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学者姓名：钟富兰
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Abstract ：
The protonic ceramic fuel cells (PCFCs) can convert the chemical energy of fuel directly into electric power, with the advantages of high efficiency and alternative fuel range at intermediate temperatures. Ammonia has been regarded as a promising fuel for PCFCs due to its carbon-free and hydrogen-rich properties, high volumetric energy density and easy storage/transportation. However, the performance of ammonia PCFCs (NH3-PCFCs) is far inferior to the hydrogen PCFCs (H2-PCFCs) because of the sluggish and complex kinetics at anodes. In this study, we established an elementary reaction kinetic model for NH3-PCFCs, investigated the effect of reaction parameters, anode components and reaction partition, and explored the coupling mechanism between the ammonia decomposition and electrochemical reaction. Importantly, the ammonia decomposition and electrochemical reaction can be flexibly regulated by adjusting anode parameters, then affecting the performance ratio of NH3-PCFCs and H2-PCFCs. The detailed rate-determining steps were further identified by experimental and model analysis. Thus, the ammonia/hydrogen performance ratio of the cell can exceed 95% at 550°C after accelerating the ammonia decomposition reaction. Our work provides insights into the kinetics in NH3-PCFCs for improving their performance with optimization. © 2024 American Institute of Chemical Engineers.
Keyword ：
ammonia decomposition ammonia decomposition ammonia protonic ceramic fuel cells ammonia protonic ceramic fuel cells coupling mechanism coupling mechanism electrochemical oxidation electrochemical oxidation elementary reaction kinetic model elementary reaction kinetic model
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| GB/T 7714 | You, J. , Chen, J. , Liu, S. et al. Insight into the complex ammonia decomposition/oxidation kinetics in ammonia protonic ceramic fuel cells via elementary modeling [J]. | AIChE Journal , 2024 , 70 (9) . |
| MLA | You, J. et al. "Insight into the complex ammonia decomposition/oxidation kinetics in ammonia protonic ceramic fuel cells via elementary modeling" . | AIChE Journal 70 . 9 (2024) . |
| APA | You, J. , Chen, J. , Liu, S. , Fang, H. , Zhong, F. , Luo, Y. et al. Insight into the complex ammonia decomposition/oxidation kinetics in ammonia protonic ceramic fuel cells via elementary modeling . | AIChE Journal , 2024 , 70 (9) . |
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Abstract ：
Ammonia is an exceptional fuel for solid oxide fuel cells (SOFCs), because of the high content of hydrogen and the advantages of carbon neutrality. However, the challenge lies in its unsatisfactory performance at intermediate temperatures (500-600 degrees C), impeding its advancement. An electrolyte-supported proton-ceramic fuel cell (PCFC) was fabricated employing BaZr0.1Ce0.7Y0.2O3-delta (BZCY) as the electrolyte and Ba0.5Sr0.5Co0.8Fe0.2O3-delta (BSCF) as the cathode. In this study, the performance of PCFC using NH3 as fuel within an operating temperature range of 500-700 degrees C was improved by adding an M(Ni,Ru)/CeO(2 )catalyst layer to reconstruct the anode surface. The electrochemical performance of direct ammonia PCFC (DA-PCFC) were improved to different extents. Compared to H-2 as fuel, the degradation ratio of peak power densities (PPDs) of Ni/CeO2-loaded PCFC fueled with NH3 decreased at 700-500 degrees C, with a decrease to 13.3% at 700 degrees C and 30.7% at 500 degrees C. The findings indicate that Ru-based catalysts have a greater promise for direct ammonia SOFCs (DA-SOFCs) at operating temperatures below 600 degrees C. However, the enhancement effect becomes less significant above 600 degrees C when compared to Ni-based catalysts.
