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学者姓名:毕进红
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Environmental concerns are driving the development of eco-friendly and effective methods for contaminant monitoring and remediation. In this study, a lanthanide porphyrin-based MOF with dual fluorescence sensing and photocatalytic properties was synthesized and applied for the detection and combined removal of Cr(VI) and ciprofloxacin (CIP). Using different excitation wavelengths, the material exhibited selective detection of Cr(VI) via fluorescence quenching and CIP through fluorescence enhancement. The variation in color intensity of Tb-MOF on 3D EEM spectra enabled simultaneous detection of both contaminants. Additionally, Tb-MOF demonstrated a synergistic removal effect, achieving over 95% removal rates of Cr(VI) and CIP within 90 min, with consistent sensing and catalytic performance across four cycles. Mechanistic investigations revealed that (i) strong coordination between Tb3+ and CIP altered the surface potential of Tb-MOF, enhancing Cr(VI) adsorption; (ii) as an efficient electron acceptor, Cr(VI) promoted electron transfer and its reduction to Cr(III); and (iii) superoxide radicals generated via a type I mechanism played a key role in CIP degradation. This research underscores the potential of Tb-MOF as a multifunctional platform for simultaneous detection and synergistic remediation of mixed pollutants.
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GB/T 7714 | Duan, Longying , Cheng, Ting , Zhu, Yanyue et al. Lanthanide-Porphyrin MOF as a Multifunctional Platform for Detection and Integrated Elimination of Cr(VI) and Ciprofloxacin [J]. | INORGANIC CHEMISTRY , 2025 , 64 (4) : 1983-1993 . |
MLA | Duan, Longying et al. "Lanthanide-Porphyrin MOF as a Multifunctional Platform for Detection and Integrated Elimination of Cr(VI) and Ciprofloxacin" . | INORGANIC CHEMISTRY 64 . 4 (2025) : 1983-1993 . |
APA | Duan, Longying , Cheng, Ting , Zhu, Yanyue , Wang, Yuping , Gao, Yanxin , Bi, Jinhong . Lanthanide-Porphyrin MOF as a Multifunctional Platform for Detection and Integrated Elimination of Cr(VI) and Ciprofloxacin . | INORGANIC CHEMISTRY , 2025 , 64 (4) , 1983-1993 . |
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The global need for clean water and sanitation drives the development of eco-friendly and efficient water treatment technologies to combat biological pollution from pathogens. In this study, a novel heterojunction photocatalyst was synthesized by incorporating ZnIn2S4 into covalent organic frameworks (COFs) to enable environmentally friendly hydrogen peroxide (H2O2) photosynthesis and explore its potential for in situ disinfection. The ZnIn2S4/COF photocatalyst achieved remarkable H2O2 yields of 1325 mu mol center dot g-(1)center dot h-(1), surpassing pristine COF and ZnIn2S4 by factors of 3.12 and 16.2, respectively. The produced H2O2 was efficiently activated into hydroxyl radicals (OH) through reaction with Fe(II), enabling rapid sterilization via a photocatalysis-self-Fenton system. Mechanistic insights, supported by physicochemical characterizations and theoretical calculations, highlighted the role of the internal electric field (IEF) in enhancing carrier separation and transfer, thereby boosting photosynthesis efficiency. This work presents a sustainable approach to H2O2 photosynthesis and activation for disinfection, offering a promising solution to global water treatment challenges.
