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学者姓名：高琰昕
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Abstract ：
The adsorptive removal of typical pharmaceuticals, carbamazepine (CBZ) and tetracycline (TC), was investigated with four zirconium-based porphyrinic metal-organic frameworks (MOFs) (PCN-221, PCN-222, PCN-223, and PCN-224). For both CBZ and TC, the adsorption capacities of the PCNs were ranked in the following order: PCN-221 < PCN-223 < PCN-224 < PCN-222. Notably, this order aligns with the BET surface areas of the PCNs. Cage-type PCN-221 showed a lower adsorption capacity than the other three channel-type MOFs due to its small apertures, which were not conducive to the activation of PCN-221 and space utilization. The amount of adsorption was proportional to the cumulative pore volume in PCNs with a width larger than that of the CBZ/TC molecule. Therefore, with high pore volume and large one-dimensional channels formed by ordered linker vacancies, PCN-222 was the best adsorbent in this work. According to the Langmuir model, PCN-222 exhibited exceptional adsorption capacities for CBZ and TC, reaching 305 mg/g and 280 mg/g, respectively. Additionally, the mechanisms for CBZ removal involved hydrogen bonding and pi-pi interactions/stacking, while electrostatic interactions, hydrogen bonding, and pi-pi interactions/stacking played crucial roles in TC adsorption onto MOFs. These findings establish a profound comprehension of the interplay between pore structure and performance, providing helpful guidance for designing MOFs to remove emerging contaminants effectively.
Keyword ：
Adsorption Adsorption Mechanism Mechanism MOFs MOFs PPCPs PPCPs Structure Structure
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| GB/T 7714 | Wu, Xiaoyu , Gao, Yanxin , Bi, Jinhong . Understanding the structure-dependent adsorption behavior of four zirconium-based porphyrinic MOFs for the removal of pharmaceuticals [J]. | MICROPOROUS AND MESOPOROUS MATERIALS , 2024 , 363 . |
| MLA | Wu, Xiaoyu 等. "Understanding the structure-dependent adsorption behavior of four zirconium-based porphyrinic MOFs for the removal of pharmaceuticals" . | MICROPOROUS AND MESOPOROUS MATERIALS 363 (2024) . |
| APA | Wu, Xiaoyu , Gao, Yanxin , Bi, Jinhong . Understanding the structure-dependent adsorption behavior of four zirconium-based porphyrinic MOFs for the removal of pharmaceuticals . | MICROPOROUS AND MESOPOROUS MATERIALS , 2024 , 363 . |
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The treatment of emerging contaminants is essential but challenging. Herein, a novel MOF/PAN fibrous composite (TCPP@UiO-66/PAN) was synthesized and used as a self-cleaning membrane for the efficient removal of a typical emerging contaminant, diclofenac sodium (DF). The introduction of the secondary linker tetra(4carboxyphenyl)porphyrin (TCPP) served to expand the pores and enhance its photocatalytic activity. TCPP@UiO-66/PAN shows higher adsorption capacity and initial adsorption rate than UiO-66/PAN. The maximum adsorption capacity of DF on TCPP@UiO-66/PAN reached 202 mg/g by Langmuir model. The DF adsorption mechanism involves the pi-pi/anion-pi interaction, Lewis acid-base interaction, and hydrogen bonding. Based on the dynamic filtration experiment, TCPP@UiO-66/PAN exhibited a remarkable treatment capacity for DF-contaminated water, measuring 3.75 x 104 kg/kg. Given its fibrous membrane structure, TCPP@UiO-66/ PAN could be easily separated from water and reused. In-situ photo-regeneration emerged as a highly effective method for regenerating TCPP@UiO-66/PAN after reaching adsorption saturation, with over 95 % DF degradation achieved under sunlight irradiation. The decomposition of DF primarily resulted from the generation of h+ and 1O2. Additionally, TCPP@UiO-66/PAN exhibited notable antibacterial properties when exposed to visible light. In vitro cytotoxicity assessments further confirmed the safety of these MOF/PAN composites. Combining the advantages of hybrid-linker strategy and fibrous composite, this work provided new insight into constructing MOF-based functional material for wastewater purification.
