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学者姓名：曹高娟
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Abstract ：
Although tremendous progress has been achieved in the field of hydrogen-bonded organic frameworks (HOFs), the low stability, small/none pores, and difficult functionality severely obstruct their development. Herein, a novel robust mesoporous HOF (HOF-FAFU-1) decorated with a high density of free hydroxy moieties has been designed and readily synthesized in the de novo synthesis. In HOF-FAFU-1, the planar building blocks are connected to each other by typical intermolecular carboxylate dimers to form two-dimensional (2D) layers with sql topology, which are further connected to their adjacent layers by face-to-face pi-pi interactions to obtain a three-dimensional (3D) open mesoporous framework. Owing to the high density of intermolecular hydrogen bonding and strong pi-pi interactions, HOFFAFU-1 is very stable, allowing it to retain its structure in aqueous solutions with a pH range of 1-9. Benefiting from the decorated hydroxy moieties, HOF-FAFU-1 was exploited as a fluorescent sensor for hypochlorite detection in water media by a turn-off mode, which cannot be realized by its nonhydroxy groups anchoring counterpart (HOF-TCBP). The proposed sensing system is highly efficient, validated by a very broad linear range (0-0.45 mM), fast response (15 s), and small limit of detection (LOD) (1.32 mu M). The fluorescent quenching of HOF-FAFU-1 toward hypochlorite was also investigated, mainly being ascribed to the transformation of building blocks from the fluorescent reduced state to the nonfluorescent oxidative state. This work not only demonstrates that HOFs integrated with high stability and large pores as well as high density of functional groups can be simultaneously realized by judicious design of building blocks but also conceptually elucidates that such HOFs can effectively extend the application fields of HOFs.
Keyword ：
) ) functional groups functional groups high stability high stability hydrogen-bonded organic framework (HOF) hydrogen-bonded organic framework (HOF) hypochlorite (ClO hypochlorite (ClO sensor sensor
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| GB/T 7714 | Lin, Zu-Jin , Qin, Jin-Ying , Zhan, Xiao-Ping et al. Robust Mesoporous Functional Hydrogen-Bonded Organic Framework for Hypochlorite Detection [J]. | ACS APPLIED MATERIALS & INTERFACES , 2022 , 14 (18) : 21098-21105 . |
| MLA | Lin, Zu-Jin et al. "Robust Mesoporous Functional Hydrogen-Bonded Organic Framework for Hypochlorite Detection" . | ACS APPLIED MATERIALS & INTERFACES 14 . 18 (2022) : 21098-21105 . |
| APA | Lin, Zu-Jin , Qin, Jin-Ying , Zhan, Xiao-Ping , Wu, KeChen , Cao, Gao-Juan , Chen, Banglin . Robust Mesoporous Functional Hydrogen-Bonded Organic Framework for Hypochlorite Detection . | ACS APPLIED MATERIALS & INTERFACES , 2022 , 14 (18) , 21098-21105 . |
