A closed-loop ammonium salt system for recovery of high-purity lead tetroxide product from spent lead-acid battery paste

Mingyang Li; Jiakuan Yang; Sha Liang; Junxiong Wang; Peiyuan Zhang; Wenhao Yu; Jingping Hu; Keke Xiao; Huijie Hou; Bingchuan Liu; R. Vasant Kumar

doi:10.1016/j.jclepro.2019.119488

A closed-loop ammonium salt system for recovery of high-purity lead tetroxide product from spent lead-acid battery paste

Mingyang Li, Jiakuan Yang^*, Sha Liang, Junxiong Wang, Peiyuan Zhang, Wenhao Yu, Jingping Hu, Keke Xiao, Huijie Hou, Bingchuan Liu, R. Vasant Kumar

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

25 Scopus citations

Abstract

Hydrometallurgical process for recovery of spent lead-acid battery paste shows great advantages in reducing SO₂ and lead particulates emissions than traditional pyrometallurgical process. However, the hydrometallurgical process usually has drawbacks of high consumption of chemical reagents and difficulty in removing impurities (especially Fe and Ba elements) from the recovered product. In this paper, a closed-loop ammonium salt system is proposed for spent lead-acid battery paste recovery. Both recirculation of leaching reagents and preparation of low-impurity recovered products have been realized. The spent lead paste is first leached by a mixed solution of ammonium acetate, acetic acid and hydrogen peroxide. After filtration, the separated lead acetate solution is reacted with ammonium carbonate to generate lead carbonate via precipitation process. The impurity elements are efficiently removed by pH control and complexation between acetate ions and impurity elements in the leaching and precipitation processes. The soluble SO₄ ²⁻ separated from the precipitation process is removed by adding barium acetate to generate solid BaSO₄ by-product. At the same time, the regenerated ammonium acetate filtrate is separated and re-used in the next-round leaching process in order to realize a closed-loop process. In the 5th round of filtrate recirculation processes, the leaching ratio of lead is maintained at levels higher than 92.7 wt%. Furthermore, high-purity lead tetroxide is prepared by calcination of lead carbonate in air at 450 °C. The contents of Fe and Ba in the final recovered lead tetroxide product are as low as 2.7 and 5.2 mg/kg, respectively. The recovered lead tetroxide product meets the specifications for use as an additive in the positive active materials for making a new lead-acid battery. This study provides a feasible technology for high-value utilization of spent lead paste.

Original language	English
Article number	119488
Journal	Journal of Cleaner Production
Volume	250
DOIs	https://doi.org/10.1016/j.jclepro.2019.119488
State	Published - 20 Mar 2020
Externally published	Yes

Keywords

Ammonium salt system
Filtrate recirculation
Impurity elements
Lead tetroxide
Spent lead-acid battery paste

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.jclepro.2019.119488

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@article{87dcca228b03401fa573a1c742a41809,

title = "A closed-loop ammonium salt system for recovery of high-purity lead tetroxide product from spent lead-acid battery paste",

abstract = "Hydrometallurgical process for recovery of spent lead-acid battery paste shows great advantages in reducing SO2 and lead particulates emissions than traditional pyrometallurgical process. However, the hydrometallurgical process usually has drawbacks of high consumption of chemical reagents and difficulty in removing impurities (especially Fe and Ba elements) from the recovered product. In this paper, a closed-loop ammonium salt system is proposed for spent lead-acid battery paste recovery. Both recirculation of leaching reagents and preparation of low-impurity recovered products have been realized. The spent lead paste is first leached by a mixed solution of ammonium acetate, acetic acid and hydrogen peroxide. After filtration, the separated lead acetate solution is reacted with ammonium carbonate to generate lead carbonate via precipitation process. The impurity elements are efficiently removed by pH control and complexation between acetate ions and impurity elements in the leaching and precipitation processes. The soluble SO4 2− separated from the precipitation process is removed by adding barium acetate to generate solid BaSO4 by-product. At the same time, the regenerated ammonium acetate filtrate is separated and re-used in the next-round leaching process in order to realize a closed-loop process. In the 5th round of filtrate recirculation processes, the leaching ratio of lead is maintained at levels higher than 92.7 wt%. Furthermore, high-purity lead tetroxide is prepared by calcination of lead carbonate in air at 450 °C. The contents of Fe and Ba in the final recovered lead tetroxide product are as low as 2.7 and 5.2 mg/kg, respectively. The recovered lead tetroxide product meets the specifications for use as an additive in the positive active materials for making a new lead-acid battery. This study provides a feasible technology for high-value utilization of spent lead paste.",

keywords = "Ammonium salt system, Filtrate recirculation, Impurity elements, Lead tetroxide, Spent lead-acid battery paste",

author = "Mingyang Li and Jiakuan Yang and Sha Liang and Junxiong Wang and Peiyuan Zhang and Wenhao Yu and Jingping Hu and Keke Xiao and Huijie Hou and Bingchuan Liu and Kumar, {R. Vasant}",

note = "Publisher Copyright: {\textcopyright} 2019 Elsevier Ltd",

year = "2020",

month = mar,

day = "20",

doi = "10.1016/j.jclepro.2019.119488",

language = "英语",

volume = "250",

journal = "Journal of Cleaner Production",

issn = "0959-6526",

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TY - JOUR

T1 - A closed-loop ammonium salt system for recovery of high-purity lead tetroxide product from spent lead-acid battery paste

