石油炼制与化工 ›› 2025, Vol. 56 ›› Issue (10): 63-77.
张承博,陈茜,王轶苇,黄婷婷
收稿日期:2025-02-12
修回日期:2025-06-06
出版日期:2025-10-12
发布日期:2025-10-09
通讯作者:
张承博
E-mail:546687121@qq.com
基金资助:
Received:2025-02-12
Revised:2025-06-06
Online:2025-10-12
Published:2025-10-09
Supported by:摘要: 采用十六烷基三甲基溴化铵(CTAB)辅助的醇铝水解法制备氧化铝的策略,成功制备出具有棒状形貌且优先暴露高能(111)晶面的载体γ-Al2O3-CT,该载体具有丰富的B酸位点和高的羟基密度。在醇铝水解的过程中,CTAB可以阻止勃姆石粒子的大量团聚;在水热过程中,表面活性剂可以作为结构导向剂定向调控棒状γ-Al2O3的形成。γ-Al2O3载体表面强烈的金属-载体相互作用可以诱导活性相的高度分散,丰富的酸性位点有利于促进加氢脱硫反应。通过X射线衍射、X射线光电子能谱、傅里叶变换红外光谱及吡啶吸附红外光谱等多种方法对催化剂物化性质进行表征,并对催化剂催化性能进行了评价。结果表明:使用CTAB制备的催化剂cat-CT在形貌、高能(111)晶面的暴露率、羟基强度以及硫化深度方面均优于同系列中其他催化剂,在二苯并噻吩的加氢脱硫反应中表现出优异的反应活性和路径选择性,显著优于同系列中其他催化剂。
张承博 陈茜 王轶苇 黄婷婷. 高能晶面γ-Al2O3载体的制备及其催化剂的柴油加氢脱硫性能[J]. 石油炼制与化工, 2025, 56(10): 63-77.
| [1] M. Lewandowski, A. Szymańska-Kolasa, C. Sayag, P. Beaunier, G. Djéga-Mariadassou, Atomic level characterization and sulfur resistance of unsupported W2C during dibenzothiophene hydrodesulfurization. Classical kinetic simulation of the reaction, Applied Catalysis B: Environmental, 144 (2014) 750-759. [2] C.J.H. Jacobsen, E. T?rnqvist, H. Tops?e, HDS, HDN and HYD activities and temperature‐programmed reduction of unsupported transition metal sulfides, Catalysis Letters, 63 (1999) 179-183. [3] S. Harris, R.R. Chianelli, Catalysis by transition metal sulfides: The relation between calculated electronic trends and HDS activity, Journal of Catalysis, 86 (1984) 400-412. [4] T.A. Pecoraro, R.R. Chianelli, Hydrodesulfurization catalysis by transition metal sulfides, Journal of Catalysis, 67 (1981) 430-445. [5] R.R. Chianelli, G. Berhault, P. Raybaud, S. Kasztelan, J. Hafner, H. Toulhoat, Periodic trends in hydrodesulfurization: In support of the Sabatier principle, Applied Catalysis A: General, 227 (2002) 83-96. [6] M.J. Ledoux, O. Michaux, G. Agostini, P. Panissod, The influence of sulfide structures on the hydrodesulfurization activity of carbon-supported catalysts, Journal of Catalysis, 102 (1986) 275-288. [7] A. López-Benítez, G. Berhault, L. Burel, A. Guevara-Lara, Novel NiW hydrodesulfurization catalysts supported on Sol-Gel Mn-Al2O3, Journal of Catalysis, 354 (2017) 197-212. [8] S. Shan, H. Liu, Y. Yue, G. Shi, X. Bao, Trimetallic WMoNi diesel ultra-deep hydrodesulfurization catalysts with enhanced synergism prepared from inorganic–organic hybrid nanocrystals, Journal of Catalysis, 344 (2016) 325-333. [9] E. Wang, Q. Li, M. Song, F. Yang, Y. Chen, G. Wang, L. Bing, Q. Zhang, F. Wang, D. Han, Melamine foam-supported CoMo catalysts with three-dimensional porous structure for effective hydrodesulfurization of thiophene, Fuel, 337 (2023) 127225. [10] Y. Xu, S. Liang, L. Sun, X. Hu, Y. Zhang, W. Lai, X. Yi, W. Fang, Management of γ-Alumina with high-efficient {111} external surfaces for HDS reactions, Catalysts, 10(11) 2020 1254. [11] M. Digne, P. Sautet, P. Raybaud, P. Euzen, H. Toulhoat, Use of DFT to achieve a rational understanding of acid–basic properties of γ-alumina surfaces, Journal of Catalysis, 226 (2004) 54-68. [12] W. Cai, S. Zhang, J. Lv, J. Chen, J. Yang, Y. Wang, X. Guo, L. Peng, W. Ding, Y. Chen, Y. Lei, Z. Chen, W. Yang, Z. Xie, Nanotubular gamma alumina with high-energy external surfaces: Synthesis and high performance for catalysis, ACS Catalysis, 7 (2017) 4083-4092. [13] J. Lv, D. Wang, L. Peng, X. Guo, W. Ding, W. Yang, Ethanol dehydration to ethylene over high-energy facets exposed gamma alumina, Catalysts, 13 (2023) 994. [14] W. Zhang, J. Zhao, L. Wang, G. Liu, D. Shen, H. Zhang, Crystal-facet effect of γ-Al2O3 on Fe–Al2O3 catalytic performance for the co-production of hydrogen and CNTs