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学者姓名：汪思波
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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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Among the current industrial hydrogen production technologies, electrolysis has attracted widespread attention due to its zero carbon emissions and sustainability. However, the existence of overpotential caused by reaction activation, mass/charge transfer, etc. makes the actual water splitting voltage higher than the theoretical value, severely limiting the industrial application of this technology. Therefore, it is particularly important to design and develop highly efficient electrocatalysts to reduce overpotential and improve energy efficiency. Among the various synthesis methods of electrocatalysts, electrochemical synthesis stands out due to its simplicity, easy reaction control, and low cost. This review article classifies and summarizes the electrochemical synthesis techniques (including electrodeposition, electrophoretic deposition, electrospinning, anodic oxidation, electrochemical intercalation, and electrochemical reconstruction), followed by their application in the field of water electrolysis. In addition, some challenges currently faced by electrochemical synthesis in electrocatalytic hydrogen production, and their potential solutions are discussed to promote the practical application of electrochemical synthesis in water electrolysis.Graphical AbstractThis review summarizes and classifies commonly used electrochemical synthesis techniques, followed by the application of electrochemical synthesis methods in research on water electrolysis. Additionally, some challenges faced by electrochemical synthesis in the field of water electrolysis and possible solutions are discussed.
Keyword ：
Electrocatalysts Electrocatalysts Electrochemical synthesis Electrochemical synthesis Green hydrogen Green hydrogen Water splitting Water splitting
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| GB/T 7714 | Wu, Yang , Xiao, Boxin , Liu, Kunlong et al. Electrochemical Synthesis of High-Efficiency Water Electrolysis Catalysts [J]. | ELECTROCHEMICAL ENERGY REVIEWS , 2025 , 8 (1) . |
| MLA | Wu, Yang et al. "Electrochemical Synthesis of High-Efficiency Water Electrolysis Catalysts" . | ELECTROCHEMICAL ENERGY REVIEWS 8 . 1 (2025) . |
| APA | Wu, Yang , Xiao, Boxin , Liu, Kunlong , Wang, Sibo , Hou, Yidong , Lu, Xue Feng et al. Electrochemical Synthesis of High-Efficiency Water Electrolysis Catalysts . | ELECTROCHEMICAL ENERGY REVIEWS , 2025 , 8 (1) . |
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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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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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Direct photocatalytic conversion of methane to value-added C1 oxygenate with O2 is of great interest but presents a significant challenge in achieving highly selective product formation. Herein, a general strategy for the construction of copper single-atom catalysts with a well-defined coordination microenvironment is developed on the basis of metal-organic framework for selective photo-oxidation of CH4 to HCHO. We propose the directional activation of O2 on the mono-copper site breaks the original equilibrium and tilts the balance of radical formation almost completely toward •OOH. The synchronously generated •OOH and •CH3 radicals rapidly combine to form HCHO while inhibiting competing reactions, thus resulting in ultra-highly selective HCHO production (nearly 100%) with a time yield of 2.75 mmol gcat−1 h−1. This work highlights the potential of rationally designing reaction sites to manipulate reaction pathways and achieve selective CH4 photo-oxidation, and could guide the further design of high-performance single-atom catalysts to meet future demand. © The Author(s) 2024.
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| GB/T 7714 | Feng, C. , Zuo, S. , Hu, M. et al. Optimizing the reaction pathway of methane photo-oxidation over single copper sites [J]. | Nature Communications , 2024 , 15 (1) . |
| MLA | Feng, C. et al. "Optimizing the reaction pathway of methane photo-oxidation over single copper sites" . | Nature Communications 15 . 1 (2024) . |
| APA | Feng, C. , Zuo, S. , Hu, M. , Ren, Y. , Xia, L. , Luo, J. et al. Optimizing the reaction pathway of methane photo-oxidation over single copper sites . | Nature Communications , 2024 , 15 (1) . |
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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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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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Abstract ：
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.
Keyword ：
charge separation charge separation hydrogen production hydrogen production photocatalysis photocatalysis poly(heptazineimide) poly(heptazineimide) water splitting water splitting
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| GB/T 7714 | Wang, Qian , Li, Shiyao , Zheng, Dandan 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, Qian 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, Qian , Li, Shiyao , Zheng, Dandan , Wang, Sibo , Hou, Yidong , Zhang, Guigang . 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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