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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Rational Design of a Cross-Linked Composite Solid Electrolyte for Li-Metal Batteries

Changhao Tian,Mengyuan Song,Jiantao Tang,Haoyang Yuan,Chao Ai,Huajun Cao,Tao Huang,Aishui Yu

The interfacial problem caused by solid–solid contact is an important issue faced by a solid-state electrolyte (SSE). Herein, a cross-linked composite solid electrolyte (CSE) poly(vinylene carbonate) (PVCA)─ethoxylated trimethylolpropane triacrylate (ETPTA)─Li1.5Al0.5Ge1.5(PO4)3 (LAGP) (PEL) is prepared by in situ thermal polymerization. The ionic conductivity and Li+ transference number (tLi+) of PEL increase significantly due to the addition of LAGP, which can reach 1.011 × 10–4 S cm–1 and 0.451 respectively. The electrochemical stable window is also widened to 4.68 V. Benefiting from the integrated interfacial structure, the assembled coin cell shows low interfacial resistance. The all-solid-state NCM622|PEL|Li coin cell exhibits an initial discharge capacity of 169.7 mA h g–1 and 70% capacity retention over 100 cycles at 0.2 C, demonstrating excellent cycling stability.

CAS / MDL: 78-67-1 50-81-7
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Journal of Materials Chemistry A · 2023 ·Vol. 12 ·期 5 ·2760-2770 · IF 11.9

Synchronous stabilization of Li–S electrodes by a 1T MoS2@AAO functional interlayer

Binchao Shi,Yue Wang,Ertai Liu,Shilin Mei,Chang-Jiang Yao

The fast capacity decay and limited cycling life are the two main issues that hinder the practical applications of lithium–sulfur batteries. They are mainly caused by the shuttle effect of polysulfide species and the growth of big lithium dendrites occurring separately on the cathode and anode sides. To simultaneously tackle these problems, we explore a multifunctional interlayer integrating the aligned nanochannel structure of an anodic aluminum oxide (AAO) membrane with porous 1T MoS2 nanotubes (namely MoS2@AAO). Benefiting from the high electronic conductivity, sulfiphilic and lithiophilic properties of 1T MoS2, and the positive surface plus low tortuosity of the straight channels of AAO, the designed interlayer not only guarantees rapid ion/electron transfer and efficacious suppression of the polysulfide shuttle, but also achieves uniform and stable lithium deposition during cycling. Consequently, the MoS2@AAO interlayer exhibits a high capacity retention of 99.6% at 0.2C after 500 cycles and 90.6% at 1.0C after 1000 cycles. The prototype cathode with a sulfur loading of 5 mg cm−2 was also investigated, which exhibited over 96% retention of the initial discharge capacity at 0.1C after 50 cycles. This work provides a new solution for simultaneously stabilizing both the lithium anode and sulfur cathode via an integrating approach.

CAS / MDL: 872-50-4 7704-34-9
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WATER RESEARCH · 2025 · IF 12.4

Lithium complexing strategy based on host-guest recognition for efficient Mg2+/Li+ separation

Xiangmin Xu,Xiaowei Zhu,Jinchao Chen,Xingran Zhang,Zhiwei Wang,Fang Li

Ion selective membranes with precise Mg 2+ /Li + separation have attracted extensive interest in lithium extraction to circumvent the lithium supply shortage. However, realizing this target remains a significant challenge mainly due to a high concentration ratio of Mg 2+ /Li + as well as the relatively close ionic hydration radius and chemical. Herein, inspired by the host-guest recognition between alkali-metal ions and crown ether (CE), a novel approach was proposed to regulate the membrane internal structure by introducing CE to strengthen the complexation between Li + and CE. The CE modified membranes achieved the unique outcome of “Li + rejection-Mg 2+ permeation” deriving from enhanced solubility ( K S ) and retarded diffusivity ( D S ) of Li + compared to that of Mg 2+ . The Mg 2+ /Li + separation factors for MgSO 4 /Li 2 SO 4 and MgCl 2 /LiCl of modified membranes ( i.e., 20.1 and 17.7) are about 21.9 and 19.9 time higher than that of pristine membranes, respectively. The results from density function theory (DFT) indicated that the stronger host-guest interaction between CE and Li + combined them closely, thereby increasing solubility and reducing diffusivity of Li + . Our findings develop a new efficient membrane-based strategy enabling the production of high-purity lithium salts from simulated brine.

