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学者姓名：张贵刚
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Abstract ：
The artificial photosynthesis of H2O2 from water and oxygen using semiconductor photocatalysts is attracting increasing levels of attention owing to its green, environmentally friendly, and energy-saving characteristics. Although covalent organic frameworks (COFs) are promising materials for promoting photocatalytic H2O2 production owing to their structural and functional diversity, they typically suffer from low charge-generation and -transfer efficiencies as well as rapid charge recombination, which restricts their use as catalysts for photocatalytic H2O2 production. Herein, we report a strategy for anchoring vinyl moieties to a COF skeleton to facilitate charge separation and migration, thereby promoting photocatalytic H2O2 generation. This vinyl-group-bearing COF photocatalyst exhibits a H2O2 -production rate of 84.5 mu mol h(-1) (per 10 mg), which is ten-times higher than that of the analog devoid of vinyl functionality and superior to most reported COF photocatalysts. Both experimental and theoretical studies provide deep insight into the origin of the improved photocatalytic performance. These findings are expected to facilitate the rational design and modification of organic semiconductors for use in photocatalytic applications.
Keyword ：
Charge separation Charge separation Covalent organic frameworks Covalent organic frameworks H2O2 production H2O2 production Photocatalysts Photocatalysts Vinyl groups Vinyl groups
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| GB/T 7714 | Yu, Hong , Zhang, Fengtao , Chen, Qian et al. Vinyl-Group-Anchored Covalent Organic Framework for Promoting the Photocatalytic Generation of Hydrogen Peroxide [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (21) . |
| MLA | Yu, Hong et al. "Vinyl-Group-Anchored Covalent Organic Framework for Promoting the Photocatalytic Generation of Hydrogen Peroxide" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 21 (2024) . |
| APA | Yu, Hong , Zhang, Fengtao , Chen, Qian , Zhou, Pan-Ke , Xing, Wandong , Wang, Sibo et al. Vinyl-Group-Anchored Covalent Organic Framework for Promoting the Photocatalytic Generation of Hydrogen Peroxide . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (21) . |
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Polymeric carbon nitride has been widely developed as a promising photocatalyst for solar hydrogen production via photocatalytic water splitting. However, pristine carbon nitride prepared by traditional solid-state polymerization usually encounters issues such as rapid carrier recombination and insufficient absorption of visible light below 460 nm. Herein, poly(heptazine imide) with a distinctive nanoplate structure was synthesized in a binary molten salt of NaCl-CaCl2. The salt template allows the formation of the thin nanoplate structure, which promotes the charge separation and migration. Besides, the intercalation of Ca2+ ions between the conjugated layers endows the activation of n-pi* electron transition due to the distortion of in-plane heptazine layers. Accordingly, the optimized poly(heptazine imide) nanoplates achieve an apparent quantum efficiency of up to 17.3% at 500 nm for photocatalytic hydrogen production from water. This work shares new idea for rational control of the optical absorption and charge carrier dynamics of poly(heptazine imide).
