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学者姓名:孙再成
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摘要 :
It is a challenging task to overcomes the bottleneck of N2 adsorption and activation in N2 reduction reaction (NRR). Regulating the catalyst surface electronic state is treated as a potential strategy to prevail over the barrier. Here, Incorporating Fe as a dopant in the TiO2 nanoparticles can generate oxygen vacancies and dopant energy levels, promoting the adsorption and activation of N2 molecules. F surface modification induces Fe (III) in the high spin state and upshifts the dopant energy level. That facilitates Fe 3d electrons backdonation to N 1ag* orbital promotes the activation of N2 molecule and reduces the limiting potential of NRR. Therefore, F-Fe: TiO2 electrocatalyst achieved the highest Faradaic efficiency and maximum NH3 production rate of 27.67% and 27.86 mu g h-1 mgcat. -1 at -0.5 V v.s. reversible hydrogen electrode. This work provides deep insights into the design surface electronic state of catalyst toward efficient N2 to NH3 conversion.
关键词 :
Electrocatalysis Electrocatalysis Iron doping Iron doping N-2 Fixation N-2 Fixation Surface electronic state manipulation Surface electronic state manipulation Surface fluorine treatment Surface fluorine treatment
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GB/T 7714 | Song, Guangxin , Gao, Rui , Zhao, Zhao et al. High-spin state Fe(III) doped TiO2 for electrocatalytic nitrogen fixation induced by surface F modification [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2022 , 301 . |
MLA | Song, Guangxin et al. "High-spin state Fe(III) doped TiO2 for electrocatalytic nitrogen fixation induced by surface F modification" . | APPLIED CATALYSIS B-ENVIRONMENTAL 301 (2022) . |
APA | Song, Guangxin , Gao, Rui , Zhao, Zhao , Zhang, Yujun , Tan, Huaqiao , Li, Haibo et al. High-spin state Fe(III) doped TiO2 for electrocatalytic nitrogen fixation induced by surface F modification . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2022 , 301 . |
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摘要 :
Highly active and efficient photocatalysts are crucial for the exploration of ammonia synthesis because of the serious problem of energy deficiency. La2TiO5 (LTO) perovskite materials have great advantages in the field of photocatalytic nitrogen fixation because of the broadly diversified properties. The rational design of surface defect is a valid method to modulate photoinduced charge traps and create defect energy levels, especially it is an effective way to suppress the photoinduced charge recombination. Herein, LTO was obtained by a simple sol-gel method and was further reduced by NaBH4 to introduce oxygen defect on its surface. UV-vis spectra proved that the surface defects could reduce the band gap value of samples, which is beneficial for improving photocatalytic nitrogen fixation activity. For the best photocatalytic samples with good cycle stability, the nitrogen fixation rate is 158.13 mu mol.g(-1).h(-1). The mechanism of photocatalytic nitrogen fixation was proposed by the PL, XPS, and PEC results, which provided possibilities for exploring more promising perovskite catalysts in the field of nitrogen fixation. (C) 2021 Elsevier Inc. All rights reserved.
关键词 :
La2TiO5 La2TiO5 Nitrogen fixation Nitrogen fixation Photocatalysis Photocatalysis Surface modification Surface modification
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GB/T 7714 | Song, Muyao , Wang, Lijing , Li, Jiaxin et al. Defect density modulation of La2TiO5: An effective method to suppress electron-hole recombination and improve photocatalytic nitrogen fixation [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2021 , 602 : 748-755 . |
MLA | Song, Muyao et al. "Defect density modulation of La2TiO5: An effective method to suppress electron-hole recombination and improve photocatalytic nitrogen fixation" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 602 (2021) : 748-755 . |
APA | Song, Muyao , Wang, Lijing , Li, Jiaxin , Sun, Dewu , Guan, Renquan , Zhai, Hongju et al. Defect density modulation of La2TiO5: An effective method to suppress electron-hole recombination and improve photocatalytic nitrogen fixation . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2021 , 602 , 748-755 . |
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摘要 :
A photocatalyst system is generally comprises a catalyst and cocatalyst to achieve light absorption, electron-hole separation, and surface reaction. It is a challenge to develop a single photocatalyst having all functions so as to lower the efficiency loss. Herein, the active GaN4 site is integrated into a polymeric carbon nitride (CN) photocatalyst (GCN), which displays an excellent H2 production rate of 9904 μmol h-1 g-1 . It is 162 and 3.3 times higher than that of CN with the absence (61 μmol h-1 g-1 ) and presence (2981 μmol h-1 g-1 ), respectively, of 1.0 wt % Pt. Under light irradiation the electron is injected and stored at the GaN4 site, where the LUMO locates. The HOMO distributes on the aromatic ring resulting in spatial charge separation. Transient photovoltage discloses the electron-storage capability of GCN. The negative GaN4 promotes proton adsorption in the excited state. The positive adsorption energy drives H2 desorption from GaN4 after passing the electron to the proton. This work opens up opportunities for exploring a novel catalyst for H2 production.
