Li Fei, Zhu Neng-Wu, Xi Yun-Hao, Xiong Wu-Wan, Ruan Ju-Jun, Wei Xiao-Rong, Guo An-Qi, Chen Yi-Jun, Wu Ping-Xiao, Dang Zhi
School of Environment and Energy, South China University of Technology, Guangzhou, 510006, China.
School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou, 510275, China.
Adv Sci (Weinh). 2024 Nov;11(43):e2405168. doi: 10.1002/advs.202405168. Epub 2024 Sep 20.
Recycling of spent lead-acid batteries (LABs) is extremely urgent in view of environmental protection and resources reuse. The current challenge is to reduce high consumption of chemical reagents. Herein, a closed-loop spent LABs paste (SLBP) recovery strategy is demonstrated through NaMoO consumption-regeneration-reuse. Experimental and DFT calculations verify that MoO competes Pb/Ca ions and weakens the metal-oxygen bond of PbSO/CaSO.2HO in SLBP, facilitating PbMoO/CaMoO formation and 99.13 wt% of SO elimination. Pb of 99.97 wt% is obtained as zero-carbon precursors (PbO and PbMoO) by green leaching coupled with re-crystallization. The regeneration of NaMoO is realized at 600 ℃ using LABs polypropylene shells and NaOH as reagents. Compared with the traditional smelting technologies, the temperature is reduced from >1000 to 600 °C. The extraction of NaMoO require only water, and satisfactory re-used desulfurization efficiency (98.67 wt%) is achieved. For the residual NaMoO after first SLBP desulfurization, the desulfurization efficiency remains above 97.36 wt% after adding fresh reagents for two running cycles. The new principle enables the reuse of 99.83 wt% of NaMoO and the recycling of 95.27 wt% of Pb without generating wastewater and slags. The techno-economic analysis indicates this strategy is efficient, economical, and environmentally-friendly.
鉴于环境保护和资源再利用,废旧铅酸电池(LABs)的回收迫在眉睫。当前的挑战是减少化学试剂的高消耗。在此,通过钼酸钠的消耗-再生-再利用展示了一种闭环废旧LABs铅膏(SLBP)回收策略。实验和密度泛函理论计算验证了钼酸根与铅/钙离子竞争,并削弱了SLBP中硫酸铅/硫酸钙·2水合物的金属-氧键,促进钼酸铅/钼酸钙的形成以及99.13 wt%的硫酸根消除。通过绿色浸出结合重结晶获得了99.97 wt%的铅作为零碳前驱体(氧化铅和钼酸铅)。利用LABs聚丙烯外壳和氢氧化钠作为试剂在600℃实现了钼酸钠的再生。与传统熔炼技术相比,温度从>1000℃降至600℃。钼酸钠的提取仅需用水,并且实现了令人满意的再利用脱硫效率(98.67 wt%)。对于首次SLBP脱硫后的残留钼酸钠,在添加新鲜试剂进行两个运行周期后,脱硫效率仍保持在97.36 wt%以上。新原理使得99.83 wt%的钼酸钠得以再利用,95.27 wt%的铅得以回收,且不产生废水和废渣。技术经济分析表明该策略高效、经济且环保。