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学者姓名：张贵刚
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Abstract ：
The efficiency of photocatalytic hydrogen evolution is fundamentally constrained by limited charge carrier separation. Herein, we deliberately engineered an electric double layer (EDL) via surface modification with positively charged molecules, which optimizes the charge carrier dynamics. The anchoring of both diethylenetriamine (DETA) molecules and Pt species on CdS (denoted as Pt/CdS-D) achieves remarkable H2 evolution performance, delivering an exceptional rate of 6295 mu mol g-1 h-1 and an apparent quantum efficiency of 14.9%, which is 26.7-fold enhanced compared to that of CdS. The synergistic modification strategy concurrently lowers the activation energy barrier for water reduction and establishes EDL-driven directional charge transport channels that boost carrier separation efficiency. This work provides a paradigm for designing high-performance photocatalysts through the rational integration of functional organic groups and cocatalysts, opening new avenues for advanced solar-to-hydrogen energy conversion systems.
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| GB/T 7714 | Deng, Jing , Xu, Xinyu , Su, Bo et al. Structural amine-induced interfacial electrical double layers for efficient photocatalytic H2 evolution [J]. | MATERIALS HORIZONS , 2025 . |
| MLA | Deng, Jing et al. "Structural amine-induced interfacial electrical double layers for efficient photocatalytic H2 evolution" . | MATERIALS HORIZONS (2025) . |
| APA | Deng, Jing , Xu, Xinyu , Su, Bo , Liu, Minghui , Lin, Xiahui , Xing, Wandong et al. Structural amine-induced interfacial electrical double layers for efficient photocatalytic H2 evolution . | MATERIALS HORIZONS , 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 , 17 (10) . |
| MLA | Sun, Qiqi et al. "Photocatalytic Reforming of Methanol Over Poly Heptazine Imide: Interlayer Stacking Modification Induced Rapid Charge Transfer" . | CHEMCATCHEM 17 . 10 (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 , 17 (10) . |
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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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Elevating the long-wavelength activation of photocatalysts represents a formidable approach to optimizing sunlight utilization. Polythiophene (PTh), although renowned for its robust light absorption and excellent conductivity, is largely overlooked for its potential as a photocatalyst due to the swift recombination of photogenerated charge carriers. Herein, we unveil that the strategic introduction of an aromatic ring containing varying nitrogen content into PTh instigates polarized charge distribution and facilitates the narrowing of the band gap, thereby achieving efficient photocatalytic activities for both hydrogen and hydrogen peroxide generation. Notably, the best sample, PTh-N2, even demonstrates photocatalytic activity in the red light region (600-700 nm). This study offers a promising avenue for the development of polymer photocatalysts with efficient photocatalytic performance for red light-induced photocatalysis.
Keyword ：
Hydrogen evolution Hydrogen evolution Hydrogen peroxide evolution Hydrogen peroxide evolution Polarized charge distribution Polarized charge distribution Polythiophene derivatives Polythiophene derivatives Red light-induced photocatalysis Red light-induced photocatalysis
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| GB/T 7714 | Chen, Qian , Tian, Lin , Ren, Wei et al. Nitrogen Modified Linear Polythiophene Derivatives with Polarized Charge Distribution for Red Light-Induced Photocatalysis [J]. | CHEMSUSCHEM , 2025 , 18 (10) . |
| MLA | Chen, Qian et al. "Nitrogen Modified Linear Polythiophene Derivatives with Polarized Charge Distribution for Red Light-Induced Photocatalysis" . | CHEMSUSCHEM 18 . 10 (2025) . |
| APA | Chen, Qian , Tian, Lin , Ren, Wei , Zhang, Xirui , Li, Guosheng , Wang, Sibo et al. Nitrogen Modified Linear Polythiophene Derivatives with Polarized Charge Distribution for Red Light-Induced Photocatalysis . | CHEMSUSCHEM , 2025 , 18 (10) . |
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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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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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| 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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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 sta-bility,providing a CO yielding rate of 17 μmol 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.
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| GB/T 7714 | Ziruo Zhou , Wenyu Guo , Tingyu Yang et al. Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction [J]. | 结构化学 , 2024 , 43 (3) : 10-18 . |
| MLA | Ziruo Zhou et al. "Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction" . | 结构化学 43 . 3 (2024) : 10-18 . |
| APA | Ziruo Zhou , Wenyu Guo , Tingyu Yang , Dandan Zheng , Yuanxing Fang , Xiahui Lin et al. Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction . | 结构化学 , 2024 , 43 (3) , 10-18 . |
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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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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.
Keyword ：
covalent organic frameworks covalent organic frameworks donor-acceptor COFs donor-acceptor COFs H-2 evolution H-2 evolution photocatalysis photocatalysis
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| GB/T 7714 | Liu, Nengyi , Xie, Shuailei , Huang, Yuxing 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, Nengyi et al. "Dual-Acceptor Engineering in Pyrene-Based Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution" . | ADVANCED ENERGY MATERIALS 14 . 40 (2024) . |
| APA | Liu, Nengyi , Xie, Shuailei , Huang, Yuxing , Lu, Jiaping , Shi, Hongjie , Xu, Shumeng 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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