SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Qihui Wang,Xingyu Yang,Changwen Li,Chenyu Zhao,Yujie Huang,Shuqi Qiu,Yaru Qin,Chenglong Shi
The titanium-based lithium ion sieve adsorbent H 2 TiO 3 (HTO), known for its structural stability and high adsorption capacity, emerges as a highly promising material. Nonetheless, its precursor, the Li 2 TiO 3 powder (LTO), synthesized via the high-temperature solid-phase method, tends to agglomerate and poses challenges in separation. This agglomeration compromises the adsorption sites and, consequently, its adsorption capacity. To counter this, we employed a strategy of doping LTO with magnetic Fe 3 O 4 nanoparticles as a Fe source, aiming to mitigate the agglomeration issue. Subsequently, Fe-doped H 2 TiO 3 (HFTO) was obtained by acid washing and used to adsorb lithium ions from an aqueous solution. Experimental results revealed that HFTO's equilibrium adsorption capacity for lithium in LiCl solution peaked at 34.27 mg/g. Moreover, even after five cycles of adsorption–desorption, HFTO maintained an adsorption capacity exceeding 32.00 mg/g. Investigations into HFTO's adsorption mechanism, utilizing Raman spectroscopy, FT-IR, and XPS , uncovered that the adsorption of Li + by HFTO occurs through the dissociation of O–H bonds and the subsequent formation of O-Li bonds.
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Shiwei Ge,Qian Zhao,Yaoyang Liu,Fangfang Wang,Guijuan Wei,Yu Liu,Bin Xu
Lithium–sulfur (Li–S) batteries are considered as promising energy storage systems due to the high energy density of 2600 W h kg–1. However, the practical application of Li–S batteries is hindered by the inadequate conductivity of sulfur and Li2S, as well as the shuttle effect caused by polysulfides during the charge–discharge process. Introducing a conductive interlayer between the cathode and the separator to physically resist polysulfides represents an effective and straightforward approach to mitigate the shuttle effect in Li–S batteries. In this paper, an ultrathin (<1 μm) 2D–2D MXene-LDH interlayer with high polysulfide adsorption ability was introduced to Li–S batteries. The synergistic effect between MXene and layered double hydroxide greatly improved the adsorption effect of the interlayers: the conductive Ti3C2Tx MXene chemically adsorbs polysulfides and promotes their fast transfer, and the NiCo-LDH alleviates the restack of MXene and facilitates Li+ diffusion. After inserting the MXene-LDH interlayer, the Li–S batteries exhibit an enhanced specific capacity of 1137.6 mA h g–1 at 0.1 C and retain 622.6 mA h g–1 after 100 cycles. The ultrathin 2D–2D interlayer offers a feasible way for the development of highly efficient and lightweight interlayers in Li–S batteries.
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PubMed
高影响因子
ACS Nano
·
2025
·
IF 16
Chenzhi Ding,Yao Ding,Kao Wang,Zhaobo Zheng,Fang Liu,Xuyun Guo,Mohsen Tamtaji,Zhengtang Luo
Heterojunction engineering, serving as a key framework for building blocks between diverse functional materials, has emerged as a highly promising strategy to address the demand for efficient catalysts in lithium–sulfur (Li–S) batteries. However, achieving full matrix electronic control in the bulk phase is a bottleneck in regulating the electrochemical catalytic behavior of heterostructure catalysts. Herein, we report a “tube-in-tube” multifunctional catalyst that can strengthen the sulfur redox reaction (SRR) in Li–S batteries. Benefiting from a large-scale and oriented two-dimensional (2D) superlattice interface, the tailored heterostructure catalysts (MoSe2/MoS2@CNTs) show a “1 + 1 > 2” synergistic effect in lithium polysulfide (LiPSs) adsorption and catalytic conversion during SRR. In situ studies and theoretical results reveal that this 2D Moiré superlattice interface not only optimizes the adsorption of polysulfides but also moderates the overall electronic density of catalysts. Consequently, Li–S batteries assembled with MoSe2/MoS2@CNTs-PP as a modified separator deliver an outstanding discharge capacity of 1225 mAh g–1 at 0.2 C with a Ketjenblack/S cathode while maintaining a specific capacity of 870 mAh g–1 even at 5 C. Additionally, due to the inhibited “shuttle effect” by heterostructure catalysts, the modified separators exhibit a less capacity fading of 0.063% per cycle after 1000 cycles (1 C) even with a high sulfur loading (3.8 mg cm–2). This work focuses on designing an adsorption–catalysis synergistic interface within a full matrix of catalysts for Li–S chemistry and providing insights into the design of multifunctional catalysts for energy-storage systems based on the catalytic reaction, e.g., Zn–I2 and metal–air batteries, etc.
