ACTA MATERIALIA
·
2024
·
IF 8.3
Wei Cao,Ziwei Chen,Maolin Yang,Hanxi Guan,Xing Cheng,Ming Zhang,Feng Lin,Yinguo Xiao,Min Ling,Chengdu Liang,Jun Chen
Point defect engineering has garnered widespread application for enhancing the dynamic behavior of anode materials and improving electrochemical performance. Herein, a hybrid point defect strategy is proposed in Ti-based oxide materials to achieve N doping induced oxygen vacancies (OVs) and subsequently accelerated electron mobility and perform better diffusion kinetics. This methodology culminates in the fabrication of self-supported nanotube arrays comprising N-doped OVs-rich TiO 2 (denoted as N-TNTs). Density functional theory (DFT) calculations and electrochemical characterizations validate that, hybrid point defects lead to high electron mobility and perform better diffusion kinetics, as well as higher Li + /Na + ions adsorption energy barrier and diffusion energy barrier, which in turn improves the rate performance and cycling stability. This research provides a forward-looking and feasible strategy for the application of point defect engineering in anode materials.
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高影响因子
Nano Energy
·
2024
·
IF 16.8
Jinwei Chen,Yuxuan Liu,Fanbo Meng,Shiman He,Jun Liu,Yujun Zhao,Kaiqiang Song,Renzong Hu,Min Zhu
Subzero temperature severely forbids the transfer of lithium ion (Li + ) between electrodes and the diffusion of Li + in interphase, which become one of the slowest steps. Especially in silicon-based battery systems, the continuous thickening and poor ionic conductivity of interface make this challenge more prominent. Maintaining a thin interface with superior ionic conductivity is an effective strategy to develop low temperature silicon-based batteries. Herein, a ternary hybrid solid electrolyte interface containing F, N, S was constructed by electrolyte design to improve Li + interface transport kinetics. Benefited from robust mechanical property of inorganics and high ionic conductivity of Li 3 N and Li x SO y , the hybrid interface sustains a thin thickness over cycles and behaves significantly reduced energy barrier for Li + diffusion. Thus, such interface enables Si-C||LCO pouch cell to maintain a high capacity retention of 56.4 % of the room-temperature capacity at −30℃, and retain 87.4 % of the capacity after 200 cycles. Even at −40℃ and a high loading of 3mAh/cm 2 , the cell can still be charged and provide a specific capacity of about 310 mAh/g with almost no capacity attenuation after 50 cycles. This work demonstrates the important role of excellent interface for low temperature silicon-based batteries, and provides a reference for the design of rapid Li + transport interface.
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高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Gaoyu Zhou,Jiangmin Jiang,Qilin Feng,Fei Zhou,Xia Qiu,Yaxin Chen,Xiangkai Kong,Zhicheng Ju,Yanhua Cui,Quanchao Zhuang
Lithium/fluorinated carbon (Li/CF x ) batteries have garnered significant interest because of their exceptionally high theoretical energy density compared to other primary energy storage systems. However, the slow ionic transport of the electrolyte during the discharge phase restricts its ability to achieve the theoretical maximum. Herein, a novel high-concentration electrolyte is proposed based on one salt (lithium tetrafluoroborate (LiBF 4 )) and two high dielectric constant solvents (propylene carbonate (PC) and N,N-dimethylacetamide (DMAC)). This innovative electrolyte formulation has significantly enhanced a notable improvement in the discharge performance of Li/CF x batteries. Specifically, Li/CF x batteries used of the high-concentration electrolyte demonstrate a higher discharge voltage platform of 2.68 V (compared to 2.50 V with a commercial electrolyte) and a higher energy density of 2175 Wh Kg −1 ( vs 1928 Wh Kg −1 with a commercial electrolyte) at a current density of 50 mA g −1 . Notably, the overall performance improvements are largely due to the utilization of a high-concentration electrolyte with high ionic conductivity and regulated solvation structure (with less coordinated solvents), leading to the superior Li + transport and facilitating more effective participation of Li + and CF x in the reaction, thereby boosting capacity. This strategy offers valuable insights into electrolyte design for the improvement of electrochemical performance of Li/CF x batteries.
