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学者姓名：朱海波
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Abstract ：
Supported noble metal cluster catalysts are typically operated under severe conditions involving switching between reducing and oxidizing atmospheres, causing irreversible transformation of the catalyst structure and thereby leading to permanent deactivation. We discovered that various platinum (Pt) precursors spontaneously disperse in a germanium-MFI (Ge-MFI) zeolite, which opposes the Ostwald ripening phenomenon, producing self-regenerating Pt/Ge-MFI catalysts for propane dehydrogenation. These catalysts reversibly switch between Pt clusters and Pt single atoms in response to reducing reaction and oxidizing regeneration conditions. This environmental adaptability allows them to completely self-regenerate over 110 reaction and regeneration cycles in propane dehydrogenation, and they exhibited unprecedented sintering resistance when exposed to air at 800 degrees C for 10 days. Such spontaneous metal dispersion in a Ge-MFI zeolite is a robust and versatile methodology for fabricating various rhodium, ruthenium, iridium, and palladium cluster catalysts.
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| GB/T 7714 | Hong, Huizhen , Xu, Zhikang , Mei, Bingbao et al. A self-regenerating Pt/Ge-MFI zeolite for propane dehydrogenation with high endurance [J]. | SCIENCE , 2025 , 388 (6746) : 497-502 . |
| MLA | Hong, Huizhen et al. "A self-regenerating Pt/Ge-MFI zeolite for propane dehydrogenation with high endurance" . | SCIENCE 388 . 6746 (2025) : 497-502 . |
| APA | Hong, Huizhen , Xu, Zhikang , Mei, Bingbao , Hu, Wende , Fornasiero, Paolo , Wang, Chuanming et al. A self-regenerating Pt/Ge-MFI zeolite for propane dehydrogenation with high endurance . | SCIENCE , 2025 , 388 (6746) , 497-502 . |
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The shale gas revolution has shifted propylene production from naphtha cracking to on-purpose production with propane dehydrogenation (PDH) as the dominant technology1, 2, 3, 4, 5, 6, 7, 8-9. Because PDH is endothermic and requires high temperatures that favour sintering and coking, the challenge is to develop active and stable catalysts1, 2-3 that are sufficiently stable10,11. Zeolite-supported Pt-Sn catalysts have been developed to balance activity, selectivity and stability12,13 and more recent work documented a PDH catalyst based on zeolite-anchored single rhodium atoms with exceptional performance and stability14. Here we show for silicalite-1 (S-1) that migration of encapsulated Pt-Sn2 clusters and hence agglomeration and anchoring within the zeolite versus agglomeration on the external surface can be controlled by adjusting the length of the S-1 crystals' b-axis. We find that, when this axis is longer than 2.00 mu m, migration of Pt-Sn2 monomers during PDH results in intracrystalline formation of (Pt-Sn2)2 dimers that are securely locked in the channels of S-1 and capable of converting pure propane feed to propylene at 550 degrees C for more than 6 months with 98.3% selectivity at 91% equilibrium conversion. This performance exceeds that of other Pt-based PDH catalysts and approaches that of the Rh-based catalyst. Although synthesis requirements and cost are at present prohibitive for industrial use, we anticipate that our approach to controlling the migration and lockup of metals in zeolites may enable the development of other noble-metal catalysts that offer extended service lifetimes in industrial applications15, 16-17.