Keyword ：
hydrogen production hydrogen production ion intercalation ion intercalation nanoplates nanoplates photocatalysis photocatalysis poly heptazine imide poly heptazine imide
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| GB/T 7714 | Zou, Yanmin , Li, Shiyao , Zheng, Dandan et al. Extended light absorption and accelerated charge migration in ultrathin twisted carbon nitride nanoplates for efficient solar hydrogen production [J]. | SCIENCE CHINA-CHEMISTRY , 2024 , 67 (7) : 2215-2223 . |
| MLA | Zou, Yanmin et al. "Extended light absorption and accelerated charge migration in ultrathin twisted carbon nitride nanoplates for efficient solar hydrogen production" . | SCIENCE CHINA-CHEMISTRY 67 . 7 (2024) : 2215-2223 . |
| APA | Zou, Yanmin , Li, Shiyao , Zheng, Dandan , Feng, Jianyong , Wang, Sibo , Hou, Yidong et al. Extended light absorption and accelerated charge migration in ultrathin twisted carbon nitride nanoplates for efficient solar hydrogen production . | SCIENCE CHINA-CHEMISTRY , 2024 , 67 (7) , 2215-2223 . |
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Sunlight -induced photocatalytic carbon dioxide (CO2) reduction to energy -rich chemicals by metal -free polymeric carbon nitride (CN) semiconductor is a promising tactic for sustained solar fuel production. However, the reaction efficiency of CO2 photoreduction is restrained seriously by the rapid recombination of photogenerated carriers on CN polymer. Herein, we incorporate 2-aminopyridine molecule with strong electron -withdrawing group into the skeleton edge of CN layers through a facile one -pot thermal polymerization strategy using urea as the precursor, which renders a modified carbon nitride (ACN) with extended optical harvesting, abundant nitrogen defects and ultrathin nanosheet structure. Consequently, the ACN photocatalyst with desirable structural features attains enhanced separation and migration of photoexcited charge carriers. Under visible light irradiation with Co(bpy)32+ as a cocatalyst, the optimized ACN sample manifests a high CO2 deoxygnative reduction activity and high stability, providing a CO yielding rate of 17 mu mol h-1, which is significantly higher than that of pristine CN. The key intermediates engaged in CO2 photoreduction reaction are determined by the in situ diffuse reflectance infrared Fourier transform spectroscopy, which sponsors the construction of the possible photocatalytic CO2 reduction mechanism on ACN nanosheets.
Keyword ：
Carbon nitride Carbon nitride CO2 reduction CO2 reduction Nanosheets Nanosheets Nitrogen defects Nitrogen defects Photocatalysis Photocatalysis
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| GB/T 7714 | Zhou, Ziruo , Guo, Wenyu , Yang, Tingyu et al. Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction [J]. | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2024 , 43 (3) . |
| MLA | Zhou, Ziruo et al. "Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction" . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY 43 . 3 (2024) . |
| APA | Zhou, Ziruo , Guo, Wenyu , Yang, Tingyu , Zheng, Dandan , Fang, Yuanxing , Lin, Xiahui et al. Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2024 , 43 (3) . |
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Photocatalytic CO2 reduction over Ru(ii)-complex/Ag/polymeric carbon nitride (PCN) was studied with respect to light intensity and the type of Ru(ii) complex. In experiments using two different Ru(ii) complex cocatalysts, the reduction potential of the Ru complex was found to balance efficient CO2 reduction on the Ru complex with electron transfer from Ag/PCN. This balance avoided the formation of H2 as a byproduct, minimized charge accumulation in Ag/PCN, and maximized the apparent quantum yield for CO2-to-HCOOH conversion.
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| GB/T 7714 | Nakada, Ryuichi , Zhang, Chao , Onodera, Jo et al. Light-intensity dependence of visible-light CO2 reduction over Ru(ii)-complex/Ag/polymeric carbon nitride hybrid photocatalysts [J]. | SUSTAINABLE ENERGY & FUELS , 2024 . |
| MLA | Nakada, Ryuichi et al. "Light-intensity dependence of visible-light CO2 reduction over Ru(ii)-complex/Ag/polymeric carbon nitride hybrid photocatalysts" . | SUSTAINABLE ENERGY & FUELS (2024) . |
| APA | Nakada, Ryuichi , Zhang, Chao , Onodera, Jo , Tanaka, Toshiya , Okazaki, Megumi , Zhang, Guigang et al. Light-intensity dependence of visible-light CO2 reduction over Ru(ii)-complex/Ag/polymeric carbon nitride hybrid photocatalysts . | SUSTAINABLE ENERGY & FUELS , 2024 . |
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Highly crystalline carbon nitride polymers have shown great opportunities in overall water photosplitting; however, their mission in light-driven CO2 conversion remains to be explored. In this work, crystalline carbon nitride (CCN) nanosheets of poly triazine imide (PTI) embedded with melon domains are fabricated by KCl/LiCl-mediated polycondensation of dicyandiamide, the surface of which is subsequently deposited with ultrafine WO3 nanoparticles to construct the CCN/WO3 heterostructure with a S-scheme interface. Systematic characterizations have been conducted to reveal the compositions and structures of the S-scheme CCN/WO3 hybrid, featuring strengthened optical capture, enhanced CO2 adsorption and activation, attractive textural properties, as well as spatial separation and directed movement of light-triggered charge carriers. Under mild conditions, the CCN/WO3 catalyst with optimized composition displays a high photocatalytic activity for reducing CO2 to CO in a rate of 23.0 mu mol/hr ( i.e., 2300 mu mol/(hr center dot g)), which is about 7-fold that of pristine CCN, along with a high CO selectivity of 90.6% against H2 formation. Moreover, it also manifests high stability and fine reusability for the CO2 conversion reaction. The CO2 adsorption and conversion processes on the catalyst are monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), identifying the crucial intermediates of CO2 *-, COOH* and CO*, which integrated with the results of performance evaluation proposes the possible CO2 reduction mechanism. (c) 2023 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.
