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学者姓名：张贵刚
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Abstract ：
Polymeric carbon nitrides (PCNs), usually the melon phase, have been extensively applied as photocatalysts for CO2 reduction; however, their performance is still unsatisfactory. The condensed allotrope, namely, poly(triazine imide) (PTI) with extended conjugation and a crystallized structure, indeed holds more favorable compositional and structural advantages for photocatalytic CO(2)reduction but remains to be fully exploited. Herein, hexagonal prism-shaped PTI crystals were synthesized and developed as a high-performance photocatalyst for CO2 reduction. With Co(bpy)(3) (2+) as a cocatalyst, the PTI crystals exhibit a CO evolution rate of 44 mu mol h(-1) (i.e., 1467 mu mol g(-1) h(-1)) with 93% selectivity, markedly superior to that of the melon counterpart. Moreover, PTI crystals manifest an apparent quantum efficiency of 12.9% at 365 nm, representing the state-of-the-art value by PCN photocatalysts for CO2-to-CO reduction without using noble metals. The surface pyridine N species of PTI are exposed as active sites to dominate CO2 activation and conversion, which, together with the high crystallinity to facilitate charge separation and transport, endows high CO2 reduction efficiency. In situ diffuse reflectance infrared Fourier transform spectroscopy determines the key intermediates during the CO2 reduction reaction and, consequently, constructs the possible reaction mechanism.
Keyword ：
active sites active sites carbon nitride carbon nitride CO2 reduction CO2 reduction photocatalysis photocatalysis poly(triazineimide) poly(triazineimide) pyridine nitrogen pyridine nitrogen
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| GB/T 7714 | Liu, Feng , Deng, Jing , Su, Bo et al. Poly(triazine imide) Crystals for Efficient CO2 Photoreduction: Surface Pyridine Nitrogen Dominates the Performance [J]. | ACS CATALYSIS , 2025 , 15 (2) : 1018-1026 . |
| MLA | Liu, Feng et al. "Poly(triazine imide) Crystals for Efficient CO2 Photoreduction: Surface Pyridine Nitrogen Dominates the Performance" . | ACS CATALYSIS 15 . 2 (2025) : 1018-1026 . |
| APA | Liu, Feng , Deng, Jing , Su, Bo , Peng, Kang-Shun , Liu, Kunlong , Lin, Xiahui et al. Poly(triazine imide) Crystals for Efficient CO2 Photoreduction: Surface Pyridine Nitrogen Dominates the Performance . | ACS CATALYSIS , 2025 , 15 (2) , 1018-1026 . |
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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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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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Abstract ：
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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The integration of electron donor (D) and acceptor (A) units into covalent organic frameworks (COFs) has received increasing interest due to its potential for efficient photocatalytic hydrogen (H2) evolution from water. Nevertheless, the advancement of D–A COFs is still constrained by the limited investigations on acceptor engineering, which enables the highly effective charge transfer pathways in COFs to deliver photoexcited electrons in a preferential orientation to enhance photocatalytic performance. Herein, two systems with D–A and D–A–A configurations based on the acceptor molecular engineering strategy are proposed to construct three distinct COFs. Specifically, TAPPy-DBTDP-COF merging one pyrene-based donor and two benzothiadiazole acceptors realized an average H2 evolution rate of 12.7 mmol h−1 g−1 under visible light, among the highest ever reported for typical D–A-type COF systems. The combination of experimental and theoretical analysis signifies the crucial role of the dual-acceptor arrangement in promoting exciton dissociation and carrier migration. These findings underscore the significant potential of D–A–A structural design, which is conducive to the efficient separation of photoexcited electrons and holes resulting in superior photocatalytic activities. © 2024 Wiley-VCH GmbH.
Keyword ：
covalent organic frameworks covalent organic frameworks donor-acceptor COFs donor-acceptor COFs H2 evolution H2 evolution photocatalysis photocatalysis
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| GB/T 7714 | Liu, N. , Xie, S. , Huang, Y. et al. Dual–Acceptor Engineering in Pyrene-Based Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution [J]. | Advanced Energy Materials , 2024 , 14 (40) . |
| MLA | Liu, N. et al. "Dual–Acceptor Engineering in Pyrene-Based Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution" . | Advanced Energy Materials 14 . 40 (2024) . |
| APA | Liu, N. , Xie, S. , Huang, Y. , Lu, J. , Shi, H. , Xu, S. et al. Dual–Acceptor Engineering in Pyrene-Based Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution . | Advanced Energy Materials , 2024 , 14 (40) . |
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| GB/T 7714 | Zheng, Dandan , Wang, Qian , Pan, Zhiming et al. Poly(triazine imide) nanospheres with spatially exposed prismatic facets for photocatalytic overall water splitting [J]. | SCIENCE CHINA-MATERIALS , 2024 , 67 (6) : 1900-1906 . |
| MLA | Zheng, Dandan et al. "Poly(triazine imide) nanospheres with spatially exposed prismatic facets for photocatalytic overall water splitting" . | SCIENCE CHINA-MATERIALS 67 . 6 (2024) : 1900-1906 . |
| APA | Zheng, Dandan , Wang, Qian , Pan, Zhiming , Wang, Sibo , Hou, Yidong , Zhang, Guigang . Poly(triazine imide) nanospheres with spatially exposed prismatic facets for photocatalytic overall water splitting . | SCIENCE CHINA-MATERIALS , 2024 , 67 (6) , 1900-1906 . |
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