18 results on '"Cheng, Rong"'
Search Results
2. Redox-active sp2-c connected metal covalent organic frameworks for selective detection and reductive separation of uranium
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Jin-Lan Liu, Zhi-Hai Peng, Jia-Xin Qi, Cheng-Rong Zhang, Zhen-Wen Zhang, Li Zhang, Ru-Ping Liang, and Jian-Ding Qiu
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Covalent organic frameworks ,Uranium ,Detection ,Adsorption ,Wastewater ,Renewable energy sources ,TJ807-830 ,Chemical technology ,TP1-1185 ,Production of electric energy or power. Powerplants. Central stations ,TK1001-1841 - Abstract
It is economically desirable to develop a material that can simultaneously detect and recover uranium. Herein, a CC-bridged two-dimensional metal-covalent organic framework (Cu-BTAN-AO MCOF) was constructed by condensation of metal single crystals with a rigid structure (Cu3(PyCA)3) and cyano monomers (BTAN) via Knoevenagel reaction for simultaneous detection and adsorption of uranium. The amidoxime group within the pore and the presence of unsaturated Cu(I) in the framework facilitate the adsorption of uranyl ions onto the amidoxime group, leading to fluorescence quenching via the photoinduced electron transfer (PET) mechanism, achieving a detection limit of as low as 167 nM uranyl ions. Furthermore, Cu-BTAN-AO demonstrates exceptional efficiency in capturing uranium from wastewater characterized by rapid kinetics and superior selectivity. It is noteworthy that Cu-BTAN-AO is the first example of simultaneous detection, adsorption and chemical reduction of uranium using metal centers and functional groups in MCOF, indicating that Cu-BTAN-AO has great potential for the detection and recovery of uranium-containing wastewater. This design strategy may also be applicable to advancing sensing and energy materials for other important metal ions.
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- 2024
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3. Regenerable, anti-biofouling covalent organic frameworks for monitoring and extraction of uranium from seawater
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Wu, Yi-Di, Cui, Wei-Rong, Zhang, Cheng-Rong, Liang, Ru-Ping, and Qiu, Jian-Ding
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- 2021
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4. Regenerable Covalent Organic Frameworks for Photo‐enhanced Uranium Adsorption from Seawater.
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Cui, Wei‐Rong, Li, Fang‐Fang, Xu, Rui‐Han, Zhang, Cheng‐Rong, Chen, Xiao‐Rong, Yan, Run‐Han, Liang, Ru‐Ping, and Qiu, Jian‐Ding
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REACTIVE oxygen species ,ADSORPTION capacity ,URANIUM ,SEAWATER ,ADSORPTION (Chemistry) ,NUCLEAR industry - Abstract
Uranium is a key resource for the development of the nuclear industry, and extracting uranium from the natural seawater is one of the most promising ways to address the shortage of uranium resources. Herein, a semiconducting covalent organic framework (named NDA‐TN‐AO) with excellent photocatalytic and photoelectric activities was synthesized. The excellent photocatalytic effect endowed NDA‐TN‐AO with a high anti‐biofouling activity by generating biotoxic reactive oxygen species and promoting photoelectrons to reduce the adsorbed UVI to insoluble UIV, thereby increasing the uranium extraction capacity. Owing to the photoinduced effect, the adsorption capacity of NDA‐TN‐AO to uranium in seawater reaches 6.07 mg g−1, which is 1.33 times of that in dark. The NDA‐TN‐AO with enhanced adsorption capacity is a promising material for extracting uranium from the natural seawater. [ABSTRACT FROM AUTHOR]
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- 2020
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5. Efficient removal of uranium under strong acid based on charge separation and protonation coupled covalent organic frameworks.