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| GB/T 7714 | Xu, Zhikang , Gao, Mingbin , Wei, Yao et al. Pt migration-lockup in zeolite for stable propane dehydrogenation catalyst [J]. | NATURE , 2025 , 643 (8072) . |
| MLA | Xu, Zhikang et al. "Pt migration-lockup in zeolite for stable propane dehydrogenation catalyst" . | NATURE 643 . 8072 (2025) . |
| APA | Xu, Zhikang , Gao, Mingbin , Wei, Yao , Yue, Yuanyuan , Bai, Zhengshuai , Yuan, Pei et al. Pt migration-lockup in zeolite for stable propane dehydrogenation catalyst . | NATURE , 2025 , 643 (8072) . |
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Pt-Cu bimetallic particles have been regarded as promising catalysts for propane dehydrogenation. The dispersion of Pt and Cu species on conventional supports always results in the formation of large Pt-Cu particles, and it is highly desirable to fabricate ultra-small Pt-Cu cluster catalysts for propane dehydrogenation. Herein, we used the isolated Cu species in the Cu-SSZ-13 to localize the Pt species, and the alloying of Pt with Cu leads to a formation of ultra-small (<1 nm) Pt-Cu bimetallic clusters in the structure of SSZ-13. The structure of synthesized PtCu-SSZ-13 catalysts was studied by XRD, SEM, STEM, XPS, CO-FTIR, H-2-TPR and EXAFS techniques, which demonstrates that Pt-Cu clusters are entrapped in the micropore of SSZ-13 and their migration can be greatly inhibited. The synthesized PtCu-SSZ-13 catalyst shows high activity and good regeneration in propane dehydrogenation. The optimized catalyst 0.3 %PtCu-SSZ-13 delivers propane conversion of 28.5 % (close to equilibrium conversion) with 100 % propane as feed under WHSV of 7.1 h(-1) at 520 degrees C, and its catalytic performance can be completely regenerated via calcination in air. Density functional theory (DFT) calculations indicate that the unique Pt-Cu bimetallic nanocluster structure reduces the energy potential for propane dehydrogenation as well as promotes the adsorption of C3H8 and desorption of C3H6, thus enhancing the activity of the PtCu-SSZ-13 catalyst.
Keyword ：
Cu-SSZ-13 zeolite Cu-SSZ-13 zeolite Highly dispersion Highly dispersion Propane dehydrogenation Propane dehydrogenation Pt-Cu bimetallic Pt-Cu bimetallic Ultra-small nanoclusters Ultra-small nanoclusters
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| GB/T 7714 | Xu, Zhikang , Gao, Mingbin , Wu, Xing et al. Pt nanoclusters entrapped within Cu-SSZ-13 zeolite for efficient propane dehydrogenation [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 511 . |
| MLA | Xu, Zhikang et al. "Pt nanoclusters entrapped within Cu-SSZ-13 zeolite for efficient propane dehydrogenation" . | CHEMICAL ENGINEERING JOURNAL 511 (2025) . |
| APA | Xu, Zhikang , Gao, Mingbin , Wu, Xing , Zhu, Haibo . Pt nanoclusters entrapped within Cu-SSZ-13 zeolite for efficient propane dehydrogenation . | CHEMICAL ENGINEERING JOURNAL , 2025 , 511 . |
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Co-based catalysts are emerging as one of the most promising catalysts for propane dehydrogenation (PDH) due to their abundant availability, environmental friendliness, and efficient activation of the C-H bond. Isolated Co (II) is recognized as the active site for activating the C-H bond in PDH; however, the controllable synthesis of Co catalysts with well-defined isolated Co(II) remains a challenge. In this study, a direct and straightforward route was developed for the synthesis of Co-Beta using a fluorine-assisted hydrothermal crystallization method. The structure of Co-Beta was studied using various characterization tools, including XRD, STEM, H2-TPR, UV-vis, XPS, solid-state 29Si MAS NMR and EXAFS techniques. It was confirmed that the Co species are incorporated into the structure of Beta zeolite, existing as isolated Co(II) sites embedded within the framework of Beta zeolite. The optimized catalyst, 1.0Co-Beta, exhibits excellent performance in PDH, achieving a propane conversion of approximately 50 % and propylene selectivity of around 96 % at 600 degrees C. This performance surpasses that of previously reported non-noble metal catalysts. This study provides fundamental insights on the design and synthesis of highly dispersed metal oxide catalysts for PDH.