Keyword ：
Adsorption Adsorption Emerging contaminants Emerging contaminants Fibrous composites Fibrous composites Metal -organic frameworks Metal -organic frameworks Self-cleaning Self-cleaning
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| GB/T 7714 | Gao, Yanxin , Cheng, Ting , Zhao, Fankang et al. A hybrid linker-MOF fibrous composite for efficient diclofenac removal and self-cleaning [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 337 . |
| MLA | Gao, Yanxin et al. "A hybrid linker-MOF fibrous composite for efficient diclofenac removal and self-cleaning" . | SEPARATION AND PURIFICATION TECHNOLOGY 337 (2024) . |
| APA | Gao, Yanxin , Cheng, Ting , Zhao, Fankang , Huang, Guocheng , Bi, Jinhong . A hybrid linker-MOF fibrous composite for efficient diclofenac removal and self-cleaning . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 337 . |
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The development of innovative multi-emission sensors for the rapid and accurate detection of contaminants is both vital and challenging. In this study, utilizing two rigid ligands (H3ICA and H4BTEC), a series of water-stable bimetallic organic frameworks (EuTb-MOFs) were synthesized. Luminescent investigations have revealed that EuTb-MOF-1 exhibits prominent multiple emission peaks, attributed to the distinctive fluorescence characteristics of Eu(III) and Tb(III) ions. Therefore, EuTb-MOF-1 efficiently recognized various metal ions and pharmaceutical compounds through 2D decoded maps. Fe3+ and Pb2+ exhibited significant quenching effects on the luminescence of EuTb-MOF-1, which were attributed to the internal filtering effect and the interaction between Lewis basic sites within EuTb-MOF-1 and Pb2+ ions, respectively. Furthermore, EuTb-MOF-1 demonstrated high sensitivity to sulfonamide antibiotics, with detection limits of 0.037 μM for SMZ and 0.041 μM for SDZ, respectively. In addition, EuTb-MOF-1 was immobilized to prepare MOF-based test strips, enabling direct visual detection of sulfonamides as a portable sensor. With excellent water stability, multi-responsive recognition capabilities, and high sensitivity to specific analytes, EuTb-MOF-1 is a promising candidate for environmental contaminant detection in aquatic systems. © 2024
Keyword ：
Lanthanide Lanthanide Luminescent sensor Luminescent sensor Metal ions Metal ions Metal-organic frameworks Metal-organic frameworks Pharmaceuticals Pharmaceuticals
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| GB/T 7714 | Gao, Y. , Zhu, Y. , Wang, Y. et al. Water-Stable Ln-MOF as a multi-emitting luminescent sensor for the detection of metal ions and pharmaceuticals [J]. | Spectrochimica Acta - Part A: Molecular and Biomolecular Spectroscopy , 2024 , 323 . |
| MLA | Gao, Y. et al. "Water-Stable Ln-MOF as a multi-emitting luminescent sensor for the detection of metal ions and pharmaceuticals" . | Spectrochimica Acta - Part A: Molecular and Biomolecular Spectroscopy 323 (2024) . |
| APA | Gao, Y. , Zhu, Y. , Wang, Y. , Bi, J. . Water-Stable Ln-MOF as a multi-emitting luminescent sensor for the detection of metal ions and pharmaceuticals . | Spectrochimica Acta - Part A: Molecular and Biomolecular Spectroscopy , 2024 , 323 . |
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The semiconductor-insulator heterostructure, characterized by outstanding economic-efficiency and catalytic activity, represents a promising photocatalyst for practical pollutants degradation. However, achieving energy band matching between semiconductors and insulators remains a challenge. In this study, we meticulously designed and synthesized a band-matched semiconductor-insulator photocatalysts (AgI-BaCO3), leveraging the in-situ nucleation of ultrafine AgI nanoparticles on BaCO3 surface. The finely crafted heterostructure notably enhanced degradation efficiency of tetracycline over both pure AgI and BaCO3, demonstrating a remarkable pseudo-first-order kinetic rate constant that surpassed them by 27.2 and 33.5 times, respectively. The density functional theory calculations uncovered that the intense covalent interaction between AgI and BaCO3 established a specific channel for interfacial charge carriers. The generated CO3·- radicals as the main active species markedly expedited the removal of antibiotics. Furthermore, the catalysts demonstrated robust activity in real wastewater and surface water. This work supplies a novel reference for constructing insulator-based photocatalysts and elucidates its potential application in actual aquatic environments. © 2024 Elsevier B.V.