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Yi, Shun-Mo, Zhang, Cheng-Rong, Liu, Xin, Chen, Xiao-Juan, Qi, Jia-Xin, Niu, Cheng-Peng, Liu, Jin-Lan, Liang, Ru-Ping, and Qiu, Jian-Ding
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PROTON transfer reactions , *INTRAMOLECULAR charge transfer , *CHEMICAL stability , *URANIUM , *LIGHT absorption , *HYDROXYL group - Abstract
[Display omitted] • A covalent organic framework (DANT-BTT) with a D-A structure was synthesized based on naphthalimide. • DANT-BTT exhibits excellent chemical stability and photocatalytic properties. • Protonated DANT-BTT with superior photocatalytic capability and higher selectivity for uranium. • DANT-BTT has excellent removal efficiency for uranium at pH 1. Efficient removal of UO 2 2+ from radioactive wastewater under strong acid conditions remains a significant challenge due to the competition of excess H+ for adsorption and reduction sites. Here, covalent organic framework with complete charge separation and protonation properties (DANT-BTT) was synthesized for efficient removal of UO 2 2+ under strong acids. The DANT-BTT with strong electron-deficient naphthalimide significantly extended light absorption and enhanced intramolecular charge transfer, which significantly improve the separation efficiency of electrons and holes. Additionally, the auxiliary coordination of hydroxyl groups after protonation provides unparalleled selectivity for UO 2 2+ in strong acids, effectively preventing the competition of H+ for adsorption sites. Protonation of nitrogen atoms and ketones also extends light absorption and store electrons, further enhancing the photocatalytic performance of DANT-BTT. Consequently, DANT-BTT can achieve 71 % photoreduction UO 2 2+ efficiency (pH 1) after 60 min irradiation, where dark adsorption accounts for 43 %. This work provides a strategy for the efficient reduction of U(VI) under strong acids. [ABSTRACT FROM AUTHOR]
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- 2023
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6. Flexible three-dimensional covalent organic frameworks for ultra-fast and selective extraction of uranium via hydrophilic engineering.
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Chen, Xiao-Juan, Zhang, Cheng-Rong, Liu, Xin, Qi, Jia-Xin, Jiang, Wei, Yi, Shun-Mo, Niu, Cheng-Peng, Cai, Yuan-Jun, Liang, Ru-Ping, and Qiu, Jian-Ding
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URANIUM , *CHEMICAL stability , *POROSITY , *ADSORPTION capacity , *UNIFORM spaces , *SORBENTS - Abstract
It has been considered challenging to develop ideal adsorbents for efficient and lower adsorption time uranium extraction, especially 3D covalent organic frameworks with interpenetrating topologies and tunable porous structures. Here, a "soft" three-dimensional (3D) covalent organic framework (TAM-DHBD) with a fivefold interpenetrating structure is prepared as a novel porous platform for the efficient extraction of radioactive uranium. The resultant TAM-DHBD appears exceptional crystallinity, prominent porosity and excellent chemical stability. Based on the strong mutual coordination between phenolic-hydroxyl/imine-N on the main chain and uranium, TAM-DHBD can effectively avert the competition of other ions, showing high selectivity for uranium extraction. Impressively, the 3D ultra-hydrophilic transport channels and multi-directional uniform pore structure of TAM-DHBD lay the foundation for the ultra-high-speed diffusion of uranium (the adsorption equilibrium can be reached within 60 min under a high-concentration environment). Furthermore, the utilization of lightweight structure not only increases the adsorption site density, but renders the adsorption process flexible, achieving a breakthrough adsorption capacity of 1263.8 mg g-1. This work not only highlights new opportunities for designing microporous 3D COFs, but paves the way for the practical application of 3D COFs for uranium adsorption. [Display omitted] • A three-dimensional covalent organic framework (TAM-DHBD) is prepared for extraction of uranium. • TAM-DHBD can effectively avoid the competition of other ions, showing high selectivity to uranium. • TAM-DHBD possesses superhydrophilic transport channels and multidirectional uniform pore structure. • The lightweight structure increases adsorption site density and makes adsorption process flexible. • TAM-DHBD achieved a breakthrough adsorption capacity of 1263.8 mg g-1. [ABSTRACT FROM AUTHOR]
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- 2023
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7. Ionic liquid modified covalent organic frameworks for efficient detection and adsorption of ReO4–/TcO4–.
