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学者姓名：方辉煌
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Abstract ：
Water gas shift reaction is an important process in hydrogen production from carbon-based materials. Cu-based catalysts are widely used in low-temperature water gas shift reactions. The problem is that Cu species are prone to sintering and deactivation, as well as the controversial reaction mechanism. Herein, CuFe2O4 modified with Al3+ is served as the Cu-based catalyst precursor, and the catalytic structure-activity relationship as well as reaction mechanism are carefully investigated. The modification of CuFe2O4 precursor by Al3+ enhances the Cu species dispersion, redox properties and electron transfer ability, leading to increasing the proportion of Cu+/ (Cu0+Cu+), which results in enhancing the ability of the catalyst to adsorb CO and dissociate H2O. The combination of temperature-programmed surface reaction (TPSR) and infrared spectroscopy shows that the catalyst with weak water dissociation ability and medium CO adsorption capacity are prone to obey the association mechanism.
Keyword ：
Association mechanism Association mechanism Copper ferrite Copper ferrite Cu plus site Cu plus site Metal-support interaction Metal-support interaction Spinel Spinel
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| GB/T 7714 | Zhi, Guo , Huang, Chunjin , Ren, Hongju et al. Ternary Cu-Fe-Al spinel catalyst for hydrogen production via water gas shift reaction: Electron transfer enhancement and reaction mechanism [J]. | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2025 , 102 : 1093-1102 . |
| MLA | Zhi, Guo et al. "Ternary Cu-Fe-Al spinel catalyst for hydrogen production via water gas shift reaction: Electron transfer enhancement and reaction mechanism" . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 102 (2025) : 1093-1102 . |
| APA | Zhi, Guo , Huang, Chunjin , Ren, Hongju , Fang, Huihuang , Chen, Chongqi , Luo, Yu et al. Ternary Cu-Fe-Al spinel catalyst for hydrogen production via water gas shift reaction: Electron transfer enhancement and reaction mechanism . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2025 , 102 , 1093-1102 . |
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Metals atomically anchored on oxides have actively realized ultimate atom efficiency. However, a "molecular cork" effect causes the intrinsically reactive sites to remain dormant in various important catalytic processes. Here, we report a strategy to waken dormant atomic Au on cobalt-doped CeO2 islands (Au/CoCeO2) that are typically recognized as barely active in acetylene hydrochlorination by precisely controlling reversible C2H2 spillover facilitated by porous carbon materials, igniting its reactivity of Au-oxo sites and enhanced stability. In this vein, the C2H2 coverage on the nitrogen-doped carbon (NC) surface reversibly spills over onto HCl-corked metal sites, uncorking the strongly bound HCl. The Au/CoCeO2 + NC system displays a 2 orders of magnitude higher activity than modular Au/CoCeO2 and obtains an enhanced catalytic activity and durability than the state-of-the-art catalyst, Au/NC. This contribution unveils a distinct Eley-Rideal-like mechanism that exists on the Au/CoCeO2 + NC system, exchanging the conventional Langmuir-Hinshelwood pathway dominated over Au/NC. Collectively, our findings reinforce the importance of taming the reaction pathways for advancing catalyst design.
Keyword ：
dormant sites dormant sites hydrochlorination catalysts hydrochlorination catalysts molecular cork molecular cork reversible spillover species reversible spillover species structure-performancerelationship structure-performancerelationship
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| GB/T 7714 | Duan, Xinping , Zhao, Yuxin , Chou, Hung-Lung et al. Reversible Spillover Wakens Reactivity of Dormant Modular Hydrochlorination Catalysts [J]. | ACS CATALYSIS , 2025 , 15 (5) : 3913-3927 . |
| MLA | Duan, Xinping et al. "Reversible Spillover Wakens Reactivity of Dormant Modular Hydrochlorination Catalysts" . | ACS CATALYSIS 15 . 5 (2025) : 3913-3927 . |
| APA | Duan, Xinping , Zhao, Yuxin , Chou, Hung-Lung , Zuo, Jiachang , Wang, Ruixin , Jiao, Weizhou et al. Reversible Spillover Wakens Reactivity of Dormant Modular Hydrochlorination Catalysts . | ACS CATALYSIS , 2025 , 15 (5) , 3913-3927 . |
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Ammonia is a carbon-free energy carrier with 17.6 wt% hydrogen content. The design of an efficient and compact ammonia decomposition reactor based on low-temperature catalysts is the key to realizing industrial hydrogen production from ammonia. In this work, a multiscale model was developed by bridging the particle-scale characteristics of catalysts and reactor performances, to fully comprehend the ammonia decomposition process. The effects of catalyst porosity and pore diameters on the reactor size, precious metal loading, and the profile of temperature and heat flux were systematically evaluated. An improved reactor design was further proposed by applying the segmented reactor packed with two-stage egg-shell-type low-temperature catalysts, which decreased the precious metal usage by 61.6% and the temperature drop by 42.9 K. This segmentation strategy balanced the reaction rate and heat flux, indicating a significant potential in highly efficient, economical, and reliable hydrogen production from ammonia.