Keyword ：
Antibiotics Antibiotics BaCO3 BaCO3 CO3·- radicals CO3·- radicals Heterostructure Heterostructure Visible-light photocatalysis Visible-light photocatalysis
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| GB/T 7714 | Yu, M. , Kong, X. , Luo, J. et al. Carbonate radicals mediated catalytic degradation of antibiotics over earth-abundant BaCO3-based system: Performance, mechanism and calculation [J]. | Journal of Alloys and Compounds , 2024 , 1004 . |
| MLA | Yu, M. et al. "Carbonate radicals mediated catalytic degradation of antibiotics over earth-abundant BaCO3-based system: Performance, mechanism and calculation" . | Journal of Alloys and Compounds 1004 (2024) . |
| APA | Yu, M. , Kong, X. , Luo, J. , Zhou, H. , Gao, Y. , Zheng, C. et al. Carbonate radicals mediated catalytic degradation of antibiotics over earth-abundant BaCO3-based system: Performance, mechanism and calculation . | Journal of Alloys and Compounds , 2024 , 1004 . |
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The construction of step-scheme (S-scheme) heterojunctions has emerged as a widely adopted strategy for achieving photocatalytic hydrogen peroxide (H2O2) generation. In this study, we employed an approach to deposit indium sulfide (In2S3) onto a Schiff-base covalent organic framework (COF), namely TpMA, for H2O2 photosynthesis and its sterilization application. The optimized photocatalyst, 10%TpMA/In2S3, exhibited remarkable photocatalytic performance, yielding a substantial H2O2 output of 311.07 mu mol/L. A series of advanced instrumental analyses and density functional theory (DFT) results indicated that the establishment of the S-scheme heterojunction played a pivotal role in facilitating efficient charge carrier transfer and separation. Specifically, the formation of a built-in electric field was probed and quantified. Furthermore, the H2O2 exhibited the capability to undergo direct catalysis by Fe(II), which substantially facilitated the inactivation of pathogenic bacteria. This work unveils insight into the COF-based S-scheme photocatalysts and offers a sustainable approach for environmentally friendly H2O2 production for sterilization purposes.
Keyword ：
Built-in Electric Field Built-in Electric Field Covalent organic frameworks Covalent organic frameworks In situ oS In situ oS S-scheme heterojunction S-scheme heterojunction
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| GB/T 7714 | Chen, Hanye , Gao, Shengjie , Huang, Guocheng et al. Built-in electric field mediated S-scheme charge migration in COF/In2S3 heterojunction for boosting H2O2 photosynthesis and sterilization [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2023 , 343 . |
| MLA | Chen, Hanye et al. "Built-in electric field mediated S-scheme charge migration in COF/In2S3 heterojunction for boosting H2O2 photosynthesis and sterilization" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 343 (2023) . |
| APA | Chen, Hanye , Gao, Shengjie , Huang, Guocheng , Chen, Qiaoshan , Gao, Yanxin , Bi, Jinhong . Built-in electric field mediated S-scheme charge migration in COF/In2S3 heterojunction for boosting H2O2 photosynthesis and sterilization . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2023 , 343 . |
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Photocatalytic hydrogen production holds great promise for alleviating the energy shortage through effective photo-to-chemical conversion, and the development of visible-light responsive, low-cost and sustainable photocatalysts remains key priority. In this study, carbon quantum dots/covalent triazine-based framework (CQDs/CTF) non-metallic photocatalyst was constructed through a simple impregnation method for photocatalytic H2 evolution. Upon 0.24% CQDs loading, a three-fold enhanced H2 production activity of 102 mmol center dot g-1 center dot h-1 was achieved compared with pristine CTF-1 (34.5 mmol center dot g-1 center dot h-1). Photoluminescence and photoelectrochemical study revealed carbon quantum dots served as the electron libraries, which was conducive to facilitate electron capture and promote the separation of photoinduced electron-hole pairs in CTF-1. Notably, the excitationindependent up-conversion fluorescent characteristics of CQDs endowed the catalysts broadened visible-light response range and higher solar energy utilization efficiency. This study deepens insights into the mechanism of CQDs modification and paves a trustworthy strategy for harvesting visible-light-driven metal-free photocatalyst with highly-active and robust performance.
