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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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Photocatalytic hydrogen peroxide (H2O2) production using conjugated polymers as photocatalysts is a green and sustainable approach to synthesizing H2O2. Nevertheless, the efficiency is still hindered by the inefficient charge separation and transfer dynamics. Herein, a series of coplanar 2D ladder polymers with different substituents were reported as metal-free photocatalysts for artificial photosynthesis of H2O2. Detailed experimental and theoretical investigations reveal that the coplanar 2D skeleton and strong electron-withdrawing substituents could profoundly facilitate charge separation and transfer. Possessing these notable merits, the cyano-substituted polymer (PAE-CN) exhibits remarkable photocatalytic performance on H2O2 evolution. This study contributes to the development of effective polymer photocatalysts tailored for potential applications in artificial photosynthesis.
Keyword ：
coplanarladder polymer coplanarladder polymer H2O2 photosynthesis H2O2 photosynthesis oxygen reductionreaction oxygen reductionreaction polymer photocatalyst polymer photocatalyst substituent regulation substituent regulation
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| GB/T 7714 | Chen, Dengke , Tian, Lin , Ren, Wei et al. Regulating Substituents in Coplanar 2D Ladder Polymers for Enhanced Photocatalytic Production of H2O2 [J]. | ACS APPLIED POLYMER MATERIALS , 2025 , 7 (2) : 1129-1135 . |
| MLA | Chen, Dengke et al. "Regulating Substituents in Coplanar 2D Ladder Polymers for Enhanced Photocatalytic Production of H2O2" . | ACS APPLIED POLYMER MATERIALS 7 . 2 (2025) : 1129-1135 . |
| APA | Chen, Dengke , Tian, Lin , Ren, Wei , Ru, Chenglong , Zhang, Fengtao , Li, Guosheng et al. Regulating Substituents in Coplanar 2D Ladder Polymers for Enhanced Photocatalytic Production of H2O2 . | ACS APPLIED POLYMER MATERIALS , 2025 , 7 (2) , 1129-1135 . |
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Lattice oxygen (LO)-mediated photothermal dry reforming of methane (DRM) presents a promising approach to syngas production. However, realizing high DRM efficiency and durability remains challenging due to the difficulty in activating LOs in catalysts. Herein, we demonstrate that partially substituting Fe sites in perovskite ferrite (LaFeO3) by Mn triggers LOs, bestowing the catalyst with superior activity and stability for photothermal DRM after modification with Ru. The Mn exchange induces a charge transfer from La to Mn, which combined with the incoming photoexcited electrons reconstructs the perovskite’s electronic structure, weakening the La-O-Mn bonds and facilitating the LO migration. Meanwhile, photogenerated holes migrate to surface LOs, further enhancing their reactivity to mediate DRM. Under light irradiation, the catalyst exhibits an outstanding syngas production rate (H2: 42.89 mol gRu-1 h-1, CO: 54.92 mol gRu-1 h-1) while stably operating over 150 h. It also achieves a methane turnover frequency of 0.9 s-1 and a light-to-chemical energy efficiency of 15.3%, setting a benchmark for light-driven DRM performance. This work underscores the significance of exact site doping in metal oxides to fine-tune LO activity, providing valuable guidance for fabricating efficient catalysts for solar-powered redox reactions proceeded via the light-supported Mars-van Krevelen mechanism. © 2025 American Chemical Society.
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| GB/T 7714 | Li, J. , Zhao, J. , Wang, S. et al. Activating Lattice Oxygen in Perovskite Ferrite for Efficient and Stable Photothermal Dry Reforming of Methane [J]. | Journal of the American Chemical Society , 2025 . |
| MLA | Li, J. et al. "Activating Lattice Oxygen in Perovskite Ferrite for Efficient and Stable Photothermal Dry Reforming of Methane" . | Journal of the American Chemical Society (2025) . |
| APA | Li, J. , Zhao, J. , Wang, S. , Peng, K.-S. , Su, B. , Liu, K. et al. Activating Lattice Oxygen in Perovskite Ferrite for Efficient and Stable Photothermal Dry Reforming of Methane . | Journal of the American Chemical Society , 2025 . |
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As a crystalline allotrope of carbon nitrides, poly (heptazine imide) (PHI) exhibits great potential for photocatalytic reforming of biomass-derived alcohols. However, its activity is greatly constrained due to insufficient charge migration and severe non-radiative recombination. To address this issue, PHI with high interlayer stacking orderliness is fabricated through a facile ion exchange strategy. Characterizations reveal that rational modification of the interlayer stacking mode of PHI could efficiently suppress non-radiative recombination and improve charge transfer efficiency. Accordingly, the optimal sample exhibits high photocatalytic reforming activity for H2 evolution, which is up to 2.16 mmolg-1h-1, and with a quantum efficiency reaches 26.7% at 400 nm.
