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学者姓名:陈巧珊
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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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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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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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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 center dot- 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.
Keyword :
Antibiotics Antibiotics Heterostructure Heterostructure Visible-light photocatalysis Visible-light photocatalysis
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GB/T 7714 | Yu, Mingfei , Kong, Xiangyu , Luo, Jianhui 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, Mingfei 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, Mingfei , Kong, Xiangyu , Luo, Jianhui , Zhou, Hanqiang , Gao, Yanxin , Zheng, Chenghui 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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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 (center dot OH) is achieved through a synergistic interplay between olefin linkage (-C = C-) and spatially separated benzene-triazine dual reaction sites within covalent organic frameworks (COFs). The upgraded -C = 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-center dot OH, separately. The optimized center dot 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 center dot OH for environmental remediation.
Keyword :
Covalent organic frameworks Covalent organic frameworks H2O2 activation H2O2 activation Hydroxyl radicals Hydroxyl radicals Photocatalysis Photocatalysis Spatial dual sites Spatial dual sites
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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-ENVIRONMENT AND ENERGY , 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-ENVIRONMENT AND ENERGY 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-ENVIRONMENT AND ENERGY , 2024 , 356 . |
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Research in contaminants photo-degradation has witnessed significant progress, recently insulator-based catalysts gaining prominence. In this study, N-containing p-type ZnO decorated BaSO4 (ZnO:N-BaSO4) were synthesized and presented a pseudo-first-order kinetic constant of 1.30 x 10-2 min-1 for TC degradation, surpassing that of ZnO:N and their physical mixture by four and seven-fold, respectively. Impressively, the electron transfer in ZnO:N/TC solution interface led to band bending on ZnO:N surface and realized the band matching between ZnO:N and BaSO4. Density functional theory (DFT) calculations unveiled that the strong Zn-O covalent interaction involving 4s states of Zn atoms and 2p states of O atoms, established a distinctive pathway for electron transfer from semiconductor to insulator. Moreover, the catalysts demonstrated robust activity and sustained long-term stability in real wastewater and surface water. This research illuminates the role of wastewater redox potential in semiconductor band adjustment and highlights abundant, eco-friendly insulators as co-catalysts for selective photo-degradation.
Keyword :
Energy band matching Energy band matching Insulator Insulator p-type ZnO p-type ZnO Tetracycline Tetracycline
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GB/T 7714 | Zhang, Ting , Luo, Jianhui , Chen, Qiaoshan et al. Reaction solution mediated photo-degradation process and mechanism of tetracycline via semiconductor-insulator composite ZnO:N-BaSO4 [J]. | APPLIED SURFACE SCIENCE , 2024 , 661 . |
MLA | Zhang, Ting et al. "Reaction solution mediated photo-degradation process and mechanism of tetracycline via semiconductor-insulator composite ZnO:N-BaSO4" . | APPLIED SURFACE SCIENCE 661 (2024) . |
APA | Zhang, Ting , Luo, Jianhui , Chen, Qiaoshan , Bi, Jinhong . Reaction solution mediated photo-degradation process and mechanism of tetracycline via semiconductor-insulator composite ZnO:N-BaSO4 . | APPLIED SURFACE SCIENCE , 2024 , 661 . |
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The construction of step-scheme (S-scheme) heterojunctions has emerged as a widely adopted strategy for achieving photocatalytic hydrogen peroxide (H2O2) generation. In this study, we employed an approach to deposit indium sulfide (In2S3) onto a Schiff-base covalent organic framework (COF), namely TpMA, for H2O2 photosynthesis and its sterilization application. The optimized photocatalyst, 10%TpMA/In2S3, exhibited remarkable photocatalytic performance, yielding a substantial H2O2 output of 311.07 mu mol/L. A series of advanced instrumental analyses and density functional theory (DFT) results indicated that the establishment of the S-scheme heterojunction played a pivotal role in facilitating efficient charge carrier transfer and separation. Specifically, the formation of a built-in electric field was probed and quantified. Furthermore, the H2O2 exhibited the capability to undergo direct catalysis by Fe(II), which substantially facilitated the inactivation of pathogenic bacteria. This work unveils insight into the COF-based S-scheme photocatalysts and offers a sustainable approach for environmentally friendly H2O2 production for sterilization purposes.
