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学者姓名：毕进红
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Abstract ：
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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Photocatalytic CO2 reduction offers a promising strategy to mitigate the greenhouse effect, yet it remains a challenging process due to the high energy barrier associated with the high stability of CO2. In this study, we synthesized Py-bTDC, a pyrene-based covalent organic framework (COF) enriched with nitrogen and sulfur atoms, and anchored palladium nanoclusters (Pd NCs) onto its structure to enhance CO2 reduction efficiency. The confined Pd NCs amplify the built-in electric field (IEF), enabling efficient photogenerated carrier migration and suppressing electron-hole recombination. Simultaneously, Pd NCs serve as catalytic active sites, optimizing CO2 adsorption and activation. Density functional theory (DFT) calculations reveal that Pd reduces the energy barrier for forming the critical intermediate (*COOH), thereby accelerating CO production. Under visible-light irradiation in a gas-solid system using water as a proton donor, the Pd-3/Py-bTDC composite achieved a CO evolution rate of 17.75 mu molh(-1)g(-1) with 86.0% selectivity. This study advances the design of COF-based photocatalysts by synergistically modulating IEF and the engineering active sites for efficient CO2 reduction.
Keyword ：
CO2 reduction CO2 reduction covalent organic framework covalent organic framework pd nanoclusters pd nanoclusters photocatalysis photocatalysis pyrene-based pyrene-based
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| GB/T 7714 | Lin, Yuling , Lai, Xiaofang , Huang, Guiting et al. Spatial Confinement of Pd Nanoclusters in Pyrene-Based Covalent Organic Frameworks for Boosting Photocatalytic CO2 Reduction [J]. | CHEMISTRY-A EUROPEAN JOURNAL , 2025 , 31 (29) . |
| MLA | Lin, Yuling et al. "Spatial Confinement of Pd Nanoclusters in Pyrene-Based Covalent Organic Frameworks for Boosting Photocatalytic CO2 Reduction" . | CHEMISTRY-A EUROPEAN JOURNAL 31 . 29 (2025) . |
| APA | Lin, Yuling , Lai, Xiaofang , Huang, Guiting , Luo, Jianhui , Chen, Qiaoshan , Huang, Guocheng et al. Spatial Confinement of Pd Nanoclusters in Pyrene-Based Covalent Organic Frameworks for Boosting Photocatalytic CO2 Reduction . | CHEMISTRY-A EUROPEAN JOURNAL , 2025 , 31 (29) . |
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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 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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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 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 , 44 (4) : 2462-2473 . |
| MLA | Liu, Cheng et al. "The defect-modulated UiO-66(Ce) MOFs for enhancing photocatalytic selective organic oxidations" . | RARE METALS 44 . 4 (2024) : 2462-2473 . |
| 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 , 44 (4) , 2462-2473 . |
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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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Here, the mixed metal nodes MOFs, Pd/MIL-100(FeaCub), were constructed as photocatalysts for hydrogenation of alpha,beta-unsaturated aldehyde (UAL) under visible light. 1 wt% Pd/MIL-100(Fe0.81Cu0.19) can convert a range of UAL to saturated aldehydes (SAL) with a high efficiency (approximate to 100 %) and selectivity (approximate to 98 %). The results of XPS and in situ DRIFTS reveal that UAL can be selectively activated via a coordination of -C--C- on Cu2+ sites, determining the high selectivity of the photocatalytic reaction. The mixed metal nodes and Pd clusters can improve the transformation and separation of photogenerated electrons-holes. EPR result suggests that photogenerated carriers can facilitate the generation of H center dot on Pd/MIL-100(Fe0.81Cu0.19), enhancing the catalytic activity. A possible mechanism is proposed for elucidating the catalytic processes at the molecular level. This work provides a valuable strategy for tailoring the selectivity of photocatalytic hydrogenation via selective coordination activation.
Keyword ：
alpha alpha beta-Unsaturated aldehydes beta-Unsaturated aldehydes Coordination activation Coordination activation Hydrogenation Hydrogenation MIL-100(Fe/Cu) MIL-100(Fe/Cu) Photocatalyst Photocatalyst
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| GB/T 7714 | Wang, Zhiwen , Kang, Yueyue , Shi, Yingzhang et al. Selective coordination activation regulating the selectivity for photocatalytic hydrogenation of α,β-unsaturated aldehyde over Pd/ MIL-100(FeaCub) [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2024 , 340 . |
| MLA | Wang, Zhiwen et al. "Selective coordination activation regulating the selectivity for photocatalytic hydrogenation of α,β-unsaturated aldehyde over Pd/ MIL-100(FeaCub)" . | APPLIED CATALYSIS B-ENVIRONMENTAL 340 (2024) . |
| APA | Wang, Zhiwen , Kang, Yueyue , Shi, Yingzhang , Liu, Cheng , Liu, Yunni , Lin, Jun et al. Selective coordination activation regulating the selectivity for photocatalytic hydrogenation of α,β-unsaturated aldehyde over Pd/ MIL-100(FeaCub) . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2024 , 340 . |
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