Facile molybdenum and aluminum recovery from spent hydrogenation catalyst

doi:10.1016/j.cjche.2024.01.006

中国化学工程学报 ›› 2024, Vol. 69 ›› Issue (5): 72-78.DOI: 10.1016/j.cjche.2024.01.006

Facile molybdenum and aluminum recovery from spent hydrogenation catalyst

Zhenhui Lv^1,2, Jianan Li¹, Dong Xue², Tao Yang², Gang Wang², Chong Peng¹

1. State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China;
2. Dalian Research Institute of Petroleum and Petrochemicals, SINOPEC, Dalian 116041, China

收稿日期:2023-08-01 修回日期:2024-01-20 出版日期:2024-05-28 发布日期:2024-07-01
通讯作者: Chong Peng,E-mail:pengchong@dlut.edu.cn
基金资助:
This work was supported by grants from the National Key Research and Development Program of China (2023YE41507601), the National Natural Science Foundation of China (22122807, 22378038), the Fundamental Research Funds for the Central Universities (DUT23RC(3)044), and State Key Laboratory of Heavy Oil Processing, China University of Petroleum (WX20230149).

Facile molybdenum and aluminum recovery from spent hydrogenation catalyst

Zhenhui Lv^1,2, Jianan Li¹, Dong Xue², Tao Yang², Gang Wang², Chong Peng¹

1. State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China;
2. Dalian Research Institute of Petroleum and Petrochemicals, SINOPEC, Dalian 116041, China

Received:2023-08-01 Revised:2024-01-20 Online:2024-05-28 Published:2024-07-01
Contact: Chong Peng,E-mail:pengchong@dlut.edu.cn
Supported by:
This work was supported by grants from the National Key Research and Development Program of China (2023YE41507601), the National Natural Science Foundation of China (22122807, 22378038), the Fundamental Research Funds for the Central Universities (DUT23RC(3)044), and State Key Laboratory of Heavy Oil Processing, China University of Petroleum (WX20230149).

摘要/Abstract

摘要： Industrial catalyst waste has emerged as a hazardous pollutant that requires safe and proper disposal after the unloading process. Finding a valuable and sustainable strategy for its treatment is a significant challenge compared to traditional methods. In this study, we present a facile method for the recovery of molybdenum and aluminum contents from spent Mo-Ni/Al₂O₃ hydrogenation catalysts through crystallization separation and coprecipitation. Furthermore, the recovered molybdenum and aluminum are utilized as active metals and carriers for the preparation of new catalysts. Their properties were thoroughly analyzed and investigated using various characterization techniques. The hydrogenation activity of these newly prepared catalysts was evaluated on a fixed-bed small-scale device and compared with a reference catalyst synthesized from commercial raw reagents. Finally, the hydrogenation activity of the catalysts was further assessed by using the entire distillate oil of coal liquefaction as the raw oil, specifically focusing on denitrogenation and aromatic saturation. This work not only offers an effective solution for recycling catalysts but also promotes sustainable development.

关键词: Waste treatment, Alumina, Hydrogenation, Catalyst, Crystallization, Precipitation

Abstract: Industrial catalyst waste has emerged as a hazardous pollutant that requires safe and proper disposal after the unloading process. Finding a valuable and sustainable strategy for its treatment is a significant challenge compared to traditional methods. In this study, we present a facile method for the recovery of molybdenum and aluminum contents from spent Mo-Ni/Al₂O₃ hydrogenation catalysts through crystallization separation and coprecipitation. Furthermore, the recovered molybdenum and aluminum are utilized as active metals and carriers for the preparation of new catalysts. Their properties were thoroughly analyzed and investigated using various characterization techniques. The hydrogenation activity of these newly prepared catalysts was evaluated on a fixed-bed small-scale device and compared with a reference catalyst synthesized from commercial raw reagents. Finally, the hydrogenation activity of the catalysts was further assessed by using the entire distillate oil of coal liquefaction as the raw oil, specifically focusing on denitrogenation and aromatic saturation. This work not only offers an effective solution for recycling catalysts but also promotes sustainable development.

Key words: Waste treatment, Alumina, Hydrogenation, Catalyst, Crystallization, Precipitation

Zhenhui Lv, Jianan Li, Dong Xue, Tao Yang, Gang Wang, Chong Peng. Facile molybdenum and aluminum recovery from spent hydrogenation catalyst[J]. 中国化学工程学报, 2024, 69(5): 72-78.

Zhenhui Lv, Jianan Li, Dong Xue, Tao Yang, Gang Wang, Chong Peng. Facile molybdenum and aluminum recovery from spent hydrogenation catalyst[J]. Chinese Journal of Chemical Engineering, 2024, 69(5): 72-78.

