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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Flexible Mn3O4/MXene Films with 2D–2D Architectures as Stable and Ultrafast Anodes for Li-Ion Batteries

He Chen,Xu Xiao,Qizhen Zhu,Peng Zhang,Xiaoxue Wang,Bin Xu

Mn3O4 is regarded as a promising anode material for lithium-ion batteries (LIBs) based on its ultrahigh theoretical capacity (937 mAh g–1) and low cost but suffers from poor electronic conductivity and large volume variation during the lithiation/delithiation process, which result in dramatic capacity fading and inferior rate capability. Ti3C2Tx MXene, a novel two-dimensional transition metal carbide with metallic conductivity, excellent mechanical properties, and hydrophilic surface, could be an ideal candidate to improve the lithium storage performance of Mn3O4. Here, a unique flexible, 2D–2D Mn3O4/MXene film is fabricated by assembling 2D Mn3O4 with Ti3C2Tx nanosheets through a simple vacuum filtration approach. In this unique 2D–2D nanostructure, MXene nanosheets buffer the volume change of Mn3O4 during the charge/discharge process. Moreover, the introduction of MXene enables the fabricated 2D–2D nanostructure with excellent flexibility and can be directly used as an electrode for LIBs, which is beneficial for enhancing the energy density of the assembled batteries. As a result, the flexible film of Mn3O4-MXene-8-2 shows excellent lithium storage performances in terms of specific capacity (931 mAh g–1 at 0.05 A g–1), rate capability (624 mAh g–1 at 1 A g–1), and cycling stability, demonstrating its great potential for the application in LIBs.

✓ 已验证 DOI 高影响因子
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CERAMICS INTERNATIONAL · 2019 · IF 3.45

Tuning the interface by a soldering method for high performance garnet-type solid-state Li metal battery

Shu Zheng,Zheng Fu,Dongju Dai,Weimin Zhao

Garnet-type solid electrolytes are promising lithium (Li) ion conductors for all-solid-state batteries. However, their poor compatibilities towards Li metal due to their inherently lithiophobic properties severely hinder their practical application in garnet-based solid-state Li metal batteries (SSLBs). Here, we demonstrated a soldering method to modify the surface of garnet ceramic by forming a thin artificial sulfur layer, which results in a homogeneous and stable Li/solid electrolyte interface. This artificial interface effectively enhances the compatibility between the garnet-type solid electrolyte and the Li metal anode . Consequently, the interfacial resistance of sulfur-coated garnet electrolyte is significantly reduced from 1750 Ω cm 2 to 160 Ω cm 2 based on the electrochemical impedance spectroscopy (EIS) measurements on Li symmetric cells. Besides, the symmetric cell exhibits an excellent lifetime of more than 1100 h at a steady state of voltage hysteresis, which indicates a stable and dendrite-free garnet/Li metal interface . The fabricated Li|garnet|LiCoO 2 SSLB using this novel interfacial treatment delivers a high specific capacity of 126 mAh g −1 and good cycling stability.

✓ 已验证 DOI 高影响因子
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JOURNAL OF POWER SOURCES · 2016 · IF 6.333

Structure and electrochemistry of B doped Li(Li0.2Ni0.13Co0.13Mn0.54)1-xBxO2 as cathode materials for lithium-ion batteries

Lingchao Pan,Yonggao Xia,Bao Qiu,Hu Zhao,Haocheng Guo,Kai Jia,Qingwen Gu,Zhaoping Liu