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细菌感染特别是多重耐药菌感染是当前临床治疗所面临的一大难题，加上细菌耐药问题越来越严峻，能用的有效药和治疗手段愈发局限。金属有机框架(metal-organic frameworks, MOFs)作为一种新型的多孔晶态材料，能释放自身抗菌组分、产生活性氧和负载抗菌剂，是当前最具潜力的抗菌材料，为克服细菌感染和耐药问题带了新的突破口。本文综述了MOFs的抗菌机理、抗菌应用和潜在的细胞毒性。总结了MOFs的金属离子、有机配体和氧化应激等主要抗菌机理，重点介绍不同结构的MOFs材料及其作为抗菌剂或抗菌载体在抗菌领域的应用，最后概述了MOFs可能存在的细胞毒性，提出MOFs抗菌应用仍需克服的一些困难，并展望了这类抗菌材料今后的发展方向。
Keyword ：
多重耐药菌 多重耐药菌 抗菌应用 抗菌应用 抗菌机理 抗菌机理 细胞毒性 细胞毒性 金属有机框架 金属有机框架
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| GB/T 7714 | 詹小平 , 秦金莹 , 曹高娟 et al. 金属有机框架基抗菌材料的应用研究与展望 [J]. | 武夷科学 , 2022 , 38 (02) : 81-98 . |
| MLA | 詹小平 et al. "金属有机框架基抗菌材料的应用研究与展望" . | 武夷科学 38 . 02 (2022) : 81-98 . |
| APA | 詹小平 , 秦金莹 , 曹高娟 , 李红芳 , 林祖金 . 金属有机框架基抗菌材料的应用研究与展望 . | 武夷科学 , 2022 , 38 (02) , 81-98 . |
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It is mandatory to decontaminate Cr(vi) species from water streams due to their high toxicity. The photoreduction of hazardous Cr(vi) to nontoxic Cr(iii) is a very promising approach to control Cr(vi) pollution. Although some MOFs and their composites have been employed as photocatalysts to reduce toxic Cr(vi), their catalytic activities are always limited by inefficient visible light absorption and inferior Cr(vi) adsorption performances. Herein, cationic Ru-UiO-dmbpy(1) that is decorated with a high density of cationic charges and also embedded with catalytically competent and visible light harvesting moieties (i.e.Ru(bpy)(3)) was successfully synthesized by a sequential mix-and-match and ionization process. The presence of Ru(bpy)(3)moieties makes Ru-UiO-dmbpy(1) an excellent visible-light harvester, extending the absorption edge from 420 nm for pristine UiO-bpy to about 780 nm for Ru-UiO-bpy/Ru-UiO-dmbpy(1). Driven by ion exchange, Ru-UiO-dmbpy(1) shows a large adsorption rate constant (k(2)) of 1.33 x 10(-2)g mg(-1)min(-1)in the adsorption of Cr2O72-, which is 8.26 times that of pristine UiO-bpy and 6.27 times that of the non-ionization counterpart Ru-UiO-bpy(1) under the same adsorption conditions. The equilibrium Cr(2)O(7)(2-)uptake capacity of Ru-UiO-dmbpy(1) reaches 101.8 mg g(-1), which is about 1.98 and 1.81 times that of UiO-bpy and Ru-UiO-bpy(1), respectively. With an efficient visible light absorption ability and superior Cr(vi) adsorption performance, Ru-UiO-dmbpy(1) shows a reaction rate constant (k(1)) of 0.011 min(-1)in the photoreduction of Cr(vi) without any sacrificial agents under visible light illumination, which is much larger than those of pristine UiO-bpy (0.003 min(-1)) and its non-ionization counterpart Ru-UiO-bpy(1) (0.007 min(-1)) under the same conditions. The result unambiguously demonstrates that the Cr(vi) photoreduction activity could be largely enhanced by photosensitiser introduction and framework ionization. To further evaluate the catalytic performance of Ru-UiO-dmbpy(1), Cr(vi) reduction was also investigated in the presence of various sacrificial agents. Remarkably, a high Cr(vi) photoreduction rate of 6.4 mg(Cr(VI))g(catalyst)(-1)min(-1)was obtained when benzyl alcohol was used as a sacrificial agent, which is a record value among those reported for MOF-based photocatalysts.
