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学者姓名：陈崇启
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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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【目的】在“双碳”背景下，氨作为无碳富氢的能源载体，体积能量密度高、易液化存储，具有广阔的发展前景。然而复杂的储运环境增加了液氨储罐和管道腐蚀的风险，因此，研究复杂输送环境下液氨腐蚀问题是“氨-氢”能源基础设施制造和安全服役的关键。【方法】通过综述液氨腐蚀的研究进展，探讨了不同环境、不同材料的氨腐蚀行为和应力腐蚀开裂机制。同时，总结了相关氨腐蚀检测方法和具体防护措施，并展望了未来氨腐蚀研究的发展方向。【结果】氧气、碳氧化合物、硫化物及氯化物的混入对氨腐蚀有促进作用，而水杂质对氨腐蚀的影响具有两面性；应力能够引起液氨应力腐蚀开裂，不同材料的应力腐蚀敏感性从大到小依次为铜及其合金、高强钢、碳钢。【结论】基于国内对液氨腐蚀行为机理尚不明确、氨腐蚀防护措施有待完善等问题，提出以下建议：(1)采用实验研究、仿真模拟等方法，探究多杂质关联作用下不同材质的液氨腐蚀行为和内在腐蚀机理；(2)需结合液氨管道实际输送环境及材料失效特征，开展管线钢及焊材-液氨临界失效边界检验与腐蚀风险评价；(3)从液氨储罐及管道的设计、选材、制造、使用等多个角度，结合多种腐蚀防腐措施，形成完善的液氨储运系统腐蚀控制、防护及评价标准体系。（图5，表2，参77）
Keyword ：
应力腐蚀 应力腐蚀 液氨储运 液氨储运 环境腐蚀 环境腐蚀 腐蚀检测 腐蚀检测 防护技术 防护技术
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| GB/T 7714 | 李加庆 , 冯智雨 , 梁辉龙 et al. 复杂输送环境下液氨腐蚀行为及防护技术研究进展 [J]. | 油气储运 , 2024 , 43 (02) : 121-133,162 . |
| MLA | 李加庆 et al. "复杂输送环境下液氨腐蚀行为及防护技术研究进展" . | 油气储运 43 . 02 (2024) : 121-133,162 . |
| APA | 李加庆 , 冯智雨 , 梁辉龙 , 尹鹏博 , 滕霖 , 陈崇启 et al. 复杂输送环境下液氨腐蚀行为及防护技术研究进展 . | 油气储运 , 2024 , 43 (02) , 121-133,162 . |
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Molybdate-intercalated magnesium–aluminum hydrotalcite-like compounds (HTlc) were synthesized by anion-exchange and used as precursor to prepare supported molybdenum nitride catalyst for ammonia decomposition. The as-synthesized precursors and the derived mixed metal oxides and nitride catalysts were characterized by ICP, XRD, Raman spectroscopy, XPS, H2-TPR, and HAADF-STEM-EDX. The characterizations indicated that molybdate was well intercalated into the HTlc interlayer as MoO42– and the Mo content was tunable by altering the intercalation degree of molybdate. Upon calcination, molybdena was dominantly presented as isolated tetrahedrally coordinated MoOx species. Upon nitridation with ammonia at 700 ºC, highly dispersed and composition-uniform molybdenum nitride (Mo2±xN) was formed. The Mo0.5Mg3Al nitride catalyst showed good activity for ammonia decomposition, providing nearly full conversion of ammonia at 625 ºC under a space velocity of 5,000 mL gcat–1 h–1. The optimal catalyst also exhibited high catalytic stability during 100 h operation at 625 ºC, and no obvious aggregation took place, attributable to the strong metal–support interaction between molybdenum nitride and Mg–Al mixed oxide. It is suggested that the hydrotalcite-derived Mg–Al mixed oxide supported highly dispersed Mo2±xN species was active and stable for ammonia decomposition. © 2024 Elsevier B.V.
