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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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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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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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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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Single-atom catalysts (SACs) hold great promise for the electrocatalytic N2 reduction reaction (NRR), yet a comprehensive understanding of coordination microenvironment modulation remains elusive. Herein, Ni SACs with diverse Ni-Nx-C configurations (square-planar: Ni-N4, triangle-cone: Ni-N1-N3, pentagon-planar: Ni-N5, and square-cone: Ni-N1-N4) were theoretically studied. Ni SACs with the Ni-N1-N4 configuration demonstrated the highest stability and suitability for N2 adsorption, hydrogenation (*NN -> *NNH), and inhibition of *H adsorption for H2 evolution. Notably, the additionally coordinated N disrupted the axisymmetric distribution of electrons in Ni-N1-N4, particularly in the z-direction of Ni d z 2 orbitals, inducing the end-adsorbed N2 to adopt an inclined position. The variation in electronic states facilitated the simultaneous sigma and pi interaction between Ni d z2 and N2, forming a strong Ni-N bond (1.89 & Aring;) and promoting N2 activation via p-d hybridization. In light of the calculation results, Ni SACs with the Ni-N1-N4 configuration (Ni20-FAN) were fabricated and displayed a superior NRR activity and Faradaic efficiency of 35.74% at -0.4 V vs RHE. In situ spectroscopic techniques together with density functional theory calculations further unraveled a facile distal pathway for ammonia evolution over Ni-N1-N4 SACs. This work offers an innovative perspective for theory-guided modulation of the SAC coordination microenvironment, introducing asymmetric coordination as an effective strategy for the activation of symmetric inert molecules.
Keyword ：
asymmetric coordination asymmetric coordination coordinationmicroenvironment modulation coordinationmicroenvironment modulation nitrogen electroreduction nitrogen electroreduction p-d hybridization p-d hybridization single atom single atom
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| GB/T 7714 | Chen, Yueling , Luo, Laihao , Wu, Houyi et al. Boosting Nitrogen Activation with Asymmetric Coordinated Ni-N1-N4 Site through p-d Hybridization [J]. | ACS CATALYSIS , 2025 , 15 (13) : 11103-11112 . |
| MLA | Chen, Yueling et al. "Boosting Nitrogen Activation with Asymmetric Coordinated Ni-N1-N4 Site through p-d Hybridization" . | ACS CATALYSIS 15 . 13 (2025) : 11103-11112 . |
| APA | Chen, Yueling , Luo, Laihao , Wu, Houyi , Kong, Xiangyu , Liu, Yan , Huang, Guocheng et al. Boosting Nitrogen Activation with Asymmetric Coordinated Ni-N1-N4 Site through p-d Hybridization . | ACS CATALYSIS , 2025 , 15 (13) , 11103-11112 . |
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The urgent need to address the high prevalence of waterborne diseases in underdeveloped regions necessitates the development of economically viable, decentralized, and sunlight-assisted disinfection techniques. An encouraging solution lies in the utilization of photosynthesized H2O2 to initiate advanced oxidation processes (AOPs). However, challenges persist in the quest to develop efficient photocatalysts and reactor designs. Herein, we present the rational design and synthesis of a metal-free supramolecular photocatalyst achieved via the postfunctionalization of fluorine-substituted covalent organic frameworks (FCOFs) with polyvinylpyrrolidone (PVP). The resulting FCOF/PVP composite establishes intermolecular C-F center dot center dot center dot C=O interactions at the interface, which facilitate accelerated charge separation and transfer, as well as promote efficient intersystem crossing to enhance the formation of molecular triplet excitons. These photophysical enhancements enable dual-pathway H2O2 generation mediated by superoxide radicals (center dot O2-) and singlet oxygen (1O2), yielding a H2O2 production rate of 1763.50 mu mol/g/h from pure water and atmospheric oxygen. The photosynthesized H2O2 is subsequently catalyzed by Fe(II) to generate hydroxyl radicals (center dot OH), achieving effective inactivation of pathogenic bacteria and viruses. A continuous-flow system was further developed to couple photocatalytic H2O2 production with Fenton disinfection, combining the benefits of heterogeneous and homogeneous catalysis while addressing limitations in photocatalyst recovery and light dependency. This system exhibited robust disinfection performance under real water matrices and intermittent light conditions. Economic analysis supports the feasibility of the system for deployment in resource-limited settings, offering a novel material-based approach for decentralized water treatment and global efforts to mitigate waterborne diseases.
