Materials Today Chemistry
·
2024
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IF 6.7
Xiangfeng Sun,Xuan Song,Dongxia Li,Yuxin Xue,Yulin Fu,Yuanhao Shi,Zhiqi Li,Chongxian Luo,Qiong Lin,Xuefeng Gui,Jiwen Hu,Kai Xu
Lithium-sulfur batteries (LSBs) have been considered as ideal candidates for next-generation energy storage equipment. However, its development has been hindered by the shuttle effect exhibited by the intermediate lithium polysulfides (LiPSs). To address this problem, covalent organic frameworks (COFs) show great promises as sulfur hosts for LSBs. We devised and synthesized a covalent organic framework (TPAS–TPB–COF) that is rich in redox sites by solution polymerization. The reactive groups in the covalent organic framework nano–channels not only inhibit the shuttling of polysulfides, but also promote the migration of Li ions. Meanwhile, the abundant cavities as well as redox sites in the COF nano–channels achieve a high sulfur loading capacity (∼71 wt%), a strong LiPS adsorption capacity, and facilitate ion diffusion. Based on these advantages, when it is used as a sulfur host for LSBs, our COF system provides a high capacity of 1134 mAh g −1 at 0.2 C (1 C = 1675 mA g −1 ), an outstanding rate capability (560 mAh g −1 at 4 C), and excellent stability.
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Advanced Energy Materials
·
2024
·Vol. 14
·期 11
·2303458
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IF 24.4
Wei Li,Huwei Wang,Jinkai Zhang,Haodong Zhang,Ming Chen,Jiali Wang,Yueteng Gao,Rongyi Zhao,Junyang Hu,Guang Feng,Dengyun Zhai,Feiyu Kang
Various electrolyte additives are developed to construct a cathode electrolyte interphase (CEI) layer for high-voltage LiCoO 2 since the cathode suffers severe interfacial degradation when increasing the cut-off voltage over 4.55 V. However, the CEI derived from the additive sacrificial reaction faces the risk of rupture due to the corrosion reaction and the volumetric variation of the cathode. Herein, a non-passivating cathode interface is realized for 4.6 V LiCoO 2 with a non-sacrificial electrolyte additive (TBAClO 4 ) by regulating the solvent environment at the interface rather than the preferential decomposition for CEI formation. Owing to the novel protection mechanism, the cell performance shows little dependence on the CEI-formation process. Therefore, an ultra-high initial coulombic efficiency (96.63%) and excellent cycling stability (81% capacity retention after 300 cycles) are achieved in Li||LiCoO 2 batteries. Moreover, even with the electrolyte containing 1000 ppm H 2 O, the remarkable water capture ability of the additive together with its interfacial regulation enables the 4.6 V Li||LiCoO 2 battery to retain 80% capacity after 200 cycles. This non-sacrificial strategy provides new insights into high-voltage electrolyte additive design for high-energy-density lithium metal batteries.
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ACS Nano
·
2025
·
IF 16
Kang Hu,Tingsong Hu,Tengyu Yao,Xueliang Cui,Qiuju Li,Laifa Shen
Li–CO2 batteries are considered promising energy storage systems for implementation in space applications. However, unsatisfactory overpotentials and poor cycling stability caused by the sluggish reaction kinetics of CO2 reduction and evolution have greatly limited the practical application of Li–CO2 batteries. Herein, we introduce a redox mediator LiI to stabilize the Bi5O7I photocathode by the successive separation of electrons and holes to accelerate the sluggish kinetics. Under illumination, LiI allows photogenerated holes to preferentially react with I– in the solid–liquid interface, thereby inhibiting the release of I– from Bi5O7I and effectively improving the lifespan of the photocathode. Thus, a high discharging platform of 3.05 V and an ultralow charging platform of 3.09 V are achieved to exhibit an energy efficiency of 98.8%. Moreover, a significantly enhanced reversibility is attained, attributed to the decomposition of Li2CO3, which further extends the cycle life to 250 h. This double-phase catalytic strategy demonstrates effectiveness in the development of high-performance Li–CO2 batteries and other energy storage devices.