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Yi, Shun-Mo, Zhang, Cheng-Rong, Jiang, Wei, Liu, Xin, Niu, Cheng-Peng, Qi, Jia-Xin, Chen, Xiao-Juan, Liang, Ru-Ping, and Qiu, Jian-Ding
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IONIC liquids ,INTRAMOLECULAR charge transfer ,ADSORPTION kinetics ,CHEMICAL stability ,COVALENT bonds ,CHARGE transfer - Abstract
The tanglesome environments of high radiation and strong acid or alkali lead to the currently reported materials used to detect ReO 4
− (surrogate for99 TcO 4− with nonradioactive) far from meeting the requirements of practical applications. Here, we report the ionic liquids modified covalent organic frameworks (ionic COFs) were applied to detect and adsorb ReO 4− for the first time. Ionic COFs are obtained by grafting ionic liquids on the channel walls of COFs. Not only the ionic liquids enhance the fluorescence performance of COFs by expanding the conjugated structure, but bring high-efficiency fluorescence response to ReO 4− through introducing specific recognition sites with the detection limit as low as 1.04 μM. Benefiting from the intramolecular charge transfer conducted by hydrogen bond and clear hydrophobic framework, ionic COFs shows ultrafast fluorescence response (2 s) and excellent selectivity to ReO 4− , which is quite suitable for on-site and real-time monitoring of ReO 4− . Meanwhile, abundant ionic liquids and regular pore channels provide ionic COFs with admirable adsorption kinetics (within 3 min) and superior adsorption capacity (439 mg/g). In other words, the strong-bond ionic COFs overcome the weak stability of other fluorescence sensors of ReO 4− and propose a new strategy for ReO 4− detection, which offer huge potential to detect and remove99 TcO 4− /ReO 4− under realistic conditions. [Display omitted] • The first example of covalent organic framework (COF) for detection of ReO 4– /TcO 4– . • Combination of the advantages of COF and ionic liquid for selectively identifying ReO 4– /TcO 4– . • Ionic COF exhibits ultra-trace detection limit and excellent recovery capacity of ReO 4– /TcO 4– . • Benefiting from the extraordinary strength of covalent bonds, ionic COF has outstanding chemical stability and reusability. [ABSTRACT FROM AUTHOR]- Published
- 2022
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8. rGO-based covalent organic framework hydrogel for synergistically enhance uranium capture capacity through photothermal desalination.
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Zhang, Cheng-Rong, Cui, Wei-Rong, Niu, Cheng-Peng, Yi, Shun-Mo, Liang, Ru-Ping, Qi, Jia-Xin, Chen, Xiao-Juan, Jiang, Wei, Zhang, Li, and Qiu, Jian-Ding
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HYDROGELS , *URANIUM , *SALINE water conversion , *SOLAR stills , *PHOTOCATALYSTS , *HONEYCOMB structures , *NUCLEAR energy , *PHOTOTHERMAL conversion - Abstract
We proposed a strategy to synergistically enhance uranium capture capacity through photothermal desalination, and prepared a COF hydrogel (KTG) through a simple process for the first time. KTG with ideal broadband light absorption capacity could be used as an outstanding photothermal conversion material. Meanwhile, the built-in elastic honeycomb structure endowed the KTG with good mechanical properties and adequate water transport performance that accelerated the diffusion and mass transfer ability of uranyl. Under a simulated sunlight, the adsorption capacity, selectivity, adsorption rate and cycle capacity of uranium could be significantly improved. Moreover, benefiting from the outstanding photocatalytic performance, KTG exhibited a high anti-fouling activity against marine biological entities, thereby achieving long-term efficient uranium adsorption and solar desalination. [Display omitted] • The first example of COF hydrogel for solar desalination and uranium recovery. • COF hydrogel for synergistically enhance uranium capture through photothermal desalination. • COF hydrogel shows a high evaporation rate and exceptional uranium recovery capacity. • COF hydrogel has high anti-biofouling activity and good reusability. Capturing of uranium from the natural seawater is considered to be one of the most promising methods to meet the current demand for nuclear energy. Herein, we prepared a reduced graphene oxide-based (rGO-based) covalent organic framework hydrogel (KTG) with three-dimensional porous structure as a platform for enhancing uranium capture capacity through photothermal desalination. Under light irradiation, the KTG produces a local heat that can be used to generate steam while promoting the rapid diffusion of uranium inside the hydrogel 3D network, thereby increasing the adsorption efficiency and capacity of uranium. KTG can achieve exceptional uranium capture capacity (521.6 mg g−1) under one sun irradiation, which is 42.4% higher than that under dark conditions. In addition, excellent photocatalytic activity and mechanical properties make KTG possess high anti-biofouling activity, good reusability, and achieving continuous uranium capture and solar distillation. [ABSTRACT FROM AUTHOR]
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- 2022
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9. Rational design of covalent organic frameworks as a groundbreaking uranium capture platform through three synergistic mechanisms.