Keyword ：
C-H bond activation C-H bond activation Isolated Co(II) Isolated Co(II) Propane dehydrogenation Propane dehydrogenation Propylene production Propylene production
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| GB/T 7714 | Xu, Zhikang , Zhang, Yunxing , Wu, Xing et al. Co(II) sites embedded within Beta zeolite as efficient catalyst for propane dehydrogenation [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 513 . |
| MLA | Xu, Zhikang et al. "Co(II) sites embedded within Beta zeolite as efficient catalyst for propane dehydrogenation" . | CHEMICAL ENGINEERING JOURNAL 513 (2025) . |
| APA | Xu, Zhikang , Zhang, Yunxing , Wu, Xing , Zhu, Haibo . Co(II) sites embedded within Beta zeolite as efficient catalyst for propane dehydrogenation . | CHEMICAL ENGINEERING JOURNAL , 2025 , 513 . |
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Cyclohexane as liquid organic hydrogen carriers has attracted considerable interest in the field of hydrogen storage technology. However, the innovation of efficient catalyst for producing H2 through cyclohexane dehydrogenation remains a substantial challenge. In this study, we have successfully developed Pt/MgAl2O4 catalysts exhibiting outstanding catalytic performance in cyclohexane dehydrogenation. Notably, the optimal catalyst Pt/ MgAl2O4-700 achieves cyclohexane conversion of 89.1 % and benzene selectivity of over 99 % at 345 degrees C, resulting in a high hydrogen evolution rate of 933 mmol/gPt/min. Moreover, this catalyst exhibits remarkable long-term stability, with no evident loss of activity in 225-hour dehydrogenation reaction. The catalyst was characterized by XRD, N2 adsorption-desorption, STEM, XPS, NH3-TPD, CO-FTIR and H2-TPR techniques, which provides detailed structure information for elucidation of structure-activity relationship. The spinel structure and moderate acid density of the support enable highly dispersed Pt species at the surface of MgAl2O4. This results in the formation of ultra-small and sintering-resistant Pt particles that exhibit exceptional activity in cyclohexane dehydrogenation. Additionally, the presence of positively charged Pt delta+ species in Pt/MgAl2O4 facilitates the rapid desorption of benzene product. This effectively prevents the formation of coke arising from benzene dehydrogenation, which ensures to achieve high stability. These findings provide valuable knowledge for the rational design of efficient metal-based catalysts for liquid organic hydrogen carriers in hydrogen storage systems.
Keyword ：
Cyclohexane dehydrogenation Cyclohexane dehydrogenation H-2 production H-2 production Liquid organic hydrogen carriers Liquid organic hydrogen carriers Positively charged Pt Positively charged Pt Pt/MgAl2O4 Pt/MgAl2O4
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| GB/T 7714 | Guo, Lipeng , Xu, Zhikang , Wang, Tinghai et al. Stable Pt/MgAl2O4 catalysts for efficient production of H2 from cyclohexane dehydrogenation [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 299 . |
| MLA | Guo, Lipeng et al. "Stable Pt/MgAl2O4 catalysts for efficient production of H2 from cyclohexane dehydrogenation" . | CHEMICAL ENGINEERING SCIENCE 299 (2024) . |
| APA | Guo, Lipeng , Xu, Zhikang , Wang, Tinghai , Zhu, Haibo . Stable Pt/MgAl2O4 catalysts for efficient production of H2 from cyclohexane dehydrogenation . | CHEMICAL ENGINEERING SCIENCE , 2024 , 299 . |
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The SO2 poisoning of a heterobimetallic FeCu-SSZ-13 in selective catalytic reduction of NO with NH3 (NH3-SCR) was systematically investigated in this study. It was shown that when SO2 is involved in the feeding flue gas, the losses in the redox ability of active metals (primary contributor to deactivation) and in the number of Bronsted acid sites both inhibit the formation of NH4NO2 intermediate, resulting in the rapid deactivation of FeCu-SSZ-13. The SO2 poisoning of FeCu-SSZ-13 at low temperature is more serious than at high temperature, because of the more severe loss of redox ability of active metals. Unlike that of monometallic Cu-/Fe-CHA, the SO(2 )poisoning of the bimetallic one is saliently featured by that partial SO2 is oxidized to SO3 and partial Bronsted acid sites are destroyed due to the formation of H2SO4. This work may provide a fundamental understanding on the SO2 poisoning of heterobimetallic zeolite-based NH3-SCR catalysts.
