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学者姓名：方辉煌
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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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A challenge hindering the development of durable solid oxide fuel cells (SOFCs) is the significant performance degradation of cathodes owing to poisoning by volatile Cr originating from the FeCr alloy interconnect. Herein, a heterogeneous catalyst coating, composed of Ba1-xCe0.8Gd0.2O3-delta and BaCO3, remarkably improves the oxygen adsorption, dissociation capability, and Cr resistance of a La0.6Sr0.4Co0.2Fe0.8O3-delta (LSCF) cathode is demonstrated. The coherent heterointerface interactions formed between the catalyst coating and LSCF result in varied levels of surface strain and electrostatic interactions, significantly suppressing Sr surface segregation on LSCF. A single cell with the catalyst coating-decorated LSCF (CC-LSCF) achieves a peak power density of 1.73 W cm-2 at 750 degrees C, with no noticeable performance degradation for 100 h. The CC-LSCF cathode also exhibits outstanding durability under accelerated Cr poisoning conditions, compared with the tremendous degradation rate of 0.42% h-1 for the bare LSCF cathode. The enhanced Cr resistance is attributed to synergy induced by the stabilization of the lattice Sr cations by heterointerface interactions and the remarkable structural stability of the catalyst coating under Cr poisoning conditions. The novel heterointerface engineering strategy in this study provides insight into the design and development of active and Cr-tolerant cathodes. A heterogeneous catalyst coating composed of Ba1-xCe0.8Gd0.2O3-delta and BaCO3 remarkably improves the oxygen adsorption, dissociation capability, and Cr tolerance of La0.6Sr0.4Co0.2Fe0.8O3-delta cathode. The enhanced Cr tolerance is attributed to synergy induced by the stabilization of the lattice Sr cations by heterointerface interactions and the remarkable structural stability of the catalyst coating under Cr poisoning conditions. image
Keyword ：
chromium tolerance chromium tolerance heterointerfaces heterointerfaces solid oxide fuel cells solid oxide fuel cells Sr surface segregation Sr surface segregation strain strain
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| GB/T 7714 | Huang, Jiongyuan , Liang, Fujun , Zhao, Sunce et al. Heterogeneous Catalyst Coating for Boosting the Activity and Chromium Tolerance of Cathodes for Solid Oxide Fuel Cells [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (26) . |
| MLA | Huang, Jiongyuan et al. "Heterogeneous Catalyst Coating for Boosting the Activity and Chromium Tolerance of Cathodes for Solid Oxide Fuel Cells" . | ADVANCED FUNCTIONAL MATERIALS 34 . 26 (2024) . |
| APA | Huang, Jiongyuan , Liang, Fujun , Zhao, Sunce , Zhao, Ling , Ai, Na , Jiang, San Ping et al. Heterogeneous Catalyst Coating for Boosting the Activity and Chromium Tolerance of Cathodes for Solid Oxide Fuel Cells . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (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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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 . |
| MLA | Yang, Shiqing et al. "Pyrochlore La2Zr2-xNixO7 anodes for direct ammonia solid oxide fuel cells" . | FRONTIERS IN ENERGY (2024) . |
| 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 . |
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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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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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Degradation of cathodes caused by the gaseous Cr species from a Fe-Cr alloy interconnect is a key issue in the development of durable solid oxide fuel cells technologies. Herein, we explore the effect of infiltration of BaCO3 nanoparticles on the electrocatalytic performance and Cr-tolerance of La0.6Sr0.4Co0.2Fe0.8O3-delta (LSCF) cathodes. The BaCO3 increases the performance of LSCF and the single-cell delivers a peak power density of 1.30 W cm-2 at 800 degrees C. The BaCO3 gives rise to no Cr deposition and Sr segregation on LSCF after exposure in gaseous CrO3, while a BaCrO4 surface layer is deposited on the cathode in contact with a Fe-Cr alloy. The synergetic effects of BaCrO4 layer on mitigating the reaction between segregated Sr and Cr2O3 and the very slow kinetics of reaction between BaCO3 and CrO3 contribute to the exceptional Cr-tolerance of the BaCO3 infiltrated LSCF cathodes.
Keyword ：
BaCO3 infiltration BaCO3 infiltration Barium chromate Barium chromate Chromium-tolerance Chromium-tolerance Solid oxide fuel cells Solid oxide fuel cells
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| GB/T 7714 | Huang, Jiongyuan , Liu, Quan , Jiang, San Ping et al. Promotional role of BaCO3 on the chromium-tolerance of La0.6Sr0.4Co0.2Fe0.8O3-delta cathodes of solid oxide fuel cells [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 321 . |
| MLA | Huang, Jiongyuan et al. "Promotional role of BaCO3 on the chromium-tolerance of La0.6Sr0.4Co0.2Fe0.8O3-delta cathodes of solid oxide fuel cells" . | APPLIED CATALYSIS B-ENVIRONMENTAL 321 (2023) . |
| APA | Huang, Jiongyuan , Liu, Quan , Jiang, San Ping , Zhao, Ling , Ai, Na , Wang, Xin et al. Promotional role of BaCO3 on the chromium-tolerance of La0.6Sr0.4Co0.2Fe0.8O3-delta cathodes of solid oxide fuel cells . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 321 . |
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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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Nanostructured air electrodes play a crucial role in improving the electrocatalytic activity of oxygen reduction and evolution reactions in solid oxide cells (SOCs). Herein, we report the fabrication of a nanostructured BaCoO3- decorated cation-deficient PrBa0.8Ca0.2Co2O5+delta (PBCC) air electrode via a combined modification and direct assembly approach. The modification approach endows the dual-phase air electrode with a large surface area and abundant oxygen vacancies. An intimate air electrode-electrolyte interface is in situ constructed with the formation of a catalytically active Co3O4 bridging layer via electrochemical polarization. The corresponding single cell exhibits a peak power density of 2.08 W cm-2, an electrolysis current density of 1.36 A cm-2 at 1.3 V, and a good operating stability at 750 degrees C for 100 h. This study provides insights into the rational design and facile utilization of an active and stable nanostructured air electrode of SOCs.
Keyword ：
cation defects cation defects dual-phase catalyst dual-phase catalyst electrolyte-electrode interface electrolyte-electrode interface nanostructured air electrode nanostructured air electrode solid oxide cells solid oxide cells
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| GB/T 7714 | Yue, Zhongwei , Jiang, Lizhen , Chen, Zhiyi et al. Ultrafine, Dual-Phase, Cation-Deficient PrBa0.8Ca0.2Co2O5+? Air Electrode for Efficient Solid Oxide Cells [J]. | ACS APPLIED MATERIALS & INTERFACES , 2023 , 15 (6) : 8138-8148 . |
| MLA | Yue, Zhongwei et al. "Ultrafine, Dual-Phase, Cation-Deficient PrBa0.8Ca0.2Co2O5+? Air Electrode for Efficient Solid Oxide Cells" . | ACS APPLIED MATERIALS & INTERFACES 15 . 6 (2023) : 8138-8148 . |
| APA | Yue, Zhongwei , Jiang, Lizhen , Chen, Zhiyi , Ai, Na , Zou, Yuanfeng , Jiang, San Ping et al. Ultrafine, Dual-Phase, Cation-Deficient PrBa0.8Ca0.2Co2O5+? Air Electrode for Efficient Solid Oxide Cells . | ACS APPLIED MATERIALS & INTERFACES , 2023 , 15 (6) , 8138-8148 . |
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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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