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Cui, Wei-Rong, Zhang, Cheng-Rong, Xu, Rui-Han, Chen, Xiao-Rong, Jiang, Wei, Li, Ya-Jie, Liang, Ru-Ping, Zhang, Li, and Qiu, Jian-Ding
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PHOTOREDUCTION , *PHOTOCATALYSTS , *CHEMICAL reduction , *ADSORPTION kinetics , *ADSORPTION capacity , *TRIAZINE derivatives , *HYDROXYL group , *URANIUM - Abstract
We report the first example of covalent organic framework (DHBD-TMT) linked by unsubstituted olefin-linkages for selective loading, chemical reduction and photocatalytic reduction of uranium. The unique structures of DHBD-TMT possess all the characteristics to be well suited as a capture platform for selective ligand complexation, efficient chemical reduction and photocatalytic reduction of uranium, thus exhibiting a groundbreaking uranium capture capacity (2640.8 mg g-1). [Display omitted] • Covalent organic framework (DHBD-TMT) as a uranium adsorbent through three synergistic mechanisms. • This is the first example of covalent organic framework for selective adsorption, chemical reduction and photocatalytic reduction of uranium. • DHBD-TMT is very suitable as a capture platform for selective ligand complexation, efficient chemical reduction and photocatalytic reduction of uranium. • DHBD-TMT exhibited a groundbreaking uranium capture capacity. Herein, we report the first example of covalent organic framework (DHBD-TMT) linked by unsubstituted olefin-linkages for selective loading, chemical reduction and photocatalytic reduction of uranium. The unique structures of DHBD-TMT possess all the characteristics to be well suited as a capture platform for selective ligand complexation, efficient chemical reduction and photocatalytic reduction of uranium, thus exhibiting a groundbreaking uranium capture capacity (2640.8 mg g-1). In the dark, DHBD-TMT can effectively adsorb uranium through the hydroxyl groups laced on the skeleton and reduce UVI to UIV in situ, leading to a higher adsorption capacity and selectivity of uranium. At the same time, the synergistic effect of the hydroquinone and triazine units in the extended π-conjugated skeleton significantly improve the photocatalytic activity of DHBD-TMT, and an additional UVI photocatalytic reduction mechanism can occur under visible light irradiation, allowing significantly higher the capacity and faster adsorption kinetics. [ABSTRACT FROM AUTHOR]
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- 2021
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10. SnS2-covalent organic framework Z-scheme van der Waals heterojunction for enhanced photocatalytic reduction of uranium (VI) in rare earth tailings wastewater.
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Liu, Xin, Bi, Rui-Xiang, Zhang, Cheng-Rong, Luo, Qiu-Xia, Liang, Ru-Ping, and Qiu, Jian-Ding
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RARE earth metals , *PHOTOREDUCTION , *HETEROJUNCTIONS , *URANIUM , *SEWAGE , *ELECTRON transport , *SILVER phosphates , *PHOTOELECTRIC effect - Abstract
[Display omitted] • The SnS 2 -covalent organic framework van der Waals heterojunction (SnS 2 COF) was constructed. • With good photoelectric properties, SnS 2 COF can realize separation and transfer of electron-hole. • The electron flow path of heterojunction conforms to Z-scheme by experimental study and theoretical calculation. • SnS 2 COF can effectively reduce and remove U (VI) from rare earth tailings wastewater under UV/Vis light. Uranium removal by photocatalytic reduction is one of the most promising methods to reduce radioactive contamination in wastewater. Herein, a Z-scheme van der Waals heterojunction photocatalyst (SnS 2 COF) was synthesized in situ by combining covalent organic frameworks (COF) with semiconductor (SnS 2) for U (VI) reduction in rare earth tailings wastewater. The synthesis method of van der Waals heterojunction is simple and solves the problem of no hanging bond in composite components. In this heterojunction, large areas of van der Waals interaction form high-speed electron transport channels. In addition, it is deduced that SnS 2 COF fits the Z-scheme heterojunction electron transport mode through the theoretical calculation of the ground state and excited state electron density difference and the related band structure. Under the photoexcitation, the direction of electron flow is reversed, which further promotes the separation of the photogenerated electron (e−)-hole (h+) under the action of the built-in electric field, maintains the high reducibility of the conduction band, and avoids the photocorrosion of SnS 2. Compared with inorganic-inorganic heterojunction, SnS 2 COF has a wider light absorption range, more active sites, and higher e−-h+ separation and transfer efficiency. Therefore, it had a higher U (VI) reduction removal capacity, up to 1123.3 mg g−1, far surpassing the SnS 2 and COF counterparts under ultraviolet/visible light. And the U (VI) removal rate reached 98.5 % in rare earth tailings wastewater. The design concept of organic–inorganic heterojunction materials provides an alternative strategy for improving the photocatalytic performance. [ABSTRACT FROM AUTHOR]
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- 2023
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11. sp2-c linked Cu-based metal-covalent organic framework for chemical and photocatalysis synergistic reduction of uranium.
