CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Xiaofeng Mo,Mengye Wang,Han Song,Jie Li,Zhen Wu,Zhang Lin
Organic lead halide perovskite is a promising piezocatalyst for piezocatalytic H 2 production, meanwhile, large amount of unutilized lead resources in lead smelting residues have caused ecological security and resource waste problems. Here, we report an efficient Pb upcycling approach to recover lead halides from lead smelting residues to create lead halide perovskites (r-FAPbBr 3-x I x ), distinguished by the remarkable piezoelectric properties, for piezocatalytic H 2 evolution. Zinc impurities, concurrently from these residues, found their utilization in the partial substitution of Pb 2+ within the halide octahedra of r-FAPbBr 3-x I x . The intervention of zinc enhancing desorption of hydrogen from r-FAPbBr 3-x I x and culminating in a pronounced H 2 yield as 157.80 μmol·g −1 ·h −1 . Notably, the used r-FAPbBr 3-x I x that lost its functional prowess could be regenerated and exhibited a piezocatalytic capacity similar to its initial state, perpetuating a sustainable cycle of utility. This pioneering route to Pb upcycling furnishes an alternative avenue for the preparation and utilization of lead-based perovskites.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2024
·
IF 9.3
Hongya Wang,Fengyin Zhou,Bingbing Wang,Muya Cai,Jingjing Zhao,Xinyu Li,Yongxin Wu,Xiaowei Liu,Xiang Chen,Dihua Wang,Huayi Yin
The sulfur transfer is key to obtaining greenness of recycling spent lead paste (SLP) since conventional recycling methods always involve generating secondary wastes such as sulfur oxides (SOx), sulfates, and sulfides. To address these challenges, we propose a combined process in which the SLP is first converted into lead sulfide (PbS) by carbothermic reduction, and then the resultant PbS is split into liquid lead (Pb) and sulfur vapor (Sx) by molten salt electrolysis (MSE). The faradaic efficiency of MSE reaches 92.29% with a Pb recovery rate of 97.85%, and the liquid Pb and gaseous Sx are respectively discharged from the bottom and top of the cell to allow the reaction to happen continuously. Compared with traditional methods, over 98.85% of SO2 emissions are reduced, and no sulfides and sulfates are generated. Furthermore, the energy consumption is only 0.32 kW h (kg-Pb)−1, which demonstrates a 67% reduction compared to mainstream recycling processes using a 50 g-scale electrolyzer. Overall, we offer a clean sulfur transfer route to reduce secondary wastes and energy consumption, which will benefit the recovery and utilization of various sulfate wastes and raw materials with low environmental footprints.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOM
·
2020
·Vol. 72
·期 9
·3195-3203
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IF 2.054
Xie Boyi,Yang Tianzu,Liu Weifeng,Zhang Duchao,Chen Lin
The treatment of spent lead paste is essential for the recycling of spent lead-acid batteries. In this study, we propose a facile route for the recovery of lead from spent lead paste by pre-desulfurization followed by low-temperature reduction smelting. The effects of two desulfurization methods, i.e., high-pressure and normal-pressure processes, on the desulfurization efficiency of spent lead paste were compared. The high-pressure process was found to be more effective than the normal-pressure process; 99.1% of sulfur was removed under the high pressure conditions with NaOH excess of 1.1 at 150°C for 30 min. Moreover, a part of PbO 2 reacted with PbO to form Pb 3 O 4 . Afterwards, the desulfurized residue, mainly consisting of Pb 3 O 4 and PbO 2 , was directly used in low-temperature reduction smelting, and the optimum smelting conditions were determined to be: starch/Pb-residue mass ratio = 1/6.3; Na 2 O/Pb-residue mass ratio = 1/15; B 2 O 3 /Pb-residue mass ratio = 1/7.5; smelting temperature 700°C; and smelting duration 90 min. The lead recovery under the optimum conditions was as high as 93%. Scanning electron microscope images of the smelting slag showed that the smelting slag mainly consisted of PbO x and Na 2 O.