Keyword ：
bimetallic FeCu-SSZ-13 bimetallic FeCu-SSZ-13 mechanism mechanism regeneration ability regeneration ability selective catalytic reduction selective catalytic reduction SO2 poisoning SO2 poisoning
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| GB/T 7714 | Lin, Zheguan , Wang, Chan , Li, Tiesen et al. Insight into the SO2 poisoning of heterobimetallic FeCu-SSZ-13 zeolite in NH3-SCR reaction [J]. | AICHE JOURNAL , 2024 , 70 (3) . |
| MLA | Lin, Zheguan et al. "Insight into the SO2 poisoning of heterobimetallic FeCu-SSZ-13 zeolite in NH3-SCR reaction" . | AICHE JOURNAL 70 . 3 (2024) . |
| APA | Lin, Zheguan , Wang, Chan , Li, Tiesen , Zhu, Haibo , Jiang, Lilong , Yue, Yuanyuan et al. Insight into the SO2 poisoning of heterobimetallic FeCu-SSZ-13 zeolite in NH3-SCR reaction . | AICHE JOURNAL , 2024 , 70 (3) . |
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Propylene is the second most important chemicals in the petrochemical industry. Propane dehydrogenation as the on -purpose propylene production route, has attracted much attentions due to great success in the exploitation of shale gas. Recently, Pt@zeolite is proven to the most promising catalyst for propane dehydrogenation, because Pt clusters encapsulated in zeolite channel show high resistance to Pt particles sintering. However, the micropore of zeolite imposes severe diffusion limitation of propylene, and thus the coke formation easily takes place which leads to a fast deactivation. Herein, we report efficient Pt/Zn-MFIhierarchical catalysts for PDH with auxiliary mesopore for accelerating mass transfer, and these Pt/Zn-MFIhierarchical exhibit not only high thermal stability but also excellent resistance to coking. The Pt/Zn-MFIhierarchical catalyst is obtained by an introduction of Pt species into the hierarchically porous Zn-MFI that is prepared from one-step hydrothermal synthesis. The formed Pt-Zn clusters are exclusively located in the micropore of MFIhierarchical, and the migrating of Pt-Zn clusters is largely prevented under the harsh reaction conditions. Mesopores in MFIhierarchical greatly enhances the diffusion rate of propylene, which significantly alleviates the coke formation arising from polymerization of propylene. The most efficient Pt/Zn-MFI-120hierarchical catalyst delivers propane conversion of around 46 % and propylene selectivity of above 98 %. This catalyst undergoes a slow loss of activity with a deactivation rate kd of as low as 0.005 h-1, and its catalytic performance can be fully restored via a simple calcination.