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Liu, Jin-Lan, Lin, Mu-Xiang, Huang, Juan, Zhang, Cheng-Rong, Qi, Jia-Xin, Cai, Yuan-Jun, Chen, Xiao-Juan, Zhang, Li, Liang, Ru-Ping, and Qiu, Jian-Ding
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URANIUM , *INTRAMOLECULAR charge transfer , *ORGANIC compounds , *METAL-organic frameworks , *PHOTOREDUCTION , *TRIAZINES - Abstract
[Display omitted] • Cu-based metal covalent organic framework (Cu-TMT) was prepared for the extraction of uranium. • Cu-TMT has unsaturated Cu centers that serve as chemical reduction sites. • Cu-TMT has excellent visible light conversion efficiency and low band gap. • Cu-TMT reduced uranium by chemical reduction and photocatalytic reduction reached 1438.8 mg g−1. The reduction of hexavalent uranium to tetravalent uranium is an effective strategy for controlling uranium contamination in wastewater. Herein, a C C bonded metal-covalent organic framework (Cu-TMT) was synthesized via the Aldol condensation reaction by using the metal cluster Cu 3 (PyCA) 3 and 2,4,6-trimethyl-1,3,5-triazine (TMT) for the chemical and photocatalytic synergistic reduction of uranium. In the Cu-TMT, the low-valent Cu in the metal clusters provides the framework with numerous distributed redox sites being capable of chemically reducing UVI. Meanwhile, the encapsulating Cu clusters in long-range ordered frameworks can provide fast transport channels for intramolecular charge transfer and effectively inhibit electron/hole complexation, making Cu-TMT suitable for photocatalytic reduction of uranium. The chemical reduction of uranium by Cu-TMT was verified under light-avoidance conditions, reaching 659.5 mg g−1. After exposure of Cu-TMT to light, the amount of reduced uranium further increases to 1438.8 mg g−1 with 98.1 % removal rate of actual uranium containing wastewater. This study not only expands the range of applications of variable valence metal covalent organic frameworks, but also provides unique insights into the effective combination of chemical and photocatalytic reduction strategies for removing UVI in a single material. [ABSTRACT FROM AUTHOR]
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- 2024
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12. Phosphorylated covalent organic framework/graphene composites for photoelectrothermal integrated collaborative reduction of uranium.
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Zhang, Rui, Tao, Liang, Niu, Cheng-Peng, Zhang, Cheng-Rong, Shi, Tie-Ying, Wang, Xiao-Xing, Wang, Ying-Ao, Zhang, Li, Liang, Ru-Ping, and Qiu, Jian-Ding
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URANIUM , *CHEMICAL stability , *PHOTOREDUCTION , *URANIUM mining , *GRAPHENE , *PHOTOTHERMAL conversion - Abstract
[Display omitted] • Phosphate functionalized COF/rGO was synthesized using post-synthetic modification. • Tb-BD-P/rGO exhibited excellent physicochemical stability and rapid uranyl mass transfer ability. • TB-BD-P/rGO enabled photoelectrothermal synergistic photocatalytic reduction of uranium. • Tb-BD-P/rGO performed excellent removal rates (>95 %) in actual strong acid nuclear wastewater. Photocatalytic reduction is becoming an effective method to remove UVI from uranium mine wastewater. Herein, 1,3,5-benzotrialdehyde (Tb) and 4,4′-diaminobiphenyl (BD) used as monomers of covalent organic framework (COF) are in situ growth on graphene oxide (GO) surfaces to obtain Tb-BD/rGO. Then, Tb-BD/rGO is converted into Tb-BD-P/rGO by asymmetric hydrogen phosphorylation, which is served as a new material for photocatalytic reduction of uranium via photoelectrothermal synergy. Benefiting from the transformation of dynamic imine bonds into irreversible carbon–nitrogen single bonds, Tb-BD-P/rGO expresses remarkable chemical and thermal stability. The introduction of phosphate groups improve the electronegativity and hydrophilicity of Tb-BD-P/rGO, which contribute to rapid transportation of uranium. In addition, the introduction of rGO achieves excellent photothermal conversion, accelerating the adsorption kinetics of uranium. Meanwhile, the π-π interaction between Tb-BD-P and rGO promotes inter-interfacial electron transfer and reduces the complexation of electron-hole pairs during the photocatalytic process, further improving photocatalytic performance. Therefore, Tb-BD-P/rGO demonstrates exceptional removal uranium rates (>95 %) in uranium mine wastewater by synergistically photoelectrothermal integration, offering a pathway for developing multifunctional and integrated photocatalysts. [ABSTRACT FROM AUTHOR]
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- 2024
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13. Vinylene-linked covalent organic frameworks with enhanced uranium adsorption through three synergistic mechanisms.
