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学者姓名:成佳佳
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Persulfate-based advanced oxidation technology, due to its high efficiency, controllability, and safety, shows great potential for the deep removal of organic pollution, yet its mineralization efficiency is hindered by the lack of synergy between radical and nonradical pathways. Herein, we present defective carbon nitride (DCN) as a highly efficient peroxymonosulfate (PMS) activation catalyst that couples nonradical aggregation with radical mineralization. The tailored electronic structure of the DCN framework enhances visible-light absorption, photogenerated charge separation, and electron transfer ability due to a built-in electric field. DCN effectively interacts with PMS to rapidly accumulate pollutants from the bulk solution onto the catalyst surface via an electron-transfer pathway. Simultaneously, the accumulated pollutants undergo in-situ decomposition by center dot SO4- radicals formed on the catalyst surface under visible light irradiation, achieving a remarkable 98 % mineralization ratio. The mixed-pathway process demonstrates excellent cyclic stability and environmental robustness. This study introduces a novel strategy to enhance the catalytic oxidation performance of metal-free catalysts by controlling persulfate activation pathways for water decontamination.
Keyword :
Carbon nitride Carbon nitride Peroxymonosulfate Peroxymonosulfate Photocatalysis Photocatalysis Pollutant mineralization Pollutant mineralization Synergistic Synergistic
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GB/T 7714 | Ming, Hongbo , Ruan, Wenqi , Yuan, Xiaoying et al. Defective carbon nitride-Mediated peroxymonosulfate activation: Synergistic radical and nonradical pathways for enhanced pollutant mineralization [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 360 . |
MLA | Ming, Hongbo et al. "Defective carbon nitride-Mediated peroxymonosulfate activation: Synergistic radical and nonradical pathways for enhanced pollutant mineralization" . | SEPARATION AND PURIFICATION TECHNOLOGY 360 (2025) . |
APA | Ming, Hongbo , Ruan, Wenqi , Yuan, Xiaoying , Cheng, Jiajia , Yang, Can , Hou, Yidong et al. Defective carbon nitride-Mediated peroxymonosulfate activation: Synergistic radical and nonradical pathways for enhanced pollutant mineralization . | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 360 . |
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The enantioselective separation of racemate, particularly those containing C(sp3 )-H bonds knowns for their high bond dissociation energies and significant polarity, presents a significant challenge in pharmaceutical synthesis. Recent advances have witnessed the fusion of photocatalysis with hydrogen atom transfer (HAT) methodologies, marking a notable trend in synthesis of chiral molecules. This technique uses the excitation of a catalyst to activate substrates, enabling the selective isomerization of chiral centers containing C(sp3 ) configurations. This process distinctively facilitates the direct activation of the C(sp3 )-H bond in targeted reagents. This review systematically discusses the photocatalytic isomerization of various chiral molecule featuring C(sp3 )-H centers, capable of undergoing deracemization through two primary HAT mechanisms: direct and indirect pathways. From the perspective of synthetic organic chemistry, this field has progressed towards the development of isomerization strategies for molecules that incorporate an activating group at the alpha-position adjacent to the C(sp3 ) chiral center. Moreover, it covers methodologies applicable to molecules characterized by specific C-C and C-S bond configurations. The integration of photocatalysis with HAT technology thus provides valuable strategies for the synthesis of enantiopure compounds with enhanced selectivity and efficiency. (c) 2025 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
Keyword :
Deracemization Deracemization Hydrogen atom transfer Hydrogen atom transfer Photocatalysis Photocatalysis
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GB/T 7714 | Liu, Yuan , Yin, Zhu , Yang, Xintuo et al. Advances in photocatalytic deracemization of sp3-hybridized chiral centers via hydrogen atom transfer [J]. | CHINESE CHEMICAL LETTERS , 2025 , 36 (5) . |
MLA | Liu, Yuan et al. "Advances in photocatalytic deracemization of sp3-hybridized chiral centers via hydrogen atom transfer" . | CHINESE CHEMICAL LETTERS 36 . 5 (2025) . |
APA | Liu, Yuan , Yin, Zhu , Yang, Xintuo , Cheng, Jiajia . Advances in photocatalytic deracemization of sp3-hybridized chiral centers via hydrogen atom transfer . | CHINESE CHEMICAL LETTERS , 2025 , 36 (5) . |
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We present here a catalytic enantioconvergent amination of alcohols for efficient access to chiral C2- and C3-substituted benzomorpholines. The racemic amino alcohol substrates of different substitution patterns, which are readily available from a common precursor, can be converted to the enantioenriched heterocycles in a highly atom- and step-economical fashion. In particular, an unprecedented asymmetric amination of racemic primary alcohols via dynamic kinetic resolution is achieved under cooperative iridium/iron catalysis, resulting in highly enantioendifficult to access otherwise. [GRAPHICS] .