AU - Li, Mingyang

AU - Yang, Jiakuan

AU - Liang, Sha

AU - Wang, Junxiong

AU - Zhang, Peiyuan

AU - Yu, Wenhao

AU - Hu, Jingping

AU - Xiao, Keke

AU - Hou, Huijie

AU - Liu, Bingchuan

AU - Kumar, R. Vasant

PY - 2020/3/20

Y1 - 2020/3/20

N2 - Hydrometallurgical process for recovery of spent lead-acid battery paste shows great advantages in reducing SO2 and lead particulates emissions than traditional pyrometallurgical process. However, the hydrometallurgical process usually has drawbacks of high consumption of chemical reagents and difficulty in removing impurities (especially Fe and Ba elements) from the recovered product. In this paper, a closed-loop ammonium salt system is proposed for spent lead-acid battery paste recovery. Both recirculation of leaching reagents and preparation of low-impurity recovered products have been realized. The spent lead paste is first leached by a mixed solution of ammonium acetate, acetic acid and hydrogen peroxide. After filtration, the separated lead acetate solution is reacted with ammonium carbonate to generate lead carbonate via precipitation process. The impurity elements are efficiently removed by pH control and complexation between acetate ions and impurity elements in the leaching and precipitation processes. The soluble SO4 2− separated from the precipitation process is removed by adding barium acetate to generate solid BaSO4 by-product. At the same time, the regenerated ammonium acetate filtrate is separated and re-used in the next-round leaching process in order to realize a closed-loop process. In the 5th round of filtrate recirculation processes, the leaching ratio of lead is maintained at levels higher than 92.7 wt%. Furthermore, high-purity lead tetroxide is prepared by calcination of lead carbonate in air at 450 °C. The contents of Fe and Ba in the final recovered lead tetroxide product are as low as 2.7 and 5.2 mg/kg, respectively. The recovered lead tetroxide product meets the specifications for use as an additive in the positive active materials for making a new lead-acid battery. This study provides a feasible technology for high-value utilization of spent lead paste.

AB - Hydrometallurgical process for recovery of spent lead-acid battery paste shows great advantages in reducing SO2 and lead particulates emissions than traditional pyrometallurgical process. However, the hydrometallurgical process usually has drawbacks of high consumption of chemical reagents and difficulty in removing impurities (especially Fe and Ba elements) from the recovered product. In this paper, a closed-loop ammonium salt system is proposed for spent lead-acid battery paste recovery. Both recirculation of leaching reagents and preparation of low-impurity recovered products have been realized. The spent lead paste is first leached by a mixed solution of ammonium acetate, acetic acid and hydrogen peroxide. After filtration, the separated lead acetate solution is reacted with ammonium carbonate to generate lead carbonate via precipitation process. The impurity elements are efficiently removed by pH control and complexation between acetate ions and impurity elements in the leaching and precipitation processes. The soluble SO4 2− separated from the precipitation process is removed by adding barium acetate to generate solid BaSO4 by-product. At the same time, the regenerated ammonium acetate filtrate is separated and re-used in the next-round leaching process in order to realize a closed-loop process. In the 5th round of filtrate recirculation processes, the leaching ratio of lead is maintained at levels higher than 92.7 wt%. Furthermore, high-purity lead tetroxide is prepared by calcination of lead carbonate in air at 450 °C. The contents of Fe and Ba in the final recovered lead tetroxide product are as low as 2.7 and 5.2 mg/kg, respectively. The recovered lead tetroxide product meets the specifications for use as an additive in the positive active materials for making a new lead-acid battery. This study provides a feasible technology for high-value utilization of spent lead paste.

KW - Ammonium salt system

KW - Filtrate recirculation

KW - Impurity elements

KW - Lead tetroxide

KW - Spent lead-acid battery paste

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U2 - 10.1016/j.jclepro.2019.119488

DO - 10.1016/j.jclepro.2019.119488

M3 - 文章

AN - SCOPUS:85076249993

SN - 0959-6526

VL - 250

JO - Journal of Cleaner Production

JF - Journal of Cleaner Production

M1 - 119488

ER -

A closed-loop ammonium salt system for recovery of high-purity lead tetroxide product from spent lead-acid battery paste

Abstract

Keywords

UN SDGs

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