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POLYMER
·
2024
·
IF 4.1
Yubing Chen,Kunyao He,Xudong Hao,Jie Du
Nowadays, single-ion conducting polymer electrolytes for high efficiency, stable, safe and dendrite-free Li-metal batteries are in great need to protect lithium metal anode. In this work, a boron-containing single-ion polymer electrolyte (BSPE), prepared by the copolymerization of allyl diglycol carbonate (ADC), lithium bis((trifluoromethyl)sulfonyl)amide (LiTFSI), and diisopropyl allylboronate (DPAB). The weak coordination interaction between Li + and polar carbonate enhances Li + transport ability. Further, the boron-containing cross-linker fixes the counter anions on the polymer backbones, limiting the movement of the anions and promoting the rapid and uniform Li + transference. The BSPE with 3 wt% DPAB exhibits higher Li + transference number ( t + = 0.77) and better ionic conductivity (1.36 × 10 −4 S cm −1 at 25 °C) compared with that without DPAB. The wider electrochemical window (5.6 V vs. Li + /Li), stable polarization and suppressed lithium dendrites during the plating/stripping cycle at a current density of 0.2 mAcm −2 for 600 h provide the metal-lithium batteries with better safety and higher efficiency. In addition, the initial discharge capacity of LiFePO 4 /BSPE/Li is 140.7 mAh g −1 with 95.2 % coulombic efficiency, and the capacity retention still remains 98.7 % after 200 cycles at 0.1C. The excellent performance endows the BSPE with the potential application in high-performance lithium metal batteries.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xianyu Sun,Shiqin Xu,Yuelin Jin,Tao Cai,Xiaodong Wang,Hongqing Niu,Dezhen Wu
Global demand for lithium (Li) is experiencing a significant growth. A green and effective solution has been devised to address the increasing demand for resource recovery of Li from recycled Li-ion batteries. The objective of this study was to chemically graft 4′-Aminobenzo-15-crown-5-ether (AB15C5) onto polyimide (PI) fiber through a three-step method, resulting in the successful fabrication of AB15C5-functionalized PI fiber (PI-g-AB15C5). The PI-g-AB15C5 fiber exhibits a specific surface area of 2.69 m 2 g −1 as determined by Brunauer-Emmett-Teller analysis. The textiles derived from PI-g-AB15C5 are particularly significant. The textiles exhibit a higher specific surface area and elevated free pore volume, which enhance the full exposure of crown ethers and the adsorption of Li + . The PI-g-AB15C5 fiber exhibits advantageous hydrophilicity, has a significant equilibrium adsorption capacity for Li + (qmax = 21.09 mg g −1 ), demonstrates remarkable repeatability in cycling tests, displays excellent tensile properties, and maintains its fabric morphology during the adsorption process. PI-g-AB15C5 fiber effectively retrieved Li + in an acidic setting. When four interfering ions (Na + , K + , Co 2+ , and Mn 2+ ) were present, the PI-g-AB15C5 fiber demonstrated a remarkable ability to adsorb Li + selectively. The selective separation factors of Li + for Na + , K + , Co 2+ , and Mn 2+ were 8.47, 18.88, 6.99, and 9.85, respectively. A literature survey revealed that PI-g-AB15C5 fiber had better selective separation factors. The selectivity of PI-g-AB15C5 fiber towards Li + is supported by Density Functional Theory (DFT) calculations, which show that the greater Gibbs free energy change of the PI-g-AB15C5–Li + complex (−1008.82 kcal mol −1 ) is responsible for this exceptional selectivity. In summary, the functionality of this study’s polymer fiber material provides an effective method for recovering Li + from recycled Li-ion batteries. It can efficiently adsorb Li + , facilitating their selective separation from other heavy metals.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xinchao Li,Ziyuan Zhou,Kuo Zhao,Jiahui Liu,Zhiqi Liu
Due to the development of new energy vehicle industry, global lithium consumption increases rapidly. Extracting lithium from abundant clay-type lithium ore is an effective strategy to secure a cost-effective lithium supply chain. However, lithium extraction from clay-type lithium ore currently faces with the problems of high solid residue yield and low extraction selectivity for lithium. In addition, the compounds of silicon and alumina in ore processing high economic value are usually ignored. Here, we developed a sustainable process for the comprehensive recovery of Li, Si and Al from clay-type lithium ore by combining NaOH-assisted roasting with sulfuric acid leaching. Firstly, the