Keyword :
atom economy atom economy divergent synthesis divergent synthesis dynamic kinetic resolution dynamic kinetic resolution enantioconvergent heterocycle synthesis enantioconvergent heterocycle synthesis redox-neutral catalysis redox-neutral catalysis substituted benzomorpholines substituted benzomorpholines
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GB/T 7714 | Gao, Yaru , Hong, Guorong , Zhang, Lei et al. Asymmetric Amination of Primary Alcohols via Dynamic Kinetic Resolution: Enantioconvergent Access to Chiral Benzomorpholines [J]. | CCS CHEMISTRY , 2025 , 7 (1) : 80-90 . |
MLA | Gao, Yaru et al. "Asymmetric Amination of Primary Alcohols via Dynamic Kinetic Resolution: Enantioconvergent Access to Chiral Benzomorpholines" . | CCS CHEMISTRY 7 . 1 (2025) : 80-90 . |
APA | Gao, Yaru , Hong, Guorong , Zhang, Lei , Ye, Ke-Yin , Cheng, Jiajia , Yang, Bin-Miao et al. Asymmetric Amination of Primary Alcohols via Dynamic Kinetic Resolution: Enantioconvergent Access to Chiral Benzomorpholines . | CCS CHEMISTRY , 2025 , 7 (1) , 80-90 . |
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Heterogeneous photoelectrocatalysis systems have recently seen significant growth in organic transformations, but are limited by the inherent physicochemical properties of electrode materials. To enhance selectivity in these processes, we propose an innovative advancement in the rational design of photoanodes. Specifically, we incorporated cobalt porphyrin co-catalysts with confined Co sites onto bismuth vanadate films as a photoanode. This photoanode significantly enhances the efficacy of styrene epoxidation, achieving selectivity and conversion rates of 90 % and 99 %, respectively. Notably, the reaction utilizes water as the sole oxygen source, operates at room temperature, and is easily scalable for gram-scale synthesis. The developed photoanode demonstrates robust performance across various alkene substrates. Operando characterizations reveal that during the epoxidation reaction, the confined Co sites within the porphyrin structure catalyze the oxidation of H2O to form Co-O*, serving as critical intermediates that facilitate cyclization reactions via one-electron processes. This study introduces an innovative heterogeneous photoelectrocatalysis strategy with customizable active sites tailored for selective catalytic organic transformations.