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Xu, Rui-Han, Cui, Wei-Rong, Zhang, Cheng-Rong, Chen, Xiao-Rong, Jiang, Wei, Liang, Ru-Ping, and Qiu, Jian-Ding
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ADSORPTION capacity , *URANIUM , *PHOTOCATALYSTS , *ADSORPTION kinetics , *PHOTOREDUCTION , *ADSORPTION (Chemistry) - Abstract
We report the first example of vinylene-linked covalent organic framework (Tp-TMT) with enhanced uranium adsorption through combined selective ligand binding, chemical reduction and photocatalytic reduction. The dense hydroxyl functional groups on the Tp-TMT framework had good selectivity and excellent chemical reduction performance for U(VI). Meanwhile, the synergistic effect of hydroxyl groups and triazine unit significantly enhanced the photocatalytic reduction activity. Thus Tp-TMT exhibited incredible adsorption kinetics and capacity for uranium. [Display omitted] • COFs effectively capture uranium through three coordinated mechanisms. • Tp-TMT has excellent visible light conversion efficiency and low band gap. • Tp-TMT enhances uranium adsorption through selective ligand binding and reduction. • Tp-TMT exhibits incredible adsorption kinetics and capacity for uranium. So far, it remains a challenge to synthesize uranium adsorbents with robust stability, high adsorption capacity, excellent photocatalytic activity and easy regeneration. Herein, we report the first example of vinylene-linked covalent organic framework (Tp-TMT) with enhanced uranium adsorption through combined selective ligand binding, chemical reduction and photocatalytic reduction. The unique structure and excellent photocatalytic activity of Tp-TMT make it very suitable for photo-enhanced uranium adsorption through three synergistic mechanisms, thus exhibiting an outstanding uranium adsorption capacity (2362.4 mg g−1). In the dark, a large number of hydroxyl groups in the Tp-TMT framework serve as selective binding sites for uranium, and reduce part of U(VI) to U(IV), thereby greatly improving the adsorption capacity. Meanwhile, the synergistic effect of the triazine units and hydroxyl groups in the highly conjugated framework greatly decreases the optical band gap of Tp-TMT, and an additional U(VI) photocatalytic reduction process can occur under light irradiation, further increasing the adsorption kinetics and capacity. This work explored the structural and functional design of covalent organic frameworks for the adsorption and reduction of uranium in nuclear industry wastewater. [ABSTRACT FROM AUTHOR]
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- 2021
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14. Synergistic effect of photocatalytic U(VI) reduction and chlorpyrifos degradation by bifunctional type-II heterojunction MOF525@BDMTp with high carrier migration performance.
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Liu, Xin, Peng, Zhi-Hai, Lei, Lan, Bi, Rui-Xiang, Zhang, Cheng-Rong, Luo, Qiu-Xia, Liang, Ru-Ping, and Qiu, Jian-Ding
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IRRADIATION , *HETEROJUNCTIONS , *CHLORPYRIFOS , *ELECTRON density , *COMPOSITE materials , *OXYGEN evolution reactions , *METAL-organic frameworks - Abstract
The radioactive ion U(VI) and organophosphorus pollutants in sewage do great harm to the ecological environment and human health. Bifunctional photocatalyst MOF525@BDMTp was prepared by in-situ covalent bridging method, and U(VI) and chlorpyrifos (CP) were removed by one-to-two strategy. MOF525@BDMTp had high carrier migration performance and conformed to the type-II heterojunction. Under light conditions, electrons were transferred from MOF525 to BDMTp due to the action of the built-in electric field, increasing the electron density of BDMTp and thus activating the U(VI) binding sites. BDMTp interacted with S and N atoms in CP to promote its hydrolysis and oxidation by h+ and ·O 2 -. Thus, MOF525@BDMTp guaranteed the simultaneous reduction of U(VI) on BDMTp and the oxidation of CP on MOF525. Therefore, designing functional integrated composites is an effective means to improve the photocatalytic performance of composite materials in complex environments. [Display omitted] • MOF525@BDMTp was prepared by in-situ covalent bond bridging method. • MOF525@BDMTp can adsorb both U (VI) and chlorpyrifos. • Type-II heterojunction in MOF525@BDMTp improved electron-hole separation. • The presence of U(VI) and CP improved the removal performance of each other. [ABSTRACT FROM AUTHOR]
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- 2024
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15. Synergistic effect of double Schottky potential well and oxygen vacancy for enhanced plasmonic photocatalytic U(VI) reduction.