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GB/T 7714 | Zhuo, Linlin , Dong, Shaofeng , Sham, Yik Tung et al. Internal electric field steering S-scheme charge transfer in ZnIn2S4/COF boosts H2O2 photosynthesis from water and air for sustainable disinfection [J]. | NPJ CLEAN WATER , 2025 , 8 (1) . |
MLA | Zhuo, Linlin et al. "Internal electric field steering S-scheme charge transfer in ZnIn2S4/COF boosts H2O2 photosynthesis from water and air for sustainable disinfection" . | NPJ CLEAN WATER 8 . 1 (2025) . |
APA | Zhuo, Linlin , Dong, Shaofeng , Sham, Yik Tung , Zhang, Jinpeng , Xu, Xiaoying , Ho, Kenrick Chun Kiu et al. Internal electric field steering S-scheme charge transfer in ZnIn2S4/COF boosts H2O2 photosynthesis from water and air for sustainable disinfection . | NPJ CLEAN WATER , 2025 , 8 (1) . |
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Covalent triazine frameworks (CTFs) are emerging as promising platform for photocatalysis, yet their highly symmetric structure leads to significant charge recombination. Herein, we employed a facile non-metallic boron (B) modification with precisely controlled doping site to introduce asymmetric local electron distribution in CTFs, achieving a 15-fold activity enhancement for CO2-to-CH4 conversion. Calculations including frontier orbitals, dipole moments and molecular electrostatic potentials firmly demonstrated the formation of localized polarized electron regions in CTF-1 via B doping. Noteworthily, the primary coordination-activation site for CO2 molecules shifted from triazine ring to benzene ring, with increased adsorption energy (-0.21 vs. -0.55 eV) and a reduced CO2 bond angle (156 degrees vs. 139 degrees). Furthermore, the CO2-to-CH4 pathway was thoroughly clarified based upon the in-situ DRIFTS and energy barriers calculations, where CTF-1 followed the formate route and B-doped CTF utilized the water gas shift reaction. The introduction of B doping lowered energy barrier of *CHO formation for improving CH4 selectivity. This study offers a strategy for enhancing product selectivity by breaking the electronic symmetry of photocatalysts.
Keyword :
Asymmetric electronic distribution Asymmetric electronic distribution Boron doping Boron doping CO2 reduction CO2 reduction Covalent triazine frameworks Covalent triazine frameworks Photocatalysis Photocatalysis
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GB/T 7714 | Chen, Shaokui , Huang, Guiting , Sheng, Hao et al. Asymmetric electronic distribution induced enhancement in photocatalytic CO2-to-CH4 conversion via boron-doped covalent triazine frameworks [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2025 , 685 : 766-773 . |
MLA | Chen, Shaokui et al. "Asymmetric electronic distribution induced enhancement in photocatalytic CO2-to-CH4 conversion via boron-doped covalent triazine frameworks" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 685 (2025) : 766-773 . |
APA | Chen, Shaokui , Huang, Guiting , Sheng, Hao , Huang, Guocheng , Sa, Rongjian , Chen, Qiaoshan et al. Asymmetric electronic distribution induced enhancement in photocatalytic CO2-to-CH4 conversion via boron-doped covalent triazine frameworks . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2025 , 685 , 766-773 . |
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The carrier transfer mechanism of S-scheme heterojunctions has been extensively explored, yet their impact on light absorption performance remains ambiguous. In this work, a finely designed S-scheme heterojunction was developed by coupling oxidation photocatalyst a specific covalent organic framework (COF)-TaTp, and reduction photocatalyst SnS2 (SS) for in-situ H2O2 photo-production and sterilization. The optimized 10% SS/TaTp achieved a 3.45- and 16.87-fold enhancement in H2O2 generation than pure TaTp and SS, respectively, with significant improvements under visible and near-infrared (NIR) light. In-situ XPS, EPR, and Kelvin probe force microscopy (KPFM) verified the S-scheme charge transfer mechanism, underscoring accelerated photo-induced electrons migration and strengthened redox capacity. The internal electric field of 10% SS/TaTp was calculated to be 2.14 and 4.63 times stronger than TaTp and SS. Intriguingly, the electron localization function and partial density of states analyses revealed that the interfacial C-N-S covalent bonds finely tuned the energy band structure and generated hybrid energy levels in the heterojunction, thus improving light harvesting and catalytic performance in both visible-light and NIR region. This work highlights the role of interfacial covalent interactions in tuning energy levels in COF-based S-scheme photocatalysts.