Keyword ：
Carbon quantum dots Carbon quantum dots Covalent triazine-based frameworks Covalent triazine-based frameworks Solar energy conversion Solar energy conversion Visible-light photocatalysis Visible-light photocatalysis Water splitting Water splitting
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| GB/T 7714 | Chen, Yueling , Huang, Guocheng , Gao, Yanxin et al. Up-conversion fluorescent carbon quantum dots decorated covalent triazine frameworks as efficient metal-free photocatalyst for hydrogen evolution [J]. | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2022 , 47 (14) : 8739-8748 . |
| MLA | Chen, Yueling et al. "Up-conversion fluorescent carbon quantum dots decorated covalent triazine frameworks as efficient metal-free photocatalyst for hydrogen evolution" . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 47 . 14 (2022) : 8739-8748 . |
| APA | Chen, Yueling , Huang, Guocheng , Gao, Yanxin , Chen, Qiaoshan , Bi, Jinhong . Up-conversion fluorescent carbon quantum dots decorated covalent triazine frameworks as efficient metal-free photocatalyst for hydrogen evolution . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2022 , 47 (14) , 8739-8748 . |
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Sulfate-radical-based wastewater treatment has re-ceived great interest due to its high-level efficiency. However, the preparation of stable and recyclable nanocatalysts remains a challenge. Herein, a highly efficient catalyst (FeCo/SC) for persulfate activation is successfully synthesized via dispersing S and Fe into carbon skeletons derived from ZIF-67. After the introduction of S, FeCo/SC exhibited excellent catalytic performance. With the action of SO4-center dot, Fe(VI), and 1O2, the degradation efficiency of carbamazepine (CBZ) (10 mg L-1) could be up to 97.9 +/- 2% within 10 min. The results showed that the larger surface area after S doping decreases the electron transfer resistance. The S0/S2- is beneficial for promoting the Fe(III)-to-Fe(II) and Co(III)-to-Co(II) conversion cycle. Moreover, the liquid chromatograph-mass spectrometer (LC-MS), density functional theory (DFT), and ecological structure-activity relationships (ECOSAR) revealed the possible degradation pathway of CBZ, which was a toxicity attenuation process. In consequence, this work offers an innovative scheme for researching the effect of trace S-doped bimetallic oxide nanoparticles on PDS heterogeneous catalytic systems.
