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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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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 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 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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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 et al. "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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A metal-insulator-semiconductor (MIS) ternary photo-system was intricately crafted through precise amalgamation polyvinylpyrrolidone (PVP)-capped metal Cu with typical covalent triazine framework CTF-1 via electrostatic self-assembly. The 2 % Cu-PVP-CTF exhibited an impressive CH4 yield of 80.7 mu mol & sdot;g � 1 & sdot;h- 1 with selectivity of 96.8 % under visible light, representing a 2.3-fold and 112-fold improvement over Schottky-type Cu-CTF and pristine CTF-1, respectively. In-situ XPS and VASP-diff calculations unfolded that the ultrathin PVP insulating layer significantly expedited interfacial charges tunneling, corroborated by smaller lifetime tau 2 determined via femtosecond transient absorption spectroscopy. The intermediates of paramount importance in CO2 reduction like *COOH and *HCHO were meticulously monitored by in-situ Fourier infrared spectroscopy. DFT calculations elucidated that Cu-PVP-CTF was notably more adept at facillitating the rate-determining step (*COOH -> *CO) to produce CH4 than Cu-CTF. This work tamps the groundwork for conceptional roadmap in designing novel MIS photo-system for CO2 conversion.
Keyword ：
Carbon dioxide reduction Carbon dioxide reduction Covalent triazine-based frameworks Covalent triazine-based frameworks Metal-insulator-semiconductor Metal-insulator-semiconductor Methane evolution Methane evolution Visible-light photocatalysis Visible-light photocatalysis
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| GB/T 7714 | Chen, Qiaoshan , Chen, Yueling , Yu, Mingfei et al. Modulating interfacial charges in CTF-based metal-insulator-semiconductor promotes selective CO2 reduction to CH4 [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 482 . |
| MLA | Chen, Qiaoshan et al. "Modulating interfacial charges in CTF-based metal-insulator-semiconductor promotes selective CO2 reduction to CH4" . | CHEMICAL ENGINEERING JOURNAL 482 (2024) . |
| APA | Chen, Qiaoshan , Chen, Yueling , Yu, Mingfei , Xu, Bin , Wu, Houyi , Li, Liuyi et al. Modulating interfacial charges in CTF-based metal-insulator-semiconductor promotes selective CO2 reduction to CH4 . | CHEMICAL ENGINEERING JOURNAL , 2024 , 482 . |
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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.
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| GB/T 7714 | Gao, Yanxin , Zheng, Lisi , Duan, Longying et al. Separable Metal-Organic Framework-Based Materials for the Adsorption of Emerging Contaminants [J]. | LANGMUIR , 2024 , 40 (30) : 15365-15388 . |
| MLA | Gao, Yanxin et al. "Separable Metal-Organic Framework-Based Materials for the Adsorption of Emerging Contaminants" . | LANGMUIR 40 . 30 (2024) : 15365-15388 . |
| APA | Gao, Yanxin , Zheng, Lisi , Duan, Longying , Bi, Jinhong . Separable Metal-Organic Framework-Based Materials for the Adsorption of Emerging Contaminants . | LANGMUIR , 2024 , 40 (30) , 15365-15388 . |
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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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