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学者姓名：成佳佳
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Abstract ：
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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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). © 2024 The Authors. Published by American Chemical Society.
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, C. , Lin, S. , Lu, Y. 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, C. 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, C. , Lin, S. , Lu, Y. , Hou, Y. , Savateev, O. , Cheng, J. . 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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Carbon nitride (CN) polymers exhibit tunable and fascinating physicochemical properties and are thus an essential class of photocatalytic materials with potential applications. Although significant progress has been made in the fabrication of CN, the preparation of metal-free crystalline CN via a straightforward method remains a considerable challenge. Herein, we describe a new attempt to synthesize crystalline carbon nitride (CCN) with a well-developed structure through regulation of the polymerization kinetics. The synthetic process involves the pre-polymerization of melamine to remove most of the ammonia and further calcination of the pre-heated melamine in the presence of copper oxide as an ammonia absorbent. Copper oxide can decompose the ammonia produced by the polymerization process, thereby promoting the reaction. These conditions facilitate the polycondensation process while avoiding carbonization of the polymeric backbone at high temperatures. Owing to the high crystallinity, nanosheet structure, and efficient charge-carrier transmission capacity, the as-prepared CCN catalyst shows much higher photocatalytic activity than its counterparts. Our study provides a novel strategy for the rational design and synthesis of high-performance carbon nitride photocatalysts by simultaneously optimizing polymerization kinetics and crystallographic structures.
Keyword ：
Carbon nitride Carbon nitride Crystalline Crystalline Hydrogen production Hydrogen production Photocatalysis Photocatalysis Polymerization kinetics Polymerization kinetics
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| GB/T 7714 | Wang, Chong , Xiao, Hongxiang , Lu, Yichun et al. Regulation of Polymerization Kinetics to Improve Crystallinity of Carbon Nitride for Photocatalytic Reactions [J]. | CHEMSUSCHEM , 2023 , 16 (16) . |
| MLA | Wang, Chong et al. "Regulation of Polymerization Kinetics to Improve Crystallinity of Carbon Nitride for Photocatalytic Reactions" . | CHEMSUSCHEM 16 . 16 (2023) . |
| APA | Wang, Chong , Xiao, Hongxiang , Lu, Yichun , Lv, Jinliang , Yuan, Zhanhui , Cheng, Jiajia . Regulation of Polymerization Kinetics to Improve Crystallinity of Carbon Nitride for Photocatalytic Reactions . | CHEMSUSCHEM , 2023 , 16 (16) . |
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The persulfate-based nonradical reaction process has gained increasing attention in removing organic contaminants, and the process dramatically needs affordable, robust, high-performance heterogeneous catalysts. Herein, dimethyl formamide (DMF) incorporated graphitic carbon nitride (DCN) was synthesized. The molecular engineering of the heptazine unit in DCN improves the electron mobility, strengthens the built-in electric field, and provides abundant active sites, thus enabling DCN to efficiently activate PMS for organic degradation, with 100 % removal of BPA within 12 min. The investigation of the reactive species and electrochemical properties confirmed the direct electron transfer in the PMS activation for organic degradation over DCN. More importantly, DCN can be used as a membrane catalyst in a flowing catalytic unit, enabling continuous water purification and catalyst regeneration. This work provides novel guidance for metal-free catalyst design and profound insights into the persulfate-based heterogeneous catalytic oxidation process for water decontamination technology.