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Liu, Xin, Bi, Rui-Xiang, Peng, Zhi-Hai, Lei, Lan, Zhang, Cheng-Rong, Luo, Qiu-Xia, Liang, Ru-Ping, and Qiu, Jian-Ding
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POTENTIAL well , *SCHOTTKY effect , *SURFACE plasmon resonance , *HOT carriers , *PLASMONICS , *URANIUM , *URANIUM compounds , *PHOTOCATALYSIS - Abstract
Plasmonic photocatalysis is an effective strategy to solve radioactive uranium hazards in wastewater. A plasmonic photocatalyst Bi/Bi 2 O 3−x @COFs was synthesized by in-situ growth of covalent organic frameworks (COFs) on Bi/Bi 2 O 3−x surface for the U(VI) adsorption and plasmonic photoreduction in rare earth tailings wastewater. The presence of oxygen vacancy in Bi/Bi 2 O 3−x and Schottky potential well formed by Bi and Bi 2 O 3−x interface increased the number of free electrons, which induced localized surface plasmon resonance (LSPR) and enhanced the light absorption performance of composites. In addition, oxygen vacancy improved the Fermi level of Bi/Bi 2 O 3−x , leading to another potential well between Bi 2 O 3−x and COFs interface. The electron transport direction was reversed, thus increasing the electron density of COFs layer. COFs was an N-type semiconductor with specific binding U(VI) groups and suitable band structure, which could be used as an active reaction site. Bi/Bi 2 O 3−x @COFs had 1411.5 mg g−1 removal capacity and high separation coefficient for U(VI) due to the synergistic action of photogenerated electrons and hot electrons. Moreover, the removal rate of uranium from rare earth tailings wastewater by regenerated Bi/Bi 2 O 3−x @COFs was over 93.9%. The scheme of introducing LSPR and Schottky potential well provides another way to improve the photocatalytic effect. [Display omitted] • Bi/Bi 2 O 3−x @COFs with core-shell structure was synthesized in-situ. • Oxygen vacancies in Bi 2 O 3−x induced LSPR and increased light absorption. • The double Schottky potential well increased the electron density of COFs. • U(VI) was reduced by the synergistic action of photogenerated and hot electrons. • Regenerated Bi/Bi 2 O 3−x @COFs had high cyclic stability. [ABSTRACT FROM AUTHOR]
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- 2023
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16. Covalent organic framework modified carbon nanotubes for removal of uranium (VI) from mining wastewater.
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Liu, Xin, Wang, Xun, Jiang, Wei, Zhang, Cheng-Rong, Zhang, Li, Liang, Ru-Ping, and Qiu, Jian-Ding
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CARBON nanotubes , *URANIUM , *SEWAGE , *URANIUM mining , *RARE earth metals , *MINES & mineral resources , *TRICHLOROPHENOL - Abstract
[Display omitted] • COFs and CNTs composites were synthesized by in-situ synthesis. • The synergistic effect improved the adsorption capacity and selectivity. • The removal mechanism of samples was clarified through various characteristic modes. • The problem of U (VI) removal from the rare earth tailings wastewater had been solved. The wastewater containing uranium produced in the mining process is harmful to the environment and life safety due to the inherent biotoxicity and radioactivity of uranium. In this paper, 4,4′-diamino-[1,1′-biphenyl]-3,3′-diol and 2,4,6-triformylphloroglucinol were in situ synthesized β -ketoenamine covalent organic frameworks (COFs) on the surface of carbon nanotubes (CNTs) to obtain a composite of CNT/COF-OH for removal uranium in the rare earth tailings wastewater. Grafting COFs with a large number of specific uranium-binding groups and redox-active sites on the surface of CNTs, CNT/COF-OH can effectively enhance the uranium ion selectivity and adsorption capacity. Furthermore, CNTs have good electron transport capacity and π-conjugation properties, electrons can be effectively transferred from CNTs to COFs, which increases the electron density of the adsorption functional groups, resulting in an increase of the adsorption energy and reductive activity for U (VI), thus improving the removal efficiency. In addition, the skeleton of COFs can be supported by CNTs, thus reducing collapse. Through the synergistic effect of composite, CNT/COF-OH had a good uranium adsorption capacity of 518.2 mg g−1. The adsorption capacity of CNT/COF-OH was increased by 390.7 %, 54.6 %, and 84.5 % compared with those of single CNTs, COF-OH, and mixed CNT + COF-OH, respectively. The selective separation coefficient of CNT/COF-OH was 1.6 times higher than that of COF-OH. The experiment of uranium removal was carried out in the rare earth tailings wastewater using CNT/COF-OH, the removal rate reached 96.7 %. The COFs modified CNTs with synergistic effect have important theoretical and practical significance for the safety problems caused by harmful ions in wastewater. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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17. Tuned-Potential Covalent organic framework Electrochemiluminescence platform for lutetium analysis.
