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学者姓名：汪思波
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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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Proton exchange membrane water electrolysis (PEMWE) technology is seen as the most compatible hydrogen production technology with renewable energy generation. However, the sluggish kinetics of the anodic oxygen evolution reaction (OER) and the scarcity of acid-resistant, high-activity, and low-cost catalysts have seriously hindered the overall efficiency and manufacturing costs of PEMWE. Recently, ruthenium (Ru)-based materials have gradually attracted attention due to their suitable binding strength toward oxygen intermediates and lowest price in the noble metal family. Herein, the great achievements and progress of Ru-based acidic OER electrocatalysts are comprehensively reviewed, which started with a general description of reaction mechanisms and in situ characterization techniques to understand the structure-activity relationships. Subsequently, some typical strategies to enhance the activity and stability of Ru-based electrocatalysts are highlighted. Insights from synthesis methods, advanced characterizations, intermediate evolution, and theoretical calculations are provided, together with our viewpoints on the daunting challenges and future endeavors of Ru-based OER electrocatalysts for their practical employment. © 2024 American Chemical Society.
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| GB/T 7714 | Li, J. , Zeng, J. , Zhao, F. et al. A Review on Highly Efficient Ru-Based Electrocatalysts for Acidic Oxygen Evolution Reaction [J]. | Energy and Fuels , 2024 , 38 (13) : 11521-11540 . |
| MLA | Li, J. et al. "A Review on Highly Efficient Ru-Based Electrocatalysts for Acidic Oxygen Evolution Reaction" . | Energy and Fuels 38 . 13 (2024) : 11521-11540 . |
| APA | Li, J. , Zeng, J. , Zhao, F. , Sun, X. , Wang, S. , Lu, X.F. . A Review on Highly Efficient Ru-Based Electrocatalysts for Acidic Oxygen Evolution Reaction . | Energy and Fuels , 2024 , 38 (13) , 11521-11540 . |
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The photocatalytic selective oxidation of CH4 to value-added higher hydrocarbons presents a promising avenue for the sustainable development of the chemical industry; however, the mild activation and conversion of CH4 remain great challenges. Herein, a novel Au/Zn2Ti3O8 hybrid photocatalyst is assembled from supporting Au nanoparticles (NPs) on the surface of Zn2Ti3O8 nanospheres. The Zn2Ti3O8 semiconductor with Zn2+ active sites drives the CH4 coupling reaction, while the Au NPs promote the separation and migration of charge carriers. When irradiated with a 365 LED light, the 1.0%-Au/Zn2Ti3O8 catalyst exhibits high activity and stability for selective CH4 coupling with O2, affording an optimal C2H6 yield of 609.49 μmol g−1 h−1 with 80.18% selectivity, which is among the state-of-the-art values under comparable conditions. Besides, the 1.0%-Au/Zn2Ti3O8 sample affords a turnover number (TON) of 239.1 and an apparent quantum efficiency (AQE) of 1.05% at 365 nm. Studies reveal that the Schottky junction interface strongly promotes photoinduced electrons to be transferred to Au from Zn2Ti3O8, realizing directed separation and migration of charge carriers for high photocatalytic activity. Various in situ spectroscopy analyses expose that the key ˙CH3 species in CH4-to-C2H6 conversion are stabilized by the surface Au sites for the subsequent coupling reaction to form C2H6, which prevents the undesirable overoxidation reaction to afford high C2H6 selectivity. A possible photocatalytic oxidative CH4 coupling mechanism over the Au/Zn2Ti3O8 hybrid is also proposed. © 2024 The Royal Society of Chemistry.