Keyword :
Covalent organic frameworks Covalent organic frameworks Hybrid energy levels Hybrid energy levels In-situ activation In-situ activation Photocatalytic H 2 O 2 production Photocatalytic H 2 O 2 production S -scheme heterojunction S -scheme heterojunction
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GB/T 7714 | Xu, Xiaoying , Dong, Shaofeng , Lv, Jialong et al. Interfacial C-N-S bridged SnS2/COF S-scheme heterojunction with upgraded near-infrared photo-activity for H2O2 synthesis [J]. | APPLIED SURFACE SCIENCE , 2025 , 689 . |
MLA | Xu, Xiaoying et al. "Interfacial C-N-S bridged SnS2/COF S-scheme heterojunction with upgraded near-infrared photo-activity for H2O2 synthesis" . | APPLIED SURFACE SCIENCE 689 (2025) . |
APA | Xu, Xiaoying , Dong, Shaofeng , Lv, Jialong , Huang, Guocheng , Chen, Qiaoshan , Bi, Jinhong . Interfacial C-N-S bridged SnS2/COF S-scheme heterojunction with upgraded near-infrared photo-activity for H2O2 synthesis . | APPLIED SURFACE SCIENCE , 2025 , 689 . |
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Herein, we report a hydrogen-bonded supramolecular hybrid composed of a cobaloxime complex and a covalent organic framework (COF) that achieves photocatalytic overall water splitting. The designed COF features ternary units and dual linkages, which induce asymmetric linkers. Upon photoexcitation, this asymmetry facilitates directed electron transfer and spatially separated redox sites, resulting in a long-lived charge-separated state. Consequently, the COF, hydrogen-bonded with cobaloxime as a hydrogen (H2) production cocatalyst, enables visible-light photocatalytic overall water splitting, simultaneously producing H2 and hydrogen peroxide (H2O2), outperforming the COFs with symmetric linker structures. This strategy of asymmetric structural design offers new insights for the design of photocatalysts with suppressed charge recombination for photocatalysis.
Keyword :
Asymmetric structure Asymmetric structure Covalent organic framework Covalent organic framework Overall water splitting Overall water splitting Photocatalysis Photocatalysis Single site Single site
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GB/T 7714 | Yu, Mingfei , Huang, Junhan , Niu, Qing et al. Asymmetric Structural Design in Cobaloxime-Integrated Covalent Organic Frameworks to Facilitate Photocatalytic Overall Water Splitting [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 . |
MLA | Yu, Mingfei et al. "Asymmetric Structural Design in Cobaloxime-Integrated Covalent Organic Frameworks to Facilitate Photocatalytic Overall Water Splitting" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2025) . |
APA | Yu, Mingfei , Huang, Junhan , Niu, Qing , Li, Liuyi , Yu, Yan , Bi, Jinhong . Asymmetric Structural Design in Cobaloxime-Integrated Covalent Organic Frameworks to Facilitate Photocatalytic Overall Water Splitting . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 . |
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Designing photocatalysts with well-defined structure-function relationships is imperative for propelling the progression of desired photocatalytic oxidation. Herein, the efficient conversion of solar energy to H2O2 and subsequently to hydroxyl radicals (•OH) is achieved through a synergistic interplay between olefin linkage (-C[dbnd]C-) and spatially separated benzene-triazine dual reaction sites within covalent organic frameworks (COFs). The upgraded -C[dbnd]C- can increase the conjugation degree of COFs, which establishes an expanded superstructure for boosting charge separation/transfer and stability. This precise modulation renders more opportunities for the hot electrons to migrate to the benzene site for solar-to-H2O2 generation, and to the triazine site for H2O2-to-•OH, separately. The optimized •OH generation pathway enables remarkable oxidation performances against recalcitrant organic pollutants, and pathogenic microorganisms under visible light irradiation. This work provides new insights for tuning the synergistic interactions of various building blocks within the COFs for the selective generation of highly reactive •OH for environmental remediation. © 2024 Elsevier B.V.