Keyword ：
ammonia decomposition ammonia decomposition catalyst micro-structure catalyst micro-structure hydrogen production hydrogen production multiscale model multiscale model precious metal reduction precious metal reduction
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| GB/T 7714 | Zhang, Lixuan , Wu, Yifan , Huang, Wenshi et al. Multiscale modeling of a low-temperature NH3 decomposition reactor for precious metal reduction and temperature control [J]. | AICHE JOURNAL , 2025 . |
| MLA | Zhang, Lixuan et al. "Multiscale modeling of a low-temperature NH3 decomposition reactor for precious metal reduction and temperature control" . | AICHE JOURNAL (2025) . |
| APA | Zhang, Lixuan , Wu, Yifan , Huang, Wenshi , Lin, Li , Wang, Luqiang , Wu, Zeyun et al. Multiscale modeling of a low-temperature NH3 decomposition reactor for precious metal reduction and temperature control . | AICHE JOURNAL , 2025 . |
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Ammonia is a carbon-free hydrogen carrier, and development of non-noble metal catalyst to decompose ammonia into hydrogen is desirable for practical applications. However, the metal catalyst is challenged by the sintering of metal particles under high-temperature reaction conditions. In this study, a series of Li-, Al-, and Co-containing hydrotalcite-like compounds (HTlc) were synthesized by co-precipitation and used as precursors to prepare well-dispersed and thermally stable Co nanoparticle catalysts for ammonia decomposition. The obtained precursors and catalysts were characterized by means of X-ray powder diffraction (XRD), temperature-programmed reduction (H-2-TPR), X-ray photoelectron spectroscopy (XPS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and so on. All of the precursors formed hydrotalcite-like phase, which consisted of Li-Al-(Co) HTlc and/or Co-Al HTlc dependent on the Co content. Upon calcination at 500 degrees C, HTlc decomposed into an Al-substituted Co3O4 spinel oxide, as confirmed by two distinctly separated reduction steps in H-2-TPR. Following reduction at 700 degrees C, well-dispersed Co metal nanoparticles with an average particle size of similar to 9.2-12.4 nm were obtained. It was suggested that the incorporation of Al3+ into Co3O4 led to a strong interaction between cobalt and aluminum, which suppressed the crystal growth of Co3O4 and the sintering of Co metal during the thermal treatments, resulting in good Co dispersion. The optimal LiAlCo(1.5) catalyst showed superior activity than that prepared by impregnation method, giving almost complete conversion of ammonia at 575 degrees C under a space velocity of 5,000 mL g(cat)(-1) h(-1). More importantly, this catalyst maintained stable activity at 625 degrees C for 100 h, exhibiting high stability and sintering resistance. The good catalytic performance was attributed to the high Co metal dispersion and strong metal-support interaction benefiting from the uniform distribution of cobalt in the HTlc precursor. These results demonstrate the applicability of HTlc to the preparation of metal catalysts with improved dispersion and thermal stability.
Keyword ：
Catalytic ammonia decomposition Catalytic ammonia decomposition Cobalt catalyst Cobalt catalyst Hydrogen production Hydrogen production Hydrotalcite-like compounds Hydrotalcite-like compounds
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| GB/T 7714 | Wei, Xiaofeng , Su, Jiaxin , Ji, Yuyin et al. Hydrotalcite-derived well-dispersed and thermally stable cobalt nanoparticle catalyst for ammonia decomposition [J]. | MOLECULAR CATALYSIS , 2025 , 572 . |
| MLA | Wei, Xiaofeng et al. "Hydrotalcite-derived well-dispersed and thermally stable cobalt nanoparticle catalyst for ammonia decomposition" . | MOLECULAR CATALYSIS 572 (2025) . |
| APA | Wei, Xiaofeng , Su, Jiaxin , Ji, Yuyin , Huang, Hongyang , Li, Dalin , Fang, Huihuang et al. Hydrotalcite-derived well-dispersed and thermally stable cobalt nanoparticle catalyst for ammonia decomposition . | MOLECULAR CATALYSIS , 2025 , 572 . |
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Trace ammonia reversible adsorption and sieving using solid adsorbents present a critical challenge in the practical deployment of ammonia-hydrogen fuel cells. Herein, we design porous polydivinylbenzene (P-PDVB) through one-pot solvothermal polymerization without additional templates. Subsequently, solvent-induced network swelling was performed to achieve deep sulfonation of the P-PDVB using chlorosulfonic acid, resulting in P-PDVB-SO3H-x, which possess large specific surface areas, abundant micro-mesoporosity, and high acid site densities. Notably, P-PDVB-SO3H-x demonstrate superior performance for the selective capture and sieving of NH3 from an N2/H2/NH3 mixture, outperforming most previously reported NH3 adsorbents. Thus, P-PDVB-SO3H-x can serve as an efficient adsorbent for the selective removal of trace ammonia from ammonia-hydrogen fuel cell systems, significantly improving both the efficiency and longevity of the fuel cells. This work highlights the potential of P-PDVB-SO3H-x as a promising candidate for enhancing ammonia-hydrogen fuel cell performance, paving the way for further exploration of advanced adsorbent materials in energy applications.
