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学者姓名：林立
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Abstract ：
The ammonia decomposition for the production of carbon-free hydrogen has triggered great attention yet still remains challenging due to its sluggish kinetics, posting the importance of precise design of efficient catalysts for ammonia decomposition under low temperatures. Constructing the metal-support interaction and interface is one of the most important strategies for promoting catalysts. In this work, by coating ceria onto the Ni nanoparticles (NPs), we discover that the Ni-CeO2 interfaces create an exceptional effect to enhance the catalytic decomposition of ammonia by over 10 folds, compared with the pristine Ni. The kinetic analysis demonstrates that the recombinative N2 desorption is the rate-determining step (RDS) and the Ni-CeO2 interface greatly increases the RDS. Based on these understandings, a strategy to fabricate the Ni/CeO2 catalyst with abundant Ni-Ce-O interfaces via one-pot sol-gel method was employed (hereafter denoted to s-Ni/CeO2). The s-Ni/CeO2 catalyst shows a high activity for ammonia decomposition, achieving a H2 formation rate of 10.5 mmol gcat-1 min-1 at 550 degrees C. Combined with a series of characterizations, the relationship between the catalyst structure and the performance was investigated for further understanding the effect of metal-oxide interfaces.
Keyword ：
Ammonia decomposition Ammonia decomposition Cerium oxide Cerium oxide Metal -oxide interfaces Metal -oxide interfaces Metal-support interaction Metal-support interaction Nickel Nickel
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| GB/T 7714 | Chen, Jiangping , Ren, Hongju , Wu, Kai et al. Boosting hydrogen production of ammonia decomposition via the construction of metal-oxide interfaces [J]. | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2024 , 43 (2) . |
| MLA | Chen, Jiangping et al. "Boosting hydrogen production of ammonia decomposition via the construction of metal-oxide interfaces" . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY 43 . 2 (2024) . |
| APA | Chen, Jiangping , Ren, Hongju , Wu, Kai , Fang, Huihuang , Chen, Chongqi , Lin, Li et al. Boosting hydrogen production of ammonia decomposition via the construction of metal-oxide interfaces . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2024 , 43 (2) . |
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Pyrochlore oxide A(2)B(2)O(7) is a potential anode catalyst of ammonia-fed solid oxide fuel cell (SOFC) due to its unique and open structure that can make some oxygen ions flow to occupy the hole position to form Frankel defect. Herein, various rare-earth ions with different radius are selected as the A site to construct defective pyrochlore oxide RE2Zr1.95Ni0.05O7+delta (REZN, RE = La, Pr, Nd, Sm, Gd, LZN/PZN/NZN/SZN/GZN) to gain insights into oxygen vacancies that can be the diffusion and adsorption active site for ammonia. In the n-type semiconductor REZN, the degree of crystal ordering decreases with the decrease of the radius of rare-earth RE3+ ions. Among them, GZN exhibits the most negative conduction band and the smallest band gap, making it easier to overcome the energy potential barrier and facilitate the movement of carriers. As a result, the conductivity of GZN is about 25 times higher than that of LZN. The average TEC value of GZN is 10.40 x 10(-6) K-1, which matches that of electrolyte YSZ (10.50 x 10(-6) K-1). The maximum power density of ammonia-fed SOFC supported by YSZ electrolyte based on GZN anode is 128.63 mW center dot cm(-2) at 800 degrees C, which is 2.3 times higher than that of NiO-based SOFC. The single cell based on GZN anode can be run continuously for 100 h at 800 degrees C without significant degradation. The preliminary results suggest that GZN oxide is promising to be a candidate catalyst for ammonia-fed SOFC anode.
