退役锂离子电池湿法回收生命周期和经济评价

doi:10.19964/j.issn.1006-4990.2022-0603

Abstract

Abstract:

Lithium-ion batteries（LIBs） have been widely used because of high energy density and high output power，resulting in a large number of spent LIBs.In recent years，the recycling and utilization of spent LIBs has attracted the attention of researchers.However，the current recovery system is not perfect，due to problems in development momentum，science and technology.The three typical recovery processes，i.e.，HCl，H₂SO₄-H₂O₂ and electrochemical leaching，with life cycle assessment（LCA） and economic evaluation were compared.SimaPro 9 software was used to conduct LCA on the recovery process，and obtain global warming potential value，non biological resource depletion potential value，resource consumption，etc.The results showed that acid dosage and energy consumption were the main factors determining environmental burden.Economic analysis of three recovery processes including pretreatment，leaching，and regeneration was carried to obtain the corresponding profits.The analysis found that the cost of the current recycling process was high，resulting in the deficit of the whole recycling process.Therefore，corresponding optimization suggestions were put forward.

Key words: spent lithium-ion batteries, hydrometallurgical recycling, life cycle assessment, economic assessment

CLC Number:

TQ131.11

ZHOU Shiyu,HE Ting,FU Tongtong,GUO Zirui,GU Shuai,YU Jianguo. Life cycle and economic assessment of recycling spent lithium-ion batteries with hydrometallurgical process[J]. Inorganic Chemicals Industry, 2023, 55(1): 26-32.