研究领域:
环境科学
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冶金工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Sustainable Metallurgy
·
2022
·Vol. 8
·期 3
·1257-1268
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IF 3.068
Geng Xiao,Ru Juan-jian,Hua Yi-xin,Zhang Wen-wen
The recovery of lead from spent lead acid battery paste (SLP) is not only related to the sustainable development of the lead industry, but also to the sustainable evolution environment. An innovative process is proposed for the recovery of high purity metallic lead from spent lead acid battery paste (SLP) by electrodeposition at 333–353 K in choline chloride-urea deep eutectic solvent (ChCl-urea DES). The electrochemical behavior of SLP on low carbon steel (LCS) electrode has been investigated by cyclic voltammetry and chronoamperometry measurement. Results imply that Pb(IV) could be reduced preferentially to Pb(II) by ChCl-urea DES, which possesses a strong reducibility. Then the reduction of Pb(II) is a diffusion-controlled quasi-reversible process and the diffusion coefficient increases gradually from 2.70 × 10 –8 cm 2 /s at 333 K to 6.79 × 10 –8 cm 2 /s at 353 K. The initial nucleation stage of lead on LCS electrode is a three-dimensional instantaneous nucleation process. In addition, the effects of temperature on the current efficiency and specific energy consumption during the recovery of lead have been discussed at 2.5 V for 1 h. The current efficiency is about 90.73% and the specific energy consumption is as low as 712.83 kW h/t at 353 K. Rod-shaped and fern-like lead powders can be obtained with a face-centered cubic structure and the predominately oriented crystallite varies from (200) at 333 K to (111) plane at 343 K and 353 K. This new system can efficiently shorten the production flow, lower the requirement for equipment, and avoiding emission of lead effluent and harmful gases. This article provides a green extraction method of lead and a theoretical guidance for the electrochemical extraction of valuable metals from spent battery materials in close neutral electrolyte. Graphical Abstract
研究领域:
环境科学
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材料科学
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电化学工程
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2019
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IF 5.107
Tianzu Yang,Boyi Xie,Weifeng Liu,Duchao Zhang,Lin Chen
Spent lead paste, an important secondary resource, calls for recycling at the request of both environmental protection and the sustainable development of lead industry. An environment-friendly process to recover lead from spent lead paste was proposed. The impurities Sb, Ca, Fe and Cu in spent lead paste were firstly removed by H 2 SO 4 at the leaching rate of 92.22%, 86.43%, 87.89% and 94.04%, respectively. And then, 99.9% of PbO 2 in spent lead paste was reduced to PbO by the hydrothermal reduction process with glucose as the reductant. In the process of hydrothermal desulfurization by NaOH, 99.46% of S in the reduced lead paste was removed and then the lead paste was converted into a single phase of 3PbO·H 2 O. Finally, metallic lead, with a purity of 99.978%, was obtained from the single-phase lead paste by a low-temperature reduction smelting process with starch as the reductant under the conditions of Na 2 O/B 2 O 3 = 1/2, PbO/B 2 O 3 = 5/1, starch/PbO = 1/7.5, smelting temperature 700 °C, and smelting duration 90 min, and the lead recovery is high up to 95.53%. Compared with the traditional lead smelting technology, the smelting temperature was reduced from 1200 °C to 700 °C, helping greatly reduce the energy consumption. The process proposed in this paper guides a new development direction for the utilization of spent lead paste.
研究领域:
冶金工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Cong Li,Suqin Li,Penghui Guo,Yongkui Li,Xingyu Liu
Copper plant residue (CPR) is a hazardous industrial by-product possessing both high toxicity and valuable metal content, necessitating its high value-added utilization. Traditional practices in smelters involve stockpiling and landfilling of CPR, leading to substantial land occupation and water contamination . This study focused on the preparation of PbO and Pb 3 O 4 using the HCl–NaCl leaching–conversion–thermal decomposition process, employing CPR as the primary raw material. The effect of various leaching process conditions on the metal leaching rate was explored. A maximum lead leaching rate of 87.65% was achieved under optimal conditions including leaching temperature, liquid–solid ratio, leaching time, HCl molar concentration, NaCl mass concentration, and particle size. The lead content in the leachate was 15.85 g/L. Experimental data indicated that ash diffusion control served as the rate-limiting step in the HCl–NaCl leaching process. The apparent activation energy was determined to be 18.374 kJ mol −1 , with a reaction order of 0.8986 concerning the HCl concentration and an L/S ratio of 0.8124. Additionally, response surface methodology enabled the determination of technological parameters for refining PbCl 2 into PbCO 3 precursors, yielding a conversion rate exceeding 96.50%. Moreover, the technical indicators of PbO and Pb 3 O 4 obtained through low-temperature thermal decomposition of PbCO 3 were investigated. The fabricated PbO and Pb 3 O 4 exhibited purities of 99.65% and 99.26%, respectively, effectively transforming CPR from hazardous waste residue into valuable products. The process ensures the efficient recovery of lead to its maximum extent and promotes residue recycling .
