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学者姓名：毕进红
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Abstract ：
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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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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Covalent organic frameworks (COFs) are promising semiconductor photocatalysts but are still limited in overall water splitting mainly owing to a lack of clear design approaches with which to ameliorate catalytic activities. Here, we demonstrate a synergy of exciton dipole orientation and dynamic reactivity of COFs that enables water splitting for stoichiometric evolution of H2 and O2. The exciton dipole orientation is responsible for driving the spatial separation of photoinduced charges, while the dynamic reactivity of imine bonds of COFs with water and holes is proven for initiating water oxidation. Accordingly, a rationally designed BtS-COF with benzotrithiophene and sulfone units exhibits a much-improved performance in H2 and O2 evolution in neutral water under visible light. Its catalytic efficiency is even superior to some photocatalysts with metal-based water oxidation cocatalyst.
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| GB/T 7714 | Niu, Qing , Deng, Wenfeng , Chen, Yanlei et al. Exciton Dipole Orientation and Dynamic Reactivity Synergistically Enable Overall Water Splitting in Covalent Organic Frameworks [J]. | ACS ENERGY LETTERS , 2024 , 9 (12) : 5830-5835 . |
| MLA | Niu, Qing et al. "Exciton Dipole Orientation and Dynamic Reactivity Synergistically Enable Overall Water Splitting in Covalent Organic Frameworks" . | ACS ENERGY LETTERS 9 . 12 (2024) : 5830-5835 . |
| APA | Niu, Qing , Deng, Wenfeng , Chen, Yanlei , Lin, Qingqing , Li, Liuyi , Liu, Zheyuan et al. Exciton Dipole Orientation and Dynamic Reactivity Synergistically Enable Overall Water Splitting in Covalent Organic Frameworks . | ACS ENERGY LETTERS , 2024 , 9 (12) , 5830-5835 . |
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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 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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Photocatalytic reduction of CO 2 with H 2 O is thought as an environment friendly approach for sustainable development. It is highly desirable but remains challenging to develop photocatalyst with metal -free site for CO 2 reduction. Here, we fabricated a heterostructure by integrating azine-based COF with ZnIn 2 S 4 , where the azine unit in COF acts as metal -free sites for CO 2 adsorption and reduction. The as -formed interfused heterointerface in the heterostructure ensures the effective electron transfer from ZnIn 2 S 4 across the interface to the COF, resulting in a spatial separation of redox sites for CO 2 reduction and water oxidation. The hybrid catalyst exhibits remarkably enhanced photocatalytic activity for CO 2 reduction to CO, which is 8 and 6 times than the COF and ZnIn 2 S 4 , respectively, and is even comparable with some metal -catalyzed CO 2 reduction systems. This study provides a new paradigm to mimic natural photosynthesis by using metal -free site for CO 2 reduction. (c) 2024, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
Keyword ：
CO 2 reduction CO 2 reduction Covalent organic framework Covalent organic framework Heterostructure Heterostructure Metal -free site Metal -free site Photocatalysis Photocatalysis
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| GB/T 7714 | Huang, Haoming , Lin, Qingqing , Niu, Qing et al. Metal- free photocatalytic reduction of CO 2 on a covalent organic framework- based heterostructure [J]. | CHINESE JOURNAL OF CATALYSIS , 2024 , 60 : 201-208 . |
| MLA | Huang, Haoming et al. "Metal- free photocatalytic reduction of CO 2 on a covalent organic framework- based heterostructure" . | CHINESE JOURNAL OF CATALYSIS 60 (2024) : 201-208 . |
| APA | Huang, Haoming , Lin, Qingqing , Niu, Qing , Ning, Jiangqi , Li, Liuyi , Bi, Jinhong et al. Metal- free photocatalytic reduction of CO 2 on a covalent organic framework- based heterostructure . | CHINESE JOURNAL OF CATALYSIS , 2024 , 60 , 201-208 . |
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Covalent organic frameworks (COFs) with excellent structural tunability have emerged as fascinating photocatalysts to fulfill future energy demands. Here, we developed a COFs heterostructure by assembling two COFs for photocatalytic overall water splitting. The resulting heterostructure exhibited an effective spatial separation of photoredox sites originating from the efficient separation of photoinduced charge carriers through an orientated interfacial electron transfer pathway. Accordingly, the heterostructure of the COFs displays excellent activity for stoichiometric water splitting into H-2 and O-2 under 5 W white LED light irradiation. Our efficiencies of H-2 and O-2 evolution rates up to 120 and 58 mu mol g(-1) h(-1) are significantly higher than those reported previously. The combination of experiments and theoretical calculations shows that water oxidation proceeds by a metal-free hydration-mediated pathway. This work sheds light on a rational design of the COF heterostructure with spatially separated photoredox for water splitting.