Keyword ：
carbamazepine carbamazepine DFT calculation DFT calculation ecotoxicity ecotoxicity peroxydisulfate activation peroxydisulfate activation sulfur sulfur
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| GB/T 7714 | Huang, Xiaoyi , Liu, Qingsong , Zhu, Jianlong et al. Trace Sulfur Accelerated Peroxydisulfate Activation Based on a ZIF-67-Derived Nanostructure for Carbamazepine Degradation [J]. | ACS APPLIED NANO MATERIALS , 2022 . |
| MLA | Huang, Xiaoyi et al. "Trace Sulfur Accelerated Peroxydisulfate Activation Based on a ZIF-67-Derived Nanostructure for Carbamazepine Degradation" . | ACS APPLIED NANO MATERIALS (2022) . |
| APA | Huang, Xiaoyi , Liu, Qingsong , Zhu, Jianlong , Gao, Yanxin , Fang, Shengqiong , Bi, Jinhong . Trace Sulfur Accelerated Peroxydisulfate Activation Based on a ZIF-67-Derived Nanostructure for Carbamazepine Degradation . | ACS APPLIED NANO MATERIALS , 2022 . |
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The development of mixed-linker metal-organic frameworks (MOFs) is an efficient strategy to improve the performance of MOFs. Herein, we successfully integrate tetrakis(4-carboxyphenyl)porphyrin (TCPP) into different Zr-MOFs via a facile one-pot solvothermal synthesis while preserving the integrity of their frameworks. The functional groups, length of primary linkers, and the inner pore structure significantly affected the properties of the synthesized TCPP@MOFs, such as surface area, average pore size, and O-1(2) productivity. Among them, TCPP@PCN-777 demonstrated the largest surface area (2386 cm(2)/g, as measured by N-2 uptake) and the highest O-1(2) generation rate (1.15 h(-1), [O-1(2)](ss) = 2.66 X 10(-12) M) under irradiation. The TCPP loading was also shown to affect the crystal phase, morphology, surface area, and photochemical properties of the synthesized MOFs. Therefore, TCPP@PCN-777s with various TCPP loadings were synthesized to investigate the optimum loading. The optimized TCPP@MOF, TCPP@PCN-777-30, was evaluated for its removal of model contaminant ranitidine (RND) through both adsorption and photodegradation. TCPP@PCN-777-30 showed a higher adsorption capacity toward RND than both the parent MOF (PCN-777) and commercially available activated carbon, and effectively degraded RND in aqueous solution (>99% photodegradation in 1 h). With irradiation, TCPP@PCN-777-30 showed a minimal loss in adsorption efficiency over four consecutive treatment cycles, confirming the reusability of the material enabled through the incorporation of TCPP into the MOF structure. This work not only developed an efficient multifunctional material for environmental remediation but also forwarded knowledge on the effect of linker environment (i.e., functional groups, framework structure, and linker ratio) on the properties of TCPP@MOFs to guide future research on mixed-linker MOFs.
Keyword ：
emerging contaminants emerging contaminants mixed-linker mixed-linker MOFs MOFs photochemistry photochemistry porphyrin porphyrin
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| GB/T 7714 | Gao, Yanxin , Suh, Min-Jeong , Kim, Jae-Hong et al. Imparting Multifunctionality in Zr-MOFs Using the One-Pot Mixed-Linker Strategy: The Effect of Linker Environment and Enhanced Pollutant Removal [J]. | ACS APPLIED MATERIALS & INTERFACES , 2022 . |
| MLA | Gao, Yanxin et al. "Imparting Multifunctionality in Zr-MOFs Using the One-Pot Mixed-Linker Strategy: The Effect of Linker Environment and Enhanced Pollutant Removal" . | ACS APPLIED MATERIALS & INTERFACES (2022) . |
| APA | Gao, Yanxin , Suh, Min-Jeong , Kim, Jae-Hong , Yu, Gang . Imparting Multifunctionality in Zr-MOFs Using the One-Pot Mixed-Linker Strategy: The Effect of Linker Environment and Enhanced Pollutant Removal . | ACS APPLIED MATERIALS & INTERFACES , 2022 . |
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Artificial photosynthesis is considered a promising strategy to mitigate environmental issues and energy crises. Herein, one-dimensional oxide-semiconductor (TiO2-nanofiber, TNF) and polyarylether-based covalent organic framework (COF-318) were composed to form a visible-light responsive heterojunction (COF-318/TNF) for artificial photosynthesis by simultaneously triggering CO2 reduction and H2O oxidation. Without additional sacrificial agents, photosensitizers or cocatalysts, the optimal sample COF-318/TNF-15 exhibited CO2-to-CO conversion efficiency of 70.1 +/- 0.7 mu mol.g(- 1).h(-1), 12.7 times higher than that of COF-318. The molar ratio of produced CO to O2 was about 2:1, suggesting H2O was the electron donor in the photocatalytic process. Pho-toelectrochemical measurements and time-resolved transient absorption spectra illustrated the high separation/ transfer efficiency of photo-generated charges in COF-318/TNF-15, which was attributed to the construction of heterojunction and the specific one-dimensional property of TiO2 nanofibers. During the CO2 photoreduction, HCOO* was detected as the key intermediate for CO production according to the in-situ FT-IR analysis. This work provides a new route for the rational design of organic-inorganic heterogeneous photocatalysts for visible-light -driven CO2 reduction.