Keyword ：
CO 2 reduction CO 2 reduction Crystalline carbon nitride Crystalline carbon nitride Photocatalysis Photocatalysis S-scheme S-scheme WO3 WO3
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| GB/T 7714 | Chen, Gongjie , Zhou, Ziruo , Li, Bifang et al. S-scheme heterojunction of crystalline carbon nitride nanosheets and ultrafine WO3 nanoparticles for photocatalytic CO2 reduction [J]. | JOURNAL OF ENVIRONMENTAL SCIENCES , 2024 , 140 : 103-112 . |
| MLA | Chen, Gongjie et al. "S-scheme heterojunction of crystalline carbon nitride nanosheets and ultrafine WO3 nanoparticles for photocatalytic CO2 reduction" . | JOURNAL OF ENVIRONMENTAL SCIENCES 140 (2024) : 103-112 . |
| APA | Chen, Gongjie , Zhou, Ziruo , Li, Bifang , Lin, Xiahui , Yang, Can , Fang, Yuanxing et al. S-scheme heterojunction of crystalline carbon nitride nanosheets and ultrafine WO3 nanoparticles for photocatalytic CO2 reduction . | JOURNAL OF ENVIRONMENTAL SCIENCES , 2024 , 140 , 103-112 . |
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In this work, protonated poly(heptazine imide) (H-PHI) was obtained by adding acid to the suspension of potassium PHI (K-PHI) in ethanol. It was established that the obtained H-PHI demonstrates very high photocatalytic activity in the reaction of hydrogen formation from ethanol in the presence of Pt nanoparticles under visible light irradiation in comparison with K-PHI. This enhancement can be attributed to improved efficiency of photogenerated charge transfer to the photocatalyst’s surface, where redox processes occur. Various factors influencing the system’s activity were evaluated. Notably, it was discovered that the conditions of acid introduction into the system can significantly affect the size of Pt (cocatalyst metal) deposition on the H-PHI surface, thereby enhancing the photocatalytic system’s stability in producing molecular hydrogen. It was established that the system can operate efficiently in the presence of air without additional components on the photocatalyst surface to block air access. Under optimal conditions, the apparent quantum yield of molecular hydrogen production at 410 nm is around 73%, the highest reported value for carbon nitride materials to date. The addition of acid not only increases the activity of the reduction part of the system but also leads to the formation of a value-added product from ethanol-1,1-diethoxyethane (acetal) with high selectivity. © 2024 The Authors. Published by American Chemical Society.