Keyword ：
Biomass conversion Biomass conversion Hydrogen production Hydrogen production Interlayer stacking modes Interlayer stacking modes Nonradiative recombination Nonradiative recombination Poly heptazine imide Poly heptazine imide
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| GB/T 7714 | Sun, Qiqi , Cheng, Xiaohong , Qie, Mingyang et al. Photocatalytic Reforming of Methanol Over Poly Heptazine Imide: Interlayer Stacking Modification Induced Rapid Charge Transfer [J]. | CHEMCATCHEM , 2025 . |
| MLA | Sun, Qiqi et al. "Photocatalytic Reforming of Methanol Over Poly Heptazine Imide: Interlayer Stacking Modification Induced Rapid Charge Transfer" . | CHEMCATCHEM (2025) . |
| APA | Sun, Qiqi , Cheng, Xiaohong , Qie, Mingyang , Pan, Zhiming , Li, Guosheng , Zhang, Xirui et al. Photocatalytic Reforming of Methanol Over Poly Heptazine Imide: Interlayer Stacking Modification Induced Rapid Charge Transfer . | CHEMCATCHEM , 2025 . |
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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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The development of effective, low-cost, and stable photocatalysts for visible-light-driven hydrogen production is desired but challenging. Herein, in the presence of a ternary eutectic salt mixture, poly(heptazine imide) with a crystalline-amorphous interface, is synthesized, which endows improved transfer of charge carriers and enhanced photocatalytic activity for hydrogen production. © 2024 American Chemical Society.
Keyword ：
charge separation charge separation hydrogen production hydrogen production photocatalysis photocatalysis poly(heptazine imide) poly(heptazine imide) water splitting water splitting
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| GB/T 7714 | Wang, Q. , Li, S. , Zheng, D. et al. Prompt Charge Separation at Crystalline-Amorphous Interfaces of Poly(heptazine imides) for Photocatalytic Hydrogen Evolution [J]. | ACS Applied Energy Materials , 2024 , 7 (15) : 6090-6095 . |
| MLA | Wang, Q. et al. "Prompt Charge Separation at Crystalline-Amorphous Interfaces of Poly(heptazine imides) for Photocatalytic Hydrogen Evolution" . | ACS Applied Energy Materials 7 . 15 (2024) : 6090-6095 . |
| APA | Wang, Q. , Li, S. , Zheng, D. , Wang, S. , Hou, Y. , Zhang, G. . Prompt Charge Separation at Crystalline-Amorphous Interfaces of Poly(heptazine imides) for Photocatalytic Hydrogen Evolution . | ACS Applied Energy Materials , 2024 , 7 (15) , 6090-6095 . |
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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 , 9 (4) . |
| 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 9 . 4 (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 , 9 (4) . |
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| GB/T 7714 | Jin, Yaxuan , Zhang, Chao , Zhang, Guigang . Atomically dispersed low-valent Au on poly(heptazine imide) boosts photocatalytic hydroxyl radical production [J]. | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2024 , 43 (12) . |
| MLA | Jin, Yaxuan et al. "Atomically dispersed low-valent Au on poly(heptazine imide) boosts photocatalytic hydroxyl radical production" . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY 43 . 12 (2024) . |
| APA | Jin, Yaxuan , Zhang, Chao , Zhang, Guigang . Atomically dispersed low-valent Au on poly(heptazine imide) boosts photocatalytic hydroxyl radical production . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2024 , 43 (12) . |
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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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Hydroxyl radical(·OH)has gained considerable attention as one of the most important reactive oxygen species,which is widely used in water purification,disinfection biomedicine and other fields[1].Espe-cially,the OH radical exhibits the highest oxidation potential,with the exception of·F radical,which plays a pivotal role in the purification of water.However,developing an effective and renewable approach to generating OH in situ represents a significant research challenge.The combination of artificial photosynthesis of H2O2 via a 2e-oxygen reduction reaction(ORR)and the Fenton reaction provides an indirect approach for the production of·OH[2].Comparatively,by consuming only 1 mol of h+via the 1e-water oxidation reaction(WOR),theoreti-cally 1 mol of·OH can be generated.This provides the most efficient way to directly generate OH,since one h+can generate one OH.
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| GB/T 7714 | Yaxuan Jin , Chao Zhang , Guigang Zhang . Atomically dispersed low-valent Au on poly(heptazine imide)boosts photocatalytic hydroxyl radical production [J]. | 结构化学 , 2024 , 43 (12) : 3-4 . |
| MLA | Yaxuan Jin et al. "Atomically dispersed low-valent Au on poly(heptazine imide)boosts photocatalytic hydroxyl radical production" . | 结构化学 43 . 12 (2024) : 3-4 . |
| APA | Yaxuan Jin , Chao Zhang , Guigang Zhang . Atomically dispersed low-valent Au on poly(heptazine imide)boosts photocatalytic hydroxyl radical production . | 结构化学 , 2024 , 43 (12) , 3-4 . |
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