Migration of transition metal (TM) ions to tetrahedral sites plays a crucial role on structural transformation and electrochemical behaviors for Li-rich layered oxides . Here, incorporating small B 3+ in the tetrahedral interstice is employed to block the migration channel of TM ions and stabilize the crystal structure. Benefiting from their good structural stability, Li-rich layered materials with B-doped Li 1.198 Ni 0.129 Co 0.129 Mn 0.535 B 0.01 O 2 and Li 1.196 Ni 0.127 Co 0.127 Mn 0.529 B 0.02 O 2 , exhibit excellent cycling performance and voltage stability. After 51 cycles at 0.2 C, 1 mol.% boron incorporated sample can deliver 211 mAh g −1 with capacity retention of 89.9%, which is much higher than that of the undoped sample of 177 mAh g −1 with the retention of 79.2%. Moreover, the declined voltage per cycle decreases from 3.6885 mV to 2.7530 mV after 2 mol.% boron doping. XRD patterns after extended cycling verified the suppression of the structural transformation by the incorporation of boron.

✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

A ketone-containing all-solid-state polymer electrolyte with rapid Li-ion conduction for lithium metal batteries

Pingping Chen,Qinghui Zeng,Qingyuan Li,Ruihua Zhao,Zhenfeng Li,Xin Wen,Wen Wen,Yu Liu,Anqi Chen,Zengxi Li,Xiangfeng Liu,Liaoyun Zhang

Solid-state polymer electrolytes (SPEs) have gained considerable attention in the application of all-solid-state lithium batteries (ASSLBs), but the low ionic conductivity at room temperature and inferior interfacial compatibility largely drag the practical development of SPEs. Herein, a ketone-containing poly(allyl acetoacetate) (PAAA) based polymer electrolyte is designed and prepared for the first time. The structure of ester and ketone groups provides PAAA polymers with not only strong dissociation of lithium salts but also weak coordination interactions with Li + ions. Thus the prepared PAAA polymer electrolytes show excellent ion conductive behavior with ionic conductivity as high as 1.1 × 10 -4  S cm −1 at 30 °C. Moreover, the PAAA polymer electrolytes still maintain superior viscoelasticity without compromising mechanical integrity. When assembling cells, the reduction-tolerant poly(ethylene oxide) (PEO) polymer electrolytes are employed as interlayers between the PAAA SPEs and lithium electrodes in order to improve interfacial stability. As a result, the hierarchical polymer electrolytes possess wide electrochemical window above 4.8 V, thus matching well with LiFePO 4 or Li 1.2 Ni 0.2 Mn 0.6 O 2 high-voltage cathode. The hierarchical structure does not affect interfacial contact, and the Li/PEO-PAAA-PEO/Li cells show low interfacial resistance and stable striping/plating behavior for at least 500 h at 0.2 mA cm −2 and 60 °C. This study enriches carbonyl-based polymer electrolytes by allying ketone with ester groups, and provides guidance for designing novel high-performance polymer electrolytes for practical application.

✓ 已验证 DOI 高影响因子
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International Journal of Electrochemical Science · 2023 · IF 1.5

Performances of Platinum and nitrogen Dual-Doped Ordered Mesoporous Carbon as Sulfur Host for Li-S Battery

Deyu Qu,Rong Li,Xinxin Zhu,Kai Chen,Yafei Shen,Dan Liu,Zhongyuan Ma,Shichao Zhang,Zhizhong Xie,Junsheng Li,Jiaheng Lei,Haolin Tang

Two types of Resorcinol - Formaldehyde (RF) resin based ordered mesoporous carbon materials were used as sulfur host in lithium sulfur battery system. The effects of carbon material structure, morphology, surface area, pore volume, sulfur loading, electrolyte/sulfur ratio and metallic Pt nanoparticle decoration impact on the adsorption of polysulfides and battery performance are studied. Results show that carbon material carrying rod-like morphology and hexagonal meso-structure can have high sulfur loading due to its high specific surface area and large pore volume. While the one with polyhedral particles and ordered cubic meso-structure exhibits good cyclic stability and good capacity retention due to its good adsorption of polysulfides upon its cage-like pores. After in-situ decorating of Pt nanoparticles, the performance of cyclic stability as well as capacity retention significantly improved and better rate performance is also gained because of the chemisorption of polysulfides and electro-catalytic activity upon Pt.