关键词 :
carbon nitride carbon nitride gallium gallium hydrogen hydrogen photocatalysis photocatalysis structure elucidation structure elucidation
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GB/T 7714 | Jiang Wenshuai , Zhao Yajie , Zong Xupeng et al. Photocatalyst for High-Performance H2 Production: Ga-Doped Polymeric Carbon Nitride. [J]. | Angewandte Chemie , 2021 , 60 (11) : 6124-6129 . |
MLA | Jiang Wenshuai et al. "Photocatalyst for High-Performance H2 Production: Ga-Doped Polymeric Carbon Nitride." . | Angewandte Chemie 60 . 11 (2021) : 6124-6129 . |
APA | Jiang Wenshuai , Zhao Yajie , Zong Xupeng , Nie Haodong , Niu Lijuan , An Li et al. Photocatalyst for High-Performance H2 Production: Ga-Doped Polymeric Carbon Nitride. . | Angewandte Chemie , 2021 , 60 (11) , 6124-6129 . |
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GB/T 7714 | Zong, Xupeng , Jiang, Wenshuai , Sun, Zaicheng . Efficient photocatalytic overall water splitting achieved with polymeric semiconductor-based Z-scheme heterostructures [J]. | SCIENCE CHINA-CHEMISTRY , 2021 , 64 (6) : 875-876 . |
MLA | Zong, Xupeng et al. "Efficient photocatalytic overall water splitting achieved with polymeric semiconductor-based Z-scheme heterostructures" . | SCIENCE CHINA-CHEMISTRY 64 . 6 (2021) : 875-876 . |
APA | Zong, Xupeng , Jiang, Wenshuai , Sun, Zaicheng . Efficient photocatalytic overall water splitting achieved with polymeric semiconductor-based Z-scheme heterostructures . | SCIENCE CHINA-CHEMISTRY , 2021 , 64 (6) , 875-876 . |
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摘要 :
Photocatalytic N-2 fixation (PNF) provides a low-cost route to generate ammonia. The poor conversion efficiency from photon to ammonia seriously hinders the step forward because of the low concentration of N-2 molecules. Herein, we demonstrate a photocatalyst with surface oxygen vacancies (Vo) and a F modified surface to facilitate N-2 adsorption and activation on the surface of catalysts. The Vo site promotes the chemical adsorption of N-2, electron transfer from catalyst to N-2. F modification switches the TiO2 surface properties from hydrophilic to aerophilic, thus facilitating the adsorption of N-2. Meanwhile, the hydrogen reduction reaction (HER) is sup-pressed, as protons hard to adsorb on F capped surfaces. The optimal NH3 production rate can reach 206 mu molh(-1)g(-1), which is similar to 9 times higher than that of pure TiO2 nanoparticles (similar to 23 mu molh(-1)g(-1)). This report provides a potential strategy to overcome mass transfer limitation and achieve a high conversion efficiency in PNF.
关键词 :
Hydrophobized Hydrophobized N-2 fixation N-2 fixation Photocatalysis Oxygen vacancy Photocatalysis Oxygen vacancy TiO2 TiO2
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GB/T 7714 | Guan, Renquan , Wang, Dandan , Zhang, Yujun et al. Enhanced photocatalytic N-2 fixation via defective and fluoride modified TiO2 surface [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2021 , 282 . |
MLA | Guan, Renquan et al. "Enhanced photocatalytic N-2 fixation via defective and fluoride modified TiO2 surface" . | APPLIED CATALYSIS B-ENVIRONMENTAL 282 (2021) . |
APA | Guan, Renquan , Wang, Dandan , Zhang, Yujun , Liu, Chen , Xu, Wei , Wang, Jiaou et al. Enhanced photocatalytic N-2 fixation via defective and fluoride modified TiO2 surface . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2021 , 282 . |
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摘要 :
碳点合成原料来源广泛,发光性能可调,生物相容性良好,在生物成像、离子检测、发光材料等领域具有巨大的应用潜力.本文综述了碳点的制备方法、发光原理以及应用,重点介绍了碳点的制备方法,总结了近年来碳点在催化、生物成像等领域的最新进展;指出未来研究中需要进一步对碳点的合成进行优化,深入探究碳点的发光机理;制备发光波长可调、尺寸可调的碳点,对其在发光器件、生物成像、传感等领域的应用具有重要意义.
