SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yi-Hong Wu,Wei Guo,Yu-Zhu Sun,Shu-Ying Sun
Coal-based solid waste, as a secondary resource, contains significant quantities of aluminum, silicon, and lithium resources. The desilication solution is a waste solution with low concentrations of lithium ions, which is produced during the resource utilization process of coal-based solid waste. Developing adsorbents with high lithium selectivity and alkaline stability is important for the recovery of lithium in coal-solid waste alkaline leachate. In this study, resin functionalized with 2-hydroxymethyl-12-crown-4 (2H12C4) is prepared by esterification. The reaction conditions, including resin type, reaction temperature, time, and catalyst dosage, are optimized. The selective adsorption of 2H12C4-D113 is evaluated in a simulated desilication solution. The results show that 2H12C4-D113 with high selectivity for Li + adsorption is successfully synthesized at 1 g of 2H12C4 per g of resin, 110 ℃ reaction temperature, 6 h reaction time, 0.5 g of catalyst per g of resin and 1 mol of anhydrous lithium chloride per mol of 2H12C4. The adsorption rate of the 2H12C4-D113 resin is relatively rapid, and its adsorption kinetics satisfy the proposed second-order kinetic curve, and its Li + adsorption capacity is greatly influenced by Li + concentration. The peaking adsorption capacity of this resin is 58.71 mg/g in pure lithium solution (Li + =200 mg/L) with high alkalinity, and the peaking adsorptive capacity is 9 mg/g in the pre-desilication solution (Li + =274 mg/L, Na + =101 g/L). Furthermore, density functional theory (DFT) is utilized to study the selective adsorption mechanisms, geometrical characteristics, and thermodynamic parameters of the complexes between crown ether and different ions. DFT simulation reveals that 2H12C4-D113 has high selectivity for Li + adsorption with a Li + -O bond length of 1.86–1.88 Å, and an adsorption energy of 2H12C4-Li + (−369 KJ/mol) being the highest among the mental ions.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
Membranes
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2021
·Vol. 11
·期 5
·351
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IF 4.106
Shanshan Yang,Shuaijun Yu,Lu Yu,Yuanwei Liu,Junbin Liao,Jiangnan Shen,Congjie Gao
Developing monovalent cation permselective membranes (MCPMs) with high-efficient permselectivity is the core concern in specific industrial applications. In this work, we have fabricated a series of novel cation exchange membranes (CEMs) based on sulfonated polysulfone (SPSF) surface modification by polyethyleneimine (PEI) and 4′-aminobenzo-12-crown-4 (12C4) codeposited with dopamine (DA) successively, which was followed by the cross-linking of glutaraldehyde (GA). The as-prepared membranes before and after modification were systematically characterized with regard to their structures as well as their physicochemical and electrochemical properties. Particularly, the codeposition sequence of modified ingredients was investigated on galvanostatic permselectivity to cations. The modified membrane (M-12C4-0.50-PEI) exhibits significantly prominent selectivity to Li+ions (PMg2+Li+= 5.23) and K+ions (PMg2+K+= 13.56) in Li+/Mg2+and K+/Mg2+systems in electrodialysis (ED), which is far superior to the pristine membrane (M-0,PMg2+Li+= 0.46,PMg2+K+= 1.23) at a constant current density of 5.0 mA·cm−2. It possibly arises from the synergistic effects of electrostatic repulsion (positively charged PEI), pore-size sieving (distribution of modified ingredients), and specific interaction effect (12C4 ~Li+). This facile strategy may provide new insights into developing selective CEMs in the separation of specific cations by ED.Keywords:electrodialysis;monovalent cation permselectivity;codeposition;polyethyleneimine;4′-aminobenzo-12-crown-4
研究领域:
材料科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
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2017
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IF 3.387
Jian Lu,Yingying Qin,Qi Zhang,Yilin Wu,Jiuyun Cui,Chunxiang Li,Liang Wang,Yongsheng Yan
High-selective multilayered Li + -imprinted membranes (Li-IIMs) with enhanced hydrophilicity and stability were developed based on polyether sulfone substrate membranes. The multilayered structure was prepared with polydopamine (pDA) as the interfacial adhesion layer, SiO 2 nanoparticles as the hydrophilic layer and Li + -imprinted polymers as the imprinted layer. The selective “Li + -recognition sites” were formed using 12-crown-4 (12C4) as the adsorbing units. The optimal relative selectivity coefficients (α) of Li + /Na + and Li + /K + reached up to 1.85 and 2.07 with the imprinting factor ( β ) of 2.51, and the high permselectivity factors ( γ ) of Na + /Li + (7.39) and K + /Li + (9.86) were achieved on Li-IIMs. The Langmuir isotherm model and the pseudo-second-order kinetics model best fitted the rebinding data of Li-IIMs, as well as the rebinding capacities reached up to 90.3% of initial binding after 5 cycles of adsorption/desorption and just declined to 88.1% after another 5 cycles a month later. Therefore, the as-prepared Li-IIMs would have potential applications for the separation of lithium ions from salt lake brines.
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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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Erhui Zhang,Weifeng Liu,Qi Liang,Xuguang Liu,Zongbin Zhao,Yongzhen Yang
To meet the requirements of industrial lithium extraction from the simulated acidic leaching solution of fly ash, one novel ion-imprinted graphene-based hybrid aerogel (LIIP@N-CMS/GA) has been developed by a combination of pulse electropolymerization and surface ion imprinting technique. The imprinted film consists of polypyrrole (PPy), graphene oxide (GO), benzo-12-crown 4-ether (B12C4) and nitrogen-doped carbon microspheres/graphene aerogel (N-CMS/GA). By integrating the electric field driving and specific recognition of B12C4 towards Li + , the LIIP@N-CMS/GA electrode achieves excellent ionic separation performance, including high adsorption capacity of 41.05 mg g −1 with superior retention ratio (keeping 91.7% of the initial value even experiencing 10 cycles of electrochemical adsorption–desorption), short equilibration time less than 2 h, and relatively high selectivity separation factor of 51.99, 19.66, 14.37 and 12.40 against Na + , K + , Mg 2+ and Al 3+ , respectively. These performances originate from the synergistic effects of the porous structure of N-CMS/GA with excellent conductivity, specific recognition of B12C4 towards Li + , and electric field driving which accelerates ion transport as well as electron transfer. Therefore, LIIP@N-CMS/GA can act as an outstanding candidate for lithium extraction in acidic environment.
研究领域:
材料科学
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环境工程
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电化学
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纳米技术
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）