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| GB/T 7714 | Zheng, He-Qi , He, Xing-Hao , Zeng, Yong-Nian et al. Boosting the photoreduction activity of Cr(vi) in metal-organic frameworks by photosensitiser incorporation and framework ionization [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2020 , 8 (33) : 17219-17228 . |
| MLA | Zheng, He-Qi et al. "Boosting the photoreduction activity of Cr(vi) in metal-organic frameworks by photosensitiser incorporation and framework ionization" . | JOURNAL OF MATERIALS CHEMISTRY A 8 . 33 (2020) : 17219-17228 . |
| APA | Zheng, He-Qi , He, Xing-Hao , Zeng, Yong-Nian , Qiu, Wei-Hua , Chen, Jin , Cao, Gao-Juan et al. Boosting the photoreduction activity of Cr(vi) in metal-organic frameworks by photosensitiser incorporation and framework ionization . | JOURNAL OF MATERIALS CHEMISTRY A , 2020 , 8 (33) , 17219-17228 . |
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Hypochlorite (ClO-) is widely used as a disinfectant, whose residue content in water should be strictly controlled due to the potential threat to human health in an inappropriate concentration. Herein, dual-emissive metal-organic frameworks with a UiO-66 prototype structure, PDA/Eu/PDA-UiO-66-NH2(x), were elegantly designed and prepared by a mixed ligand assembly and sequential post-synthesis strategy. Since blue emission is sensitive to ClO-, PDA/Eu/PDA-UiO-66-NH2(40) was selected as a model nanosensor for ratiometric and turn-on sensing of ClO- while red emission acts as a reference signal. Remarkably, PDA/Eu/PDA-UiO-66-NH2(40) shows high efficiency and specificity toward ClO- detection, as verified by a very short response time of 15 s, a wide linear range of 0.1-60 mu M, a low detection limit of 0.10 mu M, and excellent selectivity toward common competing ions. The recovery experiments show that the recoveries of spiking ClO- in tap water range from 96 to 103%. The rigidification of the coordinated H2N-BDC2- ligands should be responsible for the turn-on fluorescence of PDA/Eu/PDA-UiO-66-NH2(40). This work not only shows a highly efficient and specific fluorescent nanosensor for ClO- detection but also presents the first MOF-based fluorescent probe for turn-on and ratiometric sensing of ClO-.
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| GB/T 7714 | Zeng, Yong-Nian , Zheng, He-Qi , He, Xing-Hao et al. Dual-emissive metal-organic framework: a novel turn-on and ratiometric fluorescent sensor for highly efficient and specific detection of hypochlorite [J]. | DALTON TRANSACTIONS , 2020 , 49 (28) : 9680-9687 . |
| MLA | Zeng, Yong-Nian et al. "Dual-emissive metal-organic framework: a novel turn-on and ratiometric fluorescent sensor for highly efficient and specific detection of hypochlorite" . | DALTON TRANSACTIONS 49 . 28 (2020) : 9680-9687 . |
| APA | Zeng, Yong-Nian , Zheng, He-Qi , He, Xing-Hao , Cao, Gao-Juan , Wang, Bin , Wu, Kechen et al. Dual-emissive metal-organic framework: a novel turn-on and ratiometric fluorescent sensor for highly efficient and specific detection of hypochlorite . | DALTON TRANSACTIONS , 2020 , 49 (28) , 9680-9687 . |
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本发明属于化学分析检测技术领域，具体涉及一种定量检测次氯酸根离子的比例型荧光探针的合成方法与应用；S1：将四氯化锆、2‑氨基对苯二甲酸、吡啶‑2, 6‑二甲酸、乙酸与DMF加入反应管中，将混合液超声得到澄清溶液；再向反应管中加入超纯水，并加入磁子，在120℃油浴下加热1.5h；最后经冷却离心得到淡黄色固体；然后将该固体在甲醇中索氏提取后且60℃真空干燥得到PDA@UiO‑66‑NH2(x)；S2：将PDA@UiO‑66‑NH2(x)加入到六水合氯化铕的乙醇溶液中，混合物室温下搅拌一天，离心后固体用乙醇洗涤3次，再经干燥得到Eu/PDA@UiO‑66‑NH2(x)固体；随后，将50mg Eu/PDA@UiO‑66‑NH2(x)加入到H2PDA的甲醇溶液中，在60℃下加热12h，离心得到的固体再经甲醇索氏提取和60℃真空干燥两步得到上述荧光探针。
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| GB/T 7714 | 林祖金 , 曾勇年 , 郑和奇 et al. 一种定量检测次氯酸根离子的比例型荧光探针的合成方法与应用 : CN201911190778.2[P]. | 2019-11-28 . |
| MLA | 林祖金 et al. "一种定量检测次氯酸根离子的比例型荧光探针的合成方法与应用" : CN201911190778.2. | 2019-11-28 . |
| APA | 林祖金 , 曾勇年 , 郑和奇 , 曹高娟 . 一种定量检测次氯酸根离子的比例型荧光探针的合成方法与应用 : CN201911190778.2. | 2019-11-28 . |