参考文献

[1] H.M. Sun, J.T. Yang, H.W. Zhang, Q. Yang, S.Z. Wu, Y.X. Wang, H.B. Zhu, Y.Y. Yue, T.H. Wang, P. Yuan, Hierarchical flower-like NiCu/SiO₂ bimetallic catalysts with enhanced catalytic activity and stability for petroleum resin hydrogenation, Ind. Eng. Chem. Res. 60(15)(2021)5432-5442.
[2] J.J. Li, Z.Q. Zhang, G.F. Qin, X.D. Tang, C.X. Xiang, Fe/HZSM-5 catalytic pyrolysis cellulose as hydrogen donor for the upgrading of heavy crude oil by one-pot process, Fuel 298(2021)120880.
[3] R. Saab, K. Polychronopoulou, L.X. Zheng, S. Kumar, A. Schiffer, Synthesis and performance evaluation of hydrocracking catalysts:a review, J. Ind. Eng. Chem. 89(2020)83-103.
[4] M. Marafi, A. Stanislaus, Spent catalyst waste management:a review, Resour. Conserv. Recycl. 52(6)(2008)859-873.
[5] H. Al-Sheeha, M. Marafi, V. Raghavan, M.S. Rana, Recycling and recovery routes for spent hydroprocessing catalyst waste, Ind. Eng. Chem. Res. 52(36)(2013)12794-12801.
[6] A. Tanimu, K. Alhooshani, Advanced hydrodesulfurization catalysts:a review of design and synthesis, Energy Fuels 33(4)(2019)2810-2838.
[7] S. Bag, A.F. Gaudette, M.E. Bussell, M.G. Kanatzidis, Spongy chalcogels of non-platinum metals act as effective hydrodesulfurization catalysts, Nat. Chem. 1(3)(2009)217-224.
[8] Y.C. Lai, W.J. Lee, K.L. Huang, C.M. Wu, Metal recovery from spent hydrodesulfurization catalysts using a combined acid-leaching and electrolysis process, J. Hazard. Mater. 154(1-3)(2008)588-594.
[9] H. Wu, S.Y. Duan, D.D. Liu, X.F. Guo, A.F. Yi, H.R. Li, Recovery of nickel and molybdate from ammoniacal leach liquor of spent hydrodesulfurization catalyst using LIX84 extraction, Sep. Purif. Technol. 269(2021)118750.
[10] M. Marafi, A. Stanislaus, Waste catalyst utilization:extraction of valuable metals from spent hydroprocessing catalysts by ultrasonic-assisted leaching with acids, Ind. Eng. Chem. Res. 50(16)(2011)9495-9501.
[11] N.M. Al-Mansi, M.N.M. Abdel, Recovery of nickel oxide from spent catalyst, Waste Manag. 22(1)(2002)85-90.
[12] J.L. Liu, C.Y. Wang, X.R. Wang, C. Zhao, H.Q. Li, G.Y. Zhu, J.B. Zhang, Reconstruction and recovery of anatase TiO₂ from spent selective catalytic reduction catalyst by NaOH hydrothermal method, Chin. J. Chem. Eng. 60(2023)53-60.
[13] S.P. Barik, K.H. Park, P.K. Parhi, J.T. Park, C.W. Nam, Extraction of metal values from waste spent petroleum catalyst using acidic solutions, Sep. Purif. Technol. 101(2012)85-90.
[14] J.Z. Wang, S.N. Wang, A. Olayiwola, N. Yang, B. Liu, J.J. Weigand, M. Wenzel, H. Du, Recovering valuable metals from spent hydrodesulfurization catalyst via blank roasting and alkaline leaching, J. Hazard. Mater. 416(2021)125849.
[15] G.H. Li, D.P. Shi, H. Sun, Q.Z. Bu, J. Luo, M.J. Rao, Z.W. Peng, T. Jiang, Effects and mechanisms of ternary solution of NaOH-Na₂CO₃-Na₂SO₄ on the recovery of molybdenum from residues containing multiple molybdates, Sep. Purif. Technol. 248(2020)117059.
[16] S.J. Zhao, Z.Q. Liao, Y. Xie, X.S. Li, Y.Y. Dai, Z.R. Li, M.Y. Wang, Extraction of molybdenum from spent HDS catalyst by pressure alkaline leaching, J. Sustain. Metall. 7(3)(2021)773-782.
[17] Y.W. Wang, Z.Q. Wang, J.J. Huang, Y.T. Fang, Improved catalyst recovery combined with extracting alumina from Na₂CO₃-catalyzed gasification ash of a high-aluminium coal char, Fuel 234(2018)101-109.