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GB/T 7714 | 张震 , 曲丹 , 安丽 et al. 荧光碳点的制备、发光机理及应用 [J]. | 发光学报 , 2021 , 42 (8) : 1125-1140 . |
MLA | 张震 et al. "荧光碳点的制备、发光机理及应用" . | 发光学报 42 . 8 (2021) : 1125-1140 . |
APA | 张震 , 曲丹 , 安丽 , 汪夏燕 , 孙再成 . 荧光碳点的制备、发光机理及应用 . | 发光学报 , 2021 , 42 (8) , 1125-1140 . |
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摘要 :
The common strategy for the design of photocatalytic materials is to load small-sized cocatalysts onto large-sized photocatalysts for efficient charge separation. In this study, a new design strategy is presented to anchor smallsized TiO2 photocatalysts onto large-sized Ti3C2-Mxene cocatalysts, which can provide enriched active sites to receive photo-generated electrons, thus achieving fast charge separation. Based on this strategy, the 4h-hydrogen production rate of the optimized photocatalytic system (62.5 mu mol) is 15.2 times higher than that of pure TiO2 (4.1 mu mol), strongly demonstrating the feasibility of our design strategy. The strategy here presents an effective way to design novel photocatalytic systems with superior photocatalytic properties.
关键词 :
Design strategy Design strategy Large-sized cocatalyst Large-sized cocatalyst Photocatalytic water splitting Photocatalytic water splitting Ultra-small photocatalyst Ultra-small photocatalyst
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GB/T 7714 | Li, Weiming , Zhuang, Chunqiang , Li, Yuanli et al. Anchoring ultra-small TiO2 & nbsp;quantum dots onto ultra-thin and large-sized Mxene nanosheets for highly efficient photocatalytic water splitting [J]. | CERAMICS INTERNATIONAL , 2021 , 47 (15) : 21769-21776 . |
MLA | Li, Weiming et al. "Anchoring ultra-small TiO2 & nbsp;quantum dots onto ultra-thin and large-sized Mxene nanosheets for highly efficient photocatalytic water splitting" . | CERAMICS INTERNATIONAL 47 . 15 (2021) : 21769-21776 . |
APA | Li, Weiming , Zhuang, Chunqiang , Li, Yuanli , Gao, Chunlang , Jiang, Wenshuai , Sun, Zaicheng et al. Anchoring ultra-small TiO2 & nbsp;quantum dots onto ultra-thin and large-sized Mxene nanosheets for highly efficient photocatalytic water splitting . | CERAMICS INTERNATIONAL , 2021 , 47 (15) , 21769-21776 . |
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摘要 :
The nitrogen cycle plays an important role in nature, but N-containing products cannot meet human needs. The electrochemical synthesis of ammonia under ambient conditions has attracted the interest of many researchers because it provides a clean and pollution-free synthesis method; however, it has certain difficulties, including a high activation energy, multiple electron transfer, and hydrogenation. Thermodynamic factors limit the selectivity and activity of ammonia synthesis techniques. This review summarizes progress in the electrochemical synthesis of ammonia from theory and experiment. Theoretically, the reduction of nitrogen molecules is analyzed using orbit theory and the thermodynamic reaction pathways. Experimentally, we first discuss the effect of the experimental setup on the nitrogen reduction reaction, and then the four critical of catalysts, including size, electronic, coordination, and orientation effects. These issues must be considered to produce highly-efficient catalysts for electrochemical nitrogen reduction (eNRR). This review provides an overview of the eNRR to enable future researchers to design rational catalysts. © 2021 Science Press
关键词 :
Activation energy Activation energy Ammonia Ammonia Coordination reactions Coordination reactions Electrocatalysts Electrocatalysts Electrolytic reduction Electrolytic reduction Nitrogen Nitrogen Nitrogen fixation Nitrogen fixation
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GB/T 7714 | Niu, Lijuan , An, Li , Wang, Xiayan et al. Effect on electrochemical reduction of nitrogen to ammonia under ambient conditions: Challenges and opportunities for chemical fuels [J]. | Journal of Energy Chemistry , 2021 , 61 : 304-318 . |
MLA | Niu, Lijuan et al. "Effect on electrochemical reduction of nitrogen to ammonia under ambient conditions: Challenges and opportunities for chemical fuels" . | Journal of Energy Chemistry 61 (2021) : 304-318 . |
APA | Niu, Lijuan , An, Li , Wang, Xiayan , Sun, Zaicheng . Effect on electrochemical reduction of nitrogen to ammonia under ambient conditions: Challenges and opportunities for chemical fuels . | Journal of Energy Chemistry , 2021 , 61 , 304-318 . |
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摘要 :
Transition metal alloys and their compounds have been drafted as relatively economic and high-activity non-noble metal electrocatalysts for the oxygen reduction reaction (ORR). However, the stability of catalysts is regarded as a critical issue for practical application. Here, we report CoNi alloy nanoparticles embedded in a nitrogen-doped graphite carbon nanotube (CoNi@N-GCNT-FD) electrocatalyst, which is synthesized from metal precursors and dicyandiamide nanofibers formed by freeze-drying pretreatment. The electrocatalyst exhibits remarkable ORR performance (a positive onset potential at 0.90 V vs reversible hydrogen electrode (RHE), a half-wave potential at 0.84 V vs RHE, and a high limiting current density (6.4 mA cm(-2))) in an alkaline medium. The outstanding ORR catalytic behavior is attributable to the properties with a high specific surface area and the collaborative influence between a CoNi alloy and a nanotube protective layer. The CoNi@N-GCNT-FD also displays antimethanol toxicity and good stability over 10,000 cycles, attributed to the unique structure of N-GCNT that is more conducive to mass transfer and protects the alloy particles from corrosion under harsh conditions. This simple route can be widely used to prepare other alloy electrocatalysts with relatively economic value and high performance in power conversion and stockpile device fields.
