DESALINATION
·
2023
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IF 9.9
Tingyu Li,Xinzhu Zhang,Yu Zhang,Jixiao Wang,Zhi Wang,Song Zhao
Selective lithium recovery from salt lake brine using emerging nanofiltration membranes is expected to solve the insufficient supply of lithium resources. In this work, 1,4,7,10-tetraazacyclododecane (Cyclen) was employed as a novel structural regulator through interfacial polymerization of polyethyleneimine (PEI) and trimesoyl chloride (TMC) to develop polyamide NF membrane with efficient Li + /Mg 2+ separation performance. After the introduction of Cyclen to aqueous phase , the PEI/Cyclen-TMC selective layer was confirmed to possess a higher crosslinking degree and larger d-spacing than PEI-TMC layer, endowing a dedicated channel for Li + transport. The water permeance of PEI/Cyclen-TMC composite membrane reached 14.0 L·m −2 ·h −1 ·bar −1 , about 3.8 times higher than PEI-TMC composite membrane, and meanwhile the separation factor ( S Li,Mg ) could be stabilized as 8.7 to realize a considerable reduction of Mg 2+ /Li + mass ratio from 20 to 2.3. Additionally, PEI/Cyclen-TMC composite membrane was utilized to operate a three-stage nanofiltration treatment procedure of a simulated salt lake brine (Mg 2+ /Li + mass ratio: 40). The results indicated that Li + could be efficiently retracted to obtain a solution with 19.5 mg·L −1 Li + and Mg 2+ /Li + mass ratio of 0.3. After the subsequent precipitation and filtration, the obtained Li 2 CO 3 purity could reach 93 %, indicating the potential application of nanofiltration for lithium recovery.
研究领域:
材料科学
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环境工程
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化学工程
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 51
·2305815
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IF 19
Huawen Peng,Yafei Su,Xufei Liu,Jiapeng Li,Qiang Zhao
High performance polyamide nanofiltration membranes play important roles in Mg 2+ /Li + separation and Li + extraction, but they are prepared via multiple time-/labor demanding steps. Both the scalability of these membranes and the engineering of membrane modules remain an elusive challenge. Here the design of a Gemini-electrolyte monomer (GEM) featuring bidentate amine groups, quaternary ammonia, and endocyclic contorted conformation is reported. The monomer's low interfacial diffusivity is balanced by high condensational reactivity during its interfacial polymerization with trimesoyl chloride (TMC), leading to the straightforward formation of defect-free, ≈14 nm thick membranes. The membrane shows the highest permeance (≈19.2 L m −2 h −1 bar −1 ) among Mg 2+ /Li + nanofiltration membranes prepared via straightforward interfacial polymerization without post-modification, combined with good Mg 2+ /Li + selectivity (≈15.4) and stability. The validity of GEM design is verified by control monomers. Large-area (1 × 2 m 2 ) GEM-TMC membranes and spiral-wound modules (effective area: 0.5 m 2 ) are prepared, both of which show reproducible and high performance.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 27
·12199-12208
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IF 2.7
Shaowei Wang,Zesen Gao,Futing Sun,Yan Yang,Lang Tao,Yunluo Wang,Zhiqian Yu,Jianghua Wu,Jingshan Hou,Zhanqiang Liu,Hucheng Song,Haijie Chen
Safety concerns associated with lithium batteries suggest the development of solid-state batteries as a promising variant. In this work, we doped a lithium boracite (Li4B7O12Cl) with Mg2+ to modify the Li+ sites and observed significant improvement in ionic conductivity by two orders of magnitude (from 3.03 × 10−7 S cm−1 to 2.81 × 10−5 S cm−1 at room temperature). We attribute the enhanced ion conductivity to the artificially induced Li vacancies resulting from Mg doping. The as-fabricated symmetrical battery (Li|Li3.6Mg0.2B7O12Cl|Li) exhibited good cycling performance with a stable voltage output even after 60 hours of cycling. The battery showed a coulombic efficiency retention of ∼99.7% after the cycling test. Our work demonstrates that Li4B7O12Cl is a superior solid electrolyte for solid-state batteries and the introduction of Li vacancies can be an efficient approach to greatly improve the ionic conductivity of other electrolytes.
