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Progress in Chemistry 2023, Vol. 35 Issue (10): 1519-1533 DOI: 10.7536/PC230214 Previous Articles   Next Articles

• Review •

Preparation and Extraction Application of Lithium Ion Selective Adsorption Materials

Xinyi Chen1, Kaisheng Xia1,*(), Qiang Gao1, Zhen Yang2,*(), Yudie Li1, Yi Meng1, Liang Chen3, Chenglin Liu2   

  1. 1 Faculty of Materials Science and Chemistry, China University of Geosciences,Wuhan 430078, China
    2 School of Earth Resources, China University of Geosciences,Wuhan 430074, China
    3 School of Physics, Huazhong University of Science & Technology,Wuhan 430074, China
  • Received: Revised: Online: Published:
  • Contact: *e-mail: kaishengxia@cug.edu.cn (Kaisheng Xia);yangzhen@cug.edu.cn (Zhen Yang)
  • Supported by:
    Science and Technology Major Projects of Xinjiang Autonomous Region(2022A03009); National Natural Science Foundation of China(21975228)
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In recent years, with the rapid advancement and large-scale application of lithium battery technology and electric vehicle, the market demand for lithium resource is growing sharply. However, due to insufficient mining degree and extraction technology, the total production capacity of ore lithium and brine lithium resources is far below the actual market demand. Extracting lithium from surface salt lake brine, deep brine and other liquid resources has the advantages of large resource potential and low extraction cost, which presents an important research direction in the lithium resource extraction field. Among available lithium extraction technologies, adsorption method is suitable for extracting lithium from low concentration and large volume liquid brine resources in China, and selective lithium ion adsorption materials are the core of adsorption method. In this review, we focus on the preparation and application of lithium ion selective adsorption materials for lithium extraction from brine. The preparation methods, adsorption properties and adsorption mechanisms of organic (crown ether), inorganic (aluminum-, manganese- and titanium-based adsorbents) and composite selective lithium adsorption materials are reviewed. This review provides a brief prospect for the design and development of new lithium adsorption materials, which may push forward the efficient extraction and utilization of lithium resources from salt lake brine.

Contents

1 Introduction

2 Crown ether adsorbents

2.1 Preparation of crown ether adsorbent

2.2 Selective lithium extraction performance

2.3 Selective lithium extraction mechanism

3 Alumina-based materials

3.1 Preparation of aluminum adsorbent

3.2 Selective lithium extraction mechanism of aluminum adsorbent

3.3 Selective lithium extraction performance of aluminum-based adsorbent

4 Lithium ion sieve adsorbent

4.1 Preparation of ion sieve adsorbent

4.2 Lithium ion insertion/extraction mechanism

4.3 Selective lithium extraction performanc of lithium ion sieve

4.4 Molded lithium ion sieve adsorbent

5 Other types of adsorbents

6 Conclusion and outlook

Key words: brine, lithium extract, adsorbent, ion sieve
Fig.1 Classification of adsorbents for lithium recovery
Table 1 Performance of crown ether ligand composite adsorption materials
Crown ether ligands Matrixes Specific surface area
(m2/g)		 pH Adsorption capacity
(mg/g)		 Selectivity
α(Li/Na)		 Cycling stability ref

Aminoethylbenzo-12-crown-4		 Polymer nanosheets
(PMBA-PMA)		 / 7 14.67 / 90%
(Five cycles)		 30

1-aza-12-crown-4		 mesoporous silica
SBA-15
3-Aminopropyltriethoxy
4-ylsilane		 578 8 7.63 × 10-3 / / 31

2- (hydroxymethyl) 12-crown-4		 graphene oxide
chitosan
polyvinyl alcohol		 101.5 7 168.50 2.51 88.31%
(Five cycles)		 32

Aminoethylbenzo-12-crown-4		 Porous polymer substrate
(PVBC)		 / 7 4.22 6.59 95.0%
(Five cycles)		 35