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Luo, Qiu-Xia, Cai, Yuan-Jun, Mao, Xiang-Lan, Li, Ya-Jie, Zhang, Cheng-Rong, Liu, Xin, Chen, Xiao-Rong, Liang, Ru-Ping, and Qiu, Jian-Ding
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AZINES , *MOLECULAR structure , *LUTETIUM , *DENSITY functional theory , *REDUCTION potential , *STRUCTURAL frames , *ELECTROCHEMILUMINESCENCE - Abstract
Mechanism diagram. Through the structural design at the molecular level, the ECL-COF with electrocatalytic performance and excellent electronic structure was obtained, which display an adjustable easily potential ECL platform. Meanwhile, the advanced COF'ECL platform was developed for accurate monitoring of Lu3+, indicating the inestimable application potential of COFs in environment field. [Display omitted] • The azine-linked COFs are prepared for precise ECL performance regulation. • COFs display decrease of reduction potential and increase of intensity in ECL. • Introducing nitrogen into COFs bring electrocatalysis for ECL enhancement. • COFs show efficiently carrier transport for improving ECL. • A novel COF-ECL platform is structured for Lu3+ detection. Covalent organic frameworks (COFs) have emerged as a novel class of electrochemiluminescence (ECL) materials on account of its highly tunable structure and versatile properties. However, decoding the ECL property and its luminophor structure to improve the luminous performance remains challenging, which hinders its deeper development and wider application. Herein, by condensing triphenylarene aldehydes with varying number of nitrogen atoms with 2,4,6-trimethylbenzene-1,3,5-tricarbonitrile, a series of COFs were prepared to regulate the ECL potential, opening up a new way to precisely improve ECL performance. The electron and spatial changes in the precursor are transferred to the generated COFs skeleton, resulting in a progressively decrease in the reduction potential and a gradual increase intensity in ECL with the precise increase of nitrogen content in the skeleton. Introduction of nitrogen into COFs brings electrocatalysis and planarization of the framework for more efficiently carrier transport. The conclusion is confirmed by optical, electrical tests, as well as density functional theory calculations. As a proof-of-methodology, an ECL method was developed for the selective determination of lutetium ion with a detection limit as low as 1.6 nM (S/N = 3). This work exhibits that the advanced potential-tunable ECL-COFs can be obtained accurately and easily through design structure at the molecular level, which is expected to promote the exploration of the relationship between ECL potential and framework structure, and further apply to environment-related sensing analysis. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
18. Stable sp2 carbon-conjugated covalent organic framework for detection and efficient adsorption of uranium from radioactive wastewater.
- Author
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Li, Fang-Fang, Cui, Wei-Rong, Jiang, Wei, Zhang, Cheng-Rong, Liang, Ru-Ping, and Qiu, Jian-Ding
- Subjects
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URANIUM , *ADSORPTION (Chemistry) , *ADSORPTION capacity , *MASS transfer , *NUCLEAR industry , *URANIUM mining - Abstract
• Highly stable sp2 carbon-conjugated covalent organic framework (COF-PDAN-AO) was synthesized and characterization. • Acid and radiation resistant COF-PDAN-AO exhibits efficient adsorption of UO 2 2+ from radioactive wastewater. • COF-PDAN-AO possesses short adsorption equilibrium time and selectivity for uranium. • The emission of COF-PDAN-AO was selectively quenched upon adding UO 2 2+. Uranium is an important element in the nuclear industry while the discharge of radioactive wastewater can cause serious damages to the environment. In this work, an ultra-stable sp2 carbon-conjugated covalent organic framework (COF-PDAN-AO) is synthesized with amidoxime-substituted monomers for detection and efficient adsorption of uranium from radioactive wastewater. Abundant amidoxime groups laced on the open 1D channels of COF-PDAN-AO exhibit exceptional accessibility and the regular pores facilitate the mass transfer. Based on these features, COF-PDAN-AO achieves ultra-low detection limit of 6.5 nM, high uranium adsorption capacity (410 mg/g) and selective interaction with uranium. In addition, various spectroscopies verify COF-PDAN-AO possesses excellent radioresistance in acidic solution. Regeneration studies have shown that COF-PDAN-AO maintained good structural stability after seven cycles. These results indicate that our sp2 carbon conjugated COF can be potentially used for practical detection and adsorption of uranium from radioactive wastewater. This strategy can be extended to detection and extraction of other contaminants by designing the target ligand. [ABSTRACT FROM AUTHOR]
- Published
- 2020
- Full Text
- View/download PDF
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