Keyword :
Benzene Benzene Hot electrons Hot electrons Microorganisms Microorganisms Organic pollutants Organic pollutants Solar energy Solar energy
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GB/T 7714 | Zhang, Jinpeng , Huang, Guocheng , Chen, Qiaoshan et al. Upgrading structural conjugation in covalent organic framework with spatial dual sites enables boosting solar-to-H2O2-to-•OH for environmental remediation [J]. | Applied Catalysis B: Environmental , 2024 , 356 . |
MLA | Zhang, Jinpeng et al. "Upgrading structural conjugation in covalent organic framework with spatial dual sites enables boosting solar-to-H2O2-to-•OH for environmental remediation" . | Applied Catalysis B: Environmental 356 (2024) . |
APA | Zhang, Jinpeng , Huang, Guocheng , Chen, Qiaoshan , Wu, Ling , Li, Liuyi , Bi, Jinhong . Upgrading structural conjugation in covalent organic framework with spatial dual sites enables boosting solar-to-H2O2-to-•OH for environmental remediation . | Applied Catalysis B: Environmental , 2024 , 356 . |
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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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Thousands of chemicals have been released into the environment in recent decades. The presence of emerging contaminants (ECs) in water has emerged as a pressing concern. Adsorption is a viable solution for the removal of ECs. Metal-organic frameworks (MOFs) have shown great potential as efficient adsorbents, but their dispersed powder form limits their practical applications. Recently, researchers have developed various separable MOF-based adsorbents to improve their recyclability. The purpose of this review is to summarize the latest developments in the construction of separable MOF-based adsorbents and their applications in adsorbing ECs. The construction strategies for separable MOFs are classified into four categories: magnetic MOFs, MOF-fiber composites, MOF gels, and binder-assisted shaping. Typical emerging contaminants include pesticides, pharmaceuticals and personal care products, and endocrine-disrupting compounds. The adsorption performance of different materials is evaluated based on the results of static and dynamic adsorption experiments. Additionally, the regeneration methods of MOF-based adsorbents are discussed in detail to facilitate effective recycling and reuse. Finally, challenges and potential future research opportunities are proposed, including reducing performance losses during the shaping process, developing assessment systems based on dynamic purification and real polluted water, optimizing regeneration methods, designing multifunctional MOFs, and low-cost, large-scale synthesis of MOFs. © 2024 American Chemical Society.
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GB/T 7714 | Gao, Y. , Zheng, L. , Duan, L. et al. Separable Metal-Organic Framework-Based Materials for the Adsorption of Emerging Contaminants [J]. | Langmuir , 2024 . |
MLA | Gao, Y. et al. "Separable Metal-Organic Framework-Based Materials for the Adsorption of Emerging Contaminants" . | Langmuir (2024) . |
APA | Gao, Y. , Zheng, L. , Duan, L. , Bi, J. . Separable Metal-Organic Framework-Based Materials for the Adsorption of Emerging Contaminants . | Langmuir , 2024 . |
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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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A series of Al3+-doped UiO-66(Ce) MOFs (U(CexAl1−x)) was developed to reveal the roles of metal doping on active site formation and substrate activation in photocatalytic selective transformation of amines to imines. Al3+ doping induced crystal structure distortion to form coordinately unsaturated metal (Al, Ce) sites as Lewis acid sites to chemisorb and activate benzylamine (BA). In situ FTIR revealed that the Al site with stronger acid strength facilitated BA activation. The activation degree of N–H bonds in BA was evaluated by changes of calculated force constant. The intermediate products were confirmed through time-dependent in situ FTIR. The Al3+-doped sample U(Ce0.90Al0.10), the optimal catalyst, showed a significantly increased BA conversion (97.6 %) than that (47.5 %) of undoped sample, which was attributed to enough active sites and the optimal charge mobility. Finally, the present study proposes a synergistic photocatalytic mechanism associated with molecular activation to demonstrate selective oxidation pathways at the molecular level. © 2024 Elsevier Inc.
Keyword :
Active sites Active sites Metal doping Metal doping Photocatalysis Photocatalysis UiO-66(Ce) UiO-66(Ce)
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GB/T 7714 | Liu, C. , Chen, H. , Chen, Q. et al. Active site modulation in UiO-66(Ce) MOFs by Al3+ doping for boosting photocatalysis [J]. | Journal of Catalysis , 2024 , 437 . |
MLA | Liu, C. et al. "Active site modulation in UiO-66(Ce) MOFs by Al3+ doping for boosting photocatalysis" . | Journal of Catalysis 437 (2024) . |
APA | Liu, C. , Chen, H. , Chen, Q. , Bi, J. , Yu, J.C. , Wu, L. . Active site modulation in UiO-66(Ce) MOFs by Al3+ doping for boosting photocatalysis . | Journal of Catalysis , 2024 , 437 . |
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