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PubMed
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 8
·1833
·
IF 4.2
Chen Cheng,Hanyan Wu,Xinyang Chen,Shuiping Cai,Yingkang Tian,Xiaofei Yang,Xuejie Gao
Lithium–sulfur (Li-S) batteries have received much attention due to their high energy density and low price. In recent years, alleviating the volume expansion and suppressing the shuttle effect during the charge and discharge processes of Li-S batteries have been widely addressed. However, the slow conversion kinetics from polysulfide (LiPSs) to Li2S2/Li2S still limits the application of Li-S batteries. Therefore, we designed a ZIF-67 grown on cellulose (named ZIF-67@CL) as an electrocatalyst to improve the interconversion kinetics from LiPSs to Li2S2/Li2S for Li-S batteries. Based on the results of adsorption experiments of LiPSs, ZIF-67@CL and CL hosts were immersed in Li2S4solution to adsorb LiPSs, and the UV-Vis test was conducted on the supernatant after adsorption. The results showed that the ZIF-67@CL had a stronger adsorption for LiPSs compared with the cellulose (CL). Furthermore, in the Li2S nucleation tests, the fabricated cells were galvanostatically discharged to 2.06 V at 0.112 mA and then potentiostatically discharged at 2.05 V. Based on the results of Li2S nucleation tests, the catalytic effect of ZIF-67 was further verified. As a result, the sulfur cathode used a ZIF-67 catalyst (named S/ZIF-67@CL) and delivered an initial capacity of 1346 mAh g−1at a current density of 0.2 C. Even at a high current density of 2 C, it exhibited a high-capacity performance of 1087 mAh g−1on the first cycle and maintained a capacity output of 462 mAh g−1after 150 cycles, with a Coulombic efficiency of over 99.82%.
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PubMed
高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 13
·期 1
·399-408
·
IF 10.7
Qiangfeng Zhang,Shijie Xu,Haipeng Zhu,Zhao Chen,Libao Chen,Chunxiao Zhang,Weifeng Wei
High-voltage lithium-rich manganese-based oxides (LRMOs) are expected to become next-generation mainstream cathodes due to their higher voltage, higher specific capacity and lower cost. However, currently commercialized carbonate electrolytes still face the challenge of poor decomposition of solvents and lithium salts at high voltage, leading to serious interface side reactions and electrochemical performance degradation. Herein, we propose an interfacial chemical modification strategy based on the dual additives of fluoroethylene carbonate (FEC) and tris(trimethylsilyl)phosphate (TMSPa), to promote Li+ migration and ensure long-term cycling stability of LRMO-based batteries. Detailed characterization reveals that the dual additives FEC-TMSPa can promote the desolvation process of Li+ and reduce the adverse decomposition of electrolyte components by regulating the solvation structure of the electrolyte. Simultaneously, dual additives can facilitate the formation of a robust cathode electrolyte interphase (CEI)/solid electrolyte interphase (SEI) rich-in F/P/Si species, thereby reducing the interface side reactions, inhibiting the erosion of acidic substances on electrodes, and promoting the uniform deposition/stripping of Li+. As a result, the high-voltage LRMO-based batteries exhibit excellent rate performance and cycling stability, with a capacity retention of 82.36% after 500 cycles at 30 °C, and 86.9% after 150 cycles at a high-temperature of 55 °C, suggesting that the proposed strategy of synergistically regulating the interface chemistry with multiple additives is anticipated to facilitate the further application of high-voltage layered cathode materials.