Keyword :
Epoxidation Epoxidation Heterogeneous Heterogeneous Photoelectrocatalysis Photoelectrocatalysis Selectivity Selectivity
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GB/T 7714 | Wu, Haisu , Wang, Yankun , Huang, Meirong et al. Alkene Epoxidation with Water by Confined Active Co Sites on BiVO4 Photoanodes under Visible Light [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (7) . |
MLA | Wu, Haisu et al. "Alkene Epoxidation with Water by Confined Active Co Sites on BiVO4 Photoanodes under Visible Light" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 7 (2025) . |
APA | Wu, Haisu , Wang, Yankun , Huang, Meirong , Cheng, Jiajia , Sa, Baisheng , Fang, Yuanxing et al. Alkene Epoxidation with Water by Confined Active Co Sites on BiVO4 Photoanodes under Visible Light . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (7) . |
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The integration of heterogeneous photocatalysts with nickel catalysis is garnering considerable interest for their capacity to enable distinct metal-photoredox processes for organic synthesis. However, the challenge about robustness and recyclability of the photocatalyst persists. Herein, a crystalline carbon nitride (MCN-B) photocatalyst with intentionally introduced defects and a dedicated designed active site has been presented. Results reveal by incorporating the deprotonated cyano-group (N--CN) sites, this host material could provide stable binding sites for Ni (II) ions through the Hard-Soft Acid-Base (HSAB) effect, thereby facilitating charge transmission between semiconductor and metal centers. Consequently, the integrated carbon nitride nickel (Ni/MCNB) heterogeneous photocatalyst demonstrates high effectiveness in diverse photocatalytic C-N coupling reactions (21 examples, up to 93% yield) under conditions free from organic ligands and additives, which shows competent performance to the homogeneous catalysts. Moreover, the Ni/MCN-B catalyst demonstrates remarkable recyclability, maintaining its photoredox efficiency after 10 cycles with minimal loss of activity and a diminished metal leaching rate, which signifies a substantial advancement in the field of photocatalytic system design.
Keyword :
Carbon nitride Carbon nitride Cross-coupling Cross-coupling Crystalline polymer Crystalline polymer Photocatalysis Photocatalysis
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GB/T 7714 | Zhang, Huali , Chen, Xiaoxiao , Cheng, Jiajia et al. Heterogeneous metallaphotocatalytic Cross-Coupling reactions by a carbon Nitride-Nickel catalyst [J]. | JOURNAL OF CATALYSIS , 2024 , 433 . |
MLA | Zhang, Huali et al. "Heterogeneous metallaphotocatalytic Cross-Coupling reactions by a carbon Nitride-Nickel catalyst" . | JOURNAL OF CATALYSIS 433 (2024) . |
APA | Zhang, Huali , Chen, Xiaoxiao , Cheng, Jiajia , Yang, Xintuo , Lin, Wei , Hou, Yidong et al. Heterogeneous metallaphotocatalytic Cross-Coupling reactions by a carbon Nitride-Nickel catalyst . | JOURNAL OF CATALYSIS , 2024 , 433 . |
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A novel and efficient approach for the synthesis of alpha, beta-unsaturated sulfones through heterogeneous photocatalyzed C-S coupling reactions have been developed. The use of molten-salt method derived carbon nitride (MCN), a transition metal-free polymeric photocatalyst, combined with enhanced crystallinity and potassium iodide as an additive, effectively modulates photogenerated reactive redox species, markedly increasing the overall reaction selectivity. This method achieves the shortest reaction time (2 h) with high yield (up to 95 %) among the reported heterogeneous catalytic C-S bond formation reactions, matching the efficiency of the homogeneous photocatalysts. Furthermore, the application to challenging alkyne substrates