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOM
·
2019
·Vol. 72
·期 9
·3186-3194
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IF 2.305
Li Yun,Yang Shenghai,Taskinen Pekka,He Jing,Chen Yongming,Tang Chaobo,Jokilaakso Ari
This study proposed a cleaner pyrometallurgical lead-acid battery (LAB) recycling method for lead extraction and sulfur conservation without an excessive amount of SO 2 generation. A reducing atmosphere was introduced to the lead paste recycling system to selectively reduce PbSO 4 to PbS. At the same time, PbO and PbO 2 components contained in the lead paste were also reduced to metallic Pb. Then, the intermediate PbS further reacted with a sulfur-fixing agent, typically Fe 3 O 4 , to generate PbO and FeS. Sulfur was transformed from PbSO 4 to PbS and finally conserved as FeS. Thus, SO 2 emissions and pollution were significantly eliminated. This work investigated the thermodynamic and experimental feasibility and phase conversion mechanism of this proposed method, the detailed lead extraction and sulfur fixing mechanisms were clarified, and the phase transformation and microstructural evolution processes were characterized. Additionally, a bench experiment of industrial, end-of-life LAB paste was conducted to detect the lead recovery and sulfur fixation efficiency.
研究领域:
环境科学
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冶金工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Sheng Zhang,Lili Shen,Mianji Huang,Yu Yu,Lei Lei,Jun Shao,Qingbao Zhao,Zihua Wu,Jinmin Wang,Songwang Yang
An environmentally friendly dissolving–precipitating method is developed to recycle lead from carbon-based perovskite solar cells (PSCs). N,N-Dimethylformamide (DMF) was used to dissolve PSCs and to obtain lead containing lixivium. NH3·H2O was used as a precipitator to extract lead ions from the lixivium. The result analyzed by inductively coupled plasma optical emission (ICP-OES) shows that 99.9% of lead can be extracted by NH3·H2O. Then, HI was used to generate PbI2. ICP-OES analysis and thermodynamic calculation are used to analyze the lead content. The results show that little PbI2 transforms into [PbI4]2– due to the low concentration of hydroiodic acid (HI). The calculated lead recovery rate is 95.7%. The recycled PbI2 was used to fabricate carbon-based PSCs achieving an efficiency of 11.36%, which is comparable to that (12.17%) of carbon-based PSCs fabricated with commercial PbI2. The developed process provides a new approach for the cyclic utilization of lead in carbon-based PSCs to avoid lead pollution.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Minerals
·
2019
·Vol. 9
·期 2
·119
·
IF 2.25
Yun Li,Shenghai Yang,Wenrong Lin,Pekka Taskinen,Jing He,Yuejun Wang,Junjie Shi,Yongming Chen,Chaobo Tang,Ari Jokilaakso
A novel and cleaner process for lead and silver recycling from multiple lead-containing wastes, e.g., lead ash, lead sludge, lead slag, and ferric sludge, by reductive sulfur-fixing smelting was proposed. In this process, coke and iron-containing wastes were employed as reductive agent and sulfur-fixing agent, respectively. A Na2CO3-Na2SO4mixture was added as flux. The feasibility of this process was detected from thermodynamic and experimental perspectives. The influence of Fe/SiO2and CaO/SiO2, composition of the molten salt, coke addition, smelting temperature, and smelting time on direct Pb recovery and sulfur-fixation efficiency were investigated. The optimal process conditions were determined as follows:WCoke= 15%WPb wastes,WNa2CO3/WNa2SO4= 0.7/0.3, Fe/SiO2= 1.10, CaO/SiO2= 0.30, smelting temperature 1200 °C, and smelting time 2 h, whereWrepresents weight. Under these optimum conditions, 92.4% Pb and 98.8% Ag were directly recovered in crude lead bullion in one step treatment, and total 98.6% sulfur was fixed. The generation and emissions of SO2can be avoided. The main phases in ferrous matte obtained were FeS, NaFeS2, Fe2Zn3S5, and a little entrained Pb. The slag was a FeO-SiO2-CaO-Na2O quaternary melt.Keywords:SO2-free sulfur fixing smelting;lead recycling;wastes co-treatment and recycling;lead-iron-containing wastes;molten salt;PbO-FeO-SiO2-CaO-Na2O phase diagram
研究领域:
冶金学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 115
·94895-94902
·
IF 3.84
Cheng Ma,Yuehong Shu,Hongyu Chen