Octamethyl 14-crown-4		 methacrylate polymer / / 3.05 / / 36
Fig.2 Size of alkali metal ions and crown ethers
Fig.3 The equilibrium geometry of 15-crown-5 (a), K+ and 15-crown-5 forming a ‘pyramid structure’ (b) and K+ and 15-crown-5 forming a ‘ sandwich structure ’ (c)
Fig.4 The structural model of chlorine-ion-intercalated LiAl-layered double hydroxides (LDHs)
Table 2 Performance comparison of three metal-based adsorbent
Performance Al-based Mn-based Ti-based
Li+ Adsorption Capacity √ √√ √√√
Li+ Selectivity √ √√√ √√
Technology Maturity √√√ √√ √
Stability and Regeneration
Ability		 √√√ √ √√
Facile Operation
Conditions		 √√√ √ √√
Environmental Safety √√√ √ √√
Low Preparation Cost √√√ √ √√
Table 3 Synthesis methods and properties of aluminum-based adsorbents
Adsorbent Source Method Li+ adsorption
capacity
(mg/g)		 pH Selectivity
(α)		 Recovery rate ref
LiAl-LDHs AlCl3·6H2O
NaOH Na2CO3		 Reaction coupling
separation technology		 / / / 96.07% 55
MLDH
(Fe3O4 doped LiAl-LDHs)		 FeCl3·6H2O
AlCl3·6H2O
LiCl·H2O
NaOH
FeCl2·4H2O		 Sectional chemical co-precipitation method 5.83 7 α(Li/Mg)=
362.68		 / 56
Al(OH)3 AlCl3·6H2O
NaOH brine		 co-precipitation method / 7.5 / 76.4% 57
LiOH/Al(OH)3 NaOH
anhydrous aluminum chloride
anhydrous lithium		 single step
co-precipitation		 15.06 6~7 / / 58
Li/Al-LDHs Al(OH)3
LiOH·H2O		 hydrothermal method / / α(Li/Na)=
47.80		 91% 59
Fig.5 Mechanism of Li intercalation and deintercalation in spinel LMO adsorbent
Fig.6 A schematic diagram of Li+ extraction and insertion process in LIS
Table 4 Synthesis methods and properties of different titanium-based ion sieves
Precursor Source Method Li+ adsorption
Capacity (mg/g)		 pH Selectivity
(α)		 Cycling stability ref
Li4Ti5O12 TTIP
LiOH·H2O		 solvothermal reaction 35.5 13 / 92.5%
(Five cycles)		 12
Li4Ti5O12 Ti3AlC2
LiOH		 two-step hydrothermal method 43.20 12.1 α(Li/Mg)
=269.00		 93%
(Twenty cycles)		 70
Li4Ti5O12 TiO2LiOH Soft hydrothermal method 39.43 / / / 81
Li2TiO3 C2H3LiO2·2H2O
TiO2		 high-temperature calcination 40.16 10 α(Li/Mg)
=5441.17		 98%
(Five cycles)		 87
3DM-Li4Ti5O12 CH3COOLi
C12H28O4Ti		 hydrothermal method
low temperature calcination method		 38.24 / α(Li/Mg)
=30.00		 80%
(Six cycles)		 90
Li2TiO3 Ti(OBu)4
Li2CO3		 solid state reaction 34.2 12 α(Li/Na)
=19.96		 90.6%
(Eight cycles)		 92
Table 5 Synthesis methods and properties of different manganese ion sieves
Precursor Source Method Li+ adsorption capacity pH Selectivity Cycling stability ref
1-D Li4Mn5O12 MnSO4LiNO3 hydrothermal method
low-temperature solid-phase reaction		 6.62 mmol/g / α(Li/Mg)
=599.12		 / 66
LiMg0.56Mn1.50O4 MnCl2·4H2O
Mg(NO3)2·6H2O
LiOH		 soft chemical method 37.4 mg/g 12 / 95%
(Four cycles)		 89
LiMxMn2-xO4(M=Mg,Cu and Zn) Li2CO3
CuO ZnO
MgCO3MnO		 high-temperature calcination / / / / 88
Li1.6(Mn0.7Al0.3)1.6O4 MnO2LiCl
AlCl3		 hydrothermal method 32.32 mg/L / / 95%
(Five cycles)		 91
Li1.33Mn1.67O4 Li2CO3MnCO3 solid-phase synthesis method 10.00 mg/g / / / 95
Li1.6Mn1.6O4 KMnO4LiOH hydrothermal method
Solid high
temperature sintering method		 41 mg/g / C F L i +
=474.46		 85.37%
(Five cycles)		 97
Table 6 Summary of advantages and disadvantages of crown ether, aluminum based, lithium-ion sieve type, and other types of adsorbents
Performance Crown ether Alumina-based adsorbent Lithium ion-sieve Others
Adsorption Capacity ★★ ★ ★★★ ★★
Selectivity ★★ ★ ★★★ ★★
Technology Maturity ★ ★★★ ★★ ★
Stability and
Regeneration		 ★★ ★★★ ★ ★★
Cost ★ ★★★ ★★ ★
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