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学者姓名:朱海波

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Pt nanoclusters entrapped within Cu-SSZ-13 zeolite for efficient propane dehydrogenation SCIE
期刊论文 | 2025 , 511 | CHEMICAL ENGINEERING JOURNAL
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Abstract :

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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Pt nanoclusters entrapped within Cu-SSZ-13 zeolite for efficient propane dehydrogenation EI
期刊论文 | 2025 , 511 | Chemical Engineering Journal
Pt nanoclusters entrapped within Cu-SSZ-13 zeolite for efficient propane dehydrogenation Scopus
期刊论文 | 2025 , 511 | Chemical Engineering Journal
Pt/Al 2 O 3 as efficient catalyst for the dehydrogenation of Dodecahydro- N-ethylcarbazole SCIE
期刊论文 | 2024 , 491 | CHEMICAL ENGINEERING JOURNAL
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Abstract :

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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Pt/Al2O3 as efficient catalyst for the dehydrogenation of Dodecahydro-N-ethylcarbazole EI
期刊论文 | 2024 , 491 | Chemical Engineering Journal
Pt/Al2O3 as efficient catalyst for the dehydrogenation of Dodecahydro-N-ethylcarbazole Scopus
期刊论文 | 2024 , 491 | Chemical Engineering Journal
K-promoted Pt/meso-Al2O3 catalysts for H2 production from dehydrogenation of dodecahydro-N-ethylcarbazole SCIE
期刊论文 | 2024 , 301 | CHEMICAL ENGINEERING SCIENCE
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Abstract :

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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K-promoted Pt/meso-Al2O3 catalysts for H2 production from dehydrogenation of dodecahydro‑N‑ethylcarbazole Scopus
期刊论文 | 2025 , 301 | Chemical Engineering Science
K-promoted Pt/meso-Al2O3 catalysts for H2 production from dehydrogenation of dodecahydro‑N‑ethylcarbazole EI
期刊论文 | 2025 , 301 | Chemical Engineering Science
Stable Pt/MgAl2O4 catalysts for efficient production of H2 from cyclohexane dehydrogenation SCIE
期刊论文 | 2024 , 299 | CHEMICAL ENGINEERING SCIENCE
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Abstract :

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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Stable Pt/MgAl2O4 catalysts for efficient production of H2 from cyclohexane dehydrogenation EI
期刊论文 | 2024 , 299 | Chemical Engineering Science
Stable Pt/MgAl2O4 catalysts for efficient production of H2 from cyclohexane dehydrogenation Scopus
期刊论文 | 2024 , 299 | Chemical Engineering Science
Pt-Zn clusters encapsulated in hierarchical MFI zeolite for efficient propane dehydrogenation SCIE
期刊论文 | 2024 , 484 | CHEMICAL ENGINEERING JOURNAL
WoS CC Cited Count: 16
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Abstract :

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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Pt-Zn clusters encapsulated in hierarchical MFI zeolite for efficient propane dehydrogenation Scopus
期刊论文 | 2024 , 484 | Chemical Engineering Journal
一种功能型活性硅铝酸盐及其制备方法和应用 incoPat
专利 | 2021-11-24 00:00:00 | CN202111401128.5
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本发明提供一种功能型活性硅铝酸盐的制备方法及其应用,该方法是将天然硅铝矿物、有机酸盐和碱金属氢氧化物溶液混合打浆,然后浆液中的天然硅铝矿物和有机酸盐在喷雾干燥器内分别发生解聚和碳化,制备得到的硅铝酸盐可用于梯级孔分子筛的合成,其所含的高活性硅铝物种为合成梯级孔分子筛提供硅铝源、所含的碳颗粒作为合成梯级孔分子筛的介孔模板剂。本发明明显缩短天然硅铝矿物的解聚时间,能够实现天然硅铝矿物连续化解聚,有利于规模化生产,同时本发明制备得到的材料中碳颗粒高度分散在活性硅铝酸盐中,有效地避免碳材料作为分子筛合成的介孔模板剂时容易与硅铝原料发生相分离的问题,为梯级孔分子筛的合成提供一种高效易行的方法。

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GB/T 7714 岳源源 , 董鹏 , 鲍晓军 et al. 一种功能型活性硅铝酸盐及其制备方法和应用 : CN202111401128.5[P]. | 2021-11-24 00:00:00 .
MLA 岳源源 et al. "一种功能型活性硅铝酸盐及其制备方法和应用" : CN202111401128.5. | 2021-11-24 00:00:00 .
APA 岳源源 , 董鹏 , 鲍晓军 , 王婵 , 王廷海 , 朱海波 et al. 一种功能型活性硅铝酸盐及其制备方法和应用 : CN202111401128.5. | 2021-11-24 00:00:00 .
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一种亲油型Fe基悬浮床加氢裂化催化剂的制备方法 incoPat
专利 | 2021-11-14 00:00:00 | CN202111344021.1
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本发明公开了一种亲油型Fe基悬浮床加氢裂化催化剂的制备方法,先采用水热‑沉淀法以废弃木屑为模板剂制备出具有介孔结构的氧化铁,再利用大分子有机物(如硬脂酸等)对其进行表面修饰,获得具有亲油性氧化铁催化剂。制得的催化剂具有亲油性,用于劣质重油悬浮床加氢裂化反应,表现出良好的反应性能,有效地抑制焦炭和气体产生,提高液体馏分油收率。