A sustainable method, with minimal pollution and low energy cost in comparison with the conventional smelting method, is proposed for treating components of spent lead acid batteries with oxalate and sodium oxalate. The pure lead oxalate precursor of PbC2O4 is the only product crystallized in the leaching experiment. Lead oxalate is readily crystallized from the solution due to its low solubility and can be combusted to directly produce lead oxide as a precursor for making new battery pastes. Both lead oxalate and the oxide products have been characterized by means of thermogravimetric analysis (TGA) and X-ray diffraction (XRD). The results show that the lead oxides synthesized at different calcination temperatures are comprise of α-PbO and β-PbO. The batteries assembled using the novel lead oxide powder as the positive active material show good cyclic stability for 50 charge/discharge cycles. The cell using lead oxide powder containing 15 wt% β-PbO exhibits excellent initial capacity, cycling performance and high-rate discharge characteristics and can deliver a discharge capacity of 180 mA h g−1 at 30 mA g−1 and more than 60 mA h g−1 at 240 mA g−1. Within 50 cycles, its capacity loss is low (5%) with excellent cyclic stability.
研究领域:
环境科学
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材料科学
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化学工程
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能源技术
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可持续发展
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电化学
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资源循环利用
✓ 已验证
DOI
高影响因子
Journal of Physical Chemistry Letters
·
2021
·
IF 6.475
Lisha Xie,Qiang Zeng,Qingya Li,Shurong Wang,Linhong Li,Zhenyu Li,Fangyang Liu,Xiaojing Hao,Feng Hao
Lead is widely used as a crucial elemental for lead acid batteries (LABs) and emerging halide perovskite solar cells (PSCs). However, the use of soluble lead will raise environmental concerns. For the purpose of Pb recycling, herein, we report a reactant-recycling strategy to extract Pb from used LABs and synthesize high-purity PbI2. The recycled PbI2 shows smaller grain size, higher crystallinity, and higher thermal stability compared to the commercial sources. Perovskite films deposited with the high-quality PbI2 show larger grain size and fewer defects than the commercial ones. Consequently, the synthesized PbI2 enables a power conversation efficiency of 20.45% for the inverted MAPbI3 (MA= methylammonium) PSCs with excellent air stability. This work offers a novel strategy for lead recovery from LABs and a green path for the realization of high-performance PSCs with high defect tolerance.
研究领域:
材料科学
·
环境科学
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能源技术
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纳米技术
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Cunpeng Duan,Jiahui Xiao,Yanzhi Sun,Junqing Pan
The study of performance and economical Iridium-derived electrocatalysts for the acidic oxygen evolution reaction (OER) is a formidable obstacle for hydrometallurgy and water splitting. The sluggish oxidation mechanism of water molecules leads to high polarization, intensifying the competitive anodic oxidation process between Pb 2+ and H 2 O, resulting in low recovery rates and high energy consumption in lead hydrometallurgy. This study presents an Ir-doped Co-based catalyst (IrCoO x @CNT) through the in-situ growth of ZIF-67 on carbon nanotubes (CNTs), followed by ion exchange and thermal oxidation to realize the preferential catalytic oxidation of water molecules. The unique composite leverages the synergistic effects between highly dispersed Ir–Co active sites and conductive CNT network, and the formed electronic structure modulation of the Ir–Co dual sites lowers the overpotential of the OER process while raising the thermodynamic barrier for Pb 2+ →Pb 4+ oxidation. The catalyst exhibits a low overpotential of 166 mV at 10 mA cm −2 (90°C) and remarkable long-term stability in 1 M Methylsulfonic acid (MSA) to achieve reducing energy consumption to 422.52 kWh t −1 (Pb) by completely suppressing PbO 2 by-product formation, further revealed the incorporation of Ir into the Co 3 O 4 lattice enhances catalytic activity and acid resistance, while the CNT framework ensures rapid electron transport and prevents nanoparticle aggregation. This study presents a scalable strategy for practical application in sustainable metal recovery and hydrogen processes.
研究领域:
电化学
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催化
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纳米技术
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材料科学
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环境工程
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冶金
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）