has been demonstrated, underscoring the potential for a broad range of applications in pharmaceutical research and synthetic chemistry. A transition metal-free heterogeneous photocatalytic C-S coupling reaction has been developed. Through optimizing the crystallinity of photocatalyst and incorporating potassium iodide, the distribution of photogenerated redox species are effectively modulated to enhance the formation of the sulfonyl radical and (iodoethynyl)benzene. This method thus achieves high yields of up to 95 % in a significantly reduced reaction time of 2 hours. image
Keyword :
Carbon nitride Carbon nitride Crystallinity Crystallinity C-S coupling C-S coupling Heterogenous photocatalysis Heterogenous photocatalysis
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GB/T 7714 | Liu, Chen , Ma, Yukun , Lian, Ronghong et al. Regulation of Photogenerated Redox Species through High Crystallinity Carbon Nitride for Improved C-S Coupling Reactions [J]. | CHEMSUSCHEM , 2024 , 17 (10) . |
MLA | Liu, Chen et al. "Regulation of Photogenerated Redox Species through High Crystallinity Carbon Nitride for Improved C-S Coupling Reactions" . | CHEMSUSCHEM 17 . 10 (2024) . |
APA | Liu, Chen , Ma, Yukun , Lian, Ronghong , Chen, Jiayin , Yang, Mingcheng , Cheng, Jiajia . Regulation of Photogenerated Redox Species through High Crystallinity Carbon Nitride for Improved C-S Coupling Reactions . | CHEMSUSCHEM , 2024 , 17 (10) . |
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A photocatalytic process was developed for intermolecular reductive coupling of aliphatic ketones with alkynes/alkenes to furnish tertiary alcohols. Mechanistic studies support that boron carbonitrides (BCN) promote the single electron reduction of unactivated aliphatic ketones to generate ketyl radicals with visible light irradiation, which then react with alkynes and alkenes to afford the allylic and aliphatic alcohols, respectively. The heterogeneous photocatalytic system is compatible with diverse substrates including pharmaceutical-related molecules (43 examples) with reusability and scale-up experiments, verifying the complementary synthetic utility of this method to the homogeneous catalysts.
Keyword :
aliphatic ketones aliphatic ketones intermolecular cross-coupling intermolecular cross-coupling ketyl radical ketyl radical tertiary alcohols tertiary alcohols
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GB/T 7714 | Xia, Yanping , Sun, Luyang , Cheng, Jiajia et al. Intermolecular reductive coupling of aliphatic ketones with alkynes and alkenes by BCN photocatalysts [J]. | SCIENCE CHINA-CHEMISTRY , 2024 , 68 (1) : 181-185 . |
MLA | Xia, Yanping et al. "Intermolecular reductive coupling of aliphatic ketones with alkynes and alkenes by BCN photocatalysts" . | SCIENCE CHINA-CHEMISTRY 68 . 1 (2024) : 181-185 . |
APA | Xia, Yanping , Sun, Luyang , Cheng, Jiajia , Wang, Sibo , Zheng, Meifang , Wang, Xinchen . Intermolecular reductive coupling of aliphatic ketones with alkynes and alkenes by BCN photocatalysts . | SCIENCE CHINA-CHEMISTRY , 2024 , 68 (1) , 181-185 . |
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This study describes the synthesis and potential applications of pentaaryl-substituted pyrroles. We report a Pd-catalyzed approach for their preparation from 4,5-diyne-9-fluorenone (1,7-diyne) and aromatic amines. The target nitrogen-doped corannulenes (CO-hub-Ncor) were investigated computationally to understand their electronic properties. While the conversion of pyrroles to CO-hub-Ncor is underway, the pyrroles themselves hold promise as valuable building blocks for N-doped buckybowls. Additionally, the synthesized pyrrole derivatives exhibit interesting reactivity, including pyrrole oxidation, leading to a ring-opening product, specifically a dicarbonyl compound.
