),the flexible remote chiral pri...An electronic circular dichroism(ECD)-based chiroptical sensing method has been developed forβ-andγ-chiral primary amines via a C-H activation reaction.With the addition of Pd(OAc)_(2),the flexible remote chiral primary amine fragment in the bidentate ligand intermediate was fixed to form a cyclopalladium complex,producing an intense ECD response.The correlation between the sign of Cotton effects and the absolute configuration of substrates was proposed,together with theoretical verification using timedependent density functional theory(TDDFT).Chiroptical sensing of an important drug raw material was performed to provide rapid and accurate information on the absolute optical purity.This work introduces an alternative perspective of C-H activation reaction as well as a feasible chiroptical sensing method of remote chiral amines.展开更多
多氯联苯(PCBs),是一类有机化合物,集中式生活饮用水源地地表水中多氯联苯包含PCB1016、PCB1221、PCB1232、PCB1242、PCB1248、PCB1254、PCB1260。本文采用液液萃取结合气相色谱–电子捕获检测法(LLE-GC/ECD)测定集中式生活饮用水源地...多氯联苯(PCBs),是一类有机化合物,集中式生活饮用水源地地表水中多氯联苯包含PCB1016、PCB1221、PCB1232、PCB1242、PCB1248、PCB1254、PCB1260。本文采用液液萃取结合气相色谱–电子捕获检测法(LLE-GC/ECD)测定集中式生活饮用水源地地表水中多氯联苯的含量。结果表明:该方法测定集中式生活饮用水源地地表水中多氯联苯,有很好的校正曲线(R > 0.995),取样量为1.0 L时,检出限为0.0008~0.0058 μg/L,平均加标回收率为99.5%~120.0%,相对标准偏差(n = 9)为0.6%~4.3%。本方法具有操作简便、灵敏度高和重复性好等特点,为环境监测部门开展饮用水源地多氯联苯的日常监测提供了可靠的分析方法参考。Polychlorinated biphenyls (PCBs) are a class of organic compounds. The PCBs in surface water of centralized drinking water sources include PCB1016, PCB1221, PCB1232, PCB1242, PCB1248, PCB1254, and PCB1260. This paper uses liquid-liquid extraction combined with gas chromatography-electron capture detection (LLE-GC/ECD) to determine the content of PCBs in surface water of centralized drinking water sources. The results show that this method has a good calibration curve (R > 0.995) for the determination of PCBs in surface water of centralized drinking water sources. When the sample volume is 1.0 L, the detection limit is 0.0008~0.0058 μg/L, the average spiked recovery rate is 99.5%~120.0%, and the relative standard deviation (n = 9) is 0.6%~4.3%. This method is characterized by simplicity, high sensitivity, and good repeatability, providing a reliable analytical method reference for environmental monitoring departments to conduct routine monitoring of PCBs in drinking water sources.展开更多
基金supported by the Shaanxi Province Technological Innovation Guidance Special(No.2022QFY08-01)the National Key Research and Development Program of China(No.2021YFB3200702)+5 种基金Natural Science Foundation of China(Nos.22201228,22205172,52203240 and 22175138)China Postdoctoral Science Foundation(Nos.2022M712530,2023T160506,and 2022M712497)Fundamental Research Funds for the Central Universities(No.xzy012022017)Young Talent Fund of Association for Science and Technology in Shaanxi(No.20230624)Shaanxi Province Postdoctoral Science Foundation(No.2023b SHTBZZ04)the Youth Innovation Team of Shaanxi Universities。
文摘π-Conjugated donor-acceptor-donor-acceptor-donor(D-A-D-A-D)type pyrenoviologens(PyV^(2+)),with the 2,7 positions of pyrene serving as connection bridges,were synthesized through SN2 reactions.Specifically,pyrenoviologen 3c was modified with a methylnaphthalene group,while 3a and 3b were modified with methyl and benzyl groups,respectively,for comparison.These pyrenoviologens exhibit reversible redox properties and strong fluorescence emission.Electrochromic devices(ECDs)were prepared using pyrenoviologens as the active materials.Notably,naphthalene-containing pyrenoviologen 3c,with its DA-D-A-D conjugated structure,possesses more stable free radicals,enabling it to maintain the radical color for a longer duration after power loss.A series of color-changing devices were successfully assembled.Due to the strong fluorescence of pyrenoviologens and the unique electron transfer effect between them and picric acid(PA),a sensor film with good selectivity and high sensitivity for PA in aqueous solution was prepared using pyrenoviologens as the fluorescent probe.Specifically,3c exhibited the highest sensitivity to PA due to its lowest energy gap.The introduction of the D-A-D-A-D structure is a strategic approach to enhancing photoelectric performance and broadening the application of viologens.
基金supported by the CAMS Innovation Fund for Medical Sciences(CIFMS,No.2023-I2M-2-009).
文摘An electronic circular dichroism(ECD)-based chiroptical sensing method has been developed forβ-andγ-chiral primary amines via a C-H activation reaction.With the addition of Pd(OAc)_(2),the flexible remote chiral primary amine fragment in the bidentate ligand intermediate was fixed to form a cyclopalladium complex,producing an intense ECD response.The correlation between the sign of Cotton effects and the absolute configuration of substrates was proposed,together with theoretical verification using timedependent density functional theory(TDDFT).Chiroptical sensing of an important drug raw material was performed to provide rapid and accurate information on the absolute optical purity.This work introduces an alternative perspective of C-H activation reaction as well as a feasible chiroptical sensing method of remote chiral amines.
文摘多氯联苯(PCBs),是一类有机化合物,集中式生活饮用水源地地表水中多氯联苯包含PCB1016、PCB1221、PCB1232、PCB1242、PCB1248、PCB1254、PCB1260。本文采用液液萃取结合气相色谱–电子捕获检测法(LLE-GC/ECD)测定集中式生活饮用水源地地表水中多氯联苯的含量。结果表明:该方法测定集中式生活饮用水源地地表水中多氯联苯,有很好的校正曲线(R > 0.995),取样量为1.0 L时,检出限为0.0008~0.0058 μg/L,平均加标回收率为99.5%~120.0%,相对标准偏差(n = 9)为0.6%~4.3%。本方法具有操作简便、灵敏度高和重复性好等特点,为环境监测部门开展饮用水源地多氯联苯的日常监测提供了可靠的分析方法参考。Polychlorinated biphenyls (PCBs) are a class of organic compounds. The PCBs in surface water of centralized drinking water sources include PCB1016, PCB1221, PCB1232, PCB1242, PCB1248, PCB1254, and PCB1260. This paper uses liquid-liquid extraction combined with gas chromatography-electron capture detection (LLE-GC/ECD) to determine the content of PCBs in surface water of centralized drinking water sources. The results show that this method has a good calibration curve (R > 0.995) for the determination of PCBs in surface water of centralized drinking water sources. When the sample volume is 1.0 L, the detection limit is 0.0008~0.0058 μg/L, the average spiked recovery rate is 99.5%~120.0%, and the relative standard deviation (n = 9) is 0.6%~4.3%. This method is characterized by simplicity, high sensitivity, and good repeatability, providing a reliable analytical method reference for environmental monitoring departments to conduct routine monitoring of PCBs in drinking water sources.
