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学者姓名：陈巧珊
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Abstract ：
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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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 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·- 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. © 2024 Elsevier B.V.
Keyword ：
Antibiotics Antibiotics BaCO3 BaCO3 CO3·- radicals CO3·- radicals Heterostructure Heterostructure Visible-light photocatalysis Visible-light photocatalysis
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| GB/T 7714 | Yu, M. , Kong, X. , Luo, J. 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, M. 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, M. , Kong, X. , Luo, J. , Zhou, H. , Gao, Y. , Zheng, C. 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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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 semiconductors have created a great avenue in visible-light photocatalysis and recently insulator photocatalysis has become an appealing research spot. Herein, a novel waste eggshells derived AgBr-CaCO3 heterostructure was finely designed and constructed through a simple co-precipitation method for efficient antibiotics photo-degradation under visible light. The optimal heterostructure achieved a pseudo-first-order kinetic constant of 6.0 x 10(-2) min(-1) for tetracycline (TC) degradation, with 72 and seven-fold enhancement than eggshell (ES) and AgBr, which also exhibited superior performance towards ofloxacin and sulfamethoxazole. The density functional theory (DFT) calculations revealed that the covalent interaction of Ag-O provided a specific channel for interfacial electrons transfer from the semiconductor to the insulator and thus greatly elevated the photocatalytic activity. The highly selective .CO3- radicals generated by ES, as the main active species, also accelerated the antibiotics degradation. Furthermore, the possible degradation pathways, aquatic toxicity and mutagenicity variation of TC were thoroughly elucidated. This current study illuminated a new pathway for the design of insulator photocatalysts based upon waste solids and demonstrated its application prospect in the field of antibiotics degradation.
Keyword ：
AgBr AgBr CaCO3 CaCO3 Heterostructure Heterostructure Tetracycline Tetracycline Visible -light photocatalysis Visible -light photocatalysis
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| GB/T 7714 | Chen, Qiaoshan , Gao, Ming , Yu, Mingfei et al. Efficient photo-degradation of antibiotics by waste eggshells derived AgBr-CaCO3 heterostructure under visible light [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2023 , 314 . |
| MLA | Chen, Qiaoshan et al. "Efficient photo-degradation of antibiotics by waste eggshells derived AgBr-CaCO3 heterostructure under visible light" . | SEPARATION AND PURIFICATION TECHNOLOGY 314 (2023) . |
| APA | Chen, Qiaoshan , Gao, Ming , Yu, Mingfei , Zhang, Ting , Wang, Jianchun , Bi, Jinhong et al. Efficient photo-degradation of antibiotics by waste eggshells derived AgBr-CaCO3 heterostructure under visible light . | SEPARATION AND PURIFICATION TECHNOLOGY , 2023 , 314 . |
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Semiconductor-based solar-driven CO2 to fuels has been widely reckoned as an ingenious approach to tackle energy crisis and climate change simultaneously. However, the high carrier recombination rate of the photocatalyst severely dampens their photocatalytic uses. Herein, an inorganic-organic heterojunction was constructed by in-situ growing a dioxin-linked covalent organic framework (COF) on the surface of rod-shaped beta-Ga2O3 for solar-driven CO2 to fuel. This novel heterojunction is featured with an ultra-narrow bandgap COF-318 (absorption edge = 760 nm), which is beneficial for fully utilizing the visible light spectrum, and a wide bandgap beta-Ga2O3 (absorption edge = 280 nm) to directional conduct electrons from COF to reduce CO2 without electron-hole recombination occurred. Results showed that the solar to fuels performance over beta-Ga2O3/COF was much superb than that of COF. The optimized Ga2O3/COF achieved an outstanding CO evolution rate of 85.8 mu mol h(-1).g(-1) without the need of any sacrificial agent or cocatalyst, which was 15.6 times more efficient than COF. Moreover, the analyses of photoluminescence electrochemical characterizations and density functional theory (DFT) calculations revealed that the fascinate construction of beta-Ga2O3/COF heterojunction significantly favored charge separation and the directional transfer of photogenerated electrons from COF to beta-Ga2O3 followed by CO2. This study paves the way for developing effective COF-based semiconductor photocatalysts for solar-to-fuel conversion.