Keyword ：
Ammonia-fed solid oxide fuel cell Ammonia-fed solid oxide fuel cell Ammonia oxidation Ammonia oxidation Electrochemical performance Electrochemical performance Geometry distortion Geometry distortion RE2Zr1.95Ni0.05O7+delta anode RE2Zr1.95Ni0.05O7+delta anode
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| GB/T 7714 | Zhong, Fulan , Wang, Xinmin , Wang, Lei et al. Tuning geometry distortion of pyrochlore RE2Zr1.95Ni0.05O7+delta anodes with rich oxygen vacancies for ammonia-fed solid oxide fuel cell [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2023 , 312 . |
| MLA | Zhong, Fulan et al. "Tuning geometry distortion of pyrochlore RE2Zr1.95Ni0.05O7+delta anodes with rich oxygen vacancies for ammonia-fed solid oxide fuel cell" . | SEPARATION AND PURIFICATION TECHNOLOGY 312 (2023) . |
| APA | Zhong, Fulan , Wang, Xinmin , Wang, Lei , Fang, Huihuang , Luo, Yu , Chen, Chongqi et al. Tuning geometry distortion of pyrochlore RE2Zr1.95Ni0.05O7+delta anodes with rich oxygen vacancies for ammonia-fed solid oxide fuel cell . | SEPARATION AND PURIFICATION TECHNOLOGY , 2023 , 312 . |
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Ammonia (NH3) decomposition to release COx-free hydrogen (H2) over non-noble catalysts has gained increasing attention. In this study, three nanostructured CeO2 with different morphologies, viz. rod (R), sphere (Sph), and spindle (Spi), were fabricated and served as supports for Ni/CeO2 catalyst. The CeO2 supports are different in particle sizes, specific surface area and porosity, resulting in the formation of Ni nanoparticles with distinguished sizes and dispersions. The surface properties of the Ni/CeO2 catalysts are not only distinct but also influential, affecting the adsorption and desorption of NH3, N2, and/or H2 molecules. The Ni/CeO2-R catalyst shows superior catalytic activity compared to the other two, owing to its smaller Ni crystallite size and larger BET surface area. The most abundant strong basic sites are observed for Ni/CeO2-Spi catalyst based on its exposed CeO2(110) planes, which facilitates the donation of electrons to the Ni particles, benefiting the associative desorption of N atoms. Thus, Ni/CeO2-Spi shows higher catalytic activity than Ni/CeO2-Sph, despite their almost identical Ni crystallite sizes.& COPY; 2022 Published by Elsevier B.V. on behalf of Chinese Society of Rare Earths.
Keyword ：
CeO2 CeO2 Electron donation Electron donation Hydrogen production Hydrogen production Morphology Morphology NH 3 decomposition NH 3 decomposition Ni Ni Rare earths Rare earths
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| GB/T 7714 | Chen, Chongqi , Fan, Xiaoshuang , Zhou, Chen et al. Hydrogen production from ammonia decomposition over Ni/CeO2 catalyst: Effect of CeO2 morphology* [J]. | JOURNAL OF RARE EARTHS , 2023 , 41 (7) : 1014-1021 . |
| MLA | Chen, Chongqi et al. "Hydrogen production from ammonia decomposition over Ni/CeO2 catalyst: Effect of CeO2 morphology*" . | JOURNAL OF RARE EARTHS 41 . 7 (2023) : 1014-1021 . |
| APA | Chen, Chongqi , Fan, Xiaoshuang , Zhou, Chen , Lin, Li , Luo, Yu , Au, Chaktong et al. Hydrogen production from ammonia decomposition over Ni/CeO2 catalyst: Effect of CeO2 morphology* . | JOURNAL OF RARE EARTHS , 2023 , 41 (7) , 1014-1021 . |
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Ammonia decomposition is a structure-sensitive reaction, so the difference in structure of Ammonia decomposition is a structure-sensitive reaction, so the difference in structure of similar catalysts may have a great impact on the catalytic performance of ammonia decomposition reaction. However, it is not clear which structural properties can play a role in ammonia decomposition reaction and the degree of influence on catalytic performance. To explore this question, ammonia evaporation-hydrothermal (AEH), impregnation (IM), and evaporation-induced self-assembly (EISA) methods were used to synthesize Ni/SiO2 catalysts to obtain carbon-free hydrogen from catalyzing NH3 decomposition reaction. Among the three, the Ni/SiO2 catalyst synthesized via ammonia evaporation-hydrothermal method is the smallest in terms of Ni nanoparticles (similar to 3.0 nm) and the strongest Ni-SiO2 interaction. For ammonia decomposition, it is the highest in activity and thermal stability. The NH3 conversion at 650 degrees C and 30 000 mL g(cat)(-1)h(-1) (GHSV) over Ni/SiO2-AEH was close to 90 % and remained stable in an evaluation period of 60 h.