Figures/Tables 7

Fig.1

Fig.2

Table 1

Fig.3

Table 2

Table 3

Fig.4

References 41

1	KIM T, SONG Wentao, SON D Y, et al. Lithium-ion batteries：Outlook on present，future，and hybridized technologies[J].Journal of Materials Chemistry A, 2019, 7（7）：2942-2964.
2	GU Fu, GUO Jianfeng, YAO Xing, et al. An investigation of the current status of recycling spent lithium-ion batteries from consumer electronics in China[J].Journal of Cleaner Production, 2017, 161：765-780.
3	YAN Zhiliang, HU Qiyang, YAN Guochun, et al. Co₃O₄/Co nano-particles enclosed graphitic carbon as anode material for high performance Li-ion batteries[J].Chemical Engineering Journal, 2017, 321：495-501.
4	LI Guangzhe, HUANG Bin, PAN Zhefei, et al. Advances in three-dimensional graphene-based materials：Configurations，preparation and application in secondary metal（Li，Na，K，Mg，Al）-ion batteries[J].Energy & Environmental Science, 2019, 12（7）：2030-2053.
5	LIU Dandan, SU Zhi, WANG Lei. Pyrometallurgically regenerated LiMn₂O₄ cathode scrap material and its electrochemical properti-es[J].Ceramics International, 2021, 47（1）：42-47.
6	XIAO Hougui, JI Guanjun, YE Long, et al. Efficient regeneration and reutilization of degraded graphite as advanced anode for lithium-ion batteries[J].Journal of Alloys and Compounds, 2021, 888.Doi：10.1016/j.jallcom.2021.161593. doi: 10.1016/j.jallcom.2021.161593
7	MAKUZA B, TIAN Qinghua, GUO Xueyi, et al. Pyrometallurgical options for recycling spent lithium-ion batteries：A comprehensive review[J].Journal of Power Sources, 2021, 491.Doi：10.1016/j.jpowsour.2021.229622. doi: 10.1016/j.jpowsour.2021.229622
8	YANG Yue, HUANG Guoyong, XU Shengming, et al. Thermal treatment process for the recovery of valuable metals from spent lithium-ion batteries[J].Hydrometallurgy, 2016, 165：390-396.
9	HUANG Bin, PAN Zhefei, SU Xiangyu, et al. Recycling of lithium-ion batteries：Recent advances and perspectives[J].Journal of Power Sources, 2018, 399：274-286.
10	RAJ T， CHANDRASEKHAR K, KUMAR A N, et al. Recycling of cathode material from spent lithium-ion batteries：Challenges and future perspectives[J].Journal of Hazardous Materials, 2022, 429.Doi：10.1016/j.jhazmat.2022.128312. doi: 10.1016/j.jhazmat.2022.128312
11	HARPER G, SOMMERVILLE R, KENDRICK E, et al. Recycling lithium-ion batteries from electric vehicles[J].Nature, 2019, 575（7781）：75-86.
12	MROZIK W, RAJAEIFAR M A, HEIDRICH O, et al. Environmental impacts，pollution sources and pathways of spent lithium-ion batteries[J].Energy & Environmental Science, 2021, 14（12）：6099-6121.
13	SINGH U K, KUMAR B. Pathways of heavy metals contamination and associated human health risk in Ajay River Basin，India[J].Chemosphere, 2017, 174：183-199.
14	SHI Yang, CHEN Gen, CHEN Zheng. Effective regeneration of LiCoO₂ from spent lithium-ion batteries：A direct approach towards high-performance active particles[J].Green Chemistry, 2018, 20（4）：851-862.
15	李惜. 健全废旧锂离子电池回收利用支撑体系[N].中国矿业报, 2022-03-12（4）.
16	SHIBAZAKI K, AZUMA D, WATANABE M, et al. Hydrothermal organic acid leaching of positive electrode material of lithium-ion batteries[J].Kagaku Kogaku Ronbunshu, 2020, 46（5）：167-175.
17	LI Jishen, YANG Xiyun, YIN Zhoulan. Recovery of manganese from sulfuric acid leaching liquor of spent lithium-ion batteries and synthesis of lithium ion-sieve[J].Journal of Environmental Chemical Engineering, 2018, 6（5）：6407-6413.
18	CHEN Mengyuan, MA Xiaotu, CHEN Bin, et al. Recycling end-of-life electric vehicle lithium-ion batteries[J].Joule, 2019, 3（11）：2622-2646.
19	PETERS J F, BAUMANN M, ZIMMERMANN B, et al. The environmental impact of Li-ion batteries and the role of key parame-ters-A review[J].Renewable and Sustainable Energy Reviews, 2017, 67：491-506.
20	LYBBERT M, GHAEMI Z, BALAJI A K, et al. Integrating life cycle assessment and electrochemical modeling to study the effects of cell design and operating conditions on the environmental impacts of lithium-ion batteries[J].Renewable and Sustainable Energy Reviews, 2021, 144.Doi：10.1016/j.rser.2021.111004. doi: 10.1016/j.rser.2021.111004