Keyword ：
Coking-resistance Coking-resistance Hierarchical zeolite Hierarchical zeolite Propane dehydrogenation Propane dehydrogenation Propylene production Propylene production Pt-Zn clusters Pt-Zn clusters Sintering-resistance Sintering-resistance
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| GB/T 7714 | Lu, Jinyang , Xu, Zhikang , Yue, Yuanyuan et al. Pt-Zn clusters encapsulated in hierarchical MFI zeolite for efficient propane dehydrogenation [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 484 . |
| MLA | Lu, Jinyang et al. "Pt-Zn clusters encapsulated in hierarchical MFI zeolite for efficient propane dehydrogenation" . | CHEMICAL ENGINEERING JOURNAL 484 (2024) . |
| APA | Lu, Jinyang , Xu, Zhikang , Yue, Yuanyuan , Bao, Xiaojun , Lin, Minggui , Zhu, Haibo . Pt-Zn clusters encapsulated in hierarchical MFI zeolite for efficient propane dehydrogenation . | CHEMICAL ENGINEERING JOURNAL , 2024 , 484 . |
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The use of dodecahydro- N -ethylcarbazole in hydrogen storage for liquid organic hydrogen carrier systems holds potential for achieving large-scale application. In order to investigate the relationship between dodecahydro- N - ethylcarbazole dehydrogenation performance and Pt particles size, a series of monometallic Pt/Al 2 O 3 catalysts with different Pt particles size from 0.70 nm to 5.12 nm were controlled synthesized by a simple impregnation method. The obtained catalysts are systematically characterized via XRD, 27 Al MAS NMR, SEM-EDS, TEM, N 2 - adsorption, CO-IR, H 2 -TPR and NH 3 -TPD analyses, which provide essential micro-structure of these catalysts. The dehydrogenation of dodecahydro- N -ethylcarbazole over Pt/Al 2 O 3 is a typical consecutive reaction, which follows a reaction sequence of dodecahydro- N -ethylcarbazole -* octahydro- N -ethylcarbazole -* tetrahydro- N -ethyl- carbazole -* N -ethylcarbazole. These dehydrogenation steps are quite sensitive to the Pt particle size. Large Pt particle can greatly enhance the reaction rates in octahydro- N -ethylcarbazole -* tetrahydro- N -ethylcarbazole and tetrahydro- N -ethylcarbazole -* N -ethylcarbazole steps. However, these two steps are difficult to take place in small Pt particles. The high performance of large Pt particle in dehydrogenation can be ascribed to its highly exposed (111) crystal face. The optimized catalyst Pt 5.0 /gamma-Al 2 O 3 with Pt average size of 4.63 nm demonstrated exceptional performance in dodecahydro- N -ethylcarbazole dehydrogenation at 180 degrees C and 101 kPa, and the dodecahydro- N -ethylcarbazole conversion of 100 %, N -ethylcarbazole selectivity of 96.44 % and dehydrogenation efficiency of 98.73 % can be achieved. These results provide valuable insights for the development of efficient metal-based catalysts for liquid organic hydrogen carriers hydrogen storage system.
Keyword ：
Dehydrogenation Dehydrogenation Dodecahydro-N-ethylcarbazole Dodecahydro-N-ethylcarbazole Hydrogen storage Hydrogen storage Liquid organic hydrogen carriers Liquid organic hydrogen carriers Supported Pt catalysts Supported Pt catalysts
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| GB/T 7714 | Yao, Jihui , Xu, Zhikang , Cheng, Shuo et al. Pt/Al 2 O 3 as efficient catalyst for the dehydrogenation of Dodecahydro- N-ethylcarbazole [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 491 . |
| MLA | Yao, Jihui et al. "Pt/Al 2 O 3 as efficient catalyst for the dehydrogenation of Dodecahydro- N-ethylcarbazole" . | CHEMICAL ENGINEERING JOURNAL 491 (2024) . |
| APA | Yao, Jihui , Xu, Zhikang , Cheng, Shuo , Yue, Yuanyuan , Zhu, Haibo . Pt/Al 2 O 3 as efficient catalyst for the dehydrogenation of Dodecahydro- N-ethylcarbazole . | CHEMICAL ENGINEERING JOURNAL , 2024 , 491 . |
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N-ethylcarbazole, as a liquid organic hydrogen carrier, has shown great promise in the field of hydrogen storage technology. The development of efficient and stable catalyst for producing H-2 through N-ethylcarbazole dehydrogenation is crucial for its practical application. In this study, a series of mesoporous Al2O3-supported Pt catalysts with K modification were developed for N-ethylcarbazole dehydrogenation. These catalysts were characterization using various techniques including XRD, N-2 adsorption-desorption, TEM, Al-27 MAS NMR, XPS, NH3-TPD, H-2-TPR, CO-FTIR, and Py-IR, providing detailed structural information to elucidate the structure-activity relationship. Mesoporous Al2O3 was found to possess significant amounts of coordinatively unsaturated pentacoordinate Al3+, which greatly promotes the dispersion of Pt species for the formation of small Pt particles. The addition of K was observed to modulate the electronic structure of Pt, reduce the acidity of the catalysts, and inhibit the sintering of Pt. These synergetic effects led to Pt-3.0/K-3.0-Al2O3-m achieving remarkable performance in dodecahydro-N-ethylcarbazole dehydrogenation at 180 degrees C and 101 kPa, delivering a dodecahydro-N-ethylcarbazole conversion of 100 %, H-2 release amount of 5.63 wt% and dehydrogenation efficiency of 97.10 %. Additionally, this catalyst demonstrated high efficiency in the dehydrogenation of dodecahydro-N-propylcarbazole, octahydro-2-methylindole, and octahydro-1,2-dimethylindole, achieving dehydrogenation efficiencies of 99.60 %, 100 % and 100 %, respectively. These findings provide valuable knowledge for the rational design of efficient metal-based catalysts for liquid organic hydrogen carriers in hydrogen storage systems.