Keyword ：
Ammonia decomposition Ammonia decomposition Hydrogen production Hydrogen production Metal-support interaction Metal-support interaction Ni catalyst Ni catalyst
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| GB/T 7714 | Ren, Hongju , Cheng, Jinxing , Fang, Huihuang et al. Phyllosilicate-derived Ni catalysts with small nanoparticle size and strong metal-support interaction for efficient and robust decomposition of ammonia [J]. | APPLIED CATALYSIS A-GENERAL , 2023 , 664 . |
| MLA | Ren, Hongju et al. "Phyllosilicate-derived Ni catalysts with small nanoparticle size and strong metal-support interaction for efficient and robust decomposition of ammonia" . | APPLIED CATALYSIS A-GENERAL 664 (2023) . |
| APA | Ren, Hongju , Cheng, Jinxing , Fang, Huihuang , Zhong, Fulan , Chen, Chongqi , Lin, Li et al. Phyllosilicate-derived Ni catalysts with small nanoparticle size and strong metal-support interaction for efficient and robust decomposition of ammonia . | APPLIED CATALYSIS A-GENERAL , 2023 , 664 . |
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The oxygen hopping through oxygen defect site plays an extremely important role in cathode catalysts of solid oxide fuel cells (SOFC) application. Herein, a dual Ni2+/Ni3+ and Mn2+/Mn3+/Mn4+ redox pairs strategy is developed to construct a series of defective spinel Mg0.4NixMn2.6-xO4+delta (abbreviated MN(x)MO) to gain insights in terms of oxygen nonstoichiometry. By regulating the stoichiometric proportion of Ni and Mn, it is possible to optimize electronic conductivity and oxygen-vacancy concentration. The optimized MN(1.4)MO provides electrical conductivity as high as 68 Smiddotcm-1 at 800 degrees C, 2.72 folds that of MN(1.0)MO. Based on oxygen transport performance, the surface exchange coefficient of MN(1.4)MO at 900 degrees C is 162 folds that of commercial La0.7Sr0.3MnO3-delta (LSM). When a MN(1.4)MO cathode was used, the resulted SOFC exhibited extraordinarily high maximum power density of 0.34 Wmiddotcm-2 at 600 degrees C and 2.02 Wmiddotcm-2 at 800 degrees C. To the best of our knowledge, the performance is the best among the spinel-based cathodes ever reported for SOFC application. Endowed with optimal properties, MN(1.4)MO-based SOFC displays peak power density which is 2.27 and 1.44 folds that of LSM-based SOFC at 600 degrees C and 800 degrees C, respectively. A test of 50 h revealed the MN(1.4)MO-based SOFC is remarkably stable at 800 degrees C, continuously offering 2.02 Wmiddotcm-2 at 0.5 V. The excellent performance and stability of MN(1.4)MO-based SOFC suggests that MN(1.4)MO is a promising cathode material for the development of intermediate temperature SOFC technology.(c) 2022 Published by Elsevier B.V.
Keyword ：
Kinetics analysis Kinetics analysis Oxygen reduction reaction Oxygen reduction reaction Oxygen transport Oxygen transport SOFC SOFC Spinel oxides Spinel oxides
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| GB/T 7714 | Zhong, Fulan , Wang, Xinmin , Han, Cheng et al. Tailoring dual redox pairs strategy on a defective spinel Mg0.4NixMn2.6-xO4+delta cathode for the boosting of SOFCs performance [J]. | JOURNAL OF ALLOYS AND COMPOUNDS , 2023 , 939 . |
| MLA | Zhong, Fulan et al. "Tailoring dual redox pairs strategy on a defective spinel Mg0.4NixMn2.6-xO4+delta cathode for the boosting of SOFCs performance" . | JOURNAL OF ALLOYS AND COMPOUNDS 939 (2023) . |
| APA | Zhong, Fulan , Wang, Xinmin , Han, Cheng , Fang, Huihuang , Huang, Yunyun , Luo, Yu et al. Tailoring dual redox pairs strategy on a defective spinel Mg0.4NixMn2.6-xO4+delta cathode for the boosting of SOFCs performance . | JOURNAL OF ALLOYS AND COMPOUNDS , 2023 , 939 . |
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Ammonia(NH3)decomposition to release COx-free hydrogen(H2)over non-noble catalysts has gained increasing attention.In this study,three nanostructured CeO2 with different morphologies,viz.rod(R),sphere(Sph),and spindle(Spi),were fabricated and served as supports for Ni/CeO2 catalyst.The CeO2 supports are different in particle sizes,specific surface area and porosity,resulting in the formation of Ni nanoparticles with distinguished sizes and dispersions.The surface properties of the Ni/CeO2 catalysts are not only distinct but also influential,affecting the adsorption and desorption of NH3,N2,and/or H2 molecules.The Ni/CeO2-R catalyst shows superior catalytic activity compared to the other two,owing to its smaller Ni crystallite size and larger BET surface area.The most abundant strong basic sites are observed for Ni/CeO2-Spi catalyst based on its exposed CeO2(110)planes,which facilitates the donation of electrons to the Ni particles,benefiting the associative desorption of N atoms.Thus,Ni/CeO2-Spi shows higher catalytic activity than Ni/CeO2-Sph,despite their almost identical Ni crystallite sizes.
