Lanthanum and Nickel Recovery from Spent Catalyst using Citric Acid: Quantitative Performance Assessment using Response Surface Method

Himawan Tri Bayu Murti Petrus, Ardyanto Wijaya, Yusuf Iskandar, Danu Bratakusuma, Hendrik Setiawan, Wiratni Wiratni, Widi Astuti


Heavy metals and Rare earth elements (REEs) are nowadays being used widely in many industries from electronics to petroleum industries as catalysts. However, their disposal caused serious problems to the environment. With the sharp growth in its usage, there is a better way to use and utilize valuable metals from secondary sources such as their disposal rather than using new raw materials. The aim of this work is to study the potential of citric acid as a leaching agent to extract lanthanum and nickel in various acid concentration and leaching temperature. The raw material used in this work is spent catalyst from Pertamina Refinery Unit VI, Balongan, Indonesia. The spent catalyst is decarbonized with a heat treatment at 725°C for 10 minutes before the leaching process. The leaching process used 0.1; 1; and 2 M of citric acid with a varied temperature of 30, 60, and 80°C. The lanthanum recovery was calculated by comparing the mass percentage of lanthanum before leaching process and after leaching process using Energy Dispersive X-Ray Spectroscopy (EDX). The results were analyzed by response surface methodology (RSM) and are proved to be a reliable method to depict and analyze the leaching characteristics. The molarity of the citric acid is the most significant independent variables used in the research for lanthanum recovery response. However, based on the Pareto analysis result there are no significant variables that affect the recovery of nickel. The second order polynomial fitting model is also proved to be compatible with the response of lanthanum recovery but is less compatible with nickel recovery.


Leaching; Spent catalyst; Lanthanum; Nickel; Citric Acid


A. Isildar, J. van de Vossenberg, E. R. Rene, E. D. van Hullebusch, and P. N. L. Lens, “Two-step bioleaching of copper and gold from discarded printed circuit boards (PCB),” Waste Manag., vol. 57, pp. 149-157, 2016.

J. Li, P. Shi, Z. Wang, Y. Chen, and C. C. Chang, “A combined recovery process of metals in spent lithium-ion batteries,” Chemosphere, vol. 77, no. 8, pp. 1132-1136, 2009.

E. Alonso, A. M. Sherman, T. J. Wallington, M. P. Everson, F. R. Field, R. Roth, and R. E. Kirchain, “Evaluating rare earth element availability: A case with revolutionary demand from clean technologies,” Environ. Sci. Technol., vol. 46, pp. 3406-3414, 2012.

DOI: 10.1021/es203518d

H. Setiawan, H. T. B. M. Petrus, I. Perdana, "A kinetics study of acetic acid on cobalt leaching of spent LIBs: shrinking core model, " MATEC Web of Conferences, 2018, vol. 154, pp. 01033.

Z. Wangcheng, G. Yun, G. Xueqing, G. Yanglong, W. Yanqing, and L. Guanzhong, “Current status and perspectives of rare earth catalytic materials and catalysis,” Chinese J. Catal., vol. 35, pp. 1238-1250, 2014.

P. Dufresne, “Hydroprocessing catalysts regeneration and recycling,” Appl. Catal., vol. 322, pp. 67-75, 2007.

Z. Zhao, Z. Qiu, J. Yang, S. Lu, L. Chao, W. Zhang and Y. Xu, “Recovery of rare earth elements from spent fluid catalytic cracking catalysts using leaching and solvent extraction techniques,” Hydrometallurgy, vol. 167, pp. 183-188, 2017.

R. L. Thompson, T. Bank, E. Roth, and E. Granite, “Resolution of rare earth element interferences in fossil energy by-product samples using sector-field ICP-MS,” Fuel, vol. 185, pp. 94-101, 2016.

D. P. Sari, A. Tawfiequrahman, H. T. B. M. Petrus, F. R. Mufakir, W. Astuti, Y. Iskandar, dan D. Bratakusuma, "Valuable metals extraction from hydrocracking spent catalyst using citric acid," Seminar Nasional Teknik Kimia Kejuangan, 2018, pp. 1-4.

