Gas-phase catalysis of coal fast pyrolysis volatiles over acid, base and acid-base composite catalysts and the catalysts coking behavior

被引:0
作者
Wang, Jing-Xian [1 ,2 ]
Zou, Xuan-Jie [1 ,2 ]
Yang, Yu-Gui [1 ,2 ]
Xu, Wen-Long [1 ,2 ]
Shang, Yan-Chao [1 ,2 ]
Wang, Cheng-Biao [1 ,2 ]
Zong, Pei-Jie [1 ,2 ]
Yang, Yi-Nan [1 ,2 ]
Wang, Da-Meng [1 ,2 ]
Wang, Ning [1 ,2 ]
Qiao, Ying-Yun [1 ,2 ]
Tian, Yuan-Yu [1 ,2 ]
机构
[1] China Univ Petr East China, State Key Lab Heavy Oil Proc, Qingdao 266580, Shandong, Peoples R China
[2] Shandong Engn & Technol Res Ctr High Carbon Energy, Qingdao 266590, Shandong, Peoples R China
关键词
Coal; Fast pyrolysis; Catalytic upgrading; Acid-base catalysis; Coke deposition; HIERARCHICAL HZSM-5; AROMATIC PRODUCTS; METAL-OXIDES; BIO-OIL; LIGNITE; KETONIZATION; GASIFICATION; REGENERATION; ENHANCEMENT; SAWDUST;
D O I
10.1016/j.jaap.2025.107068
中图分类号
O65 [分析化学];
学科分类号
070302 ; 081704 ;
摘要
The gas-phase catalytic upgrading of coal rapid pyrolysis volatiles is a promising strategy for achieving high-value utilization. The catalytic reforming characteristics of coal rapid pyrolysis volatiles over solid base catalyst (calcium aluminate, AlCa), acid catalyst (HZSM-5, Z5), and acid-base composite catalyst (AlCa-Z5) were investigated using a falling bed reactor. The composition and properties of coke deposits on various catalysts were systematically compared and evaluated using NH4/CO2-TPD, XPS, Raman spectroscopy, and temperature programmed oxidation (TPO). The findings indicate that AlCa and Z5 markedly increased olefins and aromatics in tar, respectively, and the AlCa-Z5 elevated olefins, aromatics and phenols to over 70 %. The coke mainly deposited on strongly basic and acidic sites, predominantly blocking the 2-6, 1-2, and 0-6 nm pore channels of the AlCa, Z5, and AlCa-Z5 catalysts, respectively. AlCa formed less catalytic coke than the Z5 (48.76 vs. 60.09 %), although the coke graphitization and particle size were greater owing to its exceptional dehydrogenation properties. Specifically, the graphitization and particle size of coke formed on AlCa-Z5 were remarkably reduced. The oxidative weight loss temperature of thermal coke is around 450 degrees C, while the catalytic coke on AlCa reaches up to 720 degrees C, over 100 degrees C higher than that of Z5. The CC/C-C structures (>80 %) dominate in coke, exhibiting more O-CO on AlCa and more C-O on Z5. The research results support the advancement and industrialization of coal hierarchical pyrolysis gas-phase catalytic cracking technology.
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页数:10
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