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GB/T 7714 崔勍焱 , 王军 , 鲍晓军 et al. 一种亲油型Fe基悬浮床加氢裂化催化剂的制备方法 : CN202111344021.1[P]. | 2021-11-14 00:00:00 .
MLA 崔勍焱 et al. "一种亲油型Fe基悬浮床加氢裂化催化剂的制备方法" : CN202111344021.1. | 2021-11-14 00:00:00 .
APA 崔勍焱 , 王军 , 鲍晓军 , 王廷海 , 朱海波 , 王婵 . 一种亲油型Fe基悬浮床加氢裂化催化剂的制备方法 : CN202111344021.1. | 2021-11-14 00:00:00 .
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一种Ti掺杂Fe氧化物渣油悬浮床加氢裂化催化剂及其制备方法和应用 incoPat
专利 | 2022-03-10 00:00:00 | CN202210231862.X
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本发明属于石油加工技术领域,具体涉及一种Ti掺杂Fe氧化物催化剂及其制备方法和在渣油悬浮床加氢裂化中的应用。采用无机铁源和无机钛源,以氨水或氢氧化钠溶液为沉淀剂,采用共沉淀法,制备出一种性能良好的Fe基渣油悬浮床加氢裂化催化剂。本发明合成工艺绿色简单,操作方便,成本低廉,所得催化剂具有介孔结构,相比于未加入Ti源的催化剂,具有更大的孔容和比表面积,仅需较少的用量即可在渣油悬浮床加氢裂化反应中表现出良好的应用效果,显著提高渣油加氢裂化产品的质量,具有良好的工业化应用前景。

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GB/T 7714 鲍晓军 , 钱叶归 , 崔勍焱 et al. 一种Ti掺杂Fe氧化物渣油悬浮床加氢裂化催化剂及其制备方法和应用 : CN202210231862.X[P]. | 2022-03-10 00:00:00 .
MLA 鲍晓军 et al. "一种Ti掺杂Fe氧化物渣油悬浮床加氢裂化催化剂及其制备方法和应用" : CN202210231862.X. | 2022-03-10 00:00:00 .
APA 鲍晓军 , 钱叶归 , 崔勍焱 , 王廷海 , 岳源源 , 朱海波 . 一种Ti掺杂Fe氧化物渣油悬浮床加氢裂化催化剂及其制备方法和应用 : CN202210231862.X. | 2022-03-10 00:00:00 .
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一种轻质烷烃低温异构化催化剂及其制备方法和应用 incoPat
专利 | 2022-03-08 00:00:00 | CN202210218300.1
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本发明提供一种轻质烷烃低温异构化催化剂及其制备方法和应用,该催化剂是一种具有多个酸性位点且具有产物分布改善功能的轻质烷烃低温异构化催化剂,该催化剂是以阳离子部分含有多个季铵氮原子的季铵盐卤化物为中间体,然后与Lewis酸反应形成具有多个酸性位点的离子液体催化剂。本发明提供的催化剂具有多个酸性位点,可在低温不需添加引发剂的作用下高效催化轻质烷烃异构化反应,具有较高的目标产物选择性,可减少催化剂用量,降低轻质烷烃异构化成本,提高经济效益,具有较好的工业化前景和使用价值。

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GB/T 7714 白正帅 , 潘情 , 鲍晓军 et al. 一种轻质烷烃低温异构化催化剂及其制备方法和应用 : CN202210218300.1[P]. | 2022-03-08 00:00:00 .
MLA 白正帅 et al. "一种轻质烷烃低温异构化催化剂及其制备方法和应用" : CN202210218300.1. | 2022-03-08 00:00:00 .
APA 白正帅 , 潘情 , 鲍晓军 , 朱海波 , 汤育欣 , 崔勍焱 et al. 一种轻质烷烃低温异构化催化剂及其制备方法和应用 : CN202210218300.1. | 2022-03-08 00:00:00 .
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一种用于移动床的低碳烷烃脱氢催化剂的制备方法 incoPat
专利 | 2022-03-28 00:00:00 | CN202210309660.2
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本发明公开了一种用于移动床的低碳烷烃脱氢催化剂的制备方法,其是通过pH摆动法制备拟薄水铝石,并在制备过程中掺入Sn,然后以该拟薄水铝石为原料,将其经胶溶形成铝溶胶后,在其中加入酚醛树脂的前驱物,合成含Sn的氧化铝球型载体,再通过浸渍法在其上负载Pt,从而合成出移动床专用的低碳烷烃脱氢催化剂。本发明制备得到的催化剂球型度好、粒径分布均匀(平均粒径1.7 mm)、强度高、金属组分分散性好,可满足丙烷脱氢移动床的应用需求。

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GB/T 7714 朱海波 , 魏鼎 , 鲍晓军 et al. 一种用于移动床的低碳烷烃脱氢催化剂的制备方法 : CN202210309660.2[P]. | 2022-03-28 00:00:00 .
MLA 朱海波 et al. "一种用于移动床的低碳烷烃脱氢催化剂的制备方法" : CN202210309660.2. | 2022-03-28 00:00:00 .
APA 朱海波 , 魏鼎 , 鲍晓军 , 王廷海 , 岳源源 . 一种用于移动床的低碳烷烃脱氢催化剂的制备方法 : CN202210309660.2. | 2022-03-28 00:00:00 .
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