leaching behavior of lithium under different roasting conditions and acid leaching conditions was systematically investigated. Under the optimal acid leaching condition, the lithium leaching rate reached 96.8%, while the solid residue yield was only 8% based on the raw ore. Taking advantage of the gelling property of Si/Al-containing leaching solution, a lithium-containing solid was obtained by drying and roasting of the gel product. The selective extraction of lithium was easily achieved by washing the solid with water, and the high-value utilization of solid residues in the whole process to prepare nanowires mullite, alumina and corundum was realized. The mechanisms of multi-element recovery elucidated that the formation of nepheline phase during NaOH-assisted roasting promotes the efficient leaching of lithium and reduces the solid residue by acid leaching. After roasting of gel product, Si and Al combined to form mullite, while lithium remained in a free state, allowing further selective lithium elution by water and simultaneous recovery of Si and Al. This work provides fresh perspectives on the sustainable and comprehensive utilization of clay-type lithium ore.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Hanyan Wu,Ming Jiang,Xuejie Gao,Xinyang Chen,Chen Cheng,Shuiping Cai,Wenfeng Ren,Xiaofei Yang,Runcang Sun
The shuttle effect, sluggish conversion kinetics, and uncontrollable lithium dendrites seriously hinder the practical application of lithium-sulfur (Li-S) batteries. Among many modified materials, covalent organic frameworks (COFs) stand out for their excellent ability to inhibit the shuttle effect, while their role in promoting lithium nucleation and catalyzing the conversion of sulfur species has been largely ignored. In this study, an integrated COF separator (TpPa@2400) is developed as a rapid lithium nucleator and sulfur species catalyst in fast-charging Li-S batteries. According to the adsorption energy and Bader charge results, Li atoms preferentially adsorb onto the surface of the TpPa@2400 separator, and the larger Bader charge value (0.52 |e|) of the TpPa@2400 separator also signifies faster lithium transport, promoting the nucleation of Li ions. Furthermore, density functional theory (DFT) theoretically demonstrates that the TpPa@2400 separator exhibits lower free energy for sulfur species interconversion. As a result, the TpPa@2400 separator enables the Li-Li symmetric cell with an extended cycle life of 6000 h at a current density/capacity of 10 mA cm - 2 /10 mAh cm - 2 . The Li-S battery assembled using the TpPa@2400 separator delivers a high capacity of 1636.4 mAh/g at 0.1C and a rapid sulfur species conversion capacity of 513.8 mAh/g at 2C.
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PubMed
高影响因子
POLYMER
·
2024
·
IF 4.1
Haoyun Deng,Zhixiong Yang,Mengzhen Zhou,Encai Ou,Yanbing Lu,Qiulan Zhou,Kun Liu,Weijian Xu
( Z )-1,3-pentadiene (Zp) exhibits a rigid planar molecular structure and is known for the typical 1,5-sigmatropic hydrogen shift, while it is commonly considered an inert monomer during polymerization. Herein, by utilizing the steric effect of the terminal methyl in Zp, the high trans -1,4-polypentadiene (HTPD) with highly ordered microstructure and well-defined sequence are successfully synthesized using barium dithymol/ tert- butyllithium/ tri -ethylaluminum trimetallic initiators based on anionic polymerization. The significant dependence of polymerization rate and trans -1,4-selectivity on ratio of Ba/Al/Li is demonstrated. The modification in microstructure ( trans -1,4 content ranging from 75 % to 92 %) and stereo-regularity (isotactic triad mm % > 65 %) are confirmed by nuclear magnetic resonance (NMR). Compared with the poly(( Z )-1,3-pentadiene) (PZp) prepared by n -BuLi containing σ -ligand modifiers, the strategy using a large steric initiator to achieve regular insertion of Zp into polymer chains is proved to be effective. Kinetics studies demonstrated that Ba–Al–Li system is characterized by retarded anionic polymerization (RAP), yet it shows a quasi-living process and enabling the preparation of stereometric block polymers such as polyisoprene- b -HTPD (PI- b -HTPD). Thermal performance analysis indicates that the obtained highly ordered polymers show superior thermoplastic properties ( T m = 77.4 °C) with crystallinity as an elastomer. Furthermore, reasonable interpretations for the structure formation, sequence, and rate reduction effected by the Ba/Al/Li trimetallic initiator are proposed.