M. Hartono, M. A. Astrayudha, H. T. B. M. Petrus, W. Budhijanto and H. Sulistyo, "Lithium recovery of spent lithium ion battery using bioleaching from local sources microoraganism," Rasayan J.Chem., vol. 10, no. 3, pp. 897-903, 2017.

L. Jinxia, R. A. Verweij, and C. A. M. Van Gestel, “Lanthanum toxicity to fi ve different species of soil invertebrates in relation to availability in soil,” Chemosphere, vol. 193, pp. 412-420, 2018.

Abhilash, S. Sinha, M. K. Sinha, and B. D. Pandey, “Extraction of lanthanum and cerium from Indian red mud,” Int. J. Miner. Process., vol. 127, pp. 70-73, 2014.

S. Kuang, Z. Zhang, Y. Li, H. Wei, and W. Liao, “Extraction and separation of heavy rare earths from chloride medium by α-aminophosphonic acid HEHAPP,” J. Rare Earths, vol. 34, no. 3, pp. 304-310, 2017.

P. K. Parhi, K. H. Park, and G. Senanayake, “A kinetic study on hydrochloric acid leaching of nickel from Ni-Al2O3 spent catalyst,” J. Ind. Eng. Chem., vol. 19, no. 2, pp. 589-594, 2013.

W. Astuti, N. M. Prilitasari, Y. Iskandar, D. Bratakusuma, and H. T. B. M. Petrus, “Leaching behavior of lanthanum, nickel and iron from spent catalyst using inorganic acids,” IOP Conf. Ser. Mater. Sci. Eng., 2018, vol. 285, no. 1, pp. 012007.

K. C. Wanta, I. Perdana and H. T. B. M. Petrus, "Evaluation of shrinking core model in leaching process of pomalaa nickel laterite using citric acid as leachant at atmospheric conditions," IOP Conf. Ser. Mater. Sci. Eng., 2016, vol. 162, no. 1, pp. 012018.

W. Astuti W, T. Hirajima, K. Sasaki, and N. Okibe, "Comparison of effectiveness of citric acid and other acids in leaching of low-grade Indonesian saprolitic ores," Minerals Engineering, vol. 85, pp. 116, 2016.

W. Astuti, T. Hirajima, T. Sasaki, and N. Okibe, "Kinetics of nickel extraction from Indonesian saprolitic ore by citric acid leaching under atmospheric pressure," Minerals & Metallurgical Processing, vol. 32, pp. 176-185, 2015.

C. P. Faizul, C. Abdullah, B. Fazlul, and H. J. Noorina, “Extraction of silica from palm ash using organic acid leaching,” Key Eng. Mater., vol. 595, pp. 329-333, 2014.

I. C. Santos, A. P. G. O. N. Alves, C. S. Santos, M. Almeida, and M. H. Afonso, “Purification of metallurgical grade silicon by acid leaching,” Hydrometallurgy, vol. 23, pp. 237-246, 1990.

M. A. Bezerra, R. E. Santelli, E. P. Oliveira, L. S. Villar, and L. A. Escaleira, “Response surface methodology (RSM) as a tool for optimization in analytical chemistry,” Talanta, vol. 76, no. 5, pp. 965-977, 2008.

N. Vedaraman, K. V. Sandhya, N. R. .B. Charukesh, B. Venkatakrishnan, K. Haribabu, M. R. Sridharan, and R. Nagarajan, “Ultrasonic extraction of natural dye from rubia cordifolia, optimisation using response surface methodology (RSM) & comparison with artificial neural network (ANN) model and its dyeing properties on different substrates,” Chem. Eng. Process. Process Intensif., vol. 114, pp. 46-54, 2017.

Shriver and Atkins, Inorganic Chemistry, 5th ed., Great Britain by Oxford University Press New York, 2010.

Copyright (c) 2018 Metalurgi
Creative Commons License
This work is licensed under a Creative Commons Attribution-NonCommercial-ShareAlike 4.0 International License.


  • There are currently no refbacks.