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| GB/T 7714 | Niu, Qing , Chen, Wei , Pan, Guodong et al. Spatially Separated Photoredox in a Covalent Organic Frameworks Heterostructure Boosting Overall Water Splitting [J]. | ACS MATERIALS LETTERS , 2024 , 6 (4) : 1411-1417 . |
| MLA | Niu, Qing et al. "Spatially Separated Photoredox in a Covalent Organic Frameworks Heterostructure Boosting Overall Water Splitting" . | ACS MATERIALS LETTERS 6 . 4 (2024) : 1411-1417 . |
| APA | Niu, Qing , Chen, Wei , Pan, Guodong , Li, Liuyi , Yu, Yan , Bi, Jinhong et al. Spatially Separated Photoredox in a Covalent Organic Frameworks Heterostructure Boosting Overall Water Splitting . | ACS MATERIALS LETTERS , 2024 , 6 (4) , 1411-1417 . |
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The pursuit of green ammonia synthesis via electrocatalytic nitrogen reduction (NRR) faces challenges in developing high-performance, selective electrocatalysts. Inspired by the nitrogenase Fe-Mo cofactor, this study explores the catalytic efficiency of Mo clusters anchored on Fe5C2 for NRR. We investigate structural stability, N2 adsorption, and Gibbs free energy, revealing that Mon clusters on Fe5C2 demonstrate robust NRR selectivity and notable catalytic activity. Each of the three cluster structures demonstrated superior adsorption capacity in the "side-on" configuration. Among the studied cluster configurations, the Mo5-Fe5C2 shows the lowest limiting potential (-0.24 V), and the Mo4-Fe5C2 exhibits heightened selectivity for NRR, minimizing interference from the hydrogen evolution reaction (HER). This enhanced performance is attributed to the unique structure and interactive dynamics of Mon-Fe5C2 and the electron orbital interactions facilitating direct nitrogen charge transfer. Our findings underscore the potential of Mo cluster-modified Fe5C2 as a pioneering catalyst for electrocatalytic nitrogen reduction.
Keyword ：
Density functional theory Density functional theory Iron carbides Iron carbides Nitrogen reduction reaction Nitrogen reduction reaction Transition metal dope Transition metal dope
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| GB/T 7714 | Chen, Meiyan , Li, Qingyu , Liu, Diwen et al. Theoretical insights into Mo cluster modified Fe5C2 catalysts for electrocatalytic nitrogen reduction [J]. | MATERIALS TODAY COMMUNICATIONS , 2024 , 39 . |
| MLA | Chen, Meiyan et al. "Theoretical insights into Mo cluster modified Fe5C2 catalysts for electrocatalytic nitrogen reduction" . | MATERIALS TODAY COMMUNICATIONS 39 (2024) . |
| APA | Chen, Meiyan , Li, Qingyu , Liu, Diwen , Ma, Zuju , Zhang, Yanjie , Li, Dejing et al. Theoretical insights into Mo cluster modified Fe5C2 catalysts for electrocatalytic nitrogen reduction . | MATERIALS TODAY COMMUNICATIONS , 2024 , 39 . |
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Defect engineering in metal organic frameworks (MOFs) has captured significant attention in the field of photocatalysis. A series of UiO-66(Ce) (UiO = University of Oslo) MOFs with different contents of missing-linker defects have been developed for the photocatalytic selective oxidation of benzylamine (BA) and thioanisole (TA) under visible light. The introduction of missing-linker defects promotes the formation of unsaturated Ce sites with a high Ce3+ content. It also generates a high concentration of oxygen vacancies. In situ Fourier transform infrared spectroscopy (FTIR) results revealed that BA and TA molecules were activated on coordinatively unsaturated Ce sites via the H-NCe and the C-SCe interactions, respectively. Simulated in situ electron paramagnetic resonance (EPR) data indicate that O-2 activation and reduction occur at coordinatively unsaturated Ce3+ sites to form O-2(-). This is accelerated by the Ce3+/Ce4+ redox cycle associated with the photogenerated electrons. The corresponding photogenerated holes are involved in the deprotonation of the activated BA and TA. The most active sample exhibits 98.4% and 95.5% conversion rates for BA and TA oxidation. Mechanisms for the molecular activation are proposed at the molecular level.
Keyword ：
Ce3+/Ce4+ redox cycling Ce3+/Ce4+ redox cycling Defective MOFs Defective MOFs Molecular activation Molecular activation Photocatalytic selective organic oxidation Photocatalytic selective organic oxidation UiO-66(Ce) UiO-66(Ce)
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| GB/T 7714 | Liu, Cheng , Shi, Ying-Zhang , Chen, Qi et al. The defect-modulated UiO-66(Ce) MOFs for enhancing photocatalytic selective organic oxidations [J]. | RARE METALS , 2024 . |
| MLA | Liu, Cheng et al. "The defect-modulated UiO-66(Ce) MOFs for enhancing photocatalytic selective organic oxidations" . | RARE METALS (2024) . |
| APA | Liu, Cheng , Shi, Ying-Zhang , Chen, Qi , Ye, Bing-Hua , Bi, Jin-Hong , Yu, Jimmy C. et al. The defect-modulated UiO-66(Ce) MOFs for enhancing photocatalytic selective organic oxidations . | RARE METALS , 2024 . |
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