Keyword ：
Dehydrogenation Dehydrogenation Dodecahydro-N-ethylcarbazole Dodecahydro-N-ethylcarbazole Hydrogen storage Hydrogen storage K-modification K-modification Liquid organic hydrogen carriers Liquid organic hydrogen carriers Pt-based catalysts Pt-based catalysts
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| GB/T 7714 | Yao, Jihui , Su, Lijuan , Guo, Lipeng et al. K-promoted Pt/meso-Al2O3 catalysts for H2 production from dehydrogenation of dodecahydro-N-ethylcarbazole [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 301 . |
| MLA | Yao, Jihui et al. "K-promoted Pt/meso-Al2O3 catalysts for H2 production from dehydrogenation of dodecahydro-N-ethylcarbazole" . | CHEMICAL ENGINEERING SCIENCE 301 (2024) . |
| APA | Yao, Jihui , Su, Lijuan , Guo, Lipeng , Wu, Xing , Zhu, Haibo . K-promoted Pt/meso-Al2O3 catalysts for H2 production from dehydrogenation of dodecahydro-N-ethylcarbazole . | CHEMICAL ENGINEERING SCIENCE , 2024 , 301 . |
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能源是国民经济和社会发展的重要基础,为实现可持续发展,需将绿色清洁理念践行于能源发展全过程.在建设多元清洁能源供应体系的过程中,发展"低碳、零碳、负碳"技术是提高能源供给质量的有效举措."低碳"目标是从源头减少碳排放,其关注重点为高能耗的化石能源产业;"零碳"技术主要针对氢能、生物质能等可再生能源的开发和利用,以期实现对传统能源的完全替代;"负碳"技术的内涵为捕获和转化利用二氧化碳,是最有望实现碳排放断崖式下降的技术.本文针对目前传统和新能源交织发展的现状,对传统能源生产技术从降低能耗、减少污染排放以及资源深度开发利用 3 个方面进行总结,对"零碳"和"负碳"技术则主要从催化科学及技术层面进行综述,以期为构建"零碳未来城"提供参考.
Keyword ：
二氧化碳捕获和利用 二氧化碳捕获和利用 低碳技术 低碳技术 零碳能源 零碳能源
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| GB/T 7714 | 张宏伟 , 朱海波 , 吴欣茹 et al. "双碳"目标下绿色清洁能源技术现状与发展趋势 [J]. | 石油科学通报 , 2023 , 8 (5) : 555-576 . |
| MLA | 张宏伟 et al. ""双碳"目标下绿色清洁能源技术现状与发展趋势" . | 石油科学通报 8 . 5 (2023) : 555-576 . |
| APA | 张宏伟 , 朱海波 , 吴欣茹 , 李铁森 , 袁珮 , 鲍晓军 . "双碳"目标下绿色清洁能源技术现状与发展趋势 . | 石油科学通报 , 2023 , 8 (5) , 555-576 . |
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