Keyword ：
beta-Ga2O3 beta-Ga2O3 CO2 reduction CO2 reduction Covalent organic framework Covalent organic framework Narrow-wide bandgap heterojunction Narrow-wide bandgap heterojunction
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| GB/T 7714 | Yang, Rong , Chen, Qiaoshan , Huang, Guocheng et al. Interfacial engineering of novel inorganic-organic beta-Ga2O3/COF heterojunction for accelerated charge transfer towards artificial photosynthesis [J]. | ENVIRONMENTAL RESEARCH , 2023 , 216 . |
| MLA | Yang, Rong et al. "Interfacial engineering of novel inorganic-organic beta-Ga2O3/COF heterojunction for accelerated charge transfer towards artificial photosynthesis" . | ENVIRONMENTAL RESEARCH 216 (2023) . |
| APA | Yang, Rong , Chen, Qiaoshan , Huang, Guocheng , Bi, Jinhong . Interfacial engineering of novel inorganic-organic beta-Ga2O3/COF heterojunction for accelerated charge transfer towards artificial photosynthesis . | ENVIRONMENTAL RESEARCH , 2023 , 216 . |
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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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Solar-driven photocatalytic hydrogen peroxide (H2O2) production presents a promising avenue for achieving sustainable water disinfection. However, the development of a robust and durable system for practical applications remains a notable and unresolved challenge. Herein, a star photocatalyst, the covalent organic frameworks (COFs), was modified with CdS for boosting environmentally benign H2O2 synthesis. Under simulated sunlight and without sacrificial reagents, the composite material exhibited a boosting capacity for H2O2 production, which was attributable to the establishment of a "step" (S)-scheme transfer pathway and facilitation of adequate oxygen diffusion. Nevertheless, it was found that photocatalytically derived H2O2 alone exhibited inefficient disinfection performance, whereas the addition of Fe-(II) allowed rapid inactivation of Escherichia coli, emphasizing the pivotal importance of integrating photocatalysis and Fenton reactions within the photocatalytic H2O2 production system. Furthermore, a dual-compartment reactor, employing a semipermeable membrane, was devised to spatially segregate photocatalysts from microorganisms. Such an operation mode enabled H2O2 diffusion from the photocatalytic compartment to the microbial compartment, thereby achieving a "long-distance" sterilization manner and simultaneous consummating recovery strategy of the photocatalysts. This study not only provides a paradigmatic approach for boosting the production of H2O2 from a COF-based material but also illuminates an innovative technological option for sustainable photocatalytic-based water disinfection.
Keyword ：
disinfection reactor disinfection reactor Fenton reaction Fenton reaction inactivation inactivation photocatalyticH(2)O(2) production photocatalyticH(2)O(2) production S-scheme heterojunction S-scheme heterojunction
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| GB/T 7714 | He, Yuxin , Zhao, Jiusheng , Sham, Yik-Tung et al. Efficient Hydrogen Peroxide Photosynthesis over CdS/COF for Water Disinfection: The S-Scheme Pathway, Oxygen Adsorption, and Reactor Design [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2023 , 11 (49) : 17552-17563 . |
| MLA | He, Yuxin et al. "Efficient Hydrogen Peroxide Photosynthesis over CdS/COF for Water Disinfection: The S-Scheme Pathway, Oxygen Adsorption, and Reactor Design" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING 11 . 49 (2023) : 17552-17563 . |
| APA | He, Yuxin , Zhao, Jiusheng , Sham, Yik-Tung , Gao, Shengjie , Pan, Min , Chen, Qiaoshan et al. Efficient Hydrogen Peroxide Photosynthesis over CdS/COF for Water Disinfection: The S-Scheme Pathway, Oxygen Adsorption, and Reactor Design . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2023 , 11 (49) , 17552-17563 . |
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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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Vast progress in semiconductor photocatalysis has been witnessed, while the earth-abundant insulators were seldomly explored. In this work, we exploited insulator BaSO4 as photocatalyst by constructing a novel branch of insulator-semiconductor heterostructure with the narrow-gap CuS. The finely designed BaSO4-CuS heterostructure achieved a tetracycline (TC) degradation pseudo-first-order kinetic constant of 1.4 x 10(-2) min(-1), which was 311, 21 and 18 times higher than that of BaSO4, CuS and their physical mixture, respectively. Density functional theory (DFT) calculations unraveled that the intense Cu-O covalent interaction created a specific channel for interfacial electrons transfer from semiconductor to insulator. The elevated redox potential of CuS is vital for the accumulation of center dot O-2(-) and motivation of center dot OH, thus remarkedly accelerating TC mineralization. Furthermore, the degradation pathway and intermediates of TC were thoroughly studied through LC-MS. The current work provides new perspectives to harvest visible-light-driven insulator photocatalysts and demonstrates its promising applications for environmental remediation.
Keyword ：
BaSO4 BaSO4 Degradation mechanism Degradation mechanism Heterostructure Heterostructure Tetracycline Tetracycline Visible-light photocatalysis Visible-light photocatalysis
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| GB/T 7714 | Chen, Qiaoshan , Zhou, Hanqiang , Wang, Jianchun et al. Activating earth-abundant insulator BaSO4 for visible-light induced degradation of tetracycline [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2022 , 307 . |
| MLA | Chen, Qiaoshan et al. "Activating earth-abundant insulator BaSO4 for visible-light induced degradation of tetracycline" . | APPLIED CATALYSIS B-ENVIRONMENTAL 307 (2022) . |
| APA | Chen, Qiaoshan , Zhou, Hanqiang , Wang, Jianchun , Bi, Jinhong , Dong, Fan . Activating earth-abundant insulator BaSO4 for visible-light induced degradation of tetracycline . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2022 , 307 . |
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