Keyword ：
ammonia-hydrogen fuel cell ammonia-hydrogen fuel cell ammonia separation ammonia separation deep sulfonation deep sulfonation porous organic polymers porous organic polymers selective adsorption selective adsorption solvothermal synthesis solvothermal synthesis
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| GB/T 7714 | Qu, Yongfang , Zhang, Wentao , Zhong, Shouchao et al. Reversible adsorption and sieving of trace NH3 from NH3-H2 fuel cells systems using sulfonated porous polydivinylbenzene [J]. | AICHE JOURNAL , 2025 , 71 (5) . |
| MLA | Qu, Yongfang et al. "Reversible adsorption and sieving of trace NH3 from NH3-H2 fuel cells systems using sulfonated porous polydivinylbenzene" . | AICHE JOURNAL 71 . 5 (2025) . |
| APA | Qu, Yongfang , Zhang, Wentao , Zhong, Shouchao , Zhuo, Linyu , Wang, Xi , Fang, Huihuang et al. Reversible adsorption and sieving of trace NH3 from NH3-H2 fuel cells systems using sulfonated porous polydivinylbenzene . | AICHE JOURNAL , 2025 , 71 (5) . |
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Cu-based catalysts have been extensively researched for hydrogen production via water-gas shift (WGS, CO+H2O <-> CO2+H-2) reaction. Yet, the catalyst easily suffers from performance degradation due to Cu+/Cu-0 transformation and particle aggregation. Herein, copper phyllosilicate with different morphologies, i.e., tubular and lamellar, was fabricated by a modified hydrothermal method for the WGS reaction. Compared with the catalyst derived from lamellar copper phyllosilicate (30Cu/SiO2-L), the one derived from the tubular phyllosilicate (30Cu/SiO2-T) demonstrates better performance due to the high Cu+/(Cu-0+Cu+) ratio. In situ characterizations were conducted to unveil the transformation between Cu+ and Cu-0, which is highly correlated to the CO and H2O activation. Cu+ is primarily responsible for the activation of CO, while Cu-0 mainly facilitates the dissociation of H2O. The results show that 30Cu/SiO2-T follows the redox mechanism, where CO reduces Cu+ to Cu-0 and H2O oxidizes Cu-0 to Cu+, maintaining the reaction cycle.
Keyword ：
copper phyllosilicate copper phyllosilicate Cu+-Cu-0 Cu+-Cu-0 morphology morphology redox mechanism redox mechanism water-gas shift water-gas shift
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| GB/T 7714 | Huang, Chunjin , Chen, Yue , Fang, Huihuang et al. Copper Phyllosilicate-Derived Cu Catalyst for the Water-Gas Shift Reaction: Insight into the Role of Cu+-Cu0 and Reaction Mechanism [J]. | ACS CATALYSIS , 2025 , 15 (7) : 5546-5556 . |
| MLA | Huang, Chunjin et al. "Copper Phyllosilicate-Derived Cu Catalyst for the Water-Gas Shift Reaction: Insight into the Role of Cu+-Cu0 and Reaction Mechanism" . | ACS CATALYSIS 15 . 7 (2025) : 5546-5556 . |
| APA | Huang, Chunjin , Chen, Yue , Fang, Huihuang , Zhi, Guo , Chen, Chongqi , Luo, Yu et al. Copper Phyllosilicate-Derived Cu Catalyst for the Water-Gas Shift Reaction: Insight into the Role of Cu+-Cu0 and Reaction Mechanism . | ACS CATALYSIS , 2025 , 15 (7) , 5546-5556 . |
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Direct ammonia solid oxide fuel cells (DA-SOFCs) have triggered great interest due to their efficient power generation from ammonia directly. However, the compatible match of ammonia decomposition and electrooxidation in the DA-SOFCs remains greatly challenging due to their endo/exothermic properties. Herein, multi-sizes tubular DA-SOFCs were systematically investigated for performance evaluation of power output and ammonia decomposition. Accordingly, a multi-scale electro-thermo model for tubular DA-SOFC was established to intensify the synergy between complex physical-chemical processes and geometry. With the combination of experimental work and simulations, the effects of operating conditions and geometry were comprehensively evaluated. Significantly, the rates of ammonia decomposition and electrooxidation could be effectively matched through the optimization of operating conditions. The geometric design further enables the temperature-zoning of the two processes, competently enhancing the thermal coupling between them. Conclusively, the correlation equations linking the operating conditions, geometry and electrical efficiency were proposed for the scaling-up of tubular DA-SOFCs unit. The tubular DA-SOFC achieves 3.5 W with 60% electrical efficiency, and performed a satisfactory stability for over 330 h. This study provides guidance for oriented design of tubular DA-SOFCs with high electrical efficiency.