Keyword ：
Carbon nitride Carbon nitride Nanocrystals Nanocrystals Photocatalytic activity Photocatalytic activity Protonation Protonation Quantum yield Quantum yield Redox reactions Redox reactions
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| GB/T 7714 | Shvalagin, Vitaliy , Tarakina, Nadezda , Badamdorj, Bolortuya et al. Simultaneous Photocatalytic Production of H2 and Acetal from Ethanol with Quantum Efficiency over 73% by Protonated Poly(heptazine imide) under Visible Light [J]. | ACS Catalysis , 2024 , 14 (19) : 14836-14854 . |
| MLA | Shvalagin, Vitaliy et al. "Simultaneous Photocatalytic Production of H2 and Acetal from Ethanol with Quantum Efficiency over 73% by Protonated Poly(heptazine imide) under Visible Light" . | ACS Catalysis 14 . 19 (2024) : 14836-14854 . |
| APA | Shvalagin, Vitaliy , Tarakina, Nadezda , Badamdorj, Bolortuya , Lahrsen, Inga-Marie , Bargiacchi, Eleonora , Bardow, Andre et al. Simultaneous Photocatalytic Production of H2 and Acetal from Ethanol with Quantum Efficiency over 73% by Protonated Poly(heptazine imide) under Visible Light . | ACS Catalysis , 2024 , 14 (19) , 14836-14854 . |
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Surface functionalization has been considered as an effective strategy to manipulate charge separation of carbon nitride and therefore to largely improve the photocatalytic H 2 evolution efficiency. Poly heptazine imide (PHI) is a new class of crystalline carbon nitride frameworks that exhibits remarkable photocatalytic performance for hydrogen evolution. To further improve the H 2 evolution performance of PHI and explore the reaction mechanism, ammonium thiocyanate was used as a precursor for the synthesis of poly heptazine imide at elevated temperatures under molten salt conditions. The optimized PHI with an abundance of surface cyano groups shows a significantly enhanced photocatalytic performance for H 2 evolution, which is 4.3 times that on pristine PCN. Most importantly, the surface cyano group adjusts the electron intensity of the polymeric framework, enhances the light absorbance, reduces the bandgap, and improves the charge separation efficiency. The synthetic technique also could be applied to other sulfur -containing precursors for the synthesis of PHI frameworks with excellent hydrogen evolution production performance.
Keyword ：
Ammonium thiocyanate Ammonium thiocyanate Cyano group Cyano group Hydrogen evolution Hydrogen evolution Photocatalysis Photocatalysis Poly heptazine imide Poly heptazine imide
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| GB/T 7714 | Zhang, Yuhan , Yang, Zhenchun , Zheng, Dandan et al. Surface cyano groups optimize the charge transfer of poly heptazine imide for enhanced photocatalytic H 2 evolution [J]. | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2024 , 69 : 372-380 . |
| MLA | Zhang, Yuhan et al. "Surface cyano groups optimize the charge transfer of poly heptazine imide for enhanced photocatalytic H 2 evolution" . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 69 (2024) : 372-380 . |
| APA | Zhang, Yuhan , Yang, Zhenchun , Zheng, Dandan , Wang, Sibo , Hou, Yidong , Anpo, Masakazu et al. Surface cyano groups optimize the charge transfer of poly heptazine imide for enhanced photocatalytic H 2 evolution . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2024 , 69 , 372-380 . |
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Poly(heptazine imide) (PHI), a semicrystalline version of carbon nitride photocatalyst based on heptazine units, has gained significant attention for solar H2 production benefiting from its advantages including molecular synthetic versatility, excellent physicochemical stability and suitable energy band structure to capture visible photons. Typically, PHI is obtained in salt-melt synthesis in the presence of alkali metal chlorides. Herein, we examined the role of binary alkali metal bromides (LiBr/NaBr) with diverse compositions and melting points to rationally modulate the polymerization process, structure, and properties of PHI. Solid characterizations revealed that semicrystalline PHI with a condensed pi-conjugated system and rapid charge separation rates were obtained in the presence of LiBr/NaBr. Accordingly, the apparent quantum yield of hydrogen using the optimized PHI reaches up to 62.3% at 420 nm. The density functional theory calculation shows that the dehydrogenation of the ethylene glycol has a lower energy barrier than the dehydrogenation of the other alcohols from the thermodynamic point of view. This study holds great promise for rational modulation of the structure and properties of conjugated polymeric materials. A new poly(heptazine imide) was synthesized via salt-melt synthesis in binary alkali metal bromides with accelerated carrier transfer and decreased internal structural defects for photocatalytic hydrogen production. image