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| GB/T 7714 | Chongqi Chen , Xiaoshuang Fan , Chen Zhou et al. Hydrogen production from ammonia decomposition over Ni/CeO2 catalyst:Effect of CeO2 morphology [J]. | 稀土学报（英文版） , 2023 , 41 (7) : 1014-1021 . |
| MLA | Chongqi Chen et al. "Hydrogen production from ammonia decomposition over Ni/CeO2 catalyst:Effect of CeO2 morphology" . | 稀土学报（英文版） 41 . 7 (2023) : 1014-1021 . |
| APA | Chongqi Chen , Xiaoshuang Fan , Chen Zhou , Li Lin , Yu Luo , Chaktong Au et al. Hydrogen production from ammonia decomposition over Ni/CeO2 catalyst:Effect of CeO2 morphology . | 稀土学报（英文版） , 2023 , 41 (7) , 1014-1021 . |
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Green ammonia production system driven by renewable electricity will be under frequent dynamic operation due to the fluctuation of renewable energy. The nonlinear dynamic model of a green ammonia synthesis system is developed and the dynamic responses of PEM (proton exchange membrane) electrolysis subsystem, PSA (Pressure swing adsorption) subsystem and ammonia synthesis subsystem during the start-up process and under the fluctuation of renewable electrical current are analyzed. The start-up dynamic results show that the hydrogen production rate of PEM electrolysis system is positively correlated to the current. The nitrogen output of PSA system is affected by the adsorption time, adsorption pressure, bed length, and air velocity. A start-up period of 300 min from the warmed-up state to the design state can maintain the temperature rise rate of the ammonia synthesis reactor at approximately 40 K/h. The dynamic results under step fluctuations of electrical current show that the PEM electrolysis subsystem and the PSA subsystem response fast compared to the ammonia synthesis reactor and buffer tanks. Using large buffer tanks to smooth the fluctuation allows the system to slide with the variation of renewable current to some extent, resulting in a higher outlet ammonia fraction when the current increases. Different volume ratios of the hydrogen tank to the nitrogen tank volume can lead to different variations of the hydrogen/nitrogen ratio. PID controllers can effectively maintain the bed temperatures, hydrogen/ nitrogen ratio, and pressure of the ammonia synthesis reactor at their set points despite fluctuations in renewable electrical current. Buffer tanks are necessary to compensate for the imbalance between the flow rate fluctuation caused by current change and the flow rate regulation caused by PID controllers.
Keyword ：
Ammonia synthesis reactor Ammonia synthesis reactor Dynamic characteristics Dynamic characteristics Green ammonia synthesis Green ammonia synthesis PEM electrolysis PEM electrolysis PID control PID control Pressure swing adsorption Pressure swing adsorption
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| GB/T 7714 | Sun, Zhixin , Zhang, Yuanchao , Huang, Hongji et al. Modeling and simulation of dynamic characteristics of a green ammonia synthesis system [J]. | ENERGY CONVERSION AND MANAGEMENT , 2023 , 300 . |
| MLA | Sun, Zhixin et al. "Modeling and simulation of dynamic characteristics of a green ammonia synthesis system" . | ENERGY CONVERSION AND MANAGEMENT 300 (2023) . |
| APA | Sun, Zhixin , Zhang, Yuanchao , Huang, Hongji , Luo, Yu , Lin, Li , Jiang, Lilong . Modeling and simulation of dynamic characteristics of a green ammonia synthesis system . | ENERGY CONVERSION AND MANAGEMENT , 2023 , 300 . |
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Low-temperature direct ammonia fuel cell via ammonia oxidation reaction (AOR) is one of the most attractive ways for ammonia utilization. The Pt-Ir alloyed catalysts have been proven greatly efficient in AOR to overcome the sluggish kinetics and complex multi-electron processes; however, it still remains challenging for further improvement because of the complexity of alloyed types and unclear fundamental understanding. Herein, we systematically fabricated a series of PtxIry/XC-72 catalysts via tuning the Pt/Ir compositions and these catalysts demonstrate significant composition-dependent behaviours in AOR, whereas the Pt favours increasing current densities and the Ir facilitates reducing onset potentials. Importantly, the actual surface Pt/Ir atomic configuration is totally different with the classic view for homogeneous alloys by combining catalytic and characteristic analyses. The Pt prefers to be segregated on the topmost surface. Then the quantified correlations between current density/onset potential and Pt composition in Pt - Ir nanoparticles (NPs) were further established and discussed. The onset potential of AOR is significantly reduced by Ir incorporation while it is insensitive to Ir contents. Accordingly, the well-studied Pt5Ir5/XC-72 catalyst was further employed in an alkaline exchange membrane fuel cell, exhibiting a peak power density (230.0 mW cm-2). Our work provides insights into the effect of Pt/Ir compositions on AOR, with the goal of catalysts engineering for AOR and ammonia fuel cells.
