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学者姓名：张贵刚
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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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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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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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The selective conversion of ethane (C2H6) to ethylene (C2H4) under mild conditions is highly wanted, yet very challenging. Herein, it is demonstrated that a Pt/WO3-x catalyst, constructed by supporting ultrafine Pt nanoparticles on the surface of oxygen-deficient tungsten oxide (WO3-x) nanoplates, is efficient and reusable for photocatalytic C2H6 dehydrogenation to produce C2H4 with high selectivity. Specifically, under pure light irradiation, the optimized Pt/WO3-x photocatalyst exhibits C2H4 and H2 yield rates of 291.8 and 373.4 mu mol g-1 h-1, respectively, coupled with a small formation of CO (85.2 mu mol g-1 h-1) and CH4 (19.0 mu mol g-1 h-1), corresponding to a high C2H4 selectivity of 84.9%. Experimental and theoretical studies reveal that the vacancy-rich WO3-x catalyst enables broad optical harvesting to generate charge carriers by light for working the redox reactions. Meanwhile, the Pt cocatalyst reinforces adsorption of C2H6, desorption of key reaction species, and separation and migration of light-induced charges to promote the dehydrogenation reaction with high productivity and selectivity. In situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory calculation expose the key intermediates formed on the Pt/WO3-x catalyst during the reaction, which permits the construction of the possible C2H6 dehydrogenation mechanism. The Pt/WO3-x photocatalyst consisted of ultrafine Pt nanoparticles supported on the surface of oxygen-defective tungsten oxide nanoplates manifests high activity and fine reusability for selective ethylene formation from ethane dehydrogenation by simulated sunlight under mild conditions. image
Keyword ：
ethylene production ethylene production lattice oxygen lattice oxygen oxygen vacancy oxygen vacancy photocatalysis photocatalysis tungsten oxide tungsten oxide
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| GB/T 7714 | Liu, Yue , Xue, Weichao , Liu, Xiaoqing et al. Ultrafine Pt Nanoparticles on Defective Tungsten Oxide for Photocatalytic Ethylene Synthesis [J]. | SMALL , 2024 . |
| MLA | Liu, Yue et al. "Ultrafine Pt Nanoparticles on Defective Tungsten Oxide for Photocatalytic Ethylene Synthesis" . | SMALL (2024) . |
| APA | Liu, Yue , Xue, Weichao , Liu, Xiaoqing , Wei, Fen , Lin, Xiahui , Lu, Xue Feng et al. Ultrafine Pt Nanoparticles on Defective Tungsten Oxide for Photocatalytic Ethylene Synthesis . | SMALL , 2024 . |
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Thermal catalytic oxidative dehydrogenation of ethane with O2 has been extensively studied as an approach for ethene production, but this approach is energy intensive and has disadvantages of overoxidation, high-cost and safety concerns. Herein, we present ZnO-supported Pt nanoparticles that are highly active and selective for dehydrogenating ethane to ethene with simulated sunlight via a photo-supported Mars-van Krevelen mechanism. The Pt/ZnO catalyst achieves a high ethane-to-ethene conversion rate of 867.8 mu mol h-1 g-1 and an excellent selectivity of 97.56%. Besides, it is also coking-resistant and can be readily revived by exposure to O2 for refilling the consumed lattice oxygen to preserve its original activity. It is revealed that the Pt species facilitate C2H4 desorption from the catalyst to inhibit overoxidation and enhance separation of light-induced charges to boost the photocatalytic efficiency. Whilst the photogenerated holes on ZnO are captured by surface lattice oxygen to generate active O- species, H atoms were extracted from adsorbed C2H6 to produce C2H4. In situ diffuse reflectance infrared Fourier transform spectroscopy is applied to detect the key intermediates and thus propose the possible catalytic EDH process over the Pt/ZnO photocatalyst. A Pt/ZnO photocatalyst is efficient and reusable for ethene production from ethane dehydrogenation with simulated sunlight, affording outstanding C2H4 productivity of 867.8 mu mol h-1 g-1 and selectivity of 97.56%.
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| GB/T 7714 | Guo, Wenyu , Shi, Wenwen , Cai, Junjian et al. Photocatalytic ethene synthesis from ethane dehydrogenation with high selectivity by ZnO-supported Pt nanoparticles [J]. | CATALYSIS SCIENCE & TECHNOLOGY , 2024 , 14 (10) : 2921-2928 . |
| MLA | Guo, Wenyu et al. "Photocatalytic ethene synthesis from ethane dehydrogenation with high selectivity by ZnO-supported Pt nanoparticles" . | CATALYSIS SCIENCE & TECHNOLOGY 14 . 10 (2024) : 2921-2928 . |
| APA | Guo, Wenyu , Shi, Wenwen , Cai, Junjian , Wei, Fen , Lin, Xiahui , Lu, Xuefeng et al. Photocatalytic ethene synthesis from ethane dehydrogenation with high selectivity by ZnO-supported Pt nanoparticles . | CATALYSIS SCIENCE & TECHNOLOGY , 2024 , 14 (10) , 2921-2928 . |
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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 . |
| MLA | Liu, N. et al. "Dual–Acceptor Engineering in Pyrene-Based Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution" . | Advanced Energy Materials (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 . |
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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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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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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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