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It is imperative to remove organicarsenic acids (OAAs) from water because they can convert into highly toxic inorganic arsenic compounds in natural environment via biotic and abiotic degradation routes. Herein, seven Zr-based metal-organic frameworks (Zr-MOFs) including DUT-67, UiO-66, UiO-67, MOF-808, MOF-808F, NU-1000, NU-1000B with various structures were screened for the adsorptive removal of representative OAAs including parsanilic acid (ASA) and roxarsone (ROX) in water media. Initial screening found that MOF-808 and MOF-808F have the largest adsorption capacities. Therefore, their adsorption behaviors including adsorption kinetics, isotherms, specificity and effects of pH were fully investigated. Remarkably, MOF-808F had the second largest maximum adsorption capacities of ASA (621.1 mg g(-1)) and ROX (709.2 mg g(-1)) among the reported MOF-based adsorbents. In addition, MOF-808F showed excellent selectivity and reusability and no observable drop of adsorption efficiency was found in the presence of equimolar competing ions (Cl-, OAc- or SO42-) or after three successive adsorptive runs. By contrast, MOF-808 had inferior adsorption specificity and reusability in spite of the very similar structure with MOF-808F. The structure-dependent adsorption performances can be explained by the distinct adsorptive mechanisms, which were revealed by zeta potential measurements, X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculation etc. The dominant interaction between MOF-808 and ASA was coordination interactions, while ASA adsorption over MOF-808F was governed by the synergistic effect of p-p stacking, hydrogen bonding, and electrostatic interactions. This work no only presented an excellent adsorbent (MOF-808F) toward OAAs, but also revealed the structure dependent adsorption performances/mechanisms.
Keyword ：
Coordination interaction Coordination interaction Electrostatic interaction Electrostatic interaction Hydrogen bonding Hydrogen bonding Metal organic frameworks Metal organic frameworks p-Arsanilic acid p-Arsanilic acid pi-pi Interaction pi-pi Interaction
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| GB/T 7714 | Lin, Zu-Jin , Zheng, He-Qi , Zeng, Yong-Nian et al. Effective and selective adsorption of organoarsenic acids from water over a Zr-based metal-organic framework [J]. | CHEMICAL ENGINEERING JOURNAL , 2019 , 378 . |
| MLA | Lin, Zu-Jin et al. "Effective and selective adsorption of organoarsenic acids from water over a Zr-based metal-organic framework" . | CHEMICAL ENGINEERING JOURNAL 378 (2019) . |
| APA | Lin, Zu-Jin , Zheng, He-Qi , Zeng, Yong-Nian , Wang, Yu-Lin , Chen, Jin , Cao, Gao-Juan et al. Effective and selective adsorption of organoarsenic acids from water over a Zr-based metal-organic framework . | CHEMICAL ENGINEERING JOURNAL , 2019 , 378 . |
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The detection of hypochlorite (ClO-) content in tap water is extremely important because excess amounts of hypochlorite can convert into highly toxic species and inadequate amounts of hypochlorite cannot fully kill bacteria and viruses. Although several metal-organic frameworks (MOFs) have been successfully employed as fluorescent sensors for hypochlorite detection, all these sensors are based on single emission that responds to the dose of hypochlorite. Ratiometric sensors are highly desirable, which can improve the sensitivity, accuracy, and reliability via self-calibration. Herein, a nanoscale dual-emission multivariate 5-5-Eu/BPyDC@MOF-253-NH2 was synthesized by sequential mixed-ligand self-assembly and postsynthesis method. Among the two emission bands of 5-5-Eu/BPyDC@MOF-253-NH2 the strong blue emitting derived from ligands is sensitive to hypochlorite, while the red emitting derived from Eu(III) almost keeps invariable. Therefore, 5-5-Eu/BPyDC@MOF-253-NH2 was exploited as a fluorescent ratiometric nanosensor for "on-off" sensing of hypochlorite. Notably, the proposed sensing system showed an excellent performance including fast response (within 15 s), relative high specificity, wide linear range (0.1-30 mu M), and low detection limit (0.094 mu M). Besides, the suppressed blue emitting was recovered after the addition of ascorbic acid (AA) that consumes ClO- via the redox reaction. Therefore, 5-5-Eu/BPyDC@MOF-253-NH2 was further employed as a fluorescent ratiometric nanosensor for the "on-off-on" sensing of AA. This work represents the first MOF-based fluorescent "switch" for the ratiometric sensing of hypochlorite and the second for ratiometric sensing of AA.