[18] M. Marafi, M.S. Rana, H. Al-Sheeha, The recovery of valuable metals and recycling of alumina from a waste spent hydroprocessing catalyst:Extraction with Na saltsWIT Transactions on Ecology and the Environment,Waste Management and the Environment VII. Ancona, Italy, WIT Press, Southampton, UK, 2014.
[19] E. Kordouli, B. Pawelec, K. Bourikas, C. Kordulis, J.L.G. Fierro, A. Lycourghiotis, Mo promoted Ni-Al₂O₃ co-precipitated catalysts for green diesel production, Appl. Catal. B Environ. 229(2018)139-154.
[20] A. Siahvashi, D. Chesterfield, A.A. Adesina, Nonoxidative and oxidative propane dehydrogenation over bimetallic Mo-Ni/Al₂O₃ catalyst, Ind. Eng. Chem. Res. 52(11)(2013)4017-4026.
[21] L. Qu, C.T. Li, G.M. Zeng, M.Y. Zhang, M.F. Fu, J.F. Ma, F.M. Zhan, D.Q. Luo, Support modification for improving the performance of MnO_x-CeO_y/γ-Al₂O₃ in selective catalytic reduction of NO by NH₃, Chem. Eng. J. 242(2014)76-85.
[22] J.M. Rynkowski, T. Paryjczak, M. Lenik, On the nature of oxidic nickel phases in NiO/γ-Al₂O₃ catalysts, Appl. Catal. A Gen. 106(1)(1993)73-82.
[23] C. Volkringer, H. Leclerc, J.C. Lavalley, T. Loiseau, G. Ferey, M. Daturi, A. Vimont, Infrared spectroscopy investigation of the acid sites in the metal-organic framework aluminum trimesate MIL-100(Al), J. Phys. Chem. C 116(9)(2012)5710-5719.
[24] A. Travert, C. Dujardin, F. Mauge, E. Veilly, S. Cristol, J.F. Paul, E. Payen, CO adsorption on CoMo and NiMo sulfide catalysts:a combined IR and DFT study, J. Phys. Chem. B 110(3)(2006)1261-1270.
[25] K. Hadjiivanov, H. Knozinger, M. Mihaylov, FTIR study of CO adsorption on Ni-ZSM-5, J. Phys. Chem. B 106(10)(2002)2618-2624.
[26] B.M. Vogelaar, N. Kagami, T.F. van der Zijden, A.D. van Langeveld, S. Eijsbouts, J.A. Moulijn, Relation between sulfur coordination of active sites and HDS activity for Mo and NiMo catalysts, J. Mol. Catal. A Chem. 309(1-2)(2009)79-88.
[27] Q.Y. Zhao, X.L. Hou, J.L. Wang, D.G. Cheng, F.Q. Chen, X.L. Zhan, Engineering specific Mo-O bond stretching to activate lattice oxygen in V-doped Bi₂MoO₆ for enhanced oxidative dehydrogenation of 1-butene, Ind. Eng. Chem. Res. 62(1)(2023)329-340.
[28] C.I. Vargas-Consuelos, M.A. Camacho-López, V.H. Ramos-Sanchez, O.A. Graeve, Phase and morphology control of hexagonal MoO₃ crystals via Na+interactions:a Raman spectroscopy study, J. Phys. Chem. C 127(27)(2023)13136-13148.
[29] B. Courcot, A.J. Bridgeman, Structural and vibrational study of[Mo₇O₂₄] ₆^-and[W₇O₂₄]₆^-, J. Phys. Chem. A 113(39)(2009)10540-10548.
[30] W.G. Klemperer, W. Shum, Synthesis and interconversion of the isomeric.alpha.-and.beta.-molybdate (Mo₈O₂64-) ions, J. Am. Chem. Soc. 98(25)(1976)8291-8293.
[31] C.H. Liu, Q. Wei, Y.S. Zhou, X.Y. Liu, K.X. Deng, W.B. Huang, H.R. Liu, Z.Q. Yu, A study on the role of Ti/Si atomic ratios in the hydrodenitrogenation activity of NiMo/TiO₂-SiO₂ catalyst, Fuel 338(2023)126922.
[32] A. Karmakar, K. Karthick, S.S. Sankar, S. Kumaravel, M. Ragunath, S. Kundu, Oxygen vacancy enriched NiMoO₄ nanorods via microwave heating:a promising highly stable electrocatalyst for total water splitting, J. Mater. Chem. A, 9(2021)11691-11704.

Facile molybdenum and aluminum recovery from spent hydrogenation catalyst

Facile molybdenum and aluminum recovery from spent hydrogenation catalyst

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