CAS / MDL: 4422-95-1
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Journal of Energy Storage · 2023 · IF 9.4

In-situ polymerization of an organic cathode for highly efficient Li-ion batteries

Mingyue Yu,Xiaozhong Yu,Jiahui Hu,Chengbin Tang,Cong Fan

An organic polymer cathode called poly(anthraquinone- alt -benzene) (PAQB) is in-situ synthesized between the monomers of 2,6-dibromoanthraquinone and 1,4-benzenediboronic acid bis(pinacol) ester based on the matrix of carbon nanotube (CNT), leading to the growth of a polymer on CNT (PAQB@C) and the better formation of electron transportation network. After optimization, the sample (PAQB@C) of PAQB grown on 2 wt% CNT shows the best results in Li-ion batteries. In half cells, PAQB@C shows the average discharge potential around 2.2 V (vs. Li + /Li) and peak discharge capacity of 184 mAh g −1 , stably running for 1000 cycles. In full cells with the Li-intercalated graphite (LiC 6 ) as the anode, PAQB@C can deliver the peak discharge capacity of 187 mAh g −1 cathode and peak energy density of 374 Wh kg −1 cathode . And the full cells can show the long lifespan for over 2500 cycles. To the best of our knowledge, the comprehensive performance of PAQB@C is one of the best organic cathodes reported in Li-ion batteries.

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INORGANIC CHEMISTRY COMMUNICATIONS · 2023 · IF 3.8

The enhanced performance of Li-ion batteries based on Co-MOF/MXene composites

Yichong Chen,Jinbing Cheng,Aihua Wang,Congbin Liu,Hailong Yan,Yang Qiu,Zhongzheng Wang,Paul K. Chu,Yongsong Luo

Electrospinning is carried out to fabricate Ti 3 C 2 T x @Co nanocomposite films composed of 2D Ti 3 C 2 -encapsulated Co nanoparticles derived from Co-MOF precursors. The unique 1D nanochain structure inherits not only the high electrochemical activity, but also excellent electron and ionic conductivity. The Co nanoparticles with good conductivity and MXene with high electrochemical activity improve the electrochemical properties giving rise to high capacity and good cycling stability. The Ti 3 C 2 flakes partially accommodate the volume changes during Li + insertion/extraction and the electrospinning technique prevents self-aggregation of Ti 3 C 2 flakes and aggregation of ZIF-67 nanoparticles, consequently producing a larger surface area and more active sites on the flexible anode. As a result, the MXene/Co composite has excellent properties such as a high reversible capacity of 422 mA h g −1 after 500 charging-discharging cycles at a current density of 1 A/g and retained capacity of 177 mA h g −1 at a rate of 5 A/g. The materials and strategy have large potential in commercial energy storage devices.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Polyvinylpyrrolidone-assisted synthesis of ultrathin multi-nanolayered Cu2Nb34O87−x for advanced Li+ storage

Qing Li,Dan Zhao,Shijie Sun,Xing Zhang,Yu Zhang,Chao Li,Yifeng Cheng,Jincang Zhang,Renchao Che

The ultrathin multi-nanolayered structure with ultrathin monolayer thickness (<10 nm) and certain interlayer spacing can significantly shorten Li + paths and alleviate the volume effect for Li + -storage materials. However, unlike layered materials such as MXene and MoS 2 , shear ReO 3 -type niobates have difficulty forming ultrathin multi-nanolayered structures due to their crystal structures, which still remains a challenge. Herein, by a polyvinylpyrrolidone (PVP)-assisted solvothermal method , we first synthesize ultrathin multi-nanolayered Cu 2 Nb 34 O 87−x with oxygen vacancies composed of ultrathin nanolayers (2–10 nm in thickness) and interlayer spacing (1–5 nm). Oxygen vacancies can radically enhance the inherent electronic/ionic conductivity and Li + diffusion coefficient of this material. The PVP-induced formation mechanism of this material is expounded in detail. The well-preserved ultrathin multi-nanolayered structure and excellent multi-electron electrochemical reversibility (Nb 5+  ↔ Nb 4+  ↔N b 3+ and Cu 2+  ↔ Cu + ) of this material during cycling are fully verified. Based on an ultrathin multi-nanolayered structure and oxygen vacancies, this material as the anode of lithium-ion batteries is highly competitive among reported shear ReO 3 -type Cu-Nb-O anodes, displaying a high reversible capacity (315.3 mAh g −1 after 300 cycles at 1 C), durable cycling stability (85.7 % capacity retention after 1000 cycles at 10 C), and outstanding rate performance. Moreover, the application of this material to lithium-ion capacitors generates a large energy density (97.9 Wh kg −1 at 87.5 W kg −1 ) and a high power density (17,500 W kg −1 at 12.6 Wh kg −1 ), thus further indicating its fast faradaic pseudocapacitive behavior for practical applications. The results of this work indicate a breakthrough in synthesizing ultrathin multi-nanolayered shear ReO 3 -type niobates.