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高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Qianwei Zhang,Rong Yang,Chao Li,Meng Luo,Yu Jiang,Chaojiang Fan,Yinglin Yan,Yunhua Xu
Composite solid-state electrolytes have attracted growing attention due to their good flexibility and wide range of interfaces. However, the inherent poor compatibility at the organic–inorganic interface significantly impedes lithium-ion transport, limiting overall electrochemical performance. In this study, a continuous semi-immobilized ionic liquid interface layer (SIL) was constructed on the surface of three-dimensional Li 6.4 La 3 Zr 2 Al 0.2 O 12 (3D-LLZAO). The SIL facilitates Li + adsorption through the pre-exchanged TFSI - anion with Cl - ions in the ionic liquid within the SIL and promotes rapid hops migration of Li + among anionic sites. In addition, the introduced TFSI - anions reduce the interaction between poly(ethylene oxide) (PEO) chains and Li + , thus enhancing ion mobility. Moreover, the SIL effectively regulates the concentration gradient of Li at the electrolyte/anode interface, ensuring uniform Li + nucleation and deposition. As a result, the prepared 10LIP electrolyte exhibits a simulated Li + diffusion coefficient 5.16 times higher than that of the 10LP electrolyte, alongside an ionic conductivity reaching 6.98 × 10 −4 S cm −1 . This work proposes a rational strategy for enhancing interfacial ion transport in composite solid electrolytes via the introduction of a semi-immobilized ionic liquid interface layer at the organic–inorganic interface, offering valuable insights for the lithium-ion transport at organic–inorganic interface.
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高影响因子
ACS Nano
·
2025
·
IF 16
Yuhao Liu,Feng Wu,Zhengqiang Hu,Li Li,Renjie Chen
Lithium–sulfur (Li–S) batteries hold great promise due to their high theoretical energy density yet are plagued by sluggish redox kinetics and the polysulfide shuttle effect. Here, we present a light-activated solid–liquid dual-phase catalytic system that addresses these challenges by integrating soluble cobalt phthalocyanine (CoPc) molecules into the electrolyte and anchoring CoPc/carbon nanotube (CNT) composites onto the cathode. This dual-phase architecture expands the catalytic region from the electrode surface into the bulk electrolyte, establishing a dynamic and spatially extended catalytic microenvironment. Upon light irradiation, photogenerated carriers trigger a cooperative catalytic process, where liquid-phase CoPc selectively adsorbs polysulfides, while solid-phase CoPc/CNT accelerates lithium sulfide (Li2S) nucleation and growth. This synergistic mechanism significantly enhances the electrochemical performance, enabling ultrastable cycling over 2000 cycles at 8C with a capacity decay of only 0.019% per cycle. Furthermore, excellent performance is maintained under practical conditions with high sulfur loading of 10.53 mg cm–2 and low electrolyte/sulfur ratio of 4 μL mg–1. This study demonstrates a scalable strategy for constructing spatiotemporally regulated catalytic domains, providing insights into the design of advanced photoassisted energy storage systems.