21	REY I， VALLEJO C, SANTIAGO G, et al. Environmental impacts of graphite recycling from spent lithium-ion batteries based on life cycle assessment[J].ACS Sustainable Chemistry & Engineering, 2021, 9（43）：14488-14501.
22	JIANG Songyan, HUA Hui, ZHANG Ling, et al. Environmental impacts of hydrometallurgical recycling and reusing for manufacturing of lithium-ion traction batteries in China[J].Science of the Total Environment, 2022, 811.Doi：10.1016/j.scitotenv.2021.152224. doi: 10.1016/j.scitotenv.2021.152224
23	GAINES L. Lithium-ion battery recycling processes：Research towards a sustainable course[J].Sustainable Materials and Technologies, 2018, 17.Doi：10.1016/j.susmat.2018.e00068. doi: 10.1016/j.susmat.2018.e00068
24	HE Lipo, SUN Shuying, SONG Xingfu, et al. Recovery of cathode materials and Al from spent lithium-ion batteries by ultrasonic cleaning[J].Waste Management, 2015, 46：523-528.
25	GAO Wenfang, ZHANG Xihua, ZHENG Xiaohong, et al. Lithium carbonate recovery from cathode scrap of spent lithium-ion battery：A closed-loop process[J].Environmental Science & Technology, 2017, 51（3）：1662-1669.
26	LI Jia, WANG Guangxu, XU Zhenming. Environmentally-friendly oxygen-free roasting/wet magnetic separation technology for in situ recycling cobalt，lithium carbonate and graphite from spent LiCoO₂/graphite lithium batteries[J].Journal of Hazardous Materials, 2016, 302：97-104.
27	DUAN Xiaowei, ZHU Wenkun, RUAN Zhongkui, et al. Recycling of lithium batteries-A review[J].Energies, 2022, 15（5）.Doi：10.3390/en15051611. doi: 10.3390/en15051611
28	YAO Yonglin, ZHU Meiying, ZHAO Zhuo, et al. Hydrometallurgical processes for recycling spent lithium-ion batteries：A critical review[J].ACS Sustainable Chemistry & Engineering, 2018, 6（11）：13611-13627.
29	Jung J C Y, Chow N, Warkentin D D, et al. Experimental study on recycling of spent lithium-ion battery cathode materials[J].Journal of the Electrochemical Society, 2020, 167（16）.Doi：10.1149/1945-7111/abd600. doi: 10.1149/1945-7111/abd600
30	LI Jinhui, SHI Pixing, WANG Zefeng, et al. A combined recovery process of metals in spent lithium-ion batteries[J].Chemosphere, 2009, 77（8）：1132-1136.
31	SHIN S M, KIM N H, SOHN J S, et al. Development of a metal recovery process from Li-ion battery wastes[J].Hydrometallurgy, 2005, 79（3/4）：172-181.
32	MENG Qi, ZHANG Yingjie, DONG Peng. Use of electrochemical cathode-reduction method for leaching of cobalt from spent lithi-um-ion batteries[J].Journal of Cleaner Production, 2018, 180：64-70.
33	杨海波, 梁辉, 黄继承, 等. 从废旧锂离子电池中回收制备LiCoO₂的结构与性能研究[J].稀有金属材料与工程, 2006, 35（5）：836-840.
	YANG Haibo, LIANG Hui, HUANG Jicheng, et al. Research on structure and properties of LiCoO₂ prepared from spent lithium ion batteries[J].Rare Metal Materials and Engineering, 2006, 35（5）：836-840.
34	气体网. 多因素提振 2021年中国液氮价格震荡上扬[EB/OL].（2022-01-17）[2022-10-03].
35	北极星储能网. 7月12日储能材料价格：钴酸锂价格下跌 5 000元/吨！[EB/OL].（2022-07-12）[2022-10-03].
36	陈雨康. 中国硫酸工业协会：预计硫酸价格将高位运行[EB/OL].（2022-07-20）[2022-10-03].
37	吴小龙, 王晨麟, 陈曦, 等. 废旧锂离子电池市场规模及回收利用技术[J].环境科学与技术, 2020, 43（S2）：179-183.
	WU Xiaolong, WANG Chenlin, CHEN Xi, et al. Market scale and recycling technology of waste lithium-ion batteries[J].Environmental Science ＆ Technology, 2020, 43（S2）：179-183.
38	YANG Jingbo, FAN Ersha, LIN Jiao, et al. Recovery and reuse of anode graphite from spent lithium-ion batteries via citric acid leaching[J].ACS Applied Energy Materials, 2021, 4（6）：6261-6268.
39	NATARAJAN S, ARAVINDAN V. An urgent call to spent LIB recycling：Whys and wherefores for graphite recovery[J].Advanced Energy Materials, 2020, 10（37）.Doi：10.1002/aenm.202002238. doi: 10.1002/aenm.202002238
40	FAN Ersha, LI Li, WANG Zhenpo, et al. Sustainable recycling technology for Li-ion batteries and beyond：Challenges and future prospects[J].Chemical Reviews, 2020, 120（14）：7020-7063.
41	刘东旭, 蔡牧涯, 陈翔, 等. 废旧锂离子电池负极材料再生和利用进展[J].化学工业与工程, 2021, 38（6）：2-12.
	LIU Dongxu, CAI Muya, CHEN Xiang, et al. Progress on regeneration and reutilization of anode materials from spent lithium-ion batteries[J].Chemical Industry and Engineering, 2021, 38（6）：2-12.

