Reliable, environmentally friendly method for the recycling of spent Ag/α-Al2O3 catalysts using (NH4)2Ce(NO3)6

doi:10.1016/j.cjche.2018.04.018

Chin.J.Chem.Eng. ›› 2018, Vol. 26 ›› Issue (10): 2169-2175.DOI: 10.1016/j.cjche.2018.04.018

• Energy, Resources and Environmental Technology • Previous Articles Next Articles

Reliable, environmentally friendly method for the recycling of spent Ag/α-Al₂O₃ catalysts using (NH₄)₂Ce(NO₃)₆

Xulong Dong^1,2,3, Jian Li^1,2,3, Qinggui Xiao^2,3, Hui Zhang^2,3, Tao Qi^2,3

1 University of Chinese Academy of Sciences, Beijing 100049, China;
2 National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Institute of Process, Chinese Academy of Sciences, Beijing 100190, China;
3 Key Laboratory of Green Process and Engineering, Institute of Process, Chinese Academy of Sciences, Beijing 100190, China

Received:2017-12-29 Revised:2018-04-07 Online:2018-11-14 Published:2018-10-28
Contact: Hui Zhang,E-mail addresses:zhanghv@ipe.ac.cn;Tao Qi,E-mail addresses:tqgreen@home.ipe.ac.cn
Supported by:
Supported by the Key Research Program of Frontier Sciences of CAS (QYZDJ-SSWJSC021), the Science and Technology Cooperation for Yunnan Provinces and CAS (2016IB002), Science and Technology Service Network Initiative of CAS (KFJ-SW-STS-148), and National Natural Science Foundation of China (21506233, 51402303, 21606241, 51374191).

Reliable, environmentally friendly method for the recycling of spent Ag/α-Al₂O₃ catalysts using (NH₄)₂Ce(NO₃)₆

Xulong Dong^1,2,3, Jian Li^1,2,3, Qinggui Xiao^2,3, Hui Zhang^2,3, Tao Qi^2,3

1 University of Chinese Academy of Sciences, Beijing 100049, China;
2 National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Institute of Process, Chinese Academy of Sciences, Beijing 100190, China;
3 Key Laboratory of Green Process and Engineering, Institute of Process, Chinese Academy of Sciences, Beijing 100190, China

通讯作者: Hui Zhang,E-mail addresses:zhanghv@ipe.ac.cn;Tao Qi,E-mail addresses:tqgreen@home.ipe.ac.cn
基金资助:
Supported by the Key Research Program of Frontier Sciences of CAS (QYZDJ-SSWJSC021), the Science and Technology Cooperation for Yunnan Provinces and CAS (2016IB002), Science and Technology Service Network Initiative of CAS (KFJ-SW-STS-148), and National Natural Science Foundation of China (21506233, 51402303, 21606241, 51374191).

Abstract

Abstract: Traditionally, Ag-containing solid wastes are leached by nitric acid in order to recycle the noble metal. However, the huge amounts of emission of toxic nitrogen oxides demand the development of a new method for silver recycling. Recently, considering the Ce(IV) solution could be regenerated with electrolyzation method, our group invented a novel environmentally friendly process by using Ce(IV) as the oxidant to dissolve silver from the spent Ag/α-Al₂O₃ catalysts without NO_x emission. To find out the optimal parameters, in this work, the leaching reaction was thoroughly investigated with respect to the temperature, oxidant and HNO₃ concentrations, stirring speed, and time. The optimized leaching reaction gave the leaching silver rate 99.8% in 1 h. The kinetic plots suggested a shrinking core model with the internal diffusion-controlled process and the activation energy of 38.83 kJ·mol^-1. The order in which the experimental conditions influence the reaction was determined through orthogonal analysis:temperature > oxidant concentration > HNO₃ concentration > stirring speed.

Key words: Cerium ammonium nitrate (CAN), Silver, Spent catalyst, Leaching, Kinetics

摘要： Traditionally, Ag-containing solid wastes are leached by nitric acid in order to recycle the noble metal. However, the huge amounts of emission of toxic nitrogen oxides demand the development of a new method for silver recycling. Recently, considering the Ce(IV) solution could be regenerated with electrolyzation method, our group invented a novel environmentally friendly process by using Ce(IV) as the oxidant to dissolve silver from the spent Ag/α-Al₂O₃ catalysts without NO_x emission. To find out the optimal parameters, in this work, the leaching reaction was thoroughly investigated with respect to the temperature, oxidant and HNO₃ concentrations, stirring speed, and time. The optimized leaching reaction gave the leaching silver rate 99.8% in 1 h. The kinetic plots suggested a shrinking core model with the internal diffusion-controlled process and the activation energy of 38.83 kJ·mol^-1. The order in which the experimental conditions influence the reaction was determined through orthogonal analysis:temperature > oxidant concentration > HNO₃ concentration > stirring speed.

关键词: Cerium ammonium nitrate (CAN), Silver, Spent catalyst, Leaching, Kinetics

Xulong Dong, Jian Li, Qinggui Xiao, Hui Zhang, Tao Qi. Reliable, environmentally friendly method for the recycling of spent Ag/α-Al₂O₃ catalysts using (NH₄)₂Ce(NO₃)₆[J]. Chin.J.Chem.Eng., 2018, 26(10): 2169-2175.

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Reliable, environmentally friendly method for the recycling of spent Ag/α-Al₂O₃ catalysts using (NH₄)₂Ce(NO₃)₆

Reliable, environmentally friendly method for the recycling of spent Ag/α-Al₂O₃ catalysts using (NH₄)₂Ce(NO₃)₆

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