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Energy & Environmental Science
·
2012
·Vol. 5
·期 5
·6966-6972
·
IF 9.61
Lichao Yin,Jiulin Wang,Fengjiao Lin,Jun Yang,Yanna Nuli
Polyacrylonitrile/graphene (PAN/GNS) composites have been synthesized via an in situ polymerization method for the first time, which serve as a precursor to prepare a cathode material for high-rate rechargeable Li–S batteries. It is observed from scanning electron microscopy (SEM) and transmission electron microscopy (TEM) that the PAN nanoparticles, less than 100 nm in size, are anchored on the surface of the GNS and this unique structure is maintained in the sulfur composite cathode material. The electrochemical properties of the pyrolyzed PAN-S/GNS (pPAN-S/GNS) composite cathode have been evaluated by cyclic voltammograms, galvanostatic discharge–charge cycling and electrochemical impedance spectroscopy. The results show that the pPAN-S/GNS nanocomposite, with a GNS content of ca. 4 wt.%, exhibits a reversible capacity of ca. 1500 mA hg−1sulfur or 700 mA hg−1composite in the first cycle, corresponding to a sulfur utilization of ca. 90%. The capacity retention is relatively stable at 0.1 C. Even up to 6 C, a competitive capacity of ca. 800 mA hg−1sulfur is obtained. The superior performance of pPAN-S/GNS is attributed to the introduction of the GNS and the even composite structure. The GNS in the composite materials works as a three-dimensional (3-D) nano current collector, which could act not only as an electronically conductive matrix, but also as a framework to improve the electrochemical performance.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Run Li,Fan Lan,Lian Tang,Ya Huang,Siming Zhao,Baoshun Wang,Ying Han,Di Gao,Qinyuan Jiang,Yanlong Zhao,Zhuojing Zhao,Fei Wang,Rufan Zhang
Windows through heat exchange play a vital role in energy saving for realizing a net-zero carbon emission society. Dual-band electrochromic (EC) smart windows by dynamically regulate visible (VIS) and near-infrared (NIR) light are necessary for improving both building energy efficiency and habitant comfort. However, the rational design of high-performance electrochromic devices (ECDs) suffers sluggish EC response due to the slow ion transport. In this work, a locally dissociated Li + concept is proposed to construct a solid-state polymer electrolyte (SPE) with ultrafast Li + transport. The succinonitrile (SN) is employed to loosen the Li + -anion pair and the crystallographic C─O chain in the poly(ethylene glycol) methyl ether methacrylate (PEGMA) electrolyte by its strong solvation capability. The as-prepared SPE shows a high ionic conductivity of 6.48 mS cm −1 at 30 °C and a high transmittance of >90%. The SPE-based EC smart windows exhibited a fast switching speed (3.0/3.2 s for coloration/bleaching), a high coloration efficiency (CE) of 373.8 cm 2 C −1 , and a high optical modulation in the full solar spectrum (85%, 70%, 43% at 673, 1200, and 1600 nm, respectively). Finally, the SPE-based EC smart windows shows three working modes with a temperature regulation range of 19.1 °C, exhibiting great potential in practical application.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Ruzhen Zhao,Hao Sun,Lijuan Liu,Qifeng Wei,Xiulian Ren,Ziwen Ying
Lithium and its compounds are important strategic resources for the economy and national defense construction. In the Chinese lithium industry, Qinghai old brine, which is the main source of Li + , contains Mg 2+ as much as 125.6743 g/L, and the effective separation of these two elements has been a challenging task. We designed and synthesized a benzene sulfonamide acid substance N221 with stronger acidity and steric hindrance to effectively extract Li + in high Mg/Li solution. The existing acidic extractants include P204, P507 and Cyanex272, among which N221 has the highest β Li/Mg value and E Li (%) value. The thermodynamic properties of the reaction between N221 and metal ions was explored by means of thermodynamic equilibrium constant and quantum chemical calculation. A large amount of Mg 2+ in salt-lake promoted the extraction of Li + , and the mechanism was revealed by mean of molecular dynamics simulations. After stripping, the final Mg/Li (mol/mol) decreased from 15.80 in the Qinghai old brine to 1.27, which meets the conditions of further refining and can obtain high-purity lithium products. A process for separating Li + from Mg 2+ by benzene sulfonamide acid substance is proposed in this study, and the reasons are explained in depth from the experiments and molecular dynamics simulations. Hence, it can be foreseen that this study also has broad application prospects in the recovery of lithium from spent lithium-ion batteries containing a variety of high-valence metal ions.
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ChemSusChem
·
2011
·Vol. 4
·期 8
·1091-1094
·
IF 6.325
Wen Hu,Xin-bo Zhang,Yong-liang Cheng,Chao-yong Wu,Feng Cao,Li-min Wang
Graphical Crunch time! Or? Pure, single-crystalline β-Ag 0.33 V 2 O 5 nanowires are prepared to serve as electrode materials in lithium-ion batteries. In contrast to stoichiometric counterparts, the structure of the β-Ag 0.33 V 2 O 5 nanowires is retrievable upon repeated lithium-ion displacement/intercalation reactions. The proposed strategy to stabilize the crystal structure of electrode materials based on a displacement/intercalation mechanism shows promise for application in rechargeable lithium-ion batteries.
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高影响因子
危险品化学品经营许可证（带存储）