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| GB/T 7714 | Huang, Q. , Cai, J. , Wei, F. et al. Selective oxidative coupling of methane to ethane with oxygen using an Au/Zn2Ti3O8 photocatalyst under mild conditions [J]. | Journal of Materials Chemistry A , 2024 , 12 (32) : 21334-21340 . |
| MLA | Huang, Q. et al. "Selective oxidative coupling of methane to ethane with oxygen using an Au/Zn2Ti3O8 photocatalyst under mild conditions" . | Journal of Materials Chemistry A 12 . 32 (2024) : 21334-21340 . |
| APA | Huang, Q. , Cai, J. , Wei, F. , Fan, Y. , Liang, Z. , Liu, K. et al. Selective oxidative coupling of methane to ethane with oxygen using an Au/Zn2Ti3O8 photocatalyst under mild conditions . | Journal of Materials Chemistry A , 2024 , 12 (32) , 21334-21340 . |
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Developing highly efficient S-scheme photocatalysts is a subject of immense interest for harnessing so-lar energy towards sustainable hydrogen production.Herein,a novel S-scheme heterojunction of oxygen vacancy-rich CoMoO4/CN(CMO/CN)photocatalyst was rationally constructed through loading CoMoO4 nanorods on carbon nitride(CN)nanosheets via a direct one-pot calcination method.The CMO/CN S-scheme heterojunction exhibited enhanced surface area,fine CN dispersion,rich oxygen vacancies,and accelerated charge separation/transfer efficiency,which were conducive to improving photocatalytic H2 evolution performance.Of note,the optimal 3％CMO/CN sample displayed the highest H2 production rate of 8.35 mmol g-1 h-1,which is 4.6 folds that of pristine CN.In situ irradiated X-ray photoelectron spectroscopy(XPS)and electron paramagnetic resonance(EPR)characterizations confirmed the S-scheme charge transfer path between CN and CMO,which greatly promoted spatial charge separation.Density functional theory(DFT)calculations together with contact angle tests revealed the reduced activation energies for H2O dissociation and enhanced hydrophilicity of the CMO/CN.The CMO/CN photocatalysts also presented high stability and fine reusability.This work may provide insights into the combination of defect engineering and heterojunction designing for high-efficiency solar-to-chemical energy conversion.
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| GB/T 7714 | Jiani Qin , Yanli Dong , Xiaojuan Lai et al. Oxygen vacancy-rich CoMoO4/Carbon nitride S-scheme heterojunction for boosted photocatalytic H2 production:Microstructure regulation and charge transfer mechanism [J]. | 材料科学技术（英文版） , 2024 , 198 (31) : 176-185 . |
| MLA | Jiani Qin et al. "Oxygen vacancy-rich CoMoO4/Carbon nitride S-scheme heterojunction for boosted photocatalytic H2 production:Microstructure regulation and charge transfer mechanism" . | 材料科学技术（英文版） 198 . 31 (2024) : 176-185 . |
| APA | Jiani Qin , Yanli Dong , Xiaojuan Lai , Bo Su , Bao Pan , Chuanyi Wang et al. Oxygen vacancy-rich CoMoO4/Carbon nitride S-scheme heterojunction for boosted photocatalytic H2 production:Microstructure regulation and charge transfer mechanism . | 材料科学技术（英文版） , 2024 , 198 (31) , 176-185 . |
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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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Metal nanoparticle (NP) cocatalysts are widely investigated for their ability to enhance the performance of photocatalytic materials; however, their practical application is often limited by the inherent instability under light irradiation. This challenge has catalyzed interest in exploring high-entropy alloys (HEAs), which, with their increased entropy and lower Gibbs free energy, provide superior stability. In this study, 3.5 nm-sized noble-metal-free NPs composed of a FeCoNiCuMn HEA are successfully synthesized. With theoretic calculation and experiments, the electronic structure of HEA in augmenting the catalytic CO2 reduction has been uncovered, including the individual roles of each element and the collective synergistic effects. Then, their photocatalytic CO2 reduction capabilities are investigated when immobilized on TiO2. HEA NPs significantly enhance the CO2 photoreduction, achieving a 23-fold increase over pristine TiO2, with CO and CH4 production rates of 235.2 and 19.9 mu mol g(-1) h(-1), respectively. Meanwhile, HEA NPs show excellent stability under simulated solar irradiation, as well high-energy X-ray irradiation. This research emphasizes the promising role of HEA NPs, composed of earth-abundant elements, in revolutionizing the field of photocatalysis.