Keyword ：
ammonia ammonia anode anode M/CeO2 catalyst layer M/CeO2 catalyst layer proton-ceramic fuel cell (PCFC) proton-ceramic fuel cell (PCFC)
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| GB/T 7714 | Li, Xiaoxiao , Chen, Jiangping , Huang, Yunyun et al. Performance-enhanced direct ammonia protonic ceramic fuel cells using CeO2-supported Ni and Ru catalyst layer [J]. | FRONTIERS IN ENERGY , 2024 , 18 (6) : 875-884 . |
| MLA | Li, Xiaoxiao et al. "Performance-enhanced direct ammonia protonic ceramic fuel cells using CeO2-supported Ni and Ru catalyst layer" . | FRONTIERS IN ENERGY 18 . 6 (2024) : 875-884 . |
| APA | Li, Xiaoxiao , Chen, Jiangping , Huang, Yunyun , Fang, Huihuang , Chen, Chongqi , Zhong, Fulan et al. Performance-enhanced direct ammonia protonic ceramic fuel cells using CeO2-supported Ni and Ru catalyst layer . | FRONTIERS IN ENERGY , 2024 , 18 (6) , 875-884 . |
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Developing efficient anode catalysts for direct ammonia solid oxide fuel cells (NH3-SOFCs) under intermediate-temperatures is of great importance, in support of hydrogen economy via ammonia utilization. In the present work, the pyrochlore-type La2Zr2-xNixO7+delta (LZN(x), x = 0, 0.02, 0.05, 0.08, 0.10) oxides were synthesized as potential anode catalysts of NH3-SOFCs due to the abundant Frankel defect that contributes to the good conductivity and oxygen ion mobility capacity. The effects of different content of Ni2+ doping on the crystal structure, surface morphology, thermal matching with YSZ (Yttria-stabilized zirconia), conductivity, and electrochemical performance of pyrochlore oxides were examined using different characterization techniques. The findings indicate that the LZN(x) oxide behaves as an n-type semiconductor and exhibits an excellent high-temperature chemical compatibility and thermal matching with the YSZ electrolyte. Furthermore, LZN(0.05) exhibits the smallest conductive band potential and bandgap, making it have a higher power density as anode material for NH3-SOFCs compared to other anodes. As a result, the maximum power density of the LZN(0.05)-40YSZ composite anode reaches 100.86 mW/cm(2) at 800 degrees C, which is 1.8 times greater than that of NiO-based NH3-SOFCs (56.75 mW/cm(2)) under identical flow rate and temperature conditions. The extended durability indicates that the NH3-SOFCs utilizing the LZN(0.05)-40YSZ composite anode exhibits a negligible voltage degradation following uninterrupted operation at 800 degrees C for 100 h.
Keyword ：
ammonia oxidation ammonia oxidation anode catalyst anode catalyst NH3-SOFCs NH3-SOFCs Ni particles Ni particles
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| GB/T 7714 | Yang, Shiqing , Gao, Yijie , Wang, Xinmin et al. Pyrochlore La2Zr2-xNixO7 anodes for direct ammonia solid oxide fuel cells [J]. | FRONTIERS IN ENERGY , 2024 , 18 (5) : 699-711 . |
| MLA | Yang, Shiqing et al. "Pyrochlore La2Zr2-xNixO7 anodes for direct ammonia solid oxide fuel cells" . | FRONTIERS IN ENERGY 18 . 5 (2024) : 699-711 . |
| APA | Yang, Shiqing , Gao, Yijie , Wang, Xinmin , Zhong, Fulan , Fang, Huihuang , Luo, Yu et al. Pyrochlore La2Zr2-xNixO7 anodes for direct ammonia solid oxide fuel cells . | FRONTIERS IN ENERGY , 2024 , 18 (5) , 699-711 . |
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Abstract ：
The protonic ceramic fuel cells (PCFCs) can convert the chemical energy of fuel directly into electric power, with the advantages of high efficiency and alternative fuel range at intermediate temperatures. Ammonia has been regarded as a promising fuel for PCFCs due to its carbon-free and hydrogen-rich properties, high volumetric energy density and easy storage/transportation. However, the performance of ammonia PCFCs (NH3-PCFCs) is far inferior to the hydrogen PCFCs (H2-PCFCs) because of the sluggish and complex kinetics at anodes. In this study, we established an elementary reaction kinetic model for NH3-PCFCs, investigated the effect of reaction parameters, anode components and reaction partition, and explored the coupling mechanism between the ammonia decomposition and electrochemical reaction. Importantly, the ammonia decomposition and electrochemical reaction can be flexibly regulated by adjusting anode parameters, then affecting the performance ratio of NH3-PCFCs and H2-PCFCs. The detailed rate-determining steps were further identified by experimental and model analysis. Thus, the ammonia/hydrogen performance ratio of the cell can exceed 95% at 550 degrees C after accelerating the ammonia decomposition reaction. Our work provides insights into the kinetics in NH3-PCFCs for improving their performance with optimization.