Keyword :
Built-in Electric Field Built-in Electric Field Covalent organic frameworks Covalent organic frameworks In situ oS In situ oS S-scheme heterojunction S-scheme heterojunction
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GB/T 7714 | Chen, Hanye , Gao, Shengjie , Huang, Guocheng et al. Built-in electric field mediated S-scheme charge migration in COF/In2S3 heterojunction for boosting H2O2 photosynthesis and sterilization [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2023 , 343 . |
MLA | Chen, Hanye et al. "Built-in electric field mediated S-scheme charge migration in COF/In2S3 heterojunction for boosting H2O2 photosynthesis and sterilization" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 343 (2023) . |
APA | Chen, Hanye , Gao, Shengjie , Huang, Guocheng , Chen, Qiaoshan , Gao, Yanxin , Bi, Jinhong . Built-in electric field mediated S-scheme charge migration in COF/In2S3 heterojunction for boosting H2O2 photosynthesis and sterilization . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2023 , 343 . |
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Covalent organic frameworks (COFs) are crystalline porous materials with enormous potential for realiz-ing solar-driven CO2-to-fuel conversion, yet the sluggish transfer/separation of photoinduced electrons and holes remains a compelling challenge. Herein, a step (S)-scheme heterojunction photocatalyst (CuWO4-COF) was rationally fabricated by a thermal annealing method for boosting CO2 conversion to CO. The optimal CuWO4/COF composite sample, integrating 10 wt% CuWO4 with an olefin (CC) linked COF (TTCOF), achieved a remarkable gas-solid phase CO yield as high as 7.17 +/- 0.35 lmol g-1h-1 under visible light irradiation, which was significantly higher than the pure COF (1.6 +/- 0.29 lmol g-1h-1). The enhanced CO2 conversion rate could be attributable to the interface engineering effect and the formation of internal electric field (IEF) directing from TTCOF to CuWO4 according to the theoretical calculation and experimental results, which also proves the electrons transfer from TTCOF to CuWO4 upon hybridization. In addition, driven by the IEF, the photoinduced electrons can be steered from CuWO4 to TTCOF under visible light irradiation as well-elucidated by in-situ irradiated X-ray photoelectron spectroscopy, verify-ing the S-scheme charge transfer pathway over CuWO4/COF composite heterojunctions, which greatly foster the photoreduction activity of CO2. The preparation technique of the S-scheme heterojunction pho-tocatalyst in this study provides a paradigmatic protocol for photocatalytic solar fuel generation. (c) 2023 Elsevier Inc. All rights reserved.
Keyword :
CO2 reduction CO2 reduction Covalent organic frameworks Covalent organic frameworks CuWO4 CuWO4 Photocatalysis Photocatalysis S-scheme S-scheme
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GB/T 7714 | Niu, Qing , Chen, Qiaoshan , Huang, Guocheng et al. Build-in electric field in CuWO4/covalent organic frameworks S-scheme photocatalysts steer boosting charge transfer for photocatalytic CO2 reduction [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2023 , 643 : 102-114 . |
MLA | Niu, Qing et al. "Build-in electric field in CuWO4/covalent organic frameworks S-scheme photocatalysts steer boosting charge transfer for photocatalytic CO2 reduction" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 643 (2023) : 102-114 . |
APA | Niu, Qing , Chen, Qiaoshan , Huang, Guocheng , Li, Liuyi , He, Yunhui , Bi, Jinhong . Build-in electric field in CuWO4/covalent organic frameworks S-scheme photocatalysts steer boosting charge transfer for photocatalytic CO2 reduction . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2023 , 643 , 102-114 . |
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