研究领域:
材料科学
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电化学
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电池技术
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DOI
高影响因子
ACS ES&T Water
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2021
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IF 0
Guangming Tan,Xiangyang Xue,Zhigao Zhu,Jiansheng Li
Membrane distillation holds promise for further recovery of reverse osmosis (RO)-concentrated seawater to realize zero-liquid discharge; however, severe scaling induced by high-concentration salts and fouling triggered by a naturally occurring substance would result in severe wetting of the hydrophobic distillation membrane. To retard membrane wetting during the concentration process, the membrane’s interfacial structure and the seawater’s ingredients were systematically investigated to improve the membrane’s durability. The results demonstrated that the dual-layer membrane with hierarchically rough beads-on-a-string structured fibers could enlarge the water evaporation area on the membrane surface to improve membrane water flux, and superhydrophobicity can reduce the contact area between the salt and membrane surface to prevent membrane scaling. Significantly, the membrane’s durability can be further improved by adjusting the seawater ingredients. This finding revealed that the scaling resulting from Ca2+ and Mg2+ when they exist alone is more severe than when they exist together. Therefore, eliminating the dominant Ca2+, Mg2+, and naturally occurring substance in seawater and maintaining it in a neutral state can stably concentrate the seawater with a high water recovery of ∼85%. The regulation of the membrane interface integrated with optimal seawater ingredients is essential for the application of membrane distillation in the treatment of RO-concentrated seawater.
研究领域:
环境工程
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水处理
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海水淡化
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DOI
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yuanlin Chen,Yanfei Chen,Leilei Li,Jianhua Chen
During the flotation of sulfide minerals in the presence of serpentine, fine serpentine particles tend to coat the surfaces of sulfide minerals, severely deteriorating their flotation performance. To address this issue, sodium phosphate was used as a surface modifier for serpentine in this study to eliminate its detrimental effect on the flotation of sulfide minerals. Micro-flotation results indicated that under flotation conditions with pH = 8, the presence of natural serpentine in the slurry significantly reduced the recovery of pyrite. However, surface modification of serpentine with phosphate effectively eliminated its adverse effect, allowing the pyrite recovery in the mixed mineral system to nearly return to the level observed for pure pyrite. The underlying mechanism of this modification effect was elucidated through theoretical simulations and characterization techniques, revealing that phosphate readily interacted with surface-exposed Mg 2+ sites on serpentine, leading to a change of the surface charge from positive to negative. As a result, the serpentine and pyrite particles in the mixed slurry acquired similar surface charges, promoting a well-dispersed system and significantly enhancing the pyrite flotation recovery. This study highlights the potential use of phosphate for reducing the magnesium content in sulfide concentrates and provides a feasible strategy for the flotation separation of sulfide minerals from serpentine.
研究领域:
矿物加工
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表面化学
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浮选技术
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提取冶金
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Zhiyuan Zha,Tingyu Li,Ismail Hussein,Ying Wang,Song Zhao
The scarcity of lithium can be effectively addressed by extracting it from salt-lake brines. In this work, aza-crown ether (diazo-18-crown-6, DA18C6) was coupled into a polyamide (PA) network interfacial polymerized by trimesoyl chloride and polyethyleneimine (PEI) for efficient Li + /Mg 2+ separation. The embedment of DA18C6 molecule into PA network was confirmed by structural characterization and density functional theory simulation, which enhanced crosslinking degree and reduced average pore size of PA selective layer. In addition, the strong interaction between DA18C6 and Li + was proven through molecular dynamics simulation. The resulting PEI@DA18C6-PA membrane displayed a high pure water permeance of 10.4 L⋅m − 2 ⋅h − 1 ⋅bar − 1 and an excellent Li + /Mg 2+ separation factor ( S Li,Mg ) of 11.2, which was comparable with most reported Li + /Mg 2+ separation membranes . Furthermore, the PEI@DA18C6-PA membrane was employed in a three-stage NF treatment process to filtrate simulated brines containing a high Mg 2+ /Li + ratio of 57. The results demonstrated that Li + can be effectively concentrated and extracted through the membrane to obtain a permeate with an ultralow Mg 2+ /Li + ratio of only 0.03, suggesting that PEI@DA18C6-PA membrane has great application potential in lithium extraction from salt-lake brines.