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高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 39
·2407128
·
IF 27.4
Jinhui Zhu,Jiayao Luo,Jingyan Li,Senhe Huang,Haozhe Geng,Zhenying Chen,Linan Jia,Yongzhu Fu,Xi Zhang,Xiaodong Zhuang
Compared to lithium (Li) anode, the alloy/Li-alloy anodes show more compatible with sulfide solid electrolytes (SSEs), and are promising candidates for practical SSE-based all-solid-state Li batteries (ASSLBs). In this work, a porous Li–Al alloy (LiAl-p) anode is crafted using a straightforward mechanical pressing method. Various characterizations confirm the porous nature of such anode, as well as rich oxygen species on its surface. To the best knowledge, such LiAl-p anode demonstrates the best room temperature cell performance in comparison with reported Li and alloy/Li-alloy anodes in SSE-based ASSLBs. For example, the LiAl-p symmetric cells deliver a record critical current density of 6.0 mA cm −2 and an ultralong cycling of 5000 h; the LiAl-p|LiNi 0.8 Co 0.1 Mn 0.1 O 2 full cells achieve a high areal capacity of 11.9 mAh cm −2 and excellent durability of 1800 cycles. Further in situ and ex situ experiments reveal that the porous structure can accommodate volume changes of LiAl-p and ensure its integrity during cycling; and moreover, a robust Li inorganics-rich solid electrolyte interphase can be formed originated from the reaction between SSE and surface oxygen species of LiAl-p. This study offers inspiration for designing high-performance alloy anodes by focusing on designing special architecture to alleviate volume change and constructing stable interphase.
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高影响因子
Materials Today
·
2022
·
IF 26.943
Yun Liu,Qi Wang,Lai Chen,Zhiming Xiao,Xinming Fan,Shuailing Ma,Lei Ming,Akhil Tayal,Bao Zhang,Feng Wu,Xing Ou
Nickel-rich layered LiNi x Co y Mn 1- x - y O 2 (NCM, x ≥ 0.83) is considered as a promising cathode material for lithium-ion batteries (LIBs), owing to its satisfying specific energy. However, the undesired phase transformation from layered into rock-salt at the NCM surface will easily induce Li concentration gradient during cycling, which hinders the Li-ions diffusion and leads to the gradual accumulation of inner stress with the appearance of microcracks. Herein, we propose a surficial engineering strategy to promote the Li-ions transmission for single-crystalline LiNi 0.83 Co 0.11 Mn 0.06 O 2 (SCNCM) via Li 1.3 In 0.3 Ti 1.7 (PO 4 ) 3 (LITP) modification. It is noted that, as the fast Li-ion conductor, LITP can accelerate the Li-ions diffusion and alleviate the electrode–electrolyte side reaction simultaneously. More importantly, LITP can serve as the Li-ions regulator, ensuring the homogeneous distribution of Li-ions and minimizing the concentration difference at SCNCM surface. It can relieve the stress induced by the inconsistent Li-ions dispersion, which effectively decreases the degree of structural disordering and lattice mismatch at surface, eventually maintaining the high structure integrity during long-term cycling. As anticipated, even under the harsh testing conditions, the LITP modified SCNCM still can achieve a satisfied reversible capacity of 196.4 mAh g −1 under potential range of 2.75–4.6 V after 200 cycles at 25 °C in coin-type half-cells. Furthermore, it provides an extraordinary capacity retention of 88% in 2.75–4.3 V after 400 cycles at high temperature of 45 °C in pouch-type full-battery.
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高影响因子
SmartMat
·
2023
·Vol. 4
·期 5
·e1200
·
IF 20.4
Jing Li,Dan Liu,Han Sun,Deyu Qu,Zhizhong Xie,Haolin Tang,Jinping Liu
All-solid-state batteries (ASSBs) using sulfide electrolytes hold promise for next-generation battery technology. Although using a pure Li metal anode is believed to maximize battery energy density, numerous recent studies have implicated that Li-ion anodes (e.g., graphite and Si) are more realistic candidates due to their interfacial compatibility with sulfide electrolytes. However, those Li-ion ASSBs suffer from an issue similar to liquid Li-ion batteries, which is a loss of active Li inventory owing to interfacial side reactions between electrode components, resulting in reduced available capacities and shortened cycle life. Herein, for the first time, we explore the potential of Li 3 P for cathode prelithiation of Li-ion ASSBs. We identify that the crystallized Li 3 P (c-Li 3 P) has room-temperature ionic and electronic conductivities of both over 10 −4 S/cm. Such a mixed ion-electron conducting feature ensures that the neat c-Li 3 P affords a high Li + -releasing capacity of 983 mAh/g in ASSBs during the first charging. Moreover, the electrochemical delithiation of c-Li 3 P takes place below 2 V versus Li + /Li, while its lithiation dominates below 1 V versus Li + /Li. Once used as a cathode prelithiation regent for ASSBs, c-Li 3 P only functions as a Li + donor without lithiation activity and can adequately compensate for the Li loss with minimal dosage added. Besides mitigating first-cycle Li loss, c-Li 3 P prelithiation can also improve the battery cyclability by sustained release of low-dosage Li + ions in subsequent cycles, which have been embodied in several full ASSBs by coupling a LiCoO 2 cathode with various types of anodes (including graphite, in foil, Sb, and Si anode). Our work provides a universal cathode prelithiation strategy for high-efficiency Li-ion ASSBs.