Keyword ：
direct ammonia solid oxide fuel cells direct ammonia solid oxide fuel cells geometric design geometric design multi-scale electro-thermo model multi-scale electro-thermo model operating conditions operating conditions performance enhancement performance enhancement
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| GB/T 7714 | Chen, Shuai , Liao, Xiaofei , You, Jiacheng et al. Enhanced coupling of the tubular direct ammonia solid oxide fuel cells for efficient ammonia-to-power [J]. | AICHE JOURNAL , 2025 , 71 (5) . |
| MLA | Chen, Shuai et al. "Enhanced coupling of the tubular direct ammonia solid oxide fuel cells for efficient ammonia-to-power" . | AICHE JOURNAL 71 . 5 (2025) . |
| APA | Chen, Shuai , Liao, Xiaofei , You, Jiacheng , Jiang, Yiting , Zhong, Fulan , Fang, Huihuang et al. Enhanced coupling of the tubular direct ammonia solid oxide fuel cells for efficient ammonia-to-power . | AICHE JOURNAL , 2025 , 71 (5) . |
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As a carbon-free hydrogen (H2) carrier with the advantage of liquefaction storage and transportation, ammonia (NH3) is regarded as a competitive clean energy carrier for H2 production and power generation. This work designs a novel NH3-fueled hybrid power generation system, which combines ammonia decomposition reactor (ADR), proton exchange membrane fuel cell (PEMFC) and micro gas turbine (MGT) together with thermochemical recuperation for ADR. A system-level thermodynamic model has been developed to evaluate system performance with different optimization strategies. The model calculation reveals that the NH3 decomposition temperature drop from 500 degrees C to 350 degrees C can increase the energy efficiency from 33.5 % to 43.2 %, and two improved integration strategies have therefore been proposed. Mixing a part of NH3 with the exhaust gas from PEMFC anode to fuel MGT can reduce the NH3 decomposition demand and makes better use of waste heat from MGT. Integrating ADR with MGT combustor can lower the exhaust gas temperature and the efficiency loss when using high temperature NH3 decomposition catalyst. Both strategies can improve the system energy efficiency, to about 40% and 44% when NH3 decomposition temperature is 500 degrees C and 350 degrees C, respectively, and demonstrate better flexibility in adapting to changes in NH3 decomposition temperature.
Keyword ：
Ammonia decomposition Ammonia decomposition Ammonia energy Ammonia energy Power generation system Power generation system Proton exchange membrane fuel cell Proton exchange membrane fuel cell Thermochemical recuperation Thermochemical recuperation
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| GB/T 7714 | Lin, Li , Sun, Mingwei , Wu, Yifan et al. High-efficiency ammonia-fueled hybrid power generation system combining ammonia decomposition, proton exchange membrane fuel cell and micro gas turbine: A thermodynamic model and performance optimization [J]. | ENERGY CONVERSION AND MANAGEMENT , 2025 , 325 . |
| MLA | Lin, Li et al. "High-efficiency ammonia-fueled hybrid power generation system combining ammonia decomposition, proton exchange membrane fuel cell and micro gas turbine: A thermodynamic model and performance optimization" . | ENERGY CONVERSION AND MANAGEMENT 325 (2025) . |
| APA | Lin, Li , Sun, Mingwei , Wu, Yifan , Huang, Wenshi , Wu, Zeyun , Wang, Dabiao et al. High-efficiency ammonia-fueled hybrid power generation system combining ammonia decomposition, proton exchange membrane fuel cell and micro gas turbine: A thermodynamic model and performance optimization . | ENERGY CONVERSION AND MANAGEMENT , 2025 , 325 . |
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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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