✓ 已验证 DOI 高影响因子
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ChemElectroChem · 2020 ·Vol. 7 ·期 23 ·4737-4744 · IF 4.154

Restraining Polysulfide with High-Entropy Metal Nitride towards Long Cycle Life and High Capacity Li−S Batteries

Binren Fang,Xiaolu Tian,Te Wang,Tao Wang,Long Qu,Mingtao Li

Graphical Polysulfide anchor : A high-entropy metal nitride (HEMN) was prepared as an innovative anchor to restrain lithium polysulfides via the chemical bonding interaction. The composite of HEMN and sulfur was encased by graphene to reduce the interface resistance. The absorptivity of HEMN and the high conductivity of graphene improves the capacity and cycle stability concurrently because of their synergistic effect. Lithium−sulfur (Li−S) batteries with ultrahigh theoretical specific capacity (1675 mAh g −1 ) have become a research hotpot, which focuses on the solution of shuttle effect of soluble lithium polysulfides (LIPS). Chemical immobilization of LIPS and encapsulation structure of the sulfur cathode are effective strategies to suppress the shuttle effect. Herein, high entropy metal nitride (HEMN) was prepared by mechanochemical-assisted synthesis as an innovative anchor to restrain LIPS via the chemical bonding interaction between HEMN and LIPS. Furthermore, the composite of HEMN and S was encased by graphene (GR) through electrostatic attraction caused by opposite zeta potential, thus as the effective cathode (HEMN/S@GR) of Li−S batteries. HEMN has plentiful active metal sites which can chemically adsorb LIPS, enhancing the cycle life of Li−S batteries. Graphene can accelerate surface charge transfer of sulfur cathode to reduce the interface resistance because of its high conductivity. The initial specific capacity of HEMN/S@GR cathode is 1193 mAh g −1 and still maintains 695 mAh g −1 after 100 cycles at 0.1 C. When increased to 1.0 C, the initial specific capacity is 556 mAh g −1 and exhibits remarkable stability in long cycles. This study presents the synergetic effect of HEMN and graphene on LIPS in Li−S batteries, which introduces a new application way of high entropy materials in the field of energy storage devices.

✓ 已验证 DOI 高影响因子
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

A flexible and highly conductive quasi-solid single-ion polymer electrolyte for high performance Li-metal batteries

Yifeng Cai,Caixia Liu,Zhiao Yu,Haomin Wu,Yaoda Wang,Wencan Ma,Qiuhong Zhang,Xudong Jia

A series of flexible and highly conductive quasi-solid single-ion polymer electrolytes (abbreviated as PU-TFMSI) based on lithium sulfonimide are presented. Owing to the crosslinked structure with three types of segments (hard segment, soft segment and Li rich segment), PU-TFMSI displays a stretchability of 1350% and toughness of 13.6 MJ m −3 . These PU-TFMSI single-ion electrolytes deliver high ionic conductivity over 1.3 × 10 −4  S cm −1 at ambient temperature, a wide electrochemical stability window (up to 5.0 V vs Li + /Li), a high lithium transfer number (LTN ∼ 0.9), and good compatibility with electrodes. The LiFePO 4 /PU-TFMSI-2/Li coin cell exhibits stable cycling with an average Coulombic efficiency of 99.58% and superior rate performance. Furthermore, the LiFePO 4 //Li soft pouch cell with PU-TFMSI-2 single-ion electrolyte maintains functionality under bending. The flexible single-ion polymer electrolytes designed in this study have the potential to be applied in flexible devices and stretchable batteries .

✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

High-performance Li/LiNi0.8Co0.1Mn0.1O2 batteries enabled by optimizing carbonate-based electrolyte and electrode interphases via triallylamine additive

Sen Jiang,Xin Xu,Junying Yin,Yue Lei,Hongtao Guan,Yunfang Gao

Lithium (Li) metal batteries (LMBs), paired with high-energy–density cathode materials , are promising to meet the ever-increasing demand for electric energy storage. Unfortunately, the inferior electrode–electrolyte interfaces and hydrogen fluoride (HF) corrosion in the state-of-art carbonate-based electrolytes lead to dendritic Li growth and unsatisfactory cyclability of LMBs. Herein, a multifunctional electrolyte additive triallylamine (TAA) is proposed to circumvent those issues. The TAA molecule exhibits strong nucleophilicity and contains three unsaturated carbon–carbon double bonds , the former for HF elimination, the later for in-situ passivation of aggressive electrodes. As evidenced theoretically and experimentally, the preferential oxidation and reduction of carbon–carbon double bonds enable the successful regulation of components and morphologies of electrode interfaces, as well as the binding affinity to HF effectively blocks HF corrosion. In particular, the TAA-derived electrode interfaces are packed with abundant lithium-containing inorganics and oligomers , which diminishes undesired parasitic reactions of electrolyte and detrimental degradation of electrode materials . When using the TAA-containing electrolyte, the cell configuration with Li anode and nickel-rich layered oxide cathode and symmetrical Li cell deliver remarkably enhanced electrochemical performance with regard to the additive-free cell. The TAA additive shows great potential in advancing the development of carbonate-based electrolytes in LMBs.

✓ 已验证 DOI 高影响因子
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JOURNAL OF POWER SOURCES · 2021 · IF 9.127

In-situ thermal polymerization boosts succinonitrile-based composite solid-state electrolyte for high performance Li-metal battery

Chuankai Fu,Yulin Ma,Pengjian Zuo,Wei Zhao,Weichao Tang,Geping Yin,Jiajun Wang,Yunzhi Gao

Solid-state electrolytes with high room temperature ionic conductivity , broad electrochemical window, and favorable thermal stability are crucial for the practical application of all-solid-state lithium-metal batteries. Here, a novel succinonitrile (SN)-based composite solid-state electrolyte (SN-CSSE) is fabricated directly inside the glass-fiber (GF) membrane via in-situ thermal-crosslinking ethoxylate trimethylolpropane triacrylate (ETPTA) monomer , coupled with the liquid SN-based electrolyte. The ionic conductivity, oxidation potential and lithium-ion transference number (T Li + ) of SN-CSSE are 0.78 mS/cm, 5.20 V (vs. Li/Li + ) and 0.68 at ambient temperature, respectively. The coin full cells equipped with high-voltage LiCoO 2 (LCO) and modified Li metal anode deliver excellent interfacial stability, cycling reversibility , and rate capability. Moreover, the LCO/SN-CSSE/Li pouch cell exhibits more superior thermal stability than that of cell with commercial carbonate-based electrolyte during thermal shock test.

✓ 已验证 DOI 高影响因子
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Journal of Energy Chemistry · 2020 · IF 7.216

High-performance PVDF-HFP based gel polymer electrolyte with a safe solvent in Li metal polymer battery

Jing Jie,Yulong Liu,Lina Cong,Bohao Zhang,Wei Lu,Xinming Zhang,Jun Liu,Haiming Xie,Liqun Sun

Poly(vinylidenefluoride-co-hexafluoropropylene) (PVDF-HFP) based gel polymer electrolytes are widely studied owing to their electrochemical stability and high dielectric constant. However, most gel polymer electrolytes show unsatisfied safety and interface compatibility due to excessive absorption of volatile and flammable liquid solvents. Herein, by using a safe solvent (N-methyl-2-pyrrolidone) with higher boiling (203 °C) and flash points (95 °C), we initiatively fabricate a flexible PVDF-HFP based gel polymer electrolyte . The obtained gel polymer electrolyte demonstrates a high ionic conductivity of 7.24 × 10 −4  S cm −1 , an electrochemical window of 5.2 V, and a high lithium transference number of 0.57. As a result, the synthesized polymer electrolyte exhibits a capacity retention of 70% after 500 cycles at 0.5 C, and a discharge capacity of 86 mAh g −1 even at a high current rate of 10 C for LiFePO 4 based Li metal batteries. Moreover, a stable Li plating/stripping for more than 500 h is achieved under 0.1 mAh at both room temperature and 70 °C. Our results indicate that the PVDF-HFP polymer electrolyte is promising for manufacturing safe and high-performance Li metal polymer batteries.