关键词 :
CoNi alloy CoNi alloy electrocatalyst electrocatalyst N-doped graphite carbon nanotubes N-doped graphite carbon nanotubes nonprecious metal catalysts nonprecious metal catalysts oxygen reduction reaction oxygen reduction reaction
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GB/T 7714 | Niu, Lijuan , Liu, Guohua , Li, Yifan et al. CoNi Alloy Nanoparticles Encapsulated in N-Doped Graphite Carbon Nanotubes as an Efficient Electrocatalyst for Oxygen Reduction Reaction in an Alkaline Medium [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2021 , 9 (24) : 8207-8213 . |
MLA | Niu, Lijuan et al. "CoNi Alloy Nanoparticles Encapsulated in N-Doped Graphite Carbon Nanotubes as an Efficient Electrocatalyst for Oxygen Reduction Reaction in an Alkaline Medium" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING 9 . 24 (2021) : 8207-8213 . |
APA | Niu, Lijuan , Liu, Guohua , Li, Yifan , An, Jiawen , Zhao, Boyuan , Yang, Jingsu et al. CoNi Alloy Nanoparticles Encapsulated in N-Doped Graphite Carbon Nanotubes as an Efficient Electrocatalyst for Oxygen Reduction Reaction in an Alkaline Medium . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2021 , 9 (24) , 8207-8213 . |
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摘要 :
Photocatalytic hydrogen production from water splitting has received considerable attention in recent years. The bottle-neck issue for hydrogen production efficiency is the relative slow charge separation and efficient hydrogen evolution. Currently, the major strategy for developing catalysts is to anchor small noble-metal cocatalysts onto relatively large photocatalysts. In this study, extremely small photocatalysts of TiO2 quantum dots were loaded onto the low-cost micro-sized cocatalysts of porous NiO/NiS2 nanosheets, promoting the rapid charge separation of photogenerated electrons from small-sized photocatalysts to large-sized cocatalysts. The size of cocatalysts is three orders of magnitude larger than that of photocatalysts. The hydrogen production of designed catalysts is similar to 16 times higher than that of pure TiO2 photocatalysts, clearly demonstrating the critical role of large-sized porous cocatalysts. Our game-changing strategy provides a distinctive approach to design new kinds of photocatalysts with rapid charge separation and highly efficient hydrogen evolution.
关键词 :
Cocatalyst Cocatalyst Fast charge separation Fast charge separation Micro-sized porous nanosheet Micro-sized porous nanosheet Photocatalyst Photocatalyst Quantum dot Quantum dot
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GB/T 7714 | Li, Yuanli , Gao, Chunlang , Jiang, Wenshuai et al. A game-changing design of low-cost, large-size porous cocatalysts decorated by ultra-small photocatalysts for highly efficient hydrogen evolution [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2021 , 286 . |
MLA | Li, Yuanli et al. "A game-changing design of low-cost, large-size porous cocatalysts decorated by ultra-small photocatalysts for highly efficient hydrogen evolution" . | APPLIED CATALYSIS B-ENVIRONMENTAL 286 (2021) . |
APA | Li, Yuanli , Gao, Chunlang , Jiang, Wenshuai , Zhuang, Chunqiang , Tan, Wuyuan , Li, Weiming et al. A game-changing design of low-cost, large-size porous cocatalysts decorated by ultra-small photocatalysts for highly efficient hydrogen evolution . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2021 , 286 . |
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