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JOURNAL OF SOLID STATE ELECTROCHEMISTRY · 2023 · IF 2.5

Garnet-type double-layer solid electrolyte for dendrite-free solid-state Li batteries

Feng Xingyi,Zeng Yingping,Yan Deen,Zou Hanbo,Yang Wei,Chen Shengzhou

Due to its high energy density and better safety performance, all-solid-state lithium batteries are regarded as important energy storage devices to replace the traditional liquid electrolyte Li-ion batteries. However, the problems of poor wettability of Li metal anode | solid-state electrolyte interface and easy growth of lithium dendrite have not been well solved. Here, we have constructed Fe-doped Li 7-3x Fe x La 3 Zr 2 O 12 (Fe-LLZO) and Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZTO) garnet-type double-layer solid electrolyte. The high density of Li 7-3x Fe x La 3 Zr 2 O 12 electrolyte and its interfacial wettability to Li metal not only effectively reduced the interface impedance between Li and solid electrolyte but also could stably cycle for more than 200 h without the growth of lithium dendrites at the rate of 0.1 mA cm −2 . In addition, the all-solid-state lithium battery (Li|Fe 0.1 -LLZO|LLZTO|LFP) with LiFePO 4 as a cathode also showed excellent cycle stability and C-rate performance.

CAS / MDL: 1309-37-1 20344-49-4
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MATERIALS LETTERS · 2023 · IF 3

Controllable fabrication of micro-nano structure on Al-Li alloy by hydrothermal treatment

Zhengquan Zhang,Yuling Wang

The micro-nano structures were successfully fabricated on Al-Li alloy by adjusting the concentration of sodium formate and controlling the hydrothermal temperature though hydrothermal treatment. The growing directions and morphologies for micro-nano structures were studied. The results show the micro-nano structures were a mixture of AlOOH and Al(OH) 3 with good crystallinity, the intensity of diffraction peaks increases with the increase of sodium formate concentration, and the growing direction of micro-nano structure varied from (2   0   0) at 110 °C and 130 °C to (1   1   1) at 150 °C. The morphologies of the micro-nano structures exhibit patterned surface with overlapping leaf-like nano-plates at 110 °C and 130 °C, nordstandite is predominant, flower-like at 150 °C,aluminum oxide hydroxide is predominant.These findings directly demonstrate that the preferential growing direction and the morphologies of micro-nano structure has been confirmed with the concentration of sodium formate and the hydrothermal temperature.

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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Dual-function LiFePO4 modified separator for low-overpotential and stable Li-S battery

Ming Jin,Rui Gao,Guiru Sun,Haibo Li,Xiangxin Xue,Chaoqun Qu,Nan Li,Yuting Zhang,Zhao Wang,Ming Feng

Lithium sulfide (Li 2 S) compounds as cathode materials for Lithium-sulfur (Li-S) battery have attracted more and more attention recently because of its high specific capacity, lower volume expansion and higher thermal stability of Li 2 S. However, high electrochemical barrier of the Li 2 S cathode and “shuttle effect” from S species on anode still block the development of Li-S batteries. Herein, LiFePO 4 (LFP) is employed as dual-function separator modifier to establish hybrid cathode. The modified separator will reduce overpotential for effective and durable sulfur redox reactions at the same time, it can also efficiently immobilize the lithium polysulfides (LiPSs) through the Lewis acid-base interaction of LiPSs and LFP. The battery systems based on the as-developed LFP modified separator exhibit an excellent rate capability, high sulfur utilization and outstanding cycling performance. The capacity retention can reach 83.9% after 400 cycles at 0.2 C, and the capacity can reach 594 mAh g −1 at up to 2 C. Current facile and low-cost strategy to modified Li-S battery systems on one hand offers an effective pathway to enhance electrochemical performance, on the other hand inspire new strategies on reducing the activation barrier of Li 2 S for improved sulfur electrochemistry as well.