项目	预处理	HCl浸出	H₂SO₄-H₂O₂ 浸出	电化学浸出
输入	N₂，0.520 kg	HCl，7.30 kg	H₂SO₄，3.92 kg； H₂O₂，7.29 kg	苹果酸， 25.1 kg
	去离子水，156 kg	去离子水， 46.0 kg	去离子水， 14.9 kg	去离子水，134 kg
	耗电量，9.57 kW?h	耗电量， 64.9 kW?h	耗电量， 59.3 kW?h	耗电量， 123 kW?h
输出	水，156 kg；N₂，0.520 kg；
	石墨，0.069 0 kg；	废渣， 0.340 kg	废渣，0.340 kg	废渣，0.390 kg
	Co，0.046 0 kg；
	Li₂CO₃，0.007 90 kg

项目	GWP（以 CO₂计）/kg	ADP/ MJ	HTP（以1，4-DB计）/kg	化石（非可再生能源）/MJ	水（可再生能源）/MJ
预处理	11.02	95.50	6.560	100.9	7.180
HCl	19.20	346.0	894.0	372.0	139.0
H₂SO₄-H₂O₂	24.80	299.0	21.90	326.0	290.0
电化学	64.86	1 199	35.30	1 296	324.4

项目			消耗量	单价	总价/万元
预处理		N₂	0.187 0 t	665.7元/t	0.012 40
		去离子水	56.20 t	452.0元/t	2.540
		总电量	3.441 kW?h	0.693 0元/（kW?h）	2.385×10^-4
HCl 体系	浸出	HCl	2.920 t	650.0元/t（31%）	0.612 2
		去离子水	18.40 t	452.0元/t	0.831 7
		总电量	1.242×10⁴kW?h	0.693 0元/（kW?h）	0.860 7
	再制备	CoCl₂	0.024 00 t	12.20万元/t	0.292 8
		Na₂CO₃	5.230 t	2 300元/t（98%）	1.227
		无水乙醇	0.286 0 t	8 000元/t	0.228 8
		总电量	8 912 kW?h	0.693 0元/（kW?h）	0.617 6
H₂SO₄- H₂O₂ 体系	浸出	H₂SO₄	1.570 t	910.0元/t	0.142 9
		H₂O₂	2.920 t	915.0元/t（27.5%）	0.971 6
		总电量	2 300 kW?h	0.693 0元/（kW?h）	0.159 4
	再制备	CoSO₄	0.045 00 t	7.300万元/t	0.328 5
		Na₂CO₃	5.529 t	2 300元/t（98%）	1.298
		无水乙醇	0.302 0 t	8 000元/t	0.241 6
		总电量	9 421 kW?h	0.693 0元/（kW?h）	0.652 9
电化学	浸出	苹果酸	10.00 t	40.00元/kg	40.00
		去离子水	53.60 t	452.0元/t	2.423
		总电量	4.920×10⁴kW?h	0.693 0元/（kW?h）	3.410
	再制备	CoSO₄	0.068 00 t	7.300万元/t	0.496 4
		Na₂CO₃	5.298 t	2 300元/t（98%）	1.243
		无水乙醇	0.289 0 t	8 000元/t	0.231 2
		总电量	9 028 kW?h	0.693 0元/（kW?h）	0.625 6

[1]	GE Jianhua, XIE Minyan, OUYANG Quansheng, SHAO Jiaojing. Advances in regeneration processes of cathode materials for spent power batteries [J]. Inorganic Chemicals Industry, 2024, 56(12): 79-87.
[2]	WANG Xuemeng, AN Yan, LIU Hai, TIAN Mengkui. Carbon footprint analysis of yellow phosphorus products based on LCA [J]. Inorganic Chemicals Industry, 2023, 55(12): 36-42.
[3]	HE Ting,KONG Jiao,CUI Jingzhi,CHEN Zhihao,FU Tongtong,GUO Zirui,GU Shuai,YU Jianguo. Study on leaching and thermodynamic of spent lithium-ion batteries with electrochemical reduction [J]. Inorganic Chemicals Industry, 2022, 54(12): 34-43.

National Inorganic Salts Information Center

Inorganic Acid-Base-Salt Committee of CIESC

Life cycle and economic assessment of recycling spent lithium-ion batteries with hydrometallurgical process

RichHTML

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 7

References 41

Related Articles 3

Metrics

Comments

Recommended 0