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高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Xuekai Zhu,Fangmin Ye,Fuliang Xu,Yongming Jiang,Shuling Fan,Meinan Liu
Lithium (Li) metal anodes (LMA) are regarded as one of the most promising anode candidates due to their high theoretical capacity; however, Li dendrites and the volume expansion issues make their practical application very challenging. Herein, a lightweight and high nitrogen (N)-doped carbon fiber with grafted sphere-like carbon nanotubes (HN-SCNTgCFs) has been successfully fabricated as a Li platting matrix by a two-step strategy of surface engineering including solid resource assisted chemical vapor deposition (solid-CVD) and subsequent electrochemical conversion. Benefitting from this HN-SCNTgCF matrix with a fast Li+ conductor (Li3N), the HN-SCNTgCFs || Li system behaves completely stable, i.e., 900 cycles with a CE of ∼100%; the quasi-Li-anode-free HN-SCNTgCFs || LiFePO4 (LFP) cell delivers a long lifespan of 800 cycles; and the Li-HN-SCNTgCFs || LFP cell exhibits long cycling stability (1000 cycles) with a low capacity decay of 0.057 mA h g–1 per cycle. These excellent results suggest that surface engineering is a feasible strategy for constructing an effective Li matrix to stabilize LMA.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Tinghui An,Nan Wang,Jiaqi Li,Yuhao Wang,Zongxuan Bai,Dong Xiang,Kedi Cai
Cu-based electrocatalysts possesses superior potential to produce energy-dense fuels and value-added chemicals in electrocatalytic CO 2 reduction reaction (eCO 2 RR). Nevertheless, the desperately desired target C 2 selectivity is fundamentally constrained by inevitable hydrogen evolution reaction (HER), C 1 products competition and sluggish reaction kinetics, especially for ethanol. Herein, the strategy of introducing Mg on CuO is proposed to aim at modulating adsorption energetics of oxygen-associated active species, which can effectively suppress competing pathways while boosting ethanol production. Benefitting from the modified electronic structure and lattice compressive strain induced by Mg-doping, Mg 0.34 @CuO exhibited 77.5 % of C 2 FE with remarkable stability, in which FE C2H5OH could reach 48.5 % with total current density of 245.5 mA cm −2 . Density functional theory (DFT) calculation revealed that Mg-doped Cu surface exhibits multiple catalytic function, such as suppressed HER, increased surface CO coverage and accelerated H 2 O dissociation, which can be conducive to promote ethanol production. Incorporation of Mg significantly reduces the energy barrier for asymmetric CO-CHO coupling reaction and stabilizes C-O bond in *CH 2 CHO intermediate (shared by ethylene (C 2 H 4 ) and ethanol (C 2 H 5 OH)) by enhancing d-p orbital coupling, thus prioritizing C 2 H 5 OH pathway. Furthermore, it could achieve a high discharge capacity of 14944 mAh g −1 and stable charge-discharge operation of 153 cycles in Li-CO 2 batteries that utilize Mg 0.34 @CuO as cathode material. This work demonstrates a generalizable approach to regulate eCO 2 RR activity and selectivity, and meanwhile shows great application potential in rechargeable Li-CO 2 batteries.
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Nano Materials Science
·
2025
·
IF 17.9
Yang He,Qingling Ruan,Han Kang,Ling Ye,Ya-Xiong Wang,Tiefeng Liu,Hairong Cheng,Xingxing Gu
Li-S batteries (LSBs), with their exceptional theoretical energy density, are widely recognized as a leading option for future energy storage solutions. Nevertheless, on the way to commercialization, the poor conductivity of the positive electrode, the easy dissolution loss of the active substance, and the serious dendrite growth of the negative electrode are stumbling blocks. Therefore, this work designs a novel tungsten and nitrogen-co-doped nanoporous carbon (W,N-C) with multifunction: chemically adsorbs the polysulfides to inhibit shuttling behavior, accelerates Li + transfer, and catalyzes polysulfides redox to address the aforementioned issues of LSBs. As expected at the beginning of the design, the prepared W,N-C-5/S composites cathodes demonstrate excellent performances, i.e., delivering an initial capacity of 944.9 mAh g −1 and a reversible capacity of 771.7 mAh g −1 after 500 cycles at 1 C, significantly outperforming the N-C/S contrast sample. The proposed method offers a feasible solution for boosting the electrochemical performance of LSBs.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Xiaoming Zhang,Wen Xie,Xiaolei Zhou,Wenjie Zhang,Jiawei Wen,Xin Wang,Guoyong Huang,Shengming Xu
