<p>Spent lead paste (SLP) presents a major recycling challenge in lead-acid battery treatment due to its insoluble lead compounds. This study develops an innovative and environmentally sustainable approach by integrating (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub>-NH<sub>3</sub>·H<sub>2</sub>O with suspension electrolysis, effectively converting poorly soluble PbSO<sub>4</sub> into soluble [Pb(NH<sub>3</sub>)<sub>4</sub>]<sup>2+</sup> complexes. The electrolytic conversion mechanisms of SLP components are systematically elucidated, revealing four distinct transformation pathways: 1) metallic Pb undergoes complete dissolution as [Pb(NH<sub>3</sub>)<sub>4</sub>]<sup>2+</sup> complexes followed by cathodic reduction to elemental lead; 2) PbO<sub>2</sub> increases after suspension electrolysis since part of PbO is oxidized; 3) PbO demonstrates dual behavior, with 45.74% undergoing anodic oxidation to PbO<sub>2</sub> while the remainder (54.26%) participates in cathodic electrodeposition; 4) PbSO<sub>4</sub> exhibits triple conversion routes, including: 1) 32.98% transformation through intermediate (NH<sub>4</sub>)Pb(OH)SO<sub>4</sub> formation followed by anodic conversion to PbO·PbSO<sub>4</sub>, 2) 21.36% direct cathodic reduction to metallic lead, and 3) the residual fraction maintaining soluble [Pb(NH<sub>3</sub>)<sub>4</sub>]<sup>2+</sup> speciation in the electrolyte. The optimized process achieves exceptional current efficiency (95.49%) and lead recovery (45.67%), with anode residues comprising 67.58% PbO<sub>2</sub> and 32.42% PbO·PbSO<sub>4</sub>. Remarkably, this process exhibits significant economic and environmental advantages, with recycling 1 kg of SLP through the (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub>-NH<sub>3</sub>·H<sub>2</sub>O suspension electrolysis process resulting in a net profit of 0.3466 USD and a reduction in carbon emissions of 119.758 kg CO<sub>2</sub> eq., offering dual advantages of environmental and economic benefits. This work provides fundamental insights into lead phase conversion during suspension electrolysis while presenting a practical, effective solution for battery recycling industries.</p>

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A short and low-carbon approach for spent lead paste recycling via (NH4)2SO4-NH3·H2O suspension electrolysis: lead phases conversion

  • Xingyu Luo,
  • Jiqin Wang,
  • Yunhui Han,
  • Yao Huang,
  • Xiangfei Zeng,
  • Ling Hu,
  • Huimin Yang,
  • Qian Liang,
  • Xingying Fan,
  • Huan Li,
  • Shirvani Mehran,
  • Mengjun Chen

摘要

Spent lead paste (SLP) presents a major recycling challenge in lead-acid battery treatment due to its insoluble lead compounds. This study develops an innovative and environmentally sustainable approach by integrating (NH4)2SO4-NH3·H2O with suspension electrolysis, effectively converting poorly soluble PbSO4 into soluble [Pb(NH3)4]2+ complexes. The electrolytic conversion mechanisms of SLP components are systematically elucidated, revealing four distinct transformation pathways: 1) metallic Pb undergoes complete dissolution as [Pb(NH3)4]2+ complexes followed by cathodic reduction to elemental lead; 2) PbO2 increases after suspension electrolysis since part of PbO is oxidized; 3) PbO demonstrates dual behavior, with 45.74% undergoing anodic oxidation to PbO2 while the remainder (54.26%) participates in cathodic electrodeposition; 4) PbSO4 exhibits triple conversion routes, including: 1) 32.98% transformation through intermediate (NH4)Pb(OH)SO4 formation followed by anodic conversion to PbO·PbSO4, 2) 21.36% direct cathodic reduction to metallic lead, and 3) the residual fraction maintaining soluble [Pb(NH3)4]2+ speciation in the electrolyte. The optimized process achieves exceptional current efficiency (95.49%) and lead recovery (45.67%), with anode residues comprising 67.58% PbO2 and 32.42% PbO·PbSO4. Remarkably, this process exhibits significant economic and environmental advantages, with recycling 1 kg of SLP through the (NH4)2SO4-NH3·H2O suspension electrolysis process resulting in a net profit of 0.3466 USD and a reduction in carbon emissions of 119.758 kg CO2 eq., offering dual advantages of environmental and economic benefits. This work provides fundamental insights into lead phase conversion during suspension electrolysis while presenting a practical, effective solution for battery recycling industries.