Keyword ：
high-entropy alloy high-entropy alloy nanoparticle nanoparticle noble-metal-free noble-metal-free photocatalytic CO2 reduction photocatalytic CO2 reduction
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| GB/T 7714 | Huang, Haowei , Zhao, Jiwu , Guo, Hele et al. Noble-Metal-Free High-Entropy Alloy Nanoparticles for Efficient Solar-Driven Photocatalytic CO2 Reduction [J]. | ADVANCED MATERIALS , 2024 , 36 (26) . |
| MLA | Huang, Haowei et al. "Noble-Metal-Free High-Entropy Alloy Nanoparticles for Efficient Solar-Driven Photocatalytic CO2 Reduction" . | ADVANCED MATERIALS 36 . 26 (2024) . |
| APA | Huang, Haowei , Zhao, Jiwu , Guo, Hele , Weng, Bo , Zhang, Hongwen , Saha, Rafikul Ali et al. Noble-Metal-Free High-Entropy Alloy Nanoparticles for Efficient Solar-Driven Photocatalytic CO2 Reduction . | ADVANCED MATERIALS , 2024 , 36 (26) . |
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Polymer-based photoanodes for the water oxidation reaction have recently garnered attention, with carbon nitride standing out due to its numerous advantages. This study focuses on synthesizing crystalline carbon nitride photoanodes, specifically poly(heptazine imide) (PHI), and explores the role of salts in their production. Using a binary molten salt system, optimal photocurrent density of 365 μA·cm−2 was achieved with a voltage bias of 1.23 V versus the reversible hydrogen electrode under AM 1.5G illumination, this performance is ca. 18 times to the pristine PCN photoanode. In this process, NH₄SCN facilitates the growth of SnS2 seeding layers, while K2CO3 enhances film crystallinity. In situ electrochemical analyses show that this salt combination improves photoexcited charge transfer efficiency and minimizes resistance in the SnS2 layer. This study clarifies the role of salts in synthesizing the PHI photoanode and provides insights for designing high-crystallinity carbon nitride-based functional films. © Editorial office of Acta Physico-Chimica Sinica.
Keyword ：
Binary salts Binary salts Ionothermal synthesis Ionothermal synthesis Photoanode Photoanode Poly-heptazine-imide Poly-heptazine-imide Water oxidation Water oxidation
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| GB/T 7714 | Su, J. , Zhang, J. , Chai, S. et al. Optimizing Poly(heptazine imide) Photoanodes Using Binary Molten Salt Synthesis for Water Oxidation Reaction [J]. | Acta Physico - Chimica Sinica , 2024 , 40 (12) . |
| MLA | Su, J. et al. "Optimizing Poly(heptazine imide) Photoanodes Using Binary Molten Salt Synthesis for Water Oxidation Reaction" . | Acta Physico - Chimica Sinica 40 . 12 (2024) . |
| APA | Su, J. , Zhang, J. , Chai, S. , Wang, Y. , Wang, S. , Fang, Y. . Optimizing Poly(heptazine imide) Photoanodes Using Binary Molten Salt Synthesis for Water Oxidation Reaction . | Acta Physico - Chimica Sinica , 2024 , 40 (12) . |
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Thermocatalytic nonoxidative ethane dehydrogenation(EDH)is a promising strategy for ethene produc-tion but suffers from intense energy consumption and poor catalyst durability;exploring technology that permits efficient EDH by solar energy remains a giant challenge.Herein,we present that an oxygen va-cancy(Ov)-rich LaVO4(LaV04-Ov)catalyst is highly active and stable for photocatalytic EDH,through a dynamic lattice oxygen(Olatt.)and Ov co-mediated mechanism.Irradiated by simulated sunlight at mild conditions,LaVO4-Ov effectively dehydrogenates undiluted ethane to produce C2H4 and CO with a con-version of 2.3％.By loading a small amount of Pt cocatalyst,the evolution and selectivity of C2H4 are en-hanced to 275 μmol h-1 g-1 and 96.8％.Of note,LaVO4-Ov appears nearly no carbon deposition after the reaction.The isotope tracked reactions reveal that the consumed Olatt.recuperates by exposing the used catalyst with O2,thus establishing a dynamic cycle of Olatt,and achieving a facile catalyst regeneration to preserve its intrinsic activity.The refreshed LaVO4-Ov exhibits superior reusability and delivers a turnover number of about 305.The Ov promotes photo absorption,boosts ethane adsorption/activation,and accel-erates charge separation/transfer,thus improving the photocatalytic efficiency.The possible photocatalytic EDH mechanism is proposed,considering the key intermediates predicted by density functional theory(DFT)and monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS).
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| GB/T 7714 | Fen Wei , Weichao Xue , Zhiyang Yu et al. Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO4 catalyst [J]. | 中国化学快报（英文版） , 2024 , 35 (3) : 171-176 . |
| MLA | Fen Wei et al. "Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO4 catalyst" . | 中国化学快报（英文版） 35 . 3 (2024) : 171-176 . |
| APA | Fen Wei , Weichao Xue , Zhiyang Yu , Xue Feng Lu , Sibo Wang , Wei Lin et al. Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO4 catalyst . | 中国化学快报（英文版） , 2024 , 35 (3) , 171-176 . |
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