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GB/T 7714 | Yang, Sha , Zhou, Jie , Gan, Ziyang et al. Synthesis, structure, and reactivity of fully aryl-substituted pyrroles: toward the synthesis of nitrogen-doped buckybowls [J]. | ORGANIC & BIOMOLECULAR CHEMISTRY , 2024 , 23 (4) : 822-826 . |
MLA | Yang, Sha et al. "Synthesis, structure, and reactivity of fully aryl-substituted pyrroles: toward the synthesis of nitrogen-doped buckybowls" . | ORGANIC & BIOMOLECULAR CHEMISTRY 23 . 4 (2024) : 822-826 . |
APA | Yang, Sha , Zhou, Jie , Gan, Ziyang , Wu, Shuai , Shi, Dan , Yan, Hong et al. Synthesis, structure, and reactivity of fully aryl-substituted pyrroles: toward the synthesis of nitrogen-doped buckybowls . | ORGANIC & BIOMOLECULAR CHEMISTRY , 2024 , 23 (4) , 822-826 . |
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In this study, we report a sustainable, visible light and heterogeneous photocatalytic system to address these issues, using the ternary sulfide ZnIn2S4 (ZIS) as a photoredox catalyst. Our protocol uses visible light irradiation to activate the photoredox catalyst, generating acyl radicals from aldehydes. The methodology demonstrated a broad substrate scope and commendable recyclability. The method also proved capable of scaling to the gram level while maintaining high efficiency, thus highlighting the robustness and reusability of ZIS. This work not only proposes a novel method for the heterogeneous photocatalytic Minisci-type alkylation reaction, but also contributes a valuable approach towards enhancing the efficacy and sustainability of photocatalysts within the pharmaceutical industry. © 2024 Fudan University
Keyword :
Alkylation Alkylation Heterogeneous photocatalysis Heterogeneous photocatalysis Minisci reaction Minisci reaction Quinolines Quinolines ZnIn2S4 ZnIn2S4
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GB/T 7714 | He, C. , Chen, J. , Yang, M. et al. Advancing sustainable quinolines synthesis via ZnIn2S4 heterogeneous photocatalysis [J]. | Green Synthesis and Catalysis , 2024 . |
MLA | He, C. et al. "Advancing sustainable quinolines synthesis via ZnIn2S4 heterogeneous photocatalysis" . | Green Synthesis and Catalysis (2024) . |
APA | He, C. , Chen, J. , Yang, M. , Gong, X. , Cheng, J. . Advancing sustainable quinolines synthesis via ZnIn2S4 heterogeneous photocatalysis . | Green Synthesis and Catalysis , 2024 . |
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The ionic structure of poly(heptazine imides) has a strong implication in photocatalytic hydrogen generation. From numerous reports, it is evident that these materials are also superior to covalent carbon nitrides in various organic transformations. However, the reason has been remaining vague. Herein, we report the design of a molten-salt carbon nitride (MCN) featuring ionic structure represented by negatively charged organic polymeric scaffold and K+ counterions and application of this material as the photocatalyst in synthesis of pharmaceutically relevant fluorinated heterocycles under visible light under the redox neutral conditions. K(+ )ions serve as the sites for sorption of ethyl bromodifluoroacetate, while the electronically excited state of MCN acts as the single electron transfer agent, enabling generation of difluoroalkyl radicals from the substrate. Combination of these two features endows a material that outperforms homogeneous photocatalysts and covalent carbon nitrides. Our protocol expands the application of carbon nitrides in synthesis of organic compounds with complex structure and provides fresh perspectives on the factors contributing to the enhanced photocatalytic efficiency of poly(heptazine imides).
Keyword :
carbon nitride carbon nitride electron transmission electron transmission fluorine fluorine photocatalysis photocatalysis substrate activation substrate activation
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GB/T 7714 | Wang, Chong , Lin, Shiru , Lu, Yichun et al. Enhancing Photocatalytic Redox Activity of Polymeric Carbon Nitride for Valuable Fluorinated Heterocycles through Fast-Track Electron Highways [J]. | ACS CATALYSIS , 2024 , 14 (15) : 11308-11317 . |
MLA | Wang, Chong et al. "Enhancing Photocatalytic Redox Activity of Polymeric Carbon Nitride for Valuable Fluorinated Heterocycles through Fast-Track Electron Highways" . | ACS CATALYSIS 14 . 15 (2024) : 11308-11317 . |
APA | Wang, Chong , Lin, Shiru , Lu, Yichun , Hou, Yuchen , Savateev, Oleksandr , Cheng, Jiajia . Enhancing Photocatalytic Redox Activity of Polymeric Carbon Nitride for Valuable Fluorinated Heterocycles through Fast-Track Electron Highways . | ACS CATALYSIS , 2024 , 14 (15) , 11308-11317 . |
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