Keyword ：
Carbon nitride Carbon nitride Electronic structure Electronic structure Electron transfer Electron transfer Membrane Membrane Peroxymonosulfate Peroxymonosulfate
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| GB/T 7714 | Ming, Hongbo , Bian, Xiaoqiong , Cheng, Jiajia et al. Carbon nitride with a tailored electronic structure toward peroxymonosulfate activation: A direct electron transfer mechanism for organic pollutant degradation [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2023 , 341 . |
| MLA | Ming, Hongbo et al. "Carbon nitride with a tailored electronic structure toward peroxymonosulfate activation: A direct electron transfer mechanism for organic pollutant degradation" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 341 (2023) . |
| APA | Ming, Hongbo , Bian, Xiaoqiong , Cheng, Jiajia , Yang, Can , Hou, Yidong , Ding, Kaining et al. Carbon nitride with a tailored electronic structure toward peroxymonosulfate activation: A direct electron transfer mechanism for organic pollutant degradation . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2023 , 341 . |
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Light-driven fixation of CO2 in organics has emerged as an appealing alternative for the synthesis of value-added fine chemicals. Challenges remain in the transformation of CO2 as well as product selectivity due to its thermodynamic stability and kinetic inertness. Here we develop a boron carbonitride (BCN) with the abundant terminal B/N defects around the mesoporous walls, which essentially enhances surface active sites as well as charge transfer kinetics, boosting the overall rate of CO2 adsorption and activation. In this protocol, anti-Markovnikov hydrocarboxylation of alkenes with CO2 to an extended carbon chain is achieved with good functional group tolerance and specific regioselectivity under visible-light irradiation. The mechanistic studies demonstrate the formation of CO2 radical anion intermediate on defective boron carbonitride, leading to the anti-Markovnikov carboxylation. Gram-scale reaction, late-stage carboxylation of natural products and synthesis of anti-diabetic GPR40 agonists reveal the utility of this method. This study sheds new insight on the design and application of metal-free semiconductors for the conversion of CO2 in an atom-economic and sustainable manner.
Keyword ：
Alkenes Alkenes Boron Carbonitride Boron Carbonitride Carbon Dioxide Carbon Dioxide Hydrocarboxylation Hydrocarboxylation Photocatalysis Photocatalysis
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| GB/T 7714 | Yuan, Tao , Wu, Ziwei , Zhai, Senmao et al. Photosynthetic Fixation of CO2 in Alkenes by Heterogeneous Photoredox Catalysis with Visible Light [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 . |
| MLA | Yuan, Tao et al. "Photosynthetic Fixation of CO2 in Alkenes by Heterogeneous Photoredox Catalysis with Visible Light" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2023) . |
| APA | Yuan, Tao , Wu, Ziwei , Zhai, Senmao , Wang, Rong , Wu, Shiwen , Cheng, Jiajia et al. Photosynthetic Fixation of CO2 in Alkenes by Heterogeneous Photoredox Catalysis with Visible Light . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 . |
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A visible-light-induced carboxylation of styrenes using CO2 that proceeds via a halogen-atom-transfer pathway using alkyl iodides as a promoter has been developed. Alkyl iodides, reagents that are challenging to react under photoredox conditions, and CO2 could be assembled into electron-deficient styrenes for the synthesis of aryl acetic acids. The late-stage functionalization of bioactive molecules showed the synthetic utility of the halogen-atom-transfer system.
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| GB/T 7714 | Zhai, Senmao , Wang, Rong , Dong, Quan et al. A photochemical halogen-atom-transfer pathway for the carboxylation of alkenes with CO2 [J]. | ORGANIC CHEMISTRY FRONTIERS , 2023 , 10 (19) : 4816-4820 . |