CAS / MDL: 10377-48-7 872-50-4
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JOURNAL OF POWER SOURCES · 2021 · IF 9.127

Spent asphalt-derived mesoporous carbon for high-performance Li/Na/K-ion storage

Mingming Xie,Xiaobo Zhu,Danqing Li,Zhizhao Xu,Yingjia Huang,Huanyi Zha,Mei Ding,Chuankun Jia

Along with the surging demand for rechargeable alkali-ion (Li + , Na + , or K + ) batteries , cost and availability of the battery materials become critical. In this paper, we report the use of spent asphalt , which is widely available and even poses environmental risks, to produce a high-performing universal Li/Na/K-ion host material. Taking advantage of a nano-Fe 2 O 3 template, the spent asphalt is converted into mesoporous carbon with an interconnected three-dimensional porous structure , high surface area, and numerous crystal defects . As an anode material for Li-ion batteries, the mesoporous carbon exhibits a reversible capability of 674.2 mA h g −1 at 0.2 A g −1 as well as excellent rate and cycling performance (258.7 mA h g −1 at 1.0 A g −1 after 1000 cycles) owing to the shortened diffusion path of ion and easier penetration of electrolytes. The carbon anode also delivers superior reversible capacities and cycling stability in Na-ion and K-ion batteries. With the potential to simultaneously tackle energy and environmental problems, the spent asphalt-derived mesoporous carbon is promising for large-scale applications.

CAS / MDL: 1309-37-1 20344-49-4
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GREEN CHEMISTRY · 2021 ·Vol. 23 ·期 16 ·6090-6100 · IF 10.182

Insoluble small-molecule organic cathodes for highly efficient pure-organic Li-ion batteries

Xinxin Wang,Wu Tang,Yang Hu,Wenqiang Liu,Yichao Yan,Liang Xu,Cong Fan

An insoluble small-molecule organic compound [N,N′-bis(2-anthraquinone)]-perylene-3,4,9,10-tetracarboxydiimide (PTCDI-DAQ) can be a high-performance cathode in Li-ion batteries (LIBs). In half cells, PTCDI-DAQ delivers a peak specific capacity of 229 mA h g−1, along with the good retention of 82% over 3 months. Meanwhile, PTCDI-DAQ can still hold a capacity of 46 mA h g−1 at 25 A g−1. By using the reduced state (Li4TP) of lithium terephthalate (Li2TP) as an organic anode in the all-organic Li-ion batteries (OLIBs), our OLIBs can realize a high-energy density of 296 W h kg−1cathode in the voltage range of 0.2–3.2 V and fulfill a long lifespan over 20 000 cycles. To the best of our knowledge, the comprehensive performance of our PTCDI-DAQ II Li4TP OLIBs is currently one of the best pure-organic LIBs in the world.

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Inorganic Chemistry Frontiers · 2021 ·Vol. 8 ·期 14 ·3473-3481 · IF 6.569

An Al–Li alloy/water system for superior and low-temperature hydrogen production

Mili Liu,Hui Liu,Kang Chen,Jiangyong Sun,Hui Wang,Jiangwen Liu,Liuzhang Ouyang

The potential of a multiphase Al–Li alloy with the unreported Al1.08Li1.92 phase for use as a hydrolytic material to produce hydrogen was studied. This alloy enabled rapid hydrogen release in a wide temperature range with robust hydrogen yield. It could produce 1496 ml H2 per g within merely 0.5 min at 299 K and release 1076 ml H2 per g in 0.5 min even at a subzero temperature of 243 K. The hydrogen production kinetics were confirmed with a chemical step and could be well controlled by tailoring the solution components of water/ethanol mixtures. Furthermore, the alloy showed good air-resistance ability, indicating its suitability for safe handling and transport in practical applications. Our results confirmed the excellent hydrogen production achieved using this Al-based generation system. It might shed light on the progress of hydrogen production technologies for commercial use.

CAS / MDL: 7429-90-5
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