from catalytic reforming of toluene, International Journal of Hydrogen Energy, 58 (2024) 1466-1477. [15] H. Zhang, D. Zhu, S. Grasso, C. Hu, Tunable morphology of aluminum oxide whiskers grown by hydrothermal method, Ceramics International, 44 (2018) 14967-14973. [16] G. Shi, W. Han, P. Yuan, Y. Fan, X. Bao, Sulfided Mo/Al2O3 hydrodesulfurization catalyst prepared by ethanol-assisted chemical deposition method, Chinese Journal of Catalysis, 34 (2013) 659-666. [17] W. Wu, M. Zhu, D. Zhang, The role of solvent preparation in soft template assisted synthesis of mesoporous alumina, Microporous and Mesoporous Materials, 260 (2018) 9-16. [18] M. Sharbatdaran, M.M. Amini, A. Majdabadi, Effect of aluminium alkoxide with donor-functionalized group on texture and morphology of the alumina prepared by sol–gel processing, Materials Letters, 64 (2010) 503-505. [19] Y. Lin, L. Luo, Z. Yang, Y. Shi, G. Qian, C. Peng, Z. Lv, J. Zhang, X. Duan, Controlled engineering of high-purity pseudo-boehmite with large pore volume by aluminum alkoxide hydrolysis: Mechanistic understanding and reforming catalysis, Chemical Engineering Science, 298 (2024) 120372. [20] C. Bara, L. Plais, K. Larmier, E. Devers, M. Digne, A.-F. Lamic-Humblot, G.D. Pirngruber, X. Carrier, Aqueous-phase preparation of model HDS catalysts on planar alumina substrates: Support effect on Mo adsorption and sulfidation, Journal of the American Chemical Society, 137 (2015) 15915-15928. [21] J. Oh, T.W. Kim, K. Jeong, J.H. Park, Y.W. Suh, Enhanced activity and stability of a carbon-coated alumina-supported Pd catalyst in the dehydrogenation of a liquid organic hydrogen carrier, Perhydro 2-(n-methylbenzyl)Pyridine, ChemCatChem, 10 (2018) 3892-3900. [22] J. Wang, A.H. Lu, M. Li, W. Zhang, Y.S. Chen, D.X. Tian, W.C. Li, Thin porous alumina sheets as supports for stabilizing gold nanoparticles, ACS Nano, 7 (2013) 4902-4910. [23] C. Bara, A.F. Lamic-Humblot, E. Fonda, A.S. Gay, A.L. Taleb, E. Devers, M. Digne, G.D. Pirngruber, X. Carrier, Surface-dependent sulfidation and orientation of MoS2 slabs on alumina-supported model hydrodesulfurization catalysts, Journal of Catalysis, 344 (2016) 591-605. [24] J.P. Beaufils, Y. Barbaux, Détermination, par diffraction différentielle de neutrons, des faces cristallines exposées par des supports de catalyseurs en poudre, J. Chim. Phys., 78 (1981) 347-352. [25] P. Nortier, P. Fourre, A.B.M. Saad, O. Saur, J.C. Lavalley, Effects of crystallinity and morphology on the surface properties ofalumina, Applied Catalysis, 61 (1990) 141-160. [26] P. Steiner, E.A. Blekkan, Catalytic hydrodesulfurization of a light gas oil over a NiMo catalyst: kinetics of selected sulfur components, Fuel Processing Technology, 79 (2002) 1-12. [27] Z. Razavi Hesabi, H.R. Hafizpour, A. Simchi, An investigation on the compressibility of aluminum/nano-alumina composite powder prepared by blending and mechanical milling, Materials Science and Engineering: A, 454-455 (2007) 89-98. [28] Y. Yang, Y. Xu, B. Han, B. Xu, X. Liu, Z. Yan, Effects of synthetic conditions on the textural structure of pseudo-boehmite, Journal of Colloid and Interface Science, 469 (2016) 1-7. [29] T.A. Saleh, S.A. Al-Hammadi, A novel catalyst of nickel-loaded graphene decorated on molybdenum-alumina for the HDS of liquid fuels, Chemical Engineering Journal, 406 (2021) 125167. [30] A.L. Clauser, K.O. Sarfo, R. Giulian, C. Ophus, J. Ciston, L. árnadóttir, M.K. Santala, Characterization of the atomic-level structure of γ-alumina and (111) Pt/γ-alumina interfaces, Acta Materialia, 245 (2023) 