A green environmental protection and enhanced leaching process was proposed to recover all elements from spent lithium iron phosphate (LiFePO 4 ) lithium batteries. In order to reduce the influence of Al impurity in the recovery process, NaOH was used to remove impurity. After impurity removal, the spent LiFePO 4 cathode material was used as raw material under the H 2 SO 4 system, and the pressure oxidation leaching process was adopted to achieve the preferential leaching of lithium. The E-pH diagram of the Fe-P-Al-H 2 O system can determine the stable region of each element in the recovery process of spent LiFePO 4 Li-batteries. Under the optimal conditions (500 r·min –1 , 15 h, 363.15 K, 0.4 MPa, the liquid-solid ratio was 4:1 ml·g –1 and the acid-material ratio was 0.29), the leaching rate of Li was 99.24%, Fe, Al and Ti were 0.10%, 2.07% and 0.03%, respectively. The Fe and P were precipitated and recovered as FePO 4 ∙2H 2 O. The kinetic analysis shows that the process of high-pressure acid leaching of spent LiFePO 4 materials depends on the surface chemical reaction. Through the life cycle assessment (LCA) of the spent LiFePO 4 whole recovery process, eight midpoint impact categories were selected to assess the impact of recovery process. The results can provide basic environmental information on production process for recycling industry.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Shenghao Zhang,Yun Chen,Lingjie Huang,Mengyu Liu,Qingliang Lv,Zexing Wu,Jianping Lai,Yuanxiang Gu,Lei Wang,Caixia Li
Sluggish Li + ion transference kinetics and high flammability strictly hinder the practical application of lithium batteries based on solid-state polymer electrolytes (SPEs). Herein, guided by theoretical calculation, a modified organic flame retardant synthesized by blending diphenyl phosphoryl chloride and resveratrol is designed, named as DPPR and displays superior compatibility with polyethylene oxide (PEO) by hydrogen bonds. Thus, the as-constructed versatile electrolyte system (P-DPPR) can improve mechanical, flame-retardant, and migration kinetics properties of PEO simultaneously. With P-DPPR electrolyte, the Li//Li cell operates 1000 h at 0.1 cm −1 , DPPR can greatly decrease activation energy from 0.31 eV to 0.16, Li + transference number of DPPR is 0.76, the LiFePO 4 //Li cell can work from −10 to 60 °C and achieves high-capacity retention rate of 97.2 % after 100 cycles at 25 °C. As revealed by in-situ tests and simulation, the fast ion conductivity can be ascribed to the synergistic effect from promoted dissociation of LiTFSI by π-π interaction, and the accelerated delivery by P O sites in P-DPPR. This work fabricates a composite SPE with high stability, fast kinetics, and safety capabilities, offering a novel perspective for the design of intrinsically safe batteries.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Tiansheng Gao,Yuqian Yang,Wenzhong Ma,Xiaoyi Zhang,Haicun Yang,Qiuyan Bi,Jing Zhong,Hideto Matsuyama
Positively charged nanofiltration membranes effectively extract lithium resources from brine due to their excellent ion selectivity. However, current positively charged nanofiltration membranes generally suffer from low permeation flux and poor lithium ion transport efficiency. To address these issues, constructing nanoscale channels with precise ion sieving capability within nanofiltration membranes has become a recent research focus. In this study, a novel nanochannel material—quaternized γ-cyclodextrin (Q-γ-CD)—was synthesized. Q-γ-CD contains positively charged quaternary ammonium groups on its surface, which can enhance the positive charge density of the membrane surface, thereby improving the rejection of divalent cations (such as Mg 2+ ). Meanwhile, the cavity size and hydrophobic inner cavity of Q-γ-CD provide rapid transport pathways for lithium ions and water molecules. By introducing Q-γ-CD into an aqueous solution containing polyethyleneimine (PEI) and using trimesoyl chloride (TMC) as the organic-phase monomer, a high-performance PEI/Q-γ-CD/TMC nanofiltration membrane was fabricated. Under optimal formulation conditions, the fabricated nanofiltration membrane exhibited a thin separation layer (≤100 nm), a pore size of approximately 0.45 nm, and a high surface charge (isoelectric point, ≥ 9). Thanks to the precise ion-sieving nanochannels provided by Q-γ-CD, the membrane’s pure water flux increased to 13.34 L·m −2 ·h −1 ·bar −1 , while the rejection of magnesium ions reached 97.8 %, and the Li + /Mg 2+ separation factor achieved a value of 18.5. This study presents a novel design strategy for positively charged nanofiltration membranes, offering theoretical support and practical guidance for achieving efficient magnesium-lithium separation.