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| GB/T 7714 | Zeng, Yong-Nian , Zheng, He-Qi , Gu, Jia-Fang et al. Dual-Emissive Metal-Organic Framework as a Fluorescent "Switch" for Ratiometric Sensing of Hypochlorite and Ascorbic Acid [J]. | INORGANIC CHEMISTRY , 2019 , 58 (19) : 13360-13369 . |
| MLA | Zeng, Yong-Nian et al. "Dual-Emissive Metal-Organic Framework as a Fluorescent "Switch" for Ratiometric Sensing of Hypochlorite and Ascorbic Acid" . | INORGANIC CHEMISTRY 58 . 19 (2019) : 13360-13369 . |
| APA | Zeng, Yong-Nian , Zheng, He-Qi , Gu, Jia-Fang , Cao, Gao-Juan , Zhuang, Wan-E , Lin, Jian-Di et al. Dual-Emissive Metal-Organic Framework as a Fluorescent "Switch" for Ratiometric Sensing of Hypochlorite and Ascorbic Acid . | INORGANIC CHEMISTRY , 2019 , 58 (19) , 13360-13369 . |
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Noble metal nanoparticles (NPs) and their hybrids have demonstrated a strong potential to mimic the catalytic activity of natural enzymes and diminish oxidative stress. There is a large space to explore the intrinsic catalytic activity of Rh NPs with respect to reactive oxygen species (ROS) scavenging. We found that Rh NPs can quench H2O2, (OH)-O-center dot, O-2(center dot-), O-1(2) and inhibit lipid peroxidation under physiological conditions. In vitro cell experiments proved that Rh NPs have great biocompatibility and protect cells from oxidative damage caused by H2O2. This study can provide important insights that could inform future biological applications.
Keyword ：
diminishing oxidative stress diminishing oxidative stress Rh NPs Rh NPs ROS scavenging ROS scavenging
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| GB/T 7714 | Cao, Gao-Juan , Chen, Yingmei , Chen, Xiaohe et al. Intrinsic catalytic activity of rhodium nanoparticles with respect to reactive oxygen species scavenging: implication for diminishing cytotoxicity [J]. | JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH PART C-ENVIRONMENTAL CARCINOGENESIS & ECOTOXICOLOGY REVIEWS , 2019 , 37 (1) : 14-25 . |
| MLA | Cao, Gao-Juan et al. "Intrinsic catalytic activity of rhodium nanoparticles with respect to reactive oxygen species scavenging: implication for diminishing cytotoxicity" . | JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH PART C-ENVIRONMENTAL CARCINOGENESIS & ECOTOXICOLOGY REVIEWS 37 . 1 (2019) : 14-25 . |
| APA | Cao, Gao-Juan , Chen, Yingmei , Chen, Xiaohe , Weng, Peilin , Lin, Rong-Guang . Intrinsic catalytic activity of rhodium nanoparticles with respect to reactive oxygen species scavenging: implication for diminishing cytotoxicity . | JOURNAL OF ENVIRONMENTAL SCIENCE AND HEALTH PART C-ENVIRONMENTAL CARCINOGENESIS & ECOTOXICOLOGY REVIEWS , 2019 , 37 (1) , 14-25 . |
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Nitric oxide (NO) is an endogenous bioregulator with established roles in diverse fields. The difficulty in the modulation of NO release is still a significant obstacle to achieving successful clinical applications. We report herein our initial work using electron spin resonance (ESR) spectroscopy to detect NO generated from S-nitroso-N-acetylpenicillamine (SNAP) and S-nitrosoglutathione (GSNO) donors catalyzed by platinum nanoparticles (Pt NPs, 3 nm) under physiological conditions. With ESR spectroscopy coupled with spin trapping and spin labeling techniques, we identified that Pt NPs can significantly promote the generation of NO from SNAP and GSNO under physiological conditions. A classic NO colorimetric detection kit was also employed to verify that Pt NPs truly triggered the release of NO from its donors. Pt NPs can act as promising delivery vehicles for on-demand NO delivery based on time and dosage. These results, along with the detection of the resulting disulfide product, were confirmed with mass spectrometry. In addition, cellular experiments provided a convincing demonstration that the triggered release of NO from its donors by Pt NPs is efficient in killing human cancer cells in vitro. The catalytic mechanism was elucidated by X-ray photo-electron spectroscopy (XPS) and ultra-high performance liquid chromatography/high-resolution mass spectrometry (UHPLC-HRMS), which suggested that Pt-S bond formation occurs in the solution of Pt NPs and NO donors. Identification of Pt NPs capable of generating NO from S-nitrosothiols (RSNOs) is an important step in harnessing NO for investigations into its clinical applications and therapies.