Keyword ：
ammonia decomposition ammonia decomposition ammonia protonic ceramic fuel cells ammonia protonic ceramic fuel cells coupling mechanism coupling mechanism electrochemical oxidation electrochemical oxidation elementary reaction kinetic model elementary reaction kinetic model
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| GB/T 7714 | You, Jiacheng , Chen, Jiangping , Liu, Shunli et al. Insight into the complex ammonia decomposition/oxidation kinetics in ammonia protonic ceramic fuel cells via elementary modeling [J]. | AICHE JOURNAL , 2024 , 70 (9) . |
| MLA | You, Jiacheng et al. "Insight into the complex ammonia decomposition/oxidation kinetics in ammonia protonic ceramic fuel cells via elementary modeling" . | AICHE JOURNAL 70 . 9 (2024) . |
| APA | You, Jiacheng , Chen, Jiangping , Liu, Shunli , Fang, Huihuang , Zhong, Fulan , Luo, Yu et al. Insight into the complex ammonia decomposition/oxidation kinetics in ammonia protonic ceramic fuel cells via elementary modeling . | AICHE JOURNAL , 2024 , 70 (9) . |
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Kinetically sluggish ammonia oxidation and interference of H-2 competing with NH3 active sites will suppress the output performance of direct ammonia solid oxide fuel cell (DA-SOFC). Herein, we select Zn2+ doped into Pr2NiO4 as precursor of Pr2Ni1-xZnxO4 (PNZx) that can be destroyed and converted into Pr2O3 together with in-situ Ni reduction, realizing the redistribution of elements in reduction atmosphere. Meanwhile, the foreign Zn2+ as a low-valent element is retained in Pr2O3 lattice due to the high segregation Gibbs free energy to form Ni/Pr2-xZnxO3, which aggravates the change of Pr3+ and Pr4+, thus enhancing the oxygen vacancy concentration. The Zn2+ promotes the reduction of Ni and quenches the adsorption capacity of H-2, alleviating the "hydrogen poisoning" behavior. As a result, the maximum powder density of single cell based on PNZ0.1 supported by YSZ electrolyte is 134 mWcm(-2) at 800 degree celsius, which is more than twice higher than that of Ni/YSZ. Various characterizations reveal that the NH3 reaction path is the synergistic occurrence of ammonia decomposition and ammonia oxidation.
Keyword ：
Anode reaction mechanism Anode reaction mechanism DA-SOFC DA-SOFC Hydrogen poisoning Hydrogen poisoning In-situ Ni reduction In-situ Ni reduction
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| GB/T 7714 | Zhong, Fulan , Zhao, Xiaofeng , Fang, Huihuang et al. Unveiling optimal activity and mechanism of in situ Ni reduction Pr2Ni1-xZnxO4 anode for ammonia solid oxide fuel cells [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 360 . |
| MLA | Zhong, Fulan et al. "Unveiling optimal activity and mechanism of in situ Ni reduction Pr2Ni1-xZnxO4 anode for ammonia solid oxide fuel cells" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 360 (2024) . |
| APA | Zhong, Fulan , Zhao, Xiaofeng , Fang, Huihuang , Luo, Yu , Wang, Shaorong , Chen, Chongqi et al. Unveiling optimal activity and mechanism of in situ Ni reduction Pr2Ni1-xZnxO4 anode for ammonia solid oxide fuel cells . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 360 . |
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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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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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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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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 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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