Keyword ：
Artificial photosynthesis Artificial photosynthesis CO2 reduction CO2 reduction Polyarylether-COFs Polyarylether-COFs TiO2 nanofibers TiO2 nanofibers
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| GB/T 7714 | Gao, Yanxin , Tan, Zunkun , Yang, Rong et al. Integrating polyarylether-COFs with TiO2 nanofibers for enhanced visible-light-driven CO2 reduction in artificial photosynthesis [J]. | APPLIED SURFACE SCIENCE , 2022 , 605 . |
| MLA | Gao, Yanxin et al. "Integrating polyarylether-COFs with TiO2 nanofibers for enhanced visible-light-driven CO2 reduction in artificial photosynthesis" . | APPLIED SURFACE SCIENCE 605 (2022) . |
| APA | Gao, Yanxin , Tan, Zunkun , Yang, Rong , Huang, Guocheng , Bi, Jinhong . Integrating polyarylether-COFs with TiO2 nanofibers for enhanced visible-light-driven CO2 reduction in artificial photosynthesis . | APPLIED SURFACE SCIENCE , 2022 , 605 . |
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The functionalization of metal-organic frameworks (MOFs) is imperative and challenging for the devel-opment of practical MOF-based materials. Herein, a magnetically functionalized Zr-MOF (Fe3O4@MOF-525) was synthesized via secondary-growth approach to obtain an easily-separated and recyclable adsor-bent for the removal of pharmaceuticals (tetracycline (TC) and diclofenac sodium (DF)). After loading Fe(3)O(4 & nbsp;)nanoparticles (NPs), due to the increase of micropore volume and specific surface area caused by defects, the adsorption performance of Fe3O4@MOF-525 was improved. The kinetics could be described by the pseudo-second-order kinetic model. The different adsorption capacity and initial rate were attributed to the properties of the pharmaceuticals, including the molecular size and hydrophobicity/hydrophilicity. In isotherm experiments, the maximum adsorption capacities of DF and TC on Fe3O4@MOF-525 calculated by Sips model reached 745 and 277 mg.g( 1), respectively. The thermo-dynamic studies indicated the adsorption was endothermic and spontaneous. The effect of pH suggested that electrostatic interaction, p -p interaction, anion-p interaction, and H-bonding were possibly involved in the adsorption process. The adsorbent was separated by magnetic and regenerated. Washed with etha-nol, Fe3O4@MOF-525 remained about 80% adsorption capacity after four cycles. In-situ photo-regeneration under visible-light irradiation was another attractive method, where > 95% TC was degraded in 4 h. The reaction with scavengers revealed that 1O2 was the dominant reactive species in our system, indicating the occurrence of Type II photosensitization. The separability, excellent adsorption performance, and recyclability of Fe3O4@MOF-525 may lead to its beneficial applications in water treatment. (C)& nbsp;2022 Elsevier Inc. All rights reserved.
Keyword ：
Adsorption Adsorption Magnetic modification Magnetic modification Metal-organic frameworks Metal-organic frameworks PPCPs PPCPs
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| GB/T 7714 | Zhao, Fankang , Fang, Shengqiong , Gao, Yanxin et al. Removal of aqueous pharmaceuticals by magnetically functionalized Zr-MOFs: Adsorption Kinetics, Isotherms, and regeneration [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2022 , 615 : 876-886 . |
| MLA | Zhao, Fankang et al. "Removal of aqueous pharmaceuticals by magnetically functionalized Zr-MOFs: Adsorption Kinetics, Isotherms, and regeneration" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 615 (2022) : 876-886 . |
| APA | Zhao, Fankang , Fang, Shengqiong , Gao, Yanxin , Bi, Jinhong . Removal of aqueous pharmaceuticals by magnetically functionalized Zr-MOFs: Adsorption Kinetics, Isotherms, and regeneration . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2022 , 615 , 876-886 . |
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