✓ 已验证 DOI 高影响因子
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Advanced Materials Interfaces · 2022 ·Vol. 9 ·期 32 ·2201259 · IF 6.389

Phosphate Functionalized Ionic Liquid: An Efficient Li+ Migration Inhibitor and Hole Extraction Accelerator for Perovskite Solar Cells

Wenjing Hou,Yuting Ma,Jin Kang,Yaoming Xiao,Gaoyi Han

Lithium bis(trifluoromethanesulfonyl)imide (Li-TFSI) doped 2,2′,7,7′ -tetrakis( N , N -di-p-methoxyphenylamine)-9,9′-spirobifluorene (Spiro-OMeTAD) is employed as one of the most common hole transport layer. However, the Li + in Li-TFSI is easy to migrate from Spiro-OMeTAD to perovskite and SnO 2 , left the voids/pinholes in perovskite film to accelerate the invasion of oxygen and moisture, and lead to the device degradation. Here, the 1-butyl-3-methyl imidazolium phosphate dibutyl ester ([Bmim] + [DBP] − ) ionic liquid (IL) is prepared and used to modify the perovskite/Spiro-OMeTAD interface in the perovskite solar cells. The coordination interaction between  P  O in [Bmim] + [DBP] − IL and Pb 2+ can improve the morphology of perovskite film by passivating the uncoordinated Pb 2+ defects. The interaction between  P  O and Li + can suppress the undesired Li + migration. The regulated energy level assignment and ion nature of [Bmim] + [DBP] − IL can accelerate the carrier extraction at perovskite/Spiro-OMeTAD interface. The device based on the [Bmim] + [DBP] − IL interface modification yields a highly efficient photoelectric conversion efficiency of 21.16% and improved stability, outperforming that of control (19.31%) devices under the illumination of 100 mW cm −2 (AM 1.5 G).

✓ 已验证 DOI 高影响因子
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Small · 2023 ·Vol. 19 ·期 27 ·2300519 · IF 13.3

A Carbon-Free and Free-Standing Cathode From Mixed-Phase TiO2 for Photo-Assisted Li–CO2 Battery

Lizhen Long,Yaya Ding,Nina Liang,Jun Liu,Fuchi Liu,Sheng Huang,Yuezhong Meng

Li–CO 2 battery provides a new strategy to simultaneously solve the problems of energy storage and greenhouse effect. However, the severe polarization of CO 2 reduction and CO 2 evolution reaction impede the practical application. Herein, anodic TiO 2 nanotube arrays are first introduced as carbon-free and free-standing cathode for photo-assisted Li–CO 2 battery, and the photo-assisted charge and discharge mechanism is first clarified from the perspective of photocatalysis. Mixed-phase TiO 2 exhibits a long cycling life of 580 h (52 cycles) at 0.025 mA cm −2 and delivers a high discharge specific capacity of 3001 µAh cm −2 under UV illumination. The charge voltage dramatically reduces from 4.53 to 3.03 V under UV illumination. The improvement of photo-assisted Li–CO 2 battery performance relies on the synergistic effect of the hierarchical porous structure, strong UV absorption, efficient separation, and transfer of photo-generated electrons and holes at hetero-phase junction, and the facilitation of photo-generated electrons and holes on CO 2 reduction and CO 2 evolution reaction. This work can provide useful guidance for designing efficient photocathode for photo-assisted Li–CO 2 battery and other metal–air batteries.

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