Keyword ：
Alumina Alumina Aluminum nitride Aluminum nitride Aluminum oxide Aluminum oxide Ammonia Ammonia Catalyst activity Catalyst activity Hydrogen production Hydrogen production Magnesium compounds Magnesium compounds Molybdenum oxide Molybdenum oxide Nitrides Nitrides
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| GB/T 7714 | Wei, Xiaofeng , Su, Jiaxin , Xie, Guanbao et al. Supported highly dispersed molybdenum nitride derived from molybdate-intercalated Mg‒Al hydrotalcite-like compounds as a catalyst for ammonia decomposition [J]. | Molecular Catalysis , 2024 , 562 . |
| MLA | Wei, Xiaofeng et al. "Supported highly dispersed molybdenum nitride derived from molybdate-intercalated Mg‒Al hydrotalcite-like compounds as a catalyst for ammonia decomposition" . | Molecular Catalysis 562 (2024) . |
| APA | Wei, Xiaofeng , Su, Jiaxin , Xie, Guanbao , Lian, Minli , Huang, Hongyang , Chen, Chongqi et al. Supported highly dispersed molybdenum nitride derived from molybdate-intercalated Mg‒Al hydrotalcite-like compounds as a catalyst for ammonia decomposition . | Molecular Catalysis , 2024 , 562 . |
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An effective B-site doping strategy through heterovalent ions was developed to synthesize a series of pyrochlore Pr2Zr1.95X0.05O7+delta (PZX, X = Mn, Sc, Sn, Nb, Mo, Al, Ga, In) for the direct ammonia solid oxide fuel cell (DA-SOFC) cathode. To guide the design of efficient cathodes for DA-SOFC, we explore the relationships between the ionic radius/valence of dopant and electrochemical performance. In view of the energy matching and interaction between the dopant and the host lattice, the substitution of trivalent Sc3+ with similar ionic radius for tetravalent Zr4+ can greatly improve the oxygen reduction reaction activity of Pr2Zr2O7 due to the reduced bond energy of 48f-oxygen ions in octahedral [ZrO6] units. As a result, the anode-supported single cell Ni-YSZ|YSZ|PZSc-60YSZ yields an output power density of 0.44 and 1.45 Wcm(-2) at 600 and 800 degrees C with ammonia fuel, outperforming PZX (X = Mn, Sn, Nb, Mo, Al, Ga, In) and common La0.8Sr0.2MnO3 (LSM)-based DA-SOFC. The detailed characterizations are employed to gain insight into the structure-activity relationship and reaction mechanism.
Keyword ：
Direct ammonia solid oxide fuel cell Direct ammonia solid oxide fuel cell Distribution of relaxation time Distribution of relaxation time Pyrochlore Pyrochlore Structural distortion Structural distortion
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| GB/T 7714 | Fang, Huihuang , Yang, Shiqing , Ye, Weijie et al. Mechanism insight into enhanced oxygen reduction reaction over heterovalent ion incorporated pyrochlore Pr2Zr2O7 for direct ammonia solid oxide fuel cells [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 290 . |
| MLA | Fang, Huihuang et al. "Mechanism insight into enhanced oxygen reduction reaction over heterovalent ion incorporated pyrochlore Pr2Zr2O7 for direct ammonia solid oxide fuel cells" . | CHEMICAL ENGINEERING SCIENCE 290 (2024) . |
| APA | Fang, Huihuang , Yang, Shiqing , Ye, Weijie , Zhong, Fulan , Luo, Yu , Wang, Shaorong et al. Mechanism insight into enhanced oxygen reduction reaction over heterovalent ion incorporated pyrochlore Pr2Zr2O7 for direct ammonia solid oxide fuel cells . | CHEMICAL ENGINEERING SCIENCE , 2024 , 290 . |
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Ammonia decomposition for onsite hydrogen production has been regarded as an important reaction which links to efficient hydrogen storage, transport and utilization. However, it still remains challenging to develop efficient catalysts with robust stability for ammonia decomposition. Herein, an integrated strategy was employed to synthesize Ru/SiO2@N-CS via wrapping a thin layer of N-doped carbon onto the SiO2 sphere, following the anchor of Ru nanoparticles (NPs) onto the support. The obtained Ru/SiO2@N-CS (Ru loading: 1 wt%) shows a promising performance for ammonia decomposition, reaching 94.5 % at 550 °C with a gas hourly space velocity (GHSV) of 30 000 mL gcat-1h−1. The combination of the SiO2 as the core prevents the degradation of N-doped carbon layers and then enhance the durability of the catalysts, remaining stable after 50 h at evaluated temperatures. Adequate characterizations were used to illustrate the effect of microchemical environment on ammonia decomposition activity of Ru/SiO2@N-CS catalyst under different calcination atmosphere and the correlation between structure and performance. © 2024 Elsevier B.V.
Keyword ：
Ammonia decomposition Ammonia decomposition N-doped carbon N-doped carbon Ruthenium Ruthenium SiO2 SiO2 Stability Stability
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| GB/T 7714 | Huang, Y. , Ren, H. , Fang, H. et al. Ru nanoparticles embedded in Ru/SiO2@N-CS for boosting hydrogen production via ammonia decomposition with robust lifespan [J]. | Applied Surface Science , 2024 , 669 . |
| MLA | Huang, Y. et al. "Ru nanoparticles embedded in Ru/SiO2@N-CS for boosting hydrogen production via ammonia decomposition with robust lifespan" . | Applied Surface Science 669 (2024) . |
| APA | Huang, Y. , Ren, H. , Fang, H. , Ouyang, D. , Chen, C. , Luo, Y. et al. Ru nanoparticles embedded in Ru/SiO2@N-CS for boosting hydrogen production via ammonia decomposition with robust lifespan . | Applied Surface Science , 2024 , 669 . |
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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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