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| GB/T 7714 | Cao, Gao-Juan , Fisher, Christine M. , Jiang, Xiumei et al. Platinum nanoparticles: an avenue for enhancing the release of nitric oxide from S-nitroso-N-acetylpenicillamine and S-nitrosoglutathione [J]. | NANOSCALE , 2018 , 10 (23) : 11176-11185 . |
| MLA | Cao, Gao-Juan et al. "Platinum nanoparticles: an avenue for enhancing the release of nitric oxide from S-nitroso-N-acetylpenicillamine and S-nitrosoglutathione" . | NANOSCALE 10 . 23 (2018) : 11176-11185 . |
| APA | Cao, Gao-Juan , Fisher, Christine M. , Jiang, Xiumei , Chong, Yu , Zhang, Hui , Guo, Hongyu et al. Platinum nanoparticles: an avenue for enhancing the release of nitric oxide from S-nitroso-N-acetylpenicillamine and S-nitrosoglutathione . | NANOSCALE , 2018 , 10 (23) , 11176-11185 . |
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Although important progress has been achieved for the study of noble metal-based enzyme-like catalysts, there are rare reports on the enzyme mimicking applications of ruthenium nanoparticles (Ru NPs). In this work, we investigated the horseradish peroxidase (HRP) and oxidase mimetic activity of Ru NPs. Mimicking HRP, Ru NPs could catalyze the oxidation of substrates 3,3,5,5-tetramethylbenzidine (TMB), o-phenylenediamine (OPD) and dopamine hydrochloride (DA) in the presence of exogenously added H2O2 to generate the products with blue, yellow and orange colors, respectively. We also report the first evidence that Ru NPs possess intrinsic oxidase-like activity, which could catalyze the oxidization of TMB and sodium L-ascorbate (NaA) by dissolved oxygen. The HRP-like and oxidase-like activities of Ru NPs were found to be related to the concentrations of Ru NPs. The catalytic mechanism was analyzed by electron spin resonance spectroscopy (ESR), which suggested that the enzyme mimicking activities of the Ru NPs might originate from their characteristic of accelerating electron transfer between substrates and H2O2 or O-2. Our findings offer a better understanding of enzyme-mimicking Ru NPs and should provide important insights for future applications.
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| GB/T 7714 | Cao, Gao-Juan , Jiang, Xiumei , Zhang, Hui et al. Mimicking horseradish peroxidase and oxidase using ruthenium nanomaterials [J]. | RSC ADVANCES , 2017 , 7 (82) : 52210-52217 . |
| MLA | Cao, Gao-Juan et al. "Mimicking horseradish peroxidase and oxidase using ruthenium nanomaterials" . | RSC ADVANCES 7 . 82 (2017) : 52210-52217 . |
| APA | Cao, Gao-Juan , Jiang, Xiumei , Zhang, Hui , Croley, Timothy R. , Yin, Jun-Jie . Mimicking horseradish peroxidase and oxidase using ruthenium nanomaterials . | RSC ADVANCES , 2017 , 7 (82) , 52210-52217 . |
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