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Journal of Energy Storage
·
2025
·
IF 9.8
Yu Cao,Chao Ma,Qingxu Zhang,Xixi Shi,Gang Liu,Xizheng Liu
Silicon-based anodes are the most promising candidates for advanced Li ion batteries (LIBs) with energy density over 400 Whkg −1 due to its high theoretical specific capacity. However, their scale applications are still restricted by the performance fading due to particle pulverization, electrode fracture as well as high production cost. Herein, we report a hierarchical porous structured SiO x (HP-SiO x ) prepared by a facile method of etching porous diatomite. It is primarily composed of crystalline silicon and amorphous silicon oxide. The optimized porous HP-SiO x demonstrates a hierarchical pore structure with 20-80 nm pores on the wall of macropores. The macropores could well accommodate the volume expansion during deeply lithiation, while the interconnected pores promote electrolyte permeation. Evaluated as anode in LIBs, it displays a discharge capacity of 668.5 mAhg −1 after 100 cycles, it gives a discharge capacity of 330mAh/g even at a higher current density of 500 mAhg −1 . The thickness of cycled HP-SiOx anode only expands by 60 % after 10 cycles, while other reported SiO anodes normally expand over 110 %. Moreover, the ionic conductivity of HP-SiO x anodes range from 7.24 × 10−9 cm 2 /s to 3.87 × 10−11 cm 2 /s. These improvement in electrochemical performance can be attributed to the fabrication of a hierarchical porous structure, which buffers the volume expansion during lithiation and facilitates ionic transportation within the electrode. The abundant resource of diatomite endows the large-scale, low-cost production of this hierarchical porous SiO x and underscore the potential for commercial applications in lithium-ion batteries.
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Materials Today Communications
·
2025
·
IF 4.5
Zhou Jie,Siyuan Jin,Ruizhi Wu,Xiaochun Ma,Haoran Wang,Mengyao Pang,Zhe Yu,Wang Guixiang,Jinghuai Zhang,Boris Krit,Sergey Betsofen,Neshchimenko Vitalii,Buzikov Ruslan,Min Qiu,Yurong Yang,Jiaming Chen
Due to the poor corrosion resistance of Mg-Li alloys and the limited effectiveness of single surface treatment methods, developing a composite coating is essential to significantly enhance the corrosion protection. In this study, a stable ceramic coating was fabricated on the surface of a Mg-Li alloy by micro-arc oxidation with regulation of the concentration of ZnO nanoparticles added to the electrolyte. Layered double hydroxides (LDH) was subsequently prepared on the coating surface by modulating the hydrothermal temperature, contributing to blocking the micropores and cracks to enhance the compactness of the coating. Additionally, a low-surface-energy hexadecyltrimethoxysilane (HDTMS) was selected to self-assemble on a rough micro/nano structured MAO/LDH coating to obtain a superhydrophobic surface The composite coating exhibited exceptional corrosion resistance, with the R ct value increasing by four orders of magnitude compared to the substrate and the Y 0 (CPE out ) reduced to the 10 -9 range. Furthermore, the coating keeps almost non-corrosion morphology after 7 days of immersion in 3.5% NaCl solution, which is attributed to the combined effects of the superhydrophobicity of HDTMS, the physical barrier effect and chloride ion trapping ability of LDHs, and the reduction in porosity achieved through the incorporation of nano-ZnO in MAO coating.
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DESALINATION
·
2025
·
IF 9.8
Qibiao Chen,Chao Qian,Shaodong Zhou
Global demand for lithium necessitates efficient extraction technologies, especially from low-quality brines with high magnesium-to‑lithium (Mg/Li) ratios, where conventional methods falter. This study presents a novel, quantum chemistry-guided methodology for the rational design of solvent extraction systems to address this challenge. By evaluating lithium binding affinities, triisopropylphenyl phosphate (TiPPP) was identified as a superior extractant. When formulated into an TiPPP-FeCl 3 system, it demonstrated exceptional performance under optimized conditions (90 % vol extractant, Fe/Li molar ratio of 1.2, O/A ratio of 1). In a single stage, the system achieved a lithium extraction efficiency of 92.8 %, corresponding to a remarkable Li/Mg separation factor of 1699. After scrubbing and stripping, the Mg/Li mass ratio in the final product was reduced to 0.0199, a 4156-fold decrease from the initial brine (82.7), outperforming the conventional tributyl phosphate (TBP)-FeCl 3 system. A combination of DFT calculations and spectroscopic analyses (Infrared spectroscopy, Ultraviolet spectroscopy, Raman spectroscopy, and electrospray ionization mass spectrometry) confirmed that the high selectivity is governed by both the electronic environment of the phosphoryl (P=O) group and the steric hindrance effects. This study not only presents a high-performance system for direct lithium extraction but also establishes a rational design paradigm for developing advanced extractants for challenging separation tasks.
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高影响因子
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