Keyword ：
crystallinity crystallinity hydrogen evolution hydrogen evolution photocatalysis photocatalysis poly(heptazine imide) poly(heptazine imide) salt-melt synthesis salt-melt synthesis
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| GB/T 7714 | Jin, Yaxuan , Zheng, Dandan , Fang, Zhongpu et al. Salt-melt synthesis of poly(heptazine imide) in binary alkali metal bromides for enhanced visible-light photocatalytic hydrogen production [J]. | INTERDISCIPLINARY MATERIALS , 2024 , 3 (3) : 389-399 . |
| MLA | Jin, Yaxuan et al. "Salt-melt synthesis of poly(heptazine imide) in binary alkali metal bromides for enhanced visible-light photocatalytic hydrogen production" . | INTERDISCIPLINARY MATERIALS 3 . 3 (2024) : 389-399 . |
| APA | Jin, Yaxuan , Zheng, Dandan , Fang, Zhongpu , Pan, Zhiming , Wang, Sibo , Hou, Yidong et al. Salt-melt synthesis of poly(heptazine imide) in binary alkali metal bromides for enhanced visible-light photocatalytic hydrogen production . | INTERDISCIPLINARY MATERIALS , 2024 , 3 (3) , 389-399 . |
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The effect of crystallization of polymeric carbon nitride (PCN) on the photocatalytic CO2 reduction activity of a three-component hybrid comprising a Ru(II) binuclear complex ( RuRu), Ag nanoparticles, and PCN, was investigated. Crystallized carbon nitride (CCN) obtained by heat treatment of PCN in a eutectic LiCl-KCl mixture was a much better hybrid photocatalyst component than the poorly crystallized PCN. The photocatalytic activity of CCN was dependent on the temperature of the LiCl-KCl treatment: Increasing the treatment temperature improved the photocatalytic activity as much as five-fold; however, treatment at elevated temperatures (>798 K) had a detrimental effect. Also, a substantial PCN crystallization effect was promoted by the construction of another hybrid photocatalyst from a mononuclear Ru(II) complex catalyst. Time-resolved microwave photoconductivity measurements revealed a good correlation between the photocatalytic activity and the photoconductivity-charge carrier lifetime product in the CCN samples heated at milder temperatures (<= 798 K). For CCN specimens heated at higher temperatures, appreciable electron accumulation was observed during the photocatalytic reaction, indicating that the accumulated electrons could not participate in the CO2 reduction reaction. Thus, the crystallization of PCN at milder temperatures improved the mobility and lifetime of photogenerated charge carriers, thereby contributing to enhanced photocatalytic activity toward CO2 reduction.
Keyword ：
artificial photosynthesis artificial photosynthesis hydrogen carrier hydrogen carrier organic semiconductor organic semiconductor solar fuels solar fuels Z-scheme Z-scheme
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| GB/T 7714 | Tanaka, Toshiya , Zhang, Chao , Nakada, Ryuichi et al. Significant Effect of Crystallization of Polymeric Carbon Nitride on Photoconductivity and Photocatalytic Activity for Visible-Light CO2 Reduction [J]. | CCS CHEMISTRY , 2024 , 6 (12) : 2940-2949 . |
| MLA | Tanaka, Toshiya et al. "Significant Effect of Crystallization of Polymeric Carbon Nitride on Photoconductivity and Photocatalytic Activity for Visible-Light CO2 Reduction" . | CCS CHEMISTRY 6 . 12 (2024) : 2940-2949 . |
| APA | Tanaka, Toshiya , Zhang, Chao , Nakada, Ryuichi , Onodera, Jo , Ishiwari, Fumitaka , Okazaki, Megumi et al. Significant Effect of Crystallization of Polymeric Carbon Nitride on Photoconductivity and Photocatalytic Activity for Visible-Light CO2 Reduction . | CCS CHEMISTRY , 2024 , 6 (12) , 2940-2949 . |
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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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