118609. [31] J.A. Toledo-Antonio, M.A. Cortes-Jacome, J. Escobar-Aguilar, C. Angeles-Chavez, J. Navarrete-Bola?os, E. López-Salinas, Upgrading HDS activity of MoS2 catalysts by chelating thioglycolic acid to MoOx supported on alumina, Applied Catalysis B: Environmental, 213 (2017) 106-117. [32] A. Sahu, S.N. Steinmann, P. Raybaud, Genesis of MoS2 from model-Mo-oxide precursors supported on γ-alumina, Journal of Catalysis, 408 (2022) 303-315. [33] J. Lv, D. Wang, L. Peng, X. Guo, W. Ding, W. Yang, Ethanol dehydration to ethylene over high-energy facets exposed gamma alumina, Catalysts, 2023. [34] Y. Wan, P. Ma, H. Lu, J. Zhang, J. Wang, W. Fang, W. Song, Q. Zheng, W. Lai, External [111] facets on nanorod gamma alumina boosts catalytic reductive amination of carbonyl compound to primary amine, Journal of Catalysis, 429 (2024) 115285. [35] J. Reardon, A.K. Datye, A.G. Sault, Tailoring alumina surface chemistry for efficient use of supported MoS2, Journal of Catalysis, 173 (1998) 145-156. [36] Y. Zou, C. Xiao, X. Yang, Y. Wang, X. Kong, Z. Liu, C. Wang, A. Duan, C. Xu, X. Wang, Flower-like hierarchical TS-1/Al2O3 composite supported NiMo catalysts for efficient hydrodesulfurization of dibenzothiophenes, Journal of Catalysis, 435 (2024) 115576. [37] R. Selvaraj, K.R. Kalimuthu, V. Kalimuthu, A type-II MoS2/ZnO heterostructure with enhanced photocatalytic activity, Materials Letters, 243 (2019) 183-186. [38] Y. Xu, S. Liang, L. Sun, X. Hu, Y. Zhang, W. Lai, X. Yi, W. Fang, Management of γ-Alumina with High-Efficient {111} External Surfaces for HDS Reactions, Catalysts, 10 (2020) 1254. [39] P. Zheng, D. Hu, Q. Meng, C. Liu, X. Wang, J. Fan, A. Duan, C. Xu, Influence of support acidity on the HDS performance over β-SBA-16 and Al-SBA-16 substrates: A combined experimental and theoretical study, Energy & Fuels, 33 (2019) 1479-1488. [40] W. Wei, X. Zhang, X. Liu, R. Guo, B. Meng, G. Li, S. Ren, Q. Guo, B. Shen, Tuning effect of the zeolite br?nsted acidity on the FeZn bimetallic hydrodesulfurization catalyst, Energy & Fuels, 36 (2022) 527-538. [41] T. Wang, H. Shang, Q. Zhang, Adsorption behavior of thiophene on MoS2 under a microwave electric field via DFT and MD studies, Chemical Engineering Science, 228 (2020) 115950. [42] B. Liu, L. Liu, Y. Chai, J. Zhao, Y. Li, D. Liu, Y. Liu, C. Liu, Effect of sulfiding conditions on the hydrodesulfurization performance of the ex-situ presulfided CoMoS/γ-Al2O3 catalysts, Fuel, 234 (2018) 1144-1153. [43] A.V. Vutolkina, I.G. Baygildin, A.P. Glotov, K.A. Cherednichenko, A.L. Maksimov, E.A. Karakhanov, Dispersed Ni-Mo sulfide catalysts from water-soluble precursors for HDS of BT and DBT via in situ produced H2 under water gas shift conditions, Applied Catalysis B: Environmental, 282 (2021) 119616. [44] T. Huang, J. Xu, Y. Fan, Effects of concentration and microstructure of active phases on the selective hydrodesulfurization performance of sulfided CoMo/Al2O3 catalysts, Applied Catalysis B: Environmental, 220 (2018) 42-56. [45] J. Xu, C. Wen, S. He, Y. Fan, Ultradeep hydrodesulfurization of fuel over superior NiMoS phases constructed by a novel Ni(MoS4)2(C13H30N)2 precursor, Catalysis Science & Technology, 10 (2020) 6065-6075. [46] M. Digne, P. Sautet, P. Raybaud, P. Euzen, H. Toulhoat, Hydroxyl groups on γ-Alumina surfaces: a DFT study, Journal of Catalysis, 211 (2002) 1-5. [47] P. Raybaud, M. Digne, R. Iftimie, W. Wellens, P. Euzen, H. Toulhoat, Morphology and surface properties of boehmite (γ-AlOOH): a density functional theory study, Journal of Catalysis, 201 (2001) 236-246. |
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