Keyword ：
Ammonia oxidation reaction Ammonia oxidation reaction Bimetallic alloys Bimetallic alloys Direct ammonia fuel cells Direct ammonia fuel cells Iridium Iridium Platinum Platinum
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| GB/T 7714 | Fang, Huihuang , Liao, Chen , Cai, Quanying et al. Tuning surficial atomic configuration of Pt-Ir catalysts for efficient ammonia oxidation and low-temperature direct ammonia fuel cells [J]. | CHEMICAL ENGINEERING SCIENCE , 2023 , 280 . |
| MLA | Fang, Huihuang et al. "Tuning surficial atomic configuration of Pt-Ir catalysts for efficient ammonia oxidation and low-temperature direct ammonia fuel cells" . | CHEMICAL ENGINEERING SCIENCE 280 (2023) . |
| APA | Fang, Huihuang , Liao, Chen , Cai, Quanying , Zhong, Fulan , Lin, Li , Chen, Chongqi et al. Tuning surficial atomic configuration of Pt-Ir catalysts for efficient ammonia oxidation and low-temperature direct ammonia fuel cells . | CHEMICAL ENGINEERING SCIENCE , 2023 , 280 . |
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本发明提出一种逆流整体式催化燃烧与吸热反应耦合的反应系统，所使用的整体式催化燃烧‑吸热反应耦合反应器呈竖向的柱形体，其底端处设有可燃气体入口，顶部设有原料气入口，柱形体内整体式催化燃烧固定反应床与吸热反应床均呈环形柱状，两者的环层以交替套叠方式形成套层耦合结构；可燃气体经第二换热器预热至催化燃烧反应温度后，进入整体式催化燃烧固定反应床环层燃烧并加热吸热反应床环层，其燃烧尾气返回第二换热器作为热源冷却后排出；所述原料气经第一换热器预热后进入吸热反应床环层进行反应，其气态反应产物经吸热反应床的产物出口返回第一换热器作为热源冷却后输入收集装置储存；本发明能够将低浓度可燃气体治理与吸热反应相互结合。
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| GB/T 7714 | 蔡国辉 , 王智雄 , 林立 et al. 一种逆流整体式催化燃烧与吸热反应耦合的反应系统 : CN202210396416.4[P]. | 2022-04-15 00:00:00 . |
| MLA | 蔡国辉 et al. "一种逆流整体式催化燃烧与吸热反应耦合的反应系统" : CN202210396416.4. | 2022-04-15 00:00:00 . |
| APA | 蔡国辉 , 王智雄 , 林立 , 罗宇 , 陈崇启 , 肖益鸿 et al. 一种逆流整体式催化燃烧与吸热反应耦合的反应系统 : CN202210396416.4. | 2022-04-15 00:00:00 . |
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本发明公开了一种具有氨气预加热功能的氨分解反应器，包括换热器本体和反应器本体，换热器本体包覆在反应器本体外侧；换热器本体上的换热管设置在换热壳体内，其一端与氨气换热进口连通，另一端与氨气换热出口连通，换热器本体上的热媒进口和热媒出口分别与换热壳体导通；反应器本体上的催化剂管设置在反应壳体内，换热器本体上的氨气换热出口与反应器本体上的氨气进口连通，氨气进口和氨气分解气出口之间通过催化剂管连通，氨气分解气出口与换热器本体上的热媒进口连通。本发明结构紧凑，采用反应器中氨气分解气的高温气体作为换热器的热介质，给氨气提供热量进行预热，使得进入反应器的氨气处于高温状态，在反应器内进行的氨分解反应更充分。
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| GB/T 7714 | 江莉龙 , 王大彪 , 罗宇 et al. 一种具有氨气预加热功能的氨分解反应器 : CN202210707426.5[P]. | 2022-06-21 00:00:00 . |
| MLA | 江莉龙 et al. "一种具有氨气预加热功能的氨分解反应器" : CN202210707426.5. | 2022-06-21 00:00:00 . |
| APA | 江莉龙 , 王大彪 , 罗宇 , 张卿 , 陈崇启 , 林立 . 一种具有氨气预加热功能的氨分解反应器 : CN202210707426.5. | 2022-06-21 00:00:00 . |
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