研究领域:
材料科学
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环境工程
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Jia-Shuai Chen,Jing Wang,Ji-Hong Zhang,Zhi-Yuan Guo,Pan-Pan Zhang,Xiao-Fu Guo,Jie Liu,Zhi-Yong Ji
Achieving separation of lithium and magnesium with similar radii is crucial for the current lithium extraction technology from salt lakes, which usually possess a high lithium-to-magnesium ratio. Herein, we proposed the facile sequential interfacial polymerization (SIP) approach to construct electronanofiltration membranes (ENFMs) with a bilayer charged structure consisting of a high positively charged surface and a negatively charged sublayer. The trimesoyl chloride (TMC) concentration was adjusted to enhance the −COOH content and negative charge of the polyamide sublayer to promote Li+ migration, and then the quaternized polyethylenimine was introduced to the membrane surface by the SIP process to increase the positive charge density on the surface of the ENFMs, which would block the migration of Mg2+ and enhance the Li+/Mg2+ selectivity of the ENFMs. The optimal quaternary-modified ENFMs achieved outstanding selectivity for Li+/Mg2+ (49.85) and high Li+ flux (4.10 × 10–8 mol cm–2 s–1) at a current density of 10 mA cm–2. Moreover, in simulated brines with low lithium concentration and high Mg2+/Li+ ratio, the optimal ENFMs also displayed elevated Li+/Mg2+ selectivity (>45), highlighting the substantial promise of the membranes for practical applications.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2024
·
IF 7.4
Yufei Yan,Jin Wang,Wubin Wang,Chao Han,Kaili Huo,Qingyun Zhang,Ning Wang
Positively charged nanofiltration (NF) membranes are widely used to separate Li + and Mg 2+ , which play an important role in extracting lithium from salt lakes. Despite its widespread use, the polyethyleneimine-trimesoyl chloride (PEI-TMC) membrane has attracted attention due to its limited permeance and separation efficiency. To address these challenges, we introduced amine-functionalized titanium dioxide (TiO 2 -NH 2 ) nanoparticles into the interfacial polymerization (IP) reaction. The introduction of TiO 2 -NH 2 reduced the diffusion rate of PEI and formed nanoscale water channels in the polyamide (PA) layer. This modification effectively modulated the structure of the NF membrane. The NF membrane exhibited high water permeance (9.65 L·m −2 ·h −1 ·bar −1 ) and Li + /Mg 2+ selectivity ( S Li, Mg = 16.31) when 0.03 wt% TiO 2 -NH 2 was used. The DLVO theory and transition state theory showed that the introduction of TiO 2 -NH 2 improved the rejection of Li + and Mg 2+ by the membrane. Furthermore, the optimized NF membranes demonstrated excellent stability during long-term filtration and in the mixed salt solutions with varying Mg 2+ /Li + mass ratios. This work is of great significance for designing and advancing membrane materials that facilitate the efficient separation of lithium from salt lakes with high Mg 2+ /Li + mass ratios.
研究领域:
材料科学
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环境工程
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2025
·
IF 9
Yufei Yan,Jin Wang,Wubin Wang,Chao Han
Positively charged polyethyleneimine (PEI) nanofiltration (NF) membranes exhibit great potential for Li + /Mg 2+ separation. However, the dense nature of the polyamide (PA) layer presents a challenge in breaking through the permeance bottleneck, significantly hindering its further application. In this study, 1-(2-aminoethyl)piperazine (AEP) was first incorporated into the PEI solution as a structural regulator to adjust the microstructure of the PA separation layer. The structure of the PA selective layer was fine-tuned with the incorporation of AEP, enlarging the spacing between the long-chain molecules of PEI, and established hydrogen bonding interactions with PEI. This led to the generation of Turing structures on the membrane surface, which enhanced permeance. Meanwhile, the primary amine groups in AEP were protonated in water, aiding in boosting positive membrane charge and subsequently elevating its rejection capability for divalent cations. The ingenious combination of large molecule PEI and small molecule AEP served a dual purpose in promoting the membrane construction and performance. The optimized PEI/AEP-TMC NF membrane exhibited high pure water permeance (11.24 L m −2 h −1 bar −1 ) and excellent Li + /Mg 2+ selectivity ( S Li, Mg = 24.59), while also achieving higher Li purity and Li recovery. Insights into the remarkable performance of the modified membranes were gained through the transition state theory. Additionally, the internal stress generated in the NF process was determined by utilizing the principles of thin plate theory, revealing that the NF membrane possesses good pressure resistance and maintains stable operation at pressures up to 9 bar. This study demonstrates the capability of PEI/AEP-TMC NF membranes for Li + /Mg 2+ separation and offers a novel aqueous phase monomer for the preparation of NF membranes specifically for Li + /Mg 2+ separation.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Jian Lu,Chenye Dai,Shilong Li,Dong Zou,Yuqing Sun,Wenheng Jing