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高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Xuecheng Cao,Chaohui Wei,Xiangjun Zheng,Kai Zeng,Xin Chen,Mark H. Rummeli,Peter Strasser,Ruizhi Yang
Lithium–oxygen (Li–O 2 ) batteries have attracted tremendous attention due to their high specific energy density . However, their sluggish conversion kinetics and detrimental parasitic reactions would deteriorate the lifespan of batteries. Herein, a combined density functional theory (DFT) calculation and experimental approach is carried out to design an efficient cathode electrocatalyst for Li–O 2 batteries. A self-supporting film of Ru clusters anchored on Magnéli phase Ti 4 O 7 enriched with oxygen vacancy (Ru/Ti 4 O 7 ) is fabricated upon electrospinning and carbothermal reduction. In such a synergistic configuration of Ru/Ti 4 O 7 hybrid film, the strong metal-support interaction (SMSI) between Ru and Ti 4 O 7 can improve the charge transfer at the interface and enhance the adsorption energy of intermediates, accelerating the reaction kinetics of the formation/decomposition of Li 2 O 2 . Benefitting from this SMSI, the electrochemical stability of Ru/Ti 4 O 7 over cycling is also enhanced. As a result, as-prepared Ru/Ti 4 O 7 cathodes could realize excellent electrochemical performance , including high specific capacity (11000 mAh g –1 ), low discharge/charge polarization (0.36 V), long lifespan (> 100 cycles) and superior rate capability. Furthermore, a flexible Li–O 2 pouch cell, constructed with as-fabricated Ru/Ti 4 O 7 film cathode, lithium foil anode and GPE , can exert an impressive areal capacity of 5 mAh cm –2 with a low voltage gap of 0.82 V in ambient air. This work suggests that the activity of catalysts can be significantly enhanced with interfacial modification, offering an efficient approach for rational designing of electrocatalysts for use in Li–air batteries and beyond.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 35
·2204742
·
IF 19.924
Junze Guo,Weidong Zhang,Zeyu Shen,Shulan Mao,Xinyang Wang,Shichao Zhang,Jiahui Zhang,Yingying Lu
Poly(ethylene oxide) (PEO) based solid-state electrolytes with good chemical stability against Li–metal, provide a promising solution for practical all solid-state Li–metal batteries (ASSLMBs). However, the risk of short circuit using thin PEO under semi-molten state and the oxidative decomposition of PEO by cathodes under high voltage hinder the practical application of PEO-based ASSLMBs. Here, it is found that by readjusting the Li + and e – conductivity at anode/cathode interface by introducing Nanodiamonds (NDs) into PEO electrolytes can greatly improve the electrochemical performance of PEO-based batteries. Under the mediation of high modulus and insulative NDs, the lifespan of Li symmetric cells can increase by 30 times at 0.8 mA cm –2 , and high-voltage Li/LiCoO 2 cells show excellent capacity retention under practical testing conditions (50 µm Li and 30 µm PEO electrolyte).
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高影响因子
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