| MLA | Zhai, Senmao et al. "A photochemical halogen-atom-transfer pathway for the carboxylation of alkenes with CO2" . | ORGANIC CHEMISTRY FRONTIERS 10 . 19 (2023) : 4816-4820 . |
| APA | Zhai, Senmao , Wang, Rong , Dong, Quan , Cheng, Jiajia , Zheng, Meifang , Wang, Xinchen . A photochemical halogen-atom-transfer pathway for the carboxylation of alkenes with CO2 . | ORGANIC CHEMISTRY FRONTIERS , 2023 , 10 (19) , 4816-4820 . |
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本发明公开了一种含芴酮的有机共轭聚合物及其在催化烯胺酮氧化酯化合成α‑酮酯中的应用，属于光催化技术领域。该有机共轭聚合物是以2, 7‑二溴‑9‑芴酮和1, 3, 5‑三乙炔苯作为单体，通过过渡金属Pd一步催化聚合制得的。本发明制备的有机共轭聚合物可以良好的分散在乙醇中并保持稳定，且其具有较强的可见光响应能力，在绿色可见光照射下可展示出良好的光催化烯胺酮氧化酯化生成α‑酮酯的活性。
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| GB/T 7714 | 王心晨 , 成佳佳 , 吕金良 et al. 含芴酮的有机共轭聚合物及其在α-酮酯合成中的应用 : CN202210586307.9[P]. | 2022-05-27 00:00:00 . |
| MLA | 王心晨 et al. "含芴酮的有机共轭聚合物及其在α-酮酯合成中的应用" : CN202210586307.9. | 2022-05-27 00:00:00 . |
| APA | 王心晨 , 成佳佳 , 吕金良 , 冯加豪 . 含芴酮的有机共轭聚合物及其在α-酮酯合成中的应用 : CN202210586307.9. | 2022-05-27 00:00:00 . |
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Abstract ：
核磁共振是解析有机化合物结构的一种常用的方法，也是有机波谱分析课程教学中的重点内容之一。本文结合三个实例介绍了核磁共振氢谱解析思路，理论与科研实际相结合，利用核磁共振氢谱判断产物中异构体的结构，通过峰组的积分面积确定异构体的比例，以便培养学生的科学素养，激发学生的学习兴趣，提高谱图的解析能力。
Keyword ：
化学位移 化学位移 异构体 异构体 核磁共振氢谱 核磁共振氢谱 结构解析 结构解析 耦合常数 耦合常数
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| GB/T 7714 | 袁耀锋 , 王宝绪 , 黄良森 et al. 利用核磁共振氢谱分析异构化产物 [J]. | 大学化学 , 2022 , 37 (03) : 217-221 . |
| MLA | 袁耀锋 et al. "利用核磁共振氢谱分析异构化产物" . | 大学化学 37 . 03 (2022) : 217-221 . |
| APA | 袁耀锋 , 王宝绪 , 黄良森 , 成佳佳 . 利用核磁共振氢谱分析异构化产物 . | 大学化学 , 2022 , 37 (03) , 217-221 . |
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As an effective approach toward sustainability and global carbon balance, the reductive conversion of CO2 into value-added chemicals is of considerable significance. Here, by simply calcining the mixture of NH4SCN and KCl in an air atmosphere, potassium dopants and negatively charged electron-rich centers are simultaneously introduced into carbon nitride materials via a metalation engineering strategy. The resultant metalized catalysts with deprotonated imide sites and doped potassium ions demonstrate much-enhanced activity for catalyzing CO2 reductive hydrosilylation with excellent conversion and >90% selectivity, whereas the pristine carbon nitride catalyst shows only negligible activity. Both experimental and theoretical results reveal the crucial role of the negatively charged electron-rich centers and potassium dopants in tailoring the energy band positions and electronic structure for the efficient donor-acceptor interaction and much increased driving force for CO2 reduction. The present work offers molecular-level insights into the boosted CO2 reduction activity via engineering the electronic structure of the metalized carbon nitride catalyst and reducing the energy offset between frontier molecular orbitals of CO2 and the catalyst, which can provide a conceptual guide for further development of efficient catalytic CO2 reduction systems.
Keyword ：
carbon nitride carbon nitride CO2 functionalization CO2 functionalization electron-rich centers electron-rich centers metalation engineering metalation engineering value-added products value-added products
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| GB/T 7714 | Cheng, Jiajia , Hou, Yuchen , Lian, Kangkang et al. Metalized Carbon Nitrides for Efficient Catalytic Functionalization of CO2 [J]. | ACS CATALYSIS , 2022 , 12 (3) : 1797-1808 . |
| MLA | Cheng, Jiajia et al. "Metalized Carbon Nitrides for Efficient Catalytic Functionalization of CO2" . | ACS CATALYSIS 12 . 3 (2022) : 1797-1808 . |
| APA | Cheng, Jiajia , Hou, Yuchen , Lian, Kangkang , Xiao, Hongxiang , Lin, Sen , Wang, Xinchen . Metalized Carbon Nitrides for Efficient Catalytic Functionalization of CO2 . | ACS CATALYSIS , 2022 , 12 (3) , 1797-1808 . |
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