Similar physicochemical properties render the separation of Li + /Mg 2+ from salt lake brine difficult for two-dimensional (2D) membranes. Herein, ultraefficient Li + /Mg 2+ separation was achieved under the influence of an electric field using MXene/carbon nanotube (CNT) membranes developed on tubular ceramic substrates via thermal crosslinking. Crosslinking reactions between CNTs and MXene yielded well–intercalated CNTs between MXene nanosheets, forming antiswelling MXene/CNT membranes (MCMs) (interlayer spacing: 8.04 Å) suitable for Li + /Mg 2+ separation. At 2.8 V applied voltage, the MCMs exhibited Li + flux of 0.0491 mol m −2 h −1 and high Li + /Mg 2+ selectivity of 54.5, which outperform existing state–of–the–art 2D membranes. Specifically, under a positive electric field, Li + with a small hydration diameter and low hydration energy permeated through the membrane nanochannels more easily than Mg 2+ , increasing and decreasing Li + and Mg 2+ flux, respectively. Additionally, Mg 2+ retention was enhanced via the complexation of enriched Mg 2+ with –OH and –COOH on the membrane surface. The MXene membrane surface was thus reconfigured to be positively charged, inducing effective Mg 2+ rejection. This study offers a novel and practical approach for efficiently separating Li + /Mg 2+ as well as monovalent/multivalent ions.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
DESALINATION
·
2026
·
IF 9.9
Chun-Xu Zhang,Yan-Yan Chen,Ren-Jie Fan,Yu-Xuan Sun,Xiaohu Wang,Fujun Xiong,Yong Wang,Mei-Ling Liu,Shi-Peng Sun,Weihong Xing
Electric field-assisted nanofiltration (ENF) has emerged as a promising technology for Mg 2+ /Li + separation from salt lake brines. However, integrating ENF process with widely used negatively charged membranes induces a non-uniform distribution of reconstructed positive charge. This leads to reduced separation efficiency under high feed concentrations due to charge shielding effects. To overcome this limitation, we developed a strategy employing a positively charged nanofiltration (NF) membrane under an applied electric field. This configuration facilitates both the dehydration of hydrated Li + and a more uniform distribution of positive charges on the membrane surface. The optimized system demonstrated a remarkable separation performance, achieving nearly 100% rejection of Mg 2+ and − 176% rejection of Li + . The separation factor ( S Li, Mg ) represents a 162-fold improvement over the system without an electric field. The ENF process successfully separated Mg 2+ and Li + even in real Yiliping salt lake brine. Furthermore, the permeate stream containing high-purity Li + enabled the production of battery-grade Li₂CO₃ with 99.9% purity. This study demonstrates a pragmatic and efficient approach for Mg 2+ /Li + separation, showcasing considerable promise for high-purity Li + extraction from salt lakes.
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Yijing Zhang,Si Sun,Ming Wang,Yaling Han,Xuan Luo,Shenzhen Cong,Tao He,Huan Pang
Membranes featuring structural stability and precise ion selectivity are indispensable for efficient lithium recovery from magnesium-rich brines. Despite the promising potential of metal-organic framework (MOF) membranes in ion separation, the flexibility of aromatic linkers in conventional MOF structures often induces pore size fluctuations, which compromises size-based discrimination efficiency. Herein, defect-free Zr-Frustrated Trigonal-symmetry Rotor (Zr-FTR) membranes were fabricated on polyethylene terephthalate (PET) substrates via a counter-diffusion interfacial growth method. The Zr-FTR framework is constructed with bicyclopentane linkers, whose rigid geometric configuration and substantial torsional energy barriers ensure the retention of a fixed pore aperture (∼4.3 Å). This rigid confinement effect significantly suppresses transient pore expansion, enabling effective ion size sieving while retaining exceptional structural stability. The optimized Zr-FTR-24 membrane exhibits a high Li + permeability of 0.09 mol m −2 h −1 and a Li + /Mg 2+ selectivity of 235, with sustained performance stability over a 7-day continuous operation in mixed-ion solutions. This work establishes a novel design paradigm for suppressing linker dynamics in MOF membranes through rigid linker engineering, ultimately achieving structurally stable and size-exclusive ion transport.
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DOI
高影响因子
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