Keyword ：
C-F center dot center dot center dot C=O interaction C-F center dot center dot center dot C=O interaction COF-based photocatalyst COF-based photocatalyst Continuous-flow disinfection system Continuous-flow disinfection system Fenton reaction Fenton reaction
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| GB/T 7714 | He, Yuxin , Huang, Guocheng , Guo, Xuejian et al. Engineering intermolecular C-F•••C=O interactions in covalent organic framework promotes dual-path H2O2 photosynthesis for sustainable disinfection [J]. | WATER RESEARCH , 2025 , 285 . |
| MLA | He, Yuxin et al. "Engineering intermolecular C-F•••C=O interactions in covalent organic framework promotes dual-path H2O2 photosynthesis for sustainable disinfection" . | WATER RESEARCH 285 (2025) . |
| APA | He, Yuxin , Huang, Guocheng , Guo, Xuejian , Chen, Shaokui , Chen, Qiaoshan , Yang, Wenjun et al. Engineering intermolecular C-F•••C=O interactions in covalent organic framework promotes dual-path H2O2 photosynthesis for sustainable disinfection . | WATER RESEARCH , 2025 , 285 . |
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The photocatalytic ammonia production is fundamentally constrained by the inertness of N2 molecules and the spatial overlap of photo-redox sites that probably leads to competitive by-products and inevitable reverse reactions. Herein, a well-defined S-scheme heterojunction with spatially separated redox centers was constructed by integrating a covalent organic framework (COF-TaTp) with NiFe layered double hydroxide (NiFe-LDH). The resulting inorganic-organic hybrid (NF30) showcased a remarkable NH3 evolution rate of 411.7 mu g center dot L-1 in pure water without sacrificial agents-3.8-and 12.5-fold higher than the individual counterparts. The enhanced performance primarily stems from the reinforced internal electric field (IEF = 10.4) and oriented charge migration via the specific O-H-C/N interfacial channels, as validated by layered charge difference distribution and augmented surface photovoltage. In situ XPS, DRIFTS, and DFT calculations further revealed a typical Sscheme electron transfer mechanism and an alternating N2 reduction pathway with a substantially lowered energy barrier for rate-determining step (*N2 -> *NNH). This work provides mechanistic insights into charge kinetics across inorganic-organic interfaces and COF-based heterojunction design for efficient solar ammonia production.
Keyword ：
Ammonia production Ammonia production Covalent organic framework Covalent organic framework Internal electronic field Internal electronic field Photocatalysis Photocatalysis S -scheme heterojunction S -scheme heterojunction
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| GB/T 7714 | Yu, Mingfei , Chen, Yueling , Song, Xiaoping et al. Achieving spatially separated photo-redox sites via COFs-based inorganic-organic S-scheme heterojunction for boosting solar ammonia production [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 522 . |
| MLA | Yu, Mingfei et al. "Achieving spatially separated photo-redox sites via COFs-based inorganic-organic S-scheme heterojunction for boosting solar ammonia production" . | CHEMICAL ENGINEERING JOURNAL 522 (2025) . |
| APA | Yu, Mingfei , Chen, Yueling , Song, Xiaoping , Chen, Qiaoshan , Li, Liuyi , Bi, Jinhong . Achieving spatially separated photo-redox sites via COFs-based inorganic-organic S-scheme heterojunction for boosting solar ammonia production . | CHEMICAL ENGINEERING JOURNAL , 2025 , 522 . |
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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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Hydrogen peroxide (H2O2) is recognized as an environmentally benign oxidant with widespread applications in the water treatment and disinfection industry. However, conventional anthraquinone-based methods for H2O2 production are characterized by high energy consumption and the generation of hazardous byproducts, necessitating the development of more sustainable alternatives. In this study, we present an S-scheme heterojunction constructed from MnIn2S4 and a covalent organic framework (COF), which exhibits an enhanced internal electric field (IEF) to facilitate efficient photocatalytic H2O2 synthesis without the use of sacrificial agents. This heterojunction demonstrates superior charge separation and transfer capabilities, achieving a remarkably high H2O2 production rate of 4007 mu mol center dot g-1 center dot h-1 under visible light irradiation and an unprecedented apparent quantum yield of 7.14%. Mechanistic investigations reveal that the S-scheme charge transfer pathway optimizes redox reactions, while the photosynthesized H2O2 and its precursors, superoxide radicals, synergistically disrupt bacterial defense mechanisms by inhibiting key antioxidant enzymes (e.g., superoxide dismutase, catalase, and glutathione) and impairing energy metabolism, ultimately leading to bacterial cell death. Notably, the optimal sample exhibits sustained performance in diverse real water matrices, including river and seawater, under natural sunlight conditions, with negligible effluent toxicity. This work provides a sustainable strategy for H2O2 production and water purification, offering insights into the rational design of advanced photocatalytic materials for the water disinfection industry.
Keyword ：
Covalent organic frameworks Covalent organic frameworks Internal electric field Internal electric field Photocatalytic H 2 O 2 production Photocatalytic H 2 O 2 production S -scheme heterojunction S -scheme heterojunction Water disinfection industry Water disinfection industry
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| GB/T 7714 | Lai, Xiaofang , Lin, Yuling , Yang, Wenjun et al. S-scheme MnIn2S4/COF heterojunction for visible-light-driven H2O2 generation: toward green and efficient water disinfection [J]. | CHEMICAL ENGINEERING SCIENCE , 2025 , 318 . |
| MLA | Lai, Xiaofang et al. "S-scheme MnIn2S4/COF heterojunction for visible-light-driven H2O2 generation: toward green and efficient water disinfection" . | CHEMICAL ENGINEERING SCIENCE 318 (2025) . |
| APA | Lai, Xiaofang , Lin, Yuling , Yang, Wenjun , Chen, Ziyan , Chen, Qiaoshan , Huang, Guocheng et al. S-scheme MnIn2S4/COF heterojunction for visible-light-driven H2O2 generation: toward green and efficient water disinfection . | CHEMICAL ENGINEERING SCIENCE , 2025 , 318 . |
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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 , 64 (22) . |
| MLA | Yu, Mingfei et al. "Asymmetric Structural Design in Cobaloxime-Integrated Covalent Organic Frameworks to